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  • 1
    In: Remote Sensing, MDPI AG, Vol. 15, No. 1 ( 2022-12-21), p. 29-
    Abstract: In recent years (2017–2019), several moderate volcanic eruptions and wildfires have perturbed the stratospheric composition and concentration with distinct implications on radiative forcing and climate. The Stratospheric Aerosol and Gas Experiment III instruments onboard the International Space Station (SAGE III/ISS) have been providing aerosol extinction coefficient (EC) profiles at multiple wavelengths since June 2017. In this study, a method to invert the spectral stratospheric aerosol optical depth (sAOD) or EC values from SAGE III/ISS (to retrieve the number/volume size distributions and other microphysical properties) is presented, and the sensitivity of these retrievals is evaluated. It was found that the retrievals are strongly dependent on the choices of wavelengths, which in turn determine the shapes of the calculated curves. Further, we examine the changes in stratospheric aerosol spectral behavior, size distribution properties, time evolution (growth/decay) characteristics associated with subsequent moderate volcanic eruptions, namely, Ambae (15∘S, 167∘E; April and July 2018), Raikoke (48∘N, 153∘E; June 2019), and Ulawun (5∘S, 151∘E; June and August 2019), in different spatial regions. The observational period was classified with reference to Ambae eruptions into four phases (pre-Ambae, Ambae1, Ambae2, and post-Ambae). The pre-Ambae and post-Ambe periods comprise the 2017 Canadian fires and 2019 Raikoke/Ulawun eruptions, respectively. The spectral dependence of sAOD was comparable and lowest during the pre-Ambae and Ambae1 periods in all regions. The number concentration at the principal mode radius (between 0.07 and 0.2 μm) was observed to be higher during the Ambae2 period over the Northern Hemisphere (NH). The rate of change (growth/decay) in the sAOD on a global scale resembled the changes in the Southern Hemisphere (SH), unlike the time-lag-associated changes in the NH. These differences could be attributed to the prevailing horizontal and vertical dispersion mechanisms in the respective regions. Lastly, the radiative forcing estimates of Ambae and Raikoke/Ulawun eruptions, as reported in recent studies, was discussed by taking clues from other major and moderate eruptions to gain insight on their role in climate change.
    Type of Medium: Online Resource
    ISSN: 2072-4292
    Language: English
    Publisher: MDPI AG
    Publication Date: 2022
    detail.hit.zdb_id: 2513863-7
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  • 2
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 5 ( 2021-03-04), p. 3255-3274
    Abstract: Abstract. The StratoClim airborne campaign took place in Nepal from 27 July to 10 August 2017 to document the physical and chemical properties of the South Asian upper troposphere–lower stratosphere (UTLS) during the Asian summer monsoon (ASM). In the present paper, simulations with the Meso-NH cloud-chemistry model at a horizontal resolution of 15 km are performed over the Asian region to characterize the impact of monsoon deep convection on the composition of Asian monsoon anticyclone (AMA) and on the formation of the Asian tropopause aerosol layer (ATAL) during the StratoClim campaign. StratoClim took place during a break phase of the monsoon with intense convective activity over South China and Sichuan. Comparisons between brightness temperatures (BTs) at 10.8 µm observed by satellite sensors and simulated by Meso-NH highlight the ability of the model to correctly reproduce the life cycle of deep convective clouds. A comparison between CO and O3 concentrations from Meso-NH and airborne observations (StratoClim and IAGOS (In-service Aircraft for a Global Observing System)) demonstrates that the model captures most of the observed variabilities. Nevertheless, for both gases, the model tends to overestimate the concentrations and misses some thin CO plumes related to local convective events probably because the resolution is too coarse, but the convective uplift of pollution is very well captured by the model. We have therefore focused on the impact of Sichuan convection on the AMA composition. A dedicated sensitivity simulation showed that the 7 August convective event brought large amounts of CO deep into the AMA and even across the 380 K isentropic level located at 17.8 km. This Sichuan contribution enhanced the CO concentration by ∼15 % to reach more than 180 ppbv over a large area around 15 km height. It is noteworthy that Meso-NH captures the impact of the diluted Sichuan plume on the CO concentration during a StratoClim flight south of Kathmandu, highlighting its ability to reproduce the transport pathway of Sichuan pollution. According to the model, primary organic aerosol and black carbon particles originating from Sichuan are transported following the same pathway as CO. The large particles are heavily scavenged within the precipitating part of the convective clouds but remain the most important contributor to the particle mass in the AMA. Over the whole AMA region, the 7 August convective event resulted in a 0.5 % increase in CO concentration over the 10–20 km range that lasted about 2 d. The impact of pollution uplift from three regions (India, China, and Sichuan) averaged over the first 10 d of August has also been evaluated with sensitivity simulations. Even during this monsoon break phase, the results confirm the predominant role of India relative to China with respective contributions of 11 % and 7 % to CO concentration in the 10–15 km layer. Moreover, during this period a large part (35 %) of the Chinese contribution comes from the Sichuan Basin alone.
