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Two types of approaches to modeling molecular systems have demonstrated high practical efficiency. Density functional theory (DFT), the most widely used quantum chemical method, is a physical approach predicting energies and electron…

Chemical Physics · Physics 2020-03-02 Anton V. Sinitskiy , Vijay S. Pande

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

Classical density-functional theory provides an efficient alternative to molecular dynamics simulations for understanding the equilibrium properties of inhomogeneous fluids. However, application of density-functional theory to multi-site…

Computational Physics · Physics 2014-02-14 Ravishankar Sundararaman , T. A. Arias

Defects in crystalline silicon consisting of a silicon self-interstitial atom and one, two, three, or four hydrogen atoms are studied within density-functional theory (DFT). We search for low-energy defects by starting from an ensemble of…

Materials Science · Physics 2010-02-11 Andrew J. Morris , Chris J. Pickard , R. J. Needs

Kohn-Sham density functional theory is the base of modern computational approaches to electronic structures. Their accuracy vitally relies on the exchange-correlation energy functional, which encapsulates electron-electron interaction…

Computational Physics · Physics 2019-11-04 Ryo Nagai , Ryosuke Akashi , Osamu Sugino

Density Functional Theory (DFT) has become a cornerstone in the modeling of metals. However, accurately simulating metals, particularly under extreme conditions, presents two significant challenges. First, simulating complex metallic…

Chemical Physics · Physics 2024-03-08 Jake P. Vu , Ming Chen

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

Modern machine learning uses more and more advanced optimization techniques to find optimal hyper parameters. Whenever the objective function is non-convex, non continuous and with potentially multiple local minima, standard gradient…

Machine Learning · Computer Science 2019-02-13 Eric Benhamou , Jamal Atif , Rida Laraki

Classical density functional theory (cDFT) provides a systematic approach to predict the structure and thermodynamic properties of chemical systems through the single-molecule density profiles. Whereas the statistical-mechanical framework…

Chemical Physics · Physics 2024-11-07 Jinni Yang , Runtong Pan , Jikai Sun , Jianzhong Wu

Classical Density Functional Theory (DFT) is a statistical-mechanical framework to analyze fluids, which accounts for nanoscale fluid inhomogeneities and non-local intermolecular interactions. DFT can be applied to a wide range of…

Computational Engineering, Finance, and Science · Computer Science 2017-02-07 Andreas Nold , Benjamin D. Goddard , Peter Yatsyshin , Nikos Savva , Serafim Kalliadasis

We present a real-space formulation and higher-order finite-difference implementation of periodic Orbital-free Density Functional Theory (OF-DFT). Specifically, utilizing a local reformulation of the electrostatic and kernel terms, we…

Computational Physics · Physics 2015-12-23 Swarnava Ghosh , Phanish Suryanarayana

Hyperparameters of deep neural networks are often optimized by grid search, random search or Bayesian optimization. As an alternative, we propose to use the Covariance Matrix Adaptation Evolution Strategy (CMA-ES), which is known for its…

Neural and Evolutionary Computing · Computer Science 2016-04-26 Ilya Loshchilov , Frank Hutter

We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…

Computational Physics · Physics 2020-01-08 Sebastian Dick , Marivi Fernandez-Serra

Density-functional theory with extended Hubbard functionals (DFT+$U$+$V$) provides a robust framework to accurately describe complex materials containing transition-metal or rare-earth elements. It does so by mitigating self-interaction…

Materials Science · Physics 2025-01-30 Martin Uhrin , Austin Zadoks , Luca Binci , Nicola Marzari , Iurii Timrov

The growth of evolutionary computing (EC) methods in the exploration of complex potential energy landscapes of atomic and molecular clusters, as well as crystals over the last decade or so is reviewed. The trend of growth indicates that…

Materials Science · Physics 2015-09-02 Kanchan Sarkar , S. P. Bhattacharyya

Due to its favorable computational efficiency time-dependent (TD) density functional theory (DFT) enables the prediction of electronic spectra in a high-throughput manner across chemical space. Its predictions, however, can be quite…

We develop the theory of Energy Conserving Descent (ECD) and introduce ECDSep, a gradient-based optimization algorithm able to tackle convex and non-convex optimization problems. The method is based on the novel ECD framework of…

Machine Learning · Computer Science 2023-06-02 G. Bruno De Luca , Alice Gatti , Eva Silverstein

With the growth of computational resources, the scope of electronic structure simulations has increased greatly. Artificial intelligence and robust data analysis hold the promise to accelerate large-scale simulations and their analysis to…

Materials Science · Physics 2023-07-27 Lenz Fiedler , Karan Shah , Michael Bussmann , Attila Cangi

Density functional theory (DFT) is an essential building block for modern theoretical physics, chemistry, and engineering, especially those concerning electronic properties. Through decades of development, various program packages for…

Materials Science · Physics 2022-11-21 Yusuke Nomura , Ryosuke Akashi

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…

Materials Science · Physics 2013-02-25 Albert P. Bartok , Michael J. Gillan , Frederick R. Manby , Gabor Csanyi