Combining old and new de Haas-van Alphen (dHvA) and magnetoresistance data, we arrive at a detailed picture of the Fermi surface of the heavy fermion superconductor UPt3. Our work was partially motivated by a new proposal that two 5f valence electrons per formula unit in UPt3 are localized by correlation effects -- agreement with previous dHvA measurements of the Fermi surface was invoked in its support. Comprehensive comparison with our new observations shows that this 'partially localized' model fails to predict the existence of a major sheet of the Fermi surface, and is therefore less compatible with experiment than the originally proposed 'fully itinerant' model of the electronic structure of UPt3. In support of this conclusion, we offer a more complete analysis of the fully itinerant band structure calculation, where we find a number of previously unrecognized extremal orbits on the Fermi surface.
Samarium hexaboride is a classic three-dimensional mixed valence system with a high-temperature metallic phase that evolves into a paramagnetic charge insulator below 40 kelvin. A number of recent experiments have suggested the possibility that the low-temperature insulating bulk hosts electrically neutral gapless fermionic excitations. Here we show that a possible ground state of strongly correlated mixed valence insulators - composite exciton Fermi liquid - hosts a three dimensional Fermi surface of a neutral fermion, that we name the "composite exciton". We describe the mechanism responsibl…
The drastic changes of Fermi surfaces as well as transport anomalies near P=Pc~2.35 GPa in CeRhIn5 are explained theoretically from the viewpoint of sharp valence change of Ce. It is pointed out that the key mechanism is the interplay of magnetic order and Ce-valence fluctuations. It is shown that the antiferromagnetic state with "small" Fermi surfaces changes to the paramagnetic state with "large" Fermi surfaces with huge enhancement of effective mass of electrons with keeping finite c-f hybridization. This naturally explains the de Haas-van Alphen measurement and also the transport anomalies…
Ubiquity of unconventional phenomena observed in a series of heavy fermion metals is discussed on the basis of an idea of critical valence fluctuations. After surveying experimental aspects of these unconventional behaviors in prototypical compounds, CeCu_2(Si,Ge)_2, under pressure, we propose that sharp valence crossover phenomena are realized in CeCu_6, CeRhIn_5, and Ce(Ir,Rh)Si_3 by tuning the pressure and the magnetic field simultaneously, on the basis of previous results for an extended Anderson lattice model with the Coulomb repulsion U_fc between localized f-electron and itinerant condu…
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…
In a joint theoretical and experimental study we investigate the pressure dependence of the Eu valence in EuPd_3B_x (0 <= x <= 1). Density functional band structure calculations are combined with x-ray absorption and x-ray diffraction measurements under hydrostatic pressures up to 30 GPa. It is observed that the heterogenous mixed-valence state of Eu in EuPd_3B_x (x >= 0.2) can be suppressed partially in this pressure range. From the complementary measurements we conclude that the valence change in EuPd_3B_x is mainly driven by the number of additional valence electrons due to the insertion of…
$α$-YbAlB$_4$ is the locally isostructural polymorph of $β$-YbAlB$_4$, the first example of an Yb-based heavy fermion superconductor which exhibits pronounced non-Fermi-liquid behavior above $T_{\rm c}$. Interestingly, both $α$-YbAlB$_4$ and $β$-YbAlB$_4$ have strongly intermediate valence. Our single crystal study of the specific heat, magnetization and resistivity has confirmed the Fermi liquid ground state of $α$-YbAlB$_4$ ~in contrast with the quantum criticality observed in $β$-YbAlB$_4$. Both systems exhibit Kondo lattice behavior with the characteristic temperature scale $T^* \sim$ 8 K …
The valence orders at $T_a=125$ K and $T_b=105$ K in the cubic compound YbPd have been investigated by $^{105}$Pd-nuclear magnetic resonance (NMR) measurements. Significant decrease in the density of states at the Fermi energy below $T_a$ is evident from the measurement of nuclear spin lattice relaxation rate $1/T_1$, suggesting that the instabilities of Fermi surface are associated with the transitions. Moreover we observed the unusual evolution of low-energy fluctuations toward the valence transition at $T_a$ behind its drastic first-order nature. The structural transition accompanying the v…
