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Register a new userDifferent routes to pressure-induced volume collapse transitions in gadolinium and terbium metals
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The sudden decrease in molar volume exhibited by most lanthanides under high pressure is often attributed to changes in the degree of localization of their 4f-electrons. We give evidence, based on electrical resistivity measurements of dilute Y(Gd) and Y(Tb) alloys to 120 GPa, that the volume collapse transitions in Gd and Tb metals have different origins, despite their being neighbors in the periodic table. Remarkably, the change under pressure in the magnetic state of isolated Pr or Tb impurity ions in the nonmagnetic Y host appears to closely mirror corresponding changes in pure Pr or Tb metals. The collapse in Tb appears to be driven by an enhanced negative exchange interaction between 4f and conduction electrons under pressure (Kondo resonance) which, in the case of Y(Tb), dramatically alters the superconducting properties of the Y host, much like previously found for Y(Pr). In Gd our resistivity measurements suggest that a Kondo resonance is not the main driver for its volume collapse. X-ray absorption and emission spectroscopies clearly show that 4f local moments remain largely intact across both volume collapse transitions ruling out 4f band formation (delocalization) and valence transition models as possible drivers. The results highlight the richness of behavior behind the volume collapse transition in lanthanides and demonstrate the stability of the 4f level against band formation to extreme pressure.
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Pressure induced isostructural insulator to metal transition for SmS is characterised by the presence of an intermediate valence state at higher pressure which cannot be captured by the density functional theory. As a direct outcome of including the charge and spin fluctuations incorporated in dynamical mean field theory, we see the emergence of insulating and metallic phases with increasing pressure as a function of changing valence. This is accompanied by significantly improved predictions of the equilibrium lattice constants and bulk moduli for all Sm-monochalcogenides verifying experiments. Nudged Elastic Band analysis reveals the insulating states to have a finite quasiparticle weight, decreasing as the gap closes rendering the transition to be not Mott-like, and classifies these materials as correlated band insulators. The difference between the discontinuous and continuous natures of these transitions can be attributed to the closeness of the sharply resonant Sm-4f peaks to the fermi level in the predicted metallic states in SmS as compared to SmSe and SmTe.
Dramatic volume collapses under pressure are fundamental to geochemistry and of increasing importance to fields as diverse as hydrogen storage and high-temperature superconductivity. In transition metal materials, collapses are usually driven by so-called spin-state transitions, the interplay between the single-ion crystal field and the size of the magnetic moment. Here we show that the classical S=5/2 mineral Hauerite undergoes an unprecedented 22 % collapse driven by a conceptually different magnetic mechanism. Using synchrotron x-ray diffraction we show that cold compression induces the formation of a disordered intermediate. However, using an evolutionary algorithm we predict a new structure with edge-sharing chains. This is confirmed as the thermodynamic groundstate using in situ laser heating. We show that magnetism is globally absent in the new phase, as low-spin quantum S=1/2 moments are quenched by dimerisation. Our results show how the emergence of metal-metal bonding can stabilise giant spin-lattice coupling in Earths minerals.
The possible application of the barocaloric effect to produce solid state refrigerators is a topic of interest in the field of applied physics. In this work, we present experimental data about the influence of external pressure on the magnetic properties of a manganite with phase separation. Using the Jahn Teller effect associated with the presence of the charge ordering we were able to follow the transition to the ferromagnetic state induced by pressure. We also demonstrated that external pressure can assist the ferromagnetic state, decreasing the magnetic field necessary to generate the magnetic transition.
We report a new tetragonal ground-state for perovskite-structured PbCrO3 from DFT+U calculations, and explain its anomalously large volume. The new structure is stabilized due to orbital ordering of Cr-d in the presence of a large tetragonal crystal field, mainly due to off-centering of the Pb atom. At higher pressures (smaller volumes) there is a first-order transition to a cubic phase where the Cr-d orbitals are orbitally liquid. This phase-transition is accompanied by a ~11.5% volume collapse, one of the largest known for transition-metal oxides. The large ferroelasticity and its strong coupling to the orbital degrees of freedom could be exploited to form potentially useful magnetostrictive materials
A quantum critical point is approached by applying pressure in a number of magnetic metals. The observed dependence of Tc on pressure necessarily means that the magnetic energy is coupled to the lattice. A first order phase transition occurs if this coupling exceeds a critical value: this is inevitable if diverges as Tc approaches zero. It is argued that this is the cause of the first order transition that is observed in many systems. Using Landau theory we obtain expressions for the boundaries of the region where phase separation occurs that agree well with experiments done on MnSi and other materials. The theory can be used to obtain very approximate values for the temperature and pressure at the tricritical point in terms of quantities measured at ambient pressure and the measured values of along the second order line. The values of the tricritical temperature for various materials obtained from Landau theory are too low but it is shown that the predicted values will rise if the effects of fluctuations are included.
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