ALBERT

Description: The light absorption coefficient, Beta(a) of the stratospheric aerosol is an important quantity that determines its radiative effects. When combined with the aerosol scattering coefficient, Beta(a) it becomes possible to evaluate the aerosol single scatter albedo, omega = Beta(s)/(Beta(s) + Beta(a)) which is essential for modeling the overall radiative effects of the stratospheric aerosol. Pollack1 determined that omega = 0.98 is a critical value that separates stratospheric cooling from warming.

Description: Measurements of aerosol light-absorption coefficients are useful for studies of radiative transfer and heating rates. Ogren appears to have published the first light- absorption coefficients in the stratosphere in 1981, followed by Clarke in 1983 and Pueschel in 1992. Because most stratospheric soot appears to be due to aircraft operations, application of an aircraft soot aerosol emission index to projected fuel consumption suggests a threefold increase of soot loading and light absorption by 2025. Together, those four data sets indicate an increase in mid-visible light extinction at a rate of 6 % per year. This trend is similar to the increase per year of sulfuric acid aerosol and of commercial fleet size. The proportionality between stepped-up aircraft operations above the tropopause and increases in stratospheric soot and sulfuric acid aerosol implicate aircraft as a source of stratospheric pollution. Because the strongly light-absorbing soot and the predominantly light-scattering sulfuric acid aerosol increase at similar rates, however, the mid-visible stratospheric aerosol single scatter albedo is expected to remain constant and not approach a critical value of 0.98 at which stratospheric cooling could change to warming.

Description: The distribution of black carbon (soot) aerosol (BCA) in the atmosphere is of interest for several reasons: (1) Because BCA has the highest absorption cross section of any compound known, it can absorb solar radiation to cause atmospheric warming. (2) Because it is a strong adsorber of gases, it can catalyze heterogeneous reactions to change the chemical composition of the atmosphere.(3) If aircraft are a major source of BCA, it is an important tracer of aircraft emissions. Analysis for BCA of impactor samples from Arctic and Antarctic deployments, utilizing particle morphology of scanning electron microscopy images, permits the following conclusions: (1) The BCA concentration in the northern stratosphere varies between 0 and 2.6 ng m-3 averaging 0.6 ng/cu m. (2) This BCA loading is commensurate with estimated fuel consumptions in the stratosphere by the current commercial fleet and an emission index E=0.03 g BCA per kg fuel burnt which was measured in jet exhaust at al titude.Thus, most stratospheric BCA in the northern stratosphere results from aircraft emissions. The background BCA concentration in the southern stratosphere varies between 0 and 0.6 ng cu m averaging 0.1 ng/cu m. This strong meridional gradient implies that stratospheric BCA residence time- is shorter than are mixing times between hemispheres. Projected annual fuel consumption of a future supersonic commercial fleet is 7E13 g. This fleet would increase stratospheric BCA loadings by a factor of 2-3, because almost all fuel would be burnt above the tropopause. An improved EI(BCA) by a factor of ten would result in an increase of stratospheric BCA loadings by approximately 50 %.

Description: Aerosol backscatter coefficient data were examined from two nights near Japan and Hawaii undertaken during NASA's Global Backscatter Experiment (GLOBE) in May-June 1990. During each of these two nights the aircraft traversed different altitudes within a region of the atmosphere defined by the same set of latitude and longitude coordinates. This provided an ideal opportunity to allow flight level focused continuous wave (CW) lidar backscatter measured at 9.11-micron wavelength and modeled aerosol backscatter from two aerosol optical counters to be compared with pulsed lidar aerosol backscatter data at 1.06- and 9.25-micron wavelengths. The best agreement between all sensors was found in the altitude region below 7 km, where backscatter values were moderately high at all three wavelengths. Above this altitude the pulsed lidar backscatter data at 1.06- and 9.25-micron wavelengths were higher than the flight level data obtained from the CW lidar or derived from the optical counters, suggesting sample volume effects were responsible for this. Aerosol microphysics analysis of data near Japan revealed a strong sea-salt aerosol plume extending upward from the marine boundary layer. On the basis of sample volume differences, it was found that large particles were of different composition compared with the small particles for low backscatter conditions.

Description: 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 tau(sub p)(lambda = 0.526 microns) at the near-background level of 0.012 +/- 0.006 and no significant wavelength dependence in the measured range (lambda = 0.38 to 1.06 microns). 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 tau(sub p)(lambda) to an approximate power law with an exponent of about -1.4. By early September 1991, the spectrum was broadly peaked near 0.5 microns, and by July 1992, it was peaked near 0.8 microns. Our optical-depth spectra include corrections for diffuse light which increase postvolcanic midvisible tau(sub p) 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 less than 0.25 microns), 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 less than r less than 1 micron) 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 +/- 0.06 micron in July 1991 to 0.56 +/- 0.12 micron in August-September 1991 and to 0.86 +/- 0.29 micron in July 1992. Corresponding column mass values were 4.8 +/- 0.7, 9.1 +/- 2.7, and 5.5 +/- 2 micro g/sq cm, and corresponding column surface areas were 4.4 +/- 0.5, 2.9 +/- 0.2, and 1.1 +/- 0.1 sq micron/sq cm,. 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 1/sq m, 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 Pinatubo layer over MLO are 0.55 +/- 0.13 and 0.41 +/- 0.14 K/d for September 1991 and July 1992, respectively.

