| 61. |
- Browse, J., et al.
(author)
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The complex response of Arctic aerosol to sea-ice retreat
- 2014
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:14, s. 7543-7557
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Journal article (peer-reviewed)abstract
- Loss of summertime Arctic sea ice will lead to a large increase in the emission of aerosols and precursor gases from the ocean surface. It has been suggested that these enhanced emissions will exert substantial aerosol radiative forcings, dominated by the indirect effect of aerosol on clouds. Here, we investigate the potential for these indirect forcings using a global aerosol microphysics model evaluated against aerosol observations from the Arctic Summer Cloud Ocean Study (ASCOS) campaign to examine the response of Arctic cloud condensation nuclei (CCN) to sea-ice retreat. In response to a complete loss of summer ice, we find that north of 70 degrees N emission fluxes of sea salt, marine primary organic aerosol (OA) and dimethyl sulfide increase by a factor of similar to 10, similar to 4 and similar to 15 respectively. However, the CCN response is weak, with negative changes over the central Arctic Ocean. The weak response is due to the efficient scavenging of aerosol by extensive drizzling stratocumulus clouds. In the scavenging-dominated Arctic environment, the production of condensable vapour from oxidation of dimethyl sulfide grows particles to sizes where they can be scavenged. This loss is not sufficiently compensated by new particle formation, due to the suppression of nucleation by the large condensation sink resulting from sea-salt and primary OA emissions. Thus, our results suggest that increased aerosol emissions will not cause a climate feedback through changes in cloud microphysical and radiative properties.
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| 62. |
- Bruns, M., et al.
(author)
-
NO2 profile retrieval using airborne multi axis UV-visible skylight absorption measurements over central Europe
- 2006
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 6:10, s. 3049-3058
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Journal article (peer-reviewed)abstract
- Abstract. A recent development in ground-based remote sensing of atmospheric constituents by UV/visible absorption measurements of scattered light is the simultaneous use of several directions with small elevation angles in addition to the traditional zenith-sky pointing. The different light paths through the atmosphere enable the vertical distribution of some atmospheric absorbers such as NO2, BrO or O3 to be retrieved. In this study, the amount of profile information that can be retrieved from such measurements on aircraft is investigated for the trace gas NO2. A Sensitivity study on synthetic data is performed for a combination of four lines of sight (LOS) (0°(nadir), 88°, 92°, and 180° (zenith)) and three wavelength regions [center wavelengths: 362.5 nm, 437.5 nm, and 485.0 nm]. The method used in this work is a combination of two previously established methods described in Petritoli et al. (2002) and Wang et al. (2004). The investigation presented here demonstrates the potential of this LOS/wavelengths setup to retrieve a significant amount of profile information from airborne multiax is differential optical absorption spectrometer (AMAXDOAS) measurements with a vertical resolution of 3.0 to 4.5 km in the lower troposphere and 2.0 to 3.5 km near flight altitude. Above 13 km the profile information content of AMAXDOAS measurements is sparse. The retrieval algorithm used in this work is the AMAXDOAS profile retrievalalgorithm (APROVAL). Further, retrieved profiles with a significant amount (up to 3.2 ppbv) of NO2 in the boundary layer over the Po-valley (Italy) are presented. Airborne multiaxis measurements are thus a promising tool for atmospheric studies in the troposphere.
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| 63. |
- Buchholz, Angela, et al.
