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Optics and Spectroscopy

Amplified spontaneous emission and its application for population of resonant states of the Xe and Kr atoms

Vadim A. Alekseev

Published Sep 1, 2002• 16 citations
Publisher

Abstract

To extend the capabilities of the existing spectroscopic methods of investigation and diagnostics of gaseous media, we consider a macroscopic effect of an increase in the rate of spontaneous emission, which results in the transition of a considerable part of excited molecules to lower-lying optically accessible states with light pulse emission along the direction of propagation of the exciting laser radiation. As an application of the effect of amplified spontaneous emission, we propose the population with its help of optically inaccessible electronic states of atoms and molecules.

DOI
10.1134/1.1509811

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It is well known that spontaneous emission is not an intrinsic atomic property, but rather results from the coupling of the atom to the vacuum modes of the electromagnetic field. As such, it can be modified by tailoring the electromagnetic environment into which the atom can radiate. This was already realized by Purcell, who noted that the spontaneous emission rate can be enhanced if the atom placed inside a cavity is resonant with one of the cavity is resonant with one of the cavity modes, and by Kleppner, who discussed the opposite case of inhibited spontaneous emission. It has also been recognized that spontaneous emission need not be an irreversible process. Indeed, a system consisting of a single atom coupled to a single mode of the electromagnetic field undergoes a periodic exchange of excitation between the atom and the field. This periodic exchange remains dominant as long as the strength of the coupling between the atom and a cavity mode is itself dominant. 23 refs., 6 figs.

•Dec 31, 1994•0 citations
To extend the capabilities of the existing spectroscopic methods of investigation and diagnostics of gaseous media, we consider a macroscopic effect of an increase in the rate of spontaneous emission, which results in the transition of a considerable part of excited molecules to lower-lying optically accessible states with light pulse emission along the direction of propagation of the exciting laser radiation. As an application of the effect of amplified spontaneous emission, we propose the population with its help of optically inaccessible electronic states of atoms and molecules.
Saturation effects in gaseous media in the presence of a high-intensity resonant laser field and in the field of incoherent radiation caused by the intrinsic spontaneous emission are considered. A simple nonlinear set of kinetic equations is proposed for describing the saturation effect in the case of optically thin media and nondegenerate levels. The Bennett structure and the band of homogeneous saturation, whose parameters are interdependent, exist in the velocity distribution. The regularities in the behavior of the band and the Bennett structure under variation in the transition parameters and the intensity of laser radiation are elucidated.
Laser amplifiers when pumped to a significant degree of population inversion undergo decay via (1) natural spontaneous emission of radiation from individual excited atoms, and (2) a size-dependent decay due to self-amplification of the spontaneously emitted radiation which passes through a large fraction of the amplifier length before escaping. This latter effect has a definite size threshold near which the decay rate changes several orders of magnitude. The decay rate is roughly independent of size except near the threshold.
A new, simple method for the generation of Xe(6s[3/2]1) and Xe(6s′[1/2]1) atoms is described. The method involves resonant two-photon excitation of Xe(6p[1/2]0 and 6p′[3/2]2) states followed by amplified spontaneous emission (ASE) to the Xe(6s[3/2]1 and 6s′[1/2]1) states. The vacuum ultraviolet transitions, Xe(6s[3/2]1→5p6(1S0)) at 147 nm and Xe(6s′[1/2]1→5p6(1S0)) at 129.6 nm, were used to monitor the time dependence of the resonance state atom concentrations. The quenching rate constants of these resonance atoms with ten molecules were measured at 300 K. The quenching cross-sections of the Xe(6s and 6s′) resonance atoms are compared to the cross-sections of the metastable Xe(6s[3/2]2) atoms and Xe(6p[3/2]2) atoms. The correlation between quenching cross-sections and photoabsorption cross-section of the molecules predicted by the resonance dipole–dipole energy transfer model is discussed. The applicability of the two-photon driven ASE method for the generation of other resonance state atoms is considered.
The present thesis is devoted to theoretical studies of pulse propagation of light through linear and nonlinear media, and of light-induced nuclear dynamics. The first part of the thesis addresses propagation of light pulses in linear periodical media - photonic crystals. The main accent was put on studies of the angular properties of two qualitatively different types of photonic crystals: holographic photonic crystals, and impurity band based photonic crystals. The anisotropy of band structure, group velocity and pulse delay with respect to the light polarization are analyzed. In the second part of the thesis a strict theory of nonlinear propagation of a few strong interacting light beams is presented. The key idea of this approach is a self-consistent solution of the nonlinear wave equation and the density matrix equations of the material. This technique is applied to studies of dynamics of cavityless lasing generated by ultra-fast multi-photon excitation. It is shown that interaction of co- and counter-propagating pulses of amplified spontaneous emission (ASE) affects the dynamics and efficiency of nonlinear conversion. Our dynamical theory allows to explain the asymmetric spectral properties of the forward and backward ASE pulses, which were observed in recent experiment with different dye molecules. It is shown that the ASE spectral profile changes drastically when the pump intensity approaches the threshold level. The effect of the temporal self-pulsation of ASE is studied in detail. The third part of the thesis is devoted to light-induced nuclear dynamics. Time- and frequency-resolved X-ray spectroscopy of molecules driven by strong and coherent infrared (IR) pulses shows that the phase of the IR field strongly influences the trajectory of the nuclear wave packet, and hence, the X-ray spectrum. Such a dependence arises due to the interference of one (X-ray) and two-photon (X-ray + IR) excitation channels. The phase of the light influences the dynamics also when the Rabi frequency approaches the vibrational frequency, breaking down the rotating-wave approximation. The probe X-ray spectra are also sensitive to the delay time, the duration, and the shape of the pulses. The evolution of the nuclear wave packets in the dissociative core-excited state affects the dynamics of resonant Auger scattering from fixed-in-space molecules. One of the important dynamical effects is the atomic-like resonance which experiences electronic Doppler shift. We predict that the scattering of the Auger electrons by nearby atoms leads to new Doppler shifted resonances. These extra resonances show sharp maxima in the bond directions, which makes them very promising as probes for local molecular structure using energy and angular resolved electron-ion coincidence techniques. Our theory provides prediction of several new effects, but also results that are in good agreement with the available experimental data.
It is well known that spontaneous emission is not an intrinsic atomic property, but rather results from the coupling of the atom to the vacuum modes of the electromagnetic field. As such, it can be modified by tailoring the electromagnetic environment into which the atom can radiate. This was already realized by Purcell, who noted that the spontaneous emission rate can be enhanced if the atom placed inside a cavity is resonant with one of the cavity is resonant with one of the cavity modes, and by Kleppner, who discussed the opposite case of inhibited spontaneous emission. It has also been recognized that spontaneous emission need not be an irreversible process. Indeed, a system consisting of a single atom coupled to a single mode of the electromagnetic field undergoes a periodic exchange of excitation between the atom and the field. This periodic exchange remains dominant as long as the strength of the coupling between the atom and a cavity mode is itself dominant. 23 refs., 6 figs.