喷嘴-平板直流电晕放电中的OH(A2S+→X2P, 0-0)光谱研究

 为更深入地认识电晕放电低温等离子体中自由基的生成机理，以发射光谱测量为基础并结合背景气体淬灭率影响，研究了常压下喷嘴-平板电晕自由基簇射过程中放电参数、背景气体、电极气成分等因素对OH(A²S⁺→X²p, 0-0)发光的影响。结果表明：在放电参数影响中，放电电压及放电电流都会影响OH生成量，OH发光随功率增加而大大增强；在加湿氮气直流电晕放电中有明显的OH(A²S⁺→X²p, 0-0)光谱存在，但加湿空气条件下OH生成较少；载气增湿后OH生成量明显增多，而Ar和O­2的存在分别增强和减弱了OH(A²S⁺→X²p, 0-0)发光，可能的原因是这两种物质影响了放电和OH(A²S⁺)的淬灭。     

UV spectral measurements at moderately high resolution and of OH resonance scattering resolved by polarization during the MANTRA 2002-2004 stratospheric balloon flights

A moderately high-resolution (<0.1 nm) grating spectrometer designed to measure the solar radiation in the spectral range 295-315 nm was flown on the MANTRA stratospheric balloon payloads of 2002 and 2004. The instrument measures both the direct sunlight and the radiation scattered by the atmosphere. The latter can be observed in two orthogonal polarization directions, at 90° from the solar azimuth and at several elevations above the horizon. As the OH molecule is the principal resonant scatterer in this spectral region, this permits the inference of both ozone and OH column amounts as well as limited profile information. This paper describes the instrument and its in-flight characterization, the basic data processing and the influence of several aspects of the flight profile. The direct sun measurements are analyzed both to characterize the spectrometer responsivity to scattered radiation and to estimate the ozone abundance at the flight altitude and above. An example of a high-resolution solar spectrum at 37 km altitude is presented and compared with others in the literature. The measured OH and Rayleigh-scattered spectra are used to derive OH radiation intensity measurements (the OH airglow), which are compared with others in the literature.     

中高层OH自由基在紫外波段的临边散射辐射正演模拟与敏感性分析

OH自由基是中高层大气中重要的氧化剂，决定着臭氧以及其他温室气体的浓度变化，甚至气候变化。为了实现中高层大气OH自由基的精细探测与精确反演，需要构造正演模型，模拟得到仪器接收到的大气中的A2Σ+-X2Π(0，0) 309 nm波段的太阳共振荧光发射信号。本文基于分子光谱能级跃迁理论计算得到OH(0,0)振动能级上的荧光发射率因子g，结合辐射传输模型SCIATRAN模拟出的太阳辐照度和观测视线路径上的OH柱量，模拟出OH荧光发射光谱，叠加上大气背景光谱并卷积仪器函数，最终模拟得到仪器接收的包含OH浓度信息的光谱。模拟结果与国外在轨仪器MAHRSI(Middle Atmosphere High-Resolution Spectrograph Investigation)，SHIMMER(Spatial Heterodyne Imager for Mesospheric Radicals)的在轨实测结果一致性较好。还分析了影响模拟结果的因素，在之后的正演过程中加以修正，使正演模型更接近实际辐射传输过程。     

Photoemission study of the modification of the electronic structure of transition-metal overlayers on TiO2 surfaces II. Cr on TiO2(0 0 1)

The electronic states of the Cr overlayers on TiO₂(0 0 1) surfaces have been investigated using angle-resolved and resonant photoemission spectroscopy with synchrotron radiation. At lower coverages, Cr deposition on TiO₂(0 0 1) creates two well separated in-gap emissions due to the formation of surface Ti³⁺ (3d¹) ions and Cr³⁺ (3d³) ions. At higher coverages, the in-gap emission is developed into the 2-peak-structure emission of Cr 3d character. The corresponding state is considered to be of metallic nature from the viewpoint of the high ability of oxygen adsorption, but has no Fermi edge, indicating a possibility of forming small Cr clusters on TiO₂(0 0 1) at this stage.     

