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Tropospheric halogens - effect on ozone.

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The I2 absorption cross-section has been determined and the effects of column density of I2 are discussed. Citation: Spietz, P.; Gomez Martin, J.C.; Burrows, J.P., Effects of column density on I2 spectroscopy and determination of I2 absorption cross section at 500nm, accepted for publication on the Atmospheric Chemistry and Physics Discussions.
The UV absorption cross-section spectra of the atmospherically important radical BrO have been determined using the recently developed technique of time-windowing Fourier transform spectroscopy (TW-FTS). The absorption spectra of the A(2)Pi(3/2)-X(2)Pi(3/2) band system were recorded in the flash photolysis of a gaseous mixture of Br-2 and O-3. The bromine-photo sensitised decomposition of O-3 was observed at five different temperatures between 203 and 298 K. The absolute UV absorption cross-section was determined from the time-dependent observation of reactant and product absorptions and by a kinetic analysis of the BrO behaviour. The integrated UV absorption cross-section of BrO was, within the accuracy of the measurements, constant over the temperature range studied, as expected from spectroscopic considerations. For the (7, 0) vibrational band at 29 540cm-1 (338.5nm), the peak absorption cross-sections were determined to be 2.19+/-0.23 at 298K, 2.23+/-0.23 at 273K, 2.52+/-0.26 at 243K, 2.75+/-0.29 at 223K, and 3.03+/-0.31 at 203K (all in units X 10(-17) cm2 per molecule, at a spectral resolution of 3.8 cm-1, with error intervals of 2sigma). Further, vibrational constants and the dissociation limit for the electronic state A(2)Pi(3/2) were derived. The A <-- X dissociation energy was determined to be D-0 = 35 240+/-160cm-1 or 421.6+/-1.9kJ/mol. Citation: Fleischmann, O.C.; Burrows, J.P.; Hartmann, M.; Orphal, J. New ultraviolet absorption cross-sections of BrO at atmospheric temperatures measured by time-windowing Fourier-transform spectroscopy, Journal of Photochemistry and Photobiology A: Chemistry 168, 117-132, 2004
The kinetics of the BrO + HO2 reaction have been studied using the technique of flash photolysis / time resolved UV absorption spectroscopy and the rate coefficient for the reaction has been determined, at 298K and 760 Torr O2, as (2.35 +/- 0.82) E-11 / molecule / cm3/ s. In determining this reaction coefficient, work was also required on the study of the HO2 self-reaction in the presence of methanol, i.e. this result has delivered additional kinetic information, which is of use in subsequent laboratory studies here and elsewhere. The BrO + HO2 cycle is one of many inter-coupled catalytic ozone destruction cycles and, as such, accurate physico-chemical data are required for reliable modelling of atmospheric ozone. Increased reliability of physico-chemical data leads to increased reliability of models of atmospheric chemistry. The new data will be implemented in atmospheric chemistry models and it is expected to have an impact upon the accuracy of the modelling of ozone, especially in the stratosphere and in the marine boundary layer. This in turn has implications for the understanding of global change in areas of both atmospheric composition and climate. An accurate understanding of the BrO + HO2 is required in order to calculate the ozone depletion potential of source gases and hence this result may have policy implications in the regulation of source gas emissions.
