The Impact of Ion Migration on the Electro-Optic Effect in Hybrid Organic–Inorganic Perovskites

Meng Jia Sun; Randy Sabatini; Pei Xi Wang; Amin Morteza Najarian; Koen Bertens; Andrew Johnston; Sjoerd Hoogland; Edward H. Sargent

doi:10.1002/adfm.202107939

The Impact of Ion Migration on the Electro-Optic Effect in Hybrid Organic–Inorganic Perovskites

Meng Jia Sun, Randy Sabatini, Pei Xi Wang, Amin Morteza Najarian, Koen Bertens, Andrew Johnston, Sjoerd Hoogland, Edward H. Sargent^*

^*Corresponding author for this work

Chemistry

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

11 Scopus citations

Abstract

Electro-optic (EO) modulation allows the conversion of electrical signals to optical pulses and is widely employed in telecommunications and chip-to-chip interconnects. Recently, hybrid organic–inorganic perovskites (HOIPs) have been explored as candidates for EO modulators. To improve the EO performance, it is envisioned that halide doping will lower the symmetry of the crystal, enhancing spontaneous polarization. However, mixed halide perovskites are often associated with ion migration, which may impact their EO properties. Thus, the influence of ion migration on the EO efficiency is investigated using Br-doped Dion–Jacobson quasi-2D HOIPs, (4AMP)(MA)Pb₂(Br_x/I₁₋_x)₇ (4AMP = 4-(aminomethyl)piperidinium, MA = methylammonium). While density functional theory predicts a greater spontaneous polarization for the Br-doped sample, it is found that experimental results are affected by ion migration. The EO coefficient of the Br/I mixed sample is 95 pm V⁻¹ at 1 kHz (≈50× higher than the undoped sample), but the response falls off rapidly with frequency. This frequency dependence is correlated with impedance spectroscopy, showing that the large EO signal results from ion migration. This study shows that ion migration impacts the EO analysis of mixed halide perovskites and must be considered in future EO studies.

Original language	English (US)
Article number	2107939
Journal	Advanced Functional Materials
Volume	32
Issue number	4
DOIs	https://doi.org/10.1002/adfm.202107939
State	Published - Jan 19 2022

Funding

M.-J.S. and R.S. contributed equally to this work. This work was financially supported by Huawei Technologies Canada Co., Ltd. and the Natural Sciences and Engineering Research Council (NSERC). Computations were performed on the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by: the Canada Foundation for Innovation; the Government of Ontario; Ontario Research Fund-Research Excellence; and the University of Toronto. M.‐J.S. and R.S. contributed equally to this work. This work was financially supported by Huawei Technologies Canada Co., Ltd. and the Natural Sciences and Engineering Research Council (NSERC). Computations were performed on the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by: the Canada Foundation for Innovation; the Government of Ontario; Ontario Research Fund‐Research Excellence; and the University of Toronto.

ASJC Scopus subject areas

General Chemistry
General Materials Science
Condensed Matter Physics

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title = "The Impact of Ion Migration on the Electro-Optic Effect in Hybrid Organic–Inorganic Perovskites",

abstract = "Electro-optic (EO) modulation allows the conversion of electrical signals to optical pulses and is widely employed in telecommunications and chip-to-chip interconnects. Recently, hybrid organic–inorganic perovskites (HOIPs) have been explored as candidates for EO modulators. To improve the EO performance, it is envisioned that halide doping will lower the symmetry of the crystal, enhancing spontaneous polarization. However, mixed halide perovskites are often associated with ion migration, which may impact their EO properties. Thus, the influence of ion migration on the EO efficiency is investigated using Br-doped Dion–Jacobson quasi-2D HOIPs, (4AMP)(MA)Pb2(Brx/I1−x)7 (4AMP = 4-(aminomethyl)piperidinium, MA = methylammonium). While density functional theory predicts a greater spontaneous polarization for the Br-doped sample, it is found that experimental results are affected by ion migration. The EO coefficient of the Br/I mixed sample is 95 pm V−1 at 1 kHz (≈50× higher than the undoped sample), but the response falls off rapidly with frequency. This frequency dependence is correlated with impedance spectroscopy, showing that the large EO signal results from ion migration. This study shows that ion migration impacts the EO analysis of mixed halide perovskites and must be considered in future EO studies.",

