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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 6 ( 2021-04-01), p. 5235-5251
    Abstract: Abstract. We have estimated the spatial changes in NO2 levels over different regions of India during the COVID-19 lockdown (25 March–3 May 2020) using the satellite-based tropospheric column NO2 observed by the Ozone Monitoring Instrument (OMI) and the Tropospheric Monitoring Instrument (TROPOMI), as well as surface NO2 concentrations obtained from the Central Pollution Control Board (CPCB) monitoring network. A substantial reduction in NO2 levels was observed across India during the lockdown compared to the same period during previous business-as-usual years, except for some regions that were influenced by anomalous fires in 2020. The reduction (negative change) over the urban agglomerations was substantial (∼ 20 %–40 %) and directly proportional to the urban size and population density. Rural regions across India also experienced lower NO2 values by ∼ 15 %–25 %. Localised enhancements in NO2 associated with isolated emission increase scattered across India were also detected. Observed percentage changes in satellite and surface observations were consistent across most regions and cities, but the surface observations were subject to larger variability depending on their proximity to the local emission sources. Observations also indicate NO2 enhancements of up to ∼ 25 % during the lockdown associated with fire emissions over the north-east of India and some parts of the central regions. In addition, the cities located near the large fire emission sources show much smaller NO2 reduction than other urban areas as the decrease at the surface was masked by enhancement in NO2 due to the transport of the fire emissions.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 2
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 13, No. 3 ( 2020-03-17), p. 1223-1266
    Abstract: Abstract. Here we present a description of the UKCA StratTrop chemical mechanism, which is used in the UKESM1 Earth system model for CMIP6. The StratTrop chemical mechanism is a merger of previously well-evaluated tropospheric and stratospheric mechanisms, and we provide results from a series of bespoke integrations to assess the overall performance of the model. We find that the StratTrop scheme performs well when compared to a wide array of observations. The analysis we present here focuses on key components of atmospheric composition, namely the performance of the model to simulate ozone in the stratosphere and troposphere and constituents that are important for ozone in these regions. We find that the results obtained for tropospheric ozone and its budget terms from the use of the StratTrop mechanism are sensitive to the host model; simulations with the same chemical mechanism run in an earlier version of the MetUM host model show a range of sensitivity to emissions that the current model does not fall within. Whilst the general model performance is suitable for use in the UKESM1 CMIP6 integrations, we note some shortcomings in the scheme that future targeted studies will address.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2456725-5
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 21 ( 2020-11-13), p. 13627-13654
    Abstract: Abstract. Accurately quantifying volcanic impacts on climate is a key requirement for robust attribution of anthropogenic climate change. Here we use the Unified Model – United Kingdom Chemistry and Aerosol (UM-UKCA) composition–climate model to simulate the global dispersion of the volcanic aerosol clouds from the three largest eruptions of the 20th century: 1963 Mt Agung, 1982 El Chichón, and 1991 Mt Pinatubo. The model has interactive stratospheric chemistry and aerosol microphysics, with coupled aerosol–radiation interactions for realistic composition–dynamics feedbacks. Our simulations align with the design of the Interactive Stratospheric Aerosol Model Intercomparison (ISA-MIP) “Historical Eruption SO2 Emissions Assessment”. For each eruption, we perform three-member ensemble model experiments for upper, mid-point, and lower estimates of SO2 emission, each re-initialised from a control run to approximately match the observed transition in the phase of the quasi-biennial oscillation (QBO) in the 6 months after the eruptions. With this experimental design, we assess how each eruption's emitted SO2 translates into a tropical reservoir of volcanic aerosol and analyse the subsequent dispersion to mid-latitudes. We compare the simulations to the volcanic forcing datasets (e.g. Space-based Stratospheric Aerosol Climatology (GloSSAC); Sato et al., 1993, and Ammann et al., 2003) that are used in historical integrations for the two most recent Coupled Model Intercomparison Project (CMIP) assessments. For Pinatubo and El Chichón, we assess the vertical extent of the simulated volcanic clouds by comparing modelled extinction to the Stratospheric Aerosol and Gas Experiment (SAGE-II) v7.0 satellite measurements and to 1964–1965 Northern Hemisphere ground-based lidar measurements for Agung. As an independent test for the simulated volcanic forcing after Pinatubo, we also compare simulated shortwave (SW) and longwave (LW) top-of-the-atmosphere radiative forcings to the flux anomalies measured by the Earth Radiation Budget Experiment (ERBE) satellite instrument. For the Pinatubo simulations, an injection of 10 to 14 Tg SO2 gives the best match to the High Resolution Infrared Sounder (HIRS) satellite-derived global stratospheric sulfur burden, with good agreement also with SAGE-II mid-visible and near-infra-red extinction measurements. This 10–14 Tg range of emission also generates a heating of the tropical stratosphere that is consistent with the temperature anomaly present in the ERA-Interim reanalysis. For El Chichón, the simulations with 5 and 7 Tg SO2 emission give best agreement with the observations. However, these simulations predict a much deeper volcanic cloud than represented in the GloSSAC dataset, which is largely based on an interpolation between Stratospheric Aerosol Measurements (SAM-II) satellite and aircraft measurements. In contrast, these simulations show much better agreement during the SAGE-II period after October 1984. For 1963 Agung, the 9 Tg simulation compares best to the forcing datasets with the model capturing the lidar-observed signature of the altitude of peak extinction descending from 20 km in 1964 to 16 km in 1965. Overall, our results indicate that the downward adjustment to SO2 emission found to be required by several interactive modelling studies when simulating Pinatubo is also needed when simulating the Agung and El Chichón aerosol clouds. This strengthens the hypothesis that interactive stratospheric aerosol models may be missing an important removal or re-distribution process (e.g. effects of co-emitted ash) which changes how the tropical reservoir of volcanic aerosol evolves in the initial months after an eruption. Our model comparisons also identify potentially important inhomogeneities in the CMIP6 dataset for all three eruption periods that are hard to reconcile with variations predicted in the interactive stratospheric aerosol simulations. We also highlight large differences between the CMIP5 and CMIP6 volcanic aerosol datasets for the Agung and El Chichón periods. Future research should aim to reduce this uncertainty by reconciling the datasets with additional stratospheric aerosol observations.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 4
    In: Earth System Science Data, Copernicus GmbH, Vol. 13, No. 9 ( 2021-09-08), p. 4407-4423
    Abstract: Abstract. We report the recovery and processing methodology of the first ever multi-year lidar dataset of the stratospheric aerosol layer. A Q-switched ruby lidar measured 66 vertical profiles of 694 nm attenuated backscatter at Lexington, Massachusetts, between January 1964 and August 1965, with an additional nine profile measurements conducted from College, Alaska, during July and August 1964. We describe the processing of the recovered lidar backscattering ratio profiles to produce mid-visible (532 nm) stratospheric aerosol extinction profiles (sAEP532) and stratospheric aerosol optical depth (sAOD532) measurements, utilizing a number of contemporary measurements of several different atmospheric variables. Stratospheric soundings of temperature and pressure generate an accurate local molecular backscattering profile, with nearby ozone soundings determining the ozone absorption, which are used to correct for two-way ozone transmittance. Two-way aerosol transmittance corrections are also applied based on nearby observations of total aerosol optical depth (across the troposphere and stratosphere) from sun photometer measurements. We show that accounting for these two-way transmittance effects substantially increases the magnitude of the 1964/1965 stratospheric aerosol layer's optical thickness in the Northern Hemisphere mid-latitudes, then ∼ 50 % larger than represented in the Coupled Model Intercomparison Project 6 (CMIP6) volcanic forcing dataset. Compared to the uncorrected dataset, the combined transmittance correction increases the sAOD532 by up to 66 % for Lexington and up to 27 % for Fairbanks, as well as individual sAEP532 adjustments of similar magnitude. Comparisons with the few contemporary measurements available show better agreement with the corrected two-way transmittance values. Within the January 1964 to August 1965 measurement time span, the corrected Lexington sAOD532 time series is substantially above 0.05 in three distinct periods, October 1964, March 1965, and May–June 1965, whereas the 6 nights the lidar measured in December 1964 and January 1965 had sAOD values of at most ∼ 0.03. The comparison with interactive stratospheric aerosol model simulations of the Agung aerosol cloud shows that, although substantial variation in mid-latitude sAOD532 are expected from the seasonal cycle in the stratospheric circulation, the Agung cloud's dispersion from the tropics would have been at its strongest in winter and weakest in summer. The increasing trend in sAOD from January to July 1965, also considering the large variability, suggests that the observed variations are from a different source than Agung, possibly from one or both of the two eruptions that occurred in 1964/1965 with a Volcanic Explosivity Index (VEI) of 3: Trident, Alaska, and Vestmannaeyjar, Heimaey, south of Iceland. A detailed error analysis of the uncertainties in each of the variables involved in the processing chain was conducted. Relative errors for the uncorrected sAEP532 were 54 % for Fairbanks and 44 % Lexington. For the corrected sAEP532 the errors were 61 % and 64 %, respectively. The analysis of the uncertainties identified variables that with additional data recovery and reprocessing could reduce these relative error levels. Data described in this work are available at https://doi.org/10.1594/PANGAEA.922105 (Antuña-Marrero et al., 2020a).
