Electronic Spectral Weight Research Articles

Electronic interactions in Dirac fluids visualized by nano-terahertz spacetime interference of electron-photon quasiparticles.

Ultraclean graphene at charge neutrality hosts a quantum critical Dirac fluid of interacting electrons and holes. Interactions profoundly affect the charge dynamics of graphene, which is encoded in the properties of its electron-photon collective modes: surface plasmon polaritons (SPPs). Here, we show that polaritonic interference patterns are particularly well suited to unveil the interactions in Dirac fluids by tracking polaritonic interference in time at temporal scales commensurate with the electronic scattering. Spacetime SPP interference patterns recorded in terahertz (THz) frequency range provided unobstructed readouts of the group velocity and lifetime of polariton that can be directly mapped onto the electronic spectral weight and the relaxation rate. Our data uncovered prominent departures of the electron dynamics from the predictions of the conventional Fermi-liquid theory. The deviations are particularly strong when the densities of electrons and holes are approximately equal. The proposed spacetime imaging methodology can be broadly applied to probe the electrodynamics of quantum materials.

Joule heating in bad and slow metals

Heat supplied to a metal is absorbed by the electrons and then transferred to the lattice. In conventional metals energy is released to the lattice by phonons emitted from the Lindhard continuum. However in a 'bad' metal, with short mean free path, the low energy Lindhard continuum is destroyed. To describe energy transfer to the lattice in these cases we obtain a general Kubo formula for the energy relaxation rate in terms of the electronic density spectral weight \text{lm} \, G^R_{nn}(\omega_{k},k)lmGnnR(ωk,k) evaluated on the phonon dispersion \omega_kωk. We apply our Kubo formula to the high temperature Hubbard model, using recent data from quantum Monte Carlo and experiments in ultracold atoms to characterize \text{lm} \, G^R_{nn}(\omega_{k},k)lmGnnR(ωk,k). We furthermore use recent data from electron energy-loss spectroscopy to estimate the energy relaxation rate of the cuprate strange metal to a high energy optical phonon. As a second, distinct, application of our formalism we consider 'slow' metals. These are defined to have Fermi velocity less than the sound velocity, so that particle-hole pairs are kinematically unable to emit phonons. We obtain an expression for the energy relaxation rate of a slow metal in terms of the optical conductivity.

Correlation strength, orbital-selective incoherence, and local moments formation in the magnetic MAX-phaseMn2GaC

We perform a theoretical study of the electronic structure and magnetic properties of the prototypical magnetic MAX-phase Mn$_2$GaC with the main focus given to the origin of magnetic interactions in this system. Using the density functional theory+dynamical mean-field theory (DFT+DMFT) method we explore the effects of electron-electron interactions and magnetic correlations on the electronic properties, magnetic state, and spectral weight coherence of paramagnetic and magnetically-ordered phases of Mn$_2$GaC. We also benchmark the DFT-based disordered local moment approach for this system by comparing the obtained electronic and magnetic properties with that of the DFT+DMFT method. Our results reveal a complex magnetic behavior characterized by a near degeneracy of the ferro- and antiferromagnetic configurations of Mn$_2$GaC, implying a high sensitivity of its magnetic state to fine details of the crystal structure and unit-cell volume, consistent with experimental observations. We observe robust local-moment behavior and orbital-selective incoherence of the spectral properties of Mn$_2$GaC, implying the importance of orbital-dependent localization of the Mn $3d$ states. We find that Mn$_2$GaC can be described in terms of local magnetic moments, which may be modeled by DFT with disordered local moments. However, the magnetic properties are dictated by the proximity to the regime of formation of local magnetic moments, in which the localization is in fact driven by the Hund's exchange interaction, and not the Coulomb interaction.

