金传洪
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期刊论文
layer-dependent anisotropic electronic structures of freestanding quasi-two-dimensional mos2
phys. rev. b,2016,93(7):075440 | 2016年02月29日 | https://doi.org/10.1103/physrevb.93.075440
the anisotropy of the electronic transition is a well-known characteristic of low-dimensional transition-metal dichalcogenides, but their layer-thickness dependence has not been properly investigated experimentally until now. yet, it not only determines the optical properties of these low-dimensional materials, but also holds the key in revealing the underlying character of the electronic states involved. here we used both angle-resolved electron energy-loss spectroscopy and spectral analysis of angle-integrated spectra to study the evolution of the anisotropic electronic transition involving the low-energy valence electrons in the freestanding mo s 2 layers with different thicknesses. we are able to demonstrate that the well-known direct gap at 1.8 ev is only excited by the in-plane polarized field while the out-of-plane polarized optical gap is 2.4 ± 0.2 ev in monolayer mo s 2 . this contrasts with the much smaller anisotropic response found for the indirect gap in the few-layer mo s 2 systems. in addition, we determined that the joint density of states associated with the indirect gap transition in the multilayer systems and the corresponding indirect transition in the monolayer case has a characteristic three-dimensional-like character. we attribute this to the soft-edge behavior of the confining potential and it is an important factor when considering the dynamical screening of the electric field at the relevant excitation energies. our result provides a logical explanation for the large sensitivity of the indirect transition to thickness variation compared with that for the direct transition, in terms of quantum confinement effect.
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