烷烃类分子对NCO(A2∑+)自由基的猝灭

采用激光光解 激光诱导荧光 (LP LIF)的方法 ,用 2 6 6nm激光光解CHBr3 分子产生CH自由基 ,再与N2 O继续反应作为NCO自由基的产生源 ,用 4 38.6nm激光将电子基态X 2 Πi(0 0 10 )的NCO激励到激发态A2 Σ+ (0 0 0 0 )上 ,通过检测激发态NCO时间分辨荧光信号 ,测得室温 (2 98K)下NCO(A2Σ+ )被烷烃类分子猝灭的实验结果 ,获得了A 2Σ+ (0 0 0 0 )态猝灭速率常数 .实验发现 ,随着烷烃分子中C -H键数增加 ,其猝灭截面也近线性增加 ,但随着分子体积增大 ,这种增加趋缓 .     

光学泵浦的锂分子激光

以可见染料激光泵浦锂分子,在高于900℃的蒸气温度下,获得了由理分子A¹∑_u⁺态跃迁到基态X¹∑_g⁺的位于874—912nm区的许多光泵激光输出。谐振腔使输出信号增强约9倍。对部分激光跃迁的振转量子数作了标识。 关键词：     

草酰氯的激光诱导荧光激发谱

本文报道草酰氯C₂O₂Cl₂在358—372.5nm范围的激光诱导荧光(LIF)激发谱。对60多条振动谱带进行了归属,其中24条是吸收光谱中没有的。由振动结构得到C₂O₂Cl₂分子在X基态和?激发态的部分振动频率,其中v＂₇=84cm^-1和v＇₇=164cm^-1是新的数据。对4₀¹振动带的转动结构的分析给出转动常数A=0.190cm^-1,B=0.114cm^-1,C=0.048cm^-1。 关键词：     

乙醚团簇在纳秒激光场中的多价电离及其电子能量分布的研究

用5ns,1064nm的脉冲Nd:YAG激光,研究了乙醚团簇与纳秒激光的相互作用.在10¹¹ W/cm²量级光强下,观察到价电子完全剥离的O⁶⁺,C⁴⁺,且这些高价离子的强度比值基本不随激光能量而变化.用阻滞电压方法测量了电离过程中溢出电子能量分布,在最大激光能量4.0×10¹¹ W/cm²,溢出电子的平均能量为56eV,最大能量为102eV.实验结果支持了高价离子产生的“多 关键词： 高价离子 电子能量 纳秒激光 乙醚团簇     

OH自由基LIF光谱研究

利用脉冲高压直流放电技术产生H超声分子束,以纳秒染料激光二倍频输出(282 nm)作为激发光源,通过LIF光谱测量方法,获得了OH A 2Σ+-X 2Π(1, 0)带转动分辨激发荧光谱,并通过对谱线强度分布的分析和计算,得到X 2Π态H的转动温度为(30±1) K;通过对A 2Σ+-X 2Π (1, 1)带及(0, 0)带跃迁的荧光衰减时间谱测量,拟合得出H激发态 A 2Σ+ (ｖ′=1)及X 2Π (ｖ″=0)的寿命分别为(637±6)和(675±13) ns。     

