Two-Dimensional Electronic Spectroscopy with Intense Entangled-Photon Beams

Entangled photons carry nontrivial quantum correlations that defy classical physics and provide new tools for monitoring quantum dynamics in molecules. The use of low-flux entangled photons in molecular spectroscopy has been proposed in the past to probe excited-state dynamics with enhanced temporal and spectral resolutions. However, these techniques have been challenging to implement experimentally since the resulting signal has a low signal-to-noise ratio. The signal strength can be boosted by using intense entangled-photon beams, where multiple pairs of entangled photons are present in the environment. This allows the molecule under study to interact with both entangled and unentangled photons, where the classical component of the spectroscopic signal stemming from the latter can mask the spectral features associated with the former. In this Letter, we show how the signal arising from unentangled photons can be eliminated when intense entangled-photon beams are used in two-dimensional electronic spectroscopy (2DES), and demonstrate the advantage of photonic entanglement.