We present a dynamical theory of the Auger decay in one-dimensional (1D) metals described by the Tomonaga-Luttinger model. An analytic expression of the Auger current is derived in the framework of the 1-step approach, where the finite lifetime of the initial core-hole and the core-valence interaction are taken into account. This allows to capture typical dynamical features like the shake-down effect, in which the Auger spectrum shows a non-vanishing weight above the 2-step high-energy threshold. The obtained results give also a hint to understand the sizable suppression of Auger spectral weight closed to the Fermi energy recently observed in carbon nanotubes with respect to graphite.
Supercell method is used to study the relaxation and screening effects during the Auger transition in metals. In order to make the interaction between the core-holes sited at different atoms negligible, the real metal is simulated by supercells repeated periodically. The electronic states concerned by the Auger transition are calculated by using FLAPW method. The occurrence of both bandlike and quasi-atomiclike Auger spectra across transition metal series is related clearly to the different responses of these metals to the existence of a core-hole depending on whether their d-bands are partial…
CVV Auger electron spectra are calculated for a multi-band Hubbard model including correlations among the valence electrons as well as correlations between core and valence electrons. The interest is focused on the ferromagnetic 3d-transition metals. The Auger line shape is calculated from a three-particle Green function. A realistic one-particle input is taken from tight-binding band-structure calculations. Within a diagrammatic approach we can distinguish between the \textit{direct} correlations among those electrons participating in the Auger process and the \textit{indirect} correlations i…
We calculate Auger spectra given by the two-hole Green's function from orbitally degenerate Hubbard-like models as a function of correlation strength and band filling. The resulting spectra are qualitatively different from those obtained from fully-filled singly degenerate models due to the presence of screening dynamics and multielectron excitations. Application to a real system shows remarkable agreement with experimental results leading to reinterpretation of spectral features.
With on- and off- resonant excitation photons, spin-resolved Auger electron spectra of epitaxial CrO$_{2}$ thin films show an experimental evidence of the spin-selective KLL Auger decay. The on-resonance O KLL Auger electrons are found to be highly spin-polarized, while the off-resonance ones with almost zero spin polarization. These results lead to conclude that the two-hole final state in KLL Auger decay is a spin-singlet. Applications to spin-resolved absorption spectroscopy are discussed.
We propose a novel variational method to calculate the two-hole propagators relevant for Auger spectroscopy in transition metal oxides. This method can be thought of as an intermediary step between the full solution (which is difficult to generalize to systems with partially filled bands) and the impurity approximation. Like the former, our solution has full translational invariance, and like the latter, it can be generalized to certain types of systems with partially filled bands. Here we compare both our variational approximation and the impurity approximation against the exact solution for …
We propose a computationally simple model of Auger and APECS line shapes from open-band solids. Part of the intensity comes from the decay of unscreened core-holes and is obtained by the two-body Green's function $G^{(2)}_ω$, as in the case of filled bands. The rest of the intensity arises from screened core-holes and is derived using a variational description of the relaxed ground state; this involves the two-holes-one-electron propagator $G_ω$, which also contains one-hole contributions. For many transition metals, the two-hole Green's function $G^{(2)}_ω$ can be well described by the Ladder…
We review the Cini-Sawatzky approach to the line shape analysis of Auger CVV transitions, in its basic and original formulation. Then, several extensions of the theory are reviewed, namely the inclusion spin-orbit coupling, dynamical/plasmon screening, overlap effects, off-site interactions, the treatment of disorder and the formulation for partially filled bands. We conclude by highlighting what we consider to be future directions in the field.
