Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userDisrupted orbital order and the pseudo-gap in layered 1T-TaS$_2$
53
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
We present a state-of-the-art density functional theory (DFT) study which models crucial features of the partially disordered orbital order stacking in the prototypical layered transition metal dichalcogenide 1T-TaS2 . Our results not only show that DFT models with realistic assumptions about the orbital order perpendicular to the layers yield band structures which agree remarkably well with experiments. They also demonstrate that DFT correctly predicts the formation of an excitation pseudo-gap which is commonly attributed to Mott-Hubbard type electron-electron correlations. These results highlight the importance of interlayer interactions in layered transition metal dichalcogenides and serve as an intriguing example of how disorder within an electronic crystal can give rise to pseudo-gap features.
rate research
Read More
Tuning the electronic properties of a matter is of fundamental interest in scientific research as well as in applications. Recently, the Mott insulator-metal transition has been reported in a pristine layered transition metal dichalcogenides 1T-TaS$_2$, with the transition triggered by an optical excitation, a gate controlled intercalation, or a voltage pulse. However, the sudden insulator-metal transition hinders an exploration of how the transition evolves. Here, we report the strain as a possible new tuning parameter to induce Mott gap collapse in 1T-TaS$_2$. In a strain-rich area, we find a mosaic state with distinct electronic density of states within different domains. In a corrugated surface, we further observe and analyze a smooth evolution from a Mott gap state to a metallic state. Our results shed new lights on the understanding of the insulator-metal transition and promote a controllable strain engineering on the design of switching devices in the future.
New theoretical proposals and experimental findings on transition metal dichalcogenide 1T-TaS$_2$ have revived interests in its possible Mott insulating state. We perform a comprehensive scanning tunneling microscopy and spectroscopy experiment on different single-step areas in pristine 1T-TaS$_2$. After accurately determining the relative displacement of Star-of-David super-lattices in two layers, we find different stacking orders corresponding to the different electronic states measured on the upper terrace. The center-to-center stacking corresponds to the universal large gap, while other stacking orders correspond to a reduced or suppressed gap in the electronic spectrum. Adopting a unified model, we conclude that the universal large gap is a correlation-induced Mott gap from the single-layer property. Our work provides more evidence about the surface electronic state and deepens our understanding of the Mott insulating state in 1T-TaS$_2$.
1T-TaS$_2$ is a layered transition metal dichalgeonide with a very rich phase diagram. At T=180K it undergoes a metal to Mott insulator transition. Mott insulators usually display anti-ferromagnetic ordering in the insulating phase but 1T-TaS$_2$ was never shown to order magnetically. In this letter we show that 1T-TaS$_2$ has a large paramagnetic contribution to the magnetic susceptibility but it does not show any sign of magnetic ordering or freezing down to 20mK, as probed by $mu$SR, possibly indicating a quantum spin liquid ground state. Although 1T-TaS$_2$ exhibits a strong resistive behavior both in and out-of plane at low temperatures we find a linear term in the heat capacity suggesting the existence of a Fermi-surface, which has an anomalously strong magnetic field dependence.
1T-TaS$_2$ is a prototypical charge-density-wave (CDW) system with a Mott insulating ground state. Usually, a Mott insulator is accompanied by an antiferromagnetic state. However, the antiferromagnetic order had never been observed in 1T-TaS$_2$. Here, we report the stabilization of the antiferromagnetic order by the intercalation of a small amount of Fe into the van der Waals gap of 1T-TaS$_2$, i.e. forming 1T-Fe$_{0.05}$TaS$_2$. Upon cooling from 300~K, the electrical resistivity increases with a decreasing temperature before reaching a maximum value at around 15~K, which is close to the Neel temperature determined from our magnetic susceptibility measurement. The antiferromagnetic state can be fully suppressed when the sample thickness is reduced, indicating that the antiferromagnetic order in Fe$_{0.05}$TaS$_2$ has a non-negligible three-dimensional character. For the bulk Fe$_{0.05}$TaS$_2$, a comparison of our high pressure electrical transport data with that of 1T-TaS$_2$ indicates that, at ambient pressure, Fe$_{0.05}$TaS$_2$ is in the nearly commensurate charge-density-wave (NCCDW) phase near the border of the Mott insulating state. The temperature-pressure phase diagram thus reveals an interesting decoupling of the antiferromagnetism from the Mott insulating state.
Strongly correlated systems exhibit intriguing properties caused by intertwined microscopic in- teractions that are hard to disentangle in equilibrium. Employing non-equilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T-TaS$_2$, we identify a spectroscopic signature of double occupied sites (doublons) that are reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on time scales of one electronic hopping cycle $hbar/Japprox$ 14 fs. Despite strong electron-phonon coupling the dynamics can be explained by purely electronic effects captured by the single band Hubbard model, where thermalization is fast in the small-gap regime. Qualitative agreement with the experimental results however requires the assumption of an intrinsic hole-doping. The sensitivity of the doublon dynamics on the doping level provides a way to control ultrafast processes in such strongly correlated materials.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
