SO2 Column Research Articles

Anthropogenic sulphur dioxide load over China as observed from different satellite sensors

China, with its rapid economic growth and immense exporting power, has been the focus of many studies during this previous decade quantifying its increasing emissions contribution to the Earth's atmosphere. With a population slowly shifting towards enlarged power and purchasing needs, the ceaseless inauguration of new power plants, smelters, refineries and industrial parks leads infallibly to increases in sulphur dioxide, SO2, emissions. The recent capability of next generation algorithms as well as new space-borne instruments to detect anthropogenic SO2 loads has enabled a fast advancement in this field. In the following work, algorithms providing total SO2 columns over China based on SCIAMACHY/Envisat, OMI/Aura and GOME2/MetopA observations are presented. The need for post-processing and gridding of the SO2 fields is further revealed in this work, following the path of previous publications. Further, it is demonstrated that the usage of appropriate statistical tools permits studying parts of the datasets typically excluded, such as the winter months loads. Focusing on actual point sources, such as megacities and known power plant locations, instead of entire provinces, monthly mean time series have been examined in detail. The sharp decline in SO2 emissions in more than 90%–95% of the locations studied confirms the recent implementation of government desulphurisation legislation; however, locations with increases, even for the previous five years, are also identified. These belong to provinces with emerging economies which are in haste to install power plants and are possibly viewed leniently by the authorities, in favour of growth. The SO2 load seasonality has also been examined in detail with a novel mathematical tool, with 70% of the point sources having a statistically significant annual cycle with highs in winter and lows in summer, following the heating requirements of the Chinese population.

Atmospheric constituents and surface-level UVB: Implications for a paleoaltimetry proxy and attempts to reconstruct UV exposure during volcanic episodes

Chemical and morphological features of spores and pollens have been linked to changes in solar ultraviolet radiation (specifically UVB, 280–315 nm) at Earth's surface. Variation in UVB exposure as inferred from these features has been suggested as a proxy for paleoaltitude; such proxies are important in understanding the uplift history of high altitude plateaus, which in turn is important for testing models of the tectonic processes responsible for such uplift. While UVB irradiance does increase with altitude above sea level, a number of other factors affect the irradiance at any given place and time. In this modeling study we use the TUV atmospheric radiative transfer model to investigate dependence of surface-level UVB irradiance and relative biological impact on a number of constituents in Earth's atmosphere that are variable over long and short time periods. We consider changes in O3 column density, and SO2 and sulfate aerosols due to periods of volcanic activity, including that associated with the formation of the Siberian Traps. We find that UVB irradiance may be highly variable under volcanic conditions and variations in several of these atmospheric constituents can easily mimic or overwhelm changes in UVB irradiance due to changes in altitude. On the other hand, we find that relative change with altitude is not very sensitive to different sets of atmospheric conditions. Any paleoaltitude proxy based on UVB exposure requires confidence that the samples under comparison were located at roughly the same latitude, under very similar O3 and SO2 columns, with similar atmospheric aerosol conditions. In general, accurate estimates of the surface-level UVB exposure at any time and location require detailed radiative transfer modeling taking into account a number of atmospheric factors; this result is important for paleoaltitude proxies as well as attempts to reconstruct the UV environment through geologic time and to tie extinctions, such as the end-Permian mass extinction, to UVB irradiance changes.

Sulfur isotope fractionation by broadband UV radiation to optically thin SO2 under reducing atmosphere

