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     

Combined raman elastic-backscatter LIDAR for vertical profiling of moisture,aerosol extinction,backscatter, and LIDAR ratio

A combined Raman elastic-backscatter lidar has been developed. A XeCl excimer laser is used as the radiation source. Inelastic Raman backscatter signals are spectrally separated from the elastic signal with a filter or grating polychromator. Raman channels can be chosen to register signals from CO₂, O₂, N₂, and H₂O. Algorithms for the calculation of the water-vapor mixing ratio from the Raman signals and the particle extinction and backscatter coefficients from both elastic and inelastic backscatter signals are given. Nighttime measurements of the vertical humidity distribution up to the tropopause and of particle extinction, backscatter, and lidar ratio profiles in the boundary layer, in high-altitude water and ice clouds, and in the stratospheric aerosol layer are presented. Daytime boundary-layer measurements of moisture and particle extinction are made possible by the improved daylight suppression of the grating polychromator. Test measurements of the CO₂ mixing ratio indicate the problems for the Raman lidar technique in monitoring other trace gases than water vapor.     

Raman lidar measurements of tropospheric water vapor over Hefei

L625 Raman lidar has been developed for water vapor measurements over Hefei, China since September 2000. By transmitting laser beam of frequency-tripled Nd:YAG laser, Raman scattering signals of water vapor and nitrogen molecules are simultaneously detected by the cooled photomultipliers with photon counting mode. Water vapor mixing ratios measured by Raman lidar show the good agreements with radiosonde observations, which indicates this Raman lidar is reliable. Many observation cases show that aerosol optical parameters have the good correlation with water vapor distribution in the lower troposphere.     

First-time lidar measurement of water vapor flux in a volcanic plume

The CO₂ laser-based lidar ATLAS has been used to study the Stromboli volcano plume. ATLAS measured water vapor concentration in cross-sections of the plume and wind speed at the crater. Water vapor concentration and wind speed were retrieved by differential absorption lidar and correlation technique, respectively. Lidar returns were obtained up to a range of 3 km. The spatial resolution was 15 m and the temporal resolution was 20 s. By combining these measurements, the water vapor flux in the Stromboli volcano plume was found. To our knowledge, it is the first time that lidar retrieves water vapor concentrations in a volcanic plume.     

Simultaneous measurement of atmospheric temperature,humidity, and aerosol extinction and backscatter coefficients by a combined vibrational–pure-rotational Raman lidar

Implementation of the pure-rotational Raman (PRR) lidar method for simultaneous measurement of atmospheric temperature, humidity, and aerosol extinction and backscatter coefficients is reported. The isolation of two wavelength domains of the PRR spectrum and the suppression of the elastically scattered light is carried out by a double-grating polychromator. Experiments involving elastic backscatter from dense clouds and a solid target confirm the high level of suppression of the elastic light in the corresponding acquisition channels of the two selected PRR domains. Calibration of the temperature channel was done both by comparison with an experimentally verified atmospheric temperature model profile and by inter-comparison with radiosondes. Night-time temperature profiles with high vertical resolution were obtained up to the lower stratosphere. The PRR temperature profile combined with the water vapor mixing ratio obtained from the ro-vibrational Raman channel is used to estimate the relative humidity. PACS 42.68.Wt; 42.68.Mj; 33.20.Fb     

新型车载式拉曼激光雷达测量对流层水汽

水汽体积比仅仅占整个空气的0.1%~3%,但它却是大气中时空变化最为活跃的气体。拉曼激光雷达由于其测量精度高、探测范围广以及自动化程度高,成为现今测量大气水汽含量的新型工具。介绍了中国科学院安徽光学精密机械研究所于2004年10月自行研制的国内首台车载式拉曼激光雷达的总体结构和主要技术参量,给出其相应激光雷达数据的反演方法,该激光雷达在合肥地区进行了实际测量和对比实验。测量结果显示:该激光雷达夜晚探测水汽的高度范围可以从近地面到达对流层中部8 km左右。同时,该激光雷达还尝试进行了白天水汽探测实验,并首次得出突变层内的水汽混合比垂直廓线。     

