Air-water interactions: The signature of meteorological and air-quality parameters on the chemical characteristics of water produced from the atmosphere.

Atmospheric water is considered an alternative sustainable solution for global water scarcity. We analyzed the effects of meteorological and air-quality parameters on the chemical characteristics of atmospheric water. First, we measured the chemical characteristics of water produced by a unique atmospheric water generator (AWG) apparatus in Tel Aviv, Israel. To examine the complex air-water relationships, we obtained atmospheric data from several sources: adjacent air-quality-monitoring stations, aerosol robotic network (AERONET), aerosol pollution profile using PollyXT lidar, and air back-trajectory simulation (HYSPLIT). We found a strong impact of different pollution sources on the water quality. The integration between HYSPLIT, AERONET and lidar analyses shows that the pathway crossed by the air parcel three days before arrival at the site affected the chemical properties of the produced water. Nearby sea salt aerosols from the Mediterranean were persistently observed in the water (medians: sodium 69 µg/L, chloride ions 120 µg/L), corresponding to lidar identification of a sea-breeze layer (30-50 sr lidar ratio in lower elevation). Seasonal variability in climatic conditions affected the concentration of dust-related elements in the water. During dust-storm events, calcium was the most dominant element (median 900 µg/L). Thus, the chemical characteristics of the water can be considered a "footprint" of both regional, local, and phenological composition of the atmosphere.

Vertical profiles of pure dust and mixed smoke-dust plumes inferred from inversion of multiwavelength Raman/polarization lidar data and comparison to AERONET retrievals and in situ observations.

We present for the first time vertical profiles of microphysical properties of pure mineral dust (largely unaffected by any other aerosol types) on the basis of the inversion of optical data collected with multiwavelength polarization Raman lidar. The data were taken during the Saharan Mineral Dust Experiment (SAMUM) in Morocco in 2006. We also investigated two cases of mixed dust-smoke plumes on the basis of data collected during the second SAMUM field campaign that took place in the Republic of Cape Verde in 2008. Following the experience of the Aerosol Robotic Network (AERONET), the dust is modeled as a mixture of spherical particles and randomly oriented spheroids. The retrieval is performed from the full set of lidar input data (three backscatter coefficients, two extinction coefficients, and one depolarization ratio) and from a reduced set of data in which we exclude the depolarization ratio. We find differences of the microphysical properties depending on what kind of optical data combination we use. For the case of pure mineral dust, the results from these two sets of optical data are consistent and confirm the validity of the spheroid particle model for data inversion. Our results indicate that in the case of pure mineral dust we do not need depolarization information in the inversion. For the mixture of dust and biomass burning, there seem to be more limitations in the retrieval accuracy of the various data products. The evaluation of the quality of our data products is done by comparing our lidar-derived data products (vertically resolved) to results from AERONET Sun photometer observations (column-averaged) carried out at the lidar field site. Our results for dust effective radius show agreement with the AERONET observations within the retrieval uncertainties. Regarding the complex refractive index a comparison is difficult, as AERONET provides this parameter as wavelength-dependent quantity. In contrast, our inversion algorithm provides this parameter as a wavelength-independent quantity. We also show some comparison to results from airborne in situobservation. A detailed comparison to in situ results will be left for a future contribution.

Particle backscatter, extinction, and lidar ratio profiling with Raman lidar in south and north China.

Aerosol Raman lidar observations of profiles of the particle extinction and backscatter coefficients and the respective extinction-to-backscatter ratio (lidar ratio) were performed under highly polluted conditions in the Pearl River Delta (PRD) in southern China in October 2004 and at Beijing during a clear period with moderately polluted to background aerosol conditions in January 2005. The anthropogenic haze in the PRD is characterized by volume light-extinction coefficients of particles ranging from approximately 200 to 800 Mm(-1) and lidar ratios mostly between 40 and 55 sr (average of 47+/-6 sr). Almost clean air masses were observed throughout the measurements of the Beijing campaign. These air masses originated from arid desert-steppe-like regions (greater Gobi area). Extinction values usually varied between 100 and 300 Mm(-1), and the lidar ratios were considerably lower (compared with PRD values) with values mostly from 30 to 45 sr (average of 38+/-7 sr). Gobi dust partly influenced the observations. Unexpectedly low lidar ratios of approximately 25 sr were found for a case of background aerosol with a low optical depth of 0.05. The low lidar ratios are consistent with Mie-scattering calculations applied to ground-based observations of particle size distributions.

