Line-pair selections for remote sensing of atmospheric ammonia by use of a coherent CO2 differential absorption lidar system

Research on wavelength selection of CO2 laser lines for range-resolved remote sensing of atmospheric ammonia by use of a coherent differential absorption lidar system is described. Four laser line pairs are suggested for different levels of ammonia concentrations from approximately a few parts per billion to 1 part per million in a polluted atmosphere. The most suitable line for measuring ambient ammonia concentrations is 9R(30), because it has the highest absorption coefficient. 10R(14) has the lowest absorption coefficient, making it suitable for strong source mapping. 10R(8) and 10P(32) are best for intermediate levels of ammonia concentration. Absorption coefficients of ammonia calculated from the HITRAN96 database are in good agreement (mostly within +/-10% )with other experimental results.Sensitivity of measurement, interference from water-vapor lines with typical humidity in the summer,and sensitivity of ammonia absorption cross section to temperature and pressure are analyzed and calculated for the four wavelength pairs. The results show that the interference from water-vapor lines is easily correctable to a negligible amount, and errors caused by uncertainties in temperature and pressure are insignificant.     

Two-micrometer heterodyne differential absorption lidar measurements of the atmospheric CO2 mixing ratio in the boundary layer

A 2 microm heterodyne differential absorption lidar (HDIAL) has been operated at the Inst?tut Pierre Simon Laplace, Laboratoire de Météorologie Dynamique (Paris) to monitor the CO(2) mixing ratio in absolute value at high accuracy in the atmospheric boundary layer. Horizontal measurements at increasing range are made to retrieve the optical depth. The experimental setup takes advantage of a heterodyne lidar developed for wind velocity measurements. A control unit based on a photoacoustic cell filled with CO(2) is tested to correct afterward for ON-line frequency drift. The HDIAL results are validated using in situ routine measurements. The Doppler capability is used to follow the change in wind direction in the Paris suburbs.     

Coherent differential absorption lidar measurements of CO2

A differential absorption lidar has been built to measure CO2 concentration in the atmosphere. The transmitter is a pulsed single-frequency Ho:Tm:YLF laser at a 2.05-microm wavelength. A coherent heterodyne receiver was used to achieve sensitive detection, with the additional capability for wind profiling by a Doppler technique. Signal processing includes an algorithm for power measurement of a heterodyne signal. Results show a precision of the CO2 concentration measurement of 1%-2% 1sigma standard deviation over column lengths ranging from 1.2 to 2.8 km by an average of 1000 pulse pairs. A preliminary assessment of instrument sensitivity was made with an 8-h-long measurement set, along with correlative measurements with an in situ sensor, to determine that a CO2 trend could be detected.     

Sensitivity of radiometric measurements of the atmospheric CO2 column from space

Anthropogenic emissions of CO(2) over the past century has altered significantly the global carbon cycle. Our understanding of the long-term climatic effects of these emissions would be improved greatly by satellite-based remote sounding of CO(2). We provide an initial analysis of a simple satellite-based filter radiometer tuned to the spectral region around 6300 cm(-1) ( approximately 1.6 mum) to measure the atmospheric column of CO(2) from space. We find that such an instrument has potential and that the sensitivity would be limited by our knowledge of the tropospheric temperature and water-vapor profiles.     

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.     

An error estimate in the EFG method

In this paper, local and global error estimates for the element-free Galerkin (EFG) method are proposed. The essence of proposed error estimates is to use the difference between the values of the projected stress and these given directly by the EFG solution. The stress projection can be obtained simply by taking product of shape function based on a different domain of influence with the stresses at nodes. In this study, it was found that the effectivity index is optimized if the domain of influence in stress projection procedure is the smallest that retains regularity of the matrices in EFG. Numerical tests are shown for various 1D and 2D examples illustrating the good effectiveness of the proposed error estimator in the global energy norm and in the local error estimates.     

An estimate of the error of measuring sensitivity by the SINAD method

The limits of applicability of the SINAD method when measuring the signal-to-noise ratio, often used to estimate the sensitivity of receivers, are investigated. It is shown that if the systematic component of the error in measuring the harmonic coefficients of the generator being measured – the signal source – and of the high-frequency part of the receiver is ignored, there will be an unlimited increase in the error in measuring the sensitivity when the signal-to-noise ratio approaches the limiting value. The approach described enables the contribution to this error of components arising from distortions and noise of different origin to be separated.     

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.     

An a posteriori method based on photo-acoustic cell information to correct for lidar transmitter spectral shift: application to atmospheric CO(2) differential absorption lidar measurements

An a posteriori corrective method based on photo-acoustic cell (PAC) information is proposed to correct for laser transmitter spectral shift during atmospheric CO(2) measurements by 2 microm heterodyne differential absorption lidar (HDIAL) technique. The method for using the PAC signal to retrieve the actual atmospheric CO(2) absorption is presented in detail. This issue is tackled using a weighting function. The performance of the proposed corrective method is discussed and the various sources of error associated with the PAC signal are investigated. For 300 shots averaged and a frequency shift (from the CO(2) absorption line center) lower than the CO(2) absorption line half-width, the relative error on HDIAL CO(2) mixing ratio measurements is lower than 1.3%. The corrective method is validated in absolute value by comparison between HDIAL and in situ sensor measurements of CO(2).     

