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New Insights into Nonadiabatic Dynamics of Molecules at Metal Surfaces
A groundbreaking study has introduced an innovative method aimed at accurately modeling electron transfer processes that are pivotal in nonadiabatic dynamics involving molecules at metal surfaces. The findings are detailed in an article published in Physical Review Letters.
Nonadiabatic energy transfer phenomena have been observed across a variety of interfacial processes, making the investigation of these transfers essential for a deeper understanding of key areas such as chemical adsorption, electrochemistry, and plasmonic catalysis.
Interactions between molecules and metal surfaces often result in a complex interplay of molecular vibrations, rotations, translations, and their coupling with surface phonons and electrons. While traditional models that rely on electronic friction have contributed to this field, they often fail to encapsulate the intricate energy transfer dynamics seen in experimental settings.
To address these challenges, a research team led by Prof. Jiang Bin from the University of Science and Technology of China has developed a novel simulation framework that examines the energy transfer dynamics of carbon monoxide (CO) molecules as they interact with AU(111) surfaces. The team’s approach began with the calculation of charge-transfer states across various configurations of CO molecules at the metal interface, utilizing constrained density functional theory (CDFT).
The team then employed an embedded atom neural network (EANN) to efficiently learn the CDFT energies, facilitating the generation of high-dimensional diabatic potential energy surfaces (PESs). The simulation culminated in the application of the independent electron surface hopping (IESH) method to accurately replicate the energy transfer processes.
The results from this advanced simulation strategy demonstrated remarkable alignment with experimental data, particularly regarding the vibrational final state distribution of highly vibrationally excited CO (with an initial vibrational state of vi=17) following scattering events. Additionally, the simulation outcomes accurately illustrated the vibrational relaxation probabilities, mean translational energies, and scattering angle distributions for CO molecules exhibiting lower vibrational excitation (vi=2).
An interesting discovery from the simulations revealed distinct energy transfer pathways contingent upon the initial vibrational states of the CO molecules. For those starting in high vibrational states, the vibrational energy was predominantly transferred to surface electrons and through molecular translation. Conversely, molecules with low initial vibrational states showed a trend where vibrational energy was solely transferred to surface electrons.
This research marks a significant leap in our understanding of molecular-surface energy transfer mechanisms. The robust modeling framework established in this study has the potential to extend its applications to various other nonadiabatic dynamics at surfaces, which may influence future advancements in fields such as catalysis, materials science, and nanotechnology.
More information:
Gang Meng et al, First-Principles Nonadiabatic Dynamics of Molecules at Metal Surfaces with Vibrationally Coupled Electron Transfer, Physical Review Letters (2024). DOI: 10.1103/PhysRevLett.133.036203
Citation: New strategy for simulating nonadiabatic dynamics of molecules at metal surfaces (2024, September 16) retrieved 16 September 2024 from https://phys.org/news/2024-09-strategy-simulating-nonadiabatic-dynamics-molecules.html
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