Experimental Upper Bounds for Resonance-Enhanced Entangled Two-Photon Absorption Cross Section of Indocyanine Green

• URL: http://arxiv.org/abs/2312.14382v1
• Date: Fri, 22 Dec 2023 02:15:22 GMT
• Title: Experimental Upper Bounds for Resonance-Enhanced Entangled Two-Photon Absorption Cross Section of Indocyanine Green
• Authors: Manni He, Bryce P. Hickam, Nathan Harper, Scott K. Cushing
• Abstract summary: Resonant intermediate states have been proposed to increase the efficiency of entangled two-photon absorption (ETPA) We investigate for the first time r-ETPA in an organic molecular dye, indocyanine green (ICG), when excited by broadband entangled photons in near-IR.
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• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Resonant intermediate states have been proposed to increase the efficiency of entangled two-photon absorption (ETPA). Although resonance-enhanced ETPA (r-ETPA) has been demonstrated in atomic systems using bright squeezed vacuum, it has not been studied in organic molecules. We investigate for the first time r-ETPA in an organic molecular dye, indocyanine green (ICG), when excited by broadband entangled photons in near-IR. Similar to many reported virtual state mediated ETPA (v-ETPA) measurements, no r-ETPA signals are measured, with an experimental upper bound for the cross section placed at $6 \times 10^{-23}$ cm$^2$/molecule. In addition, the classical resonance-enhanced two-photon absorption (r-TPA) cross section of ICG at 800 nm is measured for the first time to be $20(\pm13)$ GM, suggesting that having a resonant intermediate state does not significantly enhance two-photon processes in ICG. The spectrotemporally resolved emission signatures of ICG excited by entangled photons are also presented to support this conclusion.

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