Second-Derivative-Based Background Drift Removal for a Tonic Dopamine Measurement in Fast-Scan Cyclic VoltammetryClick to copy article linkArticle link copied!
- Seongtak KangSeongtak KangDepartment of Electrical Engineering and Computer Science, Daegu Gyeongbuk Institute of Science and Technology (DGIST), 333, Techno jungang-daero, Hyeonpung-myeon, Dalseong-gun, Daegu 42988, Republic of KoreaMore by Seongtak Kang
- Jeongrak ParkJeongrak ParkDepartment of Brain and Cognitive Science, DGIST, 333, Techno jungang-daero, Hyeonpung-myeon, Dalseong-gun, Daegu 42988, Republic of KoreaMore by Jeongrak Park
- Yunho JeongYunho JeongCollege of Transdisciplinary studies, DGIST, 333, Techno jungang-daero, Hyeonpung-myeon, Dalseong-gun, Daegu 42988, Republic of KoreaMore by Yunho Jeong
- Yong-Seok OhYong-Seok OhDepartment of Brain and Cognitive Science, DGIST, 333, Techno jungang-daero, Hyeonpung-myeon, Dalseong-gun, Daegu 42988, Republic of KoreaMore by Yong-Seok Oh
- Ji-Woong Choi*Ji-Woong Choi*Email: [email protected]Department of Electrical Engineering and Computer Science, Daegu Gyeongbuk Institute of Science and Technology (DGIST), 333, Techno jungang-daero, Hyeonpung-myeon, Dalseong-gun, Daegu 42988, Republic of KoreaBrain Engineering Convergence Research Center, DGIST, 333, Techno jungang-daero, Hyeonpung-myeon, Dalseong-gun, Daegu 42988, Republic of KoreaMore by Ji-Woong Choi
Abstract
The dysregulation of dopamine, a neuromodulator, is associated with a broad spectrum of brain disorders, including Parkinson’s disease, addiction, and schizophrenia. Quantitative measurements of dopamine are essential for understanding dopamine functional dynamics. Fast-scan cyclic voltammetry (FSCV) is the most popular electrochemical technique for measuring real-time in vivo dopamine level changes. Standard FSCV has only analyzed “phasic dopamine” (changes in seconds) because the gradual generation of background charging current is inevitable and is the primary noise source in the low-frequency band. Although “tonic dopamine” (changes in minutes to hours) is critical for understanding the dopamine system, an electrochemical technique capable of simultaneously measuring phasic and tonic dopamine in an in vivo environment has not been established. Several modified voltammetric techniques have been developed for measuring tonic dopamine; however, the sampling rates (0.1–0.05 Hz) are too low to be useful. Further investigation of the in vivo applicability of previously developed background drift removal methods for measuring tonic dopamine levels is required. We developed a second-derivative-based background removal (SDBR) method for simultaneously measuring phasic and tonic neurotransmitter levels in real-time. The performance of this technique was tested via in silico and in vitro tonic dopamine experiments. Furthermore, its applicability was tested in vivo. SDBR is a simple, robust, postprocessing technique that can extract tonic neurotransmitter levels from all FSCV data. As SDBR is calculated in individual-scan voltammogram units, it can be applied to any real-time closed-loop system that uses a neurotransmitter as a biomarker.
This publication is licensed for personal use by The American Chemical Society.
Materials and Methods
Data Acquisition and Analysis
In Vitro Experiment
Surgery and In Vivo Dopamine Measurements
Second-Derivative-Based Background Drift Removal (SDBR) Method




Results and Discussion
SDBR In Vitro Experiments
Figure 1
Figure 1. In vitro test of SDBR to record the tonic and phasic dopamine with standard FSCV. (A) Raw FSCV color plot in vitro test. The black dotted line denotes the timing of the 200 nM dopamine drop. Each circled number and the corresponding colored-line are the voltammogram at a specific time, detailed in (E)–(H). (B) Background-subtracted color plot and current change of dopamine peak over time. (C) SDBR applied color plot and current change of dopamine peak over time. (D) A calibration plot obtained by SDBR (R2 = 0.996), slope = 0.0319 ± 0.0003 pA/V2 nM–1, limit of detection = 8.16 ± 0.08 nM (n = 5 electrodes). (E, F) Comparison of background subtraction and SDBR for three voltammograms measuring the same concentration at 2 min intervals. (G, H) Three voltammograms were measured 10 min after each drop of dopamine solution for comparison of background subtraction and SDBR. (E, G) Left: the background-subtracted voltammogram, right: the enlarged voltammogram of the red dotted box in the left image. (F, H) Left: the result of applying SDBR to the raw voltammogram, right: the enlarged SDBR result of the blue dotted box in the left image.
SDBR In Vivo Experiments
Figure 2
Figure 2. Measurement of tonic dopamine level change using SDBR during in vivo pharmacological stimulation. (A) SDBR results were measured in the striatum of healthy mice (n = 3) following saline intraperitoneal (IP) injection. (B) SDBR measured in the striatum of PD model mice (n = 3) following levodopa (10 mg kg–1) IP injection. (C) SDBR measured in the striatum of healthy mice (n = 3) following reserpine (5 mg kg–1) IP injection. Bold blue line represents mean concentrations over time, and the light blue line around the bold line represents the standard error of the mean (SEM). The upper black bar indicates significant differences compared to saline injection (2-way ANOVA, p < 0.0001, Dunnett’s multiple comparison test). Data from Figures 1 and 2 are freely available online. (36)
method | temporal resolution | simultaneous availability of phasic dopamine | need to modify the waveform of standard FSCV? | limit of detection (nM) | ref |
---|---|---|---|---|---|
FSCAV | 20 s | partially | yes | 3.7 ± 0.5 | (24) |
CBM-FSCV | 10 s | no | yes | 5.8 ± 0.9 | (26) |
convolution-based current removal | 1 s | yes | yes | <40 | (28) |
M-CSWV | 10 s | no | yes | 0.17 ± 0.03 | (25) |
SWV | 15 s | no | yes | 2.03 ± 0.09 | (27) |
SDBR | 0.1 s | yes | no | 8.16 ± 0.08 | proposed |
Conclusions
Supporting Information
The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.analchem.2c01047.
Author contributions, selectivity test, surgery, and in vivo dopamine measurement experiment details and in silico test (PDF)
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Acknowledgments
This research was supported by the Bio & Medical Technology Development Program of the National Research Foundation (NRF), funded by the Korean government (MSIT; No. 2017M3A9G8084463).
References
This article references 36 other publications.
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- 7Mohebi, A.; Pettibone, J. R.; Hamid, A. A.; Wong, J.-M. T.; Vinson, L. T.; Patriarchi, T.; Tian, L.; Kennedy, R. T.; Berke, J. D. Dissociable dopamine dynamics for learning and motivation. Nature 2019, 570 (7759), 65– 70, DOI: 10.1038/s41586-019-1235-yGoogle Scholar7https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhtVajsrjL&md5=e9ff25e5e8e976de181b597e0d516b23Dissociable dopamine dynamics for learning and motivationMohebi, Ali; Pettibone, Jeffrey R.; Hamid, Arif A.; Wong, Jenny-Marie T.; Vinson, Leah T.; Patriarchi, Tommaso; Tian, Lin; Kennedy, Robert T.; Berke, Joshua D.Nature (London, United Kingdom) (2019), 570 (7759), 65-70CODEN: NATUAS; ISSN:0028-0836. (Nature Research)The dopamine projection from ventral tegmental area (VTA) to nucleus accumbens (NAc) is crit. for motivation to work for rewards and reward-driven learning. How dopamine supports both functions is unclear. Dopamine cell spiking can encode prediction errors, which are vital learning signals in computational theories of adaptive behavior. By contrast, dopamine release ramps up as animals approach rewards, mirroring reward expectation. This mismatch might reflect differences in behavioral tasks, slower changes in dopamine cell spiking or spike-independent modulation of dopamine release. Here we compare spiking of identified VTA dopamine cells with NAc dopamine release in the same decision-making task. Cues that indicate an upcoming reward increased both spiking and release. However, NAc core dopamine release also covaried with dynamically evolving reward expectations, without corresponding changes in VTA dopamine cell spiking. Our results suggest a fundamental difference in how dopamine release is regulated to achieve distinct functions: broadcast burst signals promote learning, whereas local control drives motivation.
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- 12Wipf, D. O.; Kristensen, E. W.; Deakin, M. R.; Wightman, R. M. Fast-scan cyclic voltammetry as a method to measure rapid heterogeneous electron-transfer kinetics. Anal. Chem. 1988, 60 (4), 306– 310, DOI: 10.1021/ac00155a006Google Scholar12https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaL1cXmsVCktQ%253D%253D&md5=718c905317214cad42471414482e3f86Fast-scan cyclic voltammetry as a method to measure rapid heterogeneous electron-transfer kineticsWipf, David O.; Kristensen, Eric W.; Deakin, Mark R.; Wightman, R. MarkAnalytical Chemistry (1988), 60 (4), 306-10CODEN: ANCHAM; ISSN:0003-2700.The use of fast-scan cyclic voltammetry for the measurement of heterogeneous electron-transfer kinetics was examd. The distortions caused by the measurement instrumentation, ohmic drop, and the cell time const. were considered. These parameters combine to set an upper limit on the scan rate at which undistorted data can be achieved. At higher scan rates, meaningful data can be obtained and the distortion can be accounted for qual. With the exception of the instrumental distortion, the upper limit is inversely proportional to the radius of a disk or hemispherical electrode. Several outer-sphere electron-transfer couples were examd. The measured rate for Ru(NH3)63+ redn. agrees with literature values. In contrast, much higher heterogeneous rates were detd. for oxidn. of ferrocene and redn. of Ru(bpy)32+ (bpy = 2,2'-bipyridine) than previously reported.
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- 14Heien, M. L.; Phillips, P. E.; Stuber, G. D.; Seipel, A. T.; Wightman, R. M. Overoxidation of carbon-fiber microelectrodes enhances dopamine adsorption and increases sensitivity. Analyst 2003, 128 (12), 1413– 1419, DOI: 10.1039/b307024gGoogle Scholar14https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3sXpsFymsLY%253D&md5=6eaf749094e6cd0faf2d8d169b2220f8Overoxidation of carbon-fiber microelectrodes enhances dopamine adsorption and increases sensitivityHeien, Michael L. A. V.; Phillips, Paul E. M.; Stuber, Garret D.; Seipel, Andrew T.; Wightman, R. MarkAnalyst (Cambridge, United Kingdom) (2003), 128 (12), 1413-1419CODEN: ANALAO; ISSN:0003-2654. (Royal Society of Chemistry)The voltammetric responses of carbon-fiber microelectrodes with a 1.0 V and a 1.4 V anodic limit were compared in this study. Fast-scan cyclic voltammetry was used to characterize the response to dopamine and several other neurochems. An increase in the adsorption properties of the carbon fiber leads to an increase in sensitivity of 9-fold in vivo. However the temporal response of the sensor is slower with the more pos. anodic limit. Increased electron transfer kinetics also causes a decrease in the relative sensitivity for dopamine vs. other neurochems., and a change in their cyclic voltammograms. Stimulated release in the caudate-putamen was pharmacol. characterized in vivo using Ro-04-1284 and pargyline, and was consistent with that expected for dopamine.
- 15Venton, B. J.; Cao, Q. Fundamentals of fast-scan cyclic voltammetry for dopamine detection. Analyst 2020, 145 (4), 1158– 1168, DOI: 10.1039/C9AN01586HGoogle Scholar15https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXisVyqsrnP&md5=7c87cc2797c92a70ad60a638f9b74056Fundamentals of fast-scan cyclic voltammetry for dopamine detectionVenton, B. Jill; Cao, QunAnalyst (Cambridge, United Kingdom) (2020), 145 (4), 1158-1168CODEN: ANALAO; ISSN:0003-2654. (Royal Society of Chemistry)A review. Fast-scan cyclic voltammetry (FSCV) was used with carbon-fiber microelectrodes for the real-time detection of neurotransmitters on the subsecond time scale. With FSCV, the potential is ramped up from a holding potential to a switching potential and back, usually at a 400 V s-1 scan rate and a frequency of 10 Hz. The plot of current vs. applied potential, the cyclic voltammogram (CV), has a very different shape for FSCV than for traditional cyclic voltammetry collected at scan rates which are 1000-fold slower. Here, the authors explore the theory of FSCV, with a focus on dopamine detection. First, the authors examine the shape of the CVs. Background currents, which are 100-fold higher than faradaic currents, are subtracted out. Peak sepn. is primarily due to slow electron transfer kinetics, while the sym. peak shape is due to exhaustive electrolysis of all the adsorbed neurotransmitters. Second, the authors explain the origins of the dopamine waveform, and the factors that limit the holding potential (oxygen redn.), switching potential (water oxidn.), scan rate (electrode instability), and repetition rate (adsorption). Third, data anal., from data visualization with color plots, to the automated algorithms like principal components regression that distinguish dopamine from pH changes are discussed. Finally, newer applications are discussed, including optimization of waveforms for analyte selectivity, carbon nanomaterial electrodes that trap dopamine, and basal level measurements that facilitate neurotransmitter measurements on a longer time scale. FSCV theory is complex, but understanding it enables better development of new techniques to monitor neurotransmitters in vivo.
