| 31. |
- Collaud Coen, Martine, et al.
(författare)
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Multidecadal trend analysis of in situ aerosol radiative properties around the world
- 2020
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:14, s. 8867-8908
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Tidskriftsartikel (refereegranskat)abstract
- In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Angstrom exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann-Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010-2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient - there is a shift to statistically significant negative trends in 2009-2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes.
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| 32. |
- David, Robert, et al.
(författare)
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The role of contact angle and pore width on pore condensation and freezing
- 2020
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:15, s. 9419-9440
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Tidskriftsartikel (refereegranskat)abstract
- It has recently been shown that pore condensation and freezing (PCF) is a mechanism responsible for ice formation under cirrus cloud conditions. PCF is defined as the condensation of liquid water in narrow capillaries below water saturation due to the inverse Kelvin effect, followed by either heterogeneous or homogeneous nucleation depending on the temperature regime and presence of an ice-nucleating active site. By using sol-gel synthesized silica with well-defined pore diameters, morphology and distinct chemical surface-functionalization, the role of the water-silica contact angle and pore width on PCF is investigated. We find that for the pore diameters (2.2-9.2 nm) and water contact angles (15-78ĝ) covered in this study, our results reveal that the water contact angle plays an important role in predicting the humidity required for pore filling, while the pore diameter determines the ability of pore water to freeze. For T>235 K and below water saturation, pore diameters and water contact angles were not able to predict the freezing ability of the particles, suggesting an absence of active sites; thus ice nucleation did not proceed via a PCF mechanism. Rather, the ice-nucleating ability of the particles depended solely on chemical functionalization. Therefore, parameterizations for the ice-nucleating abilities of particles in cirrus conditions should differ from parameterizations at mixed-phase clouds conditions. Our results support PCF as the atmospherically relevant ice nucleation mechanism below water saturation when porous surfaces are encountered in the troposphere. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
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| 33. |
- Espen Yttri, Karl, et al.
(författare)
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Trends, composition, and sources of carbonaceous aerosol at the Birkenes Observatory, northern Europe, 2001-2018
- 2021
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:9, s. 7149-7170
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Tidskriftsartikel (refereegranskat)abstract
- We present 18 years (2001-2018) of aerosol measurements, including organic and elemental carbon (OC and EC), organic tracers (levoglucosan, arabitol, mannitol, trehalose, glucose, and 2-methyltetrols), trace elements, and ions, at the Birkenes Observatory (southern Norway) - a site representative of the northern European region. The OC=EC (2001-2018) and the levoglucosan (2008-2018) time series are the longest in Europe, with OC=EC available for the PM10, PM2:5 (fine), and PM10-2:5 (coarse) size fractions, providing the opportunity for a nearly 2-decade-long assessment. Using positive matrix factorization (PMF), we identify seven carbonaceous aerosol sources at Birkenes: mineraldust- dominated aerosol (MIN), traffic/industry-like aerosol (TRA/IND), short-range-transported biogenic secondary organic aerosol (BSOASRT), primary biological aerosol particles (PBAP), biomass burning aerosol (BB), ammoniumnitrate- dominated aerosol (NH4NO3), and (one low carbon fraction) sea salt aerosol (SS). We observed significant (p < 0:05), large decreases in EC in PM10 (-3:9%yr-1) and PM2:5 (-4:2%yr-1) and a smaller decline in levoglucosan (-2:8%yr-1), suggesting that OC=EC from traffic and industry is decreasing, whereas the abatement of OC=EC from biomass burning has been slightly less successful. EC abatement with respect to anthropogenic sources is further supported by decreasing EC fractions in PM2:5 (-3:9%yr-1) and PM10 (-4:5%yr-1). PMF apportioned 72% of EC to fossil fuel sources; this was further supported by PMF applied to absorption photometer data, which yielded a two-factor solution with a low aerosol ngstr m exponent (AAED0.93) fraction, assumed to be equivalent black carbon from fossil fuel combustion (eBCFF), contributing 78% to eBC mass. The higher AAE fraction (AAED2.04) is likely eBC from BB (eBCBB). Source-receptor model calculations (FLEXPART) showed that continental Europe and western Russia were the main source regions of both elevated eBCBB and eBCFF. Dominating biogenic sources explain why there was no downward trend for OC. A relative increase in the OC fraction in PM2:5 (C3:2%yr-1) and PM10 (C2:4%yr-1) underscores the importance of biogenic sources at Birkenes (BSOA and PBAP), which were higher in the vegetative season and dominated both fine (53 %) and coarse (78 %) OC. Furthermore, 77 %-91% of OC in PM2:5, PM10-2:5, and PM10 was attributed to biogenic sources in summer vs. 22 %- 37% in winter. The coarse fraction had the highest share of biogenic sources regardless of season and was dominated by PBAP, except in winter. Our results show a shift in the aerosol composition at Birkenes and, thus, also in the relative source contributions. The need for diverse offline and online carbonaceous aerosol speciation to understand carbonaceous aerosol sources, including their seasonal, annual, and long-term variability, has been demonstrated.
