Measurement of the lidar ratio for atmospheric aerosols with a 180 degrees backscatter nephelometer.

Laser radar (lidar) can be used to estimate atmospheric extinction coefficients that are due to aerosols if the ratio between optical extinction and 180 degrees backscatter (the lidar ratio) at the laser wavelength is known or if Raman or high spectral resolution data are available. Most lidar instruments, however, do not have Raman or high spectral resolution capability, which makes knowledge of the lidar ratio essential. We have modified an integrating nephelometer, which measures the scattering component of light extinction, by addition of a backward-pointing laser light source such that the detected light corresponds to integrated scattering over 176-178 degrees at a common lidar wavelength of 532 nm. Mie calculations indicate that the detected quantity is an excellent proxy for 180 degrees backscatter. When combined with existing techniques for measuring total scattering and absorption by particles, the new device permits a direct determination of the lidar ratio. A four-point calibration, run by filling the enclosed sample volume with particle-free gases of a known scattering coefficient, indicates a linear response and calibration reproducibility to within 4%. The instrument has a detection limit of 1.5 x 10(-7) m(-1) sr(-1) (approximately 10% of Rayleigh scattering by air at STP) for a 5-min average and is suitable for ground and mobile/airborne surveys. Initial field measurements yielded a lidar ratio of approximately 20 for marine aerosols and approximately 60-70 for continental aerosols, with an uncertainty of approximately 20%.

Relationship between asymmetry parameter and hemispheric backscatter ratio: implications for climate forcing by aerosols.

Calculations of direct climate forcing by anthropogenic aerosols commonly use radiative transfer parameters, including asymmetry parameter g. One method of obtaining the asymmetry parameter of a particle population is to convert measured values of the hemispheric-to-total-scatter ratio (backscatter ratio b) into their corresponding g values. We compare a conversion derived from Mie calculations with one derived from the Henyey-Greenstein (HG) phase function to show that the HG method systematically overestimates g for typical size distributions of accumulation-mode aerosols. A delta-Eddington radiative transfer calculation is used to show that a 10% overestimation of g can systematically reduce climate forcing as a result of aerosols by 12% or more. Mie computations are used to derive an empirical relationship between backscatter ratio and asymmetry parameter for log-normal accumulation-mode aerosols. This relationship can be used to convert the backscatter ratio to the asymmetry parameter, independent of geometric mean diameter D(gv) or complex refractive index m, but the conversion requires knowledge of the breadth σ(g) of the size distribution.

Climate forcing by anthropogenic aerosols.

Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol in particular has imposed a major perturbation to this forcing. Both the direct scattering of shortwavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square meter, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes.

Internal mixture of sea salt, silicates, and excess sulfate in marine aerosols.

Individual aerosol particles from the remote marine atmosphere were investigated by scanning electron microscopy and electron microprobe analysis. A large fraction of the silicate mineral component of the aerosol was found to be internally mixed with sea-salt aerosol particles. This observation explains the unexpected similarity in the size distributions of silicates and sea salt that has been observed in remote marine aerosols. Reentrainment of dust particles previously deposited onto the sea surface and collision between aerosol particles can be excluded as possible source mechanisms for these internally mixed aerosols. The internal mixing could be produced by processes within clouds, including droplet coalescence. Cloud processes may also be responsible for the observed enrichment of excess (nonsea-salt) sulfate on sea-salt particles.

Radiative properties of the background aerosol: absorption component of extinction.

The light-scattering and light-absorption coefficients of the global background aerosol define its single-scatter albedo. Continuous, simultaneous measurements of these optical coefficients were made on a daily basis for the remote marine mid-troposphere; such measurements are essential for assessment of the effects of aerosol on atmospheric radiative transfer. Measurements of light-absorption coefficients made at the Mauna Loa Observatory in Hawaii were higher than expected, and the single-scatter albedo was lower than the value often used in radiative transfer models. Soot appears to be the most likely primary absorber, and hemispheric dispersal of this combustion-derived material is suggested.

