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Experimental and theoretical investigation of third-harmonic generation in phase-matched dye solutions

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Abstract

The phase-matched third-harmonic light generation in dye solutions is studied experimentally and theoretically. In the experiments picosecond light pulses of a passive mode-locked Nd-glass laser are converted to the third-harmonic frequency. A third-harmonic conversion efficiency of up to 4×10−4 was achieved for one of the dyes investigated (1,3,3,1′,3′,3′-hexamethylindocarbocyanine iodide in hexafluoroisopropanol). The theoretical calculations determine the influence of various dye and solvent parameters on the conversion efficiency. The conversion efficiency is found to be limited by excited-state absorption of pump laser light and third-harmonic light from the S1-state to higher singlet states. The S1-state is mainly populated by two-photon absorption. Amplified spontaneous emission may reduce the limiting effects of excited-state absorption. Phase changes caused by the non-linear refractive index and the refractive index dispersion within the spectral bandwidth of the laser pulses reduce the conversion efficiency. Under ideal conditions conversion efficiencies up to 10% may be achieved.

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Authors and Affiliations

  1. Naturwissenschaftliche Fakultät II — Physik, Universität Regensburg, D-8400, Regensburg, Germany

    A. Penzkofer & W. Leupacher

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  1. A. Penzkofer
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  2. W. Leupacher
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Penzkofer, A., Leupacher, W. Experimental and theoretical investigation of third-harmonic generation in phase-matched dye solutions. Opt Quant Electron 20, 227–256 (1988). https://doi.org/10.1007/BF02029897

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