机载多轴差分吸收光谱技术获取对流层NO2 垂直柱浓度的研究

介绍了一种基于机载平台获取对流层NO₂垂直柱浓度的多轴差分吸收光谱技术. 研究了利用差分吸收光谱技术结合不同观测角度的测量光谱反演差分斜柱浓度, 并利用辐射传输模型SCIATRAN计算对流层NO₂垂直柱浓度的方法. 研究了不同海拔高度、不同地面反照率以及不同太阳天顶角等条件对天顶和天底两个观测角度的大气质量因子的影响. 报道了该系统在2008年12月10日在珠三角地区的实验结果, 结合天顶和天底两个方向反演得到了珠三角地区对流层NO₂垂直柱浓度的分布信息. 同时还将机载测量结果跟安装在珠海市的一台地基多轴差分吸收光谱仪的结果进行了对比, 二者相差仅为8%. 实验结果表明, 机载多轴DOAS技术可以实现对大区域对流层NO₂浓度的快速获取.     

Retrieval of tropospheric NO2 columns from satellite measurements in presence of cirrus: A theoretical sensitivity study using SCIATRAN and prospect application for the A-Train

A theoretical sensitivity study of the influence of cirrus cloud properties on tropospheric NO₂ columns retrieved from the spaceborne Ozone Monitoring Instrument (OMI) measurements is performed. It is conducted within the framework of the synergetic use of A-Train sensors to derive more representative trace gas products. We aim to study the potential effects of cirrus clouds on tropospheric NO₂ retrievals using a retrieval algorithm that, unlike the OMI Standard and DOMINO algorithms, does not correct for the effects of clouds. The sensitivity study is based on the radiative transfer code SCIATRAN that performs both simulations of top of atmosphere (TOA) reflectances as measured by an OMI-like band and tropospheric NO₂ column retrievals based on the differential optical absorption spectroscopy (DOAS) method. The results of the sensitivity study show that if a correction for cirrus clouds is not included in our simple retrieval that does not account for clouds in the first place, the tropospheric column can be underestimated by 55%. This underestimation depends strongly on cirrus parameters as, in order of importance, cloud fraction, cloud optical depth, asymmetry factor of cirrus cloud phase function and cloud top height. The perspective of the synergy between OMI and cloud information obtained from cloud-derived products of the A-Train is evaluated in two parts by applying a simple cloud correction scheme based on the independent pixel approximation (IPA). Firstly, we evaluated the tropospheric NO₂ column retrievals error caused by uncertainties in cirrus cloud properties. Secondly we studied the influence of subpixel cloud optical depth variability on NO₂ retrievals. From our simulations, it is demonstrated that the error will be reduced significantly if the cloud fraction is lower or equal to 0.5. In this case, the cloud fraction and the cloud optical depth must be known within accuracy less than 0.05% and 50%, respectively. The cloud top height and the asymmetry factor must be known within uncertainty of at least 1 km and less than 0.05, respectively. The latter result shows that the uncertainty of the asymmetry factor is a major source of error in the cloud correction for tropospheric NO₂ retrieval in the presence of cirrus.     

Observation of tropospheric NO_2 by airborne multi-axis differential optical absorption spectroscopy in the Pearl River Delta region,south China

An airborne multi-axis differential optical absorption spectroscopic （AMAX-DOAS） instrument was developed and applied to measure tropospheric NO2 in the Pearl River Delta region in the south of China. By combining the measurements in nadir and zenith directions and analyzing the UV and visible spectral region using the DOAS method, information about tropospheric NO2 vertical columns was obtained. Strong tropospheric NO2 signals were detected when flying over heavilly polluted regions and point sources like plants. The AMAX-DOAS results were compared with ground-based MAX-DOAS observations in the southwest of Zhuhai city using the same parameters for radiative transport calculations. The difference in vertical column data between the two instruments is about 8%. Our data were also compared with those from OMI and fair agreement was obtained with a correlation coefficient R of 0.61. The difference between the two instruments can be attributed to the different spatial resolution and the temporal mismatch during the measurements.     

