Dynamical Spectral Weight Transfer Research Articles

LDA+DMFT approach to electronic structure of sodium metal

Based on local density approximation plus dynamical mean-field theory (LDA+DMFT) calculations, we revisit the long-standing quasiparticle band narrowing problem of sodium metal. Using an on-site Coulomb interaction U derived from angle-resolved photoemission spectroscopy mass enhancement, we can describe various properties of this weakly correlated electron system. Intrinsic self-energy corrections lead to a Landau-Fermi liquid state with many-particle coherence and dynamical spectral weight transfer relevant to electronic structure and scattering rates of alkali metals.

Local entropies across the Mott transition in an exactly solvable model

We study entanglement in the Hatsugai-Kohmoto model, which exhibits a continuous interaction-driven Mott transition. By virtue of the all-to-all nature of its center-of-mass conserving interactions, the model lacks dynamical spectral weight transfer, which is the key to intractability of the Hubbard model for $d>1$. In order to maintain a non-trivial Mott-like electron propagator, SU(2) symmetry is preserved in the Hamiltonian, leading to a ground state that is mixed on both sides of the phase transition. Because of this mixture, even the metal in this model is unentangled between any pair of sites, unlike free fermions whose ground state carries a filling-dependent site-site entanglement. We focus on the scaling behavior of the one- and two-site entropies $s_1$ and $s_2$, as well as the entropy density $s$, of the ground state near the Mott transition. At low temperatures in the two-dimensional Hubbard model, it was observed numerically (Walsh et al., 2018, arXiv:1807.10409) that $s_1$ and $s$ increase continuously into the metal, across a first-order Mott transition. In the Hatsugai-Kohmoto model, $s_1$ acquires the constant value $\ln4$ even at the Mott transition. The ground state's non-trivial entanglement structure is manifest in $s_2$ and $s$ which decrease into the metal, and thereby act as sharp signals of the Mott transition in any dimension. Specifically, we find that in one dimension, $s_2$ and $s$ exhibit kinks at the transition while in $d=2$, only $s$ exhibits a kink.

Site-selective electronic structure of pure and doped Ca2O3Fe3S2

Using density functional dynamical mean-field theory we investigate the site-selective electronic structure of ${\mathrm{Ca}}_{2}{\mathrm{O}}_{3}{\mathrm{Fe}}_{3}{\mathrm{S}}_{2}$. We confirm that the parent compound with two distinct iron sites is a multiorbital Mott insulator similar to ${\mathrm{La}}_{2}{\mathrm{O}}_{3}{\mathrm{Fe}}_{2}{\mathrm{S}}_{2}$. Upon electron/hole doping, carrier localization is found to persist in the two active iron channels because the chemical potential lies in a gap structure with anisotropic and almost vanishing states near the Fermi energy. This emergent behavior stems from large electronic reconstruction caused by dynamical spectral weight transfer involving states with distinct $d$-shell occupancies and orbital character at low energies. We detail the implications of our microscopic analysis and discuss the underlying physics which will emerge in future experiments on ${\mathrm{Ca}}_{2}{\mathrm{O}}_{3}{\mathrm{Fe}}_{3}{\mathrm{S}}_{2}$.

Photoinduced ultrafast optical anisotropy encountered by spin-flip transition in La0.67Ca0.33MnO3

Understanding and controlling the transient optical anisotropy of strong correlation systems is of great interest in the quest for information processing and storage. Here, we report on ultrafast optical pump-probe measurements with linearly and circularly polarized laser pulses in the manganite La0.67Ca0.33MnO3 thin film. We show both the time-resolved reflectivity and the polarization state (Kerr rotation and ellipticity) of the probe-pulse at different temperatures, which are analyzed by the ultrafast intersite transition between Mn3+ and Mn4+ sites at photon energies around 1.55 eV. During the temperature-induced dynamical spectral weight transfer, a spin-flip photo-transition between spin up eg states of Mn3+ and spin down eg states of Mn4+ ions occurs and is imprinted on the optical anisotropy of the probe beam.

