Aerosol-radiation Interactions Research Articles

Projected near-term changes in three types of heat waves over China under RCP4.5

The changes in three aspects of frequency, intensity and duration of the compound, daytime and nighttime heat waves (HWs) over China during extended summer (May–September) in a future period of the mid-21st century (FP; 2045–2055) under RCP4.5 scenario relative to present day (PD; 1994–2011) are investigated by two models, MetUM-GOML1 and MetUM-GOML2, which comprise the atmospheric components of two state-of-the-art climate models coupled to a multi-level mixed-layer ocean model. The results show that in the mid-21st century all three types of HWs in China will occur more frequently with strengthened intensity and elongated duration relative to the PD. The compound HWs will change most dramatically, with the frequency in the FP being 4–5 times that in the PD, and the intensity and duration doubling those in the PD. The changes in daytime and nighttime HWs are also remarkable, with the changes of nighttime HWs larger than those of daytime HWs. The future changes of the three types of HWs in China in two models are similar in terms of spatial patterns and area-averaged quantities, indicating these projected changes of HWs over the China under RCP4.5 scenario are robust. Further analyses suggest that projected future changes in HWs over China are determined mainly by the increase in seasonal mean surface air temperatures with change in temperature variability playing a minor role. The seasonal mean temperature increase is due to the increase in surface downward longwave radiation and surface shortwave radiation. The increase in downward longwave radiation results from the enhanced greenhouse effect and increased water vapour in the atmosphere. The increase in surface shortwave radiation is the result of the decreased aerosol emissions, via direct aerosol–radiation interaction and indirect aerosol–cloud interaction over southeastern and northeastern China, and the reduced cloud cover related to a decrease in relative humidity.

Global aerosol modeling with MADE3 (v3.0) in EMAC (based on v2.53): model description and evaluation

Abstract. Recently, the aerosol microphysics submodel MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, third generation) was introduced as a successor to MADE and MADE-in. It includes nine aerosol species and nine lognormal modes to represent aerosol particles of three different mixing states throughout the aerosol size spectrum. Here, we describe the implementation of the most recent version of MADE3 into the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model, including a detailed evaluation of a 10-year aerosol simulation with MADE3 as part of EMAC. We compare simulation output to station network measurements of near-surface aerosol component mass concentrations, to airborne measurements of aerosol mass mixing ratio and number concentration vertical profiles, to ground-based and airborne measurements of particle size distributions, and to station network and satellite measurements of aerosol optical depth. Furthermore, we describe and apply a new evaluation method, which allows a comparison of model output to size-resolved electron microscopy measurements of particle composition. Although there are indications that fine-mode particle deposition may be underestimated by the model, we obtained satisfactory agreement with the observations. Remaining deviations are of similar size to those identified in other global aerosol model studies. Thus, MADE3 can be considered ready for application within EMAC. Due to its detailed representation of aerosol mixing state, it is especially useful for simulating wet and dry removal of aerosol particles, aerosol-induced formation of cloud droplets and ice crystals as well as aerosol–radiation interactions. Besides studies on these fundamental processes, we also plan to use MADE3 for a reassessment of the climate effects of anthropogenic aerosol perturbations.

The impact of aerosol–radiation interactions on the effectiveness of emission control measures

Temporary emission control measures in Beijing and surrounding regions have become a prevailing practice to ensure good air quality for major events (e.g. the Asia-Pacific Economic Cooperation (APEC) Summit on 5–11 November 2014) and to mitigate the severity of coming pollution episodes. Since PM2.5 affects meteorology via aerosol–meteorology interactions, a question arises how these interactions may impact the response of PM2.5 to emission reductions and thus the effectiveness of emission control measures. Here we use the coupled meteorology-chemistry model WRF-Chem to investigate this issue with focus on aerosol–radiation interactions (ARI) for the APEC week and three more polluted episodes over North China. We find a quadratic relationship between PM2.5 concentration changes due to emission reductions and PM2.5 levels, instead of an approximately linear response in the absence of ARI. The ARI effects could only change the effectiveness of emission control by 6.7% during APEC in Beijing, but reach 21.9% under more polluted conditions. Our results reveal that ARI can strongly affect the attribution of PM2.5 variability to emission changes and meteorology, and is thus important for assessing the effectiveness of emission control measures.

