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Typical Types and Formation Mechanisms of Haze in an Eastern Asia Megacity, Shanghai

An intensive aerosol and gases campaign was performed at Shanghai in the Yangtze River Delta region over Eastern China from late March to early June 2009. This study provided a complementary picture of typical haze types and the formation mechanisms in megacities over China by using a synergy of ground-based monitoring, satellite and lidar observations. During the whole study period, several extreme low visibility periods were observed with distinct characteristics, and three typical haze types were identified, i.e. secondary inorganic pollution, dust, and biomass burning. Sulfate, nitrate and ammonium accounted for a major part of PM2.5 mass during the secondary inorganic pollution, and the good correlation between SO2/NOx/CO and PM2.5 indicated that coal burning and vehicle emission were the major sources. Large-scale regions with high AOD (aerosol optical depths) and low Angstrom exponent were detected by remote-sensing observation during the dust pollution episode, and this episode corresponded to coarse particles rich in mineral components such as Al and Ca contributing 76.8% to TSP. The relatively low Ca/Al ratio of 0.75 along with the air mass backward trajectory analysis suggested the dust source was from Gobi Desert. Typical tracers for biomass burning from satellite observation (column CO and HCHO) and from ground measurement (CO, particulate K+, OC, and EC) were greatly enhanced during the biomass burning pollution episode. The exclusive linear correlation between CO and PM2.5 corroborated that organic aerosol dominated aerosol chemistry during biomass burning, and the high concentration and enrichment degree of arsenic (As) could be also partly derived from biomass burning. Aerosol optical profile observed by lidar demonstrated that aerosol was mainly constrained below the boundary layer and comprised of spheric aerosol (depolarization ratio <5%) during the secondary inorganic and biomass burning episodes, while thick dust layer distributed at altitudes from near surface to 1.4 km (average depolarization ratio = 0.122+/-0.023) with dust accounting for 44-55% of the total aerosol extinction coefficient during the dust episode. This study portrayed a good picture of the typical haze types and proposed that identification of the complicated emission sources is important for the air quality improvement in megacities in China.

haze

Can Organic Haze and O2 Plumes Explain Patterns of Sulfur Mass-Independent Fractionation During the Archean?

The existence of mass-independently fractionated sulfur in Archean rocks is almost universally accepted as evidence for low atmospheric O2 and O3 concentrations at that time. But the detailed patterns of the values and of the ratios / and / remain to be explained, and the mechanism for producing the mass-independent fractionation remains controversial. Here, we explore the hypothesis that the relatively low values seen during the Mid-Archean, 2.7-3.5 Ga, were caused by the presence of organic haze produced from photolysis of methane. This haze helped shield SO2 from photolysis, while at the same time providing surfaces on which unfractionated short-chain sulfur species could condense. The evolution of oxygenic photosynthesis, and the concomitant disappearance of organic haze towards the end of the Archean allowed more negatively fractionated S4 and S8 to form, thereby generating large positive fractionations in other sulfur species, including sulfate and H2S. Reduction of this sulfate to H2S by bacteria, followed by incorporation of H2S into pyrite, produced the large positive values observed in the Neoarchean rock record, 2.5-2.7 Ga.

Great Oxidation Event

Discrete ordinate theory of radiative transfer. 2: Scattering from maritime haze

Discrete ordinate theory was used to calculate the reflected and transmitted radiance of photons which have interacted with plane parallel maritime haze layers. The results are presented for three solar zenith angles, three values of the surface albedo, and a range of optical thicknesses from very thin to very thick. The diffuse flux at the lower boundary and the cloud albedo were tabulated. The forward peak and other features in the single scattered phase function caused the radiance in many cases to be very different from that for Rayleigh scattering. The variation of the radiance with both the zenith or nadir angle and the azimuthal angle is more marked, and the relative limb darkening under very thick layers is greater, for haze than for Rayleigh scattering. The downward diffuse flux at the lower boundary for A = O is always greater and the cloud albedo is always less for haze than for Rayleigh layers.

Kattawar, G. W.

Matrix operator theory of radiative transfer. II - Scattering from maritime haze.

