The Raman effect -- inelastic scattering of light by lattice vibrations (phonons) -- produces an optical response closely tied to a materials crystal structure. Here we show that resonant optical excitation of IR and Raman phonons gives rise to a Raman scattering effect that can induce giant shifts to the refractive index and induce new optical constants that are forbidden in the equilibrium crystal structure. We complete the description of light-matter interactions mediated by coupled IR and Raman phonons in crystalline insulators -- currently the focus of numerous experiments aiming to dynamically control material properties -- by including a forgotten pathway through the nonlinear lattice polarizability. Our work expands the toolset for control and development of new optical technologies by revealing that the absorption of light within the terahertz gap can enable control of optical properties of materials over a broad frequency range.
We report on the temperature dependence of the $ZrTe_5$ electronic properties, studied at equilibrium and out of equilibrium, by means of time and angle resolved photoelectron spectroscopy. Our results unveil the dependence of the electronic band structure across the Fermi energy on the sample temperature. This finding is regarded as the dominant mechanism responsible for the anomalous resistivity observed at T* $sim$ 160 K along with the change of the charge carrier character from holelike to electronlike. Having addressed these long-lasting questions, we prove the possibility to control, at the ultrashort time scale, both the binding energy and the quasiparticle lifetime of the valence band. These experimental evidences pave the way for optically controlling the thermoelectric and magnetoelectric transport properties of $ZrTe_5$.
We explore the hybridization of fundamental material resonances with the artificial resonances of metamaterials. A hybrid structure is presented in the waveguide environment that consists of a resonant magnetic material with a characteristic tuneable gyromagnetic response that is integrated into a complementary split ring resonator (CSRR) metamaterial structure. The combined structure exhibits a distinct hybrid resonance in which each natural resonance of the CSRR is split into a lower and upper resonance that straddle the frequency for which the magnetic materials permeability is zero. We provide an analytical understanding of this hybrid resonance and define an effective medium theory for the combined structure that demonstrates good agreement with numerical electromagnetic simulations. The designed structure demonstrates the potential for using a ferrimagnetic or ferromagnetic material as a means of creating a tunable metamaterial structure.
We study how the color and polarization of ultrashort pulses of visible light can be used to control the demagnetization processes of the antiferromagnetic insulator Cr$_2$O$_3$. We utilize time-resolved second harmonic generation (SHG) to probe how changes in the magnetic and structural state evolve in time. We show that, varying the pump photon-energy to excite either localized transitions within the Cr or charge transfer states, leads to markedly different dynamics. Through a full polarization analysis of the SHG signal, symmetry considerations and density functional theory calculations, we show that, in the non-equilibrium state, SHG is sensitive to {em both} lattice displacements and changes to the magnetic order, which allows us to conclude that different excited states couple to phonon modes of different symmetries. Furthermore, the spin-scattering rate depends on the induced distortion, enabling us to control the timescale for the demagnetization process. Our results suggest that selective photoexcitation of antiferromagnetic insulators allows fast and efficient manipulation of their magnetic state.
Resonant Raman spectra (RRS) of O-H and O-D vibration and libration modes, their combinations and higher harmonics have been observed in LiTaO3 polycrystalline thin films. RRS peaks are superimposed on photoluminescence (PL) spectrum. Monochromatic light from a xenon lamp is used as excitation source. PL spectrum shows two broad peaks, first near the band gap in UV (4.4-4.8eV) and another in the sub band gap region (< 4.0 eV). Band gap PL along with RRS peaks are reported for the first time. Photoluminescence excitation spectrum (PLE) shows a peak at 4.8 eV. Peak positions and full width at half maximum (FWHM) of RRS peaks depend upon the excitation energy. Dispersions of the fundamental and the third harmonic of the stretching mode of O-H with excitation energy are about 800 cm-1/eV and 2000 cm-1/eV respectively. This dispersion is much higher than reported in any other material.
All-optical pump-probe detection of magnetization precession has been performed for ferromagnetic EuO thin films at 10 K. We demonstrate that the circularly-polarized light can be used to control the magnetization precession on an ultrafast time scale. This takes place within the 100 fs duration of a single laser pulse, through combined contribution from two nonthermal photomagnetic effects, i.e., enhancement of the magnetization and an inverse Faraday effect. From the magnetic field dependences of the frequency and the Gilbert damping parameter, the intrinsic Gilbert damping coefficient is evaluated to be {alpha} approx 3times10^-3.