Analogy Between the "Hidden Order" and the Orbital Antiferromagnetism in URu_{2-x}Fe_{x}Si_{2}.

We study URu_{2-x}Fe_{x}Si_{2}, in which two types of staggered phases compete at low temperature as the iron concentration x is varied: the nonmagnetic "hidden order" (HO) phase below the critical concentration x_{c}, and unconventional antiferromagnetic (AFM) phase above x_{c}. By using polarization resolved Raman spectroscopy, we detect a collective mode of pseudovectorlike A_{2g} symmetry whose energy continuously evolves with increasing x; it monotonically decreases in the HO phase until it vanishes at x=x_{c}, and then reappears with increasing energy in the AFM phase. The mode's evolution provides direct evidence for a unified order parameter for both nonmagnetic and magnetic phases arising from the orbital degrees-of-freedom of the uranium-5f electrons.

Spin glasses: redux: an updated experimental/materials survey.

This article reviews the 40+ year old spin-glass field and one of its earliest model interpretations as a spin density wave. Our description is from an experimental phenomenological point of view with emphasis on new spin glass materials and their relation to topical problems and strongly correlated materials in condensed matter physics. We first simply define a spin glass (SG), give its basic ingredients and explain how the spin glasses enter into the statistical mechanics of classical phase transitions. We then consider the four basic experimental properties to solidly characterize canonical spin glass behavior and introduce the early theories and models. Here the spin density wave (SDW) concept is used to explain the difference between a short-range SDW, i.e. a SG and, in contrast, a long-range SDW, i.e. a conventional magnetic phase transition. We continue with the present state of SG, its massive computer simulations and recent proposals of chiral glasses and quantum SG. We then collect and mention the various SG 'spin-off's'. A major section uncovers the fashionable unconventional materials that display SG-like freezing and glassy ground states, such as (high temperature) superconductors, heavy fermions, intermetallics and Heuslers, pyrochlor and spinels, oxides and chalogenides and exotics, e.g. quasicrystals. Some conclusions and future directions complete the review.

High-magnetic-field lattice length changes in URu2Si2.

We report high-magnetic-field (up to 45 T) c-axis thermal-expansion and magnetostriction experiments on URu(2)Si(2) single crystals. The sample length change ΔL(c)(T(HO))/L(c) associated with the transition to the "hidden order" phase becomes increasingly discontinuous as the magnetic field is raised above 25 T. The reentrant ordered phase III is clearly observed in both the thermal expansion ΔL(c)(T)/L(c) and magnetostriction ΔL(c)(B)/L(c) above 36 T, in good agreement with previous results. The sample length is also discontinuous at the boundaries of this phase, mainly at the upper boundary. A change in the sign of the coefficient of thermal expansion α(c)=1/L(c)(∂ΔL(c)/∂T) is observed at the metamagnetic transition (B(M) ~ 38 T), which is likely related to the existence of a quantum critical end point.

Thermal transport and strong mass renormalization in NiCl2-4SC(NH2)2.

Several quantum paramagnets exhibit magnetic-field-induced quantum phase transitions to an antiferromagnetic state that exists for H c1 ≤ H ≤ H c2. For some of these compounds, there is a significant asymmetry between the low- and high-field transitions. We present specific heat and thermal conductivity measurements in NiCl2-4SC(NH2)2, together with calculations which show that the asymmetry is caused by a strong mass renormalization due to quantum fluctuations for H ≤ H c1 that are absent for H ≥ H c2. We argue that the enigmatic lack of asymmetry in thermal conductivity is due to a concomitant renormalization of the impurity scattering.

Hidden order in URu2Si2 originates from Fermi surface gapping induced by dynamic symmetry breaking.

