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Obtaining the free energy of large molecules from quantum mechanical energy functions is a longstanding challenge. We describe a method that allows us to estimate, at the quantum mechanical level, the harmonic contributions to the…

Chemical Physics · Physics 2023-03-07 Alec F. White , Chenghan Li , Xing Zhang , Garnet Kin-Lic Chan

Predicting polymer glass transition temperatures (Tg) with first-principles fidelity has long remained out of reach, as cooling multi-thousand-atom systems over a broad temperature range at acceptable rates exceeds the computational limits…

Materials Science · Physics 2026-01-27 Ashutosh Srivastava , Sakshi Agarwal , Shivank Shukla , Harikrishna Sahu , Rampi Ramprasad

The high-temperature cubic-tetragonal phase transition of pure stoichiometric zirconia is studied by molecular dynamics (MD) simulations and within the framework of the Landau theory of phase transformations. The interatomic forces are…

Materials Science · Physics 2009-11-07 Stefano Fabris , Anthony T. Paxton , Michael W. Finnis

Recently, Dammak and coworkers (H. Dammak, Y. Chalopin, M. Laroche, M. Hayoun, and J.J. Greffet. Quantumthermal bath for molecular dynamics simulation. Phys. Rev. Lett., 103:190601, 2009.) proposed that the quantum statistics of vibrations…

Materials Science · Physics 2011-05-30 Jean-Louis Barrat , David Rodney

A simple deterministic and time reversal invariant type of thermostat is proposed to be used for computer simulations of classical systems. It acts on collisions with the walls of the container exclusively. It maps the incoming and outgoing…

Statistical Mechanics · Physics 2014-11-13 Henk van Beijeren

Point defects dictate the properties of many functional materials. The standard approach to modelling the thermodynamics of defects relies on a static description, where the change in Gibbs free energy is approximated by the internal…

Materials Science · Physics 2024-12-24 Irea Mosquera-Lois , Johan Klarbring , Aron Walsh

We develop a method to fit high-temperature Gibbs free energy data for the development of interatomic potentials for atomic systems. The approach is based on Hamiltonian thermodynamic integration, enabling the identification of suitable…

Materials Science · Physics 2026-03-04 Liangrui Wei , Yang Sun

This contribution is devoted to cover some technical aspects related to the use of the recently proposed energy probability distribution zeros in the study of phase transitions. This method is based on the partial knowledge of the partition…

Statistical Mechanics · Physics 2017-12-13 L A S Mól , R G M Rodrigues , R A Stancioli , J C S Rocha , B V Costa

Atmospheric systems incorporating thermal dynamics must be stable with respect to both energy and entropy. While energy conservation can be enforced via the preservation of the skew-symmetric structure of the Hamiltonian form of the…

Numerical Analysis · Mathematics 2023-10-31 Kieran Ricardo , David Lee , Kenneth Duru

Molecular dynamics simulations provide a versatile framework to study interfacial heat transport, but their accuracy remains limited by the accuracy of available interatomic potentials. In the past, researchers have adopted the use of…

Materials Science · Physics 2021-05-11 Spencer Wyant , Andrew Rohskopf , Asegun Henry

The mechanical response of solids depends on temperature because the way atoms and molecules respond collectively to deformation is affected at various levels by thermal motion. This is a fundamental problem of solid state science and plays…

Soft Condensed Matter · Physics 2015-06-12 Alessio Zaccone , Eugene M. Terentjev

We have developed a method to accurately and efficiently determine the vibrational free energy as a function of temperature and volume for substitutional alloys from first principles. Taking Ti$_{1-x}$Al$_x$N alloy as a model system, we…

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

Phonons, as quantized vibrational modes in crystalline materials, play a crucial role in determining a wide range of physical properties, such as thermal and electrical conductivity, making their study a cornerstone in materials science. In…

Materials Science · Physics 2024-02-20 Huiju Lee , Yi Xia

We calculate the thermomechanical properties of $\alpha$-iron, and in particular its isothermal and adiabatic elastic constants, using first-principles total-energy and lattice-dynamics calculations, minimizing the quasi-harmonic…

Materials Science · Physics 2015-06-23 Daniele Dragoni , Davide Ceresoli , Nicola Marzari

The integration time step is a critical determinant of performance in molecular dynamics simulations, governing the trade-off between speed and fidelity. Although 2 fs remains the standard in atomistic biomolecular simulations, the push for…

Biological Physics · Physics 2026-03-04 Kush Coshic , Gerhard Hummer

Density functionals at the level of the Generalized Gradient Approximation (GGA) and a plane-wave basis set are widely used today to perform ab initio molecular dynamics (AIMD) simulations. Going up in the ladder of accuracy of density…

Computational Physics · Physics 2021-10-18 Sagarmoy Mandal , Ritama Kar , Tobias Kloeffel , Bernd Meyer , Nisanth N. Nair

Understanding collective phenomena in quantum materials from first principles is a promising route toward engineering materials properties on demand and designing new functionalities. This work examines the quantum paraelectric state, an…

Materials Science · Physics 2022-09-27 Luigi Ranalli , Carla Verdi , Lorenzo Monacelli , Matteo Calandra , Georg Kresse , Cesare Franchini

When studying high-dimensional dynamical systems such as macromolecules, quantum systems and polymers, a prime concern is the identification of the most probable states and their stationary probabilities or free energies. Often, these…

Data Analysis, Statistics and Probability · Physics 2013-01-01 Hao Wu , Frank Noé

The first-order phase transitions and related thermodynamics properties are primary concerns of materials sciences and engineering. In traditional atomistic simulations, the phase transitions and the estimation of their thermodynamic…

Chemical Physics · Physics 2023-08-17 Gang Seob Jung , Yoshihide Yoshimoto , Kwang Jin Oh , Shinji Tsuneyuki