氩气含量对介质阻挡放电中单丝等离子体温度的影响

在空气与氩气组成的混合气体放电中,首次研究了由中心点和外层晕组成的单丝。从照片中观察单丝结构,发现混合气体中氩气所占的比例越重,单丝的直径随之越小,同时中心点和外层晕的亮度有明显的差异,说明中心点和外层晕可能处于不同的等离子体状态。实验对单丝结构进行了光学时空分辨测量,研究了中心点和外层晕两层结构的微观特性。利用发射光谱法,详细地研究了该单丝结构的中心点和外层晕的等离子体参数随氩气含量的变化关系。实验根据氮分子第二正带系(C3Π_u→B3Π_g)谱线计算了中心点和外层晕的分子振动温度;通过氮分子离子N+₂(391.4 nm) 第一负带系谱线与氮分子N₂(394.1nm)谱线强度比,反映中心点和外层晕的电子平均能量随氩气含量的变化关系;利用氩原子763.2 nm(2P₆→1S₅)和772.077 nm(2P₂→1S₃)两条谱线的相对强度比法,估算了中心点和外层晕的电子激发温度。结果表明：中心点的光信号对应着第一个电流脉冲, 且其光信号较弱;而外层晕的光信号同时对应着第一个和第二个电流脉冲, 且其光信号较强。在相同的氩气含量条件下,外层晕比中心点的分子振动温度、电子平均能量以及电子激发温度均要高。随着氩气含量从30%逐渐增大到50%,中心点和外层晕的分子振动温度是逐渐减小的,而电子平均能量和电子激发温度均是逐渐增大的。     

激光辐照VO2薄膜温度场分布及透射特性研究

为了探究VO₂薄膜受激光辐照的温度场分布,以及1 064 nm激光直接辐照100 s内至相变的激光功率密度阈值,并比较近红外和中红外波段透过率调制特性差异。首先基于COMSOL建立了薄膜受激光辐照的模型并进行了温度场仿真,然后分别测试了薄膜正反面被不同功率密度的1 064 nm激光辐照100 s内激光透过率随时间响应特性。实验中的VO₂薄膜利用分子束外延法在Al₂O₃基底上制备得到。仿真结果表明,激光功率密度为25 W·mm^-2时,50 nm厚薄膜在被辐照1 ms时间内即达到相变温度。经激光辐照实验发现:50 nm厚的VO₂薄膜正反面受1 064 nm激光直接辐照100 s内至相变的功率密度阈值分别为4.1 W·mm^-2和5.39 W·mm^-2。30 nm厚VO₂薄膜对1 064 nmn激光的透过率调制深度约为13%,对3 459 nm激光透过率调制深度约62%,说明VO₂薄膜对近红外透过率调制特性不明显。     

一种新的芴类衍生物的三光子吸收诱导荧光和光限幅效应研究

通过对新合成的芴的一种具有对称性衍生物4-2-(7-(4-氨基苯乙烯基)-9，9-二(2-乙基己基)-9H-芴-2-)乙烯基)苯胺(BASF)的DMF溶液的研究，发现其具有很强三光子吸收频率上转换荧光发射特性，实验测出上转换荧光的波长范围是456—775nm，在510nm处的荧光强度与入射光强的三次方成正比.在0.03mol/L的浓度下就有明显的三光子吸收诱导的光限幅效应.非线性吸收系数和吸收截面分别为γ=4.34×10^-20cm³/W²和σ₃＝2.4×10^-39cm⁶/W². 关键词： 三光子吸收 光限幅 上转换荧光 吸收截面     

CO激光磁共振装置对NO2分子谱的观测

采用CO激光磁共振方法在1600cm^-1附近观测到了与Freund等人(1975年)不同的NO₂分子跃迁磁共振信号。讨论了实验方法和给出了实验结果。     

基于全息聚合物分散液晶的有机二维光子晶体激光器的研究

采用一次性曝光光路制备了基于全息聚合物分散液晶的亚微米周期染料掺杂二维光子晶体,晶格常数为582nm.选取4-(二氰亚甲基)-2-甲基-6-(4-二甲氨基苯乙烯基)-4H-吡喃作为激光染料,利用输出波长为532nm的Nd:YAG倍频脉冲激光器作为抽运光源对染料掺杂二维光子晶体进行抽运,得到了中心波长为627.4nm的窄线宽、低阈值的输出激光,激光线宽为0.4nm,阈值能量约为22.7 μJ.与目前国外的报道相比,激光线宽和阈值能量都有了很大幅度的降低.将其与基于一维光栅的分布反馈式激光器相比,线宽从1.4 关键词： 全息聚合物分散液晶 二维光子晶体激光器 带隙结构 阈值能量     

