New strategy for simulating nonadiabatic dynamics of molecules at metal surfaces
A research team led by Prof JIANG Bin from the University of Science and Technology of China (USTC) of the Chinese Academy of Sciences (CAS) proposed a novel approach to accurately describe electron transfer mediated nonadiabatic dynamics of molecules at metal surfaces. Their works were published in Physical Review Letters.
Numerous experimental phenomena have demonstrated that non-adiabatic energy transfer is widespread in various interfacial processes. Therefore, studying non-adiabatic energy transfer is crucial for understanding interfacial processes such as chemical adsorption, electrochemistry, and plasmonic catalysis. However, during the interaction between molecules and metal surfaces, molecular vibrations, rotations, and translations couple with surface phonons and electrons, leading to extremely complex energy transfer processes. Traditional models based on electronic friction have offered some insights, but they fall short in capturing the complex energy transfer observed in experimental studies.
To tackle this problem, Prof. JIANG’s team developed a simulation strategy and applied it to the energy transfer dynamics of CO molecules scattering from AU(111) surfaces. The strategy starts by calculating the charge-transfer states of various configurations of CO molecules at the metal surfaces using constrained density functional theory (CDFT). They then utilized an embedded atom neural network (EANN) to learn the CDFT energies and yield high-dimensional diabatic potential energy surfaces (PESs). Finally, they applied independent electron surface hopping (IESH) method to simulate the energy transfer process.
The results showed that the simulations closely matched the experimental data for the vibrational final state distribution of highly vibrationally excited CO (vi=17) after scattering. The vibrational relaxation probability, mean translational energy, and scattering angle distribution for low vibrationally excited CO (vi=2) were also accurately reproduced by the simulations.
Specifically, the simulation results also revealed different energy transfer pathways for different initial vibrational state. For high initial vibrational states, the molecular vibrational energy primarily transfers to surface electrons and molecular translation. In contrast, for low initial vibrational states, the molecular vibrational energy transfers exclusively to the surface electrons.
This study represents a significant advancement in understanding the energy transfer of molecule-surface system. By providing a robust and accurate framework for modeling nonadiabatic dynamics, this strategy can be extended to studying other nonadiabatic dynamics at surfaces, potentially leading to future development in catalysis, materials science, and nanotechnology.
Journal: Physical Review Letters
DOI: 10.1103/PhysRevLett.133.036203
Article Title: First-Principles Nonadiabatic Dynamics of Molecules at Metal Surfaces with Vibrationally Coupled Electron Transfer
Media Contact
Jane Fan
University of Science and Technology of China
qfan@ustc.edu.cn
All latest news from the category: Physics and Astronomy
This area deals with the fundamental laws and building blocks of nature and how they interact, the properties and the behavior of matter, and research into space and time and their structures.
innovations-report provides in-depth reports and articles on subjects such as astrophysics, laser technologies, nuclear, quantum, particle and solid-state physics, nanotechnologies, planetary research and findings (Mars, Venus) and developments related to the Hubble Telescope.
Newest articles
NASA: Mystery of life’s handedness deepens
The mystery of why life uses molecules with specific orientations has deepened with a NASA-funded discovery that RNA — a key molecule thought to have potentially held the instructions for…
What are the effects of historic lithium mining on water quality?
Study reveals low levels of common contaminants but high levels of other elements in waters associated with an abandoned lithium mine. Lithium ore and mining waste from a historic lithium…
Quantum-inspired design boosts efficiency of heat-to-electricity conversion
Rice engineers take unconventional route to improving thermophotovoltaic systems. Researchers at Rice University have found a new way to improve a key element of thermophotovoltaic (TPV) systems, which convert heat…