Reversible Pressure-Dependent Mechanochromism of Dion–Jacobson and Ruddlesden–Popper Layered Hybrid Perovskites

Loreta A. Muscarella; Algirdas Dučinskas; Mathias Dankl; Michał Andrzejewski; Nicola Pietro Maria Casati; Ursula Rothlisberger; Joachim Maier; Michael Graetzel; Bruno Ehrler; Jovana V. Milić

doi:10.1002/adma.202108720

Reversible Pressure-Dependent Mechanochromism of Dion–Jacobson and Ruddlesden–Popper Layered Hybrid Perovskites

Loreta A. Muscarella
, Algirdas Dučinskas
, Mathias Dankl
, Michał Andrzejewski
, Nicola Pietro Maria Casati
, Ursula Rothlisberger
, Joachim Maier
, Michael Graetzel
, Bruno Ehrler^*
, Jovana V. Milić

^*Corresponding author for this work

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

Abstract

Layered Dion–Jacobson (DJ) and Ruddlesden–Popper (RP) hybrid perovskites are promising materials for optoelectronic applications due to their modular structure. To fully exploit their functionality, mechanical stimuli can be used to control their properties without changing the composition. However, the responsiveness of these systems to pressure compatible with practical applications (<1 GPa) remains unexploited. Hydrostatic pressure is used to investigate the structure–property relationships in representative iodide and bromide DJ and RP 2D perovskites based on 1,4-phenylenedimethylammonium (PDMA) and benzylammonium (BzA) spacers in the 0–0.35 GPa pressure range. Pressure-dependent X-ray scattering measurements reveal that lattices of these compositions monotonically shrink and density functional theory calculations provide insights into the structural changes within the organic spacer layer. These structural changes affect the optical properties; the most significant shift in the optical absorption is observed in (BzA)₂PbBr₄ under 0.35 GPa pressure, which is attributed to an isostructural phase transition. Surprisingly, the RP and DJ perovskites behave similarly under pressure, despite the different binding modes of the spacer molecules. This study provides important insights into how the manipulation of the crystal structure affects the optoelectronic properties of such materials, whereas the reversibility of their response expands the perspectives for future applications.

Original language	English
Article number	2108720
Pages (from-to)	1-10
Journal	Advanced Materials
Volume	34
Issue number	17
DOIs	https://doi.org/10.1002/adma.202108720
Publication status	Published - 27 Apr 2022
Externally published	Yes

Bibliographical note

Funding Information:
The work of L.A.M. and B.E. was part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of A.D. was supported by the EPFL-MPI Joint Research Center. B.E. and L.A.M. are grateful for the NWO Vidi grant 016.Vidi.179.005 and J.V.M. is grateful for the Swiss National Foundation PRIMA grant no. 19374 and NCCR Bio-Inspired Materials. U.R. acknowledges Swiss National Science Foundation Grant No. 200020-185092 and the NCCR-MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge Paul Scherrer Institute, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline X04SA of the SLS. The authors thank Juliane Borchert and Ya-Ru Wang (MPI-FKF) for commenting on the manuscript, Davide Moia (MPI-FKF) for his support, and Pascal Schouwink (EPFL) for the assistance in arranging structural measurements. Open access funding provided by Universite de Fribourg.

Funding Information:
The work of L.A.M. and B.E. was part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of A.D. was supported by the EPFL‐MPI Joint Research Center. B.E. and L.A.M. are grateful for the NWO Vidi grant 016.Vidi.179.005 and J.V.M. is grateful for the Swiss National Foundation PRIMA grant no. 19374 and NCCR Bio‐Inspired Materials. U.R. acknowledges Swiss National Science Foundation Grant No. 200020‐185092 and the NCCR‐MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge Paul Scherrer Institute, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline X04SA of the SLS. The authors thank Juliane Borchert and Ya‐Ru Wang (MPI‐FKF) for commenting on the manuscript, Davide Moia (MPI‐FKF) for his support, and Pascal Schouwink (EPFL) for the assistance in arranging structural measurements.

