Aerosol Radiative Forcing Research Articles

Identifying climate model structural inconsistencies allows for tight constraint of aerosol radiative forcing

Abstract. Aerosol radiative forcing uncertainty affects estimates of climate sensitivity and limits model skill in terms of making climate projections. Efforts to improve the representations of physical processes in climate models, including extensive comparisons with observations, have not significantly constrained the range of possible aerosol forcing values. A far stronger constraint, in particular for the lower (most-negative) bound, can be achieved using global mean energy balance arguments based on observed changes in historical temperature. Here, we show that structural deficiencies in a climate model, revealed as inconsistencies among observationally constrained cloud properties in the model, limit the effectiveness of observational constraint of the uncertain physical processes. We sample the uncertainty in 37 model parameters related to aerosols, clouds, and radiation in a perturbed parameter ensemble of the UK Earth System Model and evaluate 1 million model variants (different parameter settings from Gaussian process emulators) against satellite-derived observations over several cloudy regions. Our analysis of a very large set of model variants exposes model internal inconsistencies that would not be apparent in a small set of model simulations, of an order that may be evaluated during model-tuning efforts. Incorporating observations associated with these inconsistencies weakens any forcing constraint because they require a wider range of parameter values to accommodate conflicting information. We show that, by neglecting variables associated with these inconsistencies, it is possible to reduce the parametric uncertainty in global mean aerosol forcing by more than 50 %, constraining it to a range (around −1.3 to −0.1 W m−2) in close agreement with energy balance constraints. Our estimated aerosol forcing range is the maximum feasible constraint using our structurally imperfect model and the chosen observations. Structural model developments targeted at the identified inconsistencies would enable a larger set of observations to be used for constraint, which would then very likely narrow the uncertainty further and possibly alter the central estimate. Such an approach provides a rigorous pathway to improved model realism and reduced uncertainty that has so far not been achieved through the normal model development approach.

Impacts of haze and nitrogen oxide alleviation on summertime ozone formation: A modeling study over the Yangtze River Delta, China

The strict emission control measures have profoundly changed the air pollution in the Yangtze River Delta (YRD) region, China. However, the impacts of decreasing fine particulates (PM2.5) and nitrogen oxide (NOx) on summer ozone (O3) formation still remain disputable. We perform simulations in the 2018 summer over the YRD using the WRF-Chem model that considers the aerosol radiative forcing (ARF) and HO2 heterogeneous loss on aerosol surface. The model reasonably reproduces the measured spatiotemporal surface O3 and PM2.5 concentrations and aerosol compositions. Model sensitivity experiments show that the NOx mitigation during recent years changes daytime O3 formation in summer from the transition regime to the NOx-sensitive regime in the YRD. The decreasing NOx emission generally weakens O3 formation and lowers ambient O3 levels in summer during recent years, except for some urban centers of megacities. While, the haze alleviation characterized by a decline in ambient PM2.5 concentration in the past years largely counteracts the daytime O3 decrease caused by NOx mitigation, largely contributing to the persistently high levels of summertime O3. The counteracting effect is dominantly attributed to the attenuated ARF and minorly contributed by the suppressed HO2 uptake and heterogeneous loss on aerosol surface. These results highlight that the repeated O3 pollution in the YRD is closely associated with NOx and haze alleviation and more efforts must be taken to achieve lower O3 levels.

The Regional Aerosol Model Intercomparison Project (RAMIP)

