Nuclear Quantum Effects and Nonlocal Exchange-Correlation Functionals Applied to Liquid Hydrogen at High Pressure

摘要

Using first-principles molecular dynamics, we study the influence of nuclearquantum effects (NQEs) and nonlocal exchange--correlation density functionals(DFs) near molecular dissociation in liquid hydrogen. NQEs strongly influenceintramolecular properties, such as bond stability, and are thus an essentialpart of the dissociation process. Moreover, by including DFs that account foreither the self-interaction error or dispersion interactions, we find a muchbetter description of molecular dissociation and metallization than previousstudies based on classical protons and/or local or semi-local DFs. We obtainexcellent agreement with experimentally measured optical properties alongpre-compressed Hugoniots, and while we still find a first-order liquid--liquidtransition at low temperatures, transition pressures are increased by more than100 GPa.