Nitrogen‐sulfur compounds in stratospheric aerosols

Farlow, N. H.; Snetsinger, K. G.; Hayes, Dennis M.; Lem, Homer Y.; Tooper, Bernadine M.

doi:10.1029/jc083ic12p06207

Cited by 25 publications

(13 citation statements)

References 10 publications

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“…A quantitative understanding of atmospheric motions, as well as of particle microphysics, is necessary in order to understand the spatial distribution of particle number and su~face area in the stratosphere. Fourth, several statistically robust studies of stratospheric particle composition (16,37) have not found the diversity of particle compositions typical of the mid-latitude free troposphere (1 6). However, homogeneous nucleation of H,SO,-H,O particles near the tropical tropopause, followed by vertical transport to the lower tropical stratosphere, would explain the relative homogeneity of stratospheric particle composition observed.…”

Section: O4mentioning

confidence: 99%

Particle Formation in the Upper Tropical Troposphere: A Source of Nuclei for the Stratospheric Aerosol

Brock

Hamill

Wilson

et al. 1995

Science

228

240

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to the Gleissberg minimum early in this century. However, the observed increase of about 20% is four times that expected based on the sunspot numbers.The observed high 44Ti and the inferred high GCR flux during the Gleissberg minimum suggest a much-weakened modulation of GCR during prolonged solar quiet periods. The heliosphere, during the 11vear solar cvcles. is divided into two hemispheres of dpposite polarity by a wavy heliospheric neutral sheet (HNS) whose inclination to the sun's rotational eauator increases from a few degrees at solar minimum to >70° at solar maximum and whose undulations also increase with solar activity (15). The HMF is relatively smooth during the solar minima. The enhanced GCR fluxes required for the higher production of 44Ti can be achieved if (i) the HNS becomes smooth and remains close to the helioequator; (ii) the HMF becomes weak, more regular, and orderlv; or (iii) the size of the , , . ,

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Section: O4mentioning

confidence: 99%

Particle Formation in the Upper Tropical Troposphere: A Source of Nuclei for the Stratospheric Aerosol

Brock

Hamill

Wilson

et al. 1995

Science

228

240

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“…They list several sources for producing it in the stratosphere and they carried out thermodynamic and chemical kinetic calculations at one stratospheric altitude and at one latitude. NSA has been overlooked in+all previous stratospheric model calculations, even though it has been observed in stratospheric sulfate aerosols (Farlow et al 1978). This study makes large scale atmospheric model calculations to test the proposal by Burley and Johnston [ 1992a,b] that a promising heterogeneous process for activating HC1 in sulfuric acid particles is a catalytic couple based on nitrosyl sulfuric acid (NSA).…”

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confidence: 99%

“…In re-analyzing total ozone data from a NASA satellite for the period 1978-1990(Stolarski ei al. 1991 found unexpectedly high ozone reductions at mid to high-latitudes of both hemispheres, for example a 8% ozone reduction at 60"N between 1980 and 1990.…”

Section: Introductionmentioning

confidence: 99%

“…

ABSTRACTIn re-analyzing total ozone data from a NASA satellite for the period 1978 -1990 found unexpectedly high ozone reductions at mid to high-latitudes of both hemispheres, for example a 8% ozone reduction at 60"N between 1980 and 1990. The Junge layer of particulates in the lower stratosphere is composed primarily of super-cooled liquid sulfuric acid with dissolved water and trace amounts of other species.

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confidence: 99%

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Evaluating the importance of innovative heterogeneous chemistry to explain observed stratospheric ozone depletion