author = "Sun, {Meng Jia} and Randy Sabatini and Wang, {Pei Xi} and Najarian, {Amin Morteza} and Koen Bertens and Andrew Johnston and Sjoerd Hoogland and Sargent, {Edward H.}",

note = "Funding Information: M.-J.S. and R.S. contributed equally to this work. This work was financially supported by Huawei Technologies Canada Co., Ltd. and the Natural Sciences and Engineering Research Council (NSERC). Computations were performed on the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by: the Canada Foundation for Innovation; the Government of Ontario; Ontario Research Fund-Research Excellence; and the University of Toronto. Funding Information: M.‐J.S. and R.S. contributed equally to this work. This work was financially supported by Huawei Technologies Canada Co., Ltd. and the Natural Sciences and Engineering Research Council (NSERC). Computations were performed on the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by: the Canada Foundation for Innovation; the Government of Ontario; Ontario Research Fund‐Research Excellence; and the University of Toronto. Publisher Copyright: {\textcopyright} 2021 Wiley-VCH GmbH.",

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AU - Sargent, Edward H.

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N2 - Electro-optic (EO) modulation allows the conversion of electrical signals to optical pulses and is widely employed in telecommunications and chip-to-chip interconnects. Recently, hybrid organic–inorganic perovskites (HOIPs) have been explored as candidates for EO modulators. To improve the EO performance, it is envisioned that halide doping will lower the symmetry of the crystal, enhancing spontaneous polarization. However, mixed halide perovskites are often associated with ion migration, which may impact their EO properties. Thus, the influence of ion migration on the EO efficiency is investigated using Br-doped Dion–Jacobson quasi-2D HOIPs, (4AMP)(MA)Pb2(Brx/I1−x)7 (4AMP = 4-(aminomethyl)piperidinium, MA = methylammonium). While density functional theory predicts a greater spontaneous polarization for the Br-doped sample, it is found that experimental results are affected by ion migration. The EO coefficient of the Br/I mixed sample is 95 pm V−1 at 1 kHz (≈50× higher than the undoped sample), but the response falls off rapidly with frequency. This frequency dependence is correlated with impedance spectroscopy, showing that the large EO signal results from ion migration. This study shows that ion migration impacts the EO analysis of mixed halide perovskites and must be considered in future EO studies.

AB - Electro-optic (EO) modulation allows the conversion of electrical signals to optical pulses and is widely employed in telecommunications and chip-to-chip interconnects. Recently, hybrid organic–inorganic perovskites (HOIPs) have been explored as candidates for EO modulators. To improve the EO performance, it is envisioned that halide doping will lower the symmetry of the crystal, enhancing spontaneous polarization. However, mixed halide perovskites are often associated with ion migration, which may impact their EO properties. Thus, the influence of ion migration on the EO efficiency is investigated using Br-doped Dion–Jacobson quasi-2D HOIPs, (4AMP)(MA)Pb2(Brx/I1−x)7 (4AMP = 4-(aminomethyl)piperidinium, MA = methylammonium). While density functional theory predicts a greater spontaneous polarization for the Br-doped sample, it is found that experimental results are affected by ion migration. The EO coefficient of the Br/I mixed sample is 95 pm V−1 at 1 kHz (≈50× higher than the undoped sample), but the response falls off rapidly with frequency. This frequency dependence is correlated with impedance spectroscopy, showing that the large EO signal results from ion migration. This study shows that ion migration impacts the EO analysis of mixed halide perovskites and must be considered in future EO studies.

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The Impact of Ion Migration on the Electro-Optic Effect in Hybrid Organic–Inorganic Perovskites

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