Photochemical mechanisms of Sulfur Mass-Independent Fractionation (S-MIF) are still poorly understood. Previous laboratory experiments have indicated that the S-MIF depends largely on the spectrum of the incident light source and the partial pressure of SO2, though the basic character of the Archean S-MIF (ΔS36/ΔS33=∼−1) has never been reproduced. We have conducted new photochemical experiments at low pSO2 (1–10 Pa) conditions under the presence of CO and found a reasonable mechanism to reproduce the Δ36S/Δ33S slope about −1. As previously suggested (Ono et al., 2013), the low pSO2 is key to studying the self-shielding effect within a range of realistic atmospheric conditions. Also, reducing conditions are critical for simulating the O2-poor atmosphere, whereas photolysis of pure SO2 provides excess O atoms that significantly change the overall chemistry. Our experimental results confirmed that significant S-MIF (ΔS36/ΔS33=−2.4) can be produced by self-shielding in the SO2 photolysis band (185–220 nm), even if the SO2 column density is as low as 1016 molecules cm−2. Thus, photolysis within a volcanic plume of ∼0.1 ppm SO2 is capable of producing a large S-MIF signature. The isotopic fractionations originating from the different absorption cross sections of SO2 isotopologues (i.e. wavelength dependent effect; without self-shielding) are only minor (potentially up to +4‰ for Δ33S). Under reducing conditions, however, another S-MIF signal with Δ36S/Δ33S ratio of ∼+0.7 is produced due to collision-induced intersystem crossing (ISC) from singlet to triplet states of SO2 (Whitehill et al., 2013), and should also be transferred into the final product that is responsible for changing the Δ36S/Δ33S slope. Based on a photochemical model of the S–O–C system with the two S-MIF-yielding reactions, the largest S-MIF observed in the late Archean Mt. McRae Fm. (ΔS33=+9.4‰, ΔS36=−7.5‰) can be reproduced by solar UV irradiation of a SO2 column of ∼6.4×1016 molecules cm−2 with a sufficiently high concentration of reducing gasses (∼2% CO or CH4) where the ISC-derived MIF contributes ∼3% through the photoexcitation channel initiated in the 240–340 nm region. Our work shows that a photochemical model considering the two major S-MIF-yielding reactions (SO2+hν→SO+O and SO21+M→SO23+M) can explain the behavior of the S-MIF observed in laboratory experiments. The combination of the two effects is more important under reducing condition and should be considered to interpret the geological record.

A model study of the pollution effects of the first 3 months of the Holuhraun volcanic fissure: comparison with observations and air pollution effects

Abstract. The volcanic fissure at Holuhraun, Iceland started at the end of August 2014 and continued for 6 months to the end of February 2015, with an extensive lava flow onto the Holuhraun plain. This event was associated with large SO2 emissions, amounting up to approximately 4.5 times the daily anthropogenic SO2 emitted from the 28 European Union countries, Norway, Switzerland and Iceland. In this paper we present results from EMEP/MSC-W model simulations to which we added 750 kg s−1 SO2 emissions at the Holuhraun plain from September to November (SON), testing three different emission heights. The three simulated SO2 concentrations, weighted with the OMI (Ozone Monitoring Instrument) satellite averaging kernel, are found to be within 30 % of the satellite-observed SO2 column burden. Constraining the SO2 column burden with the satellite data while using the kernel along with the three simulated height distributions of SO2, we estimate that the median of the daily burdens may have been between 13 and 40 kt in the North Atlantic area under investigation. We suggest this to be the uncertainty in the satellite-derived burdens of SO2, mainly due to the unknown vertical distribution of SO2. Surface observations in Europe outside Iceland showed concentration increases up to > 500 µg m−3 SO2 from volcanic plumes passing. Three well identified episodes, where the plume crossed several countries, are compared in detail to surface measurements. For all events, the general timing of the observed concentration peaks compared quite well to the model results. The overall changes to the European SO2 budget due to the volcanic fissure are estimated. Three-monthly wet deposition (SON) of SOx in the 28 European Union countries, Norway and Switzerland is found to be more than 30 % higher in the model simulation with Holuhraun emissions compared to a model simulation with no Holuhraun emissions. The largest increases, apart from extreme values on Iceland, are found on the coast of northern Norway, a region with frequent precipitation during westerly winds. Over a 3-month average (during SON 2014) over Europe, SO2 and PM2.5 surface concentrations, due to the volcanic emissions, increased by only ten and 6 % respectively. Although the percent increase of PM2.5 concentration is highest over Scandinavia and Scotland, an increase in PM exceedance days is found over Ireland and the already polluted Benelux region (up to 3 additional days), where any small increase in particulate matter concentration leads to an increase in exceedance days.

Effects of China’s urban form on urban air quality

Poor urban air quality in China has received global attention. This article analyses the extent to which the urban form of all provincial and prefectural cities in China affects urban air quality. A geographically weighted regression model was used to quantify the relationship between the urban form indices, as well as the satellite-derived pollutant column density of NO2 and SO2. The results show that urban form has a significant effect on the urban air quality in China. The effect of urban form on air quality varies among the cities in this vast region. The compact ratio index is negatively correlated with both NO2 and SO2 column density for most of the cities. An ‘X’- or ‘H’-shaped city has less air pollution than a rhomboid-shaped city when the city is located in northern or central China. In comparison, the fractal dimension index is not a statistically significant predictor of air quality. Urban form can have effects on air quality that are equivalent to some meteorological and socioeconomic factors.

