Cool carriers: triplet diffusion dominates upconversion yield

Colette M. Sullivan, Jason E. Kuszynski, Alexey Kovalev, Theo Siegrist, Richard D. Schaller, Geoffrey F. Strouse, Lea Nienhaus*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Perovskites have gained popularity both as the active material in photovoltaics and as bulk triplet sensitizers for solid-state triplet-triplet annihilation upconversion (TTA-UC). Prior to widespread implementation into commercial photovoltaics, an in-depth understanding of the environmental influences on device performance is required. To this point, the temperature-dependent structure-function properties of TTA-UC within methylammonium formamidinium lead triiodide (MAFA)/rubrene UC devices are explored. A strong temperature dependence of the underlying UC dynamics is observed, where the maximum UC efficiency is achieved at 170 K, reflecting the competition between triplet diffusion length, diffusion rate, and triplet-triplet encounter events. A combination of spectroscopic and structural methods and theoretical modelling illustrates that despite the significantly increased carrier lifetime of the perovskite at low temperatures, the TTA-UC dynamics are not governed by the underlying sensitizer properties but rather limited by the underlying triplet diffusion.

Original languageEnglish (US)
Pages (from-to)18832-18841
Number of pages10
JournalNanoscale
Volume15
Issue number46
DOIs
StatePublished - Nov 3 2023

Funding

C. M. S. and L. N. acknowledge funding by the National Science Foundation under Grant No. DMR-2237977 and the Camille and Henry Dreyfus Foundation (TC-23-050). J. E. K. and G. F. S. acknowledge the National Science Foundation under Grant No. DMR-1905757. J. E. K. acknowledges the U.S. Department of Defense SMART scholarship funded under OUSD/R&E, NDEP/BA-1. A. S. and T. S. performed part of the work at the National High Magnetic Field Laboratory, which is supported by the National Science Foundation under grant DMR-2128556 and the State of Florida. T. S. acknowledges funding by the National Science Foundation under grant DMR-2219906. Work performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357.

ASJC Scopus subject areas

  • General Materials Science

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