Advanced search in
Research products
arrow_drop_down
Searching FieldsTerms
Any field
arrow_drop_down
includes
arrow_drop_down
Include:
109 Research products, page 1 of 11

  • Research data
  • Other research products
  • Atmospheric Chemistry and Physics (ACP)

10
arrow_drop_down
Relevance
arrow_drop_down
  • Open Access English
    Authors: 
    Kupiainen, Kaarle Juhana; Aamaas, Borgar; Savolahti, Mikko; Karvosenoja, Niko; Paunu, Ville-Veikko;
    Project: AKA | Novel Assessment of Black... (296644), AKA | Keeping the Arctic White:... (286699), EC | ECLIPSE (282688)

    We present a case study where emission metric values from different studies are applied to estimate global and Arctic temperature impacts of emissions from a northern European country. This study assesses the climate impact of Finnish air pollutants and greenhouse gas emissions from 2000 to 2010, as well as future emissions until 2030. We consider both emission pulses and emission scenarios. The pollutants included are SO2, NOx, NH3, non-methane volatile organic compound (NMVOC), black carbon (BC), organic carbon (OC), CO, CO2, CH4 and N2O, and our study is the first one for Finland to include all of them in one coherent dataset. These pollutants have different atmospheric lifetimes and influence the climate differently; hence, we look at different climate metrics and time horizons. The study uses the global warming potential (GWP and GWP*), the global temperature change potential (GTP) and the regional temperature change potential (RTP) with different timescales for estimating the climate impacts by species and sectors globally and in the Arctic. We compare the climate impacts of emissions occurring in winter and summer. This assessment is an example of how the climate impact of emissions from small countries and sources can be estimated, as it is challenging to use climate models to study the climate effect of national policies in a multi-pollutant situation. Our methods are applicable to other countries and regions and present a practical tool to analyze the climate impacts in multiple dimensions, such as assessing different sectors and mitigation measures. While our study focuses on short-lived climate forcers, we found that the CO2 emissions have the most significant climate impact, and the significance increases over longer time horizons. In the short term, emissions of especially CH4 and BC played an important role as well. The warming impact of BC emissions is enhanced during winter. Many metric choices are available, but our findings hold for most choices.

  • 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: EC | ACTRIS-2 (654109), EC | PyroTRACH (726165), EC | BACCHUS (603445), EC | RECAP (724602), NSF | Development, Validation, ... (1550816), EC | CRESCENDO (641816)

    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: 
    Hobe, Marc; Ploeger, Felix; Konopka, Paul; Kloss, Corinna; Ulanowski, Alexey; Yushkov, Vladimir; Ravegnani, Fabrizio; Volk, C. Michael; Pan, Laura L.; Honomichl, Shawn B.; +4 more
    Project: EC | STRATOCLIM (603557)

    Every year during the Asian summer monsoon season from about mid-June to early September, a stable anticyclonic circulation system forms over the Himalayas. This Asian summer monsoon (ASM) anticyclone has been shown to promote transport of air into the stratosphere from the Asian troposphere, which contains large amounts of anthropogenic pollutants. Essential details of Asian monsoon transport, such as the exact timescales of vertical transport, the role of convection in cross-tropopause exchange, and the main location and level of export from the confined anticyclone to the stratosphere are still not fully resolved. Recent airborne observations from campaigns near the ASM anticyclone edge and centre in 2016 and 2017, respectively, show a steady decrease in carbon monoxide (CO) and increase in ozone (O3) with height starting from tropospheric values of around 100 ppb CO and 30–50 ppb O3 at about 365 K potential temperature. CO mixing ratios reach stratospheric background values below ∼25 ppb at about 420 K and do not show a significant vertical gradient at higher levels, while ozone continues to increase throughout the altitude range of the aircraft measurements. Nitrous oxide (N2O) remains at or only marginally below its 2017 tropospheric mixing ratio of 333 ppb up to about 400 K, which is above the local tropopause. A decline in N2O mixing ratios that indicates a significant contribution of stratospheric air is only visible above this level. Based on our observations, we draw the following picture of vertical transport and confinement in the ASM anticyclone: rapid convective uplift transports air to near 16 km in altitude, corresponding to potential temperatures up to about 370 K. Although this main convective outflow layer extends above the level of zero radiative heating (LZRH), our observations of CO concentration show little to no evidence of convection actually penetrating the tropopause. Rather, further ascent occurs more slowly, consistent with isentropic vertical velocities of 0.7–1.5 K d−1. For the key tracers (CO, O3, and N2O) in our study, none of which are subject to microphysical processes, neither the lapse rate tropopause (LRT) around 380 K nor the cold point tropopause (CPT) around 390 K marks a strong discontinuity in their profiles. Up to about 20 to 35 K above the LRT, isolation of air inside the ASM anticyclone prevents significant in-mixing of stratospheric air (throughout this text, the term in-mixing refers specifically to mixing processes that introduce stratospheric air into the predominantly tropospheric inner anticyclone). The observed changes in CO and O3 likely result from in situ chemical processing. Above about 420 K, mixing processes become more significant and the air inside the anticyclone is exported vertically and horizontally into the surrounding stratosphere.

