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Applied Physics Letters

Generation of single-picosecond dye laser pulses using one- and two-photon traveling-wave excitation

Anatoly N. Rubinov, Martin C. Richardson, Kenneth L. Sala, A. J. Alcock

Published Sep 15, 1975• 37 citations
Publisher

Abstract

Single-photon and two-photon traveling-wave excitation of superradiant emission in Rhodamine 6G by single-picosecond 1.06-μ laser pulses is reported. In addition, results are presented on the application of optical Kerr-effect photography to a time-resolved spectroscopic study of the dye laser emission.
DOI
10.1063/1.88476

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An image-converter streak camera with picosecond time resolution was used in a study of the kinetics of formation of pulses in a traveling-wave laser in which molecular dye solutions were subjected to two-photon optical pumping. An analytic expression was obtained for the lasing threshold of a nonresonator traveling-wave laser in the case of pulsed (τp τe) and quasicontinuous (τp > τe) pumping. Satisfactory agreement was obtained between the calculated and experimental lasing threshold. The kinetics of the compression of output pulses, determined as a function of the pump radiation intensity, was described by rate equations. At pumping rates up to 10 times the threshold a qualitative agreement between the experimental and calculated results was obtained employing a two-band energy model of the dye with a short (compared with the duration of the pump pulses τp) vibrational relaxation time τe. At rates of excitation well above the threshold the kinetics of compression and delay changed, and the output pulses were split into two components, which was interpreted (in the specific case of rhodamine 6G) using a four-band energy scheme. A practical conclusion of this investigation was in the form of recommendations on the use of the proposed approach as a simple method for generating high-intensity single picosecond superradiance pulses of duration τsr with frequency up-con version and a compression coefficient τp/τsr ~ 10.
Synchronous mode locking of two dye lasers was employed to obtain pairs of independently tunable picosecond pulses that were precisely synchronized in time. Overlapped pulses in strontium vapor were used to generate tunable picosecond pulses in the vacuum uv. The tunability was employed to study resonant enhancement of a four-wave parametric process by the 4d6p autoionizing resonance. Mutually separated pulses were employed to measure the build-up and decay of coherence for a two-quantum excited state. The decay was found to be faster than theoretical predictions that assume only velocity dephasing.
A technique is described for performing nanosecond time-resolved spectroscopy for situations of extremely low emission rates. The system utilizes a N(2) laser pumped tunable dye laser and single photon time correlation techniques. It is applicable where there is need for nanosecond time resolution on emission which is either long-lived or has extremely low quantum efficiency and especially where monochromatic excitation is required. The technique is applied to the relaxation between a pair of excited states of Tb(3+):Y(OH):(3), where 5-nsec temporal resolution with 2- cm(-1) spectral resolution is easily obtained.
Wavelength dependent study of a laser dye: Rhodamine-6G (Rh6G) by using spectrally resolved photon-echo spectroscopy is presented. The coherence and population dynamics of Rh6G solution in methanol changes as the excitation wavelength is tuned near its absorption maxima of 528 nm. Specifically, the central wavelength of the femtosecond laser pulse was set to 535 nm and to 560 nm while the respective spectra of the photon-echo signals were collected. This gives information on how the ultrafast dynamics of the Rh6G molecule changes with a change in the excitation wavelength.
I. A new technique utilizing the electro-optic frequency switching of a single mode ( 6 Mhz) dye laser was used to observe free induction decay and optical nutation in iodine gas and optical nutation in an organic mixed crystal (pentacene in p-terphenyl) at low temperature. A new technique, incoherent resonance decay (IRO) was also developed. These experiments allow one to determine T_1 and T_2, the longitudinal and transverse relaxation times of the excited ensemble, in analogy with magnetic resonance. For I_2(g) at O∙C; T_l = 2.3 x 10^(-7) sec, T_2 ≃ 1 x 10^(-7) sec. These techniques are limited to a time scale > 10 nsec. II. The construction and characterization of cw, mode-locked dye laser capable of putting out a continuous train of reproducible sub-picosecond pulses is described. Experiments utilizing this laser for the measurement of picosecond coherent transients and time resolved absorption spectroscopy are proposed.
In two recent works, the authors have investigated the spectro-temporal properties of the random laser emission from solid state dye-doped powders in picosecond pumping regime. Each emission pulse consists, both above and below threshold, in a collection of narrow peaks of a spectro-temporal width at the theoretical limit (ΔωΔt≅1). The distribution of path lengths traveled inside the diffusive active medium by photons that can be amplified by stimulated emission explains this behavior, as demonstrated by a simple theoretical model developed by the authors. The aim of the present work is, first, to develop an implemented model that does not depend on fitting parameters, and which is compatible with the energetic and spectro-temporal properties of the material; and second, to get knowledge about the spatial properties of the emission. The transverse coherence size of each emitted photon packet has been measured; and in addition, we have shown the existence of spatial fluctuations of the emission of these materials, as our model predicts.