A new method to retrieve the real part of the equivalent refractive index of atmospheric aerosols

This document is the Accepted Manuscript version of the following article: S. Vratolis, et al, ‘A new method to retrieve the real part of the equivalent refractive index of atmospheric aerosols’, Journal of Aerosol Science, Vol. 117: 54-62, March 2018. Under embargo until 29 December 2019. The final, published version is available online at DOI: https://doi.org/10.1016/j.jaerosci.2017.12.013.In the context of the international experimental campaign Hygroscopic Aerosols to Cloud Droplets (HygrA-CD, 15 May to 22 June 2014), dry aerosol size distributions were measured at Demokritos station (DEM) using a Scanning Mobility Particle Sizer (SMPS) in the size range from 10 to 550 nm (electrical mobility diameter), and an Optical Particle Counter (OPC model Grimm 107 operating at the laser wavelength of 660 nm) to acquire the particle size distribution in the size range of 250 nm to 2.5 μm optical diameter. This work describes a method that was developed to align size distributions in the overlapping range of the SMPS and the OPC, thus allowing us to retrieve the real part of the aerosol equivalent refractive index (ERI). The objective is to show that size distribution data acquired at in situ measurement stations can provide an insight to the physical and chemical properties of aerosol particles, leading to better understanding of aerosol impact on human health and earth radiative balance. The resulting ERI could be used in radiative transfer models to assess aerosol forcing direct effect, as well as an index of aerosol chemical composition. To validate the method, a series of calibration experiments were performed using compounds with known refractive index (RI). This led to a corrected version of the ERI values, (ERICOR). The ERICOR values were subsequently compared to model estimates of RI values, based on measured PM2.5 chemical composition, and to aerosol RI retrieved values by inverted lidar measurements on selected days.Peer reviewe

Initial investigation of the wavelength dependence of optical properties measured with a new multi-pass Aerosol Extinction Differential Optical Absorption Spectrometer (AE-DOAS)

Atmospheric aerosols directly affect climate by scattering and absorbing radiation. The magnitude of the impact is dependent upon the wavelength of light, but is often estimated near 550 nm. When light scattering and absorption by aerosols is approximated, the wavelength dependence of the refractive index for specific components is lost. As a result, climate models would have inherent uncertainties for aerosol contributions to radiative forcing when considering the entire solar spectrum. An aerosol extinction differential optical absorption spectrometer has been developed to directly measure aerosol extinction at mid-ultraviolet to near infrared wavelengths. The instrument consists of a spectrometer coupled to a closed White-type multi-pass gas cell with an adjustable path length of up to approximately 20 m. Laboratory measurements of various gases are compared with known absorption cross sections. Additionally, the extinction of monodisperse samples of polystyrene latex spheres are measured and compared to Mie theory generated with refractive index values from the literature to validate the new instrument. The polystyrene experiments also emphasize the ability of the new instrument to retrieve the wavelength dependent refractive index, especially in the ultraviolet wavelength regions where variability is expected. The spectrometer will be a significant advancement for determining wavelength dependent complex refractive indices in future laboratory studies as well as provide the ability to monitor ambient aerosol light extinction

Stratospheric aerosols

The current state of information on stratospheric aerosols is reviewed. Aerosol properties such as size, size distribution, composition, refractive index, number density, extinction, optical depth, and single scattering albedo are considered and generalized as much as possible to be representative of the global aerosol in times of volcanic and nonvolcanic (background) periods. Data are presented that show the global distribution of stratospheric aerosols as measured by the stratospheric aerosol and gas experiment (SAGE) satellite system for background and volcanic (post-Mount St. Helens) conditions. In addition, lidar and dustsonde data are presented that show the changes in stratospheric aerosol over an 8-year period

Retrievals of Antarctic aerosol characteristics using a Sun-sky radiometer during the 2001-2002 austral summer campaign

