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Entangled two-photon absorption by atoms and molecules: A quantum optics tutorial.

Michael G Raymer1, Tiemo Landes1, Andrew H Marcus2

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This study explores quantum-enhanced molecular spectroscopy using entangled photon pairs for two-photon absorption (TPA). It details how quantum light influences TPA rates, offering potential for enhanced molecular analysis.

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Area of Science:

  • Quantum optics
  • Molecular spectroscopy
  • Nonlinear optics

Background:

  • Two-photon absorption (TPA) and nonlinear molecular interactions with entangled photons show promise for quantum-enhanced spectroscopy.
  • Understanding the quantum nature of light is crucial for these applications.

Purpose of the Study:

  • To theoretically investigate one- and two-photon absorption by molecules using quantum light.
  • To analyze how quantum states of light affect molecular optical response.
  • To quantify the enhancement of TPA rates using entangled photon pairs.

Main Methods:

  • Review of basic quantum optics theory.
  • Density-matrix (Liouville) derivation of molecular optical response.
  • Detailed treatment of TPA using photon pairs from spontaneous parametric down-conversion.

Main Results:

  • Quantum light TPA differs significantly from classical light TPA.
  • Entangled states can enhance TPA rates, with specific quantification provided.
  • Comparison of TPA via far-off-resonant and dephasing-assisted off-resonant intermediate states.

Conclusions:

  • Theoretical framework established for quantum-enhanced TPA.
  • Demonstrated potential for significant TPA rate enhancement using entangled photons.
  • Identified challenges for experimental realization of entangled two-photon absorption.