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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Multi-quantum excitation in optically pumped alkali atom: rare gas mixtures

Kristin L. Galbally-Kinney, Wilson T. Rawlins, Steven J. Davis

Published Mar 3, 2014• 2 citations
Publisher

Abstract

Diode-pumped alkali laser (DPAL) technology offers a means of achieving high-energy gas laser output through optical pumping of the D-lines of Cs, Rb, and K. The exciplex effect, based on weak attractive forces between alkali atoms and polarizable rare gas atoms (Ar, Kr, Xe), provides an alternative approach via broadband excitation of exciplex precursors (XPAL). In XPAL configurations, we have observed multi-quantum excitation within the alkali manifolds which result in infrared emission lines between 1 and 4 μm. The observed excited states include the 42FJ states of both Cs and Rb, which are well above the two-photon energy of the excitation laser in each case. We have observed fluorescence from multi-quantum states for excitation wavelengths throughout the exciplex absorption bands of Cs-Ar, Cs-Kr, and Cs-Xe. The intensity scaling is roughly first-order or less in both pump power and alkali concentration, suggesting a collisional energy pooling excitation mechanism. Collisional up-pumping appears to present a parasitic loss term for optically pumped atomic systems at high intensities, however there may also be excitation of other lasing transitions at infrared wavelengths.