- 16Rafi, H.; Zestos, A. G. Review-Recent Advances in FSCV Detection of Neurochemicals via Waveform and Carbon Microelectrode Modification. J. Electrochem. Soc. 2021, 168 (5), 057520, DOI: 10.1149/1945-7111/ac0064Google Scholar16https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhtlOjurrK&md5=6257f3533e7a1b179f1cb9e39075422eReview-recent advances in FSCV detection of neurochemicals via waveform and carbon microelectrode modificationRafi, Harmain; Zestos, Alexander G.Journal of the Electrochemical Society (2021), 168 (5), 057520CODEN: JESOAN; ISSN:1945-7111. (IOP Publishing Ltd.)Fast scan cyclic voltammetry (FSCV) is an anal. technique that was first developed over 30 years ago. Since then, it has been extensively used to detect dopamine using carbon fiber microelectrodes (CFMEs). More recently, electrode modifications and waveform refinement have enabled the detection of a wider variety of neurochems. including nucleosides such as adenosine and guanosine, neurotransmitter metabolites of dopamine, and neuropeptides such as enkephalin. These alterations have facilitated the selectivity of certain biomols. over others to enhance the measurement of the analyte of interest while excluding interferants. In this review, we detail these modifications and how specializing CFME sensors allows neuro-anal. researchers to develop tools to understand the neurochem. of the brain in disease states and provide groundwork for translational work in clin. settings.
- 17Logman, M. J.; Budygin, E. A.; Gainetdinov, R. R.; Wightman, R. M. Quantitation of in vivo measurements with carbon fiber microelectrodes. Journal of neuroscience methods 2000, 95 (2), 95– 102, DOI: 10.1016/S0165-0270(99)00155-7Google Scholar17https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3cXhtFamsb4%253D&md5=cb7f300804ffd5ed6af21884948fc877Quantitation of in vivo measurements with carbon fiber microelectrodesLogman, M. J.; Budygin, E. A.; Gainetdinov, R. R.; Wightman, R. M.Journal of Neuroscience Methods (2000), 95 (2), 95-102CODEN: JNMEDT; ISSN:0165-0270. (Elsevier Science B.V.)Fast-scan cyclic voltammetry (FSCV) at carbon fiber disk microelectrodes and quant. microdialysis were used to measure striatal concn. changes of N-acetyl-p-aminophenol (APAP, acetaminophen) following an i.p. injection of 75 mg/kg APAP in rats. The goal of this work was to det. which in vitro calibration procedure, precalibration or postcalibration, gave the most accurate results when using carbon fiber microelectrodes in vivo. Voltammetric detection of APAP in vivo was complicated with normal electrodes by interference from pH changes. An electrode treatment was used to minimize electrode sensitivity to pH and this allowed successful APAP detection. In vitro calibrations of the treated carbon fiber disk microelectrodes before and after the in vivo expt. were used to calc. APAP concn. changes measured in vivo and compared to microdialysis results. The maximal striatal APAP concn. detd. by microdialysis, adjusted for in vitro recovery, was 23.1 μM. The electrochem. results were approx. two times greater (postcalibration) or smaller (precalibration) than the microdialysis result.
- 18Hermans, A.; Keithley, R. B.; Kita, J. M.; Sombers, L. A.; Wightman, R. M. Dopamine detection with fast-scan cyclic voltammetry used with analog background subtraction. Anal. Chem. 2008, 80 (11), 4040– 4048, DOI: 10.1021/ac800108jGoogle Scholar18https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXltVeis7k%253D&md5=2f28072cd6664925df823832c00ef287Dopamine Detection with Fast-Scan Cyclic Voltammetry Used with Analog Background SubtractionHermans, Andre; Keithley, Richard B.; Kita, Justin M.; Sombers, Leslie A.; Wightman, R. MarkAnalytical Chemistry (Washington, DC, United States) (2008), 80 (11), 4040-4048CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Fast-scan cyclic voltammetry has been used in a variety of applications and has been shown to be esp. useful to monitor chem. fluctuations of neurotransmitters such as dopamine within the mammalian brain. A major limitation of this procedure, however, is the large amplitude of the background current relative to the currents for the soln. species of interest. Furthermore, the background tends to drift, and this drift limits the use of digital background subtraction techniques to intervals less than 90 s before distortion of dopamine signals occurs. To minimize the impact of the background, a procedure termed analog background subtraction is reported here. The background is recorded, and its inverse is played back to the current transducer during data acquisition so that it cancels the background in subsequent scans. Background drift still occurs and is recorded, but its magnitude is small compared to the original background. This approach has two advantages. First it allows the use of higher gains in the current transducer, minimizing quantization noise. Second, because the background amplitude is greatly reduced, principal component regression could be used to sep. the contributions from drift, dopamine, and pH when appropriate calibrations were performed. We demonstrate the use of this approach with several applications. First, transient dopamine fluctuations were monitored for 15 min in a flowing injection app. Second, evoked release of dopamine was monitored for a similar period in the brain of an anesthetized rat. Third, dopamine was monitored in the brain of freely moving rats over a 30 min interval. By analyzing the fluctuations in each resolved component, we were able to show that cocaine causes significant fluctuations in dopamine concn. in the brain while those for the background and pH remain unchanged from their predrug value.
- 19Howell, J. O.; Kuhr, W. G.; Ensman, R. E.; Wightman, R. M. Background Subtraction for Rapid Scan Voltammetry. J. Electroanal. Chem. 1986, 209 (1), 77– 90, DOI: 10.1016/0022-0728(86)80187-5Google Scholar19https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaL28XlsVWqt7k%253D&md5=f21a3f305bfa89711aeaab3ce26d5eb1Background subtraction for rapid scan voltammetryHowell, Jonathon O.; Kuhr, Werner G.; Ensman, Robert E.; Wightman, R. MarkJournal of Electroanalytical Chemistry and Interfacial Electrochemistry (1986), 209 (1), 77-90CODEN: JEIEBC; ISSN:0022-0728.Methods for the elimination of residual current in fast scan (>300 V s-1) voltammetry were evaluated at microvoltammetric electrodes. Staircase voltammetry was found to give only a modest improvement in the ratio of the faradaic current to the residual current. Superior results are obtained when the residual current, obtained in supporting electrolyte soln., is digitally subtracted from the voltammogram obtained in the presence of the electroactive species. The subtraction process is facilitated by conducting the whole expt. in a flow injection app. so that the electrode remains in soln. while the 2 voltammograms are obtained. Undistorted voltammograms were obtained for the redn. of anthracene (∼2 mM) at scan rates up to 10,000 V s-1. At 300 V s-1, virtually undistorted voltammograms are obtained for the redn. of Tl+ at low concns. (20 μM) in aq. soln. at a Hg microvoltammetric electrode. Analog offset of the residual current was used to improve the dynamic range. The limits of this technique are caused by the electronic noise in the ideal case where flat residual current curves are obtained.
- 20Heien, M. L. A. V.; Khan, A. S.; Ariansen, J. L.; Cheer, J. F.; Phillips, P. E. M.; Wassum, K. M.; Wightman, R. M. Real-time measurement of dopamine fluctuations after cocaine in the brain of behaving rats. P Natl. Acad. Sci. USA 2005, 102 (29), 10023– 10028, DOI: 10.1073/pnas.0504657102Google Scholar20https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2MXmvVeltLc%253D&md5=2bdc42f6641711d1a5f1a282c7ee82b1Real-time measurement of dopamine fluctuations after cocaine in the brain of behaving ratsHeien, Michael L. A. V.; Khan, Amina S.; Ariansen, Jennifer L.; Cheer, Joseph F.; Phillips, Paul E. M.; Wassum, Kate M.; Wightman, R. MarkProceedings of the National Academy of Sciences of the United States of America (2005), 102 (29), 10023-10028CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)Dopamine neurotransmission has been implicated in the modulation of many cognitive processes. Both rapid (phasic) and slower (tonic) changes in its extracellular concn. contribute to its complex actions. Fast in vivo electrochem. techniques can measure extracellular dopamine on a rapid time scale but without the selectivity afforded with slower techniques that use chem. sepns. Cyclic voltammetry improves chem. resoln. over other electrochem. methods, and it can resolve dopamine changes in the brains of behaving rodents over short epochs (<10 s). With this method, however, selective detection of slower dopamine changes is still elusive. Here we demonstrate that principal component regression of cyclic voltammetry data enables quantification of changes in dopamine and extracellular pH. Using this method, we show that cocaine modifies dopamine release in two ways: dopamine concn. transients increase in frequency and magnitude, whereas a gradual increase in steady-state dopamine concn. occurs over 90 s.
- 21Taylor, I. M.; Robbins, E. M.; Catt, K. A.; Cody, P. A.; Happe, C. L.; Cui, X. T. Enhanced dopamine detection sensitivity by PEDOT/graphene oxide coating on in vivo carbon fiber electrodes. Journal of Biosensors and Bioelectronics 2017, 89, 400– 410, DOI: 10.1016/j.bios.2016.05.084Google ScholarThere is no corresponding record for this reference.
- 22Wipf, D. O.; Michael, A. C.; Wightman, R. M. Microdisk electrodes: Part II. Fast-scan cyclic voltammetry with very small electrodes. Journal of electroanalytical chemistry amd interfacial electrochemistry 1989, 269 (1), 15– 25, DOI: 10.1016/0022-0728(89)80100-7Google Scholar22https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaK3cXhtlagsw%253D%253D&md5=880cc453ba1ef38ff39f18d7cff21882Microdisk electrodes. Part II. Fast-scan cyclic voltammetry with very small electrodesWipf, David O.; Michael, Adrian C.; Wightman, R. MarkJournal of Electroanalytical Chemistry and Interfacial Electrochemistry (1989), 269 (1), 15-25CODEN: JEIEBC; ISSN:0022-0728.Cyclic voltammetry was investigated at inlaid disk electrodes with nominal radii of 0.3, 1.0, and 5.0 μm. The electrode capacitance was found to be much larger than expected for the 2 smaller radii electrodes. This effect was attributed to the capacitance between the inner conductor and the electrolyte soln. The excess capacitive current was minimized by the use of a conductive shield around the electrode which is connected to ground potential. Criteria were investigated for the degree of filtering of steady-state voltammograms to minimize noise while avoiding distortion of the exptl. data. Exptl. voltammograms for the oxidn. of ferrocene in MeCN solns. were found to be in good agreement with existing theories for scan rates in which linear and convergent diffusion occur. The factors which limit the use of very small electrodes are discussed in terms of signal-to-noise, ohmic drop, and linear diffusion.
- 23DeWaele, M.; Oh, Y.; Park, C.; Kang, Y. M.; Shin, H.; Blaha, C. D.; Bennet, K. E.; Kim, I. Y.; Lee, K. H.; Jang, D. P. A baseline drift detrending technique for fast scan cyclic voltammetry. Analyst 2017, 142 (22), 4317– 4321, DOI: 10.1039/C7AN01465AGoogle Scholar23https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhsFKitrvK&md5=7dcc3d64377be749b6fc50d01d1e7345A baseline drift detrending technique for fast scan cyclic voltammetryDeWaele, Mark; Oh, Yoonbae; Park, Cheonho; Kang, Yu Min; Shin, Hojin; Blaha, Charles D.; Bennet, Kevin E.; Kim, In Young; Lee, Kendall H.; Jang, Dong PyoAnalyst (Cambridge, United Kingdom) (2017), 142 (22), 4317-4321CODEN: ANALAO; ISSN:0003-2654. (Royal Society of Chemistry)Fast scan cyclic voltammetry (FSCV) has been commonly used to measure extracellular neurotransmitter concns. in the brain. Due to the unstable nature of the background currents inherent in FSCV measurements, anal. of FSCV data is limited to very short amts. of time using traditional background subtraction. In this paper, we propose the use of a zero-phase high pass filter (HPF) as the means to remove the background drift. Instead of the traditional method of low pass filtering across voltammograms to increase the signal to noise ratio, a HPF with a low cutoff frequency was applied to the temporal dataset at each voltage point to remove the background drift. As a result, the HPF utilizing cutoff frequencies between 0.001 Hz and 0.01 Hz could be effectively used to a set of FSCV data for removing the drifting patterns while preserving the temporal kinetics of the phasic dopamine response recorded in vivo. In addn., compared to a drift removal method using principal component anal., this was found to be significantly more effective in reducing the drift (unpaired t-test p < 0.0001, t = 10.88) when applied to data collected from Tris buffer over 24 h although a drift removal method using principal component anal. also showed the effective background drift redn. The HPF was also applied to 5 h of FSCV in vivo data. Elec. evoked dopamine peaks, obsd. in the nucleus accumbens, were clearly visible even without background subtraction. This technique provides a new, simple, and yet robust, approach to analyze FSCV data with an unstable background.
