pyHRSOA and pyTHSOA: Postprocessing Codes for the Computation of Second and Third-Order Scattering Optical Activities

IF 4.8 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Journal of Computational Chemistry Pub Date : 2025-06-25 DOI:10.1002/jcc.70149

Andrea Bonvicini, Benoît Champagne

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引用次数: 0

Abstract

We present pyHRSOA and pyTHSOA, two postprocessing Python codes for the computation of the circular differential scattering ratio, a dimensionless quantity which is the central observable for two novel and promising nonlinear chiroptical techniques: the hyper-Rayleigh scattering optical activity (HRS-OA) and the third-harmonic scattering optical activity (THS-OA) spectroscopies. From a computational point of view, the simulation of the HRS-OA (THS-OA) spectroscopy requires the calculations of five first (second) hyperpolarizabilities and these can be obtained from quadratic (cubic) responses functions by using the DALTON quantum chemistry software. However, the expressions for the chiral and achiral contributions to the scattered intensities are quite complicated because these contain a lot of terms. In particular, for HRS-OA and THS-OA 30 and 46 molecular invariants need to be computed, thus complicating their computational implementation. The postprocessing codes presented here can be used as black-box tools for the simulations of HRS-OA and THS-OA spectroscopies. The source codes are available at https://gitlab.unamur.be/abonvici/pyhrsoa_pythsoa (DOI 10.5281/zenodo.15424494).

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pyHRSOA和pyTHSOA：计算二阶和三阶散射光学活度的后处理代码

我们提出了pyHRSOA和pyTHSOA，两个用于计算圆微分散射比的后处理Python代码，圆微分散射比是两种新的和有前途的非线性光学技术：超瑞利散射光学活度（HRS-OA）和三次谐波散射光学活度（THS-OA）光谱的中心观测量。从计算的角度来看，HRS-OA （THS-OA）光谱学的模拟需要计算5个一（秒）超极化率，这些超极化率可以使用DALTON量子化学软件从二次（三次）响应函数中得到。然而，手性和非手性对散射强度的贡献的表达式非常复杂，因为它们包含很多项。特别是，对于hr - oa和hs - oa，需要计算30和46个分子不变量，从而使其计算实现变得复杂。本文提出的后处理代码可以作为模拟hs - oa和hs - oa光谱的黑盒工具。源代码可从https://gitlab.unamur.be/abonvici/pyhrsoa_pythsoa （DOI 10.5281/zenodo.15424494）获得。

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来源期刊

Journal of Computational Chemistry 化学-化学综合

CiteScore

6.60

自引率

3.30%

发文量

247

审稿时长

1.7 months

期刊介绍： This distinguished journal publishes articles concerned with all aspects of computational chemistry: analytical, biological, inorganic, organic, physical, and materials. The Journal of Computational Chemistry presents original research, contemporary developments in theory and methodology, and state-of-the-art applications. Computational areas that are featured in the journal include ab initio and semiempirical quantum mechanics, density functional theory, molecular mechanics, molecular dynamics, statistical mechanics, cheminformatics, biomolecular structure prediction, molecular design, and bioinformatics.