Airborne differential absorption lidar system for measurements of atmospheric water vapor and aerosols

An airborne differential absorption lidar (DIAL) system has been developed at the NASA Langley Research Center for remote measurements of atmospheric water vapor (H(2)O) and aerosols. A solid-state alexandrite laser with a 1-pm linewidth and > 99.85% spectral purity was used as the on-line transmitter. Solid-state avalanche photodiode detector technology has replaced photomultiplier tubes in the receiver system, providing an average increase by a factor of 1.5-2.5 in the signal-to-noise ratio of the H(2)O measurement. By incorporating advanced diagnostic and data-acquisition instrumentation into other subsystems, we achieved additional improvements in system operational reliability and measurement accuracy. Laboratory spectroscopic measurements of H(2)O absorption-line parameters were perfo med to reduce the uncertainties in our knowledge of the absorption cross sections. Line-center H(2)O absorption cross sections were determined, with errors of 3-6%, for more than 120 lines in the 720-nm region. Flight tests of the system were conducted during 1989-1991 on the NASA Wallops Flight Facility Electra aircraft, and extensive intercomparison measurements were performed with dew-point hygrometers and H(2)O radiosondes. The H(2)O distributions measured with the DIAL system differed by ≤ 10% from the profiles determined with the in situ probes in a variety of atmospheric conditions.     

Side-line tunable laser transmitter for differential absorption lidar measurements of CO2: design and application to atmospheric measurements

A 2 microm wavelength, 90 mJ, 5 Hz pulsed Ho laser is described with wavelength control to precisely tune and lock the wavelength at a desired offset up to 2.9 GHz from the center of a CO(2) absorption line. Once detuned from the line center the laser wavelength is actively locked to keep the wavelength within 1.9 MHz standard deviation about the setpoint. This wavelength control allows optimization of the optical depth for a differential absorption lidar (DIAL) measuring atmospheric CO(2) concentrations. The laser transmitter has been coupled with a coherent heterodyne receiver for measurements of CO(2) concentration using aerosol backscatter; wind and aerosols are also measured with the same lidar and provide useful additional information on atmospheric structure. Range-resolved CO(2) measurements were made with <2.4% standard deviation using 500 m range bins and 6.7 min? (1000 pulse pairs) integration time. Measurement of a horizontal column showed a precision of the CO(2) concentration to <0.7% standard deviation using a 30 min? (4500 pulse pairs) integration time, and comparison with a collocated in situ sensor showed the DIAL to measure the same trend of a diurnal variation and to detect shorter time scale CO(2) perturbations. For vertical column measurements the lidar was setup at the WLEF tall tower site in Wisconsin to provide meteorological profiles and to compare the DIAL measurements with the in situ sensors distributed on the tower up to 396 m height. Assuming the DIAL column measurement extending from 153 m altitude to 1353 m altitude should agree with the tower in situ sensor at 396 m altitude, there was a 7.9 ppm rms difference between the DIAL and the in situ sensor using a 30 min? rolling average on the DIAL measurement.     

Dual Differential Absorption Lidar for the Measurement of Atmospheric SO(2) of the Order of Parts in 10(9)

Vertical concentration profiles of atmospheric SO(2) of the order of parts in 10(9) (ppb) were measured by a multiwavelength differential absorption lidar system. The error that was due to O(3) and aerosols was successfully reduced by a three-wavelength dual differential absorption lidar (DIAL), and a SO(2) concentration of 1.2 ppb for 2400-3000-m altitude was obtained with 300-m range resolution. The measurement error in dual DIAL was estimated to be <1.1 ppb when several factors were considered. The influence of O(3) on SO(2) measurement error was experimentally evaluated from simultaneous measurements of atmospheric SO(2) and O(3) by two conventional DIAL pairs, each using two wavelengths.     