- 24Atcherley, C. W.; Wood, K. M.; Parent, K. L.; Hashemi, P.; Heien, M. L. The coaction of tonic and phasic dopamine dynamics. Chem. Commun. 2015, 51 (12), 2235– 2238, DOI: 10.1039/C4CC06165AGoogle Scholar24https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhs1WitrvF&md5=163d84a44219ae257bb3dcf9bed7d238The coaction of tonic and phasic dopamine dynamicsAtcherley, Christopher W.; Wood, Kevin M.; Parent, Kate L.; Hashemi, Parastoo; Heien, Michael L.Chemical Communications (Cambridge, United Kingdom) (2015), 51 (12), 2235-2238CODEN: CHCOFS; ISSN:1359-7345. (Royal Society of Chemistry)Tonic neurochem. dopamine activity underlies many brain functions; however a consensus on this important concn. has not yet been reached. In this work, we introduce in vivo fast-scan controlled-adsorption voltammetry to report tonic dopamine concns. (90 ± 9 nM) and the dopamine diffusion coeff. (1.05 ± 0.09 × 10-6 cm2 s-1) in the mouse brain.
- 25Oh, Y.; Heien, M. L.; Park, C.; Kang, Y. M.; Kim, J.; Boschen, S. L.; Shin, H.; Cho, H. U.; Blaha, C. D.; Bennet, K. E.; Lee, H. K.; Jung, S. J.; Kim, I. Y.; Lee, K. H.; Jang, D. P. Tracking tonic dopamine levels in vivo using multiple cyclic square wave voltammetry. Biosens Bioelectron 2018, 121, 174– 182, DOI: 10.1016/j.bios.2018.08.034Google Scholar25https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXhslSktbrF&md5=ff0dbf43f2bee824be6afe57aa5e84d3Tracking tonic dopamine levels in vivo using multiple cyclic square wave voltammetryOh, Yoonbae; Heien, Michael L.; Park, Cheonho; Kang, Yu Min; Kim, Jaekyung; Boschen, Suelen Lucio; Shin, Hojin; Cho, Hyun U.; Blaha, Charles D.; Bennet, Kevin E.; Lee, Han Kyu; Jung, Sung Jun; Kim, In Young; Lee, Kendall H.; Jang, Dong PyoBiosensors & Bioelectronics (2018), 121 (), 174-182CODEN: BBIOE4; ISSN:0956-5663. (Elsevier B.V.)For over two decades, fast-scan cyclic voltammetry (FSCV) has served as a reliable anal. method for monitoring dopamine release in near real-time in vivo. However, contemporary FSCV techniques have been limited to measure only rapid (on the order of seconds, i.e. phasic) changes in dopamine release evoked by either elec. stimulation or elicited by presentation of behaviorally salient stimuli, and not slower changes in the tonic extracellular levels of dopamine (i.e. basal concns.). This is because FSCV is inherently a differential method that requires subtraction of prestimulation tonic levels of dopamine to measure phasic changes relative to a zeroed baseline. Here, we describe the development and application of a novel voltammetric technique, multiple cyclic square wave voltammetry (M-CSWV), for anal. quantification of tonic dopamine concns. in vivo with relatively high temporal resoln. (10 s). M-CSWV enriches the electrochem. information by generating two dimensional voltammograms which enable high sensitivity (limit of detection, 0.17 nM) and selectivity against ascorbic acid, and 3,4-dihydroxyphenylacetic acid (DOPAC), including changes in pH. Using M-CSWV, a tonic dopamine concn. of 120 ± 18 nM (n = 7 rats, ± SEM) was detd. in the striatum of urethane anethetized rats. Pharmacol. treatments to elevate dopamine by selectively inhibiting dopamine reuptake and to reduce DOPAC by inhibition of monoamine oxidase supported the selective detection of dopamine in vivo. Overall, M-CSWV offers a novel voltammetric technique to quantify levels and monitor changes in tonic dopamine concns. in the brain to further our understanding of the role of dopamine in normal behavior and neuropsychiatric disorders.
- 26Oh, Y.; Park, C.; Kim, D. H.; Shin, H.; Kang, Y. M.; DeWaele, M.; Lee, J.; Min, H.-K.; Blaha, C. D.; Bennet, K. E. Monitoring in vivo changes in tonic extracellular dopamine level by charge-balancing multiple waveform fast-scan cyclic voltammetry. Anal. Chem. 2016, 88 (22), 10962– 10970, DOI: 10.1021/acs.analchem.6b02605Google Scholar26https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhslCgsrnL&md5=307c84d9a85be6e45b5ad56ea13f4cdcMonitoring In Vivo Changes in Tonic Extracellular Dopamine Level by Charge-Balancing Multiple Waveform Fast-Scan Cyclic VoltammetryOh, Yoonbae; Park, Cheonho; Kim, Do Hyoung; Shin, Hojin; Kang, Yu Min; DeWaele, Mark; Lee, Jeyeon; Min, Hoon-Ki; Blaha, Charles D.; Bennet, Kevin E.; Kim, In Young; Lee, Kendall H.; Jang, Dong PyoAnalytical Chemistry (Washington, DC, United States) (2016), 88 (22), 10962-10970CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Dopamine (DA) modulates central neuronal activity through both phasic (second to second) and tonic (minutes to hours) terminal release. Conventional fast-scan cyclic voltammetry (FSCV), in combination with carbon fiber microelectrodes, has been used to measure phasic DA release in vivo by adopting a background subtraction procedure to remove background capacitive currents. However, measuring tonic changes in DA concns. using conventional FSCV has been difficult because background capacitive currents are inherently unstable over long recording periods. To measure tonic changes in DA concns. over several hours, we applied a novel charge-balancing multiple waveform FSCV (CBM-FSCV), combined with a dual background subtraction technique, to minimize temporal variations in background capacitive currents. Using this method, in vitro, charge variations from a ref. time point were nearly zero for 48 h, whereas with conventional background subtraction, charge variations progressively increased. CBM-FSCV also demonstrated a high selectivity against 3,4-dihydroxyphenylacetic acid and ascorbic acid, two major chem. interferents in the brain, yielding a sensitivity of 85.40 ± 14.30 nA/μM and limit of detection of 5.8 ± 0.9 nM for DA while maintaining selectivity. Recorded in vivo by CBM-FSCV, pharmacol. inhibition of DA reuptake (nomifensine) resulted in a 235 ± 60 nM increase in tonic extracellular DA concns., while inhibition of DA synthesis (α-methyl-DL-tyrosine) resulted in a 72.5 ± 4.8 nM decrease in DA concns. over a 2 h period. This study showed that CBM-FSCV may serve as a unique voltammetric technique to monitor relatively slow changes in tonic extracellular DA concns. in vivo over a prolonged time period.
- 27Taylor, I. M.; Patel, N. A.; Freedman, N. C.; Castagnola, E.; Cui, X. T. Direct in vivo electrochemical detection of resting dopamine using Poly (3, 4-ethylenedioxythiophene)/Carbon Nanotube functionalized microelectrodes. Anal. Chem. 2019, 91 (20), 12917– 12927, DOI: 10.1021/acs.analchem.9b02904Google Scholar27https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhslKitrjN&md5=3073af9f96d0141f3e5d658437b2dcebDirect in Vivo Electrochemical Detection of Resting Dopamine Using Poly(3,4-ethylenedioxythiophene)/Carbon Nanotube Functionalized MicroelectrodesTaylor, Ian Mitchell; Patel, Nikita Anurag; Freedman, Noah Chaim; Castagnola, Elisa; Cui, Xinyan TracyAnalytical Chemistry (Washington, DC, United States) (2019), 91 (20), 12917-12927CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Dopamine (DA) is a monoamine neurotransmitter responsible for the maintenance of a variety of vital life functions. In vivo DA signaling occurs over multiple time scales, from sub-second phasic release due to dopamine neuron firing, to tonic release responsible for long-term DA concn. changes over minutes to hours. Due to the complex, multifaceted nature of DA signaling, anal. sensing technol. must be capable of recording DA from multiple locations and over multiple timescales. Decades of research has focused on improving in vivo detection capabilities for sub-second phasic DA, but the accurate detection of abs. resting DA levels in real time has proven challenging. The authors have developed a poly(3,4 ethylene dioxythiophene) (PEDOT)-based nanocomposite coating that exhibits excellent DA sensing capabilities for resting DA. PEDOT/functionalized carbon nanotube (PEDOT/CNT) coated carbon fiber microelectrodes (CFEs) are capable of directly measuring resting DA using square wave voltammetry (SWV) with high sensitivity and selectivity. Incorporation of a PEDOT/CNT coating significantly increases the sensitivity for the detection of resting DA by a factor of 422. SWV measurements performed at PEDOT/CNT functionalized CFEs implanted in the rat dorsal striatum reveal the abs. basal DA concn. to be 82±6 nM. Systemic administration of the dopamine transporter inhibitor, nomifensine increases resting DA to a max. 207±16 nM at 28±2 min following injection. PEDOT/CNT was also functionalized onto individual gold electrode sites along silicon microelectrode arrays (MEAs) to produce a multisite DA sensing electrode. MEA implantation allows for the quantification of basal DA from different brain regions with excellent spatial resoln. SWV detection paired with PEDOT/CNT functionalized is highly adaptable and shows great promise for tonic DA detection with high spatial and temporal resoln.
- 28Johnson, J. A.; Hobbs, C. N.; Wightman, R. M. Removal of Differential Capacitive Interferences in Fast-Scan Cyclic Voltammetry. Anal. Chem. 2017, 89 (11), 6166– 6174, DOI: 10.1021/acs.analchem.7b01005Google Scholar28https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXntlWitbo%253D&md5=83bcb6cfdccfff671ae4f7be8b3afd4aRemoval of Differential Capacitive Interferences in Fast-Scan Cyclic VoltammetryJohnson, Justin A.; Hobbs, Caddy N.; Wightman, R. MarkAnalytical Chemistry (Washington, DC, United States) (2017), 89 (11), 6166-6174CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Due to its high spatiotemporal resoln., fast-scan cyclic voltammetry (FSCV) at carbon-fiber microelectrodes enables the localized in vivo monitoring of subsecond fluctuations in electroactive neurotransmitter concns. In practice, resoln. of the anal. signal relies on digital background subtraction for removal of the large current due to charging of the elec. double layer as well as surface faradaic reactions. However, fluctuations in this background current often occur with changes in the electrode state or ionic environment, leading to nonspecific contributions to the FSCV data that confound data anal. Here, the authors both explore the origin of such shifts seen with local changes in cations and develop a model to account for their shape. Further, the authors describe a convolution-based method for removal of the differential capacitive contributions to the FSCV current. The method relies on the use of a small-amplitude pulse made prior to the FSCV sweep that probes the impedance of the system. To predict the nonfaradaic current response to the voltammetric sweep, the step current response is differentiated to provide an est. of the system's impulse response function and is used to convolute the applied waveform. The generated prediction is then subtracted from the obsd. current to the voltammetric sweep, removing artifacts assocd. with electrode impedance changes. The technique is demonstrated to remove select contributions from capacitive characteristics changes of the electrode both in vitro (i.e., in flow-injection anal.) and in vivo (i.e., during a spreading depression event in an anesthetized rat).
- 29Meunier, C. J.; McCarty, G. S.; Sombers, L. A. Drift Subtraction for Fast-Scan Cyclic Voltammetry Using Double-Waveform Partial-Least-Squares Regression. Anal. Chem. 2019, 91 (11), 7319– 7327, DOI: 10.1021/acs.analchem.9b01083Google Scholar29https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXptlKqu7g%253D&md5=c0794bcf0db185cbb20829f2d777b307Drift Subtraction for Fast-Scan Cyclic Voltammetry Using Double-Waveform Partial-Least-Squares RegressionMeunier, Carl J.; McCarty, Gregory S.; Sombers, Leslie A.Analytical Chemistry (Washington, DC, United States) (2019), 91 (11), 7319-7327CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Background-subtracted fast-scan cyclic voltammetry (FSCV) provides a method for detecting mol. fluctuations with high spatiotemporal resoln. in the brain of awake and behaving animals. The rapid scan rates generate large background currents that are subtracted to reveal changes in analyte concn. Although these background currents are relatively stable, small changes do occur over time. These changes, referred to as electrochem. drift, result in background-subtraction artifacts that constrain the utility of FSCV, particularly when quantifying chem. changes that gradually occur over long measurement times (minutes). The voltammetric features of electrochem. drift are varied and can span the entire potential window, potentially obscuring the signal from any targeted analyte. The authors present a straightforward method for extending the duration of a single FSCV recording window. First, the authors have implemented voltammetric waveforms in pairs that consist of a smaller triangular sweep followed by a conventional voltammetric scan. The initial, abbreviated waveform is used to capture drift information that can serve as a predictor for the contribution of electrochem. drift to the subsequent full voltammetric scan using partial-least-squares regression (PLSR). This double-waveform partial-least-squares regression (DW-PLSR) paradigm permits reliable subtraction of the drift component to the voltammetric data. Here, DW-PLSR is used to improve quantification of adenosine, dopamine, and hydrogen peroxide fluctuations occurring >10 min from the initial background position, both in vitro and in vivo. The results demonstrate that DW-PLSR is a powerful tool for evaluating and interpreting both rapid (seconds) and gradual (minutes) chem. changes captured in FSCV recordings over extended durations.
