ALBERT

Description: The radiative forcing of the aerosol–radiation interaction can be decomposed into clear-sky and cloudy-sky portions. Two sets of multi-model simulations within Aerosol Comparisons between Observations and Models (AeroCom), combined with observational methods, and the time evolution of aerosol emissions over the industrial era show that the contribution from cloudy-sky regions is likely weak. A mean of the simulations considered is 0.01±0.1 W m−2. Multivariate data analysis of results from AeroCom Phase II shows that many factors influence the strength of the cloudy-sky contribution to the forcing of the aerosol–radiation interaction. Overall, single-scattering albedo of anthropogenic aerosols and the interaction of aerosols with the short-wave cloud radiative effects are found to be important factors. A more dedicated focus on the contribution from the cloud-free and cloud-covered sky fraction, respectively, to the aerosol–radiation interaction will benefit the quantification of the radiative forcing and its uncertainty range.

Description: To better understand and characterize current uncertainties in the important observational constraint of climate models of aerosol optical depth (AOD), we evaluate and intercompare 14 satellite products, representing nine different retrieval algorithm families using observations from five different sensors on six different platforms. The satellite products (super-observations consisting of 1∘×1∘ daily aggregated retrievals drawn from the years 2006, 2008 and 2010) are evaluated with AErosol RObotic NETwork (AERONET) and Maritime Aerosol Network (MAN) data. Results show that different products exhibit different regionally varying biases (both under- and overestimates) that may reach ±50 %, although a typical bias would be 15 %–25 % (depending on the product). In addition to these biases, the products exhibit random errors that can be 1.6 to 3 times as large. Most products show similar performance, although there are a few exceptions with either larger biases or larger random errors. The intercomparison of satellite products extends this analysis and provides spatial context to it. In particular, we show that aggregated satellite AOD agrees much better than the spatial coverage (often driven by cloud masks) within the 1∘×1∘ grid cells. Up to ∼50 % of the difference between satellite AOD is attributed to cloud contamination. The diversity in AOD products shows clear spatial patterns and varies from 10 % (parts of the ocean) to 100 % (central Asia and Australia). More importantly, we show that the diversity may be used as an indication of AOD uncertainty, at least for the better performing products. This provides modellers with a global map of expected AOD uncertainty in satellite products, allows assessment of products away from AERONET sites, can provide guidance for future AERONET locations and offers suggestions for product improvements. We account for statistical and sampling noise in our analyses. Sampling noise, variations due to the evaluation of different subsets of the data, causes important changes in error metrics. The consequences of this noise term for product evaluation are discussed.

Description: This study assesses the change in anthropogenic aerosol forcing from the mid-1970s to the mid-2000s. Both decades had similar global-mean anthropogenic aerosol optical depths but substantially different global distributions. For both years, we quantify (i) the forcing spread due to model-internal variability and (ii) the forcing spread among models. Our assessment is based on new ensembles of atmosphere-only simulations with five state-of-the-art Earth system models. Four of these models will be used in the sixth Coupled Model Intercomparison Project (CMIP6; Eyring et al., 2016). Here, the complexity of the anthropogenic aerosol has been reduced in the participating models. In all our simulations, we prescribe the same patterns of the anthropogenic aerosol optical properties and associated effects on the cloud droplet number concentration. We calculate the instantaneous radiative forcing (RF) and the effective radiative forcing (ERF). Their difference defines the net contribution from rapid adjustments. Our simulations show a model spread in ERF from −0.4 to −0.9 W m−2. The standard deviation in annual ERF is 0.3 W m−2, based on 180 individual estimates from each participating model. This result implies that identifying the model spread in ERF due to systematic differences requires averaging over a sufficiently large number of years. Moreover, we find almost identical ERFs for the mid-1970s and mid-2000s for individual models, although there are major model differences in natural aerosols and clouds. The model-ensemble mean ERF is −0.54 W m−2 for the pre-industrial era to the mid-1970s and −0.59 W m−2 for the pre-industrial era to the mid-2000s. Our result suggests that comparing ERF changes between two observable periods rather than absolute magnitudes relative to a poorly constrained pre-industrial state might provide a better test for a model's ability to represent transient climate changes.

