Dodin Amro, Tscherbul Timur V, Brumer Paul
Chemical Physics Theory Group, Department of Chemistry, and Center for Quantum Information and Quantum Control, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
Department of Physics, University of Nevada, Reno, Nevada 89557, USA.
J Chem Phys. 2016 Dec 28;145(24):244313. doi: 10.1063/1.4972140.
Light-induced processes in nature occur by irradiation with slowly turned-on incoherent light. The general case of time-dependent incoherent excitation is solved here analytically for V-type systems using a newly developed master equation method. Clear evidence emerges for the disappearance of radiatively induced coherence as turn-on times of the radiation exceed characteristic system times. The latter is the case, in nature, for all relevant dynamical time scales for other than nearly degenerate energy levels. We estimate that, in the absence of non-radiative relaxation and decoherence, turn-on times slower than 1 ms (still short by natural standards) only induce Fano coherences between energy eigenstates that are separated by less than 0.9 cm.
自然界中的光诱导过程是通过用缓慢开启的非相干光照射来实现的。这里使用一种新开发的主方程方法,对V型系统解析求解了随时间变化的非相干激发的一般情况。随着辐射开启时间超过特征系统时间,辐射诱导的相干性消失的明显证据出现了。在自然界中,除了近简并能级外,对于所有相关的动力学时间尺度都是这种情况。我们估计,在没有非辐射弛豫和退相干的情况下,开启时间慢于1毫秒(按照自然标准仍然很短)只会在能量本征态之间诱导出分离小于0.9厘米的法诺相干。