Photoexcited dynamics of the valence states of norbornadiene
The non-radiative decay of photoexcited norbornadiene, which together with its isomer quadricyclane forms a molecular photoswitch, is investigated using surface-hopping non-adiabatic dynamics. The simulations are performed using four levels of electronic structure theory: CASSCF(2,2), CASSCF(4,4), XMS-CASPT2(2,2), and XMS-CASPT2(4,4)…
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Including Photoexcitation Explicitly in Trajectory-Based Nonadiabatic Dynamics at No Cost
Over the last decades, theoretical photochemistry has produced multiple techniques to simulate the nonadiabatic dynamics of molecules. Surprisingly, much less effort has been devoted to adequately describing the first step of a photochemical or photophysical process: photoexcitation…
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Predicting the photodynamics of cyclobutanone triggered by a laser pulse at 200 nm and its MeV-UED signals—A trajectory surface hopping and XMS-CASPT2 perspective
- Jiří Janoš, Joao Pedro Figueira Nunes, Daniel Hollas, Petr Slavíček and Basile F. E. Curchod
- Publication , Prediction challenge
This work is part of a prediction challenge that invited theoretical/computational chemists to predict the photochemistry of cyclobutanone in the gas phase, excited at 200 nm by a laser pulse, and the expected signal that will be recorded during a time-resolved megaelectronvolt ultrafast electron diffraction (MeV-UED). We present here our theoretical predictions…
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Monitoring the Evolution of Relative Product Populations at Early Times during a Photochemical Reaction
Identifying multiple rival reaction products and transient species formed during ultrafast photochemical reactions and determining their time-evolving relative populations are key steps toward understanding and predicting photochemical outcomes. Yet, most contemporary ultrafast studies struggle with clearly identifying and quantifying competing molecular structures/species among the emerging reaction products…
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