Ground‐based lidar measurements of aerosols during ACE‐2: instrument description, results, and comparisons with other ground‐based and airborne measurements

A micro‐pulse lidar system (MPL) was used to measure the vertical and horizontal distribution of aerosols during the Aerosol Characterization Experiment 2 (ACE‐2) in June and July of 1997. The MPL measurements were made at the Izaña observatory (IZO), a weather station located on a mountain ridge (28°18' N, 16°30' W, 2367 m asl) near the center of the island of Tenerife, Canary Islands. The MPL was used to acquire aerosol backscatter, extinction, and optical depth profiles for normal background periods and periods influenced by Saharan dust from North Africa. System tests and calibration procedures are discussed, and an analysis of aerosol optical profiles acquired during ACE‐2 is presented. MPL data taken during normal IZO conditions (no dust) showed that upslope aerosols appeared during the day and dissipated at night and that the layers were mostly confined to altitudes a few hundred meters above IZO. MPL data taken during a Saharan dust episode on 17 July showed that peak aerosol extinction values were an order of magnitude greater than molecular scattering over IZO, and that the dust layers extended to 5 km asl. The value of the dust backscatter–extinction ratio was determined to be 0.027±0.007 sr⁻¹. Comparisons of the MPL data with data from other co‐located instruments showed good agreement during the dust episode.     

Clear‐sky closure studies of lower tropospheric aerosol and water vapor during ACE‐2 using airborne sunphotometer, airborne in‐situ, space‐borne, and ground‐based measurements

We report on clear‐sky column closure experiments (CLEARCOLUMN) performed in the Canary Islands during the second Aerosol Characterization Experiment (ACE‐2) in June/July 1997. We present CLEARCOLUMN results obtained by combining airborne sunphotometer and in‐situ (optical particle counter, nephelometer, and absorption photometer) measurements taken aboard the Pelican aircraft, space‐borne NOAA/AVHRR data and ground‐based lidar and sunphotometer measurements. During both days discussed here, vertical profiles flown in cloud‐free air masses revealed 3 distinctly different layers: a marine boundary layer (MBL) with varying pollution levels, an elevated dust layer, and a very clean layer between the MBL and the dust layer. A key result of this study is the achievement of closure between extinction or layer aerosol optical depth (AOD) computed from continuous in‐situ aerosol size‐distributions and composition and those measured with the airborne sunphotometer. In the dust, the agreement in layer AOD (λ=380–1060 nm) is 3–8%. In the MBL there is a tendency for the in‐situ results to be slightly lower than the sunphotometer measurements (10–17% at λ=525 nm), but these differences are within the combined error bars of the measurements and computations.     

Polarising properties of the aerosols in the north‐eastern tropical Atlantic Ocean, with emphasis on the ACE‐2 period

Measurements of the polarisation state of the atmosphere were performed at Tenerife in June–July 1997, in the framework of ACE‐2 (second Aerosol Characterization Experiment), by 2 ground‐based instruments: RefPol (a LOA prototype) which took measurements at 445, 665, 870, 1610 nm in the solar principal plane; and an automatic CIMEL (CE 318) sun/sky‐photometer which measured polarised radiation at 870 nm in the same observational geometry. Measurements acquired during the campaign, as well as AERONET (AErosol RObotic NETwork) measurements acquired at the sites of Cape Verde and M'Bour, are processed with an algorithm determining the polarised single‐scattering sky‐radiance due to aerosols, directly proportional to the aerosol polarised phase function (representing the probability to scatter polarised radiation in the direction of the scattering angle). A good correlation between the Ångström exponent α, representing the spectral dependence of the extinction measurements, and the polarised phase function is observed on each set of data. The uncertainty of retrievals at 445 nm makes the determination of the spectral dependence of polarisation inconclusive but does not prevent confirming the dependence of the aerosol polarised phase function on α, at all wavelengths. An Ångström exponent of 1 corresponds to a polarised phase function of around 0.1 (±0.04), at 870 nm and at a scattering angle of 60°. For α between 0 and 0.4, the average value of the polarised phase function is 0.05. The correlation shows that polarisation is more sensitive to small particles than to large particles. The discrepancy between retrievals and Mie calculations from an AERONET size distribution, inverted from Izaña measurements acquired during a dust event, suggests the presence of small particles, not detected by total sky‐radiance measurements.     

