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  • 1
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 6, No. 5 ( 2013-05-02), p. 1111-1140
    Abstract: Abstract. The detection of atmospheric NO3 radicals is still challenging owing to its low mixing ratios (≈ 1 to 300 pptv) in the troposphere. While long-path differential optical absorption spectroscopy (DOAS) has been a well-established NO3 detection approach for over 25 yr, newly sensitive techniques have been developed in the past decade. This publication outlines the results of the first comprehensive intercomparison of seven instruments developed for the spectroscopic detection of tropospheric NO3. Four instruments were based on cavity ring-down spectroscopy (CRDS), two utilised open-path cavity-enhanced absorption spectroscopy (CEAS), and one applied "classical" long-path DOAS. The intercomparison campaign "NO3Comp" was held at the atmosphere simulation chamber SAPHIR in Jülich (Germany) in June 2007. Twelve experiments were performed in the well-mixed chamber for variable concentrations of NO3, N2O5, NO2, hydrocarbons, and water vapour, in the absence and in the presence of inorganic or organic aerosol. The overall precision of the cavity instruments varied between 0.5 and 5 pptv for integration times of 1 s to 5 min; that of the DOAS instrument was 9 pptv for an acquisition time of 1 min. The NO3 data of all instruments correlated excellently with the NOAA-CRDS instrument, which was selected as the common reference because of its superb sensitivity, high time resolution, and most comprehensive data coverage. The median of the coefficient of determination (r2) over all experiments of the campaign (60 correlations) is r2 = 0.981 (quartile 1 (Q1): 0.949; quartile 3 (Q3): 0.994; min/max: 0.540/0.999). The linear regression analysis of the campaign data set yielded very small intercepts (median: 1.1 pptv; Q1/Q3: −1.1/2.6 pptv; min/max: −14.1/28.0 pptv), and the slopes of the regression lines were close to unity (median: 1.01; Q1/Q3: 0.92/1.10; min/max: 0.72/1.36). The deviation of individual regression slopes from unity was always within the combined accuracies of each instrument pair. The very good correspondence between the NO3 measurements by all instruments for aerosol-free experiments indicates that the losses of NO3 in the inlet of the instruments were determined reliably by the participants for the corresponding conditions. In the presence of inorganic or organic aerosol, however, differences in the measured NO3 mixing ratios were detectable among the instruments. In individual experiments the discrepancies increased with time, pointing to additional NO3 radical losses by aerosol deposited onto the filters or on the inlet walls of the instruments. Instruments using DOAS analyses showed no significant effect of aerosol on the detection of NO3. No hint of a cross interference of NO2 was found. The effect of non-Lambert–Beer behaviour of water vapour absorption lines on the accuracy of the NO3 detection by broadband techniques was small and well controlled. The NO3Comp campaign demonstrated the high quality, reliability and robustness of performance of current state-of-the-art instrumentation for NO3 detection.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2013
    detail.hit.zdb_id: 2505596-3
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  • 2
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 3, No. 1 ( 2010-01-12), p. 21-37
    Abstract: Abstract. NO2 concentrations were measured by various instruments during the NO3Comp campaign at the atmosphere simulation chamber SAPHIR at Forschungszentrum Jülich, Germany, in June 2007. Analytical methods included photolytic conversion with chemiluminescence (PC-CLD), broadband cavity ring-down spectroscopy (BBCRDS), pulsed cavity ring-down spectroscopy (CRDS), incoherent broadband cavity-enhanced absorption spectroscopy (IBB\\-CEAS), and laser-induced fluorescence (LIF). All broadband absorption spectrometers were optimized for the detection of the main target species of the campaign, NO3, but were also capable of detecting NO2 simultaneously with reduced sensitivity. NO2 mixing ratios in the chamber were within a range characteristic of polluted, urban conditions, with a maximum mixing ratio of approximately 75 ppbv. The overall agreement between measurements of all instruments was excellent. Linear fits of the combined data sets resulted in slopes that differ from unity only within the stated uncertainty of each instrument. Possible interferences from species such as water vapor and ozone were negligible under the experimental conditions.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2010
    detail.hit.zdb_id: 2505596-3
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  • 3
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 8, No. 2 ( 2015-02-03), p. 129-150
    Abstract: Abstract. Representation of atmospheric transport is a major source of error in the estimation of greenhouse gas sources and sinks by inverse modelling. Here we assess the impact on trace gas mole fractions of the new physical parameterizations recently implemented in the atmospheric global climate model LMDz to improve vertical diffusion, mesoscale mixing by thermal plumes in the planetary boundary layer (PBL), and deep convection in the troposphere. At the same time, the horizontal and vertical resolution of the model used in the inverse system has been increased. The aim of this paper is to evaluate the impact of these developments on the representation of trace gas transport and chemistry, and to anticipate the implications for inversions of greenhouse gas emissions using such an updated model. Comparison of a one-dimensional version of LMDz with large eddy simulations shows that the thermal scheme simulates shallow convective tracer transport in the PBL over land very efficiently, and much better than previous versions of the model. This result is