TY - JOUR

T1 - EPR and DEER Characterization of New Mixed Weakly Coupled Nitroxide Triradicals for Molecular Three-Spin Qubits

AU - Zaytseva, Elena

AU - Timofeev, Ivan

AU - Krumkacheva, Olesya

AU - Parkhomenko, Dmitryi

AU - Mazhukin, Dmitrii

AU - Sato, Kazunobu

AU - Matsuoka, Hideto

AU - Takui, Takeji

AU - Bagryanskaya, Elena

N1 - Publisher Copyright: © 2019, Springer-Verlag GmbH Austria, part of Springer Nature.

PY - 2019/8/1

Y1 - 2019/8/1

N2 - Three new mixed triradicals with small exchange coupling parameters (J ≪ A N ) 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.

AB - Three new mixed triradicals with small exchange coupling parameters (J ≪ A N ) 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.

KW - ELECTRON RESONANCE TRIER

KW - DISTANCE MEASUREMENTS

KW - PULSED ELECTRON

KW - SERIES

KW - ELDOR

UR - http://www.scopus.com/inward/record.url?scp=85065028192&partnerID=8YFLogxK

U2 - 10.1007/s00723-019-01125-9

DO - 10.1007/s00723-019-01125-9

M3 - Article

AN - SCOPUS:85065028192

VL - 50

SP - 967

EP - 976

JO - Applied Magnetic Resonance

JF - Applied Magnetic Resonance

SN - 0937-9347

IS - 8

ER -