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 (AF) phase above $x_c$. By using polarization resolved Raman spectroscopy, we detect a collective mode of pseudovector-like $A_{2g}$ 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 AF phase. The mode's evolution provides direct evidence for unified order parameter for both nonmagnetic and magnetic phases arising from the orbital degrees-of-freedom of the uranium-5$f$ electrons.
We report simultaneous measurements of the distribution of lattice constants and the antiferromagnetic moment in high-purity URu2Si2, using both Larmor and conventional neutron diffraction, as a function of temperature and pressure up to 18 kbar. We establish that the tiny moment in the hidden order (HO) state is purely parasitic and quantitatively originates from the distribution of lattice constants. Moreover, the HO and large-moment antiferromagnetism (LMAF) at high pressure are separated by a line of first-order phase transitions, which ends in a bicritical point. Thus the HO and LMAF are …
We present muon spin rotation ($μ$SR) and susceptibility measurements on single crystals of isoelectronically doped URu$_{2-x}$T$_x$Si$_2$ (T = Fe, Os) for doping levels up to 50\%. Zero Field (ZF) $μ$SR measurements show long-lived oscillations demonstrating that an antiferromagnetic state exists down to low doping levels for both Os and Fe dopants. The measurements further show an increase in the internal field with doping for both Fe and Os. Comparison of the local moment - hybridization crossover temperature from susceptibility measurements and our magnetic transition temperature shows tha…
We report $^{31}$P and $^{29}$Si NMR in single crystals of URu$_2$Si$_{2-x}$P$_x$ for $x=0.09$ and $x=0.33$. The spectra in the $x=0.33$ sample are consistent with a homogenous commensurate antiferromagnetic phase below $T_N \sim 37$ K. The Knight shift exhibits an anomaly at the coherence temperature, $T^*$, that is slightly enhanced with P doping. Spin lattice relaxation rate data indicate that the density of states is suppressed for $x=0.09$ below 30 K, similar to the undoped compound, but there is no evidence of long range order at this concentration. Our results suggest that Si substituti…
The weak antiferromagnetism of URu${}_{2}$Si${}_{2}$ is discussed on the basis of a duality model which takes into account salient features of both itinerant fermions and "localized" component of spin degrees of freedom. The problem is analyzed in the framework of induced-moment mechanism by taking a singlet-singlet crystal field scheme together with the nesting property of partial Fermi surface of itinerant fermions . It is shown that the extremely small ordered moment $m$ of ${\cal O}$($10^{-2}$$\times$$μ_{B}$) can be compatible with the large specific-heat jump at the transition temperature…
We argue that key characteristics of the enigmatic transition at $T_0= 17.5K $ in $URu_2Si_2$ indicate that the hidden order is a density wave formed within a band of composite quasiparticles, whose detailed structure is determined by local physics. We expand on our proposal (with J.A. Mydosh) of the hidden order as incommnesurate orbital antiferromagnetism and present experimental predictions to test our ideas. We then turn towards a microscopic description of orbital antiferromagnetism, exploring possible particle-hole pairings within the context of a simple one-band model. We end with a dis…
Motivated by experiment, we review the case for phase inhomogeneity in URu_2Si_2. In this scenario, the paramagnetic hidden order phase coexists with small distinct domains of antiferromagnetism whose volume fraction increases with pressure. The implications for the nature of the hidden order are discu ssed.
We report the use of impurities to probe the hidden order parameter of the strongly correlated metal URu_2Si_2 below the transition temperature T_0 ~ 17.5 K. The nature of this order parameter has eluded researchers for more than two decades, but is accompanied by the development of a partial gap in the single particle density of states that can be detected through measurements of the electronic specific heat and nuclear spin-lattice relaxation rate. We find that impurities in the hidden order phase give rise to local patches of antiferromagnetism. An analysis of the coupling between the antif…
In matter, any spontaneous symmetry breaking induces a phase transition characterized by an order parameter, such as the magnetization vector in ferromagnets, or a macroscopic many-electron wave-function in superconductors. Phase transitions with unknown order parameter are rare but extremely appealing, as they may lead to novel physics. An emblematic, and still unsolved, example is the transition of the heavy fermion compound URu$_2$Si$_2$ (URS) into the so-called hidden-order (HO) phase when the temperature drops below $T_0 = 17.5$K. Here we show that the interaction between the heavy fermio…
The recent experimental finding of large-amplitude antiferromagnetism induced by uniaxial strain shows that the "hidden" low-field order of URu2Si2 breaks time reversal invariance. We propose a new crystal field model which supports T(beta)z octupolar order in the low-field phase, and quadrupolar order in a disjoint high-field phase. The temperature dependence of the linear and third order magnetic susceptibility is in good agreement with the observed behavior.
