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Triplets electrically turn on insulating lanthanide-doped nanoparticles.

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Peer-reviewed

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Abstract

Insulating nanomaterials have large energy gaps and are only electrically accessible under extreme conditions, such as high-intensity radiation and high temperature, pressure or voltage1,2. Lanthanide-doped insulating nanoparticles (LnNPs) are widely studied owing to their exceptional luminescence properties, including bright, narrow-linewidth, non-blinking and non-bleaching emission in the second near-infrared (NIR-II) range3,4. However, it has not been possible to electrically generate excited states in these insulating nanomaterials under low biases and, therefore, not possible to fabricate optoelectronic devices from these systems. Here we report an electrical excitation pathway to obtain emission from LnNPs. By forming LnNP@organic molecule nanohybrids, in which the recombination of electrically injected charges on the organic molecule is followed by efficient triplet energy transfer (TET) to the LnNP, it is possible to turn on LnNPs under a low operating bias. We demonstrate this excitation pathway in light-emitting diodes (LEDs), with low turn-on voltages of about 5 V, very narrow electroluminescence (EL) spectra and a peak external quantum efficiency (EQE) greater than 0.6% in the NIR-II window5. Our LnNP-based LEDs (LnLEDs) also allow for widely tunable EL properties, by changing the type and concentration of lanthanide dopants. These results open up a new field of hybrid optoelectronic devices and provide new opportunities for the electrically driven excitation sources based on lanthanide nanomaterials for biomedical and optoelectronic applications.

Description

Acknowledgements: This work was supported by a UK Research and Innovation (UKRI) Frontier Research Grant (EP/Y015584/1). Z.Y. acknowledges funding from UKRI Postdoctoral Individual Fellowships (grant reference EP/X023133X/1). Y.D. acknowledges funding from UKRI Postdoctoral Individual Fellowships (grant reference EP/Y02771X/1). J.Y. and R.L.Z.H. thank UKRI for funding through a Frontier Grant (no. EP/X022900/1), awarded through the 2021 European Research Council (ERC) Starting Grant scheme. J.Y. and R.L.Z.H. thank St. John’s College, Oxford for support through the Large Grant scheme. R.L.Z.H. also thanks the Royal Academy of Engineering for support through the Senior Research Fellowships scheme (no. RCSRF2324-18-68). L.v.T. acknowledges funding from the Winton Programme for the Physics of Sustainability and from the Engineering and Physical Sciences Research Council (EPSRC). A.T. acknowledges support from the UKRI NanoDTC Cambridge EP/S022953/1. Y.S. acknowledges funding from UKRI (grant reference EP/S030638/1) and China Scholarship Council and Cambridge Trust Scholarship. R.A. acknowledges support from St. John’s College, Cambridge, the Rutherford Foundation of the Royal Society Te Apārangi of New Zealand and the Winton Programme for the Physics of Sustainability. J.J.B. acknowledges support from the ERC under the Horizon 2020 research and innovation programme THOR (grant agreement no. 829067) and PICOFORCE (grant agreement no. 883703). Y.L. acknowledges funding from the EPSRC (EP/V06164X/1). The GIWAXS measurement was carried out with the support of Diamond Light Source, Beamline I07 (proposal SI32266).

Journal Title

Nature

Conference Name

Journal ISSN

0028-0836
1476-4687

Volume Title

647

Publisher

Springer Nature

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Except where otherwised noted, this item's license is described as http://creativecommons.org/licenses/by/4.0/
Sponsorship
Engineering and Physical Sciences Research Council (EP/S030638/1)