The separation of overlapping absorption spectra in the context of multichannel time-resolved absorption spectroscopy and chemical kinetics is a particular case in the general problem of splitting the observed data into several linear components. Here, principal and independent components analysis are applied to kinetic data of iodine–ozone chemistry, which contains overlapping spectra of different absorbers. The objective of this work is to demonstrate a method, which in spite of this overlap is able to extract separated time traces of such absorbers. These time traces are clearly a pre-requisite for any further accurate quantitative analysis. The statistical properties of data recordings obtained from flash photolysis of I2 and O3 have been studied to check if the requirements of the model are fulfilled. Results of separation in appropriate spectral windows displaying overlapped vibrational features are presented. Validation is made using prior information and conventional techniques. Citation: Juan Carlos Gomez Martin, Peter Spietz, Johannes Orphal and John P. Burrows, Principal and independent components analysis of overlapping spectra in the context of multichannel time-resolved absorption spectroscopy, Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Volume 60, Issue 11, September 2004, Pages 2673-2693
Mercury in ambient air exists in the elemental form and it is distributed on a global scale. However, Canadian researchers have recently found that total gaseous mercury is significantly depleted in the Canadian Arctic during the months after polar sunrise. This study provided the first high-resolution mercury data for the Antarctic. It was found that mercury depletion events also occur in the Antarctic after polar sunrise. One explanation for mercury depletion may be the oxidation of elemental mercury, followed by adsorption and deposition of the oxidised form. This study found indications that BrO radicals and ozone play a key role in the boundary layer chemistry of springtime mercury depletion events in the Antarctic. This work has been widely disseminated through publication in an international journal. It shows an important feature of the global cycle of mercury: an increased input of atmospheric mercury to polar ecosystems is expected during the short springtime period, which coincides with the period of highest biological activity. This has environmental and public health implications. Ebinghaus R., H. H. Kock, C. Temme, J. W. Einax, A. G. Lowe, A. Richter, J.P. Burrows, and W. H. Schroeder, Antarctic Springtime Depletion of Atmospheric Mercury, Environ. Sci. Technol., 36(6), 1238-1244, 2002.
Over clear ocean waters, photons scattered within the water body contribute significantly to the up-welling flux. In addition to elastic scattering, inelastic Vibrational Raman Scattering (VRS) by liquid water is also playing a role and can have a strong impact on the spectral distribution of the outgoing radiance. Under clear-sky conditions, VRS has an influence on trace gas retrievals from space-borne measurements of the backscattered radiance such as from e.g. GOME (Global Ozone Monitoring Experiment). The effect is particularly important for geo-locations with small solar zenith angles and over waters with low chlorophyll concentration. Vountas, M., A. Richter, F. Wittrock, and J. P. Burrows, Inelastic scattering in ocean water and its impact on trace gas retrievals from satellite data, Atmos. Chem. Phys., 3, 1365-1375, 2003.
Following recent observations of molecular iodine (I2) in the coastal marine boundary layer (MBL) (Saiz-Lopez and Plane, 2004), it has become important to determine the absolute absorption cross-section of I2 at reasonably high resolution, and also to evaluate the rate of photolysis of the molecule in the lower atmosphere. The absolute absorption cross-section of gaseous I2 at room temperature and pressure (295K, 760Torr) was therefore measured between 182 and 750nm using a Fourier Transform spectrometer at a resolution of 4cm-1 (0.1nm at 500nm). The maximum absorption cross-section in the visible region was observed at 533.0nm to be (4.24±0.50)x10-18cm2molecule-1. The spectrum is available as supplementary material accompanying this paper. The photo-dissociation rate constant (J) of gaseous I2 was also measured directly in a solar simulator, yielding J(I2)=0.12±0.03s-1 for the lower troposphere. This is in excellent agreement with the value of 0.12±0.015s-1 calculated using the measured absorption cross-section, terrestrial solar flux for clear sky conditions and assuming a photo-dissociation yield of unity. A two-stream radiation transfer model was then used to determine the variation in photolysis rate with