基于三级Fabry-Perot标准具的纯转动拉曼测温激光雷达

提出了新的纯转动拉曼测温雷达系统,即以种子激光注入锁定的Nd:YAG激光器为激发光源,采用基于三级Fabry-Perot(F-P)标准具的双通道分光结构代替双光栅单色仪结构.通过通道中宽带滤光片(带宽为7nm)及F-P标准具的组合使用,对532nm激发光的大气Mie-Rayleigh弹性回波散射抑制比可达10^-10,对量子数J=±6,J=±12的N₂纯转动拉曼散射光谱线接收带宽均小于10pm,因此能充分抑制大气背景辐射噪声及O₂纯转动拉曼谱线的干扰,从而实现了单谱线比反演温度,提高了探测精度,且可在白昼探测大气对流层温度.最后通过探空气球测得的对流层温度垂直分布逆向模拟了该系统双通道的Raman信号曲线,证实了该系统的可行性. 关键词： 拉曼激光雷达 纯转动拉曼散射 三级Fabry-Perot标准具 对流层     

Ultraviolet Raman lidar for high-accuracy profiling of aerosol extinction coefficient

An ultraviolet （UV） Raman lidar system at 354.7 nm has been developed for accurately measuring the aerosol extinction profiles. A spectroscopic filter combining a high-spectral-resolution grating with two narrowband mirrors is used to separate the vibrational Raman scattering signal of N2 at a central wavelength of 386.7 nm and the elastic scattering signal at 354.7 nm. The aerosol extinction is derived from the Raman scattering of N2 and the elastic scattering by the use of Raman method and Klett method, respectively. The derived results of aerosol extinction are used to compare the difference of two retrieval methods, and the preliminary experiment shows that the Raman lidar system operated in analog detection mode has the capability of measuring aerosol profiles up to a height of 3 km with a laser energy of 250 mJ and an integration time of 8 min.     

A pure rotational Raman lidar using double-grating monochromator for temperature profile detection

A pure rotational Raman lidar is constructed for measurements of vertical temperature profiles of atmosphere. A fiber-coupled, double-grating monochromator is used as the filter system so that a high spectral resolution of <0.23 nm and an out-of-band rejection rate of 10⁷ are achieved. Comparison with in-situ measurements indicates that the accuracy of atmospheric temperature measurements using this lidar system is better than 1.1 K up to an altitude of 10 km. Different effects on signal accuracy resulting from various noise sources are analyzed and uncertainties in temperature due to detection noises are estimated.     

Effective lidar ratios of dense dust layers over North Africa derived from the CALIOP measurements

Lidar ratio (i.e., extinction-to-backscatter ratio) is a key parameter required for retrieving extinction profiles and optical depths from elastic backscatter lidar measurements, and the quality of any extinction retrieval depends critically on the accuracy of the assumed or measured lidar ratio. In this study, we analyze the first two and a half years of the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) data acquired during nighttime. Distributions of the effective lidar ratio (ELR), which is the product of the lidar ratio and an instrument-dependent multiple scattering factor, are derived for opaque dust layers observed by CALIOP over the North Africa. The median and mean ELR values are, respectively, 36.4 and 38.5 sr at 532 nm and 47.7 and 50.3 sr at 1064 nm. For these opaque dust layers, the derived ELR decreases as the volume depolarization ratio (VDR) increases, reflecting the impact of multiple scattering within the dense layers. The particulate depolarization ratio is typically ∼0.3 at 532 nm for African dust observed by CALIOP. This ratio can increase to ∼0.4 in the presence of significant multiple scattering. Correspondingly, the calculated ELR will decrease to ∼20 sr at 532 nm and to ∼30 sr at 1064 nm. The median and mean effective lidar ratio values approach, respectively, to 38 and 40 sr at 532 nm and 52 and 55 sr at 1064 nm for smaller VDR values measured in less dense layers where the multiple scattering is relatively insignificant. These values are very close to those derived in previous case studies for moderately dense dust. Case studies are also performed to examine the impacts of multiple scattering. The results obtained are generally consistent with Monte-Carlo simulations.     

Study of atmospheric water in gaseous and. liquid state by using combined elastic–Raman. depolarization lidar

A combined elastic–Raman lidar system based on a tripled Nd:YAG laser is used for the separate detection of elastic backscatter and Raman signals from atmospheric nitrogen, water vapor and liquid water and for their depolarization measurement. Vertical profiles of water-vapor and liquid-water content measured under clear-sky conditions behave differently: inside the boundary layer the ratio of liquid-water to water-vapor Raman backscatters rises with altitude. The depolarization measurements bring additional information about atmospheric scattering. The observed depolarization ratio of the water-vapor Raman signal is about 14%, while for liquid water this ratio varies in the 30–75% range, which exceeds the depolarization of bulk water and is attributed to the water-aerosol effects. Raman contours of water vapor and liquid water are partially overlapped, and bleed-through of liquid-water Raman backscatter leads to enhancement of depolarization of the water-vapor Raman signal. This parameter may be used as a convenient indicator of liquid-water interference in water-vapor measurements. Received: 12 December 2000 / Revised version: 27 September 2001 / Published online: 7 November 2001     

