氮直流辉光放电活性粒子（N^＋，N）的产生率

在氮直流辉光放电等离子体中采用快电子和离子(N2^ ，N^ )混合的蒙特卡罗模型，模拟研究了e N2→N^ /N N 2和N2^ N2→N^ N N2过程中粒子(N^ ，N)产生率的轴向分布随放电参数(工作气压、放电电压和温度)的变化规律。结果表明：两种离解过程中氮活性粒子(N^ ，N)的产生率都随气压和电压的增加而增大，随放电气体温度的升高而降低；但N2^ —H2离解碰撞主要发生在阴极附近。电压较高时，阴极处的离子N^ 主要由N2^ —N2离解过程产生；电压较低时，N2^ —N2离解过程可忽略。中性原子N主要由电子碰撞离解过程产生。     

N+2离子在氮直流辉光放电中碰撞离解的作用

采用氮辉光放电等离子体快电子和各种重粒子（N＋２，N＋，Nf）的混合Monte Carlo模型，从不同放电条件的离解碰撞率，快原子态粒子（N+，Nf）在阴极鞘层区的输运过程及轰击阴极的能量及角分布三个方面研究了 N＋２+N２→N+＋N+N2f反应在氮气直流辉光放电中的作用.该过程在电压较高时为阴极鞘层区的重要离解过程， 且主要发生在阴极附近，其碰撞率随电压和气压增加而增加；阴极表面附近的活性粒子（N＋，Nf）主要由该离解过程产生（而不是e--N2离解电离过程），而且这些粒子具有中等的平均能量且小角入射，是 关键词： 氮直流辉光放电 Monte Carlo模拟 N＋２-N２碰撞离解     

离子(N2+, N+)在氮辉光放电等离子体光辐射中的作用

采用氮辉光放电等离子体电子与重粒子综合的Monte Carlo模型,研究了离子(N2+,N+)与氮分子碰撞产生光辐射的强度分布及其 在氮辉光放电等离子体光辐射中的作用。两种离子产生的各种碰撞激发和辐射都分布在鞘层区内,光辐射强度向阴极方向逐渐 增加,且总强度随放电电压增加而增强。相对于电子产生的碰撞激发辐射,离子(N2+,N+)引起的辐射在阴极附近引起次最大 光强,且原子离子N+的作用较分子离子N2+大。当电压较低时,离子(N2+,N+)引起的辐射可以忽略。模拟结果很好解释了两 种典型的N2辉光放电光学发射谱的实验结果,为等离子体诊断研究中的光谱数据分析提供参考。     

宏观放电参数对快原子态氮(N+,Nf)的影响

采用氮直流辉光放电等离子体中快电子和重粒子(N₂⁺,N⁺,N_f)混合的蒙特卡罗方法,模拟研究了快原子态粒子(N⁺,N_f)的产生率及轰击阴极的能量分布随宏观放电参数(P,V)的变化规律.结果表明,存在一最佳放电条件,使阴极壁处粒子(N⁺,N_f)的粒子数密度大且能量高;当电压大于800V时,轰击阴极的活性粒子(N⁺,N_f),主要由N₂⁺-N₂离解过程产生,电压小于300V时,主要由e^--N₂离解过程产生,模拟结果与实验结果相符合.     

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采用蒙特卡罗模型对氮空心阴极放电等离子体鞘层离子(N2 、N )的输运过程进行了模拟研究,计算了阴极鞘层中氮离子(N2 、N )的能量及角分布的空间变化和粒子密度及平均能量随放电参数的变化规律。研究结果表明:空心阴极放电产生的氮离子,在鞘层输运过程中,N2 是密度几乎不变的低能粒子;N 是密度逐渐减少的高能粒子。随着电压增加,N 密度减小,平均能量增加;N2 密度和平均能量变化不明显。能量及入射角的相对分布规律与平板电极氮直流辉光放电基本类似,但圆筒空心阴极放电更有利于氮离子的产生。     

等离子体金属表面氮化中放电温度对氮原子态粒子的影响

采用快电子和重粒子(N₂⁺,N⁺,N_f)混合的Monte Carlo模型,研究了氮直流辉光放电等离子体金属表面氮化过程中.e-N_2s及N₂⁺-N_2s两种碰撞离解过程产生的原子态粒子(N⁺,N)的产生率和氮化粒子(N⁺,N_f)轰击靶表面的能量、粒子数密度及入射角分布随气体温度的变化规律.结果表明,使阴极靶处活性粒子(N⁺,N_f)的能量高且粒子数密度大,存在一个最佳放电温度;粒子(N⁺,N)的产生率及在靶表面的密度数都随着放电气体温度的升高而减少;有大量中性快原子N_f在工件表面小角入射,且粒子(N⁺,N_f)角分布受温度的影响很小.     

