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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 1 ( 2023-01-16), p. 637-661
    Abstract: Abstract. As the third most important greenhouse gas (GHG) after carbon dioxide (CO2) and methane (CH4), tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of ±50 % depending on the model and the altitude. The MMM performs best, within ±8 % for most locations and seasons. However, nearly all models overestimate O3 near the tropopause (∼300 hPa or ∼8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx, and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O3.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2092549-9
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  • 2
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 16, No. 11 ( 2023-06-15), p. 2957-2988
    Abstract: Abstract. Ozone trend estimates have shown large uncertainties in the upper troposphere–lower stratosphere (UTLS) region despite multi-decadal observations available from ground-based, balloon, aircraft, and satellite platforms. These uncertainties arise from large natural variability driven by dynamics (reflected in tropopause and jet variations) as well as the strength in constituent transport and mixing. Additionally, despite all the community efforts there is still a lack of representative high-quality global UTLS measurements to capture this variability. The Stratosphere-troposphere Processes And their Role in Climate (SPARC) Observed Composition Trends and Variability in the UTLS (OCTAV-UTLS) activity aims to reduce uncertainties in UTLS composition trend estimates by accounting for this dynamically induced variability. In this paper, we describe the production of dynamical diagnostics using meteorological information from reanalysis fields that facilitate mapping observations from several platforms into numerous geophysically based coordinates (including tropopause and upper tropospheric jet relative coordinates). Suitable coordinates should increase the homogeneity of the air masses analyzed together, thus reducing the uncertainty caused by spatiotemporal sampling biases in the quantification of UTLS composition trends. This approach thus provides a framework for comparing measurements with diverse sampling patterns and leverages the meteorological context to derive maximum information on UTLS composition and trends and its relationships to dynamical variability. The dynamical diagnostics presented here are the first comprehensive set describing the meteorological context for multi-decadal observations by ozonesondes, lidar, aircraft, and satellite measurements in order to study the impact of dynamical processes on observed UTLS trends by different sensors on different platforms. Examples using these diagnostics to map multi-platform datasets into different geophysically based coordinate systems are provided. The diagnostics presented can also be applied to analysis of greenhouse gases other than ozone that are relevant to surface climate and UTLS chemistry.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 19 ( 2022-10-06), p. 12827-12855
    Abstract: Abstract. This study analyses the variability and trends of ultraviolet-B (UV-B, wavelength 280–320 nm) radiation that can cause DNA damage. The variability and trends caused by climate change due to enhanced greenhouse gas (GHG) concentrations. The analysis is based on DNA-active irradiance, total ozone, total cloud cover, and surface albedo calculations with the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) chemistry–climate model (CCM) free-running simulations following the RCP 6.0 climate scenario for the period 1960–2100. The model output is evaluated with DNA-active irradiance ground-based measurements, satellite SBUV (v8.7) total-ozone measurements, and satellite MODerate-resolution Imaging Spectroradiometer (MODIS) Terra cloud cover data. The results show that the model reproduces the observed variability and change in total ozone, DNA-active irradiance, and cloud cover for the period 2000–2018 quite well according to the statistical comparisons. Between 50∘ N–50∘ S, the DNA-damaging UV radiation is expected to decrease until 2050 and to increase thereafter, as was shown previously by Eleftheratos et al. (2020). This change is associated with decreases in the model total cloud cover and negative trends in total ozone after about 2050 due to increasing GHGs. The new study confirms the previous work by adding more stations over low latitudes and mid-latitudes (13 instead of 5 stations). In addition, we include estimates from high-latitude stations with long-term measurements of UV irradiance (three stations in the northern high latitudes and four stations in the southern high latitudes greater than 55∘). In contrast to the predictions for 50∘ N–50∘ S, it is shown that DNA-active irradiance will continue to decrease after the year 2050 over high latitudes because of upward ozone trends. At latitudes poleward of 55∘ N, we estimate that DNA-active irradiance will decrease by 8.2 %±3.8 % from 2050 to 2100. Similarly, at latitudes poleward of 55∘ S, DNA-active irradiance will decrease by 4.8 % ± 2.9 % after 2050. The results for the high latitudes refer to the summer period and not to the seasons when ozone depletion occurs, i.e. in late winter and spring. The contributions of ozone, cloud, and albedo trends to the DNA-active irradiance trends are estimated and discussed.
