J. M. Livingston

Chemical apportionment of aerosol column optical depth off the mid‐Atlantic coast of the United States

Aerosol column optical depths derived from airborne Sun photometer and in situ measurements of aerosol properties in 14 vertical profiles off the mid-Atlantic coast of the United States in June show excellent agreement. Simultaneous measurements of the chemical compositions of the aerosol allows an assessment of the chemical apportionment of the aerosol column optical depths. The optical depths had essentially three chemical components, which, in order of descending average contributions, were condensed water, carbonaceous species, and sulfate. These results do not support the common assumption that sulfate dominates aerosol optical depths in polluted regions.

Pinatubo and pre‐Pinatubo optical‐depth spectra: Mauna Loa measurements, comparisons, inferred particle size distributions, radiative effects, and relationship to lidar data

The Ames airborne tracking sunphotometer was operated at the National Oceanic and Atmospheric Administration (NOAA) Mauna Loa Observatory (MLO) in 1991 and 1992 along with the NOAA Climate Monitoring and Diagnostics Laboratory (CMDL) automated tracking sunphotometer and lidar. June 1991 measurements provided calibrations, optical-depth spectra, and intercomparisons under relatively clean conditions; later measurements provided spectra and comparisons for the Pinatubo cloud plus calibration checks. June 1991 results are similar to previous MLO springtime measurements, with midvisible particle optical depth τp(λ = 0.526μm) at the near-background level of 0.012 ± 0.006 and no significant wavelength dependence in the measured range (λ = 0.38 to 1.06μm). The arrival of the Pinatubo cloud in July 1991 increased midvisible particle optical depth by more than an order of magnitude and changed the spectral shape of τp(λ) to an approximate power law with an exponent of about −1.4. By early September 1991, the spectrum was broadly peaked near 0.5 μm, and by July 1992, it was peaked near 0.8 μm. Our optical-depth spectra include corrections for diffuse light which increase postvolcanic midvisible τp values by 1 to 3% (i.e., 0.0015 to 0.0023). NOAA- and Ames Research Center (ARC)-measured spectra are in good agreement. Columnar size distributions inverted from the spectra show that the initial (July 1991) post-Pinatubo cloud was relatively rich in small particles (r<0.25μm), which were progressively depleted in the August-September 1991 and July 1992 periods. Conversely, both of the later periods had more of the optically efficient medium-sized particles (0.25<r<1 μm) than did the fresh July 1991 cloud. These changes are consistent with particle growth by condensation and coagulation. The effective, or area-weighted, radius increased from 0.22 ± 0.06μm in July 1991 to 0.56 ± 0.12 μm in August-September 1991 and to 0.86 ± 0.29 μm in July 1992. Corresponding column mass values were 4.8 ± 0.7, 9.1 ± 2.7, and 5.5 ± 2.0 μg/cm2, and corresponding column surface areas were 4.4 ± 0.5, 2.9 ± 0.2, and 1.1 ± 0.1 μm2/cm2. Photometer-inferred column backscatter values agree with those measured by the CMDL lidar on nearby nights. Combining lidar-measured backscatter profiles with photometer-derived backscatter-to-area ratios gives peak particle areas that could cause rapid heterogeneous loss of ozone, given sufficiently low particle acidity and suitable solar zenith angles (achieved at mid- to high latitudes). Top-of-troposphere radiative forcings for the September 1991 and July 1992 optical depths and size distributions over MLO are about −5 and −3 W m−2, respectively (hence comparable in magnitude but opposite in sign to the radiative forcing caused by the increase in manmade greenhouse gases since the industrial revolution). Heating rates in the Pinatubo layer over MLO are 0.55 ± 0.13 and 0.41 ± 0.14 K d−1 for September 1991 and July 1992, respectively.

Global to Microscale Evolution of the Pinatubo Volcanic Aerosol Derived from Diverse Measurements and Analyses

