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  • 1
    Online Resource
    Online Resource
    Aerosols in the Pre-industrial Atmosphere
    Springer Science and Business Media LLC ; 2017
    In:  Current Climate Change Reports Vol. 3, No. 1 ( 2017-3), p. 1-15
    Details
    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
    URL: Article
    DOI: 10.1007/s40641-017-0061-2
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2017
    detail.hit.zdb_id: 2808618-1
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  • 2
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    Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation
    Proceedings of the National Academy of Sciences ; 2016
    In:  Proceedings of the National Academy of Sciences Vol. 113, No. 43 ( 2016-10-25), p. 12053-12058
    Details
    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
    URL: Article
    DOI: 10.1073/pnas.1602360113
    RVK:
    TA 1000
    RVK:
    WA 15000
    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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  • 3
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    Ozone loss rates in the Arctic stratosphere in the winter 1994/1995: Model simulations underestimate results of the Match analysis
    American Geophysical Union (AGU) ; 2000
    In:  Journal of Geophysical Research: Atmospheres Vol. 105, No. D12 ( 2000-06-27), p. 15175-15184
    Details
    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
    URL: Article
    DOI: 10.1029/2000JD900056
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2000
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    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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    SSG: 16,13
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  • 4
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    Evidence for the role of organics in aerosol particle formation under atmospheric conditions
    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
    Details
    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
    URL: Article
    DOI: 10.1073/pnas.0911330107
    RVK:
    TA 1000
    RVK:
    WA 15000
    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2010
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  • 5
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    Simulating organic aerosol in Delhi with WRF-Chem using the volatility-basis-set approach: exploring model uncertainty with a Gaussian process emulator
    Copernicus GmbH ; 2023
    In:  Atmospheric Chemistry and Physics Vol. 23, No. 10 ( 2023-05-23), p. 5763-5782
    Details
    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
    URL: Article
    URL: Article
    DOI: 10.5194/acp-23-5763-2023
    DOI: 10.5194/acp-23-5763-2023-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
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  • 6
    Online Resource
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    Correction to “Ozone loss rates in the Arctic stratosphere in the winter 1991/92: Model calculations compared with match results”
    American Geophysical Union (AGU) ; 1999
    In:  Geophysical Research Letters Vol. 26, No. 3 ( 1999-02-01), p. 327-327
    Details
    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
    URL: Article
    DOI: 10.1029/1999GL900010
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 1999
    detail.hit.zdb_id: 2021599-X
    detail.hit.zdb_id: 7403-2
    SSG: 16,13
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  • 7
    Online Resource
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    Aerosol and physical atmosphere model parameters are both important sources of uncertainty in aerosol ERF
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 13 ( 2018-07-13), p. 9975-10006
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 13 ( 2018-07-13), p. 9975-10006
    Abstract: Abstract. Changes in aerosols cause a change in net top-of-the-atmosphere (ToA) short-wave and long-wave radiative fluxes; rapid adjustments in clouds, water vapour and temperature; and an effective radiative forcing (ERF) of the planetary energy budget. The diverse sources of model uncertainty and the computational cost of running climate models make it difficult to isolate the main causes of aerosol ERF uncertainty and to understand how observations can be used to constrain it. We explore the aerosol ERF uncertainty by using fast model emulators to generate a very large set of aerosol–climate model variants that span the model uncertainty due to 27 parameters related to atmospheric and aerosol processes. Sensitivity analyses shows that the uncertainty in the ToA flux is dominated (around 80 %) by uncertainties in the physical atmosphere model, particularly parameters that affect cloud reflectivity. However, uncertainty in the change in ToA flux caused by aerosol emissions over the industrial period (the aerosol ERF) is controlled by a combination of uncertainties in aerosol (around 60 %) and physical atmosphere (around 40 %) parameters. Four atmospheric and aerosol parameters account for around 80 % of the uncertainty in short-wave ToA flux (mostly parameters that directly scale