In the last few years, the use of quantum states of light, such as entangled photons, generated through parametric down-conversion, has made significant progress in microscopy, imaging, and quantum computing. Non-linear optical processes employing entangled photons has increased among physical chemists since the first experimental reports of entangled two-photon absorption (ETPA) in atoms and organic molecules. ETPA provides several advantages: certain electronic states that are not easily accessible with classical light but may be excited with entangled photons at extremely low input photon flux; some electronic states in molecules that are hidden to classical light can be excited and probed by entangled photons offering new control over excited state populations and photochemical processes. In addition, the use of these nonclassical states of light in spectroscopy has given rise to the opportunity to provide new information about molecular excitations and transitions within organic molecules. This work primarily focuses on measuring the classical two-photon absorption cross-sections using a mode-locked Ti: Sapphire laser and the entangled two-photon absorption cross-sections using CW-pumped noncollinear Type-I degenerate spontaneous parametric down-conversion (SPDC) of cis and trans diblock Poly (p-phenylene vinylene) (PPV) molecules, a class of conjugated polymer, and how these cis-trans isomers impact the observed results.

Entangled two-photon absorption of diblock PPV molecules

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