scholarly journals The global middle-atmosphere aerosol model MAECHAM5-SAM2: comparison with satellite and in-situ observations

2010 ◽  
Vol 3 (3) ◽  
pp. 1359-1421
Author(s):  
R. Hommel ◽  
C. Timmreck ◽  
H. F. Graf
Keyword(s):  
Sulphuric Acid ◽  
Middle Atmosphere ◽  
Stratospheric Aerosol ◽  
Aerosol Layer ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Fine Mode ◽  
In Situ Observations ◽  
Polar Stratosphere

Abstract. In this paper we investigate results from a middle-atmosphere aerosol-climate model which has been developed to study the evolution of stratospheric aerosols. Here we focus on the stratospheric background period and evaluate several key quantities of the global dispersion of stratospheric aerosols and their precursors with observations and other model studies. It is shown that the model fairly well reproduces in situ observations of the aerosol size and number concentrations in the upper troposphere and lower stratosphere (UT/LS). Compared to measurements from the limb-sounding SAGE II satellite instrument, modelled integrated aerosol quantities are more biased the lower the moment of the aerosol population. Both findings are consistent with earlier work analysing the quality of SAGE II retrieved e.g. aerosol surface area densities from the volcanically unperturbed stratosphere (SPARC/ASAP, 2006; Thomason et al., 2008; Wurl et al., 2010). The model suggests that new particles are formed over large areas of the LS, albeit nucleation rates in the upper troposphere are at least one order of magnitude larger than those in the stratosphere. Hence, we suggest that both tropospheric sulphate aerosols and particles formed in situ in the LS are maintaining the stability of the stratospheric aerosol layer also in the absence of direct stratospheric emissions from volcanoes. Particle size distributions are clearly bimodal, except in the upper branches of the stratospheric aerosol layer where aerosols evaporate. Modelled concentrations of condensation nuclei (CN) are lesser than measured in regions of the aerosol layer where aerosol mixing ratios are largest, due to an overpredicted particle growth by coagulation. Transport regimes of tropical stratospheric aerosol have been identified from modelled aerosol mixing ratios and correspond to those deduced from satellite extinction measurements. We found that convective updraft in the Asian Monsoon region significantly contributes to both stratospheric aerosol load and size. The timing of formation and descend of layers of fine mode particles in the winter and spring polar stratosphere (CN layer) are reproduced by the model. Far above the tropopause where nucleation is inhibited due to with height increasing stratospheric temperatures, planetary wave mixing transports significant amounts of fine mode particles from the polar stratosphere to mid-latitudes. In those regions enhanced condensation rates of sulphuric acid vapour counteracts the evaporation of aerosols, hence prolonging the aerosol lifetime in the upper branches of the stratospheric aerosol layer. Measurements of the aerosol precursors SO2 and sulphuric acid vapour are fairly well reproduced by the model throughout the stratosphere.

scholarly journals The global middle-atmosphere aerosol model MAECHAM5-SAM2: comparison with satellite and in-situ observations

2011 ◽  
Vol 4 (3) ◽  
pp. 809-834 ◽  
Author(s):  
R. Hommel ◽  
C. Timmreck ◽  
H. F. Graf
Keyword(s):  
Sulphuric Acid ◽  
Middle Atmosphere ◽  
Stratospheric Aerosol ◽  
Aerosol Layer ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Fine Mode ◽  
In Situ Observations ◽  
Polar Stratosphere

