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Energy-Based Models (EBMs) have proven to be a highly effective approach for modelling densities on finite-dimensional spaces. Their ability to incorporate domain-specific choices and constraints into the structure of the model through…

Machine Learning · Computer Science 2023-02-24 Jen Ning Lim , Sebastian Vollmer , Lorenz Wolf , Andrew Duncan

We present a new simulation method to calculate the free energy and the chemical potential of hard particle systems. The method relies on the introduction of a parameter dependent potential to smoothly transform between the hard particle…

Chemical Physics · Physics 2015-05-30 Hitomi Nomura , Tomonori Koda , Akihiro Nishioka , Ken Miyata

The multiple range random walk algorithm recently proposed by Wang and Landau [Phys. Rev. Lett. 86, 2050 (2001)] is adapted to the computation of free energy profiles for molecular systems along reaction coordinates. More generally, we show…

Statistical Mechanics · Physics 2009-11-07 F. Calvo

The conventional evaluation protocols on machine learning models rely heavily on a labeled, i.i.d-assumed testing dataset, which is not often present in real world applications. The Automated Model Evaluation (AutoEval) shows an alternative…

Machine Learning · Computer Science 2024-03-18 Ru Peng , Heming Zou , Haobo Wang , Yawen Zeng , Zenan Huang , Junbo Zhao

We introduce a computational method for global optimization of structure and ordering in atomic systems. The method relies on interpolation between chemical elements, which is incorporated in a machine learning structural fingerprint. The…

Materials Science · Physics 2021-10-18 Sami Kaappa , Casper Larsen , Karsten Wedel Jacobsen

This article is concerned with the mathematical analysis of a family of adaptive importance sampling algorithms applied to diffusion processes. These methods, referred to as Adaptive Biasing Potential methods, are designed to efficiently…

Probability · Mathematics 2018-05-10 Michel Benaïm , Charles-Edouard Bréhier

We introduce a simple enhanced sampling approach for the calculation of free energy differences and barriers along a one-dimensional reaction coordinate. First, a small number of short nonequilibrium simulations are carried out along the…

Chemical Physics · Physics 2021-11-03 Kristof M. Bal

In order to efficiently explore the chemical space of all possible small molecules, a common approach is to compress the dimension of the system to facilitate downstream machine learning tasks. Towards this end, we present a data driven…

Biomolecules · Quantitative Biology 2024-01-23 Paula Mercurio , Di Liu

The free energetics of water density fluctuations in bulk water, at interfaces, and in hydrophobic confinement inform the hydration of hydrophobic solutes as well as their interactions and assembly. The characterization of such free…

Statistical Mechanics · Physics 2018-03-15 Erte Xi , Sean M. Marks , Suruchi Fialoke , Amish J. Patel

The multistate Bennett Acceptance Ratio is provably the lowest variance unbiased estimator of both free energies and ensemble averages, and has a number of important advantages over previous methods, such as WHAM. Despite its advantages,…

Statistical Mechanics · Physics 2017-12-20 Michael R. Shirts

Thermodynamic properties can be in principle derived from the partition function, which, in many-atom systems, is hard to evaluate as it involves a sum on the accessible microscopic states. Recently, the partition function has been computed…

A generic algorithm for the extraction of probabilistic (Bayesian) information about model parameters from data is presented. The algorithm propagates an ensemble of particles in the product space of model parameters and outputs. Each…

Computation · Statistics 2015-09-18 Carlo Albert

It is possible in principle to probe the many--atom potential surface using density functional theory (DFT). This will allow us to apply DFT to the Hamiltonian formulation of atomic motion in monatomic liquids [\textit{Phys. Rev. E} {\bf…

The adsorption energy of benzene on various metal substrates is predicted using the random phase approximation (RPA) for the correlation energy. Agreement with available experimental data is systematically better than 10% for both coinage…

Chemical Physics · Physics 2017-11-29 J. A. Garrido Torres , B. Ramberger , H. Früchtl , R. Schaub , G. Kresse

We present a scheme to obtain an inexpensive and reliable estimate of the uncertainty associated with the predictions of a machine-learning model of atomic and molecular properties. The scheme is based on resampling, with multiple models…

Chemical Physics · Physics 2025-10-06 Felix Musil , Michael J. Willatt , Mikhail A. Langovoy , Michele Ceriotti

The aim of this work is to propose a meta-algorithm for automatic classification in the presence of discrete binary classes. Classifier learning in the presence of overlapping class distributions is a challenging problem in machine…

Machine Learning · Statistics 2020-01-22 Vidhi Lalchand

Quantum sensors can potentially achieve the Heisenberg limit of sensitivity over a large dynamic range using quantum algorithms. The adaptive phase estimation algorithm (PEA) is one example that was proven to achieve such high sensitivities…

The energy test is a powerful binning-free, multi-dimensional and distribution-free tool that can be applied to compare a measurement to a given prediction (goodness-of-fit) or to check whether two data samples originate from the same…

Data Analysis, Statistics and Probability · Physics 2018-04-30 G. Zech

Kinetic proofreading mechanisms explain the extraordinary accuracy observed in central biological events in terms of the enhanced specificity of substrate selection networks under a nonequilibrium environment. The nonequilibrium steady…

Adaptation and Self-Organizing Systems · Physics 2022-06-29 Premashis Kumar , Kinshuk Banerjee , Gautam Gangopadhyay

We present a new interatomic potential for water captured in a charge-transfer embedded atom method (EAM) framework. The potential accounts for explicit, dynamical charge transfer in atoms as a function of the local chemical environment. As…

Materials Science · Physics 2007-05-23 Krishna Muralidharan , Steven M. Valone , Susan R. Atlas