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Register a new userPossible glass-like random singlet magnetic state in 1T-TaS2
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Two-dimensional layered transition-metal-dichalcogenide compound 1T-TaS2 shows the rare coexistence of charge density wave (CDW) and electron correlation driven Mott transition. In addition, atomic-cluster spins on the triangular lattice of the CDW state of 1T-TaS2 give rise to the possibility of the exotic spin-singlet state in which quantum fluctuations of spins are strong enough to prevent any long range magnetic ordering down to absolute zero ( 0 K). We present here the evidences of a glass-like random singlet magnetic state in 1T-TaS2 at low temperatures through a study of temperature and time dependence of magnetization. Comparing the experimental results with a representative canonical spin-glass system Au(1.8%Mn), we show that this glass-like state is distinctly different from the well established canonical spin-glass state.
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Photo-induced switching between collective quantum states of matter is a fascinating rising field with exciting opportunities for novel technologies. Presently very intensively studied examples in this regard are nanometer-thick single crystals of the layered material 1T-TaS2 , where picosecond laser pulses can trigger a fully reversible insulator-to-metal transition (IMT). This IMT is believed to be connected to the switching between metastable collective quantum states, but the microscopic nature of this so-called hidden quantum state remained largely elusive up to now. Here we determine the latter by means of state-of-the-art x-ray diffraction and show that the laser-driven IMT involves a marked rearrangement of the charge and orbital order in the direction perpendicular to the TaS2-layers. More specifically, we identify the collapse of inter-layer molecular orbital dimers, which are a characteristic feature of the insulating phase, as a key mechanism for the non-thermal IMT in 1T-TaS2, which indeed involves a collective transition between two truly long-range ordered electronic crystals.
The transient optical conductivity of photoexcited 1T-TaS2 is determined over a three-order-of-magnitude frequency range. Prompt collapse and recovery of the Mott gap is observed. However, we find important differences between this transient metallic state and that seen across the thermally-driven insulator-metal transition. Suppressed low-frequency conductivity, Fano phonon lineshapes, and a mid-infrared absorption band point to polaronic transport. This is explained by noting that the photo-induced metallic state of 1T-TaS2 is one in which the Mott gap is melted but the lattice retains its low-temperature symmetry, a regime only accessible by photo-doping.
We investigate the thermal and transport properties of CexLa1-xRu2Al10 to clarify the origin of the recently discovered mysterious phase below T0=27 K in CeRu2Al10 where a large magnetic entropy is released, however, the existence of an internal magnetic field is ruled out by 27Al-NQR measurement. We find that T0 decreases with decreasing x and disappears at x~0.45. T0 of CeRu2Al10 is suppressed down to 26 K under H=14.5 T along the a-axis. These results clearly indicate that the transition has a magnetic origin and is ascribed to the interaction between Ce ions. Considering the results of specific heat, magnetic susceptibility, thermal expansion, and electrical resistivity and also 27Al NQR, we propose that the transition originates from the singlet pair formation between Ce ions. Although its properties in a Ce dilute region is basically understood by the impurity Kondo effect, CeRu2Al10 shows a Kondo-semiconductor-like behavior. The phase transition at T0 may be characterized as a new type of phase transition that appears during the crossover from the dilute Kondo to the Kondo semiconductor.
Metallization of 1T-TaS2 is generally initiated at the domain boundary of charge density wave (CDW), at the expense of its long-range order. However, we demonstrate in this study that the metallization of 1T-TaS2 can be also realized without breaking the long-range CDW order upon surface alkali doping. By using scanning tunneling microscopy, we find the long-range CDW order is always persisting, and the metallization is instead associated with additional in-gap excitations. Interestingly, the in-gap excitation is near the top of the lower Hubbard band, in contrast to a conventional electron-doped Mott insulator where it is beneath the upper Hubbard band. In combination with the numerical calculations, we suggest that the appearance of the in-gap excitations near the lower Hubbard band is mainly due to the effectively reduced on-site Coulomb energy by the adsorbed alkali ions.
The lattice thermodynamics of a 1T-TaS2 layer, e.g. the spontaneous formation of a sqrt13*sqrt13 commensurate charge density wave (CCDW) and vibrations around the equilibrium position, is calculated by ab initio molecular dynamics. Based on that, we examine how the ground-state electronic structure is renormalized by lattice temperature. We show that the band gap within the density functional theory plus onsite-U correction shrinks by half when the temperature raises from 0 K to 200 K. The gap size reduction is one order of magnitude larger than the temperature variation in energy. This giant temperature dependence is closely related to the CCDW-triggered Mottness in 1T-TaS2, and is expected to result in unconventional thermodynamic properties.
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