期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 24, 期 11, 页码 6845-6855出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cp05663h
关键词
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资金
- Sao Paulo Research Foundation (FAPESP) [2015/172735, 2018/02257-2]
- HPC-USP
- Brazilian National Council for Scientific and Technological Development (CNPq) [304571/2018-0]
- AMOS program of the U.S. Department of Energy
Electron induced dissociation reactions play a significant role in various fields. However, simulating dissociation electron attachment (DEA) dynamics is challenging. In this study, a modified AIMS method was proposed to simulate the DEA dynamics of 5-bromouracil, successfully considering all vibrational modes.
Electron induced dissociation reactions are relevant to many fields, ranging from prebiotic chemistry to cancer treatments. However, the simulation of dissociation electron attachment (DEA) dynamics is very challenging because the auto-ionization widths of the transient negative ions must be accounted for. We propose an adaptation of the ab initio multiple spawning (AIMS) method for complex-valued potential energy surfaces, along the lines of recent developments based on surface hopping dynamics. Our approach combines models for the energy dependence of the auto-ionization widths, obtained from scattering calculations, with survival probabilities computed for the trajectory basis functions employed in the AIMS dynamics. The method is applied to simulate the DEA dynamics of 5-bromouracil in full dimensionality, i.e., taking all the vibrational modes into consideration. The propagation starts on the pi(2)* resonance state and describes the formation of Br- anions mediated by non-adiabatic couplings. The potential energies, gradients and non-adiabatic couplings were computed with the fractional-occupancy molecular orbital complete-active-space configuration-interaction method, and the calculated DEA cross section are consistent with the observed DEA intensities.
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