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  • Open Access English
    Authors: 
    Fanourgakis, George S.; Kanakidou, Maria; Nenes, Athanasios; Bauer, Susanne E.; Bergman, Tommi; Carslaw, Ken S.; Grini, Alf; Hamilton, Douglas S.; Johnson, Jill S.; Karydis, Vlassis A.; +29 more
    Project: NSF | Development, Validation, ... (1550816), EC | CRESCENDO (641816), EC | PyroTRACH (726165), EC | RECAP (724602), EC | BACCHUS (603445), EC | ACTRIS-2 (654109)

    A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011–2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of −24 % and −35 % for particles with dry diameters >50 and >120 nm, as well as −36 % and −34 % for CCN at supersaturations of 0.2 % and 1.0 %, respectively. However, they seem to behave differently for particles activating at very low supersaturations (<0.1 %) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2 % (CCN0.2) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120 nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40 % during winter and 20 % in summer. In contrast to the large spread in simulated aerosol particle and CCN number concentrations, the CDNC derived from simulated CCN spectra is less diverse and in better agreement with CDNC estimates consistently derived from the observations (average NMB −13 % and −22 % for updraft velocities 0.3 and 0.6 m s−1, respectively). In addition, simulated CDNC is in slightly better agreement with observationally derived values at lower than at higher updraft velocities (index of agreement 0.64 vs. 0.65). The reduced spread of CDNC compared to that of CCN is attributed to the sublinear response of CDNC to aerosol particle number variations and the negative correlation between the sensitivities of CDNC to aerosol particle number concentration (∂Nd/∂Na) and to updraft velocity (∂Nd/∂w). Overall, we find that while CCN is controlled by both aerosol particle number and composition, CDNC is sensitive to CCN at low and moderate CCN concentrations and to the updraft velocity when CCN levels are high. Discrepancies are found in sensitivities ∂Nd/∂Na and ∂Nd/∂w; models may be predisposed to be too “aerosol sensitive” or “aerosol insensitive” in aerosol–cloud–climate interaction studies, even if they may capture average droplet numbers well. This is a subtle but profound finding that only the sensitivities can clearly reveal and may explain inter-model biases on the aerosol indirect effect.

  • Open Access English
    Authors: 
    Blechschmidt, Anne-Marlene; Arteta, Joaquim; Coman, Adriana; Curier, Lyana; Eskes, Henk; Foret, Gilles; Gielen, Clio; Hendrick, Francois; Marécal, Virginie; Meleux, Frédérik; +13 more
    Project: EC | NORS (284421), EC | MACC-III (633080), EC | MACC II (283576)

    Multi-axis differential optical absorption spectroscopy (MAX-DOAS) tropospheric NO2 column retrievals from four European measurement stations are compared to simulations from five regional air quality models which contribute to the European regional ensemble forecasts and reanalyses of the operational Copernicus Atmosphere Monitoring Service (CAMS). Compared to other observational data usually applied for regional model evaluation, MAX-DOAS data are closer to the regional model data in terms of horizontal and vertical resolution, and multiple measurements are available during daylight, so that, for example, diurnal cycles of trace gases can be investigated. In general, there is good agreement between simulated and retrieved NO2 column values for individual MAX-DOAS measurements with correlations between 35 % and 70 % for individual models and 45 % to 75 % for the ensemble median for tropospheric NO2 vertical column densities (VCDs), indicating that emissions, transport and tropospheric chemistry of NOx are on average well simulated. However, large differences are found for individual pollution plumes observed by MAX-DOAS. Most of the models overestimate seasonal cycles for the majority of MAX-DOAS sites investigated. At the urban stations, weekly cycles are reproduced well, but the decrease towards the weekend is underestimated and diurnal cycles are overall not well represented. In particular, simulated morning rush hour peaks are not confirmed by MAX-DOAS retrievals, and models fail to reproduce observed changes in diurnal cycles for weekdays versus weekends. The results of this study show that future model development needs to concentrate on improving representation of diurnal cycles and associated temporal scalings.

