CNR-ISM, Division of Ultrafast Processes in Materials (FLASHit) , Area della Ricerca di Roma 1 , Via Salaria Km 29.3 , I-00016 Monterotondo Scalo , Italy.
Dipartimento di Fisica , Università di Roma Tor Vergata , Via della Ricerca Scientifica 1 , 00133 Rome , Italy.
J Chem Theory Comput. 2019 Aug 13;15(8):4526-4534. doi: 10.1021/acs.jctc.9b00170. Epub 2019 Jul 31.
We investigate the photoinduced ultrafast charge migration phenomenon in the glycine molecule using a recently proposed nonequilibrium Green's functions (NEGF) approach. We first consider the dynamics resulting from the sudden removal of an electron in the valence shells, finding a satisfactory agreement with available data. Then we explicitly simulate the laser-induced photoionization process and study the evolution of the system after the pulse. We disentangle polarization and correlation effects in the electron dynamics and assign the main frequencies to specific elements of the reduced one-particle density matrix. We show that electronic correlations renormalize the bare frequencies, redistribute the spectral weights, and give rise to new spectral features.
我们使用最近提出的非平衡格林函数（NEGF）方法研究甘氨酸分子中的光诱导超快电荷迁移现象。我们首先考虑价壳层中电子突然被移除所导致的动力学，发现与现有数据有令人满意的一致性。然后我们明确模拟了激光诱导的光致电离过程，并研究了脉冲后的系统演化。我们在电子动力学中分离了极化和相关效应，并将主要频率分配给简并单粒子密度矩阵的特定元素。我们表明，电子相关将基本频率正规化，重新分配谱权重，并产生新的谱特征。