- 30Espin, L. X.; Asp, A. J.; Trevathan, J. K.; Ludwig, K. A.; Lujan, J. L. Integral methods for automatic quantification of fast-scan-cyclic-voltammetry detected neurotransmitters. PLoS One 2021, 16 (7), e0254594, DOI: 10.1371/journal.pone.0254594Google Scholar30https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhs1ymt7jM&md5=7293f3e74aa31acd110a07a982944fa8Integral methods for automatic quantification of fast-scan-cyclic-voltammetry detected neurotransmittersEspin, Leonardo X.; Asp, Anders J.; Trevathan, James K.; Ludwig, Kip A.; Lujan, J. LuisPLoS One (2021), 16 (7), e0254594CODEN: POLNCL; ISSN:1932-6203. (Public Library of Science)Modern techniques for estg. basal levels of electroactive neurotransmitters rely on the measurement of oxidative charges. This requires time integration of oxidn. currents at certain intervals. Unfortunately, the selection of integration intervals relies on ad-hoc visual identification of peaks on the oxidn. currents, which introduces sources of error and precludes the development of automated procedures necessary for anal. and quantification of neurotransmitter levels in large data sets. In an effort to improve charge quantification techniques, here we present novel methods for automatic selection of integration boundaries. Our results show that these methods allow quantification of oxidn. reactions both in vitro and in vivo and of multiple analytes in vitro.
- 31Bucher, E. S.; Brooks, K.; Verber, M. D.; Keithley, R. B.; Owesson-White, C.; Carroll, S.; Takmakov, P.; McKinney, C. J.; Wightman, R. M. Flexible Software Platform for Fast-Scan Cyclic Voltammetry Data Acquisition and Analysis. Anal. Chem. 2013, 85 (21), 10344– 10353, DOI: 10.1021/ac402263xGoogle Scholar31https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXhsFGku77M&md5=116501c82a8e13a2c012f2b1b1ae48e9Flexible Software Platform for Fast-Scan Cyclic Voltammetry Data Acquisition and AnalysisBucher, Elizabeth S.; Brooks, Kenneth; Verber, Matthew D.; Keithley, Richard B.; Owesson-White, Catarina; Carroll, Susan; Takmakov, Pavel; McKinney, Collin J.; Wightman, R. MarkAnalytical Chemistry (Washington, DC, United States) (2013), 85 (21), 10344-10353CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Over the last several decades, fast-scan cyclic voltammetry (FSCV) has proved to be a valuable anal. tool for the real-time measurement of neurotransmitter dynamics in vitro and in vivo. Indeed, FSCV has found application in a wide variety of disciplines including electrochem., neurobiol., and behavioral psychol. The maturation of FSCV as an in vivo technique led users to pose increasingly complex questions that require a more sophisticated exptl. design. To accommodate recent and future advances in FSCV application, the authors' lab has developed High Definition Cyclic Voltammetry (HDCV). HDCV is an electrochem. software suite that includes data acquisition and anal. programs. The data collection program delivers greater exptl. flexibility and better user feedback through live displays. It supports expts. involving multiple electrodes with customized waveforms. It is compatible with transistor-transistor logic-based systems that are used for monitoring animal behavior, and it enables simultaneous recording of electrochem. and electrophysiol. data. HDCV anal. streamlines data processing with superior filtering options, seamlessly manages behavioral events, and integrates chemometric processing. Furthermore, anal. is capable of handling single files collected over extended periods of time, allowing the user to consider biol. events on both sub-second and multi-minute time scales. Here the authors describe and demonstrate the utility of HDCV for in vivo expts.
- 32Bath, B. D.; Michael, D. J.; Trafton, B. J.; Joseph, J. D.; Runnels, P. L.; Wightman, R. M. Subsecond adsorption and desorption of dopamine at carbon-fiber microelectrodes. Anal. Chem. 2000, 72 (24), 5994– 6002, DOI: 10.1021/ac000849yGoogle Scholar32https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3cXotVyis7s%253D&md5=6e2c2e1202ae88e8ec4bfbcd274dc976Subsecond adsorption and desorption of dopamine at carbon-fiber microelectrodesBath, Bradley D.; Michael, Darren J.; Trafton, B. Jill; Joseph, Joshua D.; Runnels, Petrise L.; Wightman, R. MarkAnalytical Chemistry (2000), 72 (24), 5994-6002CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)High-repetition fast-scan cyclic voltammetry and chronoamperometry were used to quantify and characterize the kinetics of dopamine and dopamine-o-quinone adsorption and desorption at carbon-fiber microelectrodes. A flow injection anal. system was used for the precise introduction and removal of a bolus of electroactive substance on a sub-second time scale to the disk-shaped surface of a microelectrode that was fabricated from a single carbon fiber (Thornel type T650 or P55). Pretreatment of the electrode surfaces consisted of soaking them in purified iso-Pr alc. for a min. of 10 min, which resulted in S/N increasing by 200-400% for dopamine above that for those that were soaked in reagent grade solvent. Because of adsorption, high scan rates (2000 V/s) are shown to exhibit equiv. S/N ratios as compared to slower, more traditional scan rates. In addn., the steady-state response to a concn. bolus is shown to occur more rapidly when cyclic voltammetric scans are repeated at short intervals (4 ms). The new methodologies allow for more accurate detns. of the kinetics of neurotransmitter release events (10-500 ms) in biol. systems. Brain slice and in vivo expts. using T650 cylinder microelectrodes show that voltammetrically measured uptake kinetics in the caudate are faster using 2000 V/s and 240 Hz measurements, as compared to 300 V/s and 10 Hz.
- 33Mirza, K. B.; Golden, C. T.; Nikolic, K.; Toumazou, C. Closed-Loop Implantable Therapeutic Neuromodulation Systems Based on Neurochemical Monitoring. Front. Neurosci. 2019, 13, na, DOI: 10.3389/fnins.2019.00808Google ScholarThere is no corresponding record for this reference.
- 34Kim, S.; Kang, S.; Kim, J.; Lee, D.; Kim, S.; Lee, J.; Jang, K.-I.; Oh, Y.-S.; Rah, J.-C.; Huh, M. S. Closed-Loop Neuromodulation for Parkinson’s Disease: Current State and Future Directions. IEEE Transactions on Molecular, Biological Multi-Scale Communications 2021, 7 (4), 209– 223, DOI: 10.1109/TMBMC.2020.3036756Google ScholarThere is no corresponding record for this reference.
- 35Lee, K. H.; Lujan, J. L.; Trevathan, J. K.; Ross, E. K.; Bartoletta, J. J.; Park, H. O.; Paek, S. B.; Nicolai, E. N.; Lee, J. H.; Min, H. K.; Kimble, C. J.; Blaha, C. D.; Bennet, K. E. WINCS Harmoni: Closed-loop dynamic neurochemical control of therapeutic interventions. Sci. Rep. 2017, 7, 46675, DOI: 10.1038/srep46675Google Scholar35https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BC1critV2qtQ%253D%253D&md5=8b49acf534584b18641057c54f19bc5eWINCS Harmoni: Closed-loop dynamic neurochemical control of therapeutic interventionsLee Kendall H; Lujan J Luis; Ross Erika K; Bartoletta John J; Park Hyung Ook; Nicolai Evan N; Lee Jannifer H; Min Hoon-Ki; Blaha Charles D; Bennet Kevin E; Lee Kendall H; Lujan J Luis; Min Hoon-Ki; Lee Kendall H; Trevathan James K; Paek Seungleal Brian; Kimble Christopher J; Bennet Kevin EScientific reports (2017), 7 (), 46675 ISSN:.There has been significant progress in understanding the role of neurotransmitters in normal and pathologic brain function. However, preclinical trials aimed at improving therapeutic interventions do not take advantage of real-time in vivo neurochemical changes in dynamic brain processes such as disease progression and response to pharmacologic, cognitive, behavioral, and neuromodulation therapies. This is due in part to a lack of flexible research tools that allow in vivo measurement of the dynamic changes in brain chemistry. Here, we present a research platform, WINCS Harmoni, which can measure in vivo neurochemical activity simultaneously across multiple anatomical targets to study normal and pathologic brain function. In addition, WINCS Harmoni can provide real-time neurochemical feedback for closed-loop control of neurochemical levels via its synchronized stimulation and neurochemical sensing capabilities. We demonstrate these and other key features of this platform in non-human primate, swine, and rodent models of deep brain stimulation (DBS). Ultimately, systems like the one described here will improve our understanding of the dynamics of brain physiology in the context of neurologic disease and therapeutic interventions, which may lead to the development of precision medicine and personalized therapies for optimal therapeutic efficacy.
- 36Kang, S.; Park, J.; Jeong, Y.; Oh, Y.-S; Choi, J.-W. takang0902/Open_SDBR, Zenodo 2022, na, DOI: 10.5281/zenodo.6597381Google ScholarThere is no corresponding record for this reference.
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- Jeongrak Park, Seongtak Kang, Yaebin Lee, Ji-Woong Choi, Yong-Seok Oh. Continuous long-range measurement of tonic dopamine with advanced FSCV for pharmacodynamic analysis of levodopa-induced dyskinesia in Parkinson’s disease. Frontiers in Bioengineering and Biotechnology 2024, 12 https://doi.org/10.3389/fbioe.2024.1335474
- Han Hee Jung, Jeongdae Ha, Jeongrak Park, Seongtak Kang, Jinmo Kim, Han Na Jung, Samhwan Kim, Junwoo Yea, Hyeokjun Lee, Saehyuck Oh, Janghwan Jekal, Soojeong Song, Jieun Son, Tae Sang Yu, Youngjeon Lee, Jinyoung Won, Kyung Seob Lim, Yoon Kyeung Lee, Hohyun Keum, Taeyoon Lee, Young Min Song, Jae‐Woong Jeong, Jong‐Cheol Rah, Ji‐Woong Choi, Sheng Xu, Yong‐Seok Oh, Kyung‐In Jang. Highly Deformable Double‐Sided Neural Probe with All‐in‐One Electrode System for Real‐Time In Vivo Detection of Dopamine for Parkinson's Disease. Advanced Functional Materials 2024, 34
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https://doi.org/10.1002/adfm.202311436
- Seongtak Kang, Yunho Jeong, Ji-Woong Choi. Simultaneous Estimation of Tonic Dopamine and Serotonin with High Temporal Resolution In Vitro Using Deep Learning. 2023, 1-4. https://doi.org/10.1109/EMBC40787.2023.10341045
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Abstract
Figure 1
Figure 1. In vitro test of SDBR to record the tonic and phasic dopamine with standard FSCV. (A) Raw FSCV color plot in vitro test. The black dotted line denotes the timing of the 200 nM dopamine drop. Each circled number and the corresponding colored-line are the voltammogram at a specific time, detailed in (E)–(H). (B) Background-subtracted color plot and current change of dopamine peak over time. (C) SDBR applied color plot and current change of dopamine peak over time. (D) A calibration plot obtained by SDBR (R2 = 0.996), slope = 0.0319 ± 0.0003 pA/V2 nM–1, limit of detection = 8.16 ± 0.08 nM (n = 5 electrodes). (E, F) Comparison of background subtraction and SDBR for three voltammograms measuring the same concentration at 2 min intervals. (G, H) Three voltammograms were measured 10 min after each drop of dopamine solution for comparison of background subtraction and SDBR. (E, G) Left: the background-subtracted voltammogram, right: the enlarged voltammogram of the red dotted box in the left image. (F, H) Left: the result of applying SDBR to the raw voltammogram, right: the enlarged SDBR result of the blue dotted box in the left image.
Figure 2
Figure 2. Measurement of tonic dopamine level change using SDBR during in vivo pharmacological stimulation. (A) SDBR results were measured in the striatum of healthy mice (n = 3) following saline intraperitoneal (IP) injection. (B) SDBR measured in the striatum of PD model mice (n = 3) following levodopa (10 mg kg–1) IP injection. (C) SDBR measured in the striatum of healthy mice (n = 3) following reserpine (5 mg kg–1) IP injection. Bold blue line represents mean concentrations over time, and the light blue line around the bold line represents the standard error of the mean (SEM). The upper black bar indicates significant differences compared to saline injection (2-way ANOVA, p < 0.0001, Dunnett’s multiple comparison test). Data from Figures 1 and 2 are freely available online. (36)
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- 2Trezza, V.; Baarendse, P. J.; Vanderschuren, L. J. The pleasures of play: pharmacological insights into social reward mechanisms. Trends in pharmacological sciences 2010, 31 (10), 463– 469, DOI: 10.1016/j.tips.2010.06.0082https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3cXht1Wisr7E&md5=4ece9534b253b2a49bdf9cce4d5ca397The pleasures of play: pharmacological insights into social reward mechanismsTrezza, Viviana; Baarendse, Petra J. J.; Vanderschuren, Louk J. M. J.Trends in Pharmacological Sciences (2010), 31 (10), 463-469CODEN: TPHSDY; ISSN:0165-6147. (Elsevier B.V.)A review. Like human children, most young mammals devote a significant amt. of time and energy playing together, and social play is fun. Although social play is very pleasurable, it is more than just a frivolous activity: it is crucial for the development of behavioral flexibility, the acquisition of social and cognitive competence, and the maintenance of group cohesion. Social play is a natural reinforcer, and the neurotransmitter systems intimately implicated in the motivational, pleasurable and cognitive aspects of natural and drug rewards, such as opioids, endocannabinoids, dopamine and norepinephrine, play an important modulatory role in the performance of social play. In this review, we address the notion that social play is rewarding, and discuss recent developments in the neuropharmacol. of this behavior. This provides a framework to understand how the brain processes social emotions, to make young individuals enjoy social play.