    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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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 24 ( 2023-12-21), p. 15693-15709
    Abstract: Abstract. With a few exceptions, most studies on tropospheric ozone (O3) variability during and following the COrona VIrus Disease (COVID-19) economic downturn focused on high-emission regions or urban environments. In this work, we investigated the impact of the societal restriction measures during the COVID-19 pandemic on surface O3 at several high-elevation sites across North America and western Europe. Monthly O3 anomalies were calculated for 2020 and 2021, with respect to the baseline period 2000–2019, to explore the impact of the economic downturn initiated in 2020 and its recovery in 2021. In total, 41 high-elevation sites were analyzed: 5 rural or mountaintop stations in western Europe, 19 rural sites in the western US, 4 sites in the western US downwind of highly polluted source regions, and 4 rural sites in the eastern US, plus 9 mountaintop or high-elevation sites outside Europe and the United States to provide a “global” reference. In 2020, the European high-elevation sites showed persistent negative surface O3 anomalies during spring (March–May, i.e., MAM) and summer (June–August, i.e., JJA), except for April. The pattern was similar in 2021, except for June. The rural sites in the western US showed similar behavior, with negative anomalies in MAM and JJA 2020 (except for August) and MAM 2021. The JJA 2021 seasonal mean was influenced by strong positive anomalies in July due to large and widespread wildfires across the western US. The polluted sites in the western US showed negative O3 anomalies during MAM 2020 and a slight recovery in 2021, resulting in a positive mean anomaly for MAM 2021 and a pronounced month-to-month variability in JJA 2021 anomalies. The eastern US sites were also characterized by below-mean O3 for both MAM and JJA 2020, while in 2021 the negative values exhibited an opposite structure compared to the western US sites, which were influenced by wildfires. Concerning the rest of the world, a global picture could not be drawn, as the sites, spanning a range of different environments, did not show consistent anomalies, with a few sites not experiencing any notable variation. Moreover, we also compared our surface anomalies to the variability of mid-tropospheric O3 detected by the IASI (Infrared Atmospheric Sounding Interferometer) satellite instrument. Negative anomalies were observed by IASI, consistent with published satellite and modeling studies, suggesting that the anomalies can be largely attributed to the reduction of O3 precursor emissions in 2020.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2092549-9
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 17 ( 2017-09-11), p. 10675-10690
    Abstract: Abstract. Ozone profile trends over the period 2000 to 2016 from several merged satellite ozone data sets and from ground-based data measured by four techniques at stations of the Network for the Detection of Atmospheric Composition Change indicate significant ozone increases in the upper stratosphere, between 35 and 48 km altitude (5 and 1 hPa). Near 2 hPa (42 km), ozone has been increasing by about 1.5 % per decade in the tropics (20° S to 20° N), and by 2 to 2.5 % per decade in the 35 to 60° latitude bands of both hemispheres. At levels below 35 km (5 hPa), 2000 to 2016 ozone trends are smaller and not statistically significant. The observed trend profiles are consistent with expectations from chemistry climate model simulations. This study confirms positive trends of upper stratospheric ozone already reported, e.g., in the WMO/UNEP Ozone Assessment 2014 or by Harris et al. (2015). Compared to those studies, three to four additional years of observations, updated and improved data sets with reduced drift, and the fact that nearly all individual data sets indicate ozone increase in the upper stratosphere, all give enhanced confidence. Uncertainties have been reduced, for example for the trend near 2 hPa in the 35 to 60° latitude bands from about ±5 % (2σ) in Harris et al. (2015) to less than ±2 % (2σ). Nevertheless, a thorough analysis of possible drifts and differences between various data sources is still required, as is a detailed attribution of the observed increases to declining ozone-depleting substances and to stratospheric cooling. Ongoing quality observations from multiple independent platforms are key for verifying that recovery of the ozone layer continues as expected.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 6
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 10, No. 9 ( 2017-09-27), p. 3539-3545
    Abstract: Abstract. A one-time-calibrated (in December 2013) Pandora spectrometer instrument (Pan #034) has been compared to a periodically calibrated Dobson spectroradiometer (Dobson #061) co-located in Boulder, Colorado, and compared with two satellite instruments over a 3-year period (December 2013–December 2016). The results show good agreement between Pan #034 and Dobson #061 within their statistical uncertainties. Both records are corrected for ozone retrieval sensitivity to stratospheric temperature variability obtained from the Global Modeling Initiative (GMI) and Modern-Era Retrospective analysis for Research and Applications (MERRA-2) model calculations. Pandora #034 and Dobson #061 differ by an average of 2.1 ± 3.2 % when both instruments use their standard ozone absorption cross sections in the retrieval algorithms. The results show a relative drift (0.2 ± 0.08 % yr−1) between Pandora observations against NOAA Dobson in Boulder, CO, over a 3-year period of continuous operation. Pandora drifts relative to the satellite Ozone Monitoring Instrument (OMI) and the Ozone Mapping Profiler Suite (OMPS) are +0.18 ± 0.2 % yr−1 and −0.18 ± 0.2 % yr−1, respectively, where the uncertainties are 2 standard deviations. The drift between Dobson #061 and OMPS for a 5.5-year period (January 2012–June 2017) is −0.07 ± 0.06 % yr−1.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 7
