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Title: Structure, Morphology, and Photovoltaic Implications of Halide Alloying in Lead-Free Cs 3Sb 2Cl xI 9-x 2D-Layered Perovskites

Abstract

Compositional tuning has been a major driving force behind the excellent optoelectronic properties observed in typical Pb-based perovskites. For lead-free perovskite derivatives, a challenge to understanding the connection between compositional tuning and intrinsic optoelectronic properties, hence a barrier towards boosting their performance, comes from the fact that multiple crystalline substructures can form based on composition, film processing, or both. Especially with lower dimensional (0D, 1D, 2D) substructures, the particular polymorph present in the film can be a greater determinant of optoelectronic properties than the composition itself. Herein, we report a simple method to alloy the halide site in all-inorganic lead-free Cs 3Sb 2I 9 films while maintaining a consistent 2D-layered substructure, as a means to independently study the photovoltaic implications of halide substitution. We use a broad suite of spectroscopy and device measurements to identify an optimal stoichiometric substitution of chloride for iodide (~ 8 mol%, measured) that balances both intrinsic and bulk optoelectronic properties to achieve a top power conversion efficiency of 2.2%. This work underscores the importance of controlling substructure while investigating the impacts of compositional tuning for the development of lead-free perovskites, and more broadly validates the approach towards realizing lead-free alternative perovskite solar technologies.

Authors:
 [1];  [1]; ORCiD logo [2]
  1. Indian Association for the Cultivation of Science, Jadavpur, Kolkata (India)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States). National Center for Photovoltaics (NCPV); Energy Frontier Research Centers (EFRC) (United States). Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; Council of Scientific & Industrial Research (CSIR); Bhsakara Advanced Solar Energy Fellowship; JC Bose National Fellowship
OSTI Identifier:
1677431
Report Number(s):
NREL/JA-5900-77107
Journal ID: ISSN 2367-198X; MainId:26053;UUID:1974ffef-09ef-4645-a9c6-4bbdf9322f85;MainAdminID:18589
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Solar RRL
Additional Journal Information:
Journal Name: Solar RRL; Journal ID: ISSN 2367-198X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; lead-free; layered perovskite; photovoltaic; optoelectronic properties; halide alloying

Citation Formats

Paul, Goutam, Pal, Amlan J., and Larson, Bryon W. Structure, Morphology, and Photovoltaic Implications of Halide Alloying in Lead-Free Cs3Sb2ClxI9-x 2D-Layered Perovskites. United States: N. p., 2020. Web. doi:10.1002/solr.202000422.
Paul, Goutam, Pal, Amlan J., & Larson, Bryon W. Structure, Morphology, and Photovoltaic Implications of Halide Alloying in Lead-Free Cs3Sb2ClxI9-x 2D-Layered Perovskites. United States. doi:10.1002/solr.202000422.
Paul, Goutam, Pal, Amlan J., and Larson, Bryon W. Wed . "Structure, Morphology, and Photovoltaic Implications of Halide Alloying in Lead-Free Cs3Sb2ClxI9-x 2D-Layered Perovskites". United States. doi:10.1002/solr.202000422.
@article{osti_1677431,
title = {Structure, Morphology, and Photovoltaic Implications of Halide Alloying in Lead-Free Cs3Sb2ClxI9-x 2D-Layered Perovskites},
author = {Paul, Goutam and Pal, Amlan J. and Larson, Bryon W.},
abstractNote = {Compositional tuning has been a major driving force behind the excellent optoelectronic properties observed in typical Pb-based perovskites. For lead-free perovskite derivatives, a challenge to understanding the connection between compositional tuning and intrinsic optoelectronic properties, hence a barrier towards boosting their performance, comes from the fact that multiple crystalline substructures can form based on composition, film processing, or both. Especially with lower dimensional (0D, 1D, 2D) substructures, the particular polymorph present in the film can be a greater determinant of optoelectronic properties than the composition itself. Herein, we report a simple method to alloy the halide site in all-inorganic lead-free Cs3Sb2I9 films while maintaining a consistent 2D-layered substructure, as a means to independently study the photovoltaic implications of halide substitution. We use a broad suite of spectroscopy and device measurements to identify an optimal stoichiometric substitution of chloride for iodide (~ 8 mol%, measured) that balances both intrinsic and bulk optoelectronic properties to achieve a top power conversion efficiency of 2.2%. This work underscores the importance of controlling substructure while investigating the impacts of compositional tuning for the development of lead-free perovskites, and more broadly validates the approach towards realizing lead-free alternative perovskite solar technologies.},
doi = {10.1002/solr.202000422},
journal = {Solar RRL},
issn = {2367-198X},
number = ,
volume = ,
place = {United States},
year = {2020},
month = {9}
}

Journal Article:
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