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Phonon-Assisted Reversible Thermochromism in a Lead-Free Antimony-Based Cs3Sb2Br9 Perovskite
ACS Applied Electronic Materials ( IF 4.3 ) Pub Date : 2022-07-05 , DOI: 10.1021/acsaelm.2c00361 Anupriya Singh 1 , Soumitra Satapathi 1
ACS Applied Electronic Materials ( IF 4.3 ) Pub Date : 2022-07-05 , DOI: 10.1021/acsaelm.2c00361 Anupriya Singh 1 , Soumitra Satapathi 1
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Lead-free antimony-based perovskites have emerged as promising photovoltaic materials due to their outstanding stability, lower toxicity, and easy processability. Recently, researchers have showed their successful implication in indoor energy applications, thus prompting their possible applications in buliding integrated device applications. Here, we investigate temperature-dependent band gap engineering leading to reversible thermochromism (TCM) in all-inorganic antimony-based Cs3Sb2Br9 single crystals (SCs). The 2D Cs3Sb2Br9 single crystals exhibited a color change from yellow to deep orange at elevated temperatures and returned to the original yellow when they were cooled to room temperature. Temperature-dependent UV–vis absorption spectroscopy and a differential thermal analysis (DTA) confirmed the optical band-edge modulation with no structural phase transition. Higher Urbach energy values at higher temperatures reveal that the shift in band edge is coming primarily from an extension in the indirect band edge, thus confirming that high-energy phonons are responsible for the reduced indirect band gap. X-ray diffraction (XRD) spectra were also obtained for varying temperatures, which confirmed the lattice expansion in 2D Cs3Sb2Br9 SCs. Additionally, Raman spectroscopy confirmed the enhancement in symmetric stretching at elevated temperatures. Our work studied the band gap modulation in 2D Cs3Sb2Br9 SCs with temperature and validates that the presence of high-energy phonons at elevated temperature results in an elongated Urbach tail and thus leads to the reversible TCM phenomena.
中文翻译：
无铅锑基 Cs3Sb2Br9 钙钛矿中的声子辅助可逆热致变色
无铅锑基钙钛矿因其出色的稳定性、低毒性和易加工性而成为有前途的光伏材料。最近，研究人员已经展示了他们在室内能源应用中的成功意义，从而促进了他们在建筑集成设备应用中的可能应用。在这里，我们研究了在全无机锑基 Cs 3 Sb 2 Br 9单晶 (SCs) 中导致可逆热致变色 (TCM) 的温度相关带隙工程。二维 Cs 3 Sb 2 Br 9单晶在高温下呈现出从黄色到深橙色的颜色变化，当它们冷却到室温时又恢复到原来的黄色。温度相关的紫外-可见吸收光谱和差热分析 (DTA) 证实了光学带边调制没有结构相变。较高温度下较高的 Urbach 能量值表明带边的偏移主要来自间接带边的延伸，从而证实高能声子是导致间接带隙减小的原因。还获得了不同温度下的 X 射线衍射 (XRD) 光谱，这证实了 2D Cs 3 Sb 2 Br 9中的晶格膨胀SC。此外，拉曼光谱证实了高温下对称拉伸的增强。我们的工作研究了二维 Cs 3 Sb 2 Br 9 SCs 中随温度变化的带隙调制，并验证了高温下高能声子的存在导致了拉长的 Urbach 尾，从而导致了可逆的 TCM 现象。
更新日期：2022-07-05
中文翻译：
无铅锑基 Cs3Sb2Br9 钙钛矿中的声子辅助可逆热致变色
无铅锑基钙钛矿因其出色的稳定性、低毒性和易加工性而成为有前途的光伏材料。最近，研究人员已经展示了他们在室内能源应用中的成功意义，从而促进了他们在建筑集成设备应用中的可能应用。在这里，我们研究了在全无机锑基 Cs 3 Sb 2 Br 9单晶 (SCs) 中导致可逆热致变色 (TCM) 的温度相关带隙工程。二维 Cs 3 Sb 2 Br 9单晶在高温下呈现出从黄色到深橙色的颜色变化，当它们冷却到室温时又恢复到原来的黄色。温度相关的紫外-可见吸收光谱和差热分析 (DTA) 证实了光学带边调制没有结构相变。较高温度下较高的 Urbach 能量值表明带边的偏移主要来自间接带边的延伸，从而证实高能声子是导致间接带隙减小的原因。还获得了不同温度下的 X 射线衍射 (XRD) 光谱，这证实了 2D Cs 3 Sb 2 Br 9中的晶格膨胀SC。此外，拉曼光谱证实了高温下对称拉伸的增强。我们的工作研究了二维 Cs 3 Sb 2 Br 9 SCs 中随温度变化的带隙调制，并验证了高温下高能声子的存在导致了拉长的 Urbach 尾，从而导致了可逆的 TCM 现象。
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