We assemble data on the Pinatubo aerosol from space, air, and ground measurements, develop a composite picture, and assess the consistency and uncertainties of measurement and retrieval techniques. Satellite infrared spectroscopy, particle morphology, and evaporation temperature measurements agree with theoretical calculations in showing a dominant composition of H2SO4-H2O mixture, with H2SO4 weight fraction of 65–80% for most stratospheric temperatures and humidities. Important exceptions are (1) volcanic ash, present at all heights initially and just above the tropopause until at least March 1992, and (2) much smaller H2SO4 fractions at the low temperatures of high-latitude winters and the tropical tropopause. Laboratory spectroscopy and calculations yield wavelength- and temperature-dependent refractive indices for the H2SO4-H2O droplets. These permit derivation of particle size information from measured optical depth spectra, for comparison to impactor and optical-counter measurements. All three techniques paint a generally consistent picture of the evolution of Reff, the effective radius. In the first month after the eruption, although particle numbers increased greatly, Reff outside the tropical core was similar to preeruption values of ∼0.1 to 0.2 μm, because numbers of both small (r 0.6 μm) particles increased. In the next 3–6 months, extracore Reff increased to ∼0.5 μm, reflecting particle growth through condensation and coagulation. Most data show that Reff continued to increase for ∼1 year after the eruption. Reff values up to 0.6–0.8 μm or more are consistent with 0.38–1 μm optical depth spectra in middle to late 1992 and even later. However, in this period, values from in situ measurements are somewhat less. The difference might reflect in situ undersampling of the very few largest particles, insensitivity of optical depth spectra to the smallest particles, or the inability of flat spectra to place an upper limit on particle size. Optical depth spectra extending to wavelengths λ > 1 μm are required to better constrain Reff, especially for Reff > 0.4 μm. Extinction spectra computed from in situ size distributions are consistent with optical depth measurements; both show initial spectra with λmax ≤ 0.42 μm, thereafter increasing to 0.78 ≤ λmax ≤ 1 μm. Not until 1993 do spectra begin to show a clear return to the preemption signature of λmax ≤ 0.42 μm. The twin signatures of large Reff (>0.3 μm) and relatively flat extinction spectra (0.4–1 μm) are among the longest-lived indicators of Pinatubo volcanic influence. They persist for years after the peaks in number, mass, surface area, and optical depth at all wavelengths ≤1 μm. This coupled evolution in particle size distribution and optical depth spectra helps explain the relationship between global maps of 0.5- and 1.0-μm optical depth derived from the Advanced Very High Resolution Radiometer (AVHRR) and Stratospheric Aerosol and Gas Experiment (SAGE) satellite sensors. However, there are important differences between the AVHRR and SAGE midvisible optical thickness products. We discuss possible reasons for these differences and how they might be resolved.

Aerosol-Induced Radiative Flux Changes Off the United States Mid-Atlantic Coast: Comparison of Values Calculated from Sunphotometer and In Situ Data with Those Measured by Airborne Pyranometer

The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) measured a variety of aerosol radiative effects (including flux changes) while simultaneously measuring the chemical, physical, and optical properties of the responsible aerosol particles. Here we use TARFOX-determined aerosol and surface properties to compute shortwave radiative flux changes for a variety of aerosol situations, with midvisible optical depths ranging from 0.06 to 0.55. We calculate flux changes by several techniques with varying degrees of sophistication, in part to investigate the sensitivity of results to computational approach. We then compare computed flux changes to those determined from aircraft measurements. Calculations using several approaches yield downward and upward flux changes that agree with measurements. The agreement demonstrates closure (i.e., consistency) among the TARFOX-derived aerosol properties, modeling techniques, and radiative flux measurements. Agreement between calculated and measured downward flux changes is best when the aerosols are modeled as moderately absorbing (midvisible single-scattering albedos between about 0.89 and 0.93), in accord with independent measurements of the TARFOX aerosol. The calculated values for instantaneous daytime upwelling flux changes are in the range +14 to +48 W m−2 for midvisible optical depths between 0.2 and 0.55. These values are about 30 to 100 times the global-average direct forcing expected for the global-average sulfate aerosol optical depth of 0.04. The reasons for the larger flux changes in TARFOX include the relatively large optical depths and the focus on cloud-free, daytime conditions over the dark ocean surface. These are the conditions that produce major aerosol radiative forcing events and contribute to any global-average climate effect.

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.

Comparison of Columnar Water-Vapor Measurements from Solar Transmittance Methods

In the fall of 1997 the Atmospheric Radiation Measurement program conducted a study of water-vapor-abundance-measurement at its southern Great Plains site. The large number of instruments included four solar radiometers to measure the columnar water vapor (CWV) by measuring solar transmittance in the 0.94-mum water-vapor absorption band. At first, no attempt was made to standardize our procedures to the same radiative transfer model and its underlying water-vapor spectroscopy. In the second round of comparison we used the same line-by-line code (which includes recently corrected H(2)O spectroscopy) to retrieve CWV from all four solar radiometers, thus decreasing the mean CWV by 8-13%. The remaining spread of 8% is an indication of the other-than-model uncertainties involved in the retrieval.

Comparison of aerosol optical depth from four solar radiometers during the fall 1997 ARM intensive observation period

In the Fall of 1997 the Atmospheric Radiation Measurement (ARM) program conducted an Intensive Observation Period (IOP) to study aerosols. Five sun-tracking radiometers were present to measure the total column aerosol optical depth. This comparison performed on the Southern Great Plains (SGP) demonstrates the capabilities and limitations of modern tracking sunphotometers at a location typical of where aerosol measurements are required. The key result was agreement in aerosol optical depth measured by 4 of the 5 instruments within 0.015 (rms). The key to this level of agreement was meticulous care in the calibrations of the instruments.