Matrix operator theory is used to calculate the reflected and transmitted radiance of photons that have interacted with plane-parallel maritime haze layers. The results are presented for three solar zenith angles, three values of the surface albedo, and a range of optical thicknesses from very thin to very thick. The diffuse flux at the lower boundary and the cloud albedo are tabulated. The forward peak and other features in the single-scattered phase function cause the radiance in many cases to be very different from that for Rayleigh scattering. In particular, the variation of the radiance with both the zenith or nadir angle and the azimuthal angle is more marked and the relative limb darkening under very thick layers is greater for haze M than for Rayleigh scattering. The downward diffuse flux at the lower boundary for A = 0 is always greater and the cloud albedo is always less for haze M than for Rayleigh layers.

Kattawar, G. W.

Multiple scattered radiation emerging from continental haze layers. 2: Ellipticity and direction of polarization

The ellipticity and the direction of polarization are calculated for radiation that has undergone multiple scattering from plane parallel layers. Both the radiation emerging from the top of the layer and that transmitted through the bottom are considered. Two different phase functions are used for the scattering layer: Rayleigh and haze L. The direction of polarization of the reflected radiation shows little variation as the optical depth of the layer increases, while there is a much larger variation for the transmitted radiation. When the optical thickness is small, the direction of polarization for haze L varies rapidly with zenith angle near those angles at which the single scattered polarization is zero. The ellipticity of the radiation from haze L layers increases at first in direct proportion to the optical thickness of the layer. In general the ellipticity of the transmitted radiation is considerably greater than that of the reflected because of the greater average number of photon collisions in the former case.

Plass, G. N.

Haze and sun angle effects on automatic classification of satellite data-simulation and correction

Variations in sun angle and haze level change the spectral signatures collected by multispectral scanners (MSS). This paper describes methods and computer programs that have been developed to simulate the effect of such variations and to correct for them. A basic program, Prediction of the Response of Earth Pointed Sensors (PREPS), is used to calculate the response of the sensor as a function of solar angle, atmospheric haze level, and target reflectance. It is then simply a matter of interpolating these results to simulate changes in haze level or solar angle. In principle, this can be done for any sensor, although at the present time it has been completed for only one - the ERTS-1 MSS.

Potter, J. F.

Venus - Vertical structure of stratospheric hazes from Mariner 10 pictures

An 'optical barometer' technique for determining the altitudes of haze in the stratosphere of Venus is presented wherein the Rayleigh-scattering component is derived by comparing orange and UV brightness profiles for nearby Mariner 10 television-picture pairs. The derived scale height for CO2 gas is 4.2 km, corresponding to a temperature of 200 K, in good agreement with radio occultation data. The optical barometer yields a pressure of 4 mb for the level at which the slant-path optical depth at the limb is unity. This level corresponds to a distance from the center of Venus equal to 6131 km, which is accurate to within 1 km provided that there is no appreciable contribution to the brightness by Rayleigh-scattering aerosols which mimic CO2 gas. It is possible that the limb haze layering observed between 6130 and 6140 km could be correlated with temperature inversions detected by the Mariner 5 radio-occultation experiment. A model is proposed wherein the concentration of particles increases rapidly with an effective scale height of about 2 km as one descends about 10 km from the limb haze to the main polarization cloud deck.

Oleary, B.

Multiple scattered radiation emerging from Rayleigh and continental haze layers. I - Radiance, polarization, and neutral points

The matrix operator method was used to calculate the polarization of radiation scattered on layers of various optical thicknesses, with results compared for Rayleigh scattering and for scattering from a continental haze. In both cases, there are neutral points arising from the zeros of the polarization of single scattered photons at scattering angles of zero and 180 degrees. The angular position of these Rayleigh-like neutral points (RNP) in the sky shows appreciable variation with the optical thickness of the scattering layer for a Rayleigh phase matrix, but only a small variation for haze L phase matrix. Another type of neutral point exists for non-Rayleigh phase functions that is associated with the zeros of the polarization for single scattering which occurs between the end points of the curve. A comparison of radiances calculated from the complete theory of radiative transfer using Stokes vectors with those obtained from the scalar theory shows that differences of the order of 23% may be obtained for Rayleigh scattering, while the largest difference found for a haze L phase function was of the order of 0.1%.

Kattawar, G. W.

