We investigated temperature dependent optical spectra of the one-dimensional chain compound Sr$_{2}$CuO$_{3}$. The charge transfer transition polarized along the chain direction shows a strongly asymmetric line shape as expected in one-dimensional extended Hubbard model. At low temperature the charge transfer peak shows a large blue shift and reveals additional sharp peaks at the gap. Even though many spectroscopic studies suggest that this material can not have a bound exciton based on the one-dimensional extended Hubbard model, we attribute the additional sharp peaks to excitons, which come to exist due to the long range Coulomb interaction.
We present a comparative experimental and theoretical investigation of the two--dimensional charge-transfer gap in the strongly correlated material Sr$_2$CuO$_2$Cl$_2$. We observe an Urbach behaviour in the absorption profile over a surprisingly wide range of energies and temperatures. We present a model that accounts for phonon scattering to infinite order and which allows us to explain the data accurately by assuming coupling of the charge transfer gap exciton to lower energy electronic excitations.
Cuprate materials, like those hosting high temperature superconductivity, represent a famous class of materials where the correlations between the strongly entangled charges and spins produce complex phase diagrams. Several years ago the Zhang-Rice singlet was proposed as a natural quasiparticle in hole-doped cuprates. The occurance and binding energy of this quasiparticle, consisting of a pair of bound holes with antiparallel spins on the same CuO$_4$ plaquette, depends on the local electronic interactions, which are fundamental quantities for understanding the physics of the cuprates. Here, …
We investigated excitation spectra of the one-dimensional chain compound Sr$_{2}$CuO$_{3}$. The small peak at 2.3 eV in the loss function was turned to correspond to the strong charge transfer transition at 1.8 eV in conductivity. It has the excitonic character expected in one dimensional extended Hubbard model of the transition from the lower Hubberd band to the Zhang-Rice singlet state. The strongest peak at 2.7 eV in the loss function is attributed to the continuum excitation of the excitonic charge transfer transition. The spectral weight sum rule is satisfied within these transitions.
We present an $\textit{ab initio}$ study of the excitonic states of a prototypical high-temperature superconductor La$_2$CuO$_4$ and compare them to the isostructural single-layer nickelate La$_2$NiO$_4$. Key difference in the low-energy electronic structure leads to very different excitonic behavior. Excitons in La$_2$CuO$_4$ are delocalized and can freely move in the CuO$_2$ plane without disturbing the antiferromagnetic order. In contrast, in La$_2$NiO$_4$ we find the low-lying excitonic states to be extremely localized, producing a nearly flat dispersion. The theoretically obtained exciton…
The real part of optical conductivity $\text{Re}σ(ω)$ of the Mott insulators has a large amount of information on how spin and charge degrees of freedom interact with each other. By using the time-dependent density-matrix renormalization group, we study $\text{Re}σ(ω)$ of the two-dimensional Hubbard model on a square lattice at half filling. We find an excitonic peak at the Mott-gap edge of $\text{Re}σ(ω)$ not only for the two-dimensional square lattice but also for two- and four-leg ladders. For the square lattice, however, we do not clearly find a gap between an excitonic peak and continuum …
A semi-quantitative cluster approach is developed to describe the charge transfer (CT) electron-hole excitations in insulating cuprates in a rather wide energy range up to 10- 15 eV. It generalizes the Zhang-Ng (ZN) model of CT excitons by considering the complete set of Cu3d and O2p orbitals within the CuO4 embedded molecular cluster method and by introducing one-center (intra-center) Frenkel-like and two-center (inter-center) excitons. Special attention is paid to the transition matrix element effects both in optical and electron energy loss spectra (EELS). In the latter case we obtain the m…
The layered cuprate Bi$_{2}$CuO$_{4}$ is investigated using magnetic, dielectric and pyroelectric measurements. This system is observed to be an improper multiferroic, with a robust ferroelectric state being established near the magnetic transition. Magnetic and dielectric measurements indicate the presence of a region above the antiferromagnetic Neel temperature with concomitant polar and magnetic short range order. Bi$_{2}$CuO$_{4}$ is also seen to exhibit colossal dielectric constants at higher temperatures with clearly distinguishable grain and grain boundary contributions, both of which e…