Description: Numerical prediction of aerosol particle properties has become an important activity at many research and operational weather centers. This development is due to growing interest from a diverse set of stakeholders, such as air quality regulatory bodies, aviation and military authorities, solar energy plant managers, climate services providers, and health professionals. Owing to the complexity of atmospheric aerosol processes and their sensitivity to the underlying meteorological conditions, the prediction of aerosol particle concentrations and properties in the numerical weather prediction (NWP) framework faces a number of challenges. The modeling of numerous aerosol-related parameters increases computational expense. Errors in aerosol prediction concern all processes involved in the aerosol life cycle including (a) errors on the source terms (for both anthropogenic and natural emissions), (b) errors directly dependent on the meteorology (e.g., mixing, transport, scavenging by precipitation), and (c) errors related to aerosol chemistry (e.g., nucleation, gas–aerosol partitioning, chemical transformation and growth, hygroscopicity). Finally, there are fundamental uncertainties and significant processing overhead in the diverse observations used for verification and assimilation within these systems. Indeed, a significant component of aerosol forecast development consists in streamlining aerosol-related observations and reducing the most important errors through model development and data assimilation. Aerosol particle observations from satellite- and ground-based platforms have been crucial to guide model development of the recent years and have been made more readily available for model evaluation and assimilation. However, for the sustainability of the aerosol particle prediction activities around the globe, it is crucial that quality aerosol observations continue to be made available from different platforms (space, near surface, and aircraft) and freely shared. This paper reviews current requirements for aerosol observations in the context of the operational activities carried out at various global and regional centers. While some of the requirements are equally applicable to aerosol–climate, the focus here is on global operational prediction of aerosol properties such as mass concentrations and optical parameters. It is also recognized that the term “requirements” is loosely used here given the diversity in global aerosol observing systems and that utilized data are typically not from operational sources. Most operational models are based on bulk schemes that do not predict the size distribution of the aerosol particles. Others are based on a mix of “bin” and bulk schemes with limited capability of simulating the size information. However the next generation of aerosol operational models will output both mass and number density concentration to provide a more complete description of the aerosol population. A brief overview of the state of the art is provided with an introduction on the importance of aerosol prediction activities. The criteria on which the requirements for aerosol observations are based are also outlined. Assimilation and evaluation aspects are discussed from the perspective of the user requirements.

Description: Here we present new results comparing aerosol optical depth (AOD), aerosol absorption optical depth (AAOD) and column single scattering albedo (SSA) obtained from in situ vertical profile measurements with AERONET ground-based remote sensing from two rural, continental sites in the US. The profiles are closely matched in time (within ±3 h) and space (within 15 km) with the AERONET retrievals. We have used Level 1.5 inversion retrievals when there was a valid Level 2 almucantar retrieval in order to be able to compare AAOD and column SSA below AERONET's recommended loading constraint (AOD 〉 0.4 at 440 nm). While there is reasonable agreement for the AOD comparisons, the direct comparisons of in situ-derived to AERONET-retrieved AAOD (or SSA) reveal that AERONET retrievals yield higher aerosol absorption than obtained from the in situ profiles for the low aerosol optical depth conditions prevalent at the two study sites. However, it should be noted that the majority of SSA comparisons for AOD440 〉 0.2 are, nonetheless, within the reported SSA uncertainty bounds. The observation that, relative to in situ measurements, AERONET inversions exhibit increased absorption potential at low AOD values is generally consistent with other published AERONET–in situ comparisons across a range of locations, atmospheric conditions and AOD values. This systematic difference in the comparisons suggests a bias in one or both of the methods, but we cannot assess whether the AERONET retrievals are biased towards high absorption or the in situ measurements are biased low. Based on the discrepancy between the AERONET and in situ values, we conclude that scaling modeled black carbon concentrations upwards to match AERONET retrievals of AAOD should be approached with caution as it may lead to aerosol absorption overestimates in regions of low AOD. Both AERONET retrievals and in situ measurements suggest there is a systematic relationship between SSA and aerosol amount (AOD or aerosol light scattering) – specifically that SSA decreases at lower aerosol loading. This implies that the fairly common assumption that AERONET SSA values retrieved at high-AOD conditions can be used to obtain AAOD at low-AOD conditions may not be valid.