Abstract. In this paper we investigate results from a three-dimensional middle-atmosphere aerosol-climate model which has been developed to study the evolution of stratospheric aerosols. Here we focus on the stratospheric background period and evaluate several key quantities of the global distribution of stratospheric aerosols and their precursors with observations and other model studies. It is shown that the model fairly well reproduces in situ observations of the aerosol size and number concentrations in the upper troposphere and lower stratosphere (UT/LS). Compared to measurements from the limb-sounding SAGE II satellite instrument, modelled integrated aerosol quantities are more biased the lower the moment of the aerosol population is. Both findings are consistent with earlier work analysing the quality of SAGE II retrieved e.g. aerosol surface area densities in the volcanically unperturbed stratosphere (SPARC/ASAP, 2006; Thomason et al., 2008; Wurl et al., 2010). The model suggests that new particles are formed over large areas of the LS, albeit nucleation rates in the upper troposphere are at least one order of magnitude larger than those in the stratosphere. Hence, we suggest that both, tropospheric sulphate aerosols and particles formed in situ in the LS are maintaining the stability of the stratospheric aerosol layer in the absence of direct stratospheric emissions from volcanoes. Particle size distributions are clearly bimodal, except in the upper branches of the stratospheric aerosol layer where aerosols evaporate. Modelled concentrations of condensation nuclei (CN) are smaller than measured in regions of the aerosol layer where aerosol mixing ratios are largest. This points to an overestimated particle growth by coagulation. Transport regimes of tropical stratospheric aerosol have been identified from modelled aerosol mixing ratios and correspond to those deduced from satellite extinction measurements. We found that convective updraft in the Asian Monsoon region significantly contributes to both stratospheric aerosol load and size. The timing of formation and descend of layers of fine mode particles in the winter and spring polar stratosphere (CN layer) are well reproduced by the model. Where temperatures in the stratosphere increase with altitude, nucleation is unlikely to occur. Nevertheless, in these regions we find a significant concentration of fine mode aerosols. The place of origin of these particles is in the polar stratosphere. They are mixed into the mid-latitudes by planetary waves. There enhanced condensation rates of sulphuric acid vapour counteract evaporation and extend aerosol lifetime in the upper branches of the stratospheric aerosol layer. Measured aerosol precursors concentrations, SO2 and sulphuric acid vapour, are fairly well reproduced by the model throughout the stratosphere.

scholarly journals Particulate sulfur in the upper troposphere and lowermost stratosphere – sources and climate forcing

2017 ◽  
Vol 17 (18) ◽  
pp. 10937-10953 ◽  
Author(s):  
Bengt G. Martinsson ◽  
Johan Friberg ◽  
Oscar S. Sandvik ◽  
Markus Hermann ◽  
Peter F. J. van Velthoven ◽  
...  
Keyword(s):  
Seasonal Variation ◽  
Radiative Forcing ◽  
Chemical Elements ◽  
Volcanic Eruptions ◽  
Stratospheric Aerosol ◽  
Aerosol Layer ◽  
Pixe Analysis ◽  
Upper Troposphere ◽  
Particulate Sulfur ◽  
Fine Mode

Abstract. This study is based on fine-mode aerosol samples collected in the upper troposphere (UT) and the lowermost stratosphere (LMS) of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8–12 km altitude of the IAGOS-CARIBIC platform in the time period 1999–2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission) and PESA (particle elastic scattering analysis). Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL). Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL) formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of particulate sulfur in the UT during times of volcanic influence and under background conditions.

scholarly journals Evidence for heterogeneous chlorine activation in the tropical UTLS

2010 ◽  
Vol 10 (7) ◽  
pp. 18063-18099
Author(s):  
M. von Hobe ◽  
J.-U. Grooß ◽  
G. Günther ◽  
P. Konopka ◽  
I. Gensch ◽  
...  
Keyword(s):  
Low Temperatures ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Gas Phase Chemistry ◽  
In Situ Observations ◽  
Field Campaigns ◽  
Phase Chemistry ◽  
The Tropics

Abstract. Airborne in-situ observations of ClO in the tropics were made during the TROCCINOX (Aracatuba, Brasil, February 2005) and SCOUT-O3 (Darwin, Australia, November/December 2005) field campaigns. While during most flights significant amounts of ClO (≈10–20 parts per trillion, ppt) were present only in aged stratospheric air, instances of enhanced ClO mixing ratios of up to 40 ppt – significantly exceeding those expected from gas phase chemistry – were observed in air masses of a more tropospheric character. Most of these observations concur with low temperatures or with the presence of cirrus clouds (often both), suggesting that cirrus ice particles and/or liquid aerosol at low temperatures may promote significant heterogeneous chlorine activation in the tropical upper troposphere lower stratosphere (UTLS). In two case studies, particularly high levels of ClO observed were reproduced by chemistry simulations only under the assumption that significant denoxification had occurred in the observed air. At least for one of these flights, a significant denoxification is in contrast to the observed NO levels suggesting that the coupling of chlorine and nitrogen compounds in the tropical UTLS may not be completely understood.

