基于发射光谱诊断的低温等离子体技术转化N2/NO气氛中NO的研究

建立了低温等离子体技术处理N₂/NO气氛中NO的实验系统,利用介质阻挡放电发射光谱诊断法分析了NTP技术处理NO的反应机理,以及研究了NTP系统的运行参数和N₂体积流量对NO转化率的影响规律。研究结果表明,随着V（_P-P）的增加,N₂发射光谱强度相对于NO发射光谱强度的比值增加,N₂第二正带系发射光谱强度增加,表明放电区间的高能电子浓度增大,有利于N₂离解成N原子,从而促使NO还原转化;增加N₂体积流量会使NO转化率降低,NO₂浓度升高。     

N2O Plasma表面处理对SiNx基IGZO-TFT性能的影响

采用N₂O plasma处理SiN_x薄膜作为绝缘层,以室温下沉积的铟镓锌氧化物(IGZO)作为有源层制备了 IGZO薄膜晶体管。与常规的IGZO-TFT相比,N₂O plasma处理过的IGZO-TFT的迁移率由原来的4.5 cm²·V^-1·s^-1增 加至8.1 cm²·V^-1·s^-1,阈值电压由原来的11.5 V减小至3.2 V,亚阈值摆由原来的1.25 V/decade减小至0.9 V/decade。采用C-V方法计算了两种器件的陷阱态,结果发现N₂O plasma处理过的IGZO-TFT的陷阱态明显小于普通的IGZO-TFT的陷阱态,表明N₂O plasma处理SiN_x绝缘层是一种改善IGZO-TFT器件性能的有效方法。     

N2微空心阴极放电特性及其阴极溅射的PIC/MC模拟

采用两维PIC/MCC模型模拟了氮气微空心阴极放电以及轰击离子 (N₂⁺,N⁺) 的钛阴极溅射. 主要计算了氮气微空心阴极放电离子 (N₂⁺,N⁺) 及溅射原子Ti的行为分布, 并研究了溅射Ti 原子的热化过程. 结果表明: 在模拟条件下, 空心阴极效应是负辉区叠加的电子震荡; 在对应条件下, 微空心较传统空心放电两种离子 (N₂⁺,N⁺) 密度均大两个量级, 两种离子的平均能量的分布及大小几乎相同; 在放电空间N⁺的密度约为N₂⁺的1/6, 最大能量约大2倍; 在不同参数 (P, T, V)下, 轰击阴极内表面的氮离子(N₂⁺,N⁺)的密度近似均匀, 其平均能量几乎相等; 从阴极溅射出的Ti原子的初始平均能量约6.8 eV, 离开阴极约0.15 mm处几乎完全被热化. 模拟结果为N₂微空心阴极放电等离子体特性的认识提供了参考依据. 关键词： 微空心阴极放电 PIC/MC模拟 2等离子体')" href="#">N₂等离子体     

控制双激光脉冲的宽度提高N2分子的取向

提出了通过控制双激光脉冲宽度的方法来提高N₂分子取向程度. 利用数值方法求解了N₂分子刚性转子模型在双激光脉冲作用下的薛定谔方程,计算了双原子分子N₂在总强度固定的两束激光脉冲作用下,不同脉冲宽度对于N₂分子取向的影响. 研究结果表明,通过调整两束激光脉冲的宽度,选择合适的延迟时间能够有效提高N₂分子的取向程度. 关键词： 双激光脉冲 分子取向 脉冲宽度     

等离子体增强化学气相沉积法制备立方氮化硼薄膜过程中的表面生长机理

利用感应耦合等离子体增强化学气相沉积法以Ar，He，N₂和B₂H₆为反应气体制备了高纯立方氮化硼薄膜.用四极质谱仪对等离子体状况进行了系统的分析，发现B₂H₆完全被电离而N₂只是部分被电离.H₂和过量的N₂在等离子体中生成大量中性的H原子和活化的N^*₂，它们与表面的相互作用严重地阻碍了立方 关键词： 立方氮化硼薄膜 等离子体 质谱     

C24N24负载Sc单原子催化剂催化甲烷氧化为甲醇的理论计算

甲醇是一种很有前途的清洁能源,有望替代不可再生的石油能源.因此,将储量巨大,但不易运输的甲烷氧化为甲醇具有十分重要的意义.首先通过密度泛函理论(density functional theory, DFT)计算研究了Sc原子与C₂₄N₂₄之间的稳定性.结果表明,Sc原子与C₂₄N₂₄的结合能(-9.064 eV)小于Sc原子的内聚能(-4.518 eV),即Sc@C₂₄N₂₄具有良好的稳定性.在此基础上,进一步研究了甲烷在Sc@C₂₄N₂₄表面催化氧化制备甲醇的工艺过程,以N₂O为氧化剂在Sc@C₂₄N₂₄单原子上进行甲醇的催化氧化反应.结果表明：N₂O首先吸附在Sc@C₂₄N₂₄上,然后直接分解为N₂和O_ads.N₂...     

