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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
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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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
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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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
    detail.hit.zdb_id: 2475469-9
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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:  Geophysical Research Letters Vol. 48, No. 4 ( 2021-02-28)
    In: Geophysical Research Letters, American Geophysical Union (AGU), Vol. 48, No. 4 ( 2021-02-28)
    Abstract: Large mean Arctic ( 〉 63°N) chemical ozone destruction in 2019/20 of 78 DU, similar to other extreme cold winters in the past 2 decades Anomalously weak wintertime dynamical replenishment of only ∼60 DU contributed strongly to the very low observed ozone column in March Ozone recovery caused 20 DU less mean Arctic ozone loss in March 2020 than would have occurred with stratospheric halogens at 1995 levels
    Type of Medium: Online Resource
    ISSN: 0094-8276 , 1944-8007
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2021
    detail.hit.zdb_id: 2021599-X
    detail.hit.zdb_id: 7403-2
    SSG: 16,13
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  • 7
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 126, No. 6 ( 2021-03-27)
    Abstract: Very large OClO and very low NO 2 slant columns were observed by GOME‐2A during Arctic winter 2019/20 Chemical total column ozone loss of 88 DU and 106 DU was derived from TROPOMI satellite observations and the chemical transport model Chemical ozone loss derived from OMPS‐LP satellite data reached 2.1 ppmv (80%) near the 450 K potential temperature level (∼18 km)
    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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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 5 ( 2021-03-04), p. 3317-3343
    Abstract: Abstract. As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), several climate modeling centers performed a coordinated pre-study experiment with interactive stratospheric aerosol models simulating the volcanic aerosol cloud from an eruption resembling the 1815 Mt. Tambora eruption (VolMIP-Tambora ISA ensemble). The pre-study provided the ancillary ability to assess intermodel diversity in the radiative forcing for a large stratospheric-injecting equatorial eruption when the volcanic aerosol cloud is simulated interactively. An initial analysis of the VolMIP-Tambora ISA ensemble showed large disparities between models in the stratospheric global mean aerosol optical depth (AOD). In this study, we now show that stratospheric global mean AOD differences among the participating models are primarily due to differences in aerosol size, which we track here by effective radius. We identify specific physical and chemical processes that are missing in some models and/or parameterized differently between models, which are together causing the differences in effective radius. In particular, our analysis indicates that interactively tracking hydroxyl radical (OH) chemistry following a large volcanic injection of sulfur dioxide (SO2) is an important factor in allowing for the timescale for sulfate formation to be properly simulated. In addition, depending on the timescale of sulfate formation, there can be a large difference in effective radius and subsequently AOD that results from whether the SO2 is injected in a single model grid cell near the location of the volcanic eruption, or whether it is injected as a longitudinally averaged band around the Earth.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 9
    Online Resource
    Online Resource
    Copernicus GmbH ; 2022
    In:  Atmospheric Chemistry and Physics Vol. 22, No. 16 ( 2022-08-23), p. 10635-10656
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 16 ( 2022-08-23), p. 10635-10656
    Abstract: Abstract. We use TOMCAT, a 3-dimensional (3D) offline chemical transport model (CTM) forced by two different meteorological reanalysis data sets (ERA-Interim and ERA5) from the European Centre for Medium-Range weather Forecasts (ECMWF) to analyse seasonal behaviour and long-term trends in stratospheric ozone and mean age of air. The model-simulated ozone variations are evaluated against two observation-based data sets. For total column ozone (TCO) comparisons, we use the Copernicus Climate Change Service (C3S) data (1979–2019), while for ozone profiles we use the Stratospheric Water and OzOne Satellite Homogenized (SWOOSH) data set (1984–2019). We find that the CTM simulations forced by ERA-Interim (A_ERAI) and ERA5 (B_ERA5) can both successfully reproduce the spatial and temporal variations in stratospheric ozone. Also, modelled TCO anomalies from B_ERA5 show better agreement with C3S than A_ERAI, especially in Northern Hemisphere (NH) mid latitudes, except that it gives somewhat larger positive biases (〉 15 DU, Dobson units) during winter–spring seasons. Ozone profile comparisons against SWOOSH data show larger differences between the two simulations. In the lower stratosphere, ozone differences can be directly attributed to the representation of dynamical processes, whereas in the upper stratosphere they can be directly linked to the differences in temperatures between ERAI and ERA5 data sets. Although TCO anomalies from B_ERA5 