Spatially inhomogeneous electronic states are expected to be key ingredients for the emergence of superconducting phases in quantum materials hosting charge-density-waves (CDWs). Prototypical materials are transition-metal dichalcogenides (TMDCs) and among them, 1$T$-TiSe$_2$ exhibiting intertwined CDW and superconducting states under Cu intercalation, pressure or electrical gating. Although it has been recently proposed that the emergence of superconductivity relates to CDW fluctuations and the development of spatial inhomogeneities in the CDW order, the fundamental mechanism underlying such a phase separation (PS) is still missing. Using angle-resolved photoemission spectroscopy and variable-temperature scanning tunneling microscopy, we report on the phase diagram of the CDW in 1$T$-TiSe$_2$ as a function of Ti self-doping, an overlooked degree of freedom inducing CDW texturing. We find an intrinsic tendency towards electronic PS in the vicinity of Fermi surface (FS) hot spots, i.e. locations with band crossings close to, but not at the Fermi level. We therefore demonstrate an intimate relationship between the FS topology and the emergence of spatially textured electronic phases which is expected to be generalizable to many doped CDW compounds.
We study the evolution of the band gap structure in few-layer MoTe2 crystals, by means of low-temperature microreflectance (MR) and temperature-dependent photoluminescence (PL) measurements. The analysis of the measurements indicate that in complete analogy with other semiconducting transition metal dichalchogenides (TMDs) the dominant PL emission peaks originate from direct transitions associated with recombination of excitons and trions. When we follow the evolution of the PL intensity as a function of layer thickness, however, we observe that MoTe2 behaves differently from other semiconducting TMDs investigated earlier. Specifically, the exciton PL yield (integrated PL intensity) is identical for mono and bilayer, decreases slightly for trilayer, and it is significantly lower in the tetralayer. The analysis of this behavior and of all our experimental observations is fully consistent with mono and bilayer MoTe2 being direct band gap semiconductors with tetralayer MoTe2 being an indirect gap semiconductor and with trilayers having nearly identical direct and indirect gaps. This conclusion is different from the one reached for other recently investigated semiconducting transition metal dichalcogenides for which monolayers are found to be direct band gap semiconductors, and thicker layers have indirect band gaps that are significantly smaller (by hundreds of meV) than the direct gap. We discuss the relevance of our findings for experiments of fundamental interest and possible future device applications.
Semiconducting transition metal dichalcogenides (TMDs) have emerged as materials that can be used to realize two-dimensional (2D) crystals possessing rather unique transport and optical properties. Most research has so far focused on sulfur and selenium compounds, while tellurium-based materials attracted little attention so far. As a first step in the investigation of Te-based semiconducting TMDs in this context, we have studied MoTe$_2$ crystals with thicknesses above 4 nm, focusing on surface transport and a quantitative determination of the gap structure. Using ionic-liquid gated transistors, we show that ambipolar transport at the surface of the material is reproducibly achieved, with hole and electron mobility values between 10 and 30 cm$^2$/Vs at room temperature. The gap structure is determined through three different techniques: ionic-liquid gated transistors and scanning tunneling spectroscopy, that allow the measurement of the indirect gap ($E_{ind}$), and optical transmission spectroscopy on crystals of different thickness, that enables the determination of both the direct ($E_{dir}$) and the indirect gap. We find that at room temperature $E_{ind}$ = 0.88 eV and $E_{dir}$ = 1.02 eV. Our results suggest that thin MoTe$_2$ layers may exhibit a transition to a direct gap before mono-layer thickness. They should also drastically extend the range of direct gaps accessible in 2D semiconducting TMDs.
