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.     

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.     

Sensitivity analysis of differential absorption lidar measurements in the mid-infrared region

The availability of new laser sources that are tunable in the IR spectral region opens new perspectives for differential absorption lidar (DIAL) measurements. A region of particular interest is located in the near IR, where some of the atmospheric pollutants have absorption lines that permit monitoring of emissions from industrial plants and in urban areas. In DIAL measurements, the absorption lines for the species to be measured must be carefully chosen to prevent interference from other molecules, to minimize the dependence of the absorption cross section on temperature, and to optimize the measurements with respect to the optical depth. We analyze the influence of these factors and discuss a set of criteria for selecting the best pairs of wavelengths (lambda(on) and lambda(off)) to be used in DIAL measurements of several molecular species (HCl, CO, CO(2), NO(2), CH(4), H(2)O, and O(2)). Moreover, a sensitivity study has been carried out for selected lines in three different regimes: clean air, urban polluted air, and emission from an incinerator stack.     

Lidar aerosol backscatter cross sections in the 2-νm near-infrared wavelength region

Lidar backscatter cross-sectional measurements at 1.064, 0.532, and 1.54 μm were acquired during November 1989 and May-June 1990 around the Pacific region by the NASA DC-8 aircraft as part of the Global Backscatter Experiment. The primary motivation for the Global Backscatter Experiment was the study of lidar backscatter cross sections for the development of a spaceborne wind-sensing lidar. Direct backscatter measurements obtained by the NASA Goddard Space Flight Center visible and infrared lidar are compared with backscatter cross sections calculated from aerosol size distributions obtained by particle counters. Results for one flight with pronounced aerosol layers in the upper troposphere southeast of Japan are presented. Because 2-μm region wavelengths are possible candidates for a spaceborne wind-sensing lidar, the visible and infrared lidar backscatter cross sections at 1.064, 0.532, and 1.54 μm are extrapolated to the 2-μm region. The extrapolated 2-μm cross sections are compared with lidar measurements at 9 μm. A significant range in the ratio of 2-9-μm backscatter cross sections is found, but a large number of points concentrate near ratios of three to ten. A large number of 1.064- and 1.54-μm cross sections were binned to provide an estimate of backscatter for various percentiles for the flight. The ratio of the 50-percentile backscatter values at 1.064 and 1.54 μm suggest a λ(-1.9) to λ(-3.0) wavelength dependence of aerosol backscatter cross section in the near infrared for the observational case.     

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.     

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.     

Error analysis of DIAL measurements of ozone by a Shuttle excimer lidar

An error analysis of DIAL (differential absorption lidar) measurements of stratospheric ozone from the Space Shuttle is discussed. A transmitter system consisting of a KrF excimer laser pumping gas cells of H2 or D2 producing output wavelengths in the near UV is shown to be useful for the measurement of ozone in a 15-50-km altitude range.     

Single diode laser sensor for wide-range H2O temperature measurements

A single diode laser absorption sensor (near 1477 nm) useful for simultaneous temperature and H2O concentration measurements is developed. The diode laser tunes approximately 1.2 cm(-1) over three H2O absorption transitions in each measurement. The line strengths of the transitions are measured over a temperature range from 468 to 977 K, based on high-resolution absorption measurements in a heated static cell. The results indicate that the selected transitions are suitable for sensitive temperature measurements in atmospheric pressure combustion systems using absorption line ratios. Comparing the results with HITRAN 96 data, it appears that these transitions will be sensitive over a wide range of temperatures (450-2000 K), suggesting applicability for combustion measurements.     

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.     

Turbulence-induced measurement errors in coherent differential absorption lidar ground systems

The presence of atmospheric refractive turbulence makes it necessary to use simulations of beam propagation to examine the uncertainty added to the differential absorption lidar (DIAL) measurement process of a practical heterodyne lidar. The inherent statistic uncertainty of coherent return fluctuations in ground lidar systems profiling the atmosphere along slant paths with large elevation angles translates into a lessening of accuracy and sensitivity of any practical DIAL measurement. This technique opens the door to consider realistic, nonuniform atmospheric conditions for any DIAL instrument configuration.     

