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.     

Extinction-to-backscatter ratio of Asian dust observed with high-spectral-resolution lidar and Raman lidar

Extinction-to-backscatter ratio or lidar ratio is a key parameter in the issue of backscatter-lidar inversions. The lidar ratio of Asian dust was observed with a high-spectral-resolution lidar and a combined Raman elastic-backscatter lidar during the springs of 1998 and 1999. The measured values range from 42 to55 sr in most cases, with a mean of 51 sr. These values are significantly larger than those predicted by the Mie computations that incorporate measured Asian dust size distributions and a range of refractive index with a typical value of 1.55-0.005i. The enhancement of lidar ratio is mostly due to the nonsphericity of dust particles, as indicated by the T-matrix calculations for spheroid particles and a number of other theoretical studies. In addition, possible contamination of urban aerosols may also contribute somewhat in optically thin cases. Mie theory, although it can well describe spherical particle scattering, will not be sufficient to represent the scattering characteristics of irregular particles such as Asian dust, especially in directions larger than approximately 90 degrees when the size parameter is large.     

Characteristics of aerosol optical properties in pollution and Asian dust episodes over Beijing, China

Aerosol optical properties were continuously measured with the National Institute for Environmental Studies (NIES) compact Raman lidar over Beijing, China, from 15 to 31 December 2007. The results indicated that in a moderate pollution episode, the averaged aerosol extinction below 1 km height was 0.39+/-0.15 km(-1) and the lidar ratio was 60.8+/-13.5 sr; in heavy pollution episode, they were 1.97+/-0.91 km(-1) and 43.7+/-8.3 sr; in an Asian dust episode, they were 0.33+/-0.11 km(-1) and 38.3+/-9.8 sr. The total depolarization ratio was mostly below 10% in the pollution episode, whereas it was larger than 20% in the Asian dust episode. The distinct characteristics of aerosol optical properties in moderate and heavy pollution episodes were attributed to the difference in air mass trajectory and the ambient atmospheric conditions such as relative humidity.     

Examination of the traditional raman lidar technique. II. Evaluating the ratios for water vapor and aerosols

In a companion paper [Appl. Opt. 42, 2571 (2003)] the temperature dependence of Raman scattering and its influence on the Raman and Rayleigh-Mie lidar equations were examined. New forms of the lidar equation were developed to account for this temperature sensitivity.Here those results are used to derive the temperature-dependent forms of the equations for the water vapor mixing ratio, the aerosol scattering ratio, the aerosol backscatter coefficient, and the extinction-to-backscatter ratio. The error equations are developed, the influence of differential transmission is studied, and several laser sources are considered in the analysis. The results indicate that the temperature functions become significant when narrowband detection is used. Errors of 5% and more can be introduced into the water-vapor mixing ratio calculation at high altitudes, and errors larger than 10% are possible for calculations of aerosol scattering ratio and thus of aerosol backscatter coefficient and of extinction-to-backscatter ratio.     

Lidar ratio and depolarization ratio for cirrus clouds

We report on studies of the lidar and the depolarization ratios for cirrus clouds. The optical depth and effective lidar ratio are derived from the transmission of clouds, which is determined by comparing the backscattering signals at the cloud base and cloud top. The lidar signals were fitted to a background atmospheric density profile outside the cloud region to warrant the linear response of the return signals with the scattering media. An average lidar ratio, 29 +/- 12 sr, has been found for all clouds measured in 1999 and 2000. The height and temperature dependences ofthe lidar ratio, the optical depth, and the depolarization ratio were investigated and compared with results of LITE and PROBE. Cirrus clouds detected near the tropopause are usually optically thin and mostly subvisual. Clouds with the largest optical depths were found near 12 km with a temperature of approximately -55 degrees C. The multiple-scattering effect is considered for clouds with high optical depths, and this effect lowers the lidar ratios compared with a single-scattering condition. Lidar ratios are in the 20-40 range for clouds at heights of 12.5-15 km and are smaller than approximately 30 in height above 15 km. Clouds are usually optically thin for temperatures below approximately -65 degrees C, and in this region the optical depth tends to decrease with height. The depolarization ratio is found to increase with a height at 11-15 km and smaller than 0.3 above 16 km. The variation in the depolarization ratio with the lidar ratio was also reported. The lidar and depolarization ratios were discussed in terms of the types of hexagonal ice crystals.     

