We present the implementation of an electronic-structure approach dedicated to ionization dynamics of molecules interacting with x-ray free-electron laser (XFEL) pulses. In our scheme, molecular orbitals for molecular core-hole states are represented by linear combination of numerical atomic orbitals that are solutions of corresponding atomic core-hole states. We demonstrate that our scheme efficiently calculates all possible multiple-hole configurations of molecules formed during XFEL pulses. The present method is suitable to investigate x-ray multiphoton multiple ionization dynamics and accompanying nuclear dynamics, providing essential information on the chemical dynamics relevant for high-intensity x-ray imaging.
Correlation effects in strong-field ionization of heteronuclear diatomic molecules
我们发展了一个含时理论来研究强激光场作用下双原子分子的电子动力学和光电离过程，包括电子-电子关联效应。我们结合最近提出的含时广义活性空间组态相互作用理论[D。Hochstuhl和M. Bonitz，Phys.Rev.A86，053424（2012）; S. Bauch等人，Phys.Rev.A90，062508（2014）]，其具有包括局域轨道和连续态的长球形基组以描述束缚电子和传出光电子。作为例子，我们研究了双中心四电子氢化锂分子在不同强度区域的强场电离。利用单周期脉冲，研究了非对称异质结分子的两种取向：Li-H（电场从H指向Li）和H-Li（电场从H指向Li）。确定了电离的优选取向，并且我们发现从低强度的H-Li到高强度的Li-H的过渡。在不同的近似水平的电子相关性的影响进行了研究，我们发现一个显着的变化的优先取向。对于某些强度制度，甚至互换的首选配置观察，相对于不相关的模拟。进一步的洞察力提供了详细的光电子角分布的比较，并考虑到相关效应。
The use of fast molecular descriptors and artificial neural networks approach in organochlorine compounds electron ionization mass spectra classification
A Low Cost Relativistic Algebraic Diagrammatic Construction Method Based on Cholesky Decomposition and Frozen Natural Spinors for Electronic Ionization, Attachment and Excitation Energy Problem