Regional aerosol optical depth characteristics from satellite observations: ACE‐1, TARFOX and ACE‐2 results

Analysis of the aerosol properties during 3 recent international field campaigns (ACE‐1, TARFOX and ACE‐2) are described using satellite retrievals from NOAA AVHRR data. Validation of the satellite retrieval procedure is performed with airborne, shipboard, and land‐based sunphotometry during ACE‐2. The intercomparison between satellite and surface optical depths has a correlation coefficient of 0.93 for 630 nm wavelength and 0.92 for 860 nm wavelength. The standard error of estimate is 0.025 for 630 nm wavelength and 0.023 for 860 nm wavelength. Regional aerosol properties are examined in composite analysis of aerosol optical properties from the ACE‐1, TARFOX and ACE‐2 regions. ACE‐1 and ACE‐2 regions have strong modes in the distribution of optical depth around 0.1, but the ACE‐2 tails toward higher values yielding an average of 0.16 consistent with pollution and dust aerosol intrusions. The TARFOX region has a noticeable mode of 0.2, but has significant spread of aerosol optical depth values consistent with the varied continental aerosol constituents off the eastern North American Coast.     

The 2nd Aerosol Characterization Experiment (ACE‐2): meteorological and chemical context

A review is given of the climatological and actual meteorological conditions in the sub‐tropical northeast Atlantic, during June–July 1997, when the 2nd Aerosol Characterization Experiment (ACE‐2) took place. Surface pressure maps, trajectory calculations and in‐situ measurements show how the outflow of European pollution into the marine boundary layer of this area is determined by the location of the Azores high pressure cell. Observations during ACE‐2 and 3 preceding summers show that pollution outbreaks both from the Iberian peninsula and from northern or central Europe can occur during such situations. During ACE‐2, an unusually low number of strong North African dust outbreaks were recorded at the free tropospheric station of Izaña (Tenerife, 2360 m asl), although dust was recorded aloft the station.     

Measurements of aerosol optical depth above 3570 m asl in the North Atlantic free troposphere: results from ACE‐2

As part of the 2nd A erosol C haracterisation E xperiment (ACE‐2), conducted during summer 1997 in the North Atlantic region between the Canary Islands and Portugal, we measured aerosol optical depths (AOD) at a mid‐tropospheric site, near the top of the volcanic mountain "El Teide"(28°16'N, 16°36' W, 3570 m asl). Our instrument was located at the highest altitude in a network of sunphotometers that extended down to sea level. Clear conditions dominated the ACE‐2 period, and, although suggested by back‐trajectories at 300 hPa, no evidence of anthropogenic pollution was found in our data. Three distinct dust episodes were observed. Vertical soundings and back trajectories suggested mineral dust from the Sahel region as a source. During these episodes, AOD increased an order of magnitude with respect to background conditions (from 0.017 up to 0.19 at λ=500 nm). A shift towards neutrality of the extinction spectral dependence (Ångstrom exponent α down to 0.13), indicated that the coarse mode (particle diameter >2 μm) dominated the aerosol size distribution. For 6 days during the episodes of mineral dust, a monomodal size distribution between 2 and 20 μm diameter was obtained from Mie based size distribution calculations. Estimates, at 500 nm, of the single scattering albedo ω₀(0.87–0.96), and the aerosol asymmetry parameter g (0.72–0.73) suggest that the dust layer causes a net cooling forcing at the top of the atmosphere.     

Evolution of boundary‐layer aerosol particles due to in‐cloud chemical reactions during the 2nd Lagrangian experiment of ACE‐2

