Capability of Raman lidar for monitoring the variation of atmospheric CO2 profile

Lidar （Light detection and ranging） has special capabilities for remote sensing of many different behaviours of the atmosphere. One of the techniques which show a great deal of promise for several applications is Raman scattering. The detecting capability, including maximum operation range and minimum detectable gas concentration is one of the most significant parameters for lidar remote sensing of pollutants. In this paper, based on the new method for evaluating the capabilities of a Raman lidar system, we present an evaluation of detecting capability of Raman lidar for monitoring atmospheric CO2 in Hefei. Numerical simulations about the influence of atmospheric conditions on lidar detecting capability were carried out, and a conclusion can be drawn that the maximum difference of the operation ranges caused by the weather conditions alone can reach about 0.4 to 0.5km with a measuring precision within 30ppmv. The range of minimum detectable concentration caused by the weather conditions alone can reach about 20 to 35 ppmv in vertical direction for 20000 shots at a distance of 1 km on the assumption that other parameters are kept constant. The other corresponding parameters under different conditions are also given. The capability of Raman lidar operated in vertical direction was found to be superior to that operated in horizontal direction. During practical measurement with the Raman lidar whose hardware components were fixed, aerosol scattering extinction effect would be a significant factor that influenced the capability of Raman lidar. This work may be a valuable reference for lidar system designing, measurement accuracy improving and data processing.     

探测大气中CO2的Raman激光雷达

基于大气激光后向散射光谱，研究和设计了探测大气CO₂浓度的Raman激光雷达,其发射机采用Nd∶YAG激光的三倍频354.7nm作为工作波长,发射的单脉冲能量350mJ,重复频率20Hz；接收机采用了光电倍增管(量子效率25%)和光子计数器(计数速率200MHz),探测CO₂的Raman散射371.66nm(频移1285cm^-1)信号,(1小时累加)近地面2.5km以内信噪比不小于8.采用组合滤光片来抑制强的354.7nm Mie-Rayleigh后向散射和氧气375.4nm Raman后向散射对信号的严重干扰. 比较分别来自大气CO₂和参考气体N₂的Raman后向散射回波,可反演出大气中CO₂的相对浓度. 关键词： 大气光学 激光雷达 Raman散射光谱 参考气体 Mie-Rayleigh散射     

Analysis of influence of atmosphere extinction to Raman lidar monitoring CO2 concentration profile

Lidar （Light detection and ranging） system monitoring of the atmosphere is a novel and powerful technique tool. The Raman lidar is well established today as a leading research tool in the study of numerous important areas in the atmospheric sciences. In this paper, the principle of Raman lidar technique measurement CO2 concentration profile is presented and the errors caused by molecular and aerosol extinction for CO2 concentration profile measurement with Raman lidar are also presented. The standard atmosphere extinction profile and ＇real-time＇ Hefei area extinction profile are used to conduct correction and the corresponding results are yielded. Simulation results with standard atmosphere mode correction indicate that the errors caused by molecule and aerosol extinction should be counted for the reason that they could reach about 8 ppm and 5 ppm respectively. The relative error caused by Hefei area extinction correction could reach about 6%. The errors caused by the two components extinction influence could produce significant changes for CO2 concentration profile and need to be counted in data processing which could improve the measurement accuracies.     

拉曼激光雷达探测低对流层大气二氧化碳分布

介绍了中国科学院安徽光学精密机械研究所研制成功的我国第一台测量低对流层大气CO2时空分布的拉曼激光雷达系统,选用波长355nm的紫外激光作为光源,利用光子计数卡双通道采集大气中N2和CO2的拉曼后向散射信号。详细分析了拉曼激光雷达系统的定标方法,提出采用Li7500型H2O/CO2分析仪与拉曼激光雷达系统进行对比与标定,结果显示激光雷达与CO2分析仪数据变化趋势一致性较好,激光雷达具有很高的探测灵敏度与准确性,通过线性拟合水平方向标定误差小于0.2%,垂直方向小于1.4%。由标定关系反演出大气中CO2的时空分布,给出了合肥西郊低对流层大气CO2水平方向0～2.0km与垂直方向0～2.5km分布的典型测量结果。     

地基CO2廓线探测差分吸收激光雷达

研制了一台利用气溶胶散射信号的CO₂廓线探测差分吸收激光雷达. 系统利用染料激光器实现波长调制, 采用双光路气体吸收池, 结合Voigt拟合方法实现了脉冲红外激光的高精度定标. 针对输出激光带宽较宽的问题, 采取仿真实验评估了影响, 并设计了基于吸收池的订正因子获取方案. 进而, 开展了水平、垂直和连续观测实验, 通过与地面CO₂分析仪测量值的对比, 证明了系统具备优越的精密性和精确性. 实验表明, 该样机能够俘获CO₂浓度随高程和时间变化而产生的变化.     

非线性拉曼激光雷达系统检测CO2气体的受激拉曼过程

 利用气体的受激拉曼散射增益效应的非线性雷达技术是探测大气中的CO₂气体的重要方法，用Nd:YAG固体激光器（1 064 nm）的三倍频光（354.7 nm）注入装有CO₂和N₂高压气体的拉曼管中，气体的受激拉曼散射（SRS）过程产生两种气体的一阶斯托克斯光，用来作为拉曼雷达的发射种子光源。介绍了产生光源的实验装置，论述了SRS中气体气压变化与一阶斯托克斯光能量输出变化的定量关系，得到最佳能量输出的优化条件，并对SRS中一阶斯托克斯光产生过程的物理机制进行了讨论。并根据光源的试验结果，设计了非线性受激拉曼雷达系统，对前期的普通拉曼雷达进行了实验，得到了初步的实验结果。     

绝对探测大气温度的纯转动拉曼激光雷达系统

纯转动拉曼激光雷达是探测大气温度廓线的重要手段之一,其正常工作需要配置其他并行校正设备,制约其在气象及环境监测领域中的实用化进程.基于大气氮气分子的纯转动拉曼谱型对温度的依赖性,提出并设计了绝对探测大气温度廓线的纯转动拉曼激光雷达系统.系统采用波长532 nm且脉冲能量300 m J的激光激励源和口径250 mm卡塞格林望远镜的接收器,设计了衍射光栅和光纤Bragg光栅结合的多通道并行纯转动拉曼光谱分光系统;仿真分析氮气和氧气分子的纯转动拉曼散射谱线间关系,优化选择了6条氮气分子的纯转动拉曼谱线以直接反演大气温度,设计了两级滤光器间转接光纤阵列的结构;基于最小二乘原理推导了绝对探测大气温度的反演算法,并结合标准大气模型,分析了纯转动拉曼激光雷达绝对探测大气温度的探测性能.结果表明,所设计纯转动拉曼激光雷达系统可直接反演大气温度廓线,在测量时间17 min内,温度偏差小于0.5 K的探测高度达2.0 km.     

Dy2 AlFe13 Mn3 化合物的本征磁致伸缩

通过X-射线衍射及磁测量手段研究了Dy2AlFe13Mn3化合物的结构及磁性质。研究结果表明Dy2AlFe13Mn3化合物具有六角相的Th2Ni17型结构。通过X-射线热膨胀测定法发现Dy2AlFe13Mn3化合物在245到344K的温度范围内存在负热膨胀现象，其平均热膨胀系数为α＝-1.1×10-4K-1K-1。在105到360K的温度范围内，通过比较磁性状态下的晶胞参数和由高温顺磁状态外延得到的低温顺磁状态下的晶胞参数间的差别计算了Dy2AlFe13Mn3化合物的本征磁致伸缩。结果表明Dy2AlFe13Mn3化合物的本征体磁致伸缩ωS在105到245K的温度范围内随着温度的升高而增大，由105K时的7.0×10-3 增加到245K时的9.1×10-3。随着温度的进一步升高，ωS反而减小。沿c轴方向的本征线磁致伸缩λc随着温度的升高而减小。基面内的本征线磁致伸缩λa在105到270K的温度范围内随着温度的升高而增大，从105K时的0.8×10-3增大到270K时的3.4×10-3，然后随着温度的进一步升高而减小。     

