Strong Electron Correlation in Nitrogenase Cofactor, FeMoco

The Journal of Physical Chemistry. a
Jason M Montgomery, David A Mazziotti

Abstract

FeMoco, MoFe7S9C, has been shown to be the active catalytic site for the reduction of nitrogen to ammonia in the nitrogenase protein. An understanding of its electronic structure including strong electron correlation is key to designing mimic catalysts capable of ambient nitrogen fixation. Active spaces ranging from [54, 54] to [65, 57] have been predicted for a quantitative description of FeMoco's electronic structure. However, a wave function approach for a singlet state using a [54, 54] active space would require 1029 variables. In this work, we systematically explore the active-space size necessary to qualitatively capture strong correlation in FeMoco and two related moieties, MoFe3S7 and Fe4S7. Using CASSCF and 2-RDM methods, we consider active-space sizes up to [14, 14] and [30, 30], respectively, with STO-3G, 3-21G, and DZP basis sets and use fractional natural-orbital occupation numbers to assess the level of multireference electron correlation, an examination of which reveals a competition between single-reference and multireference solutions to the electronic Schrödinger equation for smaller active spaces and a consistent multireference solution for larger active spaces.

References

Feb 15, 1993·European Journal of Biochemistry·A J PierikW R Hagen
Mar 18, 2000·Journal of Computer-aided Molecular Design·G Schaftenaar, J H Noordik
Nov 7, 1996·Chemical Reviews·James B. Howard, Douglas C. Rees
Nov 7, 1996·Chemical Reviews·Barbara K. Burgess, David J. Lowe
Sep 1, 2006·The Journal of Chemical Physics·Eric CancèsMathieu Lewin
Apr 12, 2007·Dalton Transactions : an International Journal of Inorganic Chemistry·Kallol RayFrank Neese
Aug 7, 2010·Science·Chi Chung LeeMarkus W Ribbe
Nov 3, 2010·The Journal of Chemical Physics·Loren Greenman, David A Mazziotti
Mar 17, 2011·Physical Review Letters·David A Mazziotti
Sep 26, 2012·Physical Review Letters·David A Mazziotti
Jan 29, 2014·Chemical Reviews·Brian M HoffmanLance C Seefeldt
Dec 9, 2014·Biochimica Et Biophysica Acta·Joanna Kowalska, Serena DeBeer
Jan 30, 2016·The Journal of Physical Chemistry Letters·Anthony W SchlimgenDavid A Mazziotti
Apr 12, 2016·Journal of Chemical Theory and Computation·Jacob Fosso-TandeA Eugene DePrince
Jan 27, 2017·Physical Chemistry Chemical Physics : PCCP·Alexandra R McIsaac, David A Mazziotti
Jul 5, 2017·Proceedings of the National Academy of Sciences of the United States of America·Markus ReiherMatthias Troyer
Nov 21, 2017·The Journal of Physical Chemistry. a·Anthony W Schlimgen, David A Mazziotti

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Citations

Oct 26, 2018·Proceedings of the National Academy of Sciences of the United States of America·Simone RaugeiBrian M Hoffman
Feb 20, 2019·Physical Chemistry Chemical Physics : PCCP·Tymofii Yu Nikolaienko
Jun 4, 2019·Physical Chemistry Chemical Physics : PCCP·Alexandra E Raeber, David A Mazziotti
Dec 6, 2019·Chembiochem : a European Journal of Chemical Biology·Ian Dance
Oct 20, 2020·Physical Chemistry Chemical Physics : PCCP·Alexandra E Raeber, David A Mazziotti
Dec 17, 2020·Chemical Reviews·Kade Head-MarsdenPrineha Narang
May 31, 2019·Journal of the American Chemical Society·Hannah L RutledgeF Akif Tezcan
May 30, 2020·The Journal of Physical Chemistry Letters·Jan-Niklas BoynDavid A Mazziotti
May 30, 2020·The Journal of Physical Chemistry. a·Kade Head-Marsden, David A Mazziotti
Nov 11, 2020·The Journal of Physical Chemistry. a·Jason M MontgomeryDavid A Mazziotti
Dec 29, 2020·The Journal of Physical Chemistry Letters·Daniel GibneyDavid A Mazziotti
Sep 20, 2020·Journal of the American Chemical Society·Airi KawamuraJohn S Anderson
Oct 28, 2021·Journal of the American Chemical Society·Manas SajjanSabre Kais

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