Department of Materials Science and Engineering, College of Engineering, Peking University, Beijing, 100871, P. R. China.
Center for Nanochemistry (CNC), Beijing Science and Engineering Center for Nanocarbons, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
Adv Mater. 2018 Nov;30(44):e1804616. doi: 10.1002/adma.201804616. Epub 2018 Sep 14.
2D metallic transition metal dichalcogenides (MTMDCs) are benchmark systems for uncovering the dimensionality effect on fascinating quantum physics, such as charge-density-wave (CDW) order, unconventional superconductivity, and magnetism, etc. However, the scalable and thickness-tunable syntheses of such envisioned MTMDCs are still challenging. Meanwhile, the origin of CDW order at the 2D limit is controversial. Herein, the direct synthesis of wafer-scale uniform monolayer 2H-TaSe films and thickness-tunable flakes on Au foils by chemical vapor deposition is accomplished. Based on the thickness-tunable 2H-TaSe, the robust periodic lattice distortions that relate to CDW orders by low-temperature transmission electron microscopy are directly visualized. Particularly, a phase diagram of the transition temperature from normal metallic to CDW phases with thickness by variable-temperature Raman characterizations is established. Intriguingly, dramatically enhanced transition temperature from bulk value ≈90 to ≈125 K is observed from monolayer 2H-TaSe, which can be explained by the enhanced electron-phonon coupling mechanism. More importantly, an ultrahigh specific capacitance is also obtained for the as-grown TaSe on carbon cloth as supercapacitor electrodes. The results hereby open up novel avenues toward the large-scale preparation of high-quality MTMDCs, and shed light on their applications in exploring some fundamental issues.
2D 金属过渡金属二卤族化合物(MTMDCs)是揭示迷人量子物理学中维度效应的基准体系,例如电荷密度波(CDW)有序、非常规超导和磁性等。然而,这种理想的 MTMDCs 的可扩展和厚度可调合成仍然具有挑战性。同时,CDW 有序在 2D 极限下的起源存在争议。在此,通过化学气相沉积直接合成了晶圆级均匀单层 2H-TaSe 薄膜和厚度可调的金箔上的薄片。基于厚度可调的 2H-TaSe,通过低温透射电子显微镜直接可视化了与 CDW 有序相关的稳健周期性晶格畸变。特别是,通过变温拉曼特性建立了从正常金属到 CDW 相的转变温度随厚度变化的相图。有趣的是,从单层 2H-TaSe 观察到从体值 ≈90 到 ≈125 K 的转变温度显著增强,这可以通过增强的电子-声子耦合机制来解释。更重要的是,作为超级电容器电极的在碳布上生长的 TaSe 也获得了超高的比电容。该结果为高质量 MTMDCs 的大规模制备开辟了新途径,并为探索一些基本问题提供了启示。