Room-Temperature, Strong Emission of Momentum-Forbidden Interlayer Excitons in Nanocavity-Coupled Twisted van der Waals Heterostructures

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nano Letters Pub Date : 2025-01-08 DOI:10.1021/acs.nanolett.4c05647

Bin Feng, Shixuan Zhao, Ilya Razdolski, Feihong Liu, Zhiwei Peng, Yaorong Wang, Zhedong Zhang, Zhenhua Ni, Jianbin Xu, Dangyuan Lei

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Abstract

The emission efficiency of interlayer excitons (IEs) in twisted 2D heterostructures has long suffered from momentum mismatch, limiting their applications in ultracompact excitonic devices. Here, we report strong room-temperature emission of momentum-forbidden IE in 30°-twisted MoS₂/WS₂ heterobilayers. Utilizing a plasmonic nanocavity, the Purcell effect boosts the IE emission intensity in the cavity by over 2 orders of magnitude. We further study the interplay of this Purcell enhancement and phonon assistance in 30°- and 0°-twisted heterostructures. Temperature-dependent and time-resolved spectroscopy reveal that the IE enhancement in 30°-twisted cases involves competition between IEs and intralayer excitonic emission, which is remarkably distinct from the 0°-twisted cases. We propose a comprehensive exciton decay model capturing the features of the phonon-assisted momentum compensation and the Purcell enhancement of the IE emission, showing consistency with the experimental measurements. Our results enrich the understanding of the nanocavity-assisted light–matter interaction for momentum-indirect excitonic transitions.

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纳米腔耦合扭曲范德华异质结构中动量禁止层间激子的室温强发射

扭曲二维异质结构层间激子（IEs）的发射效率长期存在动量失配问题，限制了其在超紧凑激子器件中的应用。在这里，我们报道了30°扭曲的MoS2/WS2异质层中强烈的室温禁动量IE发射。利用等离子体纳米腔，珀塞尔效应将腔内的IE发射强度提高了2个数量级以上。我们进一步研究了珀塞尔增强和声子辅助在30°和0°扭曲异质结构中的相互作用。温度依赖光谱和时间分辨光谱表明，30°扭转情况下的IE增强涉及IE和层内激子发射之间的竞争，这与0°扭转情况明显不同。我们提出了一个综合的激子衰变模型，该模型捕捉了声子辅助动量补偿和IE发射的Purcell增强的特征，显示了与实验测量的一致性。我们的研究结果丰富了对纳米腔辅助光-物质相互作用在动量间接激子跃迁中的理解。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.