| 1. |
- Burgos, Maria A., et al.
(författare)
-
A global model-measurement evaluation of particle light scattering coefficients at elevated relative humidity
- 2020
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:17, s. 10231-10258
-
Tidskriftsartikel (refereegranskat)abstract
- The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties, which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model-measurement evaluation of the particle light scattering enhancement factor f (RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f (RH) amongst the different models, which can not be explained by the site types. Based on our evaluation of sea salt scattering enhancement and simulated organic mass fraction, there is a strong indication that differences in the model parameterizations of hygroscopicity and model chemistry are driving at least some of the observed diversity in simulated f (RH). Additionally, a key point is that defining dry conditions is difficult from an observational point of view and, depending on the aerosol, may influence the measured f (RH). The definition of dry also impacts our model evaluation, because several models exhibit significant water uptake between RH = 0% and 40 %. The multisite average ratio between model outputs and measurements is 1.64 when RH = 0% is assumed as the model dry RH and 1.16 when RH = 40% is the model dry RH value. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e., not fully dried particles and hysteresis effects). This will be particularly relevant when a location is dominated by a deliquescent aerosol such as sea salt. Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms. Recommendations for future model-measurement evaluation and model improvements are provided.
|
|
| 2. |
- Cremer, Roxana, 1993-, et al.
(författare)
-
Investigating the role of air mass history on the diversity of GCMestimates of atmospheric black carbon in the Arctic
-
Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Black Carbon (BC) aerosols are known to play an important role in the Arctic, yet their exact contribution to thechanging of the Earth’s climate and Arctic amplification remains unclear. To reduce these uncertainties, the life cycle of BCneeds to be accurately described in general circulation models (GCMs). In this study, four GCMs (ECHAM6.3-HAM2.3,ECHAM6.3-HAM2.3-P3, ECHAM6.3-HAM2.3-SALSA2 and UKESM1.0) are compared in terms of their representation ofBC in the Arctic. A new Lagrangian framework is applied to investigate the history of airmasses reaching the Arctic observationalsite Zeppelin on Svalbard, and compared to the corresponding transport simulated by the GCMs, which are allnudged to reanalysis data from ERA-Interim. Aerosol processes along the trajectories are then compared between the models.ECHAM6.3-HAM2.3-P3 simulates the highest and UKESM1.0 the lowest BC loadings both globally and within the Arcticand ECHAM6.3-HAM2.3-SALSA2 is the GCM that reproduces the observations from Zeppelin station most faithfully. The BC concentration in the Arctic is largely controlled by the wet removal processes described in the models, but dry depositionalso plays a role in explaining some of the inter-model diversity. ECHAM6.3-HAM2.3-P3 is less efficient in wet removal thanthe other models, which is likely a result of an adjusted representation of ice processes compared with the other two ECHAMvariants. UKESM1.0 is the most efficient model in removing BC from the atmosphere, in large part due to more efficient dryremoval than with the ECHAM models. The Lagrangian analysis reveals that the BC concentrations at the Zeppelin station are largely determined by concentrations in airmasses older than the length of our back trajectories, i.e. ten days, highlighting theimportance of remote emissions to local BC concentrations in the Arctic. This further suggests a longer BC lifetime within theArctic as compared with the global average. Our results underline the importance of accurate descriptions of cloud and precipitation microphysics, along with realistic dry and wet scavenging schemes for improved descriptions of BC and its climateimpacts in the Arctic within GCMs.
|
|
| 3. |
- Ghan, Steven, et al.
(författare)
-
Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability
- 2016
-
Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 113:21, s. 5804-5811
-
Tidskriftsartikel (refereegranskat)abstract
- A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing.
|
|
| 4. |
- Isokääntä, Sini, et al.
