We study Na2IrO3 by angle-resolved photoemission spectroscopy, optics, and band structure calculations in the local-density approximation (LDA). The weak dispersion of the Ir 5d-t(2g) manifold highlights the importance of structural distortions and spin-orbit (SO) coupling in driving the system closer to a Mott transition. We detect an insulating gap Δ(gap)≃340  meV which, at variance with a Slater-type description, is already open at 300 K and does not show significant temperature dependence even across T(N)≃15  K. An LDA analysis with the inclusion of SO and Coulomb repulsion U reveals that, while the prodromes of an underlying insulating state are already found in LDA+SO, the correct gap magnitude can only be reproduced by LDA+SO+U, with U=3  eV. This establishes Na2IrO3 as a novel type of Mott-like correlated insulator in which Coulomb and relativistic effects have to be treated on an equal footing.

Cuprate high-T c superconductors exhibit enigmatic behavior in the nonsuperconducting state. For carrier concentrations near "optimal doping" (with respect to the highest T c s) the transport and spectroscopic properties are unlike those of a Landau-Fermi liquid. On the Mott-insulating side of the optimal carrier concentration, which corresponds to underdoping, a pseudogap removes quasiparticle spectral weight from parts of the Fermi surface and causes a breakup of the Fermi surface into disconnected nodal and antinodal sectors. Here, we show that the near-nodal excitations of underdoped cuprates obey Fermi liquid behavior. The lifetime τ(ω, T) of a quasi-particle depends on its energy ω as well as on the temperature T. For a Fermi liquid, 1/τ(ω, T) is expected to collapse on a universal function proportional to (h ω) 2 + (pπk B T) 2 . Magnetotransport experiments, which probe the properties in the limit ω = 0, have provided indications for the presence of a T 2 dependence of the dc (ω = 0) resistivity of different cuprate materials. However, Fermi liquid behavior is very much about the energy dependence of the lifetime, and this can only be addressed by spectroscopic techniques. Our optical experiments confirm the aforementioned universal ω-and T dependence of 1/τ(ω, T), with p ∼ 1.5. Our data thus provide a piece of evidence in favor of a Fermi liquid-like scenario of the pseudogap phase of the cuprates.optical spectroscopy | superconductivity | mass renormalization | self energy T he compound HgBa 2 CuO 4+δ (Hg1201) is the single-layer cuprate that exhibits the highest T c (97 K). We therefore measured the optical conductivity of strongly underdoped single crystals of Hg1201 ðT c = 67 KÞ. Here we are interested in the optical conductivity of the CuO 2 layers. We therefore express the optical conductivity as a 2D sheet conductance GðωÞ = d c σðωÞ, where d c is the interlayer spacing. The real part of the sheet conductance normalized by the conduction quantum G 0 = 2e 2 =h is shown in Fig. 1. As seen in the figure, a gap-like suppression below 140 meV is clearly observable for temperatures below T c and remains visible in the normal state up to ∼250 K. This is a clear optical signature of the pseudogap. We also observe the zero-energy mode due to the free charge carrier response, which progressively narrows upon lowering the temperature. In materials where the charge carrier relaxation is dominated by impurity scattering, the width of this "Drude" peak corresponds to the relaxation rate of the charge carriers. Relaxation processes arising from interactions have the effect of replacing the constant (frequency-independent) relaxation rate with a frequencydependent one. The general expression for the optical conductivity of interacting electrons is then Gðω; TÞ = iπK Zω + Mðω; TÞ G 0 :[1]The spectral weight K corresponds to minus the kinetic energy if the frequency integration of the experimental data is restricted to intraband transitions. The effect of electron-electron interactions and coupling to collective mo...