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| 34. |
- Flood, Victoria A., et al.
(författare)
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Evaluating modelled tropospheric columns of CH4, CO, and O3 in the Arctic using ground-based Fourier transform infrared (FTIR) measurements
- 2024
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Ingår i: Atmospheric Chemistry and Physics. - 1680-7316 .- 1680-7324. ; 24:2, s. 1079-1118
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Tidskriftsartikel (refereegranskat)abstract
- This study evaluates tropospheric columns of methane, carbon monoxide, and ozone in the Arctic simulated by 11 models. The Arctic is warming at nearly 4 times the global average rate, and with changing emissions in and near the region, it is important to understand Arctic atmospheric composition and how it is changing. Both measurements and modelling of air pollution in the Arctic are difficult, making model validation with local measurements valuable. Evaluations are performed using data from five high-latitude ground-based Fourier transform infrared (FTIR) spectrometers in the Network for the Detection of Atmospheric Composition Change (NDACC). The models were selected as part of the 2021 Arctic Monitoring and Assessment Programme (AMAP) report on short-lived climate forcers. This work augments the model-measurement comparisons presented in that report by including a new data source: column-integrated FTIR measurements, whose spatial and temporal footprint is more representative of the free troposphere than in situ and satellite measurements. Mixing ratios of trace gases are modelled at 3-hourly intervals by CESM, CMAM, DEHM, EMEP MSC-W, GEM-MACH, GEOS-Chem, MATCH, MATCH-SALSA, MRI-ESM2, UKESM1, and WRF-Chem for the years 2008, 2009, 2014, and 2015. The comparisons focus on the troposphere (0-7km partial columns) at Eureka, Canada; Thule, Greenland; Ny Ålesund, Norway; Kiruna, Sweden; and Harestua, Norway. Overall, the models are biased low in the tropospheric column, on average by -9.7% for CH4, -21% for CO, and -18% for O3. Results for CH4 are relatively consistent across the 4 years, whereas CO has a maximum negative bias in the spring and minimum in the summer and O3 has a maximum difference centered around the summer. The average differences for the models are within the FTIR uncertainties for approximately 15% of the model-location comparisons.
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| 35. |
- Flynn, Clare Marie, et al.
(författare)
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On the climate sensitivity and historical warming evolution in recent coupled model ensembles
- 2020
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:13, s. 7829-7842
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Tidskriftsartikel (refereegranskat)abstract
- The Earth's equilibrium climate sensitivity (ECS) to a doubling of atmospheric CO2, along with the transient climate response (TCR) and greenhouse gas emissions pathways, determines the amount of future warming. Coupled climate models have in the past been important tools to estimate and understand ECS. ECS estimated from Coupled Model Intercomparison Project Phase 5 (CMIP5) models lies between 2.0 and 4.7 K (mean of 3.2 K), whereas in the latest CMIP6 the spread has increased to 1.8-5.5 K (mean of 3.7 K), with 5 out of 25 models exceeding 5 K. It is thus pertinent to understand the causes underlying this shift. Here we compare the CMIP5 and CMIP6 model ensembles and find a systematic shift between CMIP eras to be unexplained as a process of random sampling from modeled forcing and feedback distributions. Instead, shortwave feedbacks shift towards more positive values, in particular over the Southern Ocean, driving the shift towards larger ECS values in many of the models. These results suggest that changes in model treatment of mixed-phase cloud processes and changes to Antarctic sea ice representation are likely causes of the shift towards larger ECS. Somewhat surprisingly, CMIP6 models exhibit less historical warming than CMIP5 models, despite an increase in TCR between CMIP eras (mean TCR increased from 1.7 to 1.9 K). The evolution of the warming suggests, however, that several of the CMIP6 models apply too strong aerosol cooling, resulting in too weak mid-20th century warming compared to the instrumental record.