Future performance of ground-based and airborne water-vapor differential absorption lidar. I. Overview and theory

The performance of a future advanced water-vapor differential absorption lidar (DIAL) system is discussed. It is shown that the system has to be a direct-detection system operating in the rhovarsigmatau band of water vapor in the 940-nm wavelength region. The most important features of the DIAL technique are introduced: its clear-air measurement capability, its flexibility, and its simultaneous high resolution and accuracy. It is demonstrated that such a DIAL system can contribute to atmospheric sciences over a large range of scales and over a large variety of humidity conditions. An extended error analysis is performed, and errors (e.g., speckle noise) are included that previously were not been discussed in detail and that become important for certain system designs and measurement conditions. The applicability of the derived equation is investigated by comparisons with real data. Excellent agreement is found.     

Solar actinic flux spectroradiometry: a technique for measuring photolysis frequencies in the atmosphere.

A spectroradiometer has been developed for direct measurement of the solar actinic UV flux (scalar intensity) and determination of photolysis frequencies in the atmosphere. The instrument is based on a scanning double monochromator with an entrance optic that exhibits an isotropic angular response over a solid angle of 2pi sr. Actinic flux spectra are measured at a resolution of 1 nm across a range of 280-420 nm, which is relevant for most tropospheric photolysis processes. The photolysis frequencies are derived from the measured radiation spectra by use of published absorption cross sections and quantum yields. The advantage of this technique compared with the traditional chemical actinometry is its versatility. It is possible to determine the photolysis frequency for any photochemical reaction of interest provided that the respective molecular photodissociation parameters are known and the absorption cross section falls within a wavelength range that is accessible by the spectroradiometer. The instrument and the calibration procedures are described in detail, and problems specific to measurement of the actinic radiation are discussed. An error analysis is presented together with a discussion of the spectral requirements of the instrument for accurate measurements of important tropospheric photolysis frequencies (J(O(1))(D), J(NO(2)), J(HCHO)). An example of measurements from previous atmospheric chemistry field campaigns are presented and discussed.     

Absorption and emission cross sections of Er(3+) in Al(2)O(3) waveguides

Al(2)O(3) slab waveguide films were doped with erbium using ion implantation to a peak concentration of 1.5 at. %. Prism coupling measurements show absorption caused by (4)I (15/2) ?(4)I (13/2) intra-4f transitions in Er(3+) with a maximum at 1.530 mum of 8 dB/cm. The Er(3+) absorption cross section is determined as a function of wavelength. We used the McCumber theory to derive the emission cross section spectrum from the absorption results, which we then compared with the Er(3+) photoluminescence spectrum. The peak absorption and emission cross sections are found to be 6 x 10(-21) cm(-2). The results are used to predict the optical gain performance of an Er-doped Al(2)O(3) optical amplifier that operates around 1.5 mum.     

Future Performance of Ground-Based and Airborne Water-Vapor Differential Absorption Lidar. II. Simulations of the Precision of a Near-Infrared, High-Power System

Taking into account Poisson, background, amplifier, and speckle noise, we can simulate the precision of water-vapor measurements by using a 10-W average-power differential absorption lidar (DIAL) system. This system is currently under development at Hohenheim University, Germany, and at the American National Center for Atmospheric Research. For operation in the 940-nm region, a large set of measurement situations is described, including configurations that are considered for the first time to the authors' knowledge. They include ultrahigh-resolution measurements in the surface layer (resolutions, 1.5 m and 0.1 s) and vertically pointing measurements (resolutions, 30 m and 1 s) from the ground to 2 km in the atmospheric boundary layer. Even during daytime, the DIAL system will have a measurement range from the ground to the upper troposphere (300 m, 10 min) that can be extended from a mountain site to the lower stratosphere. From the ground, for the first time of which the authors are aware, three-dimensional fields of water vapor in the boundary layer can be investigated within a range of the order of 15 km and with an averaging time of 10 min. From an aircraft, measurements of the atmospheric boundary layer (60 m, 1 s) can be performed from a height of 4 km to the ground. At higher altitudes, up to 18 km, water-vapor profiles can still be obtained from aircraft height level to the ground. When it is being flown either in the free troposphere or in the stratosphere, the system will measure horizontal water-vapor profiles up to 12 km. We are not aware of another remote-sensing technique that provides, simultaneously, such high resolution and accuracy.     

