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Register a new userObservation of orbital order in the Van der Waals material 1T-TiSe2
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Besides magnetic and charge order, regular arrangements of orbital occupation constitute a fundamental order parameter of condensed matter physics. Even though orbital order is difficult to identify directly in experiments, its presence was firmly established in a number of strongly correlated, three-dimensional Mott insulators. Here, reporting resonant X-ray scattering experiments on the layered Van der Waals compound $1T$-TiSe$_2$, we establish the emergence of orbital order in a weakly correlated, quasi-two-dimensional material. Our experimental scattering results are consistent with first-principles calculations that bring to the fore a generic mechanism of close interplay between charge redistribution, lattice displacements, and orbital order. It demonstrates the essential role that orbital degrees of freedom play in TiSe$_2$, and their importance throughout the family of correlated Van der Waals materials.
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CeTe3 is a unique platform to investigate the itinerant magnetism in a van der Waals (vdW) coupled metal. Despite chemical pressure being a promising route to boost quantum fluctuation in this system, a systematic study on the chemical pressure effect on Ce3+(4f1) states is absent. Here, we report on the successful growth of a series of Se doped single crystals of CeTe3. We found a fluctuation driven exotic magnetic rotation from the usual easy-axis ordering to an unusual hard-axis ordering. Unlike in localized magnetic systems, near-critical magnetism can increase itinerancy hand-in-hand with enhancing fluctuation of magnetism. Thus, seemingly unstable hard-axis ordering emerges through kinetic energy gain, with the self-consistent observation of enhanced magnetic fluctuation (disorder). As far as we recognize, this order-by-disorder process in fermionic system is observed for the first time within vdW materials. Our finding opens a unique experimental platform for direct visualization of the rich quasiparticle Fermi surface deformation associated with the Fermionic order-by-disorder process. Also, the search for emergent exotic phases by further tuning of quantum fluctuation is suggested as a promising future challenge.
Van der Waals heterostructures (VDWHs) exhibit rich properties and thus has potential for applications, and charge transfer between different layers in a heterostructure often dominates its properties and device performance. It is thus critical to reveal and understand the charge transfer effects in VDWHs, for which electronic structure measurements have proven to be effective. Using angle-resolved photoemission spectroscopy, we studied the electronic structures of (PbSe)1.16(TiSe2)m(m=1, 2), which are naturally occurring VDWHs, and discovered several striking charge transfer effects. When the thickness of the TiSe2 layers is halved from m=2 to m=1, the amount of charge transferred increases unexpectedly by more than 250%. This is accompanied by a dramatic drop in the electron-phonon interaction strength far beyond the prediction by first-principles calculations and, consequently, superconductivity only exists in the m=2 compound with strong electron-phonon interaction, albeit with lower carrier density. Furthermore, we found that the amount of charge transferred in both compounds is nearly halved when warmed from below 10 K to room temperature, due to the different thermal expansion coefficients of the constituent layers of these misfit compounds. These unprecedentedly large charge transfer effects might widely exist in VDWHs composed of metal-semiconductor contacts; thus, our results provide important insights for further understanding and applications of VDWHs.
Layered van-der-Waals 2D magnetic materials are of great interest in fundamental condensed-matter physics research, as well as for potential applications in spintronics and device physics. We present neutron powder diffraction data using new ultra-high-pressure techniques to measure the magnetic structure of Mott-insulating 2D honeycomb antiferromagnet FePS$_3$ at pressures up to 183 kbar and temperatures down to 80 K. These data are complemented by high-pressure magnetometry and reverse Monte Carlo modeling of the spin configurations. As pressure is applied, the previously-measured ambient-pressure magnetic order switches from an antiferromagnetic to a ferromagnetic interplanar interaction, and from 2D-like to 3D-like character. The overall antiferromagnetic structure within the $ab$ planes, ferromagnetic chains antiferromagnetically coupled, is preserved, but the magnetic propagation vector is altered from $(0:1:frac{1}{2})$ to $(0:1:0)$, a halving of the magnetic unit cell size. At higher pressures, coincident with the second structural transition and the insulator-metal transition in this compound, we observe a suppression of this long-range-order and emergence of a form of magnetic short-range order which survives above room temperature. Reverse Monte Carlo fitting suggests this phase to be a short-ranged version of the original ambient pressure structure - with a return to antiferromagnetic interplanar correlations. The persistence of magnetism well into the HP-II metallic state is an observation in seeming contradiction with previous x-ray spectroscopy results which suggest a spin-crossover transition.
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