The use of nonclassical states of light to probe organic molecules has received great attention due to the possibility of providing new and detailed information regarding molecular excitations, as well as enhancing nonlinear optical responses through virtual electronic state interactions. In order to predict molecular excitations with nonclassical light, we investigated the details of the state-to-state parameters important in calculating the contribution of particular transitions involved in the entangled two-photon absorption process for diatomic molecules. Using quantum chemical calculations of energy levels and transition dipole moments, we estimated in a highly accurate manner the nonmonotonic behavior of the entangled two-photon absorption cross-section. Modeling of this nonmonotonic behavior may allow us to predict and control the nonlinear absorption of a molecule. Using parameters unique to entangled two-photon absorption (in comparison to classical two-photon absorption), we can selectively enhance a molecule’s nonlinear absorption or make the molecule transparent without changing the incident light’s frequency.

Predicting and controlling entangled two-photon absorption in diatomic molecules

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.