Haflidi H. Jonsson

The cloud, aerosol and precipitation spectrometer: a new instrument for cloud investigations

A new airborne particle spectrometer has been developed with the same measurement capabilities of the Forward Scattering Spectrometer Probes (FSSP) models 100 and 300 (FSSP-300 and FSSP-100), two-dimensional optical imaging probe (2D-OAP), the Multiangle Aerosol Spectrometer Probe (MASP) and hot-wire liquid water probe, but with a single integrated system. The cloud, aerosol and precipitation spectrometer (CAPS) measures particles from 0.35 μm to 1.55 mm in diameter and liquid water content (LWC) from 0.01 to 3 g m -3 . In addition to combining five probes into one, it measures airspeed at the sample volume and transmits a data stream that requires no special interfaces to communicate with most computers.

The 2D-S (Stereo) Probe: Design and Preliminary Tests of a New Airborne, High-Speed, High-Resolution Particle Imaging Probe

The design, laboratory calibrations, and flight tests of a new optical imaging instrument, the twodimensional stereo (2D-S) probe, are presented. Two orthogonal laser beams cross in the middle of the sample volume. Custom, high-speed, 128-photodiode linear arrays and electronics produce shadowgraph images with true 10-m pixel resolution at aircraft speeds up to 250 m s 1 . An overlap region is defined by the two laser beams, improving the sample volume boundaries and sizing of small (100 m) particles, compared to conventional optical array probes. The stereo views of particles in the overlap region can also improve determination of three-dimensional properties of some particles. Data collected by three research aircraft are examined and discussed. The 2D-S sees fine details of ice crystals and small water drops coexisting in mixed-phase cloud. Measurements in warm cumuli collected by the NCAR C-130 during the Rain in Cumulus over the Ocean (RICO) project provide a test bed to compare the 2D-S with 2D cloud (2D-C) and 260X probes. The 2D-S sees thousands of cloud drops 150 m when the 2D-C and 260X probes see few or none. The data suggest that particle images and size distributions ranging from 25 to 150 m and collected at airspeeds 100 m s 1 by the 2D-C and 260X probes are probably (erroneously) generated from out-of-focus particles. Development of the 2D-S is in its infancy, and much work needs to be done to quantify its performance and generate software to analyze data.

Particle Formation in the Upper Tropical Troposphere: A Source of Nuclei for the Stratospheric Aerosol

Atmospheric measurements and numerical calculations described here indicate that binary homogeneous nucleation of H2SO4-H2O particles occurs in the upper tropical troposphere. Particle concentrations decrease with increasing altitude above the tropical tropopause as a result of coagulation during the upward air transport produced by stratospheric circulations. During the extended periods of time that volcanic eruptions do not strongly influence stratospheric particle number concentrations, particles formed in the upper tropical troposphere provide nuclei upon which oxidized sulfur gases condense in the stratosphere. This particle source, coupled with aerosol microphysical properties and atmospheric transport, governs the number concentration of particles in the lower tropical and mid-latitude stratosphere.

Comparison of methods for deriving aerosol asymmetry parameter

Received 21 December 2004; revised 19 March 2005; accepted 7 June 2005; published 21 January 2006. [1] Values for Mie-equivalent aerosol asymmetry parameter (g) were derived using a variety of methods from the large suite of measurements (in situ and remote from surface and aircraft) made in Oklahoma during the 2003 aerosol Intensive Operations Period (IOP). Median values derived for dry asymmetry parameter at 550 nm ranged between 0.55 and 0.63 over all instruments and for all derivation methods, with the exception of one instrument which did not measure over the full size range of optically important aerosol. Median values for the ‘‘wet’’ asymmetry parameter (i.e., asymmetry parameter at humidity conditions closer to ambient) were between 0.59 and 0.72. Values for g derived for surface and airborne in situ measurements were highly correlated, but in situ and remote sensing measurements both at the surface and aloft did not agree as well because of vertical inhomogeneity of the aerosol. Radiative forcing calculations suggest that a 10% decrease in g would result in a 19% reduction in top of atmosphere radiative forcing for the conditions observed during the IOP. Comparison of the different methods for deriving g suggests that in computing the asymmetry parameter, aerosol size is the most important parameter to measure; composition is less important except for how it influences the hygroscopic growth (i.e., size) of particles.

