In situ measurements of tropospheric volcanic plumes in Ecuador and Colombia during TC

A NASA DC‐8 research aircraft penetrated tropospheric gas and aerosol plumes sourced from active volcanoes in Ecuador and Colombia during the Tropical Composition, Cloud and Climate Coupling (TC4 ) mission in July–August 2007. The likely source volcanoes were Tungurahua (Ecuador) and Nevado del Huila (Colombia). The TC4 data provide rare insight into the chemistry of volcanic plumes in the tropical troposphere and permit a comparison of SO2 column amounts measured by the Ozone Monitoring Instrument (OMI) on the Aura satellite with in situ SO2 measurements. Elevated concentrations of SO2, sulfate aerosol, and particles were measured by DC‐8 instrumentation in volcanic outflow at altitudes of 3–6 km. Estimated plume ages range from ∼2 h at Huila to ∼22–48 h downwind of Ecuador. The plumes contained sulfate‐rich accumulation mode particles that were variably neutralized and often highly acidic. A significant fraction of supermicron volcanic ash was evident in one plume. In‐plume O3 concentrations were ∼70%–80% of ambient levels downwind of Ecuador, but data are insufficient to ascribe this to O3 depletion via reactive halogen chemistry. The TC4 data record rapid cloud processing of the Huila volcanic plume involving aqueous‐phase oxidation of SO2 by H2O2, but overall the data suggest average in‐plume SO2 to sulfate conversion rates of ∼1%–2% h−1 . SO2 column amounts measured in the Tungurahua plume (∼0.1–0.2 Dobson units) are commensurate with average SO2 columns retrieved from OMI measurements in the volcanic outflow region in July 2007. The TC4 data set provides further evidence of the impact of volcanic emissions on tropospheric acidity and oxidizing capacit

In situ measurements of tropospheric volcanic plumes in Ecuador and Colombia during TC^4

A NASA DC-8 research aircraft penetrated tropospheric gas and aerosol plumes sourced from active volcanoes in Ecuador and Colombia during the Tropical Composition, Cloud and Climate Coupling (TC^4) mission in July–August 2007. The likely source volcanoes were Tungurahua (Ecuador) and Nevado del Huila (Colombia). The TC^4 data provide rare insight into the chemistry of volcanic plumes in the tropical troposphere and permit a comparison of SO_2 column amounts measured by the Ozone Monitoring Instrument (OMI) on the Aura satellite with in situ SO_2 measurements. Elevated concentrations of SO_2, sulfate aerosol, and particles were measured by DC-8 instrumentation in volcanic outflow at altitudes of 3–6 km. Estimated plume ages range from ~2 h at Huila to ~22–48 h downwind of Ecuador. The plumes contained sulfate-rich accumulation mode particles that were variably neutralized and often highly acidic. A significant fraction of supermicron volcanic ash was evident in one plume. In-plume O_3 concentrations were ~70%–80% of ambient levels downwind of Ecuador, but data are insufficient to ascribe this to O_3 depletion via reactive halogen chemistry. The TC^4 data record rapid cloud processing of the Huila volcanic plume involving aqueous-phase oxidation of SO_2 by H_2O_2, but overall the data suggest average in-plume SO_2 to sulfate conversion rates of ~1%–2% h^(−1). SO_2 column amounts measured in the Tungurahua plume (~0.1–0.2 Dobson units) are commensurate with average SO_2 columns retrieved from OMI measurements in the volcanic outflow region in July 2007. The TC^4 data set provides further evidence of the impact of volcanic emissions on tropospheric acidity and oxidizing capacity

