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An active space variational calculation of the 2-electron reduced density matrix (2-RDM) is derived and implemented where the active orbitals are correlated within the pair approximation. The pair approximation considers only doubly…

Chemical Physics · Physics 2020-10-13 Kade Head-Marsden , David A. Mazziotti

We report that a recent active space model of the nitrogenase FeMo cofactor, proposed in the context of quantum simulations, is not representative of the electronic structure of the FeMo cofactor ground-state. Although quantum resource…

Chemical Physics · Physics 2019-01-30 Zhendong Li , Junhao Li , Nikesh S. Dattani , C. J. Umrigar , Garnet Kin-Lic Chan

N2 association to the FeMo-cofactor of nitrogenase, including the recently identified central N ligand, has been investigated using first-principles electronic structure calculations. The oxidation state of the resting state of the cofactor…

Biological Physics · Physics 2007-05-23 Johannes Schimpl , Helena M. Petrilli , Peter E. Bloechl

The main source of reduced nitrogen for living things comes from nitrogenase, which converts N2 to NH3 at the FeMo-cofactor (FeMo-co). Because of its role in supporting life, the uncertainty surrounding the catalytic cycle, and its…

Chemical Physics · Physics 2026-01-09 Huanchen Zhai , Chenghan Li , Xing Zhang , Zhendong Li , Seunghoon Lee , Garnet Kin-Lic Chan

This study investigates the photocatalytic nitrogen fixation on a cation-doped surface (Bi$_{x}$M$_{y}$)$_2$MoO$_6$ where (M = Fe, La, Yb) in both the orthorhombic and monoclinic configurations using a density functional theory (DFT)…

Materials Science · Physics 2018-12-13 Alhassan S. Yasin , Botong Liu , Nianqiang Wu , Terence Musho

The importance of co-adsorption for applications of porous materials in gas separation has motivated fundamental studies, which have initially focused on the comparison of the binding energies of different gas molecules in the pores (i.e.…

Materials Science · Physics 2015-04-08 Kui Tan , Sebastian Zuluaga , Qihan Gong , Yuzhi Gao , Nour Nijem , Jing Li , Timo Thonhauser , Yves J Chabal

Resistive and capacitive switching in capacitor metal/nanocomposite/metal (M/NC/M) structures based on (CoFeB)x(LiNbO3)100-x NC fabricated by ion-beam sputtering with metal content x $\approx$ 8-20 at. % is studied. The peculiarity of the…

Multi-configurational approaches yield universal wave function parameterizations that can qualitatively well describe electronic structures along reaction pathways. For quantitative results, multi-reference perturbation theory is required…

Chemical Physics · Physics 2016-09-08 Christopher J. Stein , Vera von Burg , Markus Reiher

Unravelling the origins of single-atom catalyst reactivity is a central challenge in heterogeneous catalysis research. A key question is whether the activity arises solely from atomic isolation or from distinct structural and electronic…

Materials Science · Physics 2026-03-16 Jakub Planer , Dominik Hrůza , Tadeáš Lesovský , Ayesha Jabeen , Jan Čechal , Zdeněk Jakub

In this paper I give a detailed account of an ab initio methodology for describing strong electronic correlations in nanoscale devices hosting transition metal atoms with open $d$- or $f$-shells. The method combines Kohn-Sham Density…

Mesoscale and Nanoscale Physics · Physics 2015-06-15 D. Jacob

Characterizing the electronic structure of the iron--sulfur clusters in nitrogenase is necessary to understand their role in the nitrogen fixation process. One challenging task is to determine the protonation state of the intermediates in…

Chemical Physics · Physics 2023-11-28 Huanchen Zhai , Seunghoon Lee , Zhi-Hao Cui , Lili Cao , Ulf Ryde , Garnet Kin-Lic Chan

Nitrate reduction to ammonia has attracted much attention for nitrate (NO3-) removal and ammonia (NH3) production. Identifying promising catalyst for active nitrate electroreduction reaction (NO3RR) is critical to realize efficient…

Materials Science · Physics 2023-08-29 Zheng Shu , Hongfei Chen , Xing Liu , Huaxian Jia , Hejin Yan , Yongqing Cai

Background: The secondary structure and complexity of mRNA influences its accessibility to regulatory molecules (proteins, micro-RNAs), its stability and its level of expression. The mobile elements of the RNA sequence, the wobble bases,…

Biomolecules · Quantitative Biology 2008-07-22 Jan C. Biro

The presence of complexity in the electronic structure of strongly correlated electron system NdCoO$_3$ (NCO) have sparked interest in the investigation of its physical properties. Here, we study the the Seebeck coefficient ($\alpha $) of…

Materials Science · Physics 2023-12-19 Abhishek Pandey , Sudhir K. Pandey

We investigate the electronic structure of highly conducting perovskite SrMoO$_{3}$ using valence band photoemission spectroscopy and electronic structure calculations. Large intensity corresponding to coherent feature close to Fermi level…

Strongly Correlated Electrons · Physics 2023-01-24 Asif Ali , B. H. Reddy , Ravi Shankar Singh

The properties of two molecular-based magnetic helices, composed of 3$d$ metal Co and Mn ions bridged by Nitronyl Nitroxide radicals, are investigated by density functional calculations. Their peculiar and distinctive magnetic behavior is…

Materials Science · Physics 2015-05-20 Marco Scarrozza , Alessandro Vindigni , Paolo Barone , Roberta Sessoli , Silvia Picozzi

In this work we explore the performance of a recently derived many-body effective energy theory for the calculation of photoemission spectra in the regime of strong electron correlation. We apply the theory to paramagnetic MnO, FeO, CoO,…

Strongly Correlated Electrons · Physics 2019-03-25 S. Di Sabatino , J. A. Berger , P. Romaniello

Ammonia, a versatile compound that can be used as a fertilizer, chemical or fuel, has since long been produced through the energy-intensive Haber-Bosch process. Recently, the electrochemical nitrate reduction reaction (NO3RR) using…

High resolution angle-resolved photoemission spectroscopy data along the (0,0)-($\pi$,$\pi$) nodal direction with significantly improved statistics reveal fine structure in the electron self-energy of the underdoped…

In this work, we use modern electronic structure methods to model the catalytic mechanism of different variants of the molybdenum cofactor (Moco). We investigate the dependence of various Moco model systems on structural relaxation and the…

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