Determining the effect of hot electron dissipation on molecular scattering experiments at metal surfaces

C. L. Box, Y. Zhang, R. Yin, B. Jiang, R. J. Maurer, JACS Au 1, 164-173 (2020)

"Vibrational state-to-state scattering of NO on Au(111) provides a testing ground for developing various nonadiabatic theories, including electronic friction theory. This system is often cited as the prime example for the breakdown of electronic friction theory, a very efficient model accounting for dissipative forces on metal-adsorbed molecules due to the creation of electron-hole-pair excitations in the metal. Here we present a comprehensive quantitative analysis of the performance of molecular dynamics with electronic friction (MDEF) in describing vibrational state-to-state scattering of NO on Au(111) and connect directly to fundamental approximations. Our analysis provides a firm baseline for the future development of nonadiabatic dynamics methods to tackle problems in surface chemistry and photocatalysis."

A symmetry adapted high dimensional neural network representation of electronic friction tensor of adsorbates on metals

Yaolong Zhang, Reinhard J. Maurer, Bin Jiang, J. Chem. Phys., just accepted (2019)

"In this work, we develop a new symmetry-adapted neural network representation of electronic friction, based on our recently proposed embedded atom neural network (EANN) framework. Unlike previous methods, our new approach can readily include both molecular and surface degrees of freedom, regardless of the type of surface. Tests on the H2+Ag(111) system show that this approach yields an accurate, efficient, and continuous representation of electronic friction, making it possible to perform large scale TDPT-based MDEF simulations to study both adiabatic and nonadiabatic energy dissipation in a unified framework."

Electron-Hole-Pair-Induced Vibrational Energy Relaxation of Rhenium Catalysts on Gold Surfaces

Aimin Ge, Benjamin Rudshteyn, Jingyi Zhu, Reinhard J. Maurer, VIctor S. Batista, and Tianquan Lian, J. Phys. Chem. Lett. 9, 406-412 (2018)

"Using a combination of time-resolved vibrational spectroscopy and Density Functional Theory, we study the vibrational relaxation mechanisms of a metal-adsorbed reduction catalyst."

Mode specific electronic friction in dissociative chemisorption on metal surfaces: H2 on Ag(111)

Reinhard J. Maurer, Bin Jiang, Hua Guo, John C. Tully, Phys. Rev. Lett. 118, 256001 (2017)

"Using nonadiabatic ab-initio molecular dynamics, we study how electronic friction affects mode-dependent energy loss and reaction outcomes during dissociative chemisorption of molecular Hydrogen."

Ab-initio tensorial electronic friction for molecules on metal surfaces: nonadiabatic vibrational relaxation

Reinhard J. Maurer, Mikhail Askerka, Victor S. Batista, John C. Tully, Phys. Rev. B. 94, 115432 (2016)

We present our efficient and robust ab-initio implementation of tensorial electronic friction and apply it to calculate vibrational lifetimes.

Role of Tensorial Electronic Friction in Energy Transfer at Metal Surfaces

Mikhail Askerka, Reinhard J. Maurer, Victor S. Batista, John C. Tully, Phys. Rev. Lett. 116, 217601 (2016)
Editor’s Suggestion

We use time-dependent perturbation theory to calculate the full electronic friction tensor and study its relevance in the simulation of dynamics at surfaces.