  • Open Access English
    Authors: 
    Sourdeval, Odran; Gryspeerdt, Edward; Krämer, Martina; Goren, Tom; Delanoë, Julien; Afchine, Armin; Hemmer, Friederike; Quaas, Johannes;
    Project: EC | QUAERERE (306284), EC | MSCCC (703880)

    The number concentration of cloud particles is a key quantity for understanding aerosol–cloud interactions and describing clouds in climate and numerical weather prediction models. In contrast with recent advances for liquid clouds, few observational constraints exist regarding the ice crystal number concentration (Ni). This study investigates how combined lidar–radar measurements can be used to provide satellite estimates of Ni, using a methodology that constrains moments of a parameterized particle size distribution (PSD). The operational liDAR–raDAR (DARDAR) product serves as an existing base for this method, which focuses on ice clouds with temperatures Tc<-30 ∘C. Theoretical considerations demonstrate the capability for accurate retrievals of Ni, apart from a possible bias in the concentration in small crystals when Tc≳−50 ∘C, due to the assumption of a monomodal PSD shape in the current method. This is verified via a comparison of satellite estimates to coincident in situ measurements, which additionally demonstrates the sufficient sensitivity of lidar–radar observations to Ni. Following these results, satellite estimates of Ni are evaluated in the context of a case study and a preliminary climatological analysis based on 10 years of global data. Despite a lack of other large-scale references, this evaluation shows a reasonable physical consistency in Ni spatial distribution patterns. Notably, increases in Ni are found towards cold temperatures and, more significantly, in the presence of strong updrafts, such as those related to convective or orographic uplifts. Further evaluation and improvement of this method are necessary, although these results already constitute a first encouraging step towards large-scale observational constraints for Ni. Part 2 of this series uses this new dataset to examine the controls on Ni.

  • Open Access English
    Authors: 
    Gryspeerdt, Edward; Goren, Tom; Sourdeval, Odran; Quaas, Johannes; Mülmenstädt, Johannes; Dipu, Sudhakar; Unglaub, Claudia; Gettelman, Andrew; Christensen, Matthew;
    Project: EC | MSCCC (703880), EC | QUAERERE (306284)

    The impact of aerosols on cloud properties is one of the largest uncertainties in the anthropogenic radiative forcing of the climate. Significant progress has been made in constraining this forcing using observations, but uncertainty remains, particularly in the magnitude of cloud rapid adjustments to aerosol perturbations. Cloud liquid water path (LWP) is the leading control on liquid-cloud albedo, making it important to observationally constrain the aerosol impact on LWP. Previous modelling and observational studies have shown that multiple processes play a role in determining the LWP response to aerosol perturbations, but that the aerosol effect can be difficult to isolate. Following previous studies using mediating variables, this work investigates use of the relationship between cloud droplet number concentration (Nd) and LWP for constraining the role of aerosols. Using joint-probability histograms to account for the non-linear relationship, this work finds a relationship that is broadly consistent with previous studies. There is significant geographical variation in the relationship, partly due to role of meteorological factors (particularly relative humidity). The Nd–LWP relationship is negative in the majority of regions, suggesting that aerosol-induced LWP reductions could offset a significant fraction of the instantaneous radiative forcing from aerosol–cloud interactions (RFaci). However, variations in the Nd–LWP relationship in response to volcanic and shipping aerosol perturbations indicate that the Nd–LWP relationship overestimates the causal Nd impact on LWP due to the role of confounding factors. The weaker LWP reduction implied by these “natural experiments” means that this work provides an upper bound to the radiative forcing from aerosol-induced changes in the LWP.

  • Open Access English
    Authors: 
    Kalivitis, Nikos; Kerminen, Veli-Matti; Kouvarakis, Giorgos; Stavroulas, Iasonas; Tzitzikalaki, Evaggelia; Kalkavouras, Panayiotis; Daskalakis, Nikos; Myriokefalitakis, Stelios; Bougiatioti, Aikaterini; Manninen, Hanna E.; +6 more
    Project: EC | BACCHUS (603445), EC | ACTRIS-2 (654109)

    Atmospheric new particle formation (NPF) is a common phenomenon all over the world. In this study we present the longest time series of NPF records in the eastern Mediterranean region by analyzing 10 years of aerosol number size distribution data obtained with a mobility particle sizer. The measurements were performed at the Finokalia environmental research station on Crete, Greece, during the period June 2008–June 2018. We found that NPF took place on 27 % of the available days, undefined days were 23 % and non-event days 50 %. NPF is more frequent in April and May probably due to the terrestrial biogenic activity and is less frequent in August. Throughout the period under study, nucleation was observed also during the night. Nucleation mode particles had the highest concentration in winter and early spring, mainly because of the minimum sinks, and their average contribution to the total particle number concentration was 8 %. Nucleation mode particle concentrations were low outside periods of active NPF and growth, so there are hardly any other local sources of sub-25 nm particles. Additional atmospheric ion size distribution data simultaneously collected for more than 2 years were also analyzed. Classification of NPF events based on ion spectrometer measurements differed from the corresponding classification based on a mobility spectrometer, possibly indicating a different representation of local and regional NPF events between these two measurement data sets. We used the MALTE-Box model for simulating a case study of NPF in the eastern Mediterranean region. Monoterpenes contributing to NPF can explain a large fraction of the observed NPF events according to our model simulations. However the adjusted parameterization resulting from our sensitivity tests was significantly different from the initial one that had been determined for the boreal environment.