solar zenith angle (SZA), from which an analytic expression is derived for use in atmospheric models. Photolysis appears to be the dominant loss process for I2 during daytime, and hence an important source of iodine atoms in the lower atmosphere. This work has been published on the Internet and it is freely available to scientists and the general public alike. The molecular iodine spectrum has also been published in a format suitable for use by others (as supplementary material accompanying the paper). Citation: A. Saiz-Lopez, R. W. Saunders, D. M. Joseph, S. H. Ashworth, J. M. C. Plane, Absolute absorption cross-section and photolysis rate of I2, Atmospheric Chemistry and Physics, Vol. 4, pp 1443-1450, 1-9-2004
Model computations of slant column densities (SCD) enable the comparison between ground based and satellite based absorption measurements of scattered light and are therefore a good basis to investigate the presence of tropospheric BrO amounts. In this study ground based zenith sky and GOME nadir measurements of BrO SCD are compared with simulations for the 19-21 March 1997 at Ny-Alesund. The vertical columns of tropospheric BrO amounts are estimated to be in the range 4 +/- 0.8 * 10(13) [molecules/cm2] for the investigated period and location. Citation: Muller, R.W., H. Bovensmann, J. W. Kaiser, A. Richter, A. Rozanov, F. Wittrock, and J. P. Burrows, Consistent Interpretation of Ground based and GOME BrO Slant Column Data, Adv. Space Res., 29(11), 1655-1660, 2002
A review of the halogen chemistry of the marine boundary layer has been carried out and findings have been published in the Journal de Physique IV, France. The review summarises the current understanding of the science. Publication in a European journal allows knowledge, gained within the programme, to be disseminated to other scientists. The review is particularly useful to students and junior scientists within the field of atmospheric science. Moreover, the content of the review has been used in the training of students attending European courses (ERCA: European Research Course on Atmospheres). The main expected benefit of the result is to inform scientists and stimulate further research in the area. Citation: Adams, J.W. and R.A. Cox, Halogen chemistry of the marine boundary layer, J. Phys. IV 12 (2002) PR10, 105 - 124, 2002
Laser flash photolysis coupled to resonance-fluorescence detection of I atoms was used to measure the rate coefficients for the reactions: I + O3; IO + O2 (R1), O + I2; IO + I (R6) and I + NO2 + M; INO2 + M (R7). All experiments were conducted under pseudo first-order conditions, and the accuracy of the results was enhanced by online determination of reagent concentrations by optical absorption. Bimolecular rate coefficients for reactions (R1) and (R6) were determined to be k1 = (1.28 ± 0.06) ?10-12 and k6 = (1.2 ± 0.1) ?10-10 cm3 molecule 1s-1 at 298 ± 2K, independent of pressure. Rate coefficients for the termolecular reaction (R7), also at 298 ± 2K, were found to be in the falloff region between 3rd and 2nd order behaviour and, when combined with other datasets obtained at higher and lower pressures, were adequately described by a simplified Troe function with the parameters: k7,0(He, 330K) = 1.48 ?10-31 cm6 molecule-2s-1, FC(He) = 0.43, and k7; = 1.1 ?10-10 cm3 molecule-1s-1 for He as bath gas. In N2 (or air) the following parameters were obtained k7,0(N2, 300 K) = 3.2 ?10-31cm6 molecule-2s-1, FC(N2) = 0.48, with k7; set to 1.1 ?10-10cm3 molecule 1s-1 as obtained from analysis of the falloff curve obtained in He Citation: M.E. Tucceri, T.J. Dillon, and J.N. Crowley, J.N., A Laser Photolysis - Resonance Fluorescence Study of the Reactions: I + O3 -> IO + O2, O + I2 -> IO + I, and I + NO2 + M -> INO2 + M at 298K, Phys. Chem. Chem. Phys., 7, 1657 - 1663, 2005
The result is a comprehensive review of the applications of Differential Optical Absorption Spectroscopy to the study of halogen chemistry in the lower troposphere. The review also includes a discussion of the important ways in which halogens affect this region of the atmosphere. A brief description of the DOAS technique and its capabilities is also provided. Publication in a European journal allows knowledge, gained within the programme, to be disseminated to other scientists. The review is particularly useful to students and junior scientists within the field of atmospheric science. The main expected benefit of the result is to inform scientists and stimulate further research in the area. Citation: A. Saiz-Lopez and J.M.C. Plane, Recent applications of Differential Optical Absorption Spectroscopy: Halogen chemistry in the lower troposphere, J. Phys. IV France, vol 121, pages 223-238 (2004).