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

Funding

The work of L.A.M. and B.E. was part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of A.D. was supported by the EPFL-MPI Joint Research Center. B.E. and L.A.M. are grateful for the NWO Vidi grant 016.Vidi.179.005 and J.V.M. is grateful for the Swiss National Foundation PRIMA grant no. 19374 and NCCR Bio-Inspired Materials. U.R. acknowledges Swiss National Science Foundation Grant No. 200020-185092 and the NCCR-MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge Paul Scherrer Institute, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline X04SA of the SLS. The authors thank Juliane Borchert and Ya-Ru Wang (MPI-FKF) for commenting on the manuscript, Davide Moia (MPI-FKF) for his support, and Pascal Schouwink (EPFL) for the assistance in arranging structural measurements. Open access funding provided by Universite de Fribourg. The work of L.A.M. and B.E. was part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of A.D. was supported by the EPFL‐MPI Joint Research Center. B.E. and L.A.M. are grateful for the NWO Vidi grant 016.Vidi.179.005 and J.V.M. is grateful for the Swiss National Foundation PRIMA grant no. 19374 and NCCR Bio‐Inspired Materials. U.R. acknowledges Swiss National Science Foundation Grant No. 200020‐185092 and the NCCR‐MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge Paul Scherrer Institute, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline X04SA of the SLS. The authors thank Juliane Borchert and Ya‐Ru Wang (MPI‐FKF) for commenting on the manuscript, Davide Moia (MPI‐FKF) for his support, and Pascal Schouwink (EPFL) for the assistance in arranging structural measurements.

Keywords

layered hybrid perovskites
mechanochromism
pressure-dependent optoelectronics

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Advanced Materials - 2022 - Muscarella - Reversible Pressure‐Dependent Mechanochromism of Dion Jacobson and RuddlesdenFinal published version, 1.91 MBLicence: CC BY-NC

Cite this

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title = "Reversible Pressure-Dependent Mechanochromism of Dion–Jacobson and Ruddlesden–Popper Layered Hybrid Perovskites",

abstract = "Layered Dion–Jacobson (DJ) and Ruddlesden–Popper (RP) hybrid perovskites are promising materials for optoelectronic applications due to their modular structure. To fully exploit their functionality, mechanical stimuli can be used to control their properties without changing the composition. However, the responsiveness of these systems to pressure compatible with practical applications (<1 GPa) remains unexploited. Hydrostatic pressure is used to investigate the structure–property relationships in representative iodide and bromide DJ and RP 2D perovskites based on 1,4-phenylenedimethylammonium (PDMA) and benzylammonium (BzA) spacers in the 0–0.35 GPa pressure range. Pressure-dependent X-ray scattering measurements reveal that lattices of these compositions monotonically shrink and density functional theory calculations provide insights into the structural changes within the organic spacer layer. These structural changes affect the optical properties; the most significant shift in the optical absorption is observed in (BzA)2PbBr4 under 0.35 GPa pressure, which is attributed to an isostructural phase transition. Surprisingly, the RP and DJ perovskites behave similarly under pressure, despite the different binding modes of the spacer molecules. This study provides important insights into how the manipulation of the crystal structure affects the optoelectronic properties of such materials, whereas the reversibility of their response expands the perspectives for future applications.",

keywords = "layered hybrid perovskites, mechanochromism, pressure-dependent optoelectronics",

author = "Muscarella, \{Loreta A.\} and Algirdas Du{\v c}inskas and Mathias Dankl and Micha{\l} Andrzejewski and Casati, \{Nicola Pietro Maria\} and Ursula Rothlisberger and Joachim Maier and Michael Graetzel and Bruno Ehrler and Mili{\'c}, \{Jovana V.\}",

note = "Funding Information: The work of L.A.M. and B.E. was part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of A.D. was supported by the EPFL-MPI Joint Research Center. B.E. and L.A.M. are grateful for the NWO Vidi grant 016.Vidi.179.005 and J.V.M. is grateful for the Swiss National Foundation PRIMA grant no. 19374 and NCCR Bio-Inspired Materials. U.R. acknowledges Swiss National Science Foundation Grant No. 200020-185092 and the NCCR-MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge Paul Scherrer Institute, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline X04SA of the SLS. The authors thank Juliane Borchert and Ya-Ru Wang (MPI-FKF) for commenting on the manuscript, Davide Moia (MPI-FKF) for his support, and Pascal Schouwink (EPFL) for the assistance in arranging structural measurements. Open access funding provided by Universite de Fribourg. Funding Information: The work of L.A.M. and B.E. was part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of A.D. was supported by the EPFL‐MPI Joint Research Center. B.E. and L.A.M. are grateful for the NWO Vidi grant 016.Vidi.179.005 and J.V.M. is grateful for the Swiss National Foundation PRIMA grant no. 19374 and NCCR Bio‐Inspired Materials. U.R. acknowledges Swiss National Science Foundation Grant No. 200020‐185092 and the NCCR‐MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge Paul Scherrer Institute, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline X04SA of the SLS. The authors thank Juliane Borchert and Ya‐Ru Wang (MPI‐FKF) for commenting on the manuscript, Davide Moia (MPI‐FKF) for his support, and Pascal Schouwink (EPFL) for the assistance in arranging structural measurements. Publisher Copyright: {\textcopyright} 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.",

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doi = "10.1002/adma.202108720",

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T1 - Reversible Pressure-Dependent Mechanochromism of Dion–Jacobson and Ruddlesden–Popper Layered Hybrid Perovskites

AU - Muscarella, Loreta A.

