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Autores principales: Adhikari, Surajit, Johari, Priya
Formato: Preprint
Publicado: 2025
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Acceso en línea:https://arxiv.org/abs/2502.14622
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author Adhikari, Surajit
Johari, Priya
author_facet Adhikari, Surajit
Johari, Priya
contents Lead-free chalcogenide perovskites are emerging as game-changers in the race for sustainable, high-performance photovoltaics. These materials offer a perfect trifecta: non-toxic elemental composition, exceptional phase stability, and outstanding optoelectronic properties. However, unlocking their full potential for solar cell applications requires advanced strategies to fine-tune their electronic and optical behavior. In this study, we take CaHfS$_{3}$-a promising but underexplored candidate-and revolutionize its performance by introducing targeted substitutions: Ti at the cation site and Se at the anion site. Using cutting-edge computational techniques, including density functional theory, GW calculations, and the Bethe-Salpeter equation (BSE), we reveal how these substitutions transform the material's properties. Our findings highlight that alloyed compounds such as CaHfS$_{3-x}$Se$_{x}$ and CaHf$_{1-y}$Ti$_{y}$X$_{3}$ (X = S, Se) are not only phase-stable but also feature adjustable direct G$_{0}$W$_{0}$@PBE bandgaps (1.29-2.67 eV), reduced exciton binding energies, and significantly improved polaron mobility. These modifications enable better light absorption, reduced electron-hole recombination, longer exciton lifetimes, and enhanced quantum yield. Impressively, the alloyed perovskites, specifically, for the Ti-rich Se-based perovskites, achieve a spectroscopic-limited maximum efficiency of up to 28.06%, outperforming traditional lead-based halide perovskites. Our results demonstrate that strategic alloying is a powerful tool to supercharge the optoelectronic properties of lead-free chalcogenide perovskites, positioning them as strong contenders for next-generation photovoltaic technologies.
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spellingShingle Optimizing Lead-Free Chalcogenide Perovskites for High-Efficiency Photovoltaics via Alloying Strategies
Adhikari, Surajit
Johari, Priya
Materials Science
Lead-free chalcogenide perovskites are emerging as game-changers in the race for sustainable, high-performance photovoltaics. These materials offer a perfect trifecta: non-toxic elemental composition, exceptional phase stability, and outstanding optoelectronic properties. However, unlocking their full potential for solar cell applications requires advanced strategies to fine-tune their electronic and optical behavior. In this study, we take CaHfS$_{3}$-a promising but underexplored candidate-and revolutionize its performance by introducing targeted substitutions: Ti at the cation site and Se at the anion site. Using cutting-edge computational techniques, including density functional theory, GW calculations, and the Bethe-Salpeter equation (BSE), we reveal how these substitutions transform the material's properties. Our findings highlight that alloyed compounds such as CaHfS$_{3-x}$Se$_{x}$ and CaHf$_{1-y}$Ti$_{y}$X$_{3}$ (X = S, Se) are not only phase-stable but also feature adjustable direct G$_{0}$W$_{0}$@PBE bandgaps (1.29-2.67 eV), reduced exciton binding energies, and significantly improved polaron mobility. These modifications enable better light absorption, reduced electron-hole recombination, longer exciton lifetimes, and enhanced quantum yield. Impressively, the alloyed perovskites, specifically, for the Ti-rich Se-based perovskites, achieve a spectroscopic-limited maximum efficiency of up to 28.06%, outperforming traditional lead-based halide perovskites. Our results demonstrate that strategic alloying is a powerful tool to supercharge the optoelectronic properties of lead-free chalcogenide perovskites, positioning them as strong contenders for next-generation photovoltaic technologies.
title Optimizing Lead-Free Chalcogenide Perovskites for High-Efficiency Photovoltaics via Alloying Strategies
topic Materials Science
url https://arxiv.org/abs/2502.14622