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Breakdown of volume scaling in auger recombination in CdSe/CdS heteronanocrystals: The role of the core-shell interface

机译:CdSe / CdS杂晶中螺旋重组中体积比例的分解:核-壳界面的作用

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Spatial confinement of electronic excitations in semiconductor nanocrystals (NCs) results in a significant enhancement of nonradiative Auger recombination (AR), such that AR processes can easily dominate the decay of multiexcitons. AR is especially detrimental to lasing applications of NCs, as optical gain in these structures explicitly relies on emission from multiexciton states. In standard NCs, AR rates scale linearly with inverse NC volume. Here, we investigate multiexciton dynamics in hetero-NCs composed of CdSe cores and CdS shells of tunable thickness. We observe a dramatic decrease in the AR rates at the initial stage of shell growth, which cannot be explained by traditional volume scaling alone. Rather, fluorescence-line-narrowing studies indicate that the suppression of AR correlates with the formation of an alloy layer at the core-shell interface suggesting that this effect derives primarily from the "smoothing" of the confinement potential associated with interfacial alloying. These data highlight the importance of NC interfacial structure in the AR process and provide general guidelines for the development of new nanostructures with suppressed AR for future lasing applications.
机译:半导体纳米晶体(NCs)中电子激发的空间限制导致非辐射俄歇复合(AR)的显着增强,从而AR过程可以轻松地控制多激子的衰减。由于这些结构中的光学增益明确依赖于多激子态的发射,因此AR尤其不利于NC的激光应用。在标准NC中,AR率与NC反向体积成线性比例关系。在这里,我们研究了由可调厚度的CdSe核和CdS壳组成的异质NC中的多激子动力学。我们观察到壳生长初期AR率急剧下降,这不能仅通过传统的体积缩放来解释。而是,荧光线变窄的研究表明,AR的抑制与核-壳界面处合金层的形成有关,这表明该效应主要源自与界面合金化相关的约束电位的“平滑”。这些数据凸显了NC界面结构在AR过程中的重要性,并为开发具有抑制性AR的新型纳米结构提供了一般指导,以用于未来的激光应用。

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