The second Aerosol Characterisation Experiment (ACE‐2) was aimed at investigating the physical, chemical and radiative properties of aerosol and their evolution in the North Atlantic region. In the 2nd "Lagrangian" experiment, an air mass was tracked over a 30‐h period during conditions of extensive stratocumulus cover. Boundary‐layer measurements of the aerosol size distribution obtained with a passive cavity aerosol spectrometer probe (PCASP) during the experiment show a gradual growth in size of particles in the 0.1–0.2 μm diameter mode. Simultaneously, SO₂ concentrations were found to decrease sharply from 800 to 20 ppt. The fraction of sulphate in aerosol ionic mass increased from 0.68±0.07 to 0.82±0.09 for small particles (diameter below 1.7 μm) and from 0.21±0.04 to 0.34±0.03 for large particles (diameter above 1.7 μm). The measurements were compared with a multicyclic parcel model of gas phase diffusion into cloud droplets and aqueous phase chemical reactions. The model was able to broadly reproduce the observed transformation in the aerosol spectra and the timescale for the transformation of SO₂ to sulphate aerosol. The modelled SO₂ concentration in the boundary layer fell to below half its initial value over a 6.5‐h time period due to a combination of the entrainment of cleaner tropospheric air and cloud chemical reactions. NH₃ and HCl gas were also found to play an important rôle in cloud processing in the model.     

Spatial distribution and optical properties of Saharan dust observed by airborne high spectral resolution lidar during SAMUM 2006

Airborne measurements of pure Saharan dust extinction and backscatter coefficients, the corresponding lidar ratio and the aerosol optical thickness (AOT) have been performed during the Saharan Mineral Dust Experiment 2006, with a high spectral resolution lidar. Dust layers were found to range from ground up to 4–6 km above sea level (asl). Maximum AOT values at 532 nm, encountered within these layers during the DLR Falcon research flights were 0.50–0.55. A significant horizontal variability of the AOT south of the High Atlas mountain range was observed even in cases of a well-mixed dust layer. High vertical variations of the dust lidar ratio of 38–50 sr were observed in cases of stratified dust layers. The variability of the lidar ratio was attributed to dust advection from different source regions. The aerosol depolarization ratio was about 30% at 532 nm during all measurements and showed only marginal vertical variations.     

Stratospheric aerosol measurements in the Arctic winter of 1996/1997 with the M‐55 Geophysika high‐altitude research aircraft

In‐situ aerosol measurements were performed in the northern hemispheric stratosphere up to altitudes of 21 km between 13 November 1996 and 14 January 1997, inside and outside of the polar vortex during the Airborne Polar Experiment (APE) field campaign. These are measurements of particle size distributions with a laser optical particle counter of the FSSP‐300 type operated during 9 flights on the Russian M‐55 high‐altitude research aircraft Geophysika. For specific flights, the FSSP‐300 measurements are compared with balloon‐borne data (launched from Kiruna, Sweden). It was found that the stratospheric aerosol content reached levels well below the background concentrations measured by the NASA operated ER‐2 in 1988/89 in the northern hemisphere. During the APE campaign, no PSC particle formation was observed at flight altitudes although the temperatures were below the NAT condensation point during one flight. The measured correlations between ozone and aerosol give an indication of the subsidence inside the 1996/97 polar vortex. Despite the lower aerosol content in the winter 1996/97 compared to the 1989 background, the heterogeneous reactivity of the aerosol (as calculated from the measured data with additional model input) is comparable. This is due to the dependency of the reactive uptake coefficients on the atmospheric water vapor content. Under the described assumptions the reaction rates on the background aerosol are significantly smaller than for competing gas phase chlorine activation, as can be expected for stratospheric background conditions especially inside the polar vortex.     

An overview of the ACE‐2 CLOUDYCOLUMN closure experiment

CLOUDYCOLUMN is one of the 6 ACE‐2 projects which took place in June‐July 1997, between Portugal and the Canary Islands. It was specifically dedicated to the study of changes of cloud radiative properties resulting from changes in the properties of those aerosols which act as cloud condensation nuclei. This process is also refered to as the aerosol indirect effect on climate. CLOUDYCOLUMN is focused on the contribution of stratocumulus clouds to that process. In addition to the basic aerosol measurements performed at the ground stations of the ACE‐2 project, 5 instrumented aircraft carried out in situ characterization of aerosol physical, chemical and nucleation properties and cloud dynamical and microphysical properties. Cloud radiative properties were also measured remotely with radiometers and a lidar. 11 case studies have been documented, from pure marine to significantly polluted air masses. The simultaneity of the measurements with the multi‐aircraft approach provides a unique data set for closure experiments on the aerosol indirect effect. In particular CLOUDYCOLUMN provided the 1st experimental evidence of the existence of the indirect effect in boundary layer clouds forming in polluted continental outbreacks. This paper describes the objectives of the project, the instrumental setup and the sampling strategy. Preliminary results published in additional papers are briefly summarized.     