Photoemission study of the modification of the electronic structure of transition-metal overlayers on TiO2 surfaces: I. Fe on TiO2(1 1 0)

The electronic states of the Fe overlayers on TiO₂(1 1 0) surfaces have been investigated using normal-emission and resonant photoelectron spectroscopy with synchrotron radiation. It was found that Fe grows in a Stranski-Krastanov mode. At low coverages, Fe deposition on TiO₂(1 1 0) is supposed to create surface Ti³⁺(3d¹) ions leading to the same in-gap emission as that is produced by surface oxygen vacancies of TiO₂. At high coverages, Fe-induced in-gap emission is evolved into a bulk Fe spectrum. However, at the beginning, a Fermi edge is not observed, indicating that the small Fe clusters of non-metallic nature are formed. A sharp Fermi edge is formed at higher coverages, indicating that the cluster becomes metallic as the size increases.     

CW and pulsed FIR-CO2 hybrid laser with improved efficiency and amplitude stability at short FIR wavelengths

For the first time stable cw output of a FIR-CO₂ hybrid laser has been achieved at wavelengths shorter than 300 m. Due to the saturable absorber characteristic of the FIR laser gas, cw or pulsed emission is observed on both, the CO₂ and the FIR laser output, depending on the operating conditions. Results are reported on different resonant lines in CH₃OH and the 67 m Raman line in NH₃. The good efficiency of this laser is also demonstrated by the excitation of two new emission lines in CH₃OH, namely 49 and 56 m, pumped by 9R(22) and 9R(24), respectively.On leave from the Institute of Physics, University of Beograd YU-11000, Beograd, Yugoslavia     

“Hot” bands of CO and the effect of vibration-rotation interaction on the solar CO spectrum

For the first overtone bands of CO, theoretical Herman-Wallis factors and experimental values show some inconsistencies for high excitation transitions. To resolve this problem, the relative band intensities, as well as the relative line intensities, are examined with CO lines in the solar infrared spectrum. The relative rotationless dipole-moment matrix elements and the Herman-Wallis factors for 2-0, 3-1, 4-2, 5-3 and 6-4 bands obtained from the solar CO spectrum are reasonably consistent with the theoretical predictions based on the dipole-moment function but disagree with results obtained in high-temperature emission measurements. It is shown that a reinterpretation of the high-temperature emission measurements is possible; the resulting Herman-Wallis factors become compatible with theoretical predictions as well as with the solar analysis.     

Thermal reactions of 2-iodoethanol on Cu(1 0 0)

Temperature-programmed reaction/desorption, X-ray photoelectron spectroscopy, and reflection-absorption infrared spectroscopy have been employed to investigate the reactions of ICH₂CH₂OH on Cu(1 0 0) under ultrahigh-vacuum conditions. ICH₂CH₂OH can dissociate on Cu(1 0 0) at 100 K, forming a -CH₂CH₂OH surface intermediate. Density functional theory calculations predict that the -CH₂CH₂OH is most probably adsorbed on atop site. -CH₂CH₂OH on Cu(1 0 0) further decomposes to yield C₂H₄ below 270 K. No evidence shows the formation of -CH₂CH₂O- intermediate in the reactions of ICH₂CH₂OH on Cu(1 0 0) in contrast to the decomposition of BrCH₂CH₂OH on Cu(1 0 0) and ICH₂CH₂OH on Ag(1 1 1) and Ag(1 1 0), exhibiting the effects of carbon-halogen bonds and metal surfaces.     