Perspectives and Integration in SOLAS Science

Why a chapter on Perspectives and Integration in SOLAS Science in this book? SOLAS science by its nature deals with interactions that occur: across a wide spectrum of time and space scales, involve gases and particles, between the ocean and the atmosphere, across many disciplines including chemistry, biology, optics, physics, mathematics, computing, socio-economics and consequently interactions between many different scientists and across scientific generations. This chapter provides a guide through the remarkable diversity of cross-cutting approaches and tools in the gigantic puzzle of the SOLAS realm. Here we overview the existing prime components of atmospheric and oceanic observing systems, with the acquisition of ocean–atmosphere observables either from in situ or from satellites, the rich hierarchy of models to test our knowledge of Earth System functioning, and the tremendous efforts accomplished over the last decade within the COST Action 735 and SOLAS Integration project frameworks to understand, as best we can, the current physical and biogeochemical state of the atmosphere and ocean commons. A few SOLAS integrative studies illustrate the full meaning of interactions, paving the way for even tighter connections between thematic fields. Ultimately, SOLAS research will also develop with an enhanced consideration of societal demand while preserving fundamental research coherency. The exchange of energy, gases and particles across the air-sea interface is controlled by a variety of biological, chemical and physical processes that operate across broad spatial and temporal scales. These processes influence the composition, biogeochemical and chemical properties of both the oceanic and atmospheric boundary layers and ultimately shape the Earth system response to climate and environmental change, as detailed in the previous four chapters. In this cross-cutting chapter we present some of the SOLAS achievements over the last decade in terms of integration, upscaling observational information from process-oriented studies and expeditionary research with key tools such as remote sensing and modelling. Here we do not pretend to encompass the entire legacy of SOLAS efforts but rather offer a selective view of some of the major integrative SOLAS studies that combined available pieces of the immense jigsaw puzzle. These include, for instance, COST efforts to build up global climatologies of SOLAS relevant parameters such as dimethyl sulphide, interconnection between volcanic ash and ecosystem response in the eastern subarctic North Pacific, optimal strategy to derive basin-scale CO2 uptake with good precision, or significant reduction of the uncertainties in sea-salt aerosol source functions. Predicting the future trajectory of Earth’s climate and habitability is the main task ahead. Some possible routes for the SOLAS scientific community to reach this overarching goal conclude the chapter

Direct solar FTIR measurements of CO2_2 and HCl in the plume of Popocatépetl Volcano, Mexico

Volcanic CO$_2$ emissions inventories have great importance in the understanding of the geological carbon cycle. Volcanoes provide the primary pathway for solid-earth volatiles to reach the Earth’s atmosphere and have the potential to significantly contribute to the carbon-climate feedback. Volcanic carbon emissions (both passive and eruptive degassing) included in inventories, largely stem from patchy surface measurements that suffer from difficulties in removing the atmospheric background. With a 27-year-long ongoing open-vent eruption, Popocatépetl ranks as one of the highest permanent volcanic CO$_2$ emitters worldwide and provides an excellent natural laboratory to design and experiment with new remote sensing methods for volcanic gas emission measurements. Since October 2012, infrared spectra at different spectral regions have been recorded with a solar occultation FTIR spectrometer. The near-infrared spectra allow for high precision measurements of CO$_2$ and HCl columns. Under favorable conditions, the continuous observations during sunrise allow the reconstruction of a plume cross-section of HCl and the estimation of the emission flux using wind data. Despite that the detection of CO$_2$ is more challenging, on April 26th, 2015 we captured a volcanic plume under favourable wind conditions which allowed us to reconstruct from this particular event a CO$_2$ emission rate of 116.10 ± 17.2 kg/s. The volcanic HCl emission on this event was the highest detected during the 2012-2016 period. An annual average CO$_2$ emission estimate of (41.2 ± 16.7) kg/s ((1.30 ± 0.53) Tg/yr) could be determined from a statistical treatment of the detected CO$_2$ and HCl columns in the IR spectra, and their corresponding molecular ratios, during this period. A total of 25 events were used to derive a mean CO$_2$/HCl molecule ratio of 11.4 ± 4.4 and an average HCl emission rate of (3.0 ± 0.3) kg/s could be determined. The CO$_2$ emissions of Popocatépetl were found to be around 0.32% of the total anthropogenic CO$_2$ emissions reported in the country and 3.6% of those corresponding to the Mexico City Metropolitan Area (MCMA). CO$_2$ emissions from the Popocatépetl volcano can be considered to play a negligible role in the global CO$_2$ budget, but should be taken into account