  • Open Access English
    Authors: 
    Metzger, Swen; Abdelkader, Mohamed; Steil, Benedikt; Klingmüller, Klaus;
    Project: EC | EoCoE (676629), EC | C8 (226144)

    We scrutinize the importance of aerosol water for the aerosol optical depth (AOD) calculations using a long-term evaluation of the EQuilibrium Simplified Aerosol Model v4 for climate modeling. EQSAM4clim is based on a single solute coefficient approach that efficiently parameterizes hygroscopic growth, accounting for aerosol water uptake from the deliquescence relative humidity up to supersaturation. EQSAM4clim extends the single solute coefficient approach to treat water uptake of multicomponent mixtures. The gas–aerosol partitioning and the mixed-solution water uptake can be solved analytically, preventing the need for iterations, which is computationally efficient. EQSAM4clim has been implemented in the global chemistry climate model EMAC and compared to ISORROPIA II on climate timescales. Our global modeling results show that (I) our EMAC results of the AOD are comparable to modeling results that have been independently evaluated for the period 2000–2010, (II) the results of various aerosol properties of EQSAM4clim and ISORROPIA II are similar and in agreement with AERONET and EMEP observations for the period 2000–2013, and (III) the underlying assumptions on the aerosol water uptake limitations are important for derived AOD calculations. Sensitivity studies of different levels of chemical aging and associated water uptake show larger effects on AOD calculations for the year 2005 compared to the differences associated with the application of the two gas–liquid–solid partitioning schemes. Overall, our study demonstrates the importance of aerosol water for climate studies.

  • Open Access English
    Authors: 
    Schaller, Carsten; Kittler, Fanny; Foken, Thomas; Göckede, Mathias;
    Project: EC | PAGE21 (282700), EC | PERCCOM (333796)

    Methane (CH4) emissions from biogenic sources, such as Arctic permafrost wetlands, are associated with large uncertainties because of the high variability of fluxes in both space and time. This variability poses a challenge to monitoring CH4 fluxes with the eddy covariance (EC) technique, because this approach requires stationary signals from spatially homogeneous sources. Episodic outbursts of CH4 emissions, i.e. triggered by spontaneous outgassing of bubbles or venting of methane-rich air from lower levels due to shifts in atmospheric conditions, are particularly challenging to quantify. Such events typically last for only a few minutes, which is much shorter than the common averaging interval for EC (30 min). The steady-state assumption is jeopardised, which potentially leads to a non-negligible bias in the CH4 flux. Based on data from Chersky, NE Siberia, we tested and evaluated a flux calculation method based on wavelet analysis, which, in contrast to regular EC data processing, does not require steady-state conditions and is allowed to obtain fluxes over averaging periods as short as 1 min. Statistics on meteorological conditions before, during, and after the detected events revealed that it is atmospheric mixing that triggered such events rather than CH4 emission from the soil. By investigating individual events in more detail, we identified a potential influence of various mesoscale processes like gravity waves, low-level jets, weather fronts passing the site, and cold-air advection from a nearby mountain ridge as the dominating processes. The occurrence of extreme CH4 flux events over the summer season followed a seasonal course with a maximum in early August, which is strongly correlated with the maximum soil temperature. Overall, our findings demonstrate that wavelet analysis is a powerful method for resolving highly variable flux events on the order of minutes, and can therefore support the evaluation of EC flux data quality under non-steady-state conditions.

