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Hegg, Dean A.

Publications and source records attributed to Hegg, Dean A..

Derivation of Aerosol Columnar Mass from MODIS Optical Depth

In order to verify performance, aerosol transport models (ATM) compare aerosol columnar mass (ACM) with those derived from satellite measurements. The comparison is inherently indirect since satellites derive optical depths and they use a proportionality constant to derive the ACM. Analogously, ATMs output a four dimensional ACM distribution and the optical depth is linearly derived. In both cases, the proportionality constant requires a direct intervention of the user by prescribing the aerosol composition and size distribution. This study introduces a method that minimizes the direct user intervention by making use of the new aerosol products of MODIS. A parameterization is introduced for the derivation of columnar aerosol mass (AMC) and CCN concentration (CCNC) and comparisons between sunphotometer, MODIS Airborne Simulator (MAS) and in-measurements are shown. The method still relies on the scaling between AMC and optical depth but the proportionality constant is dependent on the MODIS derived r$_{eff}$,\eta (contribution of the accumulation mode radiance to the total radiance), ambient RH and an assumed constant aerosol composition. The CCNC is derived fkom a recent parameterization of CCNC as a function of the retrieved aerosol volume. By comparing with in-situ data (ACE-2 and TARFOX campaigns), it is shown that retrievals in dry ambient conditions (dust) are improved when using a proportionality constant dependent on r$ {eff}$ and \eta derived in the same pixel. In high humidity environments, the improvement inthe new method is inconclusive because of the difficulty in accounting for the uneven vertical distribution of relative humidity. Additionally, two detailed comparisons of AMC and CCNC retrieved by the MAS algorithm and the new method are shown. The new method and MAS retrievals of AMC are within the same order of magnitude with respect to the in-situ measurements of aerosol mass. However, the proposed method is closer to the in-situ measurements than the MODIS retrievals. The retrievals of CCNC are also within the same order of magnitude for both methods. The new method is applied to an actual MODIS retrieval and although no in-situ data is available to compare, it is shown that the proposed method yields more credible values than the MODIS retrievals. In addition, recent data available from the PRIDE (Puerto Rico Dust Experiment, July 2000) will be shown by comparing sunphotometer, MODIS and in-situ data.

Gasso, Santiago

Water-soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution and Distribution

During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.

Gao, Song

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 (lambda = 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 lambda = 525 nm), but these differences are within the combined error bars of the measurements and computations.

Schmid, Beat

Clear-Sky Closure Studies of 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 (a differential mobility analyzer, three optical particle counters, three nephelometers, and one absorption photometer) measurements taken aboard the Pelican aircraft, space-borne NOAA/AVHRR data and ground-based lidars. A wide range of aerosol types was encountered throughout the ACE-2 area, including background Atlantic marine, European pollution-derived, and (although less frequently than expected) African mineral dust. During the two days discussed here, vertical profiles flown in cloud free air masses revealed three 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. Based on size-resolved composition information we have established an aerosol model that allows us to compute optical properties of the ambient aerosol using the optical particle counter results. In the dust, the agreement in layer AOD (lambda=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 lambda=525 nm), but these differences are within the combined error bars of the measurements and computations. Aerosol size-distribudon closure based on in-situ size distributions and inverted sunphotometer extinction spectra has been achieved in the MBL (total surface area and volume agree within 0.2, and 7%, respectively) but not in the dust layer. The fact that the three nephelometers operated at three different relative humidities (RH) allowed to parameterize hygroscopic growth and to therefore estimate optical properties at ambient RH. The parameters derived for different aerosol types are themselves useful for the aerosol modeling community. The fact that the nephelometers and the absorption photometer sampled the aerosol through a cyclone make those measurements less useful for thee closure study carried out here. Large corrections (especially in the dust) had to be applied. Therefore, it is not surprising that closure with the sunphotometer was not always achieved. Agreement within 0.02 in AOD was achieved in the dust layer when the airorne sunphotometer extinction or AOD was compared to ground-based lidar measurements. We found that the presence of the elevated dust layers removes the good agreement between satellite and sunphotometer AOD usually found in the absence of the dust layer. We still compare the scattering phase functions used in the satellite retrieval with those obtained from the aerosol or the sunphotometer measurements.

Schmid, Beat

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 (lambda = 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 lambda = 525 nm), but these differences are within the combined error bars of the measurements and computations.

Schmid, Beat

Cloud condensation nucleus-sulfate mass relationship and cloud albedo

Analysis of previously published, simultaneous measurements of cloud condensation nucleus number concentration and sulfate mass concentration suggest a nonlinear relationship between the two variables. This nonlinearity reduces the sensitivity of cloud albedo to changes in the sulfur cycle.

Hegg, Dean A.

Reply

While Hegg et al. (1993) accepts the criticism of Anderson et al. (1994) in principle, this involves the adoption of an aerosol composition model and the model that they propose to reconcile these observations with the assertion of Charlson et al. (1992) does not agree with many observations, particularly those made over the North Atlantic Ocean. Although the use of a gain factor (i.e. the partial derivative of aerosol mass with respect to the sulfate ion), proposed by Anderson et al., may be valid for particular cases where a proposed composition model really reflects the actual aerosol composition, this procedure is considered questionable in general. The use of sulfate as a tracer for nonsulfate aerosol mass is questionable, because in the present authors' data set, sulfate averaged only about 26% of the dry aerosol mass. The ammonium mass associated with sulfate mass is not analogous to that betwen the oxygen mass and sulfur mass in the sulfate ion. Strong chemical bonds are present between sulfur and oxygen in sulfate, whereas ammonium and sulfate in haze droplets are ions in solution that may or may not be associated with one another. Thus, there is no reason to assume that sulfate will act as a reliable tracer of ammonium mass. Hegg et al. expresses the view that their approach used for estimating sulfate light scattering efficiency is appropriate for the current level of understanding of atmospheric aerosols.

Hegg, Dean A.

Measurements of dimethyl sulfide and SO2 during GTE/CITE 3

As part of NASA's Tropospheric Experiment Chemical Instrumentation Test and Evaluation (GTE/CITE 3) Sulfur Gas Intercomparison, we conducted measurements of dimethyl sulfide (DMS) and SO2 using two techniques well suited for sampling from an aircraft due to their simplicity of design. DMS was collected by preconcentration on gold wire preceded by a KOH-impregnated filter oxidant scrubber, and analyzed by gas chromatography with flame photometric detection. SO2 was collected on K2CO3/glycerol-impregnated filters and analyzed by ion chromatography. In blind tests, both techniques produced excellent agreement with National Institutes of Standards and Technology (NIST) standards. For field measurements, the DMS technique produced excellent correlation with the mean of the six different techniques intercompared. For SO2, the five techniques intercompared were rather poorly correlated, but correlations between the three techniques which passed NIST standards tests were somewhat better. Our SO2 filter measurements exhibited rather large uncertainties due to higher than normal variabiltiy of the filter blanks, which we believe was caused by extended storage in the field. In measurements conducted off the coast of Natal, Brazil, a diurnal afternoon minimum in DMS concentrations accompanied by a corresponding maximum in SO2 concentrations was observed. However, due to rather large uncertainties in the SO2 measurements, any conclusions about the SO2 trend must by considered tentative.

Ferek, Ronald J.