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Title: Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy

Abstract

The Shockley-Queisser limit for solar cell efficiency can be overcome if hot carriers can be harvested before they thermalize. Recently, carrier cooling time up to 100 picoseconds was observed in hybrid perovskites, but it is unclear whether these long-lived hot carriers can migrate long distance for efficient collection. Here, we report direct visualization of hot-carrier migration in methylammonium lead iodide (CH 3NH 3PbI 3) thin films by ultrafast transient absorption microscopy, demonstrating three distinct transport regimes. Quasiballistic transport was observed to correlate with excess kinetic energy, resulting in up to 230 nanometers transport distance that could overcome grain boundaries. The nonequilibrium transport persisted over tens of picoseconds and ~600 nanometers before reaching the diffusive transport limit. Lastly, these results suggest potential applications of hot-carrier devices based on hybrid perovskites.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Purdue Univ., West Lafayette, IN (United States). Dept. of Chemistry
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S); National Science Foundation (NSF)
OSTI Identifier:
1351584
Report Number(s):
NREL/JA-5900-68003
Journal ID: ISSN 0036-8075
Grant/Contract Number:  
AC36-08GO28308; NSF-DMR-1507803
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 356; Journal Issue: 6333; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; hot-carrier devices; hybrid perovskites; efficiency; transport

Citation Formats

Guo, Zhi, Wan, Yan, Yang, Mengjin, Snaider, Jordan, Zhu, Kai, and Huang, Libai. Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy. United States: N. p., 2017. Web. doi:10.1126/science.aam7744.
Guo, Zhi, Wan, Yan, Yang, Mengjin, Snaider, Jordan, Zhu, Kai, & Huang, Libai. Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy. United States. doi:10.1126/science.aam7744.
Guo, Zhi, Wan, Yan, Yang, Mengjin, Snaider, Jordan, Zhu, Kai, and Huang, Libai. Fri . "Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy". United States. doi:10.1126/science.aam7744. https://www.osti.gov/servlets/purl/1351584.
@article{osti_1351584,
title = {Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy},
author = {Guo, Zhi and Wan, Yan and Yang, Mengjin and Snaider, Jordan and Zhu, Kai and Huang, Libai},
abstractNote = {The Shockley-Queisser limit for solar cell efficiency can be overcome if hot carriers can be harvested before they thermalize. Recently, carrier cooling time up to 100 picoseconds was observed in hybrid perovskites, but it is unclear whether these long-lived hot carriers can migrate long distance for efficient collection. Here, we report direct visualization of hot-carrier migration in methylammonium lead iodide (CH3NH3PbI3) thin films by ultrafast transient absorption microscopy, demonstrating three distinct transport regimes. Quasiballistic transport was observed to correlate with excess kinetic energy, resulting in up to 230 nanometers transport distance that could overcome grain boundaries. The nonequilibrium transport persisted over tens of picoseconds and ~600 nanometers before reaching the diffusive transport limit. Lastly, these results suggest potential applications of hot-carrier devices based on hybrid perovskites.},
doi = {10.1126/science.aam7744},
journal = {Science},
number = 6333,
volume = 356,
place = {United States},
year = {Fri Apr 07 00:00:00 EDT 2017},
month = {Fri Apr 07 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 35 works
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Works referenced in this record:

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journal, July 2013

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Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3
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journal, January 2015