Surface-Enhanced Raman Spectroscopy at the Interface between Drug Discovery and Personalized MedicineClick to copy article linkArticle link copied!
- Lamyaa M. AlmehmadiLamyaa M. AlmehmadiDepartment of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United StatesMore by Lamyaa M. Almehmadi
- Igor K. Lednev*Igor K. Lednev*Email: [email protected]Department of Chemistry, University at Albany, State University of New York, 1400 Washington Avenue, Albany, New York 12222, United StatesMore by Igor K. Lednev
Abstract
Personalized medicine and drug discovery are different, yet overlapping, fields, and information from each field is exchanged to improve the other. The current methods used for devising personalized therapeutic plans and developing drug discovery applications are costly, time-consuming, and complex; thus, their applicability is limited in both fields. However, surface-enhanced Raman spectroscopy (SERS) offers potential solutions to current challenges. This Mini-Review explores the utility of SERS in drug discovery and personalized medicine. The Mini-Review starts with a brief overview of these fields, including the main challenges and current methods, and then explores examples where SERS has been used to overcome some of the main challenges in both fields. It ends with brief conclusions, perspectives, and current challenges limiting the practical application of SERS.
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License Summary*
You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below:
Creative Commons (CC): This is a Creative Commons license.
Attribution (BY): Credit must be given to the creator.
*Disclaimer
This summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials.
License Summary*
You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below:
Creative Commons (CC): This is a Creative Commons license.
Attribution (BY): Credit must be given to the creator.
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Special Issue
Published as part of The Journal of Physical Chemistry C special issue “Celebrating 50 Years of Surface Enhanced Spectroscopy”.
1. Introduction
Figure 1
Figure 1. Plasmonic SERS substrates manufactured via top-down and bottom-up fabrication approaches. (a) Top-down approaches enable the fabrication of highly resolved nanostructures, such as nanopillars (reproduced from ref (16). Copyright 2013, American Chemical Society) and bowties (reproduced from ref (17). Copyright 2018, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim). (b) Bottom-up approaches, such as the Langmuir–Blodgett technique (reproduced from ref (29). Copyright 2022, Elsevier Ltd.) and the nanoparticle-on-a-mirror approach (licensed under CC-BY. Reproduced from ref (23)), are more accessible and facilitate the controlled aggregation of nanoparticles that are simpler to fabricate.
2. Drug Discovery and Personalized Medicine Fields
3. SERS Applications for Drug Discovery and Personalized Medicine
3.1. Detection and Monitoring of Validated Biomarkers and Metabolites
Figure 2
Figure 2. Detection of the binding site of the antihypertensive medication, felodipine, to its target protein, oncogenic Aurora A kinase, using label-free SERS by monitoring changes in the protein’s spectral bands. Reproduced with permission from ref (4).
3.2. Detection and Monitoring of Drug Molecules in Biological Matrices
Figure 3
Figure 3. Application of label-free SERS for monitoring the cellular metabolism of a cancer therapeutic by detecting spectral changes associated with changes in the absorption of the drug molecule on nanoparticle surfaces. Reproduced from ref (54). Copyright 2014, American Chemical Society.
3.3. Point-of-Care and Wearable SERS-Based Sensors for Biomarker, Metabolite, and Drug Detection and Monitoring
Figure 4
Figure 4. Wearable and point-of-care SERS-based sensors for detecting biomarkers, metabolites, and drugs. (a) Paper-based SERS substrate for point-of-care drug detection. Reproduced from ref (35). Copyright 2016, Elsevier B.V. (b) Concept of a SERS-based sensor, wearable directly on the skin, for detecting biomarkers and drugs. Reproduced from ref (59). Available under a CC-BY License. Copyright 2022, Limei Liu, Pablo Martinez Pancorbo, Ting-Hui Xiao, Saya Noguchi, Machiko Marumi, Hiroki Segawa, Siddhant Karhadkar, Julia Gala de Pablo, Kotaro Hiramatsu, Yasutaka Kitahama, Tamitake Itoh, Junle Qu, Kuniharu Takei, and Keisuke Goda. Advanced Optical Materials, Wiley-VCH GmbH.
4. Conclusions
Biographies
Lamyaa M. Almehmadi
Lamyaa M. Almehmadi is a Massachusetts Institute of Technology postdoctoral fellow working on developing silicon photonic chip-based sensors. She received her Ph.D. from the University at Albany (State University of New York at Albany). She is the recipient of several awards, including the Rising Star in Analytical Chemistry Award from the American Chemical Society’s (ACS’s) Analytical Chemistry Division and the prestigious Coblentz Society Student Award. Her research experience focuses on the applications of several Raman spectroscopy techniques, including SERS and deep-ultraviolet resonance and standoff Raman spectroscopies.
Igor K. Lednev
Igor K. Lednev is a Williams–Raycheff Endowed Professor in Chemistry and a SUNY Distinguished Professor at the University at Albany (State University of New York at Albany). He served as an advisory member on the White House Subcommittee for Forensic Science. His research focuses on the development and application of laser spectroscopy for forensic investigations, biomedical applications, and fundamental biochemistry. He is a cofounder of startup companies commercializing a universal method for identifying bodily fluid traces for forensic investigations and screening for the early diagnosis of Alzheimer’s disease. He has received several prestigious awards, including the Charles Mann Award for Applied Raman Spectroscopy.
Acknowledgments
This work was supported in part by a National Science Foundation grant (2233317). I.K.L. acknowledges the Williams–Raycheff Endowment. L.M.A. would like to acknowledge the KACST-MIT IBK fellowship.
References
This article references 62 other publications.
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- 4Karthigeyan, D.; Siddhanta, S.; Kishore, A. H.; Perumal, S. S. R. R.; Ågren, H.; Sudevan, S.; Bhat, A. V.; Balasubramanyam, K.; Subbegowda, R. K.; Kundu, T. K. SERS and MD simulation studies of a kinase inhibitor demonstrate the emergence of a potential drug discovery tool. Proc. Natl. Acad. Sci. U.S.A. 2014, 111 (29), 10416– 10421, DOI: 10.1073/pnas.1402695111Google Scholar4https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhtVOitL%252FF&md5=721cbafc3606ace6c0ae0834e63eb9f4SERS and MD simulation studies of a kinase inhibitor demonstrate the emergence of a potential drug discovery toolKarthigeyan, Dhanasekaran; Siddhanta, Soumik; Kishore, Annavarapu Hari; Perumal, Sathya S. R. R.; Agren, Hans; Sudevan, Surabhi; Bhat, Akshay V.; Balasubramanyam, Karanam; Subbegowda, Rangappa Kanchugarakoppal; Kundu, Tapas K.; Narayana, ChandrabhasProceedings of the National Academy of Sciences of the United States of America (2014), 111 (29), 10416-10421CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)The authors demonstrate the use of surface-enhanced Raman spectroscopy (SERS) as an excellent tool for identifying the binding site of small mols. on a therapeutically important protein. As an example, the authors show the specific binding of the common antihypertension drug felodipine to the oncogenic Aurora A kinase protein via hydrogen bonding interactions with Tyr 212 residue to specifically inhibit its activity. Based on SERS studies, mol. docking, mol. dynamics simulation, biochem. assays, and point mutation-based validation, the authors demonstrate the surface-binding mode of this mol. in two similar hydrophobic pockets in the Aurora A kinase. These binding pockets comprise the same unique hydrophobic patches that may aid in distinguishing human Aurora A vs. human Aurora B kinase in vivo. The application of SERS to identify the specific interactions between small mols. and therapeutically important proteins by differentiating competitive and noncompetitive inhibition demonstrates its ability as a complementary technique. The authors also present felodipine as a specific inhibitor for oncogenic Aurora A kinase. Felodipine retards the rate of tumor progression in a xenografted nude mice model. This study reveals a potential surface pocket that may be useful for developing small mols. by selectively targeting the Aurora family kinases.
- 5Nie, S.; Emory, S. R. Probing Single Molecules and Single Nanoparticles by Surface-Enhanced Raman Scattering. Science 1997, 275 (5303), 1102– 1106, DOI: 10.1126/science.275.5303.1102Google Scholar5https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaK2sXhtlGlsL4%253D&md5=e8968fee3a48e1f3131e8bebcc40e2b0Probing single molecules and single nanoparticles by surface-enhanced Raman scatteringNie, Shuming; Emory, Steven R.Science (Washington, D. C.) (1997), 275 (5303), 1102-1106CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)Optical detection and spectroscopy of single mols. and single nanoparticles were achieved at room temp. using surface-enhanced Raman scattering. Individual Ag colloidal nanoparticles were screened from a large heterogeneous population for special size-dependent properties and were then used to amplify the speculation for special size-dependent properties and were then used to amplify the spectroscopic signatures of adsorbed mols. For single rhodamine 6G mols. adsorbed on the selected nanoparticles, the intrinsic Raman enhancement factors were ∼1014 to 1015, much larger than the ensemble-averaged values derived from conventional measurements. This enormous enhancement leads to vibrational Raman signals that are more intense and more stable than single-mol. fluorescence.
- 6Almehmadi, L. M.; Curley, S. M.; Tokranova, N. A.; Tenenbaum, S. A.; Lednev, I. K. Surface Enhanced Raman Spectroscopy for Single Molecule Protein Detection. Sci. Rep. 2019, 9 (1), 12356, DOI: 10.1038/s41598-019-48650-yGoogle Scholar6https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BB3MrhvVGltw%253D%253D&md5=91490421ed336ec38b024dfb51146d62Surface Enhanced Raman Spectroscopy for Single Molecule Protein DetectionAlmehmadi Lamyaa M; Lednev Igor K; Almehmadi Lamyaa M; Tenenbaum Scott A; Lednev Igor K; Curley Stephanie M; Tokranova Natalya A; Tenenbaum Scott AScientific reports (2019), 9 (1), 12356 ISSN:.A two-step process of protein detection at a single molecule level using SERS was developed as a proof-of-concept platform for medical diagnostics. First, a protein molecule was bound to a linker in the bulk solution and then this adduct was chemically reacted with the SERS substrate. Traut's Reagent (TR) was used to thiolate Bovine serum albumin (BSA) in solution followed by chemical cross linking to a gold surface through a sulfhydryl group. A Glycine-TR adduct was used as a control sample to identify the protein contribution to the SER spectra. Gold SERS substrates were manufactured by electrochemical deposition. Solutions at an ultralow concentration were used for attaching the TR adducts to the SERS substrate. Samples showed the typical behavior of a single molecule SERS including spectral fluctuations, blinking and Raman signal being generated from only selected points on the substrate. The fluctuating SER spectra were examined using Principle Component Analysis. This unsupervised statistics allowed for the selecting of spectral contribution from protein moiety indicating that the method was capable of detecting a single protein molecule. Thus we have demonstrated, that the developed two-step methodology has the potential as a new platform for medical diagnostics.
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- 14Cailletaud, J.; De Bleye, C.; Dumont, E.; Sacré, P. Y.; Netchacovitch, L.; Gut, Y.; Boiret, M.; Ginot, Y. M.; Hubert, P.; Ziemons, E. Critical review of surface-enhanced Raman spectroscopy applications in the pharmaceutical field. J. Pharm. Biomed. Anal. 2018, 147, 458– 472, DOI: 10.1016/j.jpba.2017.06.056Google Scholar14https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhtFChtLnP&md5=4c1f92a24ad5cefb070fe13573e9210bCritical review of surface-enhanced Raman spectroscopy applications in the pharmaceutical fieldCailletaud, J.; De Bleye, C.; Dumont, E.; Sacre, P.-Y.; Netchacovitch, L.; Gut, Y.; Boiret, M.; Ginot, Y.-M.; Hubert, Ph.; Ziemons, E.Journal of Pharmaceutical and Biomedical Analysis (2018), 147 (), 458-472CODEN: JPBADA; ISSN:0731-7085. (Elsevier B.V.)A review. Surface-enhanced Raman spectroscopy (SERS) is a sensitive anal. tool used in the pharmaceutical field in recent years. SERS keeps all the advantages of classical Raman spectroscopy while being is more sensitive allowing its use for the detection and the quantification of low-dose substances contained in pharmaceutical samples. However, the anal. performance of SERS is limited due to the difficulty to implement a quant. methodol. correctly validated. Nevertheless, some studies reported the development of SERS quant. methods esp. in pharmaceutical approaches. In this context, this review presents the main concepts of the SERS technique. The different steps that need to be applied to develop a SERS quant. method are also deeply described. The last part of the present manuscript gives a crit. overview of the different SERS pharmaceutical applications that were developed for a non-exhaustive list of pharmaceutical compds. with the aim to highlights the validation criteria for each application.
- 15Li, W.; Zhao, X.; Yi, Z.; Glushenkov, A. M.; Kong, L. Plasmonic substrates for surface enhanced Raman scattering. Anal. Chim. Acta 2017, 984, 19– 41, DOI: 10.1016/j.aca.2017.06.002Google Scholar15https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhtFOjsLvL&md5=e076824ca1500920441ed4db6f187920Plasmonic substrates for surface enhanced Raman scatteringLi, Wenbing; Zhao, Xinchu; Yi, Zhifeng; Glushenkov, Alexey M.; Kong, LingxueAnalytica Chimica Acta (2017), 984 (), 19-41CODEN: ACACAM; ISSN:0003-2670. (Elsevier B.V.)As an advanced anal. tool, surface-enhanced Raman scattering (SERS) has broad applications in identification of colorants in paints and glazes, hazard detection to ensure food safety, biomedicine and diagnosis, environmental monitoring, detection of explosives and forensic science. In this review, main types of plasmonic substrates, which include solid substrate with metallic nanostructures and chem. synthesized noble metal colloids, and their fabrication methods are reviewed. The design principles for fabrication of ultrasensitive plasmonic substrates for SERS are presented from published literature. Finally, various applications of SERS substrates are described, indicating the potential of this technique in practical applications. As an ultrasensitive detection method, SERS is at the core of a rapidly expanding research field.
- 16Yang, J.; Palla, M.; Bosco, F. G.; Rindzevicius, T.; Alstrøm, T. S.; Schmidt, M. S.; Boisen, A.; Ju, J.; Lin, Q. Surface-enhanced Raman spectroscopy based quantitative bioassay on aptamer-functionalized nanopillars using large-area Raman mapping. ACS Nano 2013, 7 (6), 5350– 5359, DOI: 10.1021/nn401199kGoogle Scholar16https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXosVeisLg%253D&md5=ab353addeacf47cd71bc81555a006ddfSurface-Enhanced Raman Spectroscopy Based Quantitative Bioassay on Aptamer-Functionalized Nanopillars Using Large-Area Raman MappingYang, Jaeyoung; Palla, Mirko; Bosco, Filippo Giacomo; Rindzevicius, Tomas; Alstroem, Tommy Sonne; Schmidt, Michael Stenbaek; Boisen, Anja; Ju, Jingyue; Lin, QiaoACS Nano (2013), 7 (6), 5350-5359CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)Surface-enhanced Raman spectroscopy (SERS) has been used in a variety of biol. applications due to its high sensitivity and specificity. Here, we report a SERS-based biosensing approach for quant. detection of biomols. A SERS substrate bearing gold-decorated silicon nanopillars is functionalized with aptamers for sensitive and specific detection of target mols. In this study, TAMRA-labeled vasopressin mols. in the picomolar regime (1 pM to 1 nM) are specifically captured by aptamers on the nanostructured SERS substrate and monitored by using an automated SERS signal mapping technique. From the exptl. results, we show concn.-dependent SERS responses in the picomolar range by integrating SERS signal intensities over a scanning area. It is also noted that our signal mapping approach significantly improves statistical reproducibility and accounts for spot-to-spot variation in conventional SERS quantification. Furthermore, we have developed an anal. model capable of predicting exptl. intensity distributions on the substrates for reliable quantification of biomols. Lastly, we have calcd. the min. needed area of Raman mapping for efficient and reliable anal. of each measurement. Combining our SERS mapping anal. with an aptamer-functionalized nanopillar substrate is found to be extremely efficient for detection of low-abundance biomols.
- 17Zhan, P.; Wen, T.; Wang, Z.-g.; He, Y.; Shi, J.; Wang, T.; Liu, X.; Lu, G.; Ding, B. DNA Origami Directed Assembly of Gold Bowtie Nanoantennas for Single-Molecule Surface-Enhanced Raman Scattering. Angew. Chem., Int. Ed. 2018, 57 (11), 2846– 2850, DOI: 10.1002/anie.201712749Google Scholar17https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXis1Snsr4%253D&md5=ff8d9dd95cc00d4b706454a60aa7c7ebDNA Origami Directed Assembly of Gold Bowtie Nanoantennas for Single-Molecule Surface-Enhanced Raman ScatteringZhan, Pengfei; Wen, Te; Wang, Zhen-gang; He, Yingbo; Shi, Jia; Wang, Ting; Liu, Xinfeng; Lu, Guowei; Ding, BaoquanAngewandte Chemie, International Edition (2018), 57 (11), 2846-2850CODEN: ACIEF5; ISSN:1433-7851. (Wiley-VCH Verlag GmbH & Co. KGaA)Metallic bowtie nanoarchitectures can produce dramatic elec. field enhancement, which is advantageous in single-mol. anal. and optical information processing. Plasmonic bowtie nanostructures were successfully constructed using a DNA origami-based bottom-up assembly strategy, which enables precise control over the geometrical configuration of the bowtie with an ∼5 nm gap. A single Raman probe was accurately positioned at the gap of the bowtie. Single-mol. surface-enhanced Raman scattering (SM-SERS) of individual nanostructures, including ones contg. an alkyne group, was obsd. The design achieved repeatable local field enhancement of several orders of magnitude. This method opens the door on a novel strategy for the fabrication of metal bowtie structures and SM-SERS, which can be used in the design of highly-sensitive photonic devices.
