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Structure and Stability of Molecular Crystals with Many Body Dispersion Inclusive Density Functional Tight Binding

preprint
submitted on 04.12.2017, 11:28 and posted on 05.12.2017, 15:35 by Majid Mortazavi, Jan Gerit Brandenburg, Reinhard J. Maurer, Alexandre Tkatchenko

Accurate prediction of structure and stability of molecular crystals is crucial in materials science and requires reliable modeling of long-range dispersion interactions. Semi-empirical electronic structure methods are computationally more efficient than their ab initio counterparts, allowing structure sampling with significant speed-ups. Here, we combine the Tkatchenko-Scheffler van-der-Waals method (TS) and the many body dispersion method (MBD) with third-order density functional tight-binding (DFTB3) via a charge population-based method. We find an overall good performance for the X23 benchmark database of molecular crystals, despite an underestimation of crystal volume that can be traced to the DFTB parametrization. We achieve accurate lattice energy predictions with DFT+MBD energetics on top of vdW-inclusive DFTB3 structures, resulting in a speed-up of up to 3000 times compared to a full DFT treatment. This suggests that vdW-inclusive DFTB3 can serve as a viable structural prescreening tool in crystal structure prediction.

Funding

Alexander von Humboldt foundation within the Feodor-Lynen program, DFG SPP-1807, European Research Council (ERC-CoG BeStMo)

History

Topic

  • Computational chemistry and modeling
  • Theory

Email Address of Submitting Author

mortazavi@fhi-berlin.mpg.de

Email Address(es) for Other Author(s)

Jan Gerit Brandenburg:g.brandenburg@ucl.ac.uk, Reinhard J. Maurer:r.maurer@warwick.ac.uk, Alexandre Tkatchenko:alexandre.tkatchenko@uni.lu

Institution

Fritz-Haber-Institut der Max-Planck-Gesellschaft

Country

Germany

ORCID For Submitting Author

0000-0002-2944-7338

Declaration of Conflict of Interest

The authors declare no competing financial interest.

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