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Journal of Applied Spectroscopy

Effect of spatial and temporal structure of emission on two-photon absorption

Е. С. Воропай, A. M. Sarzhevskii, P. A. Torpachev

Published Sep 1, 1981• 0 citations
Publisher
DOI
10.1007/bf00615806

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Observations of a frequency-shifted coherent conical emission from systems pumped by an intense optical field that is nearly resonant with a one-photon transition1 have made it clear that propagation effects can play a major role in determining the spectrum as well as the spatial characteristics of the transmitted pulse. Proposed theories of conical emission stress the importance of transverse effects leading to four-wave mixing1 or spatial self-phase modulation.2 We report computer results on laser propagation in a two-level system and demonstrate that spatial structure, including conical emission, can result from temporal propagation effects.
Entangled photons generated by spontaneous parametric down-conversion (SPDC) have been used to investigate entangled two-photon absorption (ETPA) in multiannulene systems. The ETPA characteristics are shown to depend on the spatial orientation of the SPDC emission pattern. The expected dependence of the absorption rate on input flux is seen for emission patterns that exhibit spatial indistinguishability between the signal and idler photons, while no absorption is observed for a spatially distinguishable emission pattern. The amount of absorption of entangled photons is also seen to depend on the degree of overlap of the entangled photons for the indistinguishable conditions. Tunability of the entangled photon absorption can thus be achieved by utilizing the spatial characteristics of the entangled photon pairs.