Enhanced Raman scattering from nano-SnO2 grains

We present the Raman spectra of nano-SnO_{2} grains with sizes from 4nm to 80nm excited by 532nm and 1.06μm lines. The enhanced Raman scattering of the nanograins is observed for both exciting lines when the grain size is less than 8nm. The less the grain size is, the more intensely the Raman scattering is enhanced. According to our results, the enhancements of the Raman intensity are a few tenfolds and different for different exciting lines when the grain size is 4nm. It can be attributed to enhanced Raman scattering by electron－hole pair excitations in the nanograins that originate from sub-microscopic (10nm) size and other defect- and surface-related features. A critical size that divides respective predominance of bulk properties and the defect-, surface-, and size-related features can be determined to be about 8nm.     

The effect of composition on structural and electronic properties in polycrystalline CuGaSe2 thin film

Polycrystalline CuGaSe2 thin films on Mo-coated soda-lime glass substrates have been synthesized by coevaporation process from Cu, Ga and Se sources. Structural and electrical properties of the as-grown CuGaSe2 films strongly depend on the film composition. Stoichiometric CuGaSe2 is fabricated, as indicated by x-ray diffraction spectroscope （XRD） and x-ray fluorescence （XRF）. A two-phase region is composed of CuGaSe2 and Cu2-xSe phases for Cu-rich films, and CuGaSe2 and CuGa3Se5 phases for Ga-rich films, respectively. Morphological properties are detected by scanning electron microscope （SEM） for various compositional films, the grain sizes of the CuGaSe2films decrease with the extent of deviation from stoichiometric composition. Raman spectroscopy of Cu-rich samples shows that there exist large Cu-Se particles on the film surface. The results from Hall effect measurements for typical samples indicate that CuGaSe2 films are always of p-type semiconductor from Cu-rich to Ga-rich. Stoichiometric CuGaSe2 films exhibit relatively large mobility than any other compositional films. Finally, polycrystalline CuGaSe2 thin film solar cell with a best conversion efficiency of 6.02% has been achieved under the standard air mass （AM）1.5 spectrum for 100mW/cm^2 at room temperature （aperture area, 0.24cm^2）. The open circuit voltage of the CuGaSe2 solar cells is close to770 mV.     

Ground state for CH2 and symmetry for methane decomposition

Using the different level of methods B3P86, BLYP, B3PW91, HF, QCISD、 CASSCF （4,4） and MP2 with the various basis functions 6-311G^＊＊, D95, cc-pVTZ and DGDZVP, the calculations of this paper confirm that the ground state is X^-3B1 with C2v group for CH2. Furthermore, the three kinds of theoretical methods, i.e. B3P86、 CCSD（T, MP4） and G2 with the same basis set cc-pVTZ only are used to recalculate the zero-point energy revision which are modified by scaling factor 0.989 for the high level based on the virial theorem, and also with the correction for basis set superposition error. These results are also contrary to X^-3∑^-g for the ground state of CH2 in reference. Based on the atomic and molecular reaction statics, this paper proves that the decomposition type （1） i.e. CH4 →CH2＋H2, is forbidden and the decomposition type （2） i.e. CH4→CHa＋H is allowed for CH4. This is similar to the decomposition of SiH4.     

A detection of atmospheric relative humidity profile by UV Raman lidar

A new spectroscopic filter constructed with a high-spectral-resolution grating and two narrow-band mirrors is designed to separate the elastic scattering and the vibrational Raman scattering spectra in an ultraviolet (UV) Raman lidar system. The density of humidity and water vapor mixing ratio are calculated from the vibrational Raman scattering signals of N₂ and H₂O. Water vapor mixing ratio is retrieved from this development. With this measured water vapor mixing ratio, the relative humidity is calculated with atmospheric temperature profile obtained by another Raman temperature lidar. Preliminary experiments and comparison results between lidar and radiosonde showed that the UV Raman lidar system has the capability for profiling the water vapor mixing ratio up to a height of 2 km with less than 10% of the uncertainty under the conditions of laser energy of 300 mJ and signal-averaging time of 10 min.     

