Dissociative electron attachment to 5-bromo-uracil : non-adiabatic dynamics on complex-valued potential energy surfaces
Lucas M. Cornetta, Todd J. Martinez and Marcio T. do N. Varella
ARTIGO
Inglês
Agradecimentos: L. M. C. acknowledges financial support from São Paulo Research Foundation (FAPESP), under grants No. 2015/17273-5 and No. 2018/02257-2, and HPC-USP. M. T. do N. V. acknowledges financial support from Brazilian National Council for Scientific and Technological Development (CNPq),...
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Agradecimentos: L. M. C. acknowledges financial support from São Paulo Research Foundation (FAPESP), under grants No. 2015/17273-5 and No. 2018/02257-2, and HPC-USP. M. T. do N. V. acknowledges financial support from Brazilian National Council for Scientific and Technological Development (CNPq), under grant No. 304571/2018-0. This work was partially supported by the AMOS program of the U.S. Department of Energy
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Abstract: 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...
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Abstract: 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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FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULO - FAPESP
2015/17273-5; 2018/02257-2
CONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICO - CNPQ
304571/2018-0
Fechado
Cornetta, Lucas Medeiros
Autor
Dissociative electron attachment to 5-bromo-uracil : non-adiabatic dynamics on complex-valued potential energy surfaces
Lucas M. Cornetta, Todd J. Martinez and Marcio T. do N. Varella
Dissociative electron attachment to 5-bromo-uracil : non-adiabatic dynamics on complex-valued potential energy surfaces
Lucas M. Cornetta, Todd J. Martinez and Marcio T. do N. Varella
Fontes
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Physical chemistry chemical physics Vol. 24, n. 11 (Mar., 2022), p. 6845-6855 |