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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…

Materials Science · Physics 2024-03-14 Junsoo Park , Zhigang Wu , John W. Lawson

We introduce an efficient and robust method to compute alchemical free energy differences, resulting from the application of multiple walker Adaptive Biasing Force (ABF) in conjunction with strongly damped Langevin $\lambda$-dynamics.…

We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using…

Enhanced sampling and free energy calculation algorithms of the Thermodynamic Integration family (such as the Adaptive Biasing Force method, ABF) are not based on the direct computation of a free energy surface, but rather of its gradient.…

Computational Physics · Physics 2021-10-22 Jérôme Hénin

It is known that ab initio molecular dynamics (AIMD) simulations of liquid water, based on the generalized gradient approximation (GGA) to density functional theory (DFT), yield structural and diffusive properties in reasonable agreement…

Materials Science · Physics 2015-05-19 Jue Wang , G. Roman-Perez , Jose M. Soler , Emilio Artacho , M. -V. Fernandez-Serra

Conventional molecular dynamics (MD) simulation approaches, such as $\textit{ab initio}$ MD (AIMD) and empirical force field MD (EFFMD), face significant trade-offs between physical accuracy and computational efficiency. This work presents…

Disordered Systems and Neural Networks · Physics 2026-05-12 Hongyu Yan , Yong Wei , Minghan Chen , Hanning Chen

Smooth, highly accurate analytical representations of Fermi-Dirac (FD) integral combinations important in free-energy density functional calculations are presented. Specific forms include those that occur in the local density approximation…

Computational Physics · Physics 2015-04-21 Valentin V. Karasiev , Debajit Chakraborty , S. B. Trickey

The oxidation of NO molecules on epoxy-functionalized highly oriented pyrolytic graphite, thermalized at 300 K, was studied by means of ab initio molecular dynamics (AIMD) calculations. Four collision energies and two different orientations…

The relation between ab initio molecular dynamics formalism and the electron-phonon interaction formalism [P.B. Allen and V. Heine, J. Phys. C 9, 2305 (1976)] is explored. The fundamental quantity obtained in the AIMD formalism - total…

Materials Science · Physics 2009-06-13 T. R. S. Prasanna

We present an efficient ab initio dynamical mean-field theory (DMFT) implementation for quantitative simulations in solids. Our DMFT scheme employs ab initio Hamiltonians defined for impurities comprising the full unit cell or a supercell…

Strongly Correlated Electrons · Physics 2020-03-05 Tianyu Zhu , Zhi-Hao Cui , Garnet Kin-Lic Chan

We present a simulation scheme to calculate defect formation free energies at a molecular crystal/water interface based on force-field molecular dynamics (MD) simulations. To this end we adopt and modify existing approaches to calculate…

Materials Science · Physics 2015-06-22 Julian Schneider , Chen Zheng , Karsten Reuter

Geometry optimization is an important part of both computational materials and surface science because it is the path to finding ground state atomic structures and reaction pathways. These properties are used in the estimation of…

Materials Science · Physics 2021-07-07 Yilin Yang , Omar A. Jimenez-Negron , John R. Kitchin

We have developed and implemented a new quantum molecular dynamics approximation that allows fast and accurate simulations of dense plasmas from cold to hot conditions. The method is based on a carefully designed orbital-free implementation…

Plasma Physics · Physics 2015-06-22 Travis Sjostrom , Jerome Daligault

Path integral molecular dynamics simulations, combined with an ab initio evaluation of interactions using electronic structure theory, incorporate the quantum mechanical nature of both the electrons and nuclei, which are essential to…

Chemical Physics · Physics 2016-02-15 Ondrej Marsalek , Thomas E. Markland

Functionals of the meta-generalized gradient approximation (MGGA) are nowadays widely used in chemistry and solid-state physics for the simulation of electronic systems like molecules, solids, or surfaces. Due to their dependency on the…

Materials Science · Physics 2022-05-31 Jan Doumont , Fabien Tran , Peter Blaha

Ring polymer molecular dynamics (RPMD) has proven to be an accurate approach for calculating thermal rate coefficients of various chemical reactions. For wider application of this methodology, efficient ways to generate the underlying…

Chemical Physics · Physics 2020-01-08 Ivan S. Novikov , Alexander V. Shapeev , Yury V. Suleimanov

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…

Materials Science · Physics 2025-11-19 Ekaterina Spirande , Timofei Miryashkin , Andrei Kolmakov , Alexander Shapeev

In the framework of density functional theory (DFT) simulations of molecules and materials, anharmonic terms of the potential energy surface are commonly computed numerically, with an associated cost that rapidly increases with the size of…

Materials Science · Physics 2025-03-17 Davide Mitoli , Jefferson Maul , Alessandro Erba

For orbital-free {\it ab initio} molecular dynamics, especially on systems in extreme thermodynamic conditions, we provide the first pseudo-potential-adapted generalized gradient approximation (GGA) functional for the non-interacting free…

Chemical Physics · Physics 2020-02-19 Kai Luo , Valentin V. Karasiev , S. B. Trickey

Due to the development of efficient algorithms and the improvement of computer power it is now possible to map out potential energy surfaces (PES) of reactions at surfaces in great detail. This achievement has been accompanied by an…

Condensed Matter · Physics 2007-05-23 Axel Gross