Evaluating Computational Shortcuts in Supercell-Based Phonon Calculations of Molecular Crystals: The Instructive Case of Naphthalene

Journal of Chemical Theory and Computation
Tomas KamencekEgbert Zojer

Abstract

Phonons crucially impact a variety of properties of organic semiconductor materials. For instance, charge- and heat transport depend on low-frequency phonons, while for other properties, such as the free energy, especially high-frequency phonons count. For all these quantities one needs to know the entire phonon band structure, whose simulation becomes exceedingly expensive for more complex systems when using methods like dispersion-corrected density functional theory (DFT). Therefore, in the present contribution we evaluate the performance of more approximate methodologies, including density functional tight binding (DFTB) and a pool of force fields (FF) of varying complexity and sophistication. Beyond merely comparing phonon band structures, we also critically evaluate to what extent derived quantities, like temperature-dependent heat capacities, mean squared thermal displacements, and temperature-dependent free energies are impacted by shortcomings in the description of the phonon bands. As a benchmark system, we choose (deuterated) naphthalene, as the only organic semiconductor material for which to date experimental phonon band structures are available in the literature. Overall, the best performance among the approximate ...Continue Reading

References

Feb 1, 1987·Physical Review. B, Condensed Matter·P VinetJ H Rose
Dec 15, 1994·Physical Review. B, Condensed Matter·P E Blöchl
Oct 15, 1996·Physical Review. B, Condensed Matter·G Kresse, J Furthmüller
Jan 1, 1993·Physical Review. B, Condensed Matter·G Kresse, J Hafner
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Oct 4, 2005·Journal of Computational Chemistry·David A CaseRobert J Woods
Sep 7, 2006·Journal of Computational Chemistry·Stefan Grimme
Oct 13, 2006·The Journal of Physical Chemistry. a·Silvia C CapelliBertram T M Willis
Mar 24, 2007·Chemical Reviews·Veaceslav CoropceanuJean-Luc Brédas
Jun 15, 2007·The Journal of Physical Chemistry. a·B AradiTh Frauenheim
Mar 5, 2009·Physical Review Letters·Alexandre Tkatchenko, Matthias Scheffler
Jul 29, 2009·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Nicolas G MartinelliJérôme Cornil
Mar 20, 2010·Physical Chemistry Chemical Physics : PCCP·Linjun WangQiang Shi
Mar 4, 2011·Journal of Computational Chemistry·Stefan GrimmeLars Goerigk
Sep 26, 2012·Physical Review Letters·Alexandre TkatchenkoMatthias Scheffler
Dec 4, 2012·Journal of Chemical Theory and Computation·Michael GausMarcus Elstner
Aug 31, 2013·Science·Hiroyasu FurukawaOmar M Yaghi
May 17, 2014·The Journal of Chemical Physics·Alberto AmbrosettiAlexandre Tkatchenko
Aug 16, 2014·Physical Review Letters·Anthony M Reilly, Alexandre Tkatchenko
Dec 6, 2014·Acta Crystallographica. Section D, Biological Crystallography·S J FisherA Podjarny
Jun 5, 2014·The Journal of Physical Chemistry Letters·Jan Gerit Brandenburg, Stefan Grimme
Sep 25, 2015·Chemical Society Reviews·Aurora J Cruz-CabezaJoel Bernstein
Jan 8, 2013·Journal of Chemical Theory and Computation·Michael GausMarcus Elstner
Oct 13, 2009·Journal of Chemical Theory and Computation·Carlos CampañáTom K Woo
May 28, 2016·Physical Chemistry Chemical Physics : PCCP·Jonas NymanGraeme M Day
Apr 7, 2017·Journal of Applied Crystallography·Ai Woon YeeV Trevor Forsyth
Jun 24, 2017·Chemical Reviews·Harald OberhoferJochen Blumberger
Jul 19, 2018·Journal of Chemical Theory and Computation·Natalia Bedoya-MartínezEgbert Zojer
Mar 14, 2019·Journal of Chemical Theory and Computation·Johannes P DürholtRochus Schmid
Feb 13, 2020·Journal of Applied Crystallography·Clare F MacraePeter A Wood

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Citations

Apr 3, 2021·Journal of Chemical Theory and Computation·Samet Demir, Adem Tekin
Aug 14, 2020·The Journal of Physical Chemistry Letters·Martin StöhrAlexandre Tkatchenko

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Methods Mentioned

BETA
electron scattering
neutron scattering
X-ray
inelastic neutron scattering

Software Mentioned

FFgen
DFTB
VESTA
Turbomole
Horton
FF
GAFF
PHONOPY
VASP
Gaussian

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