Self-Healing and Light-Soaking in MAPbI3: The Effect of H2O

Davide Raffaele Ceratti; Ron Tenne; Andrea Bartezzaghi; Llorenç Cremonesi; Lior Segev; Vyacheslav Kalchenko; Dan Oron; Marco Alberto Carlo Potenza; Gary Hodes; David Cahen

doi:10.1002/adma.202110239

Self-Healing and Light-Soaking in MAPbI₃: The Effect of H₂O

Davide Raffaele Ceratti^*, Ron Tenne, Andrea Bartezzaghi, Llorenç Cremonesi, Lior Segev, Vyacheslav Kalchenko, Dan Oron, Marco Alberto Carlo Potenza, Gary Hodes^*, David Cahen^*

^*Corresponding author for this work

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

15 Citations (Scopus)

Abstract

The future of halide perovskites (HaPs) is beclouded by limited understanding of their long-term stability. While HaPs can be altered by radiation that induces multiple processes, they can also return to their original state by “self-healing.” Here two-photon (2P) absorption is used to effect light-induced modifications within MAPbI₃ single crystals. Then the changes in the photodamaged region are followed by measuring the photoluminescence, from 2P absorption with 2.5 orders of magnitude lower intensity than that used for photodamaging the MAPbI₃. After photodamage, two brightening and one darkening process are found, all of which recover but on different timescales. The first two are attributed to trap-filling (the fastest) and to proton-amine-related chemistry (the slowest), while photodamage is attributed to the lead-iodide sublattice. Surprisingly, while after 2P-irradiation of crystals that are stored in dry, inert ambient, photobrightening (or “light-soaking”) occurs, mostly photodarkening is seen after photodamage in humid ambient, showing an important connection between the self-healing of a HaP and the presence of H₂O, for long-term steady-state illumination, practically no difference remains between samples kept in dry or humid environments. This result suggests that photobrightening requires a chemical-reservoir that is sensitive to the presence of H₂O, or possibly other proton-related, particularly amine, chemistry.

Original language	English
Article number	2110239
Number of pages	11
Journal	Advanced Materials
Volume	34
Issue number	35
DOIs	https://doi.org/10.1002/adma.202110239
Publication status	Published - 1 Sept 2022

Bibliographical note

Funding Information:
The authors thank Dr. Sigalit Aharon for providing help with the cutting of halide perovskite single crystals for two-photon imaging. The authors also thank Dr. Gennady Uraltsev for the assistance with the calculations. This project has received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No. 893194. D.C. and D.O. thank the Yotam project (via the Sustainability and Energy Research Initiative, SAERI, of the Weizmann Institute), G.H. and D.C. thank the Minerva Centre for Self-Repairing Systems for Energy & Sustainability, and the CNRS-Weizmann program for support.

Funding Information:
The authors thank Dr. Sigalit Aharon for providing help with the cutting of halide perovskite single crystals for two‐photon imaging. The authors also thank Dr. Gennady Uraltsev for the assistance with the calculations. This project has received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska‐Curie grant agreement No. 893194. D.C. and D.O. thank the Yotam project (via the Sustainability and Energy Research Initiative, SAERI, of the Weizmann Institute), G.H. and D.C. thank the Minerva Centre for Self‐Repairing Systems for Energy & Sustainability, and the CNRS‐Weizmann program for support.

Publisher Copyright:
© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.

