A low-cost four-component relativistic equation of motion coupled cluster method based on frozen natural spinors: Theory, Implementation and Benchmark

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Main Authors: Surjuse, Kshitijkumar, Chamoli, Somesh, Nayak, Malaya K., Dutta, Achintya Kumar
Format: Preprint
Published: 2022
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author Surjuse, Kshitijkumar
Chamoli, Somesh
Nayak, Malaya K.
Dutta, Achintya Kumar
author_facet Surjuse, Kshitijkumar
Chamoli, Somesh
Nayak, Malaya K.
Dutta, Achintya Kumar
contents We present the theory and the implementation of a low-cost four-component relativistic equation of motion coupled cluster method for ionized states based on frozen natural spinors. A single threshold (natural spinor occupancy) can control the accuracy of the calculated ionization potential values. Frozen natural spinors can significantly reduce the computational cost for valence and core-ionization energies with systematically controllable accuracy. The convergence of the ionization potential values with respect to the natural spinor occupancy threshold becomes slower with the increase in basis set dimension. However, the use of a natural spinor threshold of 10-5 and 10-6 gives excellent agreement with experimental results for valence and core ionization energies, respectively.
format Preprint
id arxiv_https___arxiv_org_abs_2207_08627
institution arXiv
publishDate 2022
record_format arxiv
spellingShingle A low-cost four-component relativistic equation of motion coupled cluster method based on frozen natural spinors: Theory, Implementation and Benchmark
Surjuse, Kshitijkumar
Chamoli, Somesh
Nayak, Malaya K.
Dutta, Achintya Kumar
Chemical Physics
We present the theory and the implementation of a low-cost four-component relativistic equation of motion coupled cluster method for ionized states based on frozen natural spinors. A single threshold (natural spinor occupancy) can control the accuracy of the calculated ionization potential values. Frozen natural spinors can significantly reduce the computational cost for valence and core-ionization energies with systematically controllable accuracy. The convergence of the ionization potential values with respect to the natural spinor occupancy threshold becomes slower with the increase in basis set dimension. However, the use of a natural spinor threshold of 10-5 and 10-6 gives excellent agreement with experimental results for valence and core ionization energies, respectively.
title A low-cost four-component relativistic equation of motion coupled cluster method based on frozen natural spinors: Theory, Implementation and Benchmark
topic Chemical Physics
url https://arxiv.org/abs/2207.08627