Spectroscopic ellipsometry was used to study the dielectric function of LiCuVO$_{4}$, a compound comprised of chains of edge-sharing CuO$_4$ plaquettes, in the spectral range (0.75 - 6.5) eV at temperatures (7-300) K. For photon polarization along the chains, the data reveal a weak but well-resolved two-peak structure centered at 2.15 and 2.95 eV whose spectral weight is strongly enhanced upon cooling near the magnetic ordering temperature. We identify these features as an exciton doublet in the Mott-Hubbard gap that emerges as a consequence of the Coulomb interaction between electrons on near…
Motivated by the possibility of pressure-induced exciton condensation in intermediate-valence Tm[Se,Te] compounds we study the Falicov-Kimball model extended by a finite f-hole valence bandwidth. Calculating the Frenkel-type exciton propagator we obtain excitonic bound states above a characteristic value of the local interband Coulomb attraction. Depending on the system parameters coherence between c- and f-states may be established at low temperatures, leading to an excitonic insulator phase. We find strong evidence that the excitonic insulator typifies either a BCS condensate of electron-hol…
Observation of spin-conserving two-spinon continuum in the $S$=1/2 antiferromagnetic chain system Sr$_2$CuO$_3$ using Cu $K$-edge resonant inelastic x-ray scattering
An approximate solution scheme, similar to the Gutzwiller approximation, is presented for the Baeriswyl and the Baeriswyl-Gutzwiller variational wavefunctions. The phase diagram of the one-dimensional Hubbard model as a function of interaction strength and particle density is determined. For the Baeriswyl wavefunction a metal-insulator transition is found at half-filling, where the metallic phase ($U<U_c$) corresponds to the Hartree-Fock solution, the insulating phase is one with finite double occupations arising from bound excitons. This transition can be viewed as the "inverse" of the Brinkm…
Friedel oscillations induced by open boundary conditions in a two-band Hubbard model for CuO chains are numerically studied. We find that for physically realistic parameters and close to quarter filling, these oscillations have a 2k_F modulation according with experimental results on YBa_2Cu_3O_{7-delta}. In addition, we predict that, for the same parameters, as hole doping is reduced from quarter filling to half filling, Friedel oscillations would acquire a 4k_F modulation, typical of a strongly correlated electrons regime. The 4k_F modulation dominates also in the electron doped region. The …
Two-exciton bound states in the Merrifield exciton model
Center for Quantum Technology Research, and Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurements (MOE), School of Physics, Beijing Institute of Technology（北京理工大学物理学院，量子技术研究中心，先进光电子量子架构与测量教育部重点实验室）
We report quantum Monte Carlo calculations of biexciton binding energies in ideal two-dimensional bilayer systems with isotropic electron and hole masses. We have also calculated exciton-exciton interaction potentials, and pair distribution functions for electrons and holes in bound biexcitons. Comparing our data with results obtained in a recent study using a model exciton-exciton potential [C. Schindler and R. Zimmermann, Phys. Rev. B \textbf{78}, 045313 (2008)], we find a somewhat larger range of layer separations at which biexcitons are stable. We find that individual excitons retain their…
An elastic neutron scattering study has been performed on several single crystals of La$_{2-x}$Sr$_{x}$CuO$_{4}$ for {\it x} near the lower critical concentration {\it x$_{c}$} for superconductivity. % In the insulating spin-glass phase ({\it x} = 0.04 and 0.053), the previously reported one-dimensional spin modulation along the orthorhombic {\it b}-axis is confirmed. % Just inside the superconducting phase ({\it x} = 0.06), however, two pairs of incommensurate magnetic peaks are additionally observed corresponding to the spin modulation parallel to the tetragonal axes. % These two types of sp…
The Anderson model with the Coulomb interaction between the local and conduction electrons is studied in the semiconducting phase. Based on a perturbation theory from the atomic limit, leading contributions for the c-f Coulomb interaction are incorporated as a vertex correction to hybridization. An analytical solution shows that the effective attraction in the intermediate states leads to a bound state localized at the local electron site. Self-consistent equations are constructed as an extension of the non-crossing approximation (NCA) to include the vertex part yielding the bound state. A num…
We explore the effect of local charge fluctuations on the spin response of a Mott insulator by deriving an effective spin model, and studying it using Schwinger boson mean field theory. Applying this to La$_2$CuO$_4$, we show that an accurate fit to the magnon dispersion relation, measured by Coldea {\em et al.} [Phys. Rev. Lett. {\bf 86}, 5377 (2001)] is obtained with Hubbard model parameters $U \approx 2.34 eV$, and $t \approx 360 meV$. These parameters lead to estimates of the staggered magnetization ($m_s \approx 0.25$), spin wave velocity ($c\approx 800 meV$-Å), and spin stiffness ($ρ_s \…
