Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal

Guanying Chen, Jossana Damasco, Hailong Qiu, Wei Shao, Tymish Y. Ohulchanskyy, Rashid R. Valiev, Xiang Wu, Gang Han, Yan Wang, Chunhui Yang, Hans Ågren, Paras N. Prasad

Research output: Contribution to journalArticle

189 Citations (Scopus)

Abstract

Lanthanide-doped upconversion nanoparticles hold promises for bioimaging, solar cells, and volumetric displays. However, their emission brightness and excitation wavelength range are limited by the weak and narrowband absorption of lanthanide ions. Here, we introduce a concept of multistep cascade energy transfer, from broadly infrared-harvesting organic dyes to sensitizer ions in the shell of an epitaxially designed core/shell inorganic nanostructure, with a sequential nonradiative energy transfer to upconverting ion pairs in the core. We show that this concept, when implemented in a core-shell architecture with suppressed surface-related luminescence quenching, yields multiphoton (three-, four-, and five-photon) upconversion quantum efficiency as high as 19% (upconversion energy conversion efficiency of 9.3%, upconversion quantum yield of 4.8%), which is about ∼100 times higher than typically reported efficiency of upconversion at 800 nm in lanthanide-based nanostructures, along with a broad spectral range (over 150 nm) of infrared excitation and a large absorption cross-section of 1.47 × 10-14 cm2 per single nanoparticle. These features enable unprecedented three-photon upconversion (visible by naked eye as blue light) of an incoherent infrared light excitation with a power density comparable to that of solar irradiation at the Earth surface, having implications for broad applications of these organic-inorganic core/shell nanostructures with energy-cascaded upconversion.

Original languageEnglish
Pages (from-to)7400-7407
Number of pages8
JournalNano Letters
Volume15
Issue number11
DOIs
Publication statusPublished - 11 Nov 2015

Keywords

  • Core/Shell
  • Dye-Sensitized
  • Lanthanide
  • Nanoparticles
  • Rare-Earth
  • Upconversion

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

Fingerprint Dive into the research topics of 'Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal'. Together they form a unique fingerprint.

  • Cite this

    Chen, G., Damasco, J., Qiu, H., Shao, W., Ohulchanskyy, T. Y., Valiev, R. R., Wu, X., Han, G., Wang, Y., Yang, C., Ågren, H., & Prasad, P. N. (2015). Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal. Nano Letters, 15(11), 7400-7407. https://doi.org/10.1021/acs.nanolett.5b02830