4.6 Article

CdSe nanocrystal sensitized photon upconverting film

Journal

RSC ADVANCES
Volume 11, Issue 49, Pages 31042-31046

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ra06562a

Keywords

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Funding

  1. Air Force Office of Scientific Research (AFOSR) Award [FA9550-19-1-0092]
  2. National Science Foundation [CHE-2003735, OISE-1827087]
  3. Robert A. Welch Foundation [F-1885]
  4. Sloan Fellowship
  5. NSF [1532125]

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Films using CdSe nanocrystal triplet photosensitizers with DPA emitters were assembled to address challenges in solution-based photon upconversion applications. The use of poly(9-vinylcarbazole) as a phosphorescent host eliminated volatile organic solvents and achieved a 1.5% photon upconversion quantum yield. The efficiency was limited by incomplete triplet-triplet annihilation due to a slower rate compared to solution-phase systems.
Here, films using CdSe nanocrystal (NC) triplet photosensitizers in conjunction with diphenylanthracene (DPA) emitters were assembled to address several challenges to practical applications for solution-based photon upconversion. By using poly(9-vinylcarbazole) as a phosphorescent host in this film, volatile organic solvents are eliminated, the spontaneous crystallization of the emitter is significantly retarded, and similar to 1.5% photon upconversion quantum yield (out of a maximum of 50%) is obtained. Transient absorption spectroscopy on nanosecond-to-microsecond time scales reveals this efficiency is enabled by an exceptionally long triplet lifetime of 3.4 +/- 0.3 ms. Ultimately, we find the upconversion efficiency is limited by incomplete triplet-triplet annihilation, which occurs with a rate 3-4 orders of magnitude slower than in solution-phase upconversion systems.

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