COMPORTAMENTO DA COLUNA TOTAL DE DIÓXIDO DE ENXOFRE NA CAMADA LIMITE DA REGIÃO DA CIDADE DE SANTIAGO NO CHILE UTILIZANDO O SENSOR OMI

Air pollution is a major environmental problem of today's world. The sulfur dioxide gas (SO2), a pollutant studied both in remote areas as in urban areas, and can be emitted into the atmosphere through natural sources and also by human activities, and its study of great relevance for monitoring problems caused to health of the population, agriculture and economic problems mainly to the population centers of large and medium size. The objective of this study was to determine the variability of the total column of sulfur dioxide into the region of the city of Santiago in Chile using data from the sensor OMI (Ozone Monitoring Instrument) which operates within the range of UV / VIS for the period 2005-2012. Using the daily maximum values of total SO2 column, it was determined the annual and seasonal variability of the total column of sulfur dioxide into the region of Santiago in Chile. The Moving Average for 30 days (MM30) was not a particular seasonality for the period 2005-2012. It was observed increasing values of trend line in the dispersion of the data of the Santiago region.

The vertical distribution of volcanic SO<sub>2</sub> plumes measured by IASI

Abstract. 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).

Response of SO2 and particulate air pollution to local and regional emission controls: A case study in Maryland

AbstractThis paper addresses the questions of what effect local regulations can have on pollutants with different lifetimes and how surface observations and remotely sensed data can be used to determine the impacts. We investigated the decadal trends of tropospheric sulfur dioxide (SO2) and aerosol pollution over Maryland and its surrounding states, using surface, aircraft, and satellite measurements. Aircraft measurements indicated fewer isolated SO2 plumes observed in summers, a ∼40% decrease of column SO2, and a ∼20% decrease of atmospheric optical depth (AOD) over Maryland after the implementation of local regulations on sulfur emissions from power plants (∼90% reduction from 2010). Surface observations of SO2 and particulate matter (PM) concentrations in Maryland show similar trends. OMI SO2 and MODIS AOD observations were used to investigate the column contents of air pollutants over the eastern U.S.; these indicate decreasing trends in column SO2 (∼60% decrease) and AOD (∼20% decrease). The decrease of upwind SO2 emissions also reduced aerosol loadings over the downwind Atlantic Ocean near the coast by ∼20%, while indiscernible changes of the SO2 column were observed. A step change of SO2 emissions in Maryland starting in 2009–2010 had an immediate and profound benefit in terms of local surface SO2 concentrations but a modest impact on aerosol pollution, indicating that short‐lived pollutants are effectively controlled locally, while long‐lived pollutants require regional measures.

Retrieval of near-surface sulfur dioxide (SO<sub>2</sub>) concentrations at a global scale using IASI satellite observations

Abstract. SO2 from volcanic eruptions is now operationally monitored from space in both the ultraviolet (UV) and thermal infrared (TIR) spectral range, but anthropogenic SO2 has almost solely been measured from UV sounders. Indeed, TIR instruments are well known to have a poor sensitivity to the planetary boundary layer (PBL), due to generally low thermal contrast (TC) between the ground and the air above it. Recent studies have demonstrated the capability of the Infrared Atmospheric Sounding Interferometer (IASI) to measure near-surface SO2 locally, for specific atmospheric conditions. In this work, we develop a retrieval method allowing the inference of SO2 near-surface concentrations from IASI measurements at a global scale. This method consists of two steps. Both are based on the computation of radiance indexes representing the strength of the SO2 ν3 band in IASI spectra. The first step allows the peak altitude of SO2 to be retrieved and near-surface SO2 to be selected. In the second step, 0–4 km columns of SO2 are inferred using a look-up table (LUT) approach. Using this new retrieval method, we obtain the first global distribution of near-surface SO2 from IASI-A, and identify the dominant anthropogenic hotspot sources and volcanic degassing. The 7-year daily time evolution of SO2 columns above two industrial source areas (Beijing in China and Sar Cheshmeh in Iran) is investigated and correlated to the seasonal variations of the parameters that drive the IASI sensitivity to the PBL composition. Apart from TC, we show that humidity is the most important parameter which determines IR sensitivity to near-surface SO2 in the ν3 band. As IASI provides global measurements twice daily, the differences between the retrieved columns for the morning and evening orbits are investigated. This paper finally presents a first intercomparison of the measured 0–4 km columns with an independent iterative retrieval method and with observations of the Ozone Monitoring Instrument (OMI).

