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Chemical processes in closed systems are poorly controllable since they always relax to equilibrium. Living systems avoid this fate and give rise to a much richer diversity of phenomena by operating under nonequilibrium conditions. Recent…

Chemical Physics · Physics 2019-09-11 Emanuele Penocchio , Riccardo Rao , Massimiliano Esposito

We present an implementation of alchemical free energy simulations at the quantum mechanical level by directly interpolating the electronic Hamiltonian. The method is compatible with any level of electronic structure theory and requires…

Chemical Physics · Physics 2024-09-02 Chenghan Li , Xing Zhang , Garnet Kin-Lic Chan

In the long-time pursuit of the solution to calculate the partition function (or free energy) of condensed matter, Monte-Carlo-based nested sampling should be the state-of-the-art method, and very recently, we established a direct integral…

Statistical Mechanics · Physics 2020-01-08 Le-Cheng Gong , Bo-Yuan Ning , Tsu-Chien Weng , Xi-Jing Ning

We propose a proof of convergence of an adaptive method used in molecular dynamics to compute free energy profiles. Mathematically, it amounts to studying the long-time behavior of a stochastic process which satisfies a non-linear…

Analysis of PDEs · Mathematics 2007-06-13 Tony Lelievre , Felix Otto , Mathias Rousset , Gabriel Stoltz

We compare dynamical nonequilibrium molecular dynamics and continuum simulations of the dynamics of relaxation of a fluid system characterized by a non uniform density profile. Results match quite well as long as the lengthscale of density…

With the development of low order scaling methods for performing Kohn-Sham Density Functional Theory, it is now possible to perform fully quantum mechanical calculations of systems containing tens of thousands of atoms. However, with an…

Chemical Physics · Physics 2020-04-03 William Dawson , Stephan Mohr , Laura E. Ratcliff , Takahito Nakajima , Luigi Genovese

We propose a method to continually monitor the energy of a quantum system. We show that by having some previous knowledge of the system's dynamics, but not all of it, one can use the measured energy to determine many other quantities, such…

Quantum Physics · Physics 2019-03-29 Gabriel P. Martins , Nadja K. Bernardes , Marcelo F. Santos

We use a simple gas model to study non-equilibrium aspects of the multiparticle dynamics relevant to heavy ion collisions. By performing numerical simulations for various initial conditions we identify several characteristic features of the…

Nuclear Theory · Physics 2009-11-06 J. P. Bondorf , H. Feldmeier , I. N. Mishustin , G. Neergaard

Quantum chemistry calculations such as the prediction of molecular properties and modeling of chemical reactions are a few of the critical areas where near-term quantum computers can showcase quantum advantage. We present a method to…

Quantum Physics · Physics 2022-04-06 Utkarsh Azad , Harjinder Singh

We introduce a simulation technique to compute the free energy difference between two hydrate structures of different stoichiometry connected to a reservoir of gas molecules at a prescribed pressure. The method permits the determination of…

Chemical Physics · Physics 2026-04-16 Olivia S. Moro , Nigel B. Wilding , Vincent Ballenegger

Modern randomization methods in clinical trials are invariably adaptive, meaning that the assignment of the next subject to a treatment group uses the accumulated information in the trial. Some of the recent adaptive randomization methods…

Methodology · Statistics 2024-02-12 Alan R. Vazquez , Weng Kee Wong

The partition function and free energy of a quantum many-body system determine its physical properties in thermal equilibrium. Here we study the computational complexity of approximating these quantities for $n$-qubit local Hamiltonians.…

Quantum Physics · Physics 2023-09-22 Sergey Bravyi , Anirban Chowdhury , David Gosset , Pawel Wocjan

The dynamics of phase transitions plays a crucial r\^ole in the so-called interface between high energy particle physics and cosmology. Many of the interesting results generated during the last fifteen years or so rely on simplified…

High Energy Physics - Phenomenology · Physics 2007-05-23 Marcelo Gleiser

The Fourier-Galerkin method (in short FFTH) has gained popularity in numerical homogenisation because it can treat problems with a huge number of degrees of freedom. Because the method incorporates the fast Fourier transform (FFT) in the…

Numerical Analysis · Mathematics 2020-02-14 Jaroslav Vondřejc , Tom W. J. de Geus

Pre-calculated libraries of molecular fragment configurations have previously been used as a basis for both equilibrium sampling (via "library-based Monte Carlo") and for obtaining absolute free energies using a polymer-growth formalism.…

Quantitative Methods · Quantitative Biology 2018-12-26 Steven Lettieri , Artem B. Mamonov , Daniel M. Zuckerman

We develop a quantum algorithm for estimating the free energy as well as the total Gibbs state of interacting quantum Coulomb gases and molecular systems in dimensions $d \in \{2,3\}$ at finite temperature. These systems lie beyond the…

Quantum Physics · Physics 2026-04-17 Simon Becker , Cambyse Rouzé , Robert Salzmann

Double excitations are crucial to understanding numerous chemical, physical, and biological processes, but accurately predicting them remains a challenge. In this work, we explore the particle-particle random phase approximation (ppRPA) as…

Chemical Physics · Physics 2024-11-26 Jincheng Yu , Jiachen Li , Tianyu Zhu , Weitao Yang

Equilibrium free energy differences are given by exponential averages of nonequilibrium work values; such averages, however, often converge poorly, as they are dominated by rare realizations. I show that there is a simple and intuitively…

Statistical Mechanics · Physics 2009-11-11 Christopher Jarzynski

A computational revolution unleashed the power of artificial neural networks. At the heart of that revolution is automatic differentiation, which calculates the derivative of a performance measure relative to a large number of parameters.…

Quantitative Methods · Quantitative Biology 2023-12-27 Steven A. Frank

We present a method for determining the free energy of coexisting states from irreversible work measurements. Our approach is based on a fluctuation relation that is valid for dissipative transformations in partially equilibrated systems.…

Soft Condensed Matter · Physics 2009-02-21 Ivan Junier , Alessandro Mossa , Maria Manosas , Felix Ritort
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