Electronic reconstruction of hexagonal FeS: a view from density functional dynamical mean-field theory

We present a detailed study of correlation- and pressure-induced electronic reconstruction in hexagonal iron monosulfide, a system which is widely found in meteorites and one of the components of Earth’s core. Based on a perusal of experimental data, we stress the importance of multi-orbital electron-electron interactions in concert with first-principles band structure calculations for a consistent understanding of its intrinsic Mott–Hubbard insulating state. We explain the anomalous nature of pressure-induced insulator-metal-insulator transition seen in experiment, showing that it is driven by dynamical spectral weight transfer in response to changes in the crystal-field splittings under pressure. As a byproduct of this analysis, we confirm that the electronic transitions observed in pristine FeS at moderated pressures are triggered by changes in the spin state which causes orbital-selective Kondo quasiparticle electronic reconstruction at low energies.

Electronic localization and bad-metallicity in pure and electron-doped troilite: A local-density-approximation plus dynamical-mean-field-theory study of FeS for lithium-ion batteries

Iron sulfides are promising candidates for the next generation of rechargeable lithium-ion battery materials. Motivated thereby, we present a detailed study of correlation- and doping-induced electronic reconstruction in troilite. Based on local-density-approximation plus dynamical-mean-field-theory, we stress the importance of multi-orbital Coulomb interactions in concert with first-principles band structure calculations for a consistent understanding of intrinsic Mott-Hubbard insulating state in FeS. We explore the anomalous nature of electron doping-induced insulator-bad metal transition, showing that it is driven by orbital-selective dynamical spectral weight transfer. Our results are relevant for understanding charge dynamics upon electrochemical lithiation of iron monosulfides electrode materials for lithium-ion batteries.

Nonequilibrium transport in the strange metal and pseudogap phases of the cuprates

We propose that the non-equilibrium current measured in the $a-b$ plane of an underdoped cuprate (in either the strange metal or pseudogap regime) in contact with either an overdoped cuprate or a standard Fermi liquid can be used diagnose how different the pseudogap and strange metals are from a Fermi liquid. Naively one expects the strange metal to be more different from a Fermi liquid than is the pseudogap. We compute the expected non-equilibrium transport signal with the three Green functions that are available in the literature: 1) marginal Fermi liquid theory, 2) the phenomenological ansatz for the pseudogap regime and 3) the Wilsonian reduction of the Hubbard model which contains both the strange metal and pseudogap. All three give linear IV curves at low bias voltages. Significant deviations from linearity at higher voltages obtain only in the marginal Fermi liquid approach. The key finding, however, is that IV curves for the strange metal/Fermi liquid contact that exceed that of the pseudogap/Fermi liquid system. If this is borne out experimentally, this implies that the strange metal is less orthogonal to a Fermi liquid than is the pseudogap. Within the Wilsonian reduction of the Hubbard model, this result is explained in terms of a composite-particle picture. Namely, the pseudogap corresponds to a confinement transition of the charge degrees of freedom present in the strange metal. In the strange metal the composite excitations break up and electron quasiparticles scatter off bosons. The bosons here, however, do not arise from phonons but from the charge degrees of freedom responsible for dynamical spectral weight transfer.

Doping evolution of the oxygenK-edge x-ray absorption spectra of cuprate superconductors using a three-orbital Hubbard model

We study oxygen K-edge x-ray absorption spectroscopy (XAS) and investigate the validity of the Zhang-Rice singlet (ZRS) picture in overdoped cuprate superconductors. Using large-scale exact diagonalization of the three-orbital Hubbard model, we observe the effect of strong correlations manifesting in a dynamical spectral weight transfer from the upper Hubbard band to the ZRS band. The quantitative agreement between theory and experiment highlights an additional spectral weight reshuffling due to core-hole interaction. Our results confirm the important correlated nature of the cuprates and elucidate the changing orbital character of the low-energy quasi-particles, but also demonstrate the continued relevance of the ZRS even in the overdoped region.

Spectral weight transfer in multiorbital Mott systems

We develop here a general formalism for multiorbital Mott systems that can be used to understand dynamical and static spectral weight transfer. We find that the spectral weight transferred from the high-energy scales is greatly increased as a result of the multiorbital structure. As a consequence certainly dynamically generated symmetries are obtained at lower values of doping than in the single-band Hubbard model. For example, in the atomic limit for filling less than one electron per site, the particle-hole symmetric condition in the lower band shifts from the one-band result of $x=1/3$ to $x=1/(2{n}_{o}+1)$, where ${n}_{o}$ is the number of orbitals with an unpaired spin. Transport properties computed from effective low-energy theories that forbid double occupancy of bare electrons, such as the multiorbital $t$-$J$ generalization, should all be be sensitive to this particle-hole symmetric condition. Away from the atomic limit, the dynamical contributions increase the transferred spectral weight. Consequently, any phenomena that are sensitive to an emergent particle-hole symmetry should be obtained at $x<[1/(2{n}_{o}+1)]$.

