Hyper-Rayleigh scattering in centrosymmetric systems

Hyper-Rayleigh scattering in centrosymmetric systems.

Hyper-Rayleigh scattering (HRS) is an incoherent mechanism for optical second harmonic generation. The frequency-doubled light that emerges from this mechanism is not emitted in a laser-like manner, in the forward direction; it is scattered in all directions. The underlying theory for this effect involves terms that are quadratic in the incident field and involves an even-order optical suscepti...

Hyper-Rayleigh scattering of centrosymmetric molecules in solution

Second-Harmonic Rayleigh Scattering from a Sphere of Centrosymmetric Material

We describe the electromagnetic theory of second-harmonic generation from the surface of a sphere that is small compared to the wavelength of light. In a leading-order expansion, the second-harmonic radiation is emitted in nonlocally excited electric dipole and locally excited electric quadrupole modes. We analyze the problem with particular emphasis on experimental aspects, such as the radiati...

Hyper-Rayleigh scattering spectrum of liquid nitromethane.

The vertical vertical (VV), horizontal vertical (HV), and vertical horizontal (VH) hyper-Rayleigh scattering (HRS) spectra were measured for liquid CH3NO2 at T= 300 K. The main HRS spectral component has a width upsilon1=1.28 +/- 0.04 cm(-1), which gives an orientation relaxation time pi=4.1 +/- 0.1 ps in good agreement with other experiments. However, the VH spectrum also contains a previously...

Spectral measurements of hyper-Rayleigh light scattering

An apparatus is described for the measurement of second-order nonlinear optical properties via hyper-Rayleigh scattering with 1 cm spectral resolution of the scattered light. The setup allows a complete investigation of the polarization dependence of the second-harmonic scattered light. The combination of good spectral resolution, polarization analysis, and high sensitivity allows the determina...