scholarly journals Evidence for heterogeneous chlorine activation in the tropical UTLS

2011 ◽  
Vol 11 (1) ◽  
pp. 241-256 ◽  
Author(s):  
M. von Hobe ◽  
J.-U. Grooß ◽  
G. Günther ◽  
P. Konopka ◽  
I. Gensch ◽  
...  
Keyword(s):  
Low Temperatures ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Gas Phase Chemistry ◽  
In Situ Observations ◽  
Field Campaigns ◽  
Phase Chemistry ◽  
The Tropics

Abstract. Airborne in-situ observations of ClO in the tropics were made during the TROCCINOX (Aracatuba, Brazil, February 2005) and SCOUT-O3 (Darwin, Australia, November/December 2005) field campaigns. While during most flights significant amounts of ClO (≈10–20 parts per trillion, ppt) were present only in aged stratospheric air, instances of enhanced ClO mixing ratios of up to 40 ppt – significantly exceeding those expected from gas phase chemistry – were observed in air masses of a more tropospheric character. Most of these observations are associated with low temperatures or with the presence of cirrus clouds (often both), suggesting that cirrus ice particles and/or liquid aerosol at low temperatures may promote significant heterogeneous chlorine activation in the tropical upper troposphere lower stratosphere (UTLS). In two case studies, particularly high levels of ClO observed were reproduced by chemistry simulations only under the assumption that significant denoxification had occurred in the observed air. However, to reproduce the ClO observations in these simulations, O3 mixing ratios higher than observed had to be assumed, and at least for one of these flights, a significant denoxification is in contrast to the observed NO levels, suggesting that the coupling of chlorine and nitrogen compounds in the tropical UTLS may not be completely understood.

scholarly journals Simultaneous and co-located wind measurements in the middle atmosphere by lidar and rocket-borne techniques

2016 ◽  
Vol 9 (8) ◽  
pp. 3911-3919 ◽  
Author(s):  
Franz-Josef Lübken ◽  
Gerd Baumgarten ◽  
Jens Hildebrand ◽  
Francis J. Schmidlin
Keyword(s):  
Middle Atmosphere ◽  
Systematic Difference ◽  
Horizontal Distance ◽  
In Situ Method ◽  
Time Period ◽  
Meridional Winds ◽  
Wind Measurements ◽  
In Situ Observations ◽  
Mean Differences

Abstract. We present the first comparison of a new lidar technique to measure winds in the middle atmosphere, called DoRIS (Doppler Rayleigh Iodine Spectrometer), with a rocket-borne in situ method, which relies on measuring the horizontal drift of a target (“starute”) by a tracking radar. The launches took place from the Andøya Space Center (ASC), very close to the ALOMAR observatory (Arctic Lidar Observatory for Middle Atmosphere Research) at 69° N. DoRIS is part of a steerable twin lidar system installed at ALOMAR. The observations were made simultaneously and with a horizontal distance between the two lidar beams and the starute trajectories of typically 0–40 km only. DoRIS measured winds from 14 March 2015, 17:00 UTC, to 15 March 2015, 11:30 UTC. A total of eight starute flights were launched successfully from 14 March, 19:00 UTC, to 15 March, 00:19 UTC. In general there is excellent agreement between DoRIS and the in situ measurements, considering the combined range of uncertainties. This concerns not only the general height structures of zonal and meridional winds and their temporal developments, but also some wavy structures. Considering the comparison between all starute flights and all DoRIS observations in a time period of ±20 min around each individual starute flight, we arrive at mean differences of typically ±5–10 m s−1 for both wind components. Part of the remaining differences are most likely due to the detection of different wave fronts of gravity waves. There is no systematic difference between DoRIS and the in situ observations above 30 km. Below ∼ 30 km, winds from DoRIS are systematically too large by up to 10–20 m s−1, which can be explained by the presence of aerosols. This is proven by deriving the backscatter ratios at two different wavelengths. These ratios are larger than unity, which is an indication of the presence of aerosols.

scholarly journals Level 2 processing for the imaging Fourier transform spectrometer GLORIA: derivation and validation of temperature and trace gas volume mixing ratios from calibrated dynamics mode spectra

