Investigation of dual-wavelength pump schemes for optically pumped rare gas lasers.

Optically pumped rare gas lasers (OPRGLs) have shown great potential to generate high energy laser radiation with high beam quality. As an alternative to the diode-pumped alkali vapor lasers (DPALs), they have similar working principles and characteristics, but OPRGLs have the advantage that the gain medium is chemically inert and is appropriate for closed-cycle operation. One of the challenges OPRGLs are faced with is the bottleneck caused by the slow 1s4-1s5 collisional relaxations at room temperature. A 1s4-2p10 dual-wavelength pump method had been proposed to transfer the populations pooled on the 1s4 level to the lasing cycle using a steady-state laser model. We explored this method further through 1s4-2p8 and 1s4-2p7 dual-wavelength pump schemes. The enhancement efficiencies at room temperature for a repetitively pulsed discharge, CW dual-wavelength pump system were examined using a dynamic model, and an experiment with a pulsed secondary pump was conducted for qualitative evaluations.

Spectroscopic and theoretical studies of UN and UN.

The low-energy electronic states of UN and UN+ have been examined using high-level electronic structure calculations and two-color photoionization techniques. The experimental measurements provided an accurate ionization energy for UN (IE = 50 802 ± 5 cm-1). Spectra for UN+ yielded ro-vibrational constants and established that the ground state has the electronic angular momentum projection Ω = 4. Ab initio calculations were carried out using the spin-orbit state interacting approach with the complete active space second-order perturbation theory method. A series of correlation consistent basis sets were used in conjunction with small-core relativistic pseudopotentials on U to extrapolate to the complete basis set limits. The results for UN correctly obtained an Ω = 3.5 ground state and demonstrated a high density of configurationally related excited states with closely similar ro-vibrational constants. Similar results were obtained for UN+, with reduced complexity owing to the smaller number of outer-shell electrons. The calculated IE for UN was in excellent agreement with the measured value. Improved values for the dissociation energies of UN and UN+, as well as their heats of formation, were obtained using the Feller-Peterson-Dixon composite thermochemistry method, including corrections up through coupled cluster singles, doubles, triples and quadruples. An analysis of the ab initio results from the perspective of the ligand field theory shows that the patterns of electronic states for both UN and UN+ can be understood in terms of the underlying energy level structure of the atomic metal ion.

Transversely optically pumped Ar:He laser with a pulsed-periodic discharge.

Optically pumped rare gas lasers have the potential for scaling to high-power cw systems with good beam quality. Metastable atoms of heavier rare gases that are the lasing species are produced in an electric discharge at near atmospheric pressure. The key problem for this class of lasers at present is the development of a suitable discharge system. In this paper, we present the results of optimization of a pulsed discharge system with the goal of minimizing cathode sputtering and peak discharge current. The first demonstration of a transversely pumped system and measurements of the optical pumping threshold for the Ar:He laser are also presented.

O2(b1Σg+) Removal by H2, CO, N2O, CH4, and C2H4 in the 300-800 K Temperature Range.

Rate constants for the removal of O2 b1Σg+ by collisions with species relevant to combustion, H2, CO, N2O, CH4 and C2H4 have been measured in the temperature range 297-800 K. O2(b1Σg+) was produced from ground-state molecular oxygen by photoexcitation pulses from a tunable dye laser, and the deactivation kinetics were followed by observing the temporal behavior of the b1Σg+-X3Σg- fluorescence. The removal rate constants for H2, CO, N2O, CH4, and C2H4 could be represented by the modified Arrhenius expressions kH2 = (1.44 ± 0.02) × 10-16 T1.5 exp[(0 ± 10)/ T], kCO = (6.9 ± 0.4) × 10-24 T3 exp[(939 ± 33)/ T], kN2O = (2.63 ± 0.14) × 10-18 T1.5 exp[(590 ± 26)/ T], kCH4 = (3.5 ± 0.2) × 10-17 T1.5 exp[(-220 ± 24)/ T], and kC2H4 = (2.34 ± 0.10) × 10-20 T2.5 exp[(680 ± 16)/ T] cm3 molecule-1 s-1, respectively. All of the rate constants measured at room temperature were found to be in good agreement with previously reported values, whereas the values at elevated temperatures up to 800 K were systematically measured for the first time.

Demonstration of a CW diode-pumped Ar metastable laser operating at 4 W.

Optically pumped rare gas lasers are being investigated as potential high-energy, high beam quality systems. The lasing medium consists of rare gas atoms (Rg=Ne, Ar, Kr, or Xe) that have been electric discharge excited to the metastable np5(n+1)s P32 state. Following optical excitation, helium (He) at pressures of 200-1000 Torr is used as the energy transfer agent to create a population inversion. The primary technical difficulty for this scheme is the discharge production of sufficient Rg* metastables in the presence of >200 Torr of He. In this Letter, we describe a pulsed discharge that yields >1013 cm-3Ar* in the presence of He at total pressures up to 750 Torr. Using this discharge, a diode-pumped Ar* laser providing 4.1 W has been demonstrated.