    Type of Medium: Online Resource
    ISSN: 1866-3516
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 5
    In: AIP Advances, AIP Publishing, Vol. 12, No. 12 ( 2022-12-01)
    Type of Medium: Online Resource
    ISSN: 2158-3226
    Language: English
    Publisher: AIP Publishing
    Publication Date: 2022
    detail.hit.zdb_id: 2583909-3
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  • 6
    Online Resource
    Online Resource
    American Geophysical Union (AGU) ; 2021
    In:  Journal of Geophysical Research: Atmospheres Vol. 126, No. 8 ( 2021-04-27)
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 126, No. 8 ( 2021-04-27)
    Abstract: First comparison between long‐term satellite measurements (ACE‐FTS) of atmospheric HFC‐134a and a 3D chemical transport model (SLIMCAT) Observations agree well with SLIMCAT, although ACE‐FTS is biased low by up to 10–15 ppt in the troposphere between 30°S and 30°N Global trends are linear to a good approximation: 4.49 ppt/year for ACE‐FTS (2004–2018; 5.5–24.5 km) and 4.66 ppt/year for SLIMCAT
    Type of Medium: Online Resource
    ISSN: 2169-897X , 2169-8996
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2021
    detail.hit.zdb_id: 710256-2
    detail.hit.zdb_id: 2016800-7
    detail.hit.zdb_id: 2969341-X
    SSG: 16,13
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  • 7
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 126, No. 8 ( 2021-04-27)
    Abstract: Record low ozone columns ( 〈 200 DU) were observed over Eureka in spring 2020 Limited dynamical resupply of ozone and chemical destruction both contributed to reduced ozone columns Mean chemical ozone loss of 111–126 DU (27%–31%) represents similar absolute loss and greater relative loss compared to that in spring 2011
    Type of Medium: Online Resource
    ISSN: 2169-897X , 2169-8996
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2021
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    detail.hit.zdb_id: 2016800-7
    detail.hit.zdb_id: 2969341-X
    SSG: 16,13
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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 2 ( 2022-01-19), p. 903-916
    Abstract: Abstract. Until now our understanding of the 11-year solar cycle signal (SCS) in stratospheric ozone has been largely based on high-quality but sparse ozone profiles from the Stratospheric Aerosol and Gas Experiment (SAGE) II or coarsely resolved ozone profiles from the nadir-viewing Solar Backscatter Ultraviolet Radiometer (SBUV) satellite instruments. Here, we analyse 16 years (2005–2020) of ozone profile measurements from the Microwave Limb Sounder (MLS) instrument on the Aura satellite to estimate the 11-year SCS in stratospheric ozone. Our analysis of Aura-MLS data suggests a single-peak-structured SCS profile (about 3 % near 4 hPa or 40 km) in tropical stratospheric ozone, which is significantly different to the SAGE II and SBUV-based double-peak-structured SCS. We also find that MLS-observed ozone variations are more consistent with ozone from our control model simulation that uses Naval Research Laboratory (NRL) v2 solar fluxes. However, in the lowermost stratosphere modelled ozone shows a negligible SCS compared to about 1 % in Aura-MLS data. An ensemble of ordinary least squares (OLS) and three regularised (lasso, ridge and elastic net) linear regression models confirms the robustness of the estimated SCS. In addition, our analysis of MLS and model simulations shows a large SCS in the Antarctic lower stratosphere that was not seen in earlier studies. We also analyse chemical transport model simulations with alternative solar flux data. We find that in the upper (and middle) stratosphere the model simulation with Solar Radiation and Climate Experiment (SORCE) satellite solar fluxes is also consistent with the MLS-derived SCS and agrees well with the control simulation and one which uses Spectral and Total Irradiance Reconstructions (SATIRE) solar fluxes. Hence, our model simulation suggests that with recent adjustments and corrections, SORCE data can be used to analyse effects of solar flux variations. Furthermore, analysis of a simulation with fixed solar fluxes and one with fixed (annually repeating) meteorology confirms that the implicit dynamical SCS in the (re)analysis data used to force the model is not enough to simulate the observed SCS in the middle and upper stratospheric ozone. Finally, we argue that the overall significantly different SCS compared to previous estimates might be due to a combination of different factors such as much denser MLS measurements, almost linear stratospheric chlorine loading changes over the analysis period, variations in the stratospheric dynamics as well as relatively unperturbed stratospheric aerosol layer that might have influenced earlier analyses.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2092549-9
