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Krotkov, N. A.

Publications and source records attributed to Krotkov, N. A..

A Decade of Global Volcanic SO2 Emissions Measured from Space

The global flux of sulfur dioxide (SO2) emitted by passive volcanic degassing is a key parameter that constrains the fluxes of other volcanic gases (including carbon dioxide, CO2) and toxic trace metals (e.g., mercury). It is also a required input for atmospheric chemistry and climate models, since it impacts the tropospheric burden of sulfate aerosol, a major climate-forcing species. Despite its significance, an inventory of passive volcanic degassing is very difficult to produce, due largely to the patchy spatial and temporal coverage of ground-based SO2 measurements. We report here the first volcanic SO2 emissions inventory derived from global, coincident satellite measurements, made by the Ozone Monitoring Instrument (OMI) on NASA's Aura satellite in 2005-2015. The OMI measurements permit estimation of SO2 emissions from over 90 volcanoes, including new constraints on fluxes from Indonesia, Papua New Guinea, the Aleutian Islands, the Kuril Islands and Kamchatka. On average over the past decade, the volcanic SO2 sources consistently detected from space have discharged a total of approximately 63 kt/day SO2 during passive degassing, or approximately 23 +/- 2 Tg/yr. We find that approximately 30% of the sources show significant decadal trends in SO2 emissions, with positive trends observed at multiple volcanoes in some regions including Vanuatu, southern Japan, Peru and Chile.

Carn, S. A.↗

High-Resolution NO2 Observations from the Airborne Compact Atmospheric Mapper: Retrieval and Validation

Nitrogen dioxide (NO2) is a short-lived atmospheric pollutant that serves as an air quality indicator and is itself a health concern. The Airborne Compact Atmospheric Mapper (ACAM) was flown on board the NASA UC-12 aircraft during the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality Maryland field campaign in July 2011. The instrument collected hyperspectral remote sensing measurements in the 304-910 nm range, allowing daytime observations of several tropospheric pollutants, including nitrogen dioxide (NO2), at an unprecedented spatial resolution of 1.5 × 1.1 sq. km. Retrievals of slant column abundance are based on the differential optical absorption spectroscopy method. For the air mass factor computations needed to convert these retrievals to vertical column abundance, we include high-resolution information for the surface reflectivity by using bidirectional reflectance distribution function data from the Moderate Resolution Imaging Spectroradiometer. We use high-resolution simulated vertical distributions of NO2 from the Community Multiscale Air Quality and Global Modeling Initiative models to account for the temporal variation in atmospheric NO2 to retrieve middle and lower tropospheric NO2 columns (NO2 below the aircraft). We compare NO2 derived from ACAM measurements with in situ observations from NASA's P-3B research aircraft, total column observations from the ground-based Pandora spectrometers, and tropospheric column observations from the space-based Ozone Monitoring Instrument. The high-resolution ACAM measurements not only give new insights into our understanding of atmospheric composition and chemistry through observation of subsampling variability in typical satellite and model resolutions, but they also provide opportunities for testing algorithm improvements for forthcoming geostationary air quality missions.

Lamsal, L. N.↗

Using CATS Near-Real-time Lidar Observations to Monitor and Constrain Volcanic Sulfur Dioxide (SO2) Forecasts

An eruption of Italian volcano Mount Etna on 3 December 2015 produced fast-moving sulfur dioxide (SO2) and sulfate aerosol clouds that traveled across Asia and the Pacific Ocean, reaching North America in just 5 days. The Ozone Profiler and Mapping Suite's Nadir Mapping UV spectrometer aboard the U.S. National Polar-orbiting Partnership satellite observed the horizontal transport of the SO2 cloud. Vertical profiles of the colocated volcanic sulfate aerosols were observed between 11.5 and 13.5 km by the new Cloud Aerosol Transport System (CATS) space-based lidar aboard the International Space Station. Backward trajectory analysis estimates the SO2 cloud altitude at 7-12 km. Eulerian model simulations of the SO2 cloud constrained by CATS measurements produced more accurate dispersion patterns compared to those initialized with the back trajectory height estimate. The near-real-time data processing capabilities of CATS are unique, and this work demonstrates the use of these observations to monitor and model volcanic clouds.

