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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
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  • 2
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 17 ( 2020-09-11), p. 10611-10635
    Abstract: Abstract. Ozone is a key constituent of the troposphere, where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom; four deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; five deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific and Atlantic basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the atmosphere over the Pacific and ATom sampling both the Pacific and Atlantic. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53 %, 54 %, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere–lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles from these two campaigns to confirm and extend the existing knowledge of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the Northern Hemisphere, consistent with greater precursor emissions and consistent with previous modeling and satellite studies. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins, likely due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic as in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. Finally, we show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven year-round by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset provides additional constraints for global climate and chemistry models to improve our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 5 ( 2021-03-18), p. 4187-4218
    Abstract: Abstract. The evolution of tropospheric ozone from 1850 to 2100 has been studied using data from Phase 6 of the Coupled Model Intercomparison Project (CMIP6). We evaluate long-term changes using coupled atmosphere–ocean chemistry–climate models, focusing on the CMIP Historical and ScenarioMIP ssp370 experiments, for which detailed tropospheric-ozone diagnostics were archived. The model ensemble has been evaluated against a suite of surface, sonde and satellite observations of the past several decades and found to reproduce well the salient spatial, seasonal and decadal variability and trends. The multi-model mean tropospheric-ozone burden increases from 247 ± 36 Tg in 1850 to a mean value of 356 ± 31 Tg for the period 2005–2014, an increase of 44 %. Modelled present-day values agree well with previous determinations (ACCENT: 336 ± 27 Tg; Atmospheric Chemistry and Climate Model Intercomparison Project, ACCMIP: 337 ± 23 Tg; Tropospheric Ozone Assessment Report, TOAR: 340 ± 34 Tg). In the ssp370 experiments, the ozone burden increases to 416 ± 35 Tg by 2100. The ozone budget has been examined over the same period using lumped ozone production (PO3) and loss (LO3) diagnostics. Both ozone production and chemical loss terms increase steadily over the period 1850 to 2100, with net chemical production (PO3-LO3) reaching a maximum around the year 2000. The residual term, which contains contributions from stratosphere–troposphere transport reaches a minimum around the same time before recovering in the 21st century, while dry deposition increases steadily over the period 1850–2100. Differences between the model residual terms are explained in terms of variation in tropopause height and stratospheric ozone burden.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 4
    Online Resource
    Online Resource
    Copernicus GmbH ; 2021
    In:  Atmospheric Chemistry and Physics Vol. 21, No. 20 ( 2021-10-22), p. 15771-15781
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 20 ( 2021-10-22), p. 15771-15781
    Abstract: Abstract. Without the Montreal Protocol, the already extreme Arctic ozone losses in the boreal spring of 2020 would be expected to have produced an Antarctic-like ozone hole, based upon simulations performed using the specified dynamics version of the Whole Atmosphere Community Climate Model (SD-WACCM) and using an alternate emission scenario of 3.5 % growth in ozone-depleting substances from 1985 onwards. In particular, we find that the area of total ozone below 220 DU (Dobson units), a standard metric of Antarctic ozone hole size, would have covered about 20 million km2. Record observed local lows of 0.1 ppmv (parts per million by volume) at some altitudes in the lower stratosphere seen by ozonesondes in March 2020 would have reached 0.01, again similar to the Antarctic. Spring ozone depletion would have begun earlier and lasted longer without the Montreal Protocol, and by 2020, the year-round ozone depletion would have begun to dramatically diverge from the observed case. This extreme year also provides an opportunity to test parameterizations of polar stratospheric cloud impacts on denitrification and, thereby, to improve stratospheric models of both the real world and alternate scenarios. In particular, we find that decreasing the parameterized nitric acid trihydrate number density in SD-WACCM, which subsequently increases denitrification, improves the agreement with observations for both nitric acid and ozone. This study reinforces that the historically extreme 2020 Arctic ozone depletion is not cause for concern over the Montreal Protocol's effectiveness but rather demonstrates that the Montreal Protocol indeed merits celebration for avoiding an Arctic ozone hole.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 2 ( 2018-01-22), p. 773-798
