H2的振动及转动受激喇曼散射研究

本文研究了不同泵浦光偏振态及氢气气压时,氢的振动及转动受激喇曼散射的竞争效应.在5atm的氢喇曼池中,以波长为532nm的椭偏激光为泵浦源,当椭圆的压缩系数为tg26°～tg32°时,获得了60多条Q(1)和S(1)混合谱线.并在低压氢及线偏或准线偏光泵浦条件下,观察到迄今尚未见报道的受激R(1)喇曼谱线.     

LDS751染料的受激喇曼散射

报道了用532nm激光抽运LDS751染料产生720—780nm可调谐染料激光输出的同时,观察到喇曼频移为102和45cm-1的反斯托克斯线,前者谱线较强,后者较弱.与这两条强线对应的斯托克斯线未能观察到.另外,还观察到喇曼频移为34cm-1的一级和二级斯托克斯线与反斯托克斯线 关键词： LDS751染料 受激喇曼散射 喇曼位移 斯托克斯线 反斯托克斯线     

高压氢中的级联泵浦受激喇曼散射

利用XeCI准分子激光泵浦高压氢产生的受激喇曼散射(SRS)光,再次泵浦另一个长度较短的高压氢喇曼池,采用这种级联泵浦技术使高阶斯托克斯线强度增加。     

光纤中受激四光子混频和受激喇曼散射的联合效应

本文从掺杂多模石英光纤中同时记录到六对斯托克斯-反斯托克斯谱线,并在540—640nm的光谱范围内获得了受激四光子混频和受激喇曼散射联合产生的连续光谱带。在比较20m和200m光纤不同光谱特征的基础上,详细分析了受激四光子混频和受激喇曼散射谱线间的竞争和转化过程。 关键词：     

双折射光纤受激喇曼散射的研究

本文详细地研究了双折射光纤的受激喇曼散射.观测到9级斯托克斯受激喇曼谱.文中讨论和测试了阈值和频移与泵浦光偏振方向间的关系;当泵浦光偏振方向与光纤椭圆核的长轴或短轴平行时的传输损耗.并根据测得的阈值在理论上计算了各级斯托克斯线的喇曼增益系数.     

XeCl激光泵浦高压氢的衍射极限SRS斯托克斯光输出

利用XeCl准分子激光在高压氢中产生受激喇曼散射获得峰值功率为0.2MW、衍射极限发射角的一阶(353nm)斯托克斯输出,井研究了泵浦激光发散角对受激喇曼散射转换效率的影响.     

苯乙醇液芯光纤受激喇曼散射的红移和蓝移展宽

本文首次用调QYAG激光器的倍频光(λ=532.1nm)在苯乙醇液芯光纤中产生受激喇曼散射,观察到了4阶斯托克斯线和2阶反斯托克斯线.讨论了引起红移为主的斯托克斯线展宽的原因.     

光纤维中的喇曼混频

我们在656厘米^-1到1343厘米^-1的频率范围研究了光纤维的调谐喇曼混频(RM)效应。在实验中观察到下列现象:相干反斯托克斯喇曼散射(CARS)的大小与逆喇曼吸收(VRA)的大小成反比;RM对受激喇曼散射(SRS)的强度分布有强烈影响。除了观测到相干斯托克斯(CSRS)和CARS辐射,还观测到二级相干斯托克斯(SOCSRS)和相干反斯托克斯(SOCARS)辐射。对实验结果进行了讨论。 关键词：     

高阶相干喇曼散射光谱研究

本文报道了利用YAG激光系统CARS装置研究方解石的高阶相干喇曼散射(CRS)的实验结果,观察到1—6阶相干反斯托克斯喇曼散射谱(CARS)和1—2阶的相干斯托克斯喇曼散射谱(CSRS),讨论了影响高阶CRS产生的因素及有关的问题。 关键词：     

准分子激光束的喇曼整形

受激喇曼散射可以将紫外准分子激光辐射频移到特定的近紫外和可见光波长.采用喇曼整形技术还可以获得衍射极限发散角的斯托克斯输出.本文研究了注入光束质量对喇曼整形的影响,并求得不同氢压力下的喇曼增益系数和饱和参量.     

