Crystallographic Insights into the Structural Heterogeneities of 2D Ruddlesden‐Popper Perovskite Films

Abstract 2D Ruddlesden‐Popper phase perovskites (RPPs) offer significant potential for next‐generation photovoltaics owing to their excellent intrinsic stability. Fully understanding the crystalline configuration of 2D perovskite films is essential for further enhancing the power‐conversion‐efficien...

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Main Authors: Fei Zheng, Sergey Rubanov, Christopher Hall, Jingying Liu, Mei Gao, Trevor A. Smith, Dechan Angmo, Kenneth P. Ghiggino
Format: Article
Language:English
Published: Wiley-VCH 2025-07-01
Series:Advanced Materials Interfaces
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Online Access:https://doi.org/10.1002/admi.202401012
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author Fei Zheng
Sergey Rubanov
Christopher Hall
Jingying Liu
Mei Gao
Trevor A. Smith
Dechan Angmo
Kenneth P. Ghiggino
author_facet Fei Zheng
Sergey Rubanov
Christopher Hall
Jingying Liu
Mei Gao
Trevor A. Smith
Dechan Angmo
Kenneth P. Ghiggino
author_sort Fei Zheng
collection DOAJ
description Abstract 2D Ruddlesden‐Popper phase perovskites (RPPs) offer significant potential for next‐generation photovoltaics owing to their excellent intrinsic stability. Fully understanding the crystalline configuration of 2D perovskite films is essential for further enhancing the power‐conversion‐efficiency (PCE) of 2D perovskite solar cells (2D‐PSCs). Herein, the structural heterogeneities, including the profiles of crystal orientation and defect distribution, at both the microscopic and mesoscopic scales for 2D perovskite films are investigated. Empty voids are observed in the buried interface of 2D perovskite films associated with Brownian tree‐shaped dendritic structures, and the crystal orientations of 2D RPPs in the upper and lower parts of these areas are mismatched. This configuration hinders charge carrier transport along the vertical direction and is likely responsible for the lower PCE of 2D‐PSCs compared to their 3D counterparts. The formation mechanism of these voids and the crystalline mismatching are revealed based on compositional and structural analysis. The results suggest that synchronizing the rate of crystallization in different film areas may eliminate these voids and thereby reduce the PCE gap between 2D‐ and 3D‐PSCs. This work provides a comprehensive understanding of the crystallographic heterogeneities of 2D perovskite films, highlighting new pathways to design more efficient 2D‐PSCs based on 2D RPP films.
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spelling doaj-art-7077b6d9569f4d5e934cd8e425b7156e2025-08-20T02:40:59ZengWiley-VCHAdvanced Materials Interfaces2196-73502025-07-011213n/an/a10.1002/admi.202401012Crystallographic Insights into the Structural Heterogeneities of 2D Ruddlesden‐Popper Perovskite FilmsFei Zheng0Sergey Rubanov1Christopher Hall2Jingying Liu3Mei Gao4Trevor A. Smith5Dechan Angmo6Kenneth P. Ghiggino7School of Chemistry and ARC Centre of Excellence in Exciton Science The University of Melbourne Parkville VIC 3010 AustraliaIan Holmes Imaging Centre, Bio21 Institute The University of Melbourne Parkville VIC 3010 AustraliaSchool of Chemistry and ARC Centre of Excellence in Exciton Science The University of Melbourne Parkville VIC 3010 AustraliaDepartment of Materials Science and Engineering Monash University Clayton VIC 3800 AustraliaDevices and Engineered Systems CSIRO Manufacturing Clayton VIC 3168 AustraliaSchool of Chemistry and ARC Centre of Excellence in Exciton Science The University of Melbourne Parkville VIC 3010 AustraliaDevices and Engineered Systems CSIRO Manufacturing Clayton VIC 3168 AustraliaSchool of Chemistry and ARC Centre of Excellence in Exciton Science The University of Melbourne Parkville VIC 3010 AustraliaAbstract 2D Ruddlesden‐Popper phase perovskites (RPPs) offer significant potential for next‐generation photovoltaics owing to their excellent intrinsic stability. Fully understanding the crystalline configuration of 2D perovskite films is essential for further enhancing the power‐conversion‐efficiency (PCE) of 2D perovskite solar cells (2D‐PSCs). Herein, the structural heterogeneities, including the profiles of crystal orientation and defect distribution, at both the microscopic and mesoscopic scales for 2D perovskite films are investigated. Empty voids are observed in the buried interface of 2D perovskite films associated with Brownian tree‐shaped dendritic structures, and the crystal orientations of 2D RPPs in the upper and lower parts of these areas are mismatched. This configuration hinders charge carrier transport along the vertical direction and is likely responsible for the lower PCE of 2D‐PSCs compared to their 3D counterparts. The formation mechanism of these voids and the crystalline mismatching are revealed based on compositional and structural analysis. The results suggest that synchronizing the rate of crystallization in different film areas may eliminate these voids and thereby reduce the PCE gap between 2D‐ and 3D‐PSCs. This work provides a comprehensive understanding of the crystallographic heterogeneities of 2D perovskite films, highlighting new pathways to design more efficient 2D‐PSCs based on 2D RPP films.https://doi.org/10.1002/admi.202401012brownian treeburied interfaceruddlesden‐popper phase perovskitesvoids
spellingShingle Fei Zheng
Sergey Rubanov
Christopher Hall
Jingying Liu
Mei Gao
Trevor A. Smith
Dechan Angmo
Kenneth P. Ghiggino
Crystallographic Insights into the Structural Heterogeneities of 2D Ruddlesden‐Popper Perovskite Films
Advanced Materials Interfaces
brownian tree
buried interface
ruddlesden‐popper phase perovskites
voids
title Crystallographic Insights into the Structural Heterogeneities of 2D Ruddlesden‐Popper Perovskite Films
title_full Crystallographic Insights into the Structural Heterogeneities of 2D Ruddlesden‐Popper Perovskite Films
title_fullStr Crystallographic Insights into the Structural Heterogeneities of 2D Ruddlesden‐Popper Perovskite Films
title_full_unstemmed Crystallographic Insights into the Structural Heterogeneities of 2D Ruddlesden‐Popper Perovskite Films
title_short Crystallographic Insights into the Structural Heterogeneities of 2D Ruddlesden‐Popper Perovskite Films
title_sort crystallographic insights into the structural heterogeneities of 2d ruddlesden popper perovskite films
topic brownian tree
buried interface
ruddlesden‐popper phase perovskites
voids
url https://doi.org/10.1002/admi.202401012
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