Ultrafast Intraband Spectroscopy of Hot-Carrier Cooling in Lead-Halide Perovskites
Artem Bakulin a
a Department of Chemistry, Imperial College London, South Kensington Campus London, London, United Kingdom
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2018 (NFM18)
S5 Charge Carrier Dynamics at the Nanoscale
Torremolinos, Spain, 2018 October 22nd - 26th
Organizers: David Egger, Arjan Houtepen and Freddy Rabouw
Invited Speaker, Artem Bakulin, presentation 039
DOI: https://doi.org/10.29363/nanoge.nfm.2018.039
Publication date: 6th July 2018

In conventional solar cells (SCs), above-bandgap “hot” carriers (HCs) rapidly lose their excess energy to vibrations in the semiconductor lattice via electron-phonon coupling. This thermalisation to the band edge forms the main part of the Shockley-Queisser limiting efficiency. Semiconductors with reduced carrier cooling rates are desirable to exceed this limit via a hot-carrier architecture, where the hot carriers are extracted before they are fully cooled. Lead-halide perovskites are solution processible solar cell materials, which exhibit exceptional power conversion efficiencies and a tunable band gap. Recent measurements indicate slow cooling at high carrier densities in these material systems. Here we use ultrafast infrared intraband spectroscopy to directly compare the dynamics of carrier cooling in a range of five commonly studied lead-halide perovskites: FAPbI3, FAPbBr3, MAPbI3, MAPbBr3 and CsPbBr3. We measure this cooling as occuring within ~100-900 fs, depending on both the carrier density, nhot (slower cooling at higher nhot) and choice of cation (with the slowest cooling in the all-inorganic Cs-based system). These observations support the existence of a “hot-phonon bottleneck” and assert the role of lattice vibrations towards HC cooling.

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