低温等离子体活化转化煤层甲烷机理的光谱诊断

为了探究低温等离子体活化转化煤层甲烷的机理,采用自制的介质阻挡放电实验系统对体积组成为CH440%、O212%、N248%的模拟煤层甲烷进行等离子体活化转化。采用色谱分析方法对煤层甲烷介质阻挡放电稳定产物进行分析,结果表明低温等离子体活化煤层甲烷的主要产物为CH3OH、CO和CO_2。采用发射光谱原位诊断技术在200~700 nm波长范围内研究了放电气体的发射光谱,检测到O·、CH·、C·、Hα、N2(A3Σ+U)等激发态物种。基于发射光谱原位诊断和气相色谱分析结果,对煤层甲烷活化转化的自由基反应过程进行了推断。同时,明晰了反应气中N2对煤层甲烷活化和主要产物的生成具有促进作用,即N2产生了存活时间更长的亚稳态离子,该亚稳态离子将能量传递给反应气中的O2和CH4,进而加速了煤层甲烷的活化和稳定产物的生成。     

双模式放电中DBD放电参数对甲烷滑动弧火焰光谱及活性粒子的影响分析

对未燃烧的可燃混合气体进行DBD放电,放电后会产生大量的活性粒子,这些活性粒子可以辅助气体燃烧,达到提高燃料燃烧利用率等目的。以DBD激励氩气、甲烷、空气产生的自由基（CH基和OH基）等强化燃烧的关键活性粒子为探索对象,研究DBD放电激励甲烷对滑动弧火焰的影响。为此,采用自主设计的DBD-滑动弧双模式等离子体激励器,利用同轴介质阻挡放电结构对氩气、甲烷、空气混合气进行放电激励,将激励后的氩气、甲烷、空气混合气通入滑动弧端进行点火。固定氩气流量不变,调整空气流量为4.76 L·min-1,并加入甲烷0.5 L·min-1,保证进气通道内氩气与空气-甲烷的气体体积流量比达到Ar∶（CH₄+Air）=1∶30,其中空气、甲烷这两种气体达到了化学燃烧当量比φ=1,氩气、甲烷、甲烷混合气体能实现均匀而稳定的放电并燃烧。DBD段放电电压在15～20 kV范围变化,放电频率在6～10 kHz范围变化,滑动弧段的电压和频率分别保持4 kV与10 kHz恒定,通过改变DBD段放电电压和放电频率,用高速光纤光谱仪检测滑动弧火焰中自由基种类及其光谱强度,分析放电参数激励甲烷对火焰中自由基（CH基和OH基）的影响。结果表明,DBD段放电电压及放电频率的增加可以促进火焰内部的偶联反应发生,可有效提升甲烷滑动弧火焰内部的活性粒子含量,其中OH基团、CH基团在燃烧链式化学反应进程中发挥着较为重要的作用。甲烷经过DBD激励后,随放电电压和频率的增加,火焰中OH基、CH基等主要活性粒子都随之增加。DBD放电后,活性粒子的光谱强度增大,特征谱线比单模式更加明显;甲烷经过DBD激励后,火焰组成发生了变化,滑动弧段出口处甲烷燃烧反应更加充分,火焰温度越高越容易产生OH基。与单模式滑动弧相比,双模式放电可有效促进火焰内部的链式化学反应进程,促进燃料燃烧。     

Modeling the properties of methane + ethane (Propane) binary hydrates,depending on the composition of gas phase state in equilibrium with hydrate

