Year: 2025
Type: article
Abstract: Incorporating nuclear quantum effects into nonadiabatic dynamics remains a significant challenge. Herein we introduce new nonadiabatic dynamics approaches based on the recently developed constrained nuclear-electronic orbital (CNEO) theory. The CNEO approach integrates nuclear quantum effects, particularly quantum nuclear delocalization effects, into effective potential energy surfaces. When combined with Ehrenfest dynamics and surface hopping, it effectively captures both nonadiabaticity and quantum nuclear delocalization effects. We apply these new approaches to a one-dimensional proton-coupled electron transfer model and find that they outperform conventional Ehrenfest dynamics and surface hopping, particularly in accurately predicting proton transfer dynamics and proton transmission probabilities in the low-momentum regime.
Authors: Zhe Liu, Zehua Chen, Yang Yang
Institution: University of Wisconsin–Madison
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
Funder: Division of Chemistry
Award: G2567070707
OpenAlex ID: W4411400932