Theory of chemical bonds in metalloenzymes XXIV electronic and spin structures of FeMoco and Fe-S clusters by classical and quantum computing

Koichi Miyagawa, Mitsuo Shoji, Hiroshi Isobe, Shusuke Yamanaka, Takashi Kawakami, Mitsutaka Okumura, Kizashi Yamaguchi

Research output: Contribution to journalArticle

Abstract

Fundamental principles for theoretical understanding and elucidation of structure and reactivity of iron-sulfur (Fe-S) FenSm (n, m=2∼8) clusters are investigated and elucidated on the theoretical and experimental grounds. To this end, the nature of chemical bonds of these clusters is investigated by three methods; (1) the spin Hamiltonian model for analysis of EPR results, (2) broken-symmetry (BS) hybrid density functional theory (HDFT) methods for full geometry optimisations and elucidations of complete active spaces (CAS) for one-electron transfers reactions and (3) beyond HDFT methods such as CAS configuration interaction (CI) and MR CI for high precision energy calculations on classical and quantum computers. Theoretical concepts revealed are applied for elucidation of the mechanism of nitrogen fixation with FeMoco (Fe7MoS9C) cluster, indicating an important role of proton-coupled (PC) one electron spin transfer (OEST) processes instead of radical reaction mechanisms.

Original languageEnglish
JournalMolecular Physics
DOIs
Publication statusAccepted/In press - Jan 1 2020

Keywords

  • broken symmetry
  • classical and quantum computer
  • FeMoco cluster
  • iron-sulfur cluster
  • nitrogen fixation

ASJC Scopus subject areas

  • Biophysics
  • Molecular Biology
  • Condensed Matter Physics
  • Physical and Theoretical Chemistry

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