AU - Dučinskas, Algirdas

AU - Dankl, Mathias

AU - Andrzejewski, Michał

AU - Casati, Nicola Pietro Maria

AU - Rothlisberger, Ursula

AU - Maier, Joachim

AU - Graetzel, Michael

AU - Ehrler, Bruno

AU - Milić, Jovana V.

N1 - Funding Information: The work of L.A.M. and B.E. was part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of A.D. was supported by the EPFL-MPI Joint Research Center. B.E. and L.A.M. are grateful for the NWO Vidi grant 016.Vidi.179.005 and J.V.M. is grateful for the Swiss National Foundation PRIMA grant no. 19374 and NCCR Bio-Inspired Materials. U.R. acknowledges Swiss National Science Foundation Grant No. 200020-185092 and the NCCR-MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge Paul Scherrer Institute, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline X04SA of the SLS. The authors thank Juliane Borchert and Ya-Ru Wang (MPI-FKF) for commenting on the manuscript, Davide Moia (MPI-FKF) for his support, and Pascal Schouwink (EPFL) for the assistance in arranging structural measurements. Open access funding provided by Universite de Fribourg. Funding Information: The work of L.A.M. and B.E. was part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of A.D. was supported by the EPFL‐MPI Joint Research Center. B.E. and L.A.M. are grateful for the NWO Vidi grant 016.Vidi.179.005 and J.V.M. is grateful for the Swiss National Foundation PRIMA grant no. 19374 and NCCR Bio‐Inspired Materials. U.R. acknowledges Swiss National Science Foundation Grant No. 200020‐185092 and the NCCR‐MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge Paul Scherrer Institute, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline X04SA of the SLS. The authors thank Juliane Borchert and Ya‐Ru Wang (MPI‐FKF) for commenting on the manuscript, Davide Moia (MPI‐FKF) for his support, and Pascal Schouwink (EPFL) for the assistance in arranging structural measurements. Publisher Copyright: © 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.

PY - 2022/4/27

Y1 - 2022/4/27

N2 - Layered Dion–Jacobson (DJ) and Ruddlesden–Popper (RP) hybrid perovskites are promising materials for optoelectronic applications due to their modular structure. To fully exploit their functionality, mechanical stimuli can be used to control their properties without changing the composition. However, the responsiveness of these systems to pressure compatible with practical applications (<1 GPa) remains unexploited. Hydrostatic pressure is used to investigate the structure–property relationships in representative iodide and bromide DJ and RP 2D perovskites based on 1,4-phenylenedimethylammonium (PDMA) and benzylammonium (BzA) spacers in the 0–0.35 GPa pressure range. Pressure-dependent X-ray scattering measurements reveal that lattices of these compositions monotonically shrink and density functional theory calculations provide insights into the structural changes within the organic spacer layer. These structural changes affect the optical properties; the most significant shift in the optical absorption is observed in (BzA)2PbBr4 under 0.35 GPa pressure, which is attributed to an isostructural phase transition. Surprisingly, the RP and DJ perovskites behave similarly under pressure, despite the different binding modes of the spacer molecules. This study provides important insights into how the manipulation of the crystal structure affects the optoelectronic properties of such materials, whereas the reversibility of their response expands the perspectives for future applications.

AB - Layered Dion–Jacobson (DJ) and Ruddlesden–Popper (RP) hybrid perovskites are promising materials for optoelectronic applications due to their modular structure. To fully exploit their functionality, mechanical stimuli can be used to control their properties without changing the composition. However, the responsiveness of these systems to pressure compatible with practical applications (<1 GPa) remains unexploited. Hydrostatic pressure is used to investigate the structure–property relationships in representative iodide and bromide DJ and RP 2D perovskites based on 1,4-phenylenedimethylammonium (PDMA) and benzylammonium (BzA) spacers in the 0–0.35 GPa pressure range. Pressure-dependent X-ray scattering measurements reveal that lattices of these compositions monotonically shrink and density functional theory calculations provide insights into the structural changes within the organic spacer layer. These structural changes affect the optical properties; the most significant shift in the optical absorption is observed in (BzA)2PbBr4 under 0.35 GPa pressure, which is attributed to an isostructural phase transition. Surprisingly, the RP and DJ perovskites behave similarly under pressure, despite the different binding modes of the spacer molecules. This study provides important insights into how the manipulation of the crystal structure affects the optoelectronic properties of such materials, whereas the reversibility of their response expands the perspectives for future applications.

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Reversible Pressure-Dependent Mechanochromism of Dion–Jacobson and Ruddlesden–Popper Layered Hybrid Perovskites

Abstract

Bibliographical note

Funding

Keywords

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