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Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodide Perovskites
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2020-04-06 , DOI: 10.1002/adfm.201907982 Peijun Guo 1, 2 , Yi Xia 1, 3 , Jue Gong 4, 5 , Duyen H. Cao 6 , Xiaotong Li 7 , Xun Li 4 , Qi Zhang 8 , Constantinos C. Stoumpos 7, 9 , Matthew S. Kirschner 7 , Haidan Wen 8 , Vitali B. Prakapenka 10 , John B. Ketterson 11 , Alex B. F. Martinson 6 , Tao Xu 4 , Mercouri G. Kanatzidis 7 , Maria K. Y. Chan 1 , Richard D. Schaller 1, 7
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2020-04-06 , DOI: 10.1002/adfm.201907982 Peijun Guo 1, 2 , Yi Xia 1, 3 , Jue Gong 4, 5 , Duyen H. Cao 6 , Xiaotong Li 7 , Xun Li 4 , Qi Zhang 8 , Constantinos C. Stoumpos 7, 9 , Matthew S. Kirschner 7 , Haidan Wen 8 , Vitali B. Prakapenka 10 , John B. Ketterson 11 , Alex B. F. Martinson 6 , Tao Xu 4 , Mercouri G. Kanatzidis 7 , Maria K. Y. Chan 1 , Richard D. Schaller 1, 7
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Hybrid organic–inorganic perovskites such as methylammonium lead iodide have emerged as promising semiconductors for energy‐relevant applications. The interactions between charge carriers and lattice vibrations, giving rise to polarons, have been invoked to explain some of their extraordinary optoelectronic properties. Here, time‐resolved optical spectroscopy is performed, with off‐resonant pumping and electronic probing, to examine several representative lead iodide perovskites. The temporal oscillations of electronic bandgaps induced by coherent lattice vibrations are reported, which is attributed to antiphase octahedral rotations that dominate in the examined 3D and 2D hybrid perovskites. The off‐resonant pumping scheme permits a simplified observation of changes in the bandgap owing to the A g vibrational mode, which is qualitatively different from vibrational modes of other symmetries and without increased complexity of photogenerated electronic charges. The work demonstrates a strong correlation between the lead–iodide octahedral framework and electronic transitions, and provides further insights into the manipulation of coherent optical phonons and related properties in hybrid perovskites on ultrafast timescales.
中文翻译：
直接观察杂化碘化钙钛矿中光学声子引起的带隙振荡。
杂化有机-无机钙钛矿，例如甲基铵碘化铅，已经成为与能源相关应用的有前途的半导体。载流子与晶格振动之间的相互作用（产生极化子）已被用来解释其某些非凡的光电特性。在这里，使用时间分辨光谱，通过非共振泵浦和电子探测，检查了几种代表性的碘化铅钙钛矿。报告了由相干晶格振动引起的电子带隙的时间振动，这是由于在所研究的3D和2D混合钙钛矿中占主导地位的反相八面体旋转。非谐振抽运方案可以简化观察由于A g而引起的带隙变化振动模式，在质量上与其他对称振动模式不同，并且不会增加光生电子电荷的复杂性。这项工作证明了铅-碘八面体框架与电子跃迁之间有很强的相关性，并为超钙钛矿中混合钙钛矿中相干光学声子的操纵和相关特性提供了进一步的见解。
更新日期：2020-04-06
中文翻译：
直接观察杂化碘化钙钛矿中光学声子引起的带隙振荡。
杂化有机-无机钙钛矿，例如甲基铵碘化铅，已经成为与能源相关应用的有前途的半导体。载流子与晶格振动之间的相互作用（产生极化子）已被用来解释其某些非凡的光电特性。在这里，使用时间分辨光谱，通过非共振泵浦和电子探测，检查了几种代表性的碘化铅钙钛矿。报告了由相干晶格振动引起的电子带隙的时间振动，这是由于在所研究的3D和2D混合钙钛矿中占主导地位的反相八面体旋转。非谐振抽运方案可以简化观察由于A g而引起的带隙变化振动模式，在质量上与其他对称振动模式不同，并且不会增加光生电子电荷的复杂性。这项工作证明了铅-碘八面体框架与电子跃迁之间有很强的相关性，并为超钙钛矿中混合钙钛矿中相干光学声子的操纵和相关特性提供了进一步的见解。
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