We have performed elastic neutron scattering experiments under uniaxial stress sigma applied along the tetragonal [100], [110] and [001] directions for the heavy electron compound URu2Si2. We found that antiferromagnetic (AF) order with large moment is developed with sigma along the [100] and [110] directions. If the order is assumed to be homogeneous, the staggered ordered moment mu_o continuously increases from 0.02 mu_B (sigma=0) to 0.22 mu_B (0.25 GPa). The rate of increase partial mu_o/partial sigma is ~ 1.0 mu_B/GPa, which is four times larger than that for the hydrostatic pressure (part…
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 $x…
We discuss the discovery of pressure-induced antiferromagnetism in URu_2Si_2, in the context of neutron, NMR and μSR results. The identification of a critical pressure separating mean-field and Ising phase transitions leads us to propose that the system lies close to a bicritical point associated with magnetic and (non-magnetic) hidden order. We conclude that the recent observation of an isotropic, field-independent component in the silicon NMR line-width implies that the hidden order parameter breaks time-reversal invariance and present a preliminary discussion of the underlying nature of the…
Calorimetry experiments under high pressure were used to clarify the interplay between different states such as superconductivity and antiferromagnetism in CeRhIn5, spin density wave and large moment antiferromagnetism in URu2Si2. Evidences are given on the re-entrance of antiferromagnetism under magnetic field in the superconducting phase of CeRhIn5 up to pc = 2.5 GPa where the Neel temperature will collapse in the absence of superconductivity. For URu2Si2 measurements up to 10 GPa support strongly the coexistence of spin density wave and large moment antiferromagnetism at high pressures.
We report a neutron scattering study of the magnetic excitation spectrum in each of the three temperature and pressure driven phases of URu$_2$Si$_2$. We find qualitatively similar excitations throughout the (H0L) scattering plane in the hidden order and large moment phases, with no changes in the $\hbarω$-widths of the excitations at the $Σ$ = (1.407,0,0) and $Z$ = (1,0,0) points, within our experimental resolution. There is, however, an increase in the gap at the $Σ$ point from 4.2(2) meV to 5.5(3) meV, consistent with other indicators of enhanced antiferromagnetism under pressure.
When matter is cooled from high temperatures, collective instabilities develop amongst its constituent particles that lead to new kinds of order. An anomaly in the specific heat is a classic signature of this phenomenon. Usually the associated order is easily identified, but sometimes its nature remains elusive. The heavy fermion metal $URu_2Si_2$ is one such example, where the order responsible for the sharp specific heat anomaly at $T_0=17 K$ has remained unidentified despite more than seventeen years of effort. In $URu_{2}Si_{2}$, the coexistence of large electron-electron repulsion and ant…
The large $Δ$C observed at 17.5 K in URu$_{2}$Si$_{2}$ is inconsistent with the small, 0.04 $μ_{B}$ moment measured for the antiferromagnetism observed starting (perhaps coincidentally) at the same temperature. We report measurements of this specific heat transition, thought to be due to some 'hidden order', in magnetic fields between 24 and 42 T, i. e. through the field region where three metamagnetic transtions are known to occur at 35.8, 37.3, and 39.4 T. The response of $Δ$C in single crystal URu$_{2}$Si$_{2}$ to magnetic field, which includes a change to $Δ$C being possibly associated wit…
Combination of neutron scattering and thermal expansion measurements under pressure shows that the so-called hidden order phase of URu2Si2 reenters in magnetic field when antiferromagnetism (AF) collapses at H_AF (T). Macroscopic pressure studies of the HO-AF boundaries were realized at different pressures via thermal expansion measurements under magnetic field using a strain gauge. Microscopic proof at a given pressure is the reappearance of the resonance at Q_0=(1,0,0) under field which is correlated with the collapse of the AF Bragg reflections at Q_0.
