Modeling the heating and cooling of a chromophore after photoexcitation

Autor: Silmar Do monte, Mario Barbatti, Elizete Ventura do Monte, Josene M. Toldo, Mariana Telles do Casal, José Maximiano Pinheiro
Přispěvatelé: Federal University of Paraíba (UFPB), Institut de Chimie Radicalaire (ICR), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.)
Rok vydání: 2022
Předmět:
Zdroj: Physical Chemistry Chemical Physics
Physical Chemistry Chemical Physics, In press, ⟨10.1039/d2cp00686c⟩
Phys. Chem. Chem. Phys.
ISSN: 9403-9410
1463-9076
1463-9084
Popis: The heating of a chromophore due to internal conversion and its cooling down due to energy dissipation to the solvent are crucial phenomena to characterize molecular photoprocesses. In this work, we simulated the ab initio nonadiabatic dynamics of cytosine, a prototypical chromophore undergoing ultrafast internal conversion, in three solvents-argon matrix, benzene, and water-spanning an extensive range of interactions. We implemented an analytical energy-transfer model to analyze these data and extract heating and cooling times. The model accounts for nonadiabatic effects, and excited- and ground-state energy transfer, and can analyze data from any dataset containing kinetic energy as a function of time. Cytosine heats up in the subpicosecond scale and cools down within 25, 4, and 1.3 ps in argon, benzene, and water, respectively. The time constants reveal that a significant fraction of the benzene and water heating occurs while cytosine is still electronically excited. ispartof: PHYSICAL CHEMISTRY CHEMICAL PHYSICS vol:24 issue:16 pages:9403-9410 ispartof: location:England status: published
Databáze: OpenAIRE