Abstract. Changes in anthropogenic aerosol emissions have strongly contributed to global and regional trends in temperature, precipitation, and other climate characteristics and have been one of the dominant drivers of decadal trends in Asian and African precipitation. These and other influences on regional climate from changes in aerosol emissions are expected to continue and potentially strengthen in the coming decades. However, a combination of large uncertainties in emission pathways, radiative forcing, and the dynamical response to forcing makes anthropogenic aerosol a key factor in the spread of near-term climate projections, particularly on regional scales, and therefore an important one to constrain. For example, in terms of future emission pathways, the uncertainty in future global aerosol and precursor gas emissions by 2050 is as large as the total increase in emissions since 1850. In terms of aerosol effective radiative forcing, which remains the largest source of uncertainty in future climate change projections, CMIP6 models span a factor of 5, from −0.3 to −1.5 W m−2. Both of these sources of uncertainty are exacerbated on regional scales. The Regional Aerosol Model Intercomparison Project (RAMIP) will deliver experiments designed to quantify the role of regional aerosol emissions changes in near-term projections. This is unlike any prior MIP, where the focus has been on changes in global emissions and/or very idealised aerosol experiments. Perturbing regional emissions makes RAMIP novel from a scientific standpoint and links the intended analyses more directly to mitigation and adaptation policy issues. From a science perspective, there is limited information on how realistic regional aerosol emissions impact local as well as remote climate conditions. Here, RAMIP will enable an evaluation of the full range of potential influences of realistic and regionally varied aerosol emission changes on near-future climate. From the policy perspective, RAMIP addresses the burning question of how local and remote decisions affecting emissions of aerosols influence climate change in any given region. Here, RAMIP will provide the information needed to make direct links between regional climate policies and regional climate change. RAMIP experiments are designed to explore sensitivities to aerosol type and location and provide improved constraints on uncertainties driven by aerosol radiative forcing and the dynamical response to aerosol changes. The core experiments will assess the effects of differences in future global and regional (Africa and the Middle East, East Asia, North America and Europe, and South Asia) aerosol emission trajectories through 2051, while optional experiments will test the nonlinear effects of varying emission locations and aerosol types along this future trajectory. All experiments are based on the shared socioeconomic pathways and are intended to be performed with 6th Climate Model Intercomparison Project (CMIP6) generation models, initialised from the CMIP6 historical experiments, to facilitate comparisons with existing projections. Requested outputs will enable the analysis of the role of aerosol in near-future changes in, for example, temperature and precipitation means and extremes, storms, and air quality.

Shortwave absorption by wildfire smoke dominated by dark brown carbon

Wildfires emit large amounts of black carbon and light-absorbing organic carbon, known as brown carbon, into the atmosphere. These particles perturb Earth’s radiation budget through absorption of incoming shortwave radiation. It is generally thought that brown carbon loses its absorptivity after emission in the atmosphere due to sunlight-driven photochemical bleaching. Consequently, the atmospheric warming effect exerted by brown carbon remains highly variable and poorly represented in climate models compared with that of the relatively nonreactive black carbon. Given that wildfires are predicted to increase globally in the coming decades, it is increasingly important to quantify these radiative impacts. Here we present measurements of ensemble-scale and particle-scale shortwave absorption in smoke plumes from wildfires in the western United States. We find that a type of dark brown carbon contributes three-quarters of the short visible light absorption and half of the long visible light absorption. This strongly absorbing organic aerosol species is water insoluble, resists daytime photobleaching and increases in absorptivity with night-time atmospheric processing. Our findings suggest that parameterizations of brown carbon in climate models need to be revised to improve the estimation of smoke aerosol radiative forcing and associated warming.

Atmospheric heating in the US from saharan dust: Tracking the June 2020 event with surface and satellite observations