    Abstract: Abstract. Inter-annual variability and long-term trends in tropospheric ozone are both environmental and climate concerns. Ozone measured at Mt Waliguan Observatory (WLG, 3816 m a.s.l.) on the Tibetan Plateau over the period of 1994–2013 has increased significantly by 0.2–0.3 ppbv yr−1 during spring and autumn but shows a much smaller trend in winter and no significant trend in summer. Here we explore the factors driving the observed ozone changes at WLG using backward trajectory analysis, chemistry–climate model hindcast simulations (GFDL AM3), a trajectory-mapped ozonesonde data set, and several climate indices. A stratospheric ozone tracer implemented in GFDL AM3 indicates that stratosphere-to-troposphere transport (STT) can explain ∼ 60 % of the simulated springtime ozone increase at WLG, consistent with an increase in the NW air-mass frequency inferred from the trajectory analysis. Enhanced STT associated with the strengthening of the mid-latitude jet stream contributes to the observed high ozone anomalies at WLG during the springs of 1999 and 2012. During autumn, observations at WLG are more heavily influenced by polluted air masses originating from South East Asia than in the other seasons. Rising Asian anthropogenic emissions of ozone precursors are the key driver of increasing autumnal ozone observed at WLG, as supported by the GFDL AM3 model with time-varying emissions, which captures the observed ozone increase (0.26 ± 0.11 ppbv yr−1). AM3 simulates a greater ozone increase of 0.38 ± 0.11 ppbv yr−1 at WLG in autumn under conditions with strong transport from South East Asia and shows no significant ozone trend in autumn when anthropogenic emissions are held constant in time. During summer, WLG is mostly influenced by easterly air masses, but these trajectories do not extend to the polluted regions of eastern China and have decreased significantly over the last 2 decades, which likely explains why summertime ozone measured at WLG shows no significant trend despite ozone increases in eastern China. Analysis of the Trajectory-mapped Ozonesonde data set for the Stratosphere and Troposphere (TOST) and trajectory residence time reveals increases in direct ozone transport from the eastern sector during autumn, which adds to the autumnal ozone increase. We further examine the links of ozone variability at WLG to the quasi-biennial oscillation (QBO), the East Asian summer monsoon (EASM), and the sunspot cycle. Our results suggest that the 2–3-, 3–7-, and 11-year periodicities are linked to the QBO, EASM index, and sunspot cycle, respectively. A multivariate regression analysis is performed to quantify the relative contributions of various factors to surface ozone concentrations at WLG. Through an observational and modelling analysis, this study demonstrates the complex relationships between surface ozone at remote locations and its dynamical and chemical influencing factors.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 6
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 9, No. 6 ( 2016-06-08), p. 2497-2534
    Abstract: Abstract. The ozone profile records of a large number of limb and occultation satellite instruments are widely used to address several key questions in ozone research. Further progress in some domains depends on a more detailed understanding of these data sets, especially of their long-term stability and their mutual consistency. To this end, we made a systematic assessment of 14 limb and occultation sounders that, together, provide more than three decades of global ozone profile measurements. In particular, we considered the latest operational Level-2 records by SAGE II, SAGE III, HALOE, UARS MLS, Aura MLS, POAM II, POAM III, OSIRIS, SMR, GOMOS, MIPAS, SCIAMACHY, ACE-FTS and MAESTRO. Central to our work is a consistent and robust analysis of the comparisons against the ground-based ozonesonde and stratospheric ozone lidar networks. It allowed us to investigate, from the troposphere up to the stratopause, the following main aspects of satellite data quality: long-term stability, overall bias and short-term variability, together with their dependence on geophysical parameters and profile representation. In addition, it permitted us to quantify the overall consistency between the ozone profilers. Generally, we found that between 20 and 40 km the satellite ozone measurement biases are smaller than ±5 %, the short-term variabilities are less than 5–12 % and the drifts are at most ±5 % decade−1 (or even ±3 % decade−1 for a few