Condition of Retrieving Vertical Column Density of Atmospheric Pollution Gases by Using Scattered Solar Radiation

We present a method to monitor the vertical column density （VCD） of atmospheric pollution gases by using the scattered solar radiation. The necessary condition of capturing the useful scattered solar radiation is achieved. The condition is only dependent on the solar elevation angle, while independent of the solar azimuth angle, which could greatly simply the capturing equipment and procedure. Under the condition, the VCD of tropospheric NO2 in Chengdu, China is retrieved from the scattered solar radiation, which is close to that from the direct solar radiation.     

多轴差分吸收光谱技术测量近地面NO2体积混合比浓度方法研究

多轴差分吸收光谱技术(MAX-DOAS)通过测量不同角度的太阳散射光, 获取痕量气体的柱浓度信息, 广泛应用于整层NO₂柱浓度的监测. 由于缺少有效观测距离的信息, MAX-DOAS无法获取近地面NO₂的体积混合比浓度. 本文分析了消光系数和有效观测距离的关系, 提出了利用能见度信息获取有效观测距离, 进而将MAX-DOAS测量的水平方向NO₂斜柱浓度转换为体积混合比浓度的方法. 并在合肥开展了相应的观测实验, 成功实现了基于MAX-DOAS的NO₂体积混合比浓度测量. 通过与主动式长程差分吸收光谱仪测量的NO₂浓度进行对比, 结果呈现出较好的一致性, 说明了方法的可行性.研究为MAX-DOAS监测近地面NO₂体积混合比浓度提供了一种简单有效的方法, 拓展了MAX-DOAS的应用领域. 关键词： 多轴差分吸收光谱技术 大气消光系数 能见度 2体积混合比浓度')" href="#">NO₂体积混合比浓度     

发光二极管在差分吸收光谱系统中的应用研究

研究了新型发光二极管(LEDs)作为主动差分吸收光谱技术(DOAS)光源的可行性及其应用.分析了LEDs发光特性、谱的形状、光谱范围和谱的稳定性.结果表明LEDs作为主动DOAS光源是可行的,只是当温度不恒定时,LEDs光谱中的法布里-珀罗标准具效应将影响DOAS精确反演,若把其结构提取参与拟合可以很好地去除其影响.并成功地利用LEDs-DOAS系统监测了大气NO₂的浓度,与基于高压氙弧灯为光源DOAS系统测量结果的相关性达到0.99以上.当光程为0.7km时,检测限为1.1×10< 关键词： 发光二极管(LEDs) 差分吸收光谱技术(DOAS) 可行性     

Retrieval of the vertical column density of the atmospheric pollution gases by using the scattered solar radiation

The method of monitoring the vertical column density (VCD) of atmospheric pollution gases by using the scattered solar radiation is proposed and the scheme to ensure the necessary condition is put forward. Under the condition, the VCD of tropospheric NO₂ is retrieved from the scattered solar radiation, which is close to that from the direct solar radiation.     

直射太阳光差分吸收光谱法测量合肥NO2 整层柱浓度

直射太阳光差分吸收光谱技术(DS-DOAS)近 年来成功应用于大气痕量气体的垂直柱浓度测量. 本文研究了基于被动DOAS算法可用于连续测量NO₂整层垂直柱浓度的DS-DOAS技术, 介绍了测量系统的构成.利用统计最小值外推法减少了由参考谱引入的误差.分析了测量结果的误差来源, 估算了误差大小.报道了该系统在合肥地区对NO₂进行的连续11天的测量, 分析了测量结 果.通过实验验证了算法的可行性, 证实了该技术可实现连续测量NO₂整层垂直柱浓度.     