Frequency-agile bandpass filter for direct detection lidar receivers

We discuss the development of a frequency-agile receiver for CO(2) laser-based differential absorption lidar (DIAL) systems. The receiver is based on the insertion of a low-order tunable etalon into the detector field of view. The incorporation of the etalon into the receiver reduces system noise by decreasing the instantaneous spectral bandwidth of the IR detector to a narrow wavelength range centered on the transmitted CO(2) laser line, thereby improving the overall D* of the detection system. A consideration of overall lidar system performance results in a projected factor of a 2-7 reduction in detector system noise, depending on the characteristics of the environment being probed. These improvements can play a key role in extending the ability of DIAL systems to monitor chemical releases from long standoff distances.     

Ultraviolet DIAL measurements of O3 profiles in regions of spatially inhomogeneous aerosols

The differential absorption lidar (DIAL) technique generally assumes that atmospheric optical scattering is the same at the two laser wavelengths used in the DIAL measurement of a gas concentration profile. Errors can arise in this approach when the wavelengths are significantly separated, and there is a range dependence in the aerosol scattering distribution. This paper discusses the errors introduced by large DIAL wavelength separations and spatial inhomogeneity of aerosols in the atmosphere. A Bernoulli solution for determining the relative distribution of aerosol backscattering in the UV region is presented, and scattering ratio boundary values for these solutions are discussed. The results of this approach are used to derive a backscatter correction to the standard DIAL analysis method. It is shown that for the worst cases of severe range dependence in aerosol backscattering, the residual errors in the corrected DIAL O3 measurements were <10 ppbv for DIAL wavelengths at 286 and 300 nm.     

Testing carbon sequestration site monitor instruments using a controlled carbon dioxide release facility

Two laser-based instruments for carbon sequestration site monitoring have been developed and tested at a controlled carbon dioxide (CO(2)) release facility. The first instrument uses a temperature tunable distributed feedback (DFB) diode laser capable of accessing the 2.0027-2.0042 microm spectral region that contains three CO(2) absorption lines and is used for aboveground atmospheric CO(2) concentration measurements. The second instrument also uses a temperature tunable DFB diode laser capable of accessing the 2.0032-2.0055 mum spectral region that contains five CO(2) absorption lines for underground CO(2) soil gas concentration measurements. The performance of these instruments for carbon sequestration site monitoring was studied using a newly developed controlled CO(2) release facility. A 0.3 ton CO(2)/day injection experiment was performed from 3-10 August 2007. The aboveground differential absorption instrument measured an average atmospheric CO(2) concentration of 618 parts per million (ppm) over the CO(2) injection site compared with an average background atmospheric CO(2) concentration of 448 ppm demonstrating this instrument's capability for carbon sequestration site monitoring. The underground differential absorption instrument measured a CO(2) soil gas concentration of 100,000 ppm during the CO(2) injection, a factor of 25 greater than the measured background CO(2) soil gas concentration of 4000 ppm demonstrating this instrument's capability for carbon sequestration site monitoring.     

Rotational vibrational-rotational Raman differential absorption lidar for atmospheric ozone measurements: methodology and experiment

A single-laser Raman differential absorption lidar (DIAL) for ozone measurements in clouds is proposed. An injection-locked XeCl excimer laser serves as the radiation source. The ozone molecule number density is calculated from the differential absorption of the anti-Stokes rotational Raman return signals from molecular nitrogen and oxygen as the on-resonance wavelength and the vibrational-rotational Raman backscattering from molecular nitrogen or oxygen as the off-resonance wavelength. Model calculations show that the main advantage of the new rotational vibrational-rotational (RVR) Raman DIAL over conventional Raman DIAL is a 70-85% reduction in the wavelength-dependent effects of cloud-particle scattering on the measured ozone concentration; furthermore the complexity of the apparatus is reduced substantially. We describe a RVR Raman DIAL setup that uses a narrow-band interference-filter polychromator as the lidar receiver. Single-laser ozone measurements in the troposphere and lower stratosphere are presented, and it is shown that on further improvement of the receiver performance, ozone measurements in clouds are attainable with the filter-polychromator approach.     

