scholarly journals Density changes of aerosol particles as a result of chemical reaction

2005 ◽  
Vol 5 (1) ◽  
pp. 275-291 ◽  
Author(s):  
Y. Katrib ◽  
S. T. Martin ◽  
Y. Rudich ◽  
P. Davidovits ◽  
J. T. Jayne ◽  
...  
Keyword(s):  
Oleic Acid ◽  
Oxygen Content ◽  
Chemical Reactions ◽  
Aerosol Particles ◽  
Ozone Exposure ◽  
Spherical Particles ◽  
Aerodynamic Diameter ◽  
Layer Density ◽  
Aerosol Mass ◽  
Mobility Diameter

Abstract. This paper introduces the capability to study simultaneously changes in the density, the chemical composition, the mobility diameter, the aerodynamic diameter, and the layer thickness of multi-layered aerosol particles as they are being altered by heterogeneous chemical reactions. A vaporization-condensation method is used to generate aerosol particles composed of oleic acid outer layers of 2 to 30nm on 101-nm polystyrene latex cores. The layer density is modified by reaction of oleic acid with ozone for variable exposure times. For increasing ozone exposure, the mobility diameter decreases while the vacuum aerodynamic diameter increases, which, for spherical particles, implies that particle density increases. The aerosol particles are confirmed as spherical based upon the small divergence of the particle beam in the aerosol mass spectrometer. The particle and layer densities are calculated by two independent methods, namely one based on the measured aerodynamic and mobility diameters and the other based on the measured mobility diameter and particle mass. The uncertainty estimates for density calculated by the second method are two to three times greater than those of the first method. Both methods indicate that the layer density increases from 0.89 to 1.12g·cm-3 with increasing ozone exposure. Aerosol mass spectrometry shows that, concomitant with the increase in the layer density, the oxygen content of the reacted layer increases. Even after all of the oleic acid has reacted, the layer density and the oxygen content continue to increase slowly with prolonged ozone exposure, a finding which indicates continued chemical reactions of the organic products either with ozone or with themselves. The results of this paper provide new insights into the complex changes occurring for atmospheric particles during the aging processes caused by gas-phase oxidants.

scholarly journals Density changes of aerosol particles as a result of chemical reaction

2004 ◽  
Vol 4 (5) ◽  
pp. 6431-6472 ◽  
Author(s):  
Y. Katrib ◽  
S. T. Martin ◽  
Y. Rudich ◽  
P. Davidovits ◽  
J. T. Jayne ◽  
...  
Keyword(s):  
Oleic Acid ◽  
Oxygen Content ◽  
Chemical Reactions ◽  
Aerosol Particles ◽  
Ozone Exposure ◽  
Spherical Particles ◽  
Aerodynamic Diameter ◽  
Layer Density ◽  
Aerosol Mass ◽  
Mobility Diameter

Abstract. This paper introduces the capability to study simultaneously changes in the density, the chemical composition, the mobility diameter, the aerodynamic diameter, and the layer thickness of multi-layered aerosol particles as they are being altered by heterogeneous chemical reactions. A vaporization-condensation method is used to generate aerosol particles composed of oleic acid outer layers of 2 to 30 nm on 101-nm polystyrene latex cores. The layer density is modified by reaction of oleic acid with ozone for variable exposure times. For increasing ozone exposure, the mobility diameter decreases while the vacuum aerodynamic diameter increases, which, for spherical particles, implies that particle density increases. The aerosol particles are confirmed as spherical based upon the small divergence of the particle beam in the aerosol mass spectrometer. The particle and layer densities are calculated by two independent methods, namely one based on the measured aerodynamic and mobility diameters and the other based on the measured mobility diameter and particle mass. The uncertainty estimates for density calculated by the second method are two to three times greater than those of the first method. Both methods indicate that the layer density increases from 0.89 to 1.12 g·cm−3 with increasing ozone exposure. Aerosol mass spectrometry shows that, concomitant with the increase in the layer density, the oxygen content of the reacted layer increases. Even after all of the oleic acid has reacted, the layer density and the oxygen content continue to increase slowly with prolonged ozone exposure, a finding which indicates continued chemical reactions of the organic products either with ozone or with themselves. The results of this paper provide new insights into the complex changes occurring for atmospheric particles during the aging processes caused by gas-phase oxidants.

