The correlation theory of the chemical bond

Szilárd Szalay, Gergely Barcza, Tibor Szilvási, Libor Veis, O. Legeza

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

The quantum mechanical description of the chemical bond is generally given in terms of delocalized bonding orbitals, or, alternatively, in terms of correlations of occupations of localised orbitals. However, in the latter case, multiorbital correlations were treated only in terms of two-orbital correlations, although the structure of multiorbital correlations is far richer; and, in the case of bonds established by more than two electrons, multiorbital correlations represent a more natural point of view. Here, for the first time, we introduce the true multiorbital correlation theory, consisting of a framework for handling the structure of multiorbital correlations, a toolbox of true multiorbital correlation measures, and the formulation of the multiorbital correlation clustering, together with an algorithm for obtaining that. These make it possible to characterise quantitatively, how well a bonding picture describes the chemical system. As proof of concept, we apply the theory for the investigation of the bond structures of several molecules. We show that the non-existence of well-defined multiorbital correlation clustering provides a reason for debated bonding picture.

Original languageEnglish
Article number2237
JournalScientific Reports
Volume7
Issue number1
DOIs
Publication statusPublished - Dec 1 2017

Fingerprint

Correlation theory
Chemical bonds
Electron correlations
Molecules

ASJC Scopus subject areas

  • General

Cite this

The correlation theory of the chemical bond. / Szalay, Szilárd; Barcza, Gergely; Szilvási, Tibor; Veis, Libor; Legeza, O.

In: Scientific Reports, Vol. 7, No. 1, 2237, 01.12.2017.

Research output: Contribution to journalArticle

Szalay, S, Barcza, G, Szilvási, T, Veis, L & Legeza, O 2017, 'The correlation theory of the chemical bond', Scientific Reports, vol. 7, no. 1, 2237. https://doi.org/10.1038/s41598-017-02447-z
Szalay, Szilárd ; Barcza, Gergely ; Szilvási, Tibor ; Veis, Libor ; Legeza, O. / The correlation theory of the chemical bond. In: Scientific Reports. 2017 ; Vol. 7, No. 1.
@article{daf7fdd34505448384018d0251bc1c91,
title = "The correlation theory of the chemical bond",
abstract = "The quantum mechanical description of the chemical bond is generally given in terms of delocalized bonding orbitals, or, alternatively, in terms of correlations of occupations of localised orbitals. However, in the latter case, multiorbital correlations were treated only in terms of two-orbital correlations, although the structure of multiorbital correlations is far richer; and, in the case of bonds established by more than two electrons, multiorbital correlations represent a more natural point of view. Here, for the first time, we introduce the true multiorbital correlation theory, consisting of a framework for handling the structure of multiorbital correlations, a toolbox of true multiorbital correlation measures, and the formulation of the multiorbital correlation clustering, together with an algorithm for obtaining that. These make it possible to characterise quantitatively, how well a bonding picture describes the chemical system. As proof of concept, we apply the theory for the investigation of the bond structures of several molecules. We show that the non-existence of well-defined multiorbital correlation clustering provides a reason for debated bonding picture.",
author = "Szil{\'a}rd Szalay and Gergely Barcza and Tibor Szilv{\'a}si and Libor Veis and O. Legeza",
year = "2017",
month = "12",
day = "1",
doi = "10.1038/s41598-017-02447-z",
language = "English",
volume = "7",
journal = "Scientific Reports",
issn = "2045-2322",
publisher = "Nature Publishing Group",
number = "1",

}

TY - JOUR

T1 - The correlation theory of the chemical bond

AU - Szalay, Szilárd

AU - Barcza, Gergely

AU - Szilvási, Tibor

AU - Veis, Libor

AU - Legeza, O.

PY - 2017/12/1

Y1 - 2017/12/1

N2 - The quantum mechanical description of the chemical bond is generally given in terms of delocalized bonding orbitals, or, alternatively, in terms of correlations of occupations of localised orbitals. However, in the latter case, multiorbital correlations were treated only in terms of two-orbital correlations, although the structure of multiorbital correlations is far richer; and, in the case of bonds established by more than two electrons, multiorbital correlations represent a more natural point of view. Here, for the first time, we introduce the true multiorbital correlation theory, consisting of a framework for handling the structure of multiorbital correlations, a toolbox of true multiorbital correlation measures, and the formulation of the multiorbital correlation clustering, together with an algorithm for obtaining that. These make it possible to characterise quantitatively, how well a bonding picture describes the chemical system. As proof of concept, we apply the theory for the investigation of the bond structures of several molecules. We show that the non-existence of well-defined multiorbital correlation clustering provides a reason for debated bonding picture.

AB - The quantum mechanical description of the chemical bond is generally given in terms of delocalized bonding orbitals, or, alternatively, in terms of correlations of occupations of localised orbitals. However, in the latter case, multiorbital correlations were treated only in terms of two-orbital correlations, although the structure of multiorbital correlations is far richer; and, in the case of bonds established by more than two electrons, multiorbital correlations represent a more natural point of view. Here, for the first time, we introduce the true multiorbital correlation theory, consisting of a framework for handling the structure of multiorbital correlations, a toolbox of true multiorbital correlation measures, and the formulation of the multiorbital correlation clustering, together with an algorithm for obtaining that. These make it possible to characterise quantitatively, how well a bonding picture describes the chemical system. As proof of concept, we apply the theory for the investigation of the bond structures of several molecules. We show that the non-existence of well-defined multiorbital correlation clustering provides a reason for debated bonding picture.

UR - http://www.scopus.com/inward/record.url?scp=85019739295&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85019739295&partnerID=8YFLogxK

U2 - 10.1038/s41598-017-02447-z

DO - 10.1038/s41598-017-02447-z

M3 - Article

C2 - 28533506

AN - SCOPUS:85019739295

VL - 7

JO - Scientific Reports

JF - Scientific Reports

SN - 2045-2322

IS - 1

M1 - 2237

ER -