First-principles-based Machine Learning Models for Phase Behavior and Transport Properties of CO2

Reha Mathur, Maria Carolina Muniz, Shuwen Yue, Roberto Car and Athanassios Z. Panagiotopoulos, J. Phys. Chem. B, 2023, 127, 20, 4562–4569 (2023) 

 In this work, we construct distinct first-principles-based machine-learning models of CO2, reproducing the potential energy surface of the PBE-D3, BLYP-D3, SCAN and SCAN-rvv10 approximations of density functional theory. We employ the Deep Potential methodology to develop the models and consequently achieve a significant computational efficiency over ab initio molecular dynamics (AIMD) that allows for larger system sizes and time scales to be explored. Although our models are trained only with liquid phase configurations, they are able to simulate a stable interfacial system and predict vapor-liquid equilibrium properties, in good agreement with results from the literature. Because of the computational efficiency of the models, we are also able to obtain transport properties, such as viscosity and diffusion coefficients. We find that the SCAN-based model underpredicts experimental liquid densities, while the SCAN-rvv10-based model shows improvement but still exhibits a temperature shift, which remains approximately constant for all properties investigated in this work. We find that the BLYP-D3-based model generally performs better for liquid phase and vapor-liquid equilibrium properties, but the PBE-D3-based model is better suited for predicting transport properties.