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Observational evidences of the influences of tropospheric subtropical and midlatitude stratospheric westerly jets on the equatorial stratospheric intraseasonal oscillations

Using six Global Positioning System (GPS) Radio Occultation (RO) satellites (SAC-C, METOP-A and COSMIC/FORMOSAT-3, CNOFS, GRACE and TerraSAR-X) determined height profiles (1–40 km) of atmospheric temperature over the Indian tropical station of Gadanki and the European Center for Medium Range Weather Forecast (ECMWF) Interim Reanalyses (ERA-Interim) zonal wind and temperature data for four years (2009–2012), the present work reports that the tropospheric Subtropical Westerly Jet (SWJ) and the Midlatitude Stratospheric Westerly Jet (MStWJ) play important roles in controlling differently the vertical propagation of tropical Intra Seasonal Oscillations (ISO) with different period bands from the troposphere up to the stratosphere during Northern winters. In the months of December–May (Northern winter to summer, NWTS) of all these years, there is significant 10–20 day and 20–40 day oscillations in the troposphere up to the height of 13 km and above this it reappears at all heights above 21 km. The 40–80 day oscillation also shows similar characteristics except that it almost disappeared during NWTS months of the year 2010–2011 in the stratosphere. The absence of these signals in the intervening heights of ~ 17–20 km is explained on the basis that these two bands actually propagate from the tropical to subtropical region near the tropopause and then reappears in the tropical stratosphere after refracted by the subtropical westerly jet. The poleward and equatorward propagation of these bands in the troposphere and stratosphere respectively are found using the ERA-interim data. Further the two longer period bands of ISO show strong quasi-biennial oscillation in the lower atmosphere with opposite phases (when one band shows maximum the other one shows minimum in a particular year) between these two bands. It is also observed that the phase of the tropical stratospheric Quasi Biennial Oscillation (QBO) has significant control on the strength of the Mid latitude stratospheric westerly jet (MStWJ) that in turn controls the refraction of the tropical tropospheric longer (40–80 days, Longer period ISO; LISO) but not the smaller periods of ISO (SISO) back to the tropical stratosphere. In accordance with earlier theoretical modelling studies, the westerly phase of the lower stratospheric QBO occurred during NWTS months of 2010–2011 over the Indian longitudinal sector causes severe disruption of the MStWJ at 30 km height. This disruption caused the prevention of refraction back again to the tropical stratosphere of significant tropospheric LISO that arrived from the tropics through the tropopause. Further, in these four years, it is observed no direct vertical propagation of tropical tropospheric ISO to the stratosphere. The interannual variations in the tropical stratospheric LISO are related strongly to the phase of the equatorial lower stratospheric QBO in zonal wind and the strength of the MStWJ.
Non-OH chemistry in oxidation flow reactors for the study of atmospheric chemistry systematically examined by modeling

Oxidation flow reactors (OFRs) using low-pressure Hg lamp emission at 185 and 254 nm produce OH radicals efficiently and are widely used in atmospheric chemistry and other fields. However, knowledge of detailed OFR chemistry is limited, allowing speculation in the literature about whether some non-OH reactants, including several not relevant for tropospheric chemistry, may play an important role in these OFRs. These non-OH reactants are UV radiation, O(1D), O(3P), and O3. In this study, we investigate the relative importance of other reactants to OH for the fate of reactant species in OFR under a wide range of conditions via box modeling. The relative importance of non-OH species is less sensitive to UV light intensity than to water vapor mixing ratio (H2O) and external OH reactivity (OHRext), as both non-OH reactants and OH scale roughly proportionally to UV intensity. We show that for field studies in forested regions and also the urban area of Los Angeles, reactants of atmospheric interest are predominantly consumed by OH. We find that O(1D), O(3P), and O3 have relative contributions to volatile organic compound (VOC) consumption that are similar or lower than in the troposphere. The impact of O atoms can be neglected under most conditions in both OFR and troposphere. We define “riskier OFR conditions” as those with either low H2O (< 0.1 %) or high OHRext ( ≥  100 s−1 in OFR185 and > 200 s−1 in OFR254). We strongly suggest avoiding such conditions as the importance of non-OH reactants can be substantial for the most sensitive species, although OH may still dominate under some riskier conditions, depending on the species present. Photolysis at non-tropospheric wavelengths (185 and 254 nm) may play a significant (> 20 %) role in the degradation of some aromatics, as well as some oxidation intermediates, under riskier reactor conditions, if the quantum yields are high. Under riskier conditions, some biogenics can have substantial destructions by O3, similarly to the troposphere. Working under low O2 (volume mixing ratio of 0.002) with the OFR185 mode allows OH to completely dominate over O3 reactions even for the biogenic species most reactive with O3. Non-tropospheric VOC photolysis may have been a problem in some laboratory and source studies, but can be avoided or lessened in future studies by diluting source emissions and working at lower precursor concentrations in laboratory studies and by humidification. Photolysis of secondary organic aerosol (SOA) samples is estimated to be significant (> 20 %) under the upper limit assumption of unity quantum yield at medium (1 × 1013 and 1.5 × 1015 photons cm−2 s−1 at 185 and 254 nm, respectively) or higher UV flux settings. The need for quantum yield measurements of both VOC and SOA photolysis is highlighted in this study. The results of this study allow improved OFR operation and experimental design and also inform the design of future reactors.
The vertical distribution of volcanic SO2 plumes measured by IASI

