Mechanisms universally permitting hyper-Rayleigh scattering

Mathew D. Williams; Jack S. Ford; David L. Andrews

doi:10.1117/12.2080809

27 February 2015 Mechanisms universally permitting hyper-Rayleigh scattering

Mathew D. Williams, Jack S. Ford, David L. Andrews

Proceedings Volume 9347, Nonlinear Frequency Generation and Conversion: Materials, Devices, and Applications XIV; 934711 (2015) https://doi.org/10.1117/12.2080809
Event: SPIE LASE, 2015, San Francisco, California, United States

Abstract

Hyper-Rayleigh scattering (HRS) is an incoherent variant of second harmonic generation. The theory involves terms of increasing order of optical nonlinearity: for molecules or unit cells that are centrosymmetric, and which accordingly lack even-order susceptibilities, HRS is often regarded as formally forbidden. However, for the three-photon interaction, theory based on the standard electric dipole approximation, represented as E1³, does not include the detail required to describe what is observed experimentally, in the absence of a static field. New results emerge upon extending the theory to include E1²E2 and E1²M1, incorporating one electric quadrupolar or magnetic dipolar interaction respectively. Both additional interactions require the deployment of higher orders in the multipole expansion to govern these processes, with the E1²E2 interaction analogous in rank and parity to a four-wave susceptibility. A key feature of the present work is its foundation upon a formal tensor derivation which does not oversimplify the molecular components, yet leads to results whose interpretation can be correlated with experimental observations. Results are summarized for the perpendicular detection of both parallel and perpendicular polarizations. Using such methods to investigate molecular systems that might have useful nonlinear characteristics, HRS therefore provides a route to data with direct physical interpretation, to enable more sophisticated design of molecules with sought optical properties.

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Mathew D. Williams, Jack S. Ford, and David L. Andrews "Mechanisms universally permitting hyper-Rayleigh scattering", Proc. SPIE 9347, Nonlinear Frequency Generation and Conversion: Materials, Devices, and Applications XIV, 934711 (27 February 2015); https://doi.org/10.1117/12.2080809

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KEYWORDS

Molecules

Hyper Rayleigh scattering

Absorption

Nonlinear optics

Molecular quantum electrodynamics

Light scattering

Magnetism

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