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Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons

机译:通过近场探测原子级薄半导体中的暗激子   耦合到表面等离子体激元

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摘要

Transition metal dichalcogenide (TMD) monolayers are direct bandgapsemiconductors that feature tightly bound excitons, strong spin-orbit coupling,and spin-valley degrees of freedom. Depending on the spin configuration of theelectron-hole pairs, intra-valley excitons of TMD monolayers can be eitheroptically bright or dark. Dark excitons involve nominally spin-forbiddenoptical transitions with zero in-plane transition dipole moment, making theirdetection with conventional far-field optical techniques challenging. Here, weintroduce a new method for probing the optical properties of two-dimensional(2D) materials via near-field coupling to surface plasmon polaritons (SPPs),which selectively enhances optical transitions with dipole moments normal tothe 2D plane. We utilize this method to directly detect dark excitons inmonolayer TMDs. When a WSe2 monolayer is placed on top of a single-crystalsilver film, its emission into near-field-coupled SPPs displays new spectralfeatures whose energies and dipole orientations are consistent with darkneutral and charged excitons. The SPP-based near-field spectroscopysignificantly enhances experimental capabilities for probing and manipulatingexciton dynamics of atomically thin materials.
机译:过渡金属二硫化碳(TMD)单层是直接带隙半导体,具有紧密结合的激子,强自旋轨道耦合和自旋谷自由度。取决于电子-空穴对的自旋构型,TMD单层的谷内激子可以是光学亮的或暗的。暗激子涉及面内跃迁偶极矩为零的名义上自旋-禁光跃迁,因此使用传统远场光学技术进行检测很困难。在这里,我们引入了一种通过与表面等离激元极化子(SPPs)进行近场耦合来探测二维(2D)材料光学特性的新方法,该方法选择性地增强了垂直于2D平面的偶极矩的光学跃迁。我们利用这种方法直接检测单层TMD中的暗激子。当将WSe2单层放置在单晶银膜的顶部时,其发射到近场耦合的SPP中会显示出新的光谱特征,其能量和偶极子方向与暗中性和带电激子一致。基于SPP的近场光谱显着增强了探测和操纵原子薄材料的激子动力学的实验能力。

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