In order to characterize the Antarctic aerosol and to analyze the effect of katabatic winds on the properties of suspended particles, measurements of solar direct and diffuse irradiance were carried out at the Italian Terra Nova Bay station in Antarctica, during the 2001-2002 austral summer campaign. Measurements were performed by the ground-based PREDE sky radiometer and processed by using the Skyrad inversion code. Aerosol optical thickness at 500 nm was found to vary between 0.01 and 0.02. The volume size distribution curves showed bimodal features with the two modes located within 0.1-0.3 μm and 5-7 μm radius intervals, respectively. The real part of the refractive index characterizing the Antarctic aerosol was found to have a mean value of 1.40. During the katabatic event the analysis indicated that the advection of larger and drier fresh particles, together with the removal of marine suspended particles, caused the decrease in aerosol optical thickness

Aircraft vortex marking program

A simple, reliable device for identifying atmospheric vortices, principally as generated by in-flight aircraft and with emphasis on the use of nonpolluting aerosols for marking by injection into such vortex (-ices) is presented. The refractive index and droplet size were determined from an analysis of aerosol optical and transport properties as the most significant parameters in effecting vortex optimum light scattering (for visual sighting) and visual persistency of at least 300 sec. The analysis also showed that a steam-ejected tetraethylene glycol aerosol with droplet size near 1 micron and refractive index of approximately 1.45 could be a promising candidate for vortex marking. A marking aerosol was successfully generated with the steam-tetraethylene glycol mixture from breadboard system hardware. A compact 25 lb/f thrust (nominal) H2O2 rocket chamber was the key component of the system which produced the required steam by catalytic decomposition of the supplied H2O2

Bacterial atmospheric contamination during routine dental activity

Routine dental procedures cause atmospheric bacterial contamination in the dental clinic and laboratory. This environmental hazard, quantified by the Air Microbial Index, was shown in our study to be directly related to aerosol creating instruments and ventilation.peer-reviewe

Aerosol physical properties in the stratosphere (APPS) radiometer design

The measurement concepts and radiometer design developed to obtain earth-limb spectral radiance measurements for the Aerosol Physical Properties in the Stratosphere (APPS) measurement program are presented. The measurements made by a radiometer of this design can be inverted to yield vertical profiles of Rayleigh scatterers, ozone, nitrogen dioxide, aerosol extinction, and aerosol physical properties, including a Junge size-distribution parameter, and a real and imaginary index of refraction. The radiometer design provides the capacity for remote sensing of stratospheric constituents from space on platforms such as the space shuttle and satellites, and therefore provides for global measurements on a daily basis

Ultraviolet refractive index values of organic aerosol extracted from deciduous forestry, urban and marine environments

The refractive index values of atmospheric aerosols are required to address the large uncertainties in the magnitude of atmospheric radiative forcing and measurements of the refractive index dispersion with wavelength of particulate matter sampled from the atmosphere are rare over ultraviolet wavelengths. An ultraviolet-optimized spectroscopic system illuminates optically-trapped single particles from a range of tropospheric environments to determine the particle's optical properties. Aerosol from remote marine, polluted urban, and forestry environments is collected on quartz filters, and the organic fraction isextracted and nebulized to form micron-sized spherical particles. The radius and the real component of refractive index dispersion with wavelength of the optically trapped particles are determined to a precision of 0.001 mm and 0.002 respectively over a near-ultraviolet-visible wavelength range of 0.320–0.480 mm. Remote marine aerosol is observed to have the lowest refractive index (n = 1.442 (l = 0.350 mm)), with above-canopy rural forestry aerosol (n = 1.462–1.481 (l = 0.350 mm)) and polluted urban aerosol (n = 1.444–1.485 (l = 0.350 mm)) showing similar refractive index dispersions with wavelength. In-canopy rural forestry aerosol is observed to have the highest refractive index value (n = 1.508 (l = 0.350 mm)). The study presents the first single particle measurements of the dispersion of refractive index with wavelength of atmospheric aerosol samples below wavelengths of 0.350 mm. The Cauchy dispersion equation, commonly used to describe the visible refractive index variation of aerosol particles, is demonstrated to extend to ultraviolet wavelengths below 0.350 mm for the urban, forestry, and atmospheric aerosol water-insoluble extracts from these environments. A 1D radiative-transfer calculation of the difference in top-of-the-atmosphere albedo between atmospheric core–shell mineral aerosol with and without films of this material demonstrates the importance of organic films forming on mineral aerosol