Classification of particle effective shape ratios in cirrus clouds based on the lidar depolarization ratio

A shape classification technique for cirrus clouds that could be applied to future spaceborne lidars is presented. A ray-tracing code has been developed to simulate backscattered and depolarized lidar signals from cirrus clouds made of hexagonal-based crystals with various compositions and optical depth, taking into account multiple scattering. This code was used first to study the sensitivity of the linear depolarization rate to cloud optical and microphysical properties, then to classify particle shapes in cirrus clouds based on depolarization ratio measurements. As an example this technique has been applied to lidar measurements from 15 mid-latitude cirrus cloud cases taken in Palaiseau, France. Results show a majority of near-unity shape ratios as well as a strong correlation between shape ratios and temperature: The lowest temperatures lead to high shape ratios. The application of this technique to space-borne measurements would allow a large-scale classification of shape ratios in cirrus clouds, leading to better knowledge of the vertical variability of shapes, their dependence on temperature, and the formation processes of clouds.     

Calibration method for the lidar-observed stratospheric depolarization ratio in the presence of liquid aerosol particles

A fine calibration of the depolarization ratio is required for a detailed interpretation of lidar-observed polar stratospheric clouds. We propose a procedure for analyzing data by using atmospheric depolarization lidar. The method is based on a plot of deltaT versus (1 - RT(-1)), where deltaT is the total depolarization ratio and RT is the total backscattering ratio. Assuming that there are only spherical particles in some altitude ranges of the lidar data, the characteristics of the plot of deltaT versus (1 - RT(-1)) lead to a simple but effective calibration method for deltaT. Additionally, the depolarization of air molecules deltam can be determined in the process of deltaT calibration. We compared determined values with theoretically calculated values for the depolarization of air to test the proposed method. The deltam value was calculated from the lidar data acquired at Ny-Alesund (79 degrees N, 12 degrees E), Svalbard in winter 1994-1995. When only sulfate aerosols were present on 24 December 1994, deltam was 0.46 +/- 0.35%. When the particles consisted of sulfate aerosols and spherical particles of polar stratospheric clouds on 4 January 1995, deltam was 0.45 +/- 0.07%. Both deltam values were in good agreement with the theoretically calculated value, 0.50 +/- 0.03%.     

Characteristics of dust aerosols inferred from lidar depolarization measurements at two wavelengths

Lidar depolarization measurements were performed simultaneously at two wavelengths (532 and 1064 nm) in an Asian dust event. The observed particle depolarization ratio for 1064 nm was generally larger than that for 532 nm, and it was found that the mixing of Asian dust and other spherical aerosols must be taken into account. A simple two-component theory considering two types of aerosol (dust and spherical aerosols) was developed and applied to the observed data. The mixing ratio of dust and the backscatter-related Angstr?m exponents for dust and spherical aerosols was derived. These parameters can be used to infer characteristics of the aerosols and the mixed states.     

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.     

