相关论文: Improving Condensed Phase Water Dynamics with Expl…
Many model potential energy surfaces (PESs) have been reported for water; however, none are strictly from "first principles". Here we report such a potential, based on a many-body representation at the CCSD(T) level of theory up to the…
Symmetry plays a fundamental role in many-body systems, both in and out of equilibrium. The quantum Mpemba effect (QME) - a phenomenon where systems initially farther from equilibrium can thermalize faster - can be understood in terms of…
Quasi-chemical theory is utilized to analyze the roles of solute polarization and size in determining the structure and thermodynamics of bulk anion hydration for the Hofmeister series Cl$^-$, Br$^-$, and I$^-$. Excellent agreement with…
Distributed point charge models (DCM) and their minimal variants (MDCM) have been integrated with tools widely used for condensed-phase simulations, including a virial-based barostat and a slow-growth algorithm for thermodynamic…
Nuclear quantum phenomena beyond the Born-Oppenheimer approximation are known to play an important role in a growing number of chemical and biological processes. While there exists no unique consensus on a rigorous and efficient…
Simulating water accurately has been a challenge due to the complexity of describing polarization and intermolecular charge transfer. Quantum mechanical (QM) electronic structures provide an accurate description of polarization in response…
With the aim of progressing toward a practical implementation of an effective quantum-electrodynamics (QED) theory of atoms and molecules, which includes the effects of vacuum polarization through the creation of virtual electron-positron…
Various condensed phases of water, spanning from the liquid state to multiple ice phases, have been systematically investigated under extreme conditions of pressure and temperature to delineate their stability boundaries. This study focuses…
We show how machine learning techniques based on Bayesian inference can be used to reach new levels of realism in the computer simulation of molecular materials, focusing here on water. We train our machine-learning algorithm using…
First-principles molecular dynamics (FPMD) simulations were applied for the paraelectric-ferroelectric phase transition in the perovskite-type cadmium titanate, CdTiO3. Since the phase transition is reported to occur at the low temperature…
The interaction of condensed phase systems with external electric fields is crucial in myriad processes in nature and technology ranging from the field-directed motion of cells (galvanotaxis), to energy storage and conversion systems…
We present a polarizable embedding quantum mechanics/molecular mechanics (QM/MM) framework for ground- and excited-state Complete Active Space Self-Consistent Field (CASSCF) calculations on molecules within complex environments, such as…
Quantum computing (QC) provides a promising avenue toward enabling quantum chemistry calculations, which are classically impossible due to a computational complexity that increases exponentially with system size. As fully fault-tolerant…
Many physical and chemical processes in the condensed phase environment exhibit non-Markovian quantum dynamics. As such simulations are challenging on classical computers, we developed a variational quantum algorithm that is capable of…
Quantum computing promises to efficiently and accurately solve many important problems in quantum chemistry which elude classical solvers, such as the electronic structure problem of highly correlated materials. Two leading methods in…
We propose an ab-initio molecular dynamics method, capable to reduce dramatically the autocorrelation time required for the simulation of classical and quantum particles at finite temperature. The method is based on an efficient…
A frequency-dependent extension of the polarizable force field ``Atom-Condensed Kohn-Sham density functional theory approximated to the second-order'' (ACKS2) [J. Chem. Phys. 141, 194114 (2014)] is proposed, referred to as ACKS2$\omega$.…
The quantum dynamics of electron-nuclear systems is analyzed from the perspective of the exact factorization of the wavefunction, with the aim of defining gauge invariant equations of motion for both the nuclei and the electrons. For pure…
The recently observed temperature-dependent quasiphase transition of the single-file water chain confined within a carbon nanotube in experiments has been validated by the simple lattice theory and molecular dynamics simulations. It has…
Using first-principles molecular dynamics, we study the influence of nuclear quantum effects (NQEs) and nonlocal exchange--correlation density functionals (DFs) near molecular dissociation in liquid hydrogen. NQEs strongly influence…