A. B. Harris, T. Yildirim
Landau theory and symmetry considerations are invoked to give a unified treatment of charge and spin ordering in the mixed valence compound LuFe2O4. In particular, the unusual evolution of charge ordering correlations can be explained by invoking phonon mediated interactions.
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An x-ray diffraction study reveals the charge ordering structure in an intermediate valence magnet YbPd with a CsCl-structure. The valence of the Yb ions forms an incommensurate structure, characterized by the wavevector (+-0.07 +-0.07 1/2) below 130 K. At 105 K, the incommensurate structure turns into a commensurate structure, characterized by the wavevector (0 0 1/2). Based on the resonant x-ray diffraction spectra of the superlattice reflections, the valences of the Yb ions below 105 K are found to be 3+ and 2.6+. The origin of the long wavelength modulation is discussed with the aid of an …
Magnetic susceptibility, heat capacity, and electrical resistivity measurements have been carried out on single crystals of the intermediate valence compounds Yb2Rh3Ga9 and Yb2Ir3Ga9. These measurements reveal a large anisotropy due apparently to an interplay between crystalline electric field (CEF) and Kondo effects. The temperature dependence of magnetic susceptibility can be modelled using the Anderson impurity model including CEF within an approach based on the Non-Crossing Approximation.
The anomalous behavior of YbInCu4 and similar compounds is modeled by the exact solution of the spin one-half Falicov-Kimball model in infinite dimensions. The valence-fluctuating transition is related to a metal-insulator transition caused by the Falicov-Kimball interaction, and triggered by the change in the f-occupancy.
We present experimental results of electrical resistivity, Hall coefficient, magnetic susceptibility, and specific heat for single crystals of Ce-based intervalent compound CeNiSi$_2$. The results show similar behaviors observed in Yb-based intervalent compounds and support recent thoery of the Anderson lattice, in which the Fermi-liquid coherence is gloval over the whole lattice. There is a low-temperature scale $T_{coh} \sim$ 50 K for the onset of Fermi-liquid coherence, in addition to a high-temperature scale $T_K^* \sim$ 150 K for the Kondo-lattice condensation. Therefore, we conclude that…
For describing the first-order isostructural valence phase transition in mixed valence compounds we develop a new approach based on the lattice Anderson model. We take into account the Coulomb interaction between localized f and conduction band electrons and two mechanisms of electron-lattice coupling. One is related to the volume dependence of the hybridization. The other is related to local deformations produced by f- shell size fluctuations accompanying valence fluctuations. The large f -state degeneracy allows us to use the 1/N expansion method. Within the model we develop a mean-field the…
The interaction between localized f and itinerant conduction electrons is crucial in the electronic properties of heavy fermion and valence fluctuating compounds. Using high-resolution angle-resolved photoemission spectroscopy, we systematically investigate the electronic structure of the archetypical valence fluctuating compound EuNi2P2 that hosts multiple f electrons. At low temperatures, we reveal the hybridization between Eu 4f and Ni 3d states, which contributes to the electron mass enhancement, consistent with the periodic Anderson model. With increasing temperature, interestingly, we ob…
Properties of an extended periodic Anderson model with the f-c Coulomb interaction $\Ufc$ is studied as a model for \Ge and related compounds which is cosidered to exhibit a sharp valence change under pressure. The problem is treated by extending the {\it slave-boson} and large-N expansion method to treat the present system. It is shown that, as the f-level $ε_{\rm f}$ is increased relative to the Fermi level, the sharp valence change is caused by the effect of $\Ufc$ with moderate strength of the order of the bandwith of conduction electrons. The superconducting transition temperature $T_\rc$…
We study S=1/2 Heisenberg model on the honeycomb lattice with first and second neighbor antiferromagnetic exchange (J_{1}-J_{2} model), employing exact diagonalization in both S_z=0 basis and nearest neighbor singlet valence bond (NNVB) basis. We find that for 0.2<J_2/J_1<0.3, NNVB basis gives a proper description of the ground state in comparison with the exact results. By analyzing the dimer-dimer as well as plaquette-plaquette correlations and also defining appropriate structure factors, we investigate possible symmetry breaking states as the candidate for the ground state in the frustrated…
