基于OH自由基A2Σ + →X2Πr 电子带系发射光谱的温度测量技术

本文基于OH自由基所固有的分子结构特征,通过分子光谱理论系统地分析和计算了OH自由基A²Σ ⁺ →X²Π_r 电子带系发射光谱的谱线跃迁频率、能级分布以及爱因斯坦自发发射跃迁概率等重要参数.同时结合实际的光谱实验,分析了谱线的自然展宽、碰撞展宽、多普勒展宽以及仪器展宽等各种展宽因素对谱线线型的影响,从理论上计算了任意转动温度、振动温度以及谱线展宽条件下OH自由基A²Σ ^{关键词： 发射光谱 转动温度 振动温度 自发发射爱因斯坦跃迁概率}     

Electronic recoil effects in high-energy photoelectron spectroscopy

It is shown that the recoil energy imparted to the residual ion by the outgoing fast photoelectron leads to noticeable modifications of X-ray excited photoelectron spectra of molecules containing light atoms. The vibrational band envelopes may differ considerably from those predicted by the Franck-Condon principle. Al Kα excited valence electron bands are shown to exhibit, in addition to the translational recoil energy of the molecule, energy shifts of up to several tenth of an eV due to recoil-induced vibrational and rotational excitation. This effect has to be kept in mind when ionization potentials are determined from ESCA spectra. The recoil-induced vibrational and rotational excitation depends on the orbital quantum numbers of the ionized electron. Simple formulae for the shift of the centroid and the broadening of the band due to recoil effects are given for the special case of diatomic molecules.     

Spectroscopic observation of the rotational Doppler effect

We report on the first spectroscopic observation of the rotational Doppler shift associated with light beams carrying orbital angular momentum. The effect is evidenced as the broadening of a Hanle electromagnetically induced transparency coherence resonance on Rb vapor when the two incident Laguerre-Gaussian laser beams have opposite topological charges. The observations closely agree with theoretical predictions.     

Pressure broadening by argon in the hyperfine resolved P(10) and P(70) (17,1) transitions of I2 XΣ(0g)→BΠ(0u) using sub-Doppler laser saturation spectroscopy

The dependence of pressure broadening upon hyperfine component in the P(10) and P(70) lines of the (17,1) band of the I₂ X¹Σ(0_g⁺)→B³Π(0_u⁺) has been studied using laser saturation spectroscopy. By limiting absorption to the zero velocity group, Doppler broadening is removed, lineshapes with widths (FWHM) <9 MHz are detectable, and collision-induced broadening is measured at pressures of 0.2-1.2 Torr. The rates for broadening by argon are 8.3±0.3 and 10.7±0.4 MHz/Torr for the P(70) and P(10) lines, respectively. No significant variation in broadening rates is observed for the 15 hyperfine components of these even rotational lines. The effects of velocity cross-relaxation introduce a broad baseline into the spectra, which is strongly dependent on rotational state, pressure, and laser modulation frequency. The observed broadening rates correlate well with prior measurements and the polarizability of the collision partner.     

Terahertz laser velocity modulation spectroscopy of ions

Velocity modulation spectroscopy has been investigated in the terahertz region, employing pure rotational transitions of ArH⁺ and rotation-tunneling transitions of H₃O⁺ to study the competition between pressure broadening and Doppler broadening on the lineshapes, neutral suppression, and modulation efficiency. Velocity modulation is demonstrated to be effective to frequencies as low as 60 cm⁻¹, yielding S/N values for ArH⁺ (770/1) that surpass published terahertz FM results by an order of magnitude.     

Pressure Shifts and Pressure Broadening of the B and γ Bands of Oxygen

Measurements of pressure shift and pressure broadening in molecular oxygen have been made for rotational transitions in the B (1←0) and γ (2←0) vibrational bands of the b¹Σ⁺_g←X³Σ⁻_g visible electronic transition. The absorption features were measured simultaneously in two cells by photoacoustic spectroscopy using a scanning dye laser. The measurements were made with background gases of both pure oxygen and air at room temperature. The pressure shifts were all negative. The measurements show the magnitude of the pressure shift increasing with vibrational quantum number when compared with existing data for the A (0←0) band. The shifts also increase with rotational number within each vibrational band. The shifts in air are larger than in oxygen although the difference gets smaller with vibrational number. The average shifts in air for the A, B, and γ bands were 36, 11, and 0.2% higher, respectively, than in pure oxygen. The pressure broadening of the rotational lines does not change significantly with vibrational number and in general decreases with rotational number within a band. The pressure shift measurements were used by the high-resolution Doppler imager (on the Upper Atmospheric Research Satellite) to correct the Doppler wind measurements.     

