We study the ultrafast phonon response of mixed-valence perovskite Cs$_2$Au$_2$I$_6$ using pump-probe spectroscopy under high-pressure in a diamond anvil cell. We observed a remarkable softening and broadening of the Au - I stretching phonon mode with both applied pressure and photoexcitation. Using a double-pump scheme we measured a lifetime of the charge transfer excitation into single valence Au$^{2+}$ of less than 4 ps, which is an indication of the local character of the Au$^{2+}$ excitation. Furthermore, the strong similarity between the pressure and fluence dependence of the phonon softening shows that the inter-valence charge transfer plays an important role in the structural transition.
Temperature dependent optical conductivity spectra of a La0.7Ca0.3MnO3 (LCMO) sample were measured. In the metallic regime at very low temperatures, they clearly showed two types of absorption features, i.e., a sharp Drude peak and a broad mid-infrared absorption band, which could be explained as coherent and incoherent bands of a large lattice polaron. This elementary excitation in LCMO was found to be in a strong coupling regime and to have interactions with the spin degree of freedom.
Single crystals of electron-doped SrMnO3 with a cubic perovskite structure have been systematically investigated as the most canonical (orbital-degenerate) double-exchange system, whose ground states have been still theoretically controversial. With only 1-2% electron doping by Ce substitution for Sr, a G-type antiferromagnetic metal with a tiny spin canting in a cubic lattice shows up as the ground state, where the Jahn-Teller polarons with heavy mass are likely to form. Further electron doping above 4%, however, replaces this isotropic metal with an insulator with tetragonal lattice distorti…
We have studied the sub-picosecond quasiparticle dynamics in the perovskite manganite La0.7Ca0.3MnO3 and the layered manganite La1.4Sr1.6Mn2O7 using ultrafast optical spectroscopy. We found that for T > TC, initial relaxation proceeds on the time scale of several hundred femtoseconds and corresponds to the redressing of a photoexcited electron to its polaronic ground state. The temperature and dimensionality dependence of this polaron redressing time provides insight into the relationship between polaronic motion and spin dynamics on a sub-picosecond time scale. We also observe a crossover to …
Many transition metal oxides (TMOs) are Mott insulators due to strong Coulomb repulsion between electrons, and exhibit metal-insulator transitions (MITs) whose mechanisms are not always fully understood. Unlike most TMOs, minute doping in CaMnO3 induces a metallic state without any structural transformations. This material is thus an ideal platform to explore band formation through the MIT. Here, we use angle-resolved photoemission spectroscopy to visualize how electrons delocalize and couple to phonons in CaMnO3. We show the development of a Fermi surface where mobile electrons coexist with h…
Polaron-driven switching of octupolar order in doped 5d$^2$ double perovskite
University of Vienna（维也纳大学）；CPHT, CNRS, École polytechnique, Institut Polytechnique de Paris（巴黎综合理工学院）；Collège de France, Université PSL（法兰西公学院）；Department of Physics and Astronomy ”Augusto Righi”, Alma Mater Studiorum - Università di Bologna（博洛尼亚大学）
The coherence of collective modes, such as phonons, and their modulation of the electronic states are long sought in complex systems, which is a cross-cutting issue in photovoltaics and quantum electronics. In photovoltaic cells and lasers based on metal halide perovskites, the presence of polaronic coupling, i.e., photocarriers dressed by the macroscopic motion of charged lattice, assisted by terahertz (THz) longitudinal optical (LO) phonons, has been intensely studied yet still debated. This may be key for explaining the remarkable properties of the perovskite materials, e.g., defect toleran…
Time-resolved transmittance measurements performed on Ga$_{0.94}$Mn$_{0.06}$As in the vicinity of the Mn-induced mid-infrared absorption band are presented. Upon photo-excitation, a slow increase (hundreds of ps timescale) of the differential transmittance is observed and found to be directly related to demagnetization. The temporal profiles of the transmittance and of the demagnetization measured by time-resolved magneto-optical Kerr spectroscopy are found to coincide. Well below the Curie temperature, the maximum amplitude of the slow component of the differential transmittance as a function…
