Quantum control of electronic fluxes during adiabatic attosecond charge migration in degenerate superposition states of benzene
Quantum control of electronic fluxes during adiabatic attosecond charge migration in degenerate superposition states of benzene
复制标题
DOI：
10.1016/j.chemphys.2016.09.021
复制
发表时间：
2017-01-12
期刊：
影响因子：
2.3
通讯作者：
Yang, Yonggang
中科院分区：
文献类型：
--
作者：
Jia, Dongming;Manz, Jorn;Yang, Yonggang
我们设计了四个线性x-和y-偏振以及圆右（+）和左（）偏振的π/2共振激光脉冲，制备了四个不同简并叠加态的模型苯分子。这些由相等的（0.5）电子基态S-0（（1）A（1g））的人口加上四个简并激发态之一，所有这些都可以通过偶极允许的跃迁。具体地，对于在xy平面中排列的分子，这些激发态包括E-1（1u，x）和E-1（1u，y）简并态的不同复值线性组合。因此，激光脉冲诱导四种不同类型的周期性绝热阿秒（作为）电荷迁移（AACM）在苯中，所有具有相同的周期，504作为，但具有四种不同类型的角通量。这些通量的特征差异之一是零通量的两个角度，其表现为两个等价或近似等价的通量分支的“源”和“汇”的瞬时角位置，所述通量分支以钳形模式从一个分子位点（“源”）流向相对的分子位点（“汇”）。这些零通量的角度或者固定在yz对称平面中的两个相对的碳核的位置处，或者固定在xz对称平面中的两个相对的碳-碳键的中心处，或者零通量的角度分别在角度向前（+）或向后（-）方向上旋转。作为一个恢复，我们的量子模型模拟表明，在AACM过程中的电子通量的量子控制在简并叠加态，在阿秒时域，与激光偏振作为控制的关键旋钮。(C)© 2016 Elsevier B. V.版权所有。
We design four linearly x- and y-polarized as well as circularly right (+) and left () polarized, resonant pi/2-laser pulses that prepare the model benzene molecule in four different degenerate superposition states. These consist of equal (0.5) populations of the electronic ground state S-0((1)A(1g)) plus one of four degenerate excited states, all of them accessible by dipole-allowed transitions. Specifically, for the molecule aligned in the xy-plane, these excited states include different complex-valued linear combinations of the E-1(1u,x) and E-1(1u,y) degenerate states. As a consequence, the laser pulses induce four different types of periodic adiabatic attosecond (as) charge migrations (AACM) in benzene, all with the same period, 504 as, but with four different types of angular fluxes. One of the characteristic differences of these fluxes are the two angles for zero fluxes, which appear as the instantaneous angular positions of the "source" and "sink" of two equivalent, or nearly equivalent branches of the fluxes which flow in pincer-type patterns from one molecular site (the "source") to the opposite one (the "sink"). These angles of zero fluxes are either fixed at the positions of two opposite carbon nuclei in the yz-symmetry plane, or at the centers of two opposite carbon-carbon bonds in the xz-symmetry plane, or the angles of zero fluxes rotate in angular forward (+) or backward (-) directions, respectively. As a resume, our quantum model simulations demonstrate quantum control of the electronic fluxes during AACM in degenerate superposition states, in the attosecond time domain, with the laser polarization as the key knob for control. (C) 2016 Elsevier B.V. All rights reserved.