Statistical-uncertainty-based adaptive filtering of lidar signals

An adaptive filter signal processing technique is developed to overcome the problem of Raman lidar water-vapor mixing ratio (the ratio of the water-vapor density to the dry-air density) with a highly variable statistical uncertainty that increases with decreasing photomultiplier-tube signal strength and masks the true desired water-vapor structure. The technique, applied to horizontal scans, assumes only statistical horizontal homogeneity. The result is a variable spatial resolution water-vapor signal with a constant variance out to a range limit set by a specified signal-to-noise ratio. The technique was applied to Raman water-vapor lidar data obtained at a coastal pier site together with in situ instruments located 320 m from the lidar. The micrometeorological humidity data were used to calibrate the ratio of the lidar gains of the H(2)O and the N(2) photomultiplier tubes and set the water-vapor mixing ratio variance for the adaptive filter. For the coastal experiment the effective limit of the lidar range was found to be approximately 200 m for a maximum noise-to-signal variance ratio of 0.1 with the implemented data-reduction procedure. The technique can be adapted to off-horizontal scans with a small reduction in the constraints and is also applicable to other remote-sensing devices that exhibit the same inherent range-dependent signal-to-noise ratio problem.     

Development of a multiwavelength aerosol and water-vapor lidar at the Jungfraujoch Alpine Station (3580 m above sea level) in Switzerland

The Jungfraujoch Research Station (46.55 degrees N, 7.98 degrees E, 3580 m above sea level) for decades has contributed in a significant manner to the systematic observation of the Earth's atmosphere both with in situ measurements and with trace gas column detection. We report on the development of a lidar system that improves the measurement potential of highly resolved atmospheric parameters in both time and space, with the goal of achieving long-term monitoring of atmospheric aerosol optical properties and water-vapor content. From the simultaneously detected elastic-backscatter signals at 355, 532, and 1064 nm, Raman signals from nitrogen at 387 and 607 nm, and water vapor at 408 nm, the aerosol extinction and backscatter coefficients at three wavelengths and a water-vapor mixing ratio are derived. Additional information about particle shape is obtained by depolarization measurements at 532 nm. Water-vapor measurements by use of both nitrogen and water-vapor Raman returns from the 355-nm laser beam are demonstrated with a vertical range resolution of 75 m and an integration time of 2 h. The comparison to the water-vapor profile derived from balloon measurements (Snow White technique) showed excellent agreement. The system design and the results obtained by its operation are reported.     

Measurement of the lidar ratio for atmospheric aerosols with a 180 degrees backscatter nephelometer

Laser radar (lidar) can be used to estimate atmospheric extinction coefficients that are due to aerosols if the ratio between optical extinction and 180 degrees backscatter (the lidar ratio) at the laser wavelength is known or if Raman or high spectral resolution data are available. Most lidar instruments, however, do not have Raman or high spectral resolution capability, which makes knowledge of the lidar ratio essential. We have modified an integrating nephelometer, which measures the scattering component of light extinction, by addition of a backward-pointing laser light source such that the detected light corresponds to integrated scattering over 176-178 degrees at a common lidar wavelength of 532 nm. Mie calculations indicate that the detected quantity is an excellent proxy for 180 degrees backscatter. When combined with existing techniques for measuring total scattering and absorption by particles, the new device permits a direct determination of the lidar ratio. A four-point calibration, run by filling the enclosed sample volume with particle-free gases of a known scattering coefficient, indicates a linear response and calibration reproducibility to within 4%. The instrument has a detection limit of 1.5 x 10(-7) m(-1) sr(-1) (~10% of Rayleigh scattering by air at STP) for a 5-min average and is suitable for ground and mobile/airborne surveys. Initial field measurements yielded a lidar ratio of ~20 for marine aerosols and ~60-70 for continental aerosols, with an uncertainty of ~20%.     

Tropospheric aerosol optical properties derived from lidar, sun photometer, and optical particle counter measurements

Tropospheric aerosols have been observed for the period from November 1990 to April 1992 with a lidar, a sun photometer, and an optical particle counter. Variations of aerosol optical thickness derived from the lidar and the sun photometer data and measurements are presented. The simultaneous measurements of these instruments also allowed us to estimate the extinction-to-backscatter ratio (S(1)), which ranged from 20 to 70. Comparison of optical thicknesses derived from both instruments clearly shows the effect of Mt. Pinatubo's eruption and the temporal variation of optical thickness in the stratosphere over 12 km. The possible range of the complex refractive index for the columnar mean aerosols can be deduced from the probable range of S(1) derived by the use of an S(1) diagram as a function of complex refractive index (m). The imaginary part of m can be estimated provided that the real part of m is known.     

