We investigated temperature dependent Raman spectra of the one-dimensional spin-ladder compound SrCu2O3. At low temperatures a two-magnon peak is identified at 3160+/-10 cm^(-1) and its temperature dependence analyzed in terms of a thermal expansion model. We find that the two-magnon peak position must include a cyclic ring exchange of J_cycl/J_perp=0.09-0.25 with a coupling constant along the rungs of J_perp approx. 1215 cm^(-1) (1750 K) in order to be consistent with other experiments and theoretical results.
We present a theory of the Raman scattering from the orbital wave excitations in manganese oxides. Two excitation processes of the Raman scattering are proposed. The Raman scattering cross section is formulated by using the pseudospin operator for orbital degree of freedom in a Mn ion. The Raman spectra from the orbital wave excitations are calculated and their implications in the recent experimental results reported in LaMnO$_3$ are discussed.
We measure Raman scattering in an interacting spin-dimer system KCuCl3 under hydrostatic pressures up to 5 GPa mediated by He gas. In the pressure-induced quantum phase, we observe a one-magnon Raman peak, which originates from the longitudinal magnetic excitationand is observable through the second-order exchange interaction Raman process. We report the pressure dependence of the frequency, halfwidth and Raman intensity of this mode.
We consider Raman scattering of coupled two leg spin ladders in the Fleury-Loudon regime. We derive the dependence of the intensity with polarization of the incoming light and temperature and discuss the effect of interaction of the elementary excitations on the shape of the spectrum. We show that Raman scattering spectrum is sensitive to the effective dimensionality of the coupled ladder system, making Raman scattering useful to discriminate true ladder systems from quasi two dimensional spin gap systems.
We explain quantitatively why resonant Raman scattering spectroscopy, an extensively used experimental tool in studying elementary electronic excitations in doped low dimensional semiconductor nanostructures, always produces an observable peak at the so-called "single particle" excitation although the standard theory predicts that there should be no such single particle peak in the Raman spectra. We have thus resolved an experimental puzzle which dates back more than twenty-five years.
We have performed Raman scattering measurements on URu$_2$Si$_2$ single crystals on a large energy range up to $\sim$ 1300 cm$^{-1}$ and in all the Raman active symmetries as a function of temperature down to 15 K. A large excitation, active only in the E$_{g}$ symmetry, is reported. It has been assigned to a crystal electric field excitation on the Uranium site. We discuss how this constrains the crystal electric field scheme of the Uranium ions. Furthermore, three excitations in the A$_{1g}$ symmetry are observed. They have been associated to double Raman phonon processes consistently with a…
Using Raman spectroscopy, we investigate the lattice phonons, magnetic excitations, and magneto-elastic coupling in the distorted triangular-lattice Heisenberg antiferromagnet alpha-SrCr2O4, which develops helical magnetic order below 43 K. Temperature dependent phonon spectra are compared to predictions from density functional theory calculations which allows us to assign the observed modes and identify weak effects arising from coupled lattice and magnetic degrees of freedom. Raman scattering associated with two-magnon excitations is observed at 20 meV and 40 meV. These energies are in gener…
The fractionalization of elementary excitations in quantum spin systems is a central theme in current condensed matter physics. The Kitaev honeycomb spin model provides a prominent example of exotic fractionalized quasiparticles, composed of itinerant Majorana fermions and gapped gauge fluxes. However, identification of the Majorana fermions in a three-dimensional honeycomb lattice remains elusive. Here we report spectroscopic signatures of fractional excitations in the harmonic-honeycomb iridates $β$- and $γ$-Li$_2$IrO$_3$. Using polarization resolved Raman spectroscopy, we find that the dyna…