Effect of the differential geometric form factor on differential absorption lidar measurements with topographical targets

When the integrated differential absorption lidar (DIAL) technique is used to perform concentration measurements over long distances, the alignment between on and off laser beams becomes important. Here, through analysis of alignment error and of the corresponding differential geometric form factor, the effect of misalignment between off and on lines on performance of integrated concentration measurements by a coaxial DIAL system is considered.     

Trace atmospheric SO2 measurement by multiwavelength curve-fitting and wavelength-optimized dual differential absorption lidar

We present a new differential absorption lidar (DIAL) method for atmospheric trace SO2 using multi-wavelength curve fitting. With this method we use five wavelengths around a SO2 absorption peak and obtain SO2 and O3 concentrations by fitting their absorption cross sections to measured DIAL and null results. A SO, concentration of 6 parts in 10(9) (ppb) was obtained for an altitude of 1050 m with 150-m range resolution. In addition, we optimized the wavelengths for dual-DIAL SO2 measurement and demonstrated a high sensitivity of <0.5 ppb with 300-m range resolution. Comparison of these two methods is also presented.     

Diode laser sensor for measurements of CO, CO(2), and CH(4) in combustion flows

A diode laser sensor has been applied to monitor CO, CO(2), and CH(4) in combustion gases with absorption spectroscopy and fast extraction-sampling techniques. Survey spectra of the CO 3nu band (R branch) and the 2nu(1) + 2nu(2)(0) + nu(3) CO(2) band (R branch) near 6350 cm(-1) and H(2)O lines from the nu(1) + 2nu(2) and 2nu(2) + nu(3) bands in the spectral region from 6345 to 6660 cm(-1) were recorded and compared with calculated spectra (from the HITRAN 96 database) to select optimum transitions for species detection. Species concentrations above a laminar, premixed, methane-air flame were determined from measured absorption in a fast-flow multipass absorption cell containing probe-sampled combustion gases; good agreement was found with calculated chemical equilibrium values.     

Absorption cross-sections of the C-h overtone of volatile organic compounds: 2 methyl-1,3-butadiene (isoprene), 1,3-butadiene, and 2,3-dimethyl-1,3-butadiene

Many molecules or transient radicals have well-documented absorption cross-sections in the ultraviolet (UV) region, but their absorption cross-sections in the near-infrared (NIR) region are much less often known and are difficult to measure. We propose a method to determine the unknown NIR absorption cross-sections using the known absorption cross-sections in the UV region, in which single-path UV absorption spectroscopy and NIR continuous wave cavity ringdown spectroscopy (cw-CRDS) are employed in a cross-arm reaction chamber for simultaneous measurements. Without knowing the actual sample partial pressures (or concentrations), the NIR absorption cross-sections can be accurately determined through the two sets of measurements. The method is demonstrated by measuring the NIR absorption cross-section of the first overtone of the asymmetric C-H stretch of 2-methyl-1,3-butadiene (isoprene) (3.24 (+/-0.16) x 10(-22) cm(2) molecule(-1)) at 1651.52 nm using the known value of the absorption cross-section at 220 nm. The diode laser wavelength was calibrated by atmospheric cavity ringdown spectra of CH(4), CO(2), and H(2)O. By comparison with sample pressure measurements, this method can also be used as a pressure calibration means for the reaction chamber, and this has been demonstrated with two additional measurements of the absorption cross-sections of 1,3-butadiene and 2,3-dimethyl-1,3-butadiene (2.50 (+/- 0.08) x 10(-22) and 2.82 (+/-0.16) x 10(-22) cm(2) molecule(-1), respectively) at 1651.52 nm. The applicability of the method to determining absorption cross-sections using the simultaneous measurements of cw-CRDS and single-path absorption spectroscopy is discussed.     

CO(2) laser-based differential absorption lidar system for range-resolved and long-range detection of chemical vapor plumes

A dual CO(2) laser-based differential absorption lidar (DIAL) system has been constructed and demonstrated for range-resolved mapping of chemical vapor plumes. The system acquires high range resolution through the use of plasma-shutter pulse clippers that extinguish the nitrogen tail of the CO(2)-laser output. Aprogrammable servomotor-driven scanner allows full hemispherical coverage of the interrogated field. A high-speed direct-detection receiver subsystem is used to gather, process, and display vapor-concentration data in near real time. Data demonstrating range-resolved detection of low concentrations of chemical plumes from ranges of 1 to 2 km are presented. In the column-content detection mode, trace levels of secondary vapors from various organophosphate liquids were monitored. Detection of an SF(6) vapor plume released 16 km from the DIAL system is also adduced.     