In June 2020, a record level of Saharan dust was transported across the Atlantic Ocean impacting air quality in the Caribbean Basin and the United States (US). Satellite images showed the transport, while a series of ground-based monitoring stations captured the surface impacts as the Saharan dust was transported to the Caribbean basin and then moved into the Southern (Houston, Texas; WL), Eastern (Bone, North Carolina; APP) and Midwestern (Bondville, Illinois; BND) US. The present study characterizes the Saharan dust event (SDE) using a comprehensive set of satellite observations and in-situ measurements of particulate matter (PM), and aerosol optical properties (AOPs; σscat: scattering coefficient, σabs: absorption coefficient, SAE: scattering Ångström exponent and AAE: absorption Ångström exponent). The Saharan dust intrusion was identified at each site by a marked increase in σscat, and AAE and a simultaneous decrease in SAE. A maximum hourly average PM2.5 concentration and σscat (525 nm) of 97.5 μg m−3 and 190 Mm−1 was observed at WL during the SDE. The maximum hourly average σscat (550 nm) for PM10 size cut of 215 and 66.9 Mm−1 was observed at APP and BND, respectively, during the SDE. The AAE at each site reached above 1.3 with an average value of 1.39 ± 0.35, 3.34 ± 0.56 and 1.65 ± 0.27 at WL, APP, and BND, respectively, during the SDE, whereas the average SAE dropped below 0.5 at WL and APP and below 0.9 at BND. The results demonstrated that the identification of SDE using AOPs depends largely on the location of the measurement, which determines the background characteristics of a site. The results suggest that other intensive AOPs like asymmetry parameter (g) and single scattering albedo Ångström exponent (SSAAE) can also be exploited to characterize SDE. Aerosol radiative forcing (ARF) estimates indicate that the SDE resulted in the heating of the atmosphere (+5.37 to +11.8 W m−2) at the rate of 0.11–0.24 K day−1 at the US sites. This atmospheric heating from transported Saharan dust can alter the regional atmospheric dynamics and is relevant to understand potential changes in regional climate.

The worldwide COVID-19 lockdown impacts on global secondary inorganic aerosols and radiative budget.

Global lockdown measures to prevent the spread of the coronavirus disease 2019 (COVID-19) led to air pollutant emission reductions. While the COVID-19 lockdown impacts on both trace gas and total particulate pollutants have been widely investigated, secondary aerosol formation from trace gases remains unclear. To that end, we quantify the COVID-19 lockdown impacts on NOx and SO2 emissions and sulfate-nitrate-ammonium aerosols using multiconstituent satellite data assimilation and model simulations. We find that anthropogenic emissions over major polluted regions were reduced by 19 to 25% for NOx and 14 to 20% for SO2 during April 2020. These emission reductions led to 8 to 21% decreases in sulfate and nitrate aerosols over highly polluted areas, corresponding to >34% of the observed aerosol optical depth declines and a global aerosol radiative forcing of +0.14 watts per square meter relative to business-as-usual scenario. These results point to the critical importance of secondary aerosol pollutants in quantifying climate impacts of future mitigation measures.

Optical properties and cloud condensation nuclei activity of brown carbon containing α–dicarbonyls and reduced nitrogen compounds

The aqueous–phase reaction of carbonyls with reduced nitrogen compounds (RNCs) is considered an important pathway for the formation of secondary BrC, and these particles could greatly impact the global climate. However, our knowledge of their properties is still limited. In this study, we measured the optical properties, cloud condensation nuclei (CCN) activity (represented as hygroscopicity parameter κCCN), and effective density (ρeff) under varied reaction conditions for BrC mixtures formed by reactions between two α–dicarbonyls (glyoxal GX and methylglyoxal MG) and three RNCs (ammonium sulfate AS, glycine GC, and dimethylamine DA). Our results showed a wide range of particle ρeff from 1.08 to 1.66 g cm−3, depending on the type of RNCs reactant. At 532 nm wavelength, the real part n of complex refractive index ranged from 1.41 to 1.60 and the imaginary part k of BrC ranged from 0.024 to 0.043, and the absorption cross section for MG mixtures were 20.3–51.0% higher than those of GX mixtures. These values did not appear to vary significantly with mixing molar ratios between RNCs and α–dicarbonyls (10:1, 1:1, and 1:3) for mixtures with the same reactants, but the mass absorption cross section for mixtures after a reaction time of 14 days were 1.57–74.2% higher than those of mixtures after reaction times of 0.5 and 7 days. The κCCN values of different BrC were consistent with the order of κCCN for single RNCs, i.e., AS–containing (0.349–0.428) > GC–containing (0.221–0.352) > DA–containing (0.090–0.131), and showed an overall increasing trend (1.47–59.3%) with the RNCs content. Our results highlight the importance of reaction conditions on secondary BrC properties and are helpful for a more accurate assessment of aerosol radiative forcing.

