Quasi-thresholdless Photon Upconversion in Metal-Organic Framework Nanocrystals

F. Meinardi, M. Ballabio, Nobuhiro Yanai, Nobuo Kimizuka, A. Bianchi, M. Mauri, R. Simonutti, A. Ronchi, M. Campione, A. Monguzzi

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Photon upconversion based on sensitized triplet-triplet annihilation (sTTA) is considered as a promising strategy for the development of light-managing materials aimed to enhance the performance of solar devices by recovering unused low-energy photons. Here, we demonstrate that, thanks to the fast diffusion of excitons, the creation of triplet pairs in metal-organic framework nanocrystals (nMOFs) with size smaller than the exciton diffusion length implies a 100% TTA yield regardless of the illumination condition. This makes each nMOF a thresholdless, single-unit annihilator. We develop a kinetic model for describing the upconversion dynamics in a nanocrystals ensemble, which allows us to define the threshold excitation intensity Ith box required to reach the maximum conversion yield. For materials based on thresholdless annihilators, Ith box is determined by the statistical distribution of the excitation energy among nanocrystals. The model is validated by fabricating a nanocomposite material based on nMOFs, which shows efficient upconversion under a few percent of solar irradiance, matching the requirements of real life solar technologies. The statistical analysis reproduces the experimental findings, and represents a general tool for predicting the optimal compromise between dimensions and concentration of nMOFs with a given crystalline structure that minimizes the irradiance at which the system starts to fully operate.

Original languageEnglish
Pages (from-to)2169-2177
Number of pages9
JournalNano Letters
Volume19
Issue number3
DOIs
Publication statusPublished - Mar 13 2019

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Nanocrystals
nanocrystals
Photons
Metals
irradiance
Excitons
boxes
photons
excitons
metals
Excitation energy
diffusion length
statistical distributions
statistical analysis
excitation
Nanocomposites
Statistical methods
nanocomposites
Lighting
illumination

All Science Journal Classification (ASJC) codes

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

Cite this

Quasi-thresholdless Photon Upconversion in Metal-Organic Framework Nanocrystals. / Meinardi, F.; Ballabio, M.; Yanai, Nobuhiro; Kimizuka, Nobuo; Bianchi, A.; Mauri, M.; Simonutti, R.; Ronchi, A.; Campione, M.; Monguzzi, A.

In: Nano Letters, Vol. 19, No. 3, 13.03.2019, p. 2169-2177.

Research output: Contribution to journalArticle

Meinardi, F, Ballabio, M, Yanai, N, Kimizuka, N, Bianchi, A, Mauri, M, Simonutti, R, Ronchi, A, Campione, M & Monguzzi, A 2019, 'Quasi-thresholdless Photon Upconversion in Metal-Organic Framework Nanocrystals', Nano Letters, vol. 19, no. 3, pp. 2169-2177. https://doi.org/10.1021/acs.nanolett.9b00543
Meinardi, F. ; Ballabio, M. ; Yanai, Nobuhiro ; Kimizuka, Nobuo ; Bianchi, A. ; Mauri, M. ; Simonutti, R. ; Ronchi, A. ; Campione, M. ; Monguzzi, A. / Quasi-thresholdless Photon Upconversion in Metal-Organic Framework Nanocrystals. In: Nano Letters. 2019 ; Vol. 19, No. 3. pp. 2169-2177.
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