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 16 ( 2020-08-26), p. 9915-9938
    Abstract: Abstract. Detecting a tropospheric ozone trend from sparsely sampled ozonesonde profiles (typically once per week) is challenging due to the short-lived anomalies in the time series resulting from ozone's high temporal variability. To enhance trend detection, we have developed a sophisticated statistical approach that utilizes a geoadditive model to assess ozone variability across a time series of vertical profiles. Treating the profile time series as a set of individual time series on discrete pressure surfaces, a class of smoothing spline ANOVA (analysis of variance) models is used for the purpose of jointly modeling multiple correlated time series (on separate pressure surfaces) by their associated seasonal and interannual variabilities. This integrated fit method filters out the unstructured variation through a statistical regularization (i.e., a roughness penalty) by taking advantage of the additional correlated data points available on the pressure surfaces above and below the surface of interest. We have applied this technique to the trend analysis of the vertically correlated time series of tropospheric ozone observations from (1) IAGOS (In-service Aircraft for a Global Observing System) commercial aircraft profiles above Europe and China throughout 1994–2017 and (2) NOAA GML's (Global Monitoring Laboratory) ozonesonde records at Hilo, Hawaii, (1982–2018) and Trinidad Head, California (1998–2018). We illustrate the ability of this technique to detect a consistent trend estimate and its effectiveness in reducing the associated uncertainty in the profile data due to the low sampling frequency. We also conducted a sensitivity analysis of frequent IAGOS profiles above Europe (approximately 120 profiles per month) to determine how many profiles in a month are required for reliable long-term trend detection. When ignoring the vertical correlation, we found that a typical sampling strategy (i.e. four profiles per month) might result in 7 % of sampled trends falling outside the 2σ uncertainty interval derived from the full dataset with an associated 10 % of mean absolute percentage error. Based on a series of sensitivity studies, we determined optimal sampling frequencies for (1) basic trend detection and (2) accurate quantification of the trend. When applying the integrated fit method, we find that a typical sampling frequency of four profiles per month is adequate for basic trend detection; however, accurate quantification of the trend requires 14 profiles per month. Accurate trend quantification can be achieved with only 10 profiles per month if a regular sampling frequency is applied. In contrast, the standard separated fit method, which ignores the vertical correlation between pressure surfaces, requires 8 profiles per month for basic trend detection and 18 profiles per month for accurate trend quantification. While our method improves trend detection from sparse datasets, the key to substantially reducing the uncertainty is to increase the sampling frequency.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 3 ( 2022-02-04), p. 1707-1737
    Abstract: Abstract. The Fires, Asian, and Stratospheric Transport–Las Vegas Ozone Study (FAST-LVOS) was conducted in May and June of 2017 to study the transport of ozone (O3) to Clark County, Nevada, a marginal non-attainment area in the southwestern United States (SWUS). This 6-week (20 May–30 June 2017) field campaign used lidar, ozonesonde, aircraft, and in situ measurements in conjunction with a variety of models to characterize the distribution of O3 and related species above southern Nevada and neighboring California and to probe the influence of stratospheric intrusions and wildfires as well as local, regional, and Asian pollution on surface O3 concentrations in the Las Vegas Valley (≈ 900 m above sea level, a.s.l.). In this paper, we describe the FAST-LVOS campaign and present case studies illustrating the influence of different transport processes on background O3 in Clark County and southern Nevada. The companion paper by Zhang et al. (2020) describes the use of the AM4 and GEOS-Chem global models to simulate the measurements and estimate the impacts of transported O3 on surface air quality across the greater southwestern US and Intermountain West. The FAST-LVOS measurements found elevated O3 layers above Las Vegas on more than 75 % (35 of 45) of the sample days and show that entrainment of these layers contributed to mean 8 h average regional background O3 concentrations of 50–55 parts per billion by volume (ppbv), or about 85–95 µg m−3. These high background concentrations constitute 70 %–80 % of the current US National Ambient Air Quality Standard (NAAQS) of 70 ppbv (≈ 120 µg m−3 at 900 m a.s.l.) for the daily maximum 8 h average (MDA8) and will make attainment of the more stringent standards of 60 or 65 ppbv currently being considered extremely difficult in the interior SWUS.
