The Staggered Mesh Method: Accurate Exact Exchange Toward the Thermodynamic Limit for Solids DOI
Stephen Jon Quiton,

Hamlin Wu,

Xin Xing

и другие.

Journal of Chemical Theory and Computation, Год журнала: 2024, Номер unknown

Опубликована: Авг. 30, 2024

In periodic systems, the Hartree-Fock (HF) exchange energy exhibits slowest convergence of all HF components as system size approaches thermodynamic limit. We demonstrate that recently proposed staggered mesh method for Fock [Xing, Li, and Lin, Math. Comp., 2024], which is specifically designed to sidestep certain singularities in evaluation, can expedite finite-size rate exact across a range insulators semiconductors when compared regular truncated Coulomb methods. This remains true even two computationally cheaper versions this new method, we call non-SCF split-SCF mesh. Additionally, sequence numerical tests on simple solids showcases method's ability improve toward limit band gaps, bulk moduli, equilibrium lattice dimensions, energies, phonon force constants.

Язык: Английский

Condensed‐Phase Quantum Chemistry DOI
Paul J. Robinson, Adam Rettig, Hieu Q. Dinh

и другие.

Wiley Interdisciplinary Reviews Computational Molecular Science, Год журнала: 2025, Номер 15(1)

Опубликована: Янв. 1, 2025

ABSTRACT Molecular quantum chemistry has seen enormous progress in the last few decades thanks to more advanced and sophisticated numerical techniques computing power. Following recent interest extending these capabilities condensed‐phase problems, we summarize basic knowledge of for readers with experience molecular chemistry. We highlight efforts this direction, including solving electron repulsion integrals bottleneck, implementing hybrid density functional theory wavefunction methods, simulating lattice dynamics periodic systems within atom‐centered basis sets. Many computational presented here are inspired by extensive method developments rooted In Focus Article, selectively focus on chemistry, emphasize some challenges, point out open questions. hope our perspectives will encourage researchers pursue exciting promising research avenue.

Язык: Английский

Процитировано

1
Multi-GPU RI-HF Energies and Analytic Gradients─Toward High-Throughput Ab Initio Molecular Dynamics DOI
Ryan Stocks, Elise Palethorpe,

Giuseppe M. J. Barca

и другие.

Journal of Chemical Theory and Computation, Год журнала: 2024, Номер 20(17), С. 7503 - 7515

Опубликована: Авг. 28, 2024

This article presents an optimized algorithm and implementation for calculating resolution-of-the-identity Hartree-Fock (RI-HF) energies analytic gradients using multiple graphics processing units (GPUs). The is especially designed high throughput ab initio molecular dynamics simulations of small medium size molecules (10-100 atoms). Key innovations this work include the exploitation multi-GPU parallelism a workload balancing scheme that efficiently distributes computational tasks among GPUs. Our also employs techniques symmetry utilization, integral screening, leveraging sparsity to optimize memory usage. Computational results show achieves significant performance improvements, including over 3 × speedups in single GPU AIMD compared previous GPU-accelerated RI-HF traditional HF methods. Furthermore, utilizing GPUs can provide superlinear speedup when additional aggregate allows storage decompressed three-center integrals.

Язык: Английский

Процитировано

5
A general framework for active space embedding methods with applications in quantum computing DOI Creative Commons
Stefano Battaglia, Max Rossmannek, Vladimir V. Rybkin

и другие.

npj Computational Materials, Год журнала: 2024, Номер 10(1)

Опубликована: Дек. 19, 2024

We developed a general framework for hybrid quantum-classical computing of molecular and periodic embedding approaches based on an orbital space separation the fragment environment degrees freedom. demonstrate its potential by presenting specific implementation range-separated DFT coupled to quantum circuit ansatz, whereby variational eigensolver equation-of-motion algorithm are used obtain low-lying spectrum embedded Hamiltonian. The application this scheme study localized electronic states in materials is showcased through accurate prediction optical properties neutral oxygen vacancy magnesium oxide (MgO). Despite some discrepancies position main absorption band, method demonstrates competitive performance compared state-of-the-art ab initio approaches, particularly evidenced excellent agreement with experimental photoluminescence emission peak.

Язык: Английский

Процитировано

4
Efficient Hybrid-Functional-Based Force and Stress Calculations for Periodic Systems with Thousands of Atoms DOI
Peize Lin, Yuyang Ji, Lixin He

и другие.