Solar “brightening” impact on summer surface ozone between 1990 and 2010 in Europe – a model sensitivity study of the influence of the aerosol–radiation interactions

Abstract. Surface solar radiation (SSR) observations have indicated an increasing trend in Europe since the mid-1980s, referred to as solar “brightening”. In this study, we used the regional air quality model, CAMx (Comprehensive Air Quality Model with Extensions) to simulate and quantify, with various sensitivity runs (where the year 2010 served as the base case), the effects of increased radiation between 1990 and 2010 on photolysis rates (with the PHOT1, PHOT2 and PHOT3 scenarios, which represented the radiation in 1990) and biogenic volatile organic compound (BVOC) emissions (with the BIO scenario, which represented the biogenic emissions in 1990), and their consequent impacts on summer surface ozone concentrations over Europe between 1990 and 2010. The PHOT1 and PHOT2 scenarios examined the effect of doubling and tripling the anthropogenic PM2.5 concentrations, respectively, while the PHOT3 investigated the impact of an increase in just the sulfate concentrations by a factor of 3.4 (as in 1990), applied only to the calculation of photolysis rates. In the BIO scenario, we reduced the 2010 SSR by 3 % (keeping plant cover and temperature the same), recalculated the biogenic emissions and repeated the base case simulations with the new biogenic emissions. The impact on photolysis rates for all three scenarios was an increase (in 2010 compared to 1990) of 3–6 % which resulted in daytime (10:00–18:00 Local Mean Time – LMT) mean surface ozone differences of 0.2–0.7 ppb (0.5–1.5 %), with the largest hourly difference rising as high as 4–8 ppb (10–16 %). The effect of changes in BVOC emissions on daytime mean surface ozone was much smaller (up to 0.08 ppb, ∼ 0.2 %), as isoprene and terpene (monoterpene and sesquiterpene) emissions increased only by 2.5–3 and 0.7 %, respectively. Overall, the impact of the SSR changes on surface ozone was greater via the effects on photolysis rates compared to the effects on BVOC emissions, and the sensitivity test of their combined impact (the combination of PHOT3 and BIO is denoted as the COMBO scenario) showed nearly additive effects. In addition, all the sensitivity runs were repeated on a second base case with increased NOx emissions to account for any potential underestimation of modeled ozone production; the results did not change significantly in magnitude, but the spatial coverage of the effects was profoundly extended. Finally, the role of the aerosol–radiation interaction (ARI) changes in the European summer surface ozone trends was suggested to be more important when comparing to the order of magnitude of the ozone trends instead of the total ozone concentrations, indicating a potential partial damping of the effects of ozone precursor emissions' reduction.

Anthropogenic impacts on recent decadal change in temperature extremes over China: relative roles of greenhouse gases and anthropogenic aerosols

Observational analysis indicates significant changes in some temperature extremes over China across the mid-1990s. The decadal changes in hot extremes are characterized as a rise in annual hottest day and night temperature (TXx and TNx) and an increase in frequencies of summer days (SU) and tropical night (TR). The decadal changes in cold extremes are distinguished by a rise in annual coldest day and night temperature (TXn and TNn) and a decrease in frequencies of ice days (ID) and frost days (FD). These decadal changes manifest not only over China as a whole, but also over individual climate sub-regions. An atmosphere-ocean-mixed-layer coupled model forced by changes in greenhouse gases (GHG) concentrations and anthropogenic aerosol (AA) emissions realistically reproduces the general spatial patterns and magnitudes of observed changes in both hot and cold extremes across the mid-1990s, suggesting a pronounced role of anthropogenic changes in these observed decadal changes. Separately, changes in GHG forcing lead to rise in TXx, TNx, TXn and TNn, increase in frequencies of SU and TR and decrease in frequencies of ID and FD over China through increased Greenhouse Effect with positive clear sky longwave radiation and play a dominant role in simulated changes of both hot and cold extremes over China. The AA forcing changes tend to cool Southern China and warm Northern China during summer via aerosol-radiation interaction and AA-induced atmosphere-cloud feedback and therefore lead to some weak decrease in hot extremes over Southeastern China and increase over Northern China. Meanwhile, AA changes lead to warming over China during winter through cloud feedbacks related to aerosol induced cooling over tropical Indian Ocean and western tropical Pacific, and also induce changes in cold extremes the same sign as those induced by GHG, but with weak magnitude.

