Wang Lifeng, Zhu Jingyi, Wang Junhui, Wu Kaifeng
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, People's Republic of China.
University of Chinese Academy of Sciences, Beijing 100049, People's Republic of China.
Nano Lett. 2024 Aug 28;24(34):10691-10698. doi: 10.1021/acs.nanolett.4c03290. Epub 2024 Aug 19.
Intersubband transition was recently discovered in colloidal nanoplatelets, but the associated intersubband carrier relaxation dynamics remains poorly understood. In particular, it is crucial to selectively excite the intersubband transition and to follow the hot electron dynamics in the absence of valence-band holes. This is achieved herein by exciting the predoped electrons in CdSe/ZnS nanoplatelets using near-infrared femtosecond pulses and monitoring nonequilibrium electron dynamics using broad-band visible pulses. We find that the = 2 electrons relax to the = 1 subband and establish a Fermi-Dirac distribution within 200 fs, and finally reach an equilibrium with the lattice within a few ps. The cooling dynamics depend mainly on the excitation fluence but weakly on the doping density and the lattice temperature. These characteristics are well captured by our numerical simulation that explicitly accounts for the state occupation effect and optical phonon scattering.
最近在胶体纳米片中发现了子带间跃迁,但相关的子带间载流子弛豫动力学仍知之甚少。特别是,在没有价带空穴的情况下选择性地激发子带间跃迁并跟踪热电子动力学至关重要。本文通过使用近红外飞秒脉冲激发CdSe/ZnS纳米片中的预掺杂电子,并使用宽带可见脉冲监测非平衡电子动力学来实现这一点。我们发现,(n = 2)的电子在200飞秒内弛豫到(n = 1)子带并建立费米 - 狄拉克分布,最终在几皮秒内与晶格达到平衡。冷却动力学主要取决于激发通量,但对掺杂密度和晶格温度的依赖性较弱。我们的数值模拟明确考虑了态占据效应和光学声子散射,很好地捕捉了这些特性。