Comparison and validation of band residual difference algorithm and principal component analysis algorithm for retrievals of atmospheric SO2 columns from satellite observations

Remote sensing technology provides an unprecedented tool for the continuous and real-time monitoring of atmospheric SO2 from volcanic eruption and anthropogenic emission. The Global Ozone Monitoring Experiment (GOME), SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY), and Ozone Monitoring Instrument (OMI) have high SO2 monitoring capability. The OMI, which was launched on the EOS/Aura platform in July 2004, has the same hyperspectral measurements as the GOME and SCIAMACHY, but offers the improved spatial resolution at nadir (1324 km2) and daily global coverage for short-lifetime SO2. For OMI operational SO2 planetary boundary layer (PBL) retrieval, the previous band residual difference (BRD) algorithm has been replaced by principal component analysis (PCA) algorithm, which effectively reduces the systematic biases in SO2 column retrievals. However, there are few studies on the evaluations and validations of PCA SO2 retrievals over China, and the long-term comparisons with BRD SO2 retrievals also need to be conducted. In this study, the accuracies of PCA and BRD SO2 retrievals are validated by using ground-based multi axis differential optical absorption spectroscopy (MAX-DOAS) located in Beijing, and regional atmospheric modeling system, community multi-scale air quality (RAMS-CMAQ) modeling system model which can simulate the vertical distribution of atmospheric SO2. Moreover, BRD and PCA SO2 retrievals from oceanic area, eastern China and Reunion volcanic eruption are compared to find the long-term trend and spatiotemporal differences between SO2 columns. Finally, the uncertainty of SO2 retrieval, caused by measurement errors, band selection and input parameter errors in radiative transfer model, are analysed to understand the limitations of BRD and PCA algorithms. Results show that both PCA and BRD SO2 retrievals over Beijing are lower than ground-based MAX-DOAS measurements of SO2. PCA and BRD SO2 retrievals over eastern China are lower than the simulated SO2 columns from RAMS-CMAQ in winter 2008, but in July and August BRD SO2 columns are higher than RAMS-CMAQ simulations. The values of SO2 columns from BRD over China are more consistent with those from ground-based MAX-DOAS and RAMS-CMAQ model than from PCA. Although PCA algorithm effectively reduces the noise in SO2 column retrieval, SO2 columns from PCA over China are lower than those from BRD. For oceanic area where SO2 amount is nearly zero, the standard deviation of PCA results is lower than that of BRD, but the absolute value of averaged PCA SO2 column is larger than that of BRD. In the case of Reunion volcanic eruption with SO2 columns larger than 25 DU, the BRD SO2 columns are lower than PCA retrievals. Meanwhile, with the increase of SO2 column, the difference between BRD and PCA SO2 retrievals increases. Detailed uncertainty analysis shows the influences of measurement errors, band selection and inputs of radiative transfer model on the retrieval results. This study is important for developing the retrieval algorithm, and can also improve the application of OMI SO2 products.

Satellite measurements oversee China’s sulfur dioxide emission reductions from coal-fired power plants

To evaluate the real reductions in sulfur dioxide (SO2) emissions from coal-fired power plants in China, Ozone Monitoring Instrument (OMI) remote sensing SO2 columns were used to inversely model the SO2 emission burdens surrounding 26 isolated power plants before and after the effective operation of their flue gas desulfurization (FGD) facilities. An improved two-dimensional Gaussian fitting method was developed to estimate SO2 burdens under complex background conditions, by using the accurate local background columns and the customized fitting domains for each target source. The OMI-derived SO2 burdens before effective FGD operation were correlated well with the bottom-up emission estimates (R = 0.92), showing the reliability of the OMI-derived SO2 burdens as a linear indicator of the associated source strength. OMI observations indicated that the average lag time period between installation and effective operation of FGD facilities at these 26 power plants was around 2 years, and no FGD facilities have actually operated before the year 2008. The OMI estimated average SO2 removal equivalence (56.0%) was substantially lower than the official report (74.6%) for these 26 power plants. Therefore, it has been concluded that the real reductions of SO2 emissions in China associated with the FGD facilities at coal-fired power plants were considerably diminished in the context of the current weak supervision measures.