吸收谱线Doppler展宽对原子多步光电离的影响

原子法激光同位素分离的核心之一是如何高效地将原子激发电离.本文从原子法激光同位素分离的实际情况出发,研究了原子吸收谱线的Doppler展宽对原子电离率的影响.研究中使用的理论工具是原子激发电离的密度矩阵方程,并利用数值计算方法对方程进行求解.研究结果表明:当吸收谱线有Doppler展宽时,在激光参数不变的条件下原子电离率会降低;且当激光功率固定时,存在使原子电离率为最大的线宽值.这与已发表文献中无Doppler展宽时的计算结果有很大不同.为了追求最佳的原子电离效果,在原子法激光同位素分离系统中激光应该尽可能地工作在最佳线宽条件下.如果激光线宽有不可控的随机波动,在技术上让激光线宽略大于最佳线宽更为有利.无论如何控制激光线宽,尽可能地降低原子吸收谱线的Doppler展宽都有利于原子电离率的提高.     

Sharing a Common Origin Between the Rotational and Linear Doppler Effects

The well‐known linear Doppler effect arises from the linear motion between source and observer, while the less well‐known rotational Doppler effect arises from the rotational motion. Here, we present both theories and experiments illustrating the relationship between the rotational and linear Doppler effects. A spiral phaseplate is used to generate a light beam carrying orbital angular momentum and the frequency shift is measured arising from its rotational and/or linear motion. By considering either the motion‐induced time‐evolving phase or the momentum and energy conservation in light‐matter interactions, we derive the rotational Doppler shift, linear Doppler shift, and overall Doppler shift associated with rotational and linear motions. We demonstrate the relationship between rotational and linear Doppler shifts, either of which can be derived from the other effect, thereby illustrating their shared origin. Moreover, the close relationship between rotational and linear Doppler effects is also deduced for a more general moving rough surface.     

The Ag M5N45N45 Auger photoelectron coincidence spectra of disordered Ag0.5Pd0.5 alloy

An effect of disorder broadening (DB) on the Ag M₅N₄₅N₄₅ Auger spectra in the random substituted Ag_0.5Pd_0.5 has been investigated by Auger photoelectron coincidence spectroscopy (APECS). Data were collected for the Ag M₅N₄₅N₄₅ Auger line coincident with the Ag 3d_5/2 photoelectron line (and its higher and lower binding energy sides). It is shown that the broadening of the Ag M₅N₄₅N₄₅ line is directly associated with the presence of disorder broadening of the Ag 3d_5/2 photoelectron line. The APECS experiment is used to demonstrate the broadening in a novel way.     

Revision on the calculation of optically pumped FIR laser spectrum with Doppler broadening and pressure broadening effects

By means of iteration method and also taking into account Doppler broadening and pressure braodening effect of IR pumping laser, the output power density of optically pumped NH₃ molecules FIR laser is calculated by solving density matrix equations of three-level system. The results of theoretical calculation shows that, in comparison with the FIR laser under the assumption of ideal monochromatic IR pumping, the output power density of FIR laser in the case of Doppler broadening and pressure broadening IR pumping decreases much more. Meanwhile, via the revision of Doppler broadening and pressure broadening effect, the theoretical value of optimum operating gas pressure reduces, which is in better agreement with the experimental value. Further study shows that the revision of Doppler broadening effect is more fit for the conventional FIR laser with a 2m sample tuble and the revision of pressure broadening effect is much more suitable for the miniature FIR laser with a short sample tube of 5 to 20cm in length.Supported by the National Natural Sciences Foundation of P.R.China and the NSF of Guangdong Province.     

Quantitative CARS spectroscopy of the ν1 band of water vapour

The accuracy of CARS thermometry for H₂O vapour has been assessed under carefully controlled conditions for the temperature range 295 to 900 K and the pressure range 0.0066 to 2.7 atm. Excellent agreement between theory and experiment was achieved for line-broadening regimes ranging from Doppler broadening to motional narrowing. Various models for rotational energy transfer and line-broadening were compared and where pressure broadening dominated, excellent agreement was achieved with a simple linewidth model, dependent only on temperature and pressure. Excellent agreement was also achieved using either energy or angular momentum based relaxation models to model motionally narrowed spectra in the pressure range up to 2.7 atm. However, good agreement between theory and experiment depended on the inclusion of state mixing correction factors, and good thermometry accuracy at high temperature was sensitive to the value assumed for the water molecular polarisability.     

光谱法测量等离子体离子温度和旋转速度

分析多普勒展宽和多普勒频移的区别，讨论了弦积分的线形分布和高斯分布的差异，利用光谱多道分析仪测量了碳227．1nm谱线的线形分布，通过选点拟合得出辐射粒子的离子温度和旋转速度径向分布。     

Research on speckle noise of laser Doppler velocimeter for the vehicle self-contained navigation

A novel multipoint layer-type laser Doppler velocimeter (MLLDV) is designed to measure the velocity of a vehicle for the self-contained navigation system. In order to investigate the speckle's influence on the Doppler spectrum, formulas of time-lagged covariance and speckle broadening were derived for our MLLDV. Simulations and experiments are made for detailed analysis. The results show that the time-lagged covariance of photocurrent is directly proportional to the incident angle, and is inversely proportional to the elevation fluctuation of the ground together with the velocity of the vehicle. Speckle broadening is a function of the vehicle's velocity, the 1/e² Gaussian spot radius and the phase correlation length of the ground. For our MLLDV, Doppler frequency and Doppler broadening are both directly proportional to the velocity of the vehicle. Besides, the ratio between Doppler broadening and the corresponding Doppler frequency is about 0.72% when the speed of the vehicle varies from 0 to 9.6 m/s.     