Aerosol and cloud backscatter at 1.06, 1.54, and 0.53 mum by airborne hard-target-calibrated Nd:YAG /methane Raman lidar

A lidar instrument was developed to make simultaneous measurements at three distinct wavelengths in the visible and near infrared at 0.532, 1.064, and 1.54 mum with high cross-sectional calibration accuracy. Aerosol and cloud backscatter cross sections were acquired during November and December 1989 and May and June 1990 by the NASA DC-8 aircraft as part of the Global Backscatter Experiment. The instrument, methodology, and measurement results are described. A Nd:YAG laser produced 1.064- and 0.532-mum energy. The 1.54-mum transmitted pulse was generated by Raman-shifted downconversion of the 1.064-mum pulse through a Raman cell pressured with methane gas. The lidar could be pointed in the nadir or zenith direction from the aircraft. A hard-target-based calibration procedure was used to obtain the ratio of the system calibration between the three wavelengths, and the absolute calibration was referenced to the 0.532-mum lidar molecular backscatter cross section for the clearest scattering regions. From the relative wavelength calibration, the aerosol backscatter cross sections at the longer wavelengths are resolved for values as small as 1% of the molecular cross section. Backscatter measurement accuracies are better than 10(-9) (m sr)(-1) at 1.064 and 1.54 mum. Results from the Pacific Ocean region of the multiwavelength backscatter dependence are presented. Results show extensive structure and variation for the aerosol cross sections. The range of observed aerosol cross section is over 4 orders of magnitude, from less than 10(-9) (m sr)(-1) to greater than 10(-5) (m sr)(-1).     

Wide-range sounding of free-tropospheric water vapor with a differential-absorption lidar (DIAL) at a high-altitude station

A differential absorption lidar (DIAL) system has been developed for the measurement of water vapor throughout the free troposphere [3 to 12 km above sea level (asl.)] with high vertical resolution varied from 50 m next to the ground to 300 m above an altitude of 10 km. The system was installed at the Schneefernerhaus high-altitude research station (2675 m asl., Zugspitze, Germany). The DIAL system is based on a tunable single-mode laser system with a high pulse energy of currently 250 mJ and a repetition rate of 20 s(-1). For lidar operation with energies typically between 100 mJ and 150 mJ and an integration time of 1000 s (10000 laser shots for both DIAL wavelengths) a vertical range of at least 10 km has been demonstrated even under dry conditions and during daytime, while daytime measurements up to 12 km have been possible under humid conditions. The system was intercompared with radiosondes, which suggests an agreement within 5% in a major part of the operating range. Further improvements are planned in the upper troposphere to approach the accuracy requirements needed in climate research.     

Modeling of gas absorption cross sections by use of principal-component-analysis model parameters