Particle backscatter and extinction profiling with the spaceborne high-spectral-resolution Doppler lidar ALADIN: methodology and simulations.

The European Space Agency will launch the Atmospheric Laser Doppler Instrument (ALADIN) for global wind profile observations in the near future. The potential of ALADIN to measure the optical properties of aerosol and cirrus, as well, is investigated based on simulations. A comprehensive data analysis scheme is developed that includes (a) the correction of Doppler-shifted particle backscatter interference in the molecular backscatter channels (cross-talk effect), (b) a procedure that allows us to check the quality of the cross-talk correction, and (c) the procedures for the independent retrieval of profiles of the volume extinction and backscatter coefficients of particles considering the height-dependent ALADIN signal resolution. The error analysis shows that the particle backscatter and extinction coefficients, and the corresponding extinction-to-backscatter ratio (lidar ratio), can be obtained with an overall (systematic+statistical) error of 10%-15%, 15%-30%, and 20%-35%, respectively, in tropospheric aerosol and dust layers with extinction values from 50 to 200 Mm(-1); 700-shot averaging (50 km horizontal resolution) is required. Vertical signal resolution is 500 m in the lower troposphere and 1000 m in the free troposphere. In cirrus characterized by extinction coefficients of 200 Mm(-1) and an optical depth of >0.2, backscatter coefficients, optical depth, and column lidar ratios can be obtained with 25%-35% relative uncertainty and a horizontal resolution of 10 km (140 shots). In the stratosphere, only the backscatter coefficient of aerosol layers and polar stratospheric clouds can be retrieved with an acceptable uncertainty of 15%-30%. Vertical resolution is 2000 m.

Ground-truth aerosol lidar observations: can the Klett solutions obtained from ground and space be equal for the same aerosol case?

Upcoming multiyear satellite lidar aerosol observations need strong support by a worldwide ground-truth lidar network. In this context the question arises as to whether the ground stations can deliver the same results as obtained from space when the Klett formalism is applied to elastic backscatter lidar data for the same aerosol case. This question is investigated based on simulations of observed cases of simple and complex aerosol layering. The results show that the differences between spaceborne and ground-based observations can be as large as 20% for the backscatter and extinction coefficients and the optimum estimates of the column lidar ratios. In cases with complex aerosol layering, the application of the two-layer approach can lead to similar results (space, ground) and accurate products provided that horizontally homogeneous aerosol conditions are given.

Potential of lidar backscatter data to estimate solar aerosol radiative forcing.

The potential to estimate solar aerosol radiative forcing (SARF) in cloudless conditions from backscatter data measured by widespread standard lidar has been investigated. For this purpose 132 days of sophisticated ground-based Raman lidar observations (profiles of particle extinction and backscatter coefficients at 532 nm wavelength) collected during two campaigns [the European Aerosol Research Lidar Network (EARLINET) and the Indian Ocean Experiment (INDOEX)] were analyzed. Particle extinction profiles were used as input for radiative transfer simulations with which to calculate the SARF, which then was plotted as a function of the column (i.e., height-integrated) particle backscatter coefficient (beta(c)). A close correlation between the SARF and beta(c) was found. SARF-beta(c) parameterizations in the form of polynomial fits were derived that exhibit an estimated uncertainty of +/-(10-30)%. These parameterizations can be utilized to analyze data of upcoming lidar satellite missions and for other purposes. The EARLINET-based parameterizations can be applied to lidar measurements at mostly continental, highly industrialized sites with limited maritime influence (Europe, North America), whereas the INDOEX parameterizations rather can be employed in polluted maritime locations, e.g., coastal regions of south and east Asia.

Daytime operation of a pure rotational Raman lidar by use of a Fabry-Perot interferometer.

We propose to use a Fabry-Perot interferometer (FPI) in a pure rotational Raman lidar to isolate return signals that are due to pure rotational Raman scattering from atmospheric nitrogen against the sky background. The main idea of this instrumental approach is that a FPI is applied as a frequency comb filter with the transmission peaks accurately matched to a comb of practically equidistant lines of a pure rotational Raman spectrum (PRRS) of nitrogen molecules. Thus a matched FPI transmission comb cuts out the spectrally continuous sky background light from the spectral gaps between the PRRS lines of nitrogen molecules while it is transparent to light within narrow spectral intervals about these lines. As the width of the spectral gaps between the lines of the PRRS of nitrogen molecules is -114 times the width of an individual spectral line, cutting out of the sky background from these gaps drastically improves the signal-to-background ratio of the pure rotational Raman lidar returns. This application of the FPI enables one to achieve daytime temperature profiling in the atmosphere with a pure rotational Raman lidar in the visible and near-UV spectral regions. We present an analysis of application of the FPI to filtering out the pure rotational Raman lidar returns against the solar background. To demonstrate the feasibility of the approach proposed, we present temperature profiles acquired during a whole-day measurement session in which a Raman lidar equipped with a FPI was used. For comparison, temperature profiles acquired with Vaisala radiosondes launched from the measurement site are also presented.

