Nuclear-Electronic Orbital Ehrenfest Dynamics

Zhao, Luning; Wildman, Andrew; Tao, Zhen; Schneider, Patrick E.; Hammes-Schiffer, Sharon; Li, Xiaosong

doi:10.1063/5.0031019

Title: Nuclear-Electronic Orbital Ehrenfest Dynamics

Journal Article · Mon Dec 14 00:00:00 EST 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0031019· OSTI ID:1760682

Zhao, Luning ^[1]; Wildman, Andrew ^[1]; Tao, Zhen ^[2]; Schneider, Patrick E. ^[2]; Hammes-Schiffer, Sharon ^[2]; Li, Xiaosong ^[3]

University of Washington
Yale University
UNIVERSITY OF WASHINGTON (MAIN CAMPUS)

The recently developed real-time nuclear-electronic orbital (RT-NEO) approach provides an elegant framework for treating electrons and selected nuclei, typically pro- tons, quantum mechanically in nonequilibrium dynamical processes. However, the RT-NEO approach neglects the motion of the other nuclei, preventing a complete de- scription of the coupled nuclear-electronic dynamics and spectroscopy. In this work, we describe the dynamical interaction between the other nuclei and the electron-proton subsystem with the mixed quantum-classical Ehrenfest dynamics method. The NEO- Ehrenfest approach propagates the electrons and quantum protons in a time-dependent variational framework, while the remaining nuclei move classically on the correspond- ing average electron-proton vibronic surface. This approach includes the non-Born- Oppenheimer eects between the electrons and quantum protons with RT-NEO and between the classical nuclei and the electron-proton subsystem with Ehrenfest dynam- ics. Spectral features for vibrational modes involving both quantum and classical nuclei are resolved from the time-dependent dipole moments. Moreover, nuclear quantum ef- fects are included directly in nonadiabatic dynamics simulations. The excited state intramolecular proton transfer in the o-hydroxybenzaldehyde molecule is shown to be faster and to exhibit a larger kinetic isotope eect with NEO-Ehrenfest compared to classical Ehrenfest dynamics. This work shows that the NEO-Ehrenfest method is a powerful tool to study dynamical processes with coupled electronic and nuclear degrees of freedom.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1760682

Report Number(s):: PNNL-SA-156782

Journal Information:: Journal of Chemical Physics, Vol. 153, Issue 22

Country of Publication:: United States

Language:: English

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