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- 4Liu, C. L.; Goel, P.; Kaeser, P. S. Spatial and temporal scales of dopamine transmission. Nat. Rev. Neurosci 2021, 22 (6), 345– 358, DOI: 10.1038/s41583-021-00455-74https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXosVGjt78%253D&md5=c3807addc68b3a7e872b958e3b9ff1bdSpatial and temporal scales of dopamine transmissionLiu, Changliang; Goel, Pragya; Kaeser, Pascal S.Nature Reviews Neuroscience (2021), 22 (6), 345-358CODEN: NRNAAN; ISSN:1471-003X. (Nature Portfolio)A review. Abstr.: Dopamine is a prototypical neuromodulator that controls circuit function through G protein-coupled receptor signaling. Neuromodulators are vol. transmitters, with release followed by diffusion for widespread receptor activation on many target cells. Yet, we are only beginning to understand the specific organization of dopamine transmission in space and time. Although some roles of dopamine are mediated by slow and diffuse signaling, recent studies suggest that certain dopamine functions necessitate spatiotemporal precision. Here, we review the literature describing dopamine signaling in the striatum, including its release mechanisms and receptor organization. We then propose the domain-overlap model, in which release and receptors are arranged relative to one another in micrometre-scale structures. This architecture is different from both point-to-point synaptic transmission and the widespread organization that is often proposed for neuromodulation. It enables the activation of receptor subsets that are within micrometre-scale domains of release sites during baseline activity and broader receptor activation with domain overlap when firing is synchronized across dopamine neuron populations. This signaling structure, together with the properties of dopamine release, may explain how switches in firing modes support broad and dynamic roles for dopamine and may lead to distinct pathway modulation.
- 5Maia, T. V.; Conceicao, V. A. Dopaminergic Disturbances in Tourette Syndrome: An Integrative Account. Biol. Psychiat 2018, 84 (5), 332– 344, DOI: 10.1016/j.biopsych.2018.02.11725https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXnsFClurw%253D&md5=08179094c634142eb599de2938aacba6Dopaminergic Disturbances in Tourette Syndrome: An Integrative AccountMaia, Tiago V.; Conceicao, Vasco A.Biological Psychiatry (2018), 84 (5), 332-344CODEN: BIPCBF; ISSN:0006-3223. (Elsevier)Tourette syndrome (TS) is thought to involve dopaminergic disturbances, but the nature of those disturbances remains controversial. Existing hypotheses suggest that TS involves 1) supersensitive dopamine receptors, 2) overactive dopamine transporters that cause low tonic but high phasic dopamine, 3) presynaptic dysfunction in dopamine neurons, or 4) dopaminergic hyperinnervation. We review evidence that contradicts the first two hypotheses; we also note that the last two hypotheses have traditionally been considered too narrowly, explaining only small subsets of findings. We review all studies that have used positron emission tomog. and single-photon emission computerized tomog. to investigate the dopaminergic system in TS. The seemingly diverse findings from those studies have typically been interpreted as pointing to distinct mechanisms, as evidenced by the various hypotheses concerning the nature of dopaminergic disturbances in TS. We show, however, that the hyperinnervation hypothesis provides a simple, parsimonious explanation for all such seemingly diverse findings. Dopaminergic hyperinnervation likely causes increased tonic and phasic dopamine. We have previously shown, using a computational model of the role of dopamine in basal ganglia, that increased tonic dopamine and increased phasic dopamine likely increase the propensities to express and learn tics, resp. There is therefore a plausible mechanistic link between dopaminergic hyperinnervation and TS via increased tonic and phasic dopamine. To further bolster this argument, we review evidence showing that all medications that are effective for TS reduce signaling by tonic dopamine, phasic dopamine, or both.
- 6Charvin, D.; Medori, R.; Hauser, R. A.; Rascol, O. Therapeutic strategies for Parkinson disease: beyond dopaminergic drugs (vol 17, pg 844, 2018). Nat. Rev. Drug Discov 2018, 17 (11), 844– 844, DOI: 10.1038/nrd.2018.1846https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXhvV2gtr7E&md5=fafdb271fed4e7ec853d5ae58fe0d199Therapeutic strategies for Parkinson disease: beyond dopaminergic drugsCharvin, Delphine; Medori, Rossella; Hauser, Robert A.; Rascol, OlivierNature Reviews Drug Discovery (2018), 17 (11), 844CODEN: NRDDAG; ISSN:1474-1776. (Nature Research)There is no expanded citation for this reference.
- 7Mohebi, A.; Pettibone, J. R.; Hamid, A. A.; Wong, J.-M. T.; Vinson, L. T.; Patriarchi, T.; Tian, L.; Kennedy, R. T.; Berke, J. D. Dissociable dopamine dynamics for learning and motivation. Nature 2019, 570 (7759), 65– 70, DOI: 10.1038/s41586-019-1235-y7https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhtVajsrjL&md5=e9ff25e5e8e976de181b597e0d516b23Dissociable dopamine dynamics for learning and motivationMohebi, Ali; Pettibone, Jeffrey R.; Hamid, Arif A.; Wong, Jenny-Marie T.; Vinson, Leah T.; Patriarchi, Tommaso; Tian, Lin; Kennedy, Robert T.; Berke, Joshua D.Nature (London, United Kingdom) (2019), 570 (7759), 65-70CODEN: NATUAS; ISSN:0028-0836. (Nature Research)The dopamine projection from ventral tegmental area (VTA) to nucleus accumbens (NAc) is crit. for motivation to work for rewards and reward-driven learning. How dopamine supports both functions is unclear. Dopamine cell spiking can encode prediction errors, which are vital learning signals in computational theories of adaptive behavior. By contrast, dopamine release ramps up as animals approach rewards, mirroring reward expectation. This mismatch might reflect differences in behavioral tasks, slower changes in dopamine cell spiking or spike-independent modulation of dopamine release. Here we compare spiking of identified VTA dopamine cells with NAc dopamine release in the same decision-making task. Cues that indicate an upcoming reward increased both spiking and release. However, NAc core dopamine release also covaried with dynamically evolving reward expectations, without corresponding changes in VTA dopamine cell spiking. Our results suggest a fundamental difference in how dopamine release is regulated to achieve distinct functions: broadcast burst signals promote learning, whereas local control drives motivation.
- 8Venton, B. J.; Zhang, H.; Garris, P. A.; Phillips, P. E.; Sulzer, D.; Wightman, R. M. Real-time decoding of dopamine concentration changes in the caudate-putamen during tonic and phasic firing. Journal of neurochemistry 2003, 87 (5), 1284– 1295, DOI: 10.1046/j.1471-4159.2003.02109.x8https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3sXps1OhsLc%253D&md5=d0e07194d3b5a12b7908407da54c3d89Real-time decoding of dopamine concentration changes in the caudate-putamen during tonic and phasic firingVenton, B. Jill; Zhang, Hui; Garris, Paul A.; Phillips, Paul E. M.; Sulzer, David; Wightman, R. MarkJournal of Neurochemistry (2003), 87 (5), 1284-1295CODEN: JONRA9; ISSN:0022-3042. (Blackwell Publishing Ltd.)The fundamental process that underlies vol. transmission in the brain is the extracellular diffusion of neurotransmitters from release sites to distal target cells. Dopaminergic neurons display a range of activity states, from low-frequency tonic firing to bursts of high-frequency action potentials (phasic firing). However, it is not clear how this activity affects vol. transmission on a subsecond time scale. To evaluate this, we developed a finite-difference model that predicts the lifetime and diffusion of dopamine in brain tissue. We first used this model to decode in vivo amperometric measurements of elec. evoked dopamine, and obtained rate consts. for release and uptake as well as the extent of diffusion. Accurate predictions were made under a variety of conditions including different regions, different stimulation parameters and with uptake inhibited. Second, we used the decoded rate consts. to predict how heterogeneity of dopamine release and uptake sites would affect dopamine concn. fluctuations during different activity states in the absence of an electrode. These simulations show that synchronous phasic firing can produce spatially and temporally heterogeneous concn. profiles whereas asynchronous tonic firing elicits uniform, steady-state dopamine concns.
- 9Dreyer, J. K.; Herrik, K. F.; Berg, R. W.; Hounsgaard, J. D. Influence of phasic and tonic dopamine release on receptor activation. Journal of neuroscience methods 2010, 30 (42), 14273– 14283, DOI: 10.1523/JNEUROSCI.1894-10.2010There is no corresponding record for this reference.
- 10Dunlop, B. W.; Nemeroff, C. B. The role of dopamine in the pathophysiology of depression. Archives of general psychiatry 2007, 64 (3), 327– 337, DOI: 10.1001/archpsyc.64.3.32710https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXjs1yntLY%253D&md5=5d9c7f04093533d67b4bff1f6f68f3aeThe role of dopamine in the pathophysiology of depressionDunlop, Boadie W.; Nemeroff, Charles B.Archives of General Psychiatry (2007), 64 (3), 327-337CODEN: ARGPAQ; ISSN:0003-990X. (American Medical Association)A review. Multiple sources of evidence support a role for diminished dopaminergic neurotransmission in major depression. The physiol. alterations underlying reduced dopamine (DA) signaling could result from either diminished DA release from presynaptic neurons or impaired signal transduction; either due to changes in receptor no. or function and/or altered intracellular signal processing. There are data supporting each of these mechanisms, although interpretation of previous research is confounded by issues around study population, medication status, and technol. limitations. In some patients with depression, DA-related disturbances improve by treatment with antidepressants, presumably by acting on serotonergic or noradrenergic circuits, which then affect DA function. However, most antidepressant treatments do not directly enhance DA neurotransmission, which may contribute to residual symptoms, including impaired motivation, concn., and pleasure. Animal models of major depression show considerable responsiveness to manipulations of DA neurotransmission. Several studies, including postmortem investigations, particularly of subjects with severe depression, have demonstrated reduced concns. of DA metabolites both in the cerebrospinal fluid and in brain regions that mediate mood and motivation. Although the neuroimaging findings are not unequivocal, several studies support the hypothesis that major depression is assocd. with a state of reduced DA transmission, possibly reflected by a compensatory up-regulation of D2 receptors. These alternations in DA signaling may underlie the findings of increased "liking" or "high" feelings reported by severely depressed subjects treated with d-amphetamine compared with the response of less severely ill and normal control subjects. The efficacy of medications that directly act on DA neurons or receptors, such as monoamine oxidase inhibitors and pramipexole, suggests that subtypes of depression stemming from a primary DA dysfunction exist. Further research on the contribution of DA to the pathophysiol. of depression is justified to improve outcomes for patients with treatment-resistant and nonremitting depression.
- 11Meisenzahl, E.; Schmitt, G.; Scheuerecker, J.; Möller, H.-J. The role of dopamine for the pathophysiology of schizophrenia. International Review of Psychiatry 2007, 19 (4), 337– 345, DOI: 10.1080/0954026070150246811https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BD2svltlGnsw%253D%253D&md5=d9a6e1f24b2b31e7f9dc57b4382dc71cThe role of dopamine for the pathophysiology of schizophreniaMeisenzahl E M; Schmitt G J; Scheuerecker J; Moller H-JInternational review of psychiatry (Abingdon, England) (2007), 19 (4), 337-45 ISSN:0954-0261.Since decades, experimental approaches and clinical experience have suggested a dopaminergic system's dysregulation playing an important role within the pathophysiology of schizophrenia. This paper summarizes the actual standard of knowledge of the physiological fundamentals and hypothesized dysbalances of the dopamine (DA) system with respect to schizophrenia including interaction with other neurotransmitter systems (glutamate, GABA). The assumed functional role of DA with respect to physiological and illness-associated cognitive performance, especially working memory, reward, and motivation, as it was assessed by fMRI studies, is presented. A third focus concentrates on giving a short survey of SPECT and PET studies measuring the amount of the striatal and extrastriatal DA, the striatal and extrastriatal dopamine D2 receptor, and the dopamine transporter (DAT) comparing first-episode, drug-naive, treated, and relapsing schizophrenic patients and healthy control persons.
- 12Wipf, D. O.; Kristensen, E. W.; Deakin, M. R.; Wightman, R. M. Fast-scan cyclic voltammetry as a method to measure rapid heterogeneous electron-transfer kinetics. Anal. Chem. 1988, 60 (4), 306– 310, DOI: 10.1021/ac00155a00612https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaL1cXmsVCktQ%253D%253D&md5=718c905317214cad42471414482e3f86Fast-scan cyclic voltammetry as a method to measure rapid heterogeneous electron-transfer kineticsWipf, David O.; Kristensen, Eric W.; Deakin, Mark R.; Wightman, R. MarkAnalytical Chemistry (1988), 60 (4), 306-10CODEN: ANCHAM; ISSN:0003-2700.The use of fast-scan cyclic voltammetry for the measurement of heterogeneous electron-transfer kinetics was examd. The distortions caused by the measurement instrumentation, ohmic drop, and the cell time const. were considered. These parameters combine to set an upper limit on the scan rate at which undistorted data can be achieved. At higher scan rates, meaningful data can be obtained and the distortion can be accounted for qual. With the exception of the instrumental distortion, the upper limit is inversely proportional to the radius of a disk or hemispherical electrode. Several outer-sphere electron-transfer couples were examd. The measured rate for Ru(NH3)63+ redn. agrees with literature values. In contrast, much higher heterogeneous rates were detd. for oxidn. of ferrocene and redn. of Ru(bpy)32+ (bpy = 2,2'-bipyridine) than previously reported.