We propose an ab initio method to evaluate the core-valence-valence (CVV) Auger spectrum of systems with filled valence bands. The method is based on the Cini-Sawatzky theory, and aims at estimating the parameters by first-principles calculations in the framework of density-functional theory (DFT). Photoemission energies and the interaction energy for the two holes in the final state are evaluated by performing DFT simulations for the system with varied population of electronic levels. Transition matrix elements are taken from atomic results. The approach takes into account the non-sphericity …
The bulk-sensitive Ce 4$f$ spectral weights of various Ce compounds including CeFe$_2$, CeNi$_2$, and CeSi$_2$ were obtained with the resonant photoemission technique at the Ce 3d-edge. We found the lineshapes change significantly with the small change of the incident photon energy. Detailed analysis showed that this phenomenon results primarily from the Auger transition between different multiplet states of the Ce $\underline{3d_{5/2}}4f^2$ (bar denotes a hole) electronic configuration in the intermediate state of the resonant process. This tells us that extra care should be taken for the cho…
We study steady-states of semiconductor nanowires subjected to strong resonant time-periodic drives. The steady-states arise from the balance between electron-phonon scattering, electron-hole recombination via photo-emission, and Auger scattering processes. We show that tuning the strength of the driving field drives a transition between an electron-hole metal (EHM) phase and a Floquet insulator (FI) phase. We study the critical point controlling this transition. The EHM-to-FI transition can be observed by monitoring the presence of peaks in the density-density response function which are asso…
This paper reports high resolution X-ray photoelectron spectroscopy (XPS) studies on Fe$_{1-x}$Ni$_x$ (x=0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.9) alloys down to 10 K temperature. Core levels and Auger transitions of the alloys except the invar alloy (x=0.4) exhibit no observable temperature induced changes. The invar alloy exhibits changes in the core levels below 20 K temperature that strongly depend on the core level. Such core level dependent changes with temperature were attributed to the precipitation of spin glass like phase below 20 K only in the invar alloy. Ni L$_3$M$_{45}$M$_{45}$ Auger tr…
Metal-insulator transition features as a transformation, from a highly charge conductive state to another state where charge conductivity is greatly suppressed when decreasing the temperature. Here we demonstrate two consecutive transitions in NdNiO3 films with CoFe2O4 capping, in which the metal-insulator transition occurs at 85 K, followed by an unprecedented insulator-metal transition below 40 K. The emerging insulator-metal transition associated with a weak antiferromagnetic behavior is observed in 20 unit cell-thick NdNiO3 with more than 5 unit cell CoFe2O4 capping. Differently, the NdNiO…
The doping induced insulator-metal transition in $La_{1-x}Sr_{x}TiO_{3}$ is studied using the ab-initio LDA+DMFT method. Combining the LDA bandstructure for the actual, distorted structure found recently with multi-orbital DMFT to treat electronic correlations, we find: $(i)$ ferro-orbital order in the Mott insulating state without orbital degeneracy, $(ii)$ a continuous filling induced transition to the paramagnetic metal (PM) with $x$, and $(iii)$ excellent quantitative agreement with published photoemission data for the case of 6% doping. Our results imply that this system can be described …
We investigated the electronic structures of the 5$d$ Ruddlesden-Popper series Sr$_{n+1}$Ir$_{n}$O$_{3n+1}$ ($n$=1, 2, and $\infty$) using optical spectroscopy and first-principles calculations. As 5$d$ orbitals are spatially more extended than 3$d$ or 4$d$ orbitals, it has been widely accepted that correlation effects are minimal in 5$d$ compounds. However, we observed a bandwidth-controlled transition from a Mott insulator to a metal as we increased $n$. In addition, the artificially synthesized perovskite SrIrO$_{3}$ showed a very large mass enhancement of about 6, indicating that it was in…
Moiré superlattices formed in two-dimensional semiconductor heterobilayers provide a new realization of Hubbard model physics in which the number of electrons per effective atom can be tuned at will. We report on an exact diagonalization study of the electronic properties of half-filled narrow moiré bands in which correlation strengths are varied by changing twist angles or interaction strengths. We construct a phase diagram for the bilayer, identifying where the metal-insulator phase transition occurs, estimating the sizes of the charge gaps in the insulating phase, and commenting on the natu…
Understanding complex correlated oxides and their phase transitions has long been a challenge. The difficulty largely arises from the intriguing interplay between multiple degrees of freedoms. While degeneracy can play an important role in determining material characteristics, there is no well-defined way to quantify and to unveil its role in real materials having complicated band structures. Here we suggest a way to quantify the `effective degeneracy' relevant to metal-insulator transition by introducing entropy-like terms. This new quantity well describes the electronic behaviors of transiti…
We study the quantum phase transition from an antiferromagnetic metal to a heavy fermion metal in the Kondo lattice model. Based on the strong coupling approach we {\it first} diagonalize the Kondo coupling term. Since this strong coupling approach makes the resulting Kondo term {\it relevant}, the Kondo hybridization persists even in the antiferromagnetic metal, indicating that fluctuations of Kondo singlets are not critical in the phase transition. We find that the quantum transition in our strong coupling approach results from {\it softening of antiferromagnetic spin fluctuations of localiz…
The spin-one-half Falicov-Kimball model is solved exactly on an infinite-coordination-number Bethe lattice in the thermodynamic limit. This model is a paradigm for a charge-transfer metal-insulator transition where the occupancy of localized and delocalized electronic orbitals rapidly changes at the metal-insulator transition (rather than the character of the electronic states changing from insulating to metallic as in a Mott-Hubbard transition). The exact solution displays both continuous and discontinuous (first-order) transitions.
Angle-resolved photoemission spectroscopy was used to investigate the evolution of the electronic structure across the metal-insulator transition in bi-layer manganite $La_{1.24}Sr_{1.76}Mn_2O_7$. We found that this system is a metal for $T<T_C$, a local metal but global insulator for $T<T_C<T^*$, and a global insulator for $T>T^*$. These results indicate the critical role of electronic phase separation and percolation effects for the metal-insulator transition in $La_{1.24}Sr_{1.76}Mn_2O_7$.