cloud reflectivity, cloud water content or cloud droplet concentrations), and these parameters also account for around 60 % of the aerosol ERF uncertainty. The common causes of uncertainty mean that constraining the modelled planetary brightness to tightly match satellite observations changes the lower 95 % credible aerosol ERF value from −2.65 to −2.37 W m−2. This suggests the strongest forcings (below around −2.4 W m−2) are inconsistent with observations. These results show that, regardless of the fact that the ToA flux is 2 orders of magnitude larger than the aerosol ERF, the observed flux can constrain the uncertainty in ERF because their values are connected by constrainable process parameters. The key to reducing the aerosol ERF uncertainty further will be to identify observations that can additionally constrain individual parameter ranges and/or combined parameter effects, which can be achieved through sensitivity analysis of perturbed parameter ensembles.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-18-9975-2018
    DOI: 10.5194/acp-18-9975-2018-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 8
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    The importance of comprehensive parameter sampling and multiple observations for robust constraint of aerosol radiative forcing
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 17 ( 2018-09-11), p. 13031-13053
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 17 ( 2018-09-11), p. 13031-13053
    Abstract: Abstract. Observational constraint of simulated aerosol and cloud properties is an essential part of building trustworthy climate models for calculating aerosol radiative forcing. Models are usually tuned to achieve good agreement with observations, but tuning produces just one of many potential variants of a model, so the model uncertainty cannot be determined. Here we estimate the uncertainty in aerosol effective radiative forcing (ERF) in a tuned climate model by constraining 4 million variants of the HadGEM3-UKCA aerosol–climate model to match nine common observations (top-of-atmosphere shortwave flux, aerosol optical depth, PM2.5, cloud condensation nuclei at 0.2 % supersaturation (CCN0.2), and concentrations of sulfate, black carbon and organic carbon, as well as decadal trends in aerosol optical depth and surface shortwave radiation.) The model uncertainty is calculated by using a perturbed parameter ensemble that samples 27 uncertainties in both the aerosol model and the physical climate model, and we use synthetic observations generated from the model itself to determine the potential of each observational type to constrain this uncertainty. Focusing over Europe in July, we show that the aerosol ERF uncertainty can be reduced by about 30 % by constraining it to the nine observations, demonstrating that producing climate models with an observationally plausible “base state” can contribute to narrowing the uncertainty in aerosol ERF. However, the uncertainty in the aerosol ERF after observational constraint is large compared to the typical spread of a multi-model ensemble. Our results therefore raise questions about whether the underlying multi-model uncertainty would be larger if similar approaches as adopted here were applied more widely. The approach presented in this study could be used to identify the most effective observations for model constraint. It is hoped that aerosol ERF uncertainty can be further reduced by introducing process-related constraints; however, any such results will be robust only if the enormous number of potential model variants is explored.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-18-13031-2018
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
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  • 9
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    A test of our understanding of the ozone chemistry in the Arctic polar vortex based on in situ measurements of ClO, BrO, and O 3 in the 1994/1995 winter
    American Geophysical Union (AGU) ; 1999
    In:  Journal of Geophysical Research: Atmospheres Vol. 104, No. D15 ( 1999-08-20), p. 18755-18768
    Details
    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
    URL: Article
    DOI: 10.1029/1999JD900287
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 1999
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    detail.hit.zdb_id: 2016813-5
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    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
    detail.hit.zdb_id: 3094197-0
    SSG: 16,13
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  • 10
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    A marine biogenic source of atmospheric ice-nucleating particles
    Springer Science and Business Media LLC ; 2015
    In:  Nature Vol. 525, No. 7568 ( 2015-09-10), p. 234-238
    Details
    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
    URL: Article
    DOI: 10.1038/nature14986
    RVK:
    TA 1000
    RVK:
    UA 1000
    RVK:
    WA 15000
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2015
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    detail.hit.zdb_id: 1413423-8
    SSG: 11
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