Photoemission signature of momentum-dependent hybridization in CeCoIn5

Hybridization between $f$ electrons and conduction bands ($c$-$f$ hybridization) is a driving force for many unusual phenomena. To provide insight into it, systematic studies of CeCoIn$_5$ heavy fermion superconductor have been performed by angle-resolved photoemission spectroscopy (ARPES) in a large angular range at temperature of $T=6$ K. The used photon energy of 122 eV corresponds to Ce $4d$-$4f$ resonance. Calculations carried out with relativistic multiple scattering Korringa-Kohn-Rostoker method and one-step model of photoemission yielded realistic simulation of the ARPES spectra indicating that Ce-In surface termination prevails. Surface states, which have been identified in the calculations, contribute significantly to the spectra. Effects of the hybridization strongly depend on wave vector. They include a dispersion of heavy electrons and bands gaining $f$-electron character when approaching Fermi energy. We have also observed a considerable variation of $f$-electron spectral weight at $E_F$, which is normally determined by both matrix element effects and wave vector dependent $c$-$f$ hybridization. Fermi surface scans covering a few Brillouin zones revealed large matrix element effects. A symmetrization of experimental Fermi surface, which reduces matrix element contribution, yielded a specific variation of $4f$-electron enhanced spectral intensity at $E_F$ around $\bar{\Gamma}$ and $\bar{M}$ points. Tight-binding approximation calculations for Ce-In plane provided the same universal distribution of $4f$-electron density for a range of values of the parameters used in the model.

Quantum spin fluctuations and evolution of electronic structure in cuprates

Correlation effects in CuO2 layers give rise to a complicated landscape of collective excitations in high-Tc cuprates. Their description requires an accurate account for electronic fluctuations at a very broad energy range and remains a challenge for the theory. Particularly, there is no conventional explanation of the experimentally observed “resonant” antiferromagnetic mode, which is often considered to be a mediator of superconductivity. Here we model spin excitations of the hole-doped cuprates in the paramagnetic regime and show that this antiferromagnetic mode is associated with electronic transitions between anti-nodal X and Y points of the quasiparticle band that is pinned to the Fermi level. We observe that upon doping of 7–12%, the electronic spectral weight redistribution leads to the formation of a very stable quasiparticle dispersion due to strong correlation effects. The reconstruction of the Fermi surface results in a flattening of the quasiparticle band at the vicinity of the nodal MΓ/2 point, accompanied by a high density of charge carriers. Collective excitations of electrons between the nodal MΓ/2 and XM/2 points form the additional magnetic holes state in magnetic spectrum, which protects the antiferromagnetic fluctuation. Further investigation of the evolution of spin fluctuations with the temperature and doping allowed us to observe the incipience of the antiferromagnetic ordering already in the paramagnetic regime above the transition temperature. Additionally, apart from the most intensive low-energy magnetic excitations, the magnetic spectrum reveals less intensive collective spin fluctuations that correspond to electronic processes between peaks of the single-particle spectral function.

Pseudogap-generated a coexistence of Fermi arcs and Fermi pockets in cuprate superconductors

One of the most intriguing puzzle is why there is a coexistence of Fermi arcs and Fermi pockets in the pseudogap phase of cuprate superconductors? This puzzle is calling for an explanation. Based on the t−J model in the fermion-spin representation, the coexistence of the Fermi arcs and Fermi pockets in cuprate superconductors is studied by taking into account the pseudogap effect. It is shown that the pseudogap induces an energy band splitting, and then the poles of the electron Green’s function at zero energy form two contours in momentum space, however, the electron spectral weight on these two contours around the antinodal region is gapped out by the pseudogap, leaving behind the low-energy electron spectral weight only located at the disconnected segments around the nodal region. In particular, the tips of these disconnected segments converge on the hot spots to form the closed Fermi pockets, generating a coexistence of the Fermi arcs and Fermi pockets. Moreover, the single-particle coherent weight is directly related to the pseudogap, and grows linearly with doping. The calculated result of the overall dispersion of the electron excitations is in qualitative agreement with the experimental data. The theory also predicts that the pseudogap-induced peak-dip-hump structure in the electron spectrum is absent from the hot-spot directions.

Enhanced Crystallization Behaviors of Silicon-Doped Sb2Te Films: Optical Evidences.