We report $^{31}$P NMR measurements under various magnetic fields up to 7 T for the intermediate valence compound EuNi$_2$P$_2$, which shows heavy electronic states at low temperatures. In the high-temperature region above 40 K, the Knight shift followed the Curie--Weiss law reflecting localized $4f$ states. In addition, the behavior corresponding to the temperature variation of the average valence of Eu was observed in the nuclear spin-lattice relaxation rate $1/T_1$. With the occurrence of the Kondo effect, $1/T_1$ was clearly reduced below 40 K, and the Knight shift becomes almost constant …
A diffraction experiment using a high energy x-ray was carried out on YbInCu4. Below the Yb valence transition temperature, the splitting of Bragg peaks was detected in higher-order reflections. No superlattice reflections accompanying the valence ordering were found below the transition temperature. These experimental findings indicate that a structural change from a cubic structure to a tetragonal structure without valence ordering occurs at the transition temperature. Such a structural change free from any valence ordering is difficult to understand only in terms of Yb valence degrees of fr…
Electrical resistivity $ρ$, specific heat C, and magnetic susceptibility $χ$ measurements made on the filled skutterudite CeRu_4As_{12} reveal non-Fermi liquid (NFL) T - dependences at low T, i.e., $ρ$(T) $\sim$ T^{1.4} and weak power law or logarithmic divergences in C(T)/T and $χ$(T). Measurements also show that the T - dependence of the thermoelectric power S(T) deviates from that seen in other Ce systems. The NFL behavior appears to be associated with fluctuations of the Ce valence between 3^+ and 4^+ rather than a typical Kondo lattice scenario that would be appropriate for an integral Ce…
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…
We report on the study of the response to high pressures of the electronic and magnetic properties of several Sm-based compounds, which span at ambient pressure the whole range of stable charge states between the divalent and the trivalent. Our nuclear forward scattering of synchrotron radiation and specific heat investigations show that in both golden SmS and SmB6 the pressure-induced insulator to metal transitions (at 2 and about 4-7 GPa, respectively) are associated with the onset of long-range magnetic order, stable up to at least 19 and 26 GPa, respectively. This long-range magnetic order…
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 β-YbAlB4 demonstrate a scaling of its free energy indicative of zero-field quantum criticality without tuning in a metal. The …
In this paper I discuss the electronic structure and properties of a specific, rather unconventional class of transition metal (TM) compounds, e.g. TM oxides, which formally have unusually high values of the oxidation state, or valence, of TM. In contrast to the typical situation, in this case the charge-transfer gap (excitation energy for the transfer of electrons from the ligands to the TM) is very small and may even become negative. As a result a profound modification of an electronic structure and of all the properties may take place: there appear holes in the oxygen p-bands (``self-doping…
Several elements show valence skip fluctuation, for instance, Tl forms the compounds in valence states +1 and +3, and Bi forms in +3 and +5 states. This kind of fluctuation gives rise to a negative effective attractive interaction and the Kondo effect. In the compounds of valence skipping elements, the carrier doping will induce superconductivity with high critical temperature. For example, Ba$_{1-x}$K$_x$BiO$_3$ shows high $T_c$ which is unlikely from the conventional electron-phonon mechanism. The reason for the missing of some valence states in such valence skip compounds remains a mystery.…
Unusual phases and phase transitions are seen at the magnetic-nonmagnetic boundary in Ce, Eu and Yb-based compounds. EuNi$_2$P$_{2}$ is a very unusual valence fluctuating Eu system, because at low temperatures the Eu valence stays close to 2.5 instead of approaching an integer value. Eu valence and thus the magnetic property in this system can be tuned by Ge substitution in P site as EuNi$_2$Ge$_{2}$ is known to exhibit antiferromagnetc (AFM) ordering of divalent Eu moments with $T_N$ = 30 K. We have grown EuNi$_2$(P$_{1-x}$Ge$_x$)$_2$ (0.0 $\leq$ $x$ $\leq$ 0.5) single crystals and studied th…
