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We present a theoretical approach to optical spectroscopy of opennonequilibrium systems, which generalizes traditional nonlinear opticalspectroscopy tools by imposing charge and energy conservation at all levels ofapproximation. Both molecular and radiation field degrees of freedom aretreated quantum mechanically. The formulation is based on the nonequilibriumGreen's function (NEGF) approach and a double sided Feynman diagrammaticrepresentation of the photon flux is developed. Numerical simulations arepresented for a model system. Our study bridges the theoretical approaches ofquantum transport and optical spectroscopy and establishes a firm basis forapplying traditional tools of nonlinear optical spectroscopy in molecularoptoelectronics.

Flux-conserving diagrammatic formulation of optical spectroscopy of open quantum systems