Related papers: From Data-Driven Models to Physical Insight: Vibra…
Phonons, quantized vibrations of the atomic lattice, are fundamental to understanding thermal transport, structural stability, and phase behavior in crystalline solids. Despite advances in computational materials science, most predictions…
The temperature-dependent behavior of defect densities within a crystalline structure is intricately linked to the phenomenon of vibrational entropy. Traditional methods for evaluating vibrational entropy are computationally intensive,…
The vibrational entropy of a solid at finite temperature is investigated from the perspective of information theory. Ab initio molecular dynamics (AIMD) simulations generate ensembles of atomic configurations at finite temperature from…
We build a comprehensive methodology for the fast computation of entropy across both solid and liquid phases. The proposed method utilizes a single trajectory of molecular dynamics (MD) to facilitate the calculation of entropy, which is…
Ammonium sulfate is a giant inverse barocaloric material that is cheaply and commercially available. Exploiting its potential for cooling applications requires an understanding of the mechanism driving the entropy change. Here we report an…
Variational quantum algorithms offer a promising framework for solving eigenvalue problems on near-term quantum hardware, yet their applicability beyond electronic structure calculations remains relatively unexplored. In this work, we…
A thermodynamic measure of the fragility of liquids has recently (Ito et al ref.1) been defined in terms of the temperature dependence of the excess entropy of liquid over crystal, scaled by the excess entropy at the glass transition…
There is an ever-growing need for predictive models for the elasto-viscoplastic deformation of solids. Our goal in this paper is to incorporate recently developed out-of-equilibrium statistical concepts into a thermodynamically consistent,…
While the vibrational thermodynamics of materials with small anharmonicity at low temperatures has been understood well based on the harmonic phonons approximation; at high temperatures, this understanding must accommodate how phonons…
Vibrational dynamics governs the fundamental properties of molecular crystals, shaping their thermodynamics, mechanics, spectroscopy, and transport phenomena. However desirable, the first-principles calculation of solid-state vibrations,…
The rapid scaling of artificial intelligence models has revealed a fundamental tension between model capacity (storage) and inference efficiency (computation). While classical information theory focuses on transmission and storage limits,…
We present a machine learning (ML) method for efficient computation of vibrational thermal expectation values of physical properties from first principles. Our approach is based on the non-perturbative frozen phonon formulation in which…
Vibrational properties of solids are key to determining stability, response and functionality. However, they are challenging to computationally predict at Ab-Initio accuracy, even for elemental systems. Ab-Initio methods for modeling atomic…
The length-scale dependence of the dynamic entropy is studied in a molecular dynamics simulation of a binary Lennard-Jones liquid above the mode-coupling critical temperature $T_c$. A number of methods exist for estimating the entropy of…
Modern autonomous systems are driving the critical need for next-generation adaptive materials and structures with embodied intelligence, i.e., the embodiment of memory, perception, learning, and decision-making within the mechanical…
The phonon density-of-states (DOS) summarizes the lattice vibrational modes supported by a structure, and gives access to rich information about the material's stability, thermodynamic constants, and thermal transport coefficients. Here, we…
We present a rigorous and efficient approach to the calculation of classical lattice-dynamical quantities from simulations that do not require an explicit solution of the time evolution. We focus on the temperature-dependent vibrational…
The two-phase thermodynamic (2PT) model {[}J. Chem. Phys., \textbf{119}, 11792 (2003){]} provides a promising paradigm to efficiently determine the ionic entropies of liquids from molecular dynamics (MD). In this model, the vibrational…
Computing vibrational free energies ($F_{vib}$) and entropies ($S_{vib}$) has posed a long standing challenge to the high-throughput ab initio investigation of finite temperature properties of solids. Here we use machine-learning techniques…
Diamond is studied by path integral molecular dynamics simulations of the atomic nuclei in combination with a tight-binding Hamiltonian to describe its electronic structure and total energy. This approach allows us to quantify the influence…