均相条件下NO与CO、NCO的反应机理研究

基于量子化学密度泛函理论研究了NO与CO、NCO在均相条件下的反应机理并进行了动力学和平衡常数的分析. CO与NO的均相反应存在两条反应路径：两者首先反应形成中间体CNO₂,CNO₂不易稳定存在,其继续与CO、NO反应分别生成NCO、N₂O. NCO的生成速率大于N₂O,但两条反应路径的反应速率常数都很小.与已发现的反应路径相比,反应中间体CNO₂可以降低均相条件下CO与NO的反应能垒,分析发现CNO₂中的N原子是易发生反应的活性位点. NCO与NO的反应同样存在两条路径,优势反应路径随温度升高而改变,但非优势路径对反应的贡献不能忽略,分析平衡常数可知N₂的存在对反应影响可以忽略,因此燃烧环境中NCO与NO的反应既生成N₂O和CO,也生成N₂和CO₂.     

氮气射频放电与直流放电PIC/MC模拟的比较

建立氮气容性射频等离子体过程的PIC/MC模型,将模拟结果与直流放电进行比较.结果表明:射频等离子体粒子(e,N₂⁺,N⁺)的平均密度较直流放电约大-个量级,在射频电极附近粒子(e,N₂⁺,N⁺)的平均能量比直流放电阴极附近的能量低3倍左右;密度偏低的原子离子N⁺在两电极附近具较高的能量,能量较低的分子离子N₂⁺在放电空间具较高密度,N₂⁺的密度大约是N⁺的6倍;计算的电子能量几率分布与测量结果-致.     

N2在Cr(110)表面的强化学吸附与离解

用原子交叠和电子离域-分子轨道(ASED-MO)方法研究N₂在Cr(110)面的化学吸附过程。结果表明,N₂平行吸附于Cr(110)面的四度空位,N-N轴平行于[110]方向,与传统的σ施予和π弱反键作用不同,N₂在Cr(110)面平行吸附时,不仅3σ_g而且1π_μ分别向衬底施予0.97和0.54个电子,同时1π_g的反向键合增加到1.83个电子,这导致平行吸附比垂直吸附具有更低 关键词：     

飞秒激光在空气中成丝诱导氮荧光发射的空间分布

测量了线偏振飞秒激光脉冲在空气中成丝产生的氮荧光发射的空间分布.通过改变激光的偏振方向研究成丝过程中氮荧光发射的径向角分布,发现N₂⁺荧光发射在垂直于激光偏振方向上更强,而在平行于激光偏振方向上较弱;N₂荧光发射在所有方向上具有近乎相同的强度.原子和分子的激发、电离等动力学过程受激光强度的影响.在飞秒激光成丝过程中沿着激光传播方向,强度呈现先增强后减弱的分布,从而影响这些过程的产物的空间分布及其荧光发射的空间分布.沿着激光传播方向,发现N₂荧光先于N₂⁺荧光出现且在N₂⁺荧光消失之后消失.激光强度分布和激光偏振方向均会影响氮荧光的空间分布.基于实验分析,在短焦距情况下,系间窜越过程能很好的解释N₂(C³Π_u⁺)的形成,这项研究有助于理解飞秒激光成丝过程中氮荧光发射的产生机制.     

