arXiv subjects

L. L. Miller

Publications and source records attributed to L. L. Miller.

At least 19 recordsLinked to original sources

arXiv2009

Optically induced softening of the charge-transfer gap in Sr2CuO2Cl2

Energy- and time-resolved spectroscopy reveals a photoinduced softening of the charge-transfer gap in the insulating copper oxide Sr2CuO2Cl2 that indicates rapid and efficient photoproduction of optical phonons. By relating the pump-probe signal amplitude to the thermal difference spectrum, we estimate that eleven to twenty optical phonons are created for every one 3 eV photon. Assuming relaxation to the optical absorption edge at 1.5 eV, this corresponds to 70-130 meV per boson. While the lower limit is consistent with relaxation exclusively through optical phonons, the upper limit suggests a significant role for magnetic excitations. We observe a photoinduced bleaching of the gap excitation that we associate with phase space filling, and estimate the excluded area of the photoexcited state to be about nine copper oxide plaquettes. The temporal decay of the pump-probe signal is consistent with anharmonic phonon decay.

cond-mat.str-el↗

arXiv2007

Angle-resolved photoemission studies of lattice polaron formation in the cuprate Ca2CuO2Cl2

To elucidate the nature of the single-particle excitations in the undoped parent cuprates, we have performed a detailed study of Ca2CuO2Cl2 using photoemission spectroscopy. The photoemission lineshapes of the lower Hubbard band are found to be well-described by a polaron model. By comparing the lineshape and temperature dependence of the lower Hubbard band with additional O 2p and Ca 3p states, we conclude that the dominant broadening mechanism arises from the interaction between the photohole and the lattice. The strength of this interaction was observed to be strongly anisotropic and may have important implications for the momentum dependence of the first doped hole states.

cond-mat.str-el↗

arXiv2006

Field dependence of the magnetic spectrum in anisotropic and Dzyaloshinskii-Moriya antiferromagnets: II. Raman spectroscopy

We compare the theoretical predictions of the previous article [L. Benfatto and M. B. Silva Neto, cond-mat/0602419], with Raman spectroscopy experiments in Sr(2)CuO(2)Cl(2) and untwinned La(2)CuO(4) single crystals. We construct the magnetic point group for the magnetically ordered phase of the two compounds, Sr(2)CuO(2)Cl(2) and La(2)CuO(4), and we classify all the Raman active one-magnon excitations according to the irreducible co-representations for the associated magnetic point group. We then measure the evolution of the one-magnon Raman energies and intensities for low and moderate magnetic fields along the three crystallographic directions. In the case of La(2)CuO(4), we demonstrate that from the jump of the Dzyaloshinskii-Moriya gap at the critical magnetic field H_c ~ 6.6 T for the weak-ferromagnetic transition one can determine the value of the interlayer coupling J_\perp/J ~ 3.2 x 10^-5. We furthermore determine the components of the anisotropic gyromagnetic tensor as g_s^a=2.0, g_s^b=2.08, and the upper bound g_s^c=2.65. For the case of Sr(2)CuO(2)Cl(2), we compare the Raman data obtained in an in-plane magnetic field with previous magnon-gap measurements done by ESR. Using the very low magnon gap estimated by ESR (~ 0.05 meV), the data for the one-magnon Raman energies agree reasonably well with the theoretical predictions for the case of a transverse field (only hardening of the gap).

cond-mat.str-el↗

arXiv2006

Anomalous high energy dispersion in photoemission spectra from insulating cuprates

Angle resolved photoelectron spectroscopic measurements have been performed on an insulating cuprate Ca_2CuO_2Cl_2. High resolution data taken along the Γto (pi,pi) cut show an additional dispersive feature that merges with the known dispersion of the lowest binding energy feature, which follows the usual strongly renormalized dispersion of ~0.35 eV. This higher energy part reveals a dispersion that is very close to the unrenormalized band predicted by band theory. A transfer of spectral weight from the low energy feature to the high energy feature is observed as the Γpoint is approached. By comparing with theoretical calculations the high energy feature observed here demonstrates that the incoherent portion of the spectral function has significant structure in momentum space due to the presence of various energy scales.

cond-mat.str-el↗

arXiv2004

Missing Quasiparticles and the Chemical Potential Puzzle in the Doping Evolution of the Cuprate Superconductors

The evolution of Ca$_{2-x}$Na$_{x}$CuO$_{2}$Cl$_{2}$ from Mott insulator to superconductor was studied using angle-resolved photoemission spectroscopy. By measuring both the excitations near the Fermi energy as well as non-bonding states, we tracked the doping dependence of the electronic structure and the chemical potential with unprecedented precision. Our work reveals failures in the conventional quasiparticle theory, including the broad lineshapes of the insulator and the apparently paradoxical shift of the chemical potential within the Mott gap. To resolve this, we develop a model where the quasiparticle is vanishingly small at half filling and grows upon doping, allowing us to unify properties such as the dispersion and Fermi wavevector with the behavior of the chemical potential.

