Fully Consistent Density Functional Theory Determination of the Insulator-Metal Transition Boundary in Warm Dense Hydrogen

Abstract

Using conceptually and procedurally consistent density functional theory (DFT) calculations with an advanced meta-GGA exchange-correlation functional in ab initio molecular dynamics simulations, we determine the insulator-metal transition (IMT) of warm dense fluid hydrogen over the pressure range 50 to 300 GPa. Inclusion of nuclear quantum effects via path-integral molecular dynamics (PIMD) sharpens the metallic transition and lowers the transition temperature relative to results from Born-Oppenheimer (BO) MD. BOMD itself gives improved agreement with experimental results compared to previous DFT predictions. Examination of the ionic pair correlation function in the context of the abrupt conductivity increase at the transition confirms a metallic transition due to the dissociation of molecular hydrogen that coincides with an abrupt band gap closure. Direct comparison of the PIMD and BOMD results clearly demonstrates an isotope effect on the IMT. Distinct from stochastic simulations, these results do not depend upon any ad hoc combination of ground-state and finite-T methodologies.

References in corpus (24)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Van der Waals Density Functional for General Geometries
• A Higher-Accuracy van der Waals Density Functional
• Nonlocal van der Waals density functional: The simpler the better
• SCAN+rVV10: A promising van der Waals density functional
• i-PI 2.0: A Universal Force Engine for Advanced Molecular Simulations
• i-PI: A Python interface for ab initio path integral molecular dynamics simulations
• Thermophysical properties of warm dense hydrogen
• Nuclear Quantum Effects and Nonlocal Exchange-Correlation Functionals Applied to Liquid Hydrogen at High Pressure
• A First-order Phase Transition to Metallic Hydrogen
• Kubo-Greenwood Electrical Conductivity Formulation and Implementation for Projector Augmented Wave Datasets
• Nonempirical Semi-local Free-Energy Density Functional for Matter Under Extreme Conditions
• Phase diagram of hydrogen and a hydrogen-helium mixture at planetary conditions by Quantum Monte Carlo simulations
• Deorbitalized meta-GGA Exchange-Correlation Functionals in Solids
• Deorbitalization strategies for meta-GGA exchange-correlation functionals
• Equation of state of metallic hydrogen from Coupled Electron-Ion Monte Carlo simulations
• Conductivity and Dissociation in Metallic Hydrogen: Implications for Planetary Interiors
• Thermodynamic anomalies and three distinct liquid-liquid transitions in warm dense liquid hydrogen
• Optical properties of high pressure liquid hydrogen across molecular dissociation
• Striking Isotope Effect on the Metallization Phase Lines of Liquid Hydrogen and Deuterium
• Towards the same line of liquid-liquid phase transition of dense hydrogen from various theoretical predictions
• Benchmarking vdW-DF first principle predictions against Coupled Electron-Ion Monte Carlo for high pressure liquid hydrogen
• Thermodynamics of the insulator-metal transition in dense liquid deuterium

Cited by in corpus (13)

• First principles simulations of dense hydrogen
• High pressure hydrogen by machine learning and quantum Monte Carlo
• Spin-Crossover From a Well-Behaved, Low-Cost meta-GGA Density Functional
• From Density Response to Energy Functionals and Back: An ab initio perspective on Matter Under Extreme Conditions
• Electronic energy gap closure and metal-insulator transition in dense liquid hydrogen
• Isotope quantum effects in the metallization transition in liquid hydrogen
• Mott-Anderson Metal-Insulator Transitions from Entanglement
• Nature of the bonded-to-atomic transition in liquid silica to TPa pressures
• Modeling Fluid Polyamorphism Through a Maximum-Valence Approach
• Hydrogen liquid-liquid transition from first principles and machine learning
• Deep variational free energy prediction of dense hydrogen solid at 1200K
• Thermodynamic Modeling of Fluid Polyamorphism in Hydrogen at Extreme Conditions
• A Denser Hydrogen Inferred from First-Principles Simulations Challenges Jupiter's Interior Models