Electronic properties of transition-metal dichalcogenides

Graphene is not the only prominent example of two-dimensional (2D) materials. Due to their interesting combination of high mechanical strength and optical transparency, direct bandgap and atomic scale thickness transition-metal dichalcogenides (TMDCs) are an example of other materials that are now vying for the attention of the materials research community. In this article, the current state of quantum-theoretical calculations of the electronic and mechanical properties of semiconducting TMDC materials are presented. In particular, the intriguing interplay between external parameters (electric field, strain) and band structure, as well as the basic properties of heterostructures formed by vertical stacking of different 2D TMDCs are reviewed. Electrical measurements of MoS2, WS2, and WSe2 and their heterostructures, starting from simple field-effect transistors to more demanding logic circuits, high-frequency transistors, and memory devices, are also presented.

Electronic Transport in 2D Materials with Strong Spin-orbit Coupling

Artem Pulkin

The thesis describes the computational study of structural, electonic and transport properties of monolayer transition metal dichalcogenides (TMDs) in the stable 2H and the metastable 1T' phases. Several aspects have been covered by the study including the electronic properties of the topological quantum spin Hall (QSH) state in the 1T' monolayer phase as well as the effects of strain, periodic line defects, interfaces and edges of monolayer TMDs. The electronic properties of the bulk monolayer phases were described by the ab-initio density functional theory framework while the electronic and transport properties of 1D defects were calculated using the non-equilibrium Green's function formalism. A specific focus was made on the transport of spin-polarized charge carriers across line defects in the monolayer 2H phase. Subject to energy, pseudomomentum and spin conservation, the size of the transport gap is governed by both bulk properties of a material and symmetries of a line defect. Outside the transport gap energy region, the charge carriers are discriminated with respect to their spin resulting in the spin polarization of the transmitted current. Next, the properties of the metastable monolayer 1T' phase were studied. The presence of a sufficiently large band gap is crucial to observe the QSH phase in the family of materials by probing the topological boundary states. The meV-order band gaps of the 1T' phase of monolayer TMDs were found to be sensitive to materials' lattice constants suggesting the control of the band gap size by strain. In particular, the electronic band structure and the size of the band gap in monolayer 1T'-WSe2 were found to be in agreement with spectroscopy studies. The topologically protected states at the edges of the monolayer 1T' phase as well as at the boundaries between the topological 1T' phase and the trivial 2H phase of monolayer TMDs were studied. Specific atomic structure configurations were suggested to observe experimentally the topological protection of the charge carrier transport against back-scattering. Finally, in the context of lateral semiconducting device engineering, the electronic and transverse transport properties of 2H-1T' phase boundaries as well as the dimerization defects in the 1T' phase were investigated. Both kinds of defects considered exhibit a relatively large transmission probability for the charge carriers crossing the defects. However, the differences between the shapes of bulk bands of the two phases open a sizeable transport gap for charge carriers crossing periodic domain boundaries between the monolayer 2H and 1T' phases. The calculated formation energies of dimerization defects were found to be relatively low suggesting their high concentration in real samples of monolayer 1T'-TMDs. Additionally, the thesis includes studies of magnetic dopants on the surface of Bi2Te3 and atomic vacancies in monolayer 2H-MoSe2 where the electronic properties of point defects were calculated and compared to experimental results. The two possible adsorption sites of Fe on the surface of Bi2Te3 both show a large out-of-plane magnetic anisotropy in agreement with experiments. The calculated local electronic properties of Se vacancies in monolayer 2H-MoSe2 show the presence of in-gap states which are not observed in experiment. Nevertheless, the combination of theoretical and experimental scanning tunneling microscopy images allowed the unambiguous identification of the vacancy defect.

EPFL2017

Mobility engineering and a metal–insulator transition in monolayer MoS2

Andras Kis, Branimir Radisavljevic

Two-dimensional (2D) materials are a new class of materials with interesting physical properties and applications ranging from nanoelectronics to sensing and photonics. In addition to graphene, the most studied 2D material, monolayers of other layered materials such as semiconducting dichalcogenides MoS2 or WSe2 are gaining in importance as promising channel materials for field-effect transistors (FETs). The presence of a direct bandgap in monolayer MoS2 due to quantum-mechanical confinement allows room-temperature FETs with an on/off ratio exceeding 10(8). The presence of high-kappa dielectrics in these devices enhanced their mobility, but the mechanisms are not well understood. Here, we report on electrical transport measurements on MoS2 FETs in different dielectric configurations. The dependence of mobility on temperature shows clear evidence of the strong suppression of charged-impurity scattering in dual-gate devices with a top-gate dielectric. At the same time, phonon scattering shows a weaker than expected temperature dependence. High levels of doping achieved in dual-gate devices also allow the observation of a metal-insulator transition in monolayer MoS2 due to strong electron-electron interactions. Our work opens up the way to further improvements in 2D semiconductor performance and introduces MoS2 as an interesting system for studying correlation effects in mesoscopic systems.

Nature Publishing Group2013

Light Generation and Harvesting in a van der Waals Heterostructure

Esther Alarcon Llado, Andras Kis, Volodymyr Koman, Oriol López Sánchez, Aleksandra Radenovic

Two-dimensional (2D) materials are a new type of materials under intense study because of their interesting physical properties and wide range of potential applications from nanoelectronics to sensing and photonics. Monolayers of semiconducting transition metal dichalcogenides MoS2 or WSe2 have been proposed as promising channel materials for field-effect transistors. Their high mechanical flexibility, stability, and quality coupled with potentially inexpensive production methods offer potential advantages compared to organic and crystalline bulk semiconductors. Due to quantum mechanical confinement, the band gap in monolayer MoS2 is direct in nature, leading to a strong interaction with light that can be exploited for building phototransistors and ultrasensitive photodetectors. Here, we report on the realization of light-emitting diodes based on vertical heterojunctions composed of n-type monolayer MoS2 and p-type silicon. Careful interface engineering allows us to realize diodes showing rectification and light emission from the entire surface of the heterojunction. Electroluminescence spectra show clear signs of direct excitons related to the optical transitions between the conduction and valence bands. Our p-n diodes can also operate as solar cells, with typical external quantum efficiency exceeding 4%. Our work opens up the way to more sophisticated optoelectronic devices such as lasers and heterostructure solar cells based on hybrids of 2D semiconductors and silicon.

Amer Chemical Soc2014

Electronic Transport in 2D Materials with Strong Spin-orbit Coupling

Artem Pulkin

EPFL2017