We report inelastic neutron scattering experiments on a single crystal of the intermediate valence compound CePd3. At 300 K the magnetic scattering is quasielastic, with halfwidth of 23 meV, and is independent of momentum transfer Q. At low temperature, the Q-averaged magnetic spectrum is inelastic, exhibiting a broad peak centered near Emax = 55 meV. These results, together with the temperature dependence of the susceptibility, 4f occupation number, and specific heat, can be fit by the Kondo/Anderson impurity model. The low temperature scattering near Emax, however, shows significant variatio…
Transition-metal perovskite oxides exhibit a wide range of extraordinary but imperfectly understood phenomena. Charge, spin, orbital, and lattice degrees of freedom all undergo order-disorder transitions in regimes not far from where the best-known of these phenomena, namely high-temperature superconductivity of the copper oxides, and the 'colossal' magnetoresistance of the manganese oxides, occur. Mostly diffraction techniques, sensitive either to the spin or the ionic core, have been used to measure the order. Unfortunately, because they are only weakly sensitive to valence electrons and yie…
Optical reflectivity R(w) of YbInCu4 single crystals has been measured across its first-order valence transition at T_v ~ 42 K, using both polished and cleaved surfaces. R(w) measured on cleaved surfaces Rc(w) was found much lower than that on polished surface Rp(w) over the entire infrared region. Upon cooling through T_v, Rc(w) showed a rapid change over a temperature range of less than 2 K, and showed only minor changes with further cooling. In contrast, Rp(w) showed much more gradual and continuous changes across T_v, similarly to previously reported data on polished surfaces. The present …
The low-temperature electron spin resonance (ESR) spectra and the static magnetization data obtained for the stoichiometric single crystals of $β$-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 $3.4\times 10^{-3}$ $μ_B$ 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 para…
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 transitio…
We present the crystal growth as well as the structural, chemical and physical chracterization of SmRh$_2$Si$_2$ single crystals. Their ground state is antiferromagnetic, as indicated by the behaviour of the magnetic susceptibility and the specific heat at the second order phase transition observed at T$_{\rm N}$ = 64 K. The Sommerfeld coefficient is small and similar to that of LuRh$_2$Si$_2$ with $γ_0\approx$ J/(molK$^2$). Susceptibility measurements show no Curie-Weiss behaviour at high temperatures which is a consequence of the large Van-Vleck contribution of the excited multiplets of Sm$^…
Correlation Induced Magnetic Topological Phases in Mixed-Valence Compound SmB6
本文基于Γ8四重态模型研究SmB6的磁性与拓扑性质，揭示压力或对称性破缺可诱导金属反铁磁相，并阐明不同磁序对应的Dirac节线、Weyl点等拓扑特征及表面态和输运性质。
The intermediate valence compound YbAl$_3$ is known to undergo a hybridization process between itinerant and localized electrons. The resulting heavy Fermi liquid remains non-magnetic and non-superconducting. A microscopic understanding of the hybridization process in YbAl$_3$ is still lacking although some characteristic temperature and energy scales have been identified. Here we report results from novel spectroscopic measurements based on quasiparticle scattering. From the conductance spectra taken over a wide temperature range, we deduce that the band renormalization and hybridization proc…
We report on detailed low temperature measurements of the magnetization, the specific heat and the electrical resistivity on high quality CeRuSn single crystals. The compound orders antiferromagnetically at $T_{\rm N} = 2.8$ K with the Ce$^{3+}$ ions locked within the $a-c$ plane of the monoclinic structure. Magnetization shows that below $T_{\rm N}$ CeRuSn undergoes a metamagnetic transition when applying a magnetic field of 1.5 and 0.8 T along the $a$ and $c$--axis, respectively. This transition manifests in a tremendous negative jump of $\sim 25$% in the magnetoresistance. The value of the …
The effect of pressure on the unique electronic state of the antiferromagnetic (AF) compound EuCu2Ge2 has been measured in a wide temperature range from 10 mK to 300 K by electrical resistivity measurements up to 10 GPa. The Neel temperature of TN = 15 K at ambient pressure increases monotonically with increasing pressure and becomes a maximum of TN = 27 K at 6.2 GPa but suddenly drops to zero at Pc = 6.5 GPa, suggesting the quantum critical point (QCP) of the valence transition of Eu from a nearly divalent state to that with trivalent weight. The rhomag0 and A values obtained from the low-tem…