We measured the momentum dependence of magnetic excitations in the model spin-1=2 2D antiferromagnetic insulator Sr 2 CuO 2 Cl 2 (SCOC). We identify a single-spin-wave feature and a multimagnon continuum, with different polarization dependences. The spin waves display a large (70 meV) dispersion between the zone-boundary points (, 0) and (=2, =2). Employing an extended t-t 0 -t 00 -U one-band Hubbard model, we find significant electronic hopping beyond nearest-neighbor Cu ions, indicative of extended magnetic interactions. The spectral line shape at (, 0) indicates sizable quantum effects in SCOC and probably more generally in the cuprates. DOI: 10.1103/PhysRevLett.105.157006 PACS numbers: 74.72.Cj, 75.30.Ds, 78.70.Ck Magnetism in low-dimensional cuprates remains of considerable interest, in relation both to the fundamental quest to understand strong electron correlation and quantum spin effects in Mott insulators, and to the search for the mechanism of high-T c superconductivity. To lowest order, the undoped cuprate superconductors can be described by the spin 1=2 two-dimensional (2D) square-lattice nearestneighbor (NN) Heisenberg antiferromagnet, which is among the simplest and most studied models in magnetism [1]. The ground state displays classical order, reduced by quantum fluctuations at zero temperature and destroyed by thermal fluctuations at finite temperature. A possible crossover between renormalized classical [2] and quantum critical [3] scaling was tested experimentally in the undoped cuprates Sr 2 CuO 2 Cl 2 (SCOC) [4] and La 2 CuO 4 (LCO) [5], and in the organometallic salt CuðDCOOÞ 2 Á 4D 2 O (CFTD) [6]. However, while the latter shows only nearest-neighbor coupling, high-energy inelastic neutron scattering (INS) data on LCO [7] suggest that further-neighbor magnetic interactions influence the scaling measurements. Frustrated further-neighbor interactions could also bring the undoped cuprates closer to the valence bond liquid proposed as mechanism for superconductivity [8].It is therefore timely to investigate the excitation spectrum of SCOC, as an important model system. Inelastic neutron scattering (INS) measurements of SCOC have been limited to low energies and small momenta around the ordering wave vector [4]. In this Letter we report the full magnetic excitation spectrum measured by resonant inelastic x-ray scattering (RIXS). We discover a surprisingly large dispersion along the magnetic Brillouin zone boundary (ZB). An analysis of the data in terms of an extended Hubbard model yields a quantitative estimation of sizable further-neighbor electronic hopping. The resulting series of longer-ranged magnetic interactions enhance quantum fluctuations, in agreement with the reduced ordered moment. The importance of quantum fluctuations is further revealed by differences in the spectral line shapes at the (À, 0) and (À=2, =2) ZB points.SCOC is an insulating single-layer parent compound of the high-T c superconducting (SC) materials. It is isostructural to the high-temperature tetragonal phase of...

Perovskite structured materials contain myriad tunable ordered phases of electronic and magnetic origin with proven technological importance and strong promise for a variety of energy solutions. An always-contributing influence beneath these cooperative and competing interactions is the lattice, whose physics may be obscured in complex perovskites by the many coupled degrees of freedom, which makes these systems interesting. Here, we report signatures of an approach to a quantum phase transition very near the ground state of the nonmagnetic, ionic insulating, simple cubic perovskite material ScF 3 , and show that its physical properties are strongly effected as much as 100 K above the putative transition. Spatial and temporal correlations in the high-symmetry cubic phase determined using energy-and momentum-resolved inelastic x-ray scattering as well as x-ray diffraction reveal that soft mode, central peak, and thermal expansion phenomena are all strongly influenced by the transition. The class of materials with the perovskite structure and chemical formula ABX 3 contains examples of perhaps every possible type of physical behavior [1,2], much of which is difficult to understand because of the shear complexity of matter. A rich terrain of structural transitions associated with BX 6 octahedral tilting in perovskites strongly effects electronic conduction and magnetic exchange pathways, defining the framework of interactions governing a range of physical properties. The A-site tolerance appears to be an important parameter in determining the structural phase stability [1-3], but stable A-site-free perovskite structures are also thermodynamically stable. These are rare cases among oxides (X = O) because the B ions must take on rare hexavalent (+6) electronic configurations, and the only known instance is ReO 3 . In perovskites based on fluorine (X = F), however, the B ions assume the common trivalent (+3) configuration in an expanded suite of A-site-free perovskite lattices.Figure 1(a) shows a structural phase diagram of BF 3 perovskites, where B is a trivalent metal ion [4]. The 3d metal trifluorides display a reversible [5] structural cubic-torhombohedral (c-r) phase boundary. This sequence of 3d transition metal trifluoride compounds is rhombohedral at room temperature, with the exception of B = Sc, which appears at the zero-temperature terminated c-r phase boundary. Indeed, no rhombohedral phase transition has been observed for ScF 3 down to 0.4 K [6], suggesting that near this composition, the structural phase can be driven by a parameter other than temperature, implying that the ground state of this ionic insulator is very near a quantum phase transition (QPT). Cubic ScF 3 further stands out among substances in that it has the most stable structural phase of any known solid trifluoride, * Corresponding author: jason.hancock@uconn.edu retaining high cubic symmetry and a four-atom unit cell up to its high melting point, >1800 K [6,7]. Separate from the QPT reported here, further interest in this system is due t...