Annealing studies of Ti/Al multilayer film by slow positron beam

Single detector and coincidence Doppler broadening (CDB) spectroscopy measurements using slow positron beam were carried out to study as-deposited and annealed Ti/Al multilayer films. The changes of the film structure and defects in each layer by heat treatment have been investigated through the analysis of Doppler broadening lineshape variation. The coincidence Doppler broadening measurements revealed that Ti is the dominant diffusion species during the alloying process of Ti/Al by high temperature annealing. These results highlight the potential of slow positron beam in characterizing the vacancy-type defects evolution and mechanism of interlayer diffusion in Ti/Al multilayer film.     

Influence of Doppler-broadening on absorption-dispersion properties in a resonant coherent medium

We investigate the influence of Doppler broadening on absorption-dispersion properties in a four-level atomic system that can evolve from a normal dispersion to an anomalous dispersion. Our results show that the absorption-dispersion properties become strongly dependent on the propagation directions of the applied fields if Doppler broadening is taken into account. Especially, the switchover in the sign of the dispersion is still achievable even in the presence of Doppler broadening if properly arranging the propagation directions of the applied fields, which is in contrast with the otherwise behaviours in some other configurations.     

Phase modulation of propagation effect with Doppler broadening

This paper studies the propagation effect in a closed lambda-type three-level atomic system with Doppler broadening. It is shown that, Doppler broadening due to atomic motion and propagation effect associated with driving field depletion along the active medium decreases obviously the gain and output of the lasing without inversion （LWI）; the relative phase between the probe and driving fields has a remarkable modulation role to the propagation effect on LWI when Doppler broadening presents; by choosing suitable value of the relative phase, we can get the largest gain and output of LWI.     

Gain enhancing due to quantum interference effect in an open four-level atomic system with Doppler broadening

The effect of vacuum-induced coherence (VIC) on the gain of lasing without inversion (LWI) is studied in an open four-level atomic system with Doppler broadening for both cases: co- and counter-propagating probe and driving fields. The results show that: (1) in general, for a fixed VIC strength, LWI gain decreases monotonously with the value of the Doppler broadening width increasing. Regardless of the Doppler broadening being obvious or not, the LWI gain much larger than that without VIC always can be gotten by choosing suitable VIC strength, i.e. values of two factors p₁ and p₂ which represent the VIC effect. (2) Varying p₁ or p₂ will produce remarkable different influence on the LWI gain, and the influence is closely related to the value of the Doppler broadening width. (3) In the case of counter-propagating probe and driving fields, when the Doppler broadening is large enough, gain oscillation occurs. For the same value of the Doppler broadening width, the oscillation amplitude increases with increasing values of strength of VIC. (4) The atomic exit and injection rates also can dramatically affect LWI gain. (5) The LWI gain for the co-propagating probe and driving fields is always larger than that for the counter-propagating probe and driving fields. (6) A much larger LWI gain in open system than that in the corresponding closed system can be obtained.     

金属的正电子双多普勒展宽谱研究

研制了一套数字化的正电子湮没双多普勒展宽谱测量系统,用它测量了10个样品的双多普勒展宽谱,得到了一些有意义的结果.这些结果展示了一些金属单质材料的双多普勒展宽谱随着电子结构变化而发生的变化.本文简略介绍了双多普勒展宽谱仪,实验数据处理,以及这些金属单质材料的数据和分析结果.     

Steady-state formulation of optical bistability for a Doppler-broadened medium in a Fabry-Perot

A two-level model for absorptive and dispersive bistability in a Fabry-Perot is described. Doppler broadening and the effects of atomic motion through the standing wave field are included. Numerical results illustrating saturation of the Doppler line are presented and bistable transmission characteristics are obtained for systems with varying degrees of Doppler broadening.     

Collisional broadening of nitrous oxide transition lines in the ν1 + 2ν2 band by noble gases

A tunable diode laser is used to measure the foreign gas broadening for several rotational states in the R branch of the 12⁰0-00⁰0 vibration-rotation band of N₂O. The results indicate that rotational relaxation is the chief pressure broadening mechanism. The resulting cross sections for He and Ne turn out to be almost independent of the rotational quantum number. Ar and Kr, however, show a clear dependency. This seems to contradict the results of the infinite order sudden approximation.