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Critical Appraisal of Excited-State Nonadiabatic Dynamics Simulations of 9H-Adenine

MPG-Autoren
http://pubman.mpdl.mpg.de/cone/persons/resource/persons58410

Barbatti,  Mario
Research Group Barbatti, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons58496

Crespo Otero,  Rachel
Research Group Barbatti, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons59045

Thiel,  Walter
Research Department Thiel, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Zitation

Barbatti, M., Lan, Z., Crespo Otero, R., Szymczak, J., Lischka, H., & Thiel, W. (2012). Critical Appraisal of Excited-State Nonadiabatic Dynamics Simulations of 9H-Adenine. The Journal of Chemical Physics, 137(22): 22A503, pp. 1-14. doi:10.1063/1.4731649.


Zitierlink: http://hdl.handle.net/11858/00-001M-0000-000E-E6BA-F
Zusammenfassung
In spite of the importance of nonadiabatic dynamics simulations for the understanding of ultrafast photo-induced phenomena, simulations based on different methodologies have often led to contradictory results. In this work, we proceed through a comprehensive investigation of on-the-fly surface-hopping simulations of 9H-adenine in the gas phase using different electronic structure theories (ab initio, semi-empirical, and density functional methods). Simulations that employ ab initio and semi-empirical multireference configuration interaction methods predict the experimentally observed ultrafast deactivation of 9H-adenine with similar time scales, however, through different internal conversion channels. Simulations based on time-dependent density functional theory with six different hybrid and range-corrected functionals fail to predict the ultrafast deactivation. The origin of these differences is analyzed by systematic calculations of the relevant reaction pathways, which show that these discrepancies can always be traced back to topographical features of the underlying potential energy surfaces.