Sum-frequency generation at molecule-nanostructure interfaces from diagrammatic theory of nonlinear optics

Article

关键词: GOLD NANOPARTICLES;    SURFACE;    LAYERS;    TIME;    SPECTROSCOPY;    ORIENTATION;    DIPOLAR;   

DOI  :  10.1103/PhysRevB.105.205420

来源: SCIE

【 摘 要 】

We apply the loop diagrammatic method for linear and nonlinear optics to the calculation of the sumfrequency response of a molecule-nanostructure composite system. The presence of the nanostructure modifies the molecular response through dipolar energy exchange, and the molecular hyperpolarizability is factorized by nanostructure response functions of increasing orders. We provide a general method to transform these functions into products of first-order nanostructure polarizabilities, accounting for enhancements of the molecular response by coupling to plasmonic or excitonic resonances. In particular, we show how the diagrams may be directly read to determine the response functions and their factorization without explicit calculation. The methodology provides a frame for various applications to other systems, interactions, and nonlinear optical processes.

【 授权许可】

Free