Estimate Aerosol Radiative Forcing Research Articles

MieAI: a neural network for calculating optical properties of internally mixed aerosol in atmospheric models

Aerosols influence weather and climate by interacting with radiation through absorption and scattering. These effects heavily rely on the optical properties of aerosols, which are mainly governed by attributes such as morphology, size distribution, and chemical composition. These attributes undergo continuous changes due to chemical reactions and aerosol micro-physics, resulting in significant spatio-temporal variations. Most atmospheric models struggle to incorporate this variability because they use pre-calculated tables to handle aerosol optics. This offline approach often leads to substantial errors in estimating the radiative impacts of aerosols along with posing significant computational burdens. To address this challenge, we introduce a computationally efficient and robust machine learning approach called MieAI. It allows for relatively inexpensive calculation of the optical properties of internally mixed aerosols with a log-normal size distribution. Importantly, MieAI fully incorporates the variability in aerosol chemistry and microphysics. Our evaluation of MieAI against traditional Mie calculations, using number concentrations from the ICOsahedral Nonhydrostatic model with Aerosol and Reactive Trace gases (ICON-ART) simulations, demonstrates that MieAI exhibits excellent predictive accuracy for aerosol optical properties. MieAI achieves this with errors well within 10%, and it operates more than 1000 times faster than the benchmark approach of Mie calculations. Due to its generalized nature, the MieAI approach can be implemented in any chemistry transport model which represents aerosol size distribution in the form of log-normally distributed internally mixed modes. This advancement has the potential to replace frequently employed look-up tables and plays a substantial role in the ongoing attempts to reduce uncertainties in estimating aerosol radiative forcing.

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.

Aerosol characteristics over Indo-Gangetic Plain from ground-based AERONET and MERRA-2/CAMS model simulations

A comprehensive investigation of physical, optical, and chemical characteristics of columnar aerosols over two locations with distinct environmental settings in the Indo-Gangetic Plain (IGP) region, namely, Kanpur (urban and industrial area) and Gandhi College (rural area), is conducted using high-quality aerosol datasets obtained from ground-based Aerosol Robotic Network (AERONET) observations during the recent five year period (2015–2019). This study utilizes all the crucial columnar aerosol parameters necessary for accurately estimating aerosol radiative forcing. Quantification of contribution by different aerosol species originating from natural and anthropogenic sources to the total aerosol optical depth (AOD) and single scattering albedo (SSA) is important to understand the specific mechanisms that influence the aerosol composition, thereby reducing the uncertainty in aerosol radiative forcing. For the first time, two highly spatially resolved models' (Modern-Era Retrospective Analysis for Research and Applications-2 (MERRA-2) and Copernicus Atmosphere Monitoring Service (CAMS)) simulated absorbing species-wise (black carbon (BC), dust, and brown carbon (BrC)) AOD, and absorption AOD (AAOD) are compared and contrasted against the AERONET observations over the IGP region in a systematic manner. MERRA-2 AODs are mostly lower, whereas CAMS AODs are consistently higher than the AERONET AODs. A comparison of collocated time and space observations with models clearly suggests that improvements in emission inventories on a seasonal scale are essential. MERRA-2 SSA is noted lower than the AERONET SSA during the winter season due to overestimation in BC AOD. During winter in >70% of MERRA-2 simulated SSA the difference is higher than ±0.03 (the uncertainty range of AERONET SSA) whereas during pre-monsoon and monsoon seasons >60% of MERRA-2 SSA lies within the uncertainty range of AERONET SSA. Both models show a gradient in AODDust decreasing from west to east in the IGP. However, observations do not often exhibit the gradient in dust, which is validated by air mass back trajectory analyses as air masses travel through different pathways to IGP and reverse the west to east gradient in AODDust. This quantitative and comparative collocated analysis of observed aerosol characteristics with models on a seasonal scale will enable a better estimation of aerosol radiative forcing, and can help improve aerosol processes and parameterizations in models.

