Rivlin Tom, Pollak Eli
Chemical and Biological Physics Department, Weizmann Institute of Science, 76100Rehovot, Israel.
J Phys Chem Lett. 2022 Nov 17;13(45):10558-10566. doi: 10.1021/acs.jpclett.2c03008. Epub 2022 Nov 7.
Quantum tunneling is known to play an important role in the dynamics of systems with nonadiabatic couplings. However, until recently, the time-domain properties of nonadiabatic scattering have been severely under-explored. Using numerically exact quantum methods, we study the impact that nonadiabatic couplings have on the time it takes to tunnel through a barrier. We find that the Wigner phase time is the appropriate measure to use when determining the tunneling flight time also when considering nonadiabatic systems. The central result of the present study is that in an avoided crossing system in one dimension, the nonadiabatic couplings speed up the tunneling event, relative to the adiabatic case in which all nonadiabatic coupling is ignored. This has implications for both the study of quantum tunneling times and for the field of nonadiabatic scattering and chemistry.
众所周知，量子隧穿在具有非绝热耦合的系统动力学中起着重要作用。然而，直到最近，非绝热散射的时域特性仍未得到充分研究。我们使用数值精确的量子方法，研究非绝热耦合对隧穿势垒所需时间的影响。我们发现，即使在考虑非绝热系统时，维格纳相时间也是确定隧穿飞行时间时合适的度量。本研究的核心结果是，在一维的避免交叉系统中，相对于忽略所有非绝热耦合的绝热情况，非绝热耦合会加速隧穿事件。这对量子隧穿时间的研究以及非绝热散射和化学领域都有影响。