The interstellar methanol masers and their environments

To promote the understanding of massive star formation processes, we have studied the 6.6 GHz methanol (CH3OH) masers and their environments-- the dense cores and the outer regions of the molecular cloud. The physics of the CH3OH maser or the thermal emission formation region is studied by fitting the observational data of the 6.6 GHz 51-60 A+ and the 107 GHz 31-40 A+ CH3OH maser emission, using the radiative transfer calculations. The type II characteristics of the 6.6 GHz CH3OH maser are confirmed by the calculation results. A greater intensity of the radiation field leads to an increase in the peak intensity of the maser; however, high densities tend to turn off the maser. The calculation results show that to be a maser the 6.6 GHz CH3OH emission needs a radiation field of 150-300 K and a density not higher than 107cm-3, while the 107 GHz emission requires a radiation field of 210-300 K and a density not higher than 3×106 cm-3. The 6.6 GHz line is maser towards all six studied sources, while the 107 GHz line is maser towards Cep A only. Moreover, the former's intensity is much stronger than the latter. The radiative transfer calculations also indicate that the 6.6 GHz maser emission is so strong that the requirements of its formation (e.g. The radiation field, the density and the kinetic parameters) can only be satisfied at a certain stage of the processes of the massive star formation. Therefore it is often used as one of the most prominent tracers for the massive star formation regions. The calculation results of the simultaneous observations of (1,1) through (4,4) inversion lines of the ammonia (NH3) indicate that both the temperature and the density in the 6.6 GHz CH3OH maser formation regions are higher than that of the NH3 line formation regions. Furthermore, the common fact of |Vlsr(CO)| ＞ |Vlsr(NH3)| ＞ |Vlsr(CH3OH 6.6GHz maser)| in all six sources implies the ongoing developing trends of those gas flows driven by the masers.     

利用发射光谱研究脉冲电晕放电中的自由基

利用发射光谱技术在大气压下测量了以氮气为载气的不饱和水蒸气体系针-板式正脉冲电晕放电产生的OH(A^2∑→X^2Ⅱ0—O)自由基和O(3p^5P→3s^5S^02777．4nm),Ha(3P→2S 656．3nm)活性原子的发射光谱,并由N2(C^3Ⅱu→B^3Ⅱg)的△v=-3和△v=-4振动带序发射光谱强度计算得出N2(C,v)的相对振动布居及其振动温度,进而采用高斯分布拟合准确地求出了N2(C^3Ⅱu→B^3Ⅱg)的△v= 1振动带序发射光谱强度,从而可以由N2(C^3Ⅱu→B^3Ⅱg)的△v= 1振动带序与OH(A^2∑→X^2Ⅱ0—0)的重叠发射光谱中准确求出OH(A^2∑→X^2Ⅱ0—0)自由基的发射光谱强度。由发射光谱强度得到了激发态OH(A^3∑)自由基和O(3p^5P),Ha(3P)活性原子的布居。还研究了激发态OH(A^2∑)自由基和O(3p^5P),Ha(3P)活性原子的布居随放电电压和放电频率的变化以及氧气对激发态OH(A^2∑)自由基和O(3p^5P),Ha(3P)活性原子布居的影响。     

Acoustical phonon assisted two-photon excitation of excitonic molecules and resonant raman scattering in evaporated CuCl films

In evaporated CuCl films, Chase et al. have concluded the Bose-Einstein condensation of excitonic molecules for the origin of a sharp emission line which has been ascribed so far to the resonant Raman line in single crystals. A trace of the similar works on evaporated samples confirms that the sharp line shifts its energy with the change of the excitation photon energy; indicating the Raman character. When the excitation photon energy exceeds the resonant energy the Raman line shows broadening, and a new emission band appears which can be ascribed to the radiative annihilation of excitonic molecules generated by the two-photon absorption and one acoustical phonon emission.     

A twin optically-pumped far-infrared CH3OH laser for plasma diagnostics

A twin optically-pumped far-infrared CH₃OH laser has been constructed for use in plasma diagnostics. The antisymmetric doublet due to the Raman-type resonant two-photon transition is reproducibly observed at 118.8 m. With the 118.8-m line, it is obtained from the frequency separation of the anti-symmetric doublet that CH₃OH absorption line center is 16±1 MHz higher than the pump 9.7-m P(36) CO₂ laser line center. It is shown that the Raman-type resonant two-photon transition is useful in order to get several-MHz phase modulation for the far-infrared laser interferometer. Some preliminary performances of this twin laser for the modulated interferometer are described.This work was carried out under the collaborating research program at the Institute of Plasma Physics, Nagoya University, Nagoya 464, Japan.     

