Research on chemical and discharge oxygen-iodine lasers

Novel methods and device configurations for singlet oxygen and atomic iodine generation were proposed and investigated for operation of the chemical or discharge oxygen-iodine lasers (COIL/DOIL). A chemical centrifugal spray generator of singlet oxygen was developed, based on the conventional chlorine-basic hydrogen peroxide chemistry. Results of theoretical and experimental investigation of the generator parameters are presented and compared with parameters of other generator types. A design of experimental device for singlet oxygen generation by means of the hybrid DC arc and RF plasma jet is presented. An alternative method of atomic iodine generation by a radiofrequency discharge decomposition of iodine compounds like CH₃I or CF₃I is described employing advanced experimental configuration. Some representative experimental results of this investigation are presented.     

Novel concept of electric discharge oxygen-iodine laser

A novel concept of discharge oxygen-iodine laser (DOIL) is presented. The supersonic DOIL includes a discharge singlet oxygen generator (DSOG) and discharge atomic iodine generator (DAIG). The operation of DSOG is based on a fast mixing of hybrid argon plasma jet of DC electric arc and RF discharge with a neutral molecular oxygen stream. The goal of our effort is achievement of DOIL oscillations by this new discharge technique, which should provide the singlet oxygen yields exceeding 30% at the total pressures higher than 10 torr. The DAIG operation is based on a cw/pulse RF discharge dissociation of iodine donors directly inside a laser iodine injector. This method substitutes the classic dissociation of molecular iodine by energy of singlet oxygen, which saves its energy for laser generation and so can increase the laser efficiency. The laser power could be thus enhanced by up to 25% if this method is employed in a chemical oxygen-iodine laser (COIL) operation, and even 3 times in DOIL without increase in the iodine laser pumping by singlet oxygen.     

Development of the Chemical Oxygen-Iodine Laser (COIL) with chemical generation of atomic iodine

This article addresses the development of a Chemical Oxygen-Iodine Laser (COIL) with alternative chemical ways of generating atomic iodine. Injection of atomic iodine as opposed to molecular iodine has the potential to improve the COIL efficiency. This paper describes two chemical methods for generating iodine atoms based on the gas phase reactions of hydrogen/deuterium iodide with fluorine or chlorine atoms, which are also produced chemically. Simplified one-dimensional gas dynamic modeling that describes the stream-wise profiles of species concentrations within both reaction systems is used to gain a theoretical understanding of both reaction systems under COIL conditions. The modeling results are used for the design of an experimental device and the interpretation of experimental data. The first experimental investigation studies the production of iodine atoms produced from reactions of Cl with HI. Atomic iodine yields of 70–100% in nitrogen are obtained, and the gain on the I(² P _1/2)–I(² P _3/2) transition in a flow of singlet oxygen is measured. Received: 7 October 2002 / Accepted: 8 February 2003 / Published online: 28 May 2003 RID="*" ID="*"Corresponding author. Fax: +420-2/8689-0527, E-mail: kodym@fzu.cz     

Advances in the Development of Chemical Oxygen-iodine Laser

Results of three problems investigated on a Chemical Oxygen-Iodine Laser (COIL) in our laboratory are presented in connection with the advanced COIL development in the world. These problems concern: i) A gain modulation on the laser transition in iodine atom, I(²P_1/2) - (²P_3/2), by external magnetic field, and its utilization for a COIL output power stabilization, ii) An evaluation of the Einstein A-coefficient of singlet oxygen, O₂(¹ _g), and its utilization in advanced diagnostics for O₂(¹ _g) determination in COIL operation, iii) A chemically driven iodine atom delivery system for advanced COIL.     

Efficient pulsed chemical oxygen-iodine laser with instantaneous generation of atomic iodine by volumetric discharge

A pulsed chemical oxygen-iodine laser (COIL) using atomic iodine generated by volumetric discharge of CH 3 I is developed and tested. COIL with a gain length of 60 cm is energized by a square pipe-array jet singlet oxygen generator with basic hydrogen peroxide pumping circulations and operated at subsonic gas flow. Maximum output energy of 4.3 J, pulse duration of 50 μs, specific energy extraction from the active medium of 2.0 J/L, and the maximum chemical efficiency of 12.5% are achieved at a chlorine flow rate of 55 mmole/s.     

