Tunable near-infrared and visible-light transmittance in nanocrystal-in-glass composites

Abstract

Amorphous metal oxides are useful in optical1,2, electronic3,4,5 and electrochemical devices6,7. The bonding arrangement within these glasses largely determines their properties, yet it remains a challenge to manipulate their structures in a controlled manner. Recently, we developed synthetic protocols for incorporating nanocrystals that are covalently bonded into amorphous materials8,9. This ‘nanocrystal-in-glass’ approach not only combines two functional components in one material, but also the covalent link enables us to manipulate the glass structure to change its properties. Here we illustrate the power of this approach by introducing tin-doped indium oxide nanocrystals into niobium oxide glass (NbOx), and realize a new amorphous structure as a consequence of linking it to the nanocrystals. The resulting material demonstrates a previously unrealized optical switching behaviour that will enable the dynamic control of solar radiation transmittance through windows. These transparent films can block near-infrared and visible light selectively and independently by varying the applied electrochemical voltage over a range of 2.5 volts. We also show that the reconstructed NbOx glass has superior properties—its optical contrast is enhanced fivefold and it has excellent electrochemical stability, with 96 per cent of charge capacity retained after 2,000 cycles.

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Figure 1: Nanocrystal-in-glass film preparation and structural characterization.
Figure 2: Raman analysis probing the reconstruction of a NbOx glass matrix when linked to nanocrystals.
Figure 3: ITO nanocrystals covalently linked to amorphous NbOx.
Figure 4: Tunable dual-band solar control and optical contrast enhancement in nanocrystal-in-glass films.

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Acknowledgements

We thank S. Raoux and J. L. Jordan-Sweet as well as S. Mannsfeld and M. Toney for assistance in synchrotron XRD measurements at the National Synchrotron Light Source (Brookhaven National Laboratory) and Stanford Synchrotron Radiation Lightsource (SSRL); and R. Zuckermann, P. J. Schuck, R. J. Mendelsberg, and especially M. Salmeron and O. Yaghi for critical reading of the manuscript. This work was performed at the Molecular Foundry, Lawrence Berkeley National Laboratory, and was supported by the Office of Science, Office of Basic Energy Sciences, of the US Department of Energy (DOE) under contract number DE-AC02—05CH11231. D.J.M. and G.G. were supported by a DOE Early Career Research Program grant under the same contract, and J.G. was supported by Consejo Superior de Investigaciones Cientificas, CSIC, JAE. Scanning transmission electron microscopy images were taken at Oak Ridge National Laboratory (ORNL), supported by DOE-BES, Materials Sciences and Engineering Division, and by ORNL’s Shared Research Equipment (ShaRE) User Program, which is also sponsored by DOE-BES. XRD data shown in the manuscript was acquired at SSRL, beamline 11-3.

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A.L. synthesized the materials, carried out the experiments and analysed the data, with assistance from G.G. for the electrochemical characterization. J.G. carried out scanning transmission electron microscopy imaging. A.L. and D.J.M. were responsible for experimental design and wrote the manuscript, which incorporates critical input from all authors.

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Correspondence to Delia J. Milliron.

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Competing interests

G.G. and D.J.M. have a financial interest in Heliotrope Technologies, a company pursuing the commercial development of electrochromic devices.

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Llordés, A., Garcia, G., Gazquez, J. et al. Tunable near-infrared and visible-light transmittance in nanocrystal-in-glass composites. Nature 500, 323–326 (2013). https://doi.org/10.1038/nature12398

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