Embedded information of aerosol type, hygroscopicity and scattering enhancement factor revealed by the relationship between PM2.5 and aerosol optical depth.

Satellite aerosol optical depth (AOD) provides an alternative way to depict the spatial distribution of near-surface PM2.5. In this study, a mathematical formulation of how PM2.5 is related to AOD is presented. When simplified to a linear equation, a functional dependence of the slope on the aerosol type, scattering enhancement factor f(RH), and boundary layer height is revealed, while the influence of the vertical aerosol profile is embedded in the intercept. Specifically, we focus on the effects of aerosol properties and employ a new aerosol index (Normalized Gradient Aerosol Index, NGAI) for classifying aerosol subtypes. The combination of AOD difference at shorter wavelengths over longer-wavelength AOD from AERONET data could distinguish and subclassify aerosol types previously indistinguishable by AE (i.e., urban-industrial pollution, U/I, and biomass burning, BB). AOD-PM2.5 regressions are performed on these aerosol subtypes at various relative humidity (RH) levels. The results suggest that BB aerosols are nearly hydrophobic until the RH exceeds 80 %, while the AOD-PM2.5 regressions for U/I depend on RH levels. Moreover, the scattering enhancement factor f(RH) can be calculated by taking the ratio of intercepts between dry and humidity conditions, which is proposed and tested for the first time in this study. Our results show an f(RH ≥ 80 %) of ∼2.6 for U/I-dominated aerosols, whereas the value is not over 1.5 for BB aerosols. The f(RH) can be further used to derive the optical hygroscopicity parameter (κsca), demonstrating that the NGAI can be used to exploit differences in aerosol hygroscopicity and improve the AOD-PM2.5 relationship.

Sources, transport, and visibility impact of ambient submicrometer particle number size distributions in an urban area of central Taiwan.

This study applied positive matrix factorization (PMF) to identify the sources of size-resolved submicrometer (10-1000 nm) particles and quantify their contributions to impaired visibility based on the particle number size distributions (PNSDs), aerosol light extinction (bp), air pollutants (PM10, PM2.5, SO2, O3, and NO), and meteorological parameters (temperature, relative humidity, wind speed, wind direction, and ultraviolet index) measured hourly over an urban basin in central Taiwan between 2017 and 2021. The transport of source-specific PNSDs was evaluated with wind and back trajectory analyses. The PMF revealed six sources to the total particle number (TPN), surface (TPS), volume (TPV), and bp. Factor 1 (F1), the key contributor to TPN (35.0 %), represented nucleation (<25 nm) particles associated with fresh traffic emission and secondary new particle formation, which were transported from the west-southwest by stronger winds (>2.2 m s-1). F2 represented the large Aitken (50-100 nm) particles transported regionally via northerly winds, whereas F3 represented large accumulation (300-1000 nm) particles, which showed elevated concentrations under stagnant conditions (<1.1 m s-1). F4 represented small Aitken (25-50 nm) particles arising from the growth and transport of the nucleation particles (F1) via west-southwesterly winds. F5 represented large Aitken particles originating from combustion-related SO2 sources and carried by west-northwesterly winds. F6 represented small accumulation (100-300 nm) particles emitted both by local sources and by the remote SO2 sources found for F5. Overall, large accumulation particles (F3) played the greatest role in determining the TPV (66.4 %) and TPS (34.8 %), and their contribution to bp increased markedly from 17.3 % to 40.7 % as visibility decreased, indicating that TPV and TPS are better metrics than TPN for estimating bp. Furthermore, slow-moving air masses-and therefore stagnant conditions-facilitate the build-up of accumulation mode particles (F3 + F6), resulting in the poorest visibility.

Secondary inorganic aerosol chemistry and its impact on atmospheric visibility over an ammonia-rich urban area in Central Taiwan.

This study investigated the hourly inorganic aerosol chemistry and its impact on atmospheric visibility over an urban area in Central Taiwan, by relying on measurements of aerosol light extinction, inorganic gases, and PM2.5 water-soluble ions (WSIs), and simulations from a thermodynamic equilibrium model. On average, the sulfate (SO42-), nitrate (NO3-), and ammonium (NH4+) components (SNA) contributed ∼90% of WSI concentrations, which in turn made up about 50% of the PM2.5 mass. During the entire observation period, PM2.5 and SNA concentrations, aerosol pH, aerosol liquid water content (ALWC), and sulfur and nitrogen conversion ratios all increased with decreasing visibility. In particular, the NO3- contribution to PM2.5 increased, whereas the SO42- contribution decreased, with decreasing visibility. The diurnal variations of the above parameters indicate that the interaction and likely mutual promotion between NO3- and ALWC enhanced the hygroscopicity and aqueous-phase reactions conducive for NO3- formation, thus led to severely impaired visibility. The high relative humidity (RH) at the study area (average 70.7%) was a necessary but not sole factor leading to enhanced NO3- formation, which was more directly associated with elevated ALWC and aerosol pH. Simulations from the thermodynamic model depict that the inorganic aerosol system in the study area was characterized by fully neutralized SO42- (i.e. a saturated factor in visibility reduction) and excess NH4+ amidst a NH3-rich environment. As a result, PM2.5 composition was most sensitive to gas-phase HNO3, and hence NOx, and relatively insensitive to NH3. Consequently, a reduction of NOx would result in instantaneous cuts of NO3-, PM2.5, and ALWC, and hence improved visibility. On the other hand, a substantial amount of NH3 reduction (>70%) would be required to lower the aerosol pH, driving more than 50% of the particulate phase NO3- to the gas phase, thereby making NH3 a limiting factor in shifting PM2.5 composition.

Quantifying the impacts of PM2.5 constituents and relative humidity on visibility impairment in a suburban area of eastern Asia using long-term in-situ measurements.

The deterioration of visibility due to air pollutants and relative humidity has been a serious environmental problem in eastern Asia. In most previous studies, chemical compositions of atmospheric particles were provided using filter-based offline analyses, which were unable to provide long-term and in-situ measurements that resolve sufficient temporal variations of air pollution and meteorology, hindering the resolution of the relationship between air quality and visibility. Here, we present a year-long continuously measured data from a comprehensive suite of online instruments to investigate diurnal and seasonal impacts of the aerosol chemical compositions in PM2.5 on visibility seasonally and diurnally. The measured dry aerosol extinction at λ = 550 nm reached a closure with that predicted by aerosol compositions within 12%. However, the hygroscopic growth of particles under ambient RH could enhance the aerosol extinction by a factor of 2-6, matching the perceptive visibility of the public. Particulate ammonium nitrate was most sensitive to reducing visibility, while ammonium sulfate contributed the most to the light extinction. In spring and winter, the monsoon and stagnant air masses reduced the visibility and increased PM2.5 (>35 µg m-3). The moisture was found to substantially enhance the light extinction under RH = 60-90%, reducing visibility by approximately 15 km, largely attributed to hygroscopic inorganic salts. This study serves as a metric to highlight the need to consider the influence of RH, and aqueous reactions in producing secondary inorganic aerosols on atmospheric visibility, underpinning the more accurate mitigation strategies of air pollution.

Evaluating the Height of Biomass Burning Smoke Aerosols Retrieved from Synergistic Use of Multiple Satellite Sensors over Southeast Asia.

This study evaluates the height of biomass burning smoke aerosols retrieved from a combined use of Visible Infrared Imaging Radiometer Suite (VIIRS), Ozone Mapping and Profiler Suite (OMPS), and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) observations. The retrieved heights are compared against spaceborne and ground-based lidar measurements during the peak biomass burning season (March and April) over Southeast Asia from 2013 to 2015. Based on the comparison against CALIOP, a quality assurance (QA) procedure is developed. It is found that 74% (81-84%) of the retrieved heights fall within 1 km of CALIOP observations for unfiltered (QA-filtered) data, with root-mean-square error (RMSE) of 1.1 km (0.8-1.0 km). Eliminating the requirement for CALIOP observations from the retrieval process significantly increases the temporal coverage with only a slight decrease in the retrieval accuracy; for best QA data, 64% of data fall within 1 km of CALIOP observations with RMSE of 1.1 km. When compared with Micro-Pulse Lidar Network (MPLNET) measurements deployed at Doi Ang Khang, Thailand, the retrieved heights show RMSE of 1.7 km (1.1 km) for unfiltered (QA-filtered) data for the complete algorithm, and 0.9 km (0.8 km) for the simplified algorithm.

Interactions between biomass-burning aerosols and clouds over Southeast Asia: current status, challenges, and perspectives.

The interactions between aerosols, clouds, and precipitation remain among the largest sources of uncertainty in the Earth's energy budget. Biomass-burning aerosols are a key feature of the global aerosol system, with significant annually-repeating fires in several parts of the world, including Southeast Asia (SEA). SEA in particular provides a "natural laboratory" for these studies, as smoke travels from source regions downwind in which it is coupled to persistent stratocumulus decks. However, SEA has been under-exploited for these studies. This review summarizes previous related field campaigns in SEA, with a focus on the ongoing Seven South East Asian Studies (7-SEAS) and results from the most recent BASELInE deployment. Progress from remote sensing and modeling studies, along with the challenges faced for these studies, are also discussed. We suggest that improvements to our knowledge of these aerosol/cloud effects require the synergistic use of field measurements with remote sensing and modeling tools.