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N2-Ar射频放电等离子体广泛应用于微电子工业的刻蚀、氮化物薄膜的制备及金属表面氮化等技术领域。开发了N2-Ar混合气体容性耦合射频放电PIC/MC自洽模型,模型主要描述了e-,N2+,N+,Ar+等主要带电粒子的行为分布。等离子体的碰撞过程分别考虑了带电粒子(e-,N2+,N+,Ar+)与基态中性N2分子和Ar原子的21种碰撞反应过程。模拟结果表明,在纯N2及N2-Ar混合气体容性耦合射频放电中,各种带电粒子的数密度都在等离子体区达到最大值,且氮分子离子为主要粒子;在N2容性耦合射频放电中,加入10%氩气时,N+平均能量有所增加,在射频电极处两种氮离子(N2+,N+)高能粒子所占比例增加。本研究对认识N2-Ar射频放电等离子体过程微观机理具重要意义。     

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开发了氮空心阴极放电PIC/MC二维自洽模型。研究了N2传统空心阴极向微空心阴极放电转变过程中电势和电场的变化。结果表明,不同尺寸的空心阴极放电的电势及电场分布规律几乎类似,但空心阴极孔径减小且气压增加时,电场近似线性增加;典型微空心阴极电场比传统空心阴极放电电场约大3个量级;微空心阴极放电产生的电子,氮分子离子和氮原子离子的密度比传统空心阴极放电约大3个量级,且微空心阴极放电中,N2+密度比N+密度大8倍以上。     

N_2空心阴极放电向微空心阴极放电转变的PIC/MC模拟

开发了氮空心阴极放电PIC/MC二维自洽模型。研究了N2传统空心阴极向微空心阴极放电转变过程中电势和电场的变化。结果表明,不同尺寸的空心阴极放电的电势及电场分布规律几乎类似,但空心阴极孔径减小且气压增加时,电场近似线性增加;典型微空心阴极电场比传统空心阴极放电电场约大3个量级;微空心阴极放电产生的电子,氮分子离子和氮原子离子的密度比传统空心阴极放电约大3个量级,且微空心阴极放电中,N2+密度比N+密度大8倍以上。     

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开发了氢气甚高频(60MHz)容性耦合放电的PIC/MC模型.在模型中考虑了带电粒子(e,H+,H2+,H3+)与H2的21种碰撞反应过程,模拟了氢气甚高频放电射频电场和电势分布以及电子和氢离子(H+,H2+,H3+)粒子密度和平均能量分布,并与频率为13.56MHz的放电结果进行了比较.结果表明,相对于频率13.56MHz的放电,氢气甚高频放电等离子体电势增高,导致两电极附近的电场增强;另外,两鞘层厚度变窄并且电子和H3+离子平均能量减小,其总密度却增加.H3+离子为氢气甚高频放电空间的主要离子,H2+离子密度比H3+离子小约2～3个数量级.     

双波长法快速测定饮用水中的硝酸盐氮和亚硝酸盐氮

针对快速性要求较高的场合,提出基于双波长法测定硝酸盐氮和亚硝酸盐氮含量的方法,该法首先测定混合溶液在203、216、220nm处的吸光度值,其次计算216nm与203nm处的吸光度差值,通过差值的线性回归方程计算出硝酸盐氮的浓度,再通过亚硝酸盐溶液的校准曲线计算亚硝酸盐氮的含量。通过实验和分析计算,可知此法原理简单,使用方便,精密度和准确度较高,而且在没有分光光度计的情况下也能使用,大大提高了分析效率,适合用在快速估算硝酸盐氮和亚硝酸盐氮含量的场合。     

Preparation of graphitic carbon nitride with large specific surface area and outstanding N2 photofixation ability via a dissolve-regrowth process

Nitrogen fixation is the second most important chemical process in nature next to photosynthesis. Here, we report a convenient dissolve-regrowth method for synthesizing graphitic carbon nitride (g-C₃N₄) with a large surface area and nitrogen vacancies by HCl treatment. XRD, N₂adsorption, SEM, TEM, UV–Vis spectroscopy, EPR, N₂-TPD, Photoluminescence and Photocurrent were used to characterize the prepared catalysts. The results indicate that HCl treatment does not influence the crystal phase of g-C₃N₄ but change the morphology and optical property, leading to the smaller particle size, larger surface area and increased bang gap energy. It is deduced by N₂-TPD, Photoluminescence, Photocurrent and DFT simulations that the nitrogen vacancies formed by the HCl treatment not only serve as active sites to adsorb and activate N₂ molecules but also promote interfacial charge transfer from g-C₃N₄to N₂ molecules. The HCl treated g-C₃N₄ catalyst exhibits outstanding nitrogen photofixation ability under visible light, which is 13.4-fold higher than that of bulk g-C₃N₄ without nitrogen vacancy. The possible reaction mechanism is proposed.     

