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Calculating free energies is an important and notoriously difficult task for molecular simulations. The rapid increase in computational power has made it possible to probe increasingly complex systems, yet extracting accurate free energies…

Chemical Physics · Physics 2014-07-29 Viveca Lindahl , Jack Lidmar , Berk Hess

We revisit a unified methodology for the iterative solution of nonlinear equations in Hilbert spaces. Our key observation is that the general approach from [Heid & Wihler, Math. Comp. 89 (2020), Calcolo 57 (2020)] satisfies an energy…

Numerical Analysis · Mathematics 2021-02-18 Pascal Heid , Dirk Praetorius , Thomas P. Wihler

Accurate free-energy estimation is essential in molecular simulation, yet the periodic boundary conditions (PBC) commonly used in computer simulations have rarely been explicitly exploited. Equilibrium methods such as umbrella sampling,…

Statistical Mechanics · Physics 2025-11-03 Daniel Nagel , Tristan Bereau

We develop a novel data-driven approach to the inverse problem of classical statistical mechanics: given experimental data on the collective motion of a classical many-body system, how does one characterise the free energy landscape of that…

Statistical Mechanics · Physics 2022-03-01 Peter Yatsyshin , Serafim Kalliadasis , Andrew B. Duncan

This paper discusses predictive densities under the Kullback--Leibler loss for high-dimensional Poisson sequence models under sparsity constraints. Sparsity in count data implies zero-inflation. We present a class of Bayes predictive…

Statistics Theory · Mathematics 2020-09-08 Keisuke Yano , Ryoya Kaneko , Fumiyasu Komaki

We propose a new approach for metric learning by framing it as learning a sparse combination of locally discriminative metrics that are inexpensive to generate from the training data. This flexible framework allows us to naturally derive…

Machine Learning · Computer Science 2019-01-25 Yuan Shi , Aurélien Bellet , Fei Sha

We consider the prediction of a basic thermodynamic property---hydration free energies---across a large subset of the chemical space of small organic molecules. Our in silico study is based on computer simulations at the atomistic level…

Chemical Physics · Physics 2020-07-02 Clemens Rauer , Tristan Bereau

The last decade has seen an explosion in data sources available for the monitoring and prediction of environmental phenomena. While several inferential methods have been developed that make predictions on the underlying process by combining…

Methodology · Statistics 2023-03-06 Eun-Hye Yoo , Andrew Zammit-Mangion , Michael G. Chipeta

We present a new method to evaluate vibrational free energies of atomic systems without a priori specification of an interatomic potential. Our model-agnostic approach leverages descriptors, high-dimensional feature vectors of atomic…

Materials Science · Physics 2025-03-05 Thomas D Swinburne , Clovis Lapointe , Mihai-Cosmin Marinica

We derive the optimal estimates of the free energies of an arbitrary number of thermodynamic states from nonequilibrium work measurements; the work data are collected from forward and reverse switching processes and obey a fluctuation…

Statistical Mechanics · Physics 2009-11-11 Paul Maragakis , Martin Spichty , Martin Karplus

In this work we design and analyze a free energy satisfying finite difference method for solving Poisson-Nernst-Planck equations in a bounded domain. The algorithm is of second order in space, with numerical solutions satisfying all three…

Numerical Analysis · Mathematics 2015-06-17 Hailiang Liu , Zhongming Wang

The computation of free energies is a common issue in statistical physics. A natural technique to compute such high dimensional integrals is to resort to Monte Carlo simulations. However these techniques generally suffer from a high…

Statistical Mechanics · Physics 2021-05-17 Grégoire Ferré , Tobias Grafke

We present a new method to compute free energies at a quantum mechanical (QM) level of theory from molecular simulations using cheap reference potential energy functions, such as force fields. To overcome the poor overlap between the…

Computational Physics · Physics 2023-11-13 Andrea Rizzi , Paolo Carloni , Michele Parrinello

In this paper, I investigate more closely the recently proposed Free Energy Monte Carlo algorithm that is devised in particular for calculations where conventional Monte Carlo simulations struggle with ergodicity problems. The simplest…

Condensed Matter · Physics 2007-05-23 M. J. Thill

We introduce a new $hp$-adaptive strategy for self-adjoint elliptic boundary value problems that does not rely on using classical a posteriori error estimators. Instead, our approach is based on a generally applicable prediction strategy…

Numerical Analysis · Mathematics 2023-11-23 Patrick Bammer , Andreas Schröder , Thomas P. Wihler

A vast array of phenomena, ranging from chemical reactions to phase transformations, are analysed in terms of a free energy surface defined with respect to a single or multiple order parameters. Enhanced sampling methods are typically used,…

Statistical Mechanics · Physics 2023-04-26 Yagyik Goswami , Srikanth Sastry

We introduce a novel and powerful method for exploring the properties of the multidimensional free energy surfaces of complex many-body systems by means of a coarse-grained non-Markovian dynamics in the space defined by a few collective…

Statistical Mechanics · Physics 2009-11-07 A. Laio , M. Parrinello

The free energy landscapes of several fundamental processes are characterized by high barriers separating long-lived metastable states. In order to explore these type of landscapes enhanced sampling methods are used. While many such methods…

Chemical Physics · Physics 2019-04-12 Jayashrita Debnath , Michele Invernizzi , Michele Parrinello

We study the performance of sparse regression methods and propose new techniques to distill the governing equations of dynamical systems from data. We first look at the generic methodology of learning interpretable equation forms from data,…

Machine Learning · Computer Science 2019-03-25 Chinmay S. Kulkarni

Current mathematical frameworks for predicting the flux state and macromolecular composition of the cell do not rely on thermodynamic constraints to determine the spontaneous direction of reactions. These predictions may be biologically…

Optimization and Control · Mathematics 2020-08-14 Amir Akbari , Bernhard O. Palsson
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