All Science Journal Classification (ASJC) codes

General Materials Science
Mechanics of Materials
Mechanical Engineering

Access to Document

10.1002/adma.202110239Licence: CC BY-NC

Cite this

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title = "Self-Healing and Light-Soaking in MAPbI3: The Effect of H2O",

abstract = "The future of halide perovskites (HaPs) is beclouded by limited understanding of their long-term stability. While HaPs can be altered by radiation that induces multiple processes, they can also return to their original state by “self-healing.” Here two-photon (2P) absorption is used to effect light-induced modifications within MAPbI3 single crystals. Then the changes in the photodamaged region are followed by measuring the photoluminescence, from 2P absorption with 2.5 orders of magnitude lower intensity than that used for photodamaging the MAPbI3. After photodamage, two brightening and one darkening process are found, all of which recover but on different timescales. The first two are attributed to trap-filling (the fastest) and to proton-amine-related chemistry (the slowest), while photodamage is attributed to the lead-iodide sublattice. Surprisingly, while after 2P-irradiation of crystals that are stored in dry, inert ambient, photobrightening (or “light-soaking”) occurs, mostly photodarkening is seen after photodamage in humid ambient, showing an important connection between the self-healing of a HaP and the presence of H2O, for long-term steady-state illumination, practically no difference remains between samples kept in dry or humid environments. This result suggests that photobrightening requires a chemical-reservoir that is sensitive to the presence of H2O, or possibly other proton-related, particularly amine, chemistry.",

author = "Ceratti, {Davide Raffaele} and Ron Tenne and Andrea Bartezzaghi and Lloren{\c c} Cremonesi and Lior Segev and Vyacheslav Kalchenko and Dan Oron and Potenza, {Marco Alberto Carlo} and Gary Hodes and David Cahen",

note = "Funding Information: The authors thank Dr. Sigalit Aharon for providing help with the cutting of halide perovskite single crystals for two-photon imaging. The authors also thank Dr. Gennady Uraltsev for the assistance with the calculations. This project has received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No. 893194. D.C. and D.O. thank the Yotam project (via the Sustainability and Energy Research Initiative, SAERI, of the Weizmann Institute), G.H. and D.C. thank the Minerva Centre for Self-Repairing Systems for Energy & Sustainability, and the CNRS-Weizmann program for support. Funding Information: The authors thank Dr. Sigalit Aharon for providing help with the cutting of halide perovskite single crystals for two‐photon imaging. The authors also thank Dr. Gennady Uraltsev for the assistance with the calculations. This project has received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska‐Curie grant agreement No. 893194. D.C. and D.O. thank the Yotam project (via the Sustainability and Energy Research Initiative, SAERI, of the Weizmann Institute), G.H. and D.C. thank the Minerva Centre for Self‐Repairing Systems for Energy & Sustainability, and the CNRS‐Weizmann program for support. Publisher Copyright: {\textcopyright} 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.",

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AU - Ceratti, Davide Raffaele

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AU - Cremonesi, Llorenç

AU - Segev, Lior

AU - Kalchenko, Vyacheslav

AU - Oron, Dan

AU - Potenza, Marco Alberto Carlo

AU - Hodes, Gary

AU - Cahen, David

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N2 - The future of halide perovskites (HaPs) is beclouded by limited understanding of their long-term stability. While HaPs can be altered by radiation that induces multiple processes, they can also return to their original state by “self-healing.” Here two-photon (2P) absorption is used to effect light-induced modifications within MAPbI3 single crystals. Then the changes in the photodamaged region are followed by measuring the photoluminescence, from 2P absorption with 2.5 orders of magnitude lower intensity than that used for photodamaging the MAPbI3. After photodamage, two brightening and one darkening process are found, all of which recover but on different timescales. The first two are attributed to trap-filling (the fastest) and to proton-amine-related chemistry (the slowest), while photodamage is attributed to the lead-iodide sublattice. Surprisingly, while after 2P-irradiation of crystals that are stored in dry, inert ambient, photobrightening (or “light-soaking”) occurs, mostly photodarkening is seen after photodamage in humid ambient, showing an important connection between the self-healing of a HaP and the presence of H2O, for long-term steady-state illumination, practically no difference remains between samples kept in dry or humid environments. This result suggests that photobrightening requires a chemical-reservoir that is sensitive to the presence of H2O, or possibly other proton-related, particularly amine, chemistry.

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