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An autonomous photosynthetic device in which all charge carriers derive from surface plasmons

Nature Nanotechnology volume 8, pages 247–251 (2013)Cite this article

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Abstract

Solar conversion to electricity or to fuels based on electron–hole pair production in semiconductors is a highly evolved scientific and commercial enterprise1,2,3,4,5,6,7,8,9,10. Recently, it has been posited that charge carriers either directly transferred from the plasmonic structure to a neighbouring semiconductor (such as TiO2) or to a photocatalyst, or induced by energy transfer in a neighbouring medium, could augment photoconversion processes, potentially leading to an entire new paradigm in harvesting photons for practical use11,12,13,14,15,16. The strong dependence of the wavelength at which the local surface plasmon can be excited on the nanostructure makes it possible, in principle, to design plasmonic devices that can harvest photons over the entire solar spectrum and beyond. So far, however, most such systems show rather small photocatalytic activity in the visible as compared with the ultraviolet17,18,19,20,21,22,23,24,25,26. Here, we report an efficient, autonomous solar water-splitting device based on a gold nanorod array in which essentially all charge carriers involved in the oxidation and reduction steps arise from the hot electrons resulting from the excitation of surface plasmons in the nanostructured gold. Each nanorod functions without external wiring, producing 5 × 1013 H2 molecules per cm2 per s under 1 sun illumination (AM 1.5 and 100 mW cm−2), with unprecedented long-term operational stability.

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Figure 1: Structure and mechanism of operation of the autonomous plasmonic solar water splitter.
Figure 2: Hydrogen production rates and wavelength response.
Figure 3: Photocurrent output and wavelength response at the plasmonic photocathode.

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Acknowledgements

The authors acknowledge research support from the Institute for Energy Efficiency, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences (award no. DE-SC0001009). The authors made extensive use of the MRL Central Facilities at UCSB, which are supported by the MRSEC Program of the NSF (under award no. DMR 1121053), a member of the NSF-funded Materials Research Facilities Network (www.mrfn.org). N.S. is supported by the ConvEne IGERT Program (NSF-DGE 0801627). The authors thank Wei Cheng for helpful suggestions regarding GC analysis.

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Author notes

  1. Syed Mubeen and Joun Lee: These authors contributed equally to this work

Authors and Affiliations

  1. Department of Chemistry, University of California, Santa Barbara, 93106, California, USA

    Syed Mubeen, Joun Lee, Galen D. Stucky & Martin Moskovits

  2. Department of Chemical Engineering, University of California, Santa Barbara, 93106, California, USA

    Nirala Singh

  3. Materials Department, University of California, Santa Barbara, 93106, California, USA

    Stephan Krämer

Authors
  1. Syed Mubeen
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  2. Joun Lee
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  6. Martin Moskovits
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Contributions

S.M., J.L., G.D.S. and M.M. conceived the concept. S.M., J.L. and M.M. designed processing and device fabrication details. S.M. and J.L. performed the experiments and N.S. assisted S.M. in performing gas analysis. S.K. and J.L. performed optical and structural studies. S.M., J.L. and M.M. wrote the manuscript and prepared the figures. All authors discussed the results and commented on the manuscript. M.M. supervised the project.

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Correspondence to Martin Moskovits.

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The authors declare no competing financial interests.

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Mubeen, S., Lee, J., Singh, N. et al. An autonomous photosynthetic device in which all charge carriers derive from surface plasmons. Nature Nanotech 8, 247–251 (2013). https://doi.org/10.1038/nnano.2013.18

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