Application of an Online-Coupled Regional Climate Model, WRF-CAM5, over East Asia for Examination of Ice Nucleation Schemes: Part I. Comprehensive Model Evaluation and Trend Analysis for 2006 and 2011

Online-coupled climate and chemistry models are necessary to realistically represent the interactions between climate variables and chemical species and accurately simulate aerosol direct and indirect effects on cloud, precipitation, and radiation. In this Part I of a two-part paper, simulations from the Weather Research and Forecasting model coupled with the physics package of Community Atmosphere Model (WRF-CAM5) are conducted with the default heterogeneous ice nucleation parameterization over East Asia for two full years: 2006 and 2011. A comprehensive model evaluation is performed using satellite and surface observations. The model shows an overall acceptable performance for major meteorological variables at the surface and in the boundary layer, as well as column variables (e.g., precipitation, cloud fraction, precipitating water vapor, downward longwave and shortwave radiation). Moderate to large biases exist for cloud condensation nuclei over oceanic areas, cloud variables (e.g., cloud droplet number concentration, cloud liquid and ice water paths, cloud optical depth, longwave and shortwave cloud forcing). These biases indicate a need to improve the model treatments for cloud processes, especially cloud droplets and ice nucleation, as well as to reduce uncertainty in the satellite retrievals. The model simulates well the column abundances of chemical species except for column SO2 but relatively poor for surface concentrations of several species such as CO, NO2, SO2, PM2.5, and PM10. Several reasons could contribute to the underestimation of major chemical species in East Asia including underestimations of anthropogenic emissions and natural dust emissions, uncertainties in the spatial and vertical distributions of the anthropogenic emissions, as well as biases in meteorological, radiative, and cloud predictions. Despite moderate to large biases in the chemical predictions, the model performance is generally consistent with or even better than that reported for East Asia with only a few exceptions. The model generally reproduces the observed seasonal variations and the difference between 2006 and 2011 for most variables or chemical species. Overall, these results demonstrate promising skills of WRF-CAM5 for long-term simulations at a regional scale and suggest several areas of potential improvements.

Correlation between the spatio-temporal distributions of aerosols, sulphur dioxide, and formaldehyde using MODIS and SCIAMACHY satellite data for China

The spatial and temporal relationship between fine-mode aerosol optical depth (AOD) observed by the Moderate Resolution Imaging Spectroradiometer (MODIS) and tropospheric columns of SO2 and formaldehyde (HCHO) from the Scanning Imaging Absorption Chartography (SCIAMACHY) are used to infer information on the variability of sulphate aerosol, which is a major determinant of fine-mode AOD (AODf) in east China. When averaging the satellite data over specific regions of China and for longer time periods (from 2005 to 2011), we find obvious similar trends between AODf and SO2, HCHO columns for southern and eastern China. The results of satellite observations show the high spatial and temporal correlation between AODf and SO2 over the Yangtze River Delta (R2), the Pearl River Delta (R3), and the Chongqing–Chengdu region (R4), with the coefficients of determination (R2) of 0.376, 0.438, and 0.837, respectively. These regions are performing with the huge amount of anthropogenic SO2 emissions by traffic, industry, and domestic heating. The trend is consistent with fine-mode aerosol and SO2 appearing in summer because AODf is often correlated with enhanced HCHO concentrations, reflecting the importance of secondary aerosol formation over industrialized regions in that season. Over the North China Plain, distinct maximum values of AODf and HCHO were observed and the minimum value for SO2 was observed in summer. The decrease in the mean SO2 column was 35.5%, which has been attributed to the strict security measures by the government during the 2008 Olympic Games period while there was a decrease of 46% in AODf at the same time. As sulphate aerosol occurs seasonally in the North China Plain, the strong correlation between anomalies of AODf and SO2 can be used to estimate and analyse the distribution of sulphate aerosol. Singular value decomposition (SVD) analysis showed the same variation between AODf and SO2 over eastern China and Sichuan Province, and a distinct negative value of SVD variables over comparably industrialized regions in southern and eastern China and Sichuan Province. The results for SO4 from the Model for Ozone and Related chemical Tracers model for southern and eastern China and the Sichuan regions suggest much stronger sulphate contributions to aerosol formation than for other areas of China. We propose that the SVD variables between AODf and SO2, which can be inferred from the satellite data, can be used as indicators for regional pollution control.

Temporal variations of flux and altitude of sulfur dioxide emissions during volcanic eruptions: implications for long-range dispersal of volcanic clouds

Abstract. Sulfur-rich degassing, which is mostly composed of sulfur dioxide (SO2), plays a major role in the overall impact of volcanism on the atmosphere and climate. The accurate assessment of this impact is currently hampered by the poor knowledge of volcanic SO2 emissions. Here, using an inversion procedure, we show how assimilating snapshots of the volcanic SO2 load derived from the Infrared Atmospheric Sounding Interferometer (IASI) allows for reconstructing both the flux and altitude of the SO2 emissions with an hourly resolution. For this purpose, the regional chemistry-transport model CHIMERE is used to describe the dispersion of SO2 when released in the atmosphere. As proof of concept, we study the 10 April 2011 eruption of the Etna volcano (Italy), which represents one of the few volcanoes instrumented on the ground for the continuous monitoring of SO2 degassing. We find that the SO2 flux time-series retrieved from satellite imagery using the inverse scheme is in agreement with ground observations during ash-poor phases of the eruption. However, large discrepancies are observed during the ash-rich paroxysmal phase as a result of enhanced plume opacity affecting ground-based ultraviolet (UV) spectroscopic retrievals. As a consequence, the SO2 emission rate derived from the ground is underestimated by almost one order of magnitude. Altitudes of the SO2 emissions predicted by the inverse scheme are validated against an RGB image of the Moderate Resolution Imaging Spectroradiometer (MODIS) capturing the near-source atmospheric pathways followed by Etna plumes, in combination with forward trajectories from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model. At a large distance from the source, modelled SO2 altitudes are compared with independent information on the volcanic cloud height. We find that the altitude predicted by the inverse scheme is in agreement with snapshots of the SO2 height retrieved from recent algorithms exploiting the high spectral resolution of IASI. The validity of the modelled SO2 altitude is further confirmed by the detection of a layer of particles at the same altitude by the spaceborne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). Analysis of CALIOP colour and depolarization ratios suggests that these particles consist of sulfate aerosols formed from precursory volcanic SO2. The reconstruction of emission altitude, through inversion procedures which assimilate volcanic SO2 column amounts, requires specific meteorological conditions, especially sufficient wind shear so that gas parcels emitted at different altitudes follow distinct trajectories. We consequently explore the possibility and limits of assimilating in inverse schemes infrared (IR) imagery of the volcanic SO2 cloud altitude which will render the inversion procedure independent of the wind shear prerequisite.

Application of WRF/Chem over East Asia: Part I. Model evaluation and intercomparison with MM5/CMAQ

Abstract In this work, the application of the online-coupled Weather Research and Forecasting model with chemistry (WRF/Chem) version 3.3.1 is evaluated over East Asia for January, April, July, and October 2005 and compared with results from a previous application of an offline model system, i.e., the Mesoscale Model and Community Multiple Air Quality modeling system (MM5/CMAQ). The evaluation of WRF/Chem is performed using multiple observational datasets from satellites and surface networks in mainland China, Hong Kong, Taiwan, and Japan. WRF/Chem simulates well specific humidity (Q2) and downward longwave and shortwave radiation (GLW and GSW) with normalized mean biases (NMBs) within 24%, but shows moderate to large biases for temperature at 2-m (T2) (NMBs of −9.8% to 75.6%) and precipitation (NMBs of 11.4–92.7%) for some months, and wind speed at 10-m (WS10) (NMBs of 66.5–101%), for all months, indicating some limitations in the YSU planetary boundary layer scheme, the Purdue Lin cloud microphysics, and the Grell–Devenyi ensemble scheme. WRF/Chem can simulate the column abundances of gases reasonably well with NMBs within 30% for most months but moderately to significantly underpredicts the surface concentrations of major species at all sites in nearly all months with NMBs of −72% to −53.8% for CO, −99.4% to −61.7% for NOx, −84.2% to −44.5% for SO2, −63.9% to −25.2% for PM2.5, and −68.9% to 33.3% for PM10, and aerosol optical depth in all months except for October with NMBs of −38.7% to −16.2%. The model significantly overpredicts surface concentrations of O3 at most sites in nearly all months with NMBs of up to 160.3% and NO 3 - at the Tsinghua site in all months. Possible reasons for large underpredictions include underestimations in the anthropogenic emissions of CO, SO2, and primary aerosol, inappropriate vertical distributions of emissions of SO2 and NO2, uncertainties in upper boundary conditions (e.g., for O3 and CO), missing or inaccurate model representations (e.g., secondary organic aerosol formation, gas/particle partitioning, dust emissions, dry and wet deposition), and inaccurate meteorological fields (e.g., overpredictions in WS10 and precipitation, but underpredictions in T2), as well as the large uncertainties in satellite retrievals (e.g., for column SO2). Comparing to MM5, WRF generally gives worse performance in meteorological predictions, in particular, T2, WS10, GSW, GLW, and cloud fraction in all months, as well as Q2 and precipitation in January and October, due to limitations in the above physics schemes or parameterizations. Comparing to CMAQ, WRF/Chem performs better for surface CO, O3, and PM10 concentrations at most sites in most months, column CO and SO2 abundances, and AOD. It, however, gives poorer performance for surface NOx concentrations at most sites in most months, surface SO2 concentrations at all sites in all months, and column NO2 abundances in January and April. WRF/Chem also gives lower concentrations of most secondary PM and black carbon. Those differences in results are attributed to differences in simulated meteorology, gas-phase chemistry, aerosol thermodynamic and dynamic treatments, dust and sea salt emissions, and wet and dry deposition treatments in both models.