  • Open Access English
    Authors: 
    Dearden, Christopher; Hill, Adrian; Coe, Hugh; Choularton, Tom;
    Project: EC | DACCIWA (603502)

    Large-eddy simulations are performed to investigate the influence of cloud microphysics on the evolution of low-level clouds that form over southern West Africa during the monsoon season. We find that, even in clouds that are not precipitating, the size of cloud droplets has a non-negligible effect on liquid water path. This is explained through the effects of droplet sedimentation, which acts to remove liquid water from the entrainment zone close to cloud top, increasing the liquid water path. Sedimentation also produces a more heterogeneous cloud structure and lowers cloud base height. Our results imply that an appropriate parameterization of the effects of sedimentation is required to improve the representation of the diurnal cycle of the atmospheric boundary layer over southern West Africa in large-scale models.

  • Open Access English
    Authors: 
    Calmer, Radiance; Roberts, Gregory C.; Sanchez, Kevin J.; Sciare, Jean; Sellegri, Karine; Picard, David; Vrekoussis, Mihalis; Pikridas, Michael;
    Project: EC | BACCHUS (603445)

    In the framework of the EU-FP7 BACCHUS project, an intensive field campaign was performed in Cyprus (2015/03). Remotely Piloted Aircraft System (RPAS), ground-based instruments, and remote-sensing observations were operating in parallel to provide an integrated characterization of aerosol-cloud interactions. Remotely Piloted Aircraft (RPA) were equipped with a 5-hole probe, pyranometers, pressure, temperature and humidity sensors, and measured updraft velocity at cloud base and cloud optical properties of a stratocumulus layer. Ground-based measurements of dry aerosol size distributions and cloud condensation nuclei spectra, and RPA observations of vertical wind velocity and meteorological state parameters are used here to initialize an Aerosol–Cloud Parcel Model (ACPM) and compare the in situ observations of cloud optical properties measured by the RPA to those simulated in the ACPM. Two different cases are studied with the ACPM, including an adiabatic case and an entrainment case, in which the in-cloud temperature profile from RPA is taken into account. Adiabatic ACPM simulation yields cloud droplet number concentrations at cloud base (ca. 400 cm−3) that are similar to those derived from a Hoppel minimum analysis. Cloud optical properties have been inferred using the transmitted fraction of shortwave radiation profile measured by downwelling and upwelling pyranometers mounted on a RPA, and the observed transmitted fraction of solar radiation is then compared to simulations from the ACPM. ACPM simulations and RPA observations show better agreement when associated with entrainment compared to that of an adiabatic case. The mean difference between observed and adiabatic profiles of transmitted fraction of solar radiation is 0.12, while this difference is only 0.03 between observed and entrainment profiles. A sensitivity calculation is then conducted to quantify the relative impacts of two-fold changes in aerosol concentration, and updraft velocity to highlight the importance of accounting for the impact of entrainment in deriving cloud optical properties, as well as the ability of RPAs to leverage ground-based observations for studying aerosol–cloud interactions.

  • 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 II (283576), EC | MACC-III (633080)

    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: 
    Bednarz, Ewa M.; Maycock, Amanda C.; Telford, Paul J.; Braesicke, Peter; Abraham, N. Luke; Pyle, John A.;
    Project: EC | ACCI (267760)

    The 11-year solar cycle forcing is recognised as an important atmospheric forcing; however, there remain uncertainties in characterising the effects of solar variability on the atmosphere from observations and models. Here we present the first detailed assessment of the atmospheric response to the 11-year solar cycle in the UM-UKCA (Unified Model coupled to the United Kingdom Chemistry and Aerosol model) chemistry–climate model (CCM) using a three-member ensemble over the recent past (1966–2010). Comparison of the model simulations is made with satellite observations and reanalysis datasets. The UM-UKCA model produces a statistically significant response to the 11-year solar cycle in stratospheric temperatures, ozone and zonal winds. However, there are also differences in magnitude, spatial structure and timing of the signals compared to observational and reanalysis estimates. This could be due to deficiencies in the model performance, and so we include a critical discussion of the model limitations, and/or uncertainties in the current observational estimates of the solar cycle signals. Importantly, in contrast to many previous studies of the solar cycle impacts, we pay particular attention to the role of the chosen analysis method in UM-UKCA by comparing the model composite and a multiple linear regression (MLR) results. We show that the stratospheric solar responses diagnosed using both techniques largely agree with each other within the associated uncertainties; however, the results show that apparently different signals can be identified by the methods in the troposphere and in the tropical lower stratosphere. Lastly, we examine how internal atmospheric variability affects the detection of the 11-year solar responses in the model by comparing the results diagnosed from the three individual ensemble members (as opposed to those diagnosed from the full ensemble). We show overall agreement between the responses diagnosed for the ensemble members in the tropical and mid-latitude mid-stratosphere to lower mesosphere but larger apparent differences at Northern Hemisphere (NH) high latitudes during the dynamically active season. Our UM-UKCA results suggest the need for long data sets for confident detection of solar cycle impacts in the atmosphere, as well as for more research on possible interdependence of the solar cycle forcing with other atmospheric forcings and processes (e.g. Quasi-Biennial Oscillation, QBO; El Niño–Southern Oscillation, ENSO).