Determination of the refractive index of ambient aerosols

Abstract The refractive index of ambient aerosols is one of the most important parameters indicating the scattering and absorption properties of aerosols. We proposed a new method for retrieving the refractive index (RI) of ambient particles. The main advantage of our method is that it assimilates the single particle mixing states measured by a single-particle soot photometer, when compared to the traditional optical method of retrieving the ambient aerosol RI. This method was validated by good consistency between the determined RI with this method and retrieved RI with the method of Zhao et al. (2019c) using datasets from field measurements conducted in East China in June of 2018. The results show that the real part of the refractive index of the black carbon (BC)-free particles ranged between 1.37 and 1.51 and this value changed little across different tested wavelengths. The mean complex refractive index for the refractory BC was 1.67 ± 0.67i at 525 nm. The mean imaginary parts of the other non-BC components were 0.019 and 0.023 at 450 nm and 370 nm respectively. Brown carbon contributed to 5%, 13% and 29% of the ambient aerosol light absorption at 525 nm, 450 nm and 370 nm respectively in East China. This study provides the ability to determine the ambient aerosol complex refractive index and these data can be used in models to reduce the uncertainties in estimating aerosol radiative forcing.

Method to measure the size-resolved real part of aerosol refractive index using differential mobility analyzer in tandem with single-particle soot photometer

Abstract. Knowledge on the refractive index of ambient aerosols can help reduce the uncertainties in estimating aerosol radiative forcing. A new method is proposed to retrieve the size-resolved real part of the refractive index (RRI). The main principle of deriving the RRI is measuring the scattering intensity by a single-particle soot photometer (SP2) of size-selected aerosols. This method is validated by a series of calibration experiments using the components of the known RRI. The retrieved size-resolved RRI covers a wide range, from 200 to 450 nm, with uncertainty of less than 0.02. Measurements of the size-resolved RRI can improve the understanding of the aerosol radiative effects.

Aerosol optical characteristics and radiative forcing in urban Beijing

Atmospheric aerosol particles exert significant influence on the earth's radiation budget, and accurate measurement of aerosol optical properties can help reduce the uncertainties in estimating aerosol radiative forcing. Therefore, year-round measurements of aerosol optical properties from August 2016 to July 2017 at an urban site in Beijing were analysed. The results show that the annual mean scattering coefficient (σsp at 550 nm, 131 ± 135 Mm−1) was approximately half of the measurement in Beijing from 2008 to 2009 and from 2005 to 2006, mainly due to the reduction of PM2.5 and scattering aerosols in recent years. Meanwhile, annual mean of σabs (637 nm) and SSA was 14 ± 11 Mm−1 and 0.85 ± 0.06, respectively. Seasonally, σsp during winter was approximately two times higher than in other seasons, while σabs was higher during autumn and winter, which may be attributed to biomass and fossil fuel burning under a shallow and stable boundary layer. Diurnal variation of σsp showed an evening peak and a slight morning peak in spring and summer, as well as a night peak in autumn and winter. σabs in four seasons were basically unimodal, with a morning peak in spring and summer, and a night peak in autumn and winter. In addition, the scattering Ångström exponent and backscattering Ångström exponent suggested the dominance of micro-size aerosols. Seasonal variations of SAE, BAE and the backscatter fraction indicated a larger proportion of isotropic scattering and fine-mode particles in summer and autumn, as well as a dominance of coarse particles in spring and a complicated aerosol type distribution and emission sources in winter. Furthermore, radiative forcing was estimated by a radiative transfer model. Radiative forcing varied between −6.69 and −235.67 Wm-2 (with the average of −54.93 ± 39.92 Wm-2) at the surface, with a mean of 35.56 ± 22.88 Wm-2 in the atmosphere.