Quenching kinetics and small signal gain spectrum of the ZnI photodissociation laser

By photodissociation ZnI₂ with 193 nm (ArF) laser radiation, the rate constants for quenching of the upper and lower energy levels of the ZnI (B → X) laser by ZnI₂ have been measured to be (1.7 ± 0.2) × 10^-9 and (1.4 ± 0.4) × 10^-9 cm³ s^-1, respectively. Although the former rate constant was found to be laser intensity-dependent for I ? 10⁵ W cm^-2, the ZnI(B) state radiative lifetime was determined to be 26 ± 4 ns. Also, the small signal gain coefficient, g₀, of this molecular laser has a peak value of ? 15% cm^-1 at λ ? 602 nm and exceeds 5% cm^-1 for 591 nm ≤ λ ≤ 608 nm for a potential tuning range of at least 170 Å.     

Two Dimensional Rotational Temperature Measurement by Multiline Laser Induced Fluorescence of Nitric Oxide in Combustion Flame

Two-dimensional rotational temperature measurement was performed in a stable combustion flame of premixed butane and oxygen using multiline laser induced fluorescence (LIF) of nitric oxide molecules. Multiple rotational absorption lines of A²∑⁺Π;X²II(0,0) Q₁ and Q₂ lines were excited by laser light around 226 nm, and the LIF signal was observed by an image-intensified digital camera. Temperature was determined through least squares fitting correlation between LIF intensity and excitation rotational quantum number for the Boltzmann distribution function. The measured LIF intensity was approximated by the Boltzmann distribution with good accuracy, and the temperature obtained was between 500 K and 1800 K for the test flame. The measuring error of the temperature was evaluated and found to be 80 K, which corresponded to 8% of the measured fluorescence intensity. The two-line LIF scheme was evaluated by different pairs of excitation lines (Q₁(31.5)/Q₁(16.5) and Q₁(18.5)/Q₁(16.5)) for comparison with the multiline LIF approach. Temperature which was obtained by two-line LIF scheme corresponded well with multiline LIF results for Q₁(31.5)/Q₁(16.5) excitation. However, for Q₁(18.5)/Q₁(16.5) excitation, the obtained temperature did not agree with the multiline LIF result because the population of rotational states J=18.5 and J=16.5 is similar at high temperatures. We found that two-line LIF temperature measurement was reliable when excitation lines were suitably selected.     

Measurement of the absolute Raman scattering cross sections of sulfur and the standoff Raman detection of a 6‐mm‐thick sulfur specimen at 1500 m

The absolute Raman scattering cross sections (σ_RS) for the 471, 217, and 153 cm⁻¹ modes of sulfur were measured as 6.0 ± 1.2 × 10⁻²⁷, 7.7 ± 1.6 × 10⁻²⁷, and 1.2 ± 0.24 × 10⁻²⁶ cm² at 815, 799, and 794 nm, respectively, using a 785‐nm pump laser. The corresponding values of σ_RS at 1120, 1089, and 1081 nm were determined to be 1.5 ± 0.3 × 10⁻²⁷, 1.2 ± 0.24 × 10⁻²⁷, and 1.2 ± 0.24 × 10⁻²⁷ cm² using a 1064‐nm laser. A temperature‐controlled, small‐cavity (2.125 mm diameter) blackbody source was used to calibrate the signal output of the Raman spectrometers for these measurements. Standoff Raman detection of a 6‐mm‐thick sulfur specimen located at 1500 m from the pump laser and the Raman spectrometer was made using a 1.4‐W, CW, 785‐nm pump laser. Copyright © 2010 John Wiley & Sons, Ltd.     