Sb-NMR/NQR study has revealed a formation of a pseudogap at the Fermi level in the density of states in a valence fluctuating compound CeIrSb. The nuclear spin-lattice relaxation rate divided by temperature, 1/T_1T has a maximum around 300 K and decreases significantly as 1/T_1T ~ T^2, followed by a 1/T_1T = const. relation at low temperature. This temperature dependence of 1/T_1T is well reproduced by assuming a V-shaped energy gap with a residual density of states at the Fermi level. The size of energy gap for CeIrSb is estimated to be about 350 K, which is by one order of magnitude larger t…
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 Earth's magnetic field and six orders…
Structural and magnetic properties of the geometrically frustrated layered compound YBaCo4O7 have been studied by magnetization and neutron diffraction. A layered type crystal structure, with alternating tetrahedral layers of Kagomé and triangular types, along the c axis (hexagonal symmetry, space group P63mc) has been found. The oxygen content of the present compound was determined by iodometric titration to be 7.00{\pm}0.01. Presence of a short-range antiferromagnetic ordering (below TN ~ 110 K) has been concluded from the appearance of an addition broad magnetic peak (at Q ~ 1.35 Å-1) in th…
Recent state-of-the-art crystallographic investigations of transition metal spinel compounds have revealed that the d- orbital charge carriers undergo ordering transitions with the formation of local "molecular bonding" units such as dimers in MgTi2O4, octomers in CuIr2S4, and heptamers in AlV2O4. Herein, we provide a unifying scheme involving one- dimensional orbital wave ordering applicable to all of these spinels. The relative phase of the orbitals in the chains is shown to be crucial to the formation of different local units, and thus both the amplitude and phase of the orbital wave play i…
The compound EuPd2Si2 is a well-known valence-fluctuating compound with a largest variation of Eu valence in a narrow temperature interval (around 150 K). The ball-milled form of this compound was investigated to understand the Eu valence behavior in the nanoform. The compound is found to retain the ThCr2Si2-type tetragonal structure after ball-milling leading to a reduction in particle size, typically falling in the range 10 - 100 nm. We find that there is a qualitative change in the temperature dependence of magnetic susceptibility for such small particles, with respect to that known for bul…
X-ray and electron diffraction measurements on the metal-insulator (M-I) transition compound PrRu$_4$P$_{12}$ have revealed the emergence of a periodic ordering of charge density around the Pr atoms. It is found that the ordering is associated with the onset of a low temperature insulator phase. These conclusions are supported by the facts that the space group of the crystal structure transforms from Im$\bar{3}$ to Pm$\bar{3}$ below the M-I transition temperature and also that the temperature dependence of the superlattice peaks in the insulator phase follows the squared BCS function. The M-I …
In intermetallic compounds with zero-orbital momentum ($L=0$) the magnetic anisotropy and the electronic band structure are interconnected. Here, we investigate this connection on divalent Eu and trivalent Gd intermetallic compounds. We find by X-ray magnetic circular dichroism an out-of-plane easy magetization axis in 2D atom-thick EuAu$_2$. Angle-resolved photoemission and density-functional theory prove that this is due to strong $f-d$ band hybridization and Eu$^{2+}$ valence. In contrast, the easy in-plane magnetization of the structurally-equivalent GdAu$_2$ is ruled by spin-orbit-split $…
The possibility of multiferroicity arising from charge ordering in LuFe2O4 and structurally related rare earth ferrites is reviewed. Recent experimental work on macroscopic indications of ferroelectricity and microscopic determination of coupled spin and charge order indicates that this scenario does not hold. Understanding the origin of the experimentally observed charge and spin order will require further theoretical work. Other aspects of recent research in these materials, such as geometrical frustration effects, possible electric-field-induced transitions, or orbital order are also briefl…
