Ultrafast Intraband Spectroscopy of Hot-Carrier Cooling in Lead-Halide Perovskites
File(s)PPP-pskt_Paper-v23.pdf (1.23 MB)
Accepted version
Author(s)
Type
Journal Article
Abstract
The rapid relaxation of above-band-gap “hot” carriers (HCs) imposes the key efficiency limit in lead-halide perovskite (LHP) solar cells. Recent studies have indicated that HC cooling in these systems may be sensitive to materials composition, as well as the energy and density of excited states. However, the key parameters underpinning the cooling mechanism are currently under debate. Here we use a sequence of ultrafast optical pulses (visible pump–infrared push–infrared probe) to directly compare the intraband cooling dynamics in five common LHPs: FAPbI3, FAPbBr3, MAPbI3, MAPbBr3, and CsPbBr3. We observe ∼100–900 fs cooling times, with slower cooling at higher HC densities. This effect is strongest in the all-inorganic Cs-based system, compared to the hybrid analogues with organic cations. These observations, together with band structure calculations, allow us to quantify the origin of the “hot-phonon bottleneck” in LHPs and assert the thermodynamic contribution of a symmetry-breaking organic cation toward rapid HC cooling.
Date Issued
2018-09-14
Date Acceptance
2018-08-21
Citation
ACS Energy Letters, 2018, 3 (9), pp.2199-2205
ISSN
2380-8195
Publisher
American Chemical Society
Start Page
2199
End Page
2205
Journal / Book Title
ACS Energy Letters
Volume
3
Issue
9
Copyright Statement
© 2018 American Chemical Society
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Electrochemistry
Energy & Fuels
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Chemistry
Science & Technology - Other Topics
Materials Science
SOLAR-CELLS
IODIDE PEROVSKITE
HYBRID PEROVSKITES
ORGANIC CATION
TRIHALIDE PEROVSKITES
SINGLE-CRYSTALS
QUANTUM DOTS
THIN-FILMS
ELECTRON
TRANSPORT
Publication Status
Published
Date Publish Online
2018-08-21