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- W4386021945 abstract "Paramagnetic molecules offer unique advantages for quantum information science owing to their spatial compactness, synthetic tunability, room-temperature quantum coherence, and potential for optical state initialization and readout. However, current optically addressable molecular qubits are hampered by rapid spin-lattice relaxation (T1) even at sub-liquid nitrogen temperatures. Here, we use temperature- and orientation-dependent pulsed electron paramagnetic resonance (EPR) to elucidate the negative sign of the ground state zero-field splitting (ZFS) and assign T1 anisotropy to specific types of motion in an optically addressable S = 1 Cr(o-tolyl)4 molecular qubit. The anisotropy displays a distinct sin2(2θ) functional form that is not observed in S = 1/2 Cu(acac)2 or other Cu(II)/V(IV) microwave addressable molecular qubits. The Cr(o-tolyl)4T1 anisotropy is ascribed to couplings between electron spins and rotational motion in low-energy acoustic or pseudoacoustic phonons. Our findings suggest that rotational degrees of freedom should be suppressed to maximize the coherence temperature of optically addressable qubits." @default.
- W4386021945 created "2023-08-22" @default.
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- W4386021945 date "2023-08-21" @default.
- W4386021945 modified "2023-09-26" @default.
- W4386021945 title "<i>T</i><sub>1</sub> Anisotropy Elucidates Spin Relaxation Mechanisms in an <i>S</i> = 1 Cr(IV) Optically Addressable Molecular Qubit" @default.
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- W4386021945 doi "https://doi.org/10.1021/acs.jpclett.3c01964" @default.
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