Kinnison¹,

Connell²

1996

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In re-analyzing total ozone data from a NASA satellite for the period 1978 -1990 found unexpectedly high ozone reductions at mid to high-latitudes of both hemispheres, for example a 8% ozone reduction at 60"N between 1980 and 1990. The Junge layer of particulates in the lower stratosphere is composed primarily of super-cooled liquid sulfuric acid with dissolved water and trace amounts of other species. Rodriquez et al. [1991] demonstrated with model calculations that the heterogeneous reaction of N2O5 with water in sulfate aerosols may contribute to the high ozone reductions at midlatitudes. Recently, the 15 June 1991 volcanic eruption of Mt. Pinatubo resulted in large amounts of sulfur containing particles in the stratosphere. Complete conversion of SO2 to H2SO4 aerosols occurred within a few months after the eruption. Balloon sondes and satellite data suggest that stratospheric ozone decreased 6-10% in the tropics by October 1991. Ground based measurements along with ozone sonde and satellite measurements show above average loss of ozone in 1992 and 1993. Currently, there is a widespread search for additional heterogeneous reactions or combination of heterogeneous and homogeneous (gas-phase) reactions that could catalytically reduce ozone to observed levels. Burley and Johnston [1992a,b], of the University of California at Berkeley, proposed that nitrosyl sulfuric acid (NSA) NOHS04, is a promising heterogeneous reactant for activating HC1 in sulfuric acid particles. They list several sources for producing it in the stratosphere and they carried out thermodynamic and chemical kinetic calculations at one stratospheric altitude and at one latitude. NSA has been overlooked in+all previous stratospheric model calculations, even though it has been observed in stratospheric sulfate aerosols (Farlow et al. 1978). This study makes large scale atmospheric model calculations to test the proposal by Burley and Johnston [ 1992a,b] that a promising heterogeneous process for activating HC1 in sulfuric acid particles is a catalytic couple based on nitrosyl sulfuric acid (NSA). This mechanism would convert HCl, which is a reservoir species for chlorine free radicals, into a form that catalytically reduces ozone. These calculations used the LLNL 2-D zonally averaged chemical-radiative-transport model of the troposphere and stratosphere.These calculations set firm limits on the range of kinetic parameters over which this heterogeneous reaction would be important in the global ozone balance, and thus be a guide for where laboratory work is needed.

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“…Identification by electron diffraction showed that the stratospheric aerosol particles are composed mainly of ammonium sulfate (Friend, 1966;Cadle et al, 1969;Farlow et al, 1978). On the other hand, the wet chemical analysis showed that the concentration of the ammonium ion associated with sulfate ion was surprisingly low (Lazrus et al, 1971;Cadle et al, 1969).…”

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Chemical and Physical Properties of Stratospheric Aerosol Particles in the Vicinity of Tropopause Folding

Yamato

Ono

1989

Journal of the Meteorological Society of Japan

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The chemical composition and physical state of individual aerosol particles were examined for the aerosol collected on board an aircraft. The collection of aerosol particles was carried out at altitudes between 2.0 and 7.6km including the vicinity of tropopause folding and above tropopause over the Japan Sea on 14 February, 1984. The molecular state of sulfate particles was determined by vapordeposited calcium thin-film method (pre-coating) in order to avoid the possible chemical modification of samples by ammonia after collection. Nitrate and sulfate in particles were detected by use of the vapor-deposited nitron thin-film method and barium chloride thin-film method, respectively. Whether stratospheric aerosol particles are frozen or supercooled was examined by comparing the morphology of collected particles with that of frozen sulfuric acid particles produced in the laboratory.Sulfuric acid particles were predominant in the stratosphere without any serious ammoniation. These sulfuric acid particles are much larger than those in the lower troposphere. No nitrate-containing particles and few particles of tropospheric origin were found in the stratosphere. The fact that nitrate can not be detected in the particles suggests that most of the nitric acid is not dissolved in particles but exists in the gas phase in the stratosphere. Stratospheric sulfuric acid particles were not frozen, but supercooled even at -48*. Stratospheric aerosols were constituted of sulfuric acid particles, of which the chemical composition was much more uniform in space than that of tropospheric aerosols. We can safely state that supercooled sulfuric acid particles are predominant in the mid-latitude stratosphere.On the other hand, aerosols of several different origins coexisted in the troposphere. Sulfuric acid particles were mostly predominant in the middle and upper troposphere, although their ammoniated particles also existed. Acidity of the sulfate-containing particles increased with increasing altitude between 2.0 and 5.5km. It was observed that stratospheric sulfuric acid particles coexisted with particles of lower tropospheric origin (probably ammonium sulfate particles) in the tropopause folding. The observation was carried out during the period when there was a slight possibility that the effect of volcanic eruption of E1 chichon in 1982 on the stratospheric aerosol layer still remained. However, it is not possible to determine the degree of any volcanic effect from the present study.

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Nitrogen‐sulfur compounds in stratospheric aerosols

Cited by 25 publications

References 10 publications

Particle Formation in the Upper Tropical Troposphere: A Source of Nuclei for the Stratospheric Aerosol

Particle Formation in the Upper Tropical Troposphere: A Source of Nuclei for the Stratospheric Aerosol

Evaluating the importance of innovative heterogeneous chemistry to explain observed stratospheric ozone depletion

Chemical and Physical Properties of Stratospheric Aerosol Particles in the Vicinity of Tropopause Folding

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