Nitrogen Dioxide Sensing Properties and Mechanism of Copper Phthalocyanine Film

Copper phthalocyanine film, a p-type organic semiconductor, is synthesized by vacuum sublimation and its surface morphology is characterized by SEM. A silicon-based copper phthalocyanine film gas sensor for NO2 detection is fabricated by MEMS technology. The results show that the resistance and sensitivity of copper phthalocyanine film decrease obviously as the NO2 concentration increases from Oppm to lOOppm. However, the sensitivity nearly keeps a constant of O. 158 between 30 ppm and 70 ppm. The best working temperature of the gas sensor is 90℃ for NO2 gas concentrations of lOppm, 20ppm and 30ppm, which is much lower than that of general metal oxide gas sensor.     

多轴差分吸收光谱仪反演大气NO2的比对试验

为了满足卫星遥感产品地基验证平台中不同仪器观测数据一致性的要求, 2011年9月, 将3台不同设计方案、不同操作方式的多轴差分吸收光谱仪(MAX-DOAS) 集中在中国科学院大气物理研究所香河大气探测综合试验站, 进行了近20天的同步观测测试. 并对所有仪器统一观测方位角, 分别采用相同的紫外、可见光波段的特征吸收带及吸收截面进行NO₂柱浓度的反演试验. 系统的比对分析表明: 3台MAX-DOAS的反演误差大都保持在6%以内, 说明仪器性能良好, 比较稳定; 紫外波段的反演结果略小于可见光波段, 尤其在阴天, 这是由于两波段对分子及气溶胶散射的敏感性不同造成的; 以可见光波段的反演结果为标准, 对紫外波段的反演结果进行系统订正, 订正后的各组数据一致性非常好, 满足卫星大气成分NO₂柱浓度遥感产品不同地基验证站点数据稳定、一致的要求. 关键词： MAX-DOAS 2')" href="#">NO₂ 斜柱浓度 比对试验     

Effects of Different Dispersion Methods on the Microscopical Morphology of TiO2 Film

Nanocrystalline porous TiO2 films were prepared on conducting glass supports （ITO） by processed commercial TiO2 nanometre powder （P25）. Three methods of physical dispersing for TiO2 powder, i.e. grinding, magnetic stirring, sonicleaning, were used to disperse TiO2 nanometre powder. Surface morphologies of TiO2 films were observed by optic-microscope and SEM. It is found that the surface morphologies of TiO2 films are determined not only by the dispersing methods but also by the percentage of TiO2 powder in the dispersing system. Different film morphologies can be obtained under the same preparation condition but with different dispersing methods. A lot of cracks exist on the film surface for which the TiO2 slurry is dispersed by grinding. Magnetic stirring leads to some white points and micro-holes on the film surface. Only a few of micro-holes can be observed on the film surface, in which the TiO2 slurry is dispersed by sonicleaning. Different surface morphologies can also be found with different thicknesses of TiO2 films. Different film thicknesses are due to different percentages of TiO2 powder in the slurry. The related mechanism leading to different features of the surface morphologies for the TiO2 films is discussed.     

Improvement in Dielectric Tunability of Ba0.6Sr0.4TiO4-Mg2TiO4 Composite Ceramics via Heterogeneous Nucleation Processing

Dielectric tunable composite ceramics Ba0.6Sr0.4 TiO4-Mg2 TiO4 （BST-MT） are prepared with a heterogeneous nucleation sol-gel approach. The Mg2 TiO4 powders are synthesized by the conventionM solid-state reaction method. The micro-sized MT powders with dispersant Ciba-4010 are introduced into Ba-Sr-Ti sol to obtain uniform and homogeneous mixture compounds with nano-sized BST particles synthesized via heterogeneous nucleation （HN） in the sol-gel process. Thus, the mierostructural and dielectric properties can be tailored. The dielectric constants of BST-MT composite ceramics can be adjusted in a larg＇e range from 294 to 1790, and the dielectric tunability can be adjusted from 29.4% to 37.0% with different MT contents from 60wt% to 20wt%. Compared to the samples prepared by the conventional solid-state （SS） process, the BST-MT composite ceramics by the heterogeneous nucleation sol-gel process exhibit a more uniform microstructure, and improve dielectric properties.     