Field-induced ionization and Coulomb explosion of nitrogen

Femtosecond-laser field-induced ionization and Coulomb explosion of diatomic nitrogen were systematically investigated using time-of-flight mass and photoelectron spectrometry. Both linearly and circularly polarized femtosecond laser pulses were used at intensities varying from 5×10¹³ to 2×10¹⁵ W/cm². Strong N₂ ⁺, N₂ ²⁺, N⁺, N²⁺ and N³⁺ ion signals were observed for horizontally polarized pulses. Moreover, signals from the atomic ions exhibited a double-peak structure. Suppression of ionization was observed for circularly polarized pulses, while for vertically polarized pulses, only N₂ ⁺ and N₂ ²⁺ ions were observed. The angular distributions of the ions were measured under zero-field conditions in the ionization zone. The atomic ions N⁺, N²⁺ and N³⁺ exhibited highly anisotropic distributions, with maxima along the laser polarization vector and zeroes normal to the laser polarization vector. In contrast to the atomic ions, N₂ ⁺ exhibited a strong isotropic angular distribution. These observations indicate that dynamic alignment is responsible for the observed anisotropic angular distribution of the atomic ions. The kinetic energy spectrum of the photoelectrons is featureless and broad, extending above the ponderomotive potential of the laser pulse. The angular distribution is markedly anisotropic, with a maximum along the laser polarization vector. These observations further support the notion that the field-ionization mechanism is dominant under our experimental conditions. Received: 29 January 2002 / Revised version: 15 March 2002 / Published online: 12 July 2002     

New N2O laser band in the 10 μm wavelength region

Fifty new laser lines have been observed in continuous emission from an N₂O laser by placing a hot N₂O absorber cell inside the laser cavity to suppress the regular laser lines. The new lines are identified as rotation-vibration transitions of the (00⁰2–10⁰1) band of N₂O.     

Sensitive detection of methane and nitrous oxide isotopomers using a continuous wave quantum cascade laser

A continuous wave quantum cascade laser (QCL), operating near 8.1 μm, was used for wavelength modulation spectroscopy of methane (CH₄) and nitrous oxide (N₂O) stable isotopes. Several rotational transitions of ¹⁴N₂ ¹⁶O, ¹⁵N¹⁴N¹⁶O, ¹⁴N₂ ¹⁸O, ¹⁴N₂ ¹⁷O, ¹³CH₄ and ¹²CH₄ fundamental bands were detected. The noise-equivalent absorbance was measured to be less than 10^-5 in a 1-Hz bandwidth. A characterization of the laser source was also performed. The use of a QCL spectrometer for high-precision isotope ratio measurements is discussed. Received 14 March 2002     

Isotope-selective ionization utilizing molecular alignment and non-resonant multiphoton ionization

We demonstrate laser nitrogen isotope separation, which is based on field-free alignment and angular-dependent ionization of ¹⁴N₂ and ¹⁵N₂ isotopologues. A linearly polarized short laser pulse (???~?795?nm, ?????~?60?fs) creates rotational wave packets in the isotopologues, which periodically revive with different revival times as a result of different moments of inertia. Another linearly polarized short laser pulse (???~?795?nm, ?????~?60?fs) ionizes one of the isotopologues selectively as a result of their different angular distributions. In the present experiments, the ion yield ratio R [=I(¹⁵N₂ ⁺)/I(¹⁴N₂ ⁺)] can be changed in the range from 0.85 to 1.22, depending on the time delay between the two laser pulses.     

Measurement of far-infrared laser frequencies generated by optically pumped N 2 H4 and N2D4

A three-laser heterodyne system has been used to measure the frequencies of four previously observed far-infrared laser emissions generated by optically pumping either hydrazine (N₂H₄) or its fully deuterated isotope (N₂D₄) with a continuous-wave carbon dioxide laser. These newly measured frequencies have fractional uncertainties of ± 2 × 10⁻⁷ and correspond to laser wavelengths ranging from 63.9 to 158.4 μm. This work represents the first measurement of a N₂D₄ laser frequency.     

Infrared-microwave two-photon spectroscopy of the ν2 band of 14NH3

Transitions in the ν₂ band of ¹⁴NH₃ were recorded by means of an infrared laser microwave two-photon spectrometer. The spectrometer, which uses a minicomputer to step the microwave frequency and record the spectrum, is described. With sample cells outside the laser cavity good lineshapes are obtained, so that the accuracy of frequency measurement was limited by the resettability of the CO₂ or N₂O lasers employed, ～0.0002 cm^?1. The present data are compared to previously obtained results based on CO₂ or N₂O laser frequencies and to recently reported calculations. Rotational constants derived for the hypothetical inversion-free ground and v₂ = 1 states are reported.     