The origin of intrinsic quantum criticality in the heavy-fermion superconductor $β$-YbAlB$_4$ has been attributed to strong Yb valence fluctuations and its peculiar crystal structure. Here, we assess these contributions individually by studying the isostructural but fixed-valence compound $β$-LuAlB$_4$. Quantum oscillation measurements and DFT calculations reveal a Fermi surface markedly different from that of $β$-YbAlB$_4$, consistent with a `large' Fermi surface there. We also find an unexpected in-plane anisotropy of the electronic structure, in contrast to the isotropic Kondo hybridization…
To investigate valence imbalance phenomena between the surface and bulk in layered manganites, we analyze an eg-orbital degenerate double-exchange model with surfaces for two types of t2g spin structures. We reconfirm that the surface-induced Friedel oscillations occur in the charged structure and that the number of Mn4+ ions on the surface is larger than that in the bulk. This tendency is found to be more significant, when the eg-electron system has Fermi-surface structures with better nesting properties. The behavior of the Friedel oscillations depends on the nesting properties of the Fermi-…
In Kondo lattice systems with mixed valence, such as YbAl3, interactions between localized electrons in a partially filled f shell and delocalized conduction electrons can lead to fluctuations between two different valence configurations with changing temperature or pressure. The impact of this change on the momentum-space electronic structure and Fermi surface topology is essential for understanding their emergent properties, but has remained enigmatic due to a lack of appropriate experimental probes. Here by employing a combination of molecular beam epitaxy (MBE) and in situ angle-resolved p…
The spectra of Pu chalcogenides and pnictides are computed with LDA+DMFT and interpreted with the aid of valence histograms and slave-boson calculations. We find the chalcogenides are mixed-valent ($n_f = 5.2$) materials with a strongly $T$-dependent low-energy density of states and a triplet of quasiparticle peaks below the Fermi level. Furthermore, we predict a doublet of reflected peaks above the Fermi level. In the pnictides, the raising of $f^6$ states relative to $f^5$ suppresses valence fluctuations, resulting in integral-valent ($n_f = 5.0$) local moment metals.
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 …
I study an Extended Periodic Anderson Model (EPAM) with non-local hybridisation, $V_{fc}$, and a coulomb interaction, $U_{fc}$, between localised $f$ electrons and wide band conduction ($c$) electrons. Within DMFT, a quantum phase transition (QPT) driven by soft $f$-valence fluctuations, accompanied by a discontinuous jump in the Fermi volume, is found as $V_{fc}$ is tuned across a critical value. Near the associated QCP, an unconventional superconductive instability, driven by these extended, singular valence fluctuations, naturally emerges. {\it All} these phenomena are representative of obs…
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…
Intermetallic compounds containing $f$-electron elements have been prototypical materials for investigating strong electron correlations and quantum criticality (QC). Their heavy fermion ground state evoked by the magnetic $f$-electrons is susceptible to the onset of quantum phases, such as magnetism or superconductivity, due to the enhanced effective mass ($m^{*}$) and a corresponding decrease of the Fermi temperature. However, the presence of $f$-electron valence fluctuations to a non-magnetic state is regarded an anathema to QC, as it usually generates a paramagnetic Fermi-liquid state with…
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 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…
It was reported by Shiino et al in J. Phys. Soc. Jpn. 86, 123705 (2017) that Ce_xLa_{1-x} Cu_{5.62} Au_{0.38} (x=0.02-0.10) exhibits a new type of quantum criticality in both magnetic and thermal properties, which is the same as that observed in a series of materials exhibiting quantum critical valence fluctuations (QCVF), such as β-YbAlB_4, Yb_{15}Al_{34}Au_{51}, and so on. However, the temperature (T) dependence in the resistivity rho(T) for T<0.5K is quite anomalous, i.e., ρ(T)\propto (const.-T^{n}) with n \simeq 0.75 at x=0.05. We find that this anomalous exponent is given by n=2(1-ζ), wit…
