Unveiling the Interplay of Electronic and Phononic Excitations in Laser-Induced Oxygen Activation on Ru(0001)

Authors

Xiangrui Wang, Virginia Polytechnic Institute and State University
Jiamin Wang, Virginia Polytechnic Institute and State University
Paul Spiering, Leiden University
Liping Liu, Virginia Polytechnic Institute and State University
Jörg Meyer, Leiden University
Jerry L. LaRue, Chapman UniversityFollow
Hongliang Xin, Virginia Polytechnic Institute and State University

Document Type

Article

Publication Date

9-17-2025

Abstract

Understanding laser-induced dynamics on metal surfaces poses significant challenges due to the intricate interplay between electronic and phononic degrees of freedom, which evolve on distinct timescales. In this study, we introduce a machine learning-accelerated approach to molecular dynamics simulations that incorporates anisotropic electronic friction, providing deeper insights into these complex processes. Our framework extends the accessible time and length scales for nonadiabatic dynamics simulations, enabling a detailed investigation of the laser-induced activation of oxygen on the Ru(0001) surface. Statistical analysis reveals that strong electronic excitation dominates the first 800 fs after laser exposure. Beyond this timescale, energy deposited by electronic excitation continues to drive oxygen activation, while phonons, although always present as a dissipation channel, play a weaker role by buffering energy loss and redistributing kinetic energy among vibrational modes. The observed non-linear yield–fluence relationship, described by Y ∼ Fⁿ, underscores the pivotal role of electronic excitation. In addition, we identify the z-direction as the key activation mode for oxygen diffusion, with the exponent of the power law representing the quantized energy required for this process. This approach significantly accelerates dynamic simulations while offering valuable insights into the interplay between electronic and phononic excitations during laser-induced oxygen activation on Ru(0001).

Comments

This article was originally published in Journal of Chemical Physics, volume 163, issue 11, in 2025. https://doi.org/10.1063/5.0278197

Recommended Citation

Xiangrui Wang, Jiamin Wang, Paul Spiering, Liping Liu, Jörg Meyer, Jerry L. LaRue, Hongliang Xin; Unveiling the interplay of electronic and phononic excitations in laser-induced oxygen activation on Ru(0001). J. Chem. Phys. 28 September 2025; 163 (11): 114109. https://doi.org/10.1063/5.0278197

Copyright

American Institute of Physics