TY - JOUR
T1 - Lead-Free Cs2AgBiCl6 Double Perovskite
T2 - Experimental and Theoretical Insights into the Self-Trapping for Optoelectronic Applications
AU - Rahane, Swati N.
AU - Rahane, Ganesh K.
AU - Mandal, Animesh
AU - Jadhav, Yogesh
AU - Godha, Akshat
AU - Rokade, Avinash
AU - Shah, Shruti
AU - Hase, Yogesh
AU - Waghmare, Ashish
AU - Saykar, Nilesh G.
AU - Roy, Anurag
AU - Salgaonkar, Kranti N.
AU - Dubal, Deepak
AU - Makineni, Surendra K.
AU - Dzade, Nelson Y.
AU - Jadkar, Sandesh R.
AU - Rondiya, Sachin R.
N1 - Publisher Copyright:
© 2024 The Authors. Published by American Chemical Society.
PY - 2024/9/25
Y1 - 2024/9/25
N2 - Lead-free double perovskites (DPs) will emerge as viable and environmentally safe substitutes for Pb-halide perovskites, demonstrating stability and nontoxicity if their optoelectronic property is greatly improved. Doping has been experimentally validated as a powerful tool for enhancing optoelectronic properties and concurrently reducing the defect state density in DP materials. Fundamental understanding of the optical properties of DPs, particularly the self-trapped exciton (STEs) dynamics, plays a critical role in a range of optoelectronic applications. Our study investigates how Fe doping influences the structural and optical properties of Cs2AgBiCl6 DPs by understanding their STEs dynamics, which is currently lacking in the literature. A combined experimental-computational approach is employed to investigate the optoelectronic properties of pure and doped Cs2AgBiCl6 (Fe-Cs2AgBiCl6) perovskites. Successful incorporation of Fe3+ ions is confirmed by X-ray diffraction and Raman spectroscopy. Moreover, the Fe-Cs2AgBiCl6 DPs exhibit strong absorption from below 400 nm up to 700 nm, indicating sub-band gap state transitions originating from surface defects. Photoluminescence (PL) analysis demonstrates a significant enhancement in the PL intensity, attributed to an increased radiative recombination rate and higher STE density. The radiative kinetics and average lifetime are investigated by the time-resolved PL (TRPL) method; in addition, temperature-dependent PL measurements provide valuable insights into activation energy and exciton-phonon coupling strength. Our findings will not only deepen our understanding of charge carrier dynamics associated with STEs but also pave the way for the design of some promising perovskite materials for use in optoelectronics and photocatalysis.
AB - Lead-free double perovskites (DPs) will emerge as viable and environmentally safe substitutes for Pb-halide perovskites, demonstrating stability and nontoxicity if their optoelectronic property is greatly improved. Doping has been experimentally validated as a powerful tool for enhancing optoelectronic properties and concurrently reducing the defect state density in DP materials. Fundamental understanding of the optical properties of DPs, particularly the self-trapped exciton (STEs) dynamics, plays a critical role in a range of optoelectronic applications. Our study investigates how Fe doping influences the structural and optical properties of Cs2AgBiCl6 DPs by understanding their STEs dynamics, which is currently lacking in the literature. A combined experimental-computational approach is employed to investigate the optoelectronic properties of pure and doped Cs2AgBiCl6 (Fe-Cs2AgBiCl6) perovskites. Successful incorporation of Fe3+ ions is confirmed by X-ray diffraction and Raman spectroscopy. Moreover, the Fe-Cs2AgBiCl6 DPs exhibit strong absorption from below 400 nm up to 700 nm, indicating sub-band gap state transitions originating from surface defects. Photoluminescence (PL) analysis demonstrates a significant enhancement in the PL intensity, attributed to an increased radiative recombination rate and higher STE density. The radiative kinetics and average lifetime are investigated by the time-resolved PL (TRPL) method; in addition, temperature-dependent PL measurements provide valuable insights into activation energy and exciton-phonon coupling strength. Our findings will not only deepen our understanding of charge carrier dynamics associated with STEs but also pave the way for the design of some promising perovskite materials for use in optoelectronics and photocatalysis.
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U2 - 10.1021/acsphyschemau.4c00008
DO - 10.1021/acsphyschemau.4c00008
M3 - Article
AN - SCOPUS:85197782433
SN - 2694-2445
VL - 4
SP - 476
EP - 489
JO - ACS Physical Chemistry Au
JF - ACS Physical Chemistry Au
IS - 5
ER -