Numerical and Theoretical Aspects of the DMRG-TCC Method Exemplified by the Nitrogen Dimer

Fabian M. Faulstich, Mihály Máté, Andre Laestadius, Mihály András Csirik, Libor Veis, Andrej Antalik, Jiří Brabec, Reinhold Schneider, Jiří Pittner, Simen Kvaal, O. Legeza

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

In this article, we investigate the numerical and theoretical aspects of the coupled-cluster method tailored by matrix-product states. We investigate formal properties of the used method, such as energy size consistency and the equivalence of linked and unlinked formulation. The existing mathematical analysis is here elaborated in a quantum chemical framework. In particular, we highlight the use of what we have defined as a complete active space-external space gap describing the basis splitting between the complete active space and the external part generalizing the concept of a HOMO-LUMO gap. Furthermore, the behavior of the energy error for an optimal basis splitting, i.e., an active space choice minimizing the density matrix renormalization group-tailored coupled-cluster singles doubles error, is discussed. We show numerical investigations on the robustness with respect to the bond dimensions of the single orbital entropy and the mutual information, which are quantities that are used to choose a complete active space. Moreover, the dependence of the ground-state energy error on the complete active space has been analyzed numerically in order to find an optimal split between the complete active space and external space by minimizing the density matrix renormalization group-tailored coupled-cluster error.

Original languageEnglish
Pages (from-to)2206-2220
Number of pages15
JournalJournal of Chemical Theory and Computation
Volume15
Issue number4
DOIs
Publication statusPublished - Apr 9 2019

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Dimers
Nitrogen
dimers
nitrogen
Ground state
Entropy
applications of mathematics
equivalence
energy
entropy
formulations
orbitals
ground state
products

ASJC Scopus subject areas

  • Computer Science Applications
  • Physical and Theoretical Chemistry

Cite this

Numerical and Theoretical Aspects of the DMRG-TCC Method Exemplified by the Nitrogen Dimer. / Faulstich, Fabian M.; Máté, Mihály; Laestadius, Andre; Csirik, Mihály András; Veis, Libor; Antalik, Andrej; Brabec, Jiří; Schneider, Reinhold; Pittner, Jiří; Kvaal, Simen; Legeza, O.

In: Journal of Chemical Theory and Computation, Vol. 15, No. 4, 09.04.2019, p. 2206-2220.

Research output: Contribution to journalArticle

Faulstich, FM, Máté, M, Laestadius, A, Csirik, MA, Veis, L, Antalik, A, Brabec, J, Schneider, R, Pittner, J, Kvaal, S & Legeza, O 2019, 'Numerical and Theoretical Aspects of the DMRG-TCC Method Exemplified by the Nitrogen Dimer', Journal of Chemical Theory and Computation, vol. 15, no. 4, pp. 2206-2220. https://doi.org/10.1021/acs.jctc.8b00960
Faulstich, Fabian M. ; Máté, Mihály ; Laestadius, Andre ; Csirik, Mihály András ; Veis, Libor ; Antalik, Andrej ; Brabec, Jiří ; Schneider, Reinhold ; Pittner, Jiří ; Kvaal, Simen ; Legeza, O. / Numerical and Theoretical Aspects of the DMRG-TCC Method Exemplified by the Nitrogen Dimer. In: Journal of Chemical Theory and Computation. 2019 ; Vol. 15, No. 4. pp. 2206-2220.
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