  • Open Access English
    Authors: 
    Ayarzagüena, Blanca; Palmeiro, Froila M.; Barriopedro, David; Calvo, Natalia; Langematz, Ulrike; Shibata, Kiyotaka;
    Project: EC | STRATOCLIM (603557)

    Major sudden stratospheric warmings (SSWs) represent one of the most abrupt phenomena of the boreal wintertime stratospheric variability, and constitute the clearest example of coupling between the stratosphere and the troposphere. A good representation of SSWs in climate models is required to reduce their biases and uncertainties in future projections of stratospheric variability. The ability of models to reproduce these phenomena is usually assessed with just one reanalysis. However, the number of reanalyses has increased in the last decade and their own biases may affect the model evaluation. Here we compare the representation of the main aspects of SSWs across reanalyses. The examination of their main characteristics in the pre- and post-satellite periods reveals that reanalyses behave very similarly in both periods. However, discrepancies are larger in the pre-satellite period compared to afterwards, particularly for the NCEP-NCAR reanalysis. All datasets reproduce similarly the specific features of wavenumber-1 and wavenumber-2 SSWs. A good agreement among reanalyses is also found for triggering mechanisms, tropospheric precursors, and surface response. In particular, differences in blocking precursor activity of SSWs across reanalyses are much smaller than between blocking definitions.

  • Open Access English
    Authors: 
    Radenz, Martin; Seifert, Patric; Baars, Holger; Floutsi, Athena Augusta; Yin, Zhenping; Bühl, Johannes;
    Project: EC | ACTRIS-2 (654109), EC | BACCHUS (603445)

    Height-resolved air mass source attribution is crucial for the evaluation of profiling ground-based remote sensing observations, especially when using lidar (light detection and ranging) to investigate different aerosol types throughout the atmosphere. Lidar networks, such as EARLINET (European Aerosol Research Lidar Network) in the frame of ACTRIS (Aerosol, Clouds and Trace Gases), observe profiles of optical aerosol properties almost continuously, but usually, additional information is needed to support the characterization of the observed particles. This work presents an approach explaining how backward trajectories or particle positions from a dispersion model can be combined with geographical information (a land cover classification and manually defined areas) to obtain a continuous and vertically resolved estimate of an air mass source above a certain location. Ideally, such an estimate depends on as few as possible a priori information and auxiliary data. An automated framework for the computation of such an air mass source is presented, and two applications are described. First, the air mass source information is used for the interpretation of air mass sources for three case studies with lidar observations from Limassol (Cyprus), Punta Arenas (Chile) and ship-borne off Cabo Verde. Second, air mass source statistics are calculated for two multi-week campaigns to assess potential observation biases of lidar-based aerosol statistics. Such an automated approach is a valuable tool for the analysis of short-term campaigns but also for long-term data sets, for example, acquired by EARLINET.

  • Open Access English
    Authors: 
    Mülmenstädt, Johannes; Gryspeerdt, Edward; Salzmann, Marc; Ma, Po-Lun; Dipu, Sudhakar; Quaas, Johannes;
    Project: EC | QUAERERE (306284)

    Using the method of offline radiative transfer modeling within the partial radiative perturbation (PRP) approach, the effective radiative forcing by aerosol–cloud interactions (ERFaci) in the ECHAM–HAMMOZ aerosol climate model is decomposed into a radiative forcing by anthropogenic cloud droplet number change and adjustments of the liquid water path and cloud fraction. The simulated radiative forcing by anthropogenic cloud droplet number change and liquid water path adjustment are of approximately equal magnitude at −0.52 and −0.53 W m−2, respectively, while the cloud-fraction adjustment is somewhat weaker at −0.31 W m−2 (constituting 38 %, 39 %, and 23 % of the total ERFaci, respectively); geographically, all three ERFaci components in the simulation peak over China, the subtropical eastern ocean boundaries, the northern Atlantic and Pacific oceans, Europe, and eastern North America (in order of prominence). Spatial correlations indicate that the temporal-mean liquid water path adjustment is proportional to the temporal-mean radiative forcing, while the relationship between cloud-fraction adjustment and radiative forcing is less direct. While the estimate of warm-cloud ERFaci is relatively insensitive to the treatment of ice and mixed-phase cloud overlying warm cloud, there are indications that more restrictive treatments of ice in the column result in a low bias in the estimated magnitude of the liquid water path adjustment and a high bias in the estimated magnitude of the droplet number forcing. Since the present work is the first PRP decomposition of the aerosol effective radiative forcing into radiative forcing and rapid cloud adjustments, idealized experiments are conducted to provide evidence that the PRP results are accurate. The experiments show that using low-frequency (daily or monthly) time-averaged model output of the cloud property fields underestimates the ERF, but 3-hourly mean output is sufficiently frequent.

