ONETEP + TOSCAM: uniting dynamical mean field theory and linear-scaling\n density functional theory

2019/11/18 by Edward Linscott, Daniel J. Cole, Linscott, Edward B. +7
Biochemistry, Genetics and Molecular Biology · Chemistry · Energy · #Chemical Physics (physics.chem-ph) #Computational Physics (physics.comp-ph) #FOS: Physical sciences #Iron oxide chemistry and applications #Metal-Catalyzed Oxygenation Mechanisms #Photosynthetic Processes and Mechanisms #Quantum Physics (quant-ph) #Strongly Correlated Electrons (cond-mat.str-el)

paper · pdf · doi:10.48550/arxiv.1911.07752

openalex publication_date 2019/11/18 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

Abstract

We introduce the unification of dynamical mean field theory (DMFT) and\nlinear-scaling density functional theory (DFT), as recently implemented in\nONETEP, a linear-scaling DFT package, and TOSCAM, a DMFT toolbox. This code can\naccount for strongly correlated electronic behavior while simultaneously\nincluding the effects of the environment, making it ideally suited for studying\ncomplex and heterogeneous systems containing transition metals and lanthanides,\nsuch as metalloproteins. We systematically introduce the necessary formalism,\nwhich must account for the non-orthogonal basis set used by ONETEP. In order to\ndemonstrate the capabilities of this code, we apply it to carbon\nmonoxide-ligated iron porphyrin and explore the distinctly quantum-mechanical\ncharacter of the iron 3d electrons during the process of photodissociation.\n

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