    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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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 2 ( 2021-01-29), p. 1267-1285
    Abstract: Abstract. Every year during the Asian summer monsoon season from about mid-June to early September, a stable anticyclonic circulation system forms over the Himalayas. This Asian summer monsoon (ASM) anticyclone has been shown to promote transport of air into the stratosphere from the Asian troposphere, which contains large amounts of anthropogenic pollutants. Essential details of Asian monsoon transport, such as the exact timescales of vertical transport, the role of convection in cross-tropopause exchange, and the main location and level of export from the confined anticyclone to the stratosphere are still not fully resolved. Recent airborne observations from campaigns near the ASM anticyclone edge and centre in 2016 and 2017, respectively, show a steady decrease in carbon monoxide (CO) and increase in ozone (O3) with height starting from tropospheric values of around 100 ppb CO and 30–50 ppb O3 at about 365 K potential temperature. CO mixing ratios reach stratospheric background values below ∼25 ppb at about 420 K and do not show a significant vertical gradient at higher levels, while ozone continues to increase throughout the altitude range of the aircraft measurements. Nitrous oxide (N2O) remains at or only marginally below its 2017 tropospheric mixing ratio of 333 ppb up to about 400 K, which is above the local tropopause. A decline in N2O mixing ratios that indicates a significant contribution of stratospheric air is only visible above this level. Based on our observations, we draw the following picture of vertical transport and confinement in the ASM anticyclone: rapid convective uplift transports air to near 16 km in altitude, corresponding to potential temperatures up to about 370 K. Although this main convective outflow layer extends above the level of zero radiative heating (LZRH), our observations of CO concentration show little to no evidence of convection actually penetrating the tropopause. Rather, further ascent occurs more slowly, consistent with isentropic vertical velocities of 0.7–1.5 K d−1. For the key tracers (CO, O3, and N2O) in our study, none of which are subject to microphysical processes, neither the lapse rate tropopause (LRT) around 380 K nor the cold point tropopause (CPT) around 390 K marks a strong discontinuity in their profiles. Up to about 20 to 35 K above the LRT, isolation of air inside the ASM anticyclone prevents significant in-mixing of stratospheric air (throughout this text, the term in-mixing refers specifically to mixing processes that introduce stratospheric air into the predominantly tropospheric inner anticyclone). The observed changes in CO and O3 likely result from in situ chemical processing. Above about 420 K, mixing processes become more significant and the air inside the anticyclone is exported vertically and horizontally into the surrounding stratosphere.
    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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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 21 ( 2019-11-07), p. 13547-13567
    Abstract: Abstract. We show that a fire plume injected into the lower stratosphere at high northern latitudes during the Canadian wildfire event in August 2017 partly reached the tropics. The transport to the tropics was mediated by the anticyclonic flow of the Asian monsoon circulation. The fire plume reached the Asian monsoon area in late August/early September, when the Asian monsoon anticyclone (AMA) was still in place. While there is no evidence of mixing into the center of the AMA, we show that a substantial part of the fire plume is entrained into the anticyclonic flow at the AMA edge and is transported from the extratropics to the tropics, and possibly the Southern Hemisphere particularly following the north–south flow on the eastern side of the AMA. In the tropics the fire plume is lifted by ∼5 km in 7 months. Inside the AMA we find evidence of the Asian tropopause aerosol layer (ATAL) in August, doubling background aerosol conditions with a calculated top of the atmosphere shortwave radiative forcing of −0.05 W m−2. The regional climate impact of the fire signal in the wider Asian monsoon area in September exceeds the impact of the ATAL by a factor of 2–4 and compares to that of a plume coming from an advected moderate volcanic eruption. The stratospheric, trans-continental transport of this plume to the tropics and the related regional climate impact point to the importance of long-range dynamical interconnections of pollution sources.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 5
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 15, No. 19 ( 2022-10-10), p. 7471-7487
