Relating hygroscopicity and composition of organic aerosol particulate matter

Duplissy, Jonathan; DeCarlo, P. F.; Dommen, Josef; Alfarra, M. Rami; Metzger, Axel; Barmpadimos, I.; Prévôt, Andrê S. H.; Weingärtner, E.; Tritscher, T.; Gysel, M.; Aiken, A. C.; Jimenez, José L.; Canagaratna, Manjula R.; Worsnop, Douglas R.; Collins, D. R.; Tomlinson, Jason; Baltensperger, Urs

doi:10.5194/acp-11-1155-2011

Cited by 338 publications

(394 citation statements)

References 56 publications

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“…It is worth realising that the GFs for pure (NH4)2SO4 and NH4NO3 (Park et al, 2009) are substantially larger than the measured values, which indicate considerable abundance of less hygroscopic species that are internally mixed with the inorganic salts. These particles can be composed of moderately transformed aged soot-containing combustion particles comprising also partly oxygenated organics and inorganic salts (Duplissy et al, 2011; 20 Liu et al, 2013). This view is further confirmed by a high-resolution TEM/EDS study of individual particles at the BpART facility (Németh et al, 2015).…”

supporting

confidence: 50%

Winter time hygroscopicity and volatility of ambient urban aerosol particles

Enroth¹,

Mikkilä²,

Németh³

et al. 2017

Preprint

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Abstract. Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20), 50, 75, 110 and 145 nm were determined in situ by using a VH-TDMA system with a relative humidity of 90% and denuding temperature of 270 C in central Budapest during two months in winter 2014-2015. The probability density function of the hygroscopic growth factor (GF) showed a distinct bimodal distribution. One of the modes was characterised by an overall mean GF of 10 approximately 1.07 (the corresponding hygroscopicity parameter  of 0.033) independently of the particle size, and was assigned to nearly hydrophobic (NH) particles. Its mean particle number fraction was large, and it was decreasing monotonically from 71% to 41% with particle diameter. The other mode showed a mean GF increasing slightly from 1.31 to 1.38 ( values from 0.186 to 0.196) with particle diameter, and it was attributed to less hygroscopic (LH) particles. These hygroscopicity values are low in general. The mode with more hygroscopic particles was not identified. The probability density 15 function of the volatility GF also exhibited a distinct bimodal distribution with an overall mean volatility GF of approximately 0.96 independently of the particle size, and with another mean GF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV) and volatile (V) particles. The mean particle number fraction for the LV mode was decreasing from 34% to 21% with particle diameter. The bimodal distributions in the GF spectrum indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. The mean 20 diurnal variability of the particle number fractions for the NH and LV modes, and of the volatility GF for the LV mode followed the diurnal pattern of the vehicular road traffic, while the mean diurnal variability of the hygroscopicity parameter for the NH, and of the particle number fractions for the V mode on workdays were inversely linked to the road traffic. The particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic 25 compounds such as non-hygroscopic hydrocarbon-like organics. The particles related to the LH and V modes could be composed of moderately transformed aged combustion particles consisting of partly oxygenated organics, inorganic salts and soot. Both regional background sources and urban (local) emissions contribute to these particles. Dependency of the volatility GF and the volume fraction remaining after the thermal treatment on the mean hygroscopic GF suggested that the hygroscopic compounds were ordinarily volatile, and that the larger particles contained internally mixed non-volatile chemical species as 30 refractory residuals in 20-25% of the aerosol material (by volume), which could be core-like soot or organic polymers.

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supporting

confidence: 50%

Winter time hygroscopicity and volatility of ambient urban aerosol particles

Enroth¹,

Mikkilä²,

Németh³

et al. 2017

Preprint

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“…Relationships between m/z 44 and measurements of a few individual organic acids (rather than total particlephase acids) have also been observed in laboratory and field measurements [Takegawa et al, 2007;Sorooshian et al, 2010;Duplissy et al, 2011]. Takegawa et al [2007] observed good correlation (r 2 = 0.85-0.94) between m/z 44 and select dicarboxylic and ω-oxocarboxylic acids collected on filters in Tokyo, Japan.…”

