Accurate thermochemistry of covalent and ionic solids from spin-component-scaled MP2

Tamar Goldzak; Xiao Wang; Hong Zhou Ye; Timothy C. Berkelbach

doi:10.1063/5.0119633

Accurate thermochemistry of covalent and ionic solids from spin-component-scaled MP2

Tamar Goldzak
, Xiao Wang
, Hong Zhou Ye
, Timothy C. Berkelbach

Columbia University
Simons Foundation

Research output: Contribution to journal › Article › peer-review

8 Scopus citations

Abstract

We study the performance of spin-component-scaled second-order Møller-Plesset perturbation theory (SCS-MP2) for the prediction of the lattice constant, bulk modulus, and cohesive energy of 12 simple, three-dimensional covalent and ionic semiconductors and insulators. We find that SCS-MP2 and the simpler scaled opposite-spin MP2 (SOS-MP2) yield predictions that are significantly improved over the already good performance of MP2. Specifically, when compared to experimental values with zero-point vibrational corrections, SCS-MP2 (SOS-MP2) yields mean absolute errors of 0.015 (0.017) Å for the lattice constant, 3.8 (3.7) GPa for the bulk modulus, and 0.06 (0.08) eV for the cohesive energy, which are smaller than those of leading density functionals by about a factor of two or more. We consider a reparameterization of the spin-scaling parameters and find that the optimal parameters for these solids are very similar to those already in common use in molecular quantum chemistry, suggesting good transferability and reliable future applications to surface chemistry on insulators.

Original language	English
Article number	174112
Journal	Journal of Chemical Physics
Volume	157
Issue number	17
DOIs	https://doi.org/10.1063/5.0119633
State	Published - 7 Nov 2022
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2022 Author(s).

Funding

This work was supported by the National Science Foundation under Grant No. CHE-1848369 (T.G.) and Grant No. OAC-1931321 (H.-Z.Y.). We acknowledge the computing resources provided by Columbia University’s Shared Research Computing Facility project, which is supported by NIH Research Facility Improvement Grant No. 1G20RR030893-01, and associated funds from the New York State Empire State Development, Division of Science Technology and Innovation (NYSTAR) Contract No. C090171, both awarded April 15, 2010. The Flatiron Institute is a division of the Simons Foundation.

Funders	Funder number
New York State Empire State Development
National Science Foundation	OAC-1931321, CHE-1848369
National Institutes of Health	1G20RR030893-01
Columbia University
Empire State Development's Division of Science, Technology and Innovation	C090171

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Cite this

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abstract = "We study the performance of spin-component-scaled second-order M{\o}ller-Plesset perturbation theory (SCS-MP2) for the prediction of the lattice constant, bulk modulus, and cohesive energy of 12 simple, three-dimensional covalent and ionic semiconductors and insulators. We find that SCS-MP2 and the simpler scaled opposite-spin MP2 (SOS-MP2) yield predictions that are significantly improved over the already good performance of MP2. Specifically, when compared to experimental values with zero-point vibrational corrections, SCS-MP2 (SOS-MP2) yields mean absolute errors of 0.015 (0.017) {\AA} for the lattice constant, 3.8 (3.7) GPa for the bulk modulus, and 0.06 (0.08) eV for the cohesive energy, which are smaller than those of leading density functionals by about a factor of two or more. We consider a reparameterization of the spin-scaling parameters and find that the optimal parameters for these solids are very similar to those already in common use in molecular quantum chemistry, suggesting good transferability and reliable future applications to surface chemistry on insulators.",

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AB - We study the performance of spin-component-scaled second-order Møller-Plesset perturbation theory (SCS-MP2) for the prediction of the lattice constant, bulk modulus, and cohesive energy of 12 simple, three-dimensional covalent and ionic semiconductors and insulators. We find that SCS-MP2 and the simpler scaled opposite-spin MP2 (SOS-MP2) yield predictions that are significantly improved over the already good performance of MP2. Specifically, when compared to experimental values with zero-point vibrational corrections, SCS-MP2 (SOS-MP2) yields mean absolute errors of 0.015 (0.017) Å for the lattice constant, 3.8 (3.7) GPa for the bulk modulus, and 0.06 (0.08) eV for the cohesive energy, which are smaller than those of leading density functionals by about a factor of two or more. We consider a reparameterization of the spin-scaling parameters and find that the optimal parameters for these solids are very similar to those already in common use in molecular quantum chemistry, suggesting good transferability and reliable future applications to surface chemistry on insulators.

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Accurate thermochemistry of covalent and ionic solids from spin-component-scaled MP2

Abstract

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