HORTENSIA：一个用于模拟分子中非绝热自电离动力学的程序包
HORTENSIA, a program package for the simulation of nonadiabatic autoionization dynamics in molecules
AI总结：
本文介绍 HORTENSIA 程序包，它基于非绝热表面跳跃并结合量子化学接口，模拟分子阴离子的振动诱导自电离，输出时间与角度分辨的电子动能谱及几何分析工具。
摘要：
我们提出了一个程序包，用于在绝热阴离子态流形和离散化电离连续谱中模拟分子阴离子中超快的振动诱导自电离动力学。该程序名为 HORTENSIA（Hopping real-time trajectories for electron-ejection by nonadiabatic self-ionization in anions，即阴离子中非绝热自电离导致电子射出的跳跃实时轨迹），基于非绝热表面跳跃方法；在该方法中，原子核作为一个系综，沿经典轨迹在由分子体系电子密度产生的量子力学势中传播。电子 Schrödinger 方程沿轨迹进行数值积分，给出电子态系数的时间演化，并由此确定向离散电子态的切换概率。对于离散化连续谱态，这种跳跃事件被解释为一个电子的射出。含时电子 Schrödinger 方程中导出的 diabatic（透热）耦合和非绝热耦合，由阴离子和中性波函数计算得到；这些波函数来自与我们程序相接口的商用程序包所执行的量子化学计算。基于这一方法，我们展示了对同时具有时间分辨和角度分辨的自电离电子动能谱的模拟。此外，该程序生成的数据可方便地依据键长、键角等几何特征加以解释，从而有助于识别对自电离过程重要的分子构型。而且，程序还包含实用的扩展功能，即用于生成初始条件和输入文件、以及评估输出文件的工具；这些工具既可通过控制台命令使用，也可通过图形用户界面使用。
英文摘要：
We present a program package for the simulation of ultrafast vibration-induced autoionization dynamics in molecular anions in the manifold of the adiabatic anionic states and the discretized ionization continuum. This program, called HORTENSIA ($\underline{Ho}$pping $\underline{r}$eal-time $\underline{t}$rajectories for $\underline{e}$lectron-ejection by $\underline{n}$onadiabatic $\underline{s}$elf-$\underline{i}$onization in $\underline{a}$nions), is based on the nonadiabatic surface-hopping methodology, wherein nuclei are propagated as an ensemble along classical trajectories in the quantum-mechanical potential created by the electronic density of the molecular system. The electronic Schrödinger equation is numerically integrated along the trajectory, providing the time evolution of electronic state coefficients, from which switching probabilities into discrete electronic states are determined. In the case of a discretized continuum state, this hopping event is interpreted as the ejection on an electron. The derived diabatic and nonadiabatic couplings in the time-dependent electronic Schrödinger equation are calculated from anionic and neutral wavefunctions obtained from quantum chemical calculations with commercially available program packages interfaced with our program. Based on this methodology, we demonstrate the simulation of autoionization electron kinetic energy spectra that are both time- and angle-resolved. In addition, the program yields data that can be interpreted easily with respect to geometric characteristics such as bonding distances and angles, which facilitates the detection of molecular configurations important for the autoionization process. Moreover, useful extensions are included, namely generation tools for initial conditions and input files as well as for the evaluation of output files both through console commands and a graphical user interface.
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