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The operation of organic optoelectronic devices relies notably on the bulkproperties of compound molecular species, but even more so on the influence ofinterfaces thereof. The identification and characterization of elementalprocesses in these critical sections of a device thereby requires well-definedinterfaces with low defect density. In this context titanyl phthalocyanine(TiOPc) arises as an excellent candidate that reveals the formation of a stablebilayer structure with a characteristic "up-down" molecular arrangement thatoptimizes the dipole-dipole interaction within the bilayer. In our experimentalstudy, long-range ordered TiOPc bilayers have been grown on Ag(111) surfacesand analyzed using infrared absorption spectroscopy and scanning tunnelingmicroscopy. By monitoring the prominent Ti=O stretching mode in IRAS andidentifying local configurations in STM, a microscopic model for the growth ofTiOPc bilayers on Ag(111) is suggested. We demonstrate that defect structureswithin these bilayers lead to characteristic vibrational signatures which reactsensitively to the local environment of the molecules. Thermal desorptionspectroscopy reveals a high thermal stability of the TiOPc bilayer up to 500 K,which is attributed to hydrogen bonds between oxygen of the titanyl unit andthe hydrogen rim of phthalocyanines in the second layer, in addition tocontributions arising from the oppositely oriented axial dipole moments and theubiquitous van der Waals interactions.

Discrete nature of inhomogeneity: The initial stages and local configurations of TiOPc during bilayer growth on Ag(111)