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Langmuir mechanism of low-frequency stimulated Raman scattering on nanoscale objects

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 Added by Vadim Oshurko
 Publication date 2021
  fields Physics
and research's language is English




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A simple physical mechanism of stimulated light scattering on nanoscale objects in water suspension similar to Langmuir waves mechanism in plasma is proposed. The proposed mechanism is based on a dipole interaction between the light wave and the non-compensated electrical charge that inevitably exists on a nanoscale object (a virus or a nanoparticle) in water environment. The experimental data for tobacco mosaic virus and polystyrene nanospheres are presented to support the suggested physical mechanism. It has been demonstrated that stimulated amplification spectral line frequencies observed experimentally are well explained by the suggested mechanism. In particular, the absence of lower frequency lines and the generation lines shift when changing the pH are due to ion friction appearing in the ionic solution environment. The selection rules observed experimentally also confirm the dipole interaction type. It has been shown that microwave radiation on nanoscale object acoustic vibrations frequency should appear under such scattering conditions. We demonstrate that such conditions also allow for local selective heating of nanoscale objects by dozens to hundreds degrees K. This effect is controlled by the optical irradiation parameters and can be used for affecting selectively certain types of viruses.



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Laser pulses interaction with tobacco mosaic virus (TMV) in Tris-HCl pH7.5 buffer and in water has been investigated. 20 ns ruby laser pulses have been used for excitation. Spectrum of the light passing through the sample was registered with the help of Fabri-Perot interferometer. In the case of TMV in water we observed in the spectrum only one line of the exciting laser light, for TMV in Tris-HCl pH7.5 buffer second line appeared, corresponding to the stimulated low-frequency Raman scattering (SLFRS) on the breathing radial mode of TMV. SLFRS frequency shift by 2 cm-1, (60 GHz), conversion efficiency and threshold are measured for the first time to the best of our knowledge.
Stimulated low-frequency Raman scattering can give essential information about the elastic properties of different nanoparticles systems, in particular, biological nanostructures. In the present study, low-frequency vibrational modes in human and bovine serum albumin were for the first time investigated using stimulated low-frequency Raman scattering. Stimulated low-frequency Raman scattering frequency shifts, corresponding to acoustic eigenfrequencies of the sample, were registered by Fabri-Perot interferometers. Conversion efficiency, threshold and set of eigenfrequencies were also measured. Stimulated low-frequency Raman scattering can be applied for biological objects identification and impact on them.
Backward stimulated Raman scattering (BSRS) with Langmuir decay instability (LDI) and Langmuir collapse has been researched by Vlasov simulation for the first time. The decay productions of LDI cascade and their evolution with time is clearly demonstrated, which occurs simultaneously with Langmuir collapse. The BSRS reflectivity will be decreased largely through LDI cascade and Langmuir collapse. In CH plasmas, when $T_i/T_e=1/3$, the Landau damping of the slow ion-acoustic wave (IAW) is lower than that in H plasmas. Therefore, the BSRS can be further suppressed through LDI cascade by the way of controlling the species of plasmas and ions ratio. These results give an effective mechanism to suppress the BSRS and hot electrons generation.
385 - Xavier Audier 2019
We revisit laser intensity noise in the context of stimulated Raman scattering (SRS), which has recently proved to be a key technique to provide label free images of chemical bonds in biological and medical samples. Contrary to most microscopy techniques, which detect a weak photon flux resulting from light matter interactions, SRS is a pump-probe scheme that works in the high flux regime and happens as a weak modulation ($10^{-4}-10^{-6}$) in a strong laser field. As a result, laser noise is a key issue in SRS detection. This practical tutorial provides the experimentalists with the tools required to assess the amount of noise and the ultimate SRS detection limit in a conventional lock-in-based SRS system. We first define the quantities that are relevant when discussing intensity noise, and illustrate them through a conventional model of light detection by a photodiode. Stimulated Raman Scattering is then introduced in its lock-in-based implementation, and the model presented is adapted in this particular case. The power spectral density (PSD), relative intensity noise (RIN), signal to noise ratio (SNR), and sensitivity of the system are derived and discussed. Two complementary methods are presented that allow measurement of the RIN and assessment of the performance of a SRS system. Such measurements are illustrated on two commercial laser systems. Finally, the consequences of noise in SRS are discussed, and future developments are suggested. The presentation is made simple enough for under-graduated, graduated students, and newcomers in the field of stimulated Raman, and more generally in pump-probe based schemes.
We propose and theoretically analyze a new vibrational spectroscopy, termed electron- and light-induced stimulated Raman (ELISR) scattering, that combines the high spatial resolution of electron microscopy with the molecular sensitivity of surface-enhanced Raman spectroscopy. With ELISR, electron-beam excitation of plasmonic nanoparticles is utilized as a spectrally-broadband but spatially-confined Stokes beam in the presence of a diffraction-limited pump laser. To characterize this technique, we develop a numerical model and conduct full-field electromagnetic simulations to investigate two distinct nanoparticle geometries, nanorods and nanospheres, coated with a Raman-active material. Our results show the significant ($10^6$-$10^7$) stimulated Raman enhancement that is achieved with dual electron and optical excitation of these nanoparticle geometries. Importantly, the spatial resolution of this vibrational spectroscopy for electron microscopy is solely determined by the nanoparticle geometry and the plasmon mode volume. Our results highlight the promise of ELISR for simultaneous high-resolution electron microscopy with sub-diffraction-limited Raman spectroscopy, complementing advances in superresolution microscopy, correlated light and electron microscopy, and vibrational electron energy loss spectroscopy.
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