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EPR and DEER Characterization of New Mixed Weakly Coupled Nitroxide Triradicals for Molecular Three-Spin Qubits

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Abstract

Three new mixed triradicals with small exchange coupling parameters (J ≪ AN) were obtained on the base of a coupling reaction between the derivative of spirofused 2,5-dihydroimidazol-type monoradical and the two mol. equivalents of carboxylic acid derivatives of PROXYL-, TEMPO- or 2,5-dihydro-1H-pyrrol-type nitroxides. Their intramolecular magnetic interactions were characterized in terms of comparison of the CW X, Q- and W-band EPR spectra with those of the monoradical precursors. The dipole–dipole coupling parameters of the triradicals were estimated on the base of the quantum chemical calculations at UB3LYP/6-31G(d) level of theory. Two types of the spin distances were found in the triradicals: short—with the distance of 13–17 Å (D ≈ 11–24 MHz) and long—with the distance of 21–23 Å (D ≈ 4–6 MHz). The longest spin–spin as well as spin–lattice relaxation times at 50 K were detected for the triradical carrying the two TEMPO fragments, indicating the potential usage of three-spin qubit models for quantum gate operations.

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Acknowledgements

This work was supported by JSPS-RFBR (Grant 17-53-50043) under the Japan–Russia Research Cooperative Program and by the Ministry of Science and Education of the Russian Federation, Grant 14.W03.31.0034, (in particular: the synthesis of compounds, CW and DEER EPR measurements). Authors would like to acknowledge the Multi-Access Chemical Research Center SB RAS for spectral and analytical measurements. K. S, H. M. T. T. are thankful to JSPS Grants-in-Aid for Scientific Research on Innovative Areas (Quantum Cybernetics), JSPS KAKENHI Scientific Research (B) (no. 23350011, 17H03012), JSPS KAKENHI Scientific Research (C) (nos. 17K05840, 18K03465), and JSPS Grant-in-Aid for Challenging Exploratory Research (no. 25620063). We thank partial supports by FIRST Quantum Information Processing Project, Cabinet Office, Japan. We also acknowledge AOARD for support by AOARD Scientific Project on “Quantum Properties of Molecular Nanomagnets” (Award No. FA2386-13-1-4029, 4030, 4031) and AOARD Project on “Molecular Spins for Quantum Technologies” (Award no. FA2386-17-1-4040).

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Authors and Affiliations

  1. N.N. Vorozhtsov Novosibirsk Institute of Organic Chemistry SB RAS, 9 Lavrentiev Avenue, Novosibirsk, 630090, Russia

    Elena Zaytseva, Dmitryi Parkhomenko, Dmitrii Mazhukin & Elena Bagryanskaya

  2. Novosibirsk State University, Pirogova 1, Novosibirsk, 630090, Russia

    Elena Zaytseva, Ivan Timofeev, Olesya Krumkacheva, Dmitryi Parkhomenko, Dmitrii Mazhukin & Elena Bagryanskaya

  3. International Tomography Center SB RAS, Institutskaya ЗA, Novosibirsk, 630090, Russia

    Ivan Timofeev & Olesya Krumkacheva

  4. Department of Chemistry and Molecular Materials Science, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka, 558-8585, Japan

    Kazunobu Sato, Hideto Matsuoka & Takeji Takui

  5. Research Support Department/University Research Administrator Center, University Administration Division, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka, 558-8585, Japan

    Takeji Takui

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  1. Elena Zaytseva
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  2. Ivan Timofeev
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  3. Olesya Krumkacheva
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  4. Dmitryi Parkhomenko
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  5. Dmitrii Mazhukin
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  6. Kazunobu Sato
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  7. Hideto Matsuoka
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  9. Elena Bagryanskaya
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Correspondence to Elena Bagryanskaya.

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Zaytseva, E., Timofeev, I., Krumkacheva, O. et al. EPR and DEER Characterization of New Mixed Weakly Coupled Nitroxide Triradicals for Molecular Three-Spin Qubits. Appl Magn Reson 50, 967–976 (2019). https://doi.org/10.1007/s00723-019-01125-9

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  • DOI: https://doi.org/10.1007/s00723-019-01125-9

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