The optical properties and structural variations of silicon (Si) doped Sb2Te (SST) films as functions of temperature (210–620 K) and Si concentration (0–33%) have been investigated by the means of temperature dependent Raman scattering and spectroscopic ellipsometry experiments. Based upon the changes in Raman phonon modes and dielectric functions, it can be concluded that the temperature ranges for intermediates and transition states are estimated to 150, 120, 90, and 0 K, corresponding to ST, SST25%, SST28%, and SST33% films, respectively. The phenomenon also can be summarized by the thermal evolutions of interband electronic transition energies (En) and partial spectral weight integral (I). The disappearance of intermediate (INT) state for SST33% film between amorphous (AM) and hexagonal (HEX) phases can be attributed to the acceleratory crystallization of HEX phase by Si introduction. It illustrates that the risk of phase separation (Sb and Te) during the cyclic phase-change processes decreases with the increasing Si concentration. The enhanced crystallization behaviors can optimize the data retention ability and the long term stability of ST by Si doping, which are important indicators for phase change materials. The performance improvement has been analyzed qualitatively from the optical perspective.

Robustness of quantum critical pairing against disorder

The remarkable robustness of high-temperature superconductors against disorder remains a controversial obstacle towards the elucidation of their pairing state. Indeed, experiments report a weak suppression rate of the transition temperature $T_{c}$ with disorder, significantly smaller than the universal value predicted by extensions of the conventional theory of dirty superconductors. However, in many high-$T_{c}$ compounds, superconductivity appears near a putative magnetic quantum critical point, suggesting that quantum fluctuations, which suppress coherent electronic spectral weight, may also promote unconventional pairing. Here we investigate theoretically the impact of disorder on such a quantum critical pairing state, considering the coupling of impurities both to the low-energy electronic states and to the pairing interaction itself. We find a significant reduction in the suppression rate of $T_{c}$ with disorder near the magnetic quantum critical point, shedding new light on the nature of unconventional superconductivity in correlated materials.

Electronic structure in a one-Fe Brillouin zone of the iron pnictide superconductorsCsFe2As2andRbFe2As2

The multiband nature of iron-pnictide superconductors is one of the keys to the understanding of their intriguing behavior. The electronic and magnetic properties heavily rely on the multiband interactions between different electron and hole pockets near the Fermi level. At the fundamental level, though many theoretical models were constructed on the basis of the so-called 1-Fe Brillouin zone (BZ) with an emphasis of the basic square lattice of iron atoms, most electronic structure measurements were interpreted in the 2-Fe BZ. Whether the 1-Fe BZ is valid in a real system is still an open question. Using angle-resolved photoemission spectroscopy (ARPES), here we show in an extremely hole-doped iron-pnictide superconductor CsFe$_2$As$_2$ that the distribution of electronic spectral weight follows the 1-Fe BZ, and that the emerging band structure bears some features qualitatively different from theoretical band structures of the 1-Fe BZ. Our analysis suggests that the interlayer separation is an important tuning factor for the physics of FeAs layers, the increase of which can reduce the coupling between Fe and As and lead to the emergence of the electronic structure in accord with the 1-Fe symmetry of the Fe square lattice. Our finding puts strong constraints on the theoretical models constructed on the basis of the 1-Fe BZ.

Polaronic approach to strongly correlated electron systems with strong electron-phonon interaction

The three band p-d model of strongly correlated electrons interacting with optical phonon via diagonal and off-diagonal electron-phonon interaction is considered within cluster perturbation theory. At first step the exact diagonalization of the Hamiltonian of CuO4 cluster results in the construction of local polaronic eigenstates |p> with hole numbers nh=0,1,2 per unit cell. The inter cluster hoppings and interactions are exactly written in terms of Hubbard operators X(pq)= |p><q| determined within the multielectron polaronic eigenstates |p>. The Fermi type single electron quasiparticle dispersion and spectral weight are calculated for the undoped antiferromagnetic parent insulator like La2CuO4. The quasiparticle dispersion of Hubbard polarons is determined by a hybridization of the several Hubbard subbands with local Franck-Condon resonances. For small electron-phonon interaction the conductivity band is stronger renormalized then the valence band. Nevertheless for large electron-phonon interaction both bands are strongly renormalized with quasiparticle localization. Effect of partial compensation of diagonal and off-diagonal electron-phonon interaction at intermediate coupling is found.

