QuaNtum-Enhanced Second Harmonic Generation beyond the Photon Pairs Regime

Long ago, it was predicted that stimulating two-photon processes such as two-photon absorption (TPA) and second harmonic generation (SHG) with entangled photons produced by parametric down-conversion (PDC) could result in higher efficiencies compared to classical illumination [1]. This was experimentally demonstrated for SHG [2] and TPA [3], where, however, the classical comparison was performed by adding losses to the PDC state rather than employing a true classical reference. In addition, these results considered spatially single-mode PDC radiation and were conducted at low photon fluxes, where the PDC modes are, on average, populated by less than one photon. This resulted in an extremely low SHG/TPA signal, considered of limited practical use for metrological applications (such as two-photon fluorescence microscopy or SHG imaging - see, e.g., [4]). A recent theoretical investigation [5] highlighted that a proper analysis of quantum-enhanced two-photon processes requires a fully spatiotemporal model of the nonlinear interactions. It further showed that highly multimode (in space and time) entangled PDC photons can provide a quantum advantage compared to an equivalent classical pulse, even in regimes well beyond the “one-photon-per-mode” limit, considered the boundary of quantum behavior.