T 1 Anisotropy Elucidates Spin Relaxation Mechanisms in an S = 1 Cr(IV) Optically Addressable Molecular Qubit
Nathanael P. Kazmierczak, Kaitlin M. Luedecke, Elisabeth T. Gallmeier +1 more
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 degrees of freedom in an optically addressable S = 1 Cr(IV) molecular qubit. The anisotropy displays a distinct sin2(2θ) functional form that is not observed in S = ½ Cu(II) or V(IV) microwave addressable molecular qubits. The Cr(IV) T1 anisotropy is ascribed to couplings between electron spins and rotational motion in low-energy acoustic or pseudo-acoustic phonons. Our findings suggest that rotational degrees of freedom should be suppressed to maximize the coherence temperature of optically addressable qubits.
The Journal of Physical Chemistry Letters•Aug 21, 2023•30 citations