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.     

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.     

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.     

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.     

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.     

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.     

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.     

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.     

Analytical differentiation of the differential-absorption-lidar data distorted by noise

A method of analytical differentiation is developed for processing differential absorption lidar (DIAL) data. The method is based on simple analytical transformation of the DIAL on and off signal ratio. The derivatives consequently are found for either individual data points or local zones of the measurement range. The method makes possible the separation of local zones of interest and the separate investigation of these. The smoothing level is established by the selected value of the exponent in a transformation formula rather than by the selection of the resolution range. The method does not require the calculation of local signal increments. This reduces significantly the high-frequency noise in the measured concentration. The method is general and can be used for different experimental data, including inelastic (Raman) lidar data. The processing technique is practical and does not require a determination of the solution for a large set of algebraic equations. It is based on the simple repetition of the same type of calculations with different constants. The method can easily be implemented for practical computations.     

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.     

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.     

Room-temperature mid-infrared laser sensor for trace gas detection

Design and operation of a compact, portable, room-temperature mid-infrared gas sensor is reported. The sensor is based on continuous-wave difference-frequency generation (DFG) in bulk periodically poled lithium niobate at 4.6 mum, pumped by a solitary GaAlAs diode laser at 865 nm and a diode-pumped monolithic ring Nd:YAG laser at 1064.5 nm. The instrument was used for detection of CO in air at atmospheric pressure with 1 ppb precision (parts in 10(9), by mole fraction) and 0.6% accuracy for a signal averaging time of 10 s. It employed a compact multipass absorption cell with a 18-m path length and a thermoelectrically cooled HgCdTe detector. Precision was limited by residual interference fringes arising from scattering in the multipass cell. This is the first demonstration of a portable high-precision gas sensor based on diode-pumped DFG at room temperature. The use of an external-cavity diode laser can provide a tuning range of 700 cm(-1) and allow the detection of several trace gases, including N(2) O, CO(2), SO(2), H(2) CO, and CH(4).     

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.     

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.     

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.     

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.     

Optimum detection of multiple vapor materials with frequency-agile lidar

Differential absorption lidar (DIAL) is a well-established technology for estimating the concentration and its path integral CL of vapor materials using two closely spaced wavelengths. The recent development of frequency-agile lasers (FAL's) with as many as 60 wavelengths that can be rapidly scanned motivates the need for detection and estimation algorithms that are optimal for lidar employing these new sources. I derive detection and multimaterial CL estimation algorithms for FAL applications using the likelihood ratio test methodology of multivariate statistical inference theory. Three model sets of assumptions are considered with regard to the spectral properties of the backscatter from either topographic or aerosol targets. The calculations are illustrated through both simulated and actual lidar data.     

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.     

Optical properties of transparent nanocrystalline yttria stabilized zirconia

The optical properties of transparent nanocrystalline zirconia produced using a current activated method were characterized over the entire visible spectrum. The resolutions of the samples were characterized using standard resolution targets. All of the samples produced were found to have as high a resolution as detectable from the test, i.e., they are transparent not translucent. Transmission, reflectance, and absorption coefficients are reported for various wavelengths. The absorption coefficients were found to be highly dependent on processing time. Annealing experiments helped determine that oxygen vacancies (with free electrons) are the primary absorption centers in the visible wavelengths. In addition it was found that grain boundary cores or their associated defects do not contribute significantly to light absorption in the visible range. The lack of an influence of the grain boundary regions is discussed in terms of low oxygen vacancy concentration in the grain boundary space charge layer.     

Improvements of the aerosol algorithm in ozone lidar data processing by use of evolutionary strategies

The differential absorption lidar (DIAL) at the Institut für Meteorologie und Klimaforschung has been upgraded for precise ozone and aerosol studies in the entire troposphere and the lower stratosphere. Its excellent technical performance offers the opportunity to apply improved data processing. The existing inversion algorithm is extended to derive the optical coefficients from the backscatter profiles for three wavelengths. Correlating the correction terms of the DIAL equation and the ozone concentration yields the wavelength dependence of the backscatter and extinction coefficients of the aerosol. Under some conditions, in particular if homogeneous layers are present, the backscatter-to-extinction ratio and the reference value can also be retrieved. We find the solutions by applying evolutionary strategies. From the optical coefficients obtained in this way the ozone concentration can be calculated with substantially reduced error.