(författare)
-
The effect of clouds and precipitation on the aerosol concentrations and composition in a boreal forest environment
- 2022
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:17, s. 11823-11843
-
Tidskriftsartikel (refereegranskat)abstract
- Atmospheric aerosol particle concentrations are strongly affected by various wet processes, including below and in-cloud wet scavenging and in-cloud aqueous-phase oxidation. We studied how wet scavenging and cloud processes affect particle concentrations and composition during transport to a rural boreal forest site in northern Europe. For this investigation, we employed air mass history analysis and observational data. Long-term particle number size distribution (∼15 years) and composition measurements (∼8 years) were combined with air mass trajectories with relevant variables from reanalysis data. Some such variables were rainfall rate, relative humidity, and mixing layer height. Additional observational datasets, such as temperature and trace gases, helped further evaluate wet processes along trajectories with mixed effects models.All chemical species investigated (sulfate, black carbon, and organics) exponentially decreased in particle mass concentration as a function of accumulated precipitation along the air mass route. In sulfate (SO4) aerosols, clear seasonal differences in wet removal emerged, whereas organics (Org) and equivalent black carbon (eBC) exhibited only minor differences. The removal efficiency varied slightly among the different reanalysis datasets (ERA-Interim and Global Data Assimilation System; GDAS) used for the trajectory calculations due to the difference in the average occurrence of precipitation events along the air mass trajectories between the reanalysis datasets.Aqueous-phase processes were investigated by using a proxy for air masses travelling inside clouds. We compared air masses with no experience of approximated in-cloud conditions or precipitation during the past 24 h to air masses recently inside non-precipitating clouds before they entered SMEAR II (Station for Measuring Ecosystem–Atmosphere Relations). Significant increases in SO4 mass concentration were observed for the latter air masses (recently experienced non-precipitating clouds).Our mixed effects model considered other contributing factors affecting particle mass concentrations in SMEAR II: examples were trace gases, local meteorology, and diurnal variation. This model also indicated in-cloud SO4 production. Despite the reanalysis dataset used in the trajectory calculations, aqueous-phase SO4 formation was observed. Particle number size distribution measurements revealed that most of the in-cloud SO4 formed can be attributed to particle sizes larger than 200 nm (electrical mobility diameter). Aqueous-phase secondary organic aerosol (aqSOA) formation was non-significant.
|
|
| 5. |
- Zhang, Shipeng, et al.
(författare)
-
On the characteristics of aerosol indirect effect based on dynamic regimes in global climate models
- 2016
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:5, s. 2765-2783
-
Tidskriftsartikel (refereegranskat)abstract
- Aerosol-cloud interactions continue to constitute a major source of uncertainty for the estimate of climate radiative forcing. The variation of aerosol indirect effects (AIE) in climate models is investigated across different dynamical regimes, determined by monthly mean 500 hPa vertical pressure velocity (omega(500)), lower-tropospheric stability (LTS) and large-scale surface precipitation rate derived from several global climate models (GCMs), with a focus on liquid water path (LWP) response to cloud condensation nuclei (CCN) concentrations. The LWP sensitivity to aerosol perturbation within dynamic regimes is found to exhibit a large spread among these GCMs. It is in regimes of strong large-scale ascent (omega(500)aEuro-aEuro parts per thousand < aEuro-a'25 hPa day(-1)) and low clouds (stratocumulus and trade wind cumulus) where the models differ most. Shortwave aerosol indirect forcing is also found to differ significantly among different regimes. Shortwave aerosol indirect forcing in ascending regimes is close to that in subsidence regimes, which indicates that regimes with strong large-scale ascent are as important as stratocumulus regimes in studying AIE. It is further shown that shortwave aerosol indirect forcing over regions with high monthly large-scale surface precipitation rate (> 0.1 mm day(-1)) contributes the most to the total aerosol indirect forcing (from 64 to nearly 100 %). Results show that the uncertainty in AIE is even larger within specific dynamical regimes compared to the uncertainty in its global mean values, pointing to the need to reduce the uncertainty in AIE in different dynamical regimes.
|
|
