The aerosol scattering phase function (ASPF), a crucial element of aerosol optical properties, is pivotal for radiative forcing calculations and aerosol remote sensing detection. Current detection methods for the ASPF include multi-sensor detection, single-sensor rotational detection and imaging detection. However, these methods face challenges in achieving high-resolution full-angle measurement, particularly for small forward (i.e., less than 10 degrees) or backward (i.e., more than 170 degrees) scattering angles in open path. In this work, a full-angle ASPF detection system based on the multi-field-of-view Scheimpflug lidar technique has been proposed and demonstrated. A 450 nm continuous-wave semiconductor laser was utilized as the light source and four CMOS image sensors were employed as detectors. To detect the full-angle ASPF, four receiving units capture angular scattering signals across different angle ranges, namely 0 degrees-20 degrees, 10 degrees-96 degrees, 84 degrees-170 degrees, 160 degrees-180 degrees, respectively. The influence of the relative illumination and angular response of the used image sensors have been corrected, and a signal stitching algorithm was developed to obtain a complete 0-180 degrees angular scattering signal. Atmospheric measurements have been conducted by employing the full-angle ASPF detection system in open path. The experimental results of the ASPF have been compared with the AERONET data from the Socheongcho station and simulated ASPF based on the typical aerosol models in mainland China, showing excellent agreement. The promising results demonstrated in this work have shown a great potential for detecting the full-angle ASPF in open path.
This study analyzes the aerosol and precipitable water vapor (PWV) properties at six sites in the Indo-Gangetic Plains (IGP), a densely populated and highly polluted region. The main objective is to explore how the columnar PWV is related to the attenuation of shortwave solar radiation (SWR), as well as the combined role of aerosol properties and PWV on radiative forcing based on AERONET data and model (SBDART) simulations. The analysis revealed high aerosol optical depth (AOD) values (0.4-0.6) throughout the year in all the sites, associated with increased PWV (4-5 cm) during the summer monsoon. Comprehensive investigation shows that changes in PWV levels also affect aerosols' size distribution, optical properties and radiation balance in a similar way - but in different magnitudes - between the examined sites. The water vapor radiative effect (WVRE) is highly dependent on aerosol presence, with its magnitude for both surface (-130 to -140 Wm(-2)) and atmospheric forcing becoming higher under clean atmospheres (without aerosols). Aerosol presence is also considered in the computations of the WVRE. In that case, the WVRE becomes more pronounced at the top of the atmosphere (TOA) (30 to 35 Wm(-2)) but exhibits a lower forcing impact on the surface (about -45 Wm(-2)) and within the atmosphere (70-80 Wm(-2)), suggesting important aerosol-PWV interrelations. The atmospheric heating rate due to PWV is more than double (3.5-4.5 K Day(-1)) that of aerosols (1-1.9 K Day(-1)), highlighting its essential role in radiative effects and climate implications over the IGP region. The radiative impacts of PWV and aerosols are further examined as a function of the single scattering albedo, solar zenith angle, and absorbing AOD at the different sites, revealing dependence on both astronomical and atmospheric variables related to aerosol absorption, thus unravelling the combined role of aerosols and PWV in climate implications.
Characterizing vertical profiles of in-situ particle properties is relevant because being only based on the surface or column-integrated measurements cannot unambiguously conclude the radiative impact on aerosol. Vertical profiles of in-situ aerosol properties on-board an unmanned aerial vehicle (UAV) were measured above El Arenosillo (37.1 N,-6.7 W) in the southwest of Spain during four flight missions. Measured properties included particle number size distribution, total particle concentration and multiwavelength absorption coefficient up to 3100 m during cold season (February 4, 2022 and December 11, 2023) and warm season (September 20, 2023 and April 2, 2024). The heterogeneity of particle properties has been shown around two types of events: a mineral particle event of desert origin during cold season and a new particle formation event during warm season. During cold season, a comparison between the flight missions with and without desert dust episodes shows that mineral particles decrease the planetary boundary layer (PBL) height. This behavior is probably related to absorber particles aloft atmosphere, which traps solar radiation and heat up the upper layer of the atmosphere and deteriorates the vertical dispersion. In the literature, this effect is called as 'dome effect'. During warm season, new particle formation was observed above PBL. This event could be related to the presence of precursor gases in the residual layer, and enhanced by a low concentration of pre-existing particles. The characteristic parameter during the observed event was the fine-to-total particle volume concentration ratio close to zero. These observations highlight the necessity to establish a long-term multi-temporal monitoring of vertical profiles for atmospheric parameters onboard UAV systems and to integrate in Earth observations networks. For example, radiative forcing is usually estimated from surface data, but the heterogeneity in the vertical profiles of atmospheric particles properties, which are used to the forcing quantification, is a result of inaccuracies.