Mottness collapse and T -linear resistivity in cuprate superconductors

Central to the normal state of cuprate high-temperature superconductors is the collapse of the pseudo-gap, briefly reviewed here, at a critical point and the subsequent onset of the strange metal characterized by a resistivity that scales linearly with temperature. A possible clue to the resolution of this problem is the inter-relation between two facts: (i) a robust theory of T-linear resistivity resulting from quantum criticality requires an additional length scale outside the standard one-parameter scaling scenario and (ii) breaking the Landau correspondence between the Fermi gas and an interacting system with short-range repulsions requires non-fermionic degrees. We show that a low-energy theory of the Hubbard model that correctly incorporates dynamical spectral weight transfer has the extra degrees of freedom needed to describe this physics. The degrees of freedom that mix into the lower band as a result of dynamical spectral weight transfer are shown to either decouple beyond a critical doping, thereby signalling Mottness collapse, or unbind above a critical temperature, yielding strange metal behaviour characterized by T-linear resistivity.

Emergence of particle-hole symmetry near optimal doping in high-temperature copper oxide superconductors

High-temperature copper oxide superconductors (cuprates) display unconventional physics when they are lightly doped whereas the standard theory of metals prevails in the opposite regime. For example, the thermoelectric power, that is the voltage that develops across a sample in response to a temperature gradient, changes sign abruptly near optimal doping in a wide class of cuprates, a stark departure from the standard theory of metals in which the thermopower vanishes only when one electron exists per site. We show that this effect arises from proximity to a state in which particle-hole symmetry is dynamically generated. The operative mechanism is dynamical spectral weight transfer from states that lie at least 2 eV away from the chemical potential. We show that the sign change is reproduced quantitatively within the Hubbard model for moderate values of the on-site repulsion, $U$. For sufficiently large values of on-site repulsion, for example, $U=20t$ ($t$ the hopping matrix element), dynamical spectral weight transfer attenuates and our calculated results for the thermopower are in prefect agreement with exact atomic limit. The emergent particle-hole symmetry close to optimal doping points to pairing in the cuprates being driven by high-energy electronic states.

Exact integration of the high energy scale in doped Mott insulators

We expand on our earlier work [R. G. Leigh , Phys. Rev. Lett. 99, 46404 (2007)] in which we constructed the exact low energy theory of a doped Mott insulator by explicitly integrating (rather than projecting) out the degrees of freedom far away from the chemical potential. The exact low energy theory contains degrees of freedom that cannot be obtained from projective schemes. In particular, a charge +/- 2e bosonic field that is not made out of elemental excitations emerges at low energies. Such a field accounts for dynamical spectral weight transfer across the Mott gap. At half-filling, we show that two such excitations emerge which play a crucial role in preserving the Luttinger surface along which the single-particle Green’s function vanishes. In addition, the interactions with the bosonic fields defeat the artificial local SU(2) symmetry that is present in the Heisenberg model. We also apply this method to the Anderson-U impurity and show that in addition to the Kondo interaction, bosonic degrees of freedom appear as well. Finally, we show that as a result of the bosonic degree of freedom, the electron at low energies is in a linear superposition of two excitations-one arising from the standard projection into the low energy sector and the other from the binding of a hole and the boson.

Hidden Charge2eBoson in Doped Mott Insulators

We construct the low-energy theory of a doped Mott insulator, such as the high-temperature superconductors, by explicitly integrating over the degrees of freedom far away from the chemical potential. For either hole or electron doping, a charge 2e bosonic field emerges at low energy. The charge 2e boson mediates dynamical spectral weight transfer across the Mott gap and creates a new charge e excitation by binding a hole. The result is a bifurcation of the electron dispersion below the chemical potential as observed recently in angle-resolved photoemission on Pb-doped Bi2Sr2CaCu2O8+delta (Pb2212).