22nd International Symposium on Plasma Chemistry July 5-10, 2015; Antwerp, Belgium Plasma formation during operation of a diode pumped alkali laser A.H. Markosyan and M.J. Kushner University of Michigan, Electrical Engineering and Computer Science Department, 1301 Beal Avenue, US-48109-2122 Ann Arbor, MI, U.S.A. Abstract: Diode pumped alkali lasers (DPALs) achieve narrow-band lasing action on the resonant lines of alkali atoms following pumping by broad band semiconductor lasers. Resonant excitation of alkali vapor is known to lead to plasma formation through electron heating by super-elastic relaxation and associative ionization. A first principles global model was developed to investigate the operation of the Ar/Cs DPAL system and the issues that arise if plasma formation occurs. Plasma characteristics and their impact on laser performance are reported during high repetition rate, high power optical pumping. Keywords: diode pumped alkali laser, DPAL, global model, laser produced plasma 1. Introduction Semiconductor diode lasers have the advantage of high electrical-to-optical efficiency however they suffer from poor optical quality. The diode pumped alkali laser (DPAL) is a method whereby the poor optical quality of diode lasers can be converted to the high optical quality of an atomic laser [1]. In DPAL, the resonant transition of the alkali atom, typically the 2P 3/2 (D 2 line) is pumped by the diode laser followed by collisional quenching to the 2P 1/2 . Lasing then occurs on the 2P 1/2 → 2S 1/2 transition (D 1 line), which requires that the ground state be inverted. DPALs have been investigated for their potential as high-power lasers [2-5]. Recent studies of Rb and K DPAL have yielded efficiencies in excess of 50% [2, 3]. Models predict efficiencies exceeding 90%. Our interest here is on the DPAL using Cs vapor. LIBORS (Laser Ionization Based on Resonance Saturation), first proposed by Measures [6] in 1970, is an efficient means for producing plasmas in alkali vapor with low laser intensity. Electron heating by super-elastic relaxation of the laser produced resonant state M* can rapidly avalanche the alkali vapor to nearly full ionization [7]. In many alkali vapors, the process can be initiated by associative ionization (M* + M* → M 2 + + e) by resonant states. This process in Cs is endothermic, and so requires states higher than Cs(62P 1/2 , 62P 3/2 ). With pre-existing or laser generated seed electrons, super-elastic electron heating and associative ionization during DPAL operation may result in plasma formation through the LIBORS process. The resulting plasma has the potential to reduce or quench laser oscillation through electron collision mixing. In this paper, we discuss results from a computational investigation of the pulsed DPAL system in Ar/Cs/C 2 H 6 mixtures. Pumping is on the 62S 1/2 → 62P 3/2 D 2 (852.35 nm) transition of Cs and lasing occurs on the 62P 1/2 → 62S 1/2 D 1 (894.59 nm) transition. The ethane, C 2 H 6 , collisionally transfers excitation from 62P 3/2 to 62P 1/2 . This investigation focused on the formation of P-I-2-36 plasma and its consequences on laser action. A parametric study was performed of the plasma production and laser operation as a function of pump power and cell temperature (Cs vapor pressure). 2. Description of the model The simulation used in this investigation is Global_Kin, a global plasma kinetics model that is described in Ref. [8]. In Global_kin, rate equations for species densities, temperatures, pump intensities, and laser intensities are integrated as a function of time over successive pulsed periods. Electron impact processes are included for elastic and inelastic collisions, including electronic and vibrational excitation, super-elastic collisions, ionization and recombination. All rate coefficients for electron impact processes are functions of electron temperature, T e , which is determined by solving an electron energy conservation equation. The rate coefficients are obtained from solutions of Boltzmann’s equation for the electron energy distribution function. The electron impact cross sections for Cs were calculated using fully relativistic allelectron B-spline R-matrix (BSR) with pseudo-states ansatz with 311 coupled states [9]. We determined the Cs/Cs 2 densities by the vapor pressure based on the temperature of the cell (350 K – 425 K). We laser cell is 5 cm long with a 98% output mirror reflectivity. The reaction mechanism includes 629 reactions and the following 38 species: e, Cs(62S 1/2 , 62P 1/2 , 62P 3/2 , 52D 3/2 , 52D 5/2 , 72S 1/2 , 72P 1/2 , 72P 3/2 , Ryd), Cs+, Cs 2 , Cs 2 +, Cs 2 *, CsAr(A2Π 1/2 , A2Π 3/2 , B2Σ+ 1/2 ), CsAr(X)+, CsAr(A)+, Ar, Ar(1s 2 , 1s 3 , 1s 4 , 1s 5 , 4p, 4d), Ar+, Ar 2 *, Ar 2 +, C 2 H 6 , C 2 H 6 (v13, v24), C 2 H 6 +, C 2 H 6 +, C 2 H 6 -, φ pump , φ laser (894.59 nm), φ laser (852.35 nm). 