Heterodyne frequency measurements on N2O between 1257 and 1340 cm−1

Frequency measurements are given for the 00⁰1-00⁰0 and 01¹1-01¹0 bands of N₂O from 1257 to 1340 cm^?1. The measurements utilize heterodyne techniques by measuring small frequency differences between a tunable diode laser locked to the center of an N₂O absorption line and harmonic combinations of frequencies of radiation from two CO₂ Lamb-dip-stabilized lasers. The measurements are facilitated by the use of the CO laser as a transfer laser whose frequency is also measured. These measurements have been combined with other data to provide new band constants and frequency calibration tables for several band systems of N₂O in the following regions; 1215 to 1340, 1816 to 1930, and 2135 to 2268 cm^?1. A correction factor is also provided for existing calibration tables near 590 cm^?1.     

N2O emissions and source processes in snow-covered soils in the Swiss Alps

Nitrous oxide (N₂O) emissions from snow-covered soils represent a significant fraction of the annual flux from alpine, subalpine or cold-temperate regions. In winter 2010–2011, we investigated the temporal variability of N₂O emissions and source processes from a subalpine valley in the Swiss Alps. The study included regular measurements of N₂O snow profiles at a fixed location and an intensive sampling campaign along a transversal cut through the valley with grassland at the bottom and coniferous forest at the slopes. During the intensive campaign, recently developed laser spectroscopy was employed for high-precision N₂O isotopomer analysis. Maximum N₂O fluxes (0.77±0.64 nmol m^?2 h^?1) were found for periods with elevated air temperature and, in contrast to our expectations, were higher from forest than from grassland in mid-February. At maximum snow height (63 cm) the main N₂O source processes were heterotrophic denitrification and nitrifier denitrification. The reduction of N₂O by heterotrophic denitrifiers was much more pronounced for the grassland compared with the forest soil, as indicated by the ¹⁵N site preferences of 16.4±11.5 ‰ (grassland) and?1.6±2.1 ‰ (forest). This illustrates the potential of laser spectroscopic N₂O isotopomer analysis for the identification of source processes even at low emission rates in nutrient poor ecosystems.     

Laser on nitrogen-electronegative gas mixtures, pumped by inductive energy storage generator: Experiment and theoretical model

The advantages of inductive energy storage (IES) generators for increasing the pulse energy, power, and duration for nitrogen laser pumped by self-sustained transverse discharge have been experimentally demonstrated. A theoretical model is developed and the operation of IES-pumped laser on nitrogen-electronegative gas mixtures is numerically simulated. It is shown experimentally and theoretically that, adding electronegative gases, one can control the pulse shape of lasing on the C³II _u -B³II _g transition in nitrogen. The increase in the electric field strength in the laser gap in N₂-NF₃ and N₂-SF₆ mixtures produced 337.1-nm laser pulses consisting of two spaced peaks and 40–50-ns pulses close to rectangular. The increase in the laser active volume to 6 l (discharge cross section to 6×10 cm²) in N₂–SF₆ mixtures made it possible to obtain the maximum output energy (Q=110 mJ) and UV power (P _las =6 MW). In N₂-NF₃ mixtures, the laser pulse duration was up to ∼100 ns with an energy up to Q=30 mJ.     

A miniature tunable TEA CO<Subscript>2</Subscript> laser using isotope <Superscript>13</Superscript>C<Superscript>16</Superscript>O<Subscript>2</Subscript> and <Superscript>12</Superscript>C<Superscript>16</Superscript>O<Subscript>2</Subscript>

A miniature tunable TEA CO₂ laser using isotope ¹³C¹⁶O₂ as the active medium is developed to extend the spectral range of CO₂ lasers for further application. The optimization of the energy parameters of the tunable TEA ¹³C¹⁶O₂ laser and the same laser using ¹²C¹⁶O₂ are studied. When a gas mixture (¹³C¹⁶O₂: N₂: He = 1: 1: 3) at a total pressure of 6.4 × 10⁴ Pa is used, the TEA ¹³C¹⁶O₂ laser of a 45-cm³ active volume obtains 51 emission lines in the [00⁰1–10⁰0] and [00⁰1–02⁰0] bands. The maximum pulse energy of the TEA ¹³C¹⁶O₂ laser is about 357 mJ. The same laser using the conventional gas mixture (¹²C¹⁶O₂: N₂: He = 1: 1: 3) at a pressure of 6.66 × 10⁴ Pa is measured to obtain 69 laser emission lines and the maximum pulse energy of laser radiation is about 409 mJ.