Section: /2015gl064650mentioning

confidence: 68%

“…polyacids, and multifunctional acids and for acids with different carbon chain lengths [Russell et al, 2009;Duplissy et al, 2011;Canagaratna et al, 2015]; therefore, the analysis presented here can be treated as an ensemble average relationship between particle-phase organic acids and m/z 44.…”

Section: /2015gl064650mentioning

confidence: 99%

Estimating the contribution of organic acids to northern hemispheric continental organic aerosol

Yatavelli

Mohr

Stark

et al. 2015

Geophysical Research Letters

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Using chemical ionization mass spectrometry to detect particle‐phase acids and aerosol mass spectrometry (AMS) measurements from Colorado, USA, and two studies in Hyytiälä, Finland, we quantify the fraction of organic aerosol (OA) mass that is composed of molecules with acid functional groups (facid). Molecules containing one or more carboxylic acid functionality contributed approximately 29% (45–51%) of the OA mass in Colorado (Finland). Organic acid mass concentration correlates well with AMS m/z 44 (primarily CO2+), a commonly used marker for highly oxidized aerosol. Using the average empirical relationship between AMS m/z 44 and organic acids in these three studies, together with m/z 44 data from 29 continental northern hemispheric (NH) AMS data sets, we estimate that molecules containing carboxylic acid functionality constitute on average 28% (range 10–50%) of NH continental OA mass with typically higher values at rural/remote sites and during summer and lower values at urban sites and during winter.

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“…Conventional instruments report growth under subsaturated conditions with accuracies of ±1% in a w below 95% RH and ±0.1% for high-humidity instruments at >99% RH. 14,16,30 In CCN activation measurements, the uncertainty in the critical supersaturation value is typically between 30% at supersaturations between 0.1 and 1%, equivalent to uncertainties of 0.03 to 0.3% at a w > 0.99. 31 In addition, the largest uncertainties in diameter growth factor from this technique are of order ∼0.7% (see, for example, the points that have error bars larger than the point size in Figure 8); subsaturated growth measurements by conventional instruments have associated uncertainties of ±5% with large interinstrument variabilities.…”

Section: Resultsmentioning

confidence: 99%

Accurate Measurements of Aerosol Hygroscopic Growth over a Wide Range in Relative Humidity

et al. 2016

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Using a comparative evaporation kinetics approach, we describe a new and accurate method for determining the equilibrium hygroscopic growth of aerosol droplets. The time-evolving size of an aqueous droplet, as it evaporates to a steady size and composition that is in equilibrium with the gas phase relative humidity, is used to determine the time-dependent mass flux of water, yielding information on the vapor pressure of water above the droplet surface at every instant in time. Accurate characterization of the gas phase relative humidity is provided from a control measurement of the evaporation profile of a droplet of know equilibrium properties, either a pure water droplet or a sodium chloride droplet. In combination, and by comparison with simulations that account for both the heat and mass transport governing the droplet evaporation kinetics, these measurements allow accurate retrieval of the equilibrium properties of the solution droplet (i.e., the variations with water activity in the mass fraction of solute, diameter growth factor, osmotic coefficient or number of water molecules per solute molecule). Hygroscopicity measurements can be made over a wide range in water activity (from >0.99 to, in principle, <0.05) on time scales of <10 s for droplets containing involatile or volatile solutes. The approach is benchmarked for binary and ternary inorganic solution aerosols with typical uncertainties in water activity of <±0.2% at water activities >0.9 and ∼±1% below 80% RH, and maximum uncertainties in diameter growth factor of ±0.7%. For all of the inorganic systems examined, the time-dependent data are consistent with large values of the mass accommodation (or evaporation) coefficient (>0.1).

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Relating hygroscopicity and composition of organic aerosol particulate matter

Cited by 338 publications

References 56 publications

Winter time hygroscopicity and volatility of ambient urban aerosol particles

Winter time hygroscopicity and volatility of ambient urban aerosol particles

Estimating the contribution of organic acids to northern hemispheric continental organic aerosol

Accurate Measurements of Aerosol Hygroscopic Growth over a Wide Range in Relative Humidity

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