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  • 9
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 2 ( 2023-01-19), p. 921-948
    Abstract: Abstract. A previous model intercomparison of the Tambora aerosol cloud has highlighted substantial differences among simulated volcanic aerosol properties in the pre-industrial stratosphere and has led to questions about the applicability of global aerosol models for large-magnitude explosive eruptions prior to the observational period. Here, we compare the evolution of the stratospheric aerosol cloud following the well-observed June 1991 Mt. Pinatubo eruption simulated with six interactive stratospheric aerosol microphysics models to a range of observational data sets. Our primary focus is on the uncertainties regarding initial SO2 emission following the Pinatubo eruption, as prescribed in the Historical Eruptions SO2 Emission Assessment experiments (HErSEA), in the framework of the Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP). Six global models with interactive aerosol microphysics took part in this study: ECHAM6-SALSA, EMAC, ECHAM5-HAM, SOCOL-AERv2, ULAQ-CCM, and UM-UKCA. Model simulations are performed by varying the SO2 injection amount (ranging between 5 and 10 Tg S) and the altitude of injection (between 18–25 km). The comparisons show that all models consistently demonstrate faster reduction from the peak in sulfate mass burden in the tropical stratosphere. Most models also show a stronger transport towards the extratropics in the Northern Hemisphere, at the expense of the observed tropical confinement, suggesting a much weaker subtropical barrier in all the models, which results in a shorter e-folding time compared to the observations. Furthermore, simulations in which more than 5 Tg S in the form of SO2 is injected show an initial overestimation of the sulfate burden in the tropics and, in some models, in the Northern Hemisphere and a large surface area density a few months after the eruption compared to the values measured in the tropics and the in situ measurements over Laramie. This draws attention to the importance of including processes such as the ash injection for the removal of the initial SO2 and aerosol lofting through local heating.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 10
    In: Earth System Science Data, Copernicus GmbH, Vol. 13, No. 12 ( 2021-12-10), p. 5711-5729
    Abstract: Abstract. High-quality stratospheric ozone profile data sets are a key requirement for accurate quantification and attribution of long-term ozone changes. Satellite instruments provide stratospheric ozone profile measurements over typical mission durations of 5–15 years. Various methodologies have then been applied to merge and homogenise the different satellite data in order to create long-term observation-based ozone profile data sets with minimal data gaps. However, individual satellite instruments use different measurement methods, sampling patterns and retrieval algorithms which complicate the merging of these different data sets. In contrast, atmospheric chemical models can produce chemically consistent long-term ozone simulations based on specified changes in external forcings, but they are subject to the deficiencies associated with incomplete understanding of complex atmospheric processes and uncertain photochemical parameters. Here, we use chemically self-consistent output from the TOMCAT 3-D chemical transport model (CTM) and a random-forest (RF) ensemble learning method to create a merged 42-year (1979–2020) stratospheric ozone profile data set (ML-TOMCAT V1.0). The underlying CTM simulation was forced by meteorological reanalyses, specified trends in long-lived source gases, solar flux and aerosol variations. The RF is trained using the Stratospheric Water and OzOne Satellite Homogenized (SWOOSH) data set over the time periods of the Microwave Limb Sounder (MLS) from the Upper Atmosphere Research Satellite (UARS) (1991–1998) and Aura (2005–2016) missions. We find that ML-TOMCAT shows excellent agreement with available independent satellite-based data sets which use pressure as a vertical coordinate (e.g. GOZCARDS, SWOOSH for non-MLS periods) but weaker agreement with the data sets which are altitude-based (e.g. SAGE-CCI-OMPS, SCIAMACHY-OMPS). We find that at almost all stratospheric levels ML-TOMCAT ozone concentrations are well within uncertainties of the observational data sets. The ML-TOMCAT (V1.0) data set is ideally suited for the evaluation of chemical model ozone profiles from the tropopause to 0.1 hPa and is freely available via https://doi.org/10.5281/zenodo.5651194 (Dhomse et al., 2021).
    Type of Medium: Online Resource
    ISSN: 1866-3516
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2475469-9
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