Dust Impacts on the 2012 Hurricane Nadine Track during the NASA HS3 Field Campaign.

During the 2012 deployment of the NASA Hurricane and Severe Storm Sentinel (HS3) field campaign, several flights were dedicated to investigating Hurricane Nadine. Hurricane Nadine developed in close proximity to the dust-laden Saharan Air Layer, and is the fourth longest-lived Atlantic hurricane on record, experiencing two strengthening and weakening periods during its 22-day total lifecycle as a tropical cyclone. In this study, the NASA GEOS-5 atmospheric general circulation model and data assimilation system was used to simulate the impacts of dust during the first intensification and weakening phases of Hurricane Nadine using a series of GEOS-5 forecasts initialized during Nadine's intensification phase (12 September 2012). The forecasts explore a hierarchy of aerosol interactions within the model: no aerosol interaction, aerosol-radiation interactions, and aerosol-radiation and aerosol-cloud interactions simultaneously, as well as variations in assumed dust optical properties. When only aerosolradiation interactions are included, Nadine's track exhibits sensitivity to dust shortwave absorption, as a more absorbing dust introduces a shortwave temperature perturbation that impacts Nadine's structure and steering flow, leading to a northward track divergence after 5 days of simulation time. When aerosol-cloud interactions are added, the track exhibits little sensitivity to dust optical properties. This result is attributed to enhanced longwave atmospheric cooling from clouds that counters shortwave atmospheric warming by dust surrounding Nadine, suggesting that aerosol-cloud interactions are a more significant influence on Nadine's track than aerosol-radiation interactions. These findings demonstrate that tropical systems, specifically their track, can be impacted by dust interaction with the atmosphere.

Subgrid-scale variability in clear-sky relative humidity and forcing by aerosol–radiation interactions in an atmosphere model

Abstract. Atmosphere models with resolutions of several tens of kilometres take subgrid-scale variability in the total specific humidity qt into account by using a uniform probability density function (PDF) to predict fractional cloud cover. However, usually only mean relative humidity, RH, or mean clear-sky relative humidity, RHcls, is used to compute hygroscopic growth of soluble aerosol particles. While previous studies based on limited-area models and also a global model suggest that subgrid-scale variability in RH should be taken into account for estimating radiative forcing due to aerosol–radiation interactions (RFari), here we present the first estimate of RFari using a global atmospheric model with a parameterization for subgrid-scale variability in RH that is consistent with the assumptions in the model. For this, we sample the subsaturated part of the uniform RH-PDF from the cloud cover scheme for its application in the hygroscopic growth parameterization in the ECHAM6-HAM2 atmosphere model. Due to the non-linear dependence of the hygroscopic growth on RH, this causes an increase in aerosol hygroscopic growth. Aerosol optical depth (AOD) increases by a global mean of 0.009 ( ∼ 7.8 % in comparison to the control run). Especially over the tropics AOD is enhanced with a mean of about 0.013. Due to the increase in AOD, net top of the atmosphere clear-sky solar radiation, SWnet, cls, decreases by −0.22 W m−2 ( ∼ −0.08 %). Finally, the RFari changes from −0.15 to −0.19 W m−2 by about 31 %. The reason for this very disproportionate effect is that anthropogenic aerosols are disproportionally hygroscopic.