Satellite (GOSAT-2 CAI-2) retrieval and surface (ARFINET) observations of aerosol black carbon over India

Abstract. Light-absorbing black carbon (BC) aerosols strongly affect Earth's radiation budget and climate. This paper presents satellite retrieval of BC over India based on observations from the Cloud and Aerosol Imager-2 (CAI-2) on board the Greenhouse gases Observing Satellite-2 (GOSAT-2). To evaluate and validate the satellite retrievals, near-surface BC mass concentrations measured across the Aerosol Radiative Forcing over India NETwork (ARFINET) of aerosol observatories are used. Then the findings are extended to elucidate global BC features. The analysis reveals that this satellite retrieval clearly demonstrates the regional and seasonal features of BC over the Indian region, similarly to those recorded by surface observations. Validation and closure studies between the two datasets show RMSE < 1 and absolute difference below 2 µg m−3 for > 60 % of simultaneous observations, exhibiting good associations for December, January, and February (R of approximately 0.73) and March, April, and May (R approx. 0.76). Over the hotspot regions of India, satellite retrievals show a soot volume fraction of approx. 5 %, columnar single-scattering albedo of approx. 0.8, and BC column optical depth of approx. 0.1 during times of the highest BC loading, which are comparable to other in situ and satellite measurements. In terms of global spatiotemporal variation, satellite retrievals show higher BC occurring mostly in areas where biomass burning is intense. Overall, this study highlights the effectiveness of satellite retrieval of BC, which can be used effectively for the regular monitoring of BC loading attributable to vehicular, industrial, or biomass burning activities.

Optical Properties and Refractive Index of Wintertime Aerosol at a Highly Polluted North‐Indian Site

AbstractEstimation of aerosol radiative forcing continues to suffer from large uncertainties, partially from a lack of observations of aerosol optical properties. Limited measurements of the atmospheric aerosol imaginary refractive index (iRI) have been made, especially in some of the world's most polluted regions. In this study, we measured aerosol optical and micro‐physical properties at a regional site, Rohtak, India, representative of polluted cities in the Indo‐Gangetic plains in northern India. The average PM2.5 measured during the campaign was 163 μg/m3 with a single‐scatter albedo of 0.7, indicating the presence of strongly absorbing aerosol components. Measurements of aerosol absorption, scattering, and particle number size distributions were used to estimate the effective refractive index using an established Mie inversion technique. The calculated iRI was spectrally invariant in the visible region with values ranging between 0.076 and 0.145. Brown carbon absorption, estimated using an existing Mie optimization method, ranged 34–88 Mm−1, with strongly absorbing mass absorption cross‐sections (∼1.9 m2/g). Higher iRI were observed during periods with higher brown carbon absorption, which are likely directly emitted from combustion sources. Low volatility organic carbon fractions dominated during these periods, with likely persistence of atmospheric absorption. The iRI values are at the upper end of previously reported ranges of urban aerosol iRI. In a sensitivity analysis to measured parameters, the absorption had the dominant effect on estimated iRI. Measured single scatter albedos, were lower than those from climate model simulations over the region, demonstrating the need for intrinsic property measurements to evaluate and constrain climate models.

Progress of aerosol direct radiative forcing

Progress of aerosol direct radiative forcing

Analysis of Long‐Term Trends in the Vertical Distribution and Transport Paths of Atmospheric Aerosols in Typical Regions of China Using 15 Years of CALIOP Data