The origin of narrowing of the Si 2p coincidence photoelectron spectroscopy main line of Si(1 0 0) surface

The Si 2p photoelectron spectroscopy (PES) main line of Si(1 0 0) surface measured in coincidence with the singles (noncoincidence) Si L_2,3-VV Auger-electron spectroscopy (AES) elastic peak is calculated. The agreement with the experiment is good. The present work is the first many-body calculation of the experimental coincidence PES spectrum of solid surface. The narrowing of the coincidence Si 2p PES main line compared to the singles one is due to the mechanism inherent in the coincidence PES. The inherent mechanism is explained by a many-body theory by which photoemission and Auger-electron emission are treated on the same footing.     

Diagnosis of OH radical by optical emission spectroscopy in a wire-plate bi-directional pulsed corona discharge

The emission spectrum of the molecule OH (A²Σ→X²Π, 0–0) during a high-voltage, bi-directional pulsed corona discharge consisting of a gas mixture of N₂ and H₂O in a wire-plate reactor has been successfully recorded under severe electromagnetic interference at atmospheric pressure. The relative vibrational populations and the vibrational temperature of N₂ (C, v′) have also been determined. Due to the difficulty of determining the exact overlapping spectral line shape function of the OH (A²Σ→X²Π, 0–0) and the Δv=+1 vibrational transition band of N₂ (C³Π_u→B³Π_g), a practicable Gaussian form is used for calculating the emission intensity of OH (A²Σ→X²Π, 0-0) and the Δv=+1 vibrational transition band of N₂ (C³Π_u→B³Π_g). The emission intensity of OH (A²Σ→X²Π, 0–0) has been evaluated with a satisfactory accuracy by subtracting the emission intensity of the Δv=+1 vibrational transition band of N₂ (C³Π_u→B³Π_g) from the overlapping spectra. The relative population of OH (A²Σ) has been obtained by the emission intensity of OH (A²Σ→X²Π, 0–0) and Einstein's transition probability. The influences of peak voltage, pulse repetition rate and O₂ flow rate on the relative population of OH (A²Σ) radicals have also been investigated. We found that the relative population of OH (A²Σ) rises with an increase in both the peak applied voltage and the pulse repetition rate. When oxygen is added to an N₂ and H₂O gas mixture, the relative population of OH (A²Σ) radicals decreases exponentially with an increase in added oxygen. The main physicochemical processes involved are also discussed in this paper.     

High-temperature measurements of the rates of the reactions CH2O + Ar → Products and CH2O + O2 → Products

The two-channel thermal decomposition of formaldehyde [CH₂O], (1a) CH₂O + Ar → HCO + H + Ar, and (1b) CH₂O + Ar → H₂ + CO + Ar, was studied in shock tube experiments in the 2258-2687 K temperature range, at an average total pressure of 1.6 atm. OH radicals, generated on shock heating trioxane-O₂-Ar mixtures, were monitored behind the reflected shock front using narrow-linewidth laser absorption. 1,3,5 trioxane [C₃H₆O₃] was used as the CH₂O precursor in the current experiments. H-atoms formed upon CH₂O and HCO decomposition rapidly react with O₂ to produce OH via H + O₂ → O + OH. The recorded OH time-histories show dominant sensitivity to the formaldehyde decomposition pathways. The second-order reaction rate coefficients were inferred by matching measured and modeled OH profiles behind the reflected shock. Two-parameter fits for k_1a and k_1b, applicable in this temperature range, are:

     

Study of the 1s orthoexciton luminescence in Cu2O under two-photon excitation

We have studied the luminescence of 1s orthoexcitons in Cu₂O under both resonant and non-resonant two-photon excitation. The intensity of the luminescence was enhanced while resonantly exciting at the 1s or 2s orthoexciton levels. The direct and phonon-assisted emissions were observed over a wide range of temperatures (1.8-294 K) under two-photon resonant excitation. The phonon-assisted spectra can be well fit with a Maxwellian distribution with a fitting temperature close to the lattice temperature. The integrated intensity shows a minimum at 20 K and a maximum around 180 K. The existence of the direct emission feature enables us to deduce the temperature dependent bandgap and the orthoexciton line width directly up to relatively high temperatures. The red-shift of the orthoexciton energy and the increase of its line width as the temperature increases are interpreted as a temperature dependence of the real and imaginary parts of the exciton self energy.     