confirmed in three-dimensional simulations, by a much improved reproduction of the radon-222 diurnal cycle. However, the enhanced dynamics of tracer concentrations induces a stronger sensitivity of the new LMDz configuration to external meteorological forcings. At larger scales, the inter-hemispheric exchange is slightly slower when using the new version of the model, bringing them closer to observations. The increase in the vertical resolution (from 19 to 39 layers) significantly improves the representation of stratosphere/troposphere exchange. Furthermore, changes in atmospheric thermodynamic variables, such as temperature, due to changes in the PBL mixing modify chemical reaction rates, which perturb chemical equilibriums of reactive trace gases. One implication of LMDz model developments for future inversions of greenhouse gas emissions is the ability of the updated system to assimilate a larger amount of high-frequency data sampled at high-variability stations. Others implications are discussed at the end of the paper.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2015
    detail.hit.zdb_id: 2456725-5
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  • 4
    In: Climate of the Past, Copernicus GmbH, Vol. 13, No. 11 ( 2017-11-10), p. 1491-1513
    Abstract: Abstract. Here we present Antarctic snow accumulation variability at the regional scale over the past 1000 years. A total of 79 ice core snow accumulation records were gathered and assigned to seven geographical regions, separating the high-accumulation coastal zones below 2000 m of elevation from the dry central Antarctic Plateau. The regional composites of annual snow accumulation were evaluated against modelled surface mass balance (SMB) from RACMO2.3p2 and precipitation from ERA-Interim reanalysis. With the exception of the Weddell Sea coast, the low-elevation composites capture the regional precipitation and SMB variability as defined by the models. The central Antarctic sites lack coherency and either do not represent regional precipitation or indicate the model inability to capture relevant precipitation processes in the cold, dry central plateau. Our results show that SMB for the total Antarctic Ice Sheet (including ice shelves) has increased at a rate of 7 ± 0.13 Gt decade−1 since 1800 AD, representing a net reduction in sea level of ∼ 0.02 mm decade−1 since 1800 and ∼ 0.04 mm decade−1 since 1900 AD. The largest contribution is from the Antarctic Peninsula (∼ 75 %) where the annual average SMB during the most recent decade (2001–2010) is 123 ± 44 Gt yr−1 higher than the annual average during the first decade of the 19th century. Only four ice core records cover the full 1000 years, and they suggest a decrease in snow accumulation during this period. However, our study emphasizes the importance of low-elevation coastal zones, which have been under-represented in previous investigations of temporal snow accumulation.
    Type of Medium: Online Resource
    ISSN: 1814-9332
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2217985-9
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  • 5
    In: Climate of the Past, Copernicus GmbH, Vol. 9, No. 3 ( 2013-05-16), p. 1111-1140
    Abstract: Abstract. Both historical and idealized climate model experiments are performed with a variety of Earth system models of intermediate complexity (EMICs) as part of a community contribution to the Intergovernmental Panel on Climate Change Fifth Assessment Report. Historical simulations start at 850 CE and continue through to 2005. The standard simulations include changes in forcing from solar luminosity, Earth's orbital configuration, CO2, additional greenhouse gases, land use, and sulphate and volcanic aerosols. In spite of very different modelled pre-industrial global surface air temperatures, overall 20th century trends in surface air temperature and carbon uptake are reasonably well simulated when compared to observed trends. Land carbon fluxes show much more variation between models than ocean carbon fluxes, and recent land fluxes appear to be slightly underestimated. It is possible that recent modelled climate trends or climate–carbon feedbacks are overestimated resulting in too much land carbon loss or that carbon uptake due to CO2 and/or nitrogen fertilization is underestimated. Several one thousand year long, idealized, 2 × and 4 × CO2 experiments are used to quantify standard model characteristics, including transient and equilibrium climate sensitivities, and climate–carbon feedbacks. The values from EMICs generally fall within the range given by general circulation models. Seven additional historical simulations, each including a single specified forcing, are used to assess the contributions of different climate forcings to the overall climate and carbon cycle response. The response of surface air temperature is the linear sum of the individual forcings, while the carbon cycle response shows a non-linear interaction between land-use change and CO2 forcings for some models. Finally, the preindustrial portions of the last millennium simulations are used to assess historical model carbon-climate feedbacks. Given the specified forcing, there is a tendency for the EMICs to underestimate the drop in surface air temperature and CO2 between the Medieval Climate Anomaly and the Little Ice Age estimated from palaeoclimate reconstructions. This in turn could be a result of unforced variability within the climate system, uncertainty in the reconstructions of temperature and CO2, errors in the reconstructions of forcing used to drive the models, or the incomplete representation of certain processes within the models. Given the forcing datasets used in this study, the models calculate significant land-use emissions over the pre-industrial period. This implies that land-use emissions might need to be taken into account, when making estimates of climate–carbon feedbacks from palaeoclimate reconstructions.