The kinetics of uptake of gaseous N2O5 on submicron aerosols containing NaCl and natural sea salt has been investigated in a flow reactor as a function of relative humidity (RH) in the range 30-80% at 295+/-2K and a total pressure of 1 bar. The measured uptake coefficients were larger on the aerosols containing sea salt compared to those of pure NaCl, and in both cases increased with increasing RH. These observations are explained in terms of the variation in water content and hence size of the salt droplets, which leads to a limitation in the uptake rate into small particles. After correction for this effect the uptake coefficients are independent of relative humidity, and agree with those measured previously on larger droplets. A value of g=0.025 is recommended for the reactive uptake coefficient for N2O5 on deliquesced sea salt droplets at 298K and RH>40%. Stewart, D. J. , Griffiths, P. T. and Cox, R. A., Reactive uptake coefficients for heterogeneous reaction of N2O5 with submicron aerosols of NaCl and natural sea salt, Atmospheric Chemistry and Physics, Vol. 4, pp 1381-1388, 25-8-2004
A technique for recording time-resolved absorption spectra using a commercial continuous-scan Fourier transform spectrometer (FTS) is presented. The method has been designed for the observation of experiments at temporal resolutions from 10(-4) to 10-2s, with delays longer than a second between two experimental repetitions. This is accomplished by synchronizing the observed experiment to certain positions of the interferometer-scanning mirror. Unlike other interleaving or stroboscopic techniques, a trigger is not generated for every interferogram point. Instead, time windows are used that are several interferogram points wide. For experiments with a low repetition rate (0.1-1Hz), the approach has advantages concerning measurement time and spectral resolution when compared to the step-scan and to fast-synchronized continuous-scan methods. The time-windowing Fourier transform spectrometer (TW-FTS) has been implemented as a hardware and software add-on to a commercial continuous-scan Michelson interferometer. No changes were made to the instrument. Two validation experiments were carried out by observing the formation and self-reaction of BrO after the flash photolysis of a Br-2/O-3 mixture at 298K. The experimental concentration-time profiles were in good agreement with decay curves from a chemical kinetics simulation of the experiments. Further, a LTV absorption spectrum of BrO, recorded by the TW-FTS method, had a comparable quality as a static FTS recording. Citation: Fleischmann, O.C.; Orphal, J.; Burrows, J.P. Time-Windowing Fourier Transform Absorption Spectroscopy for Flash Photolysis Investigations, Journal of Photochemistry and Photobiology A: Chemistry 157, 127-136, 2003.
By the utilization of a new laboratory method to synthesize OBrO employing an electric discharge, the visible absorption spectrum of gaseous OBrO has been investigated. Absorption spectra of OBrO have been recorded at 298 K, using a continuous-scan Fourier transform spectrometer at a spectral resolution of 0.8 cm-1. A detailed vibrational and rotational analysis of the observed transitions has been carried out. The FTS measurements provide experimental evidence that the visible absorption spectrum of OBrO results from the electronic transition C(2A2)-X(2B1). Vibrational constants have been determined for the C(2A2) state (1 = 648.3 ± 1.9cm-1 and 2 = 212.8 ± 1.2cm-1) and for the X(2B1) state (1 = 804.1 ± 0.8 cm-1 and 2 = 312.2 ± 0.5cm-1). The vibrational bands (1,0,0), (2,0,0), and (1,1,0) show rotational structure, whereas the other observed bands are unstructured because of strong pre-dissociation. Rotational constants have been determined experimentally for the upper electronic state C(2A2). By modelling the band contours, pre-dissociation lifetimes have been estimated. Further, an estimate for the absorption cross-section of OBrO has been made by assessing the bromine budget within the gas mixture, and atmospheric lifetimes of OBrO have been calculated using a photochemical model. Citation: Fleischmann, O.C.; Burrows, J.P.; Orphal, J. The visible absorption spectrum of OBrO investigated by Fourier transform spectroscopy, Journal of Physical Chemistry A, 2005; ASAP Article; doi: 10.1021/jp044911x
Measurements from the Global Ozone Monitoring Experiment (GOME) have been analysed for BrO absorption. An improvement to the existing data analysis method was required, to correct for a small angle dependency of the diffuser, leading to a significant improvement of the consistency of the BrO data set. Evidence has been found for appreciable tropospheric contributions to the BrO atmospheric columns, both from the polar boundary layer in spring and a global BrO background. The latter has been further investigated resulting in an estimate of 0.5 - 2 ppt uniformly mixed BrO in the troposphere. Results of this data analysis have been published and GOME data can also be accessed from the Institute web site. GOME data sets will be used within models of atmospheric chemistry. The expected benefit is to gain further understanding of atmospheric composition, now and in the future. In particular, modelling is being carried out, within THALOZ, in order to understand the BrO / Br / O3 relationship in the free troposphere. Citation: Richter, A., F. Wittrock, A. Ladstatter-Wei?enmayer and J.P. Burrows, GOME measurements of stratospheric and tropospheric BrO, Adv. Space Res., 29(11), 1667-1672, 2002
Frost flowers grow on newly formed sea ice from a saturated water vapour layer. They provide a large effective surface area and a reservoir of sea salt ions in the liquid phase with triple the ion concentration of seawater. Recently, frost flowers have been recognised as the dominant source of sea salt aerosol in the Antarctic, and it has been speculated that they could be involved in processes causing severe tropospheric ozone depletion events during the polar sunrise. These events can be explained by heterogeneous autocatalytic reactions taking place on salt-laden ice surfaces, which exponentially increase the reactive gas phase bromine ("bromine explosion"). We analyzed tropospheric bromine monoxide (BrO) and the sea ice coverage both measured from satellite sensors. Our model based interpretation shows that young ice regions potentially covered with frost flowers seem to be the source of bromine found in bromine explosion events. Publication in an international journal allows widespread dissemination of this work. Citation: Kaleschke, L., A. Richter, J. Burrows, O. Afe, G. Heygster, J. Notholt, A. M. Rankin, H. K. Roscoe, J. Hollwedel, T. Wagner, H.-W. Jacobi (2004), Frost flowers on sea ice as a source of sea salt and their influence on tropospheric halogen chemistry, Geophys. Res. Lett., 31, L16114, doi:10.1029/ 2004GL020655.
