New Insight into the Ground State of FePc: A Diffusion Monte Carlo Study

Abstract We have applied DMC to evaluate relative stability of the possible electronic configurations of an isolated FePc under D 4h symmetry, considering some fixed nodes generated from different methods. They predict A 2g ground state consistently, supporting preceding DFT studies, with confidence...

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Main Authors:	Tom Ichibha, Zhufeng Hou, Kenta Hongo, Ryo Maezono
Format:	article
Language:	EN
Published:	Nature Portfolio 2017
Subjects:	Medicine R Science Q
Online Access:	https://doaj.org/article/09e5aad8bc664791aeb2fc8dcf6cfe98
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spelling	oai:doaj.org-article:09e5aad8bc664791aeb2fc8dcf6cfe982021-12-02T12:32:19ZNew Insight into the Ground State of FePc: A Diffusion Monte Carlo Study10.1038/s41598-017-01668-62045-2322https://doaj.org/article/09e5aad8bc664791aeb2fc8dcf6cfe982017-05-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-01668-6https://doaj.org/toc/2045-2322Abstract We have applied DMC to evaluate relative stability of the possible electronic configurations of an isolated FePc under D 4h symmetry, considering some fixed nodes generated from different methods. They predict A 2g ground state consistently, supporting preceding DFT studies, with confidence overcoming the ambiguity about exchange-correlation (XC) functionals. By comparing DMC with several XC, we clarified the importance of the short-range exchange to describe the relative stability. We examined why the predicted A 2g is excluded from possible ground states in the recent ligand field based model. Simplified assumptions made in the superposition model are identified to give unreasonably less energy gain for A 2g when compared with the reality. The state is found to have possible reasons for the stabilization, reducing the occupations from an unstable anti-bonding orbital, avoiding double occupation of a spatially localized orbital, and gaining exchange energy by putting a triplet spin pair in degenerate orbitals.Tom IchibhaZhufeng HouKenta HongoRyo MaezonoNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-6 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Tom Ichibha Zhufeng Hou Kenta Hongo Ryo Maezono New Insight into the Ground State of FePc: A Diffusion Monte Carlo Study
description	Abstract We have applied DMC to evaluate relative stability of the possible electronic configurations of an isolated FePc under D 4h symmetry, considering some fixed nodes generated from different methods. They predict A 2g ground state consistently, supporting preceding DFT studies, with confidence overcoming the ambiguity about exchange-correlation (XC) functionals. By comparing DMC with several XC, we clarified the importance of the short-range exchange to describe the relative stability. We examined why the predicted A 2g is excluded from possible ground states in the recent ligand field based model. Simplified assumptions made in the superposition model are identified to give unreasonably less energy gain for A 2g when compared with the reality. The state is found to have possible reasons for the stabilization, reducing the occupations from an unstable anti-bonding orbital, avoiding double occupation of a spatially localized orbital, and gaining exchange energy by putting a triplet spin pair in degenerate orbitals.
format	article
author	Tom Ichibha Zhufeng Hou Kenta Hongo Ryo Maezono
author_facet	Tom Ichibha Zhufeng Hou Kenta Hongo Ryo Maezono
author_sort	Tom Ichibha
title	New Insight into the Ground State of FePc: A Diffusion Monte Carlo Study
title_short	New Insight into the Ground State of FePc: A Diffusion Monte Carlo Study
title_full	New Insight into the Ground State of FePc: A Diffusion Monte Carlo Study
title_fullStr	New Insight into the Ground State of FePc: A Diffusion Monte Carlo Study
title_full_unstemmed	New Insight into the Ground State of FePc: A Diffusion Monte Carlo Study
title_sort	new insight into the ground state of fepc: a diffusion monte carlo study
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/09e5aad8bc664791aeb2fc8dcf6cfe98
work_keys_str_mv	AT tomichibha newinsightintothegroundstateoffepcadiffusionmontecarlostudy AT zhufenghou newinsightintothegroundstateoffepcadiffusionmontecarlostudy AT kentahongo newinsightintothegroundstateoffepcadiffusionmontecarlostudy AT ryomaezono newinsightintothegroundstateoffepcadiffusionmontecarlostudy
_version_	1718394078258790400

New Insight into the Ground State of FePc: A Diffusion Monte Carlo Study

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