scholarly journals Organic aerosol source apportionment by offline-AMS over a full year in Marseille

2017 ◽  
Author(s):  
Carlo Bozzetti ◽  
Imad El Haddad ◽  
Dalia Salameh ◽  
Kaspar Rudolf Daellenbach ◽  
Paola Fermo ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Air Quality ◽  
Mediterranean Sea ◽  
Source Apportionment ◽  
Organic Aerosol ◽  
Aerodynamic Diameter ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Aerosol Source

Abstract. We investigated the seasonal trends of OA sources affecting the air quality of Marseille (France) which is the largest harbor of the Mediterranean Sea. This was achieved by measurements of nebulized filter extracts using an aerosol mass spectrometer (offline-AMS). PM2.5 (particulate matter with an aerodynamic diameter

scholarly journals Polarization properties of aerosol particles over western Japan: classification, seasonal variation, and implications for air quality

2016 ◽  
Author(s):  
X. L. Pan ◽  
I. Uno ◽  
Y. Hara ◽  
K. Osada ◽  
S. Yamamoto ◽  
...  
Keyword(s):  
Air Quality ◽  
Aerosol Particles ◽  
Threshold Value ◽  
Sea Salt ◽  
Spherical Particles ◽  
Aerosol Composition ◽  
Anthropogenic Pollutants ◽  
Online Measurements ◽  
Dependent Polarization ◽  
Western Japan

Abstract. Ground-based observations of the polarization properties of aerosol particles using a polarization optical particle counter (POPC) were performed from October 2013 to January 2015 at a suburban site in the Kyushu area of Japan. By conducting an analysis of online measurements of aerosol composition, we investigated size-dependent polarization characteristics for three typical aerosol types (anthrop ogenic pollutants, dust, and sea salt). We found that, for supermicron particles, its depolarization ratio (DR, the fraction of s-polarized signal in the total back ward light scattering signal) generally increased with the particle size, and a threshold value of 0.1 could be used to identify the irsphericity. In summer, air pollution was less serious, and the DR of aerosol particles was relatively small due to the influence of spherical sea salt particles in high humidity conditions. This study indicated that air masses were transported across the Asian continent and contained not only anthropogenic pollutants, but also large amounts of non-spherical particles (i.e., dust), which could impact on the air quality in western Japan, especially in winter and spring. The variation of number fraction of spherical particles did not correlate with relative humidity averaged along the trajectories of air parcels, indicating the coexistence of hydrophobic substances (e.g., mineral dust and organics), although the sulfate and nitrate mass concentrations were high.

scholarly journals New insights into PM<sub>2.5</sub> chemical composition and sources in two major cities in China during extreme haze events using aerosol mass spectrometry

2016 ◽  
Vol 16 (5) ◽  
pp. 3207-3225 ◽  
Author(s):  
Miriam Elser ◽  
Ru-Jin Huang ◽  
Robert Wolf ◽  
Jay G. Slowik ◽  
Qiyuan Wang ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Solution Space ◽  
Primary Sources ◽  
Aerodynamic Diameter ◽  
Data Set ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Aerosol Mass Spectrometry ◽  
Polycyclic Aromatic ◽  
On Line