(author)
-
Deconvolution of FIGAERO-CIMS thermal desorption profiles using positive matrix factorisation to identify chemical and physical processes during particle evaporation
- 2020
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:13, s. 7693-7716
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Journal article (peer-reviewed)abstract
- The measurements of aerosol particles with a filter inlet for gases and aerosols (FIGAERO) together with a chemical ionisation mass spectrometer (CIMS) yield the overall chemical composition of the particle phase. In addition, the thermal desorption profiles obtained for each detected ion composition contain information about the volatility of the detected compounds, which is an important property for understanding many physical properties like gas-particle partitioning. We coupled this thermal desorption method with isothermal evaporation prior to the sample collection to investigate the chemical composition changes during isothermal particle evaporation and particulate-water-driven chemical reactions in alpha-pinene secondary organic aerosol (SOA) of three different oxidative states. The thermal desorption profiles of all detected elemental compositions were then analysed with positive matrix factorisation (PMF) to identify the drivers of the chemical composition changes observed during isothermal evaporation. The keys to this analysis were to use the error matrix as a tool to weight the parts of the data carrying most information (i.e. the peak area of each thermogram) and to run PMF on a combined data set of multiple thermograms from different experiments to enable a direct comparison of the individual factors between separate measurements. The PMF was able to identify instrument background factors and separate them from the part of the data containing particle desorption information. Additionally, PMF allowed us to separate the direct desorption of compounds detected at a specific elemental composition from other signals with the same composition that stem from the thermal decomposition of thermally instable compounds with lower volatility. For each SOA type, 7-9 factors were needed to explain the observed thermogram behaviour. The contribution of the factors depended on the prior isothermal evaporation. Decreased contributions from the factors with the lowest desorption temperatures were observed with increasing isothermal evaporation time. Thus, the factors identified by PMF could be interpreted as volatility classes. The composition changes in the particles due to isothermal evaporation could be attributed to the removal of volatile factors with very little change in the desorption profiles of the individual factors (i.e. in the respective temperatures of peak desorption, T-max). When aqueous-phase reactions took place, PMF was able to identify a new factor that directly identified the ions affected by the chemical processes. We conducted a PMF analysis of the FIGAERO-CIMS thermal desorption data for the first time using laboratory-generated SOA particles. But this method can be applied to, for example, ambient FIGAERO-CIMS measurements as well. There, the PMF analysis of the thermal desorption data identifies organic aerosol (OA) sources (such as biomass burning or oxidation of different precursors) and types, e.g. hydrocarbon-like (HOA) or oxygenated organic aerosol (OOA). This information could also be obtained with the traditional approach, namely the PMF analysis of the mass spectra data integrated for each thermogram. But only our method can also obtain the volatility information for each OA source and type. Additionally, we can identify the contribution of thermal decomposition to the overall signal.
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| 64. |
- Buchholz, Angela, et al.
(author)
-
Insights into the O : C-dependent mechanisms controlling the evaporation of alpha-pinene secondary organic aerosol particles
- 2019
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:6, s. 4061-4073
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Journal article (peer-reviewed)abstract
- The volatility of oxidation products of volatile organic compounds (VOCs) in the atmosphere is a key factor to determine if they partition into the particle phase contributing to secondary organic aerosol (SOA) mass. Thus, linking volatility and measured particle composition will provide insights into SOA formation and its fate in the atmosphere. We produced alpha-pinene SOA with three different oxidation levels (characterized by average oxygen-to-carbon ratio; (O:C) over bar = 0.53, 0.69, and 0.96) in an oxidation flow reactor. We investigated the particle volatility by isothermal evaporation in clean air as a function of relative humidity (RH < 2 %, 40 %, and 80 %) and used a filter-based thermal desorption method to gain volatility and chemical composition information. We observed reduced particle evaporation for particles with increasing <(O:C )over bar> ratio, indicating that particles become more resilient to evaporation with oxidative aging. Particle evaporation was increased in the presence of water vapour and presumably particulate water; at the same time the resistance of the residual particles to thermal desorption was increased as well. For SOA with (O:C ) over bar = 0.96, the unexpectedly large increase in mean thermal desorption temperature and changes in the thermogram shapes under wet conditions (80 % RH) were an indication of aqueous phase chemistry. For the lower (O:C ) over bar cases, some water-induced composition changes were observed. However, the enhanced evaporation under wet conditions could be explained by the reduction in particle viscosity from the semi-solid to liquid-like range, and the observed higher desorption temperature of the residual particles is a direct consequence of the increased removal of high-volatility and the continued presence of low-volatility compounds.
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| 65. |
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| 66. |
- Buehler, Stefan, et al.
