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Register a new userUltrafast doublon dynamics in photo-excited 1T-TaS$_2$
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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.
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Employing time-resolved photoelectron spectroscopy we analyze the relaxation dynamics of hot electrons in the charge density wave / Mott material 1T-TaS_2. At 1.2 eV above the Fermi level we observe a hot electron lifetime of 12 +- 5 fs in the metallic state and of 60 +- 10 fs in the broken symmetry ground state - a direct consequence of the reduced phase space for electron-electron scattering determined by the Mott gap. Boltzmann equation calculations which account for the interaction of hot electrons in a Bloch band with a doublon-holon excitation in the Mott state provide insight into the unoccupied electronic structure in the correlated state.
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.
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.
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$_2$ undergoes successive phase transitions upon cooling and eventually enters an insulating state of mysterious origin. Some consider this state to be a band insulator with interlayer stacking order, yet others attribute it to Mott physics that support a quantum spin liquid state.Here, we determine the electronic and structural properties of 1T-TaS$_2$ using angle-resolved photoemission spectroscopy and X-Ray diffraction. At low temperatures, the 2$pi$/2c-periodic band dispersion, along with half-integer-indexed diffraction peaks along the c axis, unambiguously indicates that the ground state of 1T-TaS$_2$ is a band insulator with interlayer dimerization. Upon heating, however, the system undergoes a transition into a Mott insulating state, which only exists in a narrow temperature window. Our results refute the idea of searching for quantum magnetism in 1T-TaS$_2$ only at low temperatures, and highlight the competition between on-site Coulomb repulsion and interlayer hopping as a crucial aspect for understanding the materials electronic properties.
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