Complex electronic matter exhibit subtle forms of self organization which are almost invisible to the available experimental tools, but which have dramatic physical consequences. One prominent example is provided by the actinide based heavy fermion material URu_2Si_2. At high temperature, the U-5f electrons in URu_2Si_2 carry a very large entropy. This entropy is released at 17.5K via a second order phase transition to a state which remains shrouded in mystery, and which was termed a "hidden order" state. Here we develop a first principles theoretical method to analyze the electronic spectrum of correlated materials as a function of the position inside the unit cell of the crystal, and use it to identify the low energy excitations of the URu_2Si_2. We identify the order parameter of the hidden order state, and show that it is intimately connected with magnetism. We present first principles results for the temperature evolution of the electronic states of the material. At temperature below 70K U-5f electrons undergo a multichannel Kondo effect, which is arrested at low temperature by the crystal field splitting. At lower temperatures, two broken symmetry states emerge, characterized by a complex order parameter ψ. A real $ψ$ describes the hidden order phase, and an imaginary ψcorresponds to the large moment antiferromagnetic phase, thus providing a unified picture of the two broken symmetry phases, which are realized in this material.
We derive the coupling of a localized hexadecapolar mode to conduction electrons in tetragonal symmetry. The derivation can be easily adapted to arbitrary multipoles in arbitrary environment. We relate our model to the two-channel Kondo (2CK) model and show that for an $f^2$-configuration, a relevant crystal field splitting in addition to the 2CK interaction is intrinsic to tetragonal symmetry. We discuss possible realizations of a hexadecapolar Kondo effect in URu$_2$Si$_2$. Solving our model we find good agreement with susceptibility and specific heat measurements in Th$_{1-x}$U$_x$Ru$_2$Si$…
Using a large-N approach, we demonstrate that the differential conductance and quasi-particle interference pattern measured in recent scanning tunneling spectroscopy experiments (A.R. Schmidt et al. Nature 465, 570 (2010); P. Aynajian et al., PNAS 107, 10383 (2010)) in URu2Si2 are consistent with the emergence of a coherent Kondo lattice below its hidden order transition (HOT). Its formation is driven by a significant increase in the quasi-particle lifetime, which could arise from the emergence of a yet unknown order parameter at the HOT.
A polarized electronic Raman scattering study reveals the emergence of symmetry dependence in the electronic Raman response of single crystalline URu$_{2}$Si$_{2}$ below the Kondo crossover scale $T_K\sim100K$. In particular, the development of a coherent Kondo pseudo-gap predominantly in the E$_g$ channel highlights strong anisotropy in the Kondo physics in URu$_{2}$Si$_{2}$ that has previously been neglected in theoretical models of this system. A calculation of the Raman vertices demonstrates that the strongest Raman vertex does indeed develop within the E$_g$ channel for interband transiti…
Within the framework of the Kondo-Heisenberg model, we analyse the effect of charge fluctuation on the modulated spin liquid (MSL) and antiferromagnetic (AF) orders which were established in a previous publication. We discuss the emergence of two quantum critical lines separating the coexisting Kondo-MSL and Kondo-MSL-AF phases. The various order parameters of the system possess a characteristic signature observable on the electronic band structure of each of the phases. We calculate that the MSL order is indeed a possible explanation of the hidden order phase of $URu_{2}Si_{2}$ heavy fermion …
The nature of the second order phase transition that occurs in URu2Si2 at 17.5 K remains puzzling despite intensive research over the past two and half decades. A key question emerging in the field is whether a hybridization gap between the renormalized bands can be identified as the long-sought 'hidden' order parameter. We report on the measurement of a hybridization gap in URu2Si2 employing a spectroscopic technique based on quasiparticle scattering across a ballistic metallic junction. The differential conductance exhibits an asymmetric double-peak structure, a clear signature for a Fano re…
We study, using high-resolution angle-resolved photoemission spectroscopy, the evolution of the electronic structure in URu2Si2 at the Gamma, Z and X high-symmetry points from the high-temperature Kondo-screened regime to the low-temperature `hidden-order' (HO) state. At all temperatures and symmetry points, we find structures resulting from the interaction between heavy and light bands, related to the Kondo lattice formation. At the X point, we directly measure a hybridization gap of 11 meV already open at temperatures above the ordered phase. Strikingly, we find that while the HO induces pro…