The UV-visible absorption spectrum of gaseous iodine nitrate (IONO2) has been measured over the wavelength range 245 - 415nm, using the technique of laser photolysis with time-resolved UV-visible absorption spectroscopy. Atmospheric iodine source gases are readily photolysed by sunlight yielding iodine atoms, which react with ozone to form IO. Subsequent reactions of IO can lead to catalytic ozone loss. In competition, IO can be removed into reservoir species. For example, IONO2 can be formed via reaction with nitrogen dioxide. The absorption coefficient of IONO2 is required in determining its atmospheric processing. The results indicate that IONO2 will have a photochemical lifetime of less than 1 minute under most sunlit conditions. Hence, IONO2 is not expected to act as a stable reservoir of atmospheric iodine during the day. Physico-chemical parameters, such as the IONO2 absorption cross-section, are used in models of atmospheric chemistry to gain understanding of atmospheric composition, and climate, at present and in the future. The IONO2 absorption cross-section data, measured here, is widely available to scientists due to dissemination of our results in an international journal Citation: Mossinger, J.C., D.M. Rowley and R.A. Cox, The UV-visible absorption cross-sections of IONO2, Atmos. Chem. Phys., 2, 227-234, 2002
Gaseous elemental mercury has a long atmospheric residence time. Any process that reduces this lifetime increases the potential accumulation of this toxic element in the biosphere. This study shows that rapid oxidation of mercury creates a rapidly depositing species of oxidised gaseous mercury. Data, from a remote site in the Arctic, shows that oxidised mercury can deposit to the surface in concentrations in excess of 900pg/cubic metre, following polar sunrise. A mechanism for mercury oxidation is proposed whereby halogen atoms (Br and Cl) and halogen oxide radicals (BrO and ClO) are the primary oxidants that produce the oxidised mercury. Several data sets suggest a recent increase in mercury levels in the Arctic, despite a 20-year decrease in global atmospheric mercury emissions. It is thus suggested that atmospheric mercury depletion events (i.e. events which increase deposition to the Arctic land / sea surface) are a recent phenomena and hence have implications for ecosystem (and human) health. Publication of this result in an international journal allows for wide dissemination, in the scientific community, and may prompt debate and further research into this area. Citation: Lindberg S. E., S. Brooks, C.-J. Lin, K. J. Scott, M. S. Landis, R. K. Stevens, M. Goodsite, A. Richter, Dynamic Oxidation of Gaseous Mercury in the Arctic Troposphere at Polar Sunrise, Environ. Sci. Technol., 36,1245-1256, 2002
Volcanic eruptions are known to be a major source of SO2 and some reactive halogen species notably HCl and HF. Recent studies have however observed the presence of large amounts of BrO with tight correlation to SO2 in a volcanic plume by ground-based spectroscopic measurements. In this work, upper limits of BrO columns have been estimated for a number of volcanic eruptions observed in measurements made by two satellite instruments - the Global Ozone Monitoring Experiment (GOME), and the new SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). The results obtained for the eruptions covered by satellite overpasses over the Etna, Nyamuragira, Popocate ;petl, and Reventador volcanoes show no correlation between enhanced volcanic SO2 during large eruptions and the corresponding BrO columns. Evidence for BrO enhancement was also not found in the vicinity of the Soufrie're Hills volcanoes. The possible reasons for the differences between ground-based and satellite observations are considered. A paper has been published in the scientific literature and thus is widely disseminated to the scientific community. Citation: Afe,O.T.,A.Richter,B.Sierk, F. Wittrock, and J. P. Burrows (2004), BrO emission from volcanoes: A survey using GOME and SCIAMACHY measurements, Geophys. Res. Lett., 31, L24113, doi:10.1029/ 2004GL020994.
