ABSTRACT
Ultrafast Raman loss spectroscopy (URLS) is equivalent to anti-Stokes femtosecond stimulated Raman spectroscopy (FSRS), using a broadband probe pulse that extends to the blue of the narrow bandwidth Raman pump, and can be described as inverse Raman scattering (IRS). Using the Feynman dual time-line diagram, the third-order polarization for IRS with finite pulses can be written down in terms of a four-time correlation function. An analytic expression is obtained for the latter in the harmonic approximation which facilitates computation. We simulated the URLS of crystal violet (CV) for various resonance Raman pump excitation wavelengths using the IRS polarization expression with finite pulses. The calculated results agreed well with the experimental results of S. Umapathy et al., J. Chem. Phys. 133, 024505 (2010). In the limit of monochromatic Raman pump and probe pulses, we obtain the third-order susceptibility for multi-modes, and for a single mode we recover the well-known expression for the third-order susceptibility, χ(IRS) ((3)), for IRS. The latter is used to understand the mode dependent phase changes as a function of Raman pump excitation in the URLS of CV.
ABSTRACT
Three kinds of soluble polymer grafted multi-walled carbon nanotubes (MWNTs), including poly(N-vinylcarbazole)-MWNTs (MWNTs-PVK), polystyrene-MWNTs (MWNTs-PSt) and poly(methyl methacrylate)-MWNTs (MWNTs-PMMA) were synthesized. The TEM images of these samples show that polymers are coated outside the carbon nanotubes. The UV-Vis absorption spectra of the samples in CHCl3 were taken on a HP8452 spectrophotometer at room temperature. Compared with that of MWNTs suspension, there is a characteristic absorption peak in the ultraviolet region, which can be attributed to the polymers linked covalently with MWNTs. Their nonlinear optical properties and optical limiting (OL) performances were investigated by Z-scan method with 527 nm nanosecond laser pulses. These MWNTs dissolved in chloroform possess similar optical limiting properties, which are better than that of raw MWNT suspension and C60 in toluene solution. Nonlinear refraction, nonlinear absorption and nonlinear scattering mechanism were taken into consideration for explaining the observed results. The analysis of the experimental results shows that nonlinear absorption is the dominant mechanism behind the OL performance of these samples.