- 18Mehigan, S.; Smyth, C. A.; McCabe, E. M. Bridging the Gap between SERS Enhancement and Reproducibility by Salt Aggregated Silver Nanoparticles. Nanomaterials and Nanotechnology 2015, 5, 5, DOI: 10.5772/60125Google ScholarThere is no corresponding record for this reference.
- 19Goodacre, R.; Graham, D.; Faulds, K. Recent developments in quantitative SERS: Moving towards absolute quantification. TrAC Trends in Analytical Chemistry 2018, 102, 359– 368, DOI: 10.1016/j.trac.2018.03.005Google Scholar19https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXlt1Oiur4%253D&md5=9874c21b4486f154798a2c5cffd7ef8aRecent developments in quantitative SERS: Moving towards absolute quantificationGoodacre, Royston; Graham, Duncan; Faulds, KarenTrAC, Trends in Analytical Chemistry (2018), 102 (), 359-368CODEN: TTAEDJ; ISSN:0165-9936. (Elsevier B.V.)Surface-enhanced Raman scattering (SERS) generates molecularly specific fingerprints of analytes and when the exptl. conditions are carefully controlled this is highly quant. This review critiques the development of quant. SERS from simple univariate assessment of single vibrational modes to multivariate anal. of the whole spectrum for improved quantification. SERS has also been developed for direct multiplex detection and quantification of multiple analytes and this is also discussed, as is the need for LC-SERS for analyte sepn. should multivariate chemometric approaches fail to effect quantification. Finally, to effect abs. quantification with SERS, the concepts of isotopologues is introduced along with the std. addn. method (SAM) and suitable examples that have been developed and exploit these techniques are presented. We believe that SERS will be routinely used for quant. anal. and it is only a matter of time before this technique translates from the lab. to the clin. environment.
- 20Bodelón, G.; Montes-García, V.; López-Puente, V.; Hill, E. H.; Hamon, C.; Sanz-Ortiz, M. N.; Rodal-Cedeira, S.; Costas, C.; Celiksoy, S.; Pérez-Juste, I. Detection and imaging of quorum sensing in Pseudomonas aeruginosa biofilm communities by surface-enhanced resonance Raman scattering. Nat. Mater. 2016, 15 (11), 1203– 1211, DOI: 10.1038/nmat4720Google Scholar20https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhtlSgt7%252FI&md5=bf5a3741d94520e7a953e56ae6449a89Detection and imaging of quorum sensing in Pseudomonas aeruginosa biofilm communities by surface-enhanced resonance Raman scatteringBodelon, Gustavo; Montes-Garcia, Veronica; Lopez-Puente, Vanesa; Hill, Eric H.; Hamon, Cyrille; Sanz-Ortiz, Marta N.; Rodal-Cedeira, Sergio; Costas, Celina; Celiksoy, Sirin; Perez-Juste, Ignacio; Scarabelli, Leonardo; La Porta, Andrea; Perez-Juste, Jorge; Pastoriza-Santos, Isabel; Liz-Marzan, Luis M.Nature Materials (2016), 15 (11), 1203-1211CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)Most bacteria in nature exist as biofilms, which support intercellular signaling processes such as quorum sensing (QS), a cell-to-cell communication mechanism that allows bacteria to monitor and respond to cell d. and changes in the environment. As QS and biofilms are involved in the ability of bacteria to cause disease, there is a need for the development of methods for the non-invasive anal. of QS in natural bacterial populations. Here, by using surface-enhanced resonance Raman scattering spectroscopy, the authors report rationally designed nanostructured plasmonic substrates for the in situ, label-free detection of a QS signaling metabolite in growing Pseudomonas aeruginosa biofilms and microcolonies. The in situ, non-invasive plasmonic imaging of QS in biofilms provides a powerful anal. approach for studying intercellular communication on the basis of secreted mols. as signals.
- 21Benz, F.; Chikkaraddy, R.; Salmon, A.; Ohadi, H.; de Nijs, B.; Mertens, J.; Carnegie, C.; Bowman, R. W.; Baumberg, J. J. SERS of Individual Nanoparticles on a Mirror: Size Does Matter, but so Does Shape. J. Phys. Chem. Lett. 2016, 7 (12), 2264– 2269, DOI: 10.1021/acs.jpclett.6b00986Google Scholar21https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28Xos1Slu7k%253D&md5=7d74ab505397019668d9c60efe9285c8SERS of Individual Nanoparticles on a Mirror: Size Does Matter, but so Does ShapeBenz, Felix; Chikkaraddy, Rohit; Salmon, Andrew; Ohadi, Hamid; de Nijs, Bart; Mertens, Jan; Carnegie, Cloudy; Bowman, Richard W.; Baumberg, Jeremy J.Journal of Physical Chemistry Letters (2016), 7 (12), 2264-2269CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)Coupling noble metal nanoparticles by a 1 nm gap to an underlying Au mirror confines light to extremely small vols., useful for sensing on the nanoscale. Individually measuring 10,000 of such Au nanoparticles of increasing size dramatically shows the different scaling of their optical scattering (far-field) and surface-enhanced Raman emission (SERS, near-field). Linear red shifts of the coupled plasmon modes are seen with increasing size, matching theory. The total SERS from the few hundred mols. under each nanoparticle dramatically increases with increasing size. This scaling shows that max. SERS emission is always produced from the largest nanoparticles, irresp. of tuning to any plasmonic resonances. Changes of particle facet with nanoparticle size result in vastly weaker scaling of the near-field SERS, without much modifying the far-field, and allows simple approaches for optimizing practical sensing.
- 22Zeng, P.; Ma, D.; Zheng, M.; Chen, L.; Liang, H.; Shu, Z.; Fu, Y.; Pan, M.; Zhao, Q.; Duan, H. Flexible plasmonic nanoparticle-on-a-mirror metasurface-enabled substrates for high-quality surface-enhanced Raman spectroscopy detection. Colloid and Interface Science Communications 2023, 55, 100728, DOI: 10.1016/j.colcom.2023.100728Google ScholarThere is no corresponding record for this reference.
- 23Zhang, C.; Yi, P.; Peng, L.; Lai, X.; Chen, J.; Huang, M.; Ni, J. Continuous fabrication of nanostructure arrays for flexible surface enhanced Raman scattering substrate. Sci. Rep. 2017, 7 (1), 39814, DOI: 10.1038/srep39814Google ScholarThere is no corresponding record for this reference.
- 24Romo-Herrera, J. M.; Juarez-Moreno, K.; Guerrini, L.; Kang, Y.; Feliu, N.; Parak, W. J.; Alvarez-Puebla, R. A. Paper-based plasmonic substrates as surface-enhanced Raman scattering spectroscopy platforms for cell culture applications. Materials Today Bio 2021, 11, 100125, DOI: 10.1016/j.mtbio.2021.100125Google ScholarThere is no corresponding record for this reference.
- 25Koh, E. H.; Lee, W.-C.; Choi, Y.-J.; Moon, J.-I.; Jang, J.; Park, S.-G.; Choo, J.; Kim, D.-H.; Jung, H. S. A Wearable Surface-Enhanced Raman Scattering Sensor for Label-Free Molecular Detection. ACS Appl. Mater. Interfaces 2021, 13 (2), 3024– 3032, DOI: 10.1021/acsami.0c18892Google Scholar25https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXjsl2hsw%253D%253D&md5=61192d3b6796e61f6a8c638cadfa5ec8A wearable surface-enhanced raman scattering sensor for label-free molecular detectionKoh, Eun Hye; Lee, Won-Chul; Choi, Yeong-Jin; Moon, Joung-Il; Jang, Jinah; Park, Sung-Gyu; Choo, Jaebum; Kim, Dong-Ho; Jung, Ho SangACS Applied Materials & Interfaces (2021), 13 (2), 3024-3032CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)A wearable surface-enhanced Raman scattering (SERS) sensor has been developed as a patch type to utilize as a mol. sweat sensor. Here, the SERS patch sensor is designed to comprise a sweat-absorbing layer, which is an interface to the human skin, an SERS active layer, and a dermal protecting layer that prevents damage and contaminations. A silk fibroin protein film (SFF) is a basement layer that absorbs aq. solns. and filtrates mols. larger than the nanopores created in the β-sheet matrix of the SFF. On the SFF layer, a plasmonic silver nanowire (AgNW) layer is formed to enhance the Raman signal of the mols. that penetrated through the SERS patch in a label-free method. A transparent dermal protecting layer (DP) allows laser penetration to the AgNW layer enabling Raman measurement through the SERS patch without its detachment from the surface. The mol. detection capability and time-dependent absorption properties of the SERS patch are investigated, and then, the feasibility of its use as a wearable drug detection sweat sensor is demonstrated using 2-fluoro-methamphetamine (2-FMA) on the human cadaver skin. It is believed that the developed SERS patch can be utilized as various flexible and wearable biosensors for healthcare monitoring.
- 26Hidi, I. J.; Jahn, M.; Weber, K.; Bocklitz, T.; Pletz, M. W.; Cialla-May, D.; Popp, J. Lab-on-a-Chip-Surface Enhanced Raman Scattering Combined with the Standard Addition Method: Toward the Quantification of Nitroxoline in Spiked Human Urine Samples. Anal. Chem. 2016, 88 (18), 9173– 9180, DOI: 10.1021/acs.analchem.6b02316Google Scholar26https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhsVehtrjP&md5=fdbdd1e65b53926b3019759de9e0dd82Lab-on-a-Chip-Surface Enhanced Raman Scattering Combined with the Standard Addition Method: Toward the Quantification of Nitroxoline in Spiked Human Urine SamplesHidi, Izabella J.; Jahn, Martin; Weber, Karina; Bocklitz, Thomas; Pletz, Mathias W.; Cialla-May, Dana; Popp, JuergenAnalytical Chemistry (Washington, DC, United States) (2016), 88 (18), 9173-9180CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)The emergence of antibacterial resistance and the development of new drugs lead to a continuous change of guidelines for medical treatments. Hence, new anal. tools are required for the detection of drugs in biol. fluids. In this study, the first surface enhanced Raman scattering (SERS) detection of nitroxoline (NTX) in purified water and in spiked human urine samples is reported. Insights concerning the nature of the mol.-metal interaction and its influence on the overall SERS signal are provided. Furthermore, three randomly collected urine samples originating from a healthy volunteer were spiked to assess the limit of detection (LOD), the limit of quantification (LOQ), and the linear dynamic range of the lab-on-a-chip SERS (LoC-SERS) method for NTX detection in human urine. The LOD is ∼3 μM (0.57 mg/L), LOQ ∼ 6.5 μM (1.23 mg/L) while the linear range is between 4.28 and 42.8 μM (0.81-8.13 mg/L). This covers the min. inhibitory concn. (MIC) values of the most commonly encountered uropathogens. Finally, seven clin. samples having an "unknown" NTX concn. were simulated. The LoC-SERS technique combined with the std. addn. method and statistical data anal. provided a good prediction of the unknown concns. Addnl., it is also demonstrated that the predictions carried out by multicurve resoln. alternating least-squares (MCR-ALS) algorithm provides reliable results, and it is preferred to a univariate statistical approach.
- 27Hidi, I. J.; Jahn, M.; Pletz, M. W.; Weber, K.; Cialla-May, D.; Popp, J. Toward Levofloxacin Monitoring in Human Urine Samples by Employing the LoC-SERS Technique. J. Phys. Chem. C 2016, 120 (37), 20613– 20623, DOI: 10.1021/acs.jpcc.6b01005Google Scholar27https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28Xkt1Cgtbk%253D&md5=79c81f25e4416810684819f0596fa760Toward Levofloxacin Monitoring in Human Urine Samples by Employing the LoC-SERS TechniqueHidi, Izabella J.; Jahn, Martin; Pletz, Mathias W.; Weber, Karina; Cialla-May, Dana; Popp, JuergenJournal of Physical Chemistry C (2016), 120 (37), 20613-20623CODEN: JPCCCK; ISSN:1932-7447. (American Chemical Society)The pharmacokinetics of antibiotics such as levofloxacin exhibits large interindividual differences, questioning the value of fixed dose regimens and warranting individual dosing based on therapeutic drug monitoring. Here, in a proof of principal study, it is shown that levofloxacin can be detected in human urine samples by employing lab-on-a-chip surface enhanced Raman spectroscopy (LoC-SERS). First, artificial urine is used as a matrix in order to get insights into the influence of different parameters such as matrix complexity, aggregation time, and matrix diln. on the overall SERS signal. Second, three anonymized individual and three pooled urine samples originating from patients undergoing either no or unknown medical treatments have been spiked with the target analyte. Measurements were performed with a benchtop and a portable Raman setup. In all six samples urinary levofloxacin concns. between 0.45 mM (162.6 μg/mL) and 1.8 mM (650.5 μg/mL) have been successfully detected. According to the literature, the normal levofloxacin concn. in urine is 1.38 mM ± 0.68 mM with a min. measured concn. of 0.45 mM after 4 h from the administration of a 500 mg dose. The presented results therefore show that LoC-SERS is a promising bioanal. tool for urine anal.
- 28Mühlig, A.; Bocklitz, T.; Labugger, I.; Dees, S.; Henk, S.; Richter, E.; Andres, S.; Merker, M.; Stöckel, S.; Weber, K. LOC-SERS: A Promising Closed System for the Identification of Mycobacteria. Anal. Chem. 2016, 88 (16), 7998– 8004, DOI: 10.1021/acs.analchem.6b01152Google ScholarThere is no corresponding record for this reference.
- 29Han, G.; Liu, S.; Yang, Q.; Zeng, F.; Li, W.; Mao, X.; Xu, J.; Zhu, J. Polymer-grafted nanoparticle superlattice monolayers over 100 cm2 through a modified Langmuir-Blodgett method. Polymer 2022, 259, 125308, DOI: 10.1016/j.polymer.2022.125308Google Scholar29https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XisVKis7zN&md5=43ab108e1408fbfaaaed35975c2a8040Polymer-grafted nanoparticle superlattice monolayers over 100 cm2 through a modified Langmuir-Blodgett methodHan, Guoqiang; Liu, Simeng; Yang, Qi; Zeng, Fanyi; Li, Wang; Mao, Xi; Xu, Jiangping; Zhu, JintaoPolymer (2022), 259 (), 125308CODEN: POLMAG; ISSN:0032-3861. (Elsevier Ltd.)Two-dimensional polymer/nanoparticle (NP) composite superlattice monolayers have attracted great attention, due to their applications in flexible optical, sensing, and electronic devices. The large-scale fabrication of these devices requires large-area superlattice monolayers. However, the prepn. of large-area superlattice monolayers of polymer-grafted NP still faces great challenges. Herein, we report a modified Langmuir-Blodgett method for prepg. large-area superlattice monolayers of polystyrene-grafted gold NPs (AuNP@PS). This method involves two key steps: pre-assembling the AuNP@PS on a liq. surface using mixed high/low-boiling-point solvent as the spreading solvent and then compressing the pre-assembled film in low-boiling-point solvent vapor. The discrete monolayer islands of AuNP@PS are formed in the pre-assembly process. During the surface compression process, the introduction of solvent vapor facilitates the fusion of AuNP@PS islands to form the continuous superlattice monolayers. Otherwise, discrete films with nonuniform thickness are obtained by compression without solvent vapor. This strategy enables the prepn. of large superlattice monolayer films over 100 cm2, which are useful in the manuf. of microelectronic devices.
- 30Jaworska, A.; Fornasaro, S.; Sergo, V.; Bonifacio, A. Potential of Surface Enhanced Raman Spectroscopy (SERS) in Therapeutic Drug Monitoring (TDM). A Critical Review. Biosensors 2016, 6 (3), 47, DOI: 10.3390/bios6030047Google ScholarThere is no corresponding record for this reference.
- 31Cutshaw, G.; Uthaman, S.; Hassan, N.; Kothadiya, S.; Wen, X.; Bardhan, R. The Emerging Role of Raman Spectroscopy as an Omics Approach for Metabolic Profiling and Biomarker Detection toward Precision Medicine. Chem. Rev. 2023, 123 (13), 8297– 8346, DOI: 10.1021/acs.chemrev.2c00897Google ScholarThere is no corresponding record for this reference.
- 32Sausville, E. A. Chapter 30 - Drug Discovery. In Principles of Clinical Pharmacology, 3rd ed.; Atkinson, A. J., Huang, S.-M., Lertora, J. J. L., Markey, S. P., Eds.; Academic Press, 2013; p 507– 515.Google ScholarThere is no corresponding record for this reference.
- 33Hughes, J. P.; Rees, S.; Kalindjian, S. B.; Philpott, K. L. Principles of early drug discovery. Br. J. Pharmacol. 2011, 162 (6), 1239– 1249, DOI: 10.1111/j.1476-5381.2010.01127.xGoogle Scholar33https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3MXivF2lt7o%253D&md5=05a0016f45b155f9fb5822f5c7bcc35dPrinciples of early drug discoveryHughes, J. P.; Rees, S.; Kalindjian, S. B.; Philpott, K. L.British Journal of Pharmacology (2011), 162 (6), 1239-1249CODEN: BJPCBM; ISSN:1476-5381. (Wiley-Blackwell)A review. Developing a new drug from original idea to the launch of a finished product is a complex process which can take 12-15 years and cost in excess of $1 billion. The idea for a target can come from a variety of sources including academic and clin. research and from the com. sector. It may take many years to build up a body of supporting evidence before selecting a target for a costly drug discovery program. Once a target was chosen, the pharmaceutical industry and more recently some academic centers have streamlined a no. of early processes to identify mols. which possess suitable characteristics to make acceptable drugs. This review will look at key preclin. stages of the drug discovery process, from initial target identification and validation, through assay development, high throughput screening, hit identification, lead optimization and finally the selection of a candidate mol. for clin. development.
