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Efficient and accurate computation of the single‐scattering properties of black carbon (BC) aerosols is fundamental in various fields, including remote sensing and climate simulations. In this study, we developed a composite model of fractal aggregates of BC encapsulated with hygroscopic aerosols to represent the ambient BC. We used the invariant imbedding T‐matrix method to compute the optical properties of fully and partially encapsulated BC aerosols. In this new model, the traditional assumption of unoverlapped surfaces in the super‐position T‐matrix method is unnecessary. After extensive simulations, we established a database of single‐scattering properties, including the extinction efficiency, the single‐scattering albedo, the asymmetry factor and six phase matrix elements. Moreover, we obtained deep neural networks (DNNs) from this database using a deep learning method. These DNN models provide a universal interface for predicting the optical properties of ambient BC aerosols. Specifically, through a modified architecture of the DNN, we trained two models based on the database to predict three integrated optical properties (extinction efficiency, single‐scattering albedo, and asymmetry factor) and six phase matrix elements. We performed statistical assessments based on the true values in the database and the predicted values from the DNNs, demonstrating that the DNNs accurately predicted all single‐scattering properties. Therefore, the developed DNN models can be conveniently implemented in aerosol optical parameterization for remote sensing studies and atmospheric models. Plain Language Summary: Black carbon (BC) aerosol plays a significant role in the atmosphere, influencing climate through its interactions with radiation, such as scattering and absorbing. The accurate determination of the single‐scattering properties of BC, including the extinction efficiency, the single‐scattering albedo, the asymmetry factor and six phase matrix elements, is crucial for understanding its radiation effects. In this study, we developed a comprehensive model for BC particles that incorporates complex morphological characteristics and the mixing of BC with other hygroscopic aerosols. We established a database of single‐scattering properties for these models using the invariant imbedding T‐matrix method. However, the large storage space required by this database (over 20 GB) makes it impractical for widespread applications. Therefore, we employed a deep learning method to compress the storage consumption. Two deep neural networks (DNNs) were trained using the database, enabling the prediction of all single‐scattering properties. Remarkably, the performance of the DNNs was excellent, with a coefficient of determination greater than 0.99 for all single‐scattering properties, as determined through statistical assessment. These DNN models hold great potential for various atmospheric radiation and remote sensing studies in the future. Key Points: A flexible model of partially and fully encapsulated fractal black carbon particles was developedA database of single‐scattering properties of encapsulated fractal black carbon particles was constructedTwo deep neural networks were obtained, offering a flexible approach to calculating the optical properties of black carbon aerosols [ABSTRACT FROM AUTHOR]

Sea salt aerosols were assumed to be homogeneous spheres in most climate models. However, observations show that sea salt particles are inhomogeneous during the deliquesce and crystallization processes. Using a two‐layer sphere model, we found that backscattering of solar radiation associated with sea salts is underestimated in homogeneous sea salt models. The Community Earth System Model is used to assess the inhomogeneity effect on direct radiative forcing. For global climate model simulation, the inhomogeneity effect on radiative transfer is found to be small as high RHs over widespread oceans suppress the impact of inhomogeneity. On the other hand, in coastal regions, the inhomogeneity effect can cause up to 10% radiative forcing difference of sea salt aerosols. The inhomogeneity effect of sea salt aerosols has to be considered over coastal regions, especially in the Mediterranean, Australia, and the eastern coast of South America. Plain Language Summary: In a humid environment, solid sea salt particles can be coated with water. Sea salt aerosol has a cooling effect on the Earth, but coated sea salt has even stronger cooling effect. However, in most climate models, coated sea salt is not considered. This study confirms that coated sea salt aerosols may not significantly affect the global radiation budget, but they should definitely be considered in the coastal climate where large changes in relative humidity are evident. Key Points: For some range of relative humidity (50‐80%), sea salt is assumed to be an inhomogeneous two‐layer sphereThe inhomogeneity of sea salt decreases the asymmetry factor and increases backscattering of solar radiationInhomogeneity has a relatively large impact (up to 10%) on sea salt radiative forcing over coastal waters [ABSTRACT FROM AUTHOR]

Abstract: The nonsphericity and inhomogeneity of marine aerosols (sea salts) have not been addressed in pertinent radiative transfer calculations and remote sensing studies. This study investigates the optical properties of nonspherical and inhomogeneous sea salts using invariant imbedding T‐matrix simulations. Dry sea salt aerosols are modeled based on superellipsoidal geometries with a prescribed aspect ratio and roundness parameter. Wet sea salt particles are modeled as coated superellipsoids, as spherical particles with a superellipsoidal core, and as homogeneous spheres depending on the level of relative humidity. Aspect ratio and roundness parameters are found to be critical to interpreting the linear depolarization ratios (LDRs) of NaCl crystals from laboratory measurements. The optimal morphology parameters of NaCl necessary to reproduce the measurements are found to be consistent with data gleaned from an electron micrograph. The LDRs of wet sea salts are computed based on inhomogeneous models and compared with the measured data from ground‐based LiDAR. The dependence of the LDR on relative humidity is explicitly considered. The increase in the LDR with relative humidity at the initial phase of deliquescence is attributed to both the size increase and the inhomogeneity effect. For large humidity values, the LDR substantially decreases because the overall particle shape becomes more spherical and the inhomogeneity effect in a particle on the LDR is suppressed for submicron sea salts. However, the effect of inhomogeneity on optical properties is pronounced for coarse‐mode sea salts. These findings have important implications for atmospheric radiative transfer and remote sensing involving sea salt aerosols. [ABSTRACT FROM AUTHOR]