The detection of climate change due to the enhanced greenhouse effect

The greenhouse effect is accepted as an undisputed fact from both theoretical and observational considerations. In Earth's atmosphere, the primary greenhouse gas is water vapor. The specific concern today is that increasing concentrations of anthropogenically introduced greenhouse gases will, sooner or later, irreversibly alter the climate of Earth. Detecting climate change has been complicated by uncertainties in historical observations and measurements. Thus, the primary concern for the GEDEX project is how can climate change and enhanced greenhouse effects be unambiguously detected and quantified. Specifically examined are the areas of: Earth surface temperature; the free atmosphere (850 millibars and above); space-based measurements; measurement uncertainties; and modeling the observed temperature record

Sulfur Degassing From Volcanoes: Source Conditions, Surveillance, Plume Chemistry and Earth System Impacts

International audienceDespite its relatively minor abundance in magmas (compared with H2O and CO2), sulfur degassing from volcanoes is of tremendous significance. It can exert substantial influence on magmatic evolution (potentially capable of triggering eruptions); represents one of the most convenient opportunities for volcano monitoring and hazard assessment; and can result in major impacts on the atmosphere, climate and terrestrial ecosystems at a range of spatial and temporal scales. The complex behavior of sulfur in magmas owes much to its multiple valence states (-II, 0, IV, VI), speciation (e.g., S2, H2S, SO2, OCS and SO3 in the gas phase; S2-, SO42- and SO32- in the melt; and non-volatile solid phases such as pyrrhotite and anhydrite), and variation in stable isotopic composition (32S, 33S, 34S and 36S; e.g., Métrich and Mandeville 2010). Sulfur chemistry in the atmosphere is similarly rich involving gaseous and condensed phases and invoking complex homogeneous and heterogeneous chemical reactions. Sulfur degassing from volcanoes and geothermal areas is also important since a variety of microorganisms thrive based on the redox chemistry of sulfur: by reducing sulfur, thiosulfate, sulfite and sulfate to H2S, or oxidizing sulfur and H2S to sulfate (e.g., Takano et al. 1997; Amend and Shock 2001; Shock et al. 2010). Understanding volcanic sulfur degassing thus provides vital insights into magmatic, volcanic and hydrothermal processes; the impacts of volcanism on the Earth system; and biogeochemical cycles. Here, we review the causes of variability in sulfur abundance and speciation in different geodynamic contexts; the measurement of sulfur emissions from volcanoes; links between subsurface processes and surface observations; sulfur chemistry in volcanic plumes; and the consequences of sulfur degassing for climate and the environment

The evolution of the global aerosol system in a transient climate simulation from 1860 to 2100

The evolution of the global aerosol system from 1860 to 2100 is investigated through a transient atmosphere-ocean General Circulation Model climate simulation with interactively coupled atmospheric aerosol and oceanic biogeochemistry modules. The microphysical aerosol module HAM incorporates the major global aerosol cycles with prognostic treatment of their composition, size distribution, and mixing state. Based on an SRES A1B emission scenario, the global mean sulfate burden is projected to peak in 2020 while black carbon and particulate organic matter show a lagged peak around 2070. From present day to future conditions the anthropogenic aerosol burden shifts generally from the northern high-latitudes to the developing low-latitude source regions with impacts on regional climate. Atmospheric residence- and aging-times show significant alterations under varying climatic and pollution conditions. Concurrently, the aerosol mixing state changes with an increasing aerosol mass fraction residing in the internally mixed accumulation mode. The associated increase in black carbon causes a more than threefold increase of its co-single scattering albedo from 1860 to 2100. Mid-visible aerosol optical depth increases from pre-industrial times, predominantly from the aerosol fine fraction, peaks at 0.26 around the sulfate peak in 2020 and maintains a high level thereafter, due to the continuing increase in carbonaceous aerosols. The global mean anthropogenic top of the atmosphere clear-sky short-wave direct aerosol radiative perturbation intensifies to −1.1 W m^−2 around 2020 and weakens after 2050 to −0.6 W m^−2, owing to an increase in atmospheric absorption. The demonstrated modifications in the aerosol residence- and aging-times, the microphysical state, and radiative properties challenge simplistic approaches to estimate the aerosol radiative effects from emission projections