Size‐segregated chemical, gravimetric and number distribution‐derived mass closure of the aerosol in Sagres, Portugal during ACE‐2

During the ACE‐2 field campaign in the summer of 1997 an intensive, ground‐based physical and chemical characterisation of the clean marine and continentally polluted aerosol was performed at Sagres, Portugal. Number size distributions of the dry aerosol in the size range 3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis. Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate the number size distribution at a relative humidity of 60%. A size segregated 3‐way mass closure study was performed in this investigation for the first time. Mass size distributions at 60% RH derived from number size distribution measurements and impactors samples (weighing and chemical analysis) are compared. A good agreement was found for the comparison of total gravimetrically‐determined mass with both number distribution‐derived (slope=1.23/1.09; R²>0.97; depending on the parameters humidity growth and density) and chemical mass concentration (slope=1.02; R²= 0.79) for particles smaller than 3 μm in diameter. Except for the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small deviations (R²=0.76–0.98) for the different size fractions were found. Since uncertainties in each of the 3 methods are about 20% the observed differences in the size‐segregated mass fractions can be explained by the measurement uncertainties. However, the number distribution‐derived mass is mostly higher than the chemically and gravimetrically determined mass, which can be explained by sampling losses of the impactor, but as well with measurement uncertainties as, e.g., the sizing of the DMPS/APS.     

Cloud condensation nuclei and cloud droplet measurements during ACE‐2

During the 2nd Aerosol Characterization Experiment (ACE‐2), relationships between stratocumulus cloud properties and aerosols were examined. Here, the relevant measurements including the cloud condensation nuclei (CCN) activation spectrum, updraft velocity, cloud microphysical and aerosol properties are presented. It is shown that calculations of droplet concentration based on updraft velocity and the CCN activation spectrum are consistent with direct observations. Also discussed is an apparent disparity among measurements of the CCN activation spectrum, the accumulation mode size distribution, and the composition of the submicrometric aerosol. The observed consistency between CCN, updraft and cloud droplets is a necessary refinement; however, extended analyses of the ACE‐2 data set are needed to guide improvements in model simulations of the interaction between aerosols and cloud microphysics. In particular, there is need for an examination of aerosol size spectra and chemical composition measurements with a view towards validating droplet activation schemes which relate the aerosol and cloud dynamical properties to cloud albedo.     

The SAMUM-1 experiment over Southern Morocco: overview and introduction

In May/June 2006, the largest mineral dust experiment to date (Saharan Mineral Dust Experiment, SAMUM-1) was conducted in Southern Morocco. The aim was to characterize dust particles near the world's largest mineral dust source, and to quantify dust-related radiative effects. At one of the two ground-based measurement sites dust particle size distribution, optical, hygroscopic, chemical and structural particle characteristics were measured. One research aircraft mainly measured solar spectral irradiances and surface albedo. The other aircraft provided in situ physical aerosol measurements and samples and lidar profiles through the dust layers. Three ground-based lidars were operated at the second ground-based measurement site. They determined optical dust properties, particle shape and temporal development of dust layers. Columnar, ground-based sun photometer measurements complemented the lidar data. Additionally a station in Évora, Portugal monitored dust outbreaks from the North African source region to the Iberian Peninsula during SAMUM-1.
Volumetric and columnar closure exercises utilized these detailed measurements of dust characteristics together with optical and radiative transfer models. Concurrent developments of a mesoscale dust transport model were validated with the experimental data. The paper gives an overview over rationale and design of SAMUM-1, introduces and highlights the subsequent reports on experimental and modelling results.     

