Semiconductor nanoplatelets: a new colloidal system for low-threshold high-gain stimulated emission (Presentation Recording)

M. Pelton, C. She, Igor Fedin, Dmitriy S. Dolzhnikov, S. Ithurria, Erfan Baghani, S. O’Leary, A. Demortière, R. Schaller, D. Talapin
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Abstract

Quantum wells (QWs) are thin semiconductor layers than confine electrons and holes in one dimension. They are widely used for optoelectronic devices, particularly semiconductor lasers, but have so far been produced using expensive epitaxial crystal-growth techniques. This has motivated research into the use of colloidal semiconductor nanocrystals, which can be synthesized chemically at low cost, and can be processed in the solution phase. However, initial demonstrations of optical gain from colloidal nanocrystals involved high thresholds. Recently, colloidal synthesis methods have been developed for the production of thin, atomically flat semiconductor nanocrystals, known as nanoplatelets (NPLs). We investigated relaxation of high-energy carriers in colloidal CdSe NPLs, and found that the relaxation is characteristic of a QW system. Carrier cooling and relaxation on time scales from picoseconds to hundreds of picoseconds are dominated by Auger-type exciton-exciton interactions. The picosecond-scale cooling of hot carriers is much faster than the exciton recombination rate, as required for use of these NPLs as optical gain and lasing materials. We therefore investigated amplified spontaneous emission using close-packed films of NPLs. We observed thresholds that were more than 4 times lower than the best reported value for colloidal nanocrystals. Moreover, gain in these films is 4 times higher than gain reported for other colloidal nanocrystals, and saturates at pump fluences more than two orders of magnitude above the ASE threshold. We attribute this exceptional performance to large optical cross-sections, relatively slow Auger recombination rates, and narrow ensemble emission linewidths.
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半导体纳米薄片:一种新的低阈值高增益受激发射胶体系统(演讲录音)
量子阱是一种将电子和空穴限制在一维空间内的薄半导体层。它们广泛用于光电子器件,特别是半导体激光器,但迄今为止都是使用昂贵的外延晶体生长技术生产的。这激发了对胶体半导体纳米晶体使用的研究,这种纳米晶体可以用低成本的化学方法合成,并且可以在溶液中加工。然而,胶体纳米晶体的光学增益的初始演示涉及高阈值。最近,胶体合成方法已被开发用于生产薄的,原子平面的半导体纳米晶体,称为纳米片(NPLs)。我们研究了胶体CdSe NPLs中高能载流子的弛豫,发现弛豫是量子阱系统的特征。在皮秒到数百皮秒的时间尺度上,载流子的冷却和弛豫主要是由俄歇型激子-激子相互作用控制的。热载流子的皮秒级冷却比激子复合速率快得多,这是使用这些NPLs作为光学增益和激光材料所需要的。因此,我们利用不良贷款的致密薄膜研究了放大的自发辐射。我们观察到的阈值比胶体纳米晶体的最佳报道值低4倍以上。此外,这些薄膜的增益比其他胶体纳米晶体的增益高4倍,并且在泵浦影响下比ASE阈值高两个数量级以上。我们将这种特殊的性能归因于大的光学截面,相对较慢的俄歇复合率和较窄的系综发射线宽。
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