Nanocrystal lasing in the single-exciton regime using engineered exciton-exciton interactions

V. Klimov, S. Ivanov, J. Nanda, I. Bezel, M. Achermann, L. Balet
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Abstract

Because of size-controlled emission color, good photostability, and chemical flexibility, colloidal semiconductor nanocrystals (NCs) are promising building blocks for new types of colorselectable optical gain media [1]. One factor limiting optical gain performance ofNCs is highly efficient multiexciton Auger recombination that leads to short picosecond optical gain life times [2]. Recent attempts to suppress Auger recombination utilized NC shape control [3, 4]. Using elongated CdSe NCs (quantum rods) it was possible to extend optical gain life times by almost an order of magnitude, which further allowed a many-fold reduction of the excitation threshold for amplified spontaneous emission (ASE) [4]. For both spherical and elongated particles, Auger recombination times rapidly shorten as the particle dimensions are decreased. Therefore, it becomes progressively more difficult to achieve the ASE regime for shorter wavelengths that require the use of NCs of small sizes. In particular, while demonstrating strong optical-gain performance in the red-yellow spectral ranges, CdSe NCs do not show efficient ASE in the range of green and particularly blue colors that correspond to extremely small NC sizes (< 3nm).
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利用工程激子-激子相互作用的单激子体制下的纳米晶体激光
胶体半导体纳米晶体(NCs)具有尺寸控制的发射色、良好的光稳定性和化学柔韧性,是新型可选色光学增益介质的重要组成部分[1]。限制nc光学增益性能的一个因素是高效的多激子俄歇复合,这会导致短皮秒的光学增益寿命[2]。最近尝试利用数控形状控制来抑制螺旋钻复合[3,4]。使用细长的CdSe NCs(量子棒),可以将光学增益寿命延长近一个数量级,这进一步允许将放大自发发射(ASE)的激发阈值降低许多倍[4]。对于球形和细长颗粒,随着颗粒尺寸的减小,俄歇复合时间迅速缩短。因此,在需要使用小尺寸nc的较短波长的情况下,实现ASE变得越来越困难。特别是,虽然CdSe纳米在红-黄光谱范围内表现出强大的光学增益性能,但在绿色和蓝色范围内却没有表现出有效的ASE,这对应于极小的纳米尺寸(< 3nm)。
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