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Register a new userSystematic control of Raman scattering with topologically induced chirality of light
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Stokes Raman scattering is known to be a particularly robust nonlinearity, occurring in virtually every material, with spectra defined by the material and strengths dependent on the material as well as light intensities. This ubiquity has made it an indispensable tool in spectroscopy, but also presents itself as a stubborn source of noise or parasitic emission in several applications. Here, we show that orbital angular momentum carrying light beams experiencing spin-orbit interactions can fundamentally alter the selection rules for Raman scattering. This enables tailoring its spectral shape (by over half the Raman shift in a given material) as well as strength (by about 100 times) simply by controlling the topological charge of light, which is a capability of utility across the multitude of applications where modulating Raman scattering is desired.
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Circular dichroism spectroscopy is an essential technique for understanding molecular structure and magnetic materials, but spatial resolution is limited by the wavelength of light, and sensitivity sufficient for single-molecule spectroscopy is challenging. We demonstrate that electrons can efficiently measure the interaction between circularly polarized light and chiral materials with deeply sub-wavelength resolution. By scanning a nanometer-sized focused electron beam across an optically-excited chiral nanostructure and measuring the electron energy spectrum at each probe position, we produce a high-spatial-resolution map of near-field dichroism. This technique offers a nanoscale view of a fundamental symmetry and could be employed as photon staining to increase biomolecular material contrast in electron microscopy.
We introduce a microscopy technique that facilitates the prediction of spatial features of chirality of nanoscale samples by exploiting photo-induced optical force exerted on an achiral tip in the vicinity of the test specimen. The tip-sample interactive system is illuminated by structured light to probe both the transverse and longitudinal (with respect to the beam propagation direction) components of the sample magnetoelectric polarizability as the manifestation of its sense of handedness, i.e., chirality. We specifically prove that although circularly polarized waves are adequate to detect the transverse polarizability components of the sample, they are unable to probe the longitudinal component. To overcome this inadequacy, we propose a judiciously engineered combination of radially and azimuthally polarized beams, as optical vortices possessing pure longitudinal electric and magnetic field components along their vortex axis, respectively, hence probing longitudinal chirality. The proposed technique may benefit branches of science like stereochemistry, biomedicine, physical and material science, and pharmaceutics
We examine, both experimentally and theoretically, an interaction of tightly focused polarized light with a slit on a metal surface supporting plasmon-polariton modes. Remarkably, this simple system can be highly sensitive to the polarization of the incident light and offers a perfect quantum-weak-measurement tool with a built-in post-selection in the plasmon-polariton mode. We observe the plasmonic spin Hall effect in both coordinate and momentum spaces which is interpreted as weak measurements of the helicity of light with real and imaginary weak values determined by the input polarization. Our experiment combines advantages of (i) quantum weak measurements, (ii) near-field plasmonic systems, and (iii) high-numerical aperture microscopy in employing spin-orbit interaction of light and probing light chirality.
We report the observations of spontaneous Raman scattering in silicon photonic crystal waveguides. Continuous-wave measurements of Stokes emission for both wavelength and power dependence is reported in single line-defect waveguides in hexagonal lattice photonic crystal silicon membranes. By utilizing the Bragg gap edge dispersion of the TM-like mode for pump enhancement and the TE-like fundamental mode-onset for Stokes enhancement, the Stokes emission was observed to increase by up to five times in the region of slow group velocity. The results show explicit nonlinear enhancement in a silicon photonic crystal slow-light waveguide device.
We present an experimental study of the quasi-elastic Raman scattering (QES) of plane-wave and twisted light by liquid crystals. Depending on their temperature, these crystals can exhibit isotropic, nematic and chiral nematic phases. The question is addressed of how the phase of a crystal and the state of incident light can affect the quasi-elastic energy spectra of the scattered radiation, whose shape is usually described by the combination of Lorentzian and Gaussian components. Special attention is paid to the textit{chiral phase}, for which the Raman QES spectrum is dominated by a Lorentzian with reduced linewidth, pointing to diminished disorder and configurational entropy. Moreover, this phase is also known for a regime of iridescence (selective backscattering) which arises when the wavelength of incident light becomes comparable with the chiral pitch length. Detailed measurements, performed in this textit{resonant} regime and by employing twisted light, carrying various projections of the orbital angular momentum (OAM), have indicated a low-energy scattering surplus depending on OAM. We argue that this observation might indicate a transfer of angular momentum between light and the liquid crystal.
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