Abstract
Developing light-harvesting materials with tunable emission colours has always been at the forefront of colour display technologies1,2,3. The variation in materials composition, phase and structure can provide a useful tool for producing a wide range of emission colours, but controlling the colour gamut in a material with a fixed composition remains a daunting challenge4,5. Here, we demonstrate a convenient, versatile approach to dynamically fine-tuning emission in the full colour range from a new class of core–shell upconversion nanocrystals by adjusting the pulse width of infrared laser beams. Our mechanistic investigations suggest that the unprecedented colour tunability from these nanocrystals is governed by a non-steady-state upconversion process. These findings provide keen insights into controlling energy transfer in out-of-equilibrium optical processes, while offering the possibility for the construction of true three-dimensional, full-colour display systems with high spatial resolution and locally addressable colour gamut.
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References
Matsubara, H. et al. GaN photonic-crystal surface-emitting laser at blue-violet wavelengths. Science 319, 445–447 (2008).
Lee, J. et al. Universal process-inert encoding architecture for polymer microparticles. Nature Mater. 13, 524–529 (2014).
Park, S. et al. Printed assemblies of inorganic light-emitting diodes for deformable and semitransparent displays. Science 325, 977–981 (2009).
Downing, E., Hesselink, L., Ralston, J. & Macfarlane, R. A three-color, solid-state, three-dimensional display. Science 273, 1185–1189 (1996).
Kim, T. H. et al. Full-color quantum dot displays fabricated by transfer printing. Nature Photon. 5, 176–182 (2011).
Sun, Y. et al. Quantum-sized carbon dots for bright and colorful photoluminescence. J. Am. Chem. Soc. 128, 7756–7757 (2006).
Chen, O. et al. Excitation-intensity-dependent color-tunable dual emissions from manganese-doped CdS/ZnS core/shell nanocrystals. Angew. Chem. Int. Ed. 49, 10132–10135 (2010).
Han, S., Deng, R., Xie, X. & Liu, X. Enhancing luminescence in lanthanide-doped upconversion nanoparticles. Angew. Chem. Int. Ed. 53, 11702–11715 (2014).
Gai, S., Li, C., Yang, P. & Lin, J. Recent progress in rare earth micro/nanocrystals: soft chemical synthesis, luminescent properties, and biomedical applications. Chem. Rev. 114, 2343–2389 (2014).
Bünzli, J. C. G. & Piguet, C. Taking advantage of luminescent lanthanide ions. Chem. Soc. Rev. 34, 1048–1077 (2005).
Rapaport, A., Milliez, J., Bass, M., Cassanho, A. & Jenssen, H. Review of the properties of up-conversion phosphors for new emissive displays. J. Display Technol. 2, 68–78 (2006).
Wen, H. et al. Upconverting near-infrared light through energy management in core–shell–shell nanoparticles. Angew. Chem. Int. Ed. 52, 13419–13423 (2013).
Heer, S., Kömpe, K., Güdel, H. U. & Haase, M. Highly efficient multicolour upconversion emission in transparent colloids of lanthanide-doped NaYF4 nanocrystals. Adv. Mater. 16, 2102–2105 (2004).
Li, X., Wang, R., Zhang, F. & Zhao, D. Engineering homogeneous doping in single nanoparticle to enhance upconversion efficiency. Nano Lett. 14, 3634–3639 (2014).
Wang, F. & Liu, X. Multicolor tuning of lanthanide-doped nanoparticles by single wavelength excitation. Acc. Chem. Res. 47, 1378–1385 (2014).
Haase, M. & Schäfer, H. Upconverting nanoparticles. Angew. Chem. Int. Ed. 50, 5808–5829 (2011).
Van der Ende, B. M., Aarts, L. & Meijerink, A. Lanthanide ions as spectral converters for solar cells. Phys. Chem. Chem. Phys. 11, 11081–11095 (2009).
Gargas, D. J. et al. Engineering bright sub-10-nm upconverting nanocrystals for single-molecule imaging. Nature Nanotech. 9, 300–305 (2014).
