The Role of Many-Body Dispersion Interactions in Molecular Crystals

The structure, energetics, and electronic properties of molecular crystals are studied using density functional theory (DFT) with the recently developed many-body dispersion (MBD) method [Tkatchenko et al. Phys. Rev. Lett. 108, 236402 (2012)]. It is shown that accounting for the long-range electrostatic screening in extended systems is essential for obtaining the correct dielectric constants and ensuing optical properties of molecular crystals [Schatschneider et al., arXiv:1211.1683]. Furthermore, accounting for the non-additive many-center dispersion interactions is crucial for obtaining a highly accurate description of the energetics of molecular crystals. This includes lattice energies, sublimation enthalpies [Reilly et al., to be published], and relative stabilities of polymorphs [Marom et al. arXiv: 1210.5636] \\[4pt] In collaboration with Leslie Leiserowitz, Weizmann Institute of Science, Israel; Bohdan Schatschneider, The Pennsylvania State University, Fayette; Robert DiStasio, Princeton University; Anthony Reilly and Guo-Xu Zhang, Fritz Haber Institute of the Max Planck Society, Berlin; James Chelikowsky, The University of Texas at Austin; and Alexandre Tkatchenko, Fritz Haber Institute of the Max Planck Society, Berlin.