Investigation of the chemical mixing state of individual Asian dust particles by the combined use of electron probe X-ray microanalysis and Raman microspectrometry

In this work, quantitative electron probe X-ray microanalysis (EPMA) and Raman microspectrometry (RMS) were applied in combination for the first time to characterize the complex internal structure and physicochemical properties of the same ensemble of Asian dust particles. The analytical methodology to obtain the chemical composition, mixing state, and spatial distribution of chemical species within single particles through the combined use of the two techniques is described. Asian dust aerosol particles collected in Incheon, Korea, during a moderate dust storm event were examined to assess the applicability of the methodology to resolve internal mixtures within single particles. Among 92 individual analyzed particles, EPMA and RMS identified 53% of the particles to be internally mixed with two or more chemical species. Information on the spatial distribution of chemical compounds within internally mixed individual particles can be useful for deciphering the particle aging mechanisms and sources. This study demonstrates that the characterization of individual particles, including chemical speciation and mixing state analysis, can be performed more in detail using EPMA and RMS in combination than with the two single-particle techniques alone.     

Raman lidar monitoring of extinction and backscattering of African dust layers and dust characterization

Results on the monitoring of strong African dust outbreaks at Lecce in the southeastern corner of Italy (40 degrees 20' N, 18 degrees 6' E) during May 2001 are presented. This activity has been performed in the framework of the European Aerosol Research Lidar Network (EARLINET). The lidar station of Lecce is located on a flat rural area that is approximately 800 km from the northern Africa coast. So it is closer to Africa than most of all other EARLINET stations and allow monitoring African dust transport early in its life cycle, at all levels in the plume. An elastic-backscatter Raman lidar based on a XeF excimer laser (351 nm) has been used to monitor the time evolution and vertical structure of the dust layers and get independent measurements of the aerosol extinction and backscatter coefficients. The findings are presented in terms of vertical profiles of the extinction and backscatter coefficients and of the lidar ratio. A quite deep dust layer extending between 2 and 6 km and characterized by a backscatter coefficient of approximately 0.0016 (km sr)(-1), a lidar ratio of approximately 50 sr, and an aerosol optical depth of 0.26 was observed on 17 May 2001 between 18:55 and 20:07 UT. The layer persisted for approximately five days. Dust layers of lower optical thickness and shorter persistence time have generally been monitored at the lidar site during African dust outbreaks. Results on the chemical and morphological characterization of the dust collected at the lidar station are also given to further support the origin of the monitored aerosol layers.     

Aperture dependence of the mixing efficiency, the signal-to-noise ratio, and the speckle number in coherent lidar receivers

With the aid of the van Cittert-Zernike theorem we develop an analytical expression for the ensemble-averaged heterodyne mixing efficiency in coherent lidar receivers that are looking at a diffuse target that is in the receiver's far field. Our extremely simple and straightforward analysis shows that the dependence of the mixing efficiency on the receive aperture size d(R) first follows a parabolic decrease and later approaches a (d(R))(-2) function. As a consequence, the signal-to-noise ratio does not increase proportionally to the aperture area but saturates. For the system model chosen, the heterodyne mixing efficiency exhibits the same functional dependence on the lidar geometry as the reciprocal of the number of speckle cells within the receive aperture.     

