Including Photoexcitation Explicitly in Trajectory-Based Nonadiabatic Dynamics at No Cost

Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60461373%3A22340%2F24%3A43930961" target="_blank" >RIV/60461373:22340/24:43930961 - isvavai.cz</a>
Result on the web
<a href="https://pubs.acs.org/doi/10.1021/acs.jpclett.4c02549" target="_blank" >https://pubs.acs.org/doi/10.1021/acs.jpclett.4c02549</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1021/acs.jpclett.4c02549" target="_blank" >10.1021/acs.jpclett.4c02549</a>

Result language
angličtina
Original language name
Including Photoexcitation Explicitly in Trajectory-Based Nonadiabatic Dynamics at No Cost
Original language description
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. Here, we propose a formalism to include the effect of a laser pulse in trajectory-based nonadiabatic dynamics at the level of the initial conditions, with no additional cost. The promoted density approach (PDA) decouples the excitation from the nonadiabatic dynamics by defining a new set of initial conditions, which include an excitation time. PDA with surface hopping leads to nonadiabatic dynamics simulations in excellent agreement with quantum dynamics using an explicit laser pulse and highlights the strong impact of a laser pulse on the resulting photodynamics and the limits of the (sudden) vertical excitation. Combining PDA with trajectory-based nonadiabatic methods is possible for any arbitrary-sized molecules using a code provided in this work. © 2024 The Authors. Published by American Chemical Society.
Czech name
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Czech description
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Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)

Project
<a href="/en/project/GA23-07066S" target="_blank" >GA23-07066S: Time-dependent simulations for time-resolved electronic spectroscopies</a><br>
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Publication year
2024
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

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