Ju, Q. et al. Amine-functionalized lanthanide-doped KGdF4 nanocrystals as potential optical/magnetic multimodal bioprobes. J. Am. Chem. Soc. 134, 1323–1330 (2012).
Zhou, J. et al. Ultrasensitive polarized up-conversion of Tm3+–Yb3+ doped β-NaYF4 single nanorod. Nano Lett. 13, 2241–2246 (2013).
Mahalingam, V. et al. Bright white upconversion emission from Tm3+/Yb3+/Er3+ doped Lu3Ga5O12 nanocrystals. J. Phys. Chem. C 112, 17745–17749 (2008).
Vetrone, F., Boyer, J. C., Capobianco, J. A., Speghini, A. & Bettinelli, M. Significance of Yb3+ concentration on the upconversion mechanisms in codoped Y2O3:Er3+, Yb3+ nanocrystals. J. Appl. Phys. 96, 661–667 (2004).
Sharma, G. & Trussell, H. J. Digital color imaging. IEEE Trans. Image Process. 6, 901–932 (1997).
Shen, J. et al. Engineering the upconversion nanoparticle excitation wavelength: cascade sensitization of tri-doped upconversion colloidal nanoparticles at 800 nm. Adv. Opt. Mater. 1, 644–650 (2013).
Wang, Y. et al. Nd3+-sensitized upconversion nanophosphors: efficient in vivo bioimaging probes with minimized heating effect. ACS Nano 7, 7200–7206 (2013).
Auzel, F. Upconversion and anti-Stokes processes with f and d ions in solids. Chem. Rev. 104, 139–174 (2004).
Sivakumar, S., van Veggel, F. C. J. M. & May, P. S. Near-infrared (NIR) to red and green up-conversion emission from silica sol–gel thin films made with La0.45Yb0.50Er0.05F3 nanoparticles, hetero-looping-enhanced energy transfer (hetero-LEET): a new up-conversion process. J. Am. Chem. Soc. 129, 620–625 (2007).
Fattal, D. et al. A multi-directional backlight for a wide-angle, glasses-free three-dimensional display. Nature 495, 348–351 (2013).
Zhou, J., Liu, Z. & Li, F. Upconversion nanophosphors for small-animal imaging. Chem. Soc. Rev. 41, 1323–1349 (2012).
Lu, Y. et al. Tunable lifetime multiplexing using luminescent nanocrystals. Nature Photon. 8, 32–36 (2014).
Wang, J. et al. Near-infrared-light-mediated imaging of latent fingerprints based on molecular recognition. Angew. Chem. Int. Ed. 53, 1616–1620 (2014).
Debasu, M. L. et al. All-in-one optical heater-thermometer nanoplatform operative from 300 to 2000 K based on Er3+ emission and blackbody radiation. Adv. Mater. 25, 4868–4874 (2013).
Wang, F. et al. Simultaneous phase and size control of upconversion nanocrystals through lanthanide doping. Nature 463, 1061–1065 (2010).
Acknowledgements
The work was supported by the Singapore Ministry of Education (grant no. MOE2010-T2-1-083), the Agency for Science, Technology and Research (A*STAR; grant no. 1231AFG028), the National Research Foundation and the Priority Academic Program Development of Jiangsu Higher Education Institutions, Fundamental Studies of Perovskite Solar Cells (2015CB932200), and the National Natural Science Foundation of China (grant nos. 51173081, 61136003). M.H. acknowledges the National Research Foundation, Prime Minister's Office, Singapore, for financial support under the Competitive Research Program (CRP award no. NRF-CRP10-2012-04).
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R.D. and X.L. conceived the projects with contributions from W.H. and M.H. R.D. and F.Q. were primarily responsible for the experiments. R.C. contributed to numerical simulations. M.H. and W.H. provided input into the design of the experiments. R.D. and X.L. wrote the paper. All authors discussed the results and commented on the manuscript.
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Deng, R., Qin, F., Chen, R. et al. Temporal full-colour tuning through non-steady-state upconversion. Nature Nanotech 10, 237–242 (2015). https://doi.org/10.1038/nnano.2014.317
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DOI: https://doi.org/10.1038/nnano.2014.317
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