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利用激光打印等离子体阵列调控碲化汞量子点的自发红外发射

Tailoring spontaneous infrared emission of HgTe quantum dots with laser-printed plasmonic arrays.

作者信息

Sergeev A A, Pavlov D V, Kuchmizhak A A, Lapine M V, Yiu W K, Dong Y, Ke N, Juodkazis S, Zhao N, Kershaw S V, Rogach A L

机构信息

1Institute of Automation and Control Processes, Far Eastern Branch, Russian Academy of Sciences, Vladivostok, 690041 Russia.

2Far Eastern Federal University, Vladivostok, 690090 Russia.

出版信息

Light Sci Appl. 2020 Feb 4;9:16. doi: 10.1038/s41377-020-0247-6. eCollection 2020.

Abstract

Chemically synthesized near-infrared to mid-infrared (IR) colloidal quantum dots (QDs) offer a promising platform for the realization of devices including emitters, detectors, security, and sensor systems. However, at longer wavelengths, the quantum yield of such QDs decreases as the radiative emission rate drops following Fermi's golden rule, while non-radiative recombination channels compete with light emission. Control over the radiative and non-radiative channels of the IR-emitting QDs is crucially important to improve the performance of IR-range devices. Here, we demonstrate strong enhancement of the spontaneous emission rate of near- to mid-IR HgTe QDs coupled to periodically arranged plasmonic nanoantennas, in the form of nanobumps, produced on the surface of glass-supported Au films via ablation-free direct femtosecond laser printing. The enhancement is achieved by simultaneous radiative coupling of the emission that spectrally matches the first-order lattice resonance of the arrays, as well as more efficient photoluminescence excitation provided by coupling of the pump radiation to the local surface plasmon resonances of the isolated nanoantennas. Moreover, coupling of the HgTe QDs to the lattice plasmons reduces the influence of non-radiative decay losses mediated by the formation of polarons formed between QD surface-trapped carriers and the IR absorption bands of dodecanethiol used as a ligand on the QDs, allowing us to improve the shape of the emission spectrum through a reduction in the spectral dip related to this ligand coupling. Considering the ease of the chemical synthesis and processing of the HgTe QDs combined with the scalability of the direct laser fabrication of nanoantennas with tailored plasmonic responses, our results provide an important step towards the design of IR-range devices for various applications.

摘要

化学合成的近红外到中红外(IR)胶体量子点(QDs)为实现包括发射器、探测器、安全和传感器系统在内的器件提供了一个有前景的平台。然而,在较长波长下,此类量子点的量子产率会随着辐射发射率按照费米黄金定则下降而降低,同时非辐射复合通道与发光相互竞争。控制红外发射量子点的辐射和非辐射通道对于提高红外波段器件的性能至关重要。在此,我们展示了通过无烧蚀直接飞秒激光打印在玻璃支撑的金膜表面制备的纳米凸起形式的周期性排列的等离子体纳米天线耦合后,近红外到中红外HgTe量子点的自发发射率得到了显著增强。这种增强是通过发射与阵列的一阶晶格共振在光谱上匹配的同时进行辐射耦合,以及泵浦辐射与孤立纳米天线的局域表面等离子体共振耦合提供更高效的光致发光激发来实现的。此外,HgTe量子点与晶格等离子体的耦合减少了由量子点表面捕获的载流子与用作量子点配体的十二烷硫醇的红外吸收带之间形成的极化子介导的非辐射衰减损失的影响,使我们能够通过减少与这种配体耦合相关的光谱凹陷来改善发射光谱的形状。考虑到HgTe量子点化学合成和加工的简便性以及具有定制等离子体响应的纳米天线直接激光制造的可扩展性,我们的结果为设计用于各种应用的红外波段器件迈出了重要一步。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93bd/7000696/a1aeb87340a3/41377_2020_247_Fig1_HTML.jpg

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