Absorption of visible radiation by aerosols in the volcanic plume of mount st. Helens.

Samples of particles from Mount St. Helens were collected in both the stratosphere and troposphere for measurement of the light absorption coefficient. Results indicate that the stratospheric dust had a small but finite absorption coefficient ranging up to 2 x 10(-7) per meter at a wavelength of 0.55 micrometer, which is estimated to yield an albedo for single scatter of 0.98 or greater. Tropospheric results showed similar high values of an albedo for single scatter.

Characterization of nonspherical atmospheric aerosol particles with electrooptical nephelometry.

An integrating nephelometer was adapted electronically to study the electrooptical properties of aerosol particles. The increase in light scattering coefficient due to orientation of nonspherical particles in the pulsed electric field and the decay of this signal were measured. Examples of the data for laboratory generated aerosols and atmospheric aerosols are presented.

Ammonia in the human airways: neutralization of inspired acid sulfate aerosols.

In the human being, expired ammonia concentrations from 7 to 520 micrograms per cubic meter are controlled by the last airway segment traversed by the air, and such concentrations are higher in the mouth than nose. Inspired submicrometric sulfuric acid aerosol at a mass concentration of 600 +/- 100 micrograms per cubic meter was found to be an ammonium salt with an average ammonium to sulfate molar ratio of greater than or equal to 1, when sampled within 0.5 second after exhalation.

Sulfate aerosol: its geographical extent in the midwestern and southern United States.

Sulfate particles (sulfuric acid and its neutralization products with ammonia) dominate the submicrometer-sized, light-scattering component of the aerosol in more than 90 percent of 2850 pairs of humidographic measurements made over a 3-month period at three rural midwestern and southern sites. The nearly continuous optical dominance by sulfate in the aerosol at these spatially varied locations, particularly in the Ozark Mountains, suggests that sulfate is a component of the submicrometer-sized aerosol that is distributed over a large geographical region and is not due to local sources.

Influence of relative humidity on functional effects of an inhaled SO2-aerosol mixture.

Lightly anesthetized guinea pigs were exposed to 1 ppm of sulfur dioxide (SO2) and 1 mg per m3 of sodium chloride aerosol, individually and in combination, at low and high relative humidities. At low relative humidity (less than 40 per cent) the aerosol was a crystal, at high relative humidity (greater than 80 per cent) a droplet. Exposures lasted one hour. Changes in pulmonary mechanical function characterized by an increase in flow resistance and decrease in compliance were seen only when the mixture was administered at high relative humidity. The effect is ascribed to absorption of the highly soluble SO2 into the droplet before inhalation.

Visibility of distant mountains as a measure of background aerosol pollution.

A relationship is developed between the visibility of distant mountains seen from an aircraft and a level of background aerosol pollution for a model atmosphere. It is found that the distance at which Mt. Rainier can be seen on clean-air days, which are typical of background aerosol levels, is consistent with the level of aerosol light-scattering measurements in other background situations.

Sulfuric acid-ammonium sulfate aerosol: optical detection in the St. Louis region.

Nephelometric sensing of the deliquescence of ammonium sulfate produced by the reaction of sulfuric acid or ammonium bisulfate aerosol with ammonia provides a means for detecting these substances in air. Field experiments show them to be the dominant substances in the submicrometer, light-scattering aerosol in the St. Louis region.

Blue moon: is this a property of background aerosol?

Stellar extinction measurements made at three astronomical observatories showed that on ~50% of the nights the extinction due to aerosol light scattering increased rather than decreased with increasing wavelength (anomalous extinction) for wavelengths close to 500 nm. This extinction behavior is analyzed in this paper and limits are established for the aerosol characteristics necessary for this phenomenon to exist, including geometric standard deviations, imaginary part of refractive index, mean radius, and gaseous NO(2).