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arXiv:2504.15249 · Science Advances

Quantum-enhanced second harmonic generation beyond the photon pairs regime

T. Dickinson, Ivi Afxenti, Giedre Astrauskaite, Lennart Hirsch, Samuel Nerenberg, Ottavia Jedrkiewicz, Daniele Faccio, Marie Caroline Müllenbroich, A. Gatti, Matteo Clerici, Lucia Caspani

Published Jul 4, 2025• 12 citations
arXivHTMLPDF

Abstract

Two-photon processes are crucial in applications like microscopy and microfabrication, but their low cross section requires intense illumination and limits, e.g., the penetration depth in nonlinear microscopy. Entangled states have been proposed to enhance the efficiency of two-photon interactions and have shown effectiveness at low intensities. This quantum enhancement is generally believed to be lost at high intensities, for more than one photon per mode, raising doubts about its usefulness. We explored experimentally and theoretically two-photon processes driven by entangled photons at intensities beyond this threshold and compared the results with the classical case. We found that a quantum advantage can still be observed at nearly one order of magnitude higher intensities than previously assumed. Our findings show a potential path for exploiting quantum-enhanced two-photon processes in practical applications.

DOI
10.1126/sciadv.adw4820

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Two-photon processes are crucial in applications like microscopy and microfabrication, but their low cross section requires intense illumination and limits, e.g., the penetration depth in nonlinear microscopy. Entangled states have been proposed to enhance the efficiency of two-photon interactions and have shown effectiveness at low intensities. This quantum enhancement is generally believed to be lost at high intensities, for more than one photon per mode, raising doubts about its usefulness. We explored experimentally and theoretically two-photon processes driven by entangled photons at intensities beyond this threshold and compared the results with the classical case. We found that a quantum advantage can still be observed at nearly one order of magnitude higher intensities than previously assumed. Our findings show a potential path for exploiting quantum-enhanced two-photon processes in practical applications.
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Quantum entanglement has been shown to imply correlations stronger than those allowed by classical models. The possibility of performing tasks that are classically impossible has made quantum entanglement a powerful resource for the development of novel methods and applications in various fields of research such as quantum computing, quantum cryptography, and quantum metrology. There is a great need for the development of next generation instrumentation and technologies utilizing entangled quantum light. Among the many applications of nonclassical states of light, nonlinear microscopy has the potential to make an impact in broad areas of science from physics to biology. Here, the microscopic image created by the fluorescence selectively excited by the process of the entangled two-photon absorption is reported. Entangled two-photon microscopy offers nonlinear imaging capabilities at an unprecedented low excitation intensity 10 7, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. The nonmonotonic dependence of the image on the femtosecond delay between the components of the entangled photon pair is demonstrated. This delay dependence is a result of specific quantum interference effects associated with the entanglement and this is not observable with classical excitation light. In combination with novel spectroscopic capabilities provided by a nonclassical light excitation, this is of critical importance for sensing and biological applications.