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Upconversion on the Micrometer Scale: Impact of Local Heterogeneity.

Colette M Sullivan1, Jia-Shiang Chen2,3, Xuedan Ma2,3

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Microscopic variations in perovskite/naphtho[2,3-a]pyrene (NaPy) upconversion devices significantly impact performance. Microcrystals emitting from low-energy states act as hotspots, enhancing upconversion efficiency.

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Area of Science:

  • Materials Science
  • Optoelectronics
  • Solid-State Physics

Background:

  • Perovskite/naphtho[2,3-a]pyrene (NaPy) upconversion devices are crucial for optoelectronic applications.
  • Understanding microscopic heterogeneity is key to optimizing ensemble device properties.

Purpose of the Study:

  • To investigate the impact of microscopic heterogeneity on perovskite/NaPy upconversion device properties.
  • To correlate optical properties with upconversion efficiency at the microcrystal level.

Main Methods:

  • Combined atomic force microscopy and photoluminescence mapping.
  • Analysis of emission spectra from individual NaPy microcrystals under 405 nm excitation.

Main Results:

  • Significant microscopic inhomogeneity observed due to NaPy microcrystal formation.
  • NaPy exhibits three distinct emission states: S₁' (520 nm), excimer (560 nm), and S₁″ (620 nm).
  • Microcrystals with dominant low-energy S₁″ (J-dimer) emission show higher upconversion intensity than those with high-energy S₁' (I-aggregate) emission.

Conclusions:

  • Microscopic variations in perovskite/NaPy devices arise from local NaPy microcrystal formation.
  • Individual microcrystal optical properties vary spatially, necessitating multimodal characterization.
  • Microcrystals exhibiting strong S₁″ emission act as efficient, isolated upconversion hotspots.