Abstract
Fundamental principles for theoretical understanding and elucidation of structure and reactivity of iron-sulfur (Fe-S) Fe n S m (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 language | English |
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Article number | e1760388 |
Journal | Molecular Physics |
Volume | 118 |
Issue number | 21-22 |
DOIs | |
Publication status | Published - Nov 2020 |
Keywords
- FeMoco cluster
- broken symmetry
- classical and quantum computer
- iron-sulfur cluster
- nitrogen fixation
ASJC Scopus subject areas
- Biophysics
- Molecular Biology
- Condensed Matter Physics
- Physical and Theoretical Chemistry