We measured the polarized optical conductivity of URu$_2$Si$_2$ from room temperature down to 5 K, covering the Kondo state, the coherent Kondo liquid regime, and the hidden-order phase. The normal state is characterized by an anisotropic behavior between the ab plane and c axis responses. The ab plane optical conductivity is strongly influenced by the formation of the coherent Kondo liquid: a sharp Drude peak develops and a hybridization gap at 12 meV leads to a spectral weight transfer to mid-infrared energies. The c axis conductivity has a different behavior: the Drude peak already exists a…
Heavy electronic states originating from the f atomic orbitals underlie a rich variety of quantum phases of matter. We use atomic scale imaging and spectroscopy with the scanning tunneling microscope (STM) to examine the novel electronic states that emerge from the uranium f states in URu2Si2. We find that as the temperature is lowered, partial screening of the f electrons' spins gives rise to a spatially modulated Kondo-Fano resonance that is maximal between the surface U atoms. At T=17.5 K, URu2Si2 is known to undergo a 2nd order phase transition from the Kondo lattice state into a phase wit…
We report a comprehensive investigation of the lattice dynamics of URu$_2$Si$_2$ as a function of temperature using Raman scattering, optical conductivity and inelastic neutron scattering measurements as well as theoretical {\it ab initio} calculations. The main effects on the optical phonon modes are related to Kondo physics. The B$_{1g}$ ($Γ_3$ symmetry) phonon mode slightly softens below $\sim$100~K, in connection with the previously reported softening of the elastic constant, $C_{11}-C_{12}$, of the same symmetry, both observations suggesting a B$_{1g}$ symmetry-breaking instability in the…
Within a Kondo lattice, the strong hybridization between electrons localized in real space (r-space) and those delocalized in momentum-space (k-space) generates exotic electronic states called 'heavy fermions'. In URu2Si2 these effects begin at temperatures around 55K but they are suddenly altered by an unidentified electronic phase transition at To = 17.5 K. Whether this is conventional ordering of the k-space states, or a change in the hybridization of the r-space states at each U atom, is unknown. Here we use spectroscopic imaging scanning tunnelling microscopy (SI-STM) to image the evoluti…
We use inelastic neutron scattering measurements to show that the energy gap in the magnetic excitations of URu$_2$Si$_2$, induced by the Hidden Order transition, is closed by Re substitution. The magnetic excitations remain ungapped in compositions where the specific heat anomaly associated with Hidden Order is no longer observed, which means that the entropy associated with Hidden Order is tied mostly to the magnetic gapping. Further, the onset of ferromagnetic order does not gap the excitations, reflecting the fact that Re substitution does not dramatically affect the Kondo lattice hybridiz…
We argue that near a Kondo breakdown critical point, a spin liquid with spatial modulations can form. Unlike its uniform counterpart, we find that this occurs via a second order phase transition. The amount of entropy quenched when ordering is of the same magnitude as for an antiferromagnet. Moreover, the two states are competitive, and at low temperatures are separated by a first order phase transition. The modulated spin liquid we find breaks $Z_4$ symmetry, as recently seen in the hidden order phase of URu$_2$Si$_2$. Based on this, we suggest that the modulated spin liquid is a viable candi…
We report on magneto-transport properties of the Kondo semiconducting compound CeRu$_2$Al$_{10}$, focusing on its exotic phase below $T_0$ = 27 K. In this phase, an excess thermal conductivity $κ$ emerges and is gradually suppressed by magnetic field, strikingly resembling those observed in the hidden-order phase of URu$_2$Si$_2$. Our analysis indicates that low-energy magnetic excitation is the most likely origin, as was also proposed for URu$_2$Si$_2$ recently, despite the largely reduced magnetic moments. Likewise, other transport properties such as resistivity, thermopower and Nernst effec…
Substitution of Re for Ru in the heavy fermion compound URu2Si2 suppresses the hidden order transition and gives rise to ferromagnetism at higher concentrations. The hidden order transition of URu(2-x)Re(x)Si2, tracked via specific heat and electrical resistivity measurements, decreases in temperature and broadens, and is no longer observed for x>0.1. A critical scaling analysis of the bulk magnetization indicates that the ferromagnetic ordering temperature and ordered moment are suppressed continuously towards zero at a critical concentration of x = 0.15, accompanied by the additional suppres…
By combining the results of muon spin rotation and inelastic neutron scattering in the heavy fermion compounds Ce1-xLaxAl3 (0.0 <= x <= 0.2), we show that static magnetic correlations are suppressed above a characteristic temperature, T*, by electronic dissipation rather than by thermal disorder. Below T*, an energy gap opens in the single-ion magnetic response in agreement with the predictions of the Anisotropic Kondo Model. Scaling arguments suggest that similar behavior may underlie the "hidden order" in URu2Si2.
