Department of Physics, University of Michigan, Ann Arbor, MI, 48109, USA.
Applied Physics Program, University of Michigan, Ann Arbor, MI, 48109, USA.
Nat Commun. 2023 Apr 1;14(1):1837. doi: 10.1038/s41467-023-37500-1.
The unique optical properties of transition metal dichalcogenide (TMD) monolayers have attracted significant attention for both photonics applications and fundamental studies of low-dimensional systems. TMD monolayers of high optical quality, however, have been limited to micron-sized flakes produced by low-throughput and labour-intensive processes, whereas large-area films are often affected by surface defects and large inhomogeneity. Here we report a rapid and reliable method to synthesize macroscopic-scale TMD monolayers of uniform, high optical quality. Using 1-dodecanol encapsulation combined with gold-tape-assisted exfoliation, we obtain monolayers with lateral size > 1 mm, exhibiting exciton energy, linewidth, and quantum yield uniform over the whole area and close to those of high-quality micron-sized flakes. We tentatively associate the role of the two molecular encapsulating layers as isolating the TMD from the substrate and passivating the chalcogen vacancies, respectively. We demonstrate the utility of our encapsulated monolayers by scalable integration with an array of photonic crystal cavities, creating polariton arrays with enhanced light-matter coupling strength. This work provides a pathway to achieving high-quality two-dimensional materials over large areas, enabling research and technology development beyond individual micron-sized devices.
过渡金属二卤化物(TMD)单层独特的光学性质引起了人们对光子学应用和低维系统基础研究的极大关注。然而,具有高光学质量的 TMD 单层仅限于通过低通量和劳动密集型工艺生产的微米级薄片,而大面积薄膜通常受到表面缺陷和大的不均匀性的影响。在这里,我们报告了一种快速可靠的方法来合成具有均匀、高光学质量的宏观尺度 TMD 单层。我们使用 1-十二醇封装结合金带辅助剥离,获得了横向尺寸>1mm 的单层,其激子能量、线宽和量子产率在整个区域内均匀,接近高质量微米级薄片的数值。我们初步将这两层分子封装层的作用分别假定为将 TMD 与衬底隔离和钝化硫属空位。我们通过与一系列光子晶体腔的可扩展集成证明了我们封装的单层的实用性,从而创建了具有增强的光物质耦合强度的极化激元阵列。这项工作为在大面积上实现高质量二维材料提供了一条途径,超越了单个微米级器件的研究和技术发展。