Abstract. During winter 2013–2014 aerosol mass spectrometer (AMS) measurements were conducted for the first time with a novel PM2.5 (particulate matter with aerodynamic diameter  ≤ 2.5 µm) lens in two major cities of China: Xi'an and Beijing. We denote the periods with visibility below 2 km as extreme haze and refer to the rest as reference periods. During the measurements in Xi'an an extreme haze covered the city for about a week and the total non-refractory (NR)-PM2.5 mass fraction reached peak concentrations of over 1000 µg m−3. During the measurements in Beijing two extreme haze events occurred, but the temporal extent and the total concentrations reached during these events were lower than in Xi'an. Average PM2.5 concentrations of 537 ± 146 and 243 ± 47 µg m−3 (including NR species and equivalent black carbon, eBC) were recorded during the extreme haze events in Xi'an and Beijing, respectively. During the reference periods the measured average concentrations were 140 ± 99 µg m−3 in Xi'an and 75 ± 61 µg m−3 in Beijing. The relative composition of the NR-PM2.5 evolved substantially during the extreme haze periods, with increased contributions of the inorganic components (mostly sulfate and nitrate). Our results suggest that the high relative humidity present during the extreme haze events had a strong effect on the increase of sulfate mass (via aqueous phase oxidation of sulfur dioxide). Another relevant characteristic of the extreme haze is the size of the measured particles. During the extreme haze events, the AMS showed much larger particles, with a volume weighted mode at about 800 to 1000 nm, in contrast to about 400 nm during reference periods. These large particle sizes made the use of the PM2.5 inlet crucial, especially during the severe haze events, where 39 ± 5 % of the mass would have been lost in the conventional PM1 (particulate matter with aerodynamic diameter ≤ 1 µm) inlet. A novel positive matrix factorization procedure was developed to apportion the sources of organic aerosols (OA) based on their mass spectra using the multilinear engine (ME-2) controlled via the source finder (SoFi). The procedure allows for an effective exploration of the solution space, a more objective selection of the best solution and an estimation of the rotational uncertainties. Our results clearly show an increase of the oxygenated organic aerosol (OOA) mass during extreme haze events. The contribution of OOA to the total OA increased from the reference to the extreme haze periods from 16.2 ± 1.1 to 31.3 ± 1.5 % in Xi'an and from 15.7 ± 0.7 to 25.0 ± 1.2 % in Beijing. By contrast, during the reference periods the total OA mass was dominated by domestic emissions of primary aerosols from biomass burning in Xi'an (42.2 ± 1.5 % of OA) and coal combustion in Beijing (55.2 ± 1.6 % of OA). These two sources are also mostly responsible for extremely high polycyclic aromatic hydrocarbon (PAH) concentrations measured with the AMS (campaign average of 2.1 ± 2.0 µg m−3 and frequent peak concentrations above 10 µg m−3). To the best of our knowledge, this is the first data set where the simultaneous extraction of these two primary sources could be achieved in China by conducting on-line AMS measurements at two areas with contrasted emission patterns.

scholarly journals The ozonolysis of primary aliphatic amines in fine particles

2008 ◽  
Vol 8 (5) ◽  
pp. 1181-1194 ◽  
Author(s):  
J. Zahardis ◽  
S. Geddes ◽  
G. A. Petrucci
Keyword(s):  
Fine Particles ◽  
Reaction System ◽  
Tropospheric Chemistry ◽  
Ozone Exposure ◽  
Surface Barrier ◽  
Secondary Amide ◽  
Tertiary Amide ◽  
Aerosol Mass ◽  
Criegee Intermediates ◽  
Species Specific

Abstract. The oxidative processing by ozone of the particulate amines octadecylamine (ODA) and hexadecylamine (HDA) is reported. Ozonolysis of these amines resulted in strong NO2– and NO3– ion signals that increased with ozone exposure as monitored by photoelectron resonance capture ionization aerosol mass spectrometry. These products suggest a mechanism of progressive oxidation of the particulate amines to nitroalkanes. Additionally, a strong ion signal at 125 m/z is assigned to the ion NO3– (HNO3). For ozonized mixed particles containing ODA or HDA + oleic acid (OL), with pO3≥3×10–7 atm, imine, secondary amide, and tertiary amide products were measured. These products most likely arise from reactions of amines with aldehydes (for imines) and stabilized Criegee intermediates (SCI) or secondary ozonides (for amides) from the fatty acid. The routes to amides via SCI and/or secondary ozonides were shown to be more important than comparable amide forming reactions between amines and organic acids, using azelaic acid as a test compound. Finally, direct evidence is provided for the formation of a surface barrier in the ODA + OL reaction system that resulted in the retention of OL at high ozone exposures (up to 10−3 atm for 17 s). This effect was not observed in HDA + OL or single component OL particles, suggesting that it may be a species-specific surfactant effect from an in situ generated amide or imine. Implications to tropospheric chemistry, including particle bound amines as sources of oxidized gas phase nitrogen species (e.g.~NO2, NO3), formation of nitrogen enriched HULIS via ozonolysis of amines and source apportionment are discussed.