(author)
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A cloud filtering method for microwave upper tropospheric humidity measurements
- 2007
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 7:21, s. 5531-5542
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Journal article (peer-reviewed)abstract
- The paper presents a cloud filtering method for upper tropospheric humidity (UTH) measurements at 183.31±1.00 GHz. The method uses two criteria: a viewing angle dependent threshold on the brightness temperature at 183.31±1.00 GHz, and a threshold on the brightness temperature difference between another channel and 183.31±1.00 GHz. Two different alternatives, using 183.31±3.00 GHz or 183.31±7.00 GHz as the other channel, are studied. The robustness of this cloud filtering method is demonstrated by a mid-latitudes winter case study. The paper then studies different biases on UTH climatologies. Clouds are associated with high humidity, therefore the possible dry bias introduced by cloud filtering is discussed and compared to the wet biases introduced by the clouds radiative effect if no filtering is done. This is done by means of a case study, and by means of a stochastic cloud database with representative statistics for midlatitude conditions. Both studied filter alternatives perform nearly equally well, but the alternative using 183.31±3.00 GHz as other channel is preferable, because that channel is less likely to see the Earth's surface than the one at 183.31±7.00 GHz. The consistent result of all case studies and for both filter alternatives is that both cloud wet bias and cloud filtering dry bias are modest for microwave data. The recommended strategy is to use the cloud filtered data as an estimate for the true all-sky UTH value, but retain the unfiltered data to have an estimate of the cloud induced uncertainty. The focus of the paper is on midlatitude data, since atmospheric data to test the filter for that case were readily available. The filter is expected to be applicable also to subtropical and tropical data, but should be further validated with case studies similar to the one presented here for those cases.
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| 67. |
- Buehler, Stefan, et al.
(author)
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A multi-instrument comparison of integrated water vapour measurements at a high latitude site
- 2012
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:22, s. 10925-10943
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Journal article (peer-reviewed)abstract
- We compare measurements of integrated water vapour (IWV) over a subarctic site (Kiruna, Northern Sweden) from five different sensors and retrieval methods: Radiosondes, Global Positioning System (GPS), ground-based Fourier-transform infrared (FTIR) spectrometer, ground-based microwave radiometer, and satellite-based microwave radiometer (AMSU-B). Additionally, we compare also to ERA-Interim model reanalysis data. GPS-based IWV data have the highest temporal coverage and resolution and are chosen as reference data set. All datasets agree reasonably well, but the ground-based microwave instrument only if the data are cloud-filtered. We also address two issues that are general for such intercomparison studies, the impact of different lower altitude limits for the IWV integration, and the impact of representativeness error. We develop methods for correcting for the former, and estimating the random error contribution of the latter. A literature survey reveals that reported systematic differences between different techniques are study-dependent and show no overall consistent pattern. Further improving the absolute accuracy of IWV measurements and providing climate-quality time series therefore remain challenging problems.
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| 68. |
- Buker, P., et al.
(author)
-
DO3SE modelling of soil moisture to determine ozone flux to forest trees
- 2012
-
In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:12, s. 5537-5562
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Journal article (peer-reviewed)abstract
- The DO3SE (Deposition of O-3 for Stomatal Exchange) model is an established tool for estimating ozone (O-3) deposition, stomatal flux and impacts to a variety of vegetation types across Europe. It has been embedded within the EMEP (European Monitoring and Evaluation Programme) photochemical model to provide a policy tool capable of relating the flux-based risk of vegetation damage to O-3 precursor emission scenarios for use in policy formulation. A key limitation of regional flux-based risk assessments has been the assumption that soil water deficits are not limiting O-3 flux due to the unavailability of evaluated methods for modelling soil water deficits and their influence on stomatal conductance (g(sto)), and subsequent O-3 flux. This paper describes the development and evaluation of a method to estimate soil moisture status and its influence on g(sto) for a variety of forest tree species. This DO3SE soil moisture module uses the Penman-Monteith energy balance method to drive water cycling through the soil-plant-atmosphere system and empirical data describing g(sto) relationships with pre-dawn leaf water status to estimate the biological control of transpiration. We trial four different methods to estimate this biological control of the transpiration stream, which vary from simple methods that relate soil water content or potential directly to g(sto), to more complex methods that incorporate hydraulic resistance and plant capacitance that control water flow through the plant system. These methods are evaluated against field data describing a variety of soil water variables, g(sto) and transpiration data for Norway spruce (Picea abies), Scots pine (Pinus sylvestris), birch (Betula pendula), aspen (Populus tremuloides), beech (Fagus sylvatica) and holm oak (Quercus ilex) collected from ten sites across Europe and North America. Modelled estimates of these variables show consistency with observed data when applying the simple empirical methods, with the timing and magnitude of soil drying events being captured well across all sites and reductions in transpiration with the onset of drought being predicted with reasonable accuracy. The more complex methods, which incorporate hydraulic resistance and plant capacitance, perform less well, with predicted drying cycles consistently underestimating the rate and magnitude of water loss from the soil. A sensitivity analysis showed that model performance was strongly dependent upon the local parameterisation of key model drivers such as the maximum g(sto), soil texture, root depth and leaf area index. The results suggest that the simple modelling methods that relate g(sto) directly to soil water content and potential provide adequate estimates of soil moisture and influence on g(sto) such that they are suitable to be used to assess the potential risk posed by O-3 to forest trees across Europe.