    Type of Medium: Online Resource
    ISSN: 1814-9332
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2013
    detail.hit.zdb_id: 2217985-9
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  • 6
    In: Climate of the Past, Copernicus GmbH, Vol. 7, No. 2 ( 2011-04-28), p. 397-423
    Abstract: Abstract. We compare the present and last interglacial periods as recorded in Antarctic water stable isotope records now available at various temporal resolutions from six East Antarctic ice cores: Vostok, Taylor Dome, EPICA Dome C (EDC), EPICA Dronning Maud Land (EDML), Dome Fuji and the recent TALDICE ice core from Talos Dome. We first review the different modern site characteristics in terms of ice flow, meteorological conditions, precipitation intermittency and moisture origin, as depicted by meteorological data, atmospheric reanalyses and Lagrangian moisture source diagnostics. These different factors can indeed alter the relationships between temperature and water stable isotopes. Using five records with sufficient resolution on the EDC3 age scale, common features are quantified through principal component analyses. Consistent with instrumental records and atmospheric model results, the ice core data depict rather coherent and homogenous patterns in East Antarctica during the last two interglacials. Across the East Antarctic plateau, regional differences, with respect to the common East Antarctic signal, appear to have similar patterns during the current and last interglacials. We identify two abrupt shifts in isotopic records during the glacial inception at TALDICE and EDML, likely caused by regional sea ice expansion. These regional differences are discussed in terms of moisture origin and in terms of past changes in local elevation histories, which are compared to ice sheet model results. Our results suggest that elevation changes may contribute significantly to inter-site differences. These elevation changes may be underestimated by current ice sheet models.
    Type of Medium: Online Resource
    ISSN: 1814-9332
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2011
    detail.hit.zdb_id: 2217985-9
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  • 7
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 7, No. 13 ( 2007-07-09), p. 3579-3586
    Abstract: Abstract. The results from a simulation chamber study on the formaldehyde (HCHO) absorption cross section in the UV spectral region are presented. We performed 4 experiments at ambient HCHO concentrations with simultaneous measurements of two DOAS instruments in the atmosphere simulation chamber SAPHIR in Jülich. The two instruments differ in their spectral resolution, one working at 0.2 nm (broad-band, BB-DOAS), the other at 2.7 pm (high-resolution, HR-DOAS). Both instruments use dedicated multi reflection cells to achieve long light path lengths of 960 m and 2240 m, respectively, inside the chamber. During two experiments HCHO was injected into the clean chamber by thermolysis of well defined amounts of para-formaldehyde reaching mixing rations of 30 ppbV at maximum. The HCHO concentration calculated from the injection and the chamber volume agrees with the BB-DOAS measured value when the absorption cross section of Meller and Moortgat (2000) and the temperature coefficient of Cantrell (1990) were used for data evaluation. In two further experiments we produced HCHO in-situ from the ozone + ethene reaction which was intended to provide an independent way of HCHO calibration through the measurements of ozone and ethene. However, we found an unexpected deviation from the current understanding of the ozone + ethene reaction when CO was added to suppress possible oxidation of ethene by OH radicals. The reaction of the Criegee intermediate with CO could be 240 times slower than currently assumed. Based on the BB-DOAS measurements we could deduce a high-resolution cross section for HCHO which was not measured directly so far.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2007
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 8
    Online Resource
    Online Resource
    Copernicus GmbH ; 2014
    In:  Biogeosciences Vol. 11, No. 2 ( 2014-01-30), p. 463-479
    In: Biogeosciences, Copernicus GmbH, Vol. 11, No. 2 ( 2014-01-30), p. 463-479
    Abstract: Abstract. Fast Repetition Rate fluorometry (FRRf) measurements of phytoplankton photophysiology from an across-basin South Atlantic cruise (as part of the GEOTRACES programme) characterised two dominant ecophysiological regimes which were interpreted on the basis of nutrient limitation. South of the South Subtropical Convergence (SSTC) in the northern sub-Antarctic sector of the Antarctic Circumpolar Current (ACC) in the Eastern Atlantic Basin, waters are characterised by elevated chlorophyll concentrations, a dominance by larger phytoplankton cells, and low apparent photochemical efficiency (Fv / Fm). Shipboard 24 h iron (Fe) addition incubation experiments confirmed that Fe stress was primarily responsible for the low Fv / Fm, with Fe addition to these waters, either within the artificial bottle additions or naturally occurring downstream enrichment from Gough Island, significantly increasing Fv / Fm values. To the north of the SSTC at the southern boundary of the South Atlantic Gyre, phytoplankton are characterised by high values of Fv / Fm which, coupled with the low macronutrient concentrations and increased presence of picocyanobacteria, are interpreted as conditions of Fe replete, balanced macronutrient-limited growth. Spatial correlation was found between Fv / Fm and Fe:nitrate ratios, supporting the suggestion that the relative supply ratios of these two nutrients can control patterns of limitation and consequently the ecophysiology of phytoplankton in subtropical gyre and ACC regimes.
