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Applied Optics

Optical dephasing in saturable-absorbing organic dye IR140

Carl M. Liebig, William M. Dennis

Published Mar 20, 2006• 13 citations
Publisher

Abstract

Room-temperature degenerate four-wave mixing in the forward two-pulse geometry, has been performed on ajet of organic saturable-absorbing laser dye IR140 dissolved in dimethylsulfoxide and ethylene glycol. Numerical solutions to the optical Bloch equation were fitted to the experimental data in order to extract a value of T2 = 50 +/- 5 fs for the homogeneous dephasing time; this value is comparable to those measured for similar organic dyes using other techniques.

DOI
10.1364/ao.45.002072

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Room-temperature degenerate four-wave mixing in the forward two-pulse geometry, has been performed on ajet of organic saturable-absorbing laser dye IR140 dissolved in dimethylsulfoxide and ethylene glycol. Numerical solutions to the optical Bloch equation were fitted to the experimental data in order to extract a value of T2 = 50 +/- 5 fs for the homogeneous dephasing time; this value is comparable to those measured for similar organic dyes using other techniques.
Intracavity measurements of degenerate four-wave mixing have been performed with femtosecond laser pulses to determine the phase relaxation time of the absorbing dye, diethyloxadicarbocyanine iodide (DODCI), in ethylene glycol. The influence of various broadening mechanisms (homogeneous, inhomogeneous, cross relaxation) and pulse parameters (frequency, pulse shape, phase modulation, and energy) is investigated. The dependence of the signal energy on probe delay is found to be strongly affected by the phase modulation of the pulse; hence determination of the phase relaxation time requires accurate diagnostics of the laser source. The rise of the signal provides an upper limit of 10 fsec for the phase relaxation time of the main absorption band of the dye DODCI. The decay of the signal is found to be related to the phase relaxation time of a two-photon absorption in the same dye. Accurate fitting of the data with the theory yields 50 ± 10 fsec for the dephasing time of the two-photon excitation in DODCI.
This dissertation presents experimental and theoretical studies of transient degenerate four wave mixing (DFWM) in organic dyes. Chapter 1 is an introduction to DFWM. Chapter 2 describes DFWM experiments that were performed in the gain medium of a dye laser. Chapter 3 presents the theory of DFWM of short pulses in three level saturable media. Chapter 4 presents DFWM experiments of femtosecond pulses in the saturable absorber of a passively modelocked ring dye laser. Chapter 5 presents the theory of DFWM of ultrashort pulses in resonant media.
Phase conjugation of backward-and forward-wave produced by degenerate four-wave mixing using a nearly resonantly enhanced nonlinearity in four-level organic dye solutions was investigated. The conversion efficiency of 22% has been obtained in a 2.5×10-5-molar solution of chlorophyll A in methylalcohol with a 5mm interaction length and a pumping energy of ～8mj from SH of a Q-switched Nd:YAG. Degenerate four-wave mixing by two-photon resonant-enhancement in the solution of rhodamine 6G in alcohol was investigated. Measurements were performed which described the dependance of nonlinear reflectivities on the molar concentrations of the media and the intensities of the pumping and object waves. Phase conjugation characteristics of forward-wave in four-wave mixing process were theoretically analysed. Experiments have confirmed the theoretical prediction. The method of quartet degenerate four-wave mixing has been extended to the doublet degenerate casa. Using this method, image conversion from 1.06μm to 5320 A has been realized with a conversion efficiency of 25% in a 5 mm long saturable absorber made of organic dye 9740 solution in diehloroethane. Theoretical analysis shows that using a medium, which is a near resonant absorber for the infrared object wave but transparent for the visible reconstruction wave, the conversion efficiency may be well in excess of unity.
Phase conjugation of backward-and forward-wave produced by degenerate four-wave mixing using a nearly resonantly enhanced nonlinearity in four-level organic dye solutions was investigated. The conversion efficiency of 22% had been obtained in a 2.5 X 10-5 - molar solution of Chlorophyll A in methylalcohol with a 5 mm interaction length and a pumping energy of ～ 8 mJ from SH of a Q-switched Nd: YAG. Degene-rate four-wave mixing by two-photon resonant-enhancement in the solution of rhodamine 6G in alcohol was studied. Measurements were performed which described the dependence of nonlinear reflectivities on the molar concentrations of the media and the intensities of the pumping and object waves. Phase conjugation characteristics of forward-wave in four-wave mixing process were theoretically analysed. Experiments have cofirmed the theoretical prediction. The method of quartet degenerate four-wave mixing had been ex-tended to the doublet degenerate case. Using this method image conversion from 1.06 μm to 5320 ? had been realized with a conversion efficiency of 25% in a 5 mm long satu-rable absorber made of organic dye 9740 solution in dichloroethane. Theoretical analy-sis showed that using a medium, which is a near resonant absorber for the infrared object wave but is transparent for the visible reconstruction wave, the conversion efficiency may be well in excess of unity.
The saturable absorber dye jet of a femtosecond ring dye laser provides an ideal candidate for the study of fast transients in de- generate four-wave mixing (DFWM). Since the counterpropagating pulses in the ring laser meet at the absorber jet, the problem of timing the DFWM pump pulses is solved. The energy of the pulses inside the cavity is such that the absorber is saturated. This meets one of the conditions for efficient DFWM in saturable media.1 Since the dye jet is thin, fast transients in DFWM are not masked by propagation effects.
Phase conjugation of backward-and forward-wave produced by degenerate four-wave mixing using a nearly resonantly enhanced nonlinearity in four-level organic dye solutions was investigated. The conversion efficiency of 22% had been obtained in a 2.5 X 10-5 - molar solution of Chlorophyll A in methylalcohol with a 5 mm interaction length and a pumping energy of ～ 8 mJ from SH of a Q-switched Nd: YAG. Degene-rate four-wave mixing by two-photon resonant-enhancement in the solution of rhodamine 6G in alcohol was studied. Measurements were performed which described the dependence of nonlinear reflectivities on the molar concentrations of the media and the intensities of the pumping and object waves. Phase conjugation characteristics of forward-wave in four-wave mixing process were theoretically analysed. Experiments have cofirmed the theoretical prediction. The method of quartet degenerate four-wave mixing had been ex-tended to the doublet degenerate case. Using this method image conversion from 1.06 μm to 5320 ? had been realized with a conversion efficiency of 25% in a 5 mm long satu-rable absorber made of organic dye 9740 solution in dichloroethane. Theoretical analy-sis showed that using a medium, which is a near resonant absorber for the infrared object wave but is transparent for the visible reconstruction wave, the conversion efficiency may be well in excess of unity.