Physical and optical properties of the Pinatubo volcanic aerosol: Aircraft observations with impactors and a Sun-tracking photometer

As determined in situ by impactor samplers flown on an ER-2 at 16.5- to 20.7-km pressure altitude and on a DC-8 at 9.5- to 12.6-km pressure altitudes, the 1991 Pinatubo volcanic eruption increased the particle surface area of stratospheric aerosols up to 50-fold and the particle volume up to 2 orders of magnitude. Particle composition was typical of a sulfuric acid-water mixture at ER-2 altitudes. Ash particles coated with sulfuric acid comprised a significant fraction of aerosol at DC-8 altitudes. Mie-computed light extinction increased up to 20-fold at midvisible and greater than 100-fold at near-IR wavelengths. The optical thickness measured through the aerosol layer by an autotracking Sun photometer aboard a DC-8 aircraft at 10.7- to 11.3-km pressure altitudes shows a spectral shape that is similar to the Mie-calculated spectral extinction at ER-2 altitudes. Surface area distributions calculated by inversion of spectral optical depth measurements show characteristics that are similar to the mean surface area distribution resulting from 35 in situ measurements.

In situ aerosol-size distributions and clear-column radiative closure during ACE-2

As part of the second Aerosol Characterization Experiment (ACE-2) during June and July of 1997, aerosol-size distributions were measured on board the CIRPAS Pelican aircraft through the use of a DMA and 2 OPCs. During the campaign, the boundary-layer aerosol typically possessed characteristics representative of a background marine aerosol or a continentally influenced aerosol, while the free-tropospheric aerosol was characterized by the presence or absence of a Saharan dust layer. A range of radiative closure comparisons were made using the data obtained during vertical profiles flown on 4 missions. Of particular interest here are the comparisons made between the optical properties as determined through the use of measured aerosol-size distributions and those measured directly by an airborne 14-wavelength sunphotometer and 3 nephelometers. Variations in the relative humidity associated with each of the direct measurements required consideration of the hygroscopic properties of the aerosol for size-distribution-based calculations. Simultaneous comparison with such a wide range of directly-measured optical parameters not only offers evidence of the validity of the physicochemical description of the aerosol when closure is achieved, but also provides insight into potential sources of error when some or all of the comparisons result in disagreement. Agreement between the derived and directly-measured optical properties varied for different measurements and for different cases. Averaged over the 4 case studies, the derived extinction coefficient at 525 nm exceeded that measured by the sunphotometer by 2.5% in the clean boundary layer, but underestimated measurements by 13% during pollution events. For measurements within the free troposphere, the mean derived extinction coefficient was 3.3% and 17% less than that measured by the sunphotometer during dusty and non-dusty conditions, respectively. Likewise, averaged discrepancies between the derived and measured scattering coefficient were −9.6%, +4.7%, +17%, and −41% for measurements within the clean boundary layer, polluted boundary layer, free troposphere with a dust layer, and free troposphere without a dust layer, respectively. Each of these quantities, as well as the majority of the >100 individual comparisons from which they were averaged, were within estimated uncertainties.

Comparison of aerosol single scattering albedos derived by diverse techniques in two North Atlantic experiments

Aerosol single scattering albedo v (the ratio of scattering to extinction) is important in determining aerosol climatic effects, in explaining relationships between calculated and measured radiative fluxes, and in retrieving aerosol optical depths from satellite radiances. Recently, two experiments in the North Atlantic region, the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the Second Aerosol Characterization Experiment (ACE-2), determined aerosol v by a variety of techniques. The techniques included fitting of calculated to measured radiative fluxes; retrievals of v from skylight radiances; best fits of complex refractive index to profiles of backscatter, extinction, and size distribution; and in situ measurements of scattering and absorption at the surface and aloft. Both TARFOX and ACE-2 found a fairly wide range of values for v at midvisible wavelengths (;550 nm), with 0.85 # vmidvis # 0.99 for the marine aerosol impacted by continental pollution. Frequency distributions of v could usually be approximated by lognormals in vmax 2 v, with some occurrence of bimodality, suggesting the influence of different aerosol sources or processing. In both TARFOX and ACE-2, closure tests between measured and calculated radiative fluxes yielded best-fit values of vmidvis of 0.90 6 0.04 for the polluted boundary layer. Although these results have the virtue of describing the column aerosol unperturbed by sampling, they are subject to questions about representativeness and other uncertainties (e.g., thermal offsets, unknown gas absorption). The other techniques gave larger values for vmidvis for the polluted boundary layer, with a typical result of vmidvis 5 0.95 6 0.04. Current uncertainties in v are large in terms of climate effects. More tests are needed of the consistency among different methods and of humidification effects on v.