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Machine learning thermodynamic perturbation theory (MLPT) is a promising approach to compute finite temperature properties when the goal is to compare several different levels of ab initio theory and/or to apply highly expensive…
Ab initio molecular dynamics (AIMD) is a powerful tool to predict properties of molecular and condensed matter systems. The quality of this procedure is based on accurate electronic structure calculations. The development of quantum…
We have recently developed a breakthrough methodology for rapidly computing entropy in both solids and liquids by integrating a multiscale entropy approach (known as zentropy theory) with molecular dynamics (MD) simulations. This approach…
We demonstrate an efficient and accurate, general-purpose first-principles blueprint for calculating anharmonic vibrational free energy and predicting structural phase transition temperatures of solids. Thermodynamic integration is…
For 35 years, {\it ab initio} molecular dynamics (AIMD) has been the method of choice for modeling complex atomistic phenomena from first principles. However, most AIMD applications are limited by computational cost to systems with…
This thesis describes several topics related to finite temperature studies of strongly correlated systems: finite temperature density matrix embedding theory (FT-DMET), finite temperature metal-insulator transition, and quantum algorithms…
Accounting for nuclear quantum effects (NQEs) can significantly alter material properties at finite temperatures. Atomic modeling using the path-integral molecular dynamics (PIMD) method can fully account for such effects, but requires…
In traditional finite-temperature Kohn-Sham density functional theory (KSDFT), the well-known orbitals wall restricts the use of first-principles molecular dynamics methods at extremely high temperatures. However, stochastic density…
Molecular design requires systematic and broadly applicable methods to extract structure-property relationships. The focus of this study is on learning thermodynamic properties from molecular-liquid simulations. The methodology relies on an…
We present an algorithm for computing melting points by autonomously learning from coexistence simulations in the NPT ensemble. Given the interatomic interaction model, the method makes decisions regarding the number of atoms and…
Starting from the Helmholtz free energy we calculate analytically first- and second-order derivatives, as internal energy and specific heats, for the ideal system and the exchange and correlation interactions covering a broad range of…
Variational methods are a common approach for computing properties of ground states but have not yet found analogous success in finite temperature calculations. In this work we develop a new variational finite temperature algorithm (VAFT)…
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…
Accounting for electrons and nuclei simultaneously is a powerful capability of ab initio molecular dynamics (AIMD). However, AIMD is often unable to accurately reproduce properties of systems such as water due to inaccuracies in the…
Accurate free-energy calculations are essential for predicting thermodynamic properties and phase stability, but existing methods are limited: phonon-based approaches neglect anharmonicity and liquids, while molecular dynamics (MD) is…
We discuss how to include our recently proposed thermopotentiostat technique [Phys. Rev. Lett. 126, 136803 (2021)] into any existing ab initio molecular dynamics (AIMD) package. Using thermopotentiostat AIMD simulations in the canonical…
Path-integral molecular dynamics (PIMD) simulations are crucial for accurately capturing nuclear quantum effects in materials. However, their computational intensity and reliance on multiple software packages often limit their applicability…
Ultra-fast electronic phenomena originating from finite temperature, such as nonlinear optical excitation, can be simulated with high fidelity via real-time time dependent density functional theory (rt-TDDFT) calculations with hybrid…
Recently, we developed a method to construct polynomial interatomic potentials from ab-initio calculations in order to accurately describe laser excited solids [PRL 124, 085501 (2020)]. However, ab-initio methods, and therefore analytical…
Ab initio molecular dynamics (AIMD) based on density functional theory (DFT) has become a workhorse for studying the structure, dynamics, and reactions in condensed matter systems. Currently, AIMD simulations are primarily carried out at…