Applied Physics Department, Eindhoven University of Technology , P.O. Box 513, 5600 MB, Eindhoven, The Netherlands.
Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, Utrecht University , Princetonplein 1, 3508 TA, Utrecht, The Netherlands.
ACS Nano. 2017 Nov 28;11(11):11024-11030. doi: 10.1021/acsnano.7b05033. Epub 2017 Oct 16.
We highlight the importance of carrier-phonon coupling in inorganic lead halide perovskite nanocrystals. The low-temperature photoluminescence (PL) spectrum of CsPbBr has been investigated under a nonresonant and a nonstandard, quasi-resonant excitation scheme, and phonon replicas of the main PL band have been identified as due to the Fröhlich interaction. The energy of longitudinal optical (LO) phonons has been determined from the separation of the zero phonon band and phonon replicas. We reason that the observed LO phonon coupling can only be related to an orthorhombically distorted crystal structure of the perovskite nanocrystals. Additionally, the strength of carrier-phonon coupling has been characterized using the ratio between the intensities of the first phonon replica and the zero-phonon band. PL emission from localized versus delocalized carriers has been identified as the source of the observed discrepancies between the LO phonon energy and phonon coupling strength under quasi-resonant and nonresonant excitation conditions, respectively.
我们强调了载流子-声子耦合在无机卤化铅钙钛矿纳米晶体中的重要性。在非共振和非标准的准共振激发方案下,研究了 CsPbBr 的低温光致发光(PL)光谱,并且已经确定主 PL 带的声子副本是由于 Fröhlich 相互作用引起的。从零声子带和声子副本的分离确定了纵光学(LO)声子的能量。我们认为,观察到的 LO 声子耦合只能与钙钛矿纳米晶体的正交畸变晶体结构有关。此外,还使用第一声子副本和零声子带之间的强度比来表征载流子-声子耦合的强度。局部和离域载流子的 PL 发射分别被确定为在准共振和非共振激发条件下观察到的 LO 声子能量和声子耦合强度之间差异的来源。