An infrared study of the phonon spectra of ZrW2O8 as a function of temperature which includes the low-energy (2-10 meV) region relevant to negative thermal expansion is reported and discussed in the context of specific heat and neutron density of state results. The prevalence of infrared active phonons at low energy and their observed temperature dependence are highly unusual and indicative of exotic low-energy lattice dynamics. Eigenvector calculations indicate a mixing of librational and translational motion within each low-frequency IR mode. The role of the underconstrained structure in establishing the nature of these modes and the relationship between the IR spectra and the large negative thermal expansion in ZrW2O8 are discussed.

Theoretical work on Kondo systems predicts universality in the scaling of observable quantities with the Kondo temperature, T(K). Here we report infrared-frequency optical response measurements of the correlated system YbIn(1-x)AgxCu4. We observe that x-dependent variations in the frequency and strength of a low-energy excitation are related to the x-dependent Kondo temperature. Comparison of the inferred trends with existing theory and a model calculation provides a framework in which to view these experimental results as scaling phenomena arising from local-moment/conduction electron hybridization.

We present a detailed Cu K-edge resonant inelastic X-ray scattering (RIXS) study of the Mott insulator La2CuO4 in the 1-7 eV energy loss range. As initially found for the high-temperature superconductor HgBa2CuO 4+δ , the spectra exhibit a multiplet of weakly-dispersive electron-hole excitations, which are revealed by utilizing the subtle dependence of the cross section on the incident photon energy. The close similarity between the fine structures for in-plane and out-of-plane polarizations is indicative of the central role played by the 1s core hole in inducing charge excitations within the CuO2 planes. On the other hand, we observe a polarization dependence of the spectral weight, and careful analysis reveals two separate features near 2 eV that may be related to different processes. The polarization dependence indicates that the 4p electrons contribute significantly to the RIXS cross section. Third-order perturbation arguments and a shake-up of valence excitations are then applied to account for the final-energy resonance in the spectra. As an alternative scenario, we discuss fluorescence-like emission processes due to 1s → 4p transitions into a narrow continuum 4p band.

We report a Cu -edge resonant inelastic x-ray scattering (RIXS) study of charge-transfer excitations in the 2-8 eV range in the structurally simple compound HgBa(2)CuO(4+delta) at optimal doping (T(c)=96.5 K). The spectra exhibit a significant dependence on the incident photon energy which we carefully utilize to resolve a multiplet of weakly dispersive (<0.5 eV) electron-hole excitations, including a mode at 2 eV. The observation of this 2 eV excitation suggests the existence of a remnant charge-transfer gap deep in the superconducting phase. Quite generally, our results, which include additional data for the Mott insulator La(2)CuO(4), demonstrate the importance of exploring the incident photon-energy dependence of the RIXS cross section.