-
Environmentally friendly lead-free double perovskite materials have emerged as promising alternatives to lead-based perovskites due to their excellent optoelectronic properties and improved stability. In this study, we synthesized a highly crystalline lead-free double perovskite, Cs2AgInCl6, via a mild hydrothermal method and systematically investigated its pressure-induced structural evolution and optoelectronic regulation up to 41.1 GPa at room temperature using diamond anvil cell (DAC) techniques combined with multiple in-situ characterization methods. High-pressure synchrotron X-ray diffraction revealed a structural phase transition from the cubic phase (Fm-3m) to the tetragonal phase (I4/m) at 8.9 GPa. In-situ Raman spectroscopy further confirmed this transition through the splitting of characteristic phonon modes, indicating enhanced structural anisotropy. Pressure-dependent optical absorption spectra showed a distinct reversal in the trend of bandgap evolution during the phase transition, reflecting a strong coupling between the crystal structure and the electronic band structure. Remarkably, the photocurrent exhibited continuous pressure-enhanced behavior, reaching twice the ambient pressure value at 41.1 GPa, and the enhanced performance was retained after complete pressure release, suggesting stable pressure-induced structural changes. These findings provide fundamental insights into the pressure-mediated structure-property relationships in lead-free double perovskites and propose viable strategies for optimizing optoelectronic performance through crystal engineering and strain modulation. The retained post-compression functionality highlights their potential applications in non-volatile pressure-tunable photodetectors.
-
Keywords:
- Lead-free double perovskite /
- photoelectric properties /
- pressure regulation /
- structural phase transition
-
[1] Boyd C C, Cheacharoen R, Leijtens T, McGehee M D 2019 Chem Rev 119 3418
[2] Lin D, Shi T, Xie H, Wan F, Ren X, Liu K, Zhao Y, Ke L, Lin Y, Gao Y, Xu X, Xie W, Liu P, Yuan Y 2021 Advanced Energy Materials 11
[3] Lan S, Li W, Wang S, Li J, Wang J, Wang H, Luo H, Li D 2018 Advanced Optical Materials 7
[4] Wei J-H, Liao J-F, Wang X-D, Zhou L, Jiang Y, Kuang D-B 2020 Matter 3 892
[5] Zhou L, Xu Y F, Chen B X, Kuang D B, Su C Y 2018 Small 14 e1703762
[6] Luo J, Wang X, Li S, Liu J, Guo Y, Niu G, Yao L, Fu Y, Gao L, Dong Q, Zhao C, Leng M, Ma F, Liang W, Wang L, Jin S, Han J, Zhang L, Etheridge J, Wang J, Yan Y, Sargent E H, Tang J 2018 Nature 563 541
[7] Xu J C, Gao H, Chen G Q, Wang K K, Hu J H 2024 Inorg Chem. 40 405（in Chinese）[徐锦锃, 高辉, 陈国庆, 王可可, 胡金辉 2024 无机化学学报 40 405]
[8] Xia Z, Poeppelmeier K R 2017 Acc Chem Res 50 1222
[9] Xia Z, Ma C, Molokeev M S, Liu Q, Rickert K, Poeppelmeier K R 2015 J Am Chem Soc 137 12494
[10] Zhao X G, Yang J H, Fu Y, Yang D, Xu Q, Yu L, Wei S H, Zhang L 2017 J Am Chem Soc 139 2630
[11] Ji F, Klarbring J, Wang F, Ning W, Wang L, Yin C, Figueroa J S M, Christensen C K, Etter M, Ederth T, Sun L, Simak S I, Abrikosov I A, Gao F 2020 Angew Chem Int Ed Engl 59 15191
[12] McClure E T, Ball M R, Windl W, Woodward P M 2016 Chemistry of Materials 28 1348
[13] Deng W, Deng Z-Y, He J, Wang M, Chen Z-X, Wei S-H, Feng H-J 2017 Applied Physics Letters 111
[14] Liu X, Niu G, Jiang J, Che L, Sui L, Wang X, Zeng X, Wu G, Yuan K, Yang X 2024 Laser & Photonics Reviews 19
[15] Chen L, Jiang H, Luo Z, Liu G, Wu X, Liu Y, Sun P, Jiang J 2022 Materials Advances 3 4381
[16] Li Q, Wang Y, Pan W, Yang W, Zou B, Tang J, Quan Z 2017 Angew Chem Int Ed Engl 56 15969
[17] Wu X Q, Wang L R, Yuan Y F, Ma L, Guo H Z 2023 High. Pressure. Physics. 37 21（in Chinese）[吴学仟, 王玲瑞, 袁亦方, 马良, 郭海中 2023 高压物理学报 37 21]
[18] Lu X, Wang Y, Stoumpos C C, Hu Q, Guo X, Chen H, Yang L, Smith J S, Yang W, Zhao Y, Xu H, Kanatzidis M G, Jia Q 2016 Adv Mater 28 8663
[19] Jebnouni A, Alatawi Abdullah A, Bouzidi M, Alshammari Ahlam F, Aljaloud Amjad S, Alshammari Mona A F, Jebali M, Bechir Mohamed B 2025 Applied Organometallic Chemistry 39
[20] Prescher C, Prakapenka V B 2015 High Pressure Research 35 223
[21] Li X, Li W, Xia M, Liu C, Li N, Shi Z, Xu Y, Zhang X 2022 Inorg Chem 61 5040
[22] Ning W, Gao F 2019 Adv Mater 31 e1900326
[23] Sa R, Wei Y, Zha W, Liu D 2020 Chemical Physics Letters 754
[24] Kong L, Liu G, Gong J, Hu Q, Schaller R D, Dera P, Zhang D, Liu Z, Yang W, Zhu K, Tang Y, Wang C, Wei S H, Xu T, Mao H K 2016 Proc Natl Acad Sci U S A 113 8910
[25] Wang L, Ou T, Wang K, Xiao G, Gao C, Zou B 2017 Applied Physics Letters 111
Metrics
- Abstract views: 50
- PDF Downloads: 1
- Cited By: 0
下载:
