Addressing the difficulties in quantifying the Twomey effect for marine warm clouds from multi-sensor satellite observations and reanalysis

Aerosol–cloud interaction is the most uncertain component of the overall anthropogenic forcing of the climate, in which the Twomey effect plays a fundamental role. Satellite-based estimates of the Twomey effect are especially challenging, mainly due to the difficulty in disentangling aerosol effects on cloud droplet number concentration (Nd) from possible confounders. By combining multiple satellite observations and reanalysis, this study investigates the impacts of a) updraft, b) precipitation, c) retrieval errors, as well as (d) vertical co-location between aerosol and cloud, on the assessment of Nd-toaerosol sensitivity (S) in the context of marine warm (liquid) clouds. Our analysis suggests that S increases remarkably with both cloud base height and cloud geometric thickness (proxies for vertical velocity at cloud base), consistent with stronger aerosol-cloud interactions at larger updraft velocity. In turn, introducing the confounding effect of aerosol–precipitation interaction can artificially amplify S by an estimated 21 %, highlighting the necessity of removing precipitating clouds from analyses on the Twomey effect. It is noted that the retrieval biases in aerosol and cloud appear to underestimate S, in which cloud fraction acts as a key modulator, making it practically difficult to balance the accuracies of aerosol–cloud retrievals at aggregate scales (e.g., 1° × 1° grid). Moreover, we show that using column-integrated sulfate mass concentration (SO4C) to approximate sulfate concentration at cloud base (SO4B) can result in a degradation of correlation with Nd, along with a nearly twofold enhancement of S, mostly attributed to the inability of SO4C to capture the full spatio-temporal variability of SO4B. These findings point to several potential ways forward to account for the major influential factors practically by means of satellite observations and reanalysis, aiming at an optimal observational estimate of global radiative forcing due to the Twomey effect.

Addressing the difficulties in quantifying the Twomey effect for marine warm clouds from multi-sensor satellite observations and reanalysis

<p>Aerosol–cloud interaction is the most uncertain component of the overall anthropogenic forcing of the climate, inwhich the Twomey effect plays a fundamental role. Satellite-based estimates of the Twomey effect are especially challenging, mainly due to the difficulty in disentangling aerosol effects on cloud droplet number concentration (Nd) from possible confounders. By combining multiple satellite observations and reanalysis, this study investigates the impacts of a) updraft, b) precipitation, c) retrieval errors, as well as (d) vertical co-location between aerosol and cloud, on the assessment of Nd-to-aerosol sensitivity (S) in the context of marine warm (liquid) clouds. Our analysis suggests that S increases remarkably with both cloud base height and cloud geometric thickness (proxies for vertical velocity at cloud base), consistent with stronger aerosol-cloud interactions at larger updraft velocity. In turn, introducing the confounding effect of aerosol–precipitation interaction can artificially amplify S by an estimated 21 %, highlighting the necessity of removing precipitating clouds from analyses on the Twomey effect. It is noted that the retrieval biases in aerosol and cloud appear to underestimate S, in which cloud fraction acts as a key modulator, making it practically difficult to balance the accuracies of aerosol–cloud retrievals at aggregate scales (e.g., 1◦ × 1◦ grid). Moreover, we show that using column-integrated sulfate mass concentration (SO4C) to approximate sulfate concentration at cloud base (SO4B) can result in a degradation of correlation with Nd, along with a nearly two fold enhancement of S, mostly attributed to the inability of SO4C to capture the full spatio-temporal variability of SO4B. These findings point to several potential ways forward to account for the major influential factors practically by means of satellite observations and reanalysis, aiming at an optimal observational estimate of global radiative forcing due to the Twomey effect.</p>

Quantifying the structural uncertainty of the aerosol mixing state representation in a modal model

Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. This study aims to verify the global distribution of aerosol mixing state represented by modal models. To quantify the aerosol mixing state, we used the aerosol mixing state indices for submicron aerosol based on the mixing of optically absorbing and non-absorbing species (χo), the mixing of primary carbonaceous and non-primary carbonaceous species (χc), and the mixing of hygroscopic and non-hygroscopic species (χh). To achieve a spatiotemporal comparison, we calculated the mixing state indices using output from the Community Earth System Model with the four-mode version of the Modal Aerosol Module (MAM4) and compared the results with the mixing state indices from a benchmark machine-learned model trained on high-detail particle-resolved simulations from the particle-resolved stochastic aerosol model PartMC-MOSAIC. The two methods yielded very different spatial patterns of the mixing state indices. In some regions, the yearly averaged χ value computed by the MAM4 model differed by up to 70 percentage points from the benchmark values. These errors tended to be zonally structured, with the MAM4 model predicting a more internally mixed aerosol at low latitudes and a more externally mixed aerosol at high latitudes compared to the benchmark. Our study quantifies potential model bias in simulating mixing state in different regions and provides insights into potential improvements to model process representation for a more realistic simulation of aerosols towards better quantification of radiative forcing and aerosol–cloud interactions.

Cloud droplet formation at the base of tropical convective clouds: closure between modeling and measurement results of ACRIDICON–CHUVA

Aerosol–cloud interactions contribute to the large uncertainties in current estimates of climate forcing. We investigated the effect of aerosol particles on cloud droplet formation by model calculations and aircraft measurements over the Amazon and over the western tropical Atlantic during the ACRIDICON–CHUVA campaign in September 2014. On the HALO (High Altitude Long Range Research) research aircraft, cloud droplet number concentrations (Nd) were measured near the base of clean and polluted growing convective cumuli using a cloud combination probe (CCP) and a cloud and aerosol spectrometer (CAS-DPOL). An adiabatic parcel model was used to perform cloud droplet number closure studies for flights in differently polluted air masses. Model input parameters included aerosol size distributions measured with an ultra-high sensitive aerosol spectrometer (UHSAS), in combination with a condensation particle counter (CPC). Updraft velocities (w) were measured with a boom-mounted Rosemount probe. Over the continent, the aerosol size distributions were dominated by accumulation mode particles, and good agreement between measured and modeled Nd values was obtained (deviations ≲ 10 %) assuming an average hygroscopicity of κ∼0.1, which is consistent with Amazonian biomass burning and secondary organic aerosol. Above the ocean, fair agreement was obtained assuming an average hygroscopicity of κ∼0.2 (deviations ≲ 16 %) and further improvement was achieved assuming different hygroscopicities for Aitken and accumulation mode particles (κAit=0.8, κacc=0.2; deviations ≲ 10 %), which may reflect secondary marine sulfate particles. Our results indicate that Aitken mode particles and their hygroscopicity can be important for droplet formation at low pollution levels and high updraft velocities in tropical convective clouds.

Exploring the Change in PM2.5 and Ozone Concentrations Caused by Aerosol–Radiation Interactions and Aerosol–Cloud Interactions and the Relationship with Meteorological Factors

Aerosols can interact with other meteorological variables in the air via aerosol–radiation or aerosol–cloud interactions (ARIs/ACIs), thus affecting the concentrations of particle pollutants and ozone. The online-coupled model WRF-Chem was applied to simulate the changes in the PM2.5 (particulate matter less than 2.5 μm in aerodynamic diameter) and ozone concentrations that are caused by these mechanisms in China by conducting three parallel sensitivity tests. In each case, availabilities of aerosol–radiation interactions and aerosol–cloud interactions were set differently in order to distinguish each pathway. Partial correlation coefficients were also analyzed using statistical tools. As suggested by the results, the ARIs reduced ground air temperature, wind speed, and planetary boundary height while increasing relative humidity in most places. Consequently, the ozone concentration in the corresponding region declined by 4%, with a rise in the local annual mean PM2.5 concentration by approximately 12 μm/m3. The positive feedback of the PM2.5 concentration via ACIs was also found in some city clusters across China, despite the overall enhancement value via ACIs being merely around a quarter to half that via ARIs. The change in ozone concentration via ACIs exhibited different trends. The ozone concentration level increased via ACIs, which can be attributed to the drier air in the south and the diminished solar radiation that is received in central and northern China. The correlation coefficient suggests that the suppression in the planetary boundary layer is the most significant factor for the increase in PM2.5 followed by the rise in moisture required for hygroscopic growth. Ozone showed a significant correlation with NO2, while oxidation rates and radiation variance were also shown to be vitally important.