  • 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: 
    Gong, Xianda; Radenz, Martin; Wex, Heike; Seifert, Patric; Ataei, Farnoush; Henning, Silvia; Baars, Holger; Barja, Boris; Ansmann, Albert; Stratmann, Frank;
    Project: EC | BACCHUS (603445)

    The sources and abundance of ice-nucleating particles (INPs) that initiate cloud ice formation remain understudied, especially in the Southern Hemisphere. In this study, we present INP measurement taken close to Punta Arenas, Chile, at the southernmost tip of South America from May 2019 to March 2020, during the Dynamics, Aerosol, Clouds, and Precipitation in the Pristine Environment of the Southern Ocean (DACAPO-PESO) campaign. The highest ice nucleation temperature was observed at -3 °C, and from this temperature down to ~ -10 °C, a sharp increase of INP number concentration (NINP) was observed. Roughly 90 % and 80 % of INPs are proteinaceous-based biogenic particles at > -10 and -15 °C, respectively. NINP at Punta Arenas is much higher than that in the Southern Ocean, but comparable with agricultural area in Argentina and forestry environment in the US. Ice active surface site density (ns) is much higher than that for marine aerosol in the Southern Ocean, but comparable to English fertile soil dust. Parameterization based on particle number concentration in the size range larger than 500 nm (N>500nm) from the global average (DeMott et al., 2010) overestimate the measured INP, but the parameterization representing biological particles from a forestry environment (Tobo et al., 2013) yields NINP comparable to this study. No clear seasonal variation of NINP was observed. High precipitation is one of the most important meteorological parameters to enhance the NINP both in cold and warm seasons. A comparison of data from in-situ and lidar measurements showed good agreement for concentrations of large aerosol particles (> 500 nm) when assuming continental conditions for retrieval of the lidar data, suggesting that these particles were well mixed within the planetary boundary layer. This corroborates a continental origin of these particles, consistent with the results from our INP source analysis. Overall, we suggest that high NINP of biogenic INPs originated from terrestrial sources and were added to the marine air masses during the overflow of a maximum of roughly 150 km of land before arriving at the measurement station.

  • Open Access English
    Authors: 
    Luo, Yuanyuan; Garmash, Olga; Li, Haiyan; Graeffe, Frans; Praplan, Arnaud P.; Liikanen, Anssi; Zhang, Yanjun; Meder, Melissa; Peräkylä, Otso; Peñuelas, Josep; +2 more
    Project: EC | IMBALANCE-P (610028)

    Diterpenes (C20H32) are biogenically emitted volatile compounds that only recently have been observed in ambient air. They are expected to be highly reactive, and their oxidation is likely to form condensable vapors. However, until now, no studies have investigated gas-phase diterpene oxidation. In this paper, we explored the ozonolysis of a diterpene, ent-kaurene, in a simulation chamber. Using state-of-the-art mass spectrometry, we characterized diterpene oxidation products for the first time, and we identified several products with varying oxidation levels, including highly oxygenated organic molecules (HOM), monomers, and dimers. The most abundant monomers measured using a nitrate chemical ionization mass spectrometer were C19H28O8 and C20H30O5, and the most abundant dimers were C38H60O6 and C39H62O6. The exact molar yield of HOM from kaurene ozonolysis was hard to quantify due to uncertainties in both the kaurene and HOM concentrations, but our best estimate was a few percent, which is similar to values reported earlier for many monoterpenes. We also monitored the decrease in the gas-phase oxidation products in response to an increased condensation sink in the chamber to deduce their affinity to condense. The oxygen content was a critical parameter affecting the volatility of products, with four to five O atoms needed for the main monomeric species to condense onto 80 nm particles. Finally, we report on the observed fragmentation and clustering patterns of kaurene in a Vocus proton-transfer-reaction time-of-flight mass spectrometer. Our findings highlight similarities and differences between diterpenes and smaller terpenes during their atmospheric oxidation, but more studies on different diterpenes are needed for a broader view of their role in atmospheric chemistry.

Send a message
How can we help?
We usually respond in a few hours.