Multiphoton processes, predicted1 theoretically in 1931, were for a long time considered to be mainly of academic interest. This view changed when it was shown2,3 that a two-photon absorption process could, because of a quadratic dependence of excitation on intensity, produce a spatially confined excitation useful for three-dimensional data storage and imaging. Two-photon absorption has received considerable attention recently because of the development of highly efficient two-photon-sensitive materials, leading to numerous technological applications4,5,6,7,8,9,10,11,12,13,14,15,16,17,18,19,20,21,22,23,24,25,26,27,28. These successes have created interest in exploring applications based on three-photon excitations29. For a three-photon process, a longer excitation wavelength such as those common in optical communications can be used. Also, the cubic dependence of the three-photon process on the input light intensity provides a stronger spatial confinement, so that a higher contrast in imaging can be obtained. Here we report the observation of a highly directional and up-converted stimulated emission as an amplified spontaneous emission, produced in an organic chromophore solution by a strong simultaneous three-photon absorption at 1.3 µm. This achievement suggests opportunities for a three-photon process in frequency-upconversion lasing, short-pulse optical communications, and the emerging field of biophotonics.
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This work was supported by the US Air Force Office of Scientific Research, Washington DC, and the Polymer Branch of the US Air Force Research Laboratory at Dayton.
The authors declare no competing financial interests.
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He, G., Markowicz, P., Lin, TC. et al. Observation of stimulated emission by direct three-photon excitation. Nature 415, 767–770 (2002). https://doi.org/10.1038/415767a
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