喷射型单重态氧发生器性能研究

单重态氧发生器作为氧碘化学激光的核心部件,为化学激光器提供化学能。通过对工业喷射器及旋风分离器的研究,结合产生单重态氧的化学反应环境,进行了大量模拟及设计改进工作,研制了一种新型喷射型单重态氧发生器,并进行了相关实验研究。喷射型单重态氧发生器利用喷嘴能够产生比传统发生器类型更多的气液表面,获得足够的反应效率,可以大幅度降低发生器液体使用量,从而减小发生器辅助系统,提高体积效率。为满足O2（1）停留时间短及分离效率高的要求,利用气液两相喷射的高初速度以旋风分离器完成气液分离。新型发生器氯气利用率可达97%~99%,其O2（1）产率为40%~50%。     

Features of kinetic processes in the active medium of a pulsed chemical oxygen-iodine laser

Conclusion It can be concluded from our experiments and calculations that the product CF₃O₂ of the interaction between the CF₃ radical and the O₂ molecule quenches the oxygen O₂(¹) more strongly. At low chlorine admixture density in the singlet-oxygen stream this output energy of the oxygen-iodine laser with CF₃I as the atomic iodine donor is lower compared with CH₃I. The rate constant of quenching singlet oxygen by CF₃O₂ molecules is (3–5)·10^–11 cm³·sec^–1. It would be possible to decrease the influence of CF₃O₂ by adding to the initial O₂ ^*–O₂–CF₃I–Ar active mixture some other substance causing the CF₃ radicals to enter in a chemical reaction with a shorter characteristic time than that for CF₃O₂ formation. Of course, neither the initial substance nor the reaction products should quench O₂ ^* noticeably. This role can be possibly assumed by the NO molecule.The influence of the chlorine additive on the output energy of a laser with CH₃I and CF₃I differs greatly. The choice of the chlorine donor must therefore be determined by the amount of this additive. CH₃I is preferable if the chlorine is fully utilized in the singlet-oxygen laser, and CF₃I in the opposite case.Quantum Radiophysics Division, Lebdev Physics Institute. Translation of Preprint No. 21 of the Lebedev Physics Institute, Moscow, 1991.     

Experimental investigation of chemical oxygen-iodine laser

Results of an experimental investigation of a chemical oxygen-iodine laser (COIL) are presented. We determine the factors influencing the efficiency of a chemical singlet-oxygen generator (SOG) of the bubbler type operating on the chlorination of an alkaline solution of oxygen peroxide. We describe SOG constructions. A cw COIL with output power up to 400 W is developed on the basis of the investigated SOG. The feasibility of a modular construction of high-power COIL is demonstrated. A power-output level of 1 kW was achieved with a two-section laser. The feasibility is analyzed of COIL operation in a pulsed regime by pulsed bulk accrual of iodine atoms. We show that in this regime the laser can be operated without a low-temperature trap. An advantage of such a regime is also the possibility of controlling, in a wide range, the lasing pulse duration. A strong influence of molecular chlorine on the energy content of the active medium is observed when alkyliodides are used as iodine donors. The possibilities of using a pulsed COIL for controlled thermonuclear fusion are discussed. Translated from Trudy Fizicheskogo Instituta im. P. N. Lebedeva Akademiya Nauk SSSR, Vol. 194, pp. 114–147 (1989).     

在COIL中碘量变化与激光功率波形的关系

针对碘量在一定范围内变化对激光功率影响不敏感,采用碘量变化的方法,通过对大量的250mmol/s列管式射流氧发生器的出光实验的分析,得到了激光功率波形随碘量变化的实验规律.这一实验结果可用于根据功率波形变化来调节最佳碘量.并对其机理进行了理论分析.     

