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Nonlinear optical signals and spectroscopy with quantum light


Conventional nonlinear spectroscopy uses classical light to detect matter properties through the variation of its response with frequencies or time delays. Quantum light opens up new avenues for spectroscopy by utilizing parameters of the quantum state of light as novel control knobs and through the variation of photon statistics by coupling to matter. An intuitive diagrammatic approach is presented for calculating ultrafast spectroscopy signals induced by quantum light, focusing on applications involving entangled photons with nonclassical bandwidth properties - known as "time-energy entanglement." Nonlinear optical signals induced by quantized light fields are expressed using time-ordered multipoint correlation functions of superoperators in the joint field plus matter phase space. These are distinct from Glauber's photon counting formalism which uses normally ordered products of ordinary operators in the field space. One notable advantage for spectroscopy applications is that entangled-photon pairs are not subjected to the classical Fourier limitations on the joint temporal and spectral resolution. After a brief survey of properties of entangled-photon pairs relevant to their spectroscopic applications, different optical signals, and photon counting setups are discussed and illustrated for simple multilevel model systems.

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