Angle-resolved photoemission measurements on the electron-doped cuprate Sm(1.85)Ce(0.15)CuO(4) evidence anisotropic dressing of charge-carriers due to many-body interactions. Most significantly, the scattering rate along the zone boundary saturates for binding energies larger than ~200 meV, while along the diagonal direction it increases nearly linearly with the binding energy in the energy range ~150-500 meV. These results indicate that many-body interactions along the diagonal direction are strong down to the bottom of the band, while along the zone-bounday they become very weak at energies …
We report a resonant inelastic x-ray scattering study of the dispersion relations of charge transfer excitations in insulating La$_2$CuO$_4$. These data reveal two peaks, both of which show two-dimensional characteristics. The lowest energy excitation has a gap energy of $\sim 2.2$ eV at the zone center, and a dispersion of $\sim 1$ eV. The spectral weight of this mode becomes dramatically smaller around ($π$, $π$). The second peak shows a smaller dispersion ($\sim 0.5$ eV) with a zone-center energy of $\sim 3.9$ eV. We argue that these are both highly dispersive exciton modes damped by the pr…
We propose a simple first-principles method to describe propagation of tightly bound excitons. By viewing the exciton as a composite object (an effective Frenkel exciton in Wannier orbitals), we define an exciton kinetic kernel to encapsulate the exciton propagation and decay for all binding energy. Applied to prototypical LiF, our approach produces three exciton bands, which we verified quantitatively via inelastic x-ray scattering. The proposed real-space picture is computationally inexpensive and thus enables study of the full exciton dynamics, even in the presence of surfaces and impurity …
In their comment \cite{Sun} on our study of phonon heat transport in Nd$_2$CuO$_4$ \cite{Li}, Sun and Ando estimate that the phonon mean free path at low temperature is roughly half the width of the single crystal used in our study, from which they argue that phonon scattering cannot be dominated by sample boundaries. Here we show that their use of specific heat data on Nd$_2$CuO$_4$, which contains a large magnetic contribution at low temperature that is difficult to reliably extract, leads to an underestimate of the mean free path by a factor two compared to an estimate based on the specific…
We present a computer simulation of exciton-exciton scattering in a quantum well. Specifically, we use quantum Monte Carlo techniques to study the bound and continuum states of two excitons in a 10 nm wide GaAs/Al$_{0.3}$Ga$_{0.7}$As quantum well. From these bound and continuum states we extract the momentum-dependent phase shifts for s-wave scattering. A surprising finding of this work is that a commonly studied effective-mass mode for excitons in a 10 nm quantum well actually supports two bound biexciton states. The second, weakly bound state may dramatically enhance exciton-exciton interact…
We have performed a series of elastic neutron scattering measurements on 1/8-hole doped La$_{1.875}$Ba$_{0.125-x}$Sr$_{x}$CuO$_{4}$ single crystals with {\it x} = 0.05, 0.06, 0.075 and 0.085. % Both charge-density-wave (CDW) and spin-density-wave (SDW) orders are found to develop simultaneously below the structural transition temperature between the low-temperature orthorhombic (LTO) and low-temperature tetragonal (LTT) or low-temperature less-orthorhombic (LTLO) phases. % In the ground state the CDW order is observed only in the LTT/LTLO phase and drastically degrades towards the LTO boundary…
This theoretical paper offers an explicit expression for the binding energy of excitons in a two-dimensional semiconductor with a flat valence band. The formula has been derived quasiclassically assuming that the exciton is tightly bound; i.e., its ground-state radius is determined by the intrinsic polarizability of the semiconductor rather than by the dielectric properties of the environment. The model is relevant to a few two-dimensional semiconductors discovered recently, including distorted 1T-TiSe$_2$, with a supposedly unstable electronic ground state. The valence band flatness reduces t…
We present the exact spectral function for a single oxygen hole with spin opposite to ferromagnetic order within a one-dimensional CuO$_{3}$-like spin chain. We find that local Kondo-like exchange interaction generates five different states in the strong coupling regime. It stabilizes a spin polaron which is a bound state of a moving charge dressed by magnon excitations, with essentially the same dispersion as predicted by mean field theory. We then examine in detail the evolution of the spectral function for increasing strength of the hole-magnon interaction. We also demonstrate that the $s$ …
We use a mapping of the multiband Hubbard model for $CuO_{3}$ chains in $RBa_{2}Cu_{3}0_{6+x}$ (R=Y or a rare earth) onto a $t-J$ model and the description of the charge dynamics of the latter in terms pf s spinless model, to study the electronic structure of the chains. We briefly review results for the optical conductivity and we calculate the quantum phase diagram of quarter filled chains including Coulomb repulsion up to that between next-nearest-neighbor $Cu$ atoms $V_{2}$, using the resulting effective Hamiltonian, mapped onto an XXZ chain, and the method of crossing of excitation spectr…