2015 ◽  
Vol 8 (6) ◽  
pp. 2473-2489 ◽  
Author(s):  
J. Ungermann ◽  
J. Blank ◽  
M. Dick ◽  
A. Ebersoldt ◽  
F. Friedl-Vallon ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Horizontal Resolution ◽  
Trace Gas ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Ionization Mass ◽  
Fourier Transform Spectrometer ◽  
Upper Troposphere ◽  
Mixing Ratios

Abstract. The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an airborne infrared limb imager combining a two-dimensional infrared detector with a Fourier transform spectrometer. It was operated aboard the new German Gulfstream G550 High Altitude LOng Range (HALO) research aircraft during the Transport And Composition in the upper Troposphere/lowermost Stratosphere (TACTS) and Earth System Model Validation (ESMVAL) campaigns in summer 2012. This paper describes the retrieval of temperature and trace gas (H2O, O3, HNO3) volume mixing ratios from GLORIA dynamics mode spectra that are spectrally sampled every 0.625 cm−1. A total of 26 integrated spectral windows are employed in a joint fit to retrieve seven targets using consecutively a fast and an accurate tabulated radiative transfer model. Typical diagnostic quantities are provided including effects of uncertainties in the calibration and horizontal resolution along the line of sight. Simultaneous in situ observations by the Basic Halo Measurement and Sensor System (BAHAMAS), the Fast In-situ Stratospheric Hygrometer (FISH), an ozone detector named Fairo, and the Atmospheric chemical Ionization Mass Spectrometer (AIMS) allow a validation of retrieved values for three flights in the upper troposphere/lowermost stratosphere region spanning polar and sub-tropical latitudes. A high correlation is achieved between the remote sensing and the in situ trace gas data, and discrepancies can to a large extent be attributed to differences in the probed air masses caused by different sampling characteristics of the instruments. This 1-D processing of GLORIA dynamics mode spectra provides the basis for future tomographic inversions from circular and linear flight paths to better understand selected dynamical processes of the upper troposphere and lowermost stratosphere.

scholarly journals Interactions of meteoric smoke particles with sulphuric acid in the Earth's stratosphere

2012 ◽  
Vol 12 (1) ◽  
pp. 1553-1584
Author(s):  
R. W. Saunders ◽  
S. Dhomse ◽  
W. S. Tian ◽  
M. P. Chipperfield ◽  
J. M. C. Plane
Keyword(s):  
Sulphuric Acid ◽  
Climate Model ◽  
Middle Atmosphere ◽  
Magnesium Silicate ◽  
Stratospheric Aerosol ◽  
Solution Viscosity ◽  
Time Resolved ◽  
Optical Extinction ◽  
Smoke Particles ◽  
Meteoric Smoke

Abstract. Nano-sized meteoric smoke particles (MSPs) with iron-magnesium silicate compositions, formed in the upper mesosphere as a result of meteoric ablation, may remove sulphuric acid from the gas-phase above 40 km and may also affect the composition and behaviour of supercooled H2SO4-H2O droplets in the global stratospheric aerosol (Junge) layer. This study describes a time-resolved spectroscopic analysis of the evolution of the ferric (Fe3+) ion originating from amorphous ferrous (Fe2+)-based silicate powders dissolved in varying Wt % sulphuric acid (30–75%) solutions over a temperature range of 223–295 K. Complete dissolution of the particles was observed under all conditions. The first-order rate coefficient for dissolution decreases at higher Wt % and lower temperature, which is consistent with the increased solution viscosity limiting diffusion of H2SO4 to the particle surfaces. Dissolution under stratospheric conditions should take less than a week, and is much faster than the dissolution of crystalline Fe2+ compounds. The chemistry climate model UMSLIMCAT (based on the UKMO Unified Model) was then used to study the transport of MSPs through the middle atmosphere. A series of model experiments were performed with different uptake coefficients. Setting the concentration of 1.5 nm radius MSPs at 80 km to 3000 cm−3 (based on rocket-borne charged particle measurements), the model matches the reported Wt % Fe values of 0.5–1.0 in Junge layer sulphate particles, and the MSP optical extinction between 40 and 75 km measured by a satellite-borne spectrometer, if the global meteoric input rate is about 20 t d−1. The model indicates that an uptake coefficient ≥0.01 is required to account for the observed two orders of magnitude depletion of H2SO4 vapour above 40 km.

