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  • 1
    Online Resource
    Online Resource
    Springer Science and Business Media LLC ; 2017
    In:  Current Climate Change Reports Vol. 3, No. 1 ( 2017-3), p. 1-15
    In: Current Climate Change Reports, Springer Science and Business Media LLC, Vol. 3, No. 1 ( 2017-3), p. 1-15
    Type of Medium: Online Resource
    ISSN: 2198-6061
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2017
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  • 2
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 113, No. 43 ( 2016-10-25), p. 12053-12058
    Abstract: The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol–cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20–100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by 0.22   W   m − 2 (27%) to − 0.60   W   m − 2 . Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2016
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  • 3
    Online Resource
    Online Resource
    American Geophysical Union (AGU) ; 2000
    In:  Journal of Geophysical Research: Atmospheres Vol. 105, No. D12 ( 2000-06-27), p. 15175-15184
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 105, No. D12 ( 2000-06-27), p. 15175-15184
    Abstract: We present box model simulations of ozone loss rates in the Arctic lower stratosphere for the winter 1994/1995. The ozone loss was simulated along each of the trajectories of the Match data set for 1994/1995 to conduct a quantitative comparison with the Match results. The simulated ozone loss rates reach their maximum value of ≈ 4 ppb per sunlit hour at the end of January. For this period and for potential temperatures below 475 K the model results are in good agreement with the Match results, but for potential temperatures above 475 K the model underestimates the ozone loss rate by up to a factor of 2. This difference cannot be explained by known uncertainties of the model. Enhanced ozone loss has also been observed in March 1995 for potential temperatures below 475 K. These loss rates are also substantially underestimated by the model, but are within the range of the model uncertainties. In particular, the ozone loss rates simulated for March 1995 strongly depend on the extent of denitrification.
    Type of Medium: Online Resource
    ISSN: 0148-0227
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2000
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    detail.hit.zdb_id: 2016813-5
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    detail.hit.zdb_id: 2403298-0
    detail.hit.zdb_id: 2016800-7
    detail.hit.zdb_id: 161666-3
    detail.hit.zdb_id: 161667-5
    detail.hit.zdb_id: 2969341-X
    detail.hit.zdb_id: 161665-1
    detail.hit.zdb_id: 3094268-8
    detail.hit.zdb_id: 710256-2
    detail.hit.zdb_id: 2016804-4
    detail.hit.zdb_id: 3094181-7
    detail.hit.zdb_id: 3094219-6
    detail.hit.zdb_id: 3094167-2
    detail.hit.zdb_id: 2220777-6
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  • 4
    Online Resource
    Online Resource
    Proceedings of the National Academy of Sciences ; 2010
    In:  Proceedings of the National Academy of Sciences Vol. 107, No. 15 ( 2010-04-13), p. 6646-6651
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 107, No. 15 ( 2010-04-13), p. 6646-6651
    Abstract: New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H 2 SO 4 and organic condensable species. Nucleation occurs at H 2 SO 4 concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H 2 SO 4 and an organic molecule. This suggests that only one H 2 SO 4 molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2010
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 10 ( 2023-05-23), p. 5763-5782
    Abstract: Abstract. The nature and origin of organic aerosol in the atmosphere remain unclear. The gas–particle partitioning of semi-volatile organic compounds (SVOCs) that constitute primary organic aerosols (POAs) and the multigenerational chemical aging of SVOCs are particularly poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem (Weather Research and Forecasting model with Chemistry), can be a useful tool to describe emissions of POA and its chemical evolution. However, the evaluation of model uncertainty and the optimal model parameterization may be expensive to probe using only WRF-Chem simulations. Gaussian process emulators, trained on simulations from relatively few WRF-Chem simulations, are capable of reproducing model results and estimating the sources of model uncertainty within a defined range of model parameters. In this study, a WRF-Chem VBS parameterization is proposed; we then generate a perturbed parameter ensemble of 111 model runs, perturbing 10 parameters of the WRF-Chem model relating to organic aerosol emissions and the VBS oxidation reactions. This allowed us to cover the model's uncertainty space and to compare outputs from each run to aerosol mass spectrometer observations of organic aerosol concentrations and O:C ratios measured in New Delhi, India. The simulations spanned the organic aerosol concentrations measured with the aerosol mass spectrometer (AMS). However, they also highlighted potential structural errors in the model that may be related to unsuitable diurnal cycles in the emissions and/or failure to adequately represent the dynamics of the planetary boundary layer. While the structural errors prevented us from clearly identifying an optimized VBS approach in WRF-Chem, we were able to apply the emulator in the following two periods: the full period (1–29 May) and a subperiod period of 14:00–16:00 h LT (local time) on 1–29 May. The combination of emulator analysis and model evaluation metrics allowed us to identify plausible parameter combinations for the analyzed periods. We demonstrate that the methodology presented in this study can be used to determine the model uncertainty and to identify the appropriate parameter combination for the VBS approach and hence to provide valuable information to improve our understanding of OA production.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
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  • 6
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 104, No. D15 ( 1999-08-20), p. 18755-18768
    Abstract: We present an analysis of in situ measurements of ClO, BrO, O 3 , and long‐lived tracers obtained on a balloon flight in the Arctic polar vortex launched from Kiruna, Sweden, 68°N, on February 3, 1995. Using the method of tracer correlations, we deduce that the air masses sampled at an altitude of 21 km (480 K potential temperature), where a layer of enhanced ClO mixing ratios of up to 1150 parts per trillion by volume was observed, experienced a cumulative chemical ozone loss of 1.0±0.3 ppmv between late November 1994 and early February 1995. This estimate of chemical ozone loss can be confirmed using independent data sets and independent methods. Calculations using a trajectory box model show that the simulations underestimate the cumulative ozone loss by approximately a factor of 2, although observed ClO and BrO mixing ratios are well reproduced by the model. Employing additional simulations of ozone loss rates for idealized conditions, we conclude that the known chlorine and bromine catalytic cycles destroying odd oxygen with the known rate constants and absorption cross sections do not quantitatively account for the early winter ozone losses infered for air masses observed at 21 km.