Adding a second Kondo channel to heavy fermion materials reveals new exotic symmetry breaking phases associated with the development of Kondo coherence. In this paper, we review two such phases, the "hastatic order" associated with non-Kramers doublet ground states, where the two-channel nature of the Kondo coupling is guaranteed by virtual valence fluctuations to an excited Kramers doublet, and "composite pair superconductivity," where the two channels differ by charge 2e and can be thought of as virtual valence fluctuations to a pseudo-isospin doublet. The similarities and differences betwee…
We present a detailed study of the low temperature and high magnetic field phases in the chemical substitution series URu$_2$Si$_{2-x}$P$_x$ using electrical transport and magnetization in pulsed magnetic fields up to 65T. Within the hidden order region (0 $\ x$$\ $ 0.035) the high field ordering is robust even as the hidden order temperature is suppressed. Earlier work shows that for 0.035 $\ x$ $\ $ 0.26 there is a Kondo lattice with a no-ordered state that is replaced by antiferromagnetism for 0.26 $\ x$ 0.5. We observe a simplified continuation of the high field ordering in the no-order $x…
The heavy electron Kondo liquid is an emergent state of condensed matter that displays universal behavior independent of material details. Properties of the heavy electron liquid are best probed by NMR Knight shift measurements, which provide a direct measure of the behavior of the heavy electron liquid that emerges below the Kondo lattice coherence temperature as the lattice of local moments hybridizes with the background conduction electrons. Because the transfer of spectral weight between the localized and itinerant electronic degrees of freedom is gradual, the Kondo liquid typically coexis…
The hidden order developing below 17.5K in the heavy fermion material URu2Si2 has eluded identification for over twenty five years. This paper will review the recent theory of ``hastatic order,'' a novel two-component order parameter capturing the hybridization between half-integer spin (Kramers) conduction electrons and the non-Kramers 5f^2 Ising local moments, as strongly indicated by the observation of Ising quasiparticles in de Haas-van Alphen measurements. Hastatic order differs from conventional magnetism as it is a spinor order that breaks both single and double time-reversal symmetry b…
In a large number of rare-earth and actinide systems, Kondo effect tends to suppress magnetic order by making the spin singlet between localized and conduction electron spins. In the presence of orbital degrees of freedom, however, there emerge exotic electronic orders induced by Kondo effect. The orbital Kondo effect can collectively make diagonal and off-diagonal (superconducting) orders. With the particle-hole symmetry in conduction bands, these orders are all degenerate, forming a macroscopic SO(5) multiplet. This paper discusses recent theoretical development on these electronic orders wh…
Strongly correlated materials are characterized by the presence of electron-electron interactions in their electronic structure. They often have remarkable properties and transitions between competing phases of very different electronic and magnetic order. This thesis focuses on strongly correlated $f$-electron compounds containing Ce, Sm, and U. These materials exhibit a so-called heavy-fermion or Kondo-lattice behavior. They can become insulating due to hybridization effects (Kondo-insulator) or develop multipolar (hidden) order. Kondo insulators have recently been discussed in the context o…
Magnetic critical scaling in URu2-xRexSi2 single crystals continuously evolves as the ferromagnetic critical temperature is tuned towards zero via chemical substitution. As the quantum phase transition is approached, the critical exponents gamma and (delta-1) decrease to zero in tandem with the critical temperature and ordered moment, while the exponent beta remains constant. This novel trend distinguishes URu2-xRexSi2 from stoichiometric quantum critical ferromagnets and appears to reflect an underlying competition between Kondo and ferromagnetic interactions.