We have investigated the optical conductivity of the prominent valence fluctuating compounds EuIr2Si2 and EuNi2P2 in the infrared energy range to get new insights into the electronic properties of valence fluctuating systems. For both compounds we observe upon cooling the formation of a renormalized Drude response, a partial suppression of the optical conductivity below 100 meV and the appearance of a mid-infrared peak at 0.15 eV for EuIr2Si2 and at 0.13 eV for EuNi2P2. Most remarkably, our results show a strong similarity with the optical spectra reported for many Ce- or Yb-based heavy fermio…
e have investigated the magnetic properties of YbRu$_{2}$Ge$_{2}$ by means of magnetic susceptibility $χ$(T), specific heat C(T) and electrical resistivity $ρ$(T) measurements performed on flux grown single crystals. The Curie-Weiss behavior of $χ$(T) along the easy plane, the large magnetic entropy at low temperatures and the weak Kondo like increase in $ρ$(T) proves a stable trivalent Yb state. Anomalies in C(T), $ρ$(T) and $χ$(T) at T$_{0}$ = 10.2 K, T$_{1}$ = 6.5 K and T$_{2}$ = 5.7 K evidence complex ordering phenomena, T$_{0}$ being larger than the highest Yb magnetic ordering temperatur…
Many cerium-based heavy fermion (HF) compounds have pressure-temperature phase diagrams in which a superconducting region extends far from a magnetic quantum critical point. In at least two compounds, CeCu2Si2 and CeCu2Ge2, an enhancement of the superconducting transition temperature was found to coincide with an abrupt valence change, with strong circumstantial evidence for pairing mediated by critical valence, or charge transfer, fluctuations. This pairing mechanism, and the valence instability, is a consequence of a f-c Coulomb repulsion term U_fc in the hamiltonian. While some non-supercon…
The charge ordering phenomena in quasi two-dimensional 1/4-filled organic compounds (ET)_2X (ET=BEDT-TTF) are investigated theoretically for the $θ$ and $α$-type structures, based on the Hartree approximation for the extended Hubbard models with both on-site and intersite Coulomb interactions. It is found that charge ordered states of stripe-type are stabilized for the relevant values of Coulomb energies, while the spatial pattern of the stripes sensitively depends on the anisotropy of the models. By comparing the results of calculations with the experimental facts, where the effects of quantu…
The valence level photoemission spectra in the Anderson impurity model for Ce compounds at zero temperature are studied as a function of the photon energy $ω$. Most of former studies on Ce compounds are based on the sudden approximation, which is valid in high energy region. For the photoemission in the adiabatic limit of low energy region, one should consider the dipole matrix elements and the hole-induced photoelectron scattering potential. We can manage it by combining the time-evolution formalism and the $1/N_f$ scheme in a large $f$-level degeneracy $N_f$. This gives the exact results as …
Inelastic neutron scattering measurements on a CePd3 single crystal show a magnetic response at 300 K that is independent of momentum transfer with a Lorentzian quasielastic energy spectrum with a half width of 23 meV. This is in agreement with the Anderson impurity model (AIM), that predicts local moment relaxational behavior in this temperature regime. The 7 K magnetic response has an inelastic Lorentzian spectrum, with characteristic energy of 53 meV and half width 32 meV at the (h, 1/2, 0) zone boundary. Such an inelastic spectrum is expected for the AIM at low temperature. Unlike the Q-in…
The magnetic behavior of the quaternary compounds, RCr2Si2C (R = La, Ce), has been investigated by magnetization (M) and heat-capacity (C) measurements (1.8-300 K) in the bulk polycrystals and nano forms (<1 μm) obtained by high-energy balling. Our finding is that Cr appears to exhibit magnetic ordering of an itinerant type at low temperatures (<20 K) in the bulk form, as inferred from a combined look at all the data. The magnetic ordering gets gradually suppressed with increasing milling time. Evidence for a mixed-valence state of Ce for the bulk form is obtained from the tendency of magnetic…
A study of an impurity driven phase-transition into a magnetically ordered state in the spin-liquid Haldane chain compound PbNi2V2O8 is presented. Both, macroscopic magnetization as well as 51V nuclear magnetic resonance (NMR) measurements reveal that the spin nature of dopants has a crucial role in determining the stability of the induced long-range magnetic order. In the case of nonmagnetic (Mg2+) doping on Ni2+ spin sites (S=1) a metamagnetic transition is observed in relatively low magnetic fields. On the other hand, the magnetic order in magnetically (Co2+) doped compounds survives at muc…
