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Hot-Electron Transfer from Semiconductor Nanocrystals

Science  18 Jun 2010:
Vol. 328, Issue 5985, pp. 1543-1547
DOI: 10.1126/science.1185509

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Hot on the Trail

Solar cells essentially operate by absorbing light, which needs to be above a certain energy threshold. The absorbed light then liberates charges within the solar cell to carry electrical current. Unfortunately, the liberated charges behave the same way whether they are excited right at the threshold (e.g., by visible light) or well above it (by ultraviolet light), which leads to any excess energy being dissipated as waste heat. Tisdale et al. (p. 1543) have documented a potential first step toward resolving this inefficiency. Specifically, electrons excited by light absorption in lead selenide nanocrystals were able to migrate to an adjacent titanium dioxide surface without releasing their excess energy to heat. The next step will be to devise a means of harnessing the stored energy in a circuit.

Abstract

In typical semiconductor solar cells, photons with energies above the semiconductor bandgap generate hot charge carriers that quickly cool before all of their energy can be captured, a process that limits device efficiency. Although fabricating the semiconductor in a nanocrystalline morphology can slow this cooling, the transfer of hot carriers to electron and hole acceptors has not yet been thoroughly demonstrated. We used time-resolved optical second harmonic generation to observe hot-electron transfer from colloidal lead selenide (PbSe) nanocrystals to a titanium dioxide (TiO2) electron acceptor. With appropriate chemical treatment of the nanocrystal surface, this transfer occurred much faster than expected. Moreover, the electric field resulting from sub–50-femtosecond charge separation across the PbSe-TiO2 interface excited coherent vibrations of the TiO2 surface atoms, whose motions could be followed in real time.

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