We report low-temperature (down to $\sim$5 K) Raman signatures of the recently discovered intercalated honeycomb magnet Ag$_3$LiIr$_2$O$_6$, a putative Kitaev quantum spin liquid (QSL) candidate. The Kitaev QSL is predicted to host Majorana fermions as its emergent elementary excitations through a thermal fractionalization of entangled spins $S = 1/2$. We observe evidence of this fractionalization in the low-energy magnetic continuum whose temperature evolution harbours signatures of the predicted Fermi statistics obeyed by the itinerant Majorana quasiparticles. The magnetic Raman susceptibili…
We investigate the two-magnon Raman scattering from an anisotropic S=1/2 triangular Heisenberg antiferromagnet Cs2CuCl4. We find that the Raman response is very sensitive to magnon-magnon interactions and to scattering geometries, a feature that is in remarkable contrast with the polarization-independent Raman signal from the isotropic triangular Heisenberg antiferromagnet. Since a spin-liquid ground state gives rise to a similar rotationally invariant Raman response, our results on the polarization dependence of the scattering spectrum suggest that Raman spectroscopy provides a useful probe, …
Nonlinear processes involving frequency-mixing of light fields set the basis for ultrafast coherent spectroscopy of collective modes in solids. In certain semimetals and semiconductors, generation of coherent phonon modes can occur by a displacive force on the lattice at the difference-frequency mixing of a laser pulse excitation on the electronic system. Here, as a low-frequency counterpart of this process, we demonstrate that coherent phonon excitations can be induced by the sum-frequency components of an intense terahertz light field, coupled to intraband electronic transitions. This nonlin…
We present a Raman light scattering study of the two-dimensional quantum spin system SrCu2(BO3)2 and show that the magnetic excitation spectrum has a rich structure, including several well-defined bound state modes at low temperature, and a scattering continuum and quasielastic light scattering contributions at high temperature. The key to the understanding of the unique features of SrCu2(BO3)2 is the presence of strong interactions between well-localized triplet excitations in the network of orthogonal spin dimers realized in this compound. Based on our analysis of the Heisenberg model releva…
We develop a generic theory for the resonant inelastic light (Raman) scattering by a conduction band quantum plasma taking into account the presence of the filled valence band in doped semiconductor nanostructures within a generalized resonant random phase approximation (RPA). Our generalized RPA theory explicitly incorporates the two-step resonance process where an electron from the filled valence band is first excited by the incident photon into the conduction band before an electron from the conduction band falls back into the valence band emitting the scattered photon. We show that when th…
We report the observation of the $A_{\rm g}$-symmetric one-magnon Raman peak in the magnon Bose-Einstein condensation phase of TlCuCl$_{3}$. Its Raman shift traces the one-magnon energy at the magnetic $Γ$ point, and its intensity is proportional to the squared transverse magnetization. The appearance of the one-magnon Raman scattering originates from the exchange magnon Raman process and reflects the change of the magnetic-state symmetry. Using the bond-operator representation, we theoretically clarify the Raman selection rules, being consistent with the experimental results.
Spin-orbit interaction in Sr$_2$IrO$_4$ leads to the realization of the $J_{\mathrm{eff}}$ = 1/2 state and also induces an insulating behavior. Using large-shift Raman spectroscopy, we found two high-energy excitations of the d-shell multipletat at 690 meV and 680 meV with $A_{1g}$ and $B_{1g}$ symmetry respectively. As temperature decreases, the $A_{1g}$ and $B_{1g}$ peaks narrow, and the $A_{1g}$ peak shifts to higher energy while the energy of the $B_{1g}$ peak remains the same. When 25$\%$ of Ir is substituted with Rh the $A_{1g}$ peak softens by 10$\%$ but the $B_{1g}$ peak does not. We s…
The Raman scattering spectra from magnetic excitations in an antiferromagnetic spin-1/2 two leg ladder is investigated for weak and strong interladder coupling. In the first case, a cusp in the Raman intensityis obtained at a frequency twice the gap. In the second case, a peak at twice the gap replaces the cusp. We discuss the relevance of our calculation to recent experiments on CaV2O5 and Sr14Cu24O41.