Sulfur dioxide (SO2) is an important atmospheric constituent that plays a crucial role in many atmospheric processes. Volcanic eruptions are a significant source of atmospheric SO2 and its effects and lifetime depend on the SO2 injection altitude. The Infrared Atmospheric Sounding Interferometer (IASI) on the METOP satellite can be used to study volcanic emission of SO2 using high-spectral resolution measurements from 1000 to 1200 and from 1300 to 1410 cm−1 (the 7.3 and 8.7 µm SO2 bands) returning both SO2 amount and altitude data. The scheme described in Carboni et al. (2012) has been applied to measure volcanic SO2 amount and altitude for 14 explosive eruptions from 2008 to 2012. The work includes a comparison with the following independent measurements: (i) the SO2 column amounts from the 2010 Eyjafjallajökull plumes have been compared with Brewer ground measurements over Europe; (ii) the SO2 plumes heights, for the 2010 Eyjafjallajökull and 2011 Grimsvötn eruptions, have been compared with CALIPSO backscatter profiles. The results of the comparisons show that IASI SO2 measurements are not affected by underlying cloud and are consistent (within the retrieved errors) with the other measurements. The series of analysed eruptions (2008 to 2012) show that the biggest emitter of volcanic SO2 was Nabro, followed by Kasatochi and Grímsvötn. Our observations also show a tendency for volcanic SO2 to reach the level of the tropopause during many of the moderately explosive eruptions observed. For the eruptions observed, this tendency was independent of the maximum amount of SO2 (e.g. 0.2 Tg for Dalafilla compared with 1.6 Tg for Nabro) and of the volcanic explosive index (between 3 and 5).
Developing and bounding ice particle mass- and area-dimension expressions for use in atmospheric models and remote sensing

Ice particle mass- and projected area-dimension (m-D and A-D) power laws are commonly used in the treatment of ice cloud microphysical and optical properties and the remote sensing of ice cloud properties. Although there has long been evidence that a single m-D or A-D power law is often not valid over all ice particle sizes, few studies have addressed this fact. This study develops self-consistent m-D and A-D expressions that are not power laws but can easily be reduced to power laws for the ice particle size (maximum dimension or D) range of interest, and they are valid over a much larger D range than power laws. This was done by combining ground measurements of individual ice particle m and D formed at temperature T  <  −20 °C during a cloud seeding field campaign with 2-D stereo (2D-S) and cloud particle imager (CPI) probe measurements of D and A, and estimates of m, in synoptic and anvil ice clouds at similar temperatures. The resulting m-D and A-D expressions are functions of temperature and cloud type (synoptic vs. anvil), and are in good agreement with m-D power laws developed from recent field studies considering the same temperature range (−60 °C  <  T  <  −20 °C).
Variability of water vapour in the Arctic stratosphere

