Fig.1

The root mean square error (RMSE) curves of energy and force in the training and validation set during the training process of DeePMD"

Fig.2

Comparison of DFT and DeePMD AIMD results. (a-d) Frequency density distributions of the proton transfer reaction coordinates δ in four adsorption structures. The molecular or interfacial sites where proton transfer may happen are circled in red in the sub-figures. The blue curves represent the frequency density distributions of δ in the original VASP AIMD datasets, and the orange curves represent the frequency density distributions of δ in the 50 ps AIMD trajectories calculated by DeePMD and i-Pi. (e-l) Comparison of DFT and DeePMD predicted energy (e-h) and force (i-l) of four structures on test sets. The energy has been shifted to the coordinate origin by subtracting the average value."

Fig.3

The 50 ps AIMD and 25 ps PIMD trajectories of four structures were obtained by combining the DeePMD training model with i-Pi. Frequency density distributions of the proton transfer reaction coordinates δ of the obtained four structures at (a-d) AIMD 100 K, (e-h) PIMD 100 K, (i-l) AIMD 300 K and (m-p) PIMD 300 K are shown."

Fig.4

The 20 ps time-dependent evolution curves of the transfer reaction coordinate δ corresponding to one bead of a proton in MD. Trajectories of δ in the obtained four structures at 100 K and 300 K in (a-d) AIMD and (e-h) PIMD are shown."

Fig.5

(a-b) Evolution of the centroid of the proton transfer reaction coordinates in the 1 ML_HD structure over 600 fs at 100 K and 300 K RPMD simulations. In RPMD is defined as the reaction coordinate of the average trajectory of each “bead” (i.e., the trajectory of the centroid of the “bead”). (c-d) Evolution of in the 1/2 ML_D structure over 600 fs at 300 K AIMD and RPMD simulations. (e-h) Hole transfer process corresponding to the molecular dynamics trajectories in (a-d), the evolution of holes in CH3OH. The ADM ridge structure and the overall distribution probability over time given by NAMD and RP-NAMD simulations are shown."