Spontaneous, collective ordering of electronic degrees of freedom leads to second-order phase transitions that are characterized by an order parameter driving the transition. The notion of a 'hidden order' has recently been used for a variety of materials where a clear phase transition occurs without a known order parameter. The prototype example is the heavy-fermion compound URu(2)Si(2), where a mysterious hidden-order transition occurs at 17.5 K. For more than twenty years this system has been studied theoretically and experimentally without a firm grasp of the underlying physics. Here, we provide a microscopic explanation of the hidden order using density-functional theory calculations. We identify the Fermi surface 'hot spots' where degeneracy induces a Fermi surface instability and quantify how symmetry breaking lifts the degeneracy, causing a surprisingly large Fermi surface gapping. As the mechanism for the hidden order, we deduce spontaneous symmetry breaking through a dynamic mode of antiferromagnetic moment excitations.

Parasitic small-moment antiferromagnetism and nonlinear coupling of hidden order and antiferromagnetism in URu2Si2 observed by Larmor diffraction.

We report for the first time simultaneous microscopic measurements of the lattice constants, the distribution of the lattice constants, and the antiferromagnetic moment in high-purity URu(2)Si(2), combining Larmor and conventional neutron diffraction at low temperatures and pressures up to 18 kbar. Our data demonstrate quantitatively that the small moment in the hidden order (HO) of URu(2)Si(2) is purely parasitic. The excellent experimental conditions we achieve allow us to resolve that the transition line between HO and large-moment antiferromagnetism (LMAF), which stabilizes under pressure, is intrinsically first order and ends in a bicritical point. Therefore, the HO and LMAF must have different symmetry, which supports exotic scenarios of the HO such as orbital currents, helicity order, or multipolar order.

Hidden order and beyond: an experimental-theoretical overview of the multifaceted behavior of URu2Si2.

This topical review describes the multitude of unconventional behaviors in the hidden order, heavy fermion, antiferromagnetic and superconducting phases of the intermetallic compound URu2Si2 when tuned with pressure, magnetic field, and substitutions for all three elements. Such 'perturbations' result in a variety of new phases beyond the mysterious hidden order that are only now being slowly understood through a series of state-of-the-science experimentation, along with an array of novel theoretical approaches. Despite all these efforts spanning more than 30 years, hidden order (HO) remains puzzling and non-clarified, and the search continues in 2019 into a fourth decade for its final resolution. Here we attempt to update the present situation of URu2Si2 importing the latest experimental results and theoretical proposals. First, let us consider the pristine compound as a function of temperature and report the recent measurements and models relating to its heavy Fermi liquid crossover, its HO and superconductivity (SC). Recent experiments and theories are surmized that address four-fold symmetry breaking (or nematicity), Isingness and unconventional excitation modes. Second, we review the pressure dependence of URu2Si2 and its transformation to antiferromagnetic long-range order. Next we confront the dramatic high magnetic-field phases requiring fields above 40 T. And finally, we attempt to answer how does random substitutions of other 5f elements for U, and 3d, 4d, and 5d elements for Ru, and even P for Si affect and transform the HO. Commensurately, recent theoretical models are summarized and then related to the intriguing experimental behavior.

One-component order parameter in URu2Si2 uncovered by resonant ultrasound spectroscopy and machine learning.

The unusual correlated state that emerges in URu2Si2 below T HO = 17.5 K is known as "hidden order" because even basic characteristics of the order parameter, such as its dimensionality (whether it has one component or two), are "hidden." We use resonant ultrasound spectroscopy to measure the symmetry-resolved elastic anomalies across T HO. We observe no anomalies in the shear elastic moduli, providing strong thermodynamic evidence for a one-component order parameter. We develop a machine learning framework that reaches this conclusion directly from the raw data, even in a crystal that is too small for traditional resonant ultrasound. Our result rules out a broad class of theories of hidden order based on two-component order parameters, and constrains the nature of the fluctuations from which unconventional superconductivity emerges at lower temperature. Our machine learning framework is a powerful new tool for classifying the ubiquitous competing orders in correlated electron systems.

Field-induced ferromagnetic structure in Er(2)Ni(2)Pb.