    Abstract: Abstract. Pure Lagrangian, i.e., trajectory-based transport models, take into account only the resolved advective part of transport. That means neither mixing processes between the air parcels (APs) nor unresolved subgrid-scale advective processes like convection are included. The Chemical Lagrangian Model of the Stratosphere (CLaMS 1.0) extends this approach by including mixing between the Lagrangian APs parameterizing the small-scale isentropic mixing. To improve model representation of the upper troposphere and lower stratosphere (UTLS), this approach was extended by taking into account parameterization of tropospheric mixing and unresolved convection in the recently published CLaMS 2.0 version. All three transport modes, i.e., isentropic and tropospheric mixing and the unresolved convection can be adjusted and optimized within the model. Here, we investigate the sensitivity of the model representation of tracers in the UTLS with respect to these three modes. For this reason, the CLaMS 2.0 version implemented within the Modular Earth Submodel System (MESSy), CLaMS 2.0/MESSy, is applied with meteorology based on the ERA-Interim (EI) and ERA5 (E5) reanalyses with the same horizontal resolution (1.0×1.0∘) but with 60 and 137 model levels for EI and E5, respectively. Comparisons with in situ observations are used to rate the degree of agreement between different model configurations and observations. Starting from pure advective runs as a reference and in agreement with CLaMS 1.0, we show that among the three processes considered, isentropic mixing dominates transport in the UTLS. Both the observed CO, O3, N2O, and CO2 profiles and CO–O3 correlations are clearly better reproduced in the model with isentropic mixing. The second most important transport process considered is convection which is only partially resolved in the vertical velocity fields provided by the analysis. This additional pathway of transport from the planetary boundary layer (PBL) to the main convective outflow dominates the composition of air in the lower stratosphere relative to the contribution of the resolved transport. This transport happens mainly in the tropics and sub-tropics, and significantly rejuvenates the age of air in this region. By taking into account tropospheric mixing, weakest changes in tracer distributions without any clear improvements were found.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2456725-5
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  • 6
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 1 ( 2017-01-10), p. 385-402
    Abstract: Abstract. The climate active trace-gas carbonyl sulfide (OCS) is the most abundant sulfur gas in the atmosphere. A missing source in its atmospheric budget is currently suggested, resulting from an upward revision of the vegetation sink. Tropical oceanic emissions have been proposed to close the resulting gap in the atmospheric budget. We present a bottom-up approach including (i) new observations of OCS in surface waters of the tropical Atlantic, Pacific and Indian oceans and (ii) a further improved global box model to show that direct OCS emissions are unlikely to account for the missing source. The box model suggests an undersaturation of the surface water with respect to OCS integrated over the entire tropical ocean area and, further, global annual direct emissions of OCS well below that suggested by top-down estimates. In addition, we discuss the potential of indirect emission from CS2 and dimethylsulfide (DMS) to account for the gap in the atmospheric budget. This bottom-up estimate of oceanic emissions has implications for using OCS as a proxy for global terrestrial CO2 uptake, which is currently impeded by the inadequate quantification of atmospheric OCS sources and sinks.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 7
    In: Atmosphere, MDPI AG, Vol. 5, No. 2 ( 2014-06-04), p. 420-434
    Type of Medium: Online Resource
    ISSN: 2073-4433
    Language: English
    Publisher: MDPI AG
    Publication Date: 2014
    detail.hit.zdb_id: 2605928-9
    SSG: 23
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  • 8
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 12, No. 4 ( 2019-04-08), p. 2129-2138
    Abstract: Abstract. When computing climatological averages of atmospheric trace-gas mixing ratios obtained from satellite-based measurements, sampling biases arise if data coverage is not uniform in space and time. Homogeneous spatiotemporal coverage is essentially impossible to achieve. Solar occultation measurements, by virtue of satellite orbit and the requirement of direct observation of the sun through the atmosphere, result in particularly sparse spatial coverage. In this proof-of-concept study, a method is presented to adjust for such sampling biases when calculating climatological means. The method is demonstrated using carbonyl sulfide (OCS) measurements at 16 km altitude from the ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer). At this altitude, OCS mixing ratios show a steep gradient between the poles and Equator. ACE-FTS measurements, which are provided as vertically resolved profiles, and integrated stratospheric OCS columns are used in this study. The bias adjustment procedure requires no additional information other than the satellite data product itself. In particular, the method does not rely on atmospheric models with potentially unreliable transport or chemistry parameterizations, and the results can be used uncompromised to test and validate such models. It is expected to be generally applicable when constructing climatologies of long-lived tracers from sparsely and heterogeneously sampled satellite measurements. In the first step of the adjustment procedure, a regression model is used to fit a 2-D surface to all available ACE-FTS OCS measurements as a function of day-of-year and latitude. The regression model fit is used to calculate an adjustment factor that is then used to adjust each measurement individually. The mean of the adjusted measurement points of a chosen latitude range and season is then used as the bias-free climatological value. When applying the adjustment factor to seasonal averages in 30∘ zones, the maximum spatiotemporal sampling bias adjustment was 11 % for OCS mixing ratios at 16 km and 5 % for the stratospheric OCS column. The adjustments were validated against the much denser and more homogeneous OCS data product from the limb-sounding MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) instrument, and both the direction and magnitude of the adjustments were in agreement with the adjustment of the ACE-FTS data.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2505596-3