The interdecadal worsening of weather conditions affecting aerosol pollution in the Beijing area in relation to climate warming

Abstract. The weather conditions affecting aerosol pollution in Beijing and its vicinity (BIV) in wintertime have worsened in recent years, particularly after 2010. The relation between interdecadal changes in weather conditions and climate warming is uncertain. Here, we analyze long-term variations of an integrated pollution-linked meteorological index (which is approximately and linearly related to aerosol pollution), the extent of changes in vertical temperature differences in the boundary layer (BL) in BIV, and northerly surface winds from Lake Baikal during wintertime to evaluate the potential contribution of climate warming to changes in meteorological conditions directly related to aerosol pollution in this area; this is accomplished using NCEP reanalysis data, surface observations, and long-term vertical balloon sounding observations since 1960. The weather conditions affecting BIV aerosol pollution are found to have worsened since the 1960s as a whole. This worsening is more significant after 2010, with PM2.5 reaching unprecedented high levels in many cities in China, particularly in BIV. The decadal worsening of meteorological conditions in BIV can partly be attributed to climate warming, which is defined by more warming in the higher layers of the boundary layer (BL) than the lower layers. This worsening can also be influenced by the accumulation of aerosol pollution, to a certain extent (particularly after 2010), because the increase in aerosol pollution from the ground leads to surface cooling by aerosol–radiation interactions, which facilitates temperature inversions, increases moisture accumulations, and results in the extra deterioration of meteorological conditions. If analyzed as a linear trend, weather conditions have worsened by ∼ 4 % each year from 2010 to 2017. Given such a deterioration rate, the worsening of weather conditions may lead to a corresponding amplitude increase in PM2.5 in BIV during wintertime in the next 5 years (i.e., 2018 to 2022). More stringent emission reduction measures will need to be conducted by the government.

Impacts of aerosols on seasonal precipitation and snowpack in California based on convection-permitting WRF-Chem simulations

Abstract. A version of the WRF-Chem model with fully coupled aerosol–meteorology–snowpack is employed to investigate the impacts of various aerosol sources on precipitation and snowpack in California. In particular, the impacts of locally emitted anthropogenic and dust aerosols, and aerosols transported from outside California are studied. We differentiate three pathways of aerosol effects: aerosol–radiation interaction (ARI), aerosol–snow interaction (ASI), and aerosol–cloud interaction (ACI). The convection-permitting model simulations show that precipitation, snow water equivalent (SWE), and surface air temperature averaged over the whole domain (34–42∘ N, 117–124∘ W, not including ocean points) are reduced when aerosols are included, therefore reducing large biases in these variables due to the absence of aerosol effects in the model. Aerosols affect California water resources through the warming of mountaintops and the reduction of precipitation; however, different aerosol sources play different roles in changing surface temperature, precipitation, and snowpack in California by means of various weights of the three pathways. ARI by all aerosols mainly cools the surface, leading to slightly increased SWE over the mountains. Locally emitted dust aerosols warm the surface of mountaintops through ASI, in which the reduced snow albedo associated with dusty snow leads to more surface absorption of solar radiation and reduced SWE. Transported aerosols and local anthropogenic aerosols play a dominant role in increasing nonprecipitating clouds but reducing precipitation through ACI, leading to reduced SWE and runoff on the Sierra Nevada, as well as the warming of mountaintops associated with decreased SWE and hence lower surface albedo. The average changes in surface temperature from October 2012 to June 2013 are about −0.19 and 0.22 K for the whole domain and over mountaintops, respectively. Overall, the averaged reduction during October to June is about 7 % for precipitation, 3 % for SWE, and 7 % for surface runoff for the whole domain, while the corresponding numbers are 12, 10, and 10 % for the mountaintops. The reduction in SWE is more significant in a dry year, with 9 % for the whole domain and 16 % for the mountaintops. The maximum reduction of ∼ 20 % in precipitation occurs in May and is associated with the maximum aerosol loading, leading to the largest decrease in SWE and surface runoff over that period. It is also found that dust aerosols can cause early snowmelt on the mountaintops and reduced surface runoff after April.

