Pressure-modulated bandgap and optoelectronic properties in lead-free double perovskite Cs<sub>2</sub>TeCl<sub>6</sub>

WU Shuying; MA Shuailing; ZHAO Chunyan; LI Shixin; YE Meiyan; QI Mengyao; ZHAO Xingbin; WANG Lingrui; CUI Tian

doi:10.7498/aps.74.20250693

Abstract

As a core component of modern optoelectronic systems, photodetectors play an indispensable role in optical communications, environmental monitoring, medical imaging, and military detection. With the rapid development of related technologies, the development of novel photodetector materials featuring high sensitivity, fast response, and excellent stability has become a key research focus. Among various candidate materials, A₂BX₆-type vacancy-ordered double perovskites have attracted significant attention due to their unique crystal structures and outstanding optoelectronic properties. These materials not only possess tunable bandgap structures and high carrier mobility but also demonstrate excellent environmental stability, showing broad application prospects in the field of photodetection. In this study, the optoelectronic response behaviors of a representative lead-free double perovskite, Cs₂TeCl₆, under high-pressure conditions are systematically investigated. Precise experimental observations reveal an anomalous transition in photocurrent from decrease to increase when the pressure reaches 21.7 GPa. By employing advanced characterization techniques, including high-pressure in situ Raman spectroscopy, UV-Vis absorption spectroscopy, and synchrotron X-ray diffraction, the underlying physical mechanism are elucidated: At the critical pressure of 18 GPa, the material enters an intensified compression stage, leading to a significantly accelerated bandgap narrowing rate. This continuous reduction in bandgap effectively mitigates the weak absorption limitation of the indirect bandgap, enabling efficient absorption of previously unexcitable low-energy photons and ultimately resulting in enhanced photocurrent. This finding not only clarifies the intrinsic relationship between the structure and optoelectronic properties of Cs₂TeCl₆ at a microscopic level, but, more importantly, offers new insights into regulating the optoelectronic performance of perovskite materials through pressure engineering. These outcomes in this work provide important guidance for developing novel high-performance photodetection devices and establish a valuable research method of optimizing other semiconductor materials. In the future, by further refining material compositions and pressure modulation strategies, the design and fabrication of more efficient and stable photodetector materials can be anticipated.

Keywords:

Authors and contacts

1.
Institute of High-Pressure Physics, School of Physical Science and Technology, Ningbo University, Ningbo 315211, China
2.
State Key Laboratory of Superhard Materials, Jilin University, Changchun 130015 China
3.
College of Science, Hainan Tropical Ocean University, Sanya 572022 China
4.
School of Physics, Zhengzhou University, Zhengzhou 450052 China

Corresponding author: MA Shuailing, mashuailing@nbu.edu.cn ; CUI Tian, cuitian@nbu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 12204254, 52072188), the Program for Science and Technology Innovation Team in Zhejiang, China (Grant No. 2021R01004), the Natural Science Foundation of Zhejiang Province, China (Grant No. LQ23A040005), the National Major Science Facility Synergetic Extreme Condition User Facility Achievement Transformation Platform Construction, China (Grant No. 2021FGWCXNLJSKJ01), and the Fundamental Research Funds for the Provincial Universities, China (Grant Nos. JYT2023005, JYT2024019).

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References

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Cited By

图 1 Cs₂TeCl₆在环境条件下的样品表征　(a) $Fm\bar3m $相Cs₂TeCl₆的晶体结构Cs₂TeCl₆的X射线衍射(XRD), 1 atm = 1.013 × 10⁵ Pa; (b) $Fm\bar3m $相Cs₂TeCl₆的晶体结构; (c) Cs₂TeCl₆的拉曼光谱; (d) Cs₂TeCl₆的吸收光谱

Figure 1. Characterization of Cs₂TeCl₆ under ambient conditions: (a) X-ray diffraction (XRD) pattern of $Fm\bar3m $ phase Cs₂TeCl₆, 1 atm = 1.013 × 10⁵ Pa; (b) Crystal structure of $Fm\bar3m $ phase Cs₂TeCl₆; (c) Raman spectrum of Cs₂TeCl₆; (d) Absorption spectrum of Cs₂TeCl₆.

DownLoad: Full-Size Img PowerPoint

图 2 Cs₂TeCl₆光电测试准备　(a), (b) Cs₂TeCl₆高压DAC光电性质测试装置示意图; (c) 0.69 GPa、0.1 V偏压时, Cs₂TeCl₆在不同入射波长下的光响应图谱

Figure 2. Preparation for optoelectronic measurements of Cs₂TeCl₆: (a), (b) Schematic diagram of the high-pressure DAC optoelectronic measurement setup for Cs₂TeCl₆; (c) Photoresponse spectra of Cs₂TeCl₆ under different incident wavelengths at 0.69 GPa with 0.1 V bias.