三硝基甲苯起爆机理实验研究

 用单脉冲化学激波管实验方法,使用自由基清扫剂和对比速率,测定了邻位和对位硝基甲苯在高温下,裂解瞬间（500 μs） 的化学反应机理,并测定了化学反应速率常数。作为邻位硝基甲苯的同分异构体,对位硝基甲苯的主要裂解通道与其不同。通过实验发现了邻位硝基甲苯的裂解重要通道,测到它的产1氧-2氮-3,4-环丁二稀基异嚙唑（Anthranil） 在瞬间随温度变化生成和很快消失的过程。由此,测得这一化学性质极不稳定的产物的消失速率常数为：k(Anthranil)＝3.7×10¹⁵·exp(－25 800/T) s^-1。分析这一过程的机理,认为第一步是硝基甲苯的裂解,第二步是Anthranil的生成,第三步是Anthranil中的N－O键的断裂。     

利用差分吸收光谱法测量亚硝酸和反演气溶胶参数

利用差分光学吸收光谱仪(DOAS)进行亚硝酸(HONO)气体的测量并同时在固定的波长范围内(3 07—380 nm)反演气溶胶参数包括气溶胶的平均直径、总个数和总比表面积等. 实验结果表 明利用自测的NO₂标准吸收截面可以更加准确地拟合HONO的浓度，同时在较短的 波长范围内能准确反演气溶胶参数. 关键词： 差分光学吸收光谱(DOAS) 亚硝酸 气溶胶参数     

基于QDOAS的多轴差分吸收光谱测量对流层HCHO的研究

由于甲醛在大气光化学反应中的重要性及其对环境、气候和人类健康的危害,监测、有效控制甲醛浓度已经成为一件刻不容缓的要事。目前传统的监测多局限于基于化学方法、色谱法的室内监测,或是室外较小范围的监测,室外大范围的大气中的甲醛监测往往为人们所忽视。为了有效监测大气中大范围的甲醛（HCHO）浓度,建立了地基MAX-DOAS观测系统,与主动DOAS观测系统相比,该观测系统不受光源和反射装置限制,平台搭建简单,测量范围广。2018年在合肥地区(117°17′E, 31°90′N)夏季开展了基于地基MAX-DOAS的外场连续观测实验,结合新一代光谱处理软件QDOAS利用DOAS算法的非线性最小二乘拟合反演甲醛（HCHO）的斜柱浓度,并通过大气质量因子（AMF）将甲醛（HCHO）的斜柱浓度转换为柱浓度,并分析了7月份的观测数据,结果表明,低仰角下甲醛的差分斜柱浓的值较高,说明,对流层甲醛主要集中在接近地表的位置。从实验数据还可以看到,二氧化氮与甲醛的变化趋势基本一致,说明大气中的甲醛与机动车排放或是工业排放出的的氮氧化物（NO₂等）在大气的源与汇过程中具有一定的相关性。通过地基MAX-DOAS测量数据与OMI观测值的比较发现,二者的变化趋势具有良好的一致性,且相关系数为0.518 9,并分析了OMI观测值偏低的原因。研究结果表明,地基MAX-DOAS系统不仅可以对区域污染的演变进行研究,也为甲醛的测量提供了一种实时、快速的监测手段,为分析大气甲醛的来源提供了一种新的解析手段,为验证卫星观测数据提供了一种有效的手段。     