- 34Dugger, S. A.; Platt, A.; Goldstein, D. B. Drug development in the era of precision medicine. Nat. Rev. Drug Discovery 2018, 17 (3), 183– 196, DOI: 10.1038/nrd.2017.226Google Scholar34https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhvFCjur%252FM&md5=e06762106391d7646c686e6ef773398aDrug development in the era of precision medicineDugger, Sarah A.; Platt, Adam; Goldstein, David B.Nature Reviews Drug Discovery (2018), 17 (3), 183-196CODEN: NRDDAG; ISSN:1474-1776. (Nature Research)A review. For the past three decades, the use of genomics to inform drug discovery and development pipelines has generated both excitement and scepticism. Although earlier efforts successfully identified some new drug targets, the overall clin. efficacy of developed drugs has remained unimpressive, owing in large part to the heterogeneous causes of disease. Recent technol. and anal. advances in genomics, however, have now made it possible to rapidly identify and interpret the genetic variation underlying a single patient's disease, thereby providing a window into patient-specific mechanisms that cause or contribute to disease, which could ultimately enable the 'precise' targeting of these mechanisms. Here, we first examine and highlight the successes and limitations of the earlier phases of genomics in drug discovery and development. We then review the current major efforts in precision medicine and discuss the potential broader utility of mechanistically guided treatments going forward.
- 35Berger, A. G.; Restaino, S. M.; White, I. M. Vertical-flow paper SERS system for therapeutic drug monitoring of flucytosine in serum. Anal. Chim. Acta 2017, 949, 59– 66, DOI: 10.1016/j.aca.2016.10.035Google Scholar35https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28Xhsl2isbrF&md5=58f63a65204dc6068d5351d9545184eeVertical-flow paper SERS system for therapeutic drug monitoring of flucytosine in serumBerger, Adam G.; Restaino, Stephen M.; White, Ian M.Analytica Chimica Acta (2017), 949 (), 59-66CODEN: ACACAM; ISSN:0003-2670. (Elsevier B.V.)A no. of life-saving drugs require therapeutic drug monitoring (TDM) for safe and effective use. Currently, however, TDM is performed using sophisticated anal. techniques relegated to central labs, increasing the cost per test and time to answer. Here, using a novel vertical flow membrane system with inkjet-printed surface enhanced Raman sensors, along with a portable spectrometer, we demonstrate a low cost and easy to use device to quantify levels of flucytosine, an antifungal that requires TDM for effective patient care, from undiluted human serum. To our knowledge, this work represents the first report of a passive vertical flow sample cleanup method with surface enhanced Raman detection. We first investigated and optimized the parameters of the vertical flow system for the detection of flucytosine in spiked serum samples. Then, using an optimized vertical-flow system utilizing nitrocellulose membranes and a paper SERS sensor, we achieved detection of down to 10 μg mL-1 flucytosine in undiluted serum, with quant. detection across the entire therapeutic range. This system reduces the assay time to about 15 min, far quicker than the current gold stds. We anticipate that this novel system will enable near-patient therapeutic drug monitoring, leading to the safe and effective administration of a no. of life-saving drugs. Furthermore, it will spawn the development of SERS detection systems capable of sepg. target analytes from real-world biol. matrixes.
- 36Bleker de Oliveira, M.; Koshkin, V.; Liu, G.; Krylov, S. N. Analytical Challenges in Development of Chemoresistance Predictors for Precision Oncology. Anal. Chem. 2020, 92 (18), 12101– 12110, DOI: 10.1021/acs.analchem.0c02644Google ScholarThere is no corresponding record for this reference.
- 37Ludwig, J. A.; Weinstein, J. N. Biomarkers in Cancer Staging, Prognosis and Treatment Selection. Nature Reviews Cancer 2005, 5 (11), 845– 856, DOI: 10.1038/nrc1739Google Scholar37https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2MXht1WitLbP&md5=bfc80c71bccd52dfdbf2cf5a86679c29Biomarkers in cancer staging, prognosis and treatment selectionLudwig, Joseph A.; Weinstein, John N.Nature Reviews Cancer (2005), 5 (11), 845-856CODEN: NRCAC4; ISSN:1474-175X. (Nature Publishing Group)A review. Advances in genomics, proteomics and mol. pathol. have generated many candidate biomarkers with potential clin. value. Their use for cancer staging and personalization of therapy at the time of diagnosis could improve patient care. However, translation from bench to bedside outside of the research setting has proved more difficult than might have been expected. Understanding how and when biomarkers can be integrated into clin. care is crucial if we want to translate the promise into reality.
- 38Dina, N. E.; Tahir, M. A.; Bajwa, S. Z.; Amin, I.; Valev, V. K.; Zhang, L. SERS-based antibiotic susceptibility testing: Towards point-of-care clinical diagnosis. Biosens. Bioelectron. 2023, 219, 114843, DOI: 10.1016/j.bios.2022.114843Google Scholar38https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XislKgsbbK&md5=39071904f91a964c3d0da5d3840ab3c1SERS-based antibiotic susceptibility testing: Towards point-of-care clinical diagnosisDina, Nicoleta Elena; Tahir, Muhammad Ali; Bajwa, Sadia Z.; Amin, Imran; Valev, Ventsislav K.; Zhang, LiwuBiosensors & Bioelectronics (2023), 219 (), 114843CODEN: BBIOE4; ISSN:0956-5663. (Elsevier B.V.)Emerging antibiotic resistant bacteria constitute one of the biggest threats to public health. Surface-enhanced Raman scattering (SERS) is highly promising for detecting such bacteria and for antibiotic susceptibility testing (AST). SERS is fast, non-destructive (can probe living cells) and it is technol. flexible (readily integrated with robotics and machine learning algorithms). However, in order to integrate into efficient point-of-care (PoC) devices and to effectively replace the current culture-based methods, it needs to overcome the challenges of reliability, cost and complexity. Recently, significant progress has been made with the emergence of both new questions and new promising directions of research and technol. development. This article brings together insights from several representative SERS-based AST studies and approaches oriented towards clin. PoC biosensing. It aims to serve as a ref. source that can guide progress towards PoC routines for identifying antibiotic resistant pathogens. In turn, such identification would help to trace the origin of sporadic infections, in order to prevent outbreaks and to design effective medical treatment and preventive procedures.
- 39Zhang, Q.-J.; Chen, Y.; Zou, X.-H.; Hu, W.; Ye, M.-L.; Guo, Q.-F.; Lin, X.-L.; Feng, S.-Y.; Wang, N. Promoting identification of amyotrophic lateral sclerosis based on label-free plasma spectroscopy. Annals of Clinical and Translational Neurology 2020, 7 (10), 2010– 2018, DOI: 10.1002/acn3.51194Google ScholarThere is no corresponding record for this reference.
- 40Zhang, Q.-J.; Chen, Y.; Zou, X.-H.; Hu, W.; Lin, X.-L.; Feng, S.-Y.; Chen, F.; Xu, L.-Q.; Chen, W.-J.; Wang, N. Prognostic analysis of amyotrophic lateral sclerosis based on clinical features and plasma surface-enhanced Raman spectroscopy. Journal of Biophotonics 2019, 12 (8), e201900012, DOI: 10.1002/jbio.201900012Google ScholarThere is no corresponding record for this reference.
- 41Duan, Z.; Chen, Y.; Ye, M.; Xiao, L.; Chen, Y.; Cao, Y.; Peng, Y.; Zhang, J.; Zhang, Y.; Yang, T. Differentiation and prognostic stratification of acute myeloid leukemia by serum-based spectroscopy coupling with metabolic fingerprints. The FASEB Journal 2022, 36 (7), e22416, DOI: 10.1096/fj.202200487RGoogle ScholarThere is no corresponding record for this reference.
- 42Xiao, L.; Bailey, K. A.; Wang, H.; Schultz, Z. D. Probing Membrane Receptor-Ligand Specificity with Surface- and Tip- Enhanced Raman Scattering. Anal. Chem. 2017, 89 (17), 9091– 9099, DOI: 10.1021/acs.analchem.7b01796Google Scholar42https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhtlWnsL%252FE&md5=1ef25ed06378cd9039d88debd66c54e0Probing Membrane Receptor-Ligand Specificity with Surface- and Tip- Enhanced Raman ScatteringXiao, Lifu; Bailey, Karen A.; Wang, Hao; Schultz, Zachary D.Analytical Chemistry (Washington, DC, United States) (2017), 89 (17), 9091-9099CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)The specific interaction between a ligand and a protein is a key component in minimizing off-target effects in drug discovery. Investigating these interactions with membrane protein receptors can be quite challenging. In this report, the authors show how spectral variance obsd. in surface-enhanced Raman scattering (SERS) and tip-enhanced Raman scattering (TERS) can be correlated with ligand specificity in affinity-based assays. Variations in the enhanced Raman spectra of three peptide ligands (i.e., cyclic-RGDFC, cyclic-isoDGRFC, and CisoDGRC), which have different binding affinity to αvβ3 integrin, are reported from isolated proteins and from receptors in intact cancer cell membranes. The SERS signal from the purified proteins provides basis spectra to analyze the signals in cells. Differences in the spectral variance within the SERS and TERS data for each ligand indicate larger variance for nonspecific ligand-receptor interactions. The SERS and TERS results are correlated with single particle tracking expts. of the ligand-functionalized nanoparticles with purified receptors on glass surfaces and living cells. These results demonstrate the ability to elucidate protein-ligand recognition using the obsd. vibrational spectra and provide perspective on binding specificity for small-mol. ligands in intact cell membranes, demonstrating a new approach for investigating drug specificity.
- 43Skinner, W. H.; Robinson, N.; Hardisty, G. R.; Fleming, H.; Geddis, A.; Bradley, M.; Gray, R. D.; Campbell, C. J. SERS microsensors for pH measurements in the lumen and ECM of stem cell derived human airway organoids. Chem. Commun. 2023, 59 (22), 3249– 3252, DOI: 10.1039/D2CC06582GGoogle ScholarThere is no corresponding record for this reference.
- 44Dorato, M. A.; Buckley, L. A. Toxicology Testing in Drug Discovery and Development. Current Protocols in Toxicology 2007, 31 (1), 1, DOI: 10.1002/0471141755.tx1901s31Google ScholarThere is no corresponding record for this reference.
- 45Plou, J.; Molina-Martínez, B.; García-Astrain, C.; Langer, J.; García, I.; Ercilla, A.; Perumal, G.; Carracedo, A.; Liz-Marzán, L. M. Nanocomposite Scaffolds for Monitoring of Drug Diffusion in Three-Dimensional Cell Environments by Surface-Enhanced Raman Spectroscopy. Nano Lett. 2021, 21 (20), 8785– 8793, DOI: 10.1021/acs.nanolett.1c03070Google ScholarThere is no corresponding record for this reference.
- 46Ensom, M. H.; Davis, G. A.; Cropp, C. D.; Ensom, R. J. Clinical pharmacokinetics in the 21st century. Does the evidence support definitive outcomes?. Clin Pharmacokinet 1998, 34 (4), 265– 279, DOI: 10.2165/00003088-199834040-00001Google ScholarThere is no corresponding record for this reference.
- 47Neef, C.; Touw, D.; Stolk, L. Therapeutic Drug Monitoring in Clinical Research. Pharmaceutical Medicine 2008, 22, 235– 244, DOI: 10.1007/BF03256708Google ScholarThere is no corresponding record for this reference.
- 48Panikar, S. S.; Ramírez-García, G.; Sidhik, S.; Lopez-Luke, T.; Rodriguez-Gonzalez, C.; Ciapara, I. H.; Castillo, P. S.; Camacho-Villegas, T.; De la Rosa, E. Ultrasensitive SERS Substrate for Label-Free Therapeutic-Drug Monitoring of Paclitaxel and Cyclophosphamide in Blood Serum. Anal. Chem. 2019, 91 (3), 2100– 2111, DOI: 10.1021/acs.analchem.8b04523Google Scholar48https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXisFyltbfF&md5=940c3e047d427a59c2d990b863b123ffUltrasensitive SERS substrate for label-free therapeutic-drug monitoring of paclitaxel and cyclophosphamide in blood serumPanikar, Sandeep Surendra; Ramirez-Garcia, Gonzalo; Sidhik, Siraj; Lopez-Luke, Tazara; Rodriguez-Gonzalez, Claramaria; Ciapara, Inocencio Higuera; Castillo, Pedro Salas; Camacho-Villegas, Tanya; De la Rosa, ElderAnalytical Chemistry (Washington, DC, United States) (2019), 91 (3), 2100-2111CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Surface-enhanced Raman spectroscopy (SERS) has recently emerged as an innovative tool for therapeutic-drug monitoring (TDM), making it an ideal candidate for personalized treatment. Herein, we report a layer-by-layer (LbL) approach for the fabrication of a highly reproducible hybrid SERS substrate based on graphene oxide (GO)-supported L-cysteine-functionalized starlike gold nanoparticles (SAuNPs). These designed substrates were utilized for TDM of paclitaxel and cyclophosphamide in blood serum. The SAuNPs' efficient binding at the edges of GO creates a better SERS hotspot with enhanced Raman sensitivity because of the spacing of ∼2.28 nm between the SAuNPs. In addn., the hierarchically modified substrate with a self-assembled monolayer of zwitterionic amino acid L-cysteines acts like a brush layer to prevent SERS-hotspot blockages and fouling by blood-serum proteins. The antifouling nature of the substrate was detd. quant. by a bichinchonic acid assay using bovine-serum albumin (BSA) as a protein model on the L-cysteine SAuNPs@GO hybrid substrate (the test) and a cysteamine SAuNPs@GO substrate (the control). The L-cysteine SAuNPs@GO hybrid exhibited 80.57% lower BSA fouling compared with that of the cysteamine SAuNPs@GO substrate. The SERS spectra were acquired within 20 s, with detection limits of 1.5 × 10-8 M for paclitaxel and 5 × 10-9 M for cyclophosphamide in blood serum. Such sensitivities are 4 times and 1 order of magnitude higher than the currently available sophisticated anal. techniques, which involve high costs with each anal.
- 49Litti, L.; Ramundo, A.; Biscaglia, F.; Toffoli, G.; Gobbo, M.; Meneghetti, M. A surface enhanced Raman scattering based colloid nanosensor for developing therapeutic drug monitoring. J. Colloid Interface Sci. 2019, 533, 621– 626, DOI: 10.1016/j.jcis.2018.08.107Google Scholar49https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXhs1CgurjJ&md5=64868c93dd40087330364a07768cd7a4A surface enhanced Raman scattering based colloid nanosensor for developing therapeutic drug monitoringLitti, Lucio; Ramundo, Andrea; Biscaglia, Francesca; Toffoli, Giuseppe; Gobbo, Marina; Meneghetti, MorenoJournal of Colloid and Interface Science (2019), 533 (), 621-626CODEN: JCISA5; ISSN:0021-9797. (Elsevier B.V.)Competitive reactions, on the surface of plasmonic nanostructures, allow exploiting SERS signals for quant. therapeutic drug monitoring. As an example, the concn. of Erlotinib, an anti-EGFR small mol., used for the treatment of non-small cell lung and pancreatic cancer, is detd. The numerous side effects and the variability of patient responses make Erlotinib a good candidate for monitoring. The new SERS based sensor can est. Erlotinib down to nanomolar concn. and is based on the chem. reaction of the drug and of a competitor SERS reporter on the surface of gold nanostructures. Colloid solns. of naked gold nanoparticles obtained by laser ablation in soln. were used for obtaining nanostructures with very efficient hot spots for SERS and with a clean surface for chem. Detection of the drug in the nanomolar concn. range is shown to be possible also in spiked plasma samples.
- 50Farquharson, S.; Gift, A. D.; Shende, C.; Maksymiuk, P.; Inscore, F. E.; Murran, J. Detection of 5-fluorouracil in saliva using surface-enhanced Raman spectroscopy. Vib. Spectrosc. 2005, 38 (1), 79– 84, DOI: 10.1016/j.vibspec.2005.02.021Google ScholarThere is no corresponding record for this reference.
- 51Subaihi, A.; Almanqur, L.; Muhamadali, H.; AlMasoud, N.; Ellis, D. I.; Trivedi, D. K.; Hollywood, K. A.; Xu, Y.; Goodacre, R. Rapid, Accurate, and Quantitative Detection of Propranolol in Multiple Human Biofluids via Surface-Enhanced Raman Scattering. Anal. Chem. 2016, 88 (22), 10884– 10892, DOI: 10.1021/acs.analchem.6b02041Google ScholarThere is no corresponding record for this reference.
- 52Yang, J.; Cui, Y.; Zong, S.; Zhang, R.; Song, C.; Wang, Z. Tracking Multiplex Drugs and Their Dynamics in Living Cells Using the Label-Free Surface-Enhanced Raman Scattering Technique. Mol. Pharmaceutics 2012, 9 (4), 842– 849, DOI: 10.1021/mp200667dGoogle ScholarThere is no corresponding record for this reference.