DOI
10.1117/12.2040023

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Diode-pumped alkali laser (DPAL) technology offers a means of achieving high-energy gas laser output through optical pumping of the D-lines of Cs, Rb, and K. The exciplex effect, based on weak attractive forces between alkali atoms and polarizable rare gas atoms (Ar, Kr, Xe), provides an alternative approach via broadband excitation of exciplex precursors (XPAL). In XPAL configurations, we have observed multi-quantum excitation within the alkali manifolds which result in infrared emission lines between 1 and 4 μm. The observed excited states include the 42FJ states of both Cs and Rb, which are well above the two-photon energy of the excitation laser in each case. We have observed fluorescence from multi-quantum states for excitation wavelengths throughout the exciplex absorption bands of Cs-Ar, Cs-Kr, and Cs-Xe. The intensity scaling is roughly first-order or less in both pump power and alkali concentration, suggesting a collisional energy pooling excitation mechanism. Collisional up-pumping appears to present a parasitic loss term for optically pumped atomic systems at high intensities, however there may also be excitation of other lasing transitions at infrared wavelengths.
Lasing on the 62P1/2→62S1/2(D1) resonance transition of atomic Cs at 894.3 nm has been demonstrated in mixtures of Ar, ethane, and Cs vapor by the photoexcitation of ground state Cs-Ar collision pairs and subsequent dissociation of diatomic, electronically-excited CsAr molecules (exciplexes or excimers). The blue satellites of the alkali D2 lines provide a pathway for optically pumping atomic alkali lasers on the principal series (resonance) transitions with broad linewidth (>2 nm) semiconductor diode lasers. In this paper we discuss different variations of this new laser system and the experiments of the initial demonstration.
Alternative wavelengths for optically pumped alkali vapor lasers have been developed using single photon excitation of higher lying P-states, stimulated Raman processes, two-photon excitation of S and D states, and electric quadruple excitation on S-D transitions. Two photon excitation of Cs 72D leads to competing and cascade lasing producing red and infrared lasers operating on the D-P transitions, followed by ultraviolet, blue, the standard near infrared DPAL transitions operating on P-S transitions. The S-D pump transitions are fully bleached at pump intensities exceeding 1 MW/cm2, allowing for lasing transitions that terminate on the ground state. The kinetics of these systems are complex due to competition for population inversion among the many optical transitions. An optically pumped mid-infrared rubidium pulsed, mirrorless laser has also been demonstrated in a heat pipe along both the 62P3/2 - 62S1/2 transition at 2.73 μm and the 62P1/2 - 62S1/2 transition at 2.79 μm with a maximum energy of ~100 nJ. Performance improves dramatically as the rubidium vapor density is increased, in direct contradiction with the prior work. No scaling limitations associated with energy pooling or ionization kinetics have been observed. Practical application for infrared counter measures depends on the further development of blue diode pump sources. Finally, stimulated electronic Raman scattering and hyper-Raman processes in potassium vapor near the D1 and D2 lines have been observed using a stable resonator and pulsed laser excitation. First and second order Stokes and anti-Stokes lines were observed simultaneously and independently for a pump laser tuning range exceeding 70 cm-1. When the pump is tuned between the K D1 and D2 lines, an efficient hyper-Raman process dominates with a slope efficiency that exceeds 10%. Raman shifted laser may be useful as a target illuminator or atmospheric compensation beacon for a high power diode pumped alkali laser.
Abstract We present experimental results of an exciplex-pumped alkali laser (XPAL) at 780 nm based on the 5 2 P 3/2 → 5 2 S 1/2 transition of the Rb atom in mixtures of Rb vapor and Ar. A laboratory-built Ti:sapphire laser with a pulse repetition rate of 3 kHz and a pulse width of 100 ns is used as the pump source. The maximum laser pulse energy of 0.26 µJ at 780 nm is obtained under an absorbed pump pulse energy of 42 µJ at 755 nm in mixtures of Rb vapor and Ar at a temperature of 423 K, corresponding to an optical conversion efficiency of 0.62%. Further experiments show that the output laser at 780 nm can always be detected for pump wavelengths ranging from 754 to 759 nm, indicating that Rb–Ar mixtures can be effectively pumped by commercial laser diodes (LDs) with a bandwidth of 5 nm.
Abstract : The Doppler-broadened two-photon absorption (TPA) cross-section for the 52S1/2- 52D5/2 transition in Rb is measured using direct absorption methods. A detailed model of the intensity profile was developed to account for a focused Gaussian beam propagating through a two-photon absorption medium. A peak absorbance of 24% was observed for an intensity of 6.28 kW/cm2 at the focus, a Rb density of 4.6 x 1015 cm-3 concentrations from 1.61-8.52 x 10(15) cm-3 line. Extracting the hyperfine-broadened TPA cross-section from 87 test configurations, while varying the pump power, alkali concentration and focal length, yielded an error weighted average of 6.75x10-21 cm4/W. This cross-section is sufficient for a pulsed dye laser to bleach the pump transition in the Two-Photon Pumped Alkali Laser (TPAL) that lases at 420 nm and 5.2 mum. Additionally, optically pumped atomic rubidium lasers pumped in the blue satellite of the D2 line from the ground Rb-Ar or Rb-Kr collision pair to the dissociative B2 sum 1/2 produce laser emission at 780.2 nm. Lasing is achieved for the Rb-Ar system and 757.1 - 760.4 nm for the Rb-Kr system. Slope efficiencies exceed 0.25% using a heat pipe configuration. The gain is very high with photon build-up times of 1-3.7 ns.
We describe a series of measurements of absorption and laser induced fluorescence on cells that contained cesium and rubidium and a rare gas: He, Ar, Kr, or Xe. These studies showed strong blue wing absorption to the short wavelength side of the alkali atom D2 lines due to collisionally formed Cs- or Rb-rare gas excimers. We also have observed an efficient two photon excitation of higher lying states in Cs and Rb that produces both intense blue emission and IR atomic emission in the 1.3 to 3.8 μm spectral region.
Optically pumped alkali vapor lasers are currently being developed in several laboratories. The objective is to construct high-powered lasers that also exhibit excellent beam quality. Considerable progress has been made, but there are technical challenges associated with the reactivity of the metal atoms. Rare gas atoms (Rg) excited to the np(5)(n+1)s (3)P(2) configuration are metastable and have spectral properties that are closely similar to those of the alkali metals. In principle, optically pumped lasers could be constructed using excitation of the np(5)(n+1)p←np(5)(n+1)s transitions. We have demonstrated this potential by observing gain and lasing for optically pumped Ar(*), Kr(*) and Xe(*). Three-level lasing schemes were used, with He or Ar as the collisional energy transfer agent that established the population inversion. These laser systems have the advantage of using inert reagents that are gases at room temperature.