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Updated: Jul 1, 2025

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This study reveals that linear optical losses can corrupt entangled two-photon absorption (ETPA) signals in transmission experiments. A novel approach using a Hong-Ou-Mandel interferogram effectively detects these losses, showing ETPA was not unequivocally detected under common experimental conditions.

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Area of Science:

  • Quantum optics
  • Nonlinear optics
  • Spectroscopy

Background:

  • Entangled two-photon absorption (ETPA) is an elusive quantum phenomenon studied in nonlinear materials.
  • Transmission-based ETPA experiments are prone to artifacts from linear optical losses, casting doubt on reported results.
  • Existing methods struggle to differentiate true ETPA signals from artifacts caused by optical losses.

Purpose of the Study:

  • To investigate the impact of linear optical losses on ETPA detection.
  • To introduce and validate a novel approach using Hong-Ou-Mandel (HOM) interferometry for ETPA studies.
  • To demonstrate the ability of HOM interferograms to detect linear losses and their effect on ETPA signals.

Main Methods:

  • Utilized rhodamine B solutions as a model nonlinear medium.
  • Employed a Hong-Ou-Mandel interferometer as a sensing device to analyze ETPA.
  • Introduced controlled linear losses using silica nanoparticles and varied solvent properties to study their effects.

Main Results:

  • Demonstrated the equivalence between standard transmission-based ETPA experiments and the HOM interferogram approach (transmission vs. two-photon temporal delay).
  • Quantified the detrimental effects of unrelated optical losses on ETPA signals in transmission experiments.
  • Showcased the HOM interferogram's capability to identify the presence of linear optical losses.

Conclusions:

  • Linear optical losses significantly compromise the accuracy of transmission-based ETPA experiments.
  • Hong-Ou-Mandel interferometry offers a robust method for detecting linear losses in such experiments.
  • Under the experimental conditions mimicking many published works, entangled two-photon absorption was not unequivocally detected, highlighting the need for improved detection methodologies.