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Nonlinear spectroscopy with quantum entangled photons is an emerging field ofresearch that holds the promise to achieve a superior signal-to-noise ratio andeffectively isolate many-body interactions. Photon sources used for thispurpose however lack the frequency tunability and spectral bandwidth demandedby contemporary molecular materials. Here, we present design strategies forefficient spontaneous parametric downconversion to generate biphoton stateswith adequate spectral bandwidth and at visible wavelengths. Importantly, wedemonstrate, by suitable design of the nonlinear optical interaction, the scopeto engineer the degree of spectral correlations between the photons of thepair. We also present an experimental methodology to effectively characterizesuch spectral correlations. Importantly, we believe that such acharacterization tool can be effectively adapted as a spectroscopy platform tooptically probe system-bath interactions in materials.

Measurement principles for quantum spectroscopy of molecular materials with entangled photons