space↗

Ultraviolet Satellite Measurements of Volcanic Ash

Ultraviolet (UV) remote sensing of volcanic ash and other absorbing aerosols from space began with the launch of the first Total Ozone Mapping Spectrometer (TOMS) instrument in 1978. Subsequent UV satellite missions (TOMS, GOME, SCIAMACHY, OMI, GOME-2, OMPS) have extended UV ash measurements to the present, generating a unique multidecadal record. A UV Aerosol Index (UVAI) based on two near-UV wavelengths, equally applicable to multispectral (TOMS, DSCOVR) or hyperspectral (GOME, SCIAMACHY, OMI, GOME-2, OMPS) instruments, has been used to derive a unique absorbing aerosol climatology across multiple UV satellite missions. Advantages of UV ash measurements relative to infrared (IR) techniques include the ability to detect ash at any altitude (assuming no clouds), above clouds, and over bright surfaces, where visible and IR techniques may fail. Disadvantages include the daytime-only restriction and nonspecificity to silicate ash, since UV measurements are sensitive to any UV-absorbing aerosol, including smoke, desert dust, and pollution. However, simultaneous retrieval of sulfur dioxide (SO2) abundance and UVAI provides robust discrimination of volcanic clouds. Although the UVAI is only semiquantitative, it has proved successful at detecting and tracking volcanic ash clouds from many volcanic eruptions since 1978. NASA A-Train measurements since 2006 (eg, CALIOP) have provided much improved constraints on volcanic ash altitude, and also permit identification of aerosol type through sensor synergy. Quantitative UV retrievals of ash optical depth, effective particle size, and ash column mass are possible and require assumptions of ash refractive index, particle size distribution, and ash layer altitude. The lack of extensive ash refractive index data in the UV-visible and the effects of ash particle shape on retrievals introduce significant uncertainty in the retrieved parameters, although limited validation against IR ash retrievals has been successful. In this contribution, we review UV ash detection and retrieval techniques and provide examples of volcanic eruptions detected in the approx. 37 year data record.

Multidecadal record↗

Flux Calculation Using CARIBIC DOAS Aircraft Measurements: SO2 Emission of Norilsk

Based on a case-study of the nickel smelter in Norilsk (Siberia), the retrieval of trace gas fluxes using airborne remote sensing is discussed. A DOAS system onboard an Airbus 340 detected large amounts of SO2 and NO2 near Norilsk during a regular passenger flight within the CARIBIC project. The remote sensing data were combined with ECMWF wind data to estimate the SO2 output of the Norilsk industrial complex to be around 1 Mt per year, which is in agreement with independent estimates. This value is compared to results using data from satellite remote sensing (GOME, OMI). The validity of the assumptions underlying our estimate is discussed, including the adaptation of this method to other gases and sources like the NO2 emissions of large industries or cities.

Walter, D.↗

Using Satellite Remote Sensing and Modelling for Insights into N02 Air Pollution and NO2 Emissions

Nitrogen oxides (NO(x)) are key actors in air quality and climate change. Satellite remote sensing of tropospheric NO2 has developed rapidly with enhanced spatial and temporal resolution since initial observations in 1995. We have developed an improved algorithm and retrieved tropospheric NO2 columns from Ozone Monitoring Instrument. Column observations of tropospheric NO2 from the nadir-viewing satellite sensors contain large contributions from the boundary layer due to strong enhancement of NO2 in the boundary layer. We infer ground-level NO2 concentrations from the OMI satellite instrument which demonstrate significant agreement with in-situ surface measurements. We examine how NO2 columns measured by satellite, ground-level NO2 derived from satellite, and NO(x) emissions obtained from bottom-up inventories relate to world's urban population. We perform inverse modeling analysis of NO2 measurements from OMI to estimate "top-down" surface NO(x) emissions, which are used to evaluate and improve "bottom-up" emission inventories. We use NO2 column observations from OMI and the relationship between NO2 columns and NO(x) emissions from a GEOS-Chem model simulation to estimate the annual change in bottom-up NO(x) emissions. The emission updates offer an improved estimate of NO(x) that are critical to our understanding of air quality, acid deposition, and climate change.

Lamsal, L. N.↗

A New Retrieval Algorithm for OMI NO2: Tropospheric Results and Comparisons with Measurements and Models

Nitrogen oxides (NOx =NO+NO2) are important atmospheric trace constituents that impact tropospheric air pollution chemistry and air quality. We have developed a new NASA algorithm for the retrieval of stratospheric and tropospheric NO2 vertical column densities using measurements from the nadir-viewing Ozone Monitoring Instrument (OMI) on NASA's Aura satellite. The new products rely on an improved approach to stratospheric NO2 column estimation and stratosphere-troposphere separation and a new monthly NO2 climatology based on the NASA Global Modeling Initiative chemistry-transport model. The retrieval does not rely on daily model profiles, minimizing the influence of a priori information. We evaluate the retrieved tropospheric NO2 columns using surface in situ (e.g., AQS/EPA), ground-based (e.g., DOAS), and airborne measurements (e.g., DISCOVER-AQ). The new, improved OMI tropospheric NO2 product is available at high spatial resolution for the years 200S-present. We believe that this product is valuable for the evaluation of chemistry-transport models, examining the spatial and temporal patterns of NOx emissions, constraining top-down NOx inventories, and for the estimation of NOx lifetimes.