cond-mat.supr-con↗

arXiv2003

Evolution of a Metal to Insulator Transition in Ca$_{2-x}$Na$_{x}$CuO$_{2}$Cl$_{2}$, as seen by ARPES

We present angle resolved photoemission (ARPES) data on Na-doped Ca$_2$CuO$_2$Cl$_2$. We demonstrate that the chemical potential shifts upon doping the system across the insulator to metal transition. The resulting low energy spectra reveal a gap structure which appears to deviate from the canonical $d_{x2-y2} ~ |cos(k_x a)-cos(k_y a)|$ form. To reconcile the measured gap structure with d-wave superconductivity one can understand the data in terms of two gaps, a very small one contributing to the nodal region and a very large one dominating the anti-nodal region. The latter is a result of the electronic structure observed in the undoped antiferromagnetic insulator. Furthermore, the low energy electronic structure of the metallic sample contains a two component structure in the nodal direction, and a change in velocity of the dispersion in the nodal direction at roughly 50 meV. We discuss these results in connection with photoemission data on other cuprate systems.

cond-mat.str-el↗

arXiv2002

Universality of the Electronic Structure from a Half Filled CuO_2 Plane

We present angle resolved photoemission (ARPES) data from insulating A_2CuO_2X_2 (A=Sr, Ca; X=Cl, Br), Sr_2Cu_3O_4Cl_2, and Bi_2Sr_2MCu_2O_8 (M=Er, Dy) single crystals which illustrate that the low energy electronic structure of the half-filled cuprates are independent of the apical atom. By performing a photon energy dependent study on Ca_2CuO_2Cl_2 we are able to distinguish between features which are intrinsic and those which are a result of the photoemission matrix elements. We find that the dispersion is independent of photon energy, while an asymmetry in the electron occupation probability across the antiferromagnetic zone boundary is robust to variations in photon energy. Finally, we show that the d-wave-like dispersion which exists in the insulator along the antiferromagnetic zone boundary does not precisely fit the simple d-wave functional form near the nodal direction.

cond-mat.str-el↗

arXiv2001

Parity forbidden excitations of Sr2CuO2Cl2 revealed by optical third-harmonic spectroscopy

We present the first study of nonlinear optical third harmonic generation in the strongly correlated charge-transfer insulator Sr2CuO2Cl2. For fundamental excitation in the near-infrared, the THG spectrum reveals a strongly resonant response for photon energies near 0.7 eV. Polarization analysis reveals this novel resonance to be only partially accounted for by three-photon excitation to the optical charge-transfer exciton, and indicates that an even-parity excitation at 2 eV, with a_1g symmetry, participates in the third harmonic susceptibility.

cond-mat.str-el↗

arXiv2001

Momentum-Resolved Inelastic X-ray Scattering as a Novel Tool to Study Charge Gap in Complex Insulators

We report particle-hole pair excitations in a cuprate insulator in the intermediate regimes of momentum-transfers using high energy inelastic x-ray scattering. The excitation spectra show dispersive features near the Mott edge which shed light on the momentum structure of the upper Hubbard band in cuprates. We briefly discuss the potential use of such a technique to study the momentum dependence of unoccupied bands and q-dependent charge fluctuations in complex insulators.

cond-mat.str-el↗

arXiv2001

Electronic Structure of Mott Insulators Studied by Inelastic X-ray Scattering

The electronic structure of Mott insulators continues to be a major unsolved problem in physics despite more than half-century of intense research efforts. Well-developed momentum-resolved spectroscopies such as photoemission or neutron scattering cannot probe the full Mott gap. We report observation of dispersive charge excitations across the Mott gap in a high Tc parent cuprate Ca2CuO2Cl2 using high resolution resonant inelastic x-ray scattering shedding light on the anisotropy of Mott-gap. The results provide direct support for the Hubbard model to describe charge excitations across the Mott gap.

cond-mat.str-el↗

arXiv2001

Evidence of phonon mediated coupling between charge transfer and ligand field excitons in Sr$_2$CuO$_2$Cl$_2$

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.

cond-mat.str-el↗

arXiv2000

n(k) Structure and Matrix Elements in Photoemission: Results from Insulating Ca_2CuO_2Cl_2

The photon energy dependence of angle-resolved photoemission data on Ca_2CuO_2Cl_2 is presented, and the role of the matrix element is investigated. It is shown that despite strong variations in the matrix element, the loss in intensity as one crosses the antiferromagnetic zone boundary is a robust feature of the Mott insulator. As expected for a two dimensional system, the dispersion remains independent of the photon energy even when the matrix element does not.