Radiative absorption enhancement of dust mixed with anthropogenic pollution over East Asia

The particle mixing state plays a significant yet poorly quantified role in aerosol radiative forcing, especially for the mixing of dust (mineral absorbing) and anthropogenic pollution (black carbon absorbing) over East Asia. We have investigated the absorption enhancement of mixed-type aerosols over East Asia by using the Aerosol Robotic Network observations and radiative transfer model calculations. The mixed-type aerosols exhibit significantly enhanced absorbing ability than the corresponding unmixed dust and anthropogenic aerosols, as revealed in the spectral behavior of absorbing aerosol optical depth, single scattering albedo, and imaginary refractive index. The aerosol radiative efficiencies for the dust, mixed-type, and anthropogenic aerosols are −101.0, −112.9, and −98.3 Wm⁻²τ⁻¹ at the bottom of the atmosphere (BOA); −42.3, −22.5, and −39.8 Wm⁻²τ⁻¹ at the top of the atmosphere (TOA); and 58.7, 90.3, and 58.5 Wm⁻²τ⁻¹ in the atmosphere (ATM), respectively. The BOA cooling and ATM heating efficiencies of the mixed-type aerosols are significantly higher than those of the unmixed aerosol types over the East Asia region, resulting in atmospheric stabilization. In addition, the mixed-type aerosols correspond to a lower TOA cooling efficiency, indicating that the cooling effect by the corresponding individual aerosol components is partially counteracted. We conclude that the interaction between dust and anthropogenic pollution not only represents a viable aerosol formation pathway but also results in unfavorable dispersion conditions, both exacerbating the regional air pollution in East Asia. Our results highlight the necessity to accurately account for the mixing state of aerosols in atmospheric models over East Asia in order to better understand the formation mechanism for regional air pollution and to assess its impacts on human health, weather, and climate

On the determination of a cloud condensation nuclei from satellite : Challenges and possibilities

We use aerosol size distributions measured in the size range from 0.01 to 10+ μm during Transport and Chemical Evolution over the Pacific (TRACE-P) and Aerosol Characterization Experiment-Asia (ACE-Asia), results of chemical analysis, measured/modeled humidity growth, and stratification by air mass types to explore correlations between aerosol optical parameters and aerosol number concentration. Size distributions allow us to integrate aerosol number over any size range expected to be effective cloud condensation nuclei (CCN) and to provide definition of a proxy for CCN (CCNproxy). Because of the internally mixed nature of most accumulation mode aerosol and the relationship between their measured volatility and solubility, this CCNproxy can be linked to the optical properties of these size distributions at ambient conditions. This allows examination of the relationship between CCNproxy and the aerosol spectral radiances detected by satellites. Relative increases in coarse aerosol (e.g., dust) generally add only a few particles to effective CCN but significantly increase the scattering detected by satellite and drive the Angstrom exponent (α) toward zero. This has prompted the use of a so-called aerosol index (AI) on the basis of the product of the aerosol optical depth and the nondimensional α, both of which can be inferred from satellite observations. This approach biases the AI to be closer to scattering values generated by particles in the accumulation mode that dominate particle number and is therefore dominated by sizes commonly effective as CCN. Our measurements demonstrate that AI does not generally relate well to a measured proxy for CCN unless the data are suitably stratified. Multiple layers, complex humidity profiles, dust with very low α mixed with pollution, and size distribution differences in pollution and biomass emissions appear to contribute most to method limitations. However, we demonstrate that these characteristic differences result in predictable influences on AI. These results suggest that inference of CCN from satellites will be challenging, but new satellite and model capabilities could possibly be integrated to improve this retrieval