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Progress in Crystal Growth and Characterization of Materials

Cooperative superfluorescence and time delayed 2nd harmonic generation

Xilin Lu, J. H. Brownell, Sven R. Hartmann

Published Jan 1, 1996• 0 citations
Publisher

Abstract

A 10 ps transform limited optical pump pulse two-photon-resonant with the 6 S1/2-6 D32 442 nm transition in Cs vapor generates a coherent state superposition which, after a delay exceeding the pulse width, gives rise to second harmonic emission (when a transverse magnetic field is present) and superfluorescence (SF) directed against the pump on the upper 6 D3/2-6 P1/2 transition, followed by cooperative SF along the pump simultaneously on both the upper and lower 6 P3/2 − 6 P1/2 transitions, followed in turn by SF against the pump on the lower transition. Phase locked quantum beats associated with the 1.17 GHz hyperfine splitting of the 6 P1/2 appear on all SF emissions.

DOI
10.1016/0960-8974(96)83662-x

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Physical Review A•Oct 20, 2010•52 citations
A 10 ps transform limited optical pump pulse two-photon-resonant with the 6 S1/2-6 D32 442 nm transition in Cs vapor generates a coherent state superposition which, after a delay exceeding the pulse width, gives rise to second harmonic emission (when a transverse magnetic field is present) and superfluorescence (SF) directed against the pump on the upper 6 D3/2-6 P1/2 transition, followed by cooperative SF along the pump simultaneously on both the upper and lower 6 P3/2 − 6 P1/2 transitions, followed in turn by SF against the pump on the lower transition. Phase locked quantum beats associated with the 1.17 GHz hyperfine splitting of the 6 P1/2 appear on all SF emissions.
A laser pulse two-photon resonant with the ${6S}_{1/2}\ensuremath{-}{6D}_{3/2}$ 442 nm transition in Cs vapor generates delayed superfluorescence (SF) on the upper ${6D}_{3/2}\ensuremath{-}{6P}_{1/2}$ 876 nm and lower ${6P}_{1/2}\ensuremath{-}{6S}_{1/2}$ 894 nm transitions. Yoked SF is observed in the forward (along the laser) direction as evidenced by the simultaneous appearance of SF on both transitions. Cascade SF is observed in the backward direction, where SF on the lower transition only evolves after it has terminated on the upper. The four SF signals exhibit quantum beats associated with the 6P1/2{6P}_{1/2}6P1/2​ hyperfine splitting.
Second harmonic generation has hitherto been thought of as simultaneous with the excitation pulse which generates it. Recent experiments in Cs vapor demonstrate otherwise. A short two-photon 6D - 6S resonant excitation pulse in Cs vapor generates a superposition state which would radiate immediately were it not for destructive interference arising from the sample being large compared to the radiation wavelength. The radiation pattern of an isolated radiator (atom) starts out with a null in the plane transverse to the polarization (linear) direction but then rotates about the applied transverse magnetic field developing a radiation component along the phase matched direction which we detect. Experimental results are presented in excellent agreement with theory. Previous delay discrepancies have been resolved by using a nonmetallic sample cell. Cascade and yoked superfluorescence take place but not significantly until after the second harmonic emissions. Quantitative measurements of signal intensity are also presented.
Time-delayed second harmonic generation has recently been reported in an atomic vapor of Cs at a temperature near 180 degrees Celsius and situated in a magnetic field of the order of a killogauss. Short 10 ps excitation laser pulses at 885 nm were used to excite a macroscopic electric quadrupole density which was then observed to radiate at 442 nm after a delay of a few hundred picoseconds. The experiment is complicated by the presence of several superfluorescence transitions some of which radiate close to the 442 nm wavelength. These emissions are also delayed and our strategy is to set the experimental conditions so that they only become appreciable after the second harmonic emission is complete. In this paper we show how the second harmonic develops by considering the evolution of the radiation pattern of an isolated atomic radiator (not forbidden to radiate at the second harmonic even in the absence of a magnetic field). We estimate the intensity of the superradiant second harmonic emission and obtain agreement with experiment. Excellent agreement is also obtained between measured and calculated delay.
Second harmonic generation in Cs vapor is produced by the combined action of a polarized laser pulse and a magnetic field. It is delayed from the 10 ps excitation pulse by several hundred ps. The laser is two-photon resonant with the $6{S}_{\frac{1}{2}}\ensuremath{-}6{D}_{\frac{3}{2}}$ transition and initially induces a macroscopic quadrupole moment whose radiation pattern has a null in the forward direction. The magnetic field reshapes this pattern to produce second harmonic light, which is simply a free polarization decay signal evolving in a manner akin to the free induction decay following an adiabatic demagnetization.
A dense sample of atomic rubidium vapor excited by a short (4 ps) transform-limited laser pulse two-photon resonant with the 5S-5D transition in a large Fresnel number geometry emits a delayed omnidirectional infrared superfluorescence pulse (coherent flash) on the 5D-6P transition. This superfluorescence emission involves a coherent population transfer to the 6P level and results in prompt directional yoked UV emission and coherent population transfer back to the ground 5S state. This emission completes the process of parametric four-wave mixing, selectively involving only those atoms on the 6P level whose 5D-6P emission satisfies the phase-matching condition. The unique feature of this four-wave mixing radiation is that it occurs after the termination of the pump pulse, as evidenced by direct measurement of emission timing. The multidirectional character of superfluorescent emission is confirmed by the observation of non-collinear parametric four-wave mixing when exciting the sample by two simultaneous overlapping pulses, for a wide range of beam angles. Also observed and investigated is superfluorescent transient diffraction that appears when the sample is excited by a sequence of three laser pulses.
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.