Cloud optical thickness and albedo retrievals from bidirectional reflectance measurements of POLDER instruments during ACE‐2

The POLDER instrument is devoted to global observations of the solar radiation reflected by the Earth–atmosphere system. The airborne version of the instrument was operated during the ACE‐2 experiment, more particularly as a component of the CLOUDYCOLUMN project of ACE‐2 that was conducted in summer 1997 over the subtropical northeastern Atlantic ocean. CLOUDYCOLUMN is a coordinated project specifically dedicated to the study of the indirect effect of aerosols. In this context, the airborne POLDER was assigned to remote measurements of the cloud optical and radiative properties, namely the cloud optical thickness and the cloud albedo. This paper presents the retrievals of those 2 cloud parameters for 2 golden days of the campaign 26 June and 9 July 1997. Coincident spaceborne ADEOS‐POLDER data from 2 orbits over the ACE‐2 area on 26 June are also analyzed. 26 June corresponds to a pure air marine case and 9 July is a polluted air case. The multidirectional viewing capability of airborne POLDER is here demonstrated to be very useful to estimate the effective radius of cloud droplet that characterizes the observed stratocumulus clouds. A 12 μm cloud droplet size distribution appears to be a suitable cloud droplet model in the pure marine cloud case study. For the polluted case the mean retrieved effective droplet radius is of the order of 6–10 μm. This only preliminary result can be interpreted as a confirmation of the indirect effect of aerosols. It is consistent with the significant increase in droplet concentration measured in polluted marine clouds compared to clean marine ones. Further investigations and comparisons to in‐situ microphysical measurements are now needed.     

Aircraft observations of the microphysical and optical properties of major aerosol species

We summarise the microphysical and optical parameters of some principal aerosol species obtained by instrumentation on the UK Met Office C-130 aircraft during international field campaigns since 1996. The aerosol species include Saharan dust, biomass burning aerosol, European continental pollution, eastern seaboard USA pollution, and clean maritime aerosol. The typical structure of the aerosol in the vertical from each airmass type is described. Microphysical parameters are described that comprise the mode radius and geometric standard deviation associated with 2–3 lognormal fits to the mean observed aerosol size distributions spanning the accumulation and coarse modes. Optical parameters comprising the aerosol single scattering albedo (which was both measured and derived from Mie theory), specific extinction coefficient, and asymmetry factor (which were derived from Mie theory) are also presented. Where available, evolution of the physical and optical properties of the aerosol has been highlighted. Comparisons with long-term ground-based AERONET aerosol retrievals show reasonable agreement. Our observations provide useful data for validating and improving global circulation models (GCMs) that use physically based aerosol representation and for validating satellite retrievals of the physical and optical properties of aerosols.     

Desert dust aerosol air mass mapping in the western Sahara, using particle properties derived from space-based multi-angle imaging

Coincident observations made over the Moroccan desert during the Sahara mineral dust experiment (SAMUM) 2006 field campaign are used both to validate aerosol amount and type retrieved from multi-angle imaging spectroradiometer (MISR) observations, and to place the suborbital aerosol measurements into the satellite's larger regional context. On three moderately dusty days during which coincident observations were made, MISR mid-visible aerosol optical thickness (AOT) agrees with field measurements point-by-point to within 0.05–0.1. This is about as well as can be expected given spatial sampling differences; the space-based observations capture AOT trends and variability over an extended region. The field data also validate MISR's ability to distinguish and to map aerosol air masses, from the combination of retrieved constraints on particle size, shape and single-scattering albedo. For the three study days, the satellite observations (1) highlight regional gradients in the mix of dust and background spherical particles, (2) identify a dust plume most likely part of a density flow and (3) show an aerosol air mass containing a higher proportion of small, spherical particles than the surroundings, that appears to be aerosol pollution transported from several thousand kilometres away.     

Microphysical properties of stratocumulus clouds during ACE‐2

Microphysical measurements performed during 8 flights of the CLOUDYCOLUMN component of ACE‐2, with the Meteo‐France Merlin‐IV, are analyzed in terms of droplet number concentration and size. The droplet concentration is dependent upon the aerosol properties within the boundary layer. Its mean value over a flight varies from 55 cm⁻³, for the cleanest conditions, to 244 cm⁻³, for the most polluted one. For each flight, the variability of the concentration, in selected cloud regions that are not affected by mixing with dry air or drizzle scavenging, ranges from 0.5 to 1.5 of the mean value. The mean volume diameter increases with altitude above cloud base according to the adiabatic cloud model. The frequency distribution of mean droplet volume normalized by the adiabatic value, for the selected regions, shows the same dispersion as the distribution of normalized concentration. The values of droplet concentration versus mean volume diameter are then examined in sub‐adiabatic samples to characterize the effects of mixing and drizzle scavenging. Finally, the ratio of mean volume diameter to effective diameter is analyzed and a simple relationship between these 2 crucial parameters is proposed.     