    Type of Medium: Online Resource
    ISSN: 1726-4189
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2014
    detail.hit.zdb_id: 2158181-2
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  • 9
    In: Earth System Science Data, Copernicus GmbH, Vol. 15, No. 8 ( 2023-08-03), p. 3419-3472
    Abstract: Abstract. The NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) produced a unique dataset for research into aerosol–cloud–meteorology interactions, with applications extending from process-based studies to multi-scale model intercomparison and improvement as well as to remote-sensing algorithm assessments and advancements. ACTIVATE used two NASA Langley Research Center aircraft, a HU-25 Falcon and King Air, to conduct systematic and spatially coordinated flights over the northwest Atlantic Ocean, resulting in 162 joint flights and 17 other single-aircraft flights between 2020 and 2022 across all seasons. Data cover 574 and 592 cumulative flights hours for the HU-25 Falcon and King Air, respectively. The HU-25 Falcon conducted profiling at different level legs below, in, and just above boundary layer clouds (〈 3 km) and obtained in situ measurements of trace gases, aerosol particles, clouds, and atmospheric state parameters. Under cloud-free conditions, the HU-25 Falcon similarly conducted profiling at different level legs within and immediately above the boundary layer. The King Air (the high-flying aircraft) flew at approximately ∼ 9 km and conducted remote sensing with a lidar and polarimeter while also launching dropsondes (785 in total). Collectively, simultaneous data from both aircraft help to characterize the same vertical column of the atmosphere. In addition to individual instrument files, data from the HU-25 Falcon aircraft are combined into “merge files” on the publicly available data archive that are created at different time resolutions of interest (e.g., 1, 5, 10, 15, 30, 60 s, or matching an individual data product's start and stop times). This paper describes the ACTIVATE flight strategy, instrument and complementary dataset products, data access and usage details, and data application notes. The data are publicly accessible through https://doi.org/10.5067/SUBORBITAL/ACTIVATE/DATA001 (ACTIVATE Science Team, 2020).
    Type of Medium: Online Resource
    ISSN: 1866-3516
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2475469-9
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  • 10
    In: Earth System Science Data, Copernicus GmbH, Vol. 11, No. 2 ( 2019-04-05), p. 441-454
    Abstract: Abstract. Tritium and helium isotope data provide key information on ocean circulation, ventilation, and mixing, as well as the rates of biogeochemical processes and deep-ocean hydrothermal processes. We present here global oceanic datasets of tritium and helium isotope measurements made by numerous researchers and laboratories over a period exceeding 60 years. The dataset's DOI is https://doi.org/10.25921/c1sn-9631, and the data are available at https://www.nodc.noaa.gov/ocads/data/0176626.xml (last access: 15 March 2019) or alternately http://odv.awi.de/data/ocean/jenkins-tritium-helium-data-compilation/ (last access: 13 March 2019) and includes approximately 60 000 valid tritium measurements, 63 000 valid helium isotope determinations, 57 000 dissolved helium concentrations, and 34 000 dissolved neon concentrations. Some quality control has been applied in that questionable data have been flagged and clearly compromised data excluded entirely. Appropriate metadata have been included, including geographic location, date, and sample depth. When available, we include water temperature, salinity, and dissolved oxygen. Data quality flags and data originator information (including methodology) are also included. This paper provides an introduction to the dataset along with some discussion of its broader qualities and graphics.
    Type of Medium: Online Resource
    ISSN: 1866-3516
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2475469-9
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