Direct Prediction of Calcite Surface Wettability with First-Principles Quantum Simulation.

Prediction of intrinsic surface wettability from first-principles offers great opportunities in probing new physics of natural phenomena and enhancing energy production or transport efficiency. We propose a general quantum mechanical approach to predict the macroscopic wettability of any solid crystal surfaces for different liquids directly through atomic-level density functional simulation. As a benchmark, the wetting characteristics of calcite crystal (10.4) under different types of fluids (water, hexane, and mercury), including either contact angle or spreading coefficient, are predicted and further validated with experimental measurements. A unique feature of our approach lies in its capability of capturing the interactions among various polar fluid molecules and solid surface ions, particularly their charge density difference distributions. Moreover, this approach provides insightful and quantitative predictions of complicated surface wettability alteration problems and wetting behaviors of liquid/liquid/solid triphase systems.