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Journal of Physics B Atomic Molecular and Optical Physics

Resonant dip of two-photon ionisation and stimulated emission in laser-pumped magnesium vapour

Jingyuan Zhang, Zhou Hai-tian, Li Qiong-ru, Jian Sheng Yang, Zhao Lizeng, Yuxin Nie

Published Feb 28, 1988• 3 citations
Publisher

Abstract

An anomalous resonant dip of two-photon ionisation with 3s3p 1 P as an intermediate state and a stimulated emission by the 3s4s 3 S-3s3p 3 P transition, at 518.37 nm following the pulsed laser excitation near the 3s 2 1 S-3s3p 1 P resonance at 285.21 nm in magnesium vapour are observed and studied. The mechanism of the ionisation dip is attributed to formation and predissociation of the A 1 Sigma + u Mg 2 dimer, which transfer the population from the laser-pumped 3s3p 1 P level to 3s3p 3 P levels. Re-excitation of the produced 3s3p 3 P atoms and the subsequent radiative processes are presumed to explain the generation of stimulated emission. A theoretical model is employed to interpret the experimental phenomena.

DOI
10.1088/0953-4075/21/4/013

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An anomalous resonant dip of two-photon ionisation with 3s3p 1 P as an intermediate state and a stimulated emission by the 3s4s 3 S-3s3p 3 P transition, at 518.37 nm following the pulsed laser excitation near the 3s 2 1 S-3s3p 1 P resonance at 285.21 nm in magnesium vapour are observed and studied. The mechanism of the ionisation dip is attributed to formation and predissociation of the A 1 Sigma + u Mg 2 dimer, which transfer the population from the laser-pumped 3s3p 1 P level to 3s3p 3 P levels. Re-excitation of the produced 3s3p 3 P atoms and the subsequent radiative processes are presumed to explain the generation of stimulated emission. A theoretical model is employed to interpret the experimental phenomena.
We have observed stimulated emission on the transitions 43S1−33PJ° near 518 nm following pulsed laser excitation of Mg vapor near the 31S0−33P1° resonance at 285 nm. The emission has a divergence similar to the pump laser and closely follows the incident laser in time. The mechanism apparently involves pumping an accidental coincidence 31S0−33P1° and 33PJ°−53DJ, permitting depletion of the lower level of the triplet transition. Photoionization of the Mg vapor creates a large electron density (≲1013 cm−3); electron-impact collisions are presumed to mediate the process, transferring population from the laser-pumped 31P1° level to the triplet manifold.
Laser excitation and ionization processes in dense (1–10 Torr) sodium vapor have been studied for laser wavelengths near the two-photon allowed nd 2D(n=3, 4, 5) and ns 2S(n=4, 5, 6) states. In particular, the 1 3Σ+g→1 3Σ+u excimer emission in Na2, predicted in 1980 by Konowalow and Julienne and observed recently by Dinev et al, was studied here in greater detail. Strong excimer emission (∼830 nm) was observed for two-photon pumping to both sides of the unresolved 4D states, and weak excimer emission was seen when pumping near the 5D levels. The excimer emission exhibits a complicated pump laser profile with a pronounced ‘‘dip’’ at the 4d 2D two-photon resonance. Similarly, [2+1] photon ionization via the 3d 2D and 4d 2D states shows a dramatic decrease as the sodium density increases. These results can be attributed either to depleted 3d 2D or 4d 2D population due to stimulated electronic Raman scattering (SERS) or to the interference effects recently reported by Malcuit et al. and Krasnikov et al. and treated theoretically by Manykin and Afanas’ev and by Agarwal. It is argued that both mechanisms are operative. Strong ionization and SERS signals were observed at the hybrid resonances corresponding to 3p 2P3/2, 1/2 →4d 2D transitions; however, no excimer lasing at 830 nm was detected. No excimer emission was detected upon two-photon pumping near or at the 3d 2D or ns 2S(n=4, 5, 6) states. Based on these and other observations, the 1 3Σ+g→1 3Σ+u excimer emission is attributed to a molecular Raman process involving stimulated emission or six-wave mixing via a pathway of the type 1 3Σ+u→2hν 3Δu→ j 3Πg→(k 3Πu, l 3Σ +u)→1 3Σ+g→1 3Σ +u .
Polarization and intensity spectra have been obtained for excited-state magnesium (3s3p 1P1) - rare gas optical collisions. The magnesium was excited by a linearly polarized laser tuned to the 3s21s0 → 3s3p 1P1 atomic transition at 285 nm. A second linearly polarized laser was tuned near the 3s3p 1P1 → 3s5s 1S0 transition at 571 nm (experiment A) and near the 3s3p 1P1 → 3s4d 1D2 transition at 553 nm (experiment B). The polarization vector of the second laser was oriented either parallel or perpendicular to the polarization direction of the first laser. The absorption of nonresonant light from the second laser, possible only during a collision, was monitored by cascade fluorescence from the 3s21S0 ← 3s4p 1P1 transition at 203 nm. For each detuning of the second laser from resonance, the degree of linear polarization and the intensity were measured. For experiment A, argon and neon were used as rare gases. For experiment B, argon was the rare gas used. For experiment B, fluorescence from the 3s3p 1P1 ← 3s5s 1S0 transition, and the 3s3p3Pj ← 3s5s 3S1 transition at 333 nm were also measured in an attempt to observe the region of inelastic transitions in the molecular states. No inelastic branching was observed in this experiment.
The concepts of quantum efficiency and ion yield pertinent to a photon detector consisting of an atmospheric pressure oxygen–argon–acetylene (or hydrogen) flame containing magnesium atomic vapour, and also some published experimental results obtained with this detector, are critically discussed. In these experiments, collision-induced ionization and direct photoionization of magnesium atoms are performed. In the former instance, one dye laser excites the atoms from the ground state into the 3s3p–1P10 state and another laser, in temporal and spatial coincidence with the first, brings the excited atoms into the 3s5d–1D2 state, from which collisional ionization occurs. In the last instance, direct photoionization from the 1P10 level is accomplished either with the excimer laser radiation at 308 nm or by tuning the second laser into an autoionizing resonance at 300.9 nm. It is shown that the total loss rate from the 1P10 level can be calculated by time resolving the resonance fluorescence waveform, with and without the presence of the second laser, and that, by integrating this signal over the duration of the laser pulse, the fluorescence dip obtained can be related to the ion yield of the excitation–ionization scheme. It is also stressed that, because of the presence of a metastable level which can act as a trap for the excited atoms, owing to quenching collisions in the flame, the quantum efficiency of this detector will never exceed the ‘ion branching ratio’, i.e., the ratio between the ionization rate and the total loss rate from the excited level. By evaluating several experimental results obtained with different laser systems, it is shown that, in the collision-induced ionization mode, both fluorescence and ionization measurements are necessary to derive the quantum efficiency, whereas in the direct photoionization mode, fluorescence data suffice.