We study the detailed temperature and composition dependence of the resistivity, rho(T), and thermopower, S(T), for a series of layered bismuth chalcogenides Bi2Te3-xSex, and report the stoichiometry dependence of the optical band gap. In the resistivity of the most compensated member, Bi2Te2.1Se0.9, we find a low-temperature plateau whose onset temperature correlates with the high-temperature activation energy. For the whole series S(T) can be described by a simple model for an extrinsic semiconductor. By substituting Se for Te, the Fermi level is tuned from the valence band into the conduction band. The maximum values of S(T), bulk band gap as well the activation energy in the resistivity are found for x approximate to 0.9. Copyright (C) EPLA, 2014
We study the temperature and composition dependence of the resistivity, (T ), and thermopower, S(T ), for a series of layered bismuth chalcogenides Bi2Te3 xSex. S(T ) can be semi-quantitatively described by a simple model for an extrinsic semiconductor. By substituting Se for Te, the Fermi level is tuned from the valence band into the conduction band. The maximum values of S(T ), bulk band gap as well the activation energy are found for x 0:9, where the low-temperature transport is dominated by the metallic surface states.
Single crystals of Mo and Ta dichalcogenides, MX2 (M = Mo, Ta and X = S, Se, Te), have been grown by the vapor transport method in closed atmosphere, using a novel transport reaction that involves a mixture of M, MCl5 and X as a source. The most important parameters that must be kept under control for succeeding in crystal growth are the temperature, which depends mainly on X, and the initial M:MCl5 ratio. The best growth temperature is found to be the highest in the case of tellurides, the lowest in the case of sulfides and intermediate for the selenides. The optimal M:MCl5 molar ratio decreases with the atomic number of the chalcogen, ranging from 50 for sulfides to 15 for tellurides. Values out of this range made it not possible to control the nucleation process. The high quality of the crystals grown by using this method is confirmed by X-ray diffraction studies, Raman spectroscopy and electrical resistivity measurements, and proved to be higher than that of commercially available MoS2 crystals In the case of TaS2 and TaSe2, using a high starting chloride fraction and a low reaction temperature, the growth of thin (similar to mu m) and long (similar to mm) whiskers is observed An explanation of their growth mechanism is proposed.
We study the detailed temperature and composition dependence of the resistivity, $\rho(T)$, and thermopower, $S(T)$, for a series of layered bismuth chalcogenides Bi$_2$Te$_{3-x}$Se$_x$, and report the stoichiometry dependence of the optical band gap. In the resistivity of the most compensated member, Bi$_2$Te$_{2.1}$Se$_{0.9}$, we find a low-temperature plateau whose onset temperature correlates with the high-temperature activation energy. For the whole series $S(T)$ can be described by a simple model for an extrinsic semiconductor. By substituting Se for Te, the Fermi level is tuned from the valence band into the conduction band. The maximum values of $S(T)$, bulk band gap as well the activation energy in the resistivity are found for $x \approx 0.9$.
The temperature dependence of the complex optical properties of the three-dimensional topological insulator Bi2Te2Se is reported for light polarized in the a-b planes at ambient pressure, as well as the effects of pressure at room temperature. This material displays a semiconducting character with a bulk optical gap of 300 meV at 295 K. In addition to the two expected infrared-active vibrations observed in the planes, there is additional fine structure that is attributed to either the removal of degeneracy or the activation of Raman modes due to disorder. A strong impurity band located at 200 cm^{-1} is also observed. At and just above the optical gap, several interband absorptions are found to show a strong temperature and pressure dependence. As the temperature is lowered these features increase in strength and harden. The application of pressure leads to a very abrupt closing of the gap above 8 GPa, and strongly modifies the interband absorptions in the mid-infrared spectral range. While ab initio calculations fail to predict the collapse of the gap, they do successfully describe the size of the band gap at ambient pressure, and the magnitude and shape of the optical conductivity.
Three-dimensional topological insulators are characterized by the presence of a bandgap in their bulk and gapless Dirac fermions at their surfaces. New physical phenomena originating from the presence of the Dirac fermions are predicted to occur, and to be experimentally accessible via transport measurements in suitably designed electronic devices. Here we study transport through superconducting junctions fabricated on thin Bi(2)Se(3) single crystals, equipped with a gate electrode. In the presence of perpendicular magnetic field B, sweeping the gate voltage enables us to observe the filling of the Dirac fermion Landau levels, whose character evolves continuously from electron- to hole-like. When B=0, a supercurrent appears, whose magnitude can be gate tuned, and is minimum at the charge neutrality point determined from the Landau level filling. Our results demonstrate how gated nano-electronic devices give control over normal and superconducting transport of Dirac fermions at an individual surface of a three-dimensional topological insulators.