Investigating charge dynamics at lead halide perovskite single crystal surfaces

To further develop lead halide perovskites for their application in solar cells, understanding the material’s fundamental behavior under illumination is necessary. Investigating light-induced charge dynamics in single crystals can give insight into material inherent properties. Time-resolved photoel...

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Main Authors: Birgit Kammlander, Alberto García-Fernández, Sebastian Svanström, Erika Giangrisostomi, Ruslan Ovsyannikov, Håkan Rensmo, Ute B Cappel
Format: Article
Language:English
Published: IOP Publishing 2025-01-01
Series:JPhys Energy
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Online Access:https://doi.org/10.1088/2515-7655/ada63a
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author Birgit Kammlander
Alberto García-Fernández
Sebastian Svanström
Erika Giangrisostomi
Ruslan Ovsyannikov
Håkan Rensmo
Ute B Cappel
author_facet Birgit Kammlander
Alberto García-Fernández
Sebastian Svanström
Erika Giangrisostomi
Ruslan Ovsyannikov
Håkan Rensmo
Ute B Cappel
author_sort Birgit Kammlander
collection DOAJ
description To further develop lead halide perovskites for their application in solar cells, understanding the material’s fundamental behavior under illumination is necessary. Investigating light-induced charge dynamics in single crystals can give insight into material inherent properties. Time-resolved photoelectron spectroscopy (TR-PES) allows to monitor the photovoltage build-up and decay between the sample surface and bulk over time and gives information on light-induced charge redistribution within the crystal. Additionally, this method enables us to follow compositional changes and surface degradation and distinguish these from purely electronic effects. Here we investigated the charge dynamics of two distinct lead halide perovskite single crystal surfaces (CsPbBr _3 , Cs-doped FAPbI _3 ) using TR-PES in different timescales (ps to μ s and s to min). It was found that CsPbBr _3 shows photovoltage rise and decay on the nanosecond to microsecond time-range, which can be assigned to electron–hole pair separation between surface and bulk. On the other hand, such electron dynamics could not be resolved for Cs-doped FAPbI _3 at these fast timescales. Instead, for Cs-doped FAPbI _3 , the observed photovoltage decay was dominated by much slower dynamics and relaxation to the dark equilibrium state took around 10 min. This suggests that ion migration is responsible for a photovoltage build-up between surface and bulk of the crystal.
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spelling doaj-art-4c1750a6bb764157bf421d146582ccf72025-01-17T12:32:18ZengIOP PublishingJPhys Energy2515-76552025-01-017202500510.1088/2515-7655/ada63aInvestigating charge dynamics at lead halide perovskite single crystal surfacesBirgit Kammlander0https://orcid.org/0000-0002-7390-3062Alberto García-Fernández1https://orcid.org/0000-0003-1671-9979Sebastian Svanström2Erika Giangrisostomi3Ruslan Ovsyannikov4Håkan Rensmo5Ute B Cappel6https://orcid.org/0000-0002-9432-3112Division of X-ray Photon Science, Department of Physics and Astronomy, Uppsala University , Box 516, SE-751 20 Uppsala, SwedenDivision of X-ray Photon Science, Department of Physics and Astronomy, Uppsala University , Box 516, SE-751 20 Uppsala, SwedenDivision of X-ray Photon Science, Department of Physics and Astronomy, Uppsala University , Box 516, SE-751 20 Uppsala, SwedenInstitute Methods and Instrumentation for Synchrotron Radiation Research , Helmholtz-Zentrum Berlin GmbH, Albert-Einstein-Straße 15, 12489 Berlin, GermanyInstitute Methods and Instrumentation for Synchrotron Radiation Research , Helmholtz-Zentrum Berlin GmbH, Albert-Einstein-Straße 15, 12489 Berlin, GermanyDivision of X-ray Photon Science, Department of Physics and Astronomy, Uppsala University , Box 516, SE-751 20 Uppsala, Sweden; Wallenberg Initiative Materials Science for Sustainability, Department of Physics and Astronomy, Uppsala University , 751 20 Uppsala, SwedenDivision of X-ray Photon Science, Department of Physics and Astronomy, Uppsala University , Box 516, SE-751 20 Uppsala, Sweden; Wallenberg Initiative Materials Science for Sustainability, Department of Physics and Astronomy, Uppsala University , 751 20 Uppsala, SwedenTo further develop lead halide perovskites for their application in solar cells, understanding the material’s fundamental behavior under illumination is necessary. Investigating light-induced charge dynamics in single crystals can give insight into material inherent properties. Time-resolved photoelectron spectroscopy (TR-PES) allows to monitor the photovoltage build-up and decay between the sample surface and bulk over time and gives information on light-induced charge redistribution within the crystal. Additionally, this method enables us to follow compositional changes and surface degradation and distinguish these from purely electronic effects. Here we investigated the charge dynamics of two distinct lead halide perovskite single crystal surfaces (CsPbBr _3 , Cs-doped FAPbI _3 ) using TR-PES in different timescales (ps to μ s and s to min). It was found that CsPbBr _3 shows photovoltage rise and decay on the nanosecond to microsecond time-range, which can be assigned to electron–hole pair separation between surface and bulk. On the other hand, such electron dynamics could not be resolved for Cs-doped FAPbI _3 at these fast timescales. Instead, for Cs-doped FAPbI _3 , the observed photovoltage decay was dominated by much slower dynamics and relaxation to the dark equilibrium state took around 10 min. This suggests that ion migration is responsible for a photovoltage build-up between surface and bulk of the crystal.https://doi.org/10.1088/2515-7655/ada63alead halide perovskitephotoelectron spectroscopytime-resolved photovoltage measurementsion migration
spellingShingle Birgit Kammlander
Alberto García-Fernández
Sebastian Svanström
Erika Giangrisostomi
Ruslan Ovsyannikov
Håkan Rensmo
Ute B Cappel
Investigating charge dynamics at lead halide perovskite single crystal surfaces
JPhys Energy
lead halide perovskite
photoelectron spectroscopy
time-resolved photovoltage measurements
ion migration
title Investigating charge dynamics at lead halide perovskite single crystal surfaces
title_full Investigating charge dynamics at lead halide perovskite single crystal surfaces
title_fullStr Investigating charge dynamics at lead halide perovskite single crystal surfaces
title_full_unstemmed Investigating charge dynamics at lead halide perovskite single crystal surfaces
title_short Investigating charge dynamics at lead halide perovskite single crystal surfaces
title_sort investigating charge dynamics at lead halide perovskite single crystal surfaces
topic lead halide perovskite
photoelectron spectroscopy
time-resolved photovoltage measurements
ion migration
url https://doi.org/10.1088/2515-7655/ada63a
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