Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells

Mixed-dimensional perovskites containing mixtures of organic cations hold great promise to deliver highly stable and efficient solar cells. However, although a plethora of relatively bulky organic cations have been reported for such purposes, a fundamental understanding of the materials’ structure,...

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Main Authors: Febriansyah, Benny, Li, Yongxin, Giovanni, David, Salim, Teddy, Hooper, Thomas J. N., Sim, Ying, Ma, Daphne, Laxmi, Shoba, Lekina, Yulia, Koh, Teck Ming, Shen, Ze Xiang, Pullarkat, Sumod A., Sum, Tze Chien, Mhaisalkar, Subodh Gautam, Ager, Joel W., Mathews, Nripan
Other Authors: School of Materials Science and Engineering
Format: Journal Article
Language:English
Published: 2023
Subjects:
Online Access:https://hdl.handle.net/10356/164910
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author Febriansyah, Benny
Li, Yongxin
Giovanni, David
Salim, Teddy
Hooper, Thomas J. N.
Sim, Ying
Ma, Daphne
Laxmi, Shoba
Lekina, Yulia
Koh, Teck Ming
Shen, Ze Xiang
Pullarkat, Sumod A.
Sum, Tze Chien
Mhaisalkar, Subodh Gautam
Ager, Joel W.
Mathews, Nripan
author2 School of Materials Science and Engineering
author_facet School of Materials Science and Engineering
Febriansyah, Benny
Li, Yongxin
Giovanni, David
Salim, Teddy
Hooper, Thomas J. N.
Sim, Ying
Ma, Daphne
Laxmi, Shoba
Lekina, Yulia
Koh, Teck Ming
Shen, Ze Xiang
Pullarkat, Sumod A.
Sum, Tze Chien
Mhaisalkar, Subodh Gautam
Ager, Joel W.
Mathews, Nripan
author_sort Febriansyah, Benny
collection NTU
description Mixed-dimensional perovskites containing mixtures of organic cations hold great promise to deliver highly stable and efficient solar cells. However, although a plethora of relatively bulky organic cations have been reported for such purposes, a fundamental understanding of the materials’ structure, composition, and phase, along with their correlated effects on the corresponding optoelectronic properties and degradation mechanism remains elusive. Herein, we systematically engineer the structures of bulky organic cations to template low-dimensional perovskites with contrasting inorganic framework dimensionality, connectivity, and coordination deformation. By combining X-ray single-crystal structural analysis with depth-profiling XPS, solid-state NMR, and femtosecond transient absorption, it is revealed that not all low dimensional species work equally well as dopants. Instead, it was found that inorganic architectures with lesser structural distortion tend to yield less disordered energetic and defect landscapes in the resulting mixed-dimensional perovskites, augmented in materials with a longer photoluminescence (PL) lifetime, higher PL quantum yield (up to 11%), improved solar cell performance and enhanced thermal stability (T80 up to 1000 h, unencapsulated). Our study highlights the importance of designing templating organic cations that yield low-dimensional materials with much less structural distortion profiles to be used as additives in stable and efficient perovskite solar cells.
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spelling ntu-10356/1649102023-02-28T20:12:16Z Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells Febriansyah, Benny Li, Yongxin Giovanni, David Salim, Teddy Hooper, Thomas J. N. Sim, Ying Ma, Daphne Laxmi, Shoba Lekina, Yulia Koh, Teck Ming Shen, Ze Xiang Pullarkat, Sumod A. Sum, Tze Chien Mhaisalkar, Subodh Gautam Ager, Joel W. Mathews, Nripan School of Materials Science and Engineering School of Physical and Mathematical Sciences Centre of High Field Nuclear Magnetic Resonance (NMR) Spectroscopy and Imaging, NTU Energy Research Institute @ NTU (ERI@N) Engineering::Materials::Nanostructured materials Engineering::Materials::Functional materials Degradation Mechanism Materials Structure Mixed-dimensional perovskites containing mixtures of organic cations hold great promise to deliver highly stable and efficient solar cells. However, although a plethora of relatively bulky organic cations have been reported for such purposes, a fundamental understanding of the materials’ structure, composition, and phase, along with their correlated effects on the corresponding optoelectronic properties and degradation mechanism remains elusive. Herein, we systematically engineer the structures of bulky organic cations to template low-dimensional perovskites with contrasting inorganic framework dimensionality, connectivity, and coordination deformation. By combining X-ray single-crystal structural analysis with depth-profiling XPS, solid-state NMR, and femtosecond transient absorption, it is revealed that not all low dimensional species work equally well as dopants. Instead, it was found that inorganic architectures with lesser structural distortion tend to yield less disordered energetic and defect landscapes in the resulting mixed-dimensional perovskites, augmented in materials with a longer photoluminescence (PL) lifetime, higher PL quantum yield (up to 11%), improved solar cell performance and enhanced thermal stability (T80 up to 1000 h, unencapsulated). Our study highlights the importance of designing templating organic cations that yield low-dimensional materials with much less structural distortion profiles to be used as additives in stable and efficient perovskite solar cells. Ministry of Education (MOE) National Research Foundation (NRF) Published version The authors would like to acknowledge funding from the Singapore National Research Foundation through the IntraCREATE Collaborative Grant (NRF2018-ITC001-001), Energy Innovation Research Program (NRF2015EWT-EIRP003-004 and Solar CRP: S18-1176-SCRP), and MOE Tier 2 project MOE2019-T2-2-097. 2023-02-27T02:28:25Z 2023-02-27T02:28:25Z 2023 Journal Article Febriansyah, B., Li, Y., Giovanni, D., Salim, T., Hooper, T. J. N., Sim, Y., Ma, D., Laxmi, S., Lekina, Y., Koh, T. M., Shen, Z. X., Pullarkat, S. A., Sum, T. C., Mhaisalkar, S. G., Ager, J. W. & Mathews, N. (2023). Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells. Materials Horizons, 10(2), 536-546. https://dx.doi.org/10.1039/D2MH00868H 2051-6347 https://hdl.handle.net/10356/164910 10.1039/D2MH00868H 2 10 536 546 en NRF2018-ITC001-001 NRF2015EWT-EIRP003-004 S18-1176-SCRP MOE2019-T2-2-097 Materials Horizons © 2023 The Royal Society of Chemistry. This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. application/pdf
spellingShingle Engineering::Materials::Nanostructured materials
Engineering::Materials::Functional materials
Degradation Mechanism
Materials Structure
Febriansyah, Benny
Li, Yongxin
Giovanni, David
Salim, Teddy
Hooper, Thomas J. N.
Sim, Ying
Ma, Daphne
Laxmi, Shoba
Lekina, Yulia
Koh, Teck Ming
Shen, Ze Xiang
Pullarkat, Sumod A.
Sum, Tze Chien
Mhaisalkar, Subodh Gautam
Ager, Joel W.
Mathews, Nripan
Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells
title Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells
title_full Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells
title_fullStr Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells
title_full_unstemmed Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells
title_short Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells
title_sort inorganic frameworks of low dimensional perovskites dictate the performance and stability of mixed dimensional perovskite solar cells
topic Engineering::Materials::Nanostructured materials
Engineering::Materials::Functional materials
Degradation Mechanism
Materials Structure
url https://hdl.handle.net/10356/164910
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