Carbonaceous aerosols play a crucial role in air pollution and radiative forcing, though their light-absorbing and isotopic characteristics remain insufficiently understood. This study analyzes optical absorption and isotopic composition in PM10 and PM2.5 particles from primary emission sources, focusing on traffic-related and solid fuel categories. We analyzed key optical properties, including the Angstrom absorption exponent (AAE), the contributions of black carbon (BC) and brown carbon (BrC) to total light absorption and the mass absorption efficiencies (MAE) of carbonaceous aerosols. AAE values were lower for traffic emission sources (0.9 to 1.3) than solid fuel emission sources (1.5 to 3), with similar values for both particle sizes. BrC contributions were more prominent at shorter wavelengths and were notably higher in solid fuel emission sources (61% to 88%) than in traffic emission sources (8% to 40%) at 405 nm. MAE values of BC at 405 nm were 2 to 20 times higher than BrC across different emissions. Particle size significantly affect MAE(BC) with PM2.5 higher when compared to PM10. Emissions from diesel concentrate mixer and raw coal burning exhibited the highest MAE(BC) for PM2.5 and PM10, respectively. Conversely, Coke had the lowest MAE(BC) but the highest MAE(BrC) for both sizes. Traffic emissions showed more stable carbon isotope ratios (delta C-13) enrichment (-29 parts per thousand to -24 parts per thousand) than solid fuels (-31 parts per thousand to -20 parts per thousand). delta C-13 of solid fuel combustion, unlike traffic sources, is found to be independent of size variation. These findings underscore the importance of source and size-specific aerosol characterization for unregulated emission sources.
Atmospheric brown carbon (BrC) from wildfires is a key component of light-absorbing carbon that significantly contributes to global radiative forcing, but its atmospheric evolution and lifetime remain poorly understood. In this study, we investigate BrC evolution by synthesizing data from one laboratory campaign and four aircraft campaigns spanning diverse spatial scales across North America. To estimate initial conditions for evaluating plume evolution, we develop a method to parametrize the emission ratios of BrC and other species using commonly measured inert tracers, acetonitrile and hydrogen cyanide. The evolution of BrC absorption in the free troposphere is characterized as a function of hydroxyl radical (OH) exposure, yielding an effective photochemical rate constant of 9.7-1.6 +4.8 x 10-12 cm3 molecule-1 s-1. The relatively slow reaction rate results in small BrC decay within the first few hours after emission, making it difficult to distinguish from source variability. This helps explain the absence of clear evolutionary trends in near-field studies. Assuming an OH concentration of 1.26 x 106 molecules cm-3, this rate constant corresponds to an e-folding lifetime of approximately 23 h. After extensive photooxidation (OH exposure similar to 1012 molecules cm-3 s), 4 +/- 2% of the emitted BrC persists, representing a recalcitrant fraction with potential long-term climate impacts. These results improve our understanding of BrC variability and photochemical processing and provide critical constraints for modeling its impacts on climate.
This study investigates the effects of aerosol-radiation interactions on subseasonal prediction using the Unified Forecast System, which includes atmosphere, ocean, sea ice, and wave components, coupled with an aerosol module. The aerosol module is from the current NOAA operational GEFSv12-Aerosols model, which is based on the WRF-Chem GOCART with updates to the dust scheme and the biomass burning plume rise module. It simulates five aerosol species: sulfate, dust, black carbon, organic carbon, and sea salt. The modeled aerosol optical depth (AOD) is compared to MERRA-2 reanalysis, MODIS satellite retrievals, and ATom aircraft measurements. Despite biases primarily in dust and sea salt, the AOD shows good agreement globally. The simulated radiative forcing (RF) at the top of the atmosphere (TOA) from the total aerosols is approximately -2.6 W/m2 or -16 W/m2 per unit AOD globally. In subsequent simulations, the prognostic aerosol module is replaced with climatological aerosol concentrations derived from the preceding experiments. While regional differences in RF at TOA between these two experiments are noticeable in specific events, the multi-year subseasonal simulations reveal consistent patterns in RF at TOA, surface temperature, geopotential height at 500 hPa, and precipitation. These results suggest that given the current capacities of aerosol modeling, adopting a climatology of aerosol concentrations as a cost-effective alternative to a complex aerosol module may be a practical approach for subseasonal applications.