Multiple scattered radiation emerging from Rayleigh and continental haze layers. II - Ellipticity and direction of polarization

The ellipticity and the direction of polarization are calculated for radiation that has undergone multiple scattering from plane-parallel layers. Both the radiation emerging from the top of the layer and that transmitted through the bottom are considered. Two different phase functions are used for the scattering layer: Rayleigh and haze L. The direction of polarization of the reflected radiation shows little variation as the optical depth of the layer increases, but there is a much larger variation for the transmitted radiation. When the optical thickness is small, the direction of polarization for haze L varies rapidly with zenith angle near those angles at which the single-scattered polarization is zero. The ellipticity of the radiation from haze L layers increases at first in direct proportion to the optical thickness of the layer. In general, the ellipticity of the transmitted radiation is considerably greater than that of the reflected due to the greater average number of photon collisions in the former case. When the ellipticity is small, it is shown that the product of the polarization and the ellipticity is closely equal to -V/2I, where I and V are the first and fourth components of the Stokes vector.

Plass, G. N.

The correction of Landsat data for the effects of haze, sun angle, and background reflectance

A technique has been developed for simulating the effects of haze, sun angle, and background reflectance in Landsat data and correcting for them. The atmospheric model assumes a two-layer atmosphere: a Rayleigh scattering molecular layer and a Mie scattering haze layer next to the earth's surface. Reflection and transmission matrices describe the reflection and transmission properties of the plane parallel scattering layers. The multispectral scanner response is computed for various values of the parameters under evaluation. This yields expressions for Landsat gray-scale levels used for determining the effect of changes in any parameter. The Atmospheric Correction computer program is used to determine the haze level from the data, to compute the reflectance, and to interpolate in order to find the correction coefficients necessary to make the desired correction.

Potter, J. F.

Large Area Crop Inventory Experiment (LACIE). Effect of sun angle and haze on generation of LANDSAT imagery

The author has identified the following significant results. When heavy haze was present over a nonvegetated scene, the mean radiance values for all MSS channels were lowered, with the greatest decrease occurring in channels 1 and 2. Over a vegetated scene, any apparent decrease in mean radiance values due to haze may be marked by an increase in mean radiance values which occurred as vegetation increased in vigor during its growth cycle. Mean radiance values for nonvegetated targets (except water) were closely correlated to the changes in sun elevation angle throughout the year. A sun angle correction to a fixed reference data appeared to offer the possibility of compensating for haze covered areas by predicting the mean radiance values which would be closely correlated to the normal sun declination curve.

Chesnutwood, C. M.

Cloud and haze properties from Pioneer Venus polarimetry

Linear polarization measurements made by the Pioneer Venus orbiter cloud photopolarimeter determined that the low and midlatitude visible clouds mainly contain small H2SO4 droplets with an extensive haze of submicron particles above the cloud group. The polarization of the bright areas poleward of the 55 deg latitude results from the haze which exhibits large spatial and temporal variations. Significant diurnal differences are observed at low latitudes, with more haze close to the morning terminator than near the noon meridian.

Kawabata, K.

Venus -Mesospheric hazes of ice, dust, and acid aerosols

Four distinct types of particles are suggested to be present in the upper atmosphere of Venus. The lowest and densest haze may consist of a submicron sulfuric acid aerosol which extends above the cloud tops, up to about 80 km, representing an extension of the upper cloud deck. Temperature structure measurements in the 70-120 km altitude range indicate the occasional appearance of two independent water ice layers, of which the lower may form between 80 and 100 km and is probably the detached haze layer noted in high contrast limb photography. A nucleation of this ice layer on sulfuric acid aerosols is hypothesized. Temperatures of the Venus mesopause, near 120 km altitude, are frequently cold enough to allow ice nucleation on meteoric dust or ambient ions, yielding a haze (analogous to noctilucent clouds on earth) which is expected to be tenuous to the point of optical invisibility.

Turco, R. P.

High altitude Venus haze from Pioneer Venus limb scans

High-resolution limb scans of Venus made with the Orbiter Cloud Photopolarimeter aboard Pioneer Venus have been used to observe the high altitude Venus haze and its variation over almost one half a Venusian year. A model for a spherical atmosphere with tangential viewing geometry was used to analyze the observations and derive the haze properties. Values are found for the particle size and refractive index, particle number density and scale height, and eddy diffusion coefficient. Single scattering computations show good agreement with observed intensities for particles smaller than 0.3 micron radius and refractive index less than 1.7, consistent with, but not limited to, concentrated sulfuric acid. Particle scale height in the 0.5 to 2 mbar pressure regions varies between 1 and 3 km over the season, latitude, and local time ranges of the observations. Detached layers of haze are sometimes present. An average particle scale height of 2.2 km at 84 km altitude yields an eddy diffusion coefficient of 130,000 sq cm/sec.

