Carrier-Specific Hot Phonon Bottleneck in CH3NH3PbI3Revealed by Femtosecond XUV Absorption

Max Verkamp, Joshua Leveillee, Aastha Sharma, Ming Fu Lin, André Schleife, Josh Vura-Weis

Research output: Contribution to journalArticlepeer-review


Femtosecond carrier cooling in the organohalide perovskite semiconductor CH3NH3PbI3 is measured using extreme ultraviolet (XUV) and optical transient absorption spectroscopy. XUV absorption between 44 and 58 eV measures transitions from the I 4d core to the valence and conduction bands and gives distinct signals for hole and electron dynamics. The core-to-valence-band signal directly maps the photoexcited hole distribution and provides a quantitative measurement of the hole temperature. The combination of XUV and optical probes reveals that upon excitation at 400 nm, the initial hole distribution is 3.5 times hotter than the electron distribution. At an initial carrier density of 1.4 × 1020 cm-3 both carriers are subject to a hot phonon bottleneck, but at 4.2 × 1019 cm-3 the holes cool to less than 1000 K within 400 fs. This result places significant constraints on the use of organohalide perovskites in hot-carrier photovoltaics.

Original languageEnglish (US)
Pages (from-to)20176-20182
Number of pages7
JournalJournal of the American Chemical Society
Issue number48
StatePublished - Dec 8 2021

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry


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