Characterization of ammonia two-photon laser-induced fluorescence for gas-phase diagnostics

Two-photon laser-induced fluorescence (LIF) of ammonia (NH₃) with excitation of the C′-X transition at 304.8 nm and fluorescence detection in the 565 nm C′-A band has been investigated, targeting combustion diagnostics. The impact of laser irradiance, temperature, and pressure has been studied, and simulation of NH₃-spectra, fitted to experimental data, facilitated interpretation of the results. The LIF-signal showed quadratic dependence on laser irradiance up to 2 GW/cm². Stimulated emission, resulting in loss of excited molecules, is induced above 10 GW/cm², i.e., above irradiances attainable for LIF imaging. Maximum LIF-signal was obtained for excitation at the 304.8 nm bandhead; however, lower temperature sensitivity over the range 400–700 K can be obtained probing lines around 304.9 nm. A decrease in fluorescence signal was observed with pressure up to 5 bar absolute and attributed to collisional quenching. A detection limit of 800 ppm, at signal-to-noise ratio 1.5, was identified for single-shot LIF imaging over an area of centimeter scale, whereas for single-point measurements, the technique shows potential for sub-ppm detection. Moreover, high-quality NH₃-imaging has been achieved in laminar and turbulent premixed flames. Altogether, two-photon fluorescence provides a useful tool for imaging NH₃-detection in combustion diagnostics.     

Sub-Doppler laser absorption spectroscopy of the AΠi − XΣ (1, 0) band of CN: Measurement of the N hyperfine parameters in AΠ CN

Measurements of multiple rotational lines in the (1, 0) band of the A²Π_i − X²Σ⁺ “red” system of the cyanogen radical (CN) at sub-Doppler resolution are reported. The CN radical was produced by 193 nm photodissociation of NCCN (ethane dinitrile) and detected with a Ti:sapphire ring laser operating near 10 900 cm⁻¹. The sample was exposed to a weak, frequency-modulated probe beam and a strong, counterpropagating bleach laser beam. Demodulated probe laser signals display absorption and dispersion features derived from Doppler-free saturation of the hyperfine components as the laser scans across the central region of a Doppler-broadened rotational line spectrum. Hyperfine-resolved transition frequencies were combined with known ground-state X²Σ hyperfine term values to determine A²Π state hyperfine term values, which were analyzed in terms of an effective Hamiltonian for the A²Π state. All the expected hyperfine and ¹⁴N quadrupolar parameters were determined and their values analyzed in terms of a simple molecular orbital picture of the bonding in the radical. Higher sensitivity obtained with 400 kHz amplitude modulation of the bleach laser and additional phase-sensitive detection allowed hyperfine splittings in some rotational lines of ¹³C¹⁴N to be observed in natural abundance. Excited state hyperfine splittings were determined for a selection of rotational states, but not enough to determine the ¹³C hyperfine parameters.     

Toluene laser-induced fluorescence for in-cylinder temperature imaging in internal combustion engines

A single-laser single-camera imaging technique was demonstrated for in-cylinder temperature distribution measurements in a direct-injection internal combustion engine. The single excitation wavelength two-color detection technique is based on toluene laser-induced fluorescence (LIF). Toluene-LIF emission spectra show a red-shift with increasing temperature. Temperature can thus be determined from the ratio of the signal measured in two separate wavelength ranges independent of the local tracer concentration, laser pulse energy, and the intensity distribution. An image doubling and filtering system is used for the simultaneous imaging of two wavelength ranges of toluene LIF onto the chip of a single camera upon excitation at 248 nm. The measurements were performed in a spark-ignition engine with homogeneous charge and yielded temperature images with a single-shot precision of approximately ±?6%.     

