Bredow, Thomas

Heitjans, Paul

Islam, Mazharul M.

Volgmann, Kai

Werth, Vanessa

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The Open-Access Journal for the Basic Principles of Diffusion Theory, Experiment and ApplicationEvaluation of Density Functional Theory for Lithium Ion Migration in1T-LiTiS2Vanessa Werth1, Mazharul M. Islam2, Kai Volgmann1, Paul Heitjans1, ThomasBredow21 Institut fu¨r Physikalische Chemie und Elektrochemie, Universita¨t Hannover, Callinstr. 3-3a,30167 Hannover, Germany; 2 Mulliken Center for Theoretical Chemistry, Universita¨t Bonn,Beringstr. 4-6, 53115 Bonn, GermanyE-mail: vanessa.werth@pci.uni-hannover.deWeak interactions and properties of solids containing transition metals are often problem-atic to describe with standard generalized gradient approximations (GGA). One challengefor GGA is the experimentally well studied host material 1T-TiS2, where lithium is themost prominent intercalation material. The addition of dispersion corrections [1–3] andan on-site Coulomb repulsion term [4] to the Perdew-Burke-Enzernhof (PBE) functionalis studied [5] using the plane-wave program package VASP. An overall improvement withrespect to experimental data can be observed in comparison to the PBE functional. Themost significant improvement is the structural description, in particular the c latticeparameter, of TiS2 and the calculated band gap of TiS2. Also quadrupole couplingconstants and chemical shifts are closer to experimental data, if both correction terms areincluded. The calculated activation energy in 1T-LixTiS2 for x ≈ 1 for a Li ion migrationto a tetrahedral interstitial position is 0.4 eV and close to experimental values.[1] A Consistent and Accurate Ab Intio Parametrization of Density Functional Dispersion Correction(DFT-D) for the 94 Elements H-Pu, S. Grimme, J. Antony, S. Ehrlich, H. Krieg, J. Chem. Phys. 132(2010) 154104.[2] Effect of the Damping Function in Dispersion Corrected Density Functional Theory, S. Grimme,S. Ehrlich, L. Goerigk, J. Comp. Chem. 32 (2011) 1456.[3] Accurate Molecular Van der Waals Interactions from Ground-State Electron Density and Free-AtomReference Data, A. Tkatchenko, M. Scheﬄer, Phys. Rev. Lett. 102 (2009) 073005.[4] Electron-Energy-Loss Spectra and the Structural Stability of Nickel Oxide: An LSDA+U study,S. L. Dudarev, G. A. Botton, S. Y. Savrasov, C. J. Humphreys, A. P. Sutton, Phys. Rev. B 57(1998) 1505.[5] Density Functional Theory Evaluated for Structural and Electronic Properties of 1T-LixTiS2 andLithium Ion Migration in 1T-Li0.94TiS2, V. Werth, M. M. Islam, K. Volgmann, P. Heitjans, T. Bre-dow, Z. Phys. Chem., in press, 2017 (DOI: 10.1515/zpch-2016-0919).This work is licensed under a Creative Commons Attribution 4.0 International License. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/1

Evaluation of Density Functional Theory for Lithium Ion Migration in 1T-LiTiS2

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Evaluation of Density Functional Theory for Lithium Ion Migration in 1T-LiTiS2

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