Communication: A difference density picture for the self-consistent field ansatz

Parrish, Robert M.; Liu, Fang; Martı́nez, Todd J.

doi:10.1063/1.4945277

Cited by 8 publications

(6 citation statements)

References 48 publications

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“…If we had started from a functional that includes Fock‐exchange, the Hartree energy terms would correspond to Hartree–Fock‐like energy expressions (cf. Reference 50). This is just mentioned for the sake of completeness, but not discussed further at this point.…”

Section: Theorymentioning

confidence: 99%

Extended tight‐binding quantum chemistry methods

Bannwarth

Caldeweyher

Ehlert

et al. 2020

WIREs Comput Mol Sci

851

964

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This review covers a family of atomistic, mostly quantum chemistry (QC) based semiempirical methods for the fast and reasonably accurate description of large molecules in gas and condensed phase. The theory is derived from a density functional (DFT) perturbation expansion of the electron density in fluctuation terms to various orders similar to the original density functional tight binding model. The term “eXtended” in their name (xTB) emphasizes the parameter availability for almost the entire periodic table of elements (Z ≤ 86) and improvements of the underlying theory regarding, for example, the atomic orbital basis set, the level of multipole approximation and the treatment of the important electrostatic and dispersion interactions. A common feature of most members is their consistent parameterization on accurate gas phase theoretical reference data for geometries, vibrational frequencies and noncovalent interactions, which are the primary properties of interest in typical applications to systems composed of up to a few thousand atoms. Further specialized versions were developed for the description of electronic spectra and corresponding response properties. Besides a provided common theoretical background with some important implementation details in the efficient and free xtb program, various benchmarks for structural and thermochemical properties including (transition‐)metal systems are discussed. The review is completed by recent extensions of the model to the force‐field (FF) level as well as its application to solids under periodic boundary conditions. The general applicability together with the excellent cost‐accuracy ratio and the high robustness make the xTB family of methods very attractive for various fields of computer‐aided chemical research. This article is categorized under: Electronic Structure Theory > Ab Initio Electronic Structure Methods Electronic Structure Theory > Semiempirical Electronic Structure Methods Software > Quantum Chemistry

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Section: Theorymentioning

confidence: 99%

Extended tight‐binding quantum chemistry methods

Bannwarth

Caldeweyher

Ehlert

et al. 2020

WIREs Comput Mol Sci

851

964

View full text Add to dashboard Cite

show abstract

“…Mixed precision optimization is an emerging method for accelerate quantum chemistry methods, include the integral evaluation 109,110 , the SCF iteration 111 and the CC method 112 . Previous works showed that using single-precision instead of double precision can achieve a better computational efficiency while maintaining the chemical accuracy.…”

Section: Mixed Precisionmentioning

confidence: 99%

Kylin 1.0: An Ab-Initio Density Matrix Renormalization Group Quantum Chemistry Program

Xie

Song

Peng

et al. 2022

Preprint

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The accurate evaluation of electron correlations is highly necessary for the proper descriptions of the electronic structures in strongly correlated molecules, ranging from bond-dissociating molecules, polyradicals, to large conjugated molecules and transition metal complexes. For this purpose, in this paper, a new ab-initio quantum chemistry program Kylin 1.0 for electron correlation calculations at various quantum many-body levels, including configuration interaction (CI), perturbation theory (PT), and density matrix renormalization group (DMRG), is presented. In addtion, fundamental quantum chemical methods such as Hartree-Fock self-consistent field (HF-SCF) and the complete active space SCF (CASSCF) are aslo implemented. The Kylin 1.0 program possesses these features: (1) efficient DMRG implementation based on the matrix product operator (MPO) formulation for describing static electron correlation within a large active space composed of more than 100 orbitals, supporting both $\rm U(1)_{n} \times U(1)_{S_z}$ and $\rm U(1)_{n} \times SU(2)_{S}$ symmetries; (2) efficient second-order DMRG-self-consistent field (SCF) implementation; (3) externally-contracted multi-reference CI (MRCI) and Epstein-Nesbet PT with DMRG reference wave functions for including the remaining dynamic electron correlation outside the large active spaces. In this paper, we introduce the capabilities and numerical benchmark examples of the Kylin 1.0 program.

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“…They achieved substantial speedup in systems with various sizes by finding the empirical relationship between the thresholds and errors. We also note that to accelerate electronic structure calculations, SP was used for an initial guess, and then the rest of the calculations were performed with DP. ,, However, there has been no systematic study on the DynP approach for eigenvalue problems. The large-scale eigenvalue problem is one of the time-consuming processes in electronic structure calculations.…”

Section: Introductionmentioning

confidence: 99%

Dynamic Precision Approach for Accelerating Large-Scale Eigenvalue Solvers in Electronic Structure Calculations on Graphics Processing Units

Woo

Kim

2023

J. Chem. Theory Comput.

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Single precision (SP) arithmetic can be greatly accelerated as compared to double precision (DP) arithmetic on graphics processing units (GPUs). However, the use of SP in the whole process of electronic structure calculations is inappropriate for the required accuracy. We propose a 3-fold dynamic precision approach for accelerated calculations but still with the accuracy of DP. Here, SP, DP, and mixed precision are dynamically switched during an iterative diagonalization process. We applied this approach to the locally optimal block preconditioned conjugate gradient method to accelerate a large-scale eigenvalue solver for the Kohn–Sham equation. We determined a proper threshold for switching each precision scheme by examining the convergence pattern on the eigenvalue solver only with the kinetic energy operator of the Kohn–Sham Hamiltonian. As a result, we achieved up to 8.53× and 6.60× speedups for band structure and self-consistent field calculations, respectively, for test systems under various boundary conditions on NVIDIA GPUs.

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Communication: A difference density picture for the self-consistent field ansatz

Cited by 8 publications

References 48 publications

Extended tight‐binding quantum chemistry methods

Extended tight‐binding quantum chemistry methods

Kylin 1.0: An Ab-Initio Density Matrix Renormalization Group Quantum Chemistry Program

Dynamic Precision Approach for Accelerating Large-Scale Eigenvalue Solvers in Electronic Structure Calculations on Graphics Processing Units

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