Aerosol absorption and scattering notably influence the atmospheric radiative balance. Significant uncertainties persist regarding the impact of aerosol models on aerosol radiative forcing (ARF) under distinct atmospheric conditions. The effects of various aerosol models on ARF under clear and haze conditions are analyzed utilizing MODIS data, combined with observations from Beijing, and the 6S (Second Simulation of the Satellite Signal in the Solar Spectrum) for simulations. Results showed that ARF at the surface (ARF-SFC) and top of the atmosphere (ARF-TOA) registered negative values on clear and hazy days. On hazy days, the desert model demonstrated enhanced cooling at TOA, while the urban model showed intensified surface cooling. Hazy conditions amplified ARF-TOA by 57%, 54%, and 61% for desert, urban, and continental models respectively, relative to clear days, with corresponding ARF-SFC increases of 57%, 54%, and 56%. Aerosol radiative forcing efficiency at TOA generally exhibited greater values in winter than in summer. Black carbon (BC) radiative forcing simulations using the three-component method showed positive values at TOA and negative values at the surface. During hazy days, BC intensified upper-atmosphere heating and surface cooling effects. This research will lay the scientific foundation for reducing uncertainty in ARF estimates and developing effective environmental strategies.
Altitude profiles of the mass concentrations of aerosol black carbon (BC) have been obtained,up to an altitude of 12 km, from in situ measurements over Hyderabad (17.47 degrees N, 78.57 degrees E, 557 m amsl;a tropical station in the central Indian peninsula), using three successive high altitude balloon ascents during winter and early summer seasons of 2023-2024. The profiles revealed predominant peaks at around 8 and 11 km, where the BC concentrations were reaching as high as nearly three times the surface concentrations (2.82, 2.76, and 2.60 mu g m-3, respectively), persistently in all the three flights. Detailed analyses using official data of air traffic movement, aviation statistics and emission inventory revealed a strong linkage with the emissions from commercial aircraft that touch Hyderabad and overfly the region. These elevated BC layers will have large implications to atmospheric radiative forcing and possible contributions to modification of the cirrus cloud properties.
Aerosol optical properties and radiative forcing critically influence Earth's climate, particularly in semi-arid regions. This study investigates these properties in Yinchuan, Northwest China, focusing on aerosol optical depth (AOD), single-scattering albedo (SSA), & Aring;ngstr & ouml;m Index, and direct radiative forcing (DRF) using 2023 CE-318 sun photometer data, HYSPLIT trajectory analysis, and the SBDART model. Spring AOD peaks at 0.58 +/- 0.15 (500 nm) due to desert dust, with coarse-mode particles dominating, while summer SSA reaches 0.94, driven by fine-mode aerosols. Internal mixing of dust and anthropogenic aerosols significantly alters DRF through enhanced absorption, with spring surface DRF at -101 +/- 22W m-2 indicating strong cooling and internal mixing increasing atmospheric DRF to 52.25W m-2. These findings elucidate dust-anthropogenic interactions' impact on optical properties and radiative forcing, offering critical observations for semi-arid climate research.
Air pollution is a global health issue, and events like forest fires, agricultural burning, dust storms, and fireworks can significantly worsen it. Festivals involving fireworks and wood-log fires, such as Diwali and Holi, are key examples of events that impact local air quality. During Holi, the ritual of Holika involves burning of biomass that releases large amounts of aerosols and other pollutants. To assess the impact of Holika burning, observations were conducted from March 5th to March 18th, 2017. On March 12th, 2017, around 1.8 million kg of wood and biomass were openly burned in about 2250 units of Holika, located in and around the Varanasi city (25.23 N, 82.97 E, similar to 82.20 m amsl). As the Holika burning event began the impact on the Black Carbon (BC), particulate matter 10 & 2.5 (PM10 and PM2.5), sulphur dioxide (SO2), oxides of nitrogen (NOx), ozone (O-3) and carbon monoxide (CO) concentration were observed. Thorough optical investigations have been conducted to better comprehend the radiative effects of aerosols produced due to Holika burning on the environment. The measured AOD at 500 nm values were 0.315 +/- 0.072, 0.392, and 0.329 +/- 0.037, while the BC mass was 7.09 +/- 1.78, 9.95, and 7.18 +/- 0.27 mu g/m(3) for the pre-Holika, Holika, and post-Holika periods. Aerosol radiative forcing at the top of the atmosphere (ARF-TOA), at the surface (ARF-SUR), and in the atmosphere (ARF-ATM) are 2.46 +/- 4.15, -40.22 +/- 2.35, and 42.68 +/- 4.12 W/m(2) for pre-Holika, 6.34, -53.45, and 59.80 W/m(2) for Holika, and 5.50 +/- 0.97, -47.11 +/- 5.20, and 52.61 +/- 6.17 W/m(2) for post-Holika burning. These intense observation and analysis revealed that Holika burning adversely impacts AQI, BC concentration and effects climate in terms of ARF and heating rate.