Recent experiments have revealed incommensurate charge density wave (CDW) in the pseudogap regime in underdoped cuprates, e.g. YBa$_2$Cu$_3$O$_{6+δ}$ and HgBa$_2$CuO$_{4+δ}$. However, its relationship with the pseudogap is still controversial. In this work, we take a phenomenological synthesis of the doped resonating valence bond (RVB) state and the CDW order. Starting from the Yang-Rice-Zhang Green's function ansatz for the doped RVB state [Phys. Rev. B {\bf 73}, 174501 (2006)], in which the Fermi surface is partially truncated into four nodal hole-like Fermi pockets by the antinodal RVB gap,…
CeOs$_4$Sb$_{12}$, a member of the skutterudite family, has an unusual semimetallic low-temperature $\cal{L}$-phase that inhabits a wedge-like area of the field $H$ - temperature $T$ phase diagram. We have conducted measurements of electrical transport and megahertz conductivity on CeOs$_4$Sb$_{12}$ single crystals under pressures of up to 3 GPa and in high magnetic fields of up to 41 T to investigate the influence of pressure on the different $H$-$T$ phase boundaries. While the high-temperature valence transition between the metallic $\cal{H}$-phase and the $\cal{L}$-phase is shifted to highe…
We consider competition of Kondo effect and s-wave superconductivity in heavy fermion and mixed valence superconductors, using the phenomenological approach for the periodic Anderson model. Similar to the well known results for single-impurity Kondo effect in superconductors, we have found principal possibility of a re-entrant regime of the superconducting transition temperature, $T_c$, in heavy fermion superconductors in a narrow range of model parameters and concentration of f-electrons. Suppression of $T_c$ in mixed valence superconductors is much weaker. Our theory has most validity in 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…
Some of the most remarkable phenomena---and greatest theoretical challenges---in condensed matter physics arise when $d$ or $f$ electrons are neither fully localized around their host nuclei, nor fully itinerant. This localized/itinerant "duality" underlies the correlated electronic states of the high-$T_c$ cuprate superconductors and the heavy-fermion intermetallics, and is nowhere more apparent than in the $5f$ valence electrons of plutonium. Here we report the full set of symmetry-resolved elastic moduli of $PuCoGa_5$---the highest $T_c$ superconductor of the heavy fermions ($T_c$=18.5 K)--…
We present in detail the bosonization-refermionization solution of the anisotropic version of the two-channel Anderson model at a particular manifold in the space of parameters of the theory, where we establish an equivalence with a Fermi-Majorana bi-resonant level model. The correspondence is rigorously proved by explicitly constructing the new fermionic fields and Klein factors in terms of the original ones and showing that the commutation properties between original and new Klein factors are of semionic type. We also demonstrate that the fixed points associated to the solvable manifold are …
The pseudogap phase of the underdoped cuprates is the host to a variety of novel electronic phenomenon. An example is the dc-resistivity which shows metallic behaviour in the ab-plane, while the c-axis response is insulating. We apply a model, originally formulated by Yang, Rice, and Zhang, to study the resistivity in the pseudogap phase. This model is able to reproduce the qualitative features of the resistivity, including the systematic deviations from linear behaviour for the in-plane conductivity, and the insulating behaviour along the c-axis. We compare this to the predictions of the arc …
A new universality class of quantum criticality emerging in itinerant electron systems with strong local electron correlations is discussed. The quantum criticality of a Ce- or Yb-valence transition gives us a unified explanation for unconventional criticality commonly observed in heavy fermion metals such as YbRh2Si2 and β-YbAlB4, YbCu5-xAlx, and CeIrIn5. The key origin is due to the locality of the critical valence fluctuation mode emerging near the quantum critical end point of the first-order valence transition, which is caused by strong electron correlations for f electrons. Wider relevan…
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 the observation of the de Haas-van Alphen effect in IrTe2 measured using torque magnetometry at low temperatures down to 0.4 K and in high magnetic fields up to 33T. IrTe2 undergoes a major structural transition around 283 K due to the formation of planes of Ir and Te dimers that cut diagonally through the lattice planes, with its electronic structure predicted to change significantly from a layered system with predominantly three-dimensional character to a tilted quasi-two dimensional Fermi surface. Quantum oscillations provide direct confirmation of this unusual tilted Fermi surfac…
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…
