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This study utilizes in situ measurements and numerical weather prediction forecasts curated during the Coupled Air–Sea Processes Electromagnetic Ducting Research (CASPER) east field campaign to assess how thermodynamic properties in the marine atmospheric surface layer influence evaporation duct shape independent of duct height. More specifically, we investigate evaporation duct shape through a duct shape parameter, a parameter known to affect the propagation of X-band radar signals and is directly related to the curvature of the duct. Relationships between this duct shape parameter and air sea temperature difference (ASTD) reveal that during unstable periods (ASTD < 0), the duct shape parameter is generally larger than in near-neutral or stable atmospheric conditions, indicating tighter curvature of the M-profile. Furthermore, for any specific duct height, a strong linear relationship between the near-surface-specific humidity gradient and the duct shape parameter is found, suggesting that it is primarily driven by near-surface humidity gradients. The results demonstrate that an a priori estimate of duct shape, for a given duct height, is possible if the near-surface humidity gradient is known.

The sea surface roughness parameterization and universal stability functions, as key components of the evaporation duct prediction models rooted in the Monin-Obukhov similarity theory, dictate the model performance which further impacts the efficiency and accuracy of offshore electromagnetic applications. In this paper, layered meteorological and hydrological observations are collected during two cruises and processed to obtain the reference modified refractivity profiles close to the sea surface, and then particle swarm algorithm is utilized to optimize the parameters of the sea surface roughness parameterization and universal stability functions. The results show that compared with the pre-optimization model, the prediction accuracy of the optimized model is improved by 5.09% and 8.12% under stable conditions, and by 9.97% and 31.51% under unstable conditions for observation dataset from each cruise, which proves the feasibility of the proposed method for evaporation duct prediction model optimization.

In South Asia, biomass is burned for energy and waste disposal, producing brown carbon (BrC) aerosols whose climatic impacts are highly uncertain. To assess these impacts, a real-world understanding of BrC's physio-optical properties is essential. For this region, the order-of-magnitude variability in BrC's spectral refractive index as a function of particle volatility distribution is poorly understood. This leads to oversimplified model parameterization and subsequent uncertainty in regional radiative forcing. Here we used the field-collected aerosol samples from major anthropogenic biomass activities to examine the methanol-soluble BrC optical properties. We show a strong relation between the absorption strength, wavelength dependence, and thermo-optical fractions of carbonaceous aerosols. Our observations show strongly absorbing BrC near the Himalayan foothills that may accelerate glacier melt, further highlighting the limitations of climate models where variable BrC properties are not considered. These findings provide crucial inputs for refining climate models and developing effective regional strategies to mitigate BrC emissions.

Coating enhancement of black carbon (BC) light absorption (Eabs) is a large uncertainty in modelling direct radiative forcing (DRF) by BC. Reported Eabs values after atmospheric aging vary widely and the mechanisms responsible for enhancing BC absorption remain elusive. Here, we report on the direct field measurement of size-resolved mixing state, Eabs, and aerosol single-scattering albedo (SSA) at λ = 532 nm at a rural site in east China from June to July 2016. Strong diurnal variability of Eabs, SSA, and Ox (Ox = NO2 + O3, a proxy for atmospheric photochemical aging) was observed. A method that combined Eabs and SSA was developed to retrieve the fraction contribution of BC absorption (fBC), lensing-driven enhancement (fLens), as well as the fractional contribution of coating absorption (fraction absorption contribution (fShell), the coated shell diameter (DShell) and the imaginary part of the complex refractive index (CRI) of the shell (kShell)). Parameterization of Eabs and SSA captures much of the influence of BC coating and the particle absorption. In our measurements at this site, the results showed that the absorption amplification depended on the coating thickness and the absorption of coating materials, and photochemistry plays a role in modifying the absorption of BC-containing particles. The lensing-driven enhancement was reduced by light absorption of the shell. One implication of these findings is that the contribution of light-absorbing organic compounds (brown carbon, BrC) at a longer aging time should be included in climate models.

