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

144 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

Fingerprint

Lanthanoid Series Elements
Rare earth elements
Fluorides
Nanocrystals
fluorides
Nanostructures
nanocrystals
Coloring Agents
Dyes
dyes
Ions
Infrared radiation
Energy transfer
Photons
Nanoparticles
energy transfer
Quantum yield
excitation
Quantum efficiency
Energy conversion

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

Cite this

Chen, G., Damasco, J., Qiu, H., Shao, W., Ohulchanskyy, T. Y., Valiev, R. R., ... 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

Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal. / Chen, Guanying; Damasco, Jossana; Qiu, Hailong; Shao, Wei; Ohulchanskyy, Tymish Y.; Valiev, Rashid R.; Wu, Xiang; Han, Gang; Wang, Yan; Yang, Chunhui; Ågren, Hans; Prasad, Paras N.

In: Nano Letters, Vol. 15, No. 11, 11.11.2015, p. 7400-7407.

Research output: Contribution to journalArticle

Chen, G, Damasco, J, Qiu, H, Shao, W, Ohulchanskyy, TY, Valiev, RR, Wu, X, Han, G, Wang, Y, Yang, C, Ågren, H & Prasad, PN 2015, 'Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal', Nano Letters, vol. 15, no. 11, pp. 7400-7407. https://doi.org/10.1021/acs.nanolett.5b02830
Chen, Guanying ; Damasco, Jossana ; Qiu, Hailong ; Shao, Wei ; Ohulchanskyy, Tymish Y. ; Valiev, Rashid R. ; Wu, Xiang ; Han, Gang ; Wang, Yan ; Yang, Chunhui ; Ågren, Hans ; Prasad, Paras N. / Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal. In: Nano Letters. 2015 ; Vol. 15, No. 11. pp. 7400-7407.
@article{dd1f6d4db165410bba12419ea068f7c8,
title = "Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal",
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.",
keywords = "Core/Shell, Dye-Sensitized, Lanthanide, Nanoparticles, Rare-Earth, Upconversion",
author = "Guanying Chen and Jossana Damasco and Hailong Qiu and Wei Shao and Ohulchanskyy, {Tymish Y.} and Valiev, {Rashid R.} and Xiang Wu and Gang Han and Yan Wang and Chunhui Yang and Hans {\AA}gren and Prasad, {Paras N.}",
year = "2015",
month = "11",
day = "11",
doi = "10.1021/acs.nanolett.5b02830",
language = "English",
volume = "15",
pages = "7400--7407",
journal = "Nano Letters",
issn = "1530-6984",
publisher = "American Chemical Society",
number = "11",

}

TY - JOUR

T1 - Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal

AU - Chen, Guanying

AU - Damasco, Jossana

AU - Qiu, Hailong

AU - Shao, Wei

AU - Ohulchanskyy, Tymish Y.

AU - Valiev, Rashid R.

AU - Wu, Xiang

AU - Han, Gang

AU - Wang, Yan

AU - Yang, Chunhui

AU - Ågren, Hans

AU - Prasad, Paras N.

PY - 2015/11/11

Y1 - 2015/11/11

N2 - 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.

AB - 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.

KW - Core/Shell

KW - Dye-Sensitized

KW - Lanthanide

KW - Nanoparticles

KW - Rare-Earth

KW - Upconversion

UR - http://www.scopus.com/inward/record.url?scp=84946949537&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84946949537&partnerID=8YFLogxK

U2 - 10.1021/acs.nanolett.5b02830

DO - 10.1021/acs.nanolett.5b02830

M3 - Article

VL - 15

SP - 7400

EP - 7407

JO - Nano Letters

JF - Nano Letters

SN - 1530-6984

IS - 11

ER -