ACS Publications. Most Trusted. Most Cited. Most Read
Quantum Gate Operations on a Spectrally Addressable Photogenerated Molecular Electron Spin-Qubit Pair

OR SEARCH CITATIONS

My Activity
Publications

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Am. Chem. Soc. 2023, 145, 11, 6585-6593
    Article

    Quantum Gate Operations on a Spectrally Addressable Photogenerated Molecular Electron Spin-Qubit Pair
    Click to copy article linkArticle link copied!

    • Haochuan Mao
      Haochuan Mao
      Department of Chemistry, Center for Molecular Quantum Transduction, and Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, Illinois 60208-3113, United States
      More by Haochuan Mao
      Orcidhttps://orcid.org/0000-0001-8742-089X
    • Gediminas J. Pažėra
      Gediminas J. Pažėra
      Department of Chemistry, Center for Molecular Quantum Transduction, and Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, Illinois 60208-3113, United States
      Physical and Theoretical Chemistry Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3QZ, U.K.
      More by Gediminas J. Pažėra
    • Ryan M. Young
      Ryan M. Young
      Department of Chemistry, Center for Molecular Quantum Transduction, and Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, Illinois 60208-3113, United States
      More by Ryan M. Young
      Orcidhttps://orcid.org/0000-0002-5108-0261
    • Matthew D. Krzyaniak*
      Matthew D. Krzyaniak
      Department of Chemistry, Center for Molecular Quantum Transduction, and Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, Illinois 60208-3113, United States
      *Email: [email protected]
      More by Matthew D. Krzyaniak
      Orcidhttps://orcid.org/0000-0002-8761-7323
    • Michael R. Wasielewski*
      Michael R. Wasielewski
      Department of Chemistry, Center for Molecular Quantum Transduction, and Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, Illinois 60208-3113, United States
      *Email: [email protected]
      More by Michael R. Wasielewski
      Orcidhttps://orcid.org/0000-0003-2920-5440
    Other Access OptionsSupporting Information (1)

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2023, 145, 11, 6585–6593
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.3c01243
    Published March 13, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

    Abstract

    Click to copy section linkSection link copied!
    Abstract Image

    Sub-nanosecond photodriven electron transfer from a molecular donor to an acceptor can be used to generate a radical pair (RP) having two entangled electron spins in a well-defined pure initial singlet quantum state to serve as a spin-qubit pair (SQP). Achieving good spin-qubit addressability is challenging because many organic radical ions have large hyperfine couplings (HFCs) in addition to significant g-anisotropy, which results in significant spectral overlap. Moreover, using radicals with g-factors that deviate significantly from that of the free electron results in difficulty generating microwave pulses with sufficiently large bandwidths to manipulate the two spins either simultaneously or selectively as is necessary to implement the controlled-NOT (CNOT) quantum gate essential for quantum algorithms. Here, we address these issues by using a covalently linked donor–acceptor(1)–acceptor(2) (D-A1-A2) molecule with significantly reduced HFCs that uses fully deuterated peri-xanthenoxanthene (PXX) as D, naphthalenemonoimide (NMI) as A1, and a C60 derivative as A2. Selective photoexcitation of PXX within PXX-d9-NMI-C60 results in sub-nanosecond, two-step electron transfer to generate the long-lived PXX•+-d9-NMI-C60•– SQP. Alignment of PXX•+-d9-NMI-C60•– in the nematic liquid crystal 4-cyano-4′-(n-pentyl)biphenyl (5CB) at cryogenic temperatures results in well-resolved, narrow resonances for each electron spin. We demonstrate both single-qubit gate and two-qubit CNOT gate operations using both selective and nonselective Gaussian-shaped microwave pulses and broadband spectral detection of the spin states following the gate operations.

    Copyright © 2023 American Chemical Society

    Subjects

    what are subjects

    Read this article

    To access this article, please review the available access options below.

    Get instant access

    Purchase Access

    Read this article for 48 hours. Check out below using your ACS ID or as a guest.

    Recommended

    Access through Your Institution

    You may have access to this article through your institution.

    Your institution does not have access to this content. Add or change your institution or let them know you’d like them to include access.

    Supporting Information

    Click to copy section linkSection link copied!

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.3c01243.

    • Experimental details, including synthesis, NMR, mass spec, TA spectra and kinetics, and additional EPR spectra (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    Click to copy section linkSection link copied!
    Citation Statements
    Explore this article's citation statements on scite.ai
    powered by  Scite

    This article is cited by 24 publications.

