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The electronic structure and chemical composition of efficient CH3NH3PbI3 perovskite solar cell materials deposited onto mesoporous TiO2 were studied using photoelectron spectroscopy with hard X-rays. With this technique, it is possible to directly measure the occupied energy levels of the perovskite as well as the TiO2 buried beneath and thereby determine the energy level matching of the interface. The measurements of the valence levels were in good agreement with simulated density of states, and the investigation gives information on the character of the valence levels. We also show that two different deposition techniques give results indicating similar electronic structures.

The ultrafast timescale of electron transfer processes is crucial to their role in many biological systems and technological devices. In dye-sensitized solar cells, the electron transfer from photo-excited dye molecules to nanostructured semiconductor substrates needs to be sufficiently fast to compete effectively against loss processes and thus achieve high solar energy conversion efficiencies. Time-resolved laser techniques indicate an upper limit of 20 to 100 femtoseconds for the time needed to inject an electron from a dye into a semiconductor, which corresponds to the timescale on which competing processes such as charge redistribution and intramolecular thermalization of excited states occur. Here we use resonant photoemission spectroscopy, which has previously been used to monitor electron transfer in simple systems with an order-of-magnitude improvement in time resolution, to show that electron transfer from an aromatic adsorbate to a TiO(2) semiconductor surface can occur in less than 3 fs. These results directly confirm that electronic coupling of the aromatic molecule to its substrate is sufficiently strong to suppress competing processes.

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We use x-ray emission spectroscopy to examine the influence of the intermolecular interaction on the local electronic structure of liquid water. By comparing x-ray emission spectra of the water molecule and liquid water, we find a strong involvement of the a(1)-symmetry valence-orbital in the hydrogen bonding. The local electronic structure of water molecules, where one hydrogen bond is broken at the hydrogen site, is separately determined. Our results provide an illustration of the important potential of x-ray emission spectroscopy for elucidating basic features of liquids.