Probing the electronic and local structural changes across the pressure-induced insulator-to-metal transition in VO2

Local and electronic structures of vanadium in are studied across the high-pressure insulator-to-metal (IMT) transition using V K-edge x-ray absorption spectroscopy. Unlike the temperature-induced IMT, pressure-induced metallization leads to only subtle changes in the V K-edge prepeak structure, indicating a different mechanism involving smaller electronic spectral weight transfer close to the chemical potential. Intriguingly, upon application of the hydrostatic pressure, the electronic structure begins to show substantial changes well before the occurrence of the IMT and the associated structural transition to an anisotropic compression of the monoclinic metallic phase.

Optical conductivity ofV4O7across its metal-insulator transition

The optical properties of a V4O7 single crystal have been investigated from the high temperature metallic phase down to the low temperature antiferromagnetic insulating one. The temperature dependent behavior of the optical conductivity across the metal-insulator transition (MIT) can be explained in a polaronic scenario. Charge carriers form strongly localized polarons in the insulating phase as suggested by a far-infrared charge gap abruptly opening at T_MIT = 237 K. In the metallic phase instead the presence of a Drude term is indicative of fairly delocalized charges with a moderately renormalized mass m* = 5m_e. The electronic spectral weight is almost recovered on an energy scale of 1 eV, which is much narrower compared to VO2 and V2O3 cases. Those findings suggest that electron-lattice interaction rather than electronic correlation is the driving force for V4O7 metal-insulator transition.

Spin-correlated electronic state on the surface of a spin-orbit Mott system

We use angle-resolved photoemission spectroscopy to show that the near-surface electronic structure of a bulk insulating iridate ${\mathrm{Sr}}_{3}{\mathrm{Ir}}_{2}{\mathrm{O}}_{7}$ lying near a metal-Mott insulator transition exhibits weak metallicity signified by finite electronic spectral weight at the Fermi level. The surface electrons exhibit a spin structure resulting from an interplay of spin-orbit, Coulomb interaction and surface quantum magnetism. Our results shed light on understanding the exotic quantum entanglement and transport phenomena in iridate-based oxide devices.

Theoretical Prediction and Spectroscopic Fingerprints of an Orbital Transition inCeCu2Si2

We show that the heavy-fermion compound CeCu2Si2 undergoes a transition between two regimes dominated by different crystal-field states. At low pressure P and low temperature T the Ce 4f electron resides in the atomic crystal-field ground state, while at high P or T, the electron occupancy and spectral weight is transferred to an excited crystal-field level that hybridizes more strongly with itinerant states. These findings result from first-principles dynamical-mean-field-theory calculations. We predict experimental signatures of this orbital transition in x-ray spectroscopy. The corresponding fluctuations may be responsible for the second high-pressure superconducting dome observed in this and similar materials.

Interlayer Coherence and Superconducting Condensate in thec-Axis Response of Optimally DopedBa(Fe1−xCox)2As2High-TcSuperconductor Using Infrared Spectroscopy

We report on the infrared studies of the interlayer charge dynamics of a prototypical pnictide superconductor Ba(Fe(0.926)Co(0.074))(2)As(2). We succeeded in probing the intrinsic interlayer response by performing infrared experiments on the crystals with a cleaved ac surface. Our experiments identify the coexistence of the suppression of the electronic spectral weight and the development of a coherent Drude-like response in the normal state. The formation of the interlayer condensate is clearly observed in the superconducting state and appears to be linked to coherent contribution to the normal-state conductivity.

Materials specific electronic correlation effects and spectral weight ‘hot spots’ in intermetallic actinides

ABSTRACTMany metallic actinide systems host partially filled 5f electrons in the low-energy spectrum. Consequently, they exhibit diverse quantum mechanical phenomena such as magnetism, superconductivity, a mysterious hidden-order phase, or heavy-fermion behavior. Here we present results of a unified theoretical method based on the self-consistent GW formalism for the electronic many-body self-energy. We calculate the dynamic electronic correlation spectra starting from materials specific first-principles electronic band-structure. In particular, we present results for four isostructural intermetallic actinides PuCoIn5, PuCoGa5, PuRhGa5, and UCoGa5. A common underlying property of these materials is a strong spin–orbit coupling split band structure that enables substantial spin fluctuations. In a feedback effect on the electronic structure they create electronic ‘hot spots’, where the single-particle spectral weight is maximum, resulting in a universal peak-dip-hump feature. These results are in good agreement with experiments, suggesting that actinides are adequately described by the intermediate Coulomb interaction regime, where both itinerant (peak) and localized (hump) features coexist.