A multi-sensor approach for volcanic ash cloud retrieval and eruption characterization: the 23 November 2013 Etna lava fountain

Volcanic activity is observed worldwide with a variety of ground and space-based remote sensing instruments, each with advantages and drawbacks. No single system can give a comprehensive description of eruptive activity, and so, a multi-sensor approach is required. This work integrates infrared and microwave volcanic ash retrievals obtained from the geostationary Meteosat Second Generation (MSG)-Spinning Enhanced Visible and Infrared Imager (SEVIRI), the polar-orbiting Aqua-MODIS and ground-based weather radar. The expected outcomes are improvements in satellite volcanic ash cloud retrieval (altitude, mass, aerosol optical depth and effective radius), the generation of new satellite products (ash concentration and particle number density in the thermal infrared) and better characterization of volcanic eruptions (plume altitude, total ash mass erupted and particle number density from thermal infrared to microwave). This approach is the core of the multi-platform volcanic ash cloud estimation procedure being developed within the European FP7-APhoRISM project. The Mt. Etna (Sicily, Italy) volcano lava fountaining event of 23 November 2013 was considered as a test case. The results of the integration show the presence of two volcanic cloud layers at different altitudes. The improvement of the volcanic ash cloud altitude leads to a mean difference between the SEVIRI ash mass estimations, before and after the integration, of about the 30%. Moreover, the percentage of the airborne “fine” ash retrieved from the satellite is estimated to be about 1%–2% of the total ash emitted during the eruption. Finally, all of the estimated parameters (volcanic ash cloud altitude, thickness and total mass) were also validated with ground-based visible camera measurements, HYSPLIT forward trajectories, Infrared Atmospheric Sounding Interferometer (IASI) satellite data and tephra deposits

Infrared spectroscopy of volcanic gases at Masaya, Nicaragua

Volcanic gases carry valuable information about processes occurring at active volcanoes, and so their accurate measurement and analysis are highly desirable. Masaya is a low-lying persistently active basaltic volcano, which is renowned for strong passive gas emission unaccompanied by lava extrusion, although it has also undergone plinian eruptions in the past. Its consistent behaviour sustains a reliable tropospheric plume, making it an ideal location at which to study volcanic degassing. During February-March 1998 and March 1999, Masaya's gas plume composition was investigated using the new ground-based remote sensing technique of open-path Fourier transform infrared spectroscopy. This technique meets criteria for safe and accurate quantitative characterisation of volcanic gases and on a temporal resolution previously impracticable. Flexibility of operation is the chief merit of OP-FTIR, since a range of infrared sources are available (e.g. an active lamp, the sun or hot volcanic vents). Laboratory calibration experiments using primary gas standards confirmed that the instrument and subsequent spectral analysis provide highly accurate concentration measurements for volcanic species, with errors typically around 5 %. Results showed that Masaya's plume composition was little changed between the field seasons. Average molar ratios for S02/HCl, HCl/HF, C02/S02 and H20/S02 were 1.6, 4.9, 2.2 and 72, respectively, in 1998, and 1.6, 5.1, 2.3 and 66 in 1999. These ratios, coupled with simultaneous COSPEC-derived SO2 data, indicated that emission rates, especially of HCl and HF, were high compared with other passively-degassing volcanoes. Measurements using the spectrometer with different infrared sources and at different locations downwind demonstrated that tropospheric scavenging processes had little discernible effect on plume composition. In the light of these new OP-FTIR gas data, possible physical mechanisms for the degassing behaviour at Masaya Volcano have been discussed. In order to account for all the observations, an integrated model, in which gas emission rates are primarily controlled by degassing-driven convection in the conduit, is proposed