O2(b1Σg+) Quenching by O2, CO2, H2O, and N2 at Temperatures of 300-800 K.

Rate constants for the removal of O2(b1Σg+) by collisions with O2, N2, CO2, and H2O have been determined over the temperature range from 297 to 800 K. O2(b1Σg+) was excited by pulses from a tunable dye laser, and the deactivation kinetics were followed by observing the temporal behavior of the b1Σg+-X3Σg- fluorescence. The removal rate constants for CO2, N2, and H2O were not strongly dependent on temperature and could be represented by the expressions kCO2 = (1.18 ± 0.05) × 10-17 × T1.5 × exp[Formula: see text], kN2 = (8 ± 0.3) × 10-20 × T1.5 × exp[Formula: see text], and kH2O = (1.27 ± 0.08) × 10-16 × T1.5 × exp[Formula: see text] cm3 molecule-1 s-1. Rate constants for O2(b1Σg+) removal by O2(X), being orders of magnitude lower, demonstrated a sharp increase with temperature, represented by the fitted expression kO2 = (7.4 ± 0.8) × 10-17 × T0.5 × exp[Formula: see text] cm3 molecule-1 s-1. All of the rate constants measured at room temperature were found to be in good agreement with previously reported values.

Removal of Rb(6(2)P) by H(2), CH(4), and C(2)H(6).

The saturated hydrocarbons methane and ethane are often used as collisional energy transfer agents in diode-pumped alkali vapor lasers (DPALs). Problems are encountered because the hydrocarbons eventually react with the optically pumped alkali atoms, resulting in the contamination of the gas lasing medium and damage of the gas cell windows. The reactions require excitation of the more highly excited states of the alkali atoms, which can be generated in DPAL systems by energy pooling processes. Knowledge of the production and loss rates for the higher excited states is needed for a quantitative understanding of the photochemistry. In the present study, we have used experimental and theoretical techniques to characterize the removal of Rb(6P2) by hydrogen, methane, and ethane.

Optically pumped microplasma rare gas laser.

The optically pumped rare-gas metastable laser is a chemically inert analogue to three-state optically pumped alkali laser systems. The concept requires efficient generation of electronically excited metastable atoms in a continuous-wave (CW) electric discharge in flowing gas mixtures near atmospheric pressure. We have observed CW optical gain and laser oscillation at 912.3 nm using a linear micro-discharge array to generate metastable Ar(4s, 1s(5)) atoms at atmospheric pressure. We observed the optical excitation of the 1s(5) → 2p(9) transition at 811.5 nm and the corresponding fluorescence, optical gain and laser oscillation on the 2p(10) ↔ 1s(5) transition at 912.3 nm, following 2p(9)→2p(10) collisional energy transfer. A steady-state kinetics model indicates efficient collisional coupling within the Ar(4s) manifold.

Electronic structure and spectra of the RbAr van der Waals system including spin-orbit interaction.

The potential energy curves and spectroscopic constants of the ground and excited states of the RbAr van der Waals system have been determined using a one-electron pseudopotential approach. This technique is used to replace the effect of the Rb(+) core and the electron-Ar interactions by effective potentials. The core-core interaction for Rb(+)Ar was incorporated using the accurate CCSD(T) potential of Hickling et al. [Hickling, H. L.; Viehland, L. A.; Shepherd, D. T.; Soldán, P.; Lee, E. P. F.; Wright, T. G. Phys. Chem. Chem. Phys. 2004, 6, 4233-4239]. This model reduces the number of active electrons of the RbAr van der Waals systems to just the single valence electron, permitting the use of very large basis sets for the Rb and Ar atoms. Using this approach, the potential energy curves of the ground and excited states dissociating into Rb(5s, 5p, 4d, 6s, 6p, 6d, and 7s) + Ar are calculated at the SCF level. Spin-orbit interaction was also considered within a semiempirical scheme for the states dissociating into Rb(5p) and Rb(6p). Spectroscopic constants are derived and compared with the available theoretical and experimental data. Such comparisons for RbAr show very good agreement for the ground and the first excited states. Furthermore, we have predicted the B(2)Σ(+)(1/2) ← X(2)Σ(+), A(2)Π(1/2) ← X(2)Σ(+), A(2)Π(3/2) ← X(2)Σ(+), A(2)Π(3/2) ← X(2)Σ(+), 5(2)Σ(+) ← X(2)Σ(+), 3(2)Π(1/2) ← X(2)Σ(+), and 3(2)Π(3/2) ← X(2)Σ(+) absorption spectra.