Recent developments in the P<scp>y</scp>SCF program package

Sun, Qiming; Zhang, Xing; Banerjee, Samragni; Bao, Peng; Barbry, Marc; Blunt, Nick S.; Bogdanov, Nikolay A.; Booth, George H.; Chen, Jia; Cui, Zhi Hao; Eriksen, Janus J.; Gao, Yang; Guo, S.Y.; Hermann, Jan; Hermes, Matthew R.; Koh, Kevin J.; Koval, Peter; Lehtola, Susi; Li, Zhendong; Liu, Junzi; Mardirossian, Narbe; McClain, James; Motta, Mário; Mussard, Bastien; Pham, Hung Q.; Pulkin, Artem; Purwanto, Wirawan; Robinson, Paul; Ronca, Enrico; Sayfutyarova, Elvira R.; Scheurer, Maximilian; Schurkus, Henry F.; Smith, James E. T.; Sun, Chong; Sun, Shi Ning; Upadhyay, Shiv; Wagner, Lucas K.; Wang, Xiao; White, Alec F.; Whitfield, James D.; Williamson, Mark J.; Wouters, Sebastian; Yang, Jun; Yu, Jason M.; Zhu, Tianyu; Berkelbach, Timothy C.; Sharma, Sandeep; Sokolov, Alexander Yu.; Chan, Garnet

doi:10.1063/5.0006074

Cited by 691 publications

(496 citation statements)

References 161 publications

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“…We then rigidly shift the entire absorption spectrum by this finite-size correction, which is 0.1-0.4 eV for the materials and k-point meshes considered here. All calculations were performed with PySCF [48,49].…”

Section: Computational Detailsmentioning

confidence: 99%

Excitons in Solids from Periodic Equation-of-Motion Coupled-Cluster Theory

Wang

Berkelbach

2020

J. Chem. Theory Comput.

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We present an ab initio study of electronically excited states of three-dimensional solids using Gaussian-based periodic equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). The explicit use of translational symmetry, as implemented via Brillouin zone sampling and momentum conservation, is responsible for a large reduction in cost. Our largest system studied, which samples the Brillouin zone using 64 k-points (a 4 × 4 × 4 mesh) corresponds to a canonical EOM-CCSD calculation of 768 electrons in 640 orbitals. We study eight simple semiconductors and insulators, with direct singlet excitation energies in the range of 3 to 15 eV. Our predicted excitation energies exhibit a mean absolute error of 0.27 eV when compared to experiment. We furthermore calculate the energy of excitons with nonzero momentum and compare the exciton dispersion of LiF with experimental data from inelastic X-ray scattering. By calculating excitation energies under strain, we extract hydrostatic deformation potentials in order to quantify the strength of interactions between excitons and acoustic phonons. Our results indicate that coupled-cluster theory is a promising method for the accurate study of a variety of exciton phenomena in solids.

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Section: Computational Detailsmentioning

confidence: 99%

Excitons in Solids from Periodic Equation-of-Motion Coupled-Cluster Theory

Wang

Berkelbach

2020

J. Chem. Theory Comput.

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“…As a platform for our theoretical work on MBE‐FCI over the past couple of years, we have developed our own Python‐based, open‐source PyMBE code3. All electronic structure kernels within PyMBE are formulated upon the PySCF program, 32, 33 and the MPI4Python module handles parallel communication over the message passing interface (MPI) standard 34–36 …”

Section: Methodsmentioning

confidence: 99%

Incremental treatments of the full configuration interaction problem

Eriksen

Gauß

2021

WIREs Comput Mol Sci

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The recent many‐body expanded full configuration interaction (MBE‐FCI) method is reviewed by critically assessing its advantages and drawbacks in the context of contemporary near‐exact electronic structure theory. Besides providing a succinct summary of the history of MBE‐FCI to date within a generalized and unified theoretical setting, its finer algorithmic details are discussed alongside our optimized computational implementation of the theory. A selected few of the most recent applications of MBE‐FCI are revisited, before we close by outlining its future research directions as well as its place among modern near‐exact wave function‐based methods. This article is categorized under: Electronic Structure Theory > Ab Initio Electronic Structure Methods

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“…Coupled cluster natural orbitals and Löwdin orthogonalized atomic orbitals are obtained with PySCF [83][84][85]. DOCI-optimized orbitals are generated through an in-house DOSCF code and were carefully checked to correspond to the lowest possible DOCI energy, i.e.…”

Section: Applicationsmentioning

confidence: 99%

The seniority quantum number in Tensor Network States

Gunst

Neck

Limacher³

et al. 2021

SciPost Chem.

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We employ tensor network methods for the study of the seniority quantum number – defined as the number of unpaired electrons in a many-body wave function – in molecular systems. Seniority-zero methods recently emerged as promising candidates to treat strong static correlations in molecular systems, but are prone to deficiencies related to dynamical correlation and dispersion. We systematically resolve these deficiencies by increasing the allowed seniority number using tensor network methods. In particular, we investigate the number of unpaired electrons needed to correctly describe the binding of the neon and nitrogen dimer and the \mathbf{D_{6h}}D6h symmetry of benzene.

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Recent developments in the PySCF program package

Cited by 691 publications

References 161 publications

Excitons in Solids from Periodic Equation-of-Motion Coupled-Cluster Theory

Excitons in Solids from Periodic Equation-of-Motion Coupled-Cluster Theory

Incremental treatments of the full configuration interaction problem

The seniority quantum number in Tensor Network States

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