Journal of Chemical Theory and Computation, Год журнала: 2025, Номер unknown

Опубликована: Март 20, 2025

We present an efficient linear-scaling algorithm for evaluating the analytical force and stress contributions derived from exact-exchange energy, a key component in hybrid functional calculations. The algorithm, working equally well molecular periodic systems, is formulated within framework of numerical atomic orbital (NAO) basis sets takes advantage localized resolution-of-identity (LRI) technique treating two-electron Coulomb repulsion integrals. behavior realized by fully exploiting sparsity expansion coefficients resulting strict locality NAOs LRI ansatz. Our implementation massively parallel, enables structural relaxation based on density functionals bulk materials containing thousands atoms. In this work, we will detailed description our benchmark performance using illustrating examples. By optimizing structures pristine doped halide perovskite material CsSnI3 with different functionals, find that presence lattice strain, provide more accurate stereochemical expression lone pair.

Язык: Английский

Процитировано

0
Distance-based screening of short-range integrals for periodic systems in Q-Chem DOI
Hieu Q. Dinh, Adam Rettig, Xintian Feng

и другие.

Advances in quantum chemistry, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Язык: Английский

Процитировано

0
Efficient all-electron hybrid density functionals for atomistic simulations beyond 10 000 atoms DOI
Sebastian Kokott,

F. Merz,

Yi Yao

и другие.

The Journal of Chemical Physics, Год журнала: 2024, Номер 161(2)

Опубликована: Июль 11, 2024

Hybrid density functional approximations (DFAs) offer compelling accuracy for ab initio electronic-structure simulations of molecules, nanosystems, and bulk materials, addressing some deficiencies computationally cheaper, frequently used semilocal DFAs. However, the computational bottleneck hybrid DFAs is evaluation non-local exact exchange contribution, which limiting factor application method large-scale simulations. In this work, we present a drastically optimized resolution-of-identity-based real-space implementation both non-periodic periodic boundary conditions in all-electron code FHI-aims, targeting high-performance central processing unit (CPU) compute clusters. The introduction several new refined message passing interface (MPI) parallelization layers shared memory arrays according to MPI-3 standard were key components optimization. We demonstrate significant improvements performance efficiency, scalability, workload distribution, extending reach simulation sizes beyond ten thousand atoms. addition, also compare runtime PBE, HSE06, PBE0 functionals. As necessary byproduct other parts FHI-aims have been as well, e.g., computation Hartree potential force stress components. benchmark scaling DFA-based broad range chemical systems, including organic–inorganic perovskites, organic crystals, ice crystals with up 30 576 atoms (101 920 electrons described by 244 608 basis functions).

Язык: Английский

Процитировано

1
The role of the exact Hartree-Fock exchange in the investigation of defects in crystalline systems. DOI
Alexander Platonenko, Francesco Silvio Gentile,

Khaled E. El‐Kelany

и другие.

Physical Chemistry Chemical Physics, Год журнала: 2024, Номер unknown

Опубликована: Янв. 1, 2024

The role of the exact Hartree–Fock (HF) exchange in determining band gap and other properties defects crystalline solids is investigated. Two vacancy-hydrogen diamond, VH d q , are used as test cases.

Язык: Английский

Процитировано

0
The Staggered Mesh Method: Accurate Exact Exchange Toward the Thermodynamic Limit for Solids DOI
Stephen Jon Quiton,

Hamlin Wu,

Xin Xing

и другие.

Journal of Chemical Theory and Computation, Год журнала: 2024, Номер unknown

Опубликована: Авг. 30, 2024

In periodic systems, the Hartree-Fock (HF) exchange energy exhibits slowest convergence of all HF components as system size approaches thermodynamic limit. We demonstrate that recently proposed staggered mesh method for Fock [Xing, Li, and Lin, Math. Comp., 2024], which is specifically designed to sidestep certain singularities in evaluation, can expedite finite-size rate exact across a range insulators semiconductors when compared regular truncated Coulomb methods. This remains true even two computationally cheaper versions this new method, we call non-SCF split-SCF mesh. Additionally, sequence numerical tests on simple solids showcases method's ability improve toward limit band gaps, bulk moduli, equilibrium lattice dimensions, energies, phonon force constants.

Язык: Английский

Процитировано

0