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J Phys Chem B. 2006 Dec 28;110(51):25582-5.

Entangled photon absorption in an organic porphyrin dendrimer.

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  • 1Department of Chemistry and Applied Physics, University of Michigan, Ann Arbor, Michigan 48109.


Two-photon absorption spectroscopy is an intensity dependent nonlinear effect related to the excitation of virtual intermediate states. The classical two-photon absorption has an extremely low efficiency which is quantified by its cross-section (delta approximately 10(-48) cm4 s at 800 nm). To overcome this limitation, we demonstrate a novel effect of the two-photon absorption method utilizing the high degree of quantum optical correlation between photon pairs created by the process of spontaneous parametric downconversion. A large entangled two-photon absorption cross-section (delta(e) approximately 10(-17) cm2 at 800 nm) was measured in an organic porphyrin dendrimer. We also discuss the nonmonotonic behavior of variation of the entangled two-photon absorption cross-section by controlling the entanglement time. This novel effect may open new avenues for ultrasensitive detection in chemical and biological systems. TPA spectroscopy has been considered as a powerful tool in physics, chemistry, and biology. The inherent nonlinear process of the classical TPA is distinguishable from the single photon absorption (SPA) linear process. Although the benefits of greater penetration depth and better control and reduction of scattering, the TPA spectroscopy has been restricted by the necessity of a high power optical source due to the low efficiency of the TPA effect. The use of entangled photons from a correlated source for the purpose of the two-photon effect is promising in this regard as one may obtain two-photon effects with very small numbers of photons.

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