The material KNi$_2$Se$_2$ has recently been shown to possess a number of striking physical properties, many of which are apparently related to the mixed valency of this system, in which there is on average one quasi-localized electron per every two Ni sites. Remarkably, the material exhibits a charge density wave (CDW) phase that disappears upon cooling, giving way to a low-temperature coherent phase characterized by an enhanced electron mass, reduced resistivity, and an enlarged unit cell free of structural distortion. Starting from an extended periodic Anderson model and using the slave-bos…
Field-induced magnetic ordering in the Haldane chain compound SrNi$_{2}$V$_{2}$O$_{8}$ and effect of anisotropy have been investigated using single crystals. Static susceptibility, inelastic neutron scattering, high-field magnetization, and low temperature heat-capacity studies confirm a non-magnetic spin-singlet ground state and a gap between the singlet ground state and triplet excited states. The intra-chain exchange interaction is estimated to be $J \sim 8.9{\pm}$0.1 meV. Splitting of the dispersions into two modes with minimum energies 1.57 and 2.58 meV confirms the existence of single-io…
We present electronic structure calculations for the one-dimensional magnetic chain compounds Ca_3CoRhO_6 and Ca_3FeRhO_6. The calculations are based on density functional theory and the local density approximation. We use the augmented spherical wave (ASW) method. The observed alternation of low- and high-spin states along the Co-Rh and Fe-Rh chains is related to differences in the oxygen coordination of the transition metal sites. Due to strong hybridization the O 2p states are polarized, giving rise to extended localized magnetic moments centered at the high-spin sites. Strong metal-metal o…
We report a systematic study of Sm valence in the prototypical intermediate valence compound SmB$_6$. Sm mean valence, $v_{\rm Sm}$, was measured by X-ray absorption spectroscopy as functions of pressure ($1<P<13$ GPa) and temperature ($3<T<300$ K). Pressure induced magnetic order (MO) was detected above $P_c = 10$ GPa by resistivity measurements. A shift toward localized $4f$ state with increasing $P$ and/or $T$ is evident from an increase in $v_{\rm Sm}$. However $v_{\rm Sm}$ at $P_c$ is anomalously far below 3, which differs from the general case of nonmagnetic-magnetic transition in Yb and…
Toward the understanding of incommensurate $Γ_3$ quadrupole ordering in PrPb$_3$, we develop a microscopic theory of multipole ordering in $f^2$-electron systems from an itinerant picture on the basis of a $j$-$j$ coupling scheme. For this purpose, we introduce the $Γ_7$-$Γ_8$ Hubbard model on a simple cubic lattice with the effective interactions that induce local $Γ_3$ states. By evaluating multipole susceptibility in a random phase approximation, we find that the hybridization between $Γ_7$ and $Γ_8$ orbitals plays a key role in the emergence of $Γ_3$ quadrupole ordering. We also emphasize …
The field induced quantum phase transitions in the disorder-free and disordered samples of the spin ladder material (CH_3)_2CHNH_3Cu(Cl_{1-x}Br_x)_3 are studied using magnetic calorimetry and magnetic neutron diffraction on single crystal samples. Drastically different critical indexes and correlation lengths in the high field phase are found for two different orientations of the applied field. It is argued that for a field applied along the crystallographic c axis, as in previous studies [1], the transition is best described as an Ising transition in random field and anisotropy, rather than a…
We find that the compounds for RE = Y, La-Dy, crystallize in the tetragonal Ibam (U$_2$Co$_3$Si$_5$ type) structure whereas the compounds for RE = Er-Lu, crystallize in a new orthorhombic structure with a space group Pmmn. Samples of Ho$_2$Ir$_3$Ge$_5$ were always found to be multiphase. The compounds for RE = Y to Dy which adopt the Ibam type structure show a metallic resistivity whereas the compounds with RE = Er, Tm and Lu show an anomalous behavior in the resistivity with a semiconducting increase in $ρ$ as we go down in temperature from 300K. Interestingly we had earlier found a positive …
The results of electronic structure calculations for the one-dimensional magnetic chain compound Ca3Co2O6 are presented. The calculations are based on density functional theory and the local density approximation and used the augmented spherical wave (ASW) method. Our results allow for deeper understanding of recent experimental findings. In particular, alternation of Co 3d low- and high-spin states along the characteristic chains is related to differences in the oxygen coordination at the inequivalent cobalt sites. Strong hybridization of the d states with the O 2p states lays ground for pola…