AbstractLong‐range transport and vertical distribution of aerosols are important factors for assessing the uncertainty in aerosol radiative forcing. This paper reveals the vertical distribution and trends of aerosol optical properties in China using 15 years of Cloud‐Aerosol Lidar with Orthogonal Polarization (CALIOP) data. The Hybrid Single‐Particle Lagrangian integrated trajectory model was used to analyze the transport and trends of aerosols in the layer with the highest occurrence frequencies of dust, polluted dust, polluted continental and elevated smoke aerosols. The results indicated that (a) there were significant regional and seasonal differences in the vertical distribution of aerosols. The aerosol optical depth (AOD) trend in a given region depends on the changes in the aerosol type with the highest frequency and the layer corresponding to the largest AOD in the vertical profile. The frequency of polluted dust aerosols was the highest in Beijing‐Tianjin‐Hebei (BTH) and Central China. The considerable decrease in the 0–2 km AOD led to a significant trend of the column AOD. (b) The changes of AOD and main aerosol types in a region are also affected by the changes of aerosol sources and long‐range transport pathways. In the BTH, dust aerosols originated from the Mongolian Plateau, accounting for 57.88% of the total trajectories. The Pearl River Delta was dominated by elevated smoke aerosols, with trajectories mainly originating from the Myanmar and Vietnam, accounting for 27.38% and 29.59%, respectively. The trend of 15‐year backward trajectories of dust aerosols on the Tibetan Plateau indicated that the trajectory from India is increasing.

Change from aerosol-driven to cloud-feedback-driven trend in short-wave radiative flux over the North Atlantic

Abstract. Aerosol radiative forcing and cloud–climate feedbacks each have a large effect on climate, mainly through modification of solar short-wave radiative fluxes. Here we determine what causes the long-term trends in the upwelling short-wave (SW) top-of-the-atmosphere (TOA) fluxes (FSW↑) over the North Atlantic region. Coupled atmosphere–ocean simulations from the UK Earth System Model (UKESM1) and the Hadley Centre General Environment Model (HadGEM3-GC3.1) show a positive FSW↑ trend between 1850 and 1970 (increasing SW reflection) and a negative trend between 1970 and 2014. We find that the 1850–1970 positive FSW↑ trend is mainly driven by an increase in cloud droplet number concentration due to increases in aerosol, while the 1970–2014 trend is mainly driven by a decrease in cloud fraction, which we attribute mainly to cloud feedbacks caused by greenhouse gas-induced warming. In the 1850–1970 period, aerosol-induced cooling and greenhouse gas warming roughly counteract each other, so the temperature-driven cloud feedback effect on the FSW↑ trend is weak (contributing to only 23 % of the ΔFSW↑), and aerosol forcing is the dominant effect (77 % of ΔFSW↑). However, in the 1970–2014 period the warming from greenhouse gases intensifies, and the cooling from aerosol radiative forcing reduces, resulting in a large overall warming and a reduction in FSW↑ that is mainly driven by cloud feedbacks (87 % of ΔFSW↑). The results suggest that it is difficult to use satellite observations in the post-1970 period to evaluate and constrain the magnitude of the aerosol–cloud interaction forcing but that cloud feedbacks might be evaluated. Comparisons with observations between 1985 and 2014 show that the simulated reduction in FSW↑ and the increase in temperature are too strong. However, the temperature discrepancy can account for only part of the FSW↑ discrepancy given the estimated model feedback strength (λ=∂FSW∂T). The remaining discrepancy suggests a model bias in either λ or in the strength of the aerosol forcing (aerosols are reducing during this time period) to explain the too-strong decrease in FSW↑, with a λ bias being the most likely. Both of these biases would also tend to cause too-large an increase in temperature over the 1985–2014 period, which would be consistent with the sign of the model temperature bias reported here. Either of these model biases would have important implications for future climate projections using these models.

