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Register a new userThe magnetic ordering in the mixed valence compound beta-Na0.33V2O5
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The low-temperature electron spin resonance (ESR) spectra and the static magnetization data obtained for the stoichiometric single crystals of $beta$-Na$_{0.33}$V$_2$O$_5$ indicate that this quasi-one-dimensional mixed valence (V4+/V5+) compound demonstrates at $T_N=22$ K the phase transition into the canted antiferromagnetically ordered state. The spontaneous magnetization of $3.4times 10^{-3}$ $mu_B$ per V$^{4+}$ ion was found to be oriented along the two-fold $b$ axis of the monoclinic structure, the vector of antiferromagnetism is aligned with the $a$ axis and the Dzyaloshinsky vector is parallel to the $c$-axis. The experimental data were successfully described in the frame of the macroscopic spin dynamics and the following values for the macroscopic parameters of the spin system were obtained: the Dzyaloshinsky field $H_D=6$ kOe, the energy gaps of two branches of the spin wave spectrum $Delta_1=48$ GHz and $Delta_2=24$ GHz.
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Fermi liquid theory, the standard theory of metals, has been challenged by a number of observations of anomalous metallic behavior found in the vicinity of a quantum phase transition. The breakdown of the Fermi liquid is accomplished by fine-tuning the material to a quantum critical point using a control parameter such as the magnetic field, pressure, or chemical composition. Our high precision magnetization measurements of the ultrapure f-electron based superconductor {beta}-YbAlB4 demonstrate a scaling of its free energy indicative of zero-field quantum criticality without tuning in a metal. The breakdown of Fermi-liquid behavior takes place in a mixed-valence state, in sharp contrast with other known examples of quantum critical f-electron systems that are magnetic Kondo lattice systems with integral valence.
We present the high-precision magnetization data of the valence fluctuating heavy fermion superconductor $beta$-YbAlB$_4$ in a wide temperature range from 0.02 K to 320 K spanning four orders of magnitude. We made detailed analyses of the $T/B$ scaling of the magnetization, and firmly confirmed the unconventional zero-field quantum criticality (QC) without tuning. We examined other possible scaling relationship such as $T/(B-B_c)^{delta}$ scaling, and confirmed that $delta = 1$ provides the best quality of the fit with an upper bound on the critical magnetic field $vert B_c vert <0.2$~mT. We further discuss the heavy Fermi-liquid component of the magnetization after subtracting the QC component estimated based on the $T/B$ scaling. The temperature dependence of the heavy Fermi-liquid component is found very similar to the magnetization of the polymorph $alpha$-YbAlB$_4$. In addition, the heavy Fermi-liquid component is suppressed in the magnetic field above $sim$ 5 T as in $alpha$-YbAlB$_4$. This was also confirmed by the magnetization measurements up to $sim 50$ T for both $alpha$- and $beta$-YbAlB$_4$. Interestingly, the detailed analyses revealed that the only a part of $f$ electrons participates in the zero-field QC and the heavy fermion behavior. We also present a temperature - magnetic field phase diagram of ybal to illustrate how the characteristic temperature and field scales evolves near the QC.
Here we provide the first clear evidence of Fermi-liquid breakdown in an intermediate valence system. We employ high precision magnetization measurements of the valence fluctuating superconductor beta-YbAlB4 to probe the quantum critical free energy down to temperatures far below the characteristic energy scale of the valence fluctuations. The observed T/B scaling in the magnetization over three decades not only indicates unconventional quantum criticality, but places an upper bound on the critical magnetic field |B_c| < 0.2 mT, a value comparable with the Earths magnetic field and six orders of magnitude smaller than the valence fluctuation scale. This tiny value of the upper bound on B_c, well inside the superconducting dome, raises the fascinating possibility that valence fluctuating beta-YbAlB4 is intrinsically quantum critical, without tuning the magnetic field, pressure, or composition: the first known example of such a phenomenon in a metal.
Recently, a Verwey-type transition in the mixed-valence alkali sesquioxide Cs$_4$O$_6$ was deduced from the charge ordering of molecular peroxide O$_2^{2-}$ and superoxide O$_2^-$ anions accompanied by the structural transformation and a dramatic change in electronic conductivity [Adler et al, Sci. Adv 4, eaap7581 (2018)]. Here, we report that in the sister compound Rb$_4$O$_6$ a similar Verwey-type charge ordering transition is strongly linked to O$_2^-$ orbital and spin dynamics. On cooling, a powder neutron diffraction experiment reveals a charge ordering and a cubic-to-tetragonal transition at $T_{rm CO}=290$ K, which is followed by a further structural instability at $T_{rm s}=92$ K that involves an additional reorientation of magnetic O$_2^-$ anions. Magnetic resonance techniques supported by density functional theory computations suggest the emergence of a peculiar type of $pi^*$-orbital ordering of the magnetically active O$_2^-$ units, which promotes the formation of a quantum spin state composed of weakly coupled spin dimers. These results reveal that similarly as in 3$d$ transition metal compounds, also in in the $pi^*$ open-shell alkali sesquioxides the interplay between Jahn-Teller-like electron-lattice coupling and Kugel-Khomskii-type superexchange determines the nature of orbital ordering and the magnetic ground state.
The intermediate valent systems TmSe and SmB6 have been investigated up to 16 and 18 GPa by ac microcalorimetry with a pressure (p) tuning realized in situ at low temperature. For TmSe, the transition from an antiferromagnetic insulator for p<3 GPa to an antiferromagnetic metal at higher pressure has been confirmed. A drastic change in the p variation of the Neel temperature (Tn) is observed at 3 GPa. In the metallic phase (p>3 GPa), Tn is found to increase linearly with p. A similar linear p increase of Tn is observed for the quasitrivalent compound TmS which is at ambiant pressure equivalent to TmSe at p=7 GPa. In the case of SmB6 long range magnetism has been detected above p=8 GPa, i.e. at a pressure slightly higher than the pressure of the insulator to metal transition. However a homogeneous magnetic phase occurs only above 10 GPa. The magnetic and electronic properties are related to the renormalization of the 4f wavefunction either to the divalent or the trivalent configurations. As observed in SmS, long range magnetism in SmB6 occurs already far below the pressure where a trivalent Sm3+ state will be reached. It seems possible, to describe roughly the physical properties of the intermediate valence equilibrium by assuming formulas for the Kondo lattice temperature depending on the valence configuration. Comparison is also made with the appearance of long range magnetism in cerium and ytterbium heavy fermion compounds.
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