- 53Koike, K.; Bando, K.; Ando, J.; Yamakoshi, H.; Terayama, N.; Dodo, K.; Smith, N. I.; Sodeoka, M.; Fujita, K. Quantitative Drug Dynamics Visualized by Alkyne-Tagged Plasmonic-Enhanced Raman Microscopy. ACS Nano 2020, 14 (11), 15032– 15041, DOI: 10.1021/acsnano.0c05010Google Scholar53https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BB3s7jslKltw%253D%253D&md5=05b4a214af3f7cb13e182e71fe0d6d59Quantitative Drug Dynamics Visualized by Alkyne-Tagged Plasmonic-Enhanced Raman MicroscopyKoike Kota; Bando Kazuki; Ando Jun; Fujita Katsumasa; Koike Kota; Fujita Katsumasa; Yamakoshi Hiroyuki; Terayama Naoki; Dodo Kosuke; Sodeoka Mikiko; Smith Nicholas Isaac; Fujita KatsumasaACS nano (2020), 14 (11), 15032-15041 ISSN:.Visualizing live-cell uptake of small-molecule drugs is paramount for drug development and pharmaceutical sciences. Bioorthogonal imaging with click chemistry has made significant contributions to the field, visualizing small molecules in cells. Furthermore, recent developments in Raman microscopy, including stimulated Raman scattering (SRS) microscopy, have realized direct visualization of alkyne-tagged small-molecule drugs in live cells. However, Raman and SRS microscopy still suffer from limited detection sensitivity with low concentration molecules for observing temporal dynamics of drug uptake. Here, we demonstrate the combination of alkyne-tag and surface-enhanced Raman scattering (SERS) microscopy for the real-time monitoring of drug uptake in live cells. Gold nanoparticles are introduced into lysosomes of live cells by endocytosis and work as SERS probes. Raman signals of alkynes can be boosted by enhanced electric fields generated by plasmon resonance of gold nanoparticles when alkyne-tagged small molecules are colocalized with the nanoparticles. With time-lapse 3D SERS imaging, this technique allows us to investigate drug uptake by live cells with different chemical and physical conditions. We also perform quantitative evaluation of the uptake speed at the single-cell level using digital SERS counting under different quantities of drug molecules and temperature conditions. Our results illustrate that alkyne-tag SERS microscopy has a potential to be an alternative bioorthogonal imaging technique to investigate temporal dynamics of small-molecule uptake of live cells for pharmaceutical research.
- 54Han, G.; Liu, R.; Han, M.-Y.; Jiang, C.; Wang, J.; Du, S.; Liu, B.; Zhang, Z. Label-Free Surface-Enhanced Raman Scattering Imaging to Monitor the Metabolism of Antitumor Drug 6-Mercaptopurine in Living Cells. Anal. Chem. 2014, 86 (23), 11503– 11507, DOI: 10.1021/ac503539wGoogle ScholarThere is no corresponding record for this reference.
- 55Jamieson, L. E.; Byrne, H. J. Vibrational spectroscopy as a tool for studying drug-cell interaction: Could high throughput vibrational spectroscopic screening improve drug development?. Vib. Spectrosc. 2017, 91, 16– 30, DOI: 10.1016/j.vibspec.2016.09.003Google Scholar55https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28Xhs1Srsb7O&md5=496272549a5f2d0219e4089926bf45f2Vibrational spectroscopy as a tool for studying drug-cell interaction: Could high throughput vibrational spectroscopic screening improve drug development?Jamieson, Lauren E.; Byrne, Hugh J.Vibrational Spectroscopy (2017), 91 (), 16-30CODEN: VISPEK; ISSN:0924-2031. (Elsevier B.V.)Vibrational spectroscopy is currently widely explored as a tool in biomedical applications. An area at the forefront of this field is the use of vibrational spectroscopy for disease diagnosis, ultimately aiming towards spectral pathol. However, while this field shows promising results, moving this technique into the clinic faces the challenges of widespread clin. trials and legislative approval. While spectral pathol. has received a lot of attention, there are many other biomedical applications of vibrational spectroscopy, which could potentially be translated to applications with greater ease. A particularly promising application is the use of vibrational spectroscopic techniques to study the interaction of drugs with cells. Many studies have demonstrated the ability to detect biochem. changes in cells in response to drug application, using both IR and Raman spectroscopy. This has shown potential for use in high throughput screening (HTS) applications, for screening of efficacy and mode of action of potential drug candidates, to speed up the drug discovery process. HTS is still a relatively new and growing area of research and, therefore, there is more potential for new techniques to move into and shape this field. Vibrational spectroscopic techniques come with many benefits over the techniques used currently in HTS, primarily based on fluorescence assays to detect specific binding interactions or phenotypes. They are label free, and an IR or Raman spectrum provides a wealth of biochem. information, and therefore could reveal not only information about a specific interaction, but about how the overall biochem. of a cell changes in response to application of a drug candidate. Therefore, drug mode of action could be elucidated. This review will investigate the potential for vibrational spectroscopy, particularly FTIR and Raman spectroscopy, to benefit the field of HTS and improve the drug development process. In addn. to FTIR and Raman spectroscopy, surface enhanced Raman spectroscopy (SERS), coherent anti-Stokes Raman spectroscopy (CARS) and stimulated Raman spectroscopy (SRS), will be investigated as an alternative tool in the HTS process.
- 56Kim, W.; Lee, S. H.; Kim, J. H.; Ahn, Y. J.; Kim, Y.-H.; Yu, J. S.; Choi, S. Paper-Based Surface-Enhanced Raman Spectroscopy for Diagnosing Prenatal Diseases in Women. ACS Nano 2018, 12 (7), 7100– 7108, DOI: 10.1021/acsnano.8b02917Google Scholar56https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXhtFKlsrjM&md5=89ff42790c523a9f613f31718ee5d5c1Paper-Based Surface-Enhanced Raman Spectroscopy for Diagnosing Prenatal Diseases in WomenKim, Wansun; Lee, Soo Hyun; Kim, Jin Hwi; Ahn, Yong Jin; Kim, Yeon-Hee; Yu, Jae Su; Choi, SamjinACS Nano (2018), 12 (7), 7100-7108CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)The authors report the development of a surface-enhanced Raman spectroscopy sensor chip by decorating gold nanoparticles (AuNPs) on ZnO nanorod (ZnO NR) arrays vertically grown on cellulose paper (C). These chips can enhance the Raman signal by 1.25 × 107 with an excellent reproducibility of <6%. The authors can measure trace amts. of human amniotic fluids of patients with subclin. intra-amniotic infection (IAI) and preterm delivery (PTD) using the chip in combination with a multivariate statistics-derived machine-learning-trained bioclassification method. The authors can detect the presence of prenatal diseases and identify the types of diseases from amniotic fluids with >92% clin. sensitivity and specificity. The authors' technol. has the potential to be used for the early detection of prenatal diseases and can be adapted for point-of-care applications.
- 57Torul, H.; Çiftçi, H.; Çetin, D.; Suludere, Z.; Boyacı, I. H.; Tamer, U. Paper membrane-based SERS platform for the determination of glucose in blood samples. Anal Bioanal Chem. 2015, 407 (27), 8243– 8251, DOI: 10.1007/s00216-015-8966-xGoogle Scholar57https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXhsV2jurrL&md5=01222db6845e9ebeecec7de01af46898Paper membrane-based SERS platform for the determination of glucose in blood samplesTorul, Hilal; Ciftci, Hakan; Cetin, Demet; Suludere, Zekiye; Boyaci, Ismail Hakki; Tamer, UgurAnalytical and Bioanalytical Chemistry (2015), 407 (27), 8243-8251CODEN: ABCNBP; ISSN:1618-2642. (Springer)In this report, we present a paper membrane-based surface-enhanced Raman scattering (SERS) platform for the detn. of blood glucose level using a nitrocellulose membrane as substrate paper, and the microfluidic channel was simply constructed by wax-printing method. The rod-shaped gold nanorod particles were modified with 4-mercaptophenylboronic acid (4-MBA) and 1-decanethiol (1-DT) mols. and used as embedded SERS probe for paper-based microfluidics. The SERS measurement area was simply constructed by dropping gold nanoparticles on nitrocellulose membrane, and the blood sample was dropped on the membrane hydrophilic channel. While the blood cells and proteins were held on nitrocellulose membrane, glucose mols. were moved through the channel toward the SERS measurement area. SEM was used to confirm the effective sepn. of blood matrix, and total anal. is completed in 5 min. In SERS measurements, the intensity of the band at 1070 cm-1 which is attributed to B-OH vibration decreased depending on the rise in glucose concn. in the blood sample. The glucose concn. was found to be 5.43 ± 0.51 mM in the ref. blood sample by using a calibration equation, and the certified value for glucose was 6.17 ± 0.11 mM. The recovery of the glucose in the ref. blood sample was about 88 %. According to these results, the developed paper-based microfluidic SERS platform has been found to be suitable for use for the detection of glucose in blood samples without any pretreatment procedure. We believe that paper-based microfluidic systems may provide a wide field of usage for paper-based applications.
- 58Liu, G.; Mu, Z.; Guo, J.; Shan, K.; Shang, X.; Yu, J.; Liang, X. Surface-enhanced Raman scattering as a potential strategy for wearable flexible sensing and point-of-care testing non-invasive medical diagnosis. Frontiers in Chemistry 2022, 10, 1060322, DOI: 10.3389/fchem.2022.1060322Google ScholarThere is no corresponding record for this reference.
- 59Liu, L.; Martinez Pancorbo, P.; Xiao, T.-H.; Noguchi, S.; Marumi, M.; Segawa, H.; Karhadkar, S.; Gala de Pablo, J.; Hiramatsu, K.; Kitahama, Y. Highly Scalable, Wearable Surface-Enhanced Raman Spectroscopy. Advanced Optical Materials 2022, 10 (17), 2200054, DOI: 10.1002/adom.202200054Google Scholar59https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38Xhs1Clu7jL&md5=a2a445d93dc33ab82064a629a5bfe773Highly Scalable, Wearable Surface-Enhanced Raman SpectroscopyLiu, Limei; Martinez Pancorbo, Pablo; Xiao, Ting-Hui; Noguchi, Saya; Marumi, Machiko; Segawa, Hiroki; Karhadkar, Siddhant; Gala de Pablo, Julia; Hiramatsu, Kotaro; Kitahama, Yasutaka; Itoh, Tamitake; Qu, Junle; Takei, Kuniharu; Goda, KeisukeAdvanced Optical Materials (2022), 10 (17), 2200054CODEN: AOMDAX; ISSN:2195-1071. (Wiley-VCH Verlag GmbH & Co. KGaA)The last two decades have witnessed a dramatic growth of wearable sensor technol., mainly represented by flexible, stretchable, on-skin electronic sensors that provide rich information of the wearer's health conditions and surroundings. A recent breakthrough in the field is the development of wearable chem. sensors based on surface-enhanced Raman spectroscopy (SERS) that can detect mol. fingerprints universally, sensitively, and noninvasively. However, while their sensing properties are excellent, these sensors are not scalable for widespread use beyond small-scale human health monitoring due to their cumbersome fabrication process and limited multifunctional sensing capabilities. Here, a highly scalable, wearable SERS sensor is demonstrated based on an easy-to-fabricate, low-cost, ultrathin, flexible, stretchable, adhesive, and biointegratable gold nanomesh. It can be fabricated in any shape and worn on virtually any surface for label-free, large-scale, in situ sensing of diverse analytes from low to high concns. (10-106 x 10-9M). To show the practical utility of the wearable SERS sensor, the sensor is tested for the detection of sweat biomarkers, drugs of abuse, and microplastics. This wearable SERS sensor represents a significant step toward the generalizability and practicality of wearable sensing technol.
- 60Wang, Y.; Zhao, C.; Wang, J.; Luo, X.; Xie, L.; Zhan, S.; Kim, J.; Wang, X.; Liu, X.; Ying, Y. Wearable plasmonic-metasurface sensor for noninvasive and universal molecular fingerprint detection on biointerfaces. Science Advances 2021, 7 (4), eabe4553, DOI: 10.1126/sciadv.abe4553Google ScholarThere is no corresponding record for this reference.
- 61Jeong, J. W.; Arnob, M. M. P.; Baek, K.-M.; Lee, S. Y.; Shih, W.-C.; Jung, Y. S. 3D Cross-Point Plasmonic Nanoarchitectures Containing Dense and Regular Hot Spots for Surface-Enhanced Raman Spectroscopy Analysis. Adv. Mater. 2016, 28 (39), 8695– 8704, DOI: 10.1002/adma.201602603Google Scholar61https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhtlalsLfE&md5=a614a3a6d33312f6f1fa6f6712d4659e3D cross-point plasmonic nanoarchitectures containing dense and regular hot spots for surface-enhanced raman spectroscopy analysisJeong, Jae Won; Arnob, Md Masud Parvez; Baek, Kwang-Min; Lee, Seung Yong; Shih, Wei-Chuan; Jung, Yeon SikAdvanced Materials (Weinheim, Germany) (2016), 28 (39), 8695-8704CODEN: ADVMEW; ISSN:0935-9648. (Wiley-VCH Verlag GmbH & Co. KGaA)Herein, we demonstrate the realization of vertically stacked 3D cross-point plasmonic nanostructures with excellent SERS signal intensity and uniformity over a macroscopic area based on high resoln. nanotransfer printing (nTP). For more facile and rapid stacking of multilayer nanostructures, we developed and applied a second generation solvent assisted nanotransfer printing (SnTP) technique based on a multipurpose single layer replica without using an addnl. transfer medium, thereby significantly simplifying the overall nTP steps and enabling the prompt repetition of nTP for multilayer stacking of nanowires. We report that sequentially transfer-printed sub-20 nm nanowires can provide both an in-plane coupling effect in the nanogap region and an out-of-coupling effect at the cross-points where two nanowires are closely stacked, achieving excellent enhancement of Raman signals from probed mols. with an av. enhancement factor of ≈ 4.1×107 depending on structural and material parameters. Moreover, nanowires-on-film hybrid structures obtained by sequential printing on a continuous metal film show highly intensified SERS signals due to vertical plasmonic coupling between the upper nanowires and the underlying film.
- 62Masson, J.-F. The Need for Benchmarking Surface-Enhanced Raman Scattering (SERS) Sensors. ACS Sensors 2021, 6 (11), 3822– 3823, DOI: 10.1021/acssensors.1c02275Google ScholarThere is no corresponding record for this reference.
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Abstract
Figure 1
Figure 1. Plasmonic SERS substrates manufactured via top-down and bottom-up fabrication approaches. (a) Top-down approaches enable the fabrication of highly resolved nanostructures, such as nanopillars (reproduced from ref (16). Copyright 2013, American Chemical Society) and bowties (reproduced from ref (17). Copyright 2018, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim). (b) Bottom-up approaches, such as the Langmuir–Blodgett technique (reproduced from ref (29). Copyright 2022, Elsevier Ltd.) and the nanoparticle-on-a-mirror approach (licensed under CC-BY. Reproduced from ref (23)), are more accessible and facilitate the controlled aggregation of nanoparticles that are simpler to fabricate.
Figure 2
Figure 2. Detection of the binding site of the antihypertensive medication, felodipine, to its target protein, oncogenic Aurora A kinase, using label-free SERS by monitoring changes in the protein’s spectral bands. Reproduced with permission from ref (4).
Figure 3
Figure 3. Application of label-free SERS for monitoring the cellular metabolism of a cancer therapeutic by detecting spectral changes associated with changes in the absorption of the drug molecule on nanoparticle surfaces. Reproduced from ref (54). Copyright 2014, American Chemical Society.
Figure 4
Figure 4. Wearable and point-of-care SERS-based sensors for detecting biomarkers, metabolites, and drugs. (a) Paper-based SERS substrate for point-of-care drug detection. Reproduced from ref (35). Copyright 2016, Elsevier B.V. (b) Concept of a SERS-based sensor, wearable directly on the skin, for detecting biomarkers and drugs. Reproduced from ref (59). Available under a CC-BY License. Copyright 2022, Limei Liu, Pablo Martinez Pancorbo, Ting-Hui Xiao, Saya Noguchi, Machiko Marumi, Hiroki Segawa, Siddhant Karhadkar, Julia Gala de Pablo, Kotaro Hiramatsu, Yasutaka Kitahama, Tamitake Itoh, Junle Qu, Kuniharu Takei, and Keisuke Goda. Advanced Optical Materials, Wiley-VCH GmbH.
Lamyaa M. Almehmadi
Lamyaa M. Almehmadi is a Massachusetts Institute of Technology postdoctoral fellow working on developing silicon photonic chip-based sensors. She received her Ph.D. from the University at Albany (State University of New York at Albany). She is the recipient of several awards, including the Rising Star in Analytical Chemistry Award from the American Chemical Society’s (ACS’s) Analytical Chemistry Division and the prestigious Coblentz Society Student Award. Her research experience focuses on the applications of several Raman spectroscopy techniques, including SERS and deep-ultraviolet resonance and standoff Raman spectroscopies.
Igor K. Lednev
Igor K. Lednev is a Williams–Raycheff Endowed Professor in Chemistry and a SUNY Distinguished Professor at the University at Albany (State University of New York at Albany). He served as an advisory member on the White House Subcommittee for Forensic Science. His research focuses on the development and application of laser spectroscopy for forensic investigations, biomedical applications, and fundamental biochemistry. He is a cofounder of startup companies commercializing a universal method for identifying bodily fluid traces for forensic investigations and screening for the early diagnosis of Alzheimer’s disease. He has received several prestigious awards, including the Charles Mann Award for Applied Raman Spectroscopy.
