Switching, self-assembly, and catalysis: Ab-Initio prediction of controlled surface chemistry

A fundamental understanding of molecular structure and chemical reactivity at complex interfaces is key to many technological applications ranging from modern optoelectronic devices to functionalized surfaces and light- and electron-enhancement in heterogeneous catalysis.

Predictive ab-initio electronic structure methods such as Density Functional Theory (DFT) can aid such understanding through an accurate prediction of interface structure, spectroscopy, and reactivity. In this talk, I will explain the methodological and computational challenges that need to be overcome to enable an accurate computational characterization of hybrid organic-metallic interfaces within DFT.

At hand of prototypical example systems such as metal-adsorbed single molecule switching [1] and porphyrine thin-films, [2] I will specifically address the roles of long-range van-der-Waals interactions [3] and molecule-surface charge-transfer. [4] I will furthermore report on our recent efforts to map the accuracy of DFT onto more efficient and approximate approaches to address surface chemistry at currently inaccessible length and time scales [5].


[1] Maurer, R. J. et al. Phys. Rev. Lett. 116, 146101 (2016).
[2] Diller, K., Maurer, R. J., Müller, M. & Reuter, K. J. Chem. Phys. 146, 214701 (2017).
[3] Maurer, R. J., Ruiz, V. G. & Tkatchenko, A. J. Chem. Phys. 143, 102808 (2015).
[4] Müller, M., Diller, K., Maurer, R. J. & Reuter, K. J. Chem. Phys. 144, 24701 (2016).
[5] Stöhr, M., Michelitsch, G. S., Tully, J. C., Reuter, K. & Maurer, R. J. J. Chem. Phys. 144, 151101 (2016).