The radiative forcing of black carbon (BC) is subject to many complex, interconnected sources of uncertainty. Here we isolate the role of the refractive index, which determines the extent to which BC absorbs and scatters radiation. We compare four refractive index schemes: three that are commonly used in Earth system models and a fourth more recent estimate with higher absorption. With other parameterizations held constant, changing BC's spectrally varying refractive index from the least- to most-absorbing estimate commonly used in Earth system models (m550 nm=1.75–0.44i to m550 nm=1.95–0.79i) increases simulated absorbing aerosol optical depth (AAOD) by 42 % and the effective radiative forcing from BC–radiation interactions (BC ERFari) by 47 %. The more recent estimate, m532 nm=1.48–0.84i, increases AAOD and BC ERFari by 59 % and 100 % respectively relative to the low-absorption case. The AAOD increases are comparable to those from recent updates to aerosol emission inventories and, in BC source regions, up to two-thirds as large as the difference in AAOD retrieved from MISR (Multi-angle Imaging SpectroRadiometer) and POLDER-GRASP (Polarization and Directionality of the Earth's Reflectances instrument with the Generalized Retrieval of Atmosphere and Surface Properties algorithm) satellites. The BC ERFari increases are comparable to previous assessments of overall uncertainties in BC ERFari, even though this source of uncertainty is typically overlooked. Although model sensitivity to the choice of BC refractive index is known to be modulated by other parameterization choices, our results highlight the importance of considering refractive index diversity in model intercomparison projects.

Most of the dust models underestimate the load of the large dust particles, consider spherical shapes instead of irregular ones, and have to deal with a wide range of the dust refractive index (RI) to be used. This leads to an incomplete assessment of the dust radiative effects and dust-related impacts on climate and weather. The current work aims to provide an assessment, through a sensitivity study, of the limitations of models to calculate the dust direct radiative effect (DRE) due to the underrepresentation of its size, RI, and shape. We show that the main limitations stem from the size and RI, while using a more realistic shape plays only a minor role, with our results agreeing with recent findings in the literature. At the top of the atmosphere (TOA) close to dust sources, the underestimation of size issues an underestimation of the direct warming effect of dust of ∼ 18–25 W m−2, for DOD = 1 (dust optical depth) at 0.5 µm, depending on the solar zenith angle (SZA) and RI. The underestimation of the dust size in models is less above the ocean than above dust sources, resulting in an underestimation of the direct cooling effect of dust above the ocean by up to 3 W m−2, for aerosol optical depth (AOD) of 1 at 0.5 µm. We also show that the RI of dust may change its DRE by 80 W m−2 above the dust sources and by 50 W m−2 at downwind oceanic areas for DOD = 1 at 0.5 µm at TOA. These results indicate the necessity of including more realistic sizes and RIs for dust particles in dust models, in order to derive better estimations of the dust DRE, especially near the dust sources and mostly for studies dealing with local radiation effects of dust aerosols.

This study investigates the evolution of temperature and lifetime of evaporating, supercooled cloud droplets considering initial droplet radius ( r 0 ) and temperature ( ), and environmental relative humidity (RH), temperature ( T ∞ ), and pressure ( P ). The time ( t ss ) required by droplets to reach a lower steady-state temperature ( T ss ) after sudden introduction into a new subsaturated environment, the magnitude of Δ T = T ∞ − T ss , and droplet survival time ( t st ) at T ss are calculated. The temperature difference (Δ T ) is found to increase with T ∞ , and decrease with RH and P . Δ T was typically 1–5 K lower than T ∞ , with highest values (∼10.3 K) for very low RH, low P , and T ∞ closer to 0°C. Results show that t ss is <0.5 s over the range of initial droplet and environmental conditions considered. Larger droplets ( r 0 = 30–50 μ m) can survive at T ss for about 5 s to over 10 min, depending on the subsaturation of the environment. For higher RH and larger droplets, droplet lifetimes can increase by more than 100 s compared to those with droplet cooling ignored. T ss of the evaporating droplets can be approximated by the environmental thermodynamic wet-bulb temperature. Radiation was found to play a minor role in influencing droplet temperatures, except for larger droplets in environments close to saturation. The implications for ice nucleation in cloud-top generating cells and near cloud edges are discussed. Using T ss instead of T ∞ in widely used parameterization schemes could lead to enhanced number concentrations of activated ice-nucleating particles (INPs), by a typical factor of 2–30, with the greatest increases (≥100) coincident with low RH, low P , and T ∞ closer to 0°C.