References
This article references 62 other publications.
- 1Almehmadi, L. M.; Valsangkar, V. A.; Halvorsen, K.; Zhang, Q.; Sheng, J.; Lednev, I. K. Surface-enhanced Raman spectroscopy for drug discovery: peptide-RNA binding. Anal. Bioanal. Chem. 2022, 414 (20), 6009– 6016, DOI: 10.1007/s00216-022-04190-5There is no corresponding record for this reference.
- 2Plou, J.; Valera, P. S.; García, I.; de Albuquerque, C. D. L.; Carracedo, A.; Liz-Marzán, L. M. Prospects of Surface-Enhanced Raman Spectroscopy for Biomarker Monitoring toward Precision Medicine. ACS Photonics 2022, 9 (2), 333– 350, DOI: 10.1021/acsphotonics.1c019342https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XisVGjtLs%253D&md5=df937d50a05f2117e1b542df3746f456Prospects of Surface-Enhanced Raman Spectroscopy for Biomarker Monitoring toward Precision MedicinePlou, Javier; Valera, Pablo S.; Garcia, Isabel; de Albuquerque, Carlos D. L.; Carracedo, Arkaitz; Liz-Marzan, Luis M.ACS Photonics (2022), 9 (2), 333-350CODEN: APCHD5; ISSN:2330-4022. (American Chemical Society)Future precision medicine will be undoubtedly sustained by the detection of validated biomarkers that enable a precise classification of patients based on their predicted disease risk, prognosis, and response to a specific treatment. Up to now, genomics, transcriptomics, and immunohistochem. have been the main clin. amenable tools at hand for identifying key diagnostic, prognostic, and predictive biomarkers. However, other mol. strategies, including metabolomics, are still in their infancy and require the development of new biomarker detection technologies, toward routine implementation into clin. diagnosis. In this context, surface-enhanced Raman scattering (SERS) spectroscopy has been recognized as a promising technol. for clin. monitoring thanks to its high sensitivity and label-free operation, which should help accelerate the discovery of biomarkers and their corresponding screening in a simpler, faster, and less-expensive manner. Many studies have demonstrated the excellent performance of SERS in biomedical applications. However, such studies have also revealed several variables that should be considered for accurate SERS monitoring, in particular, when the signal is collected from biol. sources (tissues, cells or biofluids). This Perspective is aimed at piecing together the puzzle of SERS in biomarker monitoring, with a view on future challenges and implications. We address the most relevant requirements of plasmonic substrates for biomedical applications, as well as the implementation of tools from artificial intelligence or biotechnol. to guide the development of highly versatile sensors.
- 3Langer, J.; Jimenez de Aberasturi, D.; Aizpurua, J.; Alvarez-Puebla, R. A.; Auguié, B.; Baumberg, J. J.; Bazan, G. C.; Bell, S. E. J.; Boisen, A.; Brolo, A. G. Present and Future of Surface-Enhanced Raman Scattering. ACS Nano 2020, 14 (1), 28– 117, DOI: 10.1021/acsnano.9b042243https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhs12jt7%252FN&md5=b9a563416413785a9548d12fcaa5d21aPresent and Future of Surface-Enhanced Raman ScatteringLanger, Judith; Jimenez de Aberasturi, Dorleta; Aizpurua, Javier; Alvarez-Puebla, Ramon A.; Auguie, Baptiste; Baumberg, Jeremy J.; Bazan, Guillermo C.; Bell, Steven E. J.; Boisen, Anja; Brolo, Alexandre G.; Choo, Jaebum; Cialla-May, Dana; Deckert, Volker; Fabris, Laura; Faulds, Karen; Garcia de Abajo, F. Javier; Goodacre, Royston; Graham, Duncan; Haes, Amanda J.; Haynes, Christy L.; Huck, Christian; Itoh, Tamitake; Kall, Mikael; Kneipp, Janina; Kotov, Nicholas A.; Kuang, Hua; Le Ru, Eric C.; Lee, Hiang Kwee; Li, Jian-Feng; Ling, Xing Yi; Maier, Stefan A.; Mayerhofer, Thomas; Moskovits, Martin; Murakoshi, Kei; Nam, Jwa-Min; Nie, Shuming; Ozaki, Yukihiro; Pastoriza-Santos, Isabel; Perez-Juste, Jorge; Popp, Juergen; Pucci, Annemarie; Reich, Stephanie; Ren, Bin; Schatz, George C.; Shegai, Timur; Schlucker, Sebastian; Tay, Li-Lin; Thomas, K. George; Tian, Zhong-Qun; Van Duyne, Richard P.; Vo-Dinh, Tuan; Wang, Yue; Willets, Katherine A.; Xu, Chuanlai; Xu, Hongxing; Xu, Yikai; Yamamoto, Yuko S.; Zhao, Bing; Liz-Marzan, Luis M.ACS Nano (2020), 14 (1), 28-117CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)A review. The discovery of the enhancement of Raman scattering by mols. adsorbed on nanostructured metal surfaces is a landmark in the history of spectroscopic and anal. techniques. Significant exptl. and theor. effort has been directed toward understanding the surface-enhanced Raman scattering (SERS) effect and demonstrating its potential in various types of ultrasensitive sensing applications in a wide variety of fields. In the 45 years since its discovery, SERS has blossomed into a rich area of research and technol., but addnl. efforts are still needed before it can be routinely used anal. and in com. products. In this Review, prominent authors from around the world joined together to summarize the state of the art in understanding and using SERS and to predict what can be expected in the near future in terms of research, applications, and technol. development. This Review is dedicated to SERS pioneer and our coauthor, the late Prof. Richard Van Duyne, whom we lost during the prepn. of this article.
- 4Karthigeyan, D.; Siddhanta, S.; Kishore, A. H.; Perumal, S. S. R. R.; Ågren, H.; Sudevan, S.; Bhat, A. V.; Balasubramanyam, K.; Subbegowda, R. K.; Kundu, T. K. SERS and MD simulation studies of a kinase inhibitor demonstrate the emergence of a potential drug discovery tool. Proc. Natl. Acad. Sci. U.S.A. 2014, 111 (29), 10416– 10421, DOI: 10.1073/pnas.14026951114https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhtVOitL%252FF&md5=721cbafc3606ace6c0ae0834e63eb9f4SERS and MD simulation studies of a kinase inhibitor demonstrate the emergence of a potential drug discovery toolKarthigeyan, Dhanasekaran; Siddhanta, Soumik; Kishore, Annavarapu Hari; Perumal, Sathya S. R. R.; Agren, Hans; Sudevan, Surabhi; Bhat, Akshay V.; Balasubramanyam, Karanam; Subbegowda, Rangappa Kanchugarakoppal; Kundu, Tapas K.; Narayana, ChandrabhasProceedings of the National Academy of Sciences of the United States of America (2014), 111 (29), 10416-10421CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)The authors demonstrate the use of surface-enhanced Raman spectroscopy (SERS) as an excellent tool for identifying the binding site of small mols. on a therapeutically important protein. As an example, the authors show the specific binding of the common antihypertension drug felodipine to the oncogenic Aurora A kinase protein via hydrogen bonding interactions with Tyr 212 residue to specifically inhibit its activity. Based on SERS studies, mol. docking, mol. dynamics simulation, biochem. assays, and point mutation-based validation, the authors demonstrate the surface-binding mode of this mol. in two similar hydrophobic pockets in the Aurora A kinase. These binding pockets comprise the same unique hydrophobic patches that may aid in distinguishing human Aurora A vs. human Aurora B kinase in vivo. The application of SERS to identify the specific interactions between small mols. and therapeutically important proteins by differentiating competitive and noncompetitive inhibition demonstrates its ability as a complementary technique. The authors also present felodipine as a specific inhibitor for oncogenic Aurora A kinase. Felodipine retards the rate of tumor progression in a xenografted nude mice model. This study reveals a potential surface pocket that may be useful for developing small mols. by selectively targeting the Aurora family kinases.
- 5Nie, S.; Emory, S. R. Probing Single Molecules and Single Nanoparticles by Surface-Enhanced Raman Scattering. Science 1997, 275 (5303), 1102– 1106, DOI: 10.1126/science.275.5303.11025https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaK2sXhtlGlsL4%253D&md5=e8968fee3a48e1f3131e8bebcc40e2b0Probing single molecules and single nanoparticles by surface-enhanced Raman scatteringNie, Shuming; Emory, Steven R.Science (Washington, D. C.) (1997), 275 (5303), 1102-1106CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)Optical detection and spectroscopy of single mols. and single nanoparticles were achieved at room temp. using surface-enhanced Raman scattering. Individual Ag colloidal nanoparticles were screened from a large heterogeneous population for special size-dependent properties and were then used to amplify the speculation for special size-dependent properties and were then used to amplify the spectroscopic signatures of adsorbed mols. For single rhodamine 6G mols. adsorbed on the selected nanoparticles, the intrinsic Raman enhancement factors were ∼1014 to 1015, much larger than the ensemble-averaged values derived from conventional measurements. This enormous enhancement leads to vibrational Raman signals that are more intense and more stable than single-mol. fluorescence.
- 6Almehmadi, L. M.; Curley, S. M.; Tokranova, N. A.; Tenenbaum, S. A.; Lednev, I. K. Surface Enhanced Raman Spectroscopy for Single Molecule Protein Detection. Sci. Rep. 2019, 9 (1), 12356, DOI: 10.1038/s41598-019-48650-y6https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BB3MrhvVGltw%253D%253D&md5=91490421ed336ec38b024dfb51146d62Surface Enhanced Raman Spectroscopy for Single Molecule Protein DetectionAlmehmadi Lamyaa M; Lednev Igor K; Almehmadi Lamyaa M; Tenenbaum Scott A; Lednev Igor K; Curley Stephanie M; Tokranova Natalya A; Tenenbaum Scott AScientific reports (2019), 9 (1), 12356 ISSN:.A two-step process of protein detection at a single molecule level using SERS was developed as a proof-of-concept platform for medical diagnostics. First, a protein molecule was bound to a linker in the bulk solution and then this adduct was chemically reacted with the SERS substrate. Traut's Reagent (TR) was used to thiolate Bovine serum albumin (BSA) in solution followed by chemical cross linking to a gold surface through a sulfhydryl group. A Glycine-TR adduct was used as a control sample to identify the protein contribution to the SER spectra. Gold SERS substrates were manufactured by electrochemical deposition. Solutions at an ultralow concentration were used for attaching the TR adducts to the SERS substrate. Samples showed the typical behavior of a single molecule SERS including spectral fluctuations, blinking and Raman signal being generated from only selected points on the substrate. The fluctuating SER spectra were examined using Principle Component Analysis. This unsupervised statistics allowed for the selecting of spectral contribution from protein moiety indicating that the method was capable of detecting a single protein molecule. Thus we have demonstrated, that the developed two-step methodology has the potential as a new platform for medical diagnostics.
- 7Han, X. X.; Rodriguez, R. S.; Haynes, C. L.; Ozaki, Y.; Zhao, B. Surface-enhanced Raman spectroscopy. Nature Reviews Methods Primers 2022, 1 (1), 87, DOI: 10.1038/s43586-021-00083-6There is no corresponding record for this reference.
- 8Le Ru, E. C.; Etchegoin, P. G. SERS enhancement factors and related topics. In Principles of Surface-Enhanced Raman Spectroscopy, Elsevier, 2009; p 185– 264.There is no corresponding record for this reference.
- 9Petryayeva, E.; Krull, U. J. Localized surface plasmon resonance: nanostructures, bioassays and biosensing-a review. Anal. Chim. Acta 2011, 706 (1), 8– 24, DOI: 10.1016/j.aca.2011.08.0209https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3MXhtlemsbjM&md5=b298d4394739737ea8c3d950052924dfLocalized surface plasmon resonance: Nanostructures, bioassays and biosensing-A reviewPetryayeva, Eleonora; Krull, Ulrich J.Analytica Chimica Acta (2011), 706 (1), 8-24CODEN: ACACAM; ISSN:0003-2670. (Elsevier B.V.)A review. Localized surface plasmon resonance (LSPR) is an optical phenomena generated by light when it interacts with conductive nanoparticles (NPs) that are smaller than the incident wavelength. As in surface plasmon resonance, the elec. field of incident light can be deposited to collectively excite electrons of a conduction band, with the result being coherent localized plasmon oscillations with a resonant frequency that strongly depends on the compn., size, geometry, dielec. environment and sepn. distance of NPs. This review serves to describe the phys. theory of LSPR formation at the surface of nanostructures, and the potential for this optical technol. to serve as a basis for the development bioassays and biosensing of high sensitivity. The benefits and challenges assocd. with various exptl. designs of nanoparticles and detection systems, as well as creative approaches that have been developed to improve sensitivity and limits of detection are highlighted using examples from the literature.
- 10Kahraman, M.; Mullen, E. R.; Korkmaz, A.; Wachsmann-Hogiu, S. Fundamentals and applications of SERS-based bioanalytical sensing. Nanophotonics 2017, 6 (5), 831– 852, DOI: 10.1515/nanoph-2016-0174There is no corresponding record for this reference.
- 11Maher, R. C. Raman Spectroscopy for Nanomaterials Characterization · SERS Hot Spots. In Raman Spectroscopy for Nanomaterials Characterization; Kumar, C. S. S. R., Ed.; Springer, 2012.There is no corresponding record for this reference.
- 12Szaniawska, A.; Kudelski, A. Applications of Surface-Enhanced Raman Scattering in Biochemical and Medical Analysis. Front Chem. 2021, 9, 664134, DOI: 10.3389/fchem.2021.66413412https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhvVektrvP&md5=6370393e05f68252aec85b3d6d148afbApplications of surface-enhanced raman scattering in biochemical and medical analysisSzaniawska, Aleksandra; Kudelski, AndrzejFrontiers in Chemistry (Lausanne, Switzerland) (2021), 9 (), 664134CODEN: FCLSAA; ISSN:2296-2646. (Frontiers Media S.A.)A review. In this mini-review, we briefly describe certain recently developed applications of the surface-enhanced Raman spectroscopy (SERS) for detg. various biochem. (esp. medically) important species from ones as simple as hydrogen cations to those as complex as specific DNA fragments. We present a SERS anal. of species whose characterization is important to our understanding of various mechanisms in the human body and to show its potential as an alternative for methods routinely used in diagnostics and clinics. Furthermore, we explain how such SERS-based sensors operate and point out future prospects in this field.
- 13Fikiet, M. A.; Khandasammy, S. R.; Mistek, E.; Ahmed, Y.; Halámková, L.; Bueno, J.; Lednev, I. K. Surface enhanced Raman spectroscopy: A review of recent applications in forensic science. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 2018, 197, 255– 260, DOI: 10.1016/j.saa.2018.02.046There is no corresponding record for this reference.
- 14Cailletaud, J.; De Bleye, C.; Dumont, E.; Sacré, P. Y.; Netchacovitch, L.; Gut, Y.; Boiret, M.; Ginot, Y. M.; Hubert, P.; Ziemons, E. Critical review of surface-enhanced Raman spectroscopy applications in the pharmaceutical field. J. Pharm. Biomed. Anal. 2018, 147, 458– 472, DOI: 10.1016/j.jpba.2017.06.05614https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhtFChtLnP&md5=4c1f92a24ad5cefb070fe13573e9210bCritical review of surface-enhanced Raman spectroscopy applications in the pharmaceutical fieldCailletaud, J.; De Bleye, C.; Dumont, E.; Sacre, P.-Y.; Netchacovitch, L.; Gut, Y.; Boiret, M.; Ginot, Y.-M.; Hubert, Ph.; Ziemons, E.Journal of Pharmaceutical and Biomedical Analysis (2018), 147 (), 458-472CODEN: JPBADA; ISSN:0731-7085. (Elsevier B.V.)A review. Surface-enhanced Raman spectroscopy (SERS) is a sensitive anal. tool used in the pharmaceutical field in recent years. SERS keeps all the advantages of classical Raman spectroscopy while being is more sensitive allowing its use for the detection and the quantification of low-dose substances contained in pharmaceutical samples. However, the anal. performance of SERS is limited due to the difficulty to implement a quant. methodol. correctly validated. Nevertheless, some studies reported the development of SERS quant. methods esp. in pharmaceutical approaches. In this context, this review presents the main concepts of the SERS technique. The different steps that need to be applied to develop a SERS quant. method are also deeply described. The last part of the present manuscript gives a crit. overview of the different SERS pharmaceutical applications that were developed for a non-exhaustive list of pharmaceutical compds. with the aim to highlights the validation criteria for each application.
- 15Li, W.; Zhao, X.; Yi, Z.; Glushenkov, A. M.; Kong, L. Plasmonic substrates for surface enhanced Raman scattering. Anal. Chim. Acta 2017, 984, 19– 41, DOI: 10.1016/j.aca.2017.06.00215https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhtFOjsLvL&md5=e076824ca1500920441ed4db6f187920Plasmonic substrates for surface enhanced Raman scatteringLi, Wenbing; Zhao, Xinchu; Yi, Zhifeng; Glushenkov, Alexey M.; Kong, LingxueAnalytica Chimica Acta (2017), 984 (), 19-41CODEN: ACACAM; ISSN:0003-2670. (Elsevier B.V.)As an advanced anal. tool, surface-enhanced Raman scattering (SERS) has broad applications in identification of colorants in paints and glazes, hazard detection to ensure food safety, biomedicine and diagnosis, environmental monitoring, detection of explosives and forensic science. In this review, main types of plasmonic substrates, which include solid substrate with metallic nanostructures and chem. synthesized noble metal colloids, and their fabrication methods are reviewed. The design principles for fabrication of ultrasensitive plasmonic substrates for SERS are presented from published literature. Finally, various applications of SERS substrates are described, indicating the potential of this technique in practical applications. As an ultrasensitive detection method, SERS is at the core of a rapidly expanding research field.