Enhancement of PM2.5 Concentrations by Aerosol‐Meteorology Interactions Over China

AbstractAerosol‐meteorology interactions can change surface aerosol concentrations via different mechanisms such as altering radiation budget or cloud microphysics. However, few studies investigated the impacts of different mechanisms on temporal and spatial distribution of PM2.5 concentrations over China. Here we used the fully coupled Weather Research and Forecasting model with online chemistry (WRF‐Chem) to quantify the enhancement of PM2.5 concentrations by aerosol‐meteorology feedback in China in 2014 for different seasons and separate the relative impacts of aerosol radiation interactions (ARIs) and aerosol‐cloud interactions (ACIs). We found that ARIs and ACIs could increase population‐weighted annual mean PM2.5 concentration over China by 4.0 μg/m3 and 1.6 μg/m3, respectively. We found that ARIs play a dominant role in aerosol‐meteorology interactions in winter, while the enhancement of PM2.5 concentration by ARIs and ACIs is comparable in other three seasons. ARIs reduced the wintertime monthly mean wind speed and planetary boundary layer (PBL) height by up to 0.1 m/s and 160 m, respectively, but increased the relative humidity by up to 4%, leading to accumulation of pollutants within PBL. Also, ARIs reduced dry deposition velocity of aerosols by up to 20%, resulting in an increase in PM2.5 lifetime and concentrations. ARIs can increase wintertime monthly mean surface PM2.5 concentration by a maximum of 30 μg/m3 in Sichuan Basin. ACIs can also increase PM2.5 concentration with more significant impacts in wet seasons via reduced wet scavenging and enhanced in‐cloud chemistry. Dominant processes in PM2.5 enhancement are also clarified in different seasons. Results show that physical process is more important than chemical processes in winter in ARIs, while chemical process of secondary inorganic aerosols production may be crucial in wet seasons via ACIs.

Developing and diagnosing climate change indicators of regional aerosol optical properties

Given the importance of aerosol particles to radiative transfer via aerosol-radiation interactions, a methodology for tracking and diagnosing causes of temporal changes in regional-scale aerosol populations is illustrated. The aerosol optical properties tracked include estimates of total columnar burden (aerosol optical depth, AOD), dominant size mode (Ångström exponent, AE), and relative magnitude of radiation scattering versus absorption (single scattering albedo, SSA), along with metrics of the structure of the spatial field of these properties. Over well-defined regions of North America, there are generally negative temporal trends in mean and extreme AOD, and SSA. These are consistent with lower aerosol burdens and transition towards a relatively absorbing aerosol, driven primarily by declining sulfur dioxide emissions. Conversely, more remote regions are characterized by increasing mean and extreme AOD that is attributed to increased local wildfire emissions and long-range (transcontinental) transport. Regional and national reductions in anthropogenic emissions of aerosol precursors are leading to declining spatial autocorrelation in the aerosol fields and increased importance of local anthropogenic emissions in dictating aerosol burdens. However, synoptic types associated with high aerosol burdens are intensifying (becoming more warm and humid), and thus changes in synoptic meteorology may be offsetting aerosol burden reductions associated with emissions legislation.

Aerosol-radiation interaction in atmospheric models: Idealized sensitivity study of simulated short-wave direct radiative effects to particle microphysical properties

We assessed the impact of the microphysical parameterization of natural and anthropogenic aerosols on simulated short-wave radiative effects due to Aerosol-Radiation Interaction (ARI). Layer radiative properties (optical depth, single scattering albedo and asymmetry factor) of dry mineral dust, organic carbon and a black carbon-sulfate mixture have been calculated with a T-matrix code in the short-wave spectral region, after perturbing relevant particle microphysical properties (size distribution, refractive index, mixing state). For each aerosol species, an idealized atmospheric layer and three events of increasing intensity have been set. Then, short-wave direct radiative effects (clear-sky) have been simulated at the top-of-atmosphere (TOA) and at surface (SFC) using the radiative transfer model RRTMG_SW (widely used in atmospheric models), separately for each aerosol species. We observed considerably variable impacts of the particle microphysical perturbations on the layer radiative properties for mineral dust and organic carbon, mainly due to the different sizes of the two species. For the black carbon-sulfate mixture, the single scattering albedo has been found to be much lower in the internal mixing case. Regarding the direct radiative effects, we observed perturbation-induced variability ranges (evaluated against the base net fluxes in absence of aerosols) always within the perturbation range set for the particle microphysical properties (±20%→40%). This work, therefore, quantitatively demonstrates that small uncertainties on the aerosol microphysical parameterization propagate on the simulated direct radiative effects mainly with a loss of strength. Considerable perturbation-induced absolute variations of the direct radiative effects have been found (above all for large aerosol amounts), which could significantly affect the model assessments of the ARI radiative effects and therefore meteorological forecasts and climate predictions.