Biomass burning organic aerosol (BBOA) impacts significantly on climate directly through scattering and absorbing solar radiation and indirectly through acting as cloud condensation nuclei. However, fundamental parameters in the simulation of BBOA radiative effects and cloud activities such as size distribution and refractive index remain poorly parameterized in models. In this study, biomass burning events with high combustion efficiency characterized by a high black carbon (BC) to BBOA ratio (0.22 on average) were frequently observed during autumn in the Pearl River Delta region, China. An improved absorption Ångström exponent (AAE) ratio method considering both variations and spectral dependence of black carbon AAE was proposed to differentiate brown carbon (BrC) absorptions from total aerosol absorptions. BBOA size distributions, mass scattering and absorption efficiency were retrieved based on the changes in aerosol number size distribution, scattering coefficients and derived BrC absorptions that occurred with BBOA spikes. Geometric mean diameter of BBOA volume size distribution Dgv depended largely on combustion conditions, ranging from 245 to 505 nm, and a linear relationship between Dgv and ΔBC/ΔBBOA​​​​​​​ was achieved. The retrieved real part of the BBOA refractive index ranges from 1.47 to 1.64, with evidence showing that its variations might depend largely on combustion efficiency, which is rarely investigated in existing literature but which however requires further comprehensive investigations. Retrieved imaginary parts of BBOA refractive index (mi,BBOA) correlated highly with ΔBC/ΔBBOA (R>0.88) but differ a lot from previous parameterization schemes. The reason behind the inconsistency might be that single formula parameterizations of mi,BBOA over the whole BC/BBOA range were used in previous studies which might deviate substantially for specific BC/BBOA ranges. Thus, a new scheme that parameterizes wavelength-dependent mi,BBOA was presented, which filled the gap for field-based BBOA absorptivity parameterizations of ​​​​​​​BC/BBOA >0.1. These findings have significant implications for simulating BBOA climate effects and suggest that linking both BBOA refractive index and BBOA volume size distributions to BC content might be a feasible and a good choice for climate models.

Calculations of aerosol radiative forcing require knowledge of wavelength-dependent aerosol optical properties, such as single-scattering albedo. These aerosol optical properties can be calculated using Mie theory from knowledge of the key microphysical properties of particle size and refractive index, assuming that atmospheric particles are well-approximated to be spherical and homogeneous. We provide refractive index determinations for aqueous aerosol particles containing the key atmospherically relevant inorganic solutes of NaCl, NaNO3, (NH4)2SO4, NH4HSO4 and Na2SO4, reporting the refractive index variation with both wavelength (400–650 nm) and relative humidity (from 100 % to the efflorescence value of the salt). The accurate and precise retrieval of refractive index is performed using single-particle cavity ring-down spectroscopy. This approach involves probing a single aerosol particle confined in a Bessel laser beam optical trap through a combination of extinction measurements using cavity ring-down spectroscopy and elastic light-scattering measurements. Further, we assess the accuracy of these refractive index measurements, comparing our data with previously reported data sets from different measurement techniques but at a single wavelength. Finally, we provide a Cauchy dispersion model that parameterises refractive index measurements in terms of both wavelength and relative humidity. Our parameterisations should provide useful information to researchers requiring an accurate and comprehensive treatment of the wavelength and relative humidity dependence of refractive index for the inorganic component of atmospheric aerosol.

The spatiotemporal distribution and characterization of aerosol particles are usually determined by remote-sensing and optical in situ measurements. These measurements are indirect with respect to microphysical properties, and thus inversion techniques are required to determine the aerosol microphysics. Scattering theory provides the link between microphysical and optical properties; it is not only needed for such inversions but also for radiative budget calculations and climate modeling. However, optical modeling can be very time-consuming, in particular if nonspherical particles or complex ensembles are involved. In this paper we present the MOPSMAP package (Modeled optical properties of ensembles of aerosol particles), which is computationally fast for optical modeling even in the case of complex aerosols. The package consists of a data set of pre-calculated optical properties of single aerosol particles, a Fortran program to calculate the properties of user-defined aerosol ensembles, and a user-friendly web interface for online calculations. Spheres, spheroids, and a small set of irregular particle shapes are considered over a wide range of sizes and refractive indices. MOPSMAP provides the fundamental optical properties assuming random particle orientation, including the scattering matrix for the selected wavelengths. Moreover, the output includes tables of frequently used properties such as the single-scattering albedo, the asymmetry parameter, or the lidar ratio. To demonstrate the wide range of possible MOPSMAP applications, a selection of examples is presented, e.g., dealing with hygroscopic growth, mixtures of absorbing and non-absorbing particles, the relevance of the size equivalence in the case of nonspherical particles, and the variability in volcanic ash microphysics. The web interface is designed to be intuitive for expert and nonexpert users. To support users a large set of default settings is available, e.g., several wavelength-dependent refractive indices, climatologically representative size distributions, and a parameterization of hygroscopic growth. Calculations are possible for single wavelengths or user-defined sets (e.g., of specific remote-sensing application). For expert users more options for the microphysics are available. Plots for immediate visualization of the results are shown. The complete output can be downloaded for further applications. All input parameters and results are stored in the user's personal folder so that calculations can easily be reproduced. The web interface is provided at https://mopsmap.net (last access: 9 July 2018) and the Fortran program including the data set is freely available for offline calculations, e.g., when large numbers of different runs for sensitivity studies are to be made.