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| 69. |
- Bulatovic, Ines, 1991-, et al.
(author)
-
Large-eddy simulation of a two-layer boundary-layer cloud system from the Arctic Ocean 2018 expedition
- 2023
-
In: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 23:12, s. 7033-7055
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Journal article (peer-reviewed)abstract
- Climate change is particularly noticeable in the Arctic. The most common type of cloud at these latitudes is mixed-phase stratocumulus. These clouds occur frequently and persistently during all seasons and play a critical role in the Arctic energy budget. Previous observations in the central (north of 80∘ N) Arctic have shown a high occurrence of prolonged periods of a shallow, single-layer mixed-phase stratocumulus at the top of the boundary layer (BL; altitudes ∼ 300 to 400 m). However, recent observations from the summer of 2018 instead showed a prevalence of a two-layer boundary-layer cloud system. Here we use large-eddy simulation to examine the maintenance of one of the cloud systems observed in the summer of 2018 and the sensitivity of the cloud layers to different micro- and macro-scale parameters. We find that the model generally reproduces the observed thermodynamic structure well, with two near-neutrally stratified layers in the BL caused by a low cloud (located within the first few hundred meters) capped by a lower-altitude temperature inversion and an upper cloud layer (based around one kilometer or slightly higher) capped by the main temperature inversion of the BL. The simulated cloud structure is persistent unless there are low aerosol number concentrations (≤ 5 cm−3), which cause the upper cloud layer to dissipate, or high large-scale wind speeds (≥ 8.5 m s−1), which erode the lower inversion and the related cloud layer. The changes in cloud structure alter both the short- and longwave cloud radiative effect at the surface. This results in changes in the net radiative effect of the modeled cloud system, which can impact the surface melting or freezing. The findings highlight the importance of better understanding and representing aerosol sources and sinks over the central Arctic Ocean. Furthermore, they underline the significance of meteorological parameters, such as the large-scale wind speed, for maintaining the two-layer boundary-layer cloud structure encountered in the lower atmosphere of the central Arctic.
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| 70. |
- Bulatovic, Ines, et al.
(author)
-
The importance of Aitken mode aerosol particles for cloud sustenance in the summertime high Arctic - a simulation study supported by observational data
- 2021
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:5, s. 3871-3897
-
Journal article (peer-reviewed)abstract
- The potential importance of Aitken mode particles (diameters similar to 25-80 nm) for stratiform mixed-phase clouds in the summertime high Arctic (> 80 degrees N) has been investigated using two large-eddy simulation models. We find that, in both models, Aitken mode particles significantly affect the simulated microphysical and radiative properties of the cloud and can help sustain the cloud when accumulation mode concentrations are low (< 10-20 cm(-3)), even when the particles have low hygroscopicity (hygroscopicity parameter - kappa = 0.1). However, the influence of the Aitken mode decreases if the overall liquid water content of the cloud is low, either due to a higher ice fraction or due to low radiative cooling rates. An analysis of the simulated supersaturation (ss) statistics shows that the ss frequently reaches 0.5 % and sometimes even exceeds 1 %, which confirms that Aitken mode particles can be activated. The modelling results are in qualitative agreement with observations of the Hoppel minimum obtained from four different expeditions in the high Arctic. Our findings highlight the importance of better understanding Aitken mode particle formation, chemical properties and emissions, particularly in clean environments such as the high Arctic.
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