Intraband Cooling in All-Inorganic and Hybrid Organic–Inorganic Perovskite Nanocrystals

Benjamin T. Diroll, Richard D Schaller

Research output: Contribution to journalArticle

Abstract

Intraband relaxation in all-inorganic cesium lead tribromide (CsPbBr3) and hybrid organic–inorganic formamidinium lead tribromide (FAPbBr3) nanocrystals is experimentally investigated for a range of particle sizes, excitation energies, sample temperatures, and excitation fluences. Hot carriers in CsPbBr3 nanocrystals consistently exhibit slower cooling than FAPbBr3 nanocrystals in the single electron–hole pair per nanocrystal regime. In both compositions, long-lived hot carriers (>3 ps) are only observed at excitation densities corresponding to production of multiple electron–hole pairs per nanocrystal—and concomitant Auger recombination. These presented results are distinct from previous reports in bulk hybrid perovskite materials that convey persistent hot carriers at low excitation fluences. Time-resolved photoluminescence confirms the rapid cooling of carriers in the low-fluence (single electron–hole pair per nanocrystal) regime. Intraband relaxation processes, as a function of excitation energy, size, and temperature are broadly consistent with other nanocrystalline semiconductor materials.

Original languageEnglish
Article number1901725
JournalAdvanced Functional Materials
DOIs
Publication statusPublished - Jan 1 2019

Fingerprint

Perovskite
Nanocrystals
nanocrystals
Hot carriers
Cooling
cooling
fluence
Excitation energy
excitation
Lead
Nanocrystalline materials
Cesium
Relaxation processes
cesium
Photoluminescence
Particle size
perovskite
Semiconductor materials
photoluminescence
Temperature

Keywords

  • hot carriers
  • intraband
  • nanocrystals
  • perovskites

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Biomaterials
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Electrochemistry

Cite this

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abstract = "Intraband relaxation in all-inorganic cesium lead tribromide (CsPbBr3) and hybrid organic–inorganic formamidinium lead tribromide (FAPbBr3) nanocrystals is experimentally investigated for a range of particle sizes, excitation energies, sample temperatures, and excitation fluences. Hot carriers in CsPbBr3 nanocrystals consistently exhibit slower cooling than FAPbBr3 nanocrystals in the single electron–hole pair per nanocrystal regime. In both compositions, long-lived hot carriers (>3 ps) are only observed at excitation densities corresponding to production of multiple electron–hole pairs per nanocrystal—and concomitant Auger recombination. These presented results are distinct from previous reports in bulk hybrid perovskite materials that convey persistent hot carriers at low excitation fluences. Time-resolved photoluminescence confirms the rapid cooling of carriers in the low-fluence (single electron–hole pair per nanocrystal) regime. Intraband relaxation processes, as a function of excitation energy, size, and temperature are broadly consistent with other nanocrystalline semiconductor materials.",
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AU - Schaller, Richard D

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N2 - Intraband relaxation in all-inorganic cesium lead tribromide (CsPbBr3) and hybrid organic–inorganic formamidinium lead tribromide (FAPbBr3) nanocrystals is experimentally investigated for a range of particle sizes, excitation energies, sample temperatures, and excitation fluences. Hot carriers in CsPbBr3 nanocrystals consistently exhibit slower cooling than FAPbBr3 nanocrystals in the single electron–hole pair per nanocrystal regime. In both compositions, long-lived hot carriers (>3 ps) are only observed at excitation densities corresponding to production of multiple electron–hole pairs per nanocrystal—and concomitant Auger recombination. These presented results are distinct from previous reports in bulk hybrid perovskite materials that convey persistent hot carriers at low excitation fluences. Time-resolved photoluminescence confirms the rapid cooling of carriers in the low-fluence (single electron–hole pair per nanocrystal) regime. Intraband relaxation processes, as a function of excitation energy, size, and temperature are broadly consistent with other nanocrystalline semiconductor materials.

AB - Intraband relaxation in all-inorganic cesium lead tribromide (CsPbBr3) and hybrid organic–inorganic formamidinium lead tribromide (FAPbBr3) nanocrystals is experimentally investigated for a range of particle sizes, excitation energies, sample temperatures, and excitation fluences. Hot carriers in CsPbBr3 nanocrystals consistently exhibit slower cooling than FAPbBr3 nanocrystals in the single electron–hole pair per nanocrystal regime. In both compositions, long-lived hot carriers (>3 ps) are only observed at excitation densities corresponding to production of multiple electron–hole pairs per nanocrystal—and concomitant Auger recombination. These presented results are distinct from previous reports in bulk hybrid perovskite materials that convey persistent hot carriers at low excitation fluences. Time-resolved photoluminescence confirms the rapid cooling of carriers in the low-fluence (single electron–hole pair per nanocrystal) regime. Intraband relaxation processes, as a function of excitation energy, size, and temperature are broadly consistent with other nanocrystalline semiconductor materials.

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