RING EFFECT: IMPACT OF ROTATIONAL RAMAN SCATTERING ON RADIATIVE TRANSFER IN EARTH’S ATMOSPHERE

One significant limitation to the accuracy of the remote sensing of trace gas constituents in the atmosphere, using UV-visible spectroscopy and scattered sunlight, has often been a reliable knowledge of the so-called Ring effect. In this study it is demonstrated that the filling-in of Fraunhofer and gas absorption features, resulting from Rotational Raman scattering (RRS), explains to high accuracy the Ring effect. A radiative transfer model has been adapted to include RRS and carefully validated by comparison with Ring effect data by other models and from ground-based and satellite data. The analysis of the principle components of the simulated Ring spectra enabled the Fraunhofer and gas absorption filling-in to be separated. This yields a simple, and therefore computational fast, parameterization of the Ring effect suitable for trace gas retrievals. This approach was tested for the retrieval of NO₂ which is considered to be a worst case with respect to absorption feature filling-in for a trace gas retrieved from scattered light. Analysis of the errors in the vertical column of NO₂ derived using differential optical absorption spectroscopy (DOAS) technique indicate that they are dependent on the amount of NO₂ present in the atmosphere when regarding the experimental Ring spectra. This implies that calculated Ring spectra may be superior for DOAS retrievals, compared to the experimentally determined Ring spectra.     

Effect of Process Parameters on Laser Damage Threshold of TiO2 Coatings

We investigate the laser damage behaviour of an electron-beam-deposited TiO2 monolayer at different process parameters. The optical properties, chemical composition, surface defects, absorption and laser-induced damage threshold （LIDT） of films are measured. It is found that TiO2 films with the minimum absorption and the highest LIDT can be fabricated using a TiO2 starting material after annealing. LIDT is mainly related to absorption and is influenced by the non-stoichiometric defects for TiO2 films. Surface defects show no evident effects on LIDT in this experiment.     

Physical Explanation on Designing Three Axes as Different Resolution Indexes from GRACE Satellite-Borne Accelerometer

The GRACE Earth＇s gravitational field complete up to degree and order 120 is recovered based on the same and different three-axis resolution indexes from satellite-borne accelerometer using the improved energy conservation principle. The results show that designing XA1（2） as low-sensitivity axis （3 × 10^-9 m/s^2） of accelerometer and designing YA1（2） and ZA1（2） as high-sensitivity axes （3 × 10^-10 m/s^2） are reasonable. The physical reason why the resolution of XA1（2） is one order of magnitude lower than YA1（2） and ZA1（2） is that non-conservative forces acting on GRACE satellites are mainly decomposed into YA1（2） and ZA1（2） in the orbital plane. Since XA1（2） is not orthogonal accurately to orbital plane during the development of accelerometer, the measurement of XA1（2） can not be thrown off entirely, but be reduced properly.     

On the validity of an approximation for the deviation of a light beam. by a prism

According to many textbooks on optics, the deviation angle of a prism with the apex angle (or prism angle), %, and the refractive index, n, with respect to the surrounding medium can be approximated by '_appr=(n-1)%, if %€?/2 and the angle of incidence !₁€?/2. The validity of this approximation is investigated considering the relative error of the deviation. It is shown that this approximation can be extended to angles of incidence !₁=n% with very fair accuracy and even to larger prism angles %<?/4 in the range of angles of incidence near the minimum of deviation depending on the acceptable relative error.     

Design and First-principles Study of a Fullerene Molecular Device

By using open-ended armchair （6, 6） single-wall carbon nanotubes as electrodes, we investigate the electron transport properties of an all-carbon molecular junction based on the C82 molecule. We find the most stable system among different isomers by performing structural optimization calculations of the Cs2 isomers and the C82 extended molecules. The calculated results show that the C82 -C2 （3） isomer and the C82 extended molecule with C82-C2 isomer are most stable. For the all-carbon hybrid system consisting of C82-C2 extended molecules, it is shown that the Landauer conductance can be tuned over several orders of magnitude both by changing the distance between two electrodes and by changing the orientation of the C82 molecule or rotating one of the tubes around the symmetry axis of the system at a fixed distance. Also, we find the most stable distance between two electrodes from the total energy curve. This fact could make this all-carbon molecular system a possible candidate for a nanoelectronic switch. Moreover, we interpret the conductance mechanism for such a molecular device.