碘气流穿透深度和碘流量对COIL激光输出功率的影响

 通过采用Cl₂流量250mmol/s列管射流式氧发生器的COIL出光实验，得到了激光输出功率随碘副气流相对于氧主气流混合穿透深度的变化规律。实验结果表明，穿透深度对激光功率影响较大，存在最佳穿透深度，约为3.16mm,计算的最佳穿透深度与实验得到的最佳穿透深度基本一致。通过逐步改变供碘系统的碘气流流量，测量激光的输出功率，在实验上证实并找到了COIL的最佳碘流量值，约为4.5mmol/s，这一结果比以往文献所登载的最佳碘流量值要确切。     

Output power enhancement of all gas-phase iodine laser by?addition of hydrocarbon gases

In this work, we studied the output power enhancement of an all gas-phase iodine laser (AGIL) by the addition of hydrocarbon gases. Enhancement is expected because hydrocarbon gases might scavenge Cl atoms, which are strong quenchers of the upper state of the laser medium, I(² P _1/2). In AGILs, suppression of the Cl atom concentration is the key to improving the efficiency of the operation of the laser because Cl atoms are inherently generated by the self-annihilation of the energy donor, NCl(a¹ Δ). We found that the addition of CH₄ gave the best results, because of its high scavenging rate constant and inertness to I(² P _1/2). An enhancement of 10% was observed in the output power when CH₄ was added at a flow rate twice that of NCl₃. On the other hand, when C₂H₄ or C₂H₂ were added at the same flow rate as that of CH₄, the output power reduced despite their fast removal rate of Cl atoms. The reason for the reduced output power was that the unsaturated bonds scavenged not only the Cl atoms but also the H atoms, resulting in a low density of H atoms, and this decelerated the production of NCl(a¹ Δ). The observed laser characteristics could reasonably be explained by numerical model calculations. To our knowledge, this is the first report of successful output power enhancement of an AGIL using a chemical agent.     

Dissociation of molecular iodine in RF discharge for oxygen-iodine lasers

The dissociation of molecular iodine in 40 MHz-RF discharge was studied experimentally. This generation of atomic iodine is aimed at use in oxygen-iodine lasers. The discharge was ignited in a mixture of I₂ + buffer gas fast-flowing through the cylindrical chamber and the discharge products were injected into a supersonic flow of nitrogen. The atomic iodine number density was measured in a low-pressure cavity after mixing with nitrogen and the dissociation fraction was calculated related to the input I₂ flow rate. The dissociation fraction of 46.2% was achieved at 0.22 mmol/s of I₂ and 7 mmol/s of Ar and RF power of 500 W. Argon and helium were used as a buffer gas; discharge stability and dissociation efficiency were better with argon. At the I₂ flow rate corresponding to the operation of a 1 kW chemical oxygen-iodine laser, the dissociation fraction was about 20%. The dissociation efficiency (the fraction of absorbed energy used for the dissociation) significantly decreased with increasing in the specific energy. At a reasonable I₂ flow rate (0.32 mmol/s), the maximum achieved efficiency was 8.5% and the corresponding energy cost was 8.9 eV per dissociating of one I₂ molecule. The input energy of more than 3 kJ per 1 mmol of I₂ is needed for dissociating at least 50% of I₂. The obtained dependencies on the gas flow rates infer a good chance for scaling-up of the tested RF discharge generator for the intended application.     

氧碘化学激光器输出功率的估算

 建立了激光在工作时的动态模型，即假设在单位时间内，激光介质的粒子数全部被泵浦到上能级。引入激光介质重复泵浦次数的概念，根据能量守恒原理，通过分析氧碘化学激光器(COIL)的传能机理，计算了沿气流方向变化的碘原子上能级的弛豫时间及沿气流方向变化的碰撞传能时间，并且计算了碘原子在出光区内被单重态氧反复泵浦的次数及相应的残余单重态氧数目，从而计算出碘原子在出光区的反复泵浦次数，修正了原计算COIL输出功率的公式。理论计算与实验结果均表明：当碘流量过低时，增益小于损耗，激光器不能起振；当增大碘流量时，激光输出功率也逐步增大，反复泵浦次数逐渐减少；当碘流量继续增大时，激光输出功率达到最大，且在一定碘流量变化范围内基本保持稳定；但随着碘流量的进一步增大，激光输出功率却逐步下降。     