- 16Yang, J.; Palla, M.; Bosco, F. G.; Rindzevicius, T.; Alstrøm, T. S.; Schmidt, M. S.; Boisen, A.; Ju, J.; Lin, Q. Surface-enhanced Raman spectroscopy based quantitative bioassay on aptamer-functionalized nanopillars using large-area Raman mapping. ACS Nano 2013, 7 (6), 5350– 5359, DOI: 10.1021/nn401199k16https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXosVeisLg%253D&md5=ab353addeacf47cd71bc81555a006ddfSurface-Enhanced Raman Spectroscopy Based Quantitative Bioassay on Aptamer-Functionalized Nanopillars Using Large-Area Raman MappingYang, Jaeyoung; Palla, Mirko; Bosco, Filippo Giacomo; Rindzevicius, Tomas; Alstroem, Tommy Sonne; Schmidt, Michael Stenbaek; Boisen, Anja; Ju, Jingyue; Lin, QiaoACS Nano (2013), 7 (6), 5350-5359CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)Surface-enhanced Raman spectroscopy (SERS) has been used in a variety of biol. applications due to its high sensitivity and specificity. Here, we report a SERS-based biosensing approach for quant. detection of biomols. A SERS substrate bearing gold-decorated silicon nanopillars is functionalized with aptamers for sensitive and specific detection of target mols. In this study, TAMRA-labeled vasopressin mols. in the picomolar regime (1 pM to 1 nM) are specifically captured by aptamers on the nanostructured SERS substrate and monitored by using an automated SERS signal mapping technique. From the exptl. results, we show concn.-dependent SERS responses in the picomolar range by integrating SERS signal intensities over a scanning area. It is also noted that our signal mapping approach significantly improves statistical reproducibility and accounts for spot-to-spot variation in conventional SERS quantification. Furthermore, we have developed an anal. model capable of predicting exptl. intensity distributions on the substrates for reliable quantification of biomols. Lastly, we have calcd. the min. needed area of Raman mapping for efficient and reliable anal. of each measurement. Combining our SERS mapping anal. with an aptamer-functionalized nanopillar substrate is found to be extremely efficient for detection of low-abundance biomols.
- 17Zhan, P.; Wen, T.; Wang, Z.-g.; He, Y.; Shi, J.; Wang, T.; Liu, X.; Lu, G.; Ding, B. DNA Origami Directed Assembly of Gold Bowtie Nanoantennas for Single-Molecule Surface-Enhanced Raman Scattering. Angew. Chem., Int. Ed. 2018, 57 (11), 2846– 2850, DOI: 10.1002/anie.20171274917https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXis1Snsr4%253D&md5=ff8d9dd95cc00d4b706454a60aa7c7ebDNA Origami Directed Assembly of Gold Bowtie Nanoantennas for Single-Molecule Surface-Enhanced Raman ScatteringZhan, Pengfei; Wen, Te; Wang, Zhen-gang; He, Yingbo; Shi, Jia; Wang, Ting; Liu, Xinfeng; Lu, Guowei; Ding, BaoquanAngewandte Chemie, International Edition (2018), 57 (11), 2846-2850CODEN: ACIEF5; ISSN:1433-7851. (Wiley-VCH Verlag GmbH & Co. KGaA)Metallic bowtie nanoarchitectures can produce dramatic elec. field enhancement, which is advantageous in single-mol. anal. and optical information processing. Plasmonic bowtie nanostructures were successfully constructed using a DNA origami-based bottom-up assembly strategy, which enables precise control over the geometrical configuration of the bowtie with an ∼5 nm gap. A single Raman probe was accurately positioned at the gap of the bowtie. Single-mol. surface-enhanced Raman scattering (SM-SERS) of individual nanostructures, including ones contg. an alkyne group, was obsd. The design achieved repeatable local field enhancement of several orders of magnitude. This method opens the door on a novel strategy for the fabrication of metal bowtie structures and SM-SERS, which can be used in the design of highly-sensitive photonic devices.
- 18Mehigan, S.; Smyth, C. A.; McCabe, E. M. Bridging the Gap between SERS Enhancement and Reproducibility by Salt Aggregated Silver Nanoparticles. Nanomaterials and Nanotechnology 2015, 5, 5, DOI: 10.5772/60125There is no corresponding record for this reference.
- 19Goodacre, R.; Graham, D.; Faulds, K. Recent developments in quantitative SERS: Moving towards absolute quantification. TrAC Trends in Analytical Chemistry 2018, 102, 359– 368, DOI: 10.1016/j.trac.2018.03.00519https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXlt1Oiur4%253D&md5=9874c21b4486f154798a2c5cffd7ef8aRecent developments in quantitative SERS: Moving towards absolute quantificationGoodacre, Royston; Graham, Duncan; Faulds, KarenTrAC, Trends in Analytical Chemistry (2018), 102 (), 359-368CODEN: TTAEDJ; ISSN:0165-9936. (Elsevier B.V.)Surface-enhanced Raman scattering (SERS) generates molecularly specific fingerprints of analytes and when the exptl. conditions are carefully controlled this is highly quant. This review critiques the development of quant. SERS from simple univariate assessment of single vibrational modes to multivariate anal. of the whole spectrum for improved quantification. SERS has also been developed for direct multiplex detection and quantification of multiple analytes and this is also discussed, as is the need for LC-SERS for analyte sepn. should multivariate chemometric approaches fail to effect quantification. Finally, to effect abs. quantification with SERS, the concepts of isotopologues is introduced along with the std. addn. method (SAM) and suitable examples that have been developed and exploit these techniques are presented. We believe that SERS will be routinely used for quant. anal. and it is only a matter of time before this technique translates from the lab. to the clin. environment.
- 20Bodelón, G.; Montes-García, V.; López-Puente, V.; Hill, E. H.; Hamon, C.; Sanz-Ortiz, M. N.; Rodal-Cedeira, S.; Costas, C.; Celiksoy, S.; Pérez-Juste, I. Detection and imaging of quorum sensing in Pseudomonas aeruginosa biofilm communities by surface-enhanced resonance Raman scattering. Nat. Mater. 2016, 15 (11), 1203– 1211, DOI: 10.1038/nmat472020https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhtlSgt7%252FI&md5=bf5a3741d94520e7a953e56ae6449a89Detection and imaging of quorum sensing in Pseudomonas aeruginosa biofilm communities by surface-enhanced resonance Raman scatteringBodelon, Gustavo; Montes-Garcia, Veronica; Lopez-Puente, Vanesa; Hill, Eric H.; Hamon, Cyrille; Sanz-Ortiz, Marta N.; Rodal-Cedeira, Sergio; Costas, Celina; Celiksoy, Sirin; Perez-Juste, Ignacio; Scarabelli, Leonardo; La Porta, Andrea; Perez-Juste, Jorge; Pastoriza-Santos, Isabel; Liz-Marzan, Luis M.Nature Materials (2016), 15 (11), 1203-1211CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)Most bacteria in nature exist as biofilms, which support intercellular signaling processes such as quorum sensing (QS), a cell-to-cell communication mechanism that allows bacteria to monitor and respond to cell d. and changes in the environment. As QS and biofilms are involved in the ability of bacteria to cause disease, there is a need for the development of methods for the non-invasive anal. of QS in natural bacterial populations. Here, by using surface-enhanced resonance Raman scattering spectroscopy, the authors report rationally designed nanostructured plasmonic substrates for the in situ, label-free detection of a QS signaling metabolite in growing Pseudomonas aeruginosa biofilms and microcolonies. The in situ, non-invasive plasmonic imaging of QS in biofilms provides a powerful anal. approach for studying intercellular communication on the basis of secreted mols. as signals.
- 21Benz, F.; Chikkaraddy, R.; Salmon, A.; Ohadi, H.; de Nijs, B.; Mertens, J.; Carnegie, C.; Bowman, R. W.; Baumberg, J. J. SERS of Individual Nanoparticles on a Mirror: Size Does Matter, but so Does Shape. J. Phys. Chem. Lett. 2016, 7 (12), 2264– 2269, DOI: 10.1021/acs.jpclett.6b0098621https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28Xos1Slu7k%253D&md5=7d74ab505397019668d9c60efe9285c8SERS of Individual Nanoparticles on a Mirror: Size Does Matter, but so Does ShapeBenz, Felix; Chikkaraddy, Rohit; Salmon, Andrew; Ohadi, Hamid; de Nijs, Bart; Mertens, Jan; Carnegie, Cloudy; Bowman, Richard W.; Baumberg, Jeremy J.Journal of Physical Chemistry Letters (2016), 7 (12), 2264-2269CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)Coupling noble metal nanoparticles by a 1 nm gap to an underlying Au mirror confines light to extremely small vols., useful for sensing on the nanoscale. Individually measuring 10,000 of such Au nanoparticles of increasing size dramatically shows the different scaling of their optical scattering (far-field) and surface-enhanced Raman emission (SERS, near-field). Linear red shifts of the coupled plasmon modes are seen with increasing size, matching theory. The total SERS from the few hundred mols. under each nanoparticle dramatically increases with increasing size. This scaling shows that max. SERS emission is always produced from the largest nanoparticles, irresp. of tuning to any plasmonic resonances. Changes of particle facet with nanoparticle size result in vastly weaker scaling of the near-field SERS, without much modifying the far-field, and allows simple approaches for optimizing practical sensing.
- 22Zeng, P.; Ma, D.; Zheng, M.; Chen, L.; Liang, H.; Shu, Z.; Fu, Y.; Pan, M.; Zhao, Q.; Duan, H. Flexible plasmonic nanoparticle-on-a-mirror metasurface-enabled substrates for high-quality surface-enhanced Raman spectroscopy detection. Colloid and Interface Science Communications 2023, 55, 100728, DOI: 10.1016/j.colcom.2023.100728There is no corresponding record for this reference.
- 23Zhang, C.; Yi, P.; Peng, L.; Lai, X.; Chen, J.; Huang, M.; Ni, J. Continuous fabrication of nanostructure arrays for flexible surface enhanced Raman scattering substrate. Sci. Rep. 2017, 7 (1), 39814, DOI: 10.1038/srep39814There is no corresponding record for this reference.
- 24Romo-Herrera, J. M.; Juarez-Moreno, K.; Guerrini, L.; Kang, Y.; Feliu, N.; Parak, W. J.; Alvarez-Puebla, R. A. Paper-based plasmonic substrates as surface-enhanced Raman scattering spectroscopy platforms for cell culture applications. Materials Today Bio 2021, 11, 100125, DOI: 10.1016/j.mtbio.2021.100125There is no corresponding record for this reference.
- 25Koh, E. H.; Lee, W.-C.; Choi, Y.-J.; Moon, J.-I.; Jang, J.; Park, S.-G.; Choo, J.; Kim, D.-H.; Jung, H. S. A Wearable Surface-Enhanced Raman Scattering Sensor for Label-Free Molecular Detection. ACS Appl. Mater. Interfaces 2021, 13 (2), 3024– 3032, DOI: 10.1021/acsami.0c1889225https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXjsl2hsw%253D%253D&md5=61192d3b6796e61f6a8c638cadfa5ec8A wearable surface-enhanced raman scattering sensor for label-free molecular detectionKoh, Eun Hye; Lee, Won-Chul; Choi, Yeong-Jin; Moon, Joung-Il; Jang, Jinah; Park, Sung-Gyu; Choo, Jaebum; Kim, Dong-Ho; Jung, Ho SangACS Applied Materials & Interfaces (2021), 13 (2), 3024-3032CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)A wearable surface-enhanced Raman scattering (SERS) sensor has been developed as a patch type to utilize as a mol. sweat sensor. Here, the SERS patch sensor is designed to comprise a sweat-absorbing layer, which is an interface to the human skin, an SERS active layer, and a dermal protecting layer that prevents damage and contaminations. A silk fibroin protein film (SFF) is a basement layer that absorbs aq. solns. and filtrates mols. larger than the nanopores created in the β-sheet matrix of the SFF. On the SFF layer, a plasmonic silver nanowire (AgNW) layer is formed to enhance the Raman signal of the mols. that penetrated through the SERS patch in a label-free method. A transparent dermal protecting layer (DP) allows laser penetration to the AgNW layer enabling Raman measurement through the SERS patch without its detachment from the surface. The mol. detection capability and time-dependent absorption properties of the SERS patch are investigated, and then, the feasibility of its use as a wearable drug detection sweat sensor is demonstrated using 2-fluoro-methamphetamine (2-FMA) on the human cadaver skin. It is believed that the developed SERS patch can be utilized as various flexible and wearable biosensors for healthcare monitoring.
- 26Hidi, I. J.; Jahn, M.; Weber, K.; Bocklitz, T.; Pletz, M. W.; Cialla-May, D.; Popp, J. Lab-on-a-Chip-Surface Enhanced Raman Scattering Combined with the Standard Addition Method: Toward the Quantification of Nitroxoline in Spiked Human Urine Samples. Anal. Chem. 2016, 88 (18), 9173– 9180, DOI: 10.1021/acs.analchem.6b0231626https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhsVehtrjP&md5=fdbdd1e65b53926b3019759de9e0dd82Lab-on-a-Chip-Surface Enhanced Raman Scattering Combined with the Standard Addition Method: Toward the Quantification of Nitroxoline in Spiked Human Urine SamplesHidi, Izabella J.; Jahn, Martin; Weber, Karina; Bocklitz, Thomas; Pletz, Mathias W.; Cialla-May, Dana; Popp, JuergenAnalytical Chemistry (Washington, DC, United States) (2016), 88 (18), 9173-9180CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)The emergence of antibacterial resistance and the development of new drugs lead to a continuous change of guidelines for medical treatments. Hence, new anal. tools are required for the detection of drugs in biol. fluids. In this study, the first surface enhanced Raman scattering (SERS) detection of nitroxoline (NTX) in purified water and in spiked human urine samples is reported. Insights concerning the nature of the mol.-metal interaction and its influence on the overall SERS signal are provided. Furthermore, three randomly collected urine samples originating from a healthy volunteer were spiked to assess the limit of detection (LOD), the limit of quantification (LOQ), and the linear dynamic range of the lab-on-a-chip SERS (LoC-SERS) method for NTX detection in human urine. The LOD is ∼3 μM (0.57 mg/L), LOQ ∼ 6.5 μM (1.23 mg/L) while the linear range is between 4.28 and 42.8 μM (0.81-8.13 mg/L). This covers the min. inhibitory concn. (MIC) values of the most commonly encountered uropathogens. Finally, seven clin. samples having an "unknown" NTX concn. were simulated. The LoC-SERS technique combined with the std. addn. method and statistical data anal. provided a good prediction of the unknown concns. Addnl., it is also demonstrated that the predictions carried out by multicurve resoln. alternating least-squares (MCR-ALS) algorithm provides reliable results, and it is preferred to a univariate statistical approach.
- 27Hidi, I. J.; Jahn, M.; Pletz, M. W.; Weber, K.; Cialla-May, D.; Popp, J. Toward Levofloxacin Monitoring in Human Urine Samples by Employing the LoC-SERS Technique. J. Phys. Chem. C 2016, 120 (37), 20613– 20623, DOI: 10.1021/acs.jpcc.6b0100527https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28Xkt1Cgtbk%253D&md5=79c81f25e4416810684819f0596fa760Toward Levofloxacin Monitoring in Human Urine Samples by Employing the LoC-SERS TechniqueHidi, Izabella J.; Jahn, Martin; Pletz, Mathias W.; Weber, Karina; Cialla-May, Dana; Popp, JuergenJournal of Physical Chemistry C (2016), 120 (37), 20613-20623CODEN: JPCCCK; ISSN:1932-7447. (American Chemical Society)The pharmacokinetics of antibiotics such as levofloxacin exhibits large interindividual differences, questioning the value of fixed dose regimens and warranting individual dosing based on therapeutic drug monitoring. Here, in a proof of principal study, it is shown that levofloxacin can be detected in human urine samples by employing lab-on-a-chip surface enhanced Raman spectroscopy (LoC-SERS). First, artificial urine is used as a matrix in order to get insights into the influence of different parameters such as matrix complexity, aggregation time, and matrix diln. on the overall SERS signal. Second, three anonymized individual and three pooled urine samples originating from patients undergoing either no or unknown medical treatments have been spiked with the target analyte. Measurements were performed with a benchtop and a portable Raman setup. In all six samples urinary levofloxacin concns. between 0.45 mM (162.6 μg/mL) and 1.8 mM (650.5 μg/mL) have been successfully detected. According to the literature, the normal levofloxacin concn. in urine is 1.38 mM ± 0.68 mM with a min. measured concn. of 0.45 mM after 4 h from the administration of a 500 mg dose. The presented results therefore show that LoC-SERS is a promising bioanal. tool for urine anal.
- 28Mühlig, A.; Bocklitz, T.; Labugger, I.; Dees, S.; Henk, S.; Richter, E.; Andres, S.; Merker, M.; Stöckel, S.; Weber, K. LOC-SERS: A Promising Closed System for the Identification of Mycobacteria. Anal. Chem. 2016, 88 (16), 7998– 8004, DOI: 10.1021/acs.analchem.6b01152There is no corresponding record for this reference.