We have studied the effect of magnetic fields up to 4.5 T on the ground-state structure in Er(2)Ni(2)Pb using powder neutron diffraction measurements at low temperatures. The zero-field magnetic state that itself is not uniform and consists of different magnetic phases is rather unstable against the magnetic field. As the field is increased, the magnetic reflections of the zero-field structure disappear and a new magnetic phase with commensurate propagation vector is clearly observed in a field of 0.5 T. At higher fields a ferromagnetic state is established in Er(2)Ni(2)Pb, which can be fully described only by a model that combines at least two irreducible representations. The refined Er magnetic moment magnitude of 9.10 ± 0.07 µ(B) is very close to the Er(3+) free ion value of 9.0 µ(B).

Heavy fermions. Chirality density wave of the "hidden order" phase in URu2Si2.

A second-order phase transition in a physical system is associated with the emergence of an "order parameter" and a spontaneous symmetry breaking. The heavy fermion superconductor URu2Si2 has a "hidden order" (HO) phase below the temperature of 17.5 kelvin; the symmetry of the associated order parameter has remained ambiguous. Here we use polarization-resolved Raman spectroscopy to specify the symmetry of the low-energy excitations above and below the HO transition. We determine that the HO parameter breaks local vertical and diagonal reflection symmetries at the uranium sites, resulting in crystal field states with distinct chiral properties, which order to a commensurate chirality density wave ground state.

(3 + 1)-dimensional crystal and antiferromagnetic structures in CeRuSn.

At 320 K, the crystal structure of CeRuSn is commensurate with the related CeCoAl-type of structure by the doubling of the c lattice parameter. However, with lowering the temperature it becomes incommensurate with x and z position parameters at all three elemental sites being modulated as one moves along the c-axis. The resulting crystal structure can be conveniently described within the superspace formalism in (3 + 1) dimensions. The modulation vector, after initially strong temperature dependence, approaches a value close to qnuc = (0 0 0.35). Below TN = 2.8 (1) K, CeRuSn orders antiferromagnetically with a propagation vector qmag = (0 0 0.175), i.e. with the magnetic unit cell doubled along the c-axis direction with respect to the incommensurate crystal structure. Ce moments appear to be nearly collinear, confined to the a-c plane, forming ferromagnetically coupled pairs. Their magnitudes are modulated between 0.11 and 0.95 µB as one moves along the c-axis.

Field-dependent thermal transport in the haldane chain compound NENP.

We present a study of the magnetic field-dependent thermal transport in the spin S=1 chain material Ni(C(2)H(8)N(2))(2)NO(2)(ClO(4)) (NENP). The measured thermal conductivity is found to be very sensitive to the field-induced changes in the spin excitation spectrum. The magnetic contribution to the total heat conductivity is analyzed in terms of a quasiparticle model, and we obtain a temperature and momentum independent mean free path. This implies that the motion of quasiparticles is effectively three dimensional despite the tiny interchain coupling.

Interplay between fermi surface topology and ordering in URu2Si2 revealed through abrupt hall coefficient changes in strong magnetic fields.

Temperature- and field-dependent measurements of the Hall effect of pure and 4% Rh-doped URu2Si2 reveal low density (0.03 hole/U) high mobility carriers to be unique to the "hidden order" phase and consistent with an itinerant density-wave order parameter. The Fermi surface undergoes a series of abrupt changes as the magnetic field is increased. When combined with existing de Haas-van Alphen data, the Hall data expose a strong interplay between the stability of the "hidden order," the degree of polarization of the Fermi liquid, and the Fermi surface topology.

Field-induced Fermi surface reconstruction and adiabatic continuity between antiferromagnetism and the hidden-order state in URu2Si2.

Shubnikov-de Haas oscillations reveal at high fields an abrupt reconstruction of the Fermi surface within the hidden-order (HO) phase of URu2Si2. Taken together with reported Hall effect results, this implies an increase in the effective carrier density and suggests that the field suppression of the HO state is ultimately related to destabilizing a gap in the spectrum of itinerant quasiparticles. While hydrostatic pressure favors antiferromagnetism in detriment to the HO state, it has a modest effect on the complex H-T phase diagram. Instead of phase separation between HO and antiferromagnetism our observations indicate adiabatic continuity between both orderings with field and pressure changing their relative weight.