show relatively better agreement with C3S compared to A_ERAI, a comparison with SWOOSH data does not confirm that B_ERA5 performs better at simulating the variations in the stratospheric ozone profiles. We employ a multivariate regression model to quantify the TCO and ozone profile trends before and after peak stratospheric halogen loading in 1997. Our results show that, compared to C3S, TCO recovery trends (since 1998) in simulation B_ERA5 are significantly overestimated in the Southern Hemisphere (SH) mid latitudes, while for A_ERAI in the NH mid latitudes, simulated ozone trends remain negative. Similarly, in the lower stratosphere, B_ERA5 shows positive ozone recovery trends for both NH and SH mid latitudes. In contrast, both SWOOSH and A_ERAI show opposite (negative) trends in the NH mid latitudes. Furthermore, we analyse age of air (AoA) trends to diagnose transport differences between the two reanalysis data sets. Simulation B_ERA5 shows a positive AoA trend after 1998 and somewhat older age in the NH lower stratosphere compared to A_ERAI, indicating that a slower Brewer–Dobson circulation does not translate into reduced wintertime ozone buildup in the NH extratropical lower stratosphere. Overall, our results show that models forced by the most recent ERA5 reanalyses may not yet be capable of reproducing observed changes in stratospheric ozone, particularly in the lower stratosphere.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 24, No. 2 ( 2024-01-19), p. 789-806
    Abstract: Abstract. Exposure to air pollution is a leading public health risk factor in India, especially over densely populated Delhi and the surrounding Indo-Gangetic Plain. During the post-monsoon seasons, the prevailing north-westerly winds are known to influence aerosol pollution events in Delhi by advecting pollutants from agricultural fires as well as from local sources. Here we investigate the year-round impact of meteorology on gaseous nitrogen oxides (NOx=NO+NO2). We use bottom-up NOx emission inventories (anthropogenic and fire) and high-resolution satellite measurement based tropospheric column NO2 (TCNO2) data, from S5P aboard TROPOMI, alongside a back-trajectory model (ROTRAJ) to investigate the balance of local and external sources influencing air pollution changes in Delhi, with a focus on different emissions sectors. Our analysis shows that accumulated emissions (i.e. integrated along the trajectory path, allowing for chemical loss) are highest under westerly, north-westerly and northerly flow during pre-monsoon (February–May) and post-monsoon (October–February) seasons. According to this analysis, during the pre-monsoon season, the highest accumulated satellite TCNO2 trajectories come from the east and north-west of Delhi. TCNO2 is elevated within Delhi and the Indo-Gangetic Plain (IGP) to the east of city. The accumulated NOx emission trajectories indicate that the transport and industry sectors together account for more than 80 % of the total accumulated emissions, which are dominated by local sources ( 〉 70 %) under easterly winds and north-westerly winds. The high accumulated emissions estimated during the pre-monsoon season under north-westerly wind directions are likely to be driven by high NOx emissions locally and in nearby regions (since NOx lifetime is reduced and the boundary layer is relatively deeper in this season). During the post-monsoon season the highest accumulated satellite TCNO2 trajectories are advected from Punjab and Haryana, where satellite TCNO2 is elevated, indicating the potential for the long-range transport of agricultural burning emissions to Delhi. However, accumulated NOx emissions indicate local (70 %) emissions from the transport sector are the largest contributor to the total accumulated emissions. High local emissions, coupled with a relatively long NOx atmospheric lifetime and shallow boundary layer, aid the build-up of emissions locally and along the trajectory path. This indicates the possibility that fire emissions datasets may not capture emissions from agricultural waste burning in the north-west sufficiently to accurately quantify their influence on Delhi air quality (AQ). Analysis of daily ground-based NO2 observations indicates that high-pollution episodes ( 〉 90th percentile) occur predominantly in the post-monsoon season, and more than 75 % of high-pollution events are primarily caused by local sources. But there is also a considerable influence from non-local (30 %) emissions from the transport sector during the post-monsoon season. Overall, we find that in the post-monsoon season, there is substantial accumulation of high local NOx emissions from the transport sector (70 % of total emissions, 70 % local), alongside the import of NOx pollution into Delhi (30 % non-local). This work indicates that both high local NOx emissions from the transport sector and the advection of highly polluted air originating from outside Delhi are of concern for the population. As a result, air quality mitigation strategies need to be adopted not only in Delhi but in the surrounding regions to successfully control this issue. In addition, our analysis suggests that the largest benefits to Delhi NOx air quality would be seen with targeted reductions in emissions from the transport and agricultural waste burning sectors, particularly during the post-monsoon season.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2024
    detail.hit.zdb_id: 2092549-9
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