We present a wave-function based method to solve the time-dependent many-electron Schrödinger equation (TDSE) with special emphasis on strong-field ionization phenomena. The theory builds on the configuration-interaction (CI) approach supplemented by the generalized-active-space (GAS) concept from quantum chemistry. The latter allows for a controllable reduction in the number of configurations in the CI expansion by imposing restrictions on the active orbital space. The method is similar to the recently formulated time-dependent restricted-active-space (TD-RAS) CI method [D. Hochstuhl, and M. Bonitz, Phys. Rev. A 86, 053424 (2012)]. We present details of our implementation and address convergence properties with respect to the active spaces and the associated account of electron correlation in both ground state and excitation scenarios. We apply the TD-GASCI theory to strong-field ionization of polar diatomic molecules and illustrate how the method allows us to uncover a strong correlation-induced shift of the preferred direction of emission of photoelectrons.
Theoretical description of circular dichroism in photoelectron angular distributions of randomly oriented chiral molecules after multi-photon photoionization
光电子圆二色性是指光电子角分布相对于圆偏振光的传播轴的前/后不对称性。最近在随机取向的樟脑和小茴香酮分子的飞秒多光子光电离实验中证实了这一点[C。Lux等人，Angew. Chem.Int.Ed.51，5001（2012）;C. S. Lehmann等人，J. Chem.Phys.139，234307（2013）]。建立了一个理论框架，将这一过程描述为（2+1）共振增强多光子电离，它包括随机取向分子的双光子光选择和光选择分子的连续单光子电离。它结合了光-物质相互作用的微扰理论与从头计算的双光子吸收和单中心扩展的光电子波函数的氢连续函数。验证了该模型正确地再现了在旋向和轻螺旋度交换下预期的基本对称行为。当它应用到茴香酮和樟脑，半定量协议与实验数据被发现，其中一个足够的d波字符的电子激发中间态是至关重要的。
Spin-current correlations in photoionization of chiral molecules
Max-Born-Institut（马克斯·伯恩研究所）；Humboldt University zu Berlin（柏林洪堡大学）；Technion - Israel Institute of Technology（以色列理工学院）；Imperial College London（伦敦帝国理工学院）；Freie Universität Berlin（柏林自由大学）；Technische Universität Berlin（柏林工业大学）
Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule
Shanghai Jiao Tong University（上海交通大学）；RIKEN Center for Interdisciplinary Theoretical and Mathematical Sciences (iTHEMS)（理化学研究所交叉理论数学科学中心（iTHEMS））；RIKEN Center for Computational Science (R-CCS)（理化学研究所计算科学中心（R-CCS））；The University of Tokyo（东京大学）