Cyclic degassing of Erebus volcano, Antarctica

Field observations have previously identified rapid cyclic changes in the behaviour of the lava lake of Erebus volcano. In order to understand more fully the nature and origins of these cycles, we present here a wavelet-based frequency analysis of time series measurements of gas emissions from the lava lake, obtained by open-path Fourier transform infrared spectroscopy. This reveals (i) a cyclic change in total gas column amount, a likely proxy for gas flux, with a period of about 10 min, and (ii) a similarly phased cyclic change in proportions of volcanic gases, which can be explained in terms of chemical equilibria and pressure-dependent solubilities. Notably, the wavelet analysis shows a persistent periodicity in the CO2/CO ratio and strong periodicity in H2O and SO2 degassing. The ‘peaks’ of the cycles, defined by maxima in H2O and SO2 column amounts, coincide with high CO2/CO ratios and proportionally smaller increases in column amounts of CO2, CO, and OCS. We interpret the cycles to arise from recharge of the lake by intermittent pulses of magma from shallow depths, which degas H2O at low pressure, combined with a background gas flux that is decoupled from this very shallow magma degassing.

Characterization of satellite-based proxies for estimating nucleation mode particles over South Africa

Abstract. Proxies for estimating nucleation mode number concentrations and further simplification for their use with satellite data have been presented in Kulmala et al. (2011). In this paper we discuss the underlying assumptions for these simplifications and evaluate the resulting proxies over an area in South Africa based on a comparison with a suite of ground-based measurements available from four different stations. The proxies are formulated in terms of sources (concentrations of precursor gases (NO2 and SO2) and UVB radiation intensity near the surface) and a sink term related to removal of the precursor gases due to condensation on pre-existing aerosols. A-Train satellite data are used as input to compute proxies. Both the input data and the resulting proxies are compared with those obtained from ground-based measurements. In particular, a detailed study is presented on the substitution of the local condensation sink (CS) with satellite aerosol optical depth (AOD), which is a column-integrated parameter. One of the main factors affecting the disagreement between CS and AOD is the presence of elevated aerosol layers. Overall, the correlation between proxies calculated from the in situ data and observed nucleation mode particle number concentrations (Nnuc) remained low. At the time of the satellite overpass (13:00–14:00 LT) the highest correlation is observed for SO2/CS (R2 = 0.2). However, when the proxies are calculated using satellite data, only NO2/AOD showed some correlation with Nnuc (R2 = 0.2). This can be explained by the relatively high uncertainties related especially to the satellite SO2 columns and by the positive correlation that is observed between the ground-based SO2 and NO2 concentrations. In fact, results show that the satellite NO2 columns compare better with in situ SO2 concentration than the satellite SO2 column. Despite the high uncertainties related to the proxies calculated using satellite data, the proxies calculated from the in situ data did not better predict Nnuc. Hence, overall improvements in the formulation of the proxies are needed.

