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Annual Meeting Optical Society of America

Transition from superfluorescence to amplified spontaneous emission in KCI : O 2 −

Michelle S. Malcuit, Jeffery J. Maki, Robert W. Boyd, David J. Simkin

Published Jan 1, 1986• 0 citations
Publisher

Abstract

We have studied the nature of the emission from a laser-excited KCI : O 2 − crystal and have observed that the emission evolves continuously from superfluorescence (SF) to amplified spontaneous emission (ASE) as the temperature of the crystal and hence the dephasing rate of the optical transition are increased. The sample is excited by a 30-ps pulse from a frequency-quadrupled Nd:YAG laser, and the 629.1-nm emission is detected using a streak camera system. At a temperature of 10 K the emission is characterized as SF with an average delay time of 200 ps and an average pulse width of 60 ps. As the temperature is increased to ~20 K, the output pulse broadens and the time delay increases to its maximum value of ~2 ns. As the temperature is increased still further, the time delay is observed to decrease, and at a temperature of 30 K the emission is characterized as ASE with a very small delay time and with an exponentially decaying time evolution. We modeled our experiment using the Maxwell-Bloch formalism and find good agreement for our measured output pulse shapes and for the dependence of delay time and pulse width on the dephasing rate.

DOI
10.1364/oam.1986.tum6

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We have studied the nature of the emission from a laser-excited KCI : O 2 − crystal and have observed that the emission evolves continuously from superfluorescence (SF) to amplified spontaneous emission (ASE) as the temperature of the crystal and hence the dephasing rate of the optical transition are increased. The sample is excited by a 30-ps pulse from a frequency-quadrupled Nd:YAG laser, and the 629.1-nm emission is detected using a streak camera system. At a temperature of 10 K the emission is characterized as SF with an average delay time of 200 ps and an average pulse width of 60 ps. As the temperature is increased to ~20 K, the output pulse broadens and the time delay increases to its maximum value of ~2 ns. As the temperature is increased still further, the time delay is observed to decrease, and at a temperature of 30 K the emission is characterized as ASE with a very small delay time and with an exponentially decaying time evolution. We modeled our experiment using the Maxwell-Bloch formalism and find good agreement for our measured output pulse shapes and for the dependence of delay time and pulse width on the dephasing rate.
Single crystals of KCl containing $\mathrm{O}_{2}^{}{}_{}{}^{\ensuremath{-}}$ centers (8\ifmmode\times\else\texttimes\fi{}1016{10}^{16}1016-7\ifmmode\times\else\texttimes\fi{}1017{10}^{17}1017 ${\mathrm{cm}}^{\ensuremath{-}3}$) were excited at low temperatures (T<30T<30T<30 K) using frequency-quadrupled single pulses of a mode-locked Nd-doped yttrium aluminum garnet laser. At excitation intensities above 20 GW/cm2{\mathrm{cm}}^{2}cm2 a spontaneous emission of coherent light was observed which could be identified as Dicke superfluorescence. This superfluorescence was observed on two of the zero-phonon lines in the vibrational progression of the $\mathrm{O}_{2}^{}{}_{}{}^{\ensuremath{-}}$ fluorescence spectrum (0-10 and 0-11 at 592.8 and 629.1 nm, respectively). We have studied the time dependence, the statistics of the delay times, and the intensities. The observed delay times vary between 0.5 and 10 ns, the observed pulse widths between 0.5 and 6 ns, and the coherence time was found to be longer than 100 ps. The observed linewidths of the superfluorescence ($0.016\mathrm{nm}\ensuremath{\cong}14\mathrm{GHz}$) is a factor of 2.5 smaller than that of the spontaneous fluorescence (0.042 nm at 4.2 K). The superfluorescence is observed only below a critical temperature which depends on the $\mathrm{O}_{2}^{}{}_{}{}^{\ensuremath{-}}$ concentration (8 to 28 K for concentrations between 8\ifmmode\times\else\texttimes\fi{}1016{10}^{16}1016 and 7\ifmmode\times\else\texttimes\fi{}1017{10}^{17}1017 ${\mathrm{cm}}^{\ensuremath{-}3}$).
The coupling of forward and backward propagating waves is studied theoretically in the transition region between superfluorescence (SF) and amplified spontaneous emission (ASE). To accomplish this a computer code has been written that solves Maxwell's equations in time and two spatial dimensions and accounts for counter-propagation, diffraction, and temporal coherence in the Bloch equations. Diffraction is ignored in the present calculations. In the SF regime the coupling is generally weak, as found by others; however, I have found a randomly occurring shot-to-shot coupling that is quite significant in cases where one wave, forward or backward, becomes established from quantum noise first in the amplified rod. In this case the wave that arises second is strongly coupled to the first. In the ASE regime the propagation shows strong forward-backward coupling and the characteristic spatial profile of the inversion that tends to zero at either end and to the small signal value of one in the middle of the amplifier. In the transion region the propagation shows mixed SF and ASE behavior.
The cooperative emission process in KCL;O2{\mathrm{O}}_{2}O2​${\mathrm{}}^{\mathrm{\ensuremath{-}}}$ has been studied as a function of the dephasing rate of the transition dipole. As the temperature of the sample is increased from 10 to 30 K, the emission evolves continuously from that characteristic of superfluorescence to that of amplified spontaneous emission. These results are in qualitative agreement with the predictions of current theories, but quantitative agreement is obtained only when current theories are modified so that the noise source that initiates the emission process is allowed to act continuously during the superfluorescent buildup.
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.
Numerical simulations of an extended sample of three-level atoms with slow dipole dephasing exhibit a superfluorescent pulse shortly after incoherent pumping begins. The operator Maxwell-Bloch equations are simulated by classical Langevin equations. The counterpropagating fields are solved for in the (one-dimensional) limit of the Fresnel number near unity, with open-end boundary conditions. An initial, ``quiet'' buildup of the inversion is followed by superfluorescence. Oscillation of the populations, coherences, and fields is observed. The superfluorescence delay time is compared with analytical predictions made in the linear regime. A transition to amplified spontaneous emission is found as the pump rate is decreased.
We study the superfluorescence (SF) from a gas of rubidium atoms. The atoms of a dense vapor are excited to the 5D5D5D state from the 5S5S5S state by a two-photon process driven by 100-fs laser pulses. The atoms decay to the 6P6P6P state and then to the 5S5S5S state. The SF emission at 420 nm on the 6P6P6P--5S5S5S transition is recorded by a streak camera with picosecond time resolution. The time duration of the generated SF is tens of picoseconds, which is much shorter than the time scale of the usual relaxation processes, including spontaneous emission and atomic coherence dephasing. The dependence of the time delay between the reference input pulse and SF is measured as a function of laser power. The experimental data are described quantitatively by a simulation based on the semiclassical atom-field interaction theory. The observed change in scaling laws for the peak intensity and delay time can be elucidated by an SF theory in which the sample length is larger than the cooperation length.