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Room Temperature Electron Spin Coherence in Photogenerated Molecular Spin Qubit Candidates

Cite this: J. Am. Chem. Soc. 2023, 145, 25, 14064–14069
Publication Date (Web):June 19, 2023
https://doi.org/10.1021/jacs.3c04021
Copyright © 2023 American Chemical Society

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    Abstract

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    One of the main challenges in the emerging field of molecular spintronics is the identification of new spin qubit materials for quantum information applications. In this regard, recent work has shown that photoexcited chromophore–radical systems are promising candidates to expand our repertoire of suitable candidate molecules. Here, we investigate a series of three chromophore–radical compounds composed of a perylene diimide (PDI) chromophore and a stable 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO) radical by transient electron paramagnetic resonance (EPR) techniques. We explore the influence of isotope labeling of the TEMPO moiety on the EPR spectra and electron spin coherence times of the molecular quartet states generated upon photoexcitation and illustrate that (i) a coherent manipulation of the spin state is possible in these systems even at room temperature and that (ii) a spin coherence time of 0.7 μs can be achieved under these conditions. This demonstration of electron spin coherence at ambient temperatures paves the way for practical applications of such systems in functional molecular devices.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.3c04021.

    • Synthetic procedures and characterization, UV–vis spectra, description of the EPR sample preparation, EPR measurement conditions and parameters, complementary EPR data, and details of the data analysis including simulation parameters (PDF)

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    Cited By

    This article is cited by 4 publications.

    1. 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
    2. Martin L. Kirk, David A. Shultz, Anil Reddy Marri, Art van der Est. Photoinduced Magnetic Exchange-Jump Promotes Ground State Biradical Electron Spin Polarization. Journal of the American Chemical Society 2024, 146 (13) , 9285-9292. https://doi.org/10.1021/jacs.4c00930
    3. 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
    4. 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