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Mechanism of Electron Spin Decoherence in a Partially Deuterated Glassy Matrix

  • Samuel M. Jahn
    Samuel M. Jahn
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
  • Elizabeth R. Canarie
    Elizabeth R. Canarie
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
  • , and 
  • Stefan Stoll*
    Stefan Stoll
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
    *Email: [email protected]
    More by Stefan Stoll
Cite this: J. Phys. Chem. Lett. 2022, 13, 24, 5474–5479
Publication Date (Web):June 10, 2022
https://doi.org/10.1021/acs.jpclett.2c00939
Copyright © 2022 American Chemical Society

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    Abstract

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    Long electron spin coherence lifetimes are essential for applications in quantum information science and electron paramagnetic resonance, for instance, for nanoscale distance measurements in biomolecular systems using double electron–electron resonance. We experimentally investigate the decoherence dynamics under the Hahn echo sequence of the organic radical d18-TEMPO in a variably deuterated frozen water:glycerol matrix. The coherence time (phase memory time) TM scales with proton concentration as [1H]−0.65. For selectively deuterated matrices, decoherence is accelerated in the presence of proton clustering, that is, substantial short-range density in the proton–proton radial distribution functions (<3 Å). Simulations using molecular dynamics and many-body spin quantum dynamics show excellent agreement with experiment and show that geminal proton pairs such as CH2 and OH2 groups are major decoherence drivers. This provides a predictive tool for designing molecular systems with long electron spin coherence times.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.2c00939.

    • Detailed descriptions of experimental parameters, molecular dynamics simulations, and spin quantum dynamics simulations (ZIP)

    • Molecular dynamics data for TEMPO (ZIP)

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    Cited By

    This article is cited by 4 publications.

    1. Jasleen K. Bindra, Jens Niklas, Yeonjun Jeong, Ahren W. Jasper, Moritz Kretzschmar, Jan Kern, Lisa M. Utschig, Oleg G. Poluektov. Coherences of Photoinduced Electron Spin Qubit Pair States in Photosystem I. The Journal of Physical Chemistry B 2023, 127 (47) , 10108-10117. https://doi.org/10.1021/acs.jpcb.3c06658
    2. C. Blake Wilson, Mian Qi, Songi Han, Mark S. Sherwin. Gadolinium Spin Decoherence Mechanisms at High Magnetic Fields. The Journal of Physical Chemistry Letters 2023, 14 (47) , 10578-10584. https://doi.org/10.1021/acs.jpclett.3c01847
    3. 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
    4. G. Jeschke. Nuclear pair electron spin echo envelope modulation. Journal of Magnetic Resonance Open 2023, 14-15 , 100094. https://doi.org/10.1016/j.jmro.2023.100094

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