Emission Measurements of the Concorde Supersonic Aircraft in the Lower Stratosphere

Emission indices of reactive gases and particles were determined from measurements in the exhaust plume of a Concorde aircraft cruising at supersonic speeds in the stratosphere. Values for NOx (sum of NO and NO2) agree well with ground-based estimates. Measurements of NOx and HOx indicate a limited role for nitric acid in the plume. The large number of submicrometer particles measured implies efficient conversion of fuel sulfur to sulfuric acid in the engine or at emission. A new fleet of supersonic aircraft with similar particle emissions would significantly increase stratospheric aerosol surface areas and may increase ozone loss above that expected for NOx emissions alone.

Oxalic acid in clear and cloudy atmospheres: Analysis of data from International Consortium for Atmospheric Research on Transport and Transformation 2004

inorganic ions (including SO4� ) and five organic acid ions (including oxalate) were measured on board the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter research aircraft by a particle-into-liquid sampler (PILS) during flights over Ohio and surrounding areas. Five local atmospheric conditions were studied: (1) cloud-free air, (2) power plant plume in cloud-free air with precipitation from scattered clouds overhead, (3) power plant plume in cloud-free air, (4) power plant plume in cloud, and (5) clouds uninfluenced by local pollution sources. The aircraft sampled from two inlets: a counterflow virtual impactor (CVI) to isolate droplet residuals in clouds and a second inlet for sampling total aerosol. A strong correlation was observed between oxalate and SO4� when sampling through both inlets in clouds. Predictions from a chemical cloud parcel model considering the aqueous-phase production of dicarboxylic acids and SO4� show good agreement for the relative magnitude of SO4� and oxalate growth for two scenarios: power plant plume in clouds and clouds uninfluenced by local pollution sources. The relative contributions of the two aqueous-phase routes responsible for oxalic acid formation were examined; the oxidation of glyoxylic acid was predicted to dominate over the decay of longer-chain dicarboxylic acids. Clear evidence is presented for aqueous-phase oxalic acid production as the primary mechanism for oxalic acid formation in ambient aerosols.

Constraining the contribution of organic acids and AMS m/z 44 to the organic aerosol budget: On the importance of meteorology, aerosol hygroscopicity, and region

Airborne measurements in regions of varying meteorology and pollution are used to quantify the contribution of organic acids and a mass spectral marker for oxygenated aerosols, m/z 44, to the total organic aerosol budget. Organic acids and m/z 44 separately are shown to exhibit their highest organic mass fractions in the vicinity of clouds. The contribution of such oxygenated species is shown to increase as a function of relative humidity, aerosol hygroscopicity (and decreasing organic mass fraction), and is typically greater off the California coast versus the continental atmospheres studied. Reasons include more efficient chemistry and partitioning of organic acid precursors with increasing water in the reaction medium, and high aqueous-phase processing times in boundary layers with higher cloud volume fractions. These results highlight the importance of secondary organic aerosol formation in both wet aerosols and cloud droplets.

Influence of Humidity On the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