Aerosol lidar intercomparison in the framework of the EARLINET project. 3. Raman lidar algorithm for aerosol extinction, backscatter, and lidar ratio.

An intercomparison of the algorithms used to retrieve aerosol extinction and backscatter starting from Raman lidar signals has been performed by 11 groups of lidar scientists involved in the European Aerosol Research Lidar Network (EARLINET). This intercomparison is part of an extended quality assurance program performed on aerosol lidars in the EARLINET. Lidar instruments and aerosol backscatter algorithms were tested separately. The Raman lidar algorithms were tested by use of synthetic lidar data, simulated at 355, 532, 386, and 607 nm, with realistic experimental and atmospheric conditions taken into account. The intercomparison demonstrates that the data-handling procedures used by all the lidar groups provide satisfactory results. Extinction profiles show mean deviations from the correct solution within 10% in the planetary boundary layer (PBL), and backscatter profiles, retrieved by use of algorithms based on the combined Raman elastic-backscatter lidar technique, show mean deviations from solutions within 20% up to 2 km. The intercomparison was also carried out for the lidar ratio and produced profiles that show a mean deviation from the solution within 20% in the PBL. The mean value of this parameter was also calculated within a lofted aerosol layer at higher altitudes that is representative of typical layers related to special events such as Saharan dust outbreaks, forest fires, and volcanic eruptions. Here deviations were within 15%.

Aerosol lidar intercomparison in the framework of the EARLINET project. 2. Aerosol backscatter algorithms.

An intercomparison of aerosol backscatter lidar algorithms was performed in 2001 within the framework of the European Aerosol Research Lidar Network to Establish an Aerosol Climatology (EARLINET). The objective of this research was to test the correctness of the algorithms and the influence of the lidar ratio used by the various lidar teams involved in the EARLINET for calculation of backscatter-coefficient profiles from the lidar signals. The exercise consisted of processing synthetic lidar signals of various degrees of difficulty. One of these profiles contained height-dependent lidar ratios to test the vertical influence of those profiles on the various retrieval algorithms. Furthermore, a realistic incomplete overlap of laser beam and receiver field of view was introduced to remind the teams to take great care in the nearest range to the lidar. The intercomparison was performed in three stages with increasing knowledge on the input parameters. First, only the lidar signals were distributed; this is the most realistic stage. Afterward the lidar ratio profiles and the reference values at calibration height were provided. The unknown height-dependent lidar ratio had the largest influence on the retrieval, whereas the unknown reference value was of minor importance. These results show the necessity of making additional independent measurements, which can provide us with a suitable approximation of the lidar ratio. The final stage proves in general, that the data evaluation schemes of the different groups of lidar systems work well.

Relative-humidity profiling in the troposphere with a Raman lidar.

We describe a Raman-lidar-based approach to acquiring profiles of the relative humidity of air. For this purpose we combined in one instrument the Raman-lidar techniques that are used for the profiling of water vapor and temperature. This approach enabled us to acquire, for the first time to our knowledge, vertical profiles of relative humidity through the entire troposphere exclusively from Raman-lidar data. The methods applied to determining the water-vapor mixing ratio, temperature, and relative humidity and the corresponding uncertainties caused by systematic errors and signal noise are presented. The lidar-derived profiles are compared with profiles measured with radiosondes. Radiosonde observations are also used to calibrate the Raman lidar. Close agreement of the profiles of relative humidity measured with lidar and those measured with radiosonde demonstrates the potential of this novel approach.

Experimental determination of the lidar overlap profile with Raman lidar.

The range-dependent overlap between the laser beam and the receiver field of view of a lidar can be determined experimentally if a pure molecular backscatter signal is measured in addition to the usually observed elastic backscatter signal, which consists of a molecular component and a particle component. Two methods, the direct determination of the overlap profile and an iterative approach, are presented and applied to a lidar measurement. The measured overlap profile accounts for actual system alignment and for all system parameters that are not explicitly known, such as actual laser beam divergence and spatial intensity distribution of the laser light.