NASA multipurpose airborne DIAL system and measurements of ozone and aerosol profiles

An airborne differential absorption lidar (DIAL) system has been developed for the remote measurement of gas and aerosol profiles in the troposphere and lower stratosphere. The multipurpose DIAL system can operate from 280 to 1064 nm for measurements of ozone, sulfur dioxide, nitrogen dioxide, water vapor, temperature,pressure, and aerosol backscattering. The laser transmitter consists of two narrow linewidth Nd: YAG pumped dye lasers with automatic wavelength control. The DIAL wavelengths are transmitted with a 00-,usec temporal separation to reduce receiver system complexity. A coaxial receiver system is used to collect and optically separate the DIAL and aerosol lidar returns. Photomultiplier tubes detect the backscattered laser returns after optical filtering, and the analog signals from three tubes are digitized and stored on high-speed magnetic tape. Real-time gas concentration profiles or aerosol backscatter distributions are calculated and displayed for experiment control. Operational parameters for the airborne DIAL system are presented for measurements of ozone, water vapor, and aerosols in the 290-, 720-, and 600-nm wavelength regions, respectively. The first ozone profile measurements from an aircraft using the DIAL technique are discussed in this paper. Comparisons between DIAL and in situ ozone measurements show agreement to within +/-5 ppbv in the lower troposphere. Lidar aerosol data obtained simultaneously with DIAL ozone measurements are presented for a flight over Virginia and the Chesapeake Bay. DIAL system performance for profiling ozone in a tropopause folding experiment is evaluated, and the applications of the DIAL system to regional and global-scale tropospheric investigations are discussed.     

CO的第二泛频(3←0)跃迁谱线线形强度测量研究

CO分子是监测大气污染气体的优异示踪气体,要实现对CO分子实时监控就需要做到对气体浓度的精确快速测量。气体分子浓度测量可以利用测量吸收光谱和谱线线形强度得到,CO的(3←0)泛频谱带是吸收较弱的跃迁波段,利用以干空气为缓冲气体的200μmol/mol的CO混合物,基于稳频的光腔衰荡装置测量了在温度293K、压力13~93kPa下的CO分子R支3条跃迁谱线的吸收光谱。HTP(Hartmann-Tran profile)线形被用来获得这些谱线的线形强度,测量结果的相对标准不确定度优于1%,与国际HITRAN、HITEMP和GEISA光谱数据库比较,相对偏差小于4%。     

Wavelength Calibrations in the Far Infrared (30 to 1000 Microns)

A discussion is presented of certain calibration procedures employed in the region 30 to 1000 microns. Calculated positions for the pure rotational absorption lines of the CO, HCN, and N₂O molecules are given, and a map of the pure rotational absorption lines of the H₂O molecule as recorded with a Perkin-Elmer model 301 spectrophotometer is shown.     

SPIRALE: a multispecies in situ balloonborne instrument with six tunable diode laser spectrometers

The balloonborne SPIRALE (a French acronym for infrared absorption spectroscopy by tunable diode lasers) instrument has been developed for in situ measurements of several tracer and chemically active species in the stratosphere. Laser absorption takes place in an open Herriott multipass cell located under the balloon gondola, with six lead salt diode lasers as light sources. One mirror is located at the extremity of a deployable mast 3.5 m below the gondola, enabling the measurement of very low abundance species throughout a very long absorption path (up to 544 m). Three successful flights have produced concentration measurements of O3, CO, CO2, CH4, N2O, NO2, NO, HNO3, HCl, HOCl, COF2, and H2O2. Fast measurements (every 1.1 s) allow one to obtain a vertical resolution of 5 m for the profiles. A detection limit of a few tens of parts per trillion in volume has been demonstrated. Uncertainties of 3%-5% are estimated for the most abundant species rising to about 30% for the less abundant ones, mainly depending on the laser linewidth and the signal-to-noise ratio.     

