Updated Tkatchenko Scheffler method and assessment of dispersion methods for alkali-containing systems

Abstract

The Tkatchenko-Scheffler (TS) pairwise method to calculate dispersion interactions is a widely used approach to incorporate missing long-range van der Waals contributions in semilocal and hybrid density functional calculations. Despite subsequent many-body extensions, this formulation remains widely used. In 2018, Fedorov et al. reported updated van der Waals radii to the seminal work published in 2009. The present work examines the accuracy of the TS method with updated van der Waals radii (TS_2018), coupled with the semilocal Perdew-Burke-Ernzerhof density functional, for structural predictions of semiconducting and insulating materials. Special attention is paid to materials containing alkali elements, for which the TS_2009 method exhibits a large overbinding, associated with potentially large errors in predicted atomic structures. We also consider a narrower reformulation (TS_alkali) where only the the alkali atoms are corrected, so the method remains otherwise compatible with TS_2009. We compare these methods with a broader set of dispersion corrections--the DFT-D3 method, the exchange-hole dipole moment method, and the beyond-pairwise, nonlocal many-body dispersion method--for ionic and alkali-containing systems more generally. We examine equilibrium geometry predictions for 45 inorganic solid compounds as well as three Cs-containing halide perovskites, CsPbX₃ (X = Cl, Br, I). Our results show that the updated van der Waals radii in the TS_2018 and TS_alkali methods resolve the overbinding that is present with TS_2009 in alkali-containing systems, bringing predictions into closer agreement with other dispersion methods. For the halide perovskites, method-dependent differences in predicted cell volumes and shapes persist, and no approach performs with perfect accuracy on all metrics for all three materials.

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BibTeX RIS

BibTeX

@misc{schankler2026updated,
  title = {{Updated Tkatchenko Scheffler method and assessment of dispersion methods for alkali-containing systems}},
  author = {Aaron M. Schankler and Ruyi Song and Sampreeti Bhattacharya and Ela Lucas and Lee Hampton III and Alexandre Tkatchenko and Yosuke Kanai and Volker Blum},
  howpublished = {arXiv},
  year = {2026},
  month = nov,
  doi = {10.48550/arxiv.2608.01501},
  eprint = {2608.01501},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2608.01501},
}

RIS

TY  - UNPB
TI  - Updated Tkatchenko Scheffler method and assessment of dispersion methods for alkali-containing systems
AU  - Aaron M. Schankler
AU  - Ruyi Song
AU  - Sampreeti Bhattacharya
AU  - Ela Lucas
AU  - Lee Hampton III
AU  - Alexandre Tkatchenko
AU  - Yosuke Kanai
AU  - Volker Blum
PY  - 2026
DA  - 2026/11/05
PB  - arXiv
DO  - 10.48550/arxiv.2608.01501
UR  - https://arxiv.org/abs/2608.01501
AB  - The Tkatchenko-Scheffler (TS) pairwise method to calculate dispersion interactions is a widely used approach to incorporate missing long-range van der Waals contributions in semilocal and hybrid density functional calculations. Despite subsequent many-body extensions, this formulation remains widely used. In 2018, Fedorov et al. reported updated van der Waals radii to the seminal work published in 2009. The present work examines the accuracy of the TS method with updated van der Waals radii (TS_2018), coupled with the semilocal Perdew-Burke-Ernzerhof density functional, for structural predictions of semiconducting and insulating materials. Special attention is paid to materials containing alkali elements, for which the TS_2009 method exhibits a large overbinding, associated with potentially large errors in predicted atomic structures. We also consider a narrower reformulation (TS_alkali) where only the the alkali atoms are corrected, so the method remains otherwise compatible with TS_2009. We compare these methods with a broader set of dispersion corrections--the DFT-D3 method, the exchange-hole dipole moment method, and the beyond-pairwise, nonlocal many-body dispersion method--for ionic and alkali-containing systems more generally. We examine equilibrium geometry predictions for 45 inorganic solid compounds as well as three Cs-containing halide perovskites, CsPbX_3 (X = Cl, Br, I). Our results show that the updated van der Waals radii in the TS_2018 and TS_alkali methods resolve the overbinding that is present with TS_2009 in alkali-containing systems, bringing predictions into closer agreement with other dispersion methods. For the halide perovskites, method-dependent differences in predicted cell volumes and shapes persist, and no approach performs with perfect accuracy on all metrics for all three materials.
ER  -

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