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Exploring photoexcitation-induced dynamic evolution of the small molecule activation at point defects

Objective

"For the photocatalytic reduction of inert small molecules using nanomaterials, surface point defects (such as vacancies and heteroatoms) play an important regulatory role. In particular, promoting the activation of adsorbed molecules is directly related to the subsequent multi-step reaction. Traditional simulations mainly focus on the relationship between the ground state fixation model and activation, while ignoring the exploration of the influence of dynamic evolution of defects and molecules on the activation process in the photoexcitation environment. Through the combination of first-principles, many-body perturbation theory, ab initio nonadiabatic molecular dynamics, and experimental verification, we will explore the dynamic evolution and the mechanism of the adsorbed molecule activation process at point defects under photoexcitation. 1) We will study the relaxation process of photogenerated hot electrons at point defects, analyze the formation and evolution of transient and vibrationally excited states of adsorbed molecules, and expand the static activation based on the conventional ""acceptance-donation"" mechanism. Simultaneously, by exploring the spin state transition and exciton effect at the point defects, we will reveal their effects on the lifetime of molecular dynamic activation intermediates. 2) By studying the dynamic evolution of point defects under molecular adsorption and photoexcitation, we will clarify the regulatory effect of point defects in semi-stable states on the evolution of adsorbed molecular excited states. 3) We will explore the effect of liquid-solid interfaces on the dynamic activation process of small molecules under photoexcitation. The implementation of this project will help resolve many contradictions between the static mechanism and the experimental results, and it will provide a reliable theoretical basis for the photocatalytic performance optimization of point defects."

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Coordinator

TECHNISCHE UNIVERSITAET DRESDEN
Net EU contribution
€ 217 965,12
Address
HELMHOLTZSTRASSE 10
01069 Dresden
Germany

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Region
Sachsen Dresden Dresden, Kreisfreie Stadt
Activity type
Higher or Secondary Education Establishments
Links
Total cost
No data