scholarly journals Origins and characterization of CO and O<sub>3</sub> in the African upper troposphere

2021 ◽  
Author(s):  
Victor Lannuque ◽  
Bastien Sauvage ◽  
Brice Barret ◽  
Hannah Clark ◽  
Gilles Athier ◽  
...  
Keyword(s):  
Wind Shear ◽  
Asian Monsoon ◽  
Shear Zones ◽  
Hadley Cell ◽  
Trade Winds ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Hadley Cells

Abstract. Between December 2005 and 2013, the In-service Aircraft for a Global Observing System (IAGOS) program produced almost daily in situ measurements of CO and O3 between Europe and southern Africa. IAGOS data combined with measurements from the IASI instrument onboard the Metop-A satellite (2008–2013) are used to characterize meridional distributions and seasonality of CO and O3 in the African upper troposphere (UT). The FLEXPART particle dispersion model and the SOFT-IO model which combines the FLEXPART model with CO emission inventories are used to explore the sources and origins of the observed transects of CO and O3. We focus our analysis on two main seasons: December to March (DJFM) and June to October (JJASO). These seasons have been defined according to the position of Intertropical Convergence Zone (ITCZ), determined using in situ measurements from IAGOS. During both seasons, the UT CO meridional transects are characterized by maximum mixing ratios located 10° from the position of the ITCZ above the dry regions inside the hemisphere of the strongest Hadley cell (132 to 165 ppb at 0–5° N in DJFM and 128 to 149 ppb at 3–7° S in JJASO), and decreasing values south- and north-ward. The O3 meridional transects are characterized by mixing ratio minima of ~ 42–54 ppb at the ITCZ (10–16° S in DJFM and 5–8° N in JJASO) framed by local maxima (~ 53–71 ppb) coincident with the wind shear zones North and South of the ITCZ. O3 gradients are strongest in the hemisphere of the strongest Hadley cell. IASI UT O3 distributions in DJFM have revealed that the maxima are a part of a crescent-shaped O3 plume above the Atlantic Ocean around the Gulf of Guinea. CO emitted at the surface is transported towards the ITCZ by the trade winds and then convectively uplifted. Once in the upper troposphere, CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maximum CO mixing ratios are found. Anthropogenic and fires both contribute, by the same order of magnitude, to the CO budget of the African upper troposphere. Local fires have the highest contribution, drive the location of the observed UT CO maxima, and are related to the following transport pathway: CO emitted at the surface is transported towards the ITCZ by the trade winds and further convectively uplifted. Then UT CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maxima are located. Anthropogenic CO contribution is mostly from Africa during the entire year, with a low seasonal variability, and is related to similar transport circulation than fire air masses. There is also a large contribution from Asia in JJASO related to the fast convective uplift of polluted air masses in the Asian monsoon region which are further westward transported by the tropical easterly jet (TEJ) and the Asian monsoon anticyclone (AMA). O3 minima correspond to air masses that were recently uplifted from the surface where mixing ratios are low at the ITCZ. The O3 maxima correspond to old high altitude air masses uplifted from either local or long distance area of high O3 precursor emissions (Africa and South America during all the year, South Asia mainly in JJASO), and must be created during transport by photochemistry. This analysis of meridional transects contribute to a better understanding of distributions of CO and O3 in the intertropical African upper troposphere and the processes which drive these distributions. Therefore, it provides a solid basis for comparison and improvement of models and satellite products in order to get the good O3 for the good reasons.

The prevalence of meteoric-sulphuric particles within the stratospheric aerosol layer

2021 ◽  
Author(s):  
Graham Mann ◽  
James Brooke ◽  
Kamalika Sengupta ◽  
Lauren Marshall ◽  
Sandip Dhomse ◽  
...  
Keyword(s):  
High Latitude ◽  
Climate Model ◽  
Polar Vortex ◽  
Stratospheric Aerosol ◽  
Light Extinction ◽  
The Arctic ◽  
Aerosol Layer ◽  
Aerosol Composition ◽  
Particle Layer

