TY - JOUR AU - Alexander Mikhaylov AU - Ryan Wilson AU - Kristen Parzuchowski AU - Michael Mazurek AU - Charles Camp AU - Martin Stevens AU - Ralph Jimenez AB - It has been proposed that entangled two-photon absorption (E2PA) can be observed with up to 10^10 lower photon flux than its classical counterpart, therefore enabling ultralow-power two-photon fluorescence microscopy. However, there is a significant controversy regarding the magnitude of this quantum enhancement in excitation efficiency. We investigated the fluorescence signals from Rhodamine 6G and LDS798 excited with a CW laser or an entangled photon pair source at ∼1060 nm. We observed a signal that originates from hot-band absorption (HBA), which is one-photon absorption from thermally populated vibrational levels of the ground electronic state. This mechanism, which has not been previously discussed in the context of E2PA, produces a signal with a linear power dependence, as would be expected for E2PA. For the typical conditions under which E2PA measurements are performed, contributions from the HBA process could lead to a several orders of magnitude overestimate of the quantum advantage. BT - The Journal of Physical Chemistry Letters DA - 2022-02 DO - 10.1021/acs.jpclett.1c03751 IS - 6 M1 - 6 N1 - PMID: 35129354 N2 - It has been proposed that entangled two-photon absorption (E2PA) can be observed with up to 10^10 lower photon flux than its classical counterpart, therefore enabling ultralow-power two-photon fluorescence microscopy. However, there is a significant controversy regarding the magnitude of this quantum enhancement in excitation efficiency. We investigated the fluorescence signals from Rhodamine 6G and LDS798 excited with a CW laser or an entangled photon pair source at ∼1060 nm. We observed a signal that originates from hot-band absorption (HBA), which is one-photon absorption from thermally populated vibrational levels of the ground electronic state. This mechanism, which has not been previously discussed in the context of E2PA, produces a signal with a linear power dependence, as would be expected for E2PA. For the typical conditions under which E2PA measurements are performed, contributions from the HBA process could lead to a several orders of magnitude overestimate of the quantum advantage. PY - 2022 SP - 1489 EP - 1493 T2 - The Journal of Physical Chemistry Letters TI - Hot-Band Absorption Can Mimic Entangled Two-Photon Absorption UR - https://doi.org/10.1021/acs.jpclett.1c03751 VL - 13 ER -