Assessment of the Moderate-Resolution Imaging Spectroradiometer algorithm for retrieval of aerosol parameters over the ocean.

The Moderate Resolution Imaging Spectroradiometer aerosol algorithm over the ocean derives spectral aerosol optical depth and aerosol size parameters from satellite measured radiances at the top of the atmosphere (TOA). It is based on the adding of apparent optical properties (AOPs): TOA reflectance is approximated as a linear combination of reflectances resulting from a small particle mode and a large particle mode. The weighting parameter eta is defined as the fraction of the optical depth at 550 nm due to the small mode. The AOP approach is correct only in the single scattering limit. For a physically correct TOA reflectance simulation, we create linear combinations of the inherent optical properties (IOPs) of small and large particle modes, in which the weighting parameter f is defined as the fraction of the number density attributed to the small particle mode. We use these IOPs as inputs to an accurate multiple scattering radiative transfer model. We find that reflectance errors incurred with the AOP method are as high as 30% for an aerosol optical depth of 2 at 550 nm. The retrieved optical depth has a relative error of up to 8%, and the retrieved fraction eta has an absolute error of approximately 6%. We show that the use of accurate radiative transfer simulations and a bimodal fraction f yields accurate values for the retrieved optical depth and the fraction f.

Geometrical-optics solution to light scattering by droxtal ice crystals.

We investigate the phase matrices of droxtals at wavelengths of 0.66 and 11 microm by using an improved geometrical-optics method. An efficient method is developed to specify the incident rays and the corresponding impinging points on the particle surface necessary to initialize the ray-tracing computations. At the 0.66-microm wavelength, the optical properties of droxtals are different from those of hexagonal ice crystals. At the 11-microm wavelength, the phase functions for droxtals are essentially featureless because of strong absorption within the particles, except for ripple structures that are caused by the phase interference of the diffracted wave.

Surface aerosol radiative forcing derived from collocated ground-based radiometric observations during PRIDE, SAFARI, and ACE-Asia.

An approach is presented to estimate the surface aerosol radiative forcing by use of collocated cloud-screened narrowband spectral and thermal-offset-corrected radiometric observations during the Puerto Rico Dust Experiment 2000, South African Fire Atmosphere Research Initiative (SAFARI) 2000, and Aerosol Characterization Experiment-Asia 2001. We show that aerosol optical depths from the Multiple-Filter Rotating Shadowband Radiometer data match closely with those from the Cimel sunphotometer data for two SAFARI-2000 dates. The observed aerosol radiative forcings were interpreted on the basis of results from the Fu-Liou radiative transfer model, and, in some cases, cross checked with satellite-derived forcing parameters. Values of the aerosol radiative forcing and forcing efficiency, which quantifies the sensitivity of the surface fluxes to the aerosol optical depth, were generated on the basis of a differential technique for all three campaigns, and their scientific significance is discussed.

Inherent and apparent scattering properties of coated or uncoated spheres embedded in an absorbing host medium.

The conventional Lorenz-Mie formalism is extended to the case for a coated sphere embedded in an absorbing medium. The apparent and inherent scattering cross sections of a particle, derived from the far field and near field, respectively, are different if the host medium is absorptive. The effect of absorption within the host medium on the phase-matrix elements associated with polarization depends on the dielectric properties of the scattering particle. For the specific cases of a soot particle coated with a water layer and an ice sphere containing an air bubble, the phase-matrix elements -P12/P11 and P33/P11 are unique if the shell is thin. The radiative transfer equation for a multidisperse particle system embedded within an absorbing medium is discussed. Conventional multiple-scattering computational algorithms can be applied if scaled apparent single-scattering properties are applied.

Piffalls in atmospheric correction of ocean color imagery: how should aerosol optical properties be computed?

Current methods for the atmospheric correction of ocean-color imagery rely on the computation of optical properties of a mixture of chemically different aerosol particles through combination of the mixture with it into an effective, single-particle component that has an average refractive index. However, a multi-component approach in which each particle type independently grows and changes its refractive index with increasing humidity is more realistic. Computations based on Mie theory and radiative transfer are used to show that the two approaches result in top-of-the-atmosphere radiances that differ more than the water-leaving radiance. Thus, proper atmospheric correction requires a multicomponent approach for the computation of realistic aerosol optical properties.