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Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit.
Light: Science & Applications ( IF 20.6 ) Pub Date : 2020-07-06 , DOI: 10.1038/s41377-020-00347-y
Ankur Sharma 1 , Linglong Zhang 1 , Jonathan O Tollerud 2, 3 , Miheng Dong 1 , Yi Zhu 1 , Robert Halbich 1 , Tobias Vogl 4 , Kun Liang 1, 5 , Hieu T Nguyen 1 , Fan Wang 6 , Shilpa Sanwlani 2, 3 , Stuart K Earl 2, 3 , Daniel Macdonald 1 , Ping Koy Lam 4 , Jeffrey A Davis 2, 3 , Yuerui Lu 1, 3, 4
Affiliation  

Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications. However, most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities, as there are large inhomogeneous broadening and dephasing effects on the transport of excitons in their native states in materials. Here, by confining coherent excitons at the 2D quantum limit, we first observed molecular aggregation-enabled ‘supertransport’ of excitons in atomically thin two-dimensional (2D) organic semiconductors between coherent states, with a measured high effective exciton diffusion coefficient of ~346.9 cm2/s at room temperature. This value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic materials. Without coupling to any optical cavities, the monolayer pentacene sample, a very clean 2D quantum system (~1.2 nm thick) with high crystallinity (J-type aggregation) and minimal interfacial states, showed superradiant emission from Frenkel excitons, which was experimentally confirmed by the temperature-dependent photoluminescence (PL) emission, highly enhanced radiative decay rate, significantly narrowed PL peak width and strongly directional in-plane emission. The coherence in monolayer pentacene samples was observed to be delocalised over ~135 molecules, which is significantly larger than the values (a few molecules) observed for other organic thin films. In addition, the supertransport of excitons in monolayer pentacene samples showed highly anisotropic behaviour. Our results pave the way for the development of future high-speed excitonic circuits, fast OLEDs, and other optoelectronic devices.



中文翻译:


原子薄有机半导体中激子在二维量子极限下的超输运。



相干激子的长距离和快速传输对于高速激子电路和量子计算应用的发展非常重要。然而,大多数相干激子仅在与空腔耦合时在一些低维半导体中观察到,因为激子在材料中的本征态传输存在很大的不均匀展宽和相移效应。在这里,通过将相干激子限制在 2D 量子极限,我们首先观察到原子薄的二维 (2D) 有机半导体中相干态之间激子的分子聚集“超级输运”,测得的高效激子扩散系数约为 346.9室温下 cm 2 /s。该值比其他有机分子聚集体和低维无机材料报道的值高一到几个数量级。在不耦合到任何光学腔的情况下,单层并五苯样品是一种非常干净的二维量子系统(约 1.2 nm 厚),具有高结晶度(J 型聚集)和最小的界面态,显示出来自 Frenkel 激子的超辐射发射,这一点通过实验证实温度依赖性光致发光(PL)发射、高度增强的辐射衰减率、显着变窄的PL峰宽度和强定向面内发射。据观察,单层并五苯样品的相干性在约 135 个分子上离域,这明显大于在其他有机薄膜中观察到的值(几个分子)。此外,单层并五苯样品中激子的超输运表现出高度各向异性行为。 我们的研究结果为未来高速激子电路、快速 OLED 和其他光电器件的发展铺平了道路。

更新日期:2020-07-06
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