Organic-inorganic hybrid metal halide perovskites(MHPs)have attracted tremendous attention for optoelectronic applications.The long photocarrier lifetime and moderate carrier mobility have been proposed as results of the large polaron formation in MHPs.However,it is challenging to measure the effective mass and carrier scattering parameters of the photogenerated large polarons in the ultrafast carrier recombination dynamics.Here,we show,in a one-step spectroscopic method,that the optical-pump and terahertz-electromagnetic probe(OPTP)technique allows us to access the nature of interplay of photoexcited unbound charge carriers and optical phonons in polycrystalline CH3NH3Pbl3(MAPbl3)of about 10 μm grain size.Firstly,we demonstrate a direct spectral evidence of the large polarons in polycrystalline MAPbl3.Using the Drude-Smith-Lorentz model along with the Fr?hlich-type electron-phonon(e-ph)coupling,we determine the effective mass and scattering parameters of photogenerated polaronic carriers.We discover that the resulting moderate polaronic carrier mobility is mainly influenced by the enhanced carrier scattering,rather than the polaron mass enhancement.While,the formation of large polarons in MAPbl3 polycrystalline grains results in a long charge carrier lifetime at room temperature.Our results provide crucial information about the photo-physics of MAPbl3 and are indispensable for optoelectronic device development with better performance.

Terahertz Technology Innovation Research Institute,Terahertz Spectrum and Imaging Technology Cooperative Innovation Center,Shanghai Key Lab of Modern Optical System,University of Shanghai for Science and Technology,Shanghai 200093,China;Qingdao Institute of Bioenergy and Bioprocess Technology,Chinese Academy of Sciences,Qingdao 266101,China;Physics Department,Materials Genome Institute,State Key Laboratory of Advanced Special Steel,Shanghai Key Laboratory of High Temperature Superconductors,International Centre of Quantum and Molecular Structures,Shanghai University,Shanghai 200444,China;Shanghai Institute of Technical Physics,Chinese Academy of Sciences,Yutian Road 500,Shanghai,China;Department of Physics,Shanghai University,99 Shangda Road,Shanghai 200444,China;University of Michigan-Shanghai Jiao Tong University Joint Institute,Shanghai Jiao Tong University,Shanghai,China;School of Physics,University of Wollongong,Wollongong,NSW 2522,Australia;Department of Physics and International Laser Center,Lomonosov Moscow State University,Leninskiie Gory 1,Moscow 19991,Russia;ILIT RAS-Branch of the FSRC,Crystallography and Photonics》RAS,Svyatoozerskaya 1,140700,Shatura,Moscow Region,Russia

[1]Zuanming Jin;Yan Peng;Yuqing Fang;Zhijiang Ye;Zhiyuan Fan;Zhilin Liu;Xichang Bao;Heng Gao;Wei Ren;Jing Wu;Guohong Ma;Qianli Chen;Chao Zhang;Alexey V.Balakin;Alexander P.Shkurinov;Yiming Zhu;Songlin Zhuang-.Photoinduced large polaron transport and dynamics in organic-inorganic hybrid lead halide perovskite with terahertz probes)[J].光：科学与应用（英文版）,2022(08):1853-1864

polarons,OPTP,CH3NH3Pbl3,polaronic

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