连续波差分吸收激光雷达测量大气CO_2

研制了一套接收硬目标回波的差分吸收激光雷达系统以用于全天候监测大气CO2浓度变化.系统采用10和12 kHz正弦波分别对处在CO2吸收峰内和吸收峰外的波长进行强度调制,利用单频检测技术提取回波信号.提出了一种利用激光扫频推算系统精度的方法,从而弥补了长期以来只能在理论上计算差分吸收激光雷达系统精度的不足,给实际系统自定标问题提供了一种解决方案.该系统采用全光纤结构,结构可靠,便于移动.利用此系统获得了上海市多天CO2浓度变化曲线,在450 m的积分路径长度上,1 s的积分时间取得了优于3.39×10-6的测量精度.     

Ab initio calculation of the growth of Te nanorods and Bi2Te3 nanoplatelets

In this paper the growth mechanism of a Te/Bi$_{2}$Te$_{3}$ novel structure is studied by \textit{ab-initio} calculations. The results show that the growth of Te nanorods is determined by the adsorption energy of Te atoms on different crystalline Te surfaces. The adsorption energy of Te on the Te (001) surface is 3.29 eV, which is about 0.25 eV higher than that of Te on the Te (110). This energy difference makes the preferential growth direction along the $<001>$ direction. In addition, the higher surface energy of Bi$_{2}$Te$_{3}$ (110) and the lattice misfit between crystalline Bi$_{2}$Te$_{3}$ and Te along $<001>$ direction are considered to explain the growth of the Bi$_{2}$Te$_{3}$ nanoplatelets, in which Volmer--Weber model is used. The theoretical results are in agreement with experimental observation.     

Numerical study of IP3-induced Ca2+ spiral pattern evolution

The effect of change in concentration of messenger molecule inositol 1,4,5-trisphosphate (IPspiral wave, Ca$^{2 + }$, IPspiral wave, Ca$^{2 + }$, IP$_{3}$Project supported by the National Natural Science Foundation of China (Grant Nos 10575041 and 10747005)0545The effect of change in concentration of messenger molecule inositol 1,4,5-trisphosphate (IP$_{3})$ on intracellular Ca$^{2 + }$spiral pattern evolution is studied numerically. The results indicate that when the IP$_{3}$ concentration decreases from 0.27\,$\mu $M, a physiologically reasonable value, to different values, the spiral centre drifts to the edge of the medium and disappears for a small enough IP$_{3}$ concentration. The instability of spiral pattern can be understood in terms of excitability-change controlled by the IP$_{3}$ concentration. On the other hand, when the IP$_{3}$ concentration increases from 0.27\,$\mu $M, a homogeneous area with a high Ca$^{2 + }$ concentration emerges and competes with the spiral pattern. A high enough IP$_{3}$ concentration can lead the homogeneous area to occupy the whole medium. The instability of spiral pattern is ascribed to the change in stability of a stationary state with a high Ca$^{2 + }$ concentration.     

First-principle study of native defects in CuScO2 and CuYO2

This paper studies the electronic structure and native defects in transparent conducting oxides CuScO2 and CuYO2 using the first-principle calculations. Some typical native copper-related and oxygen-related defects, such as vacancy, interstitials, and antisites in their relevant charge state are considered. The results of calculation show that, CuMO2（M = Sc, Y） is impossible to show n-type conductivity ability. It finds that copper vacancy and oxygen interstitial have relatively low formation energy and they are the relevant defects in CuScO2 and CuYO2. Copper vacancy is the most efficient acceptor, and under O-rich condition oxygen antisite also becomes important acceptor and plays an important role in p-type conductivity.     

