Center for Quantum Technology Research, School of Physics, Beijing Institute of Technology, Beijing 100081, China.
Beijing National Laboratory for Condensed Matter Physics, CAS Key Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
J Chem Phys. 2019 Sep 21;151(11):114704. doi: 10.1063/1.5115467.
By using femtosecond pump-probe spectroscopy with broadband detection from near-infrared to midinfrared, the carrier and phonon dynamics in few-layer 2H-MoTe after ultrafast excitation have been investigated in detail. Immediately following the photoexcitation, an ultrafast relaxation of the generated hot carriers by releasing phonons is observed within hundreds of femtoseconds. The subsequent electron-hole recombination with a time constant of ∼1.5 ps is clearly identified and demonstrated to be mediated through a defect-assisted process. Furthermore, we confirm that the observed redshift of the exciton resonance energy on longer time scales arises from the ultrafast thermalization of the 2H-MoTe lattice caused by the transfer of electronic excitation to the phonon system. As a result, the thermalization dynamics of the lattice within 2 ps and the following cooling process of the phonon system on the 100 ps time scale are directly monitored.
通过使用飞秒泵浦探测光谱技术,结合从近红外到中红外的宽带探测,详细研究了超快激发后少层 2H-MoTe 中的载流子和声子动力学。在光激发后,在几百飞秒内观察到由声子释放引起的生成热载流子的超快弛豫。随后的电子-空穴复合时间常数约为 1.5 ps,这一过程被明确识别并证明是通过缺陷辅助过程介导的。此外,我们证实观察到的较长时间尺度上激子共振能量的红移是由电子激发向声子系统的转移引起的 2H-MoTe 晶格的超快热化导致的。因此,在 2 ps 内直接监测晶格的热化动力学,以及在 100 ps 时间尺度上的声子系统的冷却过程。