Quantum channels in nonlinear optical processes

Quantum electrodynamics furnishes a new type of representation for the characterisation of nonlinear optical processes. The treatment elicits the detailed role and interplay of specific quantum channels, information that is not afforded by other methods. Following an illustrative application to the case of Rayleigh scattering, the method is applied to second and third harmonic generation. Derivations are given of parameters that quantify the various quantum channels and their interferences; the results are illustrated graphically. With given examples, it is shown in some systems that optical nonlinearity owes its origin to an isolated channel, or a small group of channels. © 2009 World Scientific Publishing Company

On the interactions between molecules in an off-resonant laser beam:Evaluating the response to energy migration and optically induced pair forces

Electronically excited molecules interact with their neighbors differently from their ground-state counterparts. Any migration of the excitation between molecules can modify intermolecular forces, reflecting changes to a local potential energy landscape. It emerges that throughput off-resonant radiation can also produce significant additional effects. The context for the present analysis of the mechanisms is a range of chemical and physical processes that fundamentally depend on intermolecular interactions resulting from second and fourth-order electric-dipole couplings. The most familiar are static dipole-dipole interactions, resonance energy transfer (both second-order interactions), and dispersion forces (fourth order). For neighboring molecules subjected to off-resonant light, additional forms of intermolecular interaction arise in the fourth order, including radiation-induced energy transfer and optical binding. Here, in a quantum electrodynamical formulation, these phenomena are cast in a unified description that establishes their inter-relationship and connectivity at a fundamental level. Theory is then developed for systems in which the interplay of these forms of interaction can be readily identified and analyzed in terms of dynamical behavior. The results are potentially significant in Förster measurements of conformational change and in the operation of microelectromechanical and nanoelectromechanical devices. © 2009 American Institute of Physics

A photonic basis for deriving nonlinear optical response

Nonlinear optics is generally first presented as an extension of conventional optics. Typically the subject is introduced with reference to a classical oscillatory electric polarization, accommodating correction terms that become significant at high intensities. The material parameters that quantify the extent of the nonlinear response are cast as coefficients in a power series - nonlinear optical susceptibilities signifying a propensity to generate optical harmonics, for example. Taking the subject to a deeper level requires a more detailed knowledge of the structure and properties of each nonlinear susceptibility tensor, the latter differing in form according to the process under investigation. Typically, the derivations involve intricate development based on time-dependent perturbation theory, assisted by recourse to a set of Feynman diagrams. This paper presents a more direct route to the required results, based on photonic rather than semiclassical principles, and offers a significantly clearer perspective on the photophysics underlying nonlinear optical response. The method, here illustrated by specific application to harmonic generation and down-conversion processes, is simple, intuitive and readily amenable for processes of arbitrary photonic order. © 2009 IOP Publishing Ltd