- 13Roberts, J. G.; Sombers, L. A. Fast scan cyclic voltammetry: Chemical sensing in the brain and beyond. Anal. Chem. 2018, 90 (1), 490, DOI: 10.1021/acs.analchem.7b0473213https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhvVOktbzF&md5=a671c64b1e5e02b055e2754457dd4d05Fast-Scan Cyclic Voltammetry: Chemical Sensing in the Brain and BeyondRoberts, James G.; Sombers, Leslie A.Analytical Chemistry (Washington, DC, United States) (2018), 90 (1), 490-504CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)A review. In this review the authors will describe the electroanal. method known as fast-scan cyclic voltammetry (FSCV), how it has advanced over the years, and in what way(s) it is impacting other sciences. To begin, a brief history is discussed. The various means to enhance chem. selectivity by manipulating the applied potential will be covered. Some limitations of this electroanal. method will be highlighted to inform and provide clarity to the scientific community. The intent is to seek out effective solns. to the difficult problems assocd. with the technique, so that the field will continue to flourish. Rounding out the review, the utility and adaptability of this powerful bioanal. technique will be addressed, as new frontiers of research were established for FSCV outside the scope of the neuroscience community.
- 14Heien, M. L.; Phillips, P. E.; Stuber, G. D.; Seipel, A. T.; Wightman, R. M. Overoxidation of carbon-fiber microelectrodes enhances dopamine adsorption and increases sensitivity. Analyst 2003, 128 (12), 1413– 1419, DOI: 10.1039/b307024g14https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3sXpsFymsLY%253D&md5=6eaf749094e6cd0faf2d8d169b2220f8Overoxidation of carbon-fiber microelectrodes enhances dopamine adsorption and increases sensitivityHeien, Michael L. A. V.; Phillips, Paul E. M.; Stuber, Garret D.; Seipel, Andrew T.; Wightman, R. MarkAnalyst (Cambridge, United Kingdom) (2003), 128 (12), 1413-1419CODEN: ANALAO; ISSN:0003-2654. (Royal Society of Chemistry)The voltammetric responses of carbon-fiber microelectrodes with a 1.0 V and a 1.4 V anodic limit were compared in this study. Fast-scan cyclic voltammetry was used to characterize the response to dopamine and several other neurochems. An increase in the adsorption properties of the carbon fiber leads to an increase in sensitivity of 9-fold in vivo. However the temporal response of the sensor is slower with the more pos. anodic limit. Increased electron transfer kinetics also causes a decrease in the relative sensitivity for dopamine vs. other neurochems., and a change in their cyclic voltammograms. Stimulated release in the caudate-putamen was pharmacol. characterized in vivo using Ro-04-1284 and pargyline, and was consistent with that expected for dopamine.
- 15Venton, B. J.; Cao, Q. Fundamentals of fast-scan cyclic voltammetry for dopamine detection. Analyst 2020, 145 (4), 1158– 1168, DOI: 10.1039/C9AN01586H15https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXisVyqsrnP&md5=7c87cc2797c92a70ad60a638f9b74056Fundamentals of fast-scan cyclic voltammetry for dopamine detectionVenton, B. Jill; Cao, QunAnalyst (Cambridge, United Kingdom) (2020), 145 (4), 1158-1168CODEN: ANALAO; ISSN:0003-2654. (Royal Society of Chemistry)A review. Fast-scan cyclic voltammetry (FSCV) was used with carbon-fiber microelectrodes for the real-time detection of neurotransmitters on the subsecond time scale. With FSCV, the potential is ramped up from a holding potential to a switching potential and back, usually at a 400 V s-1 scan rate and a frequency of 10 Hz. The plot of current vs. applied potential, the cyclic voltammogram (CV), has a very different shape for FSCV than for traditional cyclic voltammetry collected at scan rates which are 1000-fold slower. Here, the authors explore the theory of FSCV, with a focus on dopamine detection. First, the authors examine the shape of the CVs. Background currents, which are 100-fold higher than faradaic currents, are subtracted out. Peak sepn. is primarily due to slow electron transfer kinetics, while the sym. peak shape is due to exhaustive electrolysis of all the adsorbed neurotransmitters. Second, the authors explain the origins of the dopamine waveform, and the factors that limit the holding potential (oxygen redn.), switching potential (water oxidn.), scan rate (electrode instability), and repetition rate (adsorption). Third, data anal., from data visualization with color plots, to the automated algorithms like principal components regression that distinguish dopamine from pH changes are discussed. Finally, newer applications are discussed, including optimization of waveforms for analyte selectivity, carbon nanomaterial electrodes that trap dopamine, and basal level measurements that facilitate neurotransmitter measurements on a longer time scale. FSCV theory is complex, but understanding it enables better development of new techniques to monitor neurotransmitters in vivo.
- 16Rafi, H.; Zestos, A. G. Review-Recent Advances in FSCV Detection of Neurochemicals via Waveform and Carbon Microelectrode Modification. J. Electrochem. Soc. 2021, 168 (5), 057520, DOI: 10.1149/1945-7111/ac006416https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhtlOjurrK&md5=6257f3533e7a1b179f1cb9e39075422eReview-recent advances in FSCV detection of neurochemicals via waveform and carbon microelectrode modificationRafi, Harmain; Zestos, Alexander G.Journal of the Electrochemical Society (2021), 168 (5), 057520CODEN: JESOAN; ISSN:1945-7111. (IOP Publishing Ltd.)Fast scan cyclic voltammetry (FSCV) is an anal. technique that was first developed over 30 years ago. Since then, it has been extensively used to detect dopamine using carbon fiber microelectrodes (CFMEs). More recently, electrode modifications and waveform refinement have enabled the detection of a wider variety of neurochems. including nucleosides such as adenosine and guanosine, neurotransmitter metabolites of dopamine, and neuropeptides such as enkephalin. These alterations have facilitated the selectivity of certain biomols. over others to enhance the measurement of the analyte of interest while excluding interferants. In this review, we detail these modifications and how specializing CFME sensors allows neuro-anal. researchers to develop tools to understand the neurochem. of the brain in disease states and provide groundwork for translational work in clin. settings.
- 17Logman, M. J.; Budygin, E. A.; Gainetdinov, R. R.; Wightman, R. M. Quantitation of in vivo measurements with carbon fiber microelectrodes. Journal of neuroscience methods 2000, 95 (2), 95– 102, DOI: 10.1016/S0165-0270(99)00155-717https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3cXhtFamsb4%253D&md5=cb7f300804ffd5ed6af21884948fc877Quantitation of in vivo measurements with carbon fiber microelectrodesLogman, M. J.; Budygin, E. A.; Gainetdinov, R. R.; Wightman, R. M.Journal of Neuroscience Methods (2000), 95 (2), 95-102CODEN: JNMEDT; ISSN:0165-0270. (Elsevier Science B.V.)Fast-scan cyclic voltammetry (FSCV) at carbon fiber disk microelectrodes and quant. microdialysis were used to measure striatal concn. changes of N-acetyl-p-aminophenol (APAP, acetaminophen) following an i.p. injection of 75 mg/kg APAP in rats. The goal of this work was to det. which in vitro calibration procedure, precalibration or postcalibration, gave the most accurate results when using carbon fiber microelectrodes in vivo. Voltammetric detection of APAP in vivo was complicated with normal electrodes by interference from pH changes. An electrode treatment was used to minimize electrode sensitivity to pH and this allowed successful APAP detection. In vitro calibrations of the treated carbon fiber disk microelectrodes before and after the in vivo expt. were used to calc. APAP concn. changes measured in vivo and compared to microdialysis results. The maximal striatal APAP concn. detd. by microdialysis, adjusted for in vitro recovery, was 23.1 μM. The electrochem. results were approx. two times greater (postcalibration) or smaller (precalibration) than the microdialysis result.
- 18Hermans, A.; Keithley, R. B.; Kita, J. M.; Sombers, L. A.; Wightman, R. M. Dopamine detection with fast-scan cyclic voltammetry used with analog background subtraction. Anal. Chem. 2008, 80 (11), 4040– 4048, DOI: 10.1021/ac800108j18https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXltVeis7k%253D&md5=2f28072cd6664925df823832c00ef287Dopamine Detection with Fast-Scan Cyclic Voltammetry Used with Analog Background SubtractionHermans, Andre; Keithley, Richard B.; Kita, Justin M.; Sombers, Leslie A.; Wightman, R. MarkAnalytical Chemistry (Washington, DC, United States) (2008), 80 (11), 4040-4048CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Fast-scan cyclic voltammetry has been used in a variety of applications and has been shown to be esp. useful to monitor chem. fluctuations of neurotransmitters such as dopamine within the mammalian brain. A major limitation of this procedure, however, is the large amplitude of the background current relative to the currents for the soln. species of interest. Furthermore, the background tends to drift, and this drift limits the use of digital background subtraction techniques to intervals less than 90 s before distortion of dopamine signals occurs. To minimize the impact of the background, a procedure termed analog background subtraction is reported here. The background is recorded, and its inverse is played back to the current transducer during data acquisition so that it cancels the background in subsequent scans. Background drift still occurs and is recorded, but its magnitude is small compared to the original background. This approach has two advantages. First it allows the use of higher gains in the current transducer, minimizing quantization noise. Second, because the background amplitude is greatly reduced, principal component regression could be used to sep. the contributions from drift, dopamine, and pH when appropriate calibrations were performed. We demonstrate the use of this approach with several applications. First, transient dopamine fluctuations were monitored for 15 min in a flowing injection app. Second, evoked release of dopamine was monitored for a similar period in the brain of an anesthetized rat. Third, dopamine was monitored in the brain of freely moving rats over a 30 min interval. By analyzing the fluctuations in each resolved component, we were able to show that cocaine causes significant fluctuations in dopamine concn. in the brain while those for the background and pH remain unchanged from their predrug value.
- 19Howell, J. O.; Kuhr, W. G.; Ensman, R. E.; Wightman, R. M. Background Subtraction for Rapid Scan Voltammetry. J. Electroanal. Chem. 1986, 209 (1), 77– 90, DOI: 10.1016/0022-0728(86)80187-519https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaL28XlsVWqt7k%253D&md5=f21a3f305bfa89711aeaab3ce26d5eb1Background subtraction for rapid scan voltammetryHowell, Jonathon O.; Kuhr, Werner G.; Ensman, Robert E.; Wightman, R. MarkJournal of Electroanalytical Chemistry and Interfacial Electrochemistry (1986), 209 (1), 77-90CODEN: JEIEBC; ISSN:0022-0728.Methods for the elimination of residual current in fast scan (>300 V s-1) voltammetry were evaluated at microvoltammetric electrodes. Staircase voltammetry was found to give only a modest improvement in the ratio of the faradaic current to the residual current. Superior results are obtained when the residual current, obtained in supporting electrolyte soln., is digitally subtracted from the voltammogram obtained in the presence of the electroactive species. The subtraction process is facilitated by conducting the whole expt. in a flow injection app. so that the electrode remains in soln. while the 2 voltammograms are obtained. Undistorted voltammograms were obtained for the redn. of anthracene (∼2 mM) at scan rates up to 10,000 V s-1. At 300 V s-1, virtually undistorted voltammograms are obtained for the redn. of Tl+ at low concns. (20 μM) in aq. soln. at a Hg microvoltammetric electrode. Analog offset of the residual current was used to improve the dynamic range. The limits of this technique are caused by the electronic noise in the ideal case where flat residual current curves are obtained.
- 20Heien, M. L. A. V.; Khan, A. S.; Ariansen, J. L.; Cheer, J. F.; Phillips, P. E. M.; Wassum, K. M.; Wightman, R. M. Real-time measurement of dopamine fluctuations after cocaine in the brain of behaving rats. P Natl. Acad. Sci. USA 2005, 102 (29), 10023– 10028, DOI: 10.1073/pnas.050465710220https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2MXmvVeltLc%253D&md5=2bdc42f6641711d1a5f1a282c7ee82b1Real-time measurement of dopamine fluctuations after cocaine in the brain of behaving ratsHeien, Michael L. A. V.; Khan, Amina S.; Ariansen, Jennifer L.; Cheer, Joseph F.; Phillips, Paul E. M.; Wassum, Kate M.; Wightman, R. MarkProceedings of the National Academy of Sciences of the United States of America (2005), 102 (29), 10023-10028CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)Dopamine neurotransmission has been implicated in the modulation of many cognitive processes. Both rapid (phasic) and slower (tonic) changes in its extracellular concn. contribute to its complex actions. Fast in vivo electrochem. techniques can measure extracellular dopamine on a rapid time scale but without the selectivity afforded with slower techniques that use chem. sepns. Cyclic voltammetry improves chem. resoln. over other electrochem. methods, and it can resolve dopamine changes in the brains of behaving rodents over short epochs (<10 s). With this method, however, selective detection of slower dopamine changes is still elusive. Here we demonstrate that principal component regression of cyclic voltammetry data enables quantification of changes in dopamine and extracellular pH. Using this method, we show that cocaine modifies dopamine release in two ways: dopamine concn. transients increase in frequency and magnitude, whereas a gradual increase in steady-state dopamine concn. occurs over 90 s.