    1. Autumn Y. Lee, Mandefro Teferi, Frida S. Hernandez, Amisha Jain, Tiffany Tran, Kefu Wang, Tomoyasu Mani, Adam M. Schwartzberg, Ming Lee Tang, Jens Niklas, Oleg G. Poluektov, Jacob H. Olshansky. Tunable Spin Qubit Pairs in Quantum Dot–Molecule Conjugates. ACS Nano 2025, 19 (12) , 12194-12207. https://doi.org/10.1021/acsnano.5c00288
    2. Alberto Privitera, Alessandro Chiesa, Fabio Santanni, Angelo Carella, Davide Ranieri, Andrea Caneschi, Matthew D. Krzyaniak, Ryan M. Young, Michael R. Wasielewski, Stefano Carretta, Roberta Sessoli. Room-Temperature Optical Spin Polarization of an Electron Spin Qudit in a Vanadyl-Free Base Porphyrin Dimer. Journal of the American Chemical Society 2025, 147 (1) , 331-341. https://doi.org/10.1021/jacs.4c10632
    3. Olusayo J. Ogunyemi, Chanchal Rani, Oleg Varnavski, Rumaisa Wajahath, Michael Norscia, Brock Malaikal, Yunfan Qiu, Shichao Sun, Yonghao Gu, Shaul Mukamel, Michael R. Wasielewski, Theodore Goodson, III. Understanding the Correlation of the Quantum Dephasing Time and Entangled Photon Interaction in Crystalline Tetracene Derivatives. The Journal of Physical Chemistry C 2024, 128 (47) , 20287-20296. https://doi.org/10.1021/acs.jpcc.4c05907
    4. Paige J. Brown, Yunfan Qiu, Elisabeth I. Latawiec, Brian T. Phelan, Nikolai A. Tcyrulnikov, Jonathan R. Palmer, Matthew D. Krzyaniak, Sebastian M. Kopp, Yuheng Huang, Ryan M. Young, Michael R. Wasielewski. Enhancing Photogenerated Radical Pair Properties in Donor-Chromophore-Acceptor Systems for Quantum Information Applications. The Journal of Physical Chemistry A 2024, 128 (43) , 9371-9382. https://doi.org/10.1021/acs.jpca.4c05015
    5. Akio Yamauchi, Nobuhiro Yanai. Toward Quantum Noses: Quantum Chemosensing Based on Molecular Qubits in Metal–Organic Frameworks. Accounts of Chemical Research 2024, 57 (20) , 2963-2972. https://doi.org/10.1021/acs.accounts.4c00333
    6. Sebastian M. Kopp, Shunta Nakamura, Brian T. Phelan, Yong Rui Poh, Samuel B. Tyndall, Paige J. Brown, Yuheng Huang, Joel Yuen-Zhou, Matthew D. Krzyaniak, Michael R. Wasielewski. Luminescent Organic Triplet Diradicals as Optically Addressable Molecular Qubits. Journal of the American Chemical Society 2024, 146 (40) , 27935-27945. https://doi.org/10.1021/jacs.4c11116
    7. Laura A. Völker, Konstantin Herb, Darin A. Merchant, Lorenzo Bechelli, Christian L. Degen, John M. Abendroth. Charge and Spin Dynamics and Destabilization of Shallow Nitrogen–Vacancy Centers under UV and Blue Excitation. Nano Letters 2024, 24 (38) , 11895-11903. https://doi.org/10.1021/acs.nanolett.4c03064
    8. Maximilian Mayländer, Ivan V. Khariushin, Andreas Vargas Jentzsch, Sabine Richert. Correlation between Radical and Quartet State Coherence Times in Photogenerated Triplet–Radical Conjugates. The Journal of Physical Chemistry Letters 2024, 15 (22) , 5935-5938. https://doi.org/10.1021/acs.jpclett.4c01353
    9. Asif Equbal, Chandrasekhar Ramanathan, Songi Han. Dipolar Order Induced Electron Spin Hyperpolarization. The Journal of Physical Chemistry Letters 2024, 15 (20) , 5397-5406. https://doi.org/10.1021/acs.jpclett.4c00294
    10. Jonathan R. Palmer, Malik L. Williams, Ryan M. Young, Kathryn R. Peinkofer, Brian T. Phelan, Matthew D. Krzyaniak, Michael R. Wasielewski. Oriented Triplet Excitons as Long-Lived Electron Spin Qutrits in a Molecular Donor–Acceptor Single Cocrystal. Journal of the American Chemical Society 2024, 146 (1) , 1089-1099. https://doi.org/10.1021/jacs.3c12277
    11. Yunfan Qiu, Hannah J. Eckvahl, Asif Equbal, Matthew D. Krzyaniak, Michael R. Wasielewski. Enhancing Coherence Times of Chromophore-Radical Molecular Qubits and Qudits by Rational Design. Journal of the American Chemical Society 2023, 145 (47) , 25903-25909. https://doi.org/10.1021/jacs.3c10772
    12. Jie Zhang, Haifen Luo, Wen Ma, Jingqi Lv, Bo Wang, Fengwei Sun, Weijie Chi, Zhuting Fang, Zhen Yang. Semiconducting Open‐Shell Radicals for Precise Tumor Activatable Phototheranostics. Advanced Science 2025, https://doi.org/10.1002/advs.202500293