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| 36. |
- Flynn, Clare Marie, et al.
(författare)
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Strong aerosol cooling alone does not explain cold-biased mid-century temperatures in CMIP6 models
- 2023
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus Publications. - 1680-7316 .- 1680-7324. ; 23:23, s. 15121-15133
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Tidskriftsartikel (refereegranskat)abstract
- The current generation of global climate models from the Coupled Model Intercomparison Project Phase 6 (CMIP6) exhibits a surprisingly cold-biased ensemble-mean mid-20th century global-mean surface temperature anomaly, compared to the previous generation Phase 5 (CMIP5) and to the observed mid-century (1940-1970) temperature anomaly. Most CMIP6 models, 31 of 36 models in contrast to 17 of 27 CMIP5 models, are colder than the uncertainty range of the observed anomaly, indicating that the CMIP6 suppressed warming is not caused by a few cold models. However, no clear cause that sufficiently explains the tendency towards suppressed mid-20th century warming emerges. Whereas models that best match observations exclusively exhibit weaker aerosol forcing than that exhibited by colder models, there is not a clear relationship between mid-century temperatures and aerosol forcing. Likewise, no systematic differences emerge among other model aerosol representations, such as inclusion of aerosol-cloud interactions for ice clouds in the model or the type of aerosol model input data set used, nor variations in greenhouse gas forcing or climate sensitivity, that could explain the suppressed warming. This indicates the presence of another cause, or more likely a set of causes, of the suppressed warming in many CMIP6 models. Thus, the prospect of a strong constraint on present-day aerosol forcing based on the mid-century warming is weakened, even if it is encouraging that those models that do match the observed warming best all have relatively weak aerosol forcing.
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| 37. |
- Frey, Lena, et al.
(författare)
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Processes controlling the vertical aerosol distribution in marine stratocumulus regions - a sensitivity study using the climate model NorESM1-M
- 2021
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:1, s. 577-595
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Tidskriftsartikel (refereegranskat)abstract
- The vertical distribution of aerosols plays an important role in determining the effective radiative forcing from aerosol–radiation and aerosol–cloud interactions. Here, a number of processes controlling the vertical distribution of aerosol in five subtropical marine stratocumulus regions in the climate model NorESM1-M are investigated, with a focus on the total aerosol extinction. A comparison with satellite lidar data (CALIOP, Cloud–Aerosol Lidar with Orthogonal Polarization) shows that the model underestimates aerosol extinction throughout the troposphere, especially elevated aerosol layers in the two regions where they are seen in observations. It is found that the shape of the vertical aerosol distribution is largely determined by the aerosol emission and removal processes in the model, primarily through the injection height, emitted particle size, and wet scavenging. In addition, the representation of vertical transport related to shallow convection and entrainment is found to be important, whereas alterations in aerosol optical properties and cloud microphysics parameterizations have smaller effects on the vertical aerosol extinction distribution. However, none of the alterations made are sufficient for reproducing the observed vertical distribution of aerosol extinction, neither in magnitude nor in shape. Interpolating the vertical levels of CALIOP to the corresponding model levels leads to better agreement in the boundary layer and highlights the importance of the vertical resolution.
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| 38. |
- Frostenberg, Hannah, 1989, et al.