Scattering and absorption characteristics of aerosols at an urban megacity over IGB: Implications to radiative forcing

Aerosol scattering and absorption characteristics were investigated at an urban megacity Delhi in the western Indo-Gangetic Basin (IGB) during the period from October 2011 to September 2012 using different in-situ measurements. The scattering coefficient (σsp at 550 nm) varied between 71 and 3014 Mm−1 (mean ~710 ± 615 Mm−1) during the entire study period, which was about ten times higher than the absorption coefficient (σabs at 550 nm ~67 ± 40 Mm−1). Seasonally, σsp and σabs were substantially higher during the winter/post-monsoon periods, which also gave rise to single scattering albedo (SSA) by ~5%. The magnitude of SSA (at 550 nm) varied between 0.81 and 0.94 (mean: 0.89 ± 0.05). Further, the magnitude of scattering Ångström exponent (SAE) and back-scattering Ångström exponent (BAE) showed a wide range from −1.20 to 1.57 and −1.13 to 0.87, respectively which suggests large variability in aerosol sizes and emission sources. Relatively higher aerosol backscatter fraction (b at 550 nm) during the monsoon (0.25 ± 0.10) suggests more inhomogeneous scattering, associated with the coarser dust particles. However, lower value of b during winter (0.13 ± 0.02) is associated with more isotropic scattering due to dominance of smaller size particles. This is further confirmed with the estimated asymmetry parameter (AP at 550 nm), which exhibits opposite trend with b. The aerosol optical parameters were used in a radiative transfer model to estimate aerosol radiative forcing. A mean radiative forcing of −61 ± 22 W m−2 (ranging from −111 to −40 W m−2) was observed at the surface and 42 ± 24 W m−2 (ranging from 18 to 87 W m−2) into the atmosphere, which can give rise to the mean atmospheric heating rate of 1.18 K day−1.

Importance of aerosol non-sphericity in estimating aerosol radiative forcing in Indo-Gangetic Basin

Aerosols are usually presumed spherical in shape while estimating the direct radiative forcing (DRF) using observations or in the models. In the Indo-Gangetic Basin (IGB), a regional aerosol hotspot where dust is a major aerosol species and has been observed to be non-spherical in shape, it is important to test the validity of this assumption. We address this issue using measured chemical composition at megacity Delhi, a representative site of the western IGB. Based on the observation, we choose three non-spherical shapes - spheroid, cylinder and chebyshev, and compute their optical properties. Non-spherical dust enhances aerosol extinction coefficient (βext) and single scattering albedo (SSA) at visible wavelengths by >0.05km−1 and >0.04 respectively, while it decreases asymmetry parameter (g) by ~0.1. Accounting non-sphericity leads top-of-the-atmosphere (TOA) dust DRF to more cooling due to enhanced backscattering and increases surface dimming due to enhanced βext. Outgoing shortwave flux at TOA increases by up to 3.3% for composite aerosols with non-spherical dust externally mixed with other spherical species. Our results show that while non-sphericity needs to be accounted for, choice of shape may not be important in estimating aerosol DRF in the IGB.

Assessment of aerosols optical properties and radiative forcing over an Urban site in North-Western India

ABSTRACTThe present work is aimed to analyze aerosols optical properties and to estimate aerosol radiative forcing (ARF) from January to December 2013, using sky radiometer data over Rohtak, an urban site in North-Western India. The results reveal strong wavelength dependency of aerosol optical depth (AOD), with high values of AOD at shorter wavelengths and lower values at longer wavelength during the study period. The highest AOD values of 1.07 ± 0.45 at 500 nm were observed during July. A significant decline in Ångström exponent was observed during April–May, which represents the dominance of coarse mode particles due to dust-raising convective activities. Aerosols’ size distribution exhibits a bimodal structure with fine mode particles around 0.17 µm and coarse mode particles with a radius around 5.28 µm. Single scattering albedo values were lowest during November–December at all wavelengths, ranging from 0.87 to 0.76, which corresponds to the higher absorption during this period. Aerosols optical properties retrieved during observation period are used as input for SBDART (Santa Barbara DISORT Atmospheric Radiative Transfer) to estimate the direct ARF at the surface, in the atmosphere and at the top of the atmosphere (TOA). The ARF at the TOA, surface and in the atmosphere are found to be in the range of −4.98 to −19.35 W m−2, −8.01 to −57.66 W m−2 and +3.02 to +41.64 W m−2, respectively. The averaged forcing for the whole period of observations at the TOA is −11.26 W m−2, while at the surface it is −38.64 W m−2, leading to atmospheric forcing of 27.38 W m−2. The highest (1.168 K day−1) values of heating rate was estimated during November, whereas the lowest value (0.084 K day−1) was estimated for the February.