Using the natural 15N abundance to assess the main nitrogen inputs into the sand dune area of the North-Western Negev desert (ISRAEL)

The variation of the natural ¹⁵N abundance is often used to evaluate the origin of nitrogen or the pathways of N input into ecosystems. We tried to use this approach to assess the main input pathways of nitrogen into the sand dune area of the north-western Negev Desert (Israel). The following two pathways are the main sources for nitrogen input into the system:

1. Biological fixation of atmospheric nitrogen by cyanobacteria present in biological crusts and by N₂-fixing vascular plants (e.g. the shrub Retama raetam);

2. Atmospheric input of nitrogen by wet deposition with rainfall, dry deposition of dust containing N compounds, and gaseous deposition.

Samples were taken from selected environmental compartments such as biological crusts, sand underneath these crusts (down to a depth of 90?cm), N₂-fixing and non-N₂-fixing plants, atmospheric bulk deposition as well as soil from arable land north of the sandy area in three field campaigns in March 1998, 1999 and 2000. The δ¹⁵N values measured were in the following ranges: grass ?2.5‰ to +1.5‰; R. reatam: +0.5‰ to +4.5‰; non-N₂-fixing shrubs +1‰ to +7‰; sand beneath the biological crusts +4‰ to +20‰ (soil depth 2–90?cm); and arable land to the north up to 10‰. Thus, the natural ¹⁵N abundance of the different N pools varies significantly. Accordingly, it should be feasible to assess different input pathways from the various ¹⁵N abundances of nitrogen. For example, the biological N fixation rates of the Fabaceae shrub R. reatam from the ¹⁵N abundances measured were calculated to be 46–86% of biomass N derived from the atmosphere. The biological crusts themselves generally show slight negative ¹⁵N values (?3‰ to ?0.5‰), which can be explained by biological N fixation. However, areas with a high share of lichens, which are unable to fix atmospheric nitrogen, show very negative values down to ?10‰. The atmospheric N bulk deposition, which amounts to 1.9–3.8?kg?N/ha?yr, has a ¹⁵N abundance between 4.4‰ and 11.6‰ and is likely to be caused by dust from the arable land to the north. Thus, it cannot be responsible for the very negative values of lichens measured either. There must be an additional N input from the atmosphere with negative δ¹⁵N values, e.g. gaseous N forms (NO _x , NH₃). To explain these conflicting findings, detailed information is still needed on the wet, particulate and gaseous atmospheric deposition of nitrogen.     

Enhancement of the molecular nitrogen dissociation and ionization levels by argon mixture in flue nitrogen plasma

In this work, the nitrogen molecular dissociation and ionization levels in Ar/N₂ flue plasma are evaluated as functions of plasma parameters such as Ar mixture quantity and N₂ flux in order to obtain the best condition for various applications such as thin film deposition and material surface modification. This plasma is operated at 10 kV and the nitrogen dissociation rate is determined by analyzing the optical emission of the nitrogen band. For different operating conditions, the dissociation rate [N] of N₂ molecules was enhanced, as the mixture quantity of Ar increased from 0.06 m³/h to 0.9 m³/h and the max of enhancement factor is 4.3. This factor becomes bigger when the N₂ flux becomes bigger. Moreover, the molecular nitrogen ionization density is calculated from the current intensity of the plasma. The ionization density was also enhanced, as the mixture quantity of Ar increased from 0.1 m³/h to 1.5 m³/h, under three different voltages. The max of enhancement factor of 1.96 is much smaller than the factor of the dissociation rate. These results are discussed in terms of the kinetics of the electrons, nitrogen ions, atoms and molecules.     