Significance of aerosol radiative effect in energy balance control on global precipitation change

AbstractHistorical changes of global precipitation in the 20th century simulated by a climate model are investigated. The results simulated with alternate configurations of cloud microphysics are analyzed in the context of energy balance controls on global precipitation, where the latent heat changes associated with the precipitation change is nearly balanced with changes to atmospheric radiative cooling. The atmospheric radiative cooling is dominated by its clear‐sky component, which is found to correlate with changes to both column water vapor and aerosol optical depth (AOD). The water vapor‐dependent component of the clear‐sky radiative cooling is then found to scale with global temperature change through the Clausius–Clapeyron relationship. This component results in a tendency of global precipitation increase with increasing temperature at a rate of approximately 2%K−1. Another component of the clear‐sky radiative cooling, which is well correlated with changes to AOD, is also found to vary in magnitude among different scenarios with alternate configurations of cloud microphysics that controls the precipitation efficiency, a major factor influencing the aerosol scavenging process that can lead to different aerosol loadings. These results propose how different characteristics of cloud microphysics can cause different aerosol loadings that in turn perturb global energy balance to significantly change global precipitation. This implies a possible coupling of aerosol–cloud interaction with aerosol–radiation interaction in the context of global energy balance.

Aerosols characteristics, trends and their climatic implications over Northeast India and adjoining South Asia

ABSTRACTAerosol characteristics and climatic implications derived for selected locations of the north‐eastern region of India and adjoining locations Thimphu (THM), Dhaka (DAC) and Banmauk between 22–30°N and 88–98°E are reported. The region is found to reveal a distinct spatio‐temporal variability in aerosol distribution, with highest climatological mean aerosol optical depth at 550 nm (AOD550) at DAC (0.65 ± 0.07) and lowest at the high altitude location THM (0.19 ± 0.02). Seasonally the maximum AOD550 is observed in the pre‐monsoon season. Moderate resolution imaging spectroradiometer Level‐3 Collection 6 AOD550 and Ångström exponent (AE) exhibit a significant and simultaneous increasing trend in the range of ∼0.003 year−1 to 0.012 year−1 and ∼−0.001 year−1 to 0.020 year−1, respectively, during the period 2001–2014. Together with AE, increasing trend of total ozone mapping spectrometer and ozone monitoring instrument‐retrieved aerosol index (∼0.001 year−1 to 0.007 year−1 during 1979–2014) signifies an increase in anthropogenic aerosol loading, leading to an increase in number density of cloud condensation nuclei and decrease/increase of cloud effective radius /cloud optical depth (COD). This is further associated with overall decreasing trends of rainfall rate over this complex monsoon region. A slow increase in maximum temperature (Tmax) (∼0.008 °C year−1 to 0.049 °C year−1) compared to that in minimum temperature (Tmin) (∼0.007 °C year−1 to 0.068 °C year−1) is attributed to solar dimming due to increasing aerosol loading and COD (∼0.056 year−1 to 0.15 year−1). A decrease in high‐level cloud (CODhigh) counteracts decreasing trends of ground reaching solar radiation over a few locations, including Dibrugarh. This study is important from an aerosol radiation interaction and aerosol cloud interaction viewpoint, which facilitates in reaching a closure of model simulated present day climate change and future climate projections.