Phonon thermal transport of URu2Si2: broken translational symmetry and strong-coupling of the "hidden order" to the lattice.

A dramatic increase in the total thermal conductivity (kappa) is observed in the hidden order (HO) state of single crystal URu2Si2. Through measurements of the thermal Hall conductivity, we explicitly show that the electronic contribution to kappa is extremely small, so that this large increase in kappa is dominated by phonon conduction. An itinerant BCS or mean-field model describes this behavior well: the increase in kappa is associated with the opening of a large energy gap at the Fermi surface, thereby decreasing electron-phonon scattering. Our analysis implies that the "hidden order" parameter is strongly coupled to the lattice, suggestive of a broken symmetry involving charge degrees of freedom.

Optical pseudogap from iron states in filled skutterudites AFe4Sb12 (A=Yb, Ca, Ba).

Optical investigations are presented of the filled skutterudites AFe4Sb12 with divalent cations A=Yb, Ca, Ba. For each of these compounds a very similar pseudogap structure in the optical conductivity develops in the far-infrared spectral region at temperatures below 90 K. Highly accurate local-density approximation electronic band structure calculations can consistently explain the origin of the pseudogap structure generated largely by transition metal 3d states. In particular, a 4f-conduction electron hybridization or strong correlations can be ruled out as origin for the pseudogap.

Irreversible dynamics of the phase boundary in U(Ru0.96Rh0.04)2Si2 and implications for ordering.

We report measurements and analysis of the specific heat and magnetocaloric effect-induced temperature changes at the phase boundary into the single magnetic field-induced phase (phase II) of U(Ru0.96Rh0.04)2Si2, which yield irreversible properties similar to those at the valence transition of Yb(1-x)Y(x)InCu4. To explain these similarities, we propose a bootstrap mechanism by which lattice parameter changes caused by an electric quadrupolar order parameter within phase II become coupled to the 5f-electron hybridization, giving rise to a valence change at the transition.

Complete elastic tensor through the first-order transformation in U2Rh3Si5.

The complete elastic tensor of U(2)Rh(3)Si(5) has been determined over the temperature range of 5-300 K, including the dramatic first-order transition to an antiferromagnetic state at 25.5 K. Sharp upward steps in the elastic moduli as the temperature is decreased through the transition reveal the first-order nature of the phase change. In the antiferromagnetic state the temperature dependence of the elastic moduli scales with the square of the ordered moment on the uranium ion, demonstrating strong spin-lattice coupling. The temperature dependence of the moduli well above the transition indicates coupling of the ultrasonic waves to the crystal electric field levels of the uranium ion where the lowest state is a singlet. The elastic constant data suggest that the first-order phase change is magnetically driven by a bootstrap mechanism involving the ground state singlet and a magnetically active crystal electric field level.

Quantum critical 5f electrons avoid singularities in U(Ru,Rh)2Si2.

We present specific heat measurements of 4% Rh-doped URu2Si2 at magnetic fields around the proposed metamagnetic transition field H(m) approximately 34 T, revealing striking similarities to the isotructural Ce analog CeRu2Si2 for H>H(m). This suggests that strongly renormalized hybridized-band models apply equally well to both systems. The vanishing bandwidths as H-->H(m) are consistent with a quantum-critical point close to H(m). The existence of a phase transition into an ordered phase in the vicinity of H(m) for 4% Rh-doped URu2Si2, but not for CeRu2Si2, is consistent with a stronger superexchange in the case of the U 5f system. Irreversible processes at the transition indicate a strong coupling of the 5f orbitals to the lattice, most suggestive of electric quadrupolar order.

Reentrant hidden order at a metamagnetic quantum critical end point.

Magnetization measurements of URu2Si2 in pulsed magnetic fields of 44 T reveal that the hidden order phase is destroyed before appearing in the form of a reentrant phase between approximately 36 and 39 T. Evidence for conventional itinerant electron metamagnetism at higher temperatures suggests that the reentrant phase is created in the vicinity of a quantum critical end point.