We present two different theories for Raman scattering and Resonant Inelastic X-ray Scattering (RIXS) in the low temperature ferromagnetic phase of YTiO$_3$ and compare this to the available experimental data. For description of the orbital ground-state and orbital excitations, we consider two models corresponding to two theoretical limits: one where the $t_{2g}$ orbitals are degenerate, and the other where strong lattice distortions split them. In the former model the orbitals interact through superexchange. The resulting superexchange Hamiltonian yields an orbitally ordered ground state with…
We present calculations of the intensity of polariton-mediated inelastic light scattering in semiconductor microcavities within a Green's function framework. In addition to reproducing the strong coupling of light and matter, this method also enables the inclusion of damping mechanisms in a consistent way. Our results show excellent agreement with recent Raman scattering experiments.
Resonant Raman scattering of degenerate interacting two-channel quantum wire is studied. {\it All} collective excitations of two-channel quantum wire are shown to give rise to peaks in the polarized Raman spectra near resonance. If there exist certain symmetries among interactions, a resonant peak can also appear in the {\it depolarized} Raman spectra, in constrast to the single-channel case studied by Sassetti and Kramer. We also calculate the explicit form of the scattering cross-section away from the peaks. The above features may be experimentally verified in armchair carbon nanotube system…
Recent Raman scattering data in B_{1g} and B_{2g} geometries in the superconducting state of underdoped cuprates were interpreted as evidence for two distinct energy gaps. We argue that these data can be equally well explained within a one gap scenario if final state interactions are taken into account. In particular, we show that they can account for the differing doping dependences of the Raman peaks in these two geometries.
A theory of electronic Raman scattering in nearly antiferromagnetic Fermi liquids is constructed using the phenomenological electron-electron interaction introduced by Millis, Monien, and Pines. The role of "hot spots" and their resulting signatures in the channel dependent Raman spectra is highlighted, and different scaling regimes are addressed. The theory is compared to Raman spectra taken in the normal state of overdoped Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$, and it is shown that many features of the symmetry dependent spectra can be explained by the theory.
Magnetic Raman scattering from a frustrated spin-1/2 Heisenberg-chain is considered with a focus on the uniform phase of the spin-Peierls compound CuGeO_3. The Raman intensity is analyzed in terms of a Loudon-Fleury scattering process using a spinless-fermion mean-field theory developed for the frustrated spin-chain. A comparison to experimental data is presented and the frustration and temperature dependence is studied. In good agreement with observed spectra a broad inelastic four-spinon continuum is found at low temperatures above the spin-Peierls transition. At high temperatures the intens…
Low energy excitations in the multiferroic material TbMnO3 have been investigated by Raman spectroscopy. Our observations reveal the existence of two peaks at 30 cm-1 and 60 cm-1. They are observed in the cycloidal phase below the Curie temperature but not in the sinusoidal phase, suggesting their magnetoelectric origin. While the peak energies coincide with the frequencies of electromagnons measured previously by transmission spectroscopy, they show surprisingly different selection rules, with the 30 cm-1 excitation enhanced by the electric field of light along the spontaneous polarization. T…
We report a polarized Raman study of Weyl semimetal TaAs. We observe all the optical phonons, with energies and symmetries consistent with our first-principles calculations. We detect additional excitations assigned to multiple-phonon excitations. These excitations are accompanied by broad peaks separated by 140~cm$^{-1}$ that are also most likely associated with multiple-phonon excitations. We also noticed a sizable B$_1$ component for the spectral background, for which the origin remains unclear.