scholarly journals Mass Extinction Efficiency Approximation for Polydispersed Aerosol Using Harmonic Mean-Type Approximation

2020 ◽  
Vol 10 (23) ◽  
pp. 8637
Author(s):  
Junshik Um ◽  
Seonghyeon Jang ◽  
Young Jun Yoon ◽  
Seoung Soo Lee ◽  
Ji Yi Lee ◽  
...  
Keyword(s):  
Optical Properties ◽  
Chemical Composition ◽  
Extinction Coefficient ◽  
Mass Extinction ◽  
Aerosol Particles ◽  
Size Distributions ◽  
Extinction Efficiency ◽  
Type Approximation ◽  
Aerosol Mass ◽  
Mass Extinction Efficiency

Among many parameters characterizing atmospheric aerosols, aerosol mass extinction efficiency (MEE) is important for understanding the optical properties of aerosols. MEE is expressed as a function of the refractive indices (i.e., composition) and size distributions of aerosol particles. Aerosol MEE is often considered as a size-independent constant that depends only on the chemical composition of aerosol particles. The famous Malm’s reconstruction equation and subsequent revised methods express the extinction coefficient as a function of aerosol mass concentration and MEE. However, the used constant MEE does not take into account the effect of the size distribution of polydispersed chemical composition. Thus, a simplified expression of size-dependent MEE is required for accurate and conventional calculations of the aerosol extinction coefficient and also other optical properties. In this study, a simple parameterization of MEE of polydispersed aerosol particles was developed. The geometric volume–mean diameters of up to 10 µm with lognormal size distributions and varying geometric standard deviations were used to represent the sizes of various aerosol particles (i.e., ammonium sulfate and nitrate, elemental carbon, and sea salt). Integrating representations of separate small mode and large mode particles using a harmonic mean-type approximation generated the flexible and convenient parameterizations of MEE that can be readily used to process in situ observations and adopted in large-scale numerical models. The calculated MEE and the simple forcing efficiency using the method developed in this study showed high correlations with those calculated using the Mie theory without losing accuracy.

scholarly journals NMR Spectroscopic Study of Chemical Reactions in Mixtures Containing Oleic Acid, Formic Acid, and Formoxystearic Acid

2019 ◽  
Vol 58 (14) ◽  
pp. 5622-5630 ◽  
Author(s):  
Agnes Fröscher ◽  
Kai Langenbach ◽  
Erik von Harbou ◽  
Werner R. Thiel ◽  
Hans Hasse
Keyword(s):  
Oleic Acid ◽  
Formic Acid ◽  
Spectroscopic Study ◽  
Chemical Reactions

scholarly journals MOPSMAP v0.9: A versatile tool for modeling of aerosol optical properties

2018 ◽  
Author(s):  
Josef Gasteiger ◽  
Matthias Wiegner
Keyword(s):  
Remote Sensing ◽  
Optical Properties ◽  
Aerosol Particles ◽  
Particle Orientation ◽  
Spherical Particles ◽  
Refractive Indices ◽  
Hygroscopic Growth ◽  
Web Interface ◽  
Optical Modeling ◽  
Wide Range

Abstract. 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 non-spherical 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 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 case of non-spherical particles, and the variability of volcanic ash microphysics. The web interface is designed to be intuitive for expert and non-expert 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 MOPSMAP package is available on request for offline calculations, e.g., when large numbers of different runs for sensitivity studies shall be made.

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