- 29Han, G.; Liu, S.; Yang, Q.; Zeng, F.; Li, W.; Mao, X.; Xu, J.; Zhu, J. Polymer-grafted nanoparticle superlattice monolayers over 100 cm2 through a modified Langmuir-Blodgett method. Polymer 2022, 259, 125308, DOI: 10.1016/j.polymer.2022.12530829https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XisVKis7zN&md5=43ab108e1408fbfaaaed35975c2a8040Polymer-grafted nanoparticle superlattice monolayers over 100 cm2 through a modified Langmuir-Blodgett methodHan, Guoqiang; Liu, Simeng; Yang, Qi; Zeng, Fanyi; Li, Wang; Mao, Xi; Xu, Jiangping; Zhu, JintaoPolymer (2022), 259 (), 125308CODEN: POLMAG; ISSN:0032-3861. (Elsevier Ltd.)Two-dimensional polymer/nanoparticle (NP) composite superlattice monolayers have attracted great attention, due to their applications in flexible optical, sensing, and electronic devices. The large-scale fabrication of these devices requires large-area superlattice monolayers. However, the prepn. of large-area superlattice monolayers of polymer-grafted NP still faces great challenges. Herein, we report a modified Langmuir-Blodgett method for prepg. large-area superlattice monolayers of polystyrene-grafted gold NPs (AuNP@PS). This method involves two key steps: pre-assembling the AuNP@PS on a liq. surface using mixed high/low-boiling-point solvent as the spreading solvent and then compressing the pre-assembled film in low-boiling-point solvent vapor. The discrete monolayer islands of AuNP@PS are formed in the pre-assembly process. During the surface compression process, the introduction of solvent vapor facilitates the fusion of AuNP@PS islands to form the continuous superlattice monolayers. Otherwise, discrete films with nonuniform thickness are obtained by compression without solvent vapor. This strategy enables the prepn. of large superlattice monolayer films over 100 cm2, which are useful in the manuf. of microelectronic devices.
- 30Jaworska, A.; Fornasaro, S.; Sergo, V.; Bonifacio, A. Potential of Surface Enhanced Raman Spectroscopy (SERS) in Therapeutic Drug Monitoring (TDM). A Critical Review. Biosensors 2016, 6 (3), 47, DOI: 10.3390/bios6030047There is no corresponding record for this reference.
- 31Cutshaw, G.; Uthaman, S.; Hassan, N.; Kothadiya, S.; Wen, X.; Bardhan, R. The Emerging Role of Raman Spectroscopy as an Omics Approach for Metabolic Profiling and Biomarker Detection toward Precision Medicine. Chem. Rev. 2023, 123 (13), 8297– 8346, DOI: 10.1021/acs.chemrev.2c00897There is no corresponding record for this reference.
- 32Sausville, E. A. Chapter 30 - Drug Discovery. In Principles of Clinical Pharmacology, 3rd ed.; Atkinson, A. J., Huang, S.-M., Lertora, J. J. L., Markey, S. P., Eds.; Academic Press, 2013; p 507– 515.There is no corresponding record for this reference.
- 33Hughes, J. P.; Rees, S.; Kalindjian, S. B.; Philpott, K. L. Principles of early drug discovery. Br. J. Pharmacol. 2011, 162 (6), 1239– 1249, DOI: 10.1111/j.1476-5381.2010.01127.x33https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3MXivF2lt7o%253D&md5=05a0016f45b155f9fb5822f5c7bcc35dPrinciples of early drug discoveryHughes, J. P.; Rees, S.; Kalindjian, S. B.; Philpott, K. L.British Journal of Pharmacology (2011), 162 (6), 1239-1249CODEN: BJPCBM; ISSN:1476-5381. (Wiley-Blackwell)A review. Developing a new drug from original idea to the launch of a finished product is a complex process which can take 12-15 years and cost in excess of $1 billion. The idea for a target can come from a variety of sources including academic and clin. research and from the com. sector. It may take many years to build up a body of supporting evidence before selecting a target for a costly drug discovery program. Once a target was chosen, the pharmaceutical industry and more recently some academic centers have streamlined a no. of early processes to identify mols. which possess suitable characteristics to make acceptable drugs. This review will look at key preclin. stages of the drug discovery process, from initial target identification and validation, through assay development, high throughput screening, hit identification, lead optimization and finally the selection of a candidate mol. for clin. development.
- 34Dugger, S. A.; Platt, A.; Goldstein, D. B. Drug development in the era of precision medicine. Nat. Rev. Drug Discovery 2018, 17 (3), 183– 196, DOI: 10.1038/nrd.2017.22634https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhvFCjur%252FM&md5=e06762106391d7646c686e6ef773398aDrug development in the era of precision medicineDugger, Sarah A.; Platt, Adam; Goldstein, David B.Nature Reviews Drug Discovery (2018), 17 (3), 183-196CODEN: NRDDAG; ISSN:1474-1776. (Nature Research)A review. For the past three decades, the use of genomics to inform drug discovery and development pipelines has generated both excitement and scepticism. Although earlier efforts successfully identified some new drug targets, the overall clin. efficacy of developed drugs has remained unimpressive, owing in large part to the heterogeneous causes of disease. Recent technol. and anal. advances in genomics, however, have now made it possible to rapidly identify and interpret the genetic variation underlying a single patient's disease, thereby providing a window into patient-specific mechanisms that cause or contribute to disease, which could ultimately enable the 'precise' targeting of these mechanisms. Here, we first examine and highlight the successes and limitations of the earlier phases of genomics in drug discovery and development. We then review the current major efforts in precision medicine and discuss the potential broader utility of mechanistically guided treatments going forward.
- 35Berger, A. G.; Restaino, S. M.; White, I. M. Vertical-flow paper SERS system for therapeutic drug monitoring of flucytosine in serum. Anal. Chim. Acta 2017, 949, 59– 66, DOI: 10.1016/j.aca.2016.10.03535https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28Xhsl2isbrF&md5=58f63a65204dc6068d5351d9545184eeVertical-flow paper SERS system for therapeutic drug monitoring of flucytosine in serumBerger, Adam G.; Restaino, Stephen M.; White, Ian M.Analytica Chimica Acta (2017), 949 (), 59-66CODEN: ACACAM; ISSN:0003-2670. (Elsevier B.V.)A no. of life-saving drugs require therapeutic drug monitoring (TDM) for safe and effective use. Currently, however, TDM is performed using sophisticated anal. techniques relegated to central labs, increasing the cost per test and time to answer. Here, using a novel vertical flow membrane system with inkjet-printed surface enhanced Raman sensors, along with a portable spectrometer, we demonstrate a low cost and easy to use device to quantify levels of flucytosine, an antifungal that requires TDM for effective patient care, from undiluted human serum. To our knowledge, this work represents the first report of a passive vertical flow sample cleanup method with surface enhanced Raman detection. We first investigated and optimized the parameters of the vertical flow system for the detection of flucytosine in spiked serum samples. Then, using an optimized vertical-flow system utilizing nitrocellulose membranes and a paper SERS sensor, we achieved detection of down to 10 μg mL-1 flucytosine in undiluted serum, with quant. detection across the entire therapeutic range. This system reduces the assay time to about 15 min, far quicker than the current gold stds. We anticipate that this novel system will enable near-patient therapeutic drug monitoring, leading to the safe and effective administration of a no. of life-saving drugs. Furthermore, it will spawn the development of SERS detection systems capable of sepg. target analytes from real-world biol. matrixes.
- 36Bleker de Oliveira, M.; Koshkin, V.; Liu, G.; Krylov, S. N. Analytical Challenges in Development of Chemoresistance Predictors for Precision Oncology. Anal. Chem. 2020, 92 (18), 12101– 12110, DOI: 10.1021/acs.analchem.0c02644There is no corresponding record for this reference.
- 37Ludwig, J. A.; Weinstein, J. N. Biomarkers in Cancer Staging, Prognosis and Treatment Selection. Nature Reviews Cancer 2005, 5 (11), 845– 856, DOI: 10.1038/nrc173937https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2MXht1WitLbP&md5=bfc80c71bccd52dfdbf2cf5a86679c29Biomarkers in cancer staging, prognosis and treatment selectionLudwig, Joseph A.; Weinstein, John N.Nature Reviews Cancer (2005), 5 (11), 845-856CODEN: NRCAC4; ISSN:1474-175X. (Nature Publishing Group)A review. Advances in genomics, proteomics and mol. pathol. have generated many candidate biomarkers with potential clin. value. Their use for cancer staging and personalization of therapy at the time of diagnosis could improve patient care. However, translation from bench to bedside outside of the research setting has proved more difficult than might have been expected. Understanding how and when biomarkers can be integrated into clin. care is crucial if we want to translate the promise into reality.
- 38Dina, N. E.; Tahir, M. A.; Bajwa, S. Z.; Amin, I.; Valev, V. K.; Zhang, L. SERS-based antibiotic susceptibility testing: Towards point-of-care clinical diagnosis. Biosens. Bioelectron. 2023, 219, 114843, DOI: 10.1016/j.bios.2022.11484338https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XislKgsbbK&md5=39071904f91a964c3d0da5d3840ab3c1SERS-based antibiotic susceptibility testing: Towards point-of-care clinical diagnosisDina, Nicoleta Elena; Tahir, Muhammad Ali; Bajwa, Sadia Z.; Amin, Imran; Valev, Ventsislav K.; Zhang, LiwuBiosensors & Bioelectronics (2023), 219 (), 114843CODEN: BBIOE4; ISSN:0956-5663. (Elsevier B.V.)Emerging antibiotic resistant bacteria constitute one of the biggest threats to public health. Surface-enhanced Raman scattering (SERS) is highly promising for detecting such bacteria and for antibiotic susceptibility testing (AST). SERS is fast, non-destructive (can probe living cells) and it is technol. flexible (readily integrated with robotics and machine learning algorithms). However, in order to integrate into efficient point-of-care (PoC) devices and to effectively replace the current culture-based methods, it needs to overcome the challenges of reliability, cost and complexity. Recently, significant progress has been made with the emergence of both new questions and new promising directions of research and technol. development. This article brings together insights from several representative SERS-based AST studies and approaches oriented towards clin. PoC biosensing. It aims to serve as a ref. source that can guide progress towards PoC routines for identifying antibiotic resistant pathogens. In turn, such identification would help to trace the origin of sporadic infections, in order to prevent outbreaks and to design effective medical treatment and preventive procedures.
- 39Zhang, Q.-J.; Chen, Y.; Zou, X.-H.; Hu, W.; Ye, M.-L.; Guo, Q.-F.; Lin, X.-L.; Feng, S.-Y.; Wang, N. Promoting identification of amyotrophic lateral sclerosis based on label-free plasma spectroscopy. Annals of Clinical and Translational Neurology 2020, 7 (10), 2010– 2018, DOI: 10.1002/acn3.51194There is no corresponding record for this reference.
- 40Zhang, Q.-J.; Chen, Y.; Zou, X.-H.; Hu, W.; Lin, X.-L.; Feng, S.-Y.; Chen, F.; Xu, L.-Q.; Chen, W.-J.; Wang, N. Prognostic analysis of amyotrophic lateral sclerosis based on clinical features and plasma surface-enhanced Raman spectroscopy. Journal of Biophotonics 2019, 12 (8), e201900012, DOI: 10.1002/jbio.201900012There is no corresponding record for this reference.
- 41Duan, Z.; Chen, Y.; Ye, M.; Xiao, L.; Chen, Y.; Cao, Y.; Peng, Y.; Zhang, J.; Zhang, Y.; Yang, T. Differentiation and prognostic stratification of acute myeloid leukemia by serum-based spectroscopy coupling with metabolic fingerprints. The FASEB Journal 2022, 36 (7), e22416, DOI: 10.1096/fj.202200487RThere is no corresponding record for this reference.
- 42Xiao, L.; Bailey, K. A.; Wang, H.; Schultz, Z. D. Probing Membrane Receptor-Ligand Specificity with Surface- and Tip- Enhanced Raman Scattering. Anal. Chem. 2017, 89 (17), 9091– 9099, DOI: 10.1021/acs.analchem.7b0179642https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhtlWnsL%252FE&md5=1ef25ed06378cd9039d88debd66c54e0Probing Membrane Receptor-Ligand Specificity with Surface- and Tip- Enhanced Raman ScatteringXiao, Lifu; Bailey, Karen A.; Wang, Hao; Schultz, Zachary D.Analytical Chemistry (Washington, DC, United States) (2017), 89 (17), 9091-9099CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)The specific interaction between a ligand and a protein is a key component in minimizing off-target effects in drug discovery. Investigating these interactions with membrane protein receptors can be quite challenging. In this report, the authors show how spectral variance obsd. in surface-enhanced Raman scattering (SERS) and tip-enhanced Raman scattering (TERS) can be correlated with ligand specificity in affinity-based assays. Variations in the enhanced Raman spectra of three peptide ligands (i.e., cyclic-RGDFC, cyclic-isoDGRFC, and CisoDGRC), which have different binding affinity to αvβ3 integrin, are reported from isolated proteins and from receptors in intact cancer cell membranes. The SERS signal from the purified proteins provides basis spectra to analyze the signals in cells. Differences in the spectral variance within the SERS and TERS data for each ligand indicate larger variance for nonspecific ligand-receptor interactions. The SERS and TERS results are correlated with single particle tracking expts. of the ligand-functionalized nanoparticles with purified receptors on glass surfaces and living cells. These results demonstrate the ability to elucidate protein-ligand recognition using the obsd. vibrational spectra and provide perspective on binding specificity for small-mol. ligands in intact cell membranes, demonstrating a new approach for investigating drug specificity.
- 43Skinner, W. H.; Robinson, N.; Hardisty, G. R.; Fleming, H.; Geddis, A.; Bradley, M.; Gray, R. D.; Campbell, C. J. SERS microsensors for pH measurements in the lumen and ECM of stem cell derived human airway organoids. Chem. Commun. 2023, 59 (22), 3249– 3252, DOI: 10.1039/D2CC06582GThere is no corresponding record for this reference.
- 44Dorato, M. A.; Buckley, L. A. Toxicology Testing in Drug Discovery and Development. Current Protocols in Toxicology 2007, 31 (1), 1, DOI: 10.1002/0471141755.tx1901s31There is no corresponding record for this reference.
- 45Plou, J.; Molina-Martínez, B.; García-Astrain, C.; Langer, J.; García, I.; Ercilla, A.; Perumal, G.; Carracedo, A.; Liz-Marzán, L. M. Nanocomposite Scaffolds for Monitoring of Drug Diffusion in Three-Dimensional Cell Environments by Surface-Enhanced Raman Spectroscopy. Nano Lett. 2021, 21 (20), 8785– 8793, DOI: 10.1021/acs.nanolett.1c03070There is no corresponding record for this reference.
- 46Ensom, M. H.; Davis, G. A.; Cropp, C. D.; Ensom, R. J. Clinical pharmacokinetics in the 21st century. Does the evidence support definitive outcomes?. Clin Pharmacokinet 1998, 34 (4), 265– 279, DOI: 10.2165/00003088-199834040-00001There is no corresponding record for this reference.
- 47Neef, C.; Touw, D.; Stolk, L. Therapeutic Drug Monitoring in Clinical Research. Pharmaceutical Medicine 2008, 22, 235– 244, DOI: 10.1007/BF03256708There is no corresponding record for this reference.
- 48Panikar, S. S.; Ramírez-García, G.; Sidhik, S.; Lopez-Luke, T.; Rodriguez-Gonzalez, C.; Ciapara, I. H.; Castillo, P. S.; Camacho-Villegas, T.; De la Rosa, E. Ultrasensitive SERS Substrate for Label-Free Therapeutic-Drug Monitoring of Paclitaxel and Cyclophosphamide in Blood Serum. Anal. Chem. 2019, 91 (3), 2100– 2111, DOI: 10.1021/acs.analchem.8b0452348https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXisFyltbfF&md5=940c3e047d427a59c2d990b863b123ffUltrasensitive SERS substrate for label-free therapeutic-drug monitoring of paclitaxel and cyclophosphamide in blood serumPanikar, Sandeep Surendra; Ramirez-Garcia, Gonzalo; Sidhik, Siraj; Lopez-Luke, Tazara; Rodriguez-Gonzalez, Claramaria; Ciapara, Inocencio Higuera; Castillo, Pedro Salas; Camacho-Villegas, Tanya; De la Rosa, ElderAnalytical Chemistry (Washington, DC, United States) (2019), 91 (3), 2100-2111CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Surface-enhanced Raman spectroscopy (SERS) has recently emerged as an innovative tool for therapeutic-drug monitoring (TDM), making it an ideal candidate for personalized treatment. Herein, we report a layer-by-layer (LbL) approach for the fabrication of a highly reproducible hybrid SERS substrate based on graphene oxide (GO)-supported L-cysteine-functionalized starlike gold nanoparticles (SAuNPs). These designed substrates were utilized for TDM of paclitaxel and cyclophosphamide in blood serum. The SAuNPs' efficient binding at the edges of GO creates a better SERS hotspot with enhanced Raman sensitivity because of the spacing of ∼2.28 nm between the SAuNPs. In addn., the hierarchically modified substrate with a self-assembled monolayer of zwitterionic amino acid L-cysteines acts like a brush layer to prevent SERS-hotspot blockages and fouling by blood-serum proteins. The antifouling nature of the substrate was detd. quant. by a bichinchonic acid assay using bovine-serum albumin (BSA) as a protein model on the L-cysteine SAuNPs@GO hybrid substrate (the test) and a cysteamine SAuNPs@GO substrate (the control). The L-cysteine SAuNPs@GO hybrid exhibited 80.57% lower BSA fouling compared with that of the cysteamine SAuNPs@GO substrate. The SERS spectra were acquired within 20 s, with detection limits of 1.5 × 10-8 M for paclitaxel and 5 × 10-9 M for cyclophosphamide in blood serum. Such sensitivities are 4 times and 1 order of magnitude higher than the currently available sophisticated anal. techniques, which involve high costs with each anal.
