arXivDaily arXiv每日学术速递 周一至周五更新
arXiv 2103.16753cond-mat.mtrl-sciphysics.chem-ph
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二维范德瓦尔斯空间中化学和几何控制的界面扩散和氧化还原的光学成像

Optical Imaging of Chemically and Geometrically Controlled Interfacial Diffusion and Redox in 2D van der Waals Space

Haneul Kang, Sunmin Ryu

摘要:

在受限空间中发生的分子运动和化学反应在许多催化和能量存储应用中起着关键作用。然而,由于探测困难和缺乏可靠的模型系统,对它的理解一直受到阻碍。在这项工作中,我们报告的几何和化学操纵O2扩散和随后的O2介导的电荷转移(CT)发生在单层过渡金属二硫属化物(TMD)和介电基板之间的二维空间。作为一个敏感的实时宽视场成像信号,电荷密度依赖的光致发光(PL)从TMD被使用。通过增加界面间隙或引入人工缺陷作为CT反应中心,可以大大加速诱导时空PL变化的两个连续过程。我们还表明,广泛变化的CT动力学的四个TMD的速率决定的反应所需的水化程度。报道的发现将有助于设计新的功能纳米结构和设备。

英文摘要:

Molecular motions and chemical reactions occurring in constrained space play key roles in many catalysis and energy storage applications. However, its understanding has been impeded by difficulty in detection and lack of reliable model systems. In this work, we report geometric and chemical manipulation of O2 diffusion and ensuing O2-mediated charge transfer (CT) that occur in the 2D space between single-layer transition metal dichalcogenides (TMDs) and dielectric substrates. As a sensitive real-time wide-field imaging signal, charge-density-dependent photoluminescence (PL) from TMDs was used. The two sequential processes inducing spatiotemporal PL change could be drastically accelerated by increasing the interfacial gap size or introducing artificial defects serving as CT reaction centers. We also show that widely varying CT kinetics of four TMDs are rate-determined by the degree of hydration required for the reactions. The reported findings will be instrumental in designing novel functional nanostructures and devices.

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