DownLoad: Full-Size Img PowerPoint

图 3 405 nm入射波长、0.1 V偏压下, Cs₂TeCl₆高压光电测试　(a) Cs₂TeCl₆在高压下的光响应图谱; (b) 光电流密度J_ph以及光响应强度R在升压过程中随压力的变化趋势

Figure 3. High-pressure optoelectronic measurements of Cs₂TeCl₆ at 405 nm incident wavelength with 0.1 V bias: (a) Photoresponse spectra of Cs₂TeCl₆ under high pressure; (b) pressure-dependent variations of photocurrent density (J_ph) and responsivity (R) during compression.

DownLoad: Full-Size Img PowerPoint

图 4 Cs₂TeCl₆高压下带隙的变化　(a) 高压下的Cs₂TeCl₆紫外-可见吸收光谱; (b) 带隙随压力变化趋势; (c) 压力下DAC中Cs₂TeCl₆的光学显微照片

Figure 4. Bandgap evolution of Cs₂TeCl₆ under high pressure: (a) UV-Vis absorption spectra of Cs₂TeCl₆ under compression; (b) pressure dependence of the bandgap; (c) optical micrograph of Cs₂TeCl₆ in a DAC upon compression.

DownLoad: Full-Size Img PowerPoint

图 5 532 nm激光激发下, Ruby作为传压介质, Cs₂TeCl₆的高压拉曼表征　(a) Cs₂TeCl₆高压拉曼图谱; (b) Cs₂TeCl₆拉曼振动峰随压力变化趋势

Figure 5. High-pressure Raman characterization of Cs₂TeCl₆ using Ruby as pressure-transmitting medium under 532 nm laser excitation: (a) High-pressure Raman spectra of Cs₂TeCl₆; (b) pressure dependence of Raman frequencies in Cs₂TeCl₆.