Ground-based differential absorption lidar for water-vapor and temperature profiling: development and specifications of a high-performance laser transmitter

An all-solid-state laser transmitter for a water-vapor and temperature differential absorption lidar (DIAL) system in the near infrared is introduced. The laser system is based on a master-slave configuration. As the slave laser a Q-switched unidirectional alexandrite ring laser is used, which is injection seeded by the master laser, a cw Ti:sapphire ring laser. It is demonstrated that this laser system has, what is to my knowledge, the highest frequency stability (15 MHz rms), narrowest bandwidth (<40 MHz), and highest spectral purity (>99.99%) of all the laser transmitters developed to date in the near infrared. These specifications fulfill the requirements for water-vapor measurements with an error caused by laser properties of <5% and temperature measurements with an error caused by laser properties of <1 K in the whole troposphere. The specifications are maintained during long-term operation in the field. The single-mode operation of this laser system makes the narrow-band detection of the DIAL backscatter signal possible. Thus the system has the potential to be used for accurate temperature measurements and for simultaneous DIAL and Doppler wind measurements.     

High-resolution absorption coefficient and refractive index spectra of carbon monoxide gas at millimeter and submillimeter wavelengths

The use of dispersive Fourier transform techniques in interferometry allows the measurement of absorption coefficient and refractive index spectra with great precision. This paper presents the absorption coefficient and refractive index spectra of carbon monoxide (CO) gas at millimeter and submillimeter wavelengths. To assess rotational lines of CO, the gas was measured at four different pressures, giving insight into the behavior of the spectral lines with varying parameters. The measurements in this study demonstrate that varying the pressure of the gas affects only the amplitude of the absorption lines and not their exact position. This is critical in air pollution studies when trying to single out a specific gas from a field sample with unknown constituents.     

In Situ Combustion Measurements of CO(2) by Use of a Distributed-Feedback Diode-Laser Sensor Near 2.0 mum

High-resolution absorption measurements of CO(2) were made in a heated static cell and in the combustion region above a flat-flame burner for the development of an in situ CO(2) combustion diagnostic based on a distributed-feedback diode laser operating near 2.0 mum. Calculated absorption spectra of high-temperature H(2)O and CO(2) were used to find candidate transitions for CO(2) detection, and the R(50) transition at 1.997 mum (the nu(1) + 2nu(2) + nu(3) band) was selected on the basis of its line strength and its isolation from interfering high-temperature water absorption. Measurements of spectroscopic parameters such as the line strength, the self-broadening coefficient, and the line position were made for the R(50) transition, and an improved value for the line strength is reported. The combustion-product populations of CO(2) in the combustion region above a flat-flame burner were determined in situ to verify the measured spectroscopic parameters and to demonstrate the feasibility of the diode-laser sensor.     

Application of statistical methods to the determination of slope in lidar data

Assumptions made in the analysis of both Raman lidar measurements of aerosol extinction and differential absorption lidar (DIAL) measurements of an absorbing species are tested. Statistical analysis techniques are used to enhance the estimation of aerosol extinction and aerosol extinction error that is usually handled using a linear model. It is determined that the most probable extinction value can differ from that of the linear assumption by up to 10% and that differences larger than 50% can occur in the calculation of extinction error. Ignoring error in the number density alters the calculated extinction by up to 3% and that of extinction error by up to 10%. The preceding results were obtained using the least-squares technique. The least-squares technique assumes that the data being regressed are normally distributed. However, the quantity that is usually regressed in aerosol extinction and DIAL calculations is not normally distributed. A technique is presented that allows the required numerical derivative to be determined by regressing only normally distributed data. The results from this technique are compared with the usual procedure. The same concerns raised here regarding appropriate choice of a model in the context of aerosol extinction calculations should apply to DIAL calculations of absorbing species such as water vapor or ozone as well because the numerical derivative that is required is identical.