Diffusion-Dominated Luminescence Dynamics of CsPbBr3 Studied Using Cathodoluminescence and Microphotoluminescence Spectroscopy

• Published in: Nano letters Vol. 24; no. 13; pp. 3971 - 3977
• Main Authors: Nekita, Sho, Yanagimoto, Sotatsu, Sannomiya, Takumi, Akiba, Keiichirou, Takiguchi, Masato, Sumikura, Hisashi, Takagi, Itsuki, Nakamura, Kazutaka G., Yip, SenPo, Meng, You, Ho, Johnny C., Okuyama, Tetsuya, Murayama, Mitsuhiro, Saito, Hikaru
• Format: Journal Article
• Language: English
• Published: American Chemical Society 03.04.2024
• Subjects: cathodoluminescence; lifetime measurement; carrier diffusion; photoluminescence; carrier dynamics; halide perovskite
• ISSN: 1530-6984; 1530-6992
• DOI: 10.1021/acs.nanolett.4c00483

Time-resolved or time-correlation measurements using cathodoluminescence (CL) reveal the electronic and optical properties of semiconductors, such as their carrier lifetimes, at the nanoscale. However, halide perovskites, which are promising optoelectronic materials, exhibit significantly different decay dynamics in their CL and photoluminescence (PL). We conducted time-correlation CL measurements of CsPbBr3 using Hanbury Brown-Twiss interferometry and compared them with time-resolved PL. The measured CL decay time was on the order of subnanoseconds and was faster than PL decay at an excited carrier density of 2.1 × 1018 cm–3. Our experiment and analytical model revealed the CL dynamics induced by individual electron incidences, which are characterized by highly localized carrier generation followed by a rapid decrease in carrier density due to diffusion. This carrier diffusion can play a dominant role in the CL decay time for undoped semiconductors, in general, when the diffusion dynamics are faster than the carrier recombination.