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Quantum and Semiclassical Optics Journal of the European Optical Society Part B

Perturbation spectroscopy in superfluorescent emission

S Oullemine, Etienne Boursey

Published Apr 1, 1998• 0 citations
Publisher

Abstract

Enhancement of laser-induced fluorescence can be achieved via superfluorescence which is a collective spontaneous emission correlated to individual molecular states. Our present results with show that intermolecular correlations do not affect intramolecular homogeneous and heterogeneous interactions. Induced superfluorescence can provide a new insight into molecular states.

DOI
10.1088/1355-5111/10/2/010

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Enhancement of laser-induced fluorescence can be achieved via superfluorescence which is a collective spontaneous emission correlated to individual molecular states. Our present results with show that intermolecular correlations do not affect intramolecular homogeneous and heterogeneous interactions. Induced superfluorescence can provide a new insight into molecular states.
We have observed and characterized 501.6 nm collective spontaneous emission (superfluorescence) following 1s(2) → 1s3p excitation of helium atoms by 53.7 nm free-electron laser radiation. Emitted pulse energies of up to 100 nJ are observed, corresponding to a photon number conversion efficiency of up to 10%. We observe the peak intensity to scale as ρ(2) and the emitted pulse width and delay to scale as ρ(-1), where ρ is the atom number density. Emitted pulses as short as 1 ps are observed, which corresponds to a rate around 75,000 times faster than the spontaneous 1s3p → 1s2s decay rate. To our knowledge, this is the first observation of superfluorescence following pumping in the extreme ultraviolet wavelength region, and extension of the technique to the generation of extreme ultraviolet and x-ray superfluorescence pulses should be straightforward by using suitable atomic systems and pump wavelengths.
La superfluorescence est l'un des mecanismes collectifs de l'interaction rayonnement-matiere. Elle designe l'emission spontanee d'une assemblee de molecules ou d'atomes preparee initialement en etat d'inversion. L'emission est proportionnelle a n#2 et a lieu apres un temps de retard qui traduit la mise en phase de tous les moments dipolaires moleculaires ou atomiques. Mon travail s'inscrit dans le cadre de l'etude de la superfluorescence dans la molecule #1#3#0te#2 et de son application a la spectroscopie moleculaire. Il a consiste a modeliser nos resultats experimentaux pour mettre en evidence les divers phenomenes qui interviennent dans ce processus d'emission spontanee coherente : - processus de relaxation transverse et effet doppler. - processus de propagation et reexcitation. - processus de bouclage par retroaction avec une cavite resonante. Nous avons ainsi mis en evidence un nouveau modele qui nous a permis de montrer que les phenomenes d'oscillations coherentes pouvaient etre analysees en tenant compte des phenomenes de reexcitation et stimulation. Par ailleurs nous avons montre que les correlations intermoleculaires n'affectaient pas les perturbations homogenes et heterogenes intramoleculaires. L'analyse des effets spectraux et temporels nous a permis d'acceder a la mesure experimentale des coefficients de melange entre etats en interaction.
We present new results on Te2 superfluorescence induced by short YAG-pumped dye laser pulses analyzed at high resolution by comparison with C.W. laser induced fluorescence observed by Fourier transform spectroscopy. A complete identification of the transitions involved based on intensity measurements and supported by calculated Franck-Condon factors has been achieved. The cooperative emission in Te2 has been studied by time resolved spectroscopy as a function of density. As the density or temperature of the sample is increased, the emission evolves continuously from characteristic spontaneous emission to superfluorescence. The dependence of the superradiant pulse parameters (relaxation time and half-width) with respect to density will be presented and compared to predictions of current theories.