State of mixing, shape factor, number size distribution, and hygroscopic growth of the Saharan anthropogenic and mineral dust aerosol at Tinfou, Morocco

The Saharan Mineral Dust Experiment (SAMUM) was conducted in May and June 2006 in Tinfou, Morocco. A H-TDMA system and a H-DMA-APS system were used to obtain hygroscopic properties of mineral dust particles at 85% RH. Dynamic shape factors of 1.11, 1.19 and 1.25 were determined for the volume equivalent diameters 720, 840 and 960 nm, respectively.
During a dust event, the hydrophobic number fraction of 250 and 350 nm particles increased significantly from 30 and 65% to 53 and 75%, respectively, indicating that mineral dust particles can be as small as 200 nm in diameter. Log-normal functions for mineral dust number size distributions were obtained from total particle number size distributions and fractions of hydrophobic particles. The geometric mean diameter for Saharan dust particles was 715 nm during the dust event and 570 nm for the Saharan background aerosol.
Measurements of hygroscopic growth showed that the Saharan aerosol consists of an anthropogenic fraction (predominantly non natural sulphate and carbonaceous particles) and of mineral dust particles. Hygroscopic growth and hysteresis curve measurements of the 'more' hygroscopic particle fraction indicated ammonium sulphate as a main component of the anthropogenic aerosol. Particles larger than 720 nm in diameter were completely hydrophobic meaning that mineral dust particles are not hygroscopic.     

Vertically resolved dust optical properties during SAMUM: Tinfou compared to Ouarzazate

Vertical profiles of dust key optical properties are presented from measurements during the Saharan Mineral Dust Experiment (SAMUM) by Raman and depolarization lidar at two ground-based sites and by airborne high spectral resolution lidar. One of the sites, Tinfou, is located close to the border of the Sahara in Southern Morocco and was the main in situ site during SAMUM. The other site was Ouarzazate airport, the main lidar site. From the lidar measurements the spatial distribution of the dust between Tinfou and Ouarzazate was derived for 1 d. The retrieved profiles of backscatter and extinction coefficients and particle depolarization ratios show comparable dust optical properties, a similar vertical structure of the dust layer, and a height of about 4 km asl at both sites. The airborne cross-section of the extinction coefficient at the two sites confirms the low variability in dust properties. Although the general picture of the dust layer was similar, the lidar measurements reveal a higher dust load closer to the dust source. Nevertheless, the observed intensive optical properties were the same. These results indicate that the lidar measurements at two sites close to the dust source are both representative for the SAMUM dust conditions.     

Vertical profiling of Saharan dust with Raman lidars and airborne HSRL in southern Morocco during SAMUM

Three ground-based Raman lidars and an airborne high-spectral-resolution lidar (HSRL) were operated during SAMUM 2006 in southern Morocco to measure height profiles of the volume extinction coefficient, the extinction-to-backscatter ratio and the depolarization ratio of dust particles in the Saharan dust layer at several wavelengths. Aerosol Robotic Network (AERONET) Sun photometer observations and radiosoundings of meteorological parameters complemented the ground-based activities at the SAMUM station of Ouarzazate. Four case studies are presented. Two case studies deal with the comparison of observations of the three ground-based lidars during a heavy dust outbreak and of the ground-based lidars with the airborne lidar. Two further cases show profile observations during satellite overpasses on 19 May and 4 June 2006. The height resolved statistical analysis reveals that the dust layer top typically reaches 4–6 km height above sea level (a.s.l.), sometimes even 7 km a.s.l.. Usually, a vertically inhomogeneous dust plume with internal dust layers was observed in the morning before the evolution of the boundary layer started. The Saharan dust layer was well mixed in the early evening. The 500 nm dust optical depth ranged from 0.2–0.8 at the field site south of the High Atlas mountains, Ångström exponents derived from photometer and lidar data were between 0–0.4. The volume extinction coefficients (355, 532 nm) varied from 30–300 Mm⁻¹ with a mean value of 100 Mm⁻¹ in the lowest 4 km a.s.l.. On average, extinction-to-backscatter ratios of 53–55 sr (±7–13 sr) were obtained at 355, 532 and 1064 nm.