This study evaluates the stratospheric water vapour distribution and variability in the Arctic. A FinROSE chemistry transport model simulation covering the years 1990–2014 is compared to observations (satellite and frost point hygrometer soundings), and the sources of stratospheric water vapour are studied. In the simulations, the Arctic water vapour shows decadal variability with a magnitude of 0.8 ppm. Both observations and the simulations show an increase in the water vapour concentration in the Arctic stratosphere after the year 2006, but around 2012 the concentration started to decrease. Model calculations suggest that this increase in water vapour is mostly explained by transport-related processes, while the photochemically produced water vapour plays a relatively smaller role. The increase in water vapour in the presence of the low winter temperatures in the Arctic stratosphere led to more frequent occurrence of ice polar stratospheric clouds (PSCs) in the Arctic vortex. We perform a case study of ice PSC formation focusing on January 2010 when the polar vortex was unusually cold and allowed large-scale formation of PSCs. At the same time a large-scale persistent dehydration was observed. Ice PSCs and dehydration observed at Sodankylä with accurate water vapour soundings in January and February 2010 during the LAPBIAT (Lapland Atmosphere–Biosphere facility) atmospheric measurement campaign were well reproduced by the model. In particular, both the observed and simulated decrease in water vapour in the dehydration layer was up to 1.5 ppm.
Sensitivity to grid resolution in the ability of a chemical transport model to simulate observed oxidant chemistry under high-isoprene conditions

Formation of ozone and organic aerosol in continental atmospheres depends on whether isoprene emitted by vegetation is oxidized by the high-NOx pathway (where peroxy radicals react with NO) or by low-NOx pathways (where peroxy radicals react by alternate channels, mostly with HO2). We used mixed layer observations from the SEAC4RS aircraft campaign over the Southeast US to test the ability of the GEOS-Chem chemical transport model at different grid resolutions (0.25°  ×  0.3125°, 2°  ×  2.5°, 4°  ×  5°) to simulate this chemistry under high-isoprene, variable-NOx conditions. Observations of isoprene and NOx over the Southeast US show a negative correlation, reflecting the spatial segregation of emissions; this negative correlation is captured in the model at 0.25°  ×  0.3125° resolution but not at coarser resolutions. As a result, less isoprene oxidation takes place by the high-NOx pathway in the model at 0.25°  ×  0.3125° resolution (54 %) than at coarser resolution (59 %). The cumulative probability distribution functions (CDFs) of NOx, isoprene, and ozone concentrations show little difference across model resolutions and good agreement with observations, while formaldehyde is overestimated at coarse resolution because excessive isoprene oxidation takes place by the high-NOx pathway with high formaldehyde yield. The good agreement of simulated and observed concentration variances implies that smaller-scale non-linearities (urban and power plant plumes) are not important on the regional scale. Correlations of simulated vs. observed concentrations do not improve with grid resolution because finer modes of variability are intrinsically more difficult to capture. Higher model resolution leads to decreased conversion of NOx to organic nitrates and increased conversion to nitric acid, with total reactive nitrogen oxides (NOy) changing little across model resolutions. Model concentrations in the lower free troposphere are also insensitive to grid resolution. The overall low sensitivity of modeled concentrations to grid resolution implies that coarse resolution is adequate when modeling continental boundary layer chemistry for global applications.
Observation of viscosity transition in α-pinene secondary organic aerosol

Under certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the Cosmics Leaving Outdoor Droplets (CLOUD) experiment at The European Organisation for Nuclear Research (CERN), we deployed a new in situ optical method to detect the viscous state of α-pinene SOA particles and measured their transition from the amorphous highly viscous state to states of lower viscosity. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical particles at relative humidities near the deliquescence point. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to a spherical shape was observed as the RH was increased to between 35 % at −10 °C and 80 % at −38 °C, confirming previous calculations of the viscosity-transition conditions. Consequently, α-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical, and ice-nucleation properties of SOA and SOA-coated particles in the atmosphere.
Global observations and modeling of atmosphere–surface exchange of elemental mercury: a critical review

