An entangled state is represented by a wavefunction which cannot be factored into separate states. For photons, these quantum correlations lead to non-classical light-matter interactions, potentially creating new opportunities for spectroscopic techniques. For example, second-order processes with two entangled photons, such as two-photon absorption or sum frequency generation, occur at a linear rate with a cross section that should be close to that of one-photon classical processes. However, early results in the field have produced conflicting measurements about the entangled enhancement. In this talk, I will describe our measurements of entangled two photon absorption by virtual and real-state mediated processes. A custom spectrometer with a 10 femtosecond, high-flux entangled photon source is used to measure the entangled photon state before, during, and after the interaction. By temporally and spectrally characterizing the entangled photon interaction with the test molecule, one and two photon processes are easily discriminated.

Characterization of the entangled photon state before, during, and after a two-photon absorption event

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ACS Fall 2022

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