Hybrid inorganic-organic systems (HIOS) are essential ingredients of a wide range of emerging devices. Applications in which such interfaces play a crucial role include (opto)-electronics (e.g., transistors, light-emitting diodes), organic photovoltaics, and sensors. The understanding of electronic properties of complex HIOS requires a reliable method for the prediction of their structure and stability. This is a challenging task because bonding at complex interfaces arises from delicate balance between covalent bonds, van der Waals (vdW) forces, charge transfer, and Pauli repulsion. Recently, we developed a method based on density-functional theory with vdW interactions (DFT+vdWsurf [1]) to accurately model adsorbates on surfaces, by a synergetic linkage of the DFT+vdW method [2] for intermolecular interactions with the Lifshitz-Zaremba-Kohn theory [3] for the collective electronic response within the substrate surface. This method is demonstrated to reliably model a multitude of small and large molecules on metal surfaces [1,4,5,6], leading to accuracy of 0.1 � in adsorption heights and 0.1 eV in binding energies with respect to state-of-the-art experiments. We illustrate the predictive power of the DFT+vdWsurf method with applications to rigid single-molecule push button switches, low-temperature (de)hydrogenation catalysts [6], and complex interfaces composed of olympicene derivatives on the Cu(111) surface [7].[1] V. G. Ruiz et al., Phys. Rev. Lett. 108, 146103 (2012).[2] A. Tkatchenko and M. Scheffler, Phys. Rev. Lett. 102, 073005 (2009).[3] E. Zaremba and W. Kohn, Phys. Rev. B 13, 2270 (1976).[4] W. Liu et al., Phys. Rev. B 86, 245405 (2012).[5] D. Egger et al., J. Phys. Chem. C 117, 3055 (2013).[6] W. Liu et al., J. Phys. Chem. Lett. 3, 582 (2012).[7] http://en.wikipedia.org/wiki/Olympicene.

Reliable modeling of bonding for complex interfaces with applications in catalysis, molecular electronics, and photovoltaics

246th National Meeting (2013)

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