    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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  • 9
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 8 ( 2022-04-25), p. 5435-5458
    Abstract: Abstract. Stratospheric circulation is a critical part of the Arctic ozone cycle. Sudden stratospheric warming events (SSWs) manifest the strongest alteration of stratospheric dynamics. During SSWs, changes in planetary wave propagation vigorously influence zonal mean zonal wind, temperature, and tracer concentrations in the stratosphere over the high latitudes. In this study, we examine six persistent major SSWs from 2004 to 2020 using the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2). Using the unique density of observations around the Greenland sector at high latitudes, we perform comprehensive comparisons of high-latitude observations with the MERRA-2 ozone dataset during the six major SSWs. Our results show that MERRA-2 captures the high variability of mid-stratospheric ozone fluctuations during SSWs over high latitudes. However, larger uncertainties are observed in the lower stratosphere and troposphere. The zonally averaged stratospheric ozone shows a dramatic increase of 9 %–29 % in total column ozone (TCO) near the time of each SSW, which lasts up to 2 months. This study shows that the average shape of the Arctic polar vortex before SSWs influences the geographical extent, timing, and magnitude of ozone changes. The SSWs exhibit a more significant impact on ozone over high northern latitudes when the average polar vortex is mostly elongated as seen in 2009 and 2018 compared to the events in which the polar vortex is displaced towards Europe. Strong correlation (R2=90  %) is observed between the magnitude of change in average equivalent potential vorticity before and after SSWs and the associated averaged total column ozone changes over high latitudes. This paper investigates the different terms of the ozone continuity equation using MERRA-2 circulation, which emphasizes the key role of vertical advection in mid-stratospheric ozone during the SSWs and the magnified vertical advection in elongated vortex shape as seen in 2009 and 2018.
    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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  • 10
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 15, No. 6 ( 2022-03-28), p. 1849-1870
    Abstract: Abstract. The long-term record of Umkehr measurements from four NOAA Dobson spectrophotometers was reprocessed after updates to the instrument calibration procedures. In addition, a new data quality-control tool was developed for the Dobson automation software (WinDobson). This paper presents a comparison of Dobson Umkehr ozone profiles from NOAA ozone network stations – Boulder, the Haute-Provence Observatory (OHP), the Mauna Loa Observatory (MLO), Lauder – against several satellite records, including Aura Microwave Limb Sounder (MLS; ver. 4.2), and combined solar backscatter ultraviolet (SBUV) and Ozone Mapping and Profiler Suite (OMPS) records (NASA aggregated and NOAA cohesive datasets). A subset of satellite data is selected to match Dobson Umkehr observations at each station spatially (distance less than 200 km) and temporally (within 24 h). Umkehr Averaging kernels (AKs) are applied to vertically smooth all overpass satellite profiles prior to comparisons. The station Umkehr record consists of several instrumental records, which have different optical characterizations, and thus instrument-specific stray light contributes to the data processing errors and creates step changes in the record. This work evaluates the overall quality of Umkehr long-term measurements at NOAA ground-based stations and assesses the impact of the instrumental changes on the stability of the Umkehr ozone profile record. This paper describes a method designed to correct biases and discontinuities in the retrieved Umkehr profile that originate from the Dobson calibration process, repair, or optical realignment of the instrument. The Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2) Global Modeling Initiative (M2GMI) and NASA Global Modeling Initiative chemistry transport model (GMI CTM) ozone profile model output matched to station location and date of observation is used to evaluate instrumental step changes in the Umkehr record. Homogenization of the Umkehr record and discussion of the apparent stray light error in retrieved ozone profiles are the focus of this paper. Homogenization of ground-based records is of great importance for studies of long-term ozone trends and climate change.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2505596-3
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