Diagrammatic Theory of Linear and Non-Linear Optics for Composite Systems
Résumé
We present a general formalism to model and calculate linear and nonlinear optical processes in composite systems,
based on a graphical representation of light-matter interactions by loop diagrams associated with Feynman
rules. Through this formalism, we recover the usual second-order response of a simple system by drawing four
times fewer loop diagrams than doubled-sided ones. For composite systems, we introduce coupling Hamiltonians
between subsystems (for example, a molecule and a substrate), graphically represented by virtual bosons. In this
way, we enumerate all the diagrams describing the second-order response of the system and show how to select
those relevant for the calculation of the molecular second-order hyperpolarizabilities under the influence of the
substrate, including effective second-order contributions from the molecular third-order response. As it applies
to all nonlinear processes and an arbitrary number of interacting partners, this representation provides a general
frame for the calculation of the nonlinear response of arbitrarily complex systems.
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