Karton, Amir; Chan, Bun

Author(s)

Karton, Amir

Chan, Bun

Publication Date

2022-11

Abstract

Composite ab initio methods based on local coupled-cluster approaches calculate the CCSD(T)/CBS energy at a significantly reduced computational cost than the corresponding canonical methods. While showing promising performance for general thermochemistry, local composite ab initio methods have not been tested for fullerenes. Here we examine the performance of several local G4(MP2)-based methods for calculating the relative stability of a diverse set of C40 fullerenes. We use canonical G4(MP2) isomerization energies as reference data. Fullerenes provide a challenging problem for DLPNO-G4(MP2)-based methods. The DLPNO-based methods result in overall root-mean-square deviations (RMSDs) of 28.6 (NormalPNO with CCSD(T0)), 23.0 (NormalPNO with CCSD(T1)), and 16.1 (TightPNO with CCSD(T0)) kJ mol−1. The local natural orbital LNO-G4(MP2) method provides the best overall performance with an RMSD of 4.9 kJ mol−1. The DLPNO-G4(MP2) and LNO-G4(MP2) methods systematically overestimate the canonical G4(MP2) isomerization energies. Therefore, they provide valuable upper limits of the fullerene isomerization energies.

Citation

Computational and Theoretical Chemistry, v.1217, p. 1-7

ISSN

2210-2728

2210-271X

Link

https://hdl.handle.net/1959.11/56284

Publisher

Elsevier BV

Title

Performance of local G4(MP2) composite ab initio procedures for fullerene isomerization energies

Type of document

Journal Article

Entity Type

Publication

Author(s)	Karton, Amir Chan, Bun
Publication Date	2022-11
Abstract	<p>Composite ab initio methods based on local coupled-cluster approaches calculate the CCSD(T)/CBS energy at a significantly reduced computational cost than the corresponding canonical methods. While showing promising performance for general thermochemistry, local composite ab initio methods have not been tested for fullerenes. Here we examine the performance of several local G4(MP2)-based methods for calculating the relative stability of a diverse set of C<sub>40</sub> fullerenes. We use canonical G4(MP2) isomerization energies as reference data. Fullerenes provide a challenging problem for DLPNO-G4(MP2)-based methods. The DLPNO-based methods result in overall root-mean-square deviations (RMSDs) of 28.6 (NormalPNO with CCSD(T<sub>0</sub>)), 23.0 (NormalPNO with CCSD(T<sub>1</sub>)), and 16.1 (TightPNO with CCSD(T<sub>0</sub>)) kJ mol<sup>−1</sup>. The local natural orbital LNO-G4(MP2) method provides the best overall performance with an RMSD of 4.9 kJ mol<sup>−1</sup>. The DLPNO-G4(MP2) and LNO-G4(MP2) methods systematically overestimate the canonical G4(MP2) isomerization energies. Therefore, they provide valuable upper limits of the fullerene isomerization energies.</p>
Citation	Computational and Theoretical Chemistry, v.1217, p. 1-7
ISSN	2210-2728 2210-271X
Link	https://hdl.handle.net/1959.11/56284
Publisher	Elsevier BV
Title	Performance of local G4(MP2) composite ab initio procedures for fullerene isomerization energies
Type of document	Journal Article
Entity Type	Publication

Performance of local G4(MP2) composite ab initio procedures for fullerene isomerization energies

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