Lane, W. A.

Saturn's equatorial haze

The amount of Raman scattering in Saturn's equatorial zone and polar regions near the central meridian at the wavelengths of the H and K Ca II solar lines, 3934 A and 3969 A was measured. Approximately 2.1 percent of the sunlight in this wavelength range is Raman scattered out of this range in Saturn's equatorial zone. Modeling the aerosol particle distribution as a clear, Rayleigh- and Raman-scattering gas over a dense haze yields an H2 column abundance of about 40 km-Amagats. Comparison with results obtained by Pioneer 11 suggests that either the equatorial haze was 2.5 times deeper at the time of these observations (May, 1981) than at the time of the Pioneer 11 flyby (Sept., 1979); or the haze particles are much more strongly polarizing in blue light than they are in red light.

Trafton, L.

Upper limits on possible photochemical hazes on Pluto

The suggestion by Elliot et al., (1989) that a haze layer near the surface of Pluto may be photochemical in origin and similar to the aerosol hazes in the atmospheres of other outer solar system bodies is evaluated. The nature of hazes which may be produced in the Hubbard et al., (1989) atmosphere is explored as well. It is concluded that the very low pressure in Pluto's atmosphere requires an aerosol production rate equal to the total maximum methane photolysis rate expected at Pluto.

Stansberry, John A.

The Properties and Effects of Titan's Organic Haze

Titan's organic haze is the the dominant absorber of solar energy in Titan's atmosphere, creating an anti-greenhouse effect. Its variation over time may have had important implications for Titan's surface temperature. The haze is potentially an important sink of photochemically produced carbon and nitrogen compounds. Laboratory simulations and microphysical models suggest that the haze is a sink for C of 4 x 10(exp 8)/ sq cm s, and a sink for N of 1 x 10(exp 8)sq cm s. The C sink is small compared to condensation of hydrocarbons but the sink for N is comparable to the total production rate of HCN. Because estimates of the eddy diffusion profile on Titan have been based on the HCN profile, inclusion of this additional sink for N will affect estimates for all transport processes in Titan's atmosphere.

McKay, Christopher P.

Titan haze: structure and properties of cyanoacetylene and cyanoacetylene-acetylene photopolymers

The structure and morphological properties of polymers produced photochemically from the UV irradiation of cyanoacetylene and cyanoacetylene mixtures have been examined to evaluate their possible contribution to the haze layers found on Titan. A structural analysis of these polymers may contribute to our understanding of the data returned from the Huygens probe of the Cassini mission that will pass through the atmosphere of Titan in the year 2004. Infrared analysis, elemental analysis, and thermal methods (thermogravimetric analysis, thermolysis, pyrolysis) were used to examine structures of polycyanoacetylenes produced by irradiation of the gas phase HC3N at 185 and 254 nm. The resulting brown to black polymer, which exists as small particles, is believed to be a branched chain of conjugated carbon-carbon double bonds, which, on exposure to heat, cyclizes to form a graphitic structure. Similar methods of analysis were used to show that when HC3N is photolyzed in the presence of Titan's other atmospheric constituents (CH4, C2H6, C2H2, and CO), a copolymer is formed in which the added gases are incorporated as substituents on the polymer chain. Of special significance is the copolymer of HC3N and acetylene (C2H2). Even in experiments where C2H2 was absorbing nearly all of the incident photons, the ratio of C2H2 to HC3N found in the resulting polymer was only 2:1. Scanning electron microscopy was used to visually examine the polymer particles. While pure polyacetylene particles are amorphous spheres roughly 1 micrometer in diameter, polycyanoacetylenes appear to be strands of rough, solid particles slightly smaller in size. The copolymer of HC3N and C2H2 exhibits characteristics of both pure polymers. This is particularly important as pure polyacetylenes do not match the optical constants measured for Titan's atmospheric hazes. The copolymers produced by the incorporation of other minor atmospheric constituents, like HC3N, into the polyacetylenes are expected to have optical constants more comparable to those of the Titan haze.

Non-NASA Center