Description: We present final and quality-assured results of multiwavelength polarization/Raman lidar observations of the Saharan air layer (SAL) over the tropical Atlantic. Observations were performed aboard the German research vessel R/V Meteor during the 1-month transatlantic cruise from Guadeloupe to Cabo Verde over 4500 km from 61.5 to 20° W at 14–15° N in April–May 2013. First results of the shipborne lidar measurements, conducted in the framework of SALTRACE (Saharan Aerosol Long-range Transport and Aerosol–Cloud Interaction Experiment), were reported by Kanitz et al.(2014). Here, we present four observational cases representing key stages of the SAL evolution between Africa and the Caribbean in detail in terms of layering structures and optical properties of the mixture of predominantly dust and aged smoke in the SAL. We discuss to what extent the lidar results confirm the validity of the SAL conceptual model which describes the dust long-range transport and removal processes over the tropical Atlantic. Our observations of a clean marine aerosol layer (MAL, layer from the surface to the SAL base) confirm the conceptual model and suggest that the removal of dust from the MAL, below the SAL, is very efficient. However, the removal of dust from the SAL assumed in the conceptual model to be caused by gravitational settling in combination with large-scale subsidence is weaker than expected. To explain the observed homogenous (height-independent) dust optical properties from the SAL base to the SAL top, from the African coast to the Caribbean, we have to assume that the particle sedimentation strength is reduced and dust vertical mixing and upward transport mechanisms must be active in the SAL. Based on lidar observations on 20 nights at different longitudes in May 2013, we found, on average, MAL and SAL layer mean values (at 532 nm) of the extinction-to-backscatter ratio (lidar ratio) of 17±5 sr (MAL) and 43±8 sr (SAL), of the particle linear depolarization ratio of 0.025±0.015 (MAL) and 0.19±0.09 (SAL), and of the particle extinction coefficient of 67±45 Mm−1 (MAL) and 68±37 Mm−1 (SAL). The 532 nm optical depth of the lofted SAL was found to be, on average, 0.15±0.13 during the ship cruise. The comparably low values of the SAL mean lidar ratio and depolarization ratio (compared to typical pure dust values of 50–60 sr and 0.3, respectively) in combination with backward trajectories indicate a smoke contribution to light extinction of the order of 20 % during May 2013, at the end of the burning season in central-western Africa.

Description: The HD(CP)2 Observational Prototype Experiment (HOPE) was performed as a major 2-month field experiment in Jülich, Germany, in April and May 2013, followed by a smaller campaign in Melpitz, Germany, in September 2013. HOPE has been designed to provide an observational dataset for a critical evaluation of the new German community atmospheric icosahedral non-hydrostatic (ICON) model at the scale of the model simulations and further to provide information on land-surface–atmospheric boundary layer exchange, cloud and precipitation processes, as well as sub-grid variability and microphysical properties that are subject to parameterizations. HOPE focuses on the onset of clouds and precipitation in the convective atmospheric boundary layer. This paper summarizes the instrument set-ups, the intensive observation periods, and example results from both campaigns. HOPE-Jülich instrumentation included a radio sounding station, 4 Doppler lidars, 4 Raman lidars (3 of them provide temperature, 3 of them water vapour, and all of them particle backscatter data), 1 water vapour differential absorption lidar, 3 cloud radars, 5 microwave radiometers, 3 rain radars, 6 sky imagers, 99 pyranometers, and 5 sun photometers operated at different sites, some of them in synergy. The HOPE-Melpitz campaign combined ground-based remote sensing of aerosols and clouds with helicopter- and balloon-based in situ observations in the atmospheric column and at the surface. HOPE provided an unprecedented collection of atmospheric dynamical, thermodynamical, and micro- and macrophysical properties of aerosols, clouds, and precipitation with high spatial and temporal resolution within a cube of approximately 10  ×  10  ×  10 km3. HOPE data will significantly contribute to our understanding of boundary layer dynamics and the formation of clouds and precipitation. The datasets have been made available through a dedicated data portal. First applications of HOPE data for model evaluation have shown a general agreement between observed and modelled boundary layer height, turbulence characteristics, and cloud coverage, but they also point to significant differences that deserve further investigations from both the observational and the modelling perspective.