Raman Spectroscopy of Nitrogen Clathrate Hydrates

在253 K和16 MPa的压力下,于实验室内合成了氮气水合物,用显微共焦拉曼光谱对其N-N和O-H键伸缩振动的光谱特征进行了研究．结果表明,氮气水合物中的N-N和O-H键的拉曼峰分别为2322.4和3092.1 cm^-1,与天然的空气水合物中的数据十分接近．另外,还测定了液氮和溶解于水中的氮分子中N-N键的拉曼峰值,分别为2326.6和2325.0 cm^-1．氮气笼型水合物分解的拉曼谱图表明,氮分子同时进入水合物的大笼和小笼中,但由于氮分子在大、小笼中的环境氛围十分接近,其拉曼位移相差不大,故拉曼谱图只能显示N-N键伸缩振动一个峰．     

Adsorption of N2 and N2O on Ni(7 5 5) surface: ab initio periodic density functional study

Adsorption of N₂ and N₂O at various sites on Ni(7 5 5) has been investigated by density functional theory (DFT) method (periodic DMol³). Several possible adsorption structures (attaching the nitrogen atom to the surface, or lying parallel) are found for both molecules. There is a clear binding energy preference of N₂ and N₂O for step sites in contrast to the case of CO. It is revealed that the decomposition of N₂O occurs exclusively near the step, but not on the terrace. Two decomposition channels can be considered; dissociative adsorption and spontaneous decomposition during TPD ramp. Three possible candidates for the precursor of the spontaneous decomposition of N₂O during TPD ramp are discussed.     

Nutrient cycling responses to fire frequency in the Kruger National Park (South Africa) as indicated by Stable Isotope analysis

Fires, which are an intrinsic feature of southern African ecosystems, produce biogenic and pyrogenic losses of nitrogen (N) from plants and soils. Because of the long history of fires in these savannas, it was hypothesized that N 2 fixation by legumes balances the N losses caused by fires. In this study, the N 2 fixation activity of woody legumes was estimated by analyzing foliar i 15 N and proportional basal area of N 2 fixing species along experimental fire gradients in the Kruger National Park (South Africa). In addition, soil carbon (C) and N pools, foliar phosphorus (P) and gross N mineralization and nitrification rates were measured, to indicate the effects of fires on nutrient stocks and the possible N cycling processes modified by fires. Although observations of increased soil C/N and mineralization rates in frequently burned plots support previous reports of N losses caused by fires, soil %N did not decrease with increasing fire frequency (except in 1 plot), suggesting that N losses are replenished in burned areas. However, relative abundance and N 2 fixation of woody legumes decreased with fire frequency in two of the three fire gradients analyzed, suggesting that woody legume N 2 fixation is not the mechanism that balances N losses. The relatively constant %N along fire gradients suggests that these ecosystems have other mechanisms to balance the N lost by fires, which could include inputs by atmospheric deposition and N 2 fixation by forbs, grasses and soil cyanobacteria. Soil isotopic signatures have been previously used to infer patterns of fire history. However, the lack of a relationship between soil i 15 N and fire frequency found in this study indicates that the effects of fires on ecosystem i 15 N are unpredictable. Similar soil i 15 N along fire gradients may reflect the contrasting effects of increased N gaseous emissions (which increases i 15 N) and N 2 fixation other than that associated with woody legumes (which lowers i 15 N) on isotopic signatures.     

A new software suite for NO2 vertical profile retrieval from ground-based zenith-sky spectrometers

Here we present an operational method to improve accuracy and information content of ground-based measurements of stratospheric NO₂. The motive is to improve the investigation of trends in NO₂, and is important because the current trend in NO₂ appears to contradict the trend in its source, suggesting that the stratospheric circulation has changed. To do so, a new software package for retrieving NO₂ vertical profiles from slant columns measured by zenith-sky spectrometers has been created. It uses a Rodgers optimal linear inverse method coupled with a radiative transfer model for calculations of transfer functions between profiles and columns, and a chemical box model for taking into account the NO₂ variations during twilight and during the day. Each model has parameters that vary according to season and location. Forerunners of each model have been previously validated. The scheme maps random errors in the measurements and systematic errors in the models and their parameters on to the retrieved profiles. Initialisation for models is derived from well-established climatologies. The software has been tested by comparing retrieved profiles to simultaneous balloon-borne profiles at mid-latitudes in spring.     

河水中亚硝酸盐氮的生物降解

通过分光光度法测定了亚硝酸盐氮的含量,并从培养条件优化和游离氨抑制作用两方面考察了河底活性淤泥对水体中亚硝酸盐氮的生物降解情况;在最佳条件下,河水中亚硝酸盐氮的降解在2天内降解率可达83.7%.