The heavy-fermion compound URu2Si2 exhibits a hidden-order phase below the temperature, ~ 17.5 K. In spite of intense research for past three decades, no consensus on the order parameter exists and the nature has posed a long-standing mystery. Here we report the discovery of a Griffiths phase within the hidden-order phase, characterized by residual short-range correlations on the collapse of long-range orders due to the dilution effects. In the Griffiths phase scenario, strong evidence are provided for those cluster-like spins, such as the unique power-law behavior of magnetic susceptibility a…
Recent experiments on URu2Si2 show that the low-pressure hidden order is non-magnetic but it breaks time reversal invariance. Restricting our attention to local order parameters of 5f2 shells, we find that the best candidate for hidden order is staggered order of either Tz(beta) or Txyz octupoles. Group theoretical arguments for the effect of symmetry-lowering perturbations (magnetic field, mechanical stress) predict behavior in good overall agreement with observations. We illustrate our general arguments on the example of a five-state crystal field model which differs in several details from …
We report low-energy inelastic neutron scattering data of the paramagnetic (PM) to hidden-order (HO) phase transition at $T_0=17.5\,{\rm K}$ in URu$_2$Si$_2$. While confirming previous results for the HO and PM phases, our data reveal a pronounced wavevector dependence of low-energy excitations across the phase transition. To analyze the energy scans we employ a damped harmonic oscillator model containing a fit parameter $1/Γ$ which is expected to diverge at a second-order phase transition. Counter to expectations the excitations at $\vec{Q}_1=(1.44,0,0)$ show an abrupt step-like suppression o…
We use neutron scattering to compare the magnetic excitations in the hidden order (HO) and antiferromagnetic (AFM) phases in URu2-xFexSi2 as a function of Fe concentration. The magnetic excitation spectra change significantly between x = 0.05 and x = 0.10, following the enhancement of the AFM ordered moment, in good analogy to the behavior of the parent compound under applied pressure. Prominent lattice-commensurate low-energy excitations characteristic of the HO phase vanish in the AFM phase. The magnetic scattering is dominated by strong excitations along the Brillouin zone edges, underscori…
The hidden order phase in URu$_2$Si$_2$ is highly sensitive to electronic doping. A special interest in silicon-to-phosphorus substitution is due to the fact that it may allow one, in part, to isolate the effects of tuning the chemical potential from the complexity of the correlated $f$ and $d$ electronic states. We investigate the new antiferromagnetic phase that is induced in URu$_2$Si$_{2-x}$P$_x$ at $x\gtrsim0.27$. Time-of-flight neutron diffraction of a single crystal ($x=0.28$) reveals $c$-axis collinear $\mathbf{q}_\mathrm{m}=(\frac12,\frac12,\frac12)$ magnetic structure with localized …
A brief review on major advances in heavy fermion physics is presented including the Ce metal phase diagram, the huge effective mass detected in CeAl3, and the successive discoveries of unconventional superconductivity in CeCu2Si2 and three U based compounds, UBe13, UPt3 and URu2Si2. In order to track the origin of the huge effective mass, the case of intermediate valence compounds is discussed with emphasis of the differences between Yb and Ce materials. The formation of the effective mass is analyzed by two regular- and singular-part contributions. Examples are given for both, antiferromagne…
To resolve the nature of the hidden order below 17.5\,K in the heavy fermion compound URu$_2$Si$_2$, identifying which symmetries are broken below the hidden order transition is one of the most important steps. Several recent experiments on the electronic structure have shown that the Fermi surface in the hidden order phase is quite close to the result of band-structure calculations within the framework of itinerant electron picture assuming the antiferromagnetism. This provides strong evidence for the band folding along the c-axis with the ordering vector of $(0\,0\,1)$, corresponding to brok…
By ab initio many-body quantum chemistry calculations, we determine the strength of the symmetric anisotropy in the 5$d^5$ j $\approx$ 1/2 layered material Ba$_2$IrO$_4$. While the calculated anisotropic couplings come out in the range of a few meV, orders of magnitude stronger than in analogous 3d transition-metal compounds, the Heisenberg superexchange still defines the largest energy scale. The ab initio results reveal that individual layers of Ba$_2$IrO$_4$ provide a close realization of the quantum spin-1/2 Heisenberg-compass model on the square lattice. We show that the experimentally ob…
We report on detailed ac calorimetry measurements under high pressure and magnetic field of CeRhIn5. Under hydrostatic pressure the antiferromagnetic order vanishes near p_c*=2 GPa due to a first order transition. Superconductivity is found for pressures above 1.5 GPa inside the magnetic ordered phase. However, the superconductivity differ from the pure homogeneous superconducting ground state above 2 GPa. The application of an external magnetic field H || ab induces a transition inside the superconducting state above pc* which is strongly related to the re-entrance of the antiferromagnetism w…
We use the effective potential method of quantum field theory to obtain the quantum corrections to the zero temperature phase diagram of systems with competing order parameters. We are particularly interested in two different scenarios: regions of the phase diagram where there is a bicritical point, at which both phases vanish continuously, and the case where both phases coexist homogeneously. We consider different types of couplings between the order parameters, including a bilinear one. This kind of coupling breaks time-reversal symmetry and it is only allowed if both order parameters transf…
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…
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$_…
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…
Motivated by pressure experiments on FeAs-122 superconductors, we propose a scenario based on local-moment physics to explain the simultaneous disappearance of magnetism, reduction of the unit cell volume, and decrease in resistivity. In this scenario, the low-pressure magnetic phase derives from Fe moments, which become screened in the paramagnetic high-pressure phase. The quantum phase transition can be described as an orbital-selective Mott transition, which is rendered first order by coupling to the lattice, in analogy to a Kondo volume collapse. Spin-fluctuation driven superconductivity c…
