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Inorganic-organic interfaces are important for enhancing the power conversionefficiency of silicon-based solar cells through singlet exciton fission (SF).We elucidated the structure of the first monolayers of tetracene (Tc), a SFmolecule, on hydrogen-passivated Si(111) [H-Si(111)] and hydrogenated amorphousSi (a-Si:H) by combining near-edge X-ray absorption fine structure (NEXAFS) andX-ray photoelectron spectroscopy (XPS) experiments with density functionaltheory (DFT) calculations. For samples grown at or below substrate temperaturesof 265 K, the resulting ultrathin Tc films are dominated by almostupright-standing molecules. The molecular arrangement is very similar to the Tcbulk phase, with only slightly higher average angle between the conjugatedmolecular plane normal and the surface normal ($\alpha$) around 77{\deg}.Judging from carbon K-edge X-ray absorption spectra, the orientation of the Tcmolecules are almost identical when grown on H-Si(111) and a-Si:H substrates aswell as for (sub)mono- to several-monolayer coverages. Annealing to roomtemperature, however, changes the film structure towards a smaller $\alpha$ ofabout 63{\deg}. A detailed DFT-assisted analysis suggests that this structuraltransition is correlated with a lower packing density and requires awell-chosen amount of thermal energy. Therefore, we attribute the resultingstructure to a distinct monolayer configuration that features less inclined,but still well-ordered molecules. The larger overlap with the substratewavefunctions makes this arrangement attractive for an optimized interfacialelectron transfer in SF-assisted silicon solar cells.

Tetracene ultrathin film growth on silicon