Spatially resolved absolute concentration and fluorescence-lifetime determination of H2CO in atmospheric-pressure CH4/air flames

Using laser-induced fluorescence (LIF), spatially resolved concentration profiles of formaldehyde (H₂CO) were obtained in the preheating zone of atmospheric-pressure premixed CH₄/air flames stabilized on the central slot of a multiple-slot burner similar in construction to domestic boilers. The isolated pQ₁(6) rotational line (339.23 nm) in the 2¹ ₀4¹ ₀ vibronic combination transition in the ?¹A₂- ¹A₁ electronic band system around 339 nm was excited in the linear LIF intensity regime. For a quantification of quenching effects on the measured LIF signal intensities, relative fluorescence quantum yields were determined from direct fluorescence lifetime as a function of height above the slot exit. Absolute H₂CO number densities in the flames were evaluated from a calibration of measured LIF signal intensities versus those obtained in a low-pressure sample with a known H₂CO vapor pressure. Peak concentrations in the slightly lean and rich flames reached (994±298) and (174±52) ppm, respectively. Received: 25 September 2000 / Published online: 30 November 2000     

Examination of photoproducts in the ablation plume of doped PMMA

Optical emission and laser-induced fluorescence spectroscopies (OES and LIF) are employed to examine the plume ejected into vacuum upon UV pulsed laser ablation (248 nm, 20 ns, and 266 nm, 5 ns) of poly(methyl methacrylate) PMMA films doped with photostable compounds naphthalene (NapH) and phenanthrene (PhenH), and their photolabile iodide derivatives iodonaphthalene (NapI) and iodophenanthrene (PhenI). Spontaneous emissions observed in the irradiation of NapI and PhenI sensitised films can be assigned to excited products resulting from photodissociation of the dopants and to excited C₂, CH, and CN radicals. The presence in the plume of ground state products is revealed by LIF upon excitation at 266 nm. Measurements of the dependence of the spontaneous and LIF emissions on distance to the surface, ablation fluence, and flight velocities of species are discussed with reference to the mechanistic implications derived from the measurements. PACS 52.38.Mf; 61.82.Pv; 82.50     

Measurement of the absolute Raman scattering cross section of the 1584‐cm−1 band of benzenethiol and the surface‐enhanced Raman scattering cross section enhancement factor for femtosecond laser‐nanostructured substrates

The absolute Raman scattering cross section (σ_RS) for the 1584‐cm⁻¹ band of benzenethiol at 897 nm (1.383 eV) has been measured to be 8.9 ± 1.8 × 10⁻³⁰ cm² using a 785‐nm pump laser. A temperature‐controlled, small‐cavity blackbody source was used to calibrate the signal output of the Raman spectrometer. We also measured the absolute surface‐enhanced Raman scattering cross section (σ_SERS) of benzenethiol adsorbed onto a silver‐coated, femtosecond laser‐nanostructured substrate. Using the measured values of 8.9 ± 1.8 × 10⁻³⁰ and 6.6 ± 1.3 × 10⁻²⁴ cm² for σ_RS and σ_SERS respectively, we calculate an average cross‐section enhancement factor (EF) of 0.8 ± 0.3 × 10⁶. Copyright © 2009 John Wiley & Sons, Ltd.     

Fluorescence quantum yield of carbon dioxide for quantitative UV laser-induced fluorescence in high-pressure flames

The fluorescence quantum yield for ultraviolet laser-induced fluorescence of CO₂ is determined for selected excitation wavelengths in the range 215–250 nm. Wavelength-resolved laser-induced fluorescence (LIF) spectra of CO₂, NO, and O₂ are measured in the burned gases of a laminar CH₄/air flame (φ=0.9 and 1.1) at 20 bar with additional NO seeded into the flow. The fluorescence spectra are fit to determine the relative contribution of the three species to infer an estimate of fluorescence quantum yield for CO₂ that ranges from 2–8×10^?6 depending on temperature and excitation wavelength with an estimated uncertainty of ±0.5×10^?6. The CO₂ fluorescence signal increases linearly with gas pressure for flames with constant CO₂ mole fraction for the 10 to 60 bar range, indicating that collisional quenching is not an important contributor to the CO₂ fluorescence quantum yield. Spectral simulation calculations are used to choose two wavelengths for excitation of CO₂, 239.34 and 242.14 nm, which minimize interference from LIF of NO and O₂. Quantitative LIF images of CO₂ are demonstrated using these two excitation wavelengths and the measured fluorescence quantum yield.