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Approximate semi-local density functional theory (DFT) is known to underestimate surface formation energies yet paradoxically overbind adsorbates on catalytic transition-metal oxide surfaces due to delocalization error. The low-cost DFT+U…

Materials Science · Physics 2021-11-24 Akash Bajaj , Heather J. Kulik

High-throughput DFT calculations are key to screening existing/novel materials, sampling potential energy surfaces, and generating quantum mechanical data for machine learning. By including a fraction of exact exchange (EXX), hybrid…

Existing molecular machine learning force fields (MLFFs) generally focus on the learning of atoms, molecules, and simple quantum chemical properties (such as energy and force), but ignore the importance of electron density (ED) $\rho(r)$ in…

Chemical Physics · Physics 2025-09-25 Hongxin Xiang , Ke Li , Mingquan Liu , Zhixiang Cheng , Bin Yao , Wenjie Du , Jun Xia , Li Zeng , Xin Jin , Xiangxiang Zeng

We present an accurate, efficient and massively parallel finite-element code, DFT-FE, for large-scale ab-initio calculations (reaching $\sim 100,000$ electrons) using Kohn-Sham density functional theory (DFT). DFT-FE is based on a local…

Computational Physics · Physics 2020-01-08 Phani Motamarri , Sambit Das , Shiva Rudraraju , Krishnendu Ghosh , Denis Davydov , Vikram Gavini

Deep learning has advanced efficient chemical process simulations on the surfaces, accelerating high-throughput materials screening and rational design in heterogeneous catalysis, energy storage and conversion, and gas separation. However,…

Disordered Systems and Neural Networks · Physics 2026-03-12 Zhihao Zhang , Xiao-Ming Cao

We perform quantum Monte Carlo (QMC) calculations to determine minimum energy pathways of simple chemical reactions, and compare the computed geometries and reaction barriers with those obtained with density functional theory (DFT) and…

Chemical Physics · Physics 2015-06-12 Sebastiano Saccani , Claudia Filippi , Saverio Moroni

Approximate density functional theory (DFT) has become indispensable owing to its cost-accuracy trade-off in comparison to more computationally demanding but accurate correlated wavefunction theory. To date, however, no single density…

Chemical Physics · Physics 2022-07-25 Chenru Duan , Aditya Nandy , Ralf Meyer , Naveen Arunachalam , Heather J. Kulik

Fermi operator expansion (FOE) methods are powerful alternatives to diagonalization type methods for solving Kohn-Sham density functional theory (KSDFT). One example is the pole expansion and selected inversion (PEXSI) method, which…

Computational Physics · Physics 2017-10-25 Weile Jia , Lin Lin

We present DFT-FE 1.0, building on DFT-FE 0.6 [Comput. Phys. Commun. 246, 106853 (2020)], to conduct fast and accurate large-scale density functional theory (DFT) calculations (reaching ~ $100,000$ electrons) on both many-core CPU and…

Computational Physics · Physics 2022-08-31 Sambit Das , Phani Motamarri , Vishal Subramanian , David M. Rogers , Vikram Gavini

Quantum chemistry simulations that accurately predict the properties of materials are among the most highly anticipated applications of quantum computing. It is widely believed that simulations running on quantum computers will allow for…

This article solves two major tasks that frequently arise in the theory of electron collisions with a target molecular cation. First, it extends the energy-dependent frame transformation treatment(EDFT), which is needed to map fixed-nuclei…

Chemical Physics · Physics 2025-11-25 David Hvizdos , Roman Curik , Chris H Greene

High-performance catalysts are crucial for sustainable energy conversion and human health. However, the discovery of catalysts faces challenges due to the absence of efficient approaches to navigating vast and high-dimensional structure and…

Machine Learning · Computer Science 2025-11-13 Jie Chen , Pengfei Ou , Yuxin Chang , Hengrui Zhang , Xiao-Yan Li , Edward H. Sargent , Wei Chen

We developed a general framework for hybrid quantum-classical computing of molecular and periodic embedding approaches based on an orbital space separation of the fragment and environment degrees of freedom. We demonstrate its potential by…

Chemical Physics · Physics 2024-12-23 Stefano Battaglia , Max Rossmannek , Vladimir V. Rybkin , Ivano Tavernelli , Jürg Hutter

Appropriately identifying and treating molecules and materials with significant multi-reference (MR) character is crucial for achieving high data fidelity in virtual high throughput screening (VHTS). Nevertheless, most VHTS is carried out…

Chemical Physics · Physics 2022-01-13 Chenru Duan , Daniel B. K. Chu , Aditya Nandy , Heather J. Kulik

We present a simplified density functional theory (DFT) method to com- pute vertical electron and hole attachment energies to frontier orbitals of molecules absorbed on insulating films supported by a metal substrate. The adsorbate and the…

Mesoscale and Nanoscale Physics · Physics 2017-08-29 Ivan Scivetti , Mats Persson

The accuracy of density-functional theory (DFT) is determined by the quality of the approximate functionals, such as exchange-correlation in electronic DFT and the excess functional in the classical DFT formalism of fluids. The exact…

Chemically accurate and comprehensive studies of the virtual space of all possible molecules are severely limited by the computational cost of quantum chemistry. We introduce a composite strategy that adds machine learning corrections to…

Chemical Physics · Physics 2023-04-14 Raghunathan Ramakrishnan , Pavlo O. Dral , Matthias Rupp , O. Anatole von Lilienfeld

Density functional theory (DFT) is the most widely used method for calculating molecular properties; however, its accuracy is often insufficient for quantitative predictions. Coupled-cluster (CC) theory is the most successful method for…

We introduce a rapid, accurate framework for computing atomic migration barriers in crystals by combining universal machine learning force fields (MLFFs) with 3D potential energy surface sampling and interpolation. Our method suppresses…

Materials Science · Physics 2025-10-01 Hanwen Kang , Tenglong Lu , Zhanbin Qi , Jiandong Guo , Sheng Meng , Miao Liu

Energy evaluation using fast Fourier transforms enables sampling billions of putative complex structures and hence revolutionized rigid protein-protein docking. However, in current methods efficient acceleration is achieved only in either…