Structural and excited-state properties of oligoacene crystals from first principles

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Structural and excited-state properties of oligoacene crystals from first principles

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Publication Article, peer reviewed scientific
Title Structural and excited-state properties of oligoacene crystals from first principles
Author(s) Rangel, Tonatiuh ; Berland, Kristian ; Sharifzadeh, Sahar ; Brown-Altvater, Florian ; Lee, Kyuho ; Hyldgaard, Per ; Kronik, Leeor ; Neaton, Jeffree B
Date 2016
English abstract
Molecular crystals are a prototypical class of van der Waals (vdW) bound organic materials with excited state properties relevant for optoelectronic applications. Predicting the structure and excited state properties of molecular crystals presents a challenge for electronic structure theory, as standard approximations to density functional theory (DFT) does not cover the long ranged vdW dispersion interactions and do not yield excited state properties. In this work we use a a combination of DFT including vdW forces -- using both nonlocal functionals and pair-wise correction methods -- together with many-body perturbation theory (MBPT) to study the geometry and excited states, respectively, of the entire set of oligoacene crystals, from benzene to hexazene. We find that vdW methods can predict lattice constants within 1 percent of the experimental measurements, on par with the previously reported accuracy of the pair-wise approximations for the same systems. We further find that the excitations energies are sensitive to the geometry, but if optimized geometries are used MBPT can yield excited state properties within a few tenths of an eV from experiments. We elucidate trends in MBPT-charge and neutral excitation energies across the acene series and discuss the role of common approximations used in MBPT.
DOI http://dx.doi.org/10.1103/PhysRevB.93.115206 (link to publisher's fulltext)
Publisher American Physical Society
Host/Issue Physical Review B;
Volume 93
ISSN 2469-9969
Pages 115206
Language eng (iso)
Subject(s) Molecular crystals
van der Waals binding
van der Waals density functional
many-body perturbation theory
structure
excited state properties
Sciences
Research Subject Categories::NATURAL SCIENCES
Handle http://hdl.handle.net/2043/20537 (link to this page)

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