Electron-boson interaction is fundamental to a thorough understanding of various exotic properties emerging in many-body physics. In photoemission spectroscopy, photoelectron emission due to photon absorption would trigger diverse collective excitations in solids, including the emergence of phonons, magnons, electron-hole pairs, and plasmons, which naturally provides a reliable pathway to study electron-boson couplings. While fingerprints of electron-phonon/-magnon interactions in this state-of-the-art technique have been well investigated, much less is known about electron-plasmon coupling, a…
We report x-ray scattering studies of broad peaks located at a (0.5 0 0)/(0 0.5 0)-type wavevector in the paramagnetic insulating phases of La_{0.7}Ca_{0.3}MnO_{3} and Pr_{0.7}Ca_{0.3}MnO_{3}. We interpret the scattering in terms of correlated polarons and measure isotropic correlation lengths of 1-2 lattice constants in both samples. Based on the wavevector and correlation lengths, the correlated polarons are found to be consistent with CE-type bipolarons. Differences in behavior between the samples arise as they are cooled through their respective transition temperatures and become ferromagn…
A fully ab initio scheme based on quantum chemical wavefunction methods is used to investigate the correlated multiorbital electronic structure of a 3d-metal compound, LaCoO3. The strong short-range electron correlations, involving both Co and O orbitals, are treated by multireference techniques. The use of effective parameters like the Hubbard U and interorbital U', J terms and the problems associated with their explicit calculation are avoided with this approach. We provide new insight into the spin-state transition at about 90 K and the nature of charge carriers in the doped material. Our r…
We use the Momentum Average approximation together with perturbative approaches, in the appropriate limits, to study the single polaron physics on a perovskite lattice inspired by BaBiO3. We investigate electron-phonon coupling of the Peierls type whereby the motion of ions modulates the values of the hopping integrals between sites, and show that it cannot be mapped onto the simpler one-band Holstein model in the whole parameter space. This is because the dispersion of the Peierls polaron has sharp transitions where the ground-state momentum jumps between high-symmetry points in the Brillouin…
The interplay of the electron-phonon interaction and of the double and super exchange magnetic effects is analyzed in the $La_{1-x}Ca_xMnO_3$ perovskites with $0<x<0.5$. By using an analytical variational scheme that allows to treat the electron-phonon interaction in a fully quantum manner it is shown that in the intermediate electron-phonon coupling regime a charge density instability occurs near the metal-insulator transition, induced by either temperature or hole doping. The system segregates in antiferromagnetic or paramagnetic small polarons and ferromagnetic large polarons domains charac…
We present a femtosecond optical pump-probe study of the multiferroic manganite Eu$_{0.75}$Y$_{0.25}$MnO$_3$. The optical response of the material at pump energies of 1.55 and 3.1 eV is dominated by the $d$-$d$ and $p$-$d$ transitions of the Mn$^{3+}$ ions. The relaxation of photoexcited electrons includes the relaxation of the Jahn-Teller distortion and polaron trapping at Mn$^{2+}$ and Mn$^{4+}$ sites. Ultrafast switching of superexchange interactions due to modulated $e_g$ orbital occupancy creates a localized spin excitation, which then decays on a time scale of tens of picoseconds at low …
Bismuth perovskites ABiO$_3$ (A = Sr, Ba) host a variety of peculiar phenomena including bond-disproportionated insulating phases and high-temperature superconductivity upon hole doping. While the mechanisms underlying these phenomena are still debated, off-diagonal electron-phonon ($e$-ph) coupling originating from the modulation of the orbital overlaps has emerged as a promising candidate. Here, we employ classical Monte Carlo simulations to study a semiclassical three-orbital model with off-diagonal $e$-ph interactions. We demonstrate the existence of a (bi)polaron correlations that persist…
Neutron scattering has been used to study the nature of the ferromagnetic transition in a single crystal of the perovskite La0.7Ca0.3MnO3. Diffuse scattering from lattice polarons develops as the Curie temperature is approached from below, along with short range polaron correlations that are consistent with stripe formation. Both the scattering due to the polaron correlations and the anomalous quasielastic component in the magnetic fluctuation spectrum maximize very close to T_C, in a manner remarkably similar to the resistivity, indicating that they have a common origin.