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49 Research products, page 1 of 5
  • Open Access English
    Authors: 
    Fanourgakis, George S.; Kanakidou, Maria; Nenes, Athanasios; Bauer, Susanne E.; Bergman, Tommi; Carslaw, Ken S.; Grini, Alf; Hamilton, Douglas S.; Johnson, Jill S.; Karydis, Vlassis A.; +29 more
    Project: NSF | Development, Validation, ... (1550816), EC | CRESCENDO (641816), EC | PyroTRACH (726165), EC | RECAP (724602), EC | BACCHUS (603445), EC | ACTRIS-2 (654109)

    A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011–2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of −24 % and −35 % for particles with dry diameters >50 and >120 nm, as well as −36 % and −34 % for CCN at supersaturations of 0.2 % and 1.0 %, respectively. However, they seem to behave differently for particles activating at very low supersaturations (<0.1 %) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2 % (CCN0.2) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120 nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40 % during winter and 20 % in summer. In contrast to the large spread in simulated aerosol particle and CCN number concentrations, the CDNC derived from simulated CCN spectra is less diverse and in better agreement with CDNC estimates consistently derived from the observations (average NMB −13 % and −22 % for updraft velocities 0.3 and 0.6 m s−1, respectively). In addition, simulated CDNC is in slightly better agreement with observationally derived values at lower than at higher updraft velocities (index of agreement 0.64 vs. 0.65). The reduced spread of CDNC compared to that of CCN is attributed to the sublinear response of CDNC to aerosol particle number variations and the negative correlation between the sensitivities of CDNC to aerosol particle number concentration (∂Nd/∂Na) and to updraft velocity (∂Nd/∂w). Overall, we find that while CCN is controlled by both aerosol particle number and composition, CDNC is sensitive to CCN at low and moderate CCN concentrations and to the updraft velocity when CCN levels are high. Discrepancies are found in sensitivities ∂Nd/∂Na and ∂Nd/∂w; models may be predisposed to be too “aerosol sensitive” or “aerosol insensitive” in aerosol–cloud–climate interaction studies, even if they may capture average droplet numbers well. This is a subtle but profound finding that only the sensitivities can clearly reveal and may explain inter-model biases on the aerosol indirect effect.

  • Open Access English
    Authors: 
    Blechschmidt, Anne-Marlene; Arteta, Joaquim; Coman, Adriana; Curier, Lyana; Eskes, Henk; Foret, Gilles; Gielen, Clio; Hendrick, Francois; Marécal, Virginie; Meleux, Frédérik; +13 more
    Project: EC | NORS (284421), EC | MACC-III (633080), EC | MACC II (283576)

    Multi-axis differential optical absorption spectroscopy (MAX-DOAS) tropospheric NO2 column retrievals from four European measurement stations are compared to simulations from five regional air quality models which contribute to the European regional ensemble forecasts and reanalyses of the operational Copernicus Atmosphere Monitoring Service (CAMS). Compared to other observational data usually applied for regional model evaluation, MAX-DOAS data are closer to the regional model data in terms of horizontal and vertical resolution, and multiple measurements are available during daylight, so that, for example, diurnal cycles of trace gases can be investigated. In general, there is good agreement between simulated and retrieved NO2 column values for individual MAX-DOAS measurements with correlations between 35 % and 70 % for individual models and 45 % to 75 % for the ensemble median for tropospheric NO2 vertical column densities (VCDs), indicating that emissions, transport and tropospheric chemistry of NOx are on average well simulated. However, large differences are found for individual pollution plumes observed by MAX-DOAS. Most of the models overestimate seasonal cycles for the majority of MAX-DOAS sites investigated. At the urban stations, weekly cycles are reproduced well, but the decrease towards the weekend is underestimated and diurnal cycles are overall not well represented. In particular, simulated morning rush hour peaks are not confirmed by MAX-DOAS retrievals, and models fail to reproduce observed changes in diurnal cycles for weekdays versus weekends. The results of this study show that future model development needs to concentrate on improving representation of diurnal cycles and associated temporal scalings.

