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Highly efficient large-area colourless luminescent solar concentrators using heavy-metal-free colloidal quantum dots

Nature Nanotechnology volume 10, pages 878–885 (2015)Cite this article

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Abstract

Luminescent solar concentrators serving as semitransparent photovoltaic windows could become an important element in net zero energy consumption buildings of the future. Colloidal quantum dots are promising materials for luminescent solar concentrators as they can be engineered to provide the large Stokes shift necessary for suppressing reabsorption losses in large-area devices. Existing Stokes-shift-engineered quantum dots allow for only partial coverage of the solar spectrum, which limits their light-harvesting ability and leads to colouring of the luminescent solar concentrators, complicating their use in architecture. Here, we use quantum dots of ternary I–III–VI2 semiconductors to realize the first large-area quantum dot–luminescent solar concentrators free of toxic elements, with reduced reabsorption and extended coverage of the solar spectrum. By incorporating CuInSexS2–x quantum dots into photo-polymerized poly(lauryl methacrylate), we obtain freestanding, colourless slabs that introduce no distortion to perceived colours and are thus well suited for the realization of photovoltaic windows. Thanks to the suppressed reabsorption and high emission efficiencies of the quantum dots, we achieve an optical power efficiency of 3.2%. Ultrafast spectroscopy studies suggest that the Stokes-shifted emission involves a conduction-band electron and a hole residing in an intragap state associated with a native defect.

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Figure 1: Concept of a reabsorption-free colourless LSC based on CISeS quantum dots.
Figure 2: Quantum dot–polymer nanocomposites.
Figure 3: Experimental evaluation of reabsorption losses in LSCs based on CISeS quantum dots.
Figure 4: Colorimetry characterization of LSCs based on CISeS quantum dots.
Figure 5: Origin of the Stokes shift in I–III–VI2 quantum dots.

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Acknowledgements

S.B. and F.M. acknowledge support from the Cariplo Foundation (2012-0844). V.I.K., H.M., K.A.V. and N.S.M. were supported by the Center for Advanced Solar Photophysics (CASP), an Energy Frontier Research Center funded by the Office of Basic Energy Sciences, Office of Science, US Department of Energy. S.B. acknowledges financial support from the European Community's Seventh Framework Programme (FP7/2007–2013) under grant agreement no. 324603 (EDONHIST). The authors thank M. Acciarri and the staff of the MIB-SOLAR laboratory for technical assistance in the quantitative studies of solar concentration and L. Raimondo and V. Pinchetti for assistance with the colorimetric analysis.

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Author notes

  1. Francesco Meinardi and Hunter McDaniel: These authors contributed equally to this work

Authors and Affiliations

  1. Dipartimento di Scienza dei Materiali, Università degli Studi di Milano-Bicocca, via Cozzi 55, Milano, I–20125, Italy

    Francesco Meinardi, Francesco Carulli, Annalisa Colombo, Roberto Simonutti & Sergio Brovelli

  2. Center for Advanced Solar Photophysics, Los Alamos National Laboratory, Los Alamos, 87545, New Mexico, USA

    Hunter McDaniel, Nikolay S. Makarov & Victor I. Klimov

  3. UbiQD, Los Alamos, 87544, New Mexico, USA

    Hunter McDaniel

  4. Theoretical Division & Center for Advanced Solar Photophysics, Los Alamos National Laboratory, Los Alamos, 87545, New Mexico, USA

    Kirill A. Velizhanin

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Contributions

The experiment designs were the result of ongoing interactions and discussions between F.M., V.I.K. and S.B. H.M. optimized and synthesized the quantum dots. F.C. fabricated the quantum dot–polymer nanocomposites with the assistance of S.B., A.C. and R.S. S.B., F.M., H.M. and V.I.K. planned the experiments. F.C., F.M. and S.B. performed the spectroscopic experiments and characterized the LSCs. K.A.V. performed the Monte Carlo simulations. S.B. and F.M. performed the colorimetric analysis. N.S.M. performed the transient absorption measurement. F.M., V.I.K. and S.B. wrote the paper, in consultation with all the authors.

Corresponding authors

Correspondence to Francesco Meinardi, Victor I. Klimov or Sergio Brovelli.

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Meinardi, F., McDaniel, H., Carulli, F. et al. Highly efficient large-area colourless luminescent solar concentrators using heavy-metal-free colloidal quantum dots. Nature Nanotech 10, 878–885 (2015). https://doi.org/10.1038/nnano.2015.178

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