records). The agreement with ground-based data degrades somewhat towards the stratopause and especially towards the tropopause where natural variability and low ozone abundances impede a more precise analysis. In part of the stratosphere a few records deviate from the preceding general conclusions; we identified biases of 10 % and more (POAM II and SCIAMACHY), markedly higher single-profile variability (SMR and SCIAMACHY) and significant long-term drifts (SCIAMACHY, OSIRIS, HALOE and possibly GOMOS and SMR as well). Furthermore, we reflected on the repercussions of our findings for the construction, analysis and interpretation of merged data records. Most notably, the discrepancies between several recent ozone profile trend assessments can be mostly explained by instrumental drift. This clearly demonstrates the need for systematic comprehensive multi-instrument comparison analyses.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
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  • 7
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 10, No. 7 ( 2017-07-13), p. 2455-2475
    Abstract: Abstract. We validate the Ozone Monitoring Instrument (OMI) Ozone Profile (PROFOZ) product from October 2004 through December 2014 retrieved by the Smithsonian Astrophysical Observatory (SAO) algorithm against ozonesonde observations. We also evaluate the effects of OMI row anomaly (RA) on the retrieval by dividing the dataset into before and after the occurrence of serious OMI RA, i.e., pre-RA (2004–2008) and post-RA (2009–2014). The retrieval shows good agreement with ozonesondes in the tropics and midlatitudes and for pressure  〈 ∼ 50 hPa in the high latitudes. It demonstrates clear improvement over the a priori down to the lower troposphere in the tropics and down to an average of ∼ 550 (300) hPa at middle (high) latitudes. In the tropics and midlatitudes, the profile mean biases (MBs) are less than 6 %, and the standard deviations (SDs) range from 5 to 10 % for pressure  〈 ∼ 50 hPa to less than 18 % (27 %) in the tropics (midlatitudes) for pressure  〉 ∼ 50 hPa after applying OMI averaging kernels to ozonesonde data. The MBs of the stratospheric ozone column (SOC, the ozone column from the tropopause pressure to the ozonesonde burst pressure) are within 2 % with SDs of  〈 5 % and the MBs of the tropospheric ozone column (TOC) are within 6 % with SDs of 15 %. In the high latitudes, the profile MBs are within 10 % with SDs of 5–15 % for pressure  〈 ∼ 50 hPa but increase to 30 % with SDs as great as 40 % for pressure  〉 ∼ 50 hPa. The SOC MBs increase up to 3 % with SDs as great as 6 % and the TOC SDs increase up to 30 %. The comparison generally degrades at larger solar zenith angles (SZA) due to weaker signals and additional sources of error, leading to worse performance at high latitudes and during the midlatitude winter. Agreement also degrades with increasing cloudiness for pressure  〉 ∼ 100 hPa and varies with cross-track position, especially with large MBs and SDs at extreme off-nadir positions. In the tropics and midlatitudes, the post-RA comparison is considerably worse with larger SDs reaching 2 % in the stratosphere and 8 % in the troposphere and up to 6 % in TOC. There are systematic differences that vary with latitude compared to the pre-RA comparison. The retrieval comparison demonstrates good long-term stability during the pre-RA period but exhibits a statistically significant trend of 0.14–0.7 % year−1 for pressure  〈 ∼ 80 hPa, 0.7 DU year−1 in SOC, and −0. 33 DU year−1 in TOC during the post-RA period. The spatiotemporal variation of retrieval performance suggests the need to improve OMI's radiometric calibration especially during the post-RA period to maintain the long-term stability and reduce the latitude/season/SZA and cross-track dependency of retrieval quality.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 15 ( 2019-08-02), p. 9733-9751
    Abstract: Abstract. Understanding variations in atmospheric ozone in the Arctic is difficult because there are only a few long-term records of vertical ozone profiles in this region. We present 12 years of ozone profiles from February 2005 to February 2017 at four sites: Summit Station, Greenland; Ny-Ålesund, Svalbard, Norway; and Alert and Eureka, Nunavut, Canada. These profiles are created by combining ozonesonde measurements with ozone profile retrievals using data from the Microwave Limb Sounder (MLS). This combination creates a high-quality dataset with low uncertainty values by relying on in situ measurements of the maximum altitude of the ozonesondes (∼30 km) and satellite retrievals in the upper atmosphere (up to 60 km). For each station, the total column ozone (TCO) and the partial column ozone (PCO) in four atmospheric layers (troposphere to upper stratosphere) are analyzed. Overall, the seasonal cycles are similar at these sites. However, the TCO over Ny-Ålesund starts to decline 2 months later than at the other sites. In summer, the