We present a detailed study on magnetic, thermodynamic and transport properties of polycrystalline RAgAl3(R = Ce and Pr) compounds. Both compounds crystallize in orthorhombic structure, which is distorted from the tetragonal BaAl4 structure with the space group Cmcm. Heat capacity measurement indicates the bulk magnetic ordering of the compounds. CeAgAl3 and PrAgAl3 order ferromagnetically at TC = 3.8 K and 5.8 K, respectively as it was confirmed from magnetic measurements. CeAgAl3 exhibits heavy Fermion behaviour. The Schottky behaviour in heat capacity data was observed in both compounds. Th…
We present our theoretical results on the ground states in layered triangular-lattice compounds ANiO2 (A=Na, Li, Ag). To describe the interplay between charge, spin, orbital, and lattice degrees of freedom in these materials, we study a doubly-degenerate Hubbard model with electron-phonon couplings by the Hartree-Fock approximation combined with the adiabatic approximation. In a weakly-correlated region, we find a metallic state accompanied by \sqroot3x\sqroot3 charge ordering. On the other hand, we obtain an insulating phase with spin-ferro and orbital-ferro ordering in a wide range from inte…
Bulk magnetic, X-ray and neutron diffraction measurements were performed on polycrystalline Tb14Ag51 in the temperature range from 1.5 K to room temperature. Its chemical Gd14Ag51 type structure corresponds to space group P6/m. Combined with group theoretical symmetry analysis, we show that the magnetic structure of this intermetallic compound is of a new k = (1/3,1/3,0) type with three magnetic Tb sublattices ordering simultaneously below TN = 27.5(5) K according to the combined irreducible representations tau4 and tau6. Here we present a general analysis of possible magnetic A ordering for k…
This response on a Comment on Reference 2 discusses the space group Fmm2 determination of the low temperature structure of NaV2O5. We show that while conventional crystallography is consistent with 'zig-zag' charge ordering of half of the ladders, recent spectroscopic measurements suggest that the symmetry is lower than Fmm2. We suggest space group C2, consistent with full 'zig-zag' charge ordering of all the ladders.
We present the high-precision magnetization data of the valence fluctuating heavy fermion superconductor $β$-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 $T/(B-B_c)^δ$ scaling, and confirmed that $δ= 1$ 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 discu…
We report measurements and analysis of the specific heat and magnetocaloric effect at the phase boundary into the single magnetic field-induced phase (phase II) of U(Ru{0.96}Rh{0.04})2Si2, which yield striking similarities to the valence transition of Yb{1-x}YxInCu4. To explain these similarities, we propose a bootstrap mechanism by which a structural distortion causes an electric quadrupolar order parameter within phase II to become coupled to the 5f-electron hybridization, giving rise to a valence change at the transition.
We have measured the specific heat of the S = 1/2 alternating Heisenberg antiferromagnetic chain compound pentafluorophenyl nitronyl nitroxide in magnetic fields using a single crystal and powder. A sharp peak due to field-induced magnetic ordering (FIMO) is observed in both samples. The H-T phase boundary of the FIMO of the single crystal is symmetric with respect to the central field of the gapless field region HC1 < H < HC2, whereas it is distorted for the powder whose ordering temperatures are lower. An analysis employing calculations based on the finite temperature density matrix renormal…
The competition between magnetic ordering and the Kondo effect in Ce2RhSi3, ordering antiferromagnetically at 7 K, is investigated by the measurements of magnetization, heat capacity and electrical resistivity on the solid solutions, Ce(2-x)La(x)RhSi3, Ce(2-y)Y(y)RhSi3, and Ce2RhSi(3-z)Ge(z), as well as by high pressure studies on this compound. The trends in the Kondo and Neel temperature variations among these alloys are compared to infer the roles of unit-cell volume and electronic structure changes. On the basis of the results, we infer that this compound lies at the peak of Doniach-magnet…
Strong enhancement of magnetic ordering temperature and structural/valence transitions in EuPd3S4 under high pressure
通过高压电输运、X射线衍射及穆斯堡尔谱等手段研究EuPd3S4，发现压力显著提升反铁磁有序温度TN至23.5 K，随后在~28 GPa引发立方-四方结构相变并伴随Eu向完全三价态转变，导致磁有序消失。
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