The properties of methane + ethane and methane + propane hydrates of cubic structures sI and sII are theoretically investigated. It is shown that the composition of the formed binary hydrate strongly depends on the percentage of a heavier guest in gas phase. For instance, for a 1% molar ethane concentration in gas phase, even at a low pressure, ethane occupies 60% large cavities in the hydrate sII, and as the pressure grows to 100 atm, it occupies 80% large cavities at a low temperature. The tendency remains the same at a temperature of higher than the ice melting point, but the methane concentration in the hydrate decreases to 30%. In the structure sI, the influence of the component composition of the gas mixture on that of the formed hydrate is less evident. However, in this case, calculation showed also that for a 1% molar ethane concentration in gas phase, ethane molecules occupy from 8 to 10% large hydrate cavities, depending on the pressure. This work is concerned with modeling phase transitions between cubic structures sI and sII of methane + ethane binary hydrates in view of incomplete occupation of cavities in the hydrate by guest molecules. For an ethane concentration under 2% in the gas mixture, the structure sII becomes more thermodynamically stable than the structure sI. However, as the ethane concentration grows to 20% in the equilibrium ice-gas-hydrate and to 40% in the equilibrium water-gas-hydrate, the structure sI becomes more thermodynamically stable. Hence, for low ethane concentrations in a gas mixture, the structure sI can be formed only as a metastable phase. Phase equilibria of methane hydrate sI and mixed methane + propane hydrate sII are considered, depending on the gas phase composition. Similar results are obtained for this equilibrium; this can evidence simultaneous formation of hydrates sI and sII at low propane concentrations.     

Investigation of flame structure and burning intensity of partially premixed methane enrichment of syngas using OH-PLIF and kinetic simulation

Various experiments were conducted to study the combustion characteristics of partially premixed methane enrichment of syngas by using the OH-PLIF technique. Experiments were conducted on a co-flow burner, and the methane concentration (X_CH4 = CH₄/(H₂+CO+CH₄)) was varied from 0 to 20%, the overall equivalence ratio was varied from 0.4 to 1.2 and the inner equivalence ratio was varied from 1.5 to 3.5. Kinetic simulation was conducted by using OPPDIF module of CHEMKIN-Pro software. Results show that an increase in X_CH4 and ?_overall weakens the OH signal intensity. Adding methane into the fuel greatly increases the height of the inner flame front, and the increase of methane concentration has a negative effect on flame propagation speed. Meanwhile, simulation results remain consistent with the experiments. The main OH radical production reaction changes from R46: H+HO₂ = 2OH to R38: H+O₂ = O+OH when methane concentration contained in the fuel mixture increases. Sensitivity analysis also indicates that reaction which plays a dominant effect on temperature changes with the increase of methane concentration.     

Direct calculation of bubble points for alkane mixtures by molecular simulation

This paper extends to flexible molecules an algorithm proposed earlier for the calculation of bubble points of simple fluids by Monte Carlo simulation (Ungerer, P., Boutin, A., and Fuchs, A. H., 1999, Molec. Phys., 97, 523). This algorithm is based on a pseudo-ensemble in which global volume, temperature and liquid phase mole numbers are fixed. A configurational bias method is used to treat flexible molecules, and the underlying assumptions regarding the molecular partition function for flexible chains are discussed. Molecular interactions are determined with an anisotropic united atoms intermolecular potential, recently optimized to represent vapour-liquid phase equilibria of n-alkanes. Two applications examples are given, concerning a binary mixture (methane + n-pentane) and a ternary system (methane + propane + n-decane) for which experimental data are available. Satisfactory convergence is obtained, except in the vicinity of critical conditions. Densities and vapour phase compositions are well represented. Bubble pressures appear significantly underestimated, however. The origin of this discrepancy and remedial methods are discussed.     

Influence of ethylene spectral lines on methane concentration measurements with a diode laser methane sensor in the 1.65 μm region

Spectra measurements around 1.65 μm have revealed that spectral lines of ethylene are present in this range along with methane spectral lines. Furthermore, the HITRAN database has no parameters of these ethylene lines. In particular, it was found that several ethylene absorption lines are located near the methane feature often used for quantitative spectroscopy (R3 triplet of the 2ν₃ band). Ethylene can be present together with methane in the samples under study, perturbing the recorded spectrum of CH₄. This perturbation by an interfering species can produce systematic errors in the derived CH₄ concentration. We have found in this work by numerical modelling that when measuring the methane concentration by a diode laser methane sensor operating in the 6046–6048 cm^-1 range, the systematic error on the retrieved CH₄ concentration decreases, as a rule, when decreasing the width of the fitted spectral window. At equal concentrations of ethylene and methane in the sample under study, the error on the concentration of CH₄ determined by the correlation technique can reach 15%. When using the technique based on the 2nd or 3rd derivative of the spectrum, interfering or impurity lines induce a systematic error on the derived CH₄ concentration, which is less than 2%. PACS 07.07.Df; 07.88.+y; 42.62.-b     