Monitoring the amount of gaseous species in the atmosphere and exhaust gases by remote infrared spectroscopic methods calls for the use of a compilation of spectral data, which can be used to match spectra measured in a practical application. Model spectra are based on time-consuming line-by-line calculations of absorption cross sections in databases by use of temperature as input combined with path length and partial and total pressure. It is demonstrated that principal component analysis (PCA) can be used to compress the spectrum of absorption cross sections, which depend strongly on temperature, into a reduced representation of score values and loading vectors. The temperature range from 300 to 1000 K is studied. This range is divided into two subranges (300-650 K and 650-1000K), and separate PCA models are constructed for each. The relationship between the scores and the temperature values is highly nonlinear. It is shown, however, that because the score-temperature relationships are smooth and continuous, they can be modeled by polynomials of varying degrees. The accuracy of the data compression method is validated with line-by-line-calculated absorption data of carbon monoxide and water vapor. Relative deviations between the absorption cross sections reconstructed from the PCA model parameters and the line-by-line-calculated values are found to be smaller than 0.15% for cross sections exceeding 1.27 x 10(-21) cm(-1) atm(-1) (CO) and 0.20% for cross sections exceeding 4.03 x 10(-21) cm(-1) atm(-1) (H2O). The computing time is reduced by a factor of 10(4).     

Development of a Tunable, Narrow-Linewidth, CW 2.066-mum Ho:YLF Laser for Remote Sensing of Atmospheric CO(2) and H(2)O

A smoothly tunable, narrow-linewidth, cw, 32-mW, 2.066-mum Ho:YLF laser was constructed and used for the first time in preliminary spectroscopic measurements of atmospheric CO(2) and H(2)O. The laser was constructed with a 4.5-mm-long, TE-cooled, codoped 5% Tm and 0.5% Ho yttrium lithium fluoride crystal (cut at Brewster's angle) pumped by an Ar(+)-pumped 500-mW Ti:sapphire laser operating at 792 nm. Intracavity etalons were used to reduce the laser linewidth to approximately 0.025 cm(-1) (0.75 GHz), and the laser wavelength was continuously and smoothly tunable over approximately 6 cm(-1) (180 GHz). The Ho:YLF laser was used to perform spectroscopic measurements on molecular CO(2) in a laboratory absorption cell and to measure the concentration of CO(2) and water vapor in the atmosphere with an initial accuracy of approximately 5-10%. The measurement uncertainty was found to be due to several noise sources, including the effect of asymmetric intensity of the laser modes within the laser linewidth, fluctuations caused by atmospheric turbulence and laser beam/target movement, and background spectral shifts.     

Identification and correction of analog-to-digital-converter nonlinearities and their implications for differential absorption lidar measurements

Differential absorption lidar (DIAL) is a powerful remote-sensing technique widely used to probe the spatial and temporal distribution of ozone and other gaseous atmospheric trace constituents. Although conceptually simple, the DIAL technique presents many challenging and often subtle technical difficulties that can limit its useful range and accuracy. One potentially serious source of error for many DIAL experiments is nonlinearity in the analog-to-digital converters used to capture lidar return signals. The impact of digitizer nonlinearity on DIAL measurements is examined, and a simple and inexpensive low-frequency dithering technique that significantly reduces the effects of ADC nonlinearity in DIAL and other applications in which the signal is repetitively averaged is described.     

Ground-based differential absorption lidar for water-vapor profiling: assessment of accuracy, resolution, and meteorological applications

The accuracy and the resolution of water-vapor measurements by use of the ground-based differential absorption lidar (DIAL) system of the Max-Planck-Institute (MPI) are determined. A theoretical analysis, intercomparisons with radiosondes, and measurements in high-altitude clouds allow the conclusion that, with the MPI DIAL system, water-vapor measurements with a systematic error of <5% in the whole troposphere can be performed. Special emphasis is laid on the outstanding daytime and nighttime performance of the DIAL system in the lower troposphere. With a time resolution of 1 min the statistical error varies between 0.05 g/m(3) in the near range using 75 m and-depending on the meteorological conditions-approximately 0.25 g/m(3) at 2 km using 150-m vertical resolution. When the eddy correlation method is applied, this accuracy and resolution are sufficient to determine water-vapor flux profiles in the convective boundary layer with a statistical error of <10% in each data point to approximately 1700 m. The results have contributed to the fact that the DIAL method has finally won recognition as an excellent tool for tropospheric research, in particular for boundary layer research and as a calibration standard for radiosondes and satellites.