A unified description of sum frequency generation,parametric down conversion and two-photon fluorescence |
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| Authors: | Oleksiy Roslyak Shaul Mukamel |
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| Affiliation: | 1. Chemistry Department , University of California , Irvine, CA 92697-2025, USA oroslyak@uci.edu;3. Chemistry Department , University of California , Irvine, CA 92697-2025, USA |
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| Abstract: | A superoperator non-equilibrium Green's function formalism is presented for computing nonlinear optical processes involving any combination of classical and quantum optical modes. Closed correlation-function expressions based on superoperator time-ordering are derived for the combined effects of causal response and non-causal spontaneous fluctuations. Coherent three wave mixing (sum frequency generation and parametric down conversion) involving one and two quantum optical modes, respectively, are compared with their incoherent counterparts: two-photon-induced fluorescence and two-photon-emitted fluorescence. |
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| Keywords: | ab initio electronic structure quantum chemistry computational chemistry |
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