Description: Monthly global maps for aerosol properties of the Max Planck Aerosol Climatology version 2 (MACv2) are applied in an offline radiative transfer model to determine aerosol radiative effects. This model setup cannot address rapid adjustments by clouds, but current evidence suggests their contribution to be small when compared to the instantaneous radiative forcing. Global maps are presented to detail the regional and seasonal variability associated with (annual) global averages. Radiative effects caused by the aerosol presence (direct effects) and by aerosol modified clouds (indirect effects) are examined. Direct effects are determined for total aerosol, anthropogenic aerosol and extracted individual aerosol components. Indirect effects cover the impact of reduced cloud drop sizes by anthropogenic aerosol. Present-day global annual radiative effects for anthropogenic aerosol yield (1) a climate cooling of −1.0 W m−2 at the top of the atmosphere (TOA); (2) a surface net-flux reduction of −2.1 W m−2; and, by difference; (3) an atmospheric effect of +1.1 W m−2. This atmospheric solar heating is almost entirely a direct effect. On a global basis, indirect effects (−0.65 W m−2) dominate direct effects (−0.35 W m−2) for the present-day climate response at the TOA, whereas the present-day surface radiative budget is more strongly reduced by direct effects (−1.45 W m−2) than by indirect effects (−0.65 W m−2). Natural aerosols are on average less absorbing and larger in size. However, their stronger solar TOA cooling efficiency is offset by a non-negligible infrared (IR) greenhouse warming efficiency. In the sum the global average annual direct forcing efficiencies (per unit AOD) for natural and anthropogenic aerosol are similar: −12 W m−2 per unit AOD for all-sky conditions and −24 W m−2 per unit AOD for clear-sky conditions. The present-day direct TOA impact by all soot (BC) is +0.55 W m−2, when globally and annually averaged. Between +0.25 and +0.45 W m−2 of that can be attributed to anthropogenic sources, depending on assumptions for the preindustrial BC reference state. Similarly, the preindustrial fine-mode reference uncertainty has a strong influence not just on the direct effect but even more on the indirect effect. Present-day aerosol TOA forcing is estimated to stay within the −0.7 to −1.6 W m−2 range (with the best estimate at −1.0 W m−2). Calculations with scaled temporal changes to anthropogenic AOD from global modeling indicate that the global annual aerosol forcing has not changed much over the last decades, despite strong shifts in regional maxima for anthropogenic AOD. These regional shifts explain most solar insolation (brightening or dimming) trends that have been observed by ground-based radiation data.

Description: A simple plume implementation of the second version (v2) of the Max Planck Institute Aerosol Climatology, MACv2-SP, is described. MACv2-SP provides a prescription of anthropogenic aerosol optical properties and an associated Twomey effect. It was created to provide a harmonized description of post-1850 anthropogenic aerosol radiative forcing for climate modeling studies. MACv2-SP has been designed to be easy to implement, change and use, and thereby enable studies exploring the climatic effects of different patterns of aerosol radiative forcing, including a Twomey effect. MACv2-SP is formulated in terms of nine spatial plumes associated with different major anthropogenic source regions. The shape of the plumes is fit to the Max Planck Institute Aerosol Climatology, version 2, whose present-day (2005) distribution is anchored by surface-based observations. Two types of plumes are considered: one predominantly associated with biomass burning, the other with industrial emissions. These differ in the prescription of their annual cycle and in their optical properties, thereby implicitly accounting for different contributions of absorbing aerosol to the different plumes. A Twomey effect for each plume is prescribed as a change in the host model's background cloud-droplet population density using relationships derived from satellite data. Year-to-year variations in the amplitude of the plumes over the historical period (1850–2016) are derived by scaling the plumes with associated national emission sources of SO2 and NH3. Experiments using MACv2-SP are performed with the Max Planck Institute Earth System Model. The globally and annually averaged instantaneous and effective aerosol radiative forcings are estimated to be −0.6 and −0.5 W m−2, respectively. Forcing from aerosol–cloud interactions (the Twomey effect) offsets the reduction of clear-sky forcing by clouds, so that the net effect of clouds on the aerosol forcing is small; hence, the clear-sky forcing, which is more readily measurable, provides a good estimate of the total aerosol forcing.

Description: Tropospheric NO2 and stratospheric NO2 vertical column densities are important TROPOspheric Monitoring Instrument (TROPOMI) data products. In order to validate the TROPOMI NO2 products, KNMI Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instruments have measured NO2 on ship cruises over the Atlantic and the Pacific oceans. The MAX-DOAS instruments have participated in five cruises on board RV Sonne (in 2017 and 2019) and RV Maria S. Merian (in 2018). The MAX-DOAS measurements were acquired over 7 months and spanned about 90∘ in latitude and 300∘ in longitude. During the cruises aerosol measurements from Microtops sun photometers were also taken. The MAX-DOAS measured stratospheric NO2 columns between 1.5×1015 and 3.5×1015 molec cm−2 and tropospheric NO2 up to 0.6×1015 molec cm−2. The MAX-DOAS stratospheric NO2 vertical column densities have been compared with TROPOMI stratospheric NO2 vertical column densities and the stratospheric NO2 vertical column densities simulated by the global chemistry Transport Model, version 5, Massively Parallel model (TM5-MP). Good correlation is found between the MAX-DOAS and TROPOMI and TM5 stratospheric NO2 vertical column densities, with a correlation coefficient of 0.93 or larger. The TROPOMI and TM5 stratospheric NO2 vertical column densities are about 0.4×1015 molec cm−2 (19 %) higher than the MAX-DOAS measurements. The TROPOMI tropospheric NO2 also has good agreement with the MAX-DOAS measurements. The tropospheric NO2 vertical column density is as low as 0.5×1015 molec cm−2 over remote oceans.