Modeling the Excited States of Biological Chromophores within Many-Body Green's Function Theory

Autor(en): Ma, Yuchen
Rohlfing, Michael
Molteni, Carla
Stichwörter: AB-INITIO; ABSORPTION-SPECTRUM; BASE RETINAL CHROMOPHORES; Chemistry; Chemistry, Physical; COUPLED-CLUSTER; EXCITATION-ENERGIES; FULL CONFIGURATION-INTERACTION; GAS-PHASE PHOTOCHEMISTRY; OPTICAL-SPECTRA; P-COUMARIC ACID; PHOTOACTIVE YELLOW PROTEIN; Physics; Physics, Atomic, Molecular & Chemical
Erscheinungsdatum: 2010
Herausgeber: AMER CHEMICAL SOC
Journal: JOURNAL OF CHEMICAL THEORY AND COMPUTATION
Volumen: 6
Ausgabe: 1
Startseite: 257
Seitenende: 265
Zusammenfassung: 
First-principle many-body Green's function theory (MBGFT) has been successfully used to describe electronic excitations in many materials, from bulk crystals to nanoparticles. Here we assess its performance for the calculations of the excited states of biological chromophores. MBGFT is based on a set of Green's function equations, whose key ingredients are the electron's self-energy Sigma, which is obtained by Hedin's GW approach, and the electron-hole interaction, which is described by the Bethe-Salpeter equation (BSE). The GW approach and the BSE predict orbital energies and excitation energies with high accuracy, respectively. We have calculated the low-lying excited states of a series of model biological chromophores, related to the photoactive yellow protein (PYP), rhodopsin, and the green fluorescent protein (GFP), obtaining a very good agreement with the available experimental and accurate theoretical data; the order of the excited states is also correctly predicted. MBGFT bridges the gap between time-dependent density functional theory and high-level quantum chemistry methods, combining the efficiency of the former with the accuracy of the latter: this makes MBGFT a promising method for studying excitations in complex biological systems.
ISSN: 15499618
DOI: 10.1021/ct900528h

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