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Quantum tunneling of magnetization in molecular spin

Le Tuan Anh HoLiviu UngurLiviu F. Chibotaru
Dec 2022
摘要
We examine the quantum tunneling of magnetization in molecular spin in weakinteraction with a bath subject to Redfield master equation. By designing amicroscopic model for a multilevel spin system using only a generic Hamiltonianand applying stationary approximation for excited doublets/singlets, we derivea key equation of motion for the quantum tunneling of magnetization processwhich is applicable in the whole temperature domain. From this equation, wefind that in general three tunneling rates are needed to accurately describethe quantum tunneling process. More importantly, behavior of the quantumtunneling in the intermediate temperature domain where there exists atransition between incoherent and coherent quantum tunneling is also unraveledfor the first time. Limiting cases at low and high temperature and/or lowmagnetic field are also worked out where some popular well-known results arereproduced. Last but not least, a new interpretation of the quantum tunnelingof magnetization is proposed where we reveal the similarity between thisrelaxation process with a driven damped harmonic oscillator.
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