Hyper-Rayleigh scattering in centrosymmetric systems

Abstract

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 susceptibility (for a molecule, its associated hyperpolarizability). In consequence, HRS is often regarded as formally forbidden in centrosymmetric media. However, for the fundamental three-photon interaction, theory based on the standard electric dipole approximation, representable as E1 3 , does not account for all experimental observations. The relevant results emerge upon extending the theory to include E1 2 M1 and E1 2 E2 contributions, incorporating one magnetic dipolar or electric quadrupolar interaction, respectively, to a consistent level of multipolar expansion. Both additional interactions require the deployment of higher orders in the multipole expansion, with the E1 2 E2 interaction analogous in rank and parity to a four-wave susceptibility. To elicit the correct form of response from fluid or disordered media invites a tensor representation which does not oversimplify the molecular components, yet which can produce results to facilitate the interpretation of experimental observations. The detailed derivation in this work leads to results which are summarized for the following: perpendicular detection of polarization components both parallel and perpendicular to the pump radiation, leading to distinct polarization ratio results, as well as a reversal ratio for forward scattered circular polarizations. The results provide a route to handling data with direct physical interpretation, to enable the more sophisticated design of molecules with sought nonlinear optical properties. C 2015 AIP Publishing LLC. [http://dx

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“…Additionally, it was carefully checked that no signal was detected in absence of the probe pulse, even for the highest fluences used. Such signal could arise from scattered second harmonic radiation generated by the pump pulse (hyper-Rayleigh scattering [32]). Its presence would be obvious for negative delays (when the probe pulse arrives at the surface before the pump pulse).…”

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“…[88]. is accordingly governed by the fewer remaining, incoherent rate terms, in this case associated with the much weaker process known as hyper-Rayleigh scattering [82][83][84][85][86][87].…”

Linear Rayleigh and Raman scattering to the second order: Analytical results for light scattering by any scatterer of size k0d≲1/10

“…Theoretical understanding of light scattering is sufficiently advanced to enable determinations of the nature of interstellar dust [3], radar [4], studies of the structures of viruses [5] and the measurement of the salinity of seawater [6], to name but a few applications. There is much still to be explored, however, and the study of light scattering remains at the cutting edge of research [7][8][9][10][11][12][13][14][15].…”