Implications of differences between recent anthropogenic aerosol emission inventories for diagnosed AOD and radiative forcing from 1990 to 2019

Abstract. This study focuses on implications of differences between recent global emissions inventories for simulated trends in anthropogenic aerosol abundances and radiative forcing (RF) over the 1990–2019 period. We use the ECLIPSE version 6 (ECLv6) and CEDS year 2021 release (CEDS21) as input to the chemical transport model OsloCTM3 and compare the resulting aerosol evolution to corresponding results derived with the first CEDS release, as well as to observed trends in regional and global aerosol optical depth (AOD). Using CEDS21 and ECLv6 results in a 3 % and 6 % lower global mean AOD compared to CEDS in 2014, primarily driven by differences over China and India, where the area average AOD is up to 30 % lower. These differences are considerably larger than the satellite-derived interannual variability in AOD. A negative linear trend over 2005–2017 in global AOD following changes in anthropogenic emissions is found with all three inventories but is markedly stronger with CEDS21 and ECLv6. Furthermore, we confirm that the model better captures the sign and strength of the observed AOD trend over China with CEDS21 and ECLv6 compared to using CEDS, while the opposite is the case for South Asia. We estimate a net global mean aerosol-induced RF in 2014 relative to 1990 of 0.08 W m−2 for CEDS21 and 0.12 W m−2 for ECLv6, compared to 0.03 W m−2 with CEDS. Using CEDS21, we also estimate the RF in 2019 relative to 1990 to be 0.10 W m−2, reflecting the continuing decreasing trend in aerosol loads post-2014. Our results facilitate more rigorous comparison between existing and upcoming studies of climate and health effects of aerosols using different emission inventories.

Retrieval of aerosol single scattering albedo using joint satellite and surface visibility measurements

Aerosol single scattering albedo (SSA) measuring the ratio of scattering to extinction is a critical parameter in determining aerosol radiative effect. However, the retrieval of SSA from satellite platforms is limited because most existing passive satellite sensors such as Moderate Resolution Imaging Spectroradiometer (MODIS) only provide the measurements of reflected solar radiation at the top of the atmosphere (TOA), which are only capable of retrieving aerosol optical depth (AOD) on the basis of assumed SSA. In this study, we develop a machine learning based algorithm to retrieve SSA using joint surface visibility and satellite radiation measurements. With ancillary information such as meteorological condition, surface visibility can be regarded as a proxy of column AOD. By combining MODIS measured TOA apparent reflectance with ground visibility as well as other auxiliary parameters, we retrieve SSA at over 6000 visibility stations worldwide. The validation results during the period from 2010 to 2019 show high consistency with AERONET retrieved SSA, with daily, monthly, and seasonal retrievals all exhibiting high correlations of 0.68, 0.96, and 0.97, respectively. Daily, monthly, and seasonal RMSE values are 0.044, 0.012, and 0.011, respectively. The mean absolute bias (MAB) of daily retrievals is 0.031 and 62% of the samples fall within the uncertainty interval of ±0.03. Monthly and seasonal MAB values decrease to below 0.01. Over 97% of the monthly and seasonal retrievals are within the error envelope of ±0.03. Our work generates a global aerosol SSA dataset with extensive coverage over land, which can be used for validating and improving climate models and the estimation of aerosol radiative forcing.

Atmospheric aerosol size distribution impacts radiative effects over the Himalayas via modulating aerosol single-scattering albedo

The single-scattering albedo (SSA) of atmospheric aerosols is a key parameter that controls aerosol radiative effects. The variation of SSA is thought to be mainly regulated by aerosol absorption in the Himalayas and South Asia, but observations contradict this idea. In situ field campaigns conducted over two Himalayan sites revealed that SSA was strongly dependent on scattering but weakly correlated with absorption. Observational results combined with the Mie theory further illustrated that SSA was primarily modulated by size distribution rather than absorption. Aerosol Robotic Network (AERONET) data showed similar impacts of size distribution on SSA and that aerosol radiative forcing efficiencies were significantly dependent on SSA. Aerosol size distribution therefore considerably affects radiative forcing by modulating aerosol SSA over the Himalayas. This study highlighted the influence of aerosol size distribution on radiative forcing over the Himalayas, which has important implications for understanding aerosol radiative effects globally.

