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arXiv:0907.2208 · Physical Review A

Enhanced two-photon absorption using entangled states and small mode volumes

Hao You, S. M. Hendrickson, J. D. Franson

Published Oct 19, 2009• 20 citations
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Abstract

We calculate the rate of two-photon absorption for frequency-entangled photons in a tapered optical fiber whose diameter is comparable to the wavelength of the light. The confinement of the electric field in the transverse direction increases the intensity associated with a single photon, while the two-photon absorption rate is further enhanced by the fact that the sum of the frequencies of the two photons is on resonance with the upper atomic state, even though each photon has a relatively broad linewidth. As a result, the photons are effectively confined in all three dimensions and the two-photon absorption rate for frequency-entangled photons in a tapered fiber was found to be comparable to that for unentangled photons in a microcavity with a small mode volume.

DOI
10.1103/physreva.80.043823

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Applied Physics Letters•Mar 9, 2026•2 citations
We calculate the rate of two-photon absorption for frequency-entangled photons in a tapered optical fiber whose diameter is comparable to the wavelength of the light. The confinement of the electric field in the transverse direction increases the intensity associated with a single photon, while the two-photon absorption rate is further enhanced by the fact that the sum of the frequencies of the two photons is on resonance with the upper atomic state, even though each photon has a relatively broad linewidth. As a result, the photons are effectively confined in all three dimensions and the two-photon absorption rate for frequency-entangled photons in a tapered fiber was found to be comparable to that for unentangled photons in a microcavity with a small mode volume.
Resonant field enhancement in an optical cavity is a promising pathway towards realizing optical nonlinearities at the few-photon level. This quest is hampered by inevitable narrowing of the resonant linewidth as the cavity finesse is increased, which necessitates striking a compromise between the magnitude of the field enhancement and the bandwidth over which it is harnessed. This difficulty is exacerbated for broadband entangled-photon pairs, which are typically frequency-anticorrelated, so that the two photons cannot be simultaneously admitted to a cavity except when the degenerate wavelength coincides with a cavity resonance. Here we show that introducing judicious angular dispersion into single-photon and entangled-photon states before incidence on a planar Fabry-P{é}rot (FP) cavity renders these non-classical fields omni-resonant: the entire spectrum is coupled to a single longitudinal cavity mode. Making use of a planar FP cavity of finesse ≈100\approx100≈100, resonant linewidth ≈0.3\approx0.3≈0.3~nm, and free spectral range ≈22\approx22≈22~nm in the near-infrared, we couple single-photon states and frequency-anticorrelated entangled-photon states of 20-nm bandwidth to a broadband achromatic resonance associated with a single underlying narrowband longitudinal FP-cavity mode -- thereby preserving the entangled spectral structure. In general, pre-conditioning the optical field by introducing angular dispersion enables coupling non-classical states of light to a single longitudinal cavity mode, even if the field bandwidth far exceeds the resonant linewidth, or even exceeds the cavity free-spectral-range. These results pave the way to broadband resonant interactions with non-classical states of light in photon-starved applications.
Optical technologies based on two-photon absorption can provide high resolution and deep tissue penetration but require very high peak power intensities because of the extremely small absorption cross sections associated with this phenomenon. The use of quantum-entangled photon pairs has been reported to increase the two-photon absorption rate compared with that obtainable using classical coherent laser sources. However, the enhancement that can possibly be obtained using entangled two-photon absorption (ETPA) has thus far been realized only at low photon rates, typically ranging from 107 (on the pW level) to 1013 (on the μW level) photons/s. For this reason, ETPA has been regarded as impractical. The present work demonstrates an experimental evaluation of ETPA-excited fluorescence at both low (μW) and relatively high (mW) pump power levels, using a high-gain parametric down-conversion source. Both an increase in the absorption rate and a linear correlation between rate and power were observed within both power ranges. This work also compared quantum and coherent sources. Assessments of the crossover photon flux suggest that the larger spatial-mode diameter of the present quantum source at the focal point (relative to values used in prior research) may have contributed to the rate enhancement seen at high-power levels. The results presented herein are expected to provide a new route to the mitigation of damage often associated with two-photon imaging and photodynamic therapies.