Modeling Equilibration Dynamics of Hyperthermal Products of Surface Reactions Using Scalable Neural Network Potential with First-Principles Accuracy.

Equilibration dynamics of hot oxygen atoms following the dissociation of O 2 on Pd(100) and Pd(111) surfaces are investigated by molecular dynamics simulations based on a scalable neural network potential enabling first-principles description of the interaction of O 2 and O interacting with variable Pd supercells. By analyzing hundreds of trajectories with appropriate initial sampling, the measured distance distribution of equilibrated atom pairs on Pd(111) is well reproduced. However, our results on Pd(100) suggest that the ballistic motion of hot atoms predicted previously is a rare event under ideal conditions, while initial molecular orientation and surface thermal fluctuation could significantly affect the overall postdissociation dynamics. On both surfaces, dissociated hyperthermal oxygen atoms primarily locate their nascent positions and experience a similar random walk motion nearby.