Swartz, W. H.↗

Fog and Cloud Induced Aerosol Modification Observed by AERONET

Large fine mode (sub-micron radius) dominated aerosols in size distributions retrieved from AERONET have been observed after fog or low-altitude cloud dissipation events. These column-integrated size distributions have been obtained at several sites in many regions of the world, typically after evaporation of low altitude cloud such as stratocumulus or fog. Retrievals with cloud processed aerosol are sometimes bimodal in the accumulation mode with the larger size mode often approx.0.4 - 0.5 microns radius (volume distribution); the smaller mode typically approx.0.12 to aprrox.0.20 microns may be interstitial aerosol that were not modified by incorporation in droplets and/or aerosol that are less hygroscopic in nature. Bimodal accumulation mode size distributions have often been observed from in situ measurements of aerosols that have interacted with clouds, and AERONET size distribution retrievals made after dissipation of cloud or fog are in good agreement with particle sizes measured by in situ techniques for cloud-processed aerosols. Aerosols of this type and large size range (in lower concentrations) may also be formed by cloud processing in partly cloudy conditions and may contribute to the shoulder of larger size particles in the accumulation mode retrievals, especially in regions where sulfate and other soluble aerosol are a significant component of the total aerosol composition. Observed trends of increasing aerosol optical depth (AOD) as fine mode radius increased suggests higher AOD in the near cloud environment and therefore greater aerosol direct radiative forcing than typically obtained from remote sensing, due to bias towards sampling at low cloud fraction.

Eck, T. F.↗

Dispersion and Lifetime of the SO2 Cloud from the August 2008 Kasatochi Eruption

Hemispherical dispersion of the SO2 cloud from the August 2008 Kasatochi eruption is analyzed using satellite data from the Ozone Monitoring Instrument (OMI) and the Goddard Trajectory Model (GTM). The operational OMI retrievals underestimate the total SO2 mass by 20-30% on 8-11 August, as compared with more accurate offline Extended Iterative Spectral Fit (EISF) retrievals, but the error decreases with time due to plume dispersion and a drop in peak SO2 column densities. The GTM runs were initialized with and compared to the operational OMI SO2 data during early plume dispersion to constrain SO2 plume heights and eruption times. The most probable SO2 heights during initial dispersion are estimated to be 10-12 km, in agreement with direct height retrievals using EISF algorithm and IR measurements. Using these height constraints a forward GTM run was initialized on 11 August to compare with the month-long Kasatochi SO2 cloud dispersion patterns. Predicted volcanic cloud locations generally agree with OMI observations, although some discrepancies were observed. Operational OMI SO2 burdens were refined using GTM-predicted mass-weighted probability density height distributions. The total refined SO2 mass was integrated over the Northern Hemisphere to place empirical constraints on the SO2 chemical decay rate. The resulting lower limit of the Kasatochi SO2 e-folding time is approx.8-9 days. Extrapolation of the exponential decay back in time yields an initial erupted SO2 mass of approx.2.2 Tg on 8 August, twice as much as the measured mass on that day.

Krotkov, N. A.↗

What Would Have Happened to the Ozone Layer if Chlorofluorocarbons (CFCs) had not been Regulated?

Ozone depletion by chlorofluorocarbons (CFCs) was first proposed by Molina and Rowland in their 1974 Nature paper. Since that time, the sci entific connection between ozone losses and CFCs and other ozone depl eting substances (ODSs) has been firmly established with laboratory m easurements, atmospheric observations, and modeling research. This science research led to the implementation of international agreements t hat largely stopped the production of ODSs. In this study we use a fu lly-coupled radiation-chemical-dynamical model to simulate a future world where ODSs were never regulated and ODS production grew at an ann ual rate of 3%. In this "world avoided" simulation 1.7 % of the globa lly-average column ozone is destroyed by 2020, and 67% is destroyed b y 2065 in comparison to 1980. Large ozone depletions in the polar region become year-round rather than just seasonal as is currently observ ed in the Antarctic ozone hole. Very large temperature decreases are observed in response to circulation changes and decreased shortwave radiation absorption by ozone. Ozone levels in the tropical lower strat osphere remain constant until about 2053 and then collapse to near ze ro by 2058 as a result of heterogeneous chemical processes (as curren tly observed in the Antarctic ozone hole). The tropical cooling that triggers the ozone collapse is caused by an increase of the tropical upwelling. In response to ozone changes, ultraviolet radiation increa ses, more than doubling the erythemal radiation in the northern summer midlatitudes by 2060.