cond-mat.str-el↗

arXiv2000

No well-defined remnant Fermi surface in Sr2CuO2Cl2

In angle-resolved photoelectron spectra of the antiferromagnetic insulators Ca2CuO2Cl2 and Sr2CuO2Cl2 a sharp drop of the spectral intensity of the lowest-lying band is observed along a line in k space equivalent to the Fermi surface of the optimally doped high-temperature superconductors. This was interpreted as a signature of the existence of a remnant Fermi surface in the insulating phase of the high-temperature superconductors. In this paper it is shown that the drop of the spectral intensity is not related to the spectral function but is a consequence of the electron-photon matrix element

cond-mat.supr-con↗

arXiv2000

Magnetic Susceptibilities of Spin-1/2 Antiferromagnetic Heisenberg Ladders and Applications to Ladder Oxide Compounds

A comprehensive theoretical and experimental study is presented of the magnetic susceptibility versus temperature χ(T) of spin S = 1/2 two- and three-leg Heisenberg ladders and ladder oxide compounds. Extensive quantum Monte Carlo simulations of χ(T) were carried out for both isolated and coupled two-leg ladders with spatially anisotropic intraladder exchange. Accurate fits to these and related literature QMC data were obtained. We have also calculated the one- and two-magnon dispersion relations and the dynamical spin structure factor for anisotropic isolated 2 x 12 ladders. The exchange constants in the two-leg ladder compound SrCu2O3 are estimated from LDA+U calculations. We report the detailed crystal structure of SrCu2O3 and of the three-leg ladder compound Sr2Cu3O5. New experimental χ(T) data are reported for the two-leg ladder cuprates SrCu2O3 and LaCuO_{2.5}, and for the (nominally) two-leg ladder vanadates CaV2O5 and MgV2O5. The new and literature χ(T) data for these compounds and for Sr2Cu3O5 are modeled using our QMC χ(T) simulation fits, and the exchange coupling constants between the spins-1/2 are thereby estimated for each material. The surpisingly strong spatial anisotropy of the bilinear intraladder exchange constants in the cuprate compounds is discussed together with the results of other experiments sensitive to this anisotropy. Recent theoretical predictions are discussed including those which indicate that a four-spin cyclic exchange interaction within a Cu4 plaquette is important to determining the magnetic properties and which can significantly influence the exchange interactions estimated from χ(T) data assuming the presence of only bilinear exchange.

cond-mat.str-el↗

arXiv1999

Spin Liquid State around a Doped Hole in Insulating Cuprates

The numerically exact diagonalization study on small clusters of the t-J model with the second- and third- neighbor hopping terms shows that a novel spin liquid state is realized around a doped hole with momentum k=(pi,0) and energy \sim 2J compared with that with (pi/2,pi/2) in insulating cuprates, where the spin and charge degrees of freedom are approximately decoupled. Our finding implies that the excitations in the insulating cuprates are mapped onto the the d-wave resonating valence bond state.

cond-mat.str-el↗

arXiv1999

Selection Rules for Resonant Inelastic X-Ray Scattering from Tetragonal Copper-Oxides

We demonstrate the utility of point group representation theory for symmetry analysis in resonant inelastic x-ray scattering. From its polarization-dependence, we show that a 5 eV inelastic feature in Sr2CuO2Cl2 has pure B1g symmetry and assign it to a transition in the cell-perturbation calculations of Simon, et. al. [Phys. Rev. B., 54, R3780 (1996)]. We discuss how Raman selection rules are broken at nonzero momentum transfer and how this can also act as a probe of wave function symmetry.

cond-mat.str-el↗

arXiv1999

Resonant Inelastic X-Ray Scattering from Valence Excitations in Insulating Copper-Oxides

We report resonant inelastic x-ray measurements of insulating La$_2$CuO$_4$ and Sr$_2$CuO$_2$Cl$_2$ taken with the incident energy tuned near the Cu K absorption edge. We show that the spectra are well described in a shakeup picture in 3rd order perturbation theory which exhibits both incoming and outgoing resonances, and demonstrate how to extract a spectral function from the raw data. We conclude by showing {\bf q}-dependent measurements of the charge transfer gap.

cond-mat.str-el↗

arXiv1999

Photoemission Evidence for a Remnant Fermi Surface and d-Wave-Like Dispersion in Insulating Ca2CuO2Cl2

An angle resolved photoemission study on Ca2CuO2Cl2, a parent compound of high Tc superconductors is reported. Analysis of the electron occupation probability, n(k) from the spectra shows a steep drop in spectral intensity across a contour that is close to the Fermi surface predicted by the band calculation. This analysis reveals a Fermi surface remnant even though Ca2CuO2Cl2 is a Mott insulator. The lowest energy peak exhibits a dispersion with approximately the |cos(kxa)-cos(kya)| form along this remnant Fermi surface. Together with the data from Dy doped Bi2Sr2CaCu2O(8 + delta) these results suggest that this d-wave like dispersion of the insulator is the underlying reason for the pseudo gap in the underdoped regime.

cond-mat.supr-con↗