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Register a new userFirst observation of Ce volume collapse in CeN
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Authors
Julian G. Sereni
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On the occasion of the 80th anniversary of the first observation of Ce volume collapse in CeN a remembrance of the implications of that transcendent event is presented, along with a review of the knowledge of Ce physical properties available at that time. Coincident anniversary corresponds to the first proposal for Ce as a mix valence element, motivating to briefly review how the valence instability of Ce was investigated since that time.
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The thermal expansion of the heavy fermion compound CeRh2Si2 has been measured under pressure as a function of temperature using strain gages. A large anomaly associated to the Neel temperature has been detected even above the suspected critical pressure Pc = 1.05 GPa where no indication of antiferromagnetism has been observed in calorimetry experiments sensitive to the entropy change. An unexpected feature is the pressure slowdown of the antiferromagnetic-paramagnetic transition by comparison to the fast pressure collapse predicted for homogeneous first order quantum phase transition with one unique pressure singularity at Pc. A large pressure dependance is observed in the anisotropy of the thermal expansion measured parallel or perpendicular to the c axis of this tetragonal crystal. The Fermi surface reconstruction associated to the first order transition produces quite different pressure response in the transport scattering measured along different crystallographic directions. A brief discussion is made on other examples of first order quantum transitions in strongly correlated electronic systems : MnSi and CeCoIn5.
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 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.
Results of dc magnetization study are presented showing interesting thermomagnetic history effects across the antiferromagnetic to ferromagnetic transition in Ce(Fe$_{0.96}$Al$_{0.04})_2$. Specifically, we observe (i)ZFC/FC irreversibility rising with increasing field; (ii) virgin curve lying outside the envelope M-H curve. We argue that these effects are quite different from the characteristics seen in spin-glasses or in hard ferromagnets; they can be understood as metastabilities associated with a first order magnetic phase transition.
Taking the pseudobinary C15 Laves phase compound Ce(Fe$_{0.96}$Al$_{0.04}$)$_2$ as a paradigm for studying a ferromagnetic to antiferromagnetic phase transition, we present interesting thermomagnetic history effects in magnetotransport as well as magnetisation measurements across this phase transition. A comparison is made with history effects observed across the ferromagnetic to antiferromagnetic transition in R$_{0.5}$Sr$_{0.5}$MnO$_3$ crystals.
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