PCO in the upper stratosphere over Summit Station is slightly higher than at the other sites and exhibits a higher standard deviation. The decrease in PCO in the middle and upper stratosphere during fall is also lower over Summit Station. The maximum value of the lower- and middle-stratospheric PCO is reached earlier in the year over Eureka. Trend analysis over the 12-year period shows significant trends in most of the layers over Summit and Ny-Ålesund during summer and fall. To understand deseasonalized ozone variations, we identify the most important dynamical drivers of Arctic ozone at each level. These drivers are chosen based on mutual selected proxies at the four sites using stepwise multiple regression (SMR) analysis of various dynamical parameters with deseasonalized data. The final regression model is able to explain more than 80 % of the TCO and more than 70 % of the PCO in almost all of the layers. The regression model provides the greatest explanatory value in the middle stratosphere. The important proxies of the deseasonalized ozone time series at the four sites are tropopause pressure (TP) and equivalent latitude (EQL) at 370 K in the troposphere, the quasi-biennial oscillation (QBO) in the troposphere and lower stratosphere, the equivalent latitude at 550 K in the middle and upper stratosphere, and the eddy heat flux (EHF) and volume of polar stratospheric clouds throughout the stratosphere.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
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  • 9
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 9 ( 2017-05-10), p. 5775-5788
    Abstract: Abstract. Rapidly rising temperatures and loss of snow and ice cover have demonstrated the unique vulnerability of the high Arctic to climate change. There are major uncertainties in modelling the chemical depositional and scavenging processes of Arctic snow. To that end, fresh snow samples collected on average every 4 days at Alert, Nunavut, from September 2014 to June 2015 were analyzed for black carbon, major ions, and metals, and their concentrations and fluxes were reported. Comparison with simultaneous measurements of atmospheric aerosol mass loadings yields effective deposition velocities that encompass all processes by which the atmospheric species are transferred to the snow. It is inferred from these values that dry deposition is the dominant removal mechanism for several compounds over the winter while wet deposition increased in importance in the fall and spring, possibly due to enhanced scavenging by mixed-phase clouds. Black carbon aerosol was the least efficiently deposited species to the snow.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 10
    Online Resource
    Online Resource
    Copernicus GmbH ; 2019
    In:  Atmospheric Measurement Techniques Vol. 12, No. 1 ( 2019-01-18), p. 327-343
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 12, No. 1 ( 2019-01-18), p. 327-343
    Abstract: Abstract. Dobson and Brewer spectrophotometers are the primary, standard instruments for ground-based ozone measurements under the World Meteorological Organization's (WMO) Global Atmosphere Watch program. The accuracy of the data retrieval for both instruments depends on a knowledge of the ozone absorption coefficients and some assumptions underlying the data analysis. Instrumental stray light causes nonlinearity in the response of both the Brewer and Dobson to ozone at large ozone slant paths. In addition, it affects the effective ozone absorption coefficients and extraterrestrial constants that are both instrument-dependent. This effect has not been taken into account in the calculation of ozone absorption coefficients that are currently recommended by WMO for the Dobson network. The ozone absorption coefficients are calculated for each Brewer instrument individually, but in the current procedure the effect of stray light is not considered. This study documents the error caused by the effect of stray light in the Brewer and Dobson total ozone measurements using a physical model for each instrument. For the first time, new ozone absorption coefficients are calculated for the Brewer and Dobson instruments, taking into account the stray light effect. The analyses show that the differences detected between the total ozone amounts deduced from Dobson AD and CD pair wavelengths are related to the level of stray light within the instrument. The discrepancy introduced by the assumption of a fixed height for the ozone layer for ozone measurements at high latitude sites is also evaluated. The ozone data collected by two Dobson instruments during the period of December 2008 to December 2014 are compared with ozone data from a collocated double monochromator Brewer spectrophotometer (Mark III). The results illustrate the dependence of Dobson AD and CD pair measurements on stray light.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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