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[1]	Li Y, Shi Z F, Li X J, Shan C X 2019 Chin. Phys. B 28 017803 Google Scholar
[2]	Tan Z K, Moghaddam R S, Lai M L, Docampo P, Higler R, Deschler F, Price M, Sadhanala A, Pazos L M, Credgington D, Hanusch F, Bein T, Snaith H J, Friend R H 2014 Nat. Nanotechnol. 9 687 Google Scholar
[3]	Dursun I, Shen C, Parida M R, Pan J, Sarmah S P, Priante D, Alyami N, Liu J K, Saidaminov M I, Alias M S, Abdelhady A L, Ng T K, Mohammed O F, Ooi B S, Bakr O M 2016 ACS Photonics 3 1150 Google Scholar
[4]	Liu M Z, Johnston M B, Snaith H J 2013 Nature 501 395 Google Scholar
[5]	Wang J Y, Zhang C, Liu H L, R McLaughlin, Zhai Y X, Vardeny S R, Liu X J, McGill S, Semenov D, Guo H, Tsuchikawa R, Deshpande V V, Sun D, Vardeny Z V 2019 Nat. Commun. 10 129 Google Scholar
[6]	Xu Y Q, Chen Q, Zhang C F, Wang R, Wu H, Zhang X Y, Xing G H, Yu W W, Wang X Y, Zhang Y, Xiao M 2016 J. Am. Chem. Soc. 138 3761 Google Scholar
[7]	Chen J Z, Zhao X, Kim S G, Park N G 2019 Adv. Mater. 31 1902902 Google Scholar
[8]	Ghosh S, Shankar H, Kar P 2022 Mater. Adv. 3 3742 Google Scholar
[9]	Muscarella L A, Hutter E M 2022 ACS Energy Lett. 7 2128 Google Scholar
[10]	Muhammad Faizan, 赵国琪, 张天旭, 王啸宇, 贺欣, 张立军 2024 物理化学学报 40 2303004 Google Scholar Faizan M, Zhao G Q, Zhang T X, Wang X Y, He X, Zhang L J 2024 Acta Phys. Chim. Sin. 40 2303004 Google Scholar
[11]	Zhang L J, Wang Y C, Lv J, Ma Y M 2017 Nat. Rev. Mater. 2 17005 Google Scholar
[12]	Bassett W A 2009 High Pressure Res. 29 163 Google Scholar
[13]	Liang Y F, Huang X L, Huang Y P, Wang X, Li F F, Wang Y C, Tian F B, Liu B B, Shen Z X, Cui T 2019 Adv. Sci. 6 1900399 Google Scholar
[14]	Lee J H, Jaffe A, Lin Y, Karunadasa H I, Neaton J B 2020 ACS Energy Lett. 5 2174 Google Scholar
[15]	McMillan P F 2002 Nat. Mater. 1 19 Google Scholar
[16]	Yin Y F, Yan X C, Luo H, Liang Y F, Xu P, Wang Y M, Jin S Y, Tian W M 2025 Angew Chem. Int. Ed. 64 202418587 Google Scholar
[17]	Li Z L, Jia B X, Fang S X, Li Q J, Tian F Y, Li H Y, Liu R, Liu Y C, Zhang L J, Liu S Z(Frank), Liu B B 2023 Adv. Sci. 10 2205837 Google Scholar
[18]	Zhao W Y, Ma Z W, Shi Y, Fu R J, Wang K, Sui Y M, Xiao G J, Zou B 2023 Cell Rep. Phys. Sci. 4 101663 Google Scholar
[19]	Fang S X, Li Q J, Li Z L, Dong Q, Jing X L, Li C Y, Li H Y, Liu B, Liu R, Liu B B 2023 Mater. Res. Lett. 11 134 Google Scholar
[20]	Guo S H , Mao Y H, Chen C C, Zhang Y, Zhao G X, Bu K J, Hu Q Y, Zhu H M, Zou G F, Yang W G, Mao L L, Lü X J 2024 CCS Chem. 6 1748 Google Scholar
[21]	Guo S H, Mihalyi-Koch W, Mao Y H, Li X Y, Bu K J, Hong H L, Hautzinger M P, Luo H, Wang D, Gu J Z, Zhang Y F, Zhang D Z, Hu Q Y, Ding Y, Yang W G, Fu Y P, Jin S, Lü X J 2024 Nat. Commun. 15 3001 Google Scholar
[22]	Shi H, Chen L, Moutaabbid H, Feng Z B, Zhang G Z, Wang L R, Li Y W, Guo H Z, Liu C L 2024 Small 20 2405692 Google Scholar
[23]	Maughan A E, Ganose A M, Bordelon M M, Miller E M, Scanlon D O, Neilson J R 2016 J. Am. Chem. Soc. 138 8453 Google Scholar
[24]	Smith M D, Jaffe A, Dohner E R, Lindenberg A M, Karunadasa H I 2017 Chem. Sci. 8 4497 Google Scholar
[25]	Wang Y Q, Guo S H, Luo H, Zhou C K, Lin H R, Ma X D, Hu Q Y, Du M H, Ma B W, Yang W G, Lü X J 2020 J. Am. Chem. Soc. 142 16001 Google Scholar
[26]	Jiang J T, Niu G M, Sui L Z, Wang X W, Zeng X Y, Zhang Y T, Che L, Wu G R, Yuan K J, Yang X M 2023 Adv. Opt. Mater. 11 2202634 Google Scholar
[27]	姚盼盼, 王玲瑞, 王家祥, 郭海中 2020 物理学报 69 218801 Google Scholar Yao P P, Wang L R, Wang J X, Guo H Z 2020 Acta Phys. Sin. 69 218801 Google Scholar
[28]	Pi C J, Yu X, Chen W Q, Yang L L, Wang C, Liu Z C, Wang Y Y, Qiu J B, Liu B T, Xu X H 2021 Mater. Adv. 2 1043 Google Scholar
[29]	Li Z L, Li H Y, Liu N N, Du M Y, Jin X L, Li Q J, Du Y, Guo L, Liu B B 2021 Adv. Opt. Mater. 9 2101163 Google Scholar
[30]	Folgueras M C, Jin J B, Gao M Y, Quan L N, Steele J A, Srivastava S, Ross M B, Zhang R, Seeler F, Schierle-Arndt K, Asta M, Yang P D 2021 J. Phys. Chem. C 125 25126 Google Scholar

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Pressure-modulated bandgap and optoelectronic properties in lead-free double perovskite Cs₂TeCl₆

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Corresponding author: MA Shuailing, mashuailing@nbu.edu.cn ; CUI Tian, cuitian@nbu.edu.cn

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Pressure-modulated bandgap and optoelectronic properties in lead-free double perovskite Cs2TeCl6

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Corresponding author: MA Shuailing, mashuailing@nbu.edu.cn ; CUI Tian, cuitian@nbu.edu.cn

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Pressure-modulated bandgap and optoelectronic properties in lead-free double perovskite Cs₂TeCl₆