No Arabic abstract
An in-depth analysis of valley physics in 2D materials like transition metal dichalcogenides requires the measurement of many material properties as a function of Fermi level position within the electronic band structure. This is normally done by changing the charge carrier density of the 2D material via the gate electric field effect. Here, we show that a comparison of gate-dependent measurements, which were acquired under different measurement conditions can encounter significant problems due to the temporal evolution of the charging of trap states inside the dielectric layer or at its interfaces. The impact of, e.g., the gate sweep direction and the sweep rate on the overall gate dependence gets especially prominent in optical measurements due to photo-excitation of donor and acceptor states. Under such conditions the same nominal gate-voltage may lead to different gate-induced charge carrier densities and, hence, Fermi level positions. We demonstrate that a current flow from or even through the dielectric layer via leakage currents can significantly diminish the gate tunability in optical measurements of 2D materials.
Collective modes of doped two-dimensional crystalline materials, namely graphene, MoS$_2$ and phosphorene, both monolayer and bilayer structures, are explored using the density functional theory simulations together with the random phase approximation. The many-body dielectric functions of the materials are calculated using an {it ab initio} based model involving material-realistic physical properties. Having calculated the electron energy-loss, we calculate the collective modes of each material considering the in-phase and out-of-phase modes for bilayer structures. Furthermore, owing to many band structures and intreband transitions, we also find high-energy excitations in the systems. We explain that the material-specific dielectric function considering the polarizability of the crystalline material such as MoS$_2$ are needed to obtain realistic plasmon dispersions. For each material studied here, we find different collective modes and describe their physical origins.
We calculate the temperature dependent conductivity of graphene in the presence of randomly distributed Coulomb impurity charges arising from the temperature dependent screening of the Coulomb disorder without any phonons. The purely electronic temperature dependence of our theory arises from two independent mechanisms: the explicit temperature dependence of the finite temperature dielectric function $epsilon(q,T)$ and the finite temperature energy averaging of the transport scattering time. We find that the calculated temperature dependent conductivity is non-monotonic, decreasing with temperature at low temperatures, and increasing at high temperatures. We provide a critical comparison with the corresponding physics in semiconductor-based parabolic band 2D electron gas systems.
Reliable and precise measurements of the relative energy of band edges in semiconductors are needed to determine band gaps and band offsets, as well as to establish the band diagram of devices and heterostructures. These measurements are particularly important in the field of two-dimensional materials, in which many new semiconducting systems are becoming available through exfoliation of bulk crystals. For two-dimensional semiconductors, however, commonly employed techniques suffer from difficulties rooted either in the physics of these systems, or of technical nature. The very large exciton binding energy, for instance, prevents the band gap to be determined from a simple spectral analysis of photoluminescence, and the limited lateral size of atomically thin crystals makes the use of conventional scanning tunneling spectroscopy cumbersome. Ionic gate spectroscopy is a newly developed technique that exploits ionic gate field-effect transistors to determine quantitatively the relative alignment of band edges of two-dimensional semiconductors in a straightforward way, directly from transport measurements (i.e., from the transistor electrical characteristics). The technique relies on the extremely large geometrical capacitance of ionic gated devices that -- under suitable conditions -- enables a change in gate voltage to be directly related to a shift in chemical potential. Here we present an overview of ionic gate spectroscopy, and illustrate its relevance with applications to different two-dimensional semiconducting transition metal dichalcogenides and van der Waals heterostructures.
We examine the static non-linear optical response of monolayer transition metal dichalcogenides. Whereas the shift current is suppressed, we identify a strong, valley-dependent non-reciprocal response, which we term a textit{unidirectional valley-contrasting photo-current} (UVCP). It originates from Kramers symmetry breaking by trigonal warping, and its direction is set by the wave vector connecting the two valleys. The UVCP is proportional to the mobility and is enhanced by the excitonic Coulomb interaction and inter-valley scattering, enabling monitoring of inter-valley transitions. We discuss detection strategies in state-of-the-art experiments.
Through a combined theoretical and experimental effort, we uncover a yet unidentified mechanism that strengthens considerably electron-phonon coupling in materials where electron accumulation leads to population of multiple valleys. Taking atomically-thin transition-metal dichalcogenides as prototypical examples, we establish that the mechanism results from a phonon-induced out-of-phase energy shift of the different valleys, which causes inter-valley charge transfer and reduces the effectiveness of electrostatic screening, thus enhancing electron-phonon interactions. The effect is physically robust, it can play a role in many materials and phenomena, as we illustrate by discussing experimental evidence for its relevance in the occurrence of superconductivity. (short abstract due to size limitations - full abstract in the manuscript)