Decadal variation of East Asian radiative forcing due to anthropogenic aerosols during 1850–2100, and the role of atmospheric moisture

An aerosol mass dataset simulated from a chemical transport model for the period 1850 to 2100 is used in an atmospheric general circulation model to investigate anthropogenic aerosol radiative forcing (RF) with a focus on East Asia. Compared to the pre-industrial era, the calculated strongest global mean direct RF (DRF) of −0.30 W m−2 at the all-sky top of the atmosphere (TOA) occurs in the 1980s and an indirect cloud albedo forcing (CAF) of −0.67 W m−2 in the 2000s; a maximum atmospheric DRF of 0.48 W m−2, mainly by black carbon absorption, is found in the 2010s. Much larger aerosol DRF and CAF values are distributed over East Asia until the 2010s, and the negative surface and positive atmospheric DRF in Eastern China is even projected to maintain a magnitude of 5.0 W m−2 until the 2030s. Increasing East Asian aerosol loading has shifted the anthropogenic aerosol RF centers to lower latitudes in the Northern Hemisphere since the 1980s, and this trend is more severe under future midand high-range emission scenarios. Further results indicate that larger DRF values over East Asia can be partly attributed to climatological summer atmospheric moisture that is higher relative to Norther American and European regions, which enhances the aerosol hygroscopic effect, then strengthens aerosol optical depth and DRF at clear-sky TOA and surface, and even influences their long-term changes. The observational comparisons reveal that present day simulated surface concentrations of key anthropogenic aerosol species and resulting optical depth are highly underestimated in Eastern China. Further research on simulated meteorology and aerosol features is therefore recommended to reduce the uncertainties in estimating aerosol RF over East Asia.

Direct radiative forcing of anthropogenic aerosols over oceans from satellite observations

Anthropogenic aerosols play an important role in the atmospheric energy balance. Anthropogenic aerosol optical depth (AOD) and its accompanying shortwave radiative forcing (RF) are usually simulated by numerical models. Recently, with the development of space-borne instruments and sophisticated retrieval algorithms, it has become possible to estimate aerosol radiative forcing based on satellite observations. In this study, we have estimated shortwave direct radiative forcing due to anthropogenic aerosols over oceans in all-sky conditions by combining clouds and the Single Scanner Footprint data of the Clouds and Earth’s Radiant Energy System (CERES/SSF) experiment, which provide measurements of upward shortwave fluxes at the top of atmosphere, with Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol and cloud products. We found that globally averaged aerosol radiative forcing over oceans in the clear-sky conditions and all-sky conditions were −1.03±0.48 W m−2 and −0.34 ±0.16 W m−2, respectively. Direct radiative forcing by anthropogenic aerosols shows large regional and seasonal variations. In some regions and in particular seasons, the magnitude of direct forcing by anthropogenic aerosols can be comparable to the forcing of greenhouse gases. However, it shows that aerosols caused the cooling effect, rather than warming effect from global scale, which is different from greenhouse gases.

Reply to comment by S. Ramachandran on “Surface changes in solar irradiance due to aerosols over central Himalayas”

[1] Dumka et al. [2006] (hereinafter referred as D06) made extensive measurements of radiative fluxes at the surface during December 2004 at Manora Peak, in the Shivalik ranges of the Central Himalayas during a comprehensive aerosol field campaign as a part of the Indian Space Research Organisation's Geosphere Biosphere Programme (ISRO-GBP). The surface radiative fluxes were used to estimate aerosol radiative forcing. Based on the data analysis D06 concluded that the anthropogenic (from valley below) transported upwards by atmospheric boundary layer (ABL) dynamics during daytime provide an atmosphere conducive for mixed aerosols and suggested that focused efforts are needed to address this issue.

