Spin states, vibrations and spin relaxation in molecular nanomagnets and spin qubits: a critical perspective

Chemical Science 9, 3265 - 3275 (2018)

Spin states, vibrations and spin relaxation in molecular nanomagnets and spin qubits: a critical perspective

Luis Escalera-Moreno, José J. Baldoví, Alejandro Gaita-Ariño, Eugenio Coronado

Very recently the closely related fields of molecular spin qubits, single ion magnets and single atom magnets have suffered a convulsion. We have witnessed a jump in the phase memory times of spin qubits from a few microseconds to almost a millisecond in a vanadium complex, magnetic hysteresis up to 60 K in a dysprosium-based magnetic molecule and magnetic memory up to 30 K in a holmium atom deposited on a surface. With single-molecule magnets being more than two decades old, this rapid improvement in the physical properties is surprising and its explanation deserves urgent attention. The general assumption of focusing uniquely on the energy barrier is clearly insufficient to model magnetic relaxation. Other factors, as the vibrations that couple to the spin states, need to be taken into account. In fact, this coupling is currently recognised to be the key factor that accounts for the slow relaxation of the magnetisation at higher temperatures. Herein we will present a critical perspective of the recent advances in molecular nanomagnetism towards the goal of integrating spin-phonon interactions in current computational methodologies of spin relaxation. This presentation will be placed in the context of the well-known models developed in solid state physics, which, as we will explain, are severely limited for molecular systems.

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http://dx.doi.org/10.1039/C7SC05464E

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