  • Open Access English
    Authors: 
    Sourdeval, Odran; Gryspeerdt, Edward; Krämer, Martina; Goren, Tom; Delanoë, Julien; Afchine, Armin; Hemmer, Friederike; Quaas, Johannes;
    Project: EC | QUAERERE (306284), EC | MSCCC (703880)

    The number concentration of cloud particles is a key quantity for understanding aerosol–cloud interactions and describing clouds in climate and numerical weather prediction models. In contrast with recent advances for liquid clouds, few observational constraints exist regarding the ice crystal number concentration (Ni). This study investigates how combined lidar–radar measurements can be used to provide satellite estimates of Ni, using a methodology that constrains moments of a parameterized particle size distribution (PSD). The operational liDAR–raDAR (DARDAR) product serves as an existing base for this method, which focuses on ice clouds with temperatures Tc<-30 ∘C. Theoretical considerations demonstrate the capability for accurate retrievals of Ni, apart from a possible bias in the concentration in small crystals when Tc≳−50 ∘C, due to the assumption of a monomodal PSD shape in the current method. This is verified via a comparison of satellite estimates to coincident in situ measurements, which additionally demonstrates the sufficient sensitivity of lidar–radar observations to Ni. Following these results, satellite estimates of Ni are evaluated in the context of a case study and a preliminary climatological analysis based on 10 years of global data. Despite a lack of other large-scale references, this evaluation shows a reasonable physical consistency in Ni spatial distribution patterns. Notably, increases in Ni are found towards cold temperatures and, more significantly, in the presence of strong updrafts, such as those related to convective or orographic uplifts. Further evaluation and improvement of this method are necessary, although these results already constitute a first encouraging step towards large-scale observational constraints for Ni. Part 2 of this series uses this new dataset to examine the controls on Ni.

  • Open Access English
    Authors: 
    Gryspeerdt, Edward; Goren, Tom; Sourdeval, Odran; Quaas, Johannes; Mülmenstädt, Johannes; Dipu, Sudhakar; Unglaub, Claudia; Gettelman, Andrew; Christensen, Matthew;
    Project: EC | MSCCC (703880), EC | QUAERERE (306284)

    The impact of aerosols on cloud properties is one of the largest uncertainties in the anthropogenic radiative forcing of the climate. Significant progress has been made in constraining this forcing using observations, but uncertainty remains, particularly in the magnitude of cloud rapid adjustments to aerosol perturbations. Cloud liquid water path (LWP) is the leading control on liquid-cloud albedo, making it important to observationally constrain the aerosol impact on LWP. Previous modelling and observational studies have shown that multiple processes play a role in determining the LWP response to aerosol perturbations, but that the aerosol effect can be difficult to isolate. Following previous studies using mediating variables, this work investigates use of the relationship between cloud droplet number concentration (Nd) and LWP for constraining the role of aerosols. Using joint-probability histograms to account for the non-linear relationship, this work finds a relationship that is broadly consistent with previous studies. There is significant geographical variation in the relationship, partly due to role of meteorological factors (particularly relative humidity). The Nd–LWP relationship is negative in the majority of regions, suggesting that aerosol-induced LWP reductions could offset a significant fraction of the instantaneous radiative forcing from aerosol–cloud interactions (RFaci). However, variations in the Nd–LWP relationship in response to volcanic and shipping aerosol perturbations indicate that the Nd–LWP relationship overestimates the causal Nd impact on LWP due to the role of confounding factors. The weaker LWP reduction implied by these “natural experiments” means that this work provides an upper bound to the radiative forcing from aerosol-induced changes in the LWP.

  • Open Access English
    Authors: 
    Kalivitis, Nikos; Kerminen, Veli-Matti; Kouvarakis, Giorgos; Stavroulas, Iasonas; Tzitzikalaki, Evaggelia; Kalkavouras, Panayiotis; Daskalakis, Nikos; Myriokefalitakis, Stelios; Bougiatioti, Aikaterini; Manninen, Hanna E.; +6 more
    Project: EC | BACCHUS (603445), EC | ACTRIS-2 (654109)

    Atmospheric new particle formation (NPF) is a common phenomenon all over the world. In this study we present the longest time series of NPF records in the eastern Mediterranean region by analyzing 10 years of aerosol number size distribution data obtained with a mobility particle sizer. The measurements were performed at the Finokalia environmental research station on Crete, Greece, during the period June 2008–June 2018. We found that NPF took place on 27 % of the available days, undefined days were 23 % and non-event days 50 %. NPF is more frequent in April and May probably due to the terrestrial biogenic activity and is less frequent in August. Throughout the period under study, nucleation was observed also during the night. Nucleation mode particles had the highest concentration in winter and early spring, mainly because of the minimum sinks, and their average contribution to the total particle number concentration was 8 %. Nucleation mode particle concentrations were low outside periods of active NPF and growth, so there are hardly any other local sources of sub-25 nm particles. Additional atmospheric ion size distribution data simultaneously collected for more than 2 years were also analyzed. Classification of NPF events based on ion spectrometer measurements differed from the corresponding classification based on a mobility spectrometer, possibly indicating a different representation of local and regional NPF events between these two measurement data sets. We used the MALTE-Box model for simulating a case study of NPF in the eastern Mediterranean region. Monoterpenes contributing to NPF can explain a large fraction of the observed NPF events according to our model simulations. However the adjusted parameterization resulting from our sensitivity tests was significantly different from the initial one that had been determined for the boreal environment.

