Ab Initio Multiple Spawning Nonadiabatic Dynamics with Different CASPT2 Flavors: A Fully Open-Source PySpawn/OpenMolcas Interface,Journal of Chemical Theory and Computation

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Ab Initio Multiple Spawning Nonadiabatic Dynamics with Different CASPT2 Flavors: A Fully Open-Source PySpawn/OpenMolcas Interface
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2024-09-04 , DOI: 10.1021/acs.jctc.4c00855
Lea M Ibele ₁ , Arshad Memhood ₂ , Benjamin G Levine ₂ , Davide Avagliano ₃

Affiliation

We introduce an interface between PySpawn, a simulation package to run ab initio multiple spawning (AIMS) nonadiabatic dynamics, and OpenMolcas, a software package to perform multiconfigurational perturbations theory (CASPT2) electronic structure calculations. Our interface allows us to exploit all the functionalities of the two codes: the modular and efficient Python implementation of the AIMS algorithm and the extensive analysis tools offered by PySpawn, with the cutting-edge implementation of CASPT2 equations in OpenMolcas, including the recently introduced analytical gradients and different flavors. Both are fully open-source and free of charge, making the following implementation unique in the current plethora of software for nonadiabatic dynamics. This represents an important step toward a wider application of AIMS-based nonadiabatic dynamics combined with high-accuracy excited-state calculations. The importance and the need for such an implementation are demonstrated by application to the ultrafast relaxation of fulvene from S₁ to S₀, which is drastically affected by the potential energy surface on which the nuclear wavepacket is propagated. Additionally, the decay is influenced by the CASPT2 flavor adopted, posing interesting questions in the choice of one over the other and opening the door to deeper studies on the effect of CASPT2 formulations in nonadiabatic dynamics.

中文翻译：

具有不同 CASPT2 风格的从头算多重生成非绝热动力学：完全开源的 PySpawn/OpenMolcas 接口

我们引入了 PySpawn 和 OpenMolcas 之间的接口。PySpawn 是一个用于运行从头多重生成 (AIMS) 非绝热动力学的模拟软件包，而 OpenMolcas 是一个用于执行多配置扰动理论 (CASPT2) 电子结构计算的软件包。我们的界面使我们能够利用这两个代码的所有功能：AIMS 算法的模块化且高效的 Python 实现以及 PySpawn 提供的广泛分析工具，以及 OpenMolcas 中 CASPT2 方程的前沿实现，包括最近引入的分析渐变和不同的口味。两者都是完全开源且免费的，使得以下实现在当前众多非绝热动力学软件中独一无二。这代表着基于 AIMS 的非绝热动力学与高精度激发态计算的更广泛应用迈出了重要一步。这种实现的重要性和必要性通过应用于富烯从S ₁到S ₀的超快弛豫来证明，这极大地受到核波包在其上传播的势能表面的影响。此外，衰减受到所采用的 CASPT2 风格的影响，在选择一种而不是另一种时提出了有趣的问题，并为更深入地研究 CASPT2 配方在非绝热动力学中的影响打开了大门。

更新日期：2024-09-04

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