We investigate the interplay of electron-phonon (EP) coupling and strong electronic correlations in the frame of the two-dimensional (2D) Holstein t-J model (HtJM), focusing on polaronic ordering phenomena for the quarter-filled band case. The use of direct Lanczos diagonalization on finite lattices allows us to include the effects of quantum phonon fluctuations in the calculation of spin/charge structure factors and hole-phonon correlation functions. In the adiabatic strong coupling regime we found evidence for ``self-localization'' of polaronic carriers in a $(π,π)$ charge-modulated structur…
A previously unreported Pb-based perovskite PbMoO$_3$ is obtained by high-pressure and high-temperature synthesis. This material crystallizes in the $Pm\bar{3}m$ cubic structure at room temperature, making it distinct from typical Pb-based perovskite oxides with a structural distortion. PbMoO$_3$ exhibits a metallic behavior down to 0.1 K with an unusual $T$-sub linear dependence of the electrical resistivity. Moreover, a large specific heat is observed at low temperatures accompanied by a peak in $C_P/T^3$ around 10 K, in marked contrast to the isostructural metallic system SrMoO$_3$. These t…
In order to reveal many-body interactions in the three-dimensional (3D) perovskite manganite, we have performed an $in$ $situ$ angle-resolved photoemission spectroscopy (ARPES) on La$_{0.6}$Sr$_{0.4}$MnO$_3$ (LSMO) and investigated the behaviors of quasiparticles. We observe quasiparticle peaks around the Fermi momentum, both in the electron and the hole bands, and clear kinks throughout the hole Fermi surface in the ARPES band dispersion. The isotropic behavior sharply contrasts to the strong anisotropic quasiparticle excitation observed in layered manganites. These results suggest that polar…
Recent research suggests that the charge carriers in the paramagnetic state of the magnetoresistive manganites are small polarons. Here we report studies of the oxygen-isotope effects on the intrinsic resistivity and thermoelectric power in several ferromagnetic manganites. The precise measurements of these isotope effects allow us to make a quantitative data analysis. Our results do not support a simple small-polaron model, but rather provide compelling evidence for the presence of small immobile bipolarons, i.e., pairs of small polarons. Since the bipolarons in the manganites are immobile, t…
We explore the competiton of doped holes and defects that leads to the loss of orbital order in vanadate perovskites. In compounds such as La$_{1-{\sf x}}$Ca$_{\,\sf x}$VO$_3$ spin and orbital order result from super-exchange interactions described by an extended three-orbital degenerate Hubbard-Hund model for the vanadium $t_{2g}$ electrons. Long-range Coulomb potentials of charged Ca$^{2+}$ defects and $e$-$e$ interactions control the emergence of defect states inside the Mott gap. The quadrupolar components of the Coulomb fields of doped holes induce anisotropic orbital rotations of degener…
We apply the Dynamical Mean Field Theory to the problem of charge ordering. In the normal state as well as in the Charge Ordered (CO) state the existence of polarons, i.e. electrons strongly coupled to local lattice deformation, is associated to the qualitative properties of the Lattice Polarization Distribution Function (LPDF). At intermediate and strong coupling a CO state characterized by a certain amount of thermally activated defects arise from the spatial ordering of preexisting randomly distributed polarons. Properties of this particular CO state gives a qualitative understanding of the…
We calculate the magnetic susceptibility in the pseudogap phase of cuprates using the two-dimensional $t-J$ model and the Mori projection operator technique. In this phase, the Fermi arcs lead to a quasi-elastic incommensurate magnetic response for low temperatures. The theory accounts for the reorientation of the susceptibility maxima from the axial to the diagonal direction occurring at small hole concentrations in La$_{2-x}$Sr$_x$CuO$_4$. A small cusp of the hole dispersion near the Fermi level, which is connected with the spin-polaron band, affords the growth of the maxima with decreasing …
Recently a growing number of experiments have provided indications of the key role of polarons (composite particles formed by a charge strongly coupled with a local lattice deformation) in doped perovskites, hosting colossal magnetoresistance (CMR) and high Tc superconductivity. While the role of polarons is generally recognized in manganites due to the large amplitude of the local lattice deformation, the scientific debate remains open on the cuprates where the lattice deformation is smaller and the anomalous normal metallic phase becomes complex due to the coexistence of polarons with itiner…
An analytical method of studying strong long-range electron-phonon and Coulomb interactions in complex lattices is presented. The method is applied to a perovskite layer with anisotropic coupling of holes to the vibrations of apical atoms. Depending on the relative strength of the polaronic shift, Ep, and the inter-site Coulomb repulsion, Vc, the system is either a polaronic Fermi liquid, Vc > 1.23 Ep, a bipolaronic superconductor, 1.16 Ep < Vc < 1.23 Ep, or a charge segregated insulator, Vc < 1.16 Ep. In the superconducting window, the carriers are mobile bipolarons with a remarkably low effe…