在COIL中碘量变化与激光功率波形的关系

 针对碘量在一定范围内变化对激光功率影响不敏感,采用碘量变化的方法,通过对大量的250mmol/s列管式射流氧发生器的出光实验的分析,得到了激光功率波形随碘量变化的实验规律。这一实验结果可用于根据功率波形变化来调节最佳碘量。并对其机理进行了理论分析。     

方列管型射流式O2（^1△）发生器的COIL出光研究

方列管型射流式O2(^1△)发生器是一种新型高效的氧碘化学激光器(COIL)化学能源供给装置。描述了采用该发生器在COIL上所做的一系列出光实验,这些实验着重于考察该发生器的性能参数及相应的COIL化学效率。结果在Cl2流量为0．25mol／s、无冷阱、稳定腔条件下获得化学效率高达26％。     

方列管型射流式O2(1Δ)发生器的COIL出光研究

 方列管型射流式O₂(¹Δ)发生器是一种新型高效的氧碘化学激光器(COIL)化学能源供给装置。描述了采用该发生器在COIL上所做的一系列出光实验,这些实验着重于考察该发生器的性能参数及相应的COIL化学效率。结果在Cl₂流量为0.25mol/s、无冷阱、稳定腔条件下获得化学效率高达26% 。     

High-pressure subsonic mode operation of chemical oxygen-iodine laser

A new regime of chemical oxygen-iodine laser (COIL), high-pressure subsonic mode operation, was demonstrated using a jet-type singlet oxygen generator (SOG). The laser output power of 342 W with chemical efficiency of 20.9% was obtained at the Cl₂ flow rate of 18 mmol/s and the operating pressure of 6.4 Torr in the laser cavity. The specific energy was 3.1 J/l which was four times higher than our supersonic device, and was comparable to the highest value for the supersonic regime. The experimental results were in good agreement with the numerical simulation results. Received: 26 February 1999 / Revised version: 13 July 1999 / Published online: 30 November 1999     

Effect of helium/argon gas ratio in a He-Ar-Cu<Superscript>+</Superscript> IR hollow-cathode discharge laser: modeling study and comparison with experiments

The He-Ar-Cu⁺ IR laser operates in a hollow-cathode discharge, typically in a mixture of helium with a few-% Ar. The population inversion of the Cu⁺ ion levels, responsible for laser action, is attributed to asymmetric charge transfer between He⁺ ions and sputtered Cu atoms. The Ar gas is added to promote sputtering of the Cu cathode. In this paper, a hybrid modeling network consisting of several different models for the various plasma species present in a He-Ar-Cu hollow-cathode discharge is applied to investigate the effect of Ar concentration in the gas mixture on the discharge behavior, and to find the optimum He/Ar gas ratio for laser operation. It is found that the densities of electrons, Ar⁺ ions, Ar_m ^* metastable atoms, sputtered Cu atoms and Cu⁺ ions increase upon the addition of more Ar gas, whereas the densities of He⁺ ions, He₂ ⁺ ions and He_m ^* metastable atoms drop considerably. The product of the calculated Cu atom and He⁺ ion densities, which determines the production rate of the upper laser levels, and hence probably also the laser output power, is found to reach a maximum around 1–5 % Ar addition. This calculation result is compared to experimental measurements, and reasonable agreement has been reached. Received: 14 October 2002 / Revised version: 28 November 2002 / Published online: 19 March 2003 RID="*" ID="*"Corresponding author. Fax: +32-3/820-23-76, E-mail: annemie.bogaerts@ua.ac.be     

Discharged generator of singlet oxygen for oxygen-iodine laser. Transport kinetics of O2(a 1δg) and O2(b 1σ g + ) molecules and O(3 P) atoms in Ar:O2 and He:O2 flows excited by a 13.56-MHz discharge

