Li Qiuyang, Liu Qiliang, Schaller Richard D, Lian Tianquan
Department of Chemistry , Emory University , 1515 Dickey Drive Northeast , Atlanta , Georgia 30322 , United States.
Center for Nanoscale Materials , Argonne National Laboratory , Argonne , Illinois 60439 , United States.
J Phys Chem Lett. 2019 Apr 4;10(7):1624-1632. doi: 10.1021/acs.jpclett.9b00759. Epub 2019 Mar 25.
Two-dimensional CdSe nanoplatelets are promising lasing materials. Their large lateral areas reduce the optical gain threshold by increasing the oscillator strength and multiexciton lifetimes but also increase the gain threshold by requiring multiple band-edge excitons (>2) to reach the optical gain. We observe that the optical gain threshold of CdSe nanoplatelets at 4 K is ∼4-fold lower than that at room temperature. Transient absorption spectroscopy measurements indicate that the exciton center-of-mass coherent area is smaller than the lateral size at room temperature and extends to nearly the whole nanoplatelets at 4 K. This suggests that the reduction in the optical gain threshold at a low temperature can be attributed to exciton coherent area extension that reduces the saturation number of band-edge excitons to enable biexciton gain and increases the radiative decay rate, consistent with the giant oscillator strength transition effect. This work demonstrates a new direction for lowering the optical gain threshold of nanomaterials.
二维CdSe纳米片是很有前景的激光材料。它们较大的横向面积通过增加振子强度和多激子寿命降低了光学增益阈值,但也因需要多个带边激子(>2个)达到光学增益而提高了增益阈值。我们观察到,CdSe纳米片在4 K时的光学增益阈值比室温下低约4倍。瞬态吸收光谱测量表明,激子质心相干面积在室温下小于横向尺寸,而在4 K时扩展到几乎整个纳米片。这表明低温下光学增益阈值的降低可归因于激子相干面积的扩展,这减少了带边激子的饱和数量以实现双激子增益,并增加了辐射衰减率,这与巨振子强度跃迁效应一致。这项工作展示了降低纳米材料光学增益阈值的一个新方向。