    Type of Medium: Online Resource
    ISSN: 0148-0227
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 1999
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    detail.hit.zdb_id: 3094104-0
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    detail.hit.zdb_id: 2403298-0
    detail.hit.zdb_id: 2016800-7
    detail.hit.zdb_id: 161666-3
    detail.hit.zdb_id: 161667-5
    detail.hit.zdb_id: 2969341-X
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    detail.hit.zdb_id: 3094268-8
    detail.hit.zdb_id: 710256-2
    detail.hit.zdb_id: 2016804-4
    detail.hit.zdb_id: 3094181-7
    detail.hit.zdb_id: 3094219-6
    detail.hit.zdb_id: 3094167-2
    detail.hit.zdb_id: 2220777-6
    detail.hit.zdb_id: 3094197-0
    SSG: 16,13
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  • 7
    Online Resource
    Online Resource
    American Geophysical Union (AGU) ; 1999
    In:  Geophysical Research Letters Vol. 26, No. 3 ( 1999-02-01), p. 327-327
    In: Geophysical Research Letters, American Geophysical Union (AGU), Vol. 26, No. 3 ( 1999-02-01), p. 327-327
    Type of Medium: Online Resource
    ISSN: 0094-8276
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 1999
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    detail.hit.zdb_id: 7403-2
    SSG: 16,13
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  • 8
    In: Nature, Springer Science and Business Media LLC, Vol. 525, No. 7568 ( 2015-09-10), p. 234-238
    Type of Medium: Online Resource
    ISSN: 0028-0836 , 1476-4687
    RVK:
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    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2015
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  • 9
    Online Resource
    Online Resource
    Proceedings of the National Academy of Sciences ; 2014
    In:  Proceedings of the National Academy of Sciences Vol. 111, No. 52 ( 2014-12-30), p. 18466-18471
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 111, No. 52 ( 2014-12-30), p. 18466-18471
    Abstract: Natural aerosols define a preindustrial baseline state from which the magnitude of anthropogenic aerosol effects on climate are calculated and are a major component of the large uncertainty in anthropogenic aerosol−cloud radiative forcing. This uncertainty would be reduced if aerosol environments unperturbed by air pollution could be studied in the present-day atmosphere, but the pervasiveness of air pollution makes identification of unperturbed regions difficult. Here, we use global model simulations to define unperturbed aerosol regions in terms of two measures that compare 1750 and 2000 conditions—the number of days with similar aerosol concentrations and the similarity of the aerosol response to perturbations in model processes and emissions. The analysis shows that the aerosol system in many present-day environments looks and behaves like it did in the preindustrial era. On a global annual mean, unperturbed aerosol regions cover 12% of the Earth (16% of the ocean surface and 2% of the land surface). There is a strong seasonal variation in unperturbed regions of between 4% in August and 27% in January, with the most persistent conditions occurring over the equatorial Pacific. About 90% of unperturbed regions occur in the Southern Hemisphere, but in the Northern Hemisphere, unperturbed conditions are transient and spatially patchy. In cloudy regions with a radiative forcing relative to 1750, model results suggest that unperturbed aerosol conditions could still occur on a small number of days per month. However, these environments are mostly in the Southern Hemisphere, potentially limiting the usefulness in reducing Northern Hemisphere forcing uncertainty.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2014
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  • 10
    Online Resource
    Online Resource
    Proceedings of the National Academy of Sciences ; 2016
    In:  Proceedings of the National Academy of Sciences Vol. 113, No. 21 ( 2016-05-24), p. 5812-5819
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 113, No. 21 ( 2016-05-24), p. 5812-5819
    Abstract: The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol−cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol−cloud interactions adequately. There is a dearth of observational constraints on aerosol−cloud interactions. We develop a conceptual approach to systematically constrain the aerosol−cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol−cloud radiation system.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2016
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    detail.hit.zdb_id: 1461794-8
    SSG: 11
    SSG: 12
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