Unconventional peak structure in the Raman spectra due to magnon excitation at low temperature is observed in spinel magnet ${\rm MnV_2O_4}$, where a noncollinear spin state is realized by geometrical frustration. We propose a new mechanism to induce such a Raman scattering process due to a one-magnon excitation of the noncollinear spin state. Novel features of the scattering such as selection rules and peak position observed experimentally in ${\rm MnV_2O_4}$ can be explained quite naturally by considering the present one-magnon process. We also discuss that such one-magnon process may exist …
Inelastic low-energy Raman and high-energy X-ray scatterings have made great progress in instrumentation to investigate the strong electronic correlations in matter. However, theoretical study of the relevant scattering spectrum is still a challenge. In this article, we present a Schwinger-Keldysh canonical perturbation formalism for the electronic Raman scattering, where all the resonant, non-resonant and mixed responses are considered uniformly. We show how to use this formalism to evaluate the cross section of the electronic Raman scattering off an one-band superconductor. All the two-photo…
We show that the low-energy peak in the polarized resonant Raman spectra of quantum wires, which is commonly associated with ``single particle excitations'', can be interpreted as signature of intra-band collective spin excitations. A broad maximum in the resonant depolarized spectra is predicted to exist above the frequency of the spin density excitation, due to simultaneous but independent propagation of spin- and charge-density modes.
Calculations are presented for electronic Raman scattering and infrared conductivity in a $d_{x^{2}-y^{2}}$ superconductor including the effects of elastic scattering via anisotropic impurities and inelastic spin-fluctuation scattering. A consistent description of experiments on optimally doped Bi-2212 is made possible by considering the effects of correlations on both inelastic and elastic scattering.
We calculate the resonant electronic Raman scattering for the Falicov-Kimball model near the Mott transition on a hypercubic lattice. The solution is exact, and employs dynamical mean field theory.
We report on the lattice and spin dynamics in the monopnictide CrAs using polarized Raman scattering. This system exhibits a first-order magneto-structural phase transition at T_N~ 265 K, below which the magnetic moments of Cr form an incommensurate double helical magnetic structure while the unit cell volume abruptly expands. Across the transition, the frequencies of the fully symmetric Ag phonons strongly renormalize, which along with the results of first-principle calculations suggest the presence of a sizeable coupling of the phonons to the magnetic degrees of freedom in this compound. In …
Motivated by recent transport and neutron scattering experiments suggesting an orientational symmetry breaking in underdoped cuprates we present a theoretical study of Raman scattering near a d-wave Pomeranchuk instability (PI). The d-wave component of Raman scattering from electrons and phonons allows to study directly order parameter fluctuations associated with the PI. Approaching the PI from the normal state by lowering the temperature a central peak emerges both in electronic and, as an additional low-frequency feature, in phononic scattering. Approaching the PI in the superconducting sta…
The numerically exact solution for nonresonant B1g Raman scattering is presented for the half-filled Hubbard model in infinite dimensions. This solution illustrates the modifications of the Raman response (in a system tuned through the quantum-critical point of a metal-insulator transition) due to Fermi-liquid properties in the metallic phase. In the insulating phase, we recover the predicted universal behavior, while we find the Raman response is quite anomalous on the metallic side of the transition. Our calculated results are similar to those measured in FeSi, SmB6, and underdoped cuprates.
We present an exact solution for electronic Raman scattering in a single-band, strongly correlated material, including nonresonant, resonant and mixed contributions. Results are derived for the spinless Falicov-Kimball model, employing dynamical mean field theory; this system can be tuned through a Mott metal-insulator transition.
The Raman response of the metallic glass Ni$_{67}$Zr$_{33}$ is measured as a function of polarization and temperature and analyzed theoretically. Unexpectedly, the intensity in the range up to 300\wn increases upon cooling, which is counterintuitive when the response originates from vibrations alone as in insulators. The increase finds a natural explanation if the conduction electrons are assumed to scatter on localized vibrations with a scattering probability proportional to the Debye-Waller factor. None of our assumptions is material specific, and the results are expected to be relevant for …
We study theoretically the Raman scattering spectra in the one-dimensional (1D) quantum spin-1/2 antiferromagnets. The analysis reveals that their low-energy dynamics is exquisitely sensitive to various perturbations to the Heisenberg chain with nearest-neighbor exchange interactions, such as magnetic anisotropy, longer-range exchange interactions, and bond dimerization. These weak interactions are mainly responsible for the Raman scattering and give rise to different types of spectra as functions of frequency, temperature, and external field. In contrast to the Raman spectra in higher dimensi…