Regional effects of atmospheric aerosols on temperature: an evaluation of an ensemble of online coupled models

Abstract. The climate effect of atmospheric aerosols is associated with their influence on the radiative budget of the Earth due to the direct aerosol–radiation interactions (ARIs) and indirect effects, resulting from aerosol–cloud–radiation interactions (ACIs). Online coupled meteorology–chemistry models permit the description of these effects on the basis of simulated atmospheric aerosol concentrations, although there is still some uncertainty associated with the use of these models. Thus, the objective of this work is to assess whether the inclusion of atmospheric aerosol radiative feedbacks of an ensemble of online coupled models improves the simulation results for maximum, mean and minimum temperature at 2 m over Europe. The evaluated models outputs originate from EuMetChem COST Action ES1004 simulations for Europe, differing in the inclusion (or omission) of ARI and ACI in the various models. The cases studies cover two important atmospheric aerosol episodes over Europe in the year 2010: (i) a heat wave event and a forest fire episode (July–August 2010) and (ii) a more humid episode including a Saharan desert dust outbreak in October 2010. The simulation results are evaluated against observational data from the E-OBS gridded database. The results indicate that, although there is only a slight improvement in the bias of the simulation results when including the radiative feedbacks, the spatiotemporal variability and correlation coefficients are improved for the cases under study when atmospheric aerosol radiative effects are included.

Impact of aerosols and clouds on decadal trends in all-sky solar radiation over the Netherlands (1966–2015)

Abstract. A 50-year hourly data set of global shortwave radiation, cloudiness and visibility over the Netherlands was used to quantify the contribution of aerosols and clouds to the trend in yearly-averaged all-sky radiation (1.81 ± 1.07 W m−2 decade−1). Yearly-averaged clear-sky and cloud-base radiation data show large year-to-year fluctuations caused by yearly changes in the occurrence of clear and cloudy periods and cannot be used for trend analysis. Therefore, proxy clear-sky and cloud-base radiations were computed. In a proxy analysis hourly radiation data falling within a fractional cloudiness value are fitted by monotonic increasing functions of solar zenith angle and summed over all zenith angles occurring in a single year to produce an average. Stable trends can then be computed from the proxy radiation data. A functional expression is derived whereby the trend in proxy all-sky radiation is a linear combination of trends in fractional cloudiness, proxy clear-sky radiation and proxy cloud-base radiation. Trends (per decade) in fractional cloudiness, proxy clear-sky and proxy cloud-base radiation were, respectively, 0.0097 ± 0.0062, 2.78 ± 0.50 and 3.43 ± 1.17 W m−2. To add up to the all-sky radiation the three trends have weight factors, namely the difference between the mean cloud-base and clear-sky radiation, the clear-sky fraction and the fractional cloudiness, respectively. Our analysis clearly demonstrates that all three components contribute significantly to the observed trend in all-sky radiation. Radiative transfer calculations using the aerosol optical thickness derived from visibility observations indicate that aerosol–radiation interaction (ARI) is a strong candidate to explain the upward trend in the clear-sky radiation. Aerosol–cloud interaction (ACI) may have some impact on cloud-base radiation, but it is suggested that decadal changes in cloud thickness and synoptic-scale changes in cloud amount also play an important role.

Revising the hygroscopicity of inorganic sea salt particles

Sea spray is one of the largest natural aerosol sources and plays an important role in the Earth’s radiative budget. These particles are inherently hygroscopic, that is, they take-up moisture from the air, which affects the extent to which they interact with solar radiation. We demonstrate that the hygroscopic growth of inorganic sea salt is 8–15% lower than pure sodium chloride, most likely due to the presence of hydrates. We observe an increase in hygroscopic growth with decreasing particle size (for particle diameters <150 nm) that is independent of the particle generation method. We vary the hygroscopic growth of the inorganic sea salt within a general circulation model and show that a reduced hygroscopicity leads to a reduction in aerosol-radiation interactions, manifested by a latitudinal-dependent reduction of the aerosol optical depth by up to 15%, while cloud-related parameters are unaffected. We propose that a value of κs=1.1 (at RH=90%) is used to represent the hygroscopicity of inorganic sea salt particles in numerical models.