Ground-based imaging differential optical absorption spectroscopy of atmospheric gases

We describe a compact remote-sensing instrument that permits spatially resolved mapping of atmospheric trace gases by passive differential optical absorption spectroscopy (DOAS) and present our first applications of imaging of the nitrogen dioxide contents of the exhaust plumes of two industrial emitters. DOAS permits the identification and quantification of various gases, e.g., NO2, SO2, and CH2O, from their specific narrowband (differential) absorption structures with high selectivity and sensitivity. With scattered sunlight as the light source, DOAS is used with an imaging spectrometer that is simultaneously acquiring spectral information on the incident light in one spatial dimension (column). The second spatial dimension is scanned by a moving mirror.     

Spaceborne profiling of atmospheric temperature and particle extinction with pure rotational Raman lidar and of relative humidity in combination with differential absorption lidar: performance simulations

The performance of a spaceborne temperature lidar based on the pure rotational Raman (RR) technique in the UV has been simulated. Results show that such a system deployed onboard a low-Earth-orbit satellite would provide global-scale clear-sky temperature measurements in the troposphere and lower stratosphere with precisions that satisfy World Meteorological Organization (WMO) threshold observational requirements for numerical weather prediction and climate research applications. Furthermore, nighttime temperature measurements would still be within the WMO threshold observational requirements in the presence of several cloud structures. The performance of aerosol extinction measurements from space, which can be carried out simultaneously with temperature measurements by RR lidar, is also assessed. Furthermore, we discuss simulations of relative humidity measurements from space obtained from RR temperature measurements and water-vapor data measured with the differential absorption lidar (DIAL) technique.     

Numerical analysis and estimation of the statistical error of differential optical absorption spectroscopy measurements with least-squares methods

Differential optical absorption spectroscopy (DOAS) has become a widely used method to measure trace gases in the atmosphere. Their concentration is retrieved by a numerical analysis of the atmospheric absorption spectra, which often are a combination of overlapping absorption structures of several trace gases. A new analysis procedure was developed, modeling atmospheric spectra with the absorption structures of the individual trace gases, to determine their concentrations. The procedure also corrects differences in the wavelength-pixel mapping of these spectra. A new method to estimate the error of the concentrations considers the uncertainty of this correction and the influence of random residual structures in the absorption spectra.     

Influence of CO2-laser linewidth on the measured absorption coefficients of atmospheric water vapor and ammonia

We describe the results of analysis of the experimental and calculated data on the water vapor and ammonia absorption coefficients of CO(2)-laser radiation. We believe that the different halfwidths of CO(2)-laser lines, caused by different pressures of the working mixtures in specific experiments, are probably the reason for discrepancies between data presented in various papers.     

Experimental comparison of heterodyne and direct detection for pulsed differential absorption CO2 lidar

A pulsed dual-wavelength dual-CO2-laser differential-absorption lidar (DIAL) system has been developed which permits simultaneous heterodyne and direct detection of the same lidar returns. This system has been used to make an experimental comparison of the SNRs and statistical and temporal characteristics of the DIAL returns from several topographic targets. These results were found to be in general agreement with theory and were used to quantify the relative merits of the two detection techniques. The measured parameter values were applied to an analytical treatment to predict system trade-offs for the remote sensing of atmospheric species, with application to both path-averaged and range-resolved measurements.     

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.     

A postprocessed error estimate and an adaptive procedure for the semidiscrete finite element method in dynamic analysis

In the paper we present a postprocessed type of a posteriori error estimate and a h-version adaptive procedure for the semidiscrete finite element method in dynamic analysis. In space the super-convergent patch recovery technique is used for determining higher-order accurate stresses and, thus, a spatial error estimate. In time a postprocessing technique is developed for obtaining a local error estimate for one step time integration schemes (the HHT-α method). Coupling the error estimate with a mesh generator, a h-version adaptive finite element procedure is presented for two-dimensional dynamic analysis. It updates the spatial mesh and time step automatically so that the discretization errors are controlled within specified tolerances. Numerical studies on different problems are presented for demonstrating the performances of the proposed adaptive procedure.     

Atmospheric water vapor differential absorption measurements on vertical paths with a CO2 lidar

Ground based vertical path differential absorption measurements were obtained up to a height of 1.5 km with a CO2 lidar transmitting alternatively on the R(20) (10.247-microm) and R(18) (10.260-microm) lines during daylight in conditions of both strong and weak temperature inversions. The differential absorption between these lines for typical middle latitude lower atmosphere water vapor concentrations appears to be well suited to this type of measurement as the power loss on the more absorbed backscattered line [R(20)] is not too great as to unduly restrict the operating range, while the power differential is still sufficiently large to be readily measureable. In one set of measurements a strong temperature inversion at a height of 1 km resulted in a rapid vertical lapse in aerosol concentration with a consequent loss of SNR on the returns and severe distortion to the differential absorption profiles at this level. Water vapor profiles were derived from all measurements except in the region of the strong temperature inversion where the atmospheric backscattering cross section decayed rapidly. Reasonable results were obtained through the weak inversion region. The measurement capability of the lidar was found to be restricted by the length of the laser pulse tail and an inadequate signal-to-noise performance in regions of strong temperature inversions due to the associated decreases in aerosol concentration.     

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.