Sulfur dioxide vertical column DOAS retrievals from the Ozone Monitoring Instrument: Global observations and comparison to ground‐based and satellite data

AbstractWe present a new data set of sulfur dioxide (SO2) vertical columns from observations of the Ozone Monitoring Instrument (OMI)/AURA instrument between 2004 and 2013. The retrieval algorithm used is an advanced Differential Optical Absorption Spectroscopy (DOAS) scheme combined with radiative transfer calculation. It is developed in preparation for the operational processing of SO2 data product for the upcoming TROPOspheric Monitoring Instrument/Sentinel 5 Precursor mission. We evaluate the SO2 column results with those inferred from other satellite retrievals such as Infrared Atmospheric Sounding Interferometer and OMI (Linear Fit and Principal Component Analysis algorithms). A general good agreement between the different data sets is found for both volcanic and anthropogenic SO2 emission scenarios. We show that our algorithm produces SO2 columns with low noise and is able to provide accurate estimates of SO2. This conclusion is supported by important validation results over the heavily polluted site of Xianghe (China). Nearly 4 years of OMI and ground‐based multiaxis DOAS SO2 columns are compared, and an excellent match is found. We also highlight the improved performance of the algorithm in capturing weak SO2 sources by detecting shipping SO2 emissions in long‐term averaged data, an unreported measurement from space.

Quantification of the depletion of ozone in the plume of Mount Etna

Abstract. Volcanoes are an important source of inorganic halogen species into the atmosphere. Chemical processing of these species generates oxidised, highly reactive, halogen species which catalyse considerable O3 destruction within volcanic plumes. A campaign of ground-based in situ O3, SO2 and meteorology measurements was undertaken at the summit of Mount Etna volcano in July/August 2012. At the same time, spectroscopic measurements were made of BrO and SO2 columns in the plume downwind. Depletions of ozone were seen at all in-plume measurement locations, with average O3 depletions ranging from 11–35 nmol mol−1 (15–45%). Atmospheric processing times of the plume were estimated to be between 1 and 4 min. A 1-D numerical model of early plume evolution was also used. It was found that in the early plume O3 was destroyed at an approximately constant rate relative to an inert plume tracer. This is ascribed to reactive halogen chemistry, and the data suggests the majority of the reactive halogen that destroys O3 in the early plume is generated within the crater, including a substantial proportion generated in a high-temperature "effective source region" immediately after emission. The model could approximately reproduce the main measured features of the ozone chemistry. Model results show a strong dependence of the near-vent bromine chemistry on the presence or absence of volcanic NOx emissions and suggest that near-vent ozone measurements can be used as a qualitative indicator of NOx emission.

Detection and characterization of Io’s atmosphere from high-resolution 4-μm spectroscopy

We report on high-resolution and spatially-resolved spectra of Io in the 4.0μm region, recorded with the VLT/CRIRES instrument in 2008 and 2010, which provide the first detection of the ν1+ν3 band of SO2 in Io’s atmosphere. Data are analyzed to constrain the latitudinal, longitudinal, and diurnal distribution of Io’s SO2 atmosphere as well as its characteristic temperature. Equatorial SO2 column densities clearly show longitudinal asymmetry, but with a maximum of ∼1.5×1017cm−2 at central meridian longitude L=200–220 and a minimum of ∼3×1016cm−2 at L=285–300, the longitudinal pattern somewhat differs from earlier inferences from Ly α and thermal IR measurements. Within the accuracy of the measurements, no evolution of the atmospheric density from mid-2008 to mid-2010 can be distinguished. The decrease of the SO2 column density towards high latitudes is apparent, and the typical latitudinal extent of the atmosphere found to be ±40° at half-maximum. The data show moderate diurnal variations of the equatorial atmosphere, which is evidence for a partially sublimation-supported atmospheric component. Compared to local noon, factor of 2 lower densities are observed ∼40° before and ∼80° after noon. Best-fit gas temperatures range from 150 to 220K, with a weighted mean value of 170±20K, which should represent the column-weighted mean kinetic temperature of Io’s atmosphere. Finally, although the data include clear thermal emission due to Pillan (in outburst in July 2008) and Loki, no detectable enhancements in the SO2 atmosphere above these volcanic regions are found, with an upper limit of 4×1016cm−2 at Pillan and 1×1017cm−2 at Loki.