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Quantum computation offers significant potential for accelerating the simulation of molecules and materials through algorithms such as quantum phase estimation (QPE). However, the expected speedup in ground-state energy estimation depends…

Quantum Physics · Physics 2025-06-17 Zhendong Li

Using random walk sampling methods for feature learning on networks, we develop a method for generating low-dimensional node embeddings for directed graphs and identifying transition states of stochastic chemical reacting systems. We…

Numerical Analysis · Mathematics 2020-10-30 Paula Mercurio , Di Liu

We perform a thorough analysis on the choice of estimators for random series path integral methods. In particular, we show that both the thermodynamic (T-method) and the direct (H-method) energy estimators have finite variances and are…

Statistical Mechanics · Physics 2009-11-10 Cristian Predescu , Dubravko Sabo , J. D. Doll , David L. Freeman

Transition states and minimum energy paths are essential to understand and predict chemical reactivity. Double-ended methods represent a standard approach for their determination. We introduce a new double-ended method that optimizes…

Chemical Physics · Physics 2020-02-18 Alain C. Vaucher , Markus Reiher

A multilevel approach to sample the potential energy surface in a path integral formalism is proposed. The purpose is to reduce the required number of ab initio evaluations of energy and forces in ab initio path integral molecular dynamics…

Computational Physics · Physics 2014-12-22 Hua Y. Geng

Simulating chemical reactions is a central challenge in computational chemistry, characterized by an uneven difficulty profile: while equilibrium reactant and product geometries are often classically tractable, intermediate transition…

We present a methodology for accelerating the estimation of the free energy from path integral Monte Carlo simulations by considering an intermediate artificial reference system where interactions are inexpensive to evaluate numerically.…

The shift in chemical equilibria due to isotope substitution is often exploited to gain insight into a wide variety of chemical and physical processes. It is a purely quantum mechanical effect, which can be computed exactly using…

Statistical Mechanics · Physics 2014-07-04 Michele Ceriotti , Thomas E. Markland

The convergence of self-consistent field equations in mean-field nuclear-electronic orbital methods strongly depends on the choice of initial guesses for quantum nuclei. Although several such guesses have been proposed in the literature, a…

Chemical Physics · Physics 2026-02-18 Denis G. Artiukhin

Finding Minimum Energy Configurations (MECs) is essential in fields such as physics, chemistry, and materials science, as they represent the most stable states of the systems. In particular, identifying such MECs in multi-component alloys…

Materials Science · Physics 2025-01-27 Md Rajib Khan Musa , Yichen Qian , Jie Peng , David Cereceda

High-temperature reactions widely exist in nature. However, they are difficult to be characterized either experimentally or computationally. The routinely used minimum energy path (MEP) model in computational modeling of chemical reactions…

Chemical Physics · Physics 2020-05-13 Xiongzhi Zeng , Zongyang Qiu , Pai Li , Zhenyu Li , Jinlong Yang

Using a random-matrix approach and Monte-Carlo simulations, we generate scattering matrices and cross sections for compound-nucleus reactions. In the absence of direct reactions we compare the average cross sections with the analytic…

Nuclear Theory · Physics 2015-09-03 T. Kawano , P. Talou , H. A. Weidenmüller

Under certain conditions, the dynamics of coarse-grained models of solvated proteins can be described using a Markov state model, which tracks the evolution of populations of configurations. The transition rates among states that appear in…

Soft Condensed Matter · Physics 2022-09-26 Margarita Colberg , Jeremy Schofield

With an expected energy of 7.8(5) eV, the isomeric first excited state in $^{229}$Th exhibits the lowest excitation energy of all known nuclei. Until today, a value for the excitation energy has been inferred only by indirect measurements.…

Instrumentation and Detectors · Physics 2017-08-23 Benedict Seiferle , Lars von der Wense , Peter G. Thirolf

The Minimum Ignition Energy (MIE) of an initially Gaussian temperature profile is found both by Direct Numerical Simulations (DNS) and from a new novel model. The model is based on solving the heat diffusion equation in zero dimensions for…

Chemical Physics · Physics 2011-10-07 Jens Tarjei Jensen , Nils Erland L. Haugen , Natalia Babkovskaia

We introduce a rigorous method to microscopically compute the observables which characterize the thermodynamics and kinetics of rare macromolecular transitions for which it is possible to identify a priori a slow reaction coordinate. In…

Biomolecules · Quantitative Biology 2015-06-05 P. Faccioli , F. Pederiva

We compare the predicted phase behaviour of lead (Pb) using three different interatomic potential models, including an embedded atom method (EAM), a modified embedded atom method (MEAM), and a neural network-based machine-learned model in…

We present a Bayesian approach to identify optimal transformations that map model input points to low dimensional latent variables. The "projection" mapping consists of an orthonormal matrix that is considered a priori unknown and needs to…

Machine Learning · Statistics 2021-09-22 Panagiotis Tsilifis , Piyush Pandita , Sayan Ghosh , Valeria Andreoli , Thomas Vandeputte , Liping Wang

In finite systems, such as nanoparticles and gas-phase molecules, calculations of minimum energy paths (MEPs) connecting initial and final states of transitions as well as searches for saddle points are complicated by the presence of…

Chemical Physics · Physics 2015-06-09 Marko Melander , Kari Laasonen , Hannes Jonsson

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