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Frequency-upconverted stimulated emission by simultaneous five-photon absorption

Abstract

Since the invention of the laser in 1960, multiphoton effects have become useful in techniques for real applications as well as conceptual predictions. Here, we report the first experimental observation of frequency-upconverted stimulated emission from a novel fluorophore through simultaneous five-photon absorption. Compared to lower-order nonlinear absorption, the fifth-order dependence on input light intensity of the five-photon absorption process will provide much stronger spatial confinement, allowing the achievement of a much higher contrast in imaging. Stimulated emission has also been achieved by the absorption of two to four photons under near-infrared laser excitation, making this gain medium a promising multiphoton imaging probe with attractive features, including the absence of autofluorescence from biological samples, large penetration depth, and improved sensitivity and resolution.

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Figure 1: Absorption, transmission and emission.
Figure 2: Emission spectra, energy diagrams and photographs.
Figure 3: Output/input power characteristics and far-field distributions of 3PP pumped stimulated emission.
Figure 4: Output/input power characteristics and far-field distributions of 5PP stimulated emission.

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Acknowledgements

This work was supported by National Science Foundation of China (21102144, 51173186) and the 100 Talents Programme of the Chinese Academy of Sciences. X.C. and H.Z. acknowledge financial support from the Knowledge Innovation Program of CAS for Key Topics (no. KJCX2-YW-358) and the 863 Program of MOST (no. 2011AA03A407).

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Contributions

Q.Z. conceived the experiments. Q.Z. and H.Z. were primarily responsible for the experiments. H.Z., E.M., X.C. and Q.Z. carried out stimulated emission experiments and the time-decay measurements. S.C. and C.T. carried out linear optical property measurements and characterizations of the multiphoton absorbing material. All authors discussed the results and the manuscript.

Corresponding authors

Correspondence to Qingdong Zheng or Xueyuan Chen.

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The authors declare no competing financial interests.

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Zheng, Q., Zhu, H., Chen, SC. et al. Frequency-upconverted stimulated emission by simultaneous five-photon absorption. Nature Photon 7, 234–239 (2013). https://doi.org/10.1038/nphoton.2012.344

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