Time-resolved infrared spectroscopy directly probes free and trapped carriers in organo-halide perovskites

Kyle T. Munson; Christopher Grieco; Eric R. Kennehan; Robert J. Stewart; John B. Asbury

doi:10.1021/acsenergylett.7b00033

Time-resolved infrared spectroscopy directly probes free and trapped carriers in organo-halide perovskites

Kyle T. Munson, Christopher Grieco, Eric R. Kennehan, Robert J. Stewart, John B. Asbury

Research output: Contribution to journal › Article › peer-review

37 Scopus citations

Abstract

Free carrier dynamics in organo-halide perovskites can directly reveal information about their carrier lifetimes and indirectly reveal information about trap state distributions, both of which are critical to improving their performance and stability. Time-resolved photoluminescence (TRPL) spectroscopy is commonly used to probe carrier dynamics in these materials, but the technique is only sensitive to radiative decay pathways and may not reveal the true carrier dynamics. We used time-resolved infrared (TRIR) spectroscopy in comparison to TRPL to show that photogenerated charges relax into free carrier states with lower radiative recombination probabilities, which complicates TRPL measurements. Furthermore, we showed that trapped carriers exhibit distinct mid-infrared absorptions that can be uniquely probed using TRIR spectroscopy. We used the technique to demonstrate the first simultaneous measurements of trapped and free carriers in organo-halide perovskites, which opens new opportunities to clarify how charge trapping and surface passivation influence the optoelectronic properties of these materials.

Original language	English (US)
Pages (from-to)	651-658
Number of pages	8
Journal	ACS Energy Letters
Volume	2
Issue number	3
DOIs	https://doi.org/10.1021/acsenergylett.7b00033
State	Published - Mar 10 2017

All Science Journal Classification (ASJC) codes

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

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10.1021/acsenergylett.7b00033

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title = "Time-resolved infrared spectroscopy directly probes free and trapped carriers in organo-halide perovskites",

abstract = "Free carrier dynamics in organo-halide perovskites can directly reveal information about their carrier lifetimes and indirectly reveal information about trap state distributions, both of which are critical to improving their performance and stability. Time-resolved photoluminescence (TRPL) spectroscopy is commonly used to probe carrier dynamics in these materials, but the technique is only sensitive to radiative decay pathways and may not reveal the true carrier dynamics. We used time-resolved infrared (TRIR) spectroscopy in comparison to TRPL to show that photogenerated charges relax into free carrier states with lower radiative recombination probabilities, which complicates TRPL measurements. Furthermore, we showed that trapped carriers exhibit distinct mid-infrared absorptions that can be uniquely probed using TRIR spectroscopy. We used the technique to demonstrate the first simultaneous measurements of trapped and free carriers in organo-halide perovskites, which opens new opportunities to clarify how charge trapping and surface passivation influence the optoelectronic properties of these materials.",

author = "Munson, {Kyle T.} and Christopher Grieco and Kennehan, {Eric R.} and Stewart, {Robert J.} and Asbury, {John B.}",

note = "Funding Information: K.T.M., C.G., E.R.K., and J.B.A. are grateful for support of this work from the U.S. National Science Foundation under Grant Number CHE-1464735. R.J.S. and J.B.A. were also supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the U.S. Department of Energy through Grant DE-SC0008120. Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

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AU - Stewart, Robert J.

AU - Asbury, John B.

N1 - Funding Information: K.T.M., C.G., E.R.K., and J.B.A. are grateful for support of this work from the U.S. National Science Foundation under Grant Number CHE-1464735. R.J.S. and J.B.A. were also supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the U.S. Department of Energy through Grant DE-SC0008120. Publisher Copyright: © 2017 American Chemical Society.

PY - 2017/3/10

Y1 - 2017/3/10

N2 - Free carrier dynamics in organo-halide perovskites can directly reveal information about their carrier lifetimes and indirectly reveal information about trap state distributions, both of which are critical to improving their performance and stability. Time-resolved photoluminescence (TRPL) spectroscopy is commonly used to probe carrier dynamics in these materials, but the technique is only sensitive to radiative decay pathways and may not reveal the true carrier dynamics. We used time-resolved infrared (TRIR) spectroscopy in comparison to TRPL to show that photogenerated charges relax into free carrier states with lower radiative recombination probabilities, which complicates TRPL measurements. Furthermore, we showed that trapped carriers exhibit distinct mid-infrared absorptions that can be uniquely probed using TRIR spectroscopy. We used the technique to demonstrate the first simultaneous measurements of trapped and free carriers in organo-halide perovskites, which opens new opportunities to clarify how charge trapping and surface passivation influence the optoelectronic properties of these materials.

AB - Free carrier dynamics in organo-halide perovskites can directly reveal information about their carrier lifetimes and indirectly reveal information about trap state distributions, both of which are critical to improving their performance and stability. Time-resolved photoluminescence (TRPL) spectroscopy is commonly used to probe carrier dynamics in these materials, but the technique is only sensitive to radiative decay pathways and may not reveal the true carrier dynamics. We used time-resolved infrared (TRIR) spectroscopy in comparison to TRPL to show that photogenerated charges relax into free carrier states with lower radiative recombination probabilities, which complicates TRPL measurements. Furthermore, we showed that trapped carriers exhibit distinct mid-infrared absorptions that can be uniquely probed using TRIR spectroscopy. We used the technique to demonstrate the first simultaneous measurements of trapped and free carriers in organo-halide perovskites, which opens new opportunities to clarify how charge trapping and surface passivation influence the optoelectronic properties of these materials.

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Time-resolved infrared spectroscopy directly probes free and trapped carriers in organo-halide perovskites

Abstract

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