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  • 9
    In: Remote Sensing, MDPI AG, Vol. 13, No. 16 ( 2021-08-05), p. 3092-
    Abstract: The present study contributes to the scientific effort for a better understanding of the potential of the Australian biomass burning events to influence tropospheric trace gas abundances at the regional scale. In order to exclude the influence of the long-range transport of ozone precursors from biomass burning plumes originating from Southern America and Africa, the analysis of the Australian smoke plume has been driven over the period December 2019 to January 2020. This study uses satellite (IASI, MLS, MODIS, CALIOP) and ground-based (sun-photometer, FTIR, ozone radiosondes) observations. The highest values of aerosol optical depth (AOD) and carbon monoxide total columns are observed over Southern and Central Australia. Transport is responsible for the spatial and temporal distributions of aerosols and carbon monoxide over Australia, and also the transport of the smoke plume outside the continent. The dispersion of the tropospheric smoke plume over Oceania and Southern Pacific extends from tropical to extratropical latitudes. Ozone radiosonde measurements performed at Samoa (14.4°S, 170.6°W) and Lauder (45.0°S, 169.4°E) indicate an increase in mid-tropospheric ozone (6–9 km) (from 10% to 43%) linked to the Australian biomass burning plume. This increase in mid-tropospheric ozone induced by the transport of the smoke plume was found to be consistent with MLS observations over the tropical and extratropical latitudes. The smoke plume over the Southern Pacific was organized as a stretchable anticyclonic rolling which impacted the ozone variability in the tropical and subtropical upper-troposphere over Oceania. This is corroborated by the ozone profile measurements at Samoa which exhibit an enhanced ozone layer (29%) in the upper-troposphere. Our results suggest that the transport of Australian biomass burning plumes have significantly impacted the vertical distribution of ozone in the mid-troposphere southern tropical to extratropical latitudes during the 2019–20 extreme Australian bushfires.
    Type of Medium: Online Resource
    ISSN: 2072-4292
    Language: English
    Publisher: MDPI AG
    Publication Date: 2021
    detail.hit.zdb_id: 2513863-7
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  • 10
    Online Resource
    Online Resource
    Frontiers Media SA ; 2021
    In:  Frontiers in Environmental Science Vol. 9 ( 2021-7-8)
    In: Frontiers in Environmental Science, Frontiers Media SA, Vol. 9 ( 2021-7-8)
    Abstract: The historically large and severe wildfires in Australia from September 2019 to March 2020 are known to have injected a smoke plume into the stratosphere around New Year, due to pyro-cumulonimbus (pyro-Cb) activity, that was subsequently distributed throughout the Southern Hemisphere (SH). We show with satellite, ground based remote sensing, and in situ observations that the fires before New Year, had already a substantial impact on the SH atmosphere, starting as early as September 2019, with subsequent long-range transport of trace gas plumes in the upper-troposphere. Airborne in situ measurements above Southern Argentina in November 2019 show elevated CO mixing ratios at an altitude of 11 km and can be traced back using FLEXPART trajectories to the Australian fires in mid-November 2019. Ground based solar-FTS (Fourier Transform Spectroscopy) observations of biomass burning tracers CO, HCN and C 2 H 6 at Lauder, South Island, New Zealand show enhanced tropospheric columns already starting in September 2019. In MLS observations averaged over 30°–60°S, enhanced CO mixing ratios compared to previous years become visible in late October 2019 only at and below the 147 hPa pressure level. Peak differences are found with satellite and ground-based observations for all altitude levels in the Southern Hemisphere in January. With still increased aerosol values following the Ulawun eruption in 2019, averaged satellite observations show no clear stratospheric and upper-tropospheric aerosol enhancements from the Australian fires, before the pyro-Cb events at the end of December 2019. However, with the clear enhancement of fire tracers, we suggest the period September to December 2019 (prior to the major pyro-Cb events) should be taken into account in terms of fire pollutant emissions when studying the impact of the Australian fires on the SH atmosphere.
    Type of Medium: Online Resource
    ISSN: 2296-665X
    Language: Unknown
    Publisher: Frontiers Media SA
    Publication Date: 2021
    detail.hit.zdb_id: 2741535-1
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