Frequency shifts in stimulated Raman scattering

The nonresonant contributions to the nonlinear susceptibility χ(3) produce a frequency chirp during stimulated Raman scattering. In the case of transient stimulated Raman scattering, the spectrum of the generated Stokes pulse is found at higher frequencies than expected from spontaneous Raman data. The frequency difference can be calculated from the theory of stimulated Raman scattering

Sum-frequency ionic Raman scattering

In a recent report sum-frequency excitation of a Raman-active phonon was experimentally demonstrated for the first time. This mechanism is the sibling of impulsive stimulated Raman scattering, in which difference-frequency components of a light field excite a Raman-active mode. Here we propose that ionic Raman scattering analogously has a sum-frequency counterpart. We compare the four Raman mechanisms, photonic and ionic difference- and sum-frequency excitation, for three different example materials using a generalized oscillator model for which we calculate the parameters with density functional theory. Sum-frequency ionic Raman scattering completes the toolkit for controlling materials properties by means of selective excitation of lattice vibrations

Theory of Raman Scattering from Orbital Excitations in Manganese Oxides

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.Comment: 10 pages, 7 figure

Electronic Raman scattering in Tl2Ba2CuO6+x: symmetry of the order parameter, oxygen doping effects, and normal state scattering

Single crystals of the optimally doped, moderately and strongly overdoped high temperature superconductor Tl2Ba2CuO6+x (Tl-2201) with Tc=80, 56 and 30K, respectively, have been investigated by polarized Raman scattering. By taking the peak position of the B_1g component of electronic Raman scattering as 2Delta_0 we found that the reduced gap value (2Delta_0/k_BT_c) strongly decreases with increasing doping. The behavior of the low frequency scattering for the B_1g and B_2g scattering components is similar for optimally doped and overdoped crystals and can be described by a w^3 - and w -law, respectively, which is consistent with a d-wave symmetry of the order parameter. In contrast to the optimally doped Tl-2201 in both, moderately and strongly overdoped Tl-2201, the relative (compared to the B_1g) intensity of the A_1g scattering component is suppressed. We suggest that the van Hove singularity is responsible for the observed changes of Raman intensity and reduced gap value with doping. Electronic Raman scattering in the normal state is discussed in the context of the scattering from impurities and compared to the existing infrared data. The scattering rate evaluated from the Raman measurements is smaller for the overdoped samples, compared to the moderately overdoped samples.Comment: 7 pages, 7 figure

A micro-magneto-Raman scattering study of graphene on a bulk graphite substrate

We report on a magneto-Raman scattering study of graphene flakes located on the surface of a bulk graphite substrate. By spatially mapping the Raman scattering response of the surface of bulk graphite with an applied magnetic field, we pinpoint specific locations which show the electronic excitation spectrum of graphene. We present the characteristic Raman scattering signatures of these specific locations. We show that such flakes can be superimposed with another flake and still exhibit a graphene-like excitation spectrum. Two different excitation laser energies (514.5 and 720 nm) are used to investigate the excitation wavelength dependence of the electronic Raman scattering signal.Comment: 6 pages, 5 figure

Phonon Raman scattering of perovskite LaNiO3 thin films

We report an investigation of perovskite-type LaNiO3 thin films by Raman scattering in both various scattering configurations and as a function of temperature. The room-temperature Raman spectra and the associated phonon mode assignment provide reference data for phonon calculations and for the use of Raman scattering for structural investigations of LaNiO3, namely the effect of strain in thin films or heterostructures. The temperature-dependent Raman spectra from 80 to 900 K are characterized by the softening of the rotational A1g mode, which suggest a decreasing rhombohedral distortion towards the ideal cubic structure with increasing temperature

Raman scattering in current carrying molecular junctions. A preliminary account

This is a preliminary acount of a theory for Raman scattering by current-carrying molecular junctions. The approach combines a non-equilibrium Green's function (NEGF) description of the non-equilibrium junction with a generalized scattering theory formulation for evaluating the light scattering signal. This generalizes our previous study (Phys. Rev. Lett. 95, 206802 (2005); J. Chem. Phys. 124, 234709 (2006)) of junction spectroscopy by including molecular vibrations and developing machinery for calculation of state-to-state (Raman scattering) fluxes within the NEGF formalism. For large enough voltage bias we find that the light scattering signal contains, in addition to the normal signal associated with the molecular ground electronic state, also a contribution from the inverse process originated from the excited molecular state as well as an interference component. The effect of coupling to the electrodes and of the imposed bias on the total Raman scattering as well as its components are discussed. Our result reduces to the standard expression for Raman scattering in the isolated molecule case, i.e. in the absence of coupling to the electrodes. The theory is used to discuss the charge transfer contribution to surface enhanced Raman scattering for molecules adsorbed on metal surfaces and its manifestation in the biased junction.Comment: 46 pages, 7 figure