We obtain exact numerical solutions of the degenerate Hubbard model in the limit of large dimensions (or large lattice connectivity). Successive Mott-Hubbard metal insulator transitions at integer fillings occur at intermediate values of the interaction and low enough temperature in the paramagnetic phase. The results are relevant for transition metal oxides with partially filled narrow degenerate bands.
A brief review of metal-insulator transitions in three-dimensional doped semiconductors, with emphasis on the "critical exponent puzzle"; and new experimental findings that signal the possibility of an unexpected metal-insulator transition in dilute two-dimensional systems, such as silicon MOSFETs and GaAs/AlGaAs heterostructures.
The role of orbital ordering on metal-insulator transition of transition-metal oxides is investigated by the cluster self-consistent field approach in the strong correlation regime. A clear dependence of the insulating gap on the orbital order parameter is found in the single-particle excitation spectra. The thermal fluctuation drives the orbital order-disorder transition, diminishes the gap and leads to the metal-insulator transition. The interplay between spins and orbits results in unusual temperature dependence of the orbital polarization in the orbital insulator, which can be seen in the …
We establish that a doping-driven first-order metal-to-metal transition, from a pseudogap metal to Fermi Liquid, can occur in correlated quantum materials. Our result is based on the exact Dynamical Mean Field Theory solution of the Dimer Hubbard Model. This transition elucidates the origin of many exotic features in doped Mott materials, like the pseudogap in cuprates, incoherent bad metals, enhanced compressibility and orbital selective Mott transition. This phenomenon is suggestive to be at the roots of the many exotic phases appearing in the phase diagram of correlated materials.
Exotic features of a metal/oxide/metal (MOM) sandwich, which will be the basis for a drastically innovative nonvolatile memory device, is brought to light from a physical point of view. Here the insulator is one of the ubiquitous and classic binary-transition-metal oxides (TMO), such as Fe2O3, NiO, and CoO. The sandwich exhibits a resistance that reversibly switches between two states: one is a highly resistive off-state and the other is a conductive on-state. Several distinct features were universally observed in these binary TMO sandwiches: namely, nonpolar switching, non-volatile threshold …
Although most metal-insulator transitions in doped insulators are generally viewed as Mott transitions, some systems seem to deviate from this scenario. Alkali metal-ammonia solutions are a brilliant example of that. They reveal a phase separation in the range of metal concentrations where a metal-insulator transition occurs. Using a mean spherical approximation for quantum polarizable fluids, we argue that the origin of the metal-insulator transition in such a system is likely similar to that proposed by Herzfeld a long time ago, namely, due to fluctuations of solvated electrons. We also show…
Metal-ion doping can effectively regulate the metal-insulator transition temperature in $\mathrm{VO}_2$. Experiments found that the pentavalent and hexavalent ion doping dramatically reduces the transition temperature while the trivalent ion doping increases the transition temperature and induces intermediate phases. Based on the phase-field model of the metal-insulator transition in $\mathrm{VO}_2$ we developed previously, we formulate a Landau potential of the metal-ion-doped $\mathrm{VO}_2$ taking account of the effects of doping on the electron correlation and lattice structure. The effect…
Previous work on the physical content of exchange correlation functionals that depend on both charge and spin densities is extended to elemental transition metals and a wider range of perovskite transition metal oxides. A comparison of spectra and magnetic moments calculated using exchange correlation functionals depending on charge density only or on both charge and spin densities, as well as the $+U$ and $+J$ extensions of these methods confirms previous conclusions that the spin-dependent part of the exchange correlation functional provides an effective Hund's interaction acting on the tran…
We propose new methodologies for stabilizing all-metal antiaromatic clusters like: Al$_{4}$Li$_{4}$. We demonstrate that these all-metal species can be stabilized by complexation with 3d-transition metals very similar to its organic counterpart, C$_4$H$_4$. Complexation to transition metal ions reduce the frontier orbital energies and introduces aromaticity. We consider a series of such complexes [$η$$^4$(Al$_4$Li$_4$)-Fe(CO)$_3$, $η$$^2$$σ$$^2$(Al$_4$Li$_4$)-Ni and (Al$_{4}$Li$_{4}$)$_{2}$Ni] and make a comparison between the all-metal species and the organometallic compounds to prove conclus…
By treating the electron-ion interaction as perturbation in the first-principles Hamiltonian, we have calculated the density response functions of a fluid alkali metal to find an interesting charge instability due to anomalous electronic density fluctuations occurring at some finite wave vector ${\bi Q}$ in a dilute fluid phase above the liquid-gas critical point. Since $|{\bi Q}|$ is smaller than the diameter of the Fermi surface, this instability necessarily impedes the electric conduction, implying its close relevance to the metal-insulator transition in fluid alkali metals.
