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A Photonic System for Generating Unconditional Polarization-Entangled Photons Based on Multiple Quantum Interference

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Predicting and Controlling Entangled Two-Photon Absorption in Diatomic Molecules.

Ryan K Burdick¹, Oleg Varnavski¹, Andrew Molina¹

¹Department of Chemistry , University of Michigan , Ann Arbor , Michigan 48109 , United States.

The Journal of Physical Chemistry. A

|September 19, 2018

Summary

Investigating entangled two-photon absorption in diatomic molecules reveals new parameters for controlling molecular excitations. This quantum approach offers enhanced prediction and control over nonlinear optical responses, advancing molecular spectroscopy.

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Area of Science:

Quantum optics
Molecular spectroscopy
Nonlinear optics

Background:

Nonclassical light states offer novel insights into molecular excitations.
Entangled photons can significantly enhance nonlinear optical responses in organic materials.
Understanding state-to-state parameters is crucial for predicting molecular excitations with nonclassical light.

Purpose of the Study:

To investigate state-to-state parameters in entangled two-photon absorption for diatomic molecules.
To provide detailed quantum chemical calculations for predicting molecular excitations.
To enhance the accuracy of nonlinear optical response predictions.

Main Methods:

Theoretical investigation of entangled two-photon absorption processes.
Quantum chemical calculations of energies and transition moments for diatomic molecules.
Derivation of approximations for predicting entanglement-induced transparencies.

Main Results:

Accurate energies and transition moments for intermediate states in diatomic molecules were calculated.
Nonmonotonic behavior of entangled two-photon absorption cross-sections was estimated more accurately.
Approximations were derived to predict entanglement-induced transparencies without exact transition dipole moments.

Conclusions:

Entangled two-photon absorption provides additional parameters compared to classical methods.
These parameters may enable prediction and control of molecular nonlinear absorption and transparency.
This research advances the potential for manipulating molecular optical properties.