水汽探测拉曼激光雷达的新型光谱分光系统设计与分析

提出并设计了一套新型的大气水汽和气溶胶探测用紫外域拉曼激光雷达系统, 以二向色镜和超窄带滤光片构成高效率拉曼光谱分光系统, 实现激光雷达大气回波信号中米-瑞利散射信号、 氮气和水汽的振动拉曼散射信号的精细分离和高效率提取. 利用美国标准大气的分子散射模型和实测的大气米散射信号模型, 对分光系统的米-瑞利散射信号的抑制率、大气水汽测量的信噪比和误差进行数值仿真设计. 搭建实验系统对西安地区夜间的大气水汽进行实验观测, 并利用有云天气下实测的激光雷达回波信号, 反演获得大气后向散射比和水汽混合比的相关特性, 验证了该拉曼光谱分光系统对米-瑞利信号的抑制率达到10^-7以上量级. 理论和实验结果表明, 设计的新型拉曼光谱分光系统可以在大气后向散射比为17时, 实现水汽探测误差小于15%, 满足拉曼激光雷达系统对大气水汽的高效率探测. 关键词： 拉曼激光雷达 水汽混合比 大气后向散射比     

Spin polarization effect for Cr2 molecule

Density functional theory （DFT） （B3P86） of Gaussian 03 has been used to optimize the structure of the Cr2 molecule, a transition metal element molecule. The result shows that the ground state for the Cr2 molecule is a 13- multiple state, indicating that there exists a spin polarization effect in the Cr2 molecule. Meanwhile, we have not found any spin pollution because the wave function of the ground state does not mingle with wave functions of higher-energy states. So the ground state for Cr2 molecule being a 13-multiple state is indicative of spin polarization effect of the Cr2 molecule among transition metal elements, that is, there are 12 parallel spin electrons in the Cr2 molecule. The number of non-conjugated electrons is greatest. These electrons occupy different spatial orbitals so that the energy of the Cr2 molecule is minimized. It can be concluded that the effect of parallel spin in the Cr2 molecule is larger than the effect of the conjugated molecule, which is obviously related to the effect of electron d delocalization. In addition, the Murrell Sorbie potential functions with the parameters for the ground state and other states of the Cr2 molecule are derived. The dissociation energy De for the ground state of the Cr2 molecule is 0.1034eV, equilibrium bond length Re is 0.3396 nm, and vibration frequency we is 73.81cm^-1. Its force constants f2, f3 and f4 are 0.0835, -0.2831 and 0.3535 aJ. nm^-4 respectively. The other spectroscopic data for the ground state of the Cr2 molecule ωeχe, Be and αe are 1.2105, 0.0562 and 7.2938 x 10^-4cm^-1 respectively.     

合肥上空大气二氧化碳Raman激光雷达探测研究

Raman激光雷达是用于大气成分探测与特性研究的有效工具.介绍了中科院安徽光学精密机械研究所自行研制的一台用于测量低对流层大气CO₂时空分布的Raman激光雷达系统,并进行了一系列观测实验和对比分析.系统选用波长355 nm的紫外激光作为光源,利用光子计数卡双通道采集大气中N₂和CO₂的Raman后向散射信号与Li-7500型H₂O/CO₂分析仪进行对比标定,通过反演获得了大气CO₂水平与垂直方向时空分布廓线,并且获得了合肥地区大气边界层CO₂的夜变化趋势.结果表明,大气CO₂在空间的分布相对均匀,Raman激光雷达与CO₂分析仪变化趋势一致性较好,能够对大气CO₂时空分布进行有效、连续的观测.     

Ultraviolet and visible upconversion dynamics in Er^3＋：YAlO3 under ^2H11/2 excitation

The luminescence of Er^3＋：YAlO3 in ultraviolet visible and infrared ranges under the 518 nm excitation of the multiples ^2H11/2 have been investigated. Ultraviolet （275 nm and 318 nm）, violet （405 nm and 413 nm） and blue （474 nm） upconversion and infrared downconversion luminescence has been observed. By means of measuring the fluorescence decay curves and using the theory of rate equations, the luminescence kinetics was studied in detail and the processes of energy transfer upconversion （ETU） and excitation state absorption （ESA） were proposed to explain the upconversion phenomena.