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…
Electric conductivity and structural details of the hole-doped polaron conductor La0.9Sr0.1FeO3 (LSF10) are reported. The conductivity of a single crystal shows an exponential increase with temperature with a maxi-mum of 100 S/cm at 700 K and with activation energy of about 375 meV, and a decrease for higher temperatures that follows a power law. The exponential increase of the electric conductivity for 300 K {\leg} T {\leg} 700 is accompanied by a shift of spectral weight in the photoemission valence band towards the Fermi level, indicative of a strong electron-phonon interaction. The subsequ…
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…
An unconventional superconducting phase is explored developing out of a non Fermi-liquid phase of the two-channel Anderson lattice model. It is characterized by a composite order parameter comprising of a local spin or orbital degree of freedom bound to triplet Cooper pairs with an isotropic and a nearest neighbour form factor. The superconducting transition temperature peaks in the moderate intermediate valence regime and vanishes at integral valence. The gap function is non analytic and odd in frequency, and a pseudo-gap develops in the conduction electron density of states which vanishes as…
The effects of electron-electron correlations on the low-energy electronic structure and their relationship with unconventional superconductivity are central aspects in the research on the iron-based pnictide superconductors. Here we use soft X-ray angle-resolved photoemission spectroscopy (SX-ARPES) to study how electronic correlations evolve in different chemically substituted iron pnictides. We find that correlations are intrinsically related to the effective filling of the correlated orbitals, rather than to the filling obtained by valence counting. Combined density functional theory (DFT)…
We have performed Diffusion Quantum Monte Carlo simulations of Li clusters showing that Resonating-Valence-Bond (RVB) pairing correlations between electrons provide a substantial contribution to the cohesive energy. The RVB effects are identified in terms of electron transfers from s- to p-like character, constituting a possible explanation for the breakdown of the Fermi liquid picture observed in recent high resolution Compton scattering experiments for bulk Li.
The localized-itinerant nature of Ce-4$f$ valence electrons in heavy fermion compound CeIn$_{3}$ under pressure is studied thoroughly by means of the combination of density functional theory and single-site dynamical mean-field theory. The detailed evolutions of electronic structures of CeIn$_{3}$, including total and partial density of states, momentum-resolved spectral functions, and valence state histograms etc., are calculated in a wide pressure range where the corresponding volume compression $V/V_0 \in [0.6,1.0]$ (here $V_0$ is the experimental crystal volume) at $T \cong 116$ K. Upon in…
We demonstrate that the conductance through a single-electron transistor at low temperature is in quantitative agreement with predictions of the equilibrium Anderson model. When an unpaired electron is localized within the transistor, the Kondo effect is observed. Tuning the unpaired electron's energy toward the Fermi level in nearby leads produces a cross-over between the Kondo and mixed-valence regimes of the Anderson model.
The electronic structure of (Ce,Yb)CoIn5 has been studied by a combination of photoemission, x-ray absorption and bulk property measurements. Previous findings of a Ce valence near 3+ for all x and of an Yb valence near 2.3+ for x>0.3 were confirmed. One new result of this study is that the Yb valence for x<0.2 increases rapidly with decreasing x from 2.3+ toward 3+, which correlates well with de Haas van Alphen results showing a change of Fermi surface around x=0.2. Another new result is the direct observation by angle resolved photoemission Fermi surface maps of about 50% cross sectional are…
We report on the valence fluctuation of Ce in CeMo$_{2}$Si$_{2}$C as studied by means of magnetic susceptibility $χ(T)$, specific heat $C(T)$, electrical resistivity $ρ(T)$ and x-ray absorption spectroscopy. Powder x-ray diffraction revealed that CeMo$_{2}$Si$_{2}$C crystallizes in CeCr$_{2}$Si$_{2}$C-type layered tetragonal crystal structure (space group \textit{P4/mmm}). The unit cell volume of CeMo$_{2}$Si$_{2}$C deviates from the expected lanthanide contraction, indicating non-trivalent state of Ce ions in this compound. The observed weak temperature dependence of the magnetic susceptibili…