Description: During February/March 1994, a series of aircraft-based aerosol measurements were carried out in the Pacific Basin troposphere using a differential absorption lidar system deployed by NASA Langley, and optical spectrometer probes and a wire-impactor system operated by NASA Ames. A modified Klett inversion algorithm was applied to extract altitude profiles of aerosol backscattering from the IR lidar signal. The algorithm that we have designed for this purpose utilizes the in situ aerosol measurements to normalize the lidar profile at the aircraft altitude and to supply the lidar ratio as a function of height. The lidar-derived aerosol backscattering coefficients were then compared to the backscattering coefficients calculated from the in situ measurements. During several local aircraft descents, we found good agreement between the remote lidar and in situ results for the absolute value of the aerosol backscattering coefficient and its altitude variation only when we allowed for several layers with different aerosol refractive indices. The agreement validates our lidar calibration method and provides an indication of the variation in aerosol refractive index as a function of altitude. Two of the three case studies performed in this paper reveal layers of anthropogenic aerosols transported long distances into the Pacific Basin troposphere. A third case implies the existence of a layer of dustlike aerosol particles in the lower troposphere, most likely of Asian origin.

Description: In January and March 1992, DC-8-measured stratospheric particle optical depth spectra, (tau)(sub p)(lambda), peaked broadly at midvisible or longer wavelengths. At mid-to-high northern latitudes outside the vortex, tau(sub p)(526 microns) above about 11 km was as large as 0.22 in both January and March, reflecting continued Pinatubo volcanic influence. In both months, in-vortex tau(sub p) above 11 km was smaller than outside-vortex values by a factor of two or more, and in January a strong anticorrelation was observed between tau(sub p)(lambda) and HF column content (an indicator of vortex penetration). In late January at 18-20S, near the edge of the southern subtropical jet, tau(sub p)(526 microns) above 12 km was only about 0.07- 0.09, with a flatter spectral shape than northern mid-to high-latitude measurements in both January and March. Occasional high-latitude vertical profiles indicate 6-1 km slab optical depths, delta(tau)(sub p)(526 micron), of 0.05 to 0.1, which should be added to the above-11-km values to yield values above 6 km.

Description: During NASA's Global Backscatter Experiment (GLOBE) mission flights in November 1989 and May 1990, a DC-8 research aircraft probed the Pacific Basin free troposphere for about 90 flight hours in each month between +72 and -62 degrees latitude, +130 and -120 degrees longitude, and up to 39,000 feet pressure altitudes. Aerosols were sampled continuously in situ by optical particle counters to measure concentration and particle size, and during 48 10-min intervals during each mission by wire impactors for concentration, size, composition, phase and shape analyses. The optical particle counters cover a particle diameter range between 0.3 and 20 microns; wire impactors extend the range down to 0.03 microns. Results of particle number, size, shape, together with the assumption of a refractive index corresponding to (NH4)2SO4 to account for the prevalence of aerosol sulfur, were utilized in a Mie algorithm to calculate aerosol extinction and backscatter for a range of wavelengths (0.385 less than lambda less than 10.64 microns). Computations for 22 randomly selected size distributions yield coefficients of extinction E(0.525) = (2.03 +/- 1.20) x 10(exp -4) km(exp -1) and backscatter beta(0.525) = (6.45 +/- 3.49) x 10(exp -6) km(exp -1) sr(exp -1) in the visible, and E(10.64) = (8.13 +/- 6.47) x 10(exp -6) km(exp -1) and beta(10.64) = (9.98 +/- 10.69) x 10(exp -8) km(exp -1) sr(exp -1) in the infrared, respectively. Large particles (D greater than 0.3 microns) contribute two-thirds to the total extinction in the visible (lambda = 0.525 microns), and almost 100% in the infrared (lambda = 10.64 microns). These results have been used to define an IR optical aerosol climatology of the Pacific Basin free troposphere, from which it follows that the infrared backscatter coefficient at lambda = 9.25 microns wavelength fluctuates between 5.0 x 10(exp -10) and 2.0 x 10(exp -7) km(exp -1) sr(exp -1) with a modal value 2.0 x 10(exp -8) km(exp -1) sr(exp -1).

Description: We have used two approaches to measure BCA in the stratosphere. The first method consists of collecting aerosols by impaction on quartz rods, upon which are mounted strips of polystyrene filter material. Each 25 mm by 0.5 mm filter strip is alternately masked and exposed in 5 mm long sections. After sampling, the optical density of the exposed sections is measured and compared with the optical density of the masked (unexposed) sections. The filter strip is a Lambertian collector, the scattering property of which is not affected by the deposition of liquid sulfuric acid droplets which dominate the stratospheric aerosol. Hence, all attenuation greater in the exposed than in the non-exposed sections is due to absorption by BCA or rare opaque materials such as meteoritic iron. In a second approach we expose carbon-coated gold or palladium wires to air outside the aircraft boundary layer [Farlow et al., 1979; Pueschel et al., 1989]. With a field emission scanning electron microscope we are able to characterize BCA particles in addition to the dominant sulfuric acid droplets. Typically, soot is comprised of 20 nm diameter spheres linked together as branching chains or loosely packed aggregates (Figure 1a). The microscope has a lateral image resolution of 1.5 nm and can clearly resolve individual spheres making up BCA aggregates. Their morphology is uniquely different from that of the liquid sulfuric acid-water aerosol (Figure 1b). We approximate the size of each BCA particle by that of a sphere of equivalent volume and fit a lognormal size distribution to both the BCA and H2SO4/H2O aerosols. Both sampler types have been mounted on NASA's ER-2 high-altitude research aircraft (altitude ceiling of 70,000 feet), and on NASA's DC-8 (40,000 feet ceiling) aircraft to sample aerosols from a significant portion of the atmosphere.