UC Santa Barbara

The conversion of sunlight into electricity by photovoltaics is currently a mature science and the foundation of a lucrative industry. In conventional excitonic solar cells, electron-hole pairs are generated by light absorption in a semiconductor and separated by the "built in" potential resulting from charge transfer accompanying Fermi-level equalization either at a p-n or a Schottky junction, followed by carrier collection at appropriate electrodes. Here we report a stable, wholly plasmonic photovoltaic device in which photon absorption and carrier generation take place exclusively in the plasmonic metal. The field established at a metal-semiconductor Schottky junction separates charges. The negative carriers are high-energy (hot) electrons produced immediately following the plasmon's dephasing. Some of the carriers are energetic enough to clear the Schottky barrier or quantum mechanically tunnel through it, thereby producing the output photocurrent. Short circuit photocurrent densities in the range 70-120 μA cm(-2) were obtained for simulated one-sun AM1.5 illumination with devices based on arrays of parallel gold nanorods, conformally coated with 10 nm TiO2 films and fashioned with a Ti metal collector. For the device with short circuit currents of 120 μA cm(-2), the internal quantum efficiency is ∼2.75%, and its wavelength response tracks the absorption spectrum of the transverse plasmon of the gold nanorods indicating that the absorbed photon-to-electron conversion process resulted exclusively in the Au, with the TiO2 playing a negligible role in charge carrier production. Devices fabricated with 50 nm TiO2 layers had open-circuit voltages as high as 210 mV, short circuit current densities of 26 μA cm(-2), and a fill factor of 0.3. For these devices, the TiO2 contributed a very small but measurable fraction of the charge carriers.