Influence of vapor transport equilibration on Raman spectra of Er:LiNbO3 crystals

Raman spectra of as-grown and vapor transport equilibration (VTE) treated Er:LiNbO₃ crystals, which have different cut orientations (X-cut and Z-cut), different Er-doping levels (Er:(0.2, 0.4 and 2.0 mol%)LiNbO₃) and different VTE durations (80, 120, 150 and 180 h), were recorded at room temperature in the wavenumber range 50-1000 cm⁻¹ by using backward scattering geometry. The spectra were attributed on the basis of their spectral features and the previous experimental work and the most recent theoretical progress in lattice dynamics on pure LiNbO₃. In comparison with the pure crystal the most remarkable effect of Er-doping on the Raman spectrum is observed for the E(TO₉) mode. It does not appear at 610 cm⁻¹ as the pure crystal, but locates at 633 cm⁻¹. In addition, the doping also results in the lowering of the Raman phonon frequency, the broadening of the Raman linewidth and the changes of the relative Raman intensity of some peaks. The VTE treatment results in the narrowing of the linewidth, the recovery of the lowered phonon frequency and the further changes of relative Raman intensity. The narrowing of Raman linewidth indicates that the VTE processing has brought these crystals closer to stoichiometric composition. The VTE treatment has induced the formation of a precipitate ErNbO₄ in the high-doped Er(2.0%):LiNbO₃ crystals whether X- or Z-cut. For these precipitated crystals, besides above linewidth and phonon frequency features, they also display more significant Raman intensity changes compared with those not precipitated crystals. In addition, a slight mixing between A₁(TO) and E(TO) spectra is also observed for these precipitated crystals. Above doping and VTE effects on Raman spectra were quantitatively or qualitatively correlated with the characteristics of the crystal structure and phonon vibrational system.     

The growth and optical properties of ZnO nanowires at the junctions of nanowalls

Highly pure ZnO nanowires at the junctions of nanowalls have been successfully prepared via a simple vapor phase route at relative low temperature in the absence of catalyst. SEM, TEM, Raman scattering and PL were employed to characterize as-grown samples. The nanowires have average diameter of 10 nm with [001] growth direction. Raman scattering shifted from higher frequency to lower frequency and the enhancement of PL intensity of the green emission to the UV may be attributed to smaller nanowires and thinner nanowalls. This nanostructure may have important applications in batteries, light-emitting and energy conversion devices and other fields demanding high surface area materials.     

Raman scattering studies of polycrystalline 3C-SiC deposited on SiO2 and AlN thin films

This paper describes the Raman scattering characteristics of the Raman spectra of 0.4- and 2.0-μm-thick polycrystalline (poly) 3C-SiC on AlN /Si and SiO₂/Si by using atmosphere pressure chemical vapor deposition (APCVD) with hexamethyldisilane (HMDS) and carrier gases (Ar+H₂). In the Raman spectra for all growth temperatures, the D and G peaks of nanocrystalline graphite were measured. The C/Si rate of poly 3C-SiC deposited in (Ar+H₂) atmosphere was higher than that in H₂ gas, although HMDS C/Si rate is 3. The biaxial stresses of 2.0-μm-thick 3C-SiC on SiO₂ and AlN, which was deposited at the growth temperature of 1180 °C after annealing AlN at 800 and 1100 °C, were calculated as 428 and 896 MPa, respectively. Therefore, poly 3C-SiC should admix with nanocrystalline graphite due to the addition of Ar gas and poly 3C-SiC on SiO₂ should be better than on AlN for harsh environmental MEMS applications.     

The Raman spectra and cross-sections of the ν2 band of H2O, D2O, and HDO

We report the experimental Raman spectra of the ν₂ band of H₂O, D₂O, and HDO in the vapor phase at room temperature. A complete interpretation of the Raman intensities is carried out employing the variational rovibrational wavefunctions obtained from a Hamiltonian in Radau coordinates and an ab initio polarizability surface at 514.5 nm. We show the importance of the rotation-vibration coupling to obtain the correct line intensities. Several tables with the assignments of the individual rotational-vibrational transitions and their Raman scattering strengths are reported. From these tables, the ν₂ Raman spectra can be simulated up to 2000 K for H₂O, and up to 300 K for D₂O and HDO.     