- 21Taylor, I. M.; Robbins, E. M.; Catt, K. A.; Cody, P. A.; Happe, C. L.; Cui, X. T. Enhanced dopamine detection sensitivity by PEDOT/graphene oxide coating on in vivo carbon fiber electrodes. Journal of Biosensors and Bioelectronics 2017, 89, 400– 410, DOI: 10.1016/j.bios.2016.05.084There is no corresponding record for this reference.
- 22Wipf, D. O.; Michael, A. C.; Wightman, R. M. Microdisk electrodes: Part II. Fast-scan cyclic voltammetry with very small electrodes. Journal of electroanalytical chemistry amd interfacial electrochemistry 1989, 269 (1), 15– 25, DOI: 10.1016/0022-0728(89)80100-722https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaK3cXhtlagsw%253D%253D&md5=880cc453ba1ef38ff39f18d7cff21882Microdisk electrodes. Part II. Fast-scan cyclic voltammetry with very small electrodesWipf, David O.; Michael, Adrian C.; Wightman, R. MarkJournal of Electroanalytical Chemistry and Interfacial Electrochemistry (1989), 269 (1), 15-25CODEN: JEIEBC; ISSN:0022-0728.Cyclic voltammetry was investigated at inlaid disk electrodes with nominal radii of 0.3, 1.0, and 5.0 μm. The electrode capacitance was found to be much larger than expected for the 2 smaller radii electrodes. This effect was attributed to the capacitance between the inner conductor and the electrolyte soln. The excess capacitive current was minimized by the use of a conductive shield around the electrode which is connected to ground potential. Criteria were investigated for the degree of filtering of steady-state voltammograms to minimize noise while avoiding distortion of the exptl. data. Exptl. voltammograms for the oxidn. of ferrocene in MeCN solns. were found to be in good agreement with existing theories for scan rates in which linear and convergent diffusion occur. The factors which limit the use of very small electrodes are discussed in terms of signal-to-noise, ohmic drop, and linear diffusion.
- 23DeWaele, M.; Oh, Y.; Park, C.; Kang, Y. M.; Shin, H.; Blaha, C. D.; Bennet, K. E.; Kim, I. Y.; Lee, K. H.; Jang, D. P. A baseline drift detrending technique for fast scan cyclic voltammetry. Analyst 2017, 142 (22), 4317– 4321, DOI: 10.1039/C7AN01465A23https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhsFKitrvK&md5=7dcc3d64377be749b6fc50d01d1e7345A baseline drift detrending technique for fast scan cyclic voltammetryDeWaele, Mark; Oh, Yoonbae; Park, Cheonho; Kang, Yu Min; Shin, Hojin; Blaha, Charles D.; Bennet, Kevin E.; Kim, In Young; Lee, Kendall H.; Jang, Dong PyoAnalyst (Cambridge, United Kingdom) (2017), 142 (22), 4317-4321CODEN: ANALAO; ISSN:0003-2654. (Royal Society of Chemistry)Fast scan cyclic voltammetry (FSCV) has been commonly used to measure extracellular neurotransmitter concns. in the brain. Due to the unstable nature of the background currents inherent in FSCV measurements, anal. of FSCV data is limited to very short amts. of time using traditional background subtraction. In this paper, we propose the use of a zero-phase high pass filter (HPF) as the means to remove the background drift. Instead of the traditional method of low pass filtering across voltammograms to increase the signal to noise ratio, a HPF with a low cutoff frequency was applied to the temporal dataset at each voltage point to remove the background drift. As a result, the HPF utilizing cutoff frequencies between 0.001 Hz and 0.01 Hz could be effectively used to a set of FSCV data for removing the drifting patterns while preserving the temporal kinetics of the phasic dopamine response recorded in vivo. In addn., compared to a drift removal method using principal component anal., this was found to be significantly more effective in reducing the drift (unpaired t-test p < 0.0001, t = 10.88) when applied to data collected from Tris buffer over 24 h although a drift removal method using principal component anal. also showed the effective background drift redn. The HPF was also applied to 5 h of FSCV in vivo data. Elec. evoked dopamine peaks, obsd. in the nucleus accumbens, were clearly visible even without background subtraction. This technique provides a new, simple, and yet robust, approach to analyze FSCV data with an unstable background.
- 24Atcherley, C. W.; Wood, K. M.; Parent, K. L.; Hashemi, P.; Heien, M. L. The coaction of tonic and phasic dopamine dynamics. Chem. Commun. 2015, 51 (12), 2235– 2238, DOI: 10.1039/C4CC06165A24https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhs1WitrvF&md5=163d84a44219ae257bb3dcf9bed7d238The coaction of tonic and phasic dopamine dynamicsAtcherley, Christopher W.; Wood, Kevin M.; Parent, Kate L.; Hashemi, Parastoo; Heien, Michael L.Chemical Communications (Cambridge, United Kingdom) (2015), 51 (12), 2235-2238CODEN: CHCOFS; ISSN:1359-7345. (Royal Society of Chemistry)Tonic neurochem. dopamine activity underlies many brain functions; however a consensus on this important concn. has not yet been reached. In this work, we introduce in vivo fast-scan controlled-adsorption voltammetry to report tonic dopamine concns. (90 ± 9 nM) and the dopamine diffusion coeff. (1.05 ± 0.09 × 10-6 cm2 s-1) in the mouse brain.
- 25Oh, Y.; Heien, M. L.; Park, C.; Kang, Y. M.; Kim, J.; Boschen, S. L.; Shin, H.; Cho, H. U.; Blaha, C. D.; Bennet, K. E.; Lee, H. K.; Jung, S. J.; Kim, I. Y.; Lee, K. H.; Jang, D. P. Tracking tonic dopamine levels in vivo using multiple cyclic square wave voltammetry. Biosens Bioelectron 2018, 121, 174– 182, DOI: 10.1016/j.bios.2018.08.03425https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXhslSktbrF&md5=ff0dbf43f2bee824be6afe57aa5e84d3Tracking tonic dopamine levels in vivo using multiple cyclic square wave voltammetryOh, Yoonbae; Heien, Michael L.; Park, Cheonho; Kang, Yu Min; Kim, Jaekyung; Boschen, Suelen Lucio; Shin, Hojin; Cho, Hyun U.; Blaha, Charles D.; Bennet, Kevin E.; Lee, Han Kyu; Jung, Sung Jun; Kim, In Young; Lee, Kendall H.; Jang, Dong PyoBiosensors & Bioelectronics (2018), 121 (), 174-182CODEN: BBIOE4; ISSN:0956-5663. (Elsevier B.V.)For over two decades, fast-scan cyclic voltammetry (FSCV) has served as a reliable anal. method for monitoring dopamine release in near real-time in vivo. However, contemporary FSCV techniques have been limited to measure only rapid (on the order of seconds, i.e. phasic) changes in dopamine release evoked by either elec. stimulation or elicited by presentation of behaviorally salient stimuli, and not slower changes in the tonic extracellular levels of dopamine (i.e. basal concns.). This is because FSCV is inherently a differential method that requires subtraction of prestimulation tonic levels of dopamine to measure phasic changes relative to a zeroed baseline. Here, we describe the development and application of a novel voltammetric technique, multiple cyclic square wave voltammetry (M-CSWV), for anal. quantification of tonic dopamine concns. in vivo with relatively high temporal resoln. (10 s). M-CSWV enriches the electrochem. information by generating two dimensional voltammograms which enable high sensitivity (limit of detection, 0.17 nM) and selectivity against ascorbic acid, and 3,4-dihydroxyphenylacetic acid (DOPAC), including changes in pH. Using M-CSWV, a tonic dopamine concn. of 120 ± 18 nM (n = 7 rats, ± SEM) was detd. in the striatum of urethane anethetized rats. Pharmacol. treatments to elevate dopamine by selectively inhibiting dopamine reuptake and to reduce DOPAC by inhibition of monoamine oxidase supported the selective detection of dopamine in vivo. Overall, M-CSWV offers a novel voltammetric technique to quantify levels and monitor changes in tonic dopamine concns. in the brain to further our understanding of the role of dopamine in normal behavior and neuropsychiatric disorders.
- 26Oh, Y.; Park, C.; Kim, D. H.; Shin, H.; Kang, Y. M.; DeWaele, M.; Lee, J.; Min, H.-K.; Blaha, C. D.; Bennet, K. E. Monitoring in vivo changes in tonic extracellular dopamine level by charge-balancing multiple waveform fast-scan cyclic voltammetry. Anal. Chem. 2016, 88 (22), 10962– 10970, DOI: 10.1021/acs.analchem.6b0260526https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhslCgsrnL&md5=307c84d9a85be6e45b5ad56ea13f4cdcMonitoring In Vivo Changes in Tonic Extracellular Dopamine Level by Charge-Balancing Multiple Waveform Fast-Scan Cyclic VoltammetryOh, Yoonbae; Park, Cheonho; Kim, Do Hyoung; Shin, Hojin; Kang, Yu Min; DeWaele, Mark; Lee, Jeyeon; Min, Hoon-Ki; Blaha, Charles D.; Bennet, Kevin E.; Kim, In Young; Lee, Kendall H.; Jang, Dong PyoAnalytical Chemistry (Washington, DC, United States) (2016), 88 (22), 10962-10970CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Dopamine (DA) modulates central neuronal activity through both phasic (second to second) and tonic (minutes to hours) terminal release. Conventional fast-scan cyclic voltammetry (FSCV), in combination with carbon fiber microelectrodes, has been used to measure phasic DA release in vivo by adopting a background subtraction procedure to remove background capacitive currents. However, measuring tonic changes in DA concns. using conventional FSCV has been difficult because background capacitive currents are inherently unstable over long recording periods. To measure tonic changes in DA concns. over several hours, we applied a novel charge-balancing multiple waveform FSCV (CBM-FSCV), combined with a dual background subtraction technique, to minimize temporal variations in background capacitive currents. Using this method, in vitro, charge variations from a ref. time point were nearly zero for 48 h, whereas with conventional background subtraction, charge variations progressively increased. CBM-FSCV also demonstrated a high selectivity against 3,4-dihydroxyphenylacetic acid and ascorbic acid, two major chem. interferents in the brain, yielding a sensitivity of 85.40 ± 14.30 nA/μM and limit of detection of 5.8 ± 0.9 nM for DA while maintaining selectivity. Recorded in vivo by CBM-FSCV, pharmacol. inhibition of DA reuptake (nomifensine) resulted in a 235 ± 60 nM increase in tonic extracellular DA concns., while inhibition of DA synthesis (α-methyl-DL-tyrosine) resulted in a 72.5 ± 4.8 nM decrease in DA concns. over a 2 h period. This study showed that CBM-FSCV may serve as a unique voltammetric technique to monitor relatively slow changes in tonic extracellular DA concns. in vivo over a prolonged time period.
- 27Taylor, I. M.; Patel, N. A.; Freedman, N. C.; Castagnola, E.; Cui, X. T. Direct in vivo electrochemical detection of resting dopamine using Poly (3, 4-ethylenedioxythiophene)/Carbon Nanotube functionalized microelectrodes. Anal. Chem. 2019, 91 (20), 12917– 12927, DOI: 10.1021/acs.analchem.9b0290427https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhslKitrjN&md5=3073af9f96d0141f3e5d658437b2dcebDirect in Vivo Electrochemical Detection of Resting Dopamine Using Poly(3,4-ethylenedioxythiophene)/Carbon Nanotube Functionalized MicroelectrodesTaylor, Ian Mitchell; Patel, Nikita Anurag; Freedman, Noah Chaim; Castagnola, Elisa; Cui, Xinyan TracyAnalytical Chemistry (Washington, DC, United States) (2019), 91 (20), 12917-12927CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Dopamine (DA) is a monoamine neurotransmitter responsible for the maintenance of a variety of vital life functions. In vivo DA signaling occurs over multiple time scales, from sub-second phasic release due to dopamine neuron firing, to tonic release responsible for long-term DA concn. changes over minutes to hours. Due to the complex, multifaceted nature of DA signaling, anal. sensing technol. must be capable of recording DA from multiple locations and over multiple timescales. Decades of research has focused on improving in vivo detection capabilities for sub-second phasic DA, but the accurate detection of abs. resting DA levels in real time has proven challenging. The authors have developed a poly(3,4 ethylene dioxythiophene) (PEDOT)-based nanocomposite coating that exhibits excellent DA sensing capabilities for resting DA. PEDOT/functionalized carbon nanotube (PEDOT/CNT) coated carbon fiber microelectrodes (CFEs) are capable of directly measuring resting DA using square wave voltammetry (SWV) with high sensitivity and selectivity. Incorporation of a PEDOT/CNT coating significantly increases the sensitivity for the detection of resting DA by a factor of 422. SWV measurements performed at PEDOT/CNT functionalized CFEs implanted in the rat dorsal striatum reveal the abs. basal DA concn. to be 82±6 nM. Systemic administration of the dopamine transporter inhibitor, nomifensine increases resting DA to a max. 207±16 nM at 28±2 min following injection. PEDOT/CNT was also functionalized onto individual gold electrode sites along silicon microelectrode arrays (MEAs) to produce a multisite DA sensing electrode. MEA implantation allows for the quantification of basal DA from different brain regions with excellent spatial resoln. SWV detection paired with PEDOT/CNT functionalized is highly adaptable and shows great promise for tonic DA detection with high spatial and temporal resoln.