Reliable quantification of air–surface fluxes of elemental Hg vapor (Hg0) is crucial for understanding mercury (Hg) global biogeochemical cycles. There have been extensive measurements and modeling efforts devoted to estimating the exchange fluxes between the atmosphere and various surfaces (e.g., soil, canopies, water, snow, etc.) in the past three decades. However, large uncertainties remain due to the complexity of Hg0 bidirectional exchange, limitations of flux quantification techniques and challenges in model parameterization. In this study, we provide a critical review on the state of science in the atmosphere–surface exchange of Hg0. Specifically, the advancement of flux quantification techniques, mechanisms in driving the air–surface Hg exchange and modeling efforts are presented. Due to the semi-volatile nature of Hg0 and redox transformation of Hg in environmental media, Hg deposition and evasion are influenced by multiple environmental variables including seasonality, vegetative coverage and its life cycle, temperature, light, moisture, atmospheric turbulence and the presence of reactants (e.g., O3, radicals, etc.). However, the effects of these processes on flux have not been fundamentally and quantitatively determined, which limits the accuracy of flux modeling. We compile an up-to-date global observational flux database and discuss the implication of flux data on the global Hg budget. Mean Hg0 fluxes obtained by micrometeorological measurements do not appear to be significantly greater than the fluxes measured by dynamic flux chamber methods over unpolluted surfaces (p = 0.16, one-tailed, Mann–Whitney U test). The spatiotemporal coverage of existing Hg0 flux measurements is highly heterogeneous with large data gaps existing in multiple continents (Africa, South Asia, Middle East, South America and Australia). The magnitude of the evasion flux is strongly enhanced by human activities, particularly at contaminated sites. Hg0 flux observations in East Asia are comparatively larger in magnitude than the rest of the world, suggesting substantial re-emission of previously deposited mercury from anthropogenic sources. The Hg0 exchange over pristine surfaces (e.g., background soil and water) and vegetation needs better constraints for global analyses of the atmospheric Hg budget. The existing knowledge gap and the associated research needs for future measurements and modeling efforts for the air–surface exchange of Hg0 are discussed.
Technical Note: Development of chemoinformatic tools to enumerate functional groups in molecules for organic aerosol characterization

Functional groups (FGs) can be used as a reduced representation of organic aerosol composition in both ambient and controlled chamber studies, as they retain a certain chemical specificity. Furthermore, FG composition has been informative for source apportionment, and various models based on a group contribution framework have been developed to calculate physicochemical properties of organic compounds. In this work, we provide a set of validated chemoinformatic patterns that correspond to (1) a complete set of functional groups that can entirely describe the molecules comprised in the α-pinene and 1,3,5-trimethylbenzene MCMv3.2 oxidation schemes, (2) FGs that are measurable by Fourier transform infrared spectroscopy (FTIR), (3) groups incorporated in the SIMPOL.1 vapor pressure estimation model, and (4) bonds necessary for the calculation of carbon oxidation state. We also provide example applications for this set of patterns. We compare available aerosol composition reported by chemical speciation measurements and FTIR for different emission sources, and calculate the FG contribution to the O : C ratio of simulated gas-phase composition generated from α-pinene photooxidation (using the MCMv3.2 oxidation scheme).
Characteristics of monsoon inversions over the Arabian Sea observed by satellite sounder and reanalysis data sets

Monsoon inversion (MI) over the Arabian Sea (AS) is one of the important characteristics associated with the monsoon activity over Indian region during summer monsoon season. In the present study, we have used 5 years (2009–2013) of temperature and water vapour measurement data obtained from satellite sounder instrument, an Infrared Atmospheric Sounding Interferometer (IASI) onboard MetOp satellite, in addition to ERA-Interim data, to study their characteristics. The lower atmospheric data over the AS have been examined first to identify the areas where MIs are predominant and occur with higher strength. Based on this information, a detailed study has been made to investigate their characteristics separately in the eastern AS (EAS) and western AS (WAS) to examine their contrasting features. The initiation and dissipation times of MIs, their percentage occurrence, strength, etc., has been examined using the huge database. The relation with monsoon activity (rainfall) over Indian region during normal and poor monsoon years is also studied. WAS ΔT values are ∼  2 K less than those over the EAS, ΔT being the temperature difference between 950 and 850 hPa. A much larger contrast between the WAS and EAS in ΔT is noticed in ERA-Interim data set vis-à-vis those observed by satellites. The possibility of detecting MI from another parameter, refractivity N, obtained directly from another satellite constellation of GPS Radio Occultation (RO) (COSMIC), has also been examined. MI detected from IASI and Atmospheric Infrared Sounder (AIRS) onboard the NOAA satellite have been compared to see how far the two data sets can be combined to study the MI characteristics. We suggest MI could also be included as one of the semipermanent features of southwest monsoon along with the presently accepted six parameters.