Surface changes in solar irradiance due to aerosols over central Himalayas

During a comprehensive aerosol field campaign as a part of the ISRO‐GBP, extensive measurements of radiative fluxes at the surface were made during December 2004 at Manora Peak, in the Shivalik ranges of the Central Himalayas. The surface radiative fluxes were used to estimate aerosol radiative forcing. Our analysis clearly shows that during the clean atmospheric conditions over Manora Peak, the observed aerosol radiative forcing is in good agreement to those of modeled ones, while for the higher aerosol optical depths (AODs), modeled values are significantly smaller than the observed ones. It was observed that at Manora Peak, the anthropogenic aerosols (from valley below) transported upwards by evolution of boundary layer during the daytime provide an atmosphere conducive for ‘mixed’ aerosols. Focused efforts are needed to address this issue for which simultaneous observations at high altitude site with those in nearby valley are essential.

Wintertime aerosol properties during foggy and nonfoggy days over urban center Delhi and their implications for shortwave radiative forcing

We present results from complimentary measurements of physical and optical properties of aerosols carried out at Delhi, as part of the Indian Space Research Organization Geosphere Biosphere Programme's Land Campaign II in December 2004. For the first time we unravel ground truth values of several radiatively important aerosol parameters such as their wavelength dependency in absorption, scattering behavior, single‐scattering albedo, number size distribution, and vertical distribution in the atmosphere from this polluted megacity in south Asia. Interesting features are observed in the behavior of aerosol parameters under intermittent foggy, hazy, and clear‐sky conditions prevalent during the campaign. All aerosol parameters exhibited a large distribution in their values, with variabilities being particularly higher on hazy and foggy days. The average clear‐sky aerosol optical depth (AOD) value is 0.91 ± 0.48, which is higher than the AOD value reported for most other cities in India during this season of the year. Increases in AOD on hazy and foggy days are found to be spectrally nonuniform. The percentage increase in AOD at shorter wavelengths was higher on hazy days compared to clear days. Diurnally averaged BC mass concentration varied from a low of 15 μg/m3 during clear days to a high of about 65 μg/m3 on hazy days. The wavelength dependency of aerosol absorption shows signatures of the presence of a significant amount of absorbing aerosols produced from biofuel/biomass burning. Single‐scattering albedo at 525 nm is found to vary between 0.6 and 0.8 with an average value of 0.68 for the entire period. Lidar observations reveal that during a fog event there is a subsidence of aerosols to an extremely dense and shallow atmospheric layer of less than 200 m height from the surface. The presence of an aerosol layer at elevated altitudes is also detected. All the results are combined and used for estimating aerosol radiative forcing using a discrete ordinate radiative transfer model. We find a large negative forcing at the surface level in the range of −40 to −86 W/m2, while forcing at the top of the atmosphere varied between −2 and +3 W/m2.

A Method to Estimate Aerosol Radiative Forcing from Spectral Optical Depths

Abstract Radiative forcing of aerosols is much more difficult to estimate than that of well-mixed gases due to the large spatial variability of aerosols and the lack of an adequate database on their radiative properties. Estimation of aerosol radiative forcing generally requires knowledge of its chemical composition, which is sparse. Ground-based sky radiance measurements [e.g., aerosol robotic network (AERONET)] can provide key parameters such as the single-scattering albedo, but in shipborne experiments over the ocean it is difficult to make sky radiance measurements and hence these experiments cannot provide parameters such as the single-scattering albedo. However, aerosol spectral optical depth data (cruise based as well as satellite retrieved) are available quite extensively over the ocean. Spectral optical depth measurements have been available since the 1970s, and spectral turbidity measurements (carried out at meteorological departments all over the world) have been available for several decades, while long-term continuous chemical composition information is not available. A new method to differentiate between scattering and absorbing aerosols is proposed here. This can be used to derive simple aerosol models that are optically equivalent and can simulate the observed aerosol optical properties and radiative fluxes, from spectral optical depth measurements. Thus, aerosol single-scattering albedo and, hence, aerosol radiative forcing can be estimated. Note that the proposed method is to estimate clear-sky aerosol radiative forcing (over regions where chemical composition data or sky radiance data are not available) and not to infer its exact chemical composition. Using several independent datasets from field experiments, it is demonstrated that the proposed method can be used to estimate aerosol radiative forcing (from spectral optical depths) with an accuracy of ±2 W m−2.