&lt;p&gt;The widespread presence of meteoric smoke particles (MSPs) within a distinct class of stratospheric aerosol particles has become clear from in-situ measurements in the Arctic, Antarctic and at mid-latitudes.&lt;br&gt;&amp;#160;&lt;br&gt;We apply an adapted version of the interactive stratosphere aerosol configuration of the composition-climate model UM-UKCA, to predict the global distribution of meteoric-sulphuric particles nucleated heterogeneously on MSP cores. We compare the UM-UKCA results to new MSP-sulphuric simulations with the European stratosphere-troposphere chemistry-aerosol modelling system IFS-CB05-BASCOE-GLOMAP.&lt;/p&gt;&lt;p&gt;&lt;br&gt;The simulations show a strong seasonal cycle in meteoric-sulphuric particle abundance results from the winter-time source of MSPs transported down into the stratosphere in the polar vortex. Coagulation during downward transport sees high latitude MSP concentrations reduce from ~500 per cm3 at 40km to ~20 per cm3 at 25km, the uppermost extent of the stratospheric aerosol particle layer (the Junge layer).&lt;br&gt;&amp;#160;&lt;br&gt;Once within the Junge layer's supersaturated environment, meteoric-sulphuric particles form readily on the MSP cores, growing to 50-70nm dry-diameter (Dp) at 20-25km. Further inter-particle coagulation between these non-volatile particles reduces their number to 1-5 per cc at 15-20km, particle sizes there larger, at Dp ~100nm.&lt;/p&gt;&lt;p&gt;&lt;br&gt;The model predicts meteoric-sulphurics in high-latitude winter comprise &gt;90% of Dp&gt;10nm particles above 25km, reducing to ~40% at 20km, and ~10% at 15km.&lt;br&gt;&amp;#160;&lt;br&gt;These non-volatile particle fractions are slightly less than measured from high-altitude aircraft in the lowermost Arctic stratosphere (Curtius et al., 2005; Weigel et al., 2014), and consistent with mid-latitude aircraft measurements of lower stratospheric aerosol composition (Murphy et al., 1998), total particle concentrations &amp;#160;also matching in-situ balloon measurements from Wyoming (Campbell and Deshler, 2014).&lt;br&gt;&amp;#160;&lt;br&gt;The MSP-sulphuric interactions also improve agreement with SAGE-II observed stratospheric aerosol extinction in the quiescent 1998-2002 period.&amp;#160;&lt;br&gt;&amp;#160;&lt;br&gt;Simulations with a factor-8-elevated MSP input form more Dp&gt;10nm meteoric-sulphurics, but the increased number sees fewer growing to Dp ~100nm, the increased MSPs reducing the stratospheric aerosol layer&amp;#8217;s light extinction.&lt;/p&gt;

scholarly journals Chlorine nitrate in the atmosphere

2018 ◽  
Vol 18 (20) ◽  
pp. 15363-15386 ◽  
Author(s):  
Thomas von Clarmann ◽  
Sören Johansson
Keyword(s):  
Atmospheric Chemistry ◽  
Infrared Emission ◽  
Chlorine Nitrate ◽  
Rotational Bands ◽  
In Situ Techniques ◽  
Mixing Ratios ◽  
Gas Phase Chemistry ◽  
Polar Stratosphere ◽  
Phase Chemistry

Abstract. This review article compiles the characteristics of the gas chlorine nitrate and discusses its role in atmospheric chemistry. Chlorine nitrate is a reservoir of both stratospheric chlorine and nitrogen. It is formed by a termolecular reaction of ClO and NO2. Sink processes include gas-phase chemistry, photo-dissociation, and heterogeneous chemistry on aerosols. The latter sink is particularly important in the context of polar spring stratospheric chlorine activation. ClONO2 has vibrational–rotational bands in the infrared, notably at 779, 809, 1293, and 1735 cm−1, which are used for remote sensing of ClONO2 in the atmosphere. Mid-infrared emission and absorption spectroscopy have long been the only concepts for atmospheric ClONO2 measurements. More recently, fluorescence and mass spectroscopic in situ techniques have been developed. Global ClONO2 distributions have a maximum at polar winter latitudes at about 20–30 km altitude, where mixing ratios can exceed 2 ppbv. The annual cycle is most pronounced in the polar stratosphere, where ClONO2 concentrations are an indicator of chlorine activation and de-activation.

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