Electrodynamics of the vanadium oxidesVO2andV2O3

The optical and infrared properties of films of vanadium dioxide $(\mathrm{V}{\mathrm{O}}_{2})$ and vanadium sesquioxide $({\mathrm{V}}_{2}{\mathrm{O}}_{3})$ have been investigated via ellipsometry and near-normal incidence reflectance measurements from far infrared to ultraviolet frequencies. Significant changes occur in the optical conductivity of both $\mathrm{V}{\mathrm{O}}_{2}$ and ${\mathrm{V}}_{2}{\mathrm{O}}_{3}$ across the metal-insulator transitions at least up to (and possibly beyond) $6\phantom{\rule{0.3em}{0ex}}\mathrm{eV}$. We argue that such changes in optical conductivity and electronic spectral weight over a broad frequency range are evidence of the important role of electronic correlations to the metal-insulator transitions in both of these vanadium oxides. We observe a sharp optical transition with possible final state (exciton) effects in the insulating phase of $\mathrm{V}{\mathrm{O}}_{2}$. This sharp optical transition occurs between narrow ${a}_{1g}$ bands that arise from the quasi-one-dimensional chains of vanadium dimers. Electronic correlations in the metallic phases of both $\mathrm{V}{\mathrm{O}}_{2}$ and ${\mathrm{V}}_{2}{\mathrm{O}}_{3}$ lead to reduction of the kinetic energy of the charge carriers compared to band theory values, with paramagnetic metallic ${\mathrm{V}}_{2}{\mathrm{O}}_{3}$ showing evidence of stronger correlations compared to rutile metallic $\mathrm{V}{\mathrm{O}}_{2}$.

Free Fermion limit of the strong-coupling Kondo lattice model

The strong-coupling Kondo lattice model is an interacting dense Fermi system for which conventional Fermi gas analysis has thus far failed. We will see that there exists, in fact, an exact transformation that maps the singlet Mott insulator to a Fermi vacuum and simultaneously maps bare c-electron and f-electron operators to Fermion electron and hole quasiparticles. For strong coupling, the quasiparticle dynamics are very simple. The complexity of describing the dynamics of the conventional electron operators in the singlet Mott insulator can be reduced to a complicated but precise relation between quasiparticle and bare electrons operators which exactly obey the electron spectral weight sum rules.

Strong coupling Kondo lattice model as a Fermi gas

The strong coupling half-filled Kondo lattice model is an important example of a strongly interacting dense Fermi system for which conventional Fermi gas analysis has thus far failed. We remedy this by deriving an exact transformation that maps the model to a dilute gas of weakly interacting electron and hole quasiparticles that can then be analyzed by conventional dilute Fermi gas methods. The quasiparticle vacuum is a singlet Mott insulator for which the quasiparticle dynamics are simple. Since the transformation is exact, the electron spectral weight sum rules are obeyed exactly. Subtleties in understanding the behavior of electrons in the singlet Mott insulator can be reduced to a fairly complicated but precise relation between quasiparticles and bare electrons. The theory of free quasiparticles can be interpreted as an exactly solvable model for a singlet Mott insulator, providing an exact model in which to explore the strong coupling regime of a singlet Kondo insulator.

Electrodynamics near the metal-to-insulator transition inV3O5

The electrodynamics near the metal-to-insulator transitions (MIT) induced, in V3O5 single crystals, by both temperature (T) and pressure (P) has been studied by infrared spectroscopy. The T- and P-dependence of the optical conductivity may be explained within a polaronic scenario. The insulating phase at ambient T and P corresponds to strongly localized small polarons. Meanwhile the T-induced metallic phase at ambient pressure is related to a liquid of polarons showing incoherent dc transport, in the P-induced metallic phase at room T strongly localized polarons coexist with partially delocalized ones. The electronic spectral weight is almost recovered, in both the T and P induced metallization processes, on an energy scale of 1 eV, thus supporting the key-role of electron-lattice interaction in the V3O5 metal-to-insulator transition.