  • Open Access English
    Authors: 
    Metzger, Swen; Abdelkader, Mohamed; Steil, Benedikt; Klingmüller, Klaus;
    Project: EC | EoCoE (676629), EC | C8 (226144)

    We scrutinize the importance of aerosol water for the aerosol optical depth (AOD) calculations using a long-term evaluation of the EQuilibrium Simplified Aerosol Model v4 for climate modeling. EQSAM4clim is based on a single solute coefficient approach that efficiently parameterizes hygroscopic growth, accounting for aerosol water uptake from the deliquescence relative humidity up to supersaturation. EQSAM4clim extends the single solute coefficient approach to treat water uptake of multicomponent mixtures. The gas–aerosol partitioning and the mixed-solution water uptake can be solved analytically, preventing the need for iterations, which is computationally efficient. EQSAM4clim has been implemented in the global chemistry climate model EMAC and compared to ISORROPIA II on climate timescales. Our global modeling results show that (I) our EMAC results of the AOD are comparable to modeling results that have been independently evaluated for the period 2000–2010, (II) the results of various aerosol properties of EQSAM4clim and ISORROPIA II are similar and in agreement with AERONET and EMEP observations for the period 2000–2013, and (III) the underlying assumptions on the aerosol water uptake limitations are important for derived AOD calculations. Sensitivity studies of different levels of chemical aging and associated water uptake show larger effects on AOD calculations for the year 2005 compared to the differences associated with the application of the two gas–liquid–solid partitioning schemes. Overall, our study demonstrates the importance of aerosol water for climate studies.

  • Open Access English
    Authors: 
    Schaller, Carsten; Kittler, Fanny; Foken, Thomas; Göckede, Mathias;
    Project: EC | PAGE21 (282700), EC | PERCCOM (333796)

    Methane (CH4) emissions from biogenic sources, such as Arctic permafrost wetlands, are associated with large uncertainties because of the high variability of fluxes in both space and time. This variability poses a challenge to monitoring CH4 fluxes with the eddy covariance (EC) technique, because this approach requires stationary signals from spatially homogeneous sources. Episodic outbursts of CH4 emissions, i.e. triggered by spontaneous outgassing of bubbles or venting of methane-rich air from lower levels due to shifts in atmospheric conditions, are particularly challenging to quantify. Such events typically last for only a few minutes, which is much shorter than the common averaging interval for EC (30 min). The steady-state assumption is jeopardised, which potentially leads to a non-negligible bias in the CH4 flux. Based on data from Chersky, NE Siberia, we tested and evaluated a flux calculation method based on wavelet analysis, which, in contrast to regular EC data processing, does not require steady-state conditions and is allowed to obtain fluxes over averaging periods as short as 1 min. Statistics on meteorological conditions before, during, and after the detected events revealed that it is atmospheric mixing that triggered such events rather than CH4 emission from the soil. By investigating individual events in more detail, we identified a potential influence of various mesoscale processes like gravity waves, low-level jets, weather fronts passing the site, and cold-air advection from a nearby mountain ridge as the dominating processes. The occurrence of extreme CH4 flux events over the summer season followed a seasonal course with a maximum in early August, which is strongly correlated with the maximum soil temperature. Overall, our findings demonstrate that wavelet analysis is a powerful method for resolving highly variable flux events on the order of minutes, and can therefore support the evaluation of EC flux data quality under non-steady-state conditions.