Si-based erbium-doped light-emitting devices

We report on the fabrication and performance of Si-based light sources. The devices consist of MOS structures with erbium (Er)-doped silicon rich oxide (SRO) film as gate dielectric. The devices exhibit electroluminescence (EL) at 1.54 μm at room temperature with a 0.2% external quantum efficiency. These devices show a high stability due to the silicon excess in the film. The Er-doped SRO films have been introduced in a Si/SiO₂ Fabry-Perot Microcavity in order to increase the spontaneous emission rate, the extraction efficiency and the spectral purity at the resonant wavelength. The active medium in the cavity has been electrically pumped and the conduction mechanisms have been analyzed. The EL spectra have also been acquired and compared with photoluminescence (PL) ones for the same resonant cavity light-emitting device (RCLED). The EL and PL peak intensities of the on-axis emission at the resonant wavelength are over 20 times above that of the similar Er-doped SRO film without a cavity. The Si-based RCLEDs exhibit different quality factors, ranging from 60 to 170. The spectra shape and intensity have been correlated with the quality factor. A high directionality of the emitted light, due to the presence of the resonant cavity, has also been observed: the overall luminescence is confined within 10° cone from the sample normal.     

Alternative mechanism for omega(0)/2 emission in laser-produced plasmas

Several models have been proposed to explain the broad spectral features characteristic of omega(0)/2 emission observed in laser-produced plasmas. In this article, the electromagnetic decay instability is examined as an alternative explanation for this emission. It is shown that the electromagnetic decay instability is able to explain some of the spectral features observed from laser-produced plasmas. In addition, the electromagnetic decay instability is consistent with two other features observed in experiments: the efficient generation of electromagnetic energy and the discrepancy in the levels of emission between the omega(0)/2 emission and the 3omega(0)/2 emission.     

A study of non-thermalized luminescence spectra: the case of Cu2O

The emission spectra of a non-thermalized distribution of excitons in Cu₂O have been studied experimentally and theoretically. The emission spectra were found to exhibit interesting dependence on both the excitation frequencies and on the sample temperatures. These experimental results are explained quantitatively by a simple model calculation of the exciton distribution in Cu₂O under continuous excitation. Using this model the exciton non-radiative lifetime was deduced from the emission spectra. In addition, the present theory accounts for the lineshape of the resonant Raman peaks in Cu₂O more satisfactorily than the existing theory.     

First-principles study of oxygenated diamond (0 0 1) surfaces with and without hydrogen

The structural characterization of oxygenated diamond (0 0 1) surface with and without H-presence has been investigated by the density-functional theory within the generalized gradient approximation and the plane-wave pseudopotential method. It is shown that, without the H, the O-bridge site has lower energy than the O-on-top site for both half and fully monolayer (ML) oxygen coverage. For hydrogenated diamond (0 0 1) surfaces, we found for half ML O coverage, a more stable (2 × 2):0.5H&0.5(OH) phase than the previously reported (2 × 1):0.5H&0.5(OH) phase [H. Tamura, H. Zhou, K. Sugisako, Y. Yokoi, S. Takami, M. Kubo, K. Teraishi, A. Miyamoto, A. Imamura, M.N. Gamo, T. Ando, Phys. Rev. B 61 (2000) 11025]. Furthermore, at one ML O coverage, a (2 × 2):(OH) phase is the most stable structure than the previously reported (2 × 1):(OH) phase. With the increase of the (OH) coverage, the importance of the hydrogen bonds increases in terms of stabilizing these structures.