Bredesen Center for Interdisciplinary and Graduate Education, University of Tennessee , Knoxville, Tennessee 37996, United States.
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory , Oak Ridge, Tennessee 37831, United States.
J Am Chem Soc. 2017 Oct 11;139(40):14090-14097. doi: 10.1021/jacs.7b04865. Epub 2017 Sep 26.
Most studied two-dimensional (2D) materials exhibit isotropic behavior due to high lattice symmetry; however, lower-symmetry 2D materials such as phosphorene and other elemental 2D materials exhibit very interesting anisotropic properties. In this work, we report the atomic structure, electronic properties, and vibrational modes of few-layered PdSe exfoliated from bulk crystals, a pentagonal 2D layered noble transition metal dichalcogenide with a puckered morphology that is air-stable. Micro-absorption optical spectroscopy and first-principles calculations reveal a wide band gap variation in this material from 0 (bulk) to 1.3 eV (monolayer). The Raman-active vibrational modes of PdSe were identified using polarized Raman spectroscopy, and a strong interlayer interaction was revealed from large, thickness-dependent Raman peak shifts, agreeing with first-principles Raman simulations. Field-effect transistors made from the few-layer PdSe display tunable ambipolar charge carrier conduction with a high electron field-effect mobility of ∼158 cm V s, indicating the promise of this anisotropic, air-stable, pentagonal 2D material for 2D electronics.
大多数经过研究的二维(2D)材料由于晶格对称性高而表现出各向同性行为;然而,较低对称性的 2D 材料,如磷烯和其他元素二维材料,表现出非常有趣的各向异性性质。在这项工作中,我们报告了从体相晶体剥离的少层 PdSe 的原子结构、电子性质和振动模式,这是一种具有褶皱形态的五边形 2D 层状贵金属二卤代物,具有空气稳定性。微吸收光学光谱和第一性原理计算表明,该材料的带隙从 0(体相)到 1.3 eV(单层)变化很大。通过偏振拉曼光谱确定了 PdSe 的拉曼活性振动模式,并且从大的、厚度依赖的拉曼峰位移揭示了强烈的层间相互作用,这与第一性原理拉曼模拟一致。由少层 PdSe 制成的场效应晶体管显示出可调谐的双极性电荷载流子传导,电子场效应迁移率高达约 158 cm V s,表明这种各向异性、空气稳定的五边形 2D 材料在二维电子学中有应用前景。