- 28Johnson, J. A.; Hobbs, C. N.; Wightman, R. M. Removal of Differential Capacitive Interferences in Fast-Scan Cyclic Voltammetry. Anal. Chem. 2017, 89 (11), 6166– 6174, DOI: 10.1021/acs.analchem.7b0100528https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXntlWitbo%253D&md5=83bcb6cfdccfff671ae4f7be8b3afd4aRemoval of Differential Capacitive Interferences in Fast-Scan Cyclic VoltammetryJohnson, Justin A.; Hobbs, Caddy N.; Wightman, R. MarkAnalytical Chemistry (Washington, DC, United States) (2017), 89 (11), 6166-6174CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Due to its high spatiotemporal resoln., fast-scan cyclic voltammetry (FSCV) at carbon-fiber microelectrodes enables the localized in vivo monitoring of subsecond fluctuations in electroactive neurotransmitter concns. In practice, resoln. of the anal. signal relies on digital background subtraction for removal of the large current due to charging of the elec. double layer as well as surface faradaic reactions. However, fluctuations in this background current often occur with changes in the electrode state or ionic environment, leading to nonspecific contributions to the FSCV data that confound data anal. Here, the authors both explore the origin of such shifts seen with local changes in cations and develop a model to account for their shape. Further, the authors describe a convolution-based method for removal of the differential capacitive contributions to the FSCV current. The method relies on the use of a small-amplitude pulse made prior to the FSCV sweep that probes the impedance of the system. To predict the nonfaradaic current response to the voltammetric sweep, the step current response is differentiated to provide an est. of the system's impulse response function and is used to convolute the applied waveform. The generated prediction is then subtracted from the obsd. current to the voltammetric sweep, removing artifacts assocd. with electrode impedance changes. The technique is demonstrated to remove select contributions from capacitive characteristics changes of the electrode both in vitro (i.e., in flow-injection anal.) and in vivo (i.e., during a spreading depression event in an anesthetized rat).
- 29Meunier, C. J.; McCarty, G. S.; Sombers, L. A. Drift Subtraction for Fast-Scan Cyclic Voltammetry Using Double-Waveform Partial-Least-Squares Regression. Anal. Chem. 2019, 91 (11), 7319– 7327, DOI: 10.1021/acs.analchem.9b0108329https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXptlKqu7g%253D&md5=c0794bcf0db185cbb20829f2d777b307Drift Subtraction for Fast-Scan Cyclic Voltammetry Using Double-Waveform Partial-Least-Squares RegressionMeunier, Carl J.; McCarty, Gregory S.; Sombers, Leslie A.Analytical Chemistry (Washington, DC, United States) (2019), 91 (11), 7319-7327CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Background-subtracted fast-scan cyclic voltammetry (FSCV) provides a method for detecting mol. fluctuations with high spatiotemporal resoln. in the brain of awake and behaving animals. The rapid scan rates generate large background currents that are subtracted to reveal changes in analyte concn. Although these background currents are relatively stable, small changes do occur over time. These changes, referred to as electrochem. drift, result in background-subtraction artifacts that constrain the utility of FSCV, particularly when quantifying chem. changes that gradually occur over long measurement times (minutes). The voltammetric features of electrochem. drift are varied and can span the entire potential window, potentially obscuring the signal from any targeted analyte. The authors present a straightforward method for extending the duration of a single FSCV recording window. First, the authors have implemented voltammetric waveforms in pairs that consist of a smaller triangular sweep followed by a conventional voltammetric scan. The initial, abbreviated waveform is used to capture drift information that can serve as a predictor for the contribution of electrochem. drift to the subsequent full voltammetric scan using partial-least-squares regression (PLSR). This double-waveform partial-least-squares regression (DW-PLSR) paradigm permits reliable subtraction of the drift component to the voltammetric data. Here, DW-PLSR is used to improve quantification of adenosine, dopamine, and hydrogen peroxide fluctuations occurring >10 min from the initial background position, both in vitro and in vivo. The results demonstrate that DW-PLSR is a powerful tool for evaluating and interpreting both rapid (seconds) and gradual (minutes) chem. changes captured in FSCV recordings over extended durations.
- 30Espin, L. X.; Asp, A. J.; Trevathan, J. K.; Ludwig, K. A.; Lujan, J. L. Integral methods for automatic quantification of fast-scan-cyclic-voltammetry detected neurotransmitters. PLoS One 2021, 16 (7), e0254594, DOI: 10.1371/journal.pone.025459430https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhs1ymt7jM&md5=7293f3e74aa31acd110a07a982944fa8Integral methods for automatic quantification of fast-scan-cyclic-voltammetry detected neurotransmittersEspin, Leonardo X.; Asp, Anders J.; Trevathan, James K.; Ludwig, Kip A.; Lujan, J. LuisPLoS One (2021), 16 (7), e0254594CODEN: POLNCL; ISSN:1932-6203. (Public Library of Science)Modern techniques for estg. basal levels of electroactive neurotransmitters rely on the measurement of oxidative charges. This requires time integration of oxidn. currents at certain intervals. Unfortunately, the selection of integration intervals relies on ad-hoc visual identification of peaks on the oxidn. currents, which introduces sources of error and precludes the development of automated procedures necessary for anal. and quantification of neurotransmitter levels in large data sets. In an effort to improve charge quantification techniques, here we present novel methods for automatic selection of integration boundaries. Our results show that these methods allow quantification of oxidn. reactions both in vitro and in vivo and of multiple analytes in vitro.
- 31Bucher, E. S.; Brooks, K.; Verber, M. D.; Keithley, R. B.; Owesson-White, C.; Carroll, S.; Takmakov, P.; McKinney, C. J.; Wightman, R. M. Flexible Software Platform for Fast-Scan Cyclic Voltammetry Data Acquisition and Analysis. Anal. Chem. 2013, 85 (21), 10344– 10353, DOI: 10.1021/ac402263x31https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXhsFGku77M&md5=116501c82a8e13a2c012f2b1b1ae48e9Flexible Software Platform for Fast-Scan Cyclic Voltammetry Data Acquisition and AnalysisBucher, Elizabeth S.; Brooks, Kenneth; Verber, Matthew D.; Keithley, Richard B.; Owesson-White, Catarina; Carroll, Susan; Takmakov, Pavel; McKinney, Collin J.; Wightman, R. MarkAnalytical Chemistry (Washington, DC, United States) (2013), 85 (21), 10344-10353CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Over the last several decades, fast-scan cyclic voltammetry (FSCV) has proved to be a valuable anal. tool for the real-time measurement of neurotransmitter dynamics in vitro and in vivo. Indeed, FSCV has found application in a wide variety of disciplines including electrochem., neurobiol., and behavioral psychol. The maturation of FSCV as an in vivo technique led users to pose increasingly complex questions that require a more sophisticated exptl. design. To accommodate recent and future advances in FSCV application, the authors' lab has developed High Definition Cyclic Voltammetry (HDCV). HDCV is an electrochem. software suite that includes data acquisition and anal. programs. The data collection program delivers greater exptl. flexibility and better user feedback through live displays. It supports expts. involving multiple electrodes with customized waveforms. It is compatible with transistor-transistor logic-based systems that are used for monitoring animal behavior, and it enables simultaneous recording of electrochem. and electrophysiol. data. HDCV anal. streamlines data processing with superior filtering options, seamlessly manages behavioral events, and integrates chemometric processing. Furthermore, anal. is capable of handling single files collected over extended periods of time, allowing the user to consider biol. events on both sub-second and multi-minute time scales. Here the authors describe and demonstrate the utility of HDCV for in vivo expts.
- 32Bath, B. D.; Michael, D. J.; Trafton, B. J.; Joseph, J. D.; Runnels, P. L.; Wightman, R. M. Subsecond adsorption and desorption of dopamine at carbon-fiber microelectrodes. Anal. Chem. 2000, 72 (24), 5994– 6002, DOI: 10.1021/ac000849y32https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3cXotVyis7s%253D&md5=6e2c2e1202ae88e8ec4bfbcd274dc976Subsecond adsorption and desorption of dopamine at carbon-fiber microelectrodesBath, Bradley D.; Michael, Darren J.; Trafton, B. Jill; Joseph, Joshua D.; Runnels, Petrise L.; Wightman, R. MarkAnalytical Chemistry (2000), 72 (24), 5994-6002CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)High-repetition fast-scan cyclic voltammetry and chronoamperometry were used to quantify and characterize the kinetics of dopamine and dopamine-o-quinone adsorption and desorption at carbon-fiber microelectrodes. A flow injection anal. system was used for the precise introduction and removal of a bolus of electroactive substance on a sub-second time scale to the disk-shaped surface of a microelectrode that was fabricated from a single carbon fiber (Thornel type T650 or P55). Pretreatment of the electrode surfaces consisted of soaking them in purified iso-Pr alc. for a min. of 10 min, which resulted in S/N increasing by 200-400% for dopamine above that for those that were soaked in reagent grade solvent. Because of adsorption, high scan rates (2000 V/s) are shown to exhibit equiv. S/N ratios as compared to slower, more traditional scan rates. In addn., the steady-state response to a concn. bolus is shown to occur more rapidly when cyclic voltammetric scans are repeated at short intervals (4 ms). The new methodologies allow for more accurate detns. of the kinetics of neurotransmitter release events (10-500 ms) in biol. systems. Brain slice and in vivo expts. using T650 cylinder microelectrodes show that voltammetrically measured uptake kinetics in the caudate are faster using 2000 V/s and 240 Hz measurements, as compared to 300 V/s and 10 Hz.
- 33Mirza, K. B.; Golden, C. T.; Nikolic, K.; Toumazou, C. Closed-Loop Implantable Therapeutic Neuromodulation Systems Based on Neurochemical Monitoring. Front. Neurosci. 2019, 13, na, DOI: 10.3389/fnins.2019.00808There is no corresponding record for this reference.
- 34Kim, S.; Kang, S.; Kim, J.; Lee, D.; Kim, S.; Lee, J.; Jang, K.-I.; Oh, Y.-S.; Rah, J.-C.; Huh, M. S. Closed-Loop Neuromodulation for Parkinson’s Disease: Current State and Future Directions. IEEE Transactions on Molecular, Biological Multi-Scale Communications 2021, 7 (4), 209– 223, DOI: 10.1109/TMBMC.2020.3036756There is no corresponding record for this reference.
- 35Lee, K. H.; Lujan, J. L.; Trevathan, J. K.; Ross, E. K.; Bartoletta, J. J.; Park, H. O.; Paek, S. B.; Nicolai, E. N.; Lee, J. H.; Min, H. K.; Kimble, C. J.; Blaha, C. D.; Bennet, K. E. WINCS Harmoni: Closed-loop dynamic neurochemical control of therapeutic interventions. Sci. Rep. 2017, 7, 46675, DOI: 10.1038/srep4667535https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BC1critV2qtQ%253D%253D&md5=8b49acf534584b18641057c54f19bc5eWINCS Harmoni: Closed-loop dynamic neurochemical control of therapeutic interventionsLee Kendall H; Lujan J Luis; Ross Erika K; Bartoletta John J; Park Hyung Ook; Nicolai Evan N; Lee Jannifer H; Min Hoon-Ki; Blaha Charles D; Bennet Kevin E; Lee Kendall H; Lujan J Luis; Min Hoon-Ki; Lee Kendall H; Trevathan James K; Paek Seungleal Brian; Kimble Christopher J; Bennet Kevin EScientific reports (2017), 7 (), 46675 ISSN:.There has been significant progress in understanding the role of neurotransmitters in normal and pathologic brain function. However, preclinical trials aimed at improving therapeutic interventions do not take advantage of real-time in vivo neurochemical changes in dynamic brain processes such as disease progression and response to pharmacologic, cognitive, behavioral, and neuromodulation therapies. This is due in part to a lack of flexible research tools that allow in vivo measurement of the dynamic changes in brain chemistry. Here, we present a research platform, WINCS Harmoni, which can measure in vivo neurochemical activity simultaneously across multiple anatomical targets to study normal and pathologic brain function. In addition, WINCS Harmoni can provide real-time neurochemical feedback for closed-loop control of neurochemical levels via its synchronized stimulation and neurochemical sensing capabilities. We demonstrate these and other key features of this platform in non-human primate, swine, and rodent models of deep brain stimulation (DBS). Ultimately, systems like the one described here will improve our understanding of the dynamics of brain physiology in the context of neurologic disease and therapeutic interventions, which may lead to the development of precision medicine and personalized therapies for optimal therapeutic efficacy.
- 36Kang, S.; Park, J.; Jeong, Y.; Oh, Y.-S; Choi, J.-W. takang0902/Open_SDBR, Zenodo 2022, na, DOI: 10.5281/zenodo.6597381There is no corresponding record for this reference.
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Author contributions, selectivity test, surgery, and in vivo dopamine measurement experiment details and in silico test (PDF)
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