The consistency of BrO column amounts derived from GOME spectra and from correlative ground-based and balloon measurements performed in 1998-1999 during the Third European Stratospheric Experiment on Ozone (THESEO) has been investigated. The study relies on UV-visible observations at several mid- and high latitude ground-based stations in both hemispheres, complemented by balloon-borne solar occultation profile measurements and 3D chemical transport model simulations. Previous investigations have reported GOME BrO columns systematically larger than those deduced from balloon, suggesting BrO being present, possibly ubiquitously, in the free troposphere. The robustness of this hypothesis has been further tested based on the presently available correlative data set. It is shown that when accounting for the BrO diurnal variation and the solar zenith angle dependency of the sensitivity of correlative data to the troposphere, measurements from all platforms are consistent with the presence of a tropospheric BrO background of 1-3 x10(13)molec/cm2 extending over mid- and high latitudes. Citation: van Roozendael, M., T. Wagner, A. Richter, I. Pundt, D. W. Arlander, J.P. Burrows, M. Chipperfield, C. Fayt, P.V. Johnston, J.-C. Lambert, K. Kreher, K. Pfeilsticker, U. Platt, J.-P. Pommereau, B.-M. Sinnhuber, K. K. Toernkvist, and F. Wittrock: Intercomparison of BrO Measurements from ERS
The kinetics of the reactions of O(3P) with various alkyl iodides (RI) was investigated using both discharge-flow (DF-RF) and the pulsed laser photolysis-resonance fluorescence (PLP-RF) technique at temperatures between 223 and 363K. The reactions studied were: (1) O(3P) + CF3I, (2) O(3P) + CH3I, (3) O(3P) + CH2I2, (4) O(3P) + C2H5I, (5) O(3P) + 1-C3H7I and (6) O(3P) + 2-C3H7I. Arrhenius expressions were obtained, with the exception of k1 and k3, all other rate coefficients display a negative temperature dependence, which highlights the importance of association complex formation in reactions of O(3P) + RI. Citation: Teruel MA, Dillon TJ, Horowitz A, Crowley JN, Reaction of O(P-3) with the alkyl iodides: CF3I, CH3I, CH2I2, C2H5I, 1-C3H7I and 2-C3H7I, PHYSICAL CHEMISTRY CHEMICAL PHYSICS 6 (9): 2172-2178 MAY 7 2004.
A simulation of marine boundary layer chemistry has been carried out in order to investigate chlorine atom release from marine aerosols. Measurements of iodine oxide (IO) and nitrate (NO3) radicals from field experiments were used to constrain model simulations. The results of these calculations show that the uptake of both HOI and N2O5 in the marine boundary layer has the potential to liberate chlorine atoms from sea-salt aerosol at a significant rate. Simulations show that a burst of chlorine production should be expected at sunrise due to photolysis of ICl formed overnight from HOI and Cl-. During the rest of the day, calculations show chlorine production to be steady, leading to steady state concentrations of Cl in the range of several hundred to a few thousand / cc, in accordance with some field studies. Chlorine atoms concentrations of a magnitude (10,000atoms /cc) capable of significantly influencing the oxidation potential of the atmosphere (for gases that are normally expected to react with OH e.g. methane, ethane and DMS) could be sustained by iodine-catalysed release alone. The production of chlorine is complex and depends upon the relative abundance of NOx and HOx chemistry and the abundance and mixing state of the aerosol. These results have been disseminated in the scientific press and are likely to provoke further research. The work may also prove to be of use in future field experiments e.g. the burst of chlorine at sunrise could be used as a diagnostic for this mechanism in future field experiments. Citation: McFiggans G, R.A. Cox, J.C. Mossinger, B.J. Allan and J.M.C. Plane, Active chlorine release from marine aerosols: Roles for reactive iodine and nitrogen species, J. Geophys. Res. 107 (D15) art. no. 4271, 2002.

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