4.8 Article

Six-photon upconverted excitation energy lock-in for ultraviolet-C enhancement

Journal

NATURE COMMUNICATIONS
Volume 12, Issue 1, Pages -

Publisher

NATURE PORTFOLIO
DOI: 10.1038/s41467-021-24664-x

Keywords

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Funding

  1. National Basic Research Program of China [2016YFA0201600]
  2. National Natural Science Foundation of China [21701109, 31771105]
  3. Shanghai Shuguang Program [18SG29]
  4. Natural Science Foundation of Shanghai [18ZR1401700]

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The paper presents a novel six-photon upconversion process in nanoparticles with a heterogeneous core-multishell structure, which efficiently regulates energy transfer pathways to enhance ultraviolet emission under near-infrared excitation.
Photon upconversion of near-infrared (NIR) irradiation into ultraviolet-C (UVC) emission offers many exciting opportunities for drug release in deep tissues, photodynamic therapy, solid-state lasing, energy storage, and photocatalysis. However, NIR-to-UVC upconversion remains a daunting challenge due to low quantum efficiency. Here, we report an unusual six-photon upconversion process in Gd3+/Tm3+-codoped nanoparticles following a heterogeneous core-multishell architecture. This design efficiently suppresses energy consumption induced by interior energy traps, maximizes cascade sensitizations of the NIR excitation, and promotes upconverted UVC emission from high-lying excited states. We realized the intense six-photon-upconverted UV emissions at 253nm under 808nm excitation. This work provides insight into mechanistic understanding of the upconversion process within the heterogeneous architecture, while offering exciting opportunities for developing nanoscale UVC emitters that can be remotely controlled through deep tissues upon NIR illumination. Photon upconversion with near-infrared excitation and ultraviolet emission has many applications, but suffers from low quantum efficiency. Here, the authors report a six-photon upconversion process in nanoparticles with heterogeneous core-multishell structure, that regulate the energy transfer pathway.

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