Related papers: Statistical mechanical approximations to more effi…
We evaluate the accuracy of varying thermal expansion models for the quasi-harmonic approximation (QHA) relative to molecular dynamics (MD) for 10 sets of enantiotropic organic polymorphs. Relative to experiment we find that MD, using an…
Quantitative evaluations of the free energy of materials must take into account thermal and zero-point energy fluctuations. While these effects can easily be estimated within a harmonic approximation, corrections arising from the anharmonic…
A first-principles approach called the {\it{self-consistent quasiharmonic approximation}} (SC-QHA) method is formulated to calculate the thermal expansion, thermomechanics, and thermodynamic functions of solids at finite temperatures with…
The quasiharmonic approximation (QHA), in its simplest form also called the statically constrained (SC) QHA, has been shown to be a straightforward method to compute thermoelastic properties of crystals. Recently we showed that for…
Efficient computational methods that are capable of supporting experimental measures obtained at constant values of pH and redox potential are important tools as they serve to, among other things, provide additional atomic level information…
We present a method to accurately predict the Helmholtz harmonic free energies of molecular crystals in high-throughput settings. This is achieved by devising a computationally efficient framework that employs a Gaussian Process Regression…
We develop a novel method of replica-exchange molecular dynamics (REMD) simulation, mass-scaling REMD (MSREMD) method, which improves trajectory accuracy at high temperatures, and thereby contributes to numerical stability. In addition, the…
Two of the most successful methods that are presently available for simulating the quantum dynamics of condensed phase systems are centroid molecular dynamics (CMD) and ring polymer molecular dynamics (RPMD). Despite their conceptual…
The ability to reliably predict the structures and stabilities of a molecular crystal and its polymorphs without any prior experimental information would be an invaluable tool for a number of fields, with specific and immediate applications…
Accurate calculations of molecular crystals are crucial for drug design and crystal engineering. However, periodic high-level density functional calculations using hybrid functionals are often prohibitively expensive for relevant systems.…
Ensuring a satisfactory statistical convergence of anharmonic thermodynamic properties requires sampling of many atomic configurations, however the methods to obtain those necessarily produce correlated samples, thereby reducing the…
The quasi-harmonic approximation (QHA) is a powerful method that uses the volume dependence of non-interacting phonons to compute the free energy of materials at high pressures (P) and temperatures (T). However, anharmonicity, electronic…
Molecules can form myriad crystalline polymorphs, each with distinct properties affecting their performance across diverse applications, from pharmaceuticals to functional materials and more. Predicting the thermodynamically most stable…
We introduce a novel simple algorithm for thermostatting path integral molecular dynamics (PIMD) with the Langevin equation. The staging transformation of path integral beads is employed for demonstration. The optimum friction coefficients…
Accelerating the calculations of finite-temperature thermodynamic properties is a major challenge for rational materials design. Reliable methods can be quite expensive, limiting their effective applicability in autonomous high-throughput…
Methods that combine collective variable (CV) based enhanced sampling and global tempering approaches are used in speeding-up the conformational sampling and free energy calculation of large and soft systems with a plethora of energy…
We studied acetylhistidine (AcH), bare or microsolvated with a zinc cation by simulations in isolation. First, a global search for minima of the potential energy surface combining both, empirical and first-principles methods, is performed…
We describe improvements to the quasicentroid molecular dynamics (QCMD) path-integral method, which was developed recently for computing the infrared spectra of condensed-phase systems. The main development is an improved estimator for the…
We describe how the fast quasi-centroid molecular dynamics (f-QCMD) method can be applied to condensed phase systems by approximating the quasi-centroid potential of mean force as a sum of inter- and intra-molecular corrections to the…
Classical free energies for the cage and prism isomers of water hexamer computed by the self- consistent phonons (SCP) method and reversible scaling (RS) method are presented for several flexible water potentials. Both methods have been…