Absorbing Aerosol Optical Properties and Radiative Effects on Near-Surface Photochemistry in East Asia

Absorbing aerosols have significant influences on tropospheric photochemistry and regional climate change. Here, the direct radiative effects of absorbing aerosols at the major AERONET sites in East Asia and corresponding impacts on near-surface photochemical processes were quantified by employing a radiation transfer model. The average annual aerosol optical depth (AOD) of sites in China, Korea, and Japan was 1.15, 1.02 and 0.94, respectively, and the corresponding proportion of absorbing aerosol optical depth (AAOD) was 8.61%, 6.69%, and 6.49%, respectively. The influence of absorbing aerosol on ultraviolet (UV) radiation mainly focused on UV-A band (315–400 nm). Under the influence of such radiative effect, the annual mean near-surface J[NO2] (J[O1D]) of sites in China, Korea, and Japan decreased by 16.95% (22.42%), 9.61% (13.55%), and 9.63% (13.79%), respectively. In Beijing–Tianjin–Hebei (BTH) and Yangtze River Delta (YRD) region, the annual average AOD was 1.48 and 1.29, and the AAOD was 0.14 and 0.13, respectively. The UV radiative forcing caused by aerosols dominated by black carbon (BC-dominated aerosols) on the surface was −3.19 and −2.98 W m−2, respectively, accounting for about 40% of the total aerosol radiative forcing, indicating that the reduction efficiency of BC-dominated aerosols on solar radiation was higher than that of other types of aerosols. The annual mean J[NO2] (J[O1D]) decreased by 14.90% (20.53%) and 13.71% (18.20%) due to the BC-dominated aerosols. The daily maximum photolysis rate usually occurred near noon due to the diurnal variation of solar zenith angle and, thus, the daily average photolysis rate decreased by 2–3% higher than that average during 10:00–14:00.

A new method to estimate aerosol radiative forcing on photosynthetically active radiation

A new method to estimate aerosol radiative forcing (ARF) on photosynthetically active radiation (PAR) is proposed using as input only the solar position and global irradiance measurements, available in many radiometric stations worldwide. The main contribution of this work is the proposal of a new and simple tool (max-kt method) based in the parameterization of the envelope of the relationship between clearness index (kt) and the solar position. To this aim, a 1-year database (2020) of cloud-free data acquired in a Southwest Mediterranean site was used for the proposal and two more years (2017 and 2018) were used to extend the results. The ARF values retrieved using the new method were compared with estimates calculated by two physical models widely employed in the literature, such as the SBDART (Santa Barbara DISORT Atmospheric Radiative Transfer model) and an improved version of the CPCR2 (Code for Physical Computation of Radiation, 2 bands) model. The new method provided ARF values of the order of those provided by these physical models, especially with the SBDART model, confirming the validity of this new method. An ARF seasonal pattern was found with higher values in summer, (−30,7 ± 9,0) Wm−2 in August during 2017, (−40,1 ± 11,8) Wm−2 in June during 2018 and (−28,8 ± 7,7) Wm−2 in July during 2020 and minimum values in winter, (−8,1 ± 5,1) Wm−2 in January during 2017, (−5,7 ± 5,8) Wm−2 in December during 2018 and (−7,8 ± 5,4) Wm−2 in December during 2020. Moreover, a dependence on solar zenith angle (θz) was detected excepting during the year 2018, increasing ARF absolute values at θz from 0° to 45°-60° and decreasing to zero for the Sun near the horizon. This technique is very useful due to the difficulty of knowing all the inputs requested by the physical models.

Broadband spectrum characteristics and radiative effects of primary brown carbon from wood pyrolysis