We present direct experimental observation of exciton-phonon bound states in the photoluminescence excitation spectra of isolated single walled carbon nanotubes in aqueous suspension. The photoluminescence excitation spectra from several distinct single-walled carbon nanotubes show the presence of at least one sideband related to the tangential modes, lying {200 meV} above the main absorption/emission peak. Both the energy position and line shapes of the sidebands are in excellent agreement with recent calculations [PRL {\bf 94},027402 (2005)] that predict the existence of exciton-phonon bound…
The phase diagram of hole-doped copper oxides shows four different electronic phases existing at zero temperature. Familiar among these are the Mott insulator, high-transition-temperature superconductor and metallic phases. A fourth phase, ofunknown identity, occurs at light doping along the zero-temperature bound of the `pseudogap' regime. This regime is rich in peculiar electronic phenomena, prompting numerous proposals that it contains some form of hidden electronic order. Here we present low-temperature electronic structure imaging studies of a lightly hole-doped copper oxide: Ca_{2-x}Na_{…
The transition temperature $T_\textrm{c}$ of unconventional superconductivity is often tunable. For a monolayer of FeSe, for example, the sweet spot is uniquely bound to titanium-oxide substrates. By contrast for La$_{2-\mathrm{x}}$Sr$_\mathrm{x}$CuO$_4$ thin films, such substrates are sub-optimal and the highest $T_\textrm{c}$ is instead obtained using LaSrAlO$_4$. An outstanding challenge is thus to understand the optimal conditions for superconductivity in thin films: which microscopic parameters drive the change in $T_\mathrm{c}$ and how can we tune them? Here we demonstrate, by a combinat…
Charge excitations were studied for stipe-ordered 214 compounds, La$_{5/3}$Sr$_{1/3}$NiO$_{4}$ and 1/8-doped La$_{2}$(Ba, Sr)$_{x}$CuO$_{4}$ using resonant inelastic x-ray scattering in hard x-ray regime. We have observed charge excitations at the energy transfer of 1 eV with the momentum transfer corresponding to the charge stripe spatial period both for the diagonal (nikelate) and parallel (cuprates) stripes. These new excitations can be interpreted as a collective stripe excitation or charge excitonic mode to a stripe-related in-gap state.
Using the numerical diagonalization method, we examine the one-dimensional t_1-t_2-J_1-J_2 model (zigzag chain t-J model) which represents an effective model for metallic CuO double chain in the superconductor Pr_2Ba_4Cu_7O_15-δ. Based on the Tomonaga-Luttinger liquid theory, we calculate the Luttinger-liquid parameter K_ρas a function of electron density n. It is found that superconductivity is realized in parameter region corresponding to the experimental result. We show phase diagram of spin gap on the t_2/|t_1|-n plane by analyzing the expectation value of twist-operator Z_σin the spin sec…
The effect of impurities which induce local interlayer tunneling in bilayer exciton condensates is discussed. We show that a localized single fermion bound state emerges inside the gap for any strength of impurity scattering and calculate the dependence of the impurity state energy and wave function on the potential strength. We show that such an impurity induced single fermion state enhances the interlayer coherence around it, and is similar to the superconducting proximity effect. As a direct consequence of these single impurity states, we predict that a finite concentration of such impuriti…
Excitonic insulators (EI) arise from the formation of bound electron-hole pairs (excitons) in semiconductors and provide a solid-state platform for quantum many-boson physics. Strong exciton-exciton repulsion is expected to stabilize condensed superfluid and crystalline phases by suppressing both density and phase fluctuations. Although spectroscopic signatures of EIs have been reported, conclusive evidence for strongly correlated EI states has remained elusive. Here, we demonstrate a strongly correlated spatially indirect two-dimensional (2D) EI ground state formed in transition metal dichalc…
In contrast to interband excitons in undoped quantum wells, doped quantum wells do not display sharp resonances due to excitonic bound states. In these systems the effective Coulomb interaction between electrons and holes typically only leads to a depolarization shift of the single-electron intersubband transitions. Non-perturbative light-matter interaction in solid-state devices has been investigated as a pathway to tune optoelectronic properties of materials. A recent theoretical work [Cortese et al., Optica 6, 354 (2019)] predicted that, when the doped quantum wells are embedded in a photon…