Newman, Paul A.↗

Compilation of a Global Emission Inventory from 1980 to 2000 for Global Model Simulations of the Long-term Trend of Tropospheric Aerosols

The approach to create a comprehensive emission inventory for the time period 1980 to 2000 is described in this paper. We have recently compiled an emission database, which we will use for a 21 year simulation of tropospheric aerosols with the GOCART model. Particular attention was paid to the time-dependent SO2, black carbon and organic carbon aerosol emissions. For the emission of SO2 from sporadically erupting volcanoes, we assembled emission data from the Global Volcanism Program of the Smithsonian Institution, using the VEI to derive the volcanic cloud height and the SO2 amount, and amended this dataset by the SO2 emission data from the TOMS instrument when available. 3-dimensional aircraft emission data was obtained for a number of years from the AEAP project, converted from burned fuel to SO2 and interpolated to each year, taking the sparsity of the flight patterns into account. Other anthopogenic SO2 emissions are based on gridded emissions from the EDGAR 2000 database (excluding sources from aircraft, biomass burning and international ship traffic), which were scaled to individual years with country/regional based emission inventories. Gridded SO2 emissions from international ship traffic for 2000 and the scaling factors for other years are from [Eyring et al., 2005]. We used gridded anthropogenic black and organic carbon emissions for 1996 [Bond et al., 2005], again excluding aircraft, biomass burning and ship sources. These emissions were scaled with regional based emission inventories from 1980 to 2000 to derive gridded emissions for each year. The biomass burning emissions are based on a climatology, which is scaled with regional scaling factors derived from the TOMS aerosol index and the AVHRR/ATSR fire counts to each year [Duncan et al., 2003]. Details on the integration of the information from the various sources will be provided and the distribution patterns and total emissions in the final product will be discussed.

Diehl, T. L.↗

Accuracy Assessments and Validation of an Expanded UV Irradiance Database from Satellite Total Ozone Mapping Spectrometer (TOMS)

The TOMS UV irradiance database (1978 to 2000) has been expanded to include 5 new products (noon irradiance at 305, 310, 324, and 380 nm, and noon erythemal-weighted irradiance), in addition to the existing erythemal daily exposure, which permit direct Comparisons with ground-based measurements from UV spectrometers. Sensitivity studies are conducted to estimate uncertainties of the new TOMS UV irradiance data due to algorithm apriori assumptions. Comparisons with Brewer spectrometers as well as filter radiometers are used to review of the sources of known errors. Inability to distinguish between snow and cloud cover using only TOMS data results in large errors in estimating surface UV using snow climatology. A correction is suggested for the case when the regional snow albedo is known from an independent source. The summer-time positive bias between TOMS UV estimations and Brewer measurements can be seen at all wavelengths. This suggests the difference is not related to ozone absorption effects. We emphasize that uncertainty of boundary layer UV aerosol absorption properties remains a major source of error in modeling UV irradiance in clear sky conditions. Neglecting aerosol absorption by the present TOMS algorithm results in a positive summertime bias in clear-sky UV estimations over many locations. Due to high aerosol variability the bias is strongly site dependent. Data from UV-shadow-band radiometer and well-calibrated CIMEL sun-sky radiometer are used to quantify the bias at NASA/GSFC site in Greenbelt, MD. Recommendations are given to enable potential users to better account for local conditions by combining standard TOMS UV data with ancillary ground measurements.

Krotkov, N. A.↗

The Sulfur Dioxide Plume from the February 26, 2000 Eruption of Mt. Hekla, Iceland

The February 2000 fissure eruption of Mt. Hekla, Iceland was captured in sulfur dioxide data from the Earth Probe TOMS. A special algorithm is used to discriminate sulfur dioxide from ozone. The eruption began at 18:19 GMT on February 26, 2000 and was first viewed by TOMS at 09:55 GMT on February 27. The volcanic cloud at that time appeared as a very long and narrow arc extending west from the volcano in southern Iceland, then north across Greenland, and finally east towards Norway. The cloud altitude was reported from aircraft sightings and data to be above 10 km. The circulation of a ridge located north of Iceland produced the large arc shaped cloud. As the eruption is non-explosive the high altitude cloud contains little ash. Almost all the ash from the eruption fell out locally across Iceland. By February 29, the sulfur dioxide cloud had drifted eastward in a band along the Barents Sea coast of Norway and Russia. The analysis includes an assessment of the initial sulfur dioxide content and its rate of conversion to sulfate.

Krueger, Arlin J.↗