Advancing intercalation strategies in layered hybrid perovskites by bringing together synthesis and simulations

Abstract Finding ways to modify the electronic structure of halide perovskites is desireable as they have applications in a variety of devices, from photovoltaics to LEDs. Additionally, designing functional materials can be facilitated through the use of computation. Here, we have used a combination...

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Main Authors: Lin-Jie Yang, Wenye Xuan, Sara Henda, Shaoyang Wang, Sai Kiran Rajendran, David B. Cordes, David N. Miller, Alexandra M. Z. Slawin, Lethy Krishnan Jagadamma, Hamid Ohadi, Hsin-Yi Tiffany Chen, Matthew S. Dyer, Julia L. Payne
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-60880-5
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author Lin-Jie Yang
Wenye Xuan
Sara Henda
Shaoyang Wang
Sai Kiran Rajendran
David B. Cordes
David N. Miller
Alexandra M. Z. Slawin
Lethy Krishnan Jagadamma
Hamid Ohadi
Hsin-Yi Tiffany Chen
Matthew S. Dyer
Julia L. Payne
author_facet Lin-Jie Yang
Wenye Xuan
Sara Henda
Shaoyang Wang
Sai Kiran Rajendran
David B. Cordes
David N. Miller
Alexandra M. Z. Slawin
Lethy Krishnan Jagadamma
Hamid Ohadi
Hsin-Yi Tiffany Chen
Matthew S. Dyer
Julia L. Payne
author_sort Lin-Jie Yang
collection DOAJ
description Abstract Finding ways to modify the electronic structure of halide perovskites is desireable as they have applications in a variety of devices, from photovoltaics to LEDs. Additionally, designing functional materials can be facilitated through the use of computation. Here, we have used a combination of synthesis and computation to screen for intercalated, layered hybrid perovskites. 54 compositions were screened and five compounds containing intercalated halogens were prepared as single crystals. A further compound, which was not screened and contained IBr, was prepared. We computationally identified an intercalated layered hybrid perovskite with a low bandgap and prepared it as a thin-film. Through examination of single crystal X-ray diffraction data, we provide some design guidelines for intercalation. The conformational flexibility in the organic ammonium cation allows rotations in the carbon backbone which change upon intercalation. Optoelectronic properties were studied using photoluminescence spectroscopy and preliminary photovoltaic device testing.
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spelling doaj-art-07c0cc6f75ec4f7996029de304ce25642025-08-20T03:37:38ZengNature PortfolioNature Communications2041-17232025-07-0116111410.1038/s41467-025-60880-5Advancing intercalation strategies in layered hybrid perovskites by bringing together synthesis and simulationsLin-Jie Yang0Wenye Xuan1Sara Henda2Shaoyang Wang3Sai Kiran Rajendran4David B. Cordes5David N. Miller6Alexandra M. Z. Slawin7Lethy Krishnan Jagadamma8Hamid Ohadi9Hsin-Yi Tiffany Chen10Matthew S. Dyer11Julia L. Payne12School of Chemistry, University of St Andrews, North HaughDepartment of Chemistry, University of Liverpool, Crown St, Liverpool, L69 7ZD and Materials Innovation Factory, University of LiverpoolSUPA, School of Physics and Astronomy, University of St Andrews, North Haugh, St AndrewsSUPA, School of Physics and Astronomy, University of St Andrews, North Haugh, St AndrewsSUPA, School of Physics and Astronomy, University of St Andrews, North Haugh, St AndrewsSchool of Chemistry, University of St Andrews, North HaughSchool of Chemistry, University of St Andrews, North HaughSchool of Chemistry, University of St Andrews, North HaughSUPA, School of Physics and Astronomy, University of St Andrews, North Haugh, St AndrewsSUPA, School of Physics and Astronomy, University of St Andrews, North Haugh, St AndrewsDepartment of Engineering and System Science, National Tsing Hua UniversityDepartment of Chemistry, University of Liverpool, Crown St, Liverpool, L69 7ZD and Materials Innovation Factory, University of LiverpoolSchool of Chemistry, University of St Andrews, North HaughAbstract Finding ways to modify the electronic structure of halide perovskites is desireable as they have applications in a variety of devices, from photovoltaics to LEDs. Additionally, designing functional materials can be facilitated through the use of computation. Here, we have used a combination of synthesis and computation to screen for intercalated, layered hybrid perovskites. 54 compositions were screened and five compounds containing intercalated halogens were prepared as single crystals. A further compound, which was not screened and contained IBr, was prepared. We computationally identified an intercalated layered hybrid perovskite with a low bandgap and prepared it as a thin-film. Through examination of single crystal X-ray diffraction data, we provide some design guidelines for intercalation. The conformational flexibility in the organic ammonium cation allows rotations in the carbon backbone which change upon intercalation. Optoelectronic properties were studied using photoluminescence spectroscopy and preliminary photovoltaic device testing.https://doi.org/10.1038/s41467-025-60880-5
spellingShingle Lin-Jie Yang
Wenye Xuan
Sara Henda
Shaoyang Wang
Sai Kiran Rajendran
David B. Cordes
David N. Miller
Alexandra M. Z. Slawin
Lethy Krishnan Jagadamma
Hamid Ohadi
Hsin-Yi Tiffany Chen
Matthew S. Dyer
Julia L. Payne
Advancing intercalation strategies in layered hybrid perovskites by bringing together synthesis and simulations
Nature Communications
title Advancing intercalation strategies in layered hybrid perovskites by bringing together synthesis and simulations
title_full Advancing intercalation strategies in layered hybrid perovskites by bringing together synthesis and simulations
title_fullStr Advancing intercalation strategies in layered hybrid perovskites by bringing together synthesis and simulations
title_full_unstemmed Advancing intercalation strategies in layered hybrid perovskites by bringing together synthesis and simulations
title_short Advancing intercalation strategies in layered hybrid perovskites by bringing together synthesis and simulations
title_sort advancing intercalation strategies in layered hybrid perovskites by bringing together synthesis and simulations
url https://doi.org/10.1038/s41467-025-60880-5
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