3. Lasing and plasma formation As a base case, the diode laser pump pulses at 852.35 nm are 1μs long with a 1 kHz frequency. The pump radiation propagates through a quartz cell heated to 375 K containing 600 Torr of Ar/C 2 H 6 /Cs = 83/17/1.1 × 10-6. 1 A pulse-periodic steady state is reached after 10-20 pump pulses with electron densities of (0.9-1.4) × 1011 cm-3. The electron densities over successive pulses of 10 kW cm-2 are shown in Fig. 1. The electron density increases over tens of pulses to 1011 cm-3 due to electron impact following super-elastic heating and associative ionization. The densities of species responsible for lasing are shown in Fig. 1 for the 100th pulse for a 7.5 kW cm-2 pump. Laser oscillation occurs for nearly the entire pump period. The laser transition is saturated, as indicated by the equal densities of the 62P 1/2 and 62S 1/2 states. The positive charge is mainly concentrated in Cs+ and Cs 2 +, as there is little ionization of either Ar. or C 2 H 6 since the electron temperature is no greater than 0.1 eV. During the pump pulse a significant amount of Cs(72P 1/2 , 72P 3/2 ) created, which enables associative ionization and creation of Cs+ (e.g. Cs(62P 1/2 ) + Cs(72P 1/2,3/2 ) → Cs+ + Cs + e). slope efficiency. That is, more pump power produces more laser intensity. At high pump power or low vapor density, laser intensity is limited by the absolute Cs density available to absorb the pump power. This causes saturation in the laser intensity with increasing pump power. Fig. 2. D 1 (894.59 nm) laser intensity as a function of pump power for various cell temperatures and vapor pressures. Lasing efficiency as a function of pump power for various cell temperatures and Cs vapor pressures is shown in Fig. 3. Laser efficiency is the time integrated laser intensity (laser pulse energy) divided by the time integrated pump intensity (pump energy). Due to saturation of the laser intensity at high pump powers or low vapor densities the laser efficiency decreases. On the other hand, the higher laser power (and efficiency) can be “bootstrapped” by raising the cell temperature (and so Cs vapor pressure) with pump rate. Other limiting factors for efficiency at high pump rate are associative ionization, photo-ionization of higher lying excited states of Cs and electron quenching of the laser levels. Fig. 1. (Top) Electron density after 100 pulses of 10 kW cm-2. (Bottom) The densities of Cs excited states and ions at pump power of 7.5 kW cm-2. Laser intensity as a function of pump power is shown in Fig. 2 for various cell temperatures and Cs vapor densities. At low pump power or high vapor density, laser action is limited by pump rate resulting positive 2 4. Concluding Remarks Using a global model, a computational parametric study was performed of the DPAL system in Ar/C 2 H 6 /Cs mixture with lasing on Cs(62P 1/2 ) → Cs(62S 1/2 ) (894.59 nm) transition. Plasma formation is unavoidable when populating resonant states of alkali atoms (i.e., LIBORS) given seed electrons. Due to lack of associative ionization, which naturally provides seed electrons, significant plasma formation occurs only at higher pump rates. For example, in high repetition rate operation with high pump intensities produces plasma densities exceeds 1012 cm-3. These densities decrease laser intensity by electron collisional mixing. P-I-2-36 modeling an excimer-pumped alkali laser”. Plasma Sources Sci. Technol., 23 035011 (2014) Fig. 3. D 1 Laser efficiency as a function of pump power for various cell temperatures and Cs vapor pressures. 5. Acknowledgements This work was supported by the US Department of Defense High Energy Laser Multidisciplinary Research Initiative. 6. References [1] W.F. Krupke. “Diode pumped alkali lasers (DPALs)-A review”. Prog. Quant. Electron., 36, 4 (2012) [2] [3] B.V. Zhdanov, T. Ehrenreich, R.J. Knize. “Highly Efficient Optically Pumped Cesium Vapor Laser”. Opt. Comm., 260, 696 (2006) [4] B.D. Barmashenko and S. Rosenwaks. “Detailed analysis of kinetic and fluid dynamic processes in diode pumped alkali lasers”. J. Opt. Soc. Am. B, 30, 1118 (2013) [5] G. Perram. SPIE Newsroom, 2012, 10.1117/ 2.1201211.004560 [6] B.V. Zhdanov, M.D. Rorondaro, M.K. Shaffer and R.J. Knize. “Efficient potassium diode pumped alkali laser operating in pulsed mode”. Opt. Exp., 22, 17266 (2014) [7] R.M. 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