Aerosol scattering coefficients (σsp) have been measured over the ocean at different relative humidities (RH) as a function of altitude in the region surrounding the Canary Islands during the Second Aerosol Characterization Experiment (ACE-2) in June and July 1997. The data were collected by the University of Washington passive humidigraph (UWPH) mounted on the Pelican research aircraft. Concurrently, particle size distributions, absorption coefficients and aerosol optical depth were measured throughout 17 flights. A parameterization of σsp as a function of RH was utilized to assess the impact of aerosol hydration on the upwelling radiance (normalized to the solar constant and cosine of zenith angle). The top of the atmosphere radiance signal was simulated at wavelengths corresponding to visible and near-infrared bands of the EOS-AM )“Terra” (detectors, MODIS and MISR. The UWPH measured σsp at 2 RHs, one below and the other above ambient conditions. Ambient σsp was obtained by interpolation of these 2 measurements. The data were stratified in terms of 3 types of aerosols: Saharan dust, clean marine (marine boundary layer background) and polluted marine aerosols (i.e., 2- or 1-day old polluted aerosols advected from Europe). An empirical relation for the dependence of σsp on RH, defined by σsp(RH)=k. (1−RH/100)−γ, was used with the hygroscopic exponent γ derived from the data. The following γ values were obtained for the 3 aerosol types: γ(dust)=0.23±0.05, γ(clean marine)= 0.69±0.06 and γ(polluted marine)=0.57±0.06. Based on the measured γs, the above equation was utilized to derive aerosol models with different hygroscopicities. The satellite simulation signal code 6S was used to compute the upwelling radiance corresponding to each of those aerosol models at several ambient humidities. For the pre-launch estimated precision of the sensors and the assumed viewing geometry of the instrument, the simulations suggest that the spectral and angular dependence of the reflectance measured by MISR is not sufficient to distinguish aerosol models with various different combinations of values for dry composition, γ and ambient RH. A similar behavior is observed for MODIS at visible wavelengths. However, the 2100 nm band of MODIS appears to be able to differentiate between at least same aerosol models with different aerosol hygroscopicity given the MODIS calibration error requirements. This result suggests the possibility of retrieval of aerosol hygroscopicity by MODIS.

The Marine Stratus/Stratocumulus Experiment (MASE): Aerosol‐cloud relationships in marine stratocumulus

The Marine Stratus/Stratocumulus Experiment (MASE) field campaign was undertaken in July 2005 off the coast of Monterey, California to evaluate aerosol-cloud relationships in the climatically important regime of eastern Pacific marine stratocumulus. Aerosol and cloud properties were measured onboard the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. One cloud that was clearly impacted by ship emissions as well as the ensemble of clouds observed over the entire mission are analyzed in detail. Results at both the individual and ensemble scales clearly confirm the Twomey effect (first indirect effect of aerosols) and demonstrate drizzle suppression at elevated aerosol number concentration. For the ship track impacted cloud, suppressed drizzle in the track led to a larger cloud liquid water path (LWP) at the same cloud thickness, in accord with the so-called second indirect effect. Ensemble averages over all clouds sampled over the entire 13-flight mission show the opposite effect of aerosol number concentration on LWP, presumably the result of other dynamic influences (e.g., updraft velocity and ambient sounding profile). Individual polluted clouds were found to exhibit a narrower cloud drop spectral width in accord with theoretical prediction (M.-L. Lu and J. H. Seinfeld, Effect of aerosol number concentration on cloud droplet dispersion: A large-eddy simulation study and implications for aerosol indirect forcing, Journal of Geophysical Research, 2006). This field experiment demonstrates both the indirect aerosol effect on ship track perturbed clouds, as well as the subtleties involved in extracting these effects over an ensemble of clouds sampled over a 1-month period.

CCN measurements during ACE-2 and their relationship to cloud microphysical properties

Measurements of cloud condensation nuclei (CCN) concentration at 0.1% supersaturation were made onboard the CIRPAS Pelican over the northeast Atlantic during June and July, 1997, in the vicinity of Tenerife, Spain, as part of the second Aerosol Characterization Experiment (ACE-2). The average CCN concentration (N ccn ) in the marine boundary layer for clean air masses was 27±8 and 42±14 cm’3 for cloudy and clear conditions, respectively, consistent with measurements made near the British Isles and close to Tasmania, Australia, during ACE-1 for similar conditions. A local CCN closure experiment was conducted. Measured N ccn is compared with predictions based on aerosol number size distributions and size-resolved chemical composition profiles determined from measurements and the literature. A sublinear relationship between measured and predicted N ccn ,N ccn ~N0.51 , was found. This result is consistent with some previous studies, but others have obtained results much closer to the expected 1 : 1 relationship between measured and predicted N ccn . A large variability between measured and predicted N ccn was also observed, leading to the conclusion that, for 95% of the data, the predictions agree with measurements to within a factor of 11. Relationships between belowcloud N ccn and aerosol accumulation mode concentration, and in-cloud cloud droplet number