No Arabic abstract
Negative thermal expansion is an unusual phenomenon appearing in only a handful of materials, but pursuit and mastery of the phenomenon holds great promise for applications across disciplines and industries. Here we report use of X-ray spectroscopy and diffraction to investigate the 4f-electronic properties in Y-doped SmS and employ the Kondo volume collapse model to interpret the results. Our measurements reveal an unparalleled decrease of the bulk Sm valence by over 20% at low temperatures in the mixed-valent golden phase, which we show is caused by a strong coupling between an emergent Kondo lattice state and a large isotropic volume change. The amplitude and temperature range of the negative thermal expansion appear strongly dependent on the Y concentration and the associated chemical disorder, providing control over the observed effect. This finding opens new avenues for the design of Kondo lattice materials with tunable, giant and isotropic negative thermal expansion.
Perovskite structured materials contain myriad tunable ordered phases of electronic and magnetic origin with proven technological importance and strong promise for a variety of energy solutions. An always-contributing influence beneath these cooperative and competing interactions is the lattice, whose physics may be obscured in complex perovskites by the many coupled degrees of freedom which makes these systems interesting. Here we report signatures of an approach to a quantum phase transition very near the ground state of the nonmagnetic, ionic insulating, simple cubic perovskite material ScF3 and show that its physical properties are strongly effected as much as 100 K above the putative transition. Spatial and temporal correlations in the high-symmetry cubic phase determined using energy- and momentum-resolved inelastic X-ray scattering as well as X-ray diffraction reveal that soft mode, central peak and thermal expansion phenomena are all strongly influenced by the transition.
The failed Kondo insulator CeNiSn has long been suspected to be a nodal metal, with a node in the hybridization matrix elements. Here we carry out a series of Nernst effect experiments to delineate whether the severely anisotropic magnetotransport coefficients do indeed derive from a nodal metal or can simply be explained by a highly anisotropic Fermi surface. Our experiments reveal that despite an almost 20-fold anisotropy in the Hall conductivity, the large Nernst signal is isotropic. Taken in conjunction with the magnetotransport anisotropy, these results provide strong support for an isotropic Fermi surface with a large anisotropy in quasiparticle mass derived from a nodal hybridization.
We theoretically propose possible magnetism-induced negative thermal expansion in honeycomb-lattice antiferromagnets with edge-sharing networks of $MX_6$ octahedra where $M$ and $X$ are transition-metal and ligand ions, respectively. In this crystal structure, the nearest-neighbor exchange interaction is composed of two competing contributions, i.e., the antiferromagnetic contribution from a direct 180$^circ$ $M$-$M$ bond and the ferromagnetic contribution from 90$^circ$ $M$-$X$-$M$ bonds, amplitudes of which have different bond-length dependence. Numerical analysis of the spin-lattice model of the honeycomb-lattice antiferromagnets demonstrates that the negative thermal expansion can occur when the system enters the antiferromagnetic phase with lowering temperature so as to maximize the energy gain associated with the bond-length dependent antiferromagnetic exchange interaction. The present work provides a guiding principle for searching new materials and eventually contributes to diversify the family of materials that host the negative thermal expansion originating from the spin-lattice coupling on the honeycomb lattices or related crystal structures.
Materials with negative thermal expansion (NTE), which contract upon heating, are of great interest both technically and fundamentally. Here, we report giant NTE covering room temperature in mechanically milled antiperovksite GaNxMn3 compounds. The micrograin GaNxMn3 exhibits a large volume contraction at the antiferromagnetic (AFM) to paramagnetic (PM) (AFM-PM) transition within a temperature window ({Delta}T) of only a few kelvins. The grain size reduces to ~ 30 nm after slight milling, while {Delta}T is broadened to 50K. The corresponding coefficient of linear thermal expansion ({alpha}) reaches ~ -70 ppm/K, which is almost two times larger than those obtained in chemically doped antiperovskite compounds. Further reducing grain size to ~ 10 nm, {Delta}T exceeds 100 K and {alpha} remains as large as -30 ppm/K (-21 ppm/K) for x = 1.0 (x = 0.9). Excess atomic displacements together with the reduced structural coherence, revealed by high-energy X-ray pair distribution functions, are suggested to delay the AFM-PM transition. By controlling the grain size via mechanically alloying or grinding, giant NTE may also be achievable in other materials with large lattice contraction due to electronic or magnetic phase transitions.
Recent experiments have examined the impact of a magnetic field on ferroquadrupolar orders in the intermetallic Kondo material PrTi$_2$Al$_{20}$. Motivated by this, we use extensive Monte Carlo simulations to study a diamond lattice XY model of non-Kramers pseudospin-$1/2$ Pr$^{3+}$ moments which crucially incorporates three-spin interactions. This model supports a thermal $Z_3$ Potts ordering transition upon cooling from the paramagnetic phase into the ferroquadrupolar phase. An applied magnetic field along the [110] direction leads to a thermal Ising transition out of the quadrupolar ordered phase. A magnetic field along the [001] direction leads to only thermal crossovers, but supports a spinodal transition out of metastable domains which could be strongly pinned by coupling to elastic lattice deformations. We propose noise measurements as a potential probe to hear the spinodal transition. Our work highlights the importance of multispin interactions in Kondo materials near the small-to-large Fermi surface transition.