Replacing a magnetic atom by a spinless atom in a heavy fermion compound generates a quantum state often referred to as a 'Kondo-hole'. No experimental imaging has been achieved of the atomic-scale electronic structure of a Kondo-hole, or of their destructive impact (Lawrence JM, et al. (1996) Kondo hole behavior in Ce0. 97La0. 03Pd3. Phys Rev B 53:12559-12562; Bauer ED, et al. (2011) Electronic inhomogeneity in a Kondo lattice. Proc Natl Acad Sci. 108:6857-6861) on the hybridization process between conduction and localized electrons which generates the heavy fermion state. Here we report visu…
An attractive proposal for the hidden order (HO) in the heavy electron compound URu2Si2 is an itinerant multipole order of high rank. It is due to the pairing of electrons and holes centered on zone center and boundary, respectively in states that have maximally different total angular momentum components. Due to the pairing with commensurate zone boundary ordering vector the translational symmetry is broken and a HO quasiparticle gap opens below the transition temperature T_HO. Inelastic neutron scattering (INS) has demonstrated that for T<T_HO the collective magnetic response is dominated by…
Novel electronic phenomena frequently form in heavy fermions as a consequence of the mutual nature of localization and itineracy of f electrons. On the magnetically ordered side of the heavy fermion phase diagram, f moments are expected to be localized and decoupled from the Fermi surface. It remains ambiguous whether a Kondo lattice can develop inside the magnetically ordered phase. Using spectroscopic imaging with the scanning tunneling microscope, complemented by neutron scattering, x ray absorption spectroscopy, and dynamical mean field theory, we probe the electronic states in the antifer…
We report the observation of a universal scaling of the Nernst coefficient over a wide intermediate temperature range in heavy fermion materials, including the superconductors CeCu$_2$Si$_2$, CeCoIn$_5$, and Ce$_2$PdIn$_8$, the ferromagnetic Kondo lattice Ce$_3$RhSi$_3$, the nonmagnetic CeRu$_2$Si$_2$, the intermediate valent YbAl$_3$, and the hidden order compound URu$_2$Si$_2$, that cover a broad spectrum of heavy fermion materials with different crystal, valence and ground state properties. The scaling formula follows exactly the magnetic susceptibility of emergent heavy quasiparticles as p…
In this paper we introduce an exactly solvable Kondo lattice model without any fine-tuning local gauge symmetry. This model describes itinerant electrons interplaying with a localized magnetic moment via only longitudinal Kondo exchange. Its solvability results from conservation of the localized moment at each site, and is valid for arbitrary lattice geometry and electron filling. A case study on square lattice shows that the ground state is a Néel antiferromagnetic insulator at half-filling. At finite temperature, paramagnetic phases including a Mott insulator and correlated metal are found. …
The heavy quasiparticle bands in Kondo materials which originate in the hybridization of f- and conduction electrons exhibit numerous, sometimes coexisting, broken symmetry phases. Most notable are unconventional superconductivity, itinerant small moment antiferromagnetism and hidden order of higher order multipoles of f-electrons which all lead to a gapping of the heavy bands. In rare cases the chemical potential lies within the hybridization gap and the ground state is a Kondo semiconductor without ordering. The dynamical magnetic response of such gapped f-electron systems has been investiga…
Despite more than half a century of studies in heavy-fermion compounds, a full understanding of the various possible magnetic ordering phenomena is still far from complete. Some heavy-fermion materials show so-called hidden-order phases, which are invisible to conventional diffraction techniques. The multipolar moments of the $f$-electrons in their specific crystal field environment play a decisive role in the formation of these phases. Such hidden-order phases have been observed in a variety of compounds containing $4f$ and $5f$ elements, like URu$_2$Si$_2$, NpO$_2$, YbRu$_2$Ge$_2$, and CeB$_…
Only few selected examples among the great diversity of anomalous rare earth skutterudite are reviewed. Focus is first given on PrFe4P12 in comparison with URu2Si2. For PrFe4P12, great progress has been made on determining the nature of the order parameter (OP). A non magnetic order parameter with a multipolar component emerges here while for URu2Si2 the nature of the so-called hidden order remains mysterious. The two systems have several similarities in their temperature--pressure (T, P) and magnetic field--temperature (H, T) phase diagrams, in their spin dynamics, in their nesting character …
