We report on comprehensive results identifying the ground state of a triangular-lattice structured as a spin glass, including no long-range magnetic order, prominent broad excitation continua, and the absence of magnetic thermal conductivity. More crucially, from the ultralow-temperature ac susceptibility measurements, we unambiguously observe frequency-dependent peaks around 0.1 K, indicating the spin-glass ground state. We suggest this conclusion holds also for its sister compound , which is confirmed by the observation of spin freezing at low temperatures. We consider disorder and frustration to be the main driving force for the spin-glass phase.
20 March 2019 in Proceedings of the National Academy of Sciences
Nearly a century of research has established the Born–Oppenheimer approximation as a cornerstone of condensed-matter systems, stating that the motion of the atomic nuclei and electrons may be treated separately. Interactions beyond the Born–Oppenheimer approximation are at the heart of magneto-elastic functionalities and instabilities. We report comprehensive neutron spectroscopy and ab initio phonon calculations of the coupling between phonons, CEF-split localized 4 electron states, and conduction electrons in the paramagnetic regime of , an archetypal Kondo lattice compound. We identify two distinct magneto-elastic hybrid excitations that form even though all coupling constants are small. First, we find a CEF–phonon bound state reminiscent of the vibronic bound state (VBS) observed in other materials. However, in contrast to an abundance of optical phonons, so far believed to be essential for a VBS, the VBS in arises from a comparatively low density of states of acoustic phonons. Second, we find a pronounced anticrossing of the CEF excitations with acoustic phonons at zero magnetic field not observed before. Remarkably, both magneto-elastic excitations are well developed despite considerable damping of the CEFs that arises dominantly by the conduction electrons. Taking together the weak coupling with the simultaneous existence of a distinct VBS and anticrossing in the same material in the presence of damping suggests strongly that similarly well-developed magneto-elastic hybrid excitations must be abundant in a wide range of materials. In turn, our study of the excitation spectra of identifies a tractable point of reference in the search for magneto-elastic functionalities and instabilities.
The results of a single-crystal x-ray-diffraction study of the evolution of the crystal structures of with temperature with an emphasis on phase transitions are presented. Some related specific-heat and magnetization data are included. The existence of the room-temperature trigonal crystal structure (148) has been confirmed. Upon cooling, undergoes a structural phase transition to a monoclinic phase at . is reduced in magnetic fields applied along the trigonal axis. When becomes ferromagnetic at , magnetostriction-induced changes of the monoclinic-structure parameters are observed. Upon further cooling, the monoclinic structure transforms into a triclinic variant at 32 K which is most likely occurring in conjunction with the previously reported transformation of the ferromagnetic structure. The observed phenomena are preliminarily attributed to strong magnetoelastic interactions.
Evolution of magnetism in single crystals of the van der Waals compound in external pressure up to 7.3 GPa studied by measuring magnetization and ac magnetic susceptibility is reported. Four magnetic phase transitions, at , and , respectively, have been observed at ambient pressure. The first two have been attributed to the onset of ferromagnetism in specific crystal-surface layers. The bulk ferromagnetism is characterized by the magnetic ordering transition at Curie temperature and the transition between two different ferromagnetic phases , accompanied by a structure transition from monoclinic to triclinic symmetry upon cooling. The pressure effects on magnetic parameters were studied with three independent techniques. was found to be almost unaffected by pressures up to 0.6 GPa whereas increases rapidly with increasing pressure and reaches at a triple point at ≈ 0.85 GPa. At higher pressures, only one magnetic phase transition is observed moving to higher temperatures with increasing pressure to reach 99 K at 7.3 GPa. In contrast, the low-temperature bulk magnetization is significantly reduced by applying pressure (by more than 50% at 2.5 GPa) suggesting a possible pressure-induced reduction of vanadium magnetic moment. First-principles calculations of under pressure allow us to ascribe the evolution of with pressure to the reduction of interplanar distance, including the observed slope change at 0.6 GPa. These calculations also describe the associated band gap closing, showing that with a modest compression the material would become metallic. Overall, the large pressure range covered corresponds to a significant change of interplanar interactions. The obtained data thus allow us to shed light on how does the transition between the three-dimensional (3D) and quasi-2D system affect magnetic interactions in the system.
19 August 2015 in Journal of large-scale research facilities JLSRF
The cold three axes spectrometer PANDA, operated by JCNS, Forschungszentrum Jülich, offers high neutron flux over a large dynamic range keeping the instrumental background comparably low.