  • Open Access English
    Authors: 
    Ayarzagüena, Blanca; Palmeiro, Froila M.; Barriopedro, David; Calvo, Natalia; Langematz, Ulrike; Shibata, Kiyotaka;
    Project: EC | STRATOCLIM (603557)

    Major sudden stratospheric warmings (SSWs) represent one of the most abrupt phenomena of the boreal wintertime stratospheric variability, and constitute the clearest example of coupling between the stratosphere and the troposphere. A good representation of SSWs in climate models is required to reduce their biases and uncertainties in future projections of stratospheric variability. The ability of models to reproduce these phenomena is usually assessed with just one reanalysis. However, the number of reanalyses has increased in the last decade and their own biases may affect the model evaluation. Here we compare the representation of the main aspects of SSWs across reanalyses. The examination of their main characteristics in the pre- and post-satellite periods reveals that reanalyses behave very similarly in both periods. However, discrepancies are larger in the pre-satellite period compared to afterwards, particularly for the NCEP-NCAR reanalysis. All datasets reproduce similarly the specific features of wavenumber-1 and wavenumber-2 SSWs. A good agreement among reanalyses is also found for triggering mechanisms, tropospheric precursors, and surface response. In particular, differences in blocking precursor activity of SSWs across reanalyses are much smaller than between blocking definitions.

  • Open Access English
    Authors: 
    Radenz, Martin; Seifert, Patric; Baars, Holger; Floutsi, Athena Augusta; Yin, Zhenping; Bühl, Johannes;
    Project: EC | ACTRIS-2 (654109), EC | BACCHUS (603445)

    Height-resolved air mass source attribution is crucial for the evaluation of profiling ground-based remote sensing observations, especially when using lidar (light detection and ranging) to investigate different aerosol types throughout the atmosphere. Lidar networks, such as EARLINET (European Aerosol Research Lidar Network) in the frame of ACTRIS (Aerosol, Clouds and Trace Gases), observe profiles of optical aerosol properties almost continuously, but usually, additional information is needed to support the characterization of the observed particles. This work presents an approach explaining how backward trajectories or particle positions from a dispersion model can be combined with geographical information (a land cover classification and manually defined areas) to obtain a continuous and vertically resolved estimate of an air mass source above a certain location. Ideally, such an estimate depends on as few as possible a priori information and auxiliary data. An automated framework for the computation of such an air mass source is presented, and two applications are described. First, the air mass source information is used for the interpretation of air mass sources for three case studies with lidar observations from Limassol (Cyprus), Punta Arenas (Chile) and ship-borne off Cabo Verde. Second, air mass source statistics are calculated for two multi-week campaigns to assess potential observation biases of lidar-based aerosol statistics. Such an automated approach is a valuable tool for the analysis of short-term campaigns but also for long-term data sets, for example, acquired by EARLINET.

  • Open Access English
    Authors: 
    Mülmenstädt, Johannes; Gryspeerdt, Edward; Salzmann, Marc; Ma, Po-Lun; Dipu, Sudhakar; Quaas, Johannes;
    Project: EC | QUAERERE (306284)

    Using the method of offline radiative transfer modeling within the partial radiative perturbation (PRP) approach, the effective radiative forcing by aerosol–cloud interactions (ERFaci) in the ECHAM–HAMMOZ aerosol climate model is decomposed into a radiative forcing by anthropogenic cloud droplet number change and adjustments of the liquid water path and cloud fraction. The simulated radiative forcing by anthropogenic cloud droplet number change and liquid water path adjustment are of approximately equal magnitude at −0.52 and −0.53 W m−2, respectively, while the cloud-fraction adjustment is somewhat weaker at −0.31 W m−2 (constituting 38 %, 39 %, and 23 % of the total ERFaci, respectively); geographically, all three ERFaci components in the simulation peak over China, the subtropical eastern ocean boundaries, the northern Atlantic and Pacific oceans, Europe, and eastern North America (in order of prominence). Spatial correlations indicate that the temporal-mean liquid water path adjustment is proportional to the temporal-mean radiative forcing, while the relationship between cloud-fraction adjustment and radiative forcing is less direct. While the estimate of warm-cloud ERFaci is relatively insensitive to the treatment of ice and mixed-phase cloud overlying warm cloud, there are indications that more restrictive treatments of ice in the column result in a low bias in the estimated magnitude of the liquid water path adjustment and a high bias in the estimated magnitude of the droplet number forcing. Since the present work is the first PRP decomposition of the aerosol effective radiative forcing into radiative forcing and rapid cloud adjustments, idealized experiments are conducted to provide evidence that the PRP results are accurate. The experiments show that using low-frequency (daily or monthly) time-averaged model output of the cloud property fields underestimates the ERF, but 3-hourly mean output is sufficiently frequent.

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