Core-level spectroscopy of the photodissociation process of BrCN molecule

doi:10.1088/1674-1056/ad0cc9

中国物理B ›› 2024, Vol. 33 ›› Issue (1): 18702-18702.doi: 10.1088/1674-1056/ad0cc9

所属专题： SPECIAL TOPIC — States and new effects in nonequilibrium

Core-level spectroscopy of the photodissociation process of BrCN molecule

Kun Zhou(周坤)^1,2 and Han Wang(王涵)^1,2,†

1 School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China;
2 Center for Transformative Science, ShanghaiTech University, Shanghai 201210, China

收稿日期:2023-08-23 修回日期:2023-11-09 接受日期:2023-11-16 出版日期:2023-12-13 发布日期:2024-01-03
通讯作者: Han Wang E-mail:wanghan3@shanghaitech.edu.cn
基金资助:
g H. W. and K. Z. were supported by the start-up funding of ShanghaiTech University in China. This work was also supported by a user project at the Molecular Foundry (LBNL) and its computing resources administered by the HighPerformance Computing Services Group at LBNL. Work at the Molecular Foundry was supported by the Office of Science and Office of Basic Energy Sciences of the U.S. Department of Energy (Grant No. DE-AC02-05CH11231). This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U. S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory (Grant No. DE-AC02-05CH11231). This work was also supported by the High-Performance Computing (HPC) Platform of ShanghaiTech University. We would like to thank Jingxiang Zou for the discussion of NTO analysis.

Core-level spectroscopy of the photodissociation process of BrCN molecule

Kun Zhou(周坤)^1,2 and Han Wang(王涵)^1,2,†

1 School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China;
2 Center for Transformative Science, ShanghaiTech University, Shanghai 201210, China

Received:2023-08-23 Revised:2023-11-09 Accepted:2023-11-16 Online:2023-12-13 Published:2024-01-03
Contact: Han Wang E-mail:wanghan3@shanghaitech.edu.cn
Supported by:
g H. W. and K. Z. were supported by the start-up funding of ShanghaiTech University in China. This work was also supported by a user project at the Molecular Foundry (LBNL) and its computing resources administered by the HighPerformance Computing Services Group at LBNL. Work at the Molecular Foundry was supported by the Office of Science and Office of Basic Energy Sciences of the U.S. Department of Energy (Grant No. DE-AC02-05CH11231). This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U. S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory (Grant No. DE-AC02-05CH11231). This work was also supported by the High-Performance Computing (HPC) Platform of ShanghaiTech University. We would like to thank Jingxiang Zou for the discussion of NTO analysis.

1. 2024-018702-SI.pdf(402KB)

摘要/Abstract

摘要： Fewest-switches surfacing hopping (FSSH) simulations have been performed with the high-level multi-reference electronic structure method to explore the coupled electronic and nuclear dynamics upon photoexcitation of cyanogen bromide (BrCN). The potential energy surfaces (PES) of BrCN are charted as functions of the Jacobi coordinates (R, θ). An in-depth examination of the FSSH trajectories reveals the temporal dynamics of the molecule and the population changes of the lowest twelve states during BrCN's photodissociation process, which presents a rich tapestry of dynamical information. Furthermore, the carbon K-edge x-ray absorption spectroscopy (XAS) is calculated with multi-reference inner-shell spectral simulations. The rotation of the CN fragment and the elongation of the C—Br bond are found to be the reason for the peak shifting in the XAS. Our findings offer a nuanced interpretation for inner-shell probe investigations of BrCN, setting the stage for a deeper understanding of the photodissociation process of cyanogen halides molecules.

关键词: x-ray absorption spectroscopy, photodissociation, fewest-switches surface hopping

Abstract: Fewest-switches surfacing hopping (FSSH) simulations have been performed with the high-level multi-reference electronic structure method to explore the coupled electronic and nuclear dynamics upon photoexcitation of cyanogen bromide (BrCN). The potential energy surfaces (PES) of BrCN are charted as functions of the Jacobi coordinates (R, θ). An in-depth examination of the FSSH trajectories reveals the temporal dynamics of the molecule and the population changes of the lowest twelve states during BrCN's photodissociation process, which presents a rich tapestry of dynamical information. Furthermore, the carbon K-edge x-ray absorption spectroscopy (XAS) is calculated with multi-reference inner-shell spectral simulations. The rotation of the CN fragment and the elongation of the C—Br bond are found to be the reason for the peak shifting in the XAS. Our findings offer a nuanced interpretation for inner-shell probe investigations of BrCN, setting the stage for a deeper understanding of the photodissociation process of cyanogen halides molecules.

Key words: x-ray absorption spectroscopy, photodissociation, fewest-switches surface hopping

中图分类号: (Ultrafast dynamics; charge transfer)

87.15.ht

78.70.Dm (X-ray absorption spectra) 31.50.Df (Potential energy surfaces for excited electronic states) 33.20.-t (Molecular spectra)

Kun Zhou(周坤) and Han Wang(王涵). Core-level spectroscopy of the photodissociation process of BrCN molecule[J]. 中国物理B, 2024, 33(1): 18702-18702.

Kun Zhou(周坤) and Han Wang(王涵). Core-level spectroscopy of the photodissociation process of BrCN molecule[J]. Chin. Phys. B, 2024, 33(1): 18702-18702.

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Core-level spectroscopy of the photodissociation process of BrCN molecule

Core-level spectroscopy of the photodissociation process of BrCN molecule

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