(författare)
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The chance of freezing - a conceptional study to parameterize temperature-dependent freezing by including randomness of ice-nucleating particle concentrations
- 2023
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Ingår i: ATMOSPHERIC CHEMISTRY AND PHYSICS. - 1680-7316 .- 1680-7324. ; 23:19, s. 10883-10900
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Tidskriftsartikel (refereegranskat)abstract
- Ice-nucleating particle concentrations (INPCs) can spread over several orders of magnitude at any given temperature. However, this variability is rarely accounted for in heterogeneous ice-nucleation parameterizations. In this paper, we present an approach to incorporate the random variation in the INPC into the parameterization of immersion freezing and analyze this novel concept with various sensitivity tests. In the new scheme, the INPC is drawn from a relative frequency distribution of cumulative INPCs. At each temperature, this distribution describing the INPCs is expressed as a lognormal frequency distribution. The new parameterization scheme does not require aerosol information from the driving model to represent the heterogeneity of INPCs. The scheme's performance is tested in a large-eddy simulation of a relatively warm Arctic mixed-phase stratocumulus. We find that it leads to reasonable ice masses in the cloud, especially when compared to immersion freezing schemes that yield one fixed INPC per temperature and lead to almost no ice production in the simulated cloud. The scheme is sensitive to the median of the frequency distribution and highly sensitive to the standard deviation of the distribution, as well as to the frequency of drawing a new INPC and the resolution of the model. Generally, a higher probability of drawing large INPCs leads to substantially more ice in the simulated cloud. We expose inherent challenges to introducing such a parameterization and explore possible solutions and potential developments.
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| 39. |
- Gao, Linyu, et al.
(författare)
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Kinetics, SOA yields, and chemical composition of secondary organic aerosol from β-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K
- 2022
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:9, s. 6001-6020
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Tidskriftsartikel (refereegranskat)abstract
- β-caryophyllene (BCP) is one of the most important sesquiterpenes (SQTs) in the atmosphere, with a large potential contribution to secondary organic aerosol (SOA) formation mainly from reactions with ozone (O3) and nitrate radicals (NO3). In this work, we study the temperature dependence of the kinetics of BCP ozonolysis, SOA yields, and SOA chemical composition in the dark and in the absence and presence of nitrogen oxides including nitrate radicals (NO3). We cover a temperature range of 213–313 K, representative of tropospheric conditions. The oxidized components in both gas and particle phases were characterized on a molecular level by a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols using iodide as the reagent ion (FIGAERO-iodide-CIMS). The batch mode experiments were conducted in the 84.5 m3 aluminium simulation chamber AIDA at the Karlsruhe Institute of Technology (KIT). In the absence of nitrogen oxides, the temperature-dependent rate coefficient of the endocyclic double bond in BCP reacting with ozone between 243–313 K is negatively correlated with temperature, corresponding to the following Arrhenius equation: k= (1.6 ± 0.4) × 10−15 × exp((559 ± 97)/T). The SOA yields increase from 16 ± 5 % to 37 ± 11 %, with temperatures decreasing from 313 to 243 K at a total organic particle mass of 10 µg m−3. The variation in the ozonolysis temperature leads to a substantial impact on the abundance of individual organic molecules. In the absence of nitrogen oxides, monomers C14−15H22−24O3−7 (37.4 %), dimers C28−30H44−48O5−9 (53.7 %), and trimers C41−44H62−66O9−11 (8.6 %) are abundant in the particle phase at 213 K. At 313 K, we observed more oxidized monomers (mainly C14−15H22−24O6−9, 67.5 %) and dimers (mainly C27−29H42−44O9−11, 27.6 %), including highly oxidized molecules (HOMs; C14H22O7,9, C15H22O7,9C15H24O7,9), which can be formed via hydrogen shift mechanisms, but no significant trimers. In the presence of nitrogen oxides, the organonitrate fraction increased from 3 % at 213 K to 12 % and 49 % at 243 and 313 K, respectively. Most of the organonitrates were monomers with C15 skeletons and only one nitrate group. More highly oxygenated organonitrates were observed at higher temperatures, with their signal-weighted O:C atomic ratio increasing from 0.41 to 0.51 from 213 to 313 K. New dimeric and trimeric organic species without nitrogen atoms (C20, C35) were formed in the presence of nitrogen oxides at 298–313 K, indicating potential new reaction pathways. Overall, our results show that increasing temperatures lead to a relatively small decrease in the rate coefficient of the endocyclic double bond in BCP reacting with ozone but to a strong decrease in SOA yields. In contrast, the formation of HOMs and organonitrates increases significantly with temperature.
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| 40. |
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