The impact of sampling strategy on the cloud droplet number concentration estimated from satellite data

Cloud droplet number concentration (Nd) is of central importance to observation-based estimates of aerosol indirect effects, being used to quantify both the cloud sensitivity to aerosol and the base state of the cloud. However, the derivation of Nd from satellite data depends on a number of assumptions about the cloud and the accuracy of the retrievals of the cloud properties from which it is derived, making it prone to systematic biases. A number of sampling strategies have been proposed to address these biases by selecting the most accurate Nd retrievals in the satellite data. This work compares the impact of these strategies on the accuracy of the satellite retrieved Nd, using a selection of insitu measurements. In stratocumulus regions, the MODIS Nd retrieval is able to achieve a high precision (r2 of 0.5–0.8). This is lower in other cloud regimes, but can be increased by appropriate sampling choices. Although the Nd sampling can have significant effects on the Nd climatology, it produces only a 20 % variation in the implied radiative forcing from aerosol-cloud interactions, with the choice of aerosol proxy driving the overall uncertainty. The results are summarised into recommendations for using MODIS Nd products and appropriate sampling.

Observation of aerosol induced ‘lower tropospheric cooling’ over Indian core monsoon region

Aerosols play a significant role in regional scale pollution that alters the cloud formation process, radiation budget, and climate. Here, using long-term (2003-2019) observations from multi-satellite and ground-based remote sensors, we show robust aerosol-induced instantaneous daytime lower tropospheric cooling during the pre-monsoon season over the Indian core monsoon region (ICMR). Quantitatively, an average cooling of -0.82±0.11 °C to -1.84±0.25 °C is observed in the lower troposphere. The observed cooling is associated with both aerosol-radiation and aerosol-cloud-radiation interactions processes. The elevated dust and polluted-dust layers cause extinction of the incoming solar radiation, thereby decreasing the lower tropospheric temperature. The aerosol-cloud interactions also contribute to enhancement of cloud fraction which further contributes to the lower tropospheric cooling. The observed cooling results in a stable lower tropospheric structure during polluted conditions, which can also feedback to cloud systems. Our findings suggest that aerosol induced lower tropospheric cooling can strongly affect the cloud distribution and circulation dynamics over the ICMR, a region of immense hydroclimatic importance.

Quantifying Albedo Susceptibility Biases in Shallow Clouds

The evaluation of radiative forcing associated with aerosol-cloud interactions remains a significant source of uncertainty in future climate projections. The problem is confounded by the fact that aerosol particles influence clouds locally, and that averaging to larger spatial and/or temporal scales carries biases that depend on the heterogeneity and spatial correlation of the interacting fields and the non-linearity of the responses. Mimicking commonly applied satellite data analyses for calculation of albedo susceptibility So, we quantify So aggregation biases using an ensemble of 127 large eddy simulations of marine stratocumulus. We explore the cloud field properties that control this spatial aggregation bias, and quantify the bias for a large range of shallow stratocumulus cloud conditions manifesting a variety of morphologies and range of cloud fractions. We show that So spatial aggregation biases can be on the order of 100s of percent, depending on methodology. Key uncertainties emanate from the typically applied adiabatic drop concentration Nd retrieval, the correlation between aerosol and cloud fields, and the extent to which averaging reduces the variance in cloud albedo Ac and Nd. Biases are more often positive than negative. So biases are highly correlated to biases in the adjustment. Temporal aggregation biases are shown to offset spatial averaging biases. Both spatial and temporal biases have significant implications for observationally based assessments of aerosol indirect effects and our inferences of underlying aerosol-cloud-radiation effects.

Aerosol–cloud interactions: the representation of heterogeneous ice activation in cloud models

The homogeneous nucleation of ice in supercooled liquid-water clouds is characterized by time-dependent freezing rates. By contrast, water phase transitions induced heterogeneously by ice-nucleating particles (INPs) are described by time-independent ice-active fractions depending on ice supersaturation (s). Laboratory studies report ice-active particle number fractions (AFs) that are cumulative in s. Cloud models budget INP and ice crystal numbers to conserve total particle number during water phase transitions. Here, we show that ice formation from INPs with time-independent nucleation behavior is overpredicted when models budget particle numbers and at the same time derive ice crystal numbers from s-cumulative AFs. This causes a bias towards heterogeneous ice formation in situations where INPs compete with homogeneous droplet freezing during cloud formation. We resolve this issue by introducing differential AFs, thereby moving us one step closer to more robust simulations of aerosol–cloud interactions.