Brown carbon (BrC), known as light-absorbing organic aerosol in the near-ultraviolet (UV) and short visible region, plays a significant role in the global and regional climate change. A detailed understanding of the spectral optical properties of BrC is beneficial for reducing the uncertainty in radiative forcing calculation. In this work, the spectral properties of primary BrC were investigated by using a four-wavelength broadband cavity-enhanced albedometer with central wavelengths at 365, 405, 532 and 660 nm. The BrC samples were generated by the pyrolysis of three types of wood. During the pyrolysis process, the measured average single scattering albedo (SSA) at 365 nm was about 0.66 to 0.86, where the average absorption Ångström exponent (AAE) was between 5.8 and 7.8, and the average extinction Ångström exponent (EAE) was within 2.1 to 3.5. The full spectral measurement of SSA (300–700 nm) was realized by an optical retrieval method and the retrieved SSA spectrum was directly applied to evaluate aerosol direct radiative forcing (DRF) efficiency. The DRF efficiency over ground of various primary BrC emissions increased from 5.3 % to 68 % as compared to the non-absorbing organic aerosol assumption. A decrease of about 35 % in SSA would cause the DRF efficiency over ground to change from cooling effect to warming effect (from −0.33 W/m2 to +0.15 W/m2) in the near-UV band (365–405 nm). The DRF efficiency over ground of strongly absorptive primary BrC (lower SSA) contributed 66 % more than weakly absorptive primary BrC (higher SSA). These findings proved the importance of broadband spectral properties of BrC, which are substantial for radiative forcing evaluation of BrC and should be considered in global climate models.

Small and large particle limits of the asymmetry parameter for homogeneous, spherical particles

The aerosol single scattering asymmetry parameter g is an important intensive particle parameter in determining aerosol direct radiative forcing and radiation pressure. For homogeneous spherical particles and a complex refractive index that is independent of wavelength, g is solely dependent on the size parameter x, the ratio of the particle circumference to the wavelength, and the complex refractive index m of the particle. Here, we explore this dependency for the small and large particle limits with size parameters much smaller and much larger than one. We show that in the small particle (Rayleigh) regime, g is proportional to x2, and give the proportionality factor as a function of the complex m. In addition, we separate regions in the complex refractive index space where the asymmetry parameter is negative (dominantly backscattering) and where it is positive (dominantly forward scattering). In the large particle limit, the geometric optics regime, g converges to a constant value that is a function of m.

Evaluation of aerosol–cloud interactions in E3SM using a Lagrangian framework

Abstract. A Lagrangian framework is used to evaluate aerosol–cloud interactions in the U.S. Department of Energy's Energy Exascale Earth System Model (E3SM) version 1 (E3SMv1) for measurements taken at Graciosa Island in the Azores where a U.S. Department of Energy Atmosphere Radiation Measurement (ARM) site is located. This framework uses direct measurements of cloud condensation nuclei (CCN) concentration (instead of relying on satellite retrievals of aerosol optical depth) and incorporates a suite of ground-based ARM measurements, satellite retrievals, and meteorological reanalysis products that when applied to over a 1500 trajectories provides key insights into the evolution of low-level clouds and aerosol radiative forcing that is not feasible from a traditional Eulerian analysis framework. Significantly lower concentrations (40 %) of surface CCN concentration are measured when precipitation rates in 48 h back trajectories average above 1.2 mm d−1 in the Integrated Multi-satellitE Retrievals for Global Precipitation Measurement (IMERG) product. The depletion of CCN concentration when precipitation rates are elevated is nearly twice as large in the ARM observations compared to E3SMv1 simulations. The model CCN concentration bias remains significant despite modifying the autoconversion and accretion rates in warm clouds. As the clouds in trajectories associated with larger surface-based CCN concentration advect away from Graciosa Island, they maintain higher values of droplet number concentrations (Nd) over multiple days in observations and E3SM simulations compared to trajectories that start with lower CCN concentrations. The response remains robust even after controlling for meteorological factors such as lower troposphere stability, the degree of cloud coupling with the surface, and island wake effects. E3SMv1 simulates a multi-day aerosol effect on clouds and a Twomey radiative effect that is within 30 % of the ARM and satellite observations. However, the mean cloud droplet concentration is more than 2–3 times larger than in the observations. While Twomey radiative effects are similar amongst autoconversion and accretion sensitivity experiments, the liquid water path and cloud fraction adjustments are positive when using a regression model as opposed to negative when using the present-day minus pre-industrial aerosol emissions approach. This result suggests that tuning the autoconversion and accretion alone is unlikely to produce the desired aerosol susceptibilities in E3SMv1.