Effect of relative humidity on morphology of YBCO films prepared by CSD method

YBa₂Cu₃O_7−x (YBCO) films have been prepared on LaAlO₃ (1 0 0) substrates by chemical solution deposition using metal trifluoroacetates. The influence of relative humidity in coating circumstance on the morphology of YBCO films was examined by optical microscopy and atomic force microscopy. The crack-free YBCO film was obtained if the relative humidity in coating circumstance was lower than 30%. During the decomposition step, the influences of the water vapor partial pressure and the heating rate within the temperature range from 200 °C to 320 °C were discussed. A smooth YBCO pyrolzed film could be obtained if the suitable water vapor partial pressure and the suitable heating rate within the temperature range from 200 °C to 320 °C were chosen. Furthermore, the smooth crystallized films show a high critical current density of 3 MA/cm² at 77 K.     

Surface acoustic phonon modes of Ge nanocrystals embedded in SiO2

Ge nanocrystals (NCs) embedded in SiO₂ are synthesized by ion implantation, and the surface vibrational modes of the Ge NCs are investigated using the low-frequency Raman scattering (LFRS) technique. LFRS studies show distinct low-frequency Raman modes in the range 6.5-21.2 cm⁻¹ for the Ge NCs depending on the implant dose and annealing temperature. These low-frequency Raman modes are attributed to the confined surface acoustic phonon modes of Ge NCs with (0,0) spheroidal mode and (0,3) torsional modes. Our results are in excellent agreement with the recent theoretical predictions of surface vibrational modes in Ge NCs.     

Diode laser spectroscopic measurements and theoretical calculations of line parameters of nitrogen-broadened water vapor overtone transitions in the 818-834 nm wavelength region

Nitrogen-broadened water vapor line parameters of the (2 1 1) ← (0 0 0) overtone band transitions in the 818-834 nm wavelength region are measured by using a tunable diode laser spectrometer. Water vapor is kept at its saturated vapor pressure at room temperature within a sample cell. Use of a balanced detector and a lock-in amplifier helps to increase the detection efficiency and the signal-to-noise ratio. The collisional broadening coefficients are extracted from the fitting of the experimental data by using a standard Voigt line profile. Collisional half-widths of water vapor lines perturbed by nitrogen are evaluated using the complex-valued implementation of the Robert-Bonamy (CRB) formalism. The rotational wave functions and the energy eigenvalues in the (2 1 1) vibrational state of water molecule are assumed on the basis of symmetry properties. Hence the outcome of this work also tests the validity of the theoretical approximations. The experimental data are compared with the corresponding theoretical values and the possible causes of deviation between the two have also been discussed.     

Structural and optical properties of ZnO film by plasma-assisted MOCVD

High quality ZnO film was deposited by plasma-assisted metal-organic chemical vapor deposition (MOCVD). We observed a dominant peak at 34.6° due to (0 0 2) ZnO, which indicated that the growth of ZnO film was strongly C-oriented. The full-width at half-maximum (FWHM) of the -rocking curve was 0.56° indicating relatively small mosaicity. Photoluminescence (PL) measurement was performed at both room temperature and low temperature. Ultraviolet (UV) emission at 3.30 eV was found with high intensity at room temperature while the deep level transition was weakly observed at 2.513 eV. The ratio of the intensity of UV emission to that of deep level emission was as high as 193, which implied high quality of ZnO film. From PL spectrum at 10 K, we observed A-exciton emission at 3.377 eV and D°X bound exciton transition at 3.370 eV. The donor–acceptor transition and LO phonon replicas were observed at 3.333 and 3.241 eV respectively. Raman scattering was performed in back scattering at room temperature. The E₂, A_1(LO) and A_1(TO) mode was seen at 437.6, 575.8 and 380 cm^–1 respectively. In comparison with Raman spectrum of ZnO powder, we found that ZnO film was nearly free of strain, which indicated high crystal quality.     

Low-uncertainty H2O line intensities for the 930-nm region

We measured room-temperature H₂O spectra of the 3ν polyad within the wave number range 10 603 cm⁻¹ to 10 852 cm⁻¹ using frequency-stabilized cavity ring-down spectroscopy. More than 70 transitions, divisible into two groups based on their relative intensities (strong and weak) were investigated. For the 23 lines comprising the set of strong transitions, the water vapor sample was prepared as a dilute mixture in a steady flow of N₂ carrier gas, and the measurement of the water vapor sample number density was linked to primary methods of humidity generation. For these strong transitions, the measured line intensities were within 1% of previous measurements. The line intensity measurements of the weaker H₂O transitions, were made on samples of static pure water vapor, and these results were systematically greater than previous measurements by approximately 20%.