To understand and reveal the basic physical factors providing the possibility of scaling of a discharged singlet oxygen generator (DSOG) in an oxygen-iodine laser, the production, and transport kinetics of metastable O₂(a ¹δ_g) and O₂(b ¹σ _g ⁺ ) molecules, as well as O(³ P) atoms, were investigated in Ar:O₂ and He:O₂ gas flows excited by a 13.56-MHz discharge in a wide range of pressures (4–40 Torr) and oxygen percentages. It is shown that the densities and transport kinetics of O₂(a ¹δ_g), O₂(b ¹σ _g ⁺ ), and O(³ P) appear similar for oxygen mixtures with argon and helium in the same conditions independent of discharge mode. Compared to pure O₂, the dilution of oxygen with an inert gas allows higher energy inputs per an oxygen molecule to achieved, especially under conditions of the homogeneous discharge mode (α-mode), which gives a higher efficiency of O₂(a ¹δ_g) excitation in Ar:O₂ and He:O₂ mixtures. But the maximum attainable yield of singlet oxygen in Ar:O₂ and He:O₂ at fixed partial O₂ pressure is found to be comparable with the O₂(a ¹δ_g) yield in pure oxygen at the same pressure. The reason for this is the increased three-body deactivation of O₂(a ¹δ_g) by atomic oxygen in the mixtures because of the greater total pressure. The estimation of the rate constant of O₂(a ¹δ_g) three-body quenching by O(³ P) in Ar:O₂ and He:O₂ mixtures as (1.5 ± 0.5) × 10^?32 cm⁶/s was carried out from the analysis of transport kinetics of singlet and atomic oxygen in the discharge afterglow at high pressures exceeding ～10 Torr. A similar analysis for the lower pressures has revealed that losses both of metastable O₂(a ¹δ_g) and O₂(b ¹σ _g ⁺ ) molecules, and of O(³ P) atoms on the surface of the discharge tube, are determined by the density of each of the components. The obtained loss probabilities of O₂(a ¹δ_g), O₂(b ¹σ _g ⁺ ), and O(³ P) on the silica surface show that the surface loss probabilities of all the species can increase noticeably under the discharge exposure. Thus, the key parameters determining the maximal O₂(a ¹δ_g) yield in the DSOG are a homogeneous volumetric mode of the discharge, energy input per oxygen molecule in this mode, and a low rate of O₂(a ¹δ_g) quenching. Just three-body quenching of O₂(a ¹δ_g) by O(³ P) limits the singlet oxygen yield with increasing pressure. The fast removal of atomic oxygen both in discharge and in the earlier afterglow could provide DSOG scaling with pressure.     

Multiphoton ionization of iodine atoms and CF<Subscript> 3</Subscript>I molecules by XeCl laser radiation

We report about effective ionization of iodine atoms and CF₃I molecules under the action of intense XeCl laser radiation (308 nm). The only ion fragment resulting from the irradiation of the CF₃I molecules is the I⁺ ion. We have studied the influence of the intensity, spectral composition, and polarization of the laser radiation used on the intensity of the ion signal and the shape of its time-of-flight peak. Based on the analysis of the results obtained, we have suggested the mechanism of this effect. The conclusion drawn is that the ionization of the iodine atoms by the ordinary XeCl laser with a nonselective cavity results from a three- (2 + 1)-photon REMPI process. This process is in turn due to the presence of accidental two-photon resonances between various spectral components of the laser radiation and the corresponding intermediate excited states of the iodine atom. The probability of ionization of the atoms from their ground state I(²P_3/2) by the radiation of the ordinary XeCl laser is more than two orders of magnitude higher than the probability of their ionization from the metastable state I^*(²P_1/2). The ionization of the CF₃I molecules by the XeCl laser radiation occurs as a result of a four-photon process involving the preliminary one-photon dissociation of these molecules and the subsequent (2 + 1)-photon REMPI of the resultant neutral iodine atoms.