Implementation of aerosol–cloud interactions in the regional atmosphere–aerosol model COSMO-MUSCAT(5.0) and evaluation using satellite data

Abstract. The regional atmospheric model Consortium for Small-scale Modeling (COSMO) coupled to the Multi-Scale Chemistry Aerosol Transport model (MUSCAT) is extended in this work to represent aerosol–cloud interactions. Previously, only one-way interactions (scavenging of aerosol and in-cloud chemistry) and aerosol–radiation interactions were included in this model. The new version allows for a microphysical aerosol effect on clouds. For this, we use the optional two-moment cloud microphysical scheme in COSMO and the online-computed aerosol information for cloud condensation nuclei concentrations (Cccn), replacing the constant Cccn profile. In the radiation scheme, we have implemented a droplet-size-dependent cloud optical depth, allowing now for aerosol–cloud–radiation interactions. To evaluate the models with satellite data, the Cloud Feedback Model Intercomparison Project Observation Simulator Package (COSP) has been implemented. A case study has been carried out to understand the effects of the modifications, where the modified modeling system is applied over the European domain with a horizontal resolution of 0.25° × 0.25°. To reduce the complexity in aerosol–cloud interactions, only warm-phase clouds are considered. We found that the online-coupled aerosol introduces significant changes for some cloud microphysical properties. The cloud effective radius shows an increase of 9.5 %, and the cloud droplet number concentration is reduced by 21.5 %.

Simulated effects of internal mixing of anthropogenic aerosols on the aerosol–radiation interaction and global temperature

ABSTRACTA partial internal mixing (PIM) treatment of black carbon (BC), organic carbon (OC), and sulphate was examined, and the core‐shell model was used to represent the internally mixed aerosols with BC as the core and sulphate or OC as the shell. The influences of PIM treatment on the effective radiative forcing due to aerosol–radiative interaction (ERFari) and global temperature were examined and compared to those of external mixing (EM) treatment using an aerosol‐climate online coupled model of BCC_AGCM2.0_CUACE/Aero. Radiative forcing due to aerosol–radiation interaction (RFari) of the anthropogenic aerosols since the preindustrial era was −0.34 W m−2 for EM and −0.23 W m−2 for PIM, respectively. The global annual mean ERFari of anthropogenic aerosols since the preindustrial era was −0.42 W m−2 for EM and −0.34 W m−2 for PIM, respectively. The change in global annual mean surface temperature increased accordingly from −0.18 K in the EM case to −0.125 K in the PIM case. Well geographic consistence between the change in low‐level cloud amount and the change in temperature can be found. The atmospheric temperature in the troposphere was markedly less reduced in the PIM case than in the EM case. The RFari/ERFari for 50% and 100% were −0.11/–0.07 and 0.13/0.14 W m−2, respectively. RFari, ERFari, and surface temperature changed approximately linearly with the internal mixing proportion.

Interactive nature of climate change and aerosol forcing

The effect of changing cloud cover on climate, based on cloud-aerosol interactions, is one of the major unknowns for climate forcing and climate sensitivity. It has two components: (1) the impact of aerosols on clouds and climate due to in situ interactions (i.e., rapid response) and (2) the effect of aerosols on the cloud feedback that arises as climate changes-climate feedback response. We examine both effects utilizing the NASA Goddard Institute for Space Studies ModelE2 to assess the indirect effect, with both mass-based and microphysical aerosol schemes, in transient twentieth century simulations. We separate the rapid response and climate feedback effects by making simulations with a coupled version of the model as well as one with no sea surface temperature or sea ice response ("atmosphere-only" simulations). We show that the indirect effect of aerosols on temperature is altered by the climate feedbacks following the ocean response, and this change differs depending upon which aerosol model is employed. Overall, the effective radiative forcing (ERF) for the "direct effect" of aerosol-radiation interaction (ERFari) ranges between -0.2 and -0.6 W m-2 for atmosphere-only experiments, while the total effective radiative forcing, including[C0]the indirect effect (ERFari+aci) varies between about -0.4 and -1.1 W m-2 for atmosphere-only simulations; both ranges are in agreement with those given in Intergovernmental Panel on Climate Change (2013). Including the full feedback of the climate system lowers these ranges to -0.2 to -0.5 W m-2 for ERFari and -0.3 to -0.74 W m-2 for ERFari+aci. With both aerosol schemes, the climate change feedbacks have reduced the global average indirect radiative effect of atmospheric aerosols relative to what the emission changes would have produced, at least partially due to its effect on tropical upper tropospheric clouds.