Effects of particle size and region width on the mixing and dispersion of pebbles in two-region pebble bed

Granular systems and their mixing processes are widely used in various industries. The effects of size ratio and region width on the mixing and dispersion of pebbles in the two-region pebble bed are studied by discrete element method (DEM). The particle-scale mixing index (PSMI) and mixing entropy are used to quantify the particle mixing process. A similarity of mixing under different discharge rates is found after a stable two-region distribution structure is established. From qualitative observation and quantitative analysis, the mixing region is complicated in shape for the cases with greater particle size ratios. There is an increasing tendency of PSMI for two-region pebble bed when the region ratio or size ratio rises. The size ratio has greater effects on the mixing and dispersion of pebble than the region ratio, since the occupied volumes and entropies in the mixing region in the relatively steady state are more strongly affected by the size ratio rather than by the region ratio. As particles in the side regions can be easily driven by large ones, the stagnant region will decrease greatly when large size particles flow in the central region.     

Effects of mixing ratio and order of admixed particles with two diameters on improvement of compacted packing fraction

To improve particle flowability, a technique is used in which fine particles are admixed with the main particles. However, the effects of coating structure on the improvement in flowability are not yet fully understood. Thus, predicting the improvement resulting from this technique is difficult. In this study, we focused on the effects of the particle diameter distribution of the admixed particles on coating structures and improvement of flowability in terms of the compacted packing fraction in a particle bed. Main particles of size 397 nm with admixed particles of sizes 8 and 104 nm were used. Bimodal particle diameter distributions were adjusted by changing the mixing ratios of the two admixed particles. Furthermore, the main and admixed particles were mixed in various orders. We examined the compacted packing fractions for these different mixing ratios and orders. Scanning electron microscopy images were obtained in order to analyze the coating structures on the main particle surfaces. The results show that the main particle packing fraction was most greatly improved by pre-mixing the two admixed particles. This can be explained by a linked rigid-3-bodies model with leverage based on increasing the apparent diameter of the main particles.     

Examination of the traditional Raman lidar technique. I. Evaluating the temperature-dependent lidar equations

The essential information required for the analysis of Raman lidar water vapor and aerosol data acquired by use of a single laser wavelength is compiled here and in a companion paper [Appl. Opt. 42, 2593 (2003)]. Various details concerning the evaluation of the lidar equations when Raman scattering is measured are covered. These details include the influence of the temperature dependence of both pure rotational and vibrational-rotational Raman scattering on the lidar profile. The full temperature dependence of the Rayleigh-Mie and Raman lidar equations are evaluated by use of a new form of the lidar equation where all the temperature dependence is carried in a single term. The results indicate that, for the range of temperatures encountered in the troposphere, the magnitude of the temperature-dependent effect can reach 10% or more for narrowband Raman water-vapor measurements. Also, the calculation of atmospheric transmission, including the effects of depolarization, is examined carefully. Various formulations of Rayleigh cross-section determination commonly used in the lidar field are compared and reveal differences of as much as 5% among the formulations. The influence of multiple scattering on the measurement of aerosol extinction with the Raman lidar technique is considered, as are several photon pulse pileup-correction techniques.     

Cirrus cloud iridescence: a rare case study

On the evening of 25 November 1998, a cirrus cloud revealing the pastel colors of the iridescence phenomenon was photographed and studied by a polarization lidar system at the University of Utah Facility for Atmospheric Remote Sensing (FARS). The diffraction of sunlight falling on relatively minute cloud particles, which display spatial gradients in size, is the cause of iridescence. According to the 14-year study of midlatitude cirrus clouds at FARS, cirrus rarely produce even poor iridescent patches, making this particularly long-lived and vivid occurrence unique. In this unusually high (13.2-14.4-km) and cold (-69.7 degrees to -75.5 degrees) tropopause-topped cirrus cloud, iridescence was noted from approximately 6.0 degrees to approximately 13.5 degrees from the Sun. On the basis of simple diffraction theory, this indicates the presence of particles of 2.5-5.5-microm effective diameter. The linear depolarization ratios of delta = 0.5 measured by the lidar verify that the cloud particles were nonspherical ice crystals. The demonstration that ice clouds can generate iridescence has led to the conclusion that iridescence is rarely seen in midlatitude cirrus clouds because populations of such small particles do not exist for long in the presence of the relatively high water-vapor supersaturations needed for ice-particle nucleation.