- 49Litti, L.; Ramundo, A.; Biscaglia, F.; Toffoli, G.; Gobbo, M.; Meneghetti, M. A surface enhanced Raman scattering based colloid nanosensor for developing therapeutic drug monitoring. J. Colloid Interface Sci. 2019, 533, 621– 626, DOI: 10.1016/j.jcis.2018.08.10749https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXhs1CgurjJ&md5=64868c93dd40087330364a07768cd7a4A surface enhanced Raman scattering based colloid nanosensor for developing therapeutic drug monitoringLitti, Lucio; Ramundo, Andrea; Biscaglia, Francesca; Toffoli, Giuseppe; Gobbo, Marina; Meneghetti, MorenoJournal of Colloid and Interface Science (2019), 533 (), 621-626CODEN: JCISA5; ISSN:0021-9797. (Elsevier B.V.)Competitive reactions, on the surface of plasmonic nanostructures, allow exploiting SERS signals for quant. therapeutic drug monitoring. As an example, the concn. of Erlotinib, an anti-EGFR small mol., used for the treatment of non-small cell lung and pancreatic cancer, is detd. The numerous side effects and the variability of patient responses make Erlotinib a good candidate for monitoring. The new SERS based sensor can est. Erlotinib down to nanomolar concn. and is based on the chem. reaction of the drug and of a competitor SERS reporter on the surface of gold nanostructures. Colloid solns. of naked gold nanoparticles obtained by laser ablation in soln. were used for obtaining nanostructures with very efficient hot spots for SERS and with a clean surface for chem. Detection of the drug in the nanomolar concn. range is shown to be possible also in spiked plasma samples.
- 50Farquharson, S.; Gift, A. D.; Shende, C.; Maksymiuk, P.; Inscore, F. E.; Murran, J. Detection of 5-fluorouracil in saliva using surface-enhanced Raman spectroscopy. Vib. Spectrosc. 2005, 38 (1), 79– 84, DOI: 10.1016/j.vibspec.2005.02.021There is no corresponding record for this reference.
- 51Subaihi, A.; Almanqur, L.; Muhamadali, H.; AlMasoud, N.; Ellis, D. I.; Trivedi, D. K.; Hollywood, K. A.; Xu, Y.; Goodacre, R. Rapid, Accurate, and Quantitative Detection of Propranolol in Multiple Human Biofluids via Surface-Enhanced Raman Scattering. Anal. Chem. 2016, 88 (22), 10884– 10892, DOI: 10.1021/acs.analchem.6b02041There is no corresponding record for this reference.
- 52Yang, J.; Cui, Y.; Zong, S.; Zhang, R.; Song, C.; Wang, Z. Tracking Multiplex Drugs and Their Dynamics in Living Cells Using the Label-Free Surface-Enhanced Raman Scattering Technique. Mol. Pharmaceutics 2012, 9 (4), 842– 849, DOI: 10.1021/mp200667dThere is no corresponding record for this reference.
- 53Koike, K.; Bando, K.; Ando, J.; Yamakoshi, H.; Terayama, N.; Dodo, K.; Smith, N. I.; Sodeoka, M.; Fujita, K. Quantitative Drug Dynamics Visualized by Alkyne-Tagged Plasmonic-Enhanced Raman Microscopy. ACS Nano 2020, 14 (11), 15032– 15041, DOI: 10.1021/acsnano.0c0501053https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BB3s7jslKltw%253D%253D&md5=05b4a214af3f7cb13e182e71fe0d6d59Quantitative Drug Dynamics Visualized by Alkyne-Tagged Plasmonic-Enhanced Raman MicroscopyKoike Kota; Bando Kazuki; Ando Jun; Fujita Katsumasa; Koike Kota; Fujita Katsumasa; Yamakoshi Hiroyuki; Terayama Naoki; Dodo Kosuke; Sodeoka Mikiko; Smith Nicholas Isaac; Fujita KatsumasaACS nano (2020), 14 (11), 15032-15041 ISSN:.Visualizing live-cell uptake of small-molecule drugs is paramount for drug development and pharmaceutical sciences. Bioorthogonal imaging with click chemistry has made significant contributions to the field, visualizing small molecules in cells. Furthermore, recent developments in Raman microscopy, including stimulated Raman scattering (SRS) microscopy, have realized direct visualization of alkyne-tagged small-molecule drugs in live cells. However, Raman and SRS microscopy still suffer from limited detection sensitivity with low concentration molecules for observing temporal dynamics of drug uptake. Here, we demonstrate the combination of alkyne-tag and surface-enhanced Raman scattering (SERS) microscopy for the real-time monitoring of drug uptake in live cells. Gold nanoparticles are introduced into lysosomes of live cells by endocytosis and work as SERS probes. Raman signals of alkynes can be boosted by enhanced electric fields generated by plasmon resonance of gold nanoparticles when alkyne-tagged small molecules are colocalized with the nanoparticles. With time-lapse 3D SERS imaging, this technique allows us to investigate drug uptake by live cells with different chemical and physical conditions. We also perform quantitative evaluation of the uptake speed at the single-cell level using digital SERS counting under different quantities of drug molecules and temperature conditions. Our results illustrate that alkyne-tag SERS microscopy has a potential to be an alternative bioorthogonal imaging technique to investigate temporal dynamics of small-molecule uptake of live cells for pharmaceutical research.
- 54Han, G.; Liu, R.; Han, M.-Y.; Jiang, C.; Wang, J.; Du, S.; Liu, B.; Zhang, Z. Label-Free Surface-Enhanced Raman Scattering Imaging to Monitor the Metabolism of Antitumor Drug 6-Mercaptopurine in Living Cells. Anal. Chem. 2014, 86 (23), 11503– 11507, DOI: 10.1021/ac503539wThere is no corresponding record for this reference.
- 55Jamieson, L. E.; Byrne, H. J. Vibrational spectroscopy as a tool for studying drug-cell interaction: Could high throughput vibrational spectroscopic screening improve drug development?. Vib. Spectrosc. 2017, 91, 16– 30, DOI: 10.1016/j.vibspec.2016.09.00355https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28Xhs1Srsb7O&md5=496272549a5f2d0219e4089926bf45f2Vibrational spectroscopy as a tool for studying drug-cell interaction: Could high throughput vibrational spectroscopic screening improve drug development?Jamieson, Lauren E.; Byrne, Hugh J.Vibrational Spectroscopy (2017), 91 (), 16-30CODEN: VISPEK; ISSN:0924-2031. (Elsevier B.V.)Vibrational spectroscopy is currently widely explored as a tool in biomedical applications. An area at the forefront of this field is the use of vibrational spectroscopy for disease diagnosis, ultimately aiming towards spectral pathol. However, while this field shows promising results, moving this technique into the clinic faces the challenges of widespread clin. trials and legislative approval. While spectral pathol. has received a lot of attention, there are many other biomedical applications of vibrational spectroscopy, which could potentially be translated to applications with greater ease. A particularly promising application is the use of vibrational spectroscopic techniques to study the interaction of drugs with cells. Many studies have demonstrated the ability to detect biochem. changes in cells in response to drug application, using both IR and Raman spectroscopy. This has shown potential for use in high throughput screening (HTS) applications, for screening of efficacy and mode of action of potential drug candidates, to speed up the drug discovery process. HTS is still a relatively new and growing area of research and, therefore, there is more potential for new techniques to move into and shape this field. Vibrational spectroscopic techniques come with many benefits over the techniques used currently in HTS, primarily based on fluorescence assays to detect specific binding interactions or phenotypes. They are label free, and an IR or Raman spectrum provides a wealth of biochem. information, and therefore could reveal not only information about a specific interaction, but about how the overall biochem. of a cell changes in response to application of a drug candidate. Therefore, drug mode of action could be elucidated. This review will investigate the potential for vibrational spectroscopy, particularly FTIR and Raman spectroscopy, to benefit the field of HTS and improve the drug development process. In addn. to FTIR and Raman spectroscopy, surface enhanced Raman spectroscopy (SERS), coherent anti-Stokes Raman spectroscopy (CARS) and stimulated Raman spectroscopy (SRS), will be investigated as an alternative tool in the HTS process.
- 56Kim, W.; Lee, S. H.; Kim, J. H.; Ahn, Y. J.; Kim, Y.-H.; Yu, J. S.; Choi, S. Paper-Based Surface-Enhanced Raman Spectroscopy for Diagnosing Prenatal Diseases in Women. ACS Nano 2018, 12 (7), 7100– 7108, DOI: 10.1021/acsnano.8b0291756https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXhtFKlsrjM&md5=89ff42790c523a9f613f31718ee5d5c1Paper-Based Surface-Enhanced Raman Spectroscopy for Diagnosing Prenatal Diseases in WomenKim, Wansun; Lee, Soo Hyun; Kim, Jin Hwi; Ahn, Yong Jin; Kim, Yeon-Hee; Yu, Jae Su; Choi, SamjinACS Nano (2018), 12 (7), 7100-7108CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)The authors report the development of a surface-enhanced Raman spectroscopy sensor chip by decorating gold nanoparticles (AuNPs) on ZnO nanorod (ZnO NR) arrays vertically grown on cellulose paper (C). These chips can enhance the Raman signal by 1.25 × 107 with an excellent reproducibility of <6%. The authors can measure trace amts. of human amniotic fluids of patients with subclin. intra-amniotic infection (IAI) and preterm delivery (PTD) using the chip in combination with a multivariate statistics-derived machine-learning-trained bioclassification method. The authors can detect the presence of prenatal diseases and identify the types of diseases from amniotic fluids with >92% clin. sensitivity and specificity. The authors' technol. has the potential to be used for the early detection of prenatal diseases and can be adapted for point-of-care applications.
- 57Torul, H.; Çiftçi, H.; Çetin, D.; Suludere, Z.; Boyacı, I. H.; Tamer, U. Paper membrane-based SERS platform for the determination of glucose in blood samples. Anal Bioanal Chem. 2015, 407 (27), 8243– 8251, DOI: 10.1007/s00216-015-8966-x57https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXhsV2jurrL&md5=01222db6845e9ebeecec7de01af46898Paper membrane-based SERS platform for the determination of glucose in blood samplesTorul, Hilal; Ciftci, Hakan; Cetin, Demet; Suludere, Zekiye; Boyaci, Ismail Hakki; Tamer, UgurAnalytical and Bioanalytical Chemistry (2015), 407 (27), 8243-8251CODEN: ABCNBP; ISSN:1618-2642. (Springer)In this report, we present a paper membrane-based surface-enhanced Raman scattering (SERS) platform for the detn. of blood glucose level using a nitrocellulose membrane as substrate paper, and the microfluidic channel was simply constructed by wax-printing method. The rod-shaped gold nanorod particles were modified with 4-mercaptophenylboronic acid (4-MBA) and 1-decanethiol (1-DT) mols. and used as embedded SERS probe for paper-based microfluidics. The SERS measurement area was simply constructed by dropping gold nanoparticles on nitrocellulose membrane, and the blood sample was dropped on the membrane hydrophilic channel. While the blood cells and proteins were held on nitrocellulose membrane, glucose mols. were moved through the channel toward the SERS measurement area. SEM was used to confirm the effective sepn. of blood matrix, and total anal. is completed in 5 min. In SERS measurements, the intensity of the band at 1070 cm-1 which is attributed to B-OH vibration decreased depending on the rise in glucose concn. in the blood sample. The glucose concn. was found to be 5.43 ± 0.51 mM in the ref. blood sample by using a calibration equation, and the certified value for glucose was 6.17 ± 0.11 mM. The recovery of the glucose in the ref. blood sample was about 88 %. According to these results, the developed paper-based microfluidic SERS platform has been found to be suitable for use for the detection of glucose in blood samples without any pretreatment procedure. We believe that paper-based microfluidic systems may provide a wide field of usage for paper-based applications.
- 58Liu, G.; Mu, Z.; Guo, J.; Shan, K.; Shang, X.; Yu, J.; Liang, X. Surface-enhanced Raman scattering as a potential strategy for wearable flexible sensing and point-of-care testing non-invasive medical diagnosis. Frontiers in Chemistry 2022, 10, 1060322, DOI: 10.3389/fchem.2022.1060322There is no corresponding record for this reference.
- 59Liu, L.; Martinez Pancorbo, P.; Xiao, T.-H.; Noguchi, S.; Marumi, M.; Segawa, H.; Karhadkar, S.; Gala de Pablo, J.; Hiramatsu, K.; Kitahama, Y. Highly Scalable, Wearable Surface-Enhanced Raman Spectroscopy. Advanced Optical Materials 2022, 10 (17), 2200054, DOI: 10.1002/adom.20220005459https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38Xhs1Clu7jL&md5=a2a445d93dc33ab82064a629a5bfe773Highly Scalable, Wearable Surface-Enhanced Raman SpectroscopyLiu, Limei; Martinez Pancorbo, Pablo; Xiao, Ting-Hui; Noguchi, Saya; Marumi, Machiko; Segawa, Hiroki; Karhadkar, Siddhant; Gala de Pablo, Julia; Hiramatsu, Kotaro; Kitahama, Yasutaka; Itoh, Tamitake; Qu, Junle; Takei, Kuniharu; Goda, KeisukeAdvanced Optical Materials (2022), 10 (17), 2200054CODEN: AOMDAX; ISSN:2195-1071. (Wiley-VCH Verlag GmbH & Co. KGaA)The last two decades have witnessed a dramatic growth of wearable sensor technol., mainly represented by flexible, stretchable, on-skin electronic sensors that provide rich information of the wearer's health conditions and surroundings. A recent breakthrough in the field is the development of wearable chem. sensors based on surface-enhanced Raman spectroscopy (SERS) that can detect mol. fingerprints universally, sensitively, and noninvasively. However, while their sensing properties are excellent, these sensors are not scalable for widespread use beyond small-scale human health monitoring due to their cumbersome fabrication process and limited multifunctional sensing capabilities. Here, a highly scalable, wearable SERS sensor is demonstrated based on an easy-to-fabricate, low-cost, ultrathin, flexible, stretchable, adhesive, and biointegratable gold nanomesh. It can be fabricated in any shape and worn on virtually any surface for label-free, large-scale, in situ sensing of diverse analytes from low to high concns. (10-106 x 10-9M). To show the practical utility of the wearable SERS sensor, the sensor is tested for the detection of sweat biomarkers, drugs of abuse, and microplastics. This wearable SERS sensor represents a significant step toward the generalizability and practicality of wearable sensing technol.
- 60Wang, Y.; Zhao, C.; Wang, J.; Luo, X.; Xie, L.; Zhan, S.; Kim, J.; Wang, X.; Liu, X.; Ying, Y. Wearable plasmonic-metasurface sensor for noninvasive and universal molecular fingerprint detection on biointerfaces. Science Advances 2021, 7 (4), eabe4553, DOI: 10.1126/sciadv.abe4553There is no corresponding record for this reference.
- 61Jeong, J. W.; Arnob, M. M. P.; Baek, K.-M.; Lee, S. Y.; Shih, W.-C.; Jung, Y. S. 3D Cross-Point Plasmonic Nanoarchitectures Containing Dense and Regular Hot Spots for Surface-Enhanced Raman Spectroscopy Analysis. Adv. Mater. 2016, 28 (39), 8695– 8704, DOI: 10.1002/adma.20160260361https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhtlalsLfE&md5=a614a3a6d33312f6f1fa6f6712d4659e3D cross-point plasmonic nanoarchitectures containing dense and regular hot spots for surface-enhanced raman spectroscopy analysisJeong, Jae Won; Arnob, Md Masud Parvez; Baek, Kwang-Min; Lee, Seung Yong; Shih, Wei-Chuan; Jung, Yeon SikAdvanced Materials (Weinheim, Germany) (2016), 28 (39), 8695-8704CODEN: ADVMEW; ISSN:0935-9648. (Wiley-VCH Verlag GmbH & Co. KGaA)Herein, we demonstrate the realization of vertically stacked 3D cross-point plasmonic nanostructures with excellent SERS signal intensity and uniformity over a macroscopic area based on high resoln. nanotransfer printing (nTP). For more facile and rapid stacking of multilayer nanostructures, we developed and applied a second generation solvent assisted nanotransfer printing (SnTP) technique based on a multipurpose single layer replica without using an addnl. transfer medium, thereby significantly simplifying the overall nTP steps and enabling the prompt repetition of nTP for multilayer stacking of nanowires. We report that sequentially transfer-printed sub-20 nm nanowires can provide both an in-plane coupling effect in the nanogap region and an out-of-coupling effect at the cross-points where two nanowires are closely stacked, achieving excellent enhancement of Raman signals from probed mols. with an av. enhancement factor of ≈ 4.1×107 depending on structural and material parameters. Moreover, nanowires-on-film hybrid structures obtained by sequential printing on a continuous metal film show highly intensified SERS signals due to vertical plasmonic coupling between the upper nanowires and the underlying film.
- 62Masson, J.-F. The Need for Benchmarking Surface-Enhanced Raman Scattering (SERS) Sensors. ACS Sensors 2021, 6 (11), 3822– 3823, DOI: 10.1021/acssensors.1c02275There is no corresponding record for this reference.