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Quantum Electronics

Influence of spontaneous emission on the threshold longitudinal pump power of dye lasers

V. P. Klochkov, E. B. Verkhovskiĭ

Published Nov 30, 1994• 1 citation
Publisher

Abstract

The stimulated emission threshold of a dye laser was found to depend on the method of formation of a longitudinal pulsed laser beam used as the pump. Excitation with a focused pump beam reduced the lasing threshold. The effect was strongest when the Q factor of the resonator cavity was low. This reduction in the lasing threshold by focusing the pump laser beam was attributed to an increase in the rate of spontaneous emission resulting from lasing of desqueezed states (enhancement of 'zero-field' fluctuations responsible for the appearance of spontaneous emission). An increase in the spontaneous emission rate reduced the buildup time of stimulated emission during the early stages and thus reduced the lasing threshold.

DOI
10.1070/qe1994v024n11abeh000216

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The stimulated emission threshold of a dye laser was found to depend on the method of formation of a longitudinal pulsed laser beam used as the pump. Excitation with a focused pump beam reduced the lasing threshold. The effect was strongest when the Q factor of the resonator cavity was low. This reduction in the lasing threshold by focusing the pump laser beam was attributed to an increase in the rate of spontaneous emission resulting from lasing of desqueezed states (enhancement of 'zero-field' fluctuations responsible for the appearance of spontaneous emission). An increase in the spontaneous emission rate reduced the buildup time of stimulated emission during the early stages and thus reduced the lasing threshold.
The threshold pump power density for lasing in dye solutions is found to depend on the photon energy of pumping radiation. An increase in the pumping photon energy can significantly lower the threshold pump power of dye lasers. For an ethanol solution of rhodamine 6G with a concentration of 4×10 18 cm −3 , the threshold power density for pumping radiation with a wavelength of 532 nm is 20-fold higher than for pumping radiation with a wavelength of 347 nm. This phenomenon is associated with the competition of collective spontaneous emission, which can lead to the efficient deactivation of excited molecules in femtosecond times, and the dephasing of excited molecules due to the intramolecular nonradiative processes of absorbed-energy conversion. An increase in the dephasing rate with the increasing energy of exciting photons lowers the efficiency of collective spontaneous emission and increases the concentration of dephased excited molecules responsible for lasing.
We review the physics underlying the process of spontaneous emission, with a special focus on spontaneous emission into a resonator mode. We define the mode volume, verify the fundamental modal dimensions, present the spectral mode profile, the coherence time, the Q-factor, the Füchtbauer-Ladenburg equation, and the Purcell factor, and discuss their influence on different types of lasers. We obtain the relation between peak emission cross section, radiative lifetime, and emission linewidth. By interpreting spontaneous emission as stimulated emission driven by vacuum fluctuations, we derive the spontaneous-emission rate into a resonator mode and establish physical expressions for the fractions of spontaneous emission and total decay from the upper laser level into this mode. Furthermore, we discuss coupling of the atomic system with the coherent field inside a lasing resonator mode, resulting in the formation of a Mollow triplet, and demonstrate that it leads to a reduction of the spontaneous-emission rate by a factor of 2.
We report an observation of nonsaturable absorption of light. When a laser medium in a small aspect ratio geometry is uniformly and transversely pumped, amplified spontaneous emission (ASE) builds up along the longitudinal axis. The higher ASE intensity at the ends of the cell repopulates the ground state through the stimulated emission process more rapidly than at the center of the cell. Therefore, the absorption of the pump light is enhanced at the ends and the transmitted pump beam shows a nonuniform profile with a peak at the center. When the occupation of the states other than the upper lasing state and the ground state can be ignored, the normalized profile of the transmitted pump beam becomes identical to that of the fluorescence depicting the upper state population distribution. This fact has been confirmed experimentally with a R6G dye cell pumped with various intensities of frequency doubled Nd:YAG laser (λ = 532 nm, 10-ns pulse duration). The percentage of the absorbed pump energy at the ends of the cell remains the same, virtually nonsaturable, whereas at the center it decreases as the pump intensity increases.
We consider the problem of reducing the contributions of pump and spontaneous-emission noise to the output noise of a laser field. We consider two models based on an atomic medium, one analytic, the other involving numerical simulation of a sequence of pump cycles. The predictions of both models are shown to agree. For regular pump excitation the intensity fluctuations of a laser well above threshold may be reduced to zero at the cavity resonance frequency if the ratio of the lifetimes of the upper and lower lasing levels is sufficiently large that spontaneous emission is suppressed. When the atomic lifetimes are comparable, spontaneous emission reduces the amount of noise reduction. For example, for equal atomic lifetimes regular pump excitation will result in a maximum noise reduction in the output field of one-half the shot-noise limit.
The relative mean square fluctuations $\frac{〈{(\ensuremath{\Delta}I)}^{2}〉}{{〈I〉}^{2}}$ of the intensity III of a single-mode dye laser have been measured by a photon counting technique, in the region from about threshold to intensities 1000 times below threshold. The results show a steady increase of $\frac{〈{(\ensuremath{\Delta}I)}^{2}〉}{{〈I〉}^{2}}$ from less than 1 to about 150 as 〈I〉〈I〉〈I〉 is reduced, followed by a rapid drop to zero. This behavior appears to be described fairly well by an equation of motion containing both additive spontaneous emission fluctuations and multiplicative pumping fluctuations.
The dependence of the emission of a concentrated (∼10 19 cm −3 solution of Rhodamine C on the power density Φ of exciting laser radiation was studied. The emission intensity for the power density of exciting radiation above ∼10 25 cm −2 s −1 was found to have a nearly quadratic dependence on the power density Φ, and this emission was interpreted as the cooperative spontaneous emission of a Dicke type. For Φ≲10 25 cm −2 s −1 , the emission intensity increased with increasing Φ according to the exponential law. This emission was interpreted as the amplified spontaneous emission. The spectra of cooperative emission depended on the pump radiation power only weakly. The absence of lasing in dye solutions at high concentrations, which is a well-known phenomenon, was shown to be caused by the development of the cooperative spontaneous emission and not by the concentration quenching, and the former process is more rapid than the latter.