    13. Cong‐Hui Wu, Qi Xiong, Xing‐Quan Tao, Geng‐Ming Zhang, Zheng Liu, Li‐Nan Zhou, Song Gao, Ye‐Xin Wang, Shen Zhou, Shang‐Da Jiang. Photoexcited Triplet State of Fullerene‐Palladium Porphyrin Dyad as a Spin Qutrit. Advanced Functional Materials 2025, 264 https://doi.org/10.1002/adfm.202426013
    14. Timothy J. Krogmeier, Anthony W. Schlimgen, Kade Head-Marsden. Low temperature decoherence dynamics in molecular spin systems using the Lindblad master equation. Chemical Science 2024, 15 (47) , 19834-19841. https://doi.org/10.1039/D4SC05627B
    15. F. F. Murzakhanov, D. V. Shurtakova, E. I. Oleynikova, G. V. Mamin, M. A. Sadovnikova, O. P. Kazarova, E. N. Mokhov, M. R. Gafurov, V. A. Soltamov. Spin Alignment of NV− Centers in 4H- and 6H-SiC Crystals Induced by IR and Visible Optical Excitation. Applied Magnetic Resonance 2024, 55 (9) , 1175-1182. https://doi.org/10.1007/s00723-024-01690-8
    16. Aimei Zhou, Zhecheng Sun, Lei Sun. Stable organic radical qubits and their applications in quantum information science. The Innovation 2024, 5 (5) , 100662. https://doi.org/10.1016/j.xinn.2024.100662
    17. Fabio Santanni, Alberto Privitera. Metalloporphyrins as Building Blocks for Quantum Information Science. Advanced Optical Materials 2024, 12 (18) https://doi.org/10.1002/adom.202303036
    18. K. M. Salikhov, A. A. Sukhanov, I. T. Khairutdinov. Features of the Primary Electron Spin Echo Signal for Spin-Correlated Radical Pairs. Applied Magnetic Resonance 2024, 55 (4) , 463-475. https://doi.org/10.1007/s00723-023-01636-6
    19. Farhan T. Chowdhury, Matt C.J. Denton, Daniel C. Bonser, Daniel R. Kattnig. Quantum Control of Radical-Pair Dynamics beyond Time-Local Optimization. PRX Quantum 2024, 5 (2) https://doi.org/10.1103/PRXQuantum.5.020303
    20. Daniele Panariti, Sarah M. Conron, Jinyuan Zhang, Michael R. Wasielewski, Marilena Di Valentin, Claudia E. Tait. Control of excitation selectivity in pulse EPR on spin-correlated radical pairs with shaped pulses. Physical Chemistry Chemical Physics 2024, 26 (5) , 3842-3856. https://doi.org/10.1039/D3CP06009H
    21. Lauren E. McNamara, Aimei Zhou, Tijana Rajh, Lei Sun, John S. Anderson. Realizing solution-phase room temperature quantum coherence in a tetrathiafulvalene-based diradicaloid complex. Cell Reports Physical Science 2023, 4 (12) , 101693. https://doi.org/10.1016/j.xcrp.2023.101693
    22. Arthur H. G. David, Daryna Shymon, Hayley Melville, Lou-Ann Accou, Adèle Gapin, Magali Allain, Olivier Alévêque, Maximilien Force, Alexis Grosjean, Piétrick Hudhomme, Laura Le Bras, Antoine Goujon. ortho O -Annulated azabenzannulated perylenediimide and bisazacoronenediimide. Journal of Materials Chemistry C 2023, 11 (42) , 14631-14640. https://doi.org/10.1039/D3TC02376A
    23. Hannah J. Eckvahl, Nikolai A. Tcyrulnikov, Alessandro Chiesa, Jillian M. Bradley, Ryan M. Young, Stefano Carretta, Matthew D. Krzyaniak, Michael R. Wasielewski. Direct observation of chirality-induced spin selectivity in electron donor–acceptor molecules. Science 2023, 382 (6667) , 197-201. https://doi.org/10.1126/science.adj5328
    24. Akihiro Tateno, Kenta Masuzawa, Hiroki Nagashima, Kiminori Maeda. Anisotropic and Coherent Control of Radical Pairs by Optimized RF Fields. International Journal of Molecular Sciences 2023, 24 (11) , 9700. https://doi.org/10.3390/ijms24119700
    Download PDF
    Go to Journal of the American Chemical Society
    Get e-Alerts
    Get e-Alerts

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2023, 145, 11, 6585–6593
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.3c01243
    Published March 13, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

    Article Views

    3318

    Altmetric

    -

    Citations

    24
    Learn about these metrics

    Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.

    Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.

    The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.