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.     

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.     

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.     

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.     

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.     

Altitude range resolution of differential absorption lidar ozone profiles

A method is described for the empirical determination of altitude range resolutions of ozone profiles obtained by differential absorption lidar (DIAL) analysis. The algorithm is independent of the implementation of the DIAL analysis, in particular of the type and order of the vertical smoothing filter applied. An interpretation of three definitions of altitude range resolution is given on the basis of simulations carried out with the Jet Propulsion Laboratory ozone DIAL analysis program, SO3ANL. These definitions yield altitude range resolutions that differ by as much as a factor of 2. It is shown that the altitude resolution calculated by SO3ANL, and reported with all Jet Propulsion Laboratory lidar ozone profiles, corresponds closely to the full width at half-maximum of a retrieved ozone profile if an impulse function is used as the input ozone profile.     

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.     

Laser remote sensing of atmospheric ammonia using a CO2 lidar system

A CO2 differential-absorption lidar system has been used for the remote sensing of ammonia in the atmosphere. For CO2 lidar returns backscattered from topographic targets at ranges up to 2.7 km, the path-averaged sensitivity of the DIAL system was 5 ppb of NH3 . Concentrations of atmospheric ammonia were found to vary during the day from undetectable levels (<5 ppb) to as high as 20 ppb, depending on temperature and humidity conditions.     

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.     

Laser prf considerations in differential absorption lidar applications

Laser pulse repetition frequency (prf) is a major factor in determining the performance of differential absorption lidar (DIAL) systems. The effects of laser prf on concentration measurement accuracy and maximum usable range are quantified. Heterodyne-detection (coherent) and direct-detection (noncoherent) as well as path-averaged and range-resolved DIAL systems are analyzed.     

Sum-frequency-generation system for differential absorption lidar measurement of atmospheric nitrogen dioxide

A sum-frequency-generation system for differential absorption lidar measurement of atmospheric nitrogen dioxide in the lower troposphere was developed. The system uses a combination of a pair of KD*P crystals and a tunable dye laser with LDS 765 dye pumped by the second harmonic of a Nd:YAG laser to generate lambdaon and lambdaoff alternatively. Compared with the conventional system that uses Coumarin 445 dye pumped by the third harmonic, the output energy and long-term stability were improved. By use of this system, atmospheric NO2 concentrations of approximately 10-50 ppb were measured, with an instrumental error of approximately 7 ppb.     

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.     

Complementary study of differential absorption lidar optimization in direct and heterodyne detections

A detailed study using both analytical and numerical calculations of direct and heterodyne differential absorption lidar (DIAL) techniques is conducted to complement previous studies. The DIAL measurement errors depend on key experimental parameters, some of which can be adjusted to minimize the statistical error. Accordingly, the pertinent criteria on optical thickness, the number of photons emitted at the on and off wavelengths, are discussed to reduce the relative error on the total column content or range-resolved measurements that rely on either hard target or atmospheric backscatter returns. In direct detection, the optimal optical thickness decreases from 1.3 to 0.8 when the background increases while the on-line-to-off-line optimal energy ratio decreases from 3.6 to 2.7. In heterodyne detection, the minimum error is obtained for an optical thickness of 1.2 and an energy ratio of 4.3.     

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.     

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.     

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.     

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.     

Improved speckle statistics in coherent differential absorption lidar with in-fiber wavelength multiplexing

Remote detection of gaseous pollutants and other atmospheric constituents can be achieved with differential absorption lidar (DIAL) methods. The technique relies on the transmission of two or more laser wavelengths and exploits absorption features in the target gas by measuring the ratio of their detected powers to determine gas concentration. A common mode of operation is when the transmitter and receiver are collocated, and the absorption is measured over a return trip by a randomly scattering topographic target. Hence, in coherent DIAL, speckle fluctuation leads to a large uncertainty in the detected powers unless the signal is averaged over multiple correlation times, i.e., over many independent speckles. We examine a continuous-wave coherent DIAL system in which the laser wavelengths are transmitted and received by the same single-mode optical fibers. This ensures that the two wavelengths share a common spatial mode, which, for certain transmitter and target parameters, enables highly correlated speckle fluctuations to be readily achieved in practice. For a DIAL system, this gives the potential for improved accuracy in a given observation time. A theoretical analysis quantifies this benefit as a function of the degree of correlation between the two time series (which depends on wavelength separation and target depth). The results are compared with both a numerical simulation and a laboratory-based experiment.     

Monitoring O3 with solar-blind Raman lidars

The benefits of retrieving ozone concentration profiles by a use of a single Raman signal rather than the Raman differential absorption lidar (DIAL) technique are investigated by numerical simulations applied either to KrF- (248 nm) or to quadrupled Nd:YAG- (266 nm) based Raman lidars, which are used for both daytime and nighttime monitoring of the tropospheric water-vapor mixing ratio. It is demonstrated that ozone concentration profiles of adequate accuracy and spatial and temporal resolution can be retrieved under low aerosol loading by a single Raman lidar because of the large value of the ozone absorption cross section both at 248 nm and at 266 nm. Then experimental measurements of Raman signals provided by the KrF-based lidar operating at the University of Lecce (40 degrees 20'N, 18 degrees 6'E) are used to retrieve ozone concentration profiles by use of the Raman DIAL technique and the nitrogen Raman signal.