大气压非平衡等离子体甲烷干法重整零维数值模拟

大气压非平衡等离子体由于其独特的非平衡特性,可为甲烷和二氧化碳稳定温室气体分子活化和重整提供非热平衡和活化环境.本文采用了零维等离子体化学反应动力学模型,考虑了详细的CH₄/CO₂等离子体化学反应集,重点研究了反应气体CH₄/CO₂摩尔分数(5%—95%)对大气压非平衡等离子体甲烷干法重整制合成气和重要含氧化合物的影响.首先,给出了进料气体不同体积比时电子密度和温度随时间的演化规律,结果表明初始甲烷摩尔分数的提高有利于获得较高的电子密度和电子温度.随后,讨论了主要自由基和离子数密度在不同的甲烷摩尔分数下随着时间的变化规律,并给出了反应气体的转化率、合成气体和重要含氧化合物的选择性.此外,还明确了合成气和含氧化合物主要生成和损耗的化学反应路径,发现甲基和羟基是合成含氧化合物的关键中间体.最后,归纳总结给出了主要等离子体粒子之间的总体等离子体化学反应流程图.     

甲烷在多孔硅表面物理吸附特征研究

在密度泛函理论耦合超软贋势第一性原理的平台上,研究了甲烷在Si(111)表面的物理吸附特性。通过建立硅晶胞的不同吸附位置（top、bridge、fcc）模型,对比分析了甲烷在相应位置吸附界面变化的键结构、吸附能和态密度,获得了相应吸附点的吸附特征。对比分析的结果表明,甲烷只有在top位置物理吸附状态较为理想。分析态密度、键长及键角等数据揭示top位甲烷吸附对体系硅晶胞有很大的影响,其体系的键能最低,即此时体系结构最稳定。本文所得研究成果可用于Si表面对甲烷气体的敏感性分析及气体传感器领域。     

甲烷在多孔硅表面物理吸附特征研究(英文)

在密度泛函理论耦合超软贋势第一性原理的平台上,研究了甲烷在Si(111)表面的物理吸附特性.通过建立硅晶胞的不同吸附位置(top、bridge、fcc)模型,对比分析了甲烷在相应位置吸附界面变化的键结构、吸附能和态密度,获得了相应吸附点的吸附特征.对比分析的结果表明,甲烷只有在fcc位置物理吸附状态较为理想.分析态密度、键长及键角等数据揭示fcc位甲烷吸附对体系硅晶胞有很大的影响,其体系的键能最低,即此时体系结构最稳定.本文所得研究成果可用于Si表面对甲烷气体的敏感性分析及气体传感器领域.     

Collision parameters of N2-broadened methane lines in R5 multiplet of 2ν3 band. Multispectrum fitting of overlapping spectral lines

The results of the investigation of absorption spectra of the methane R5 multiplet of 2ν ₃ band, broadened by nitrogen, are presented. The absorption spectra of the methane-nitrogen mixture (CH₄:N₂ = 1:113.36) were recorded, using a two-channel photometric spectrometer, based on a tunable diode laser. The multispectrum least-squares fitting procedure was applied to all experimental spectra, recorded at different pressures, using the program, developed at IAO SB RAS (Protasevich, 2011). The program is based on a relatively simple line-profile model proposed in Pine (J. Quant. Spectrosc. Radiat. Transf. 57:145, 1997) and linear pressure dependence of the line-profile parameters. The line center positions, intensities, broadening, shifting, and mixing coefficients were determined for four lines of the methane R5 multiplet. The results have been compared with other available data.