Volatility of secondary organic aerosol during OH radical induced ageing

Salo, Kent; Hallquist, Mattias; Jönsson, Anders; Saathoff, H.; Naumann, K.‐H.; Spindler, C.; Tillmann, Ralf; Fuchs, Hendrik; Bohn, Birger; Rubach, Florian; Mentel, Thomas F.; Müller, Lars Peter; Reinnig, Marc-Christopher; Hoffmann, Thorsten; Donahue, Neil M.

doi:10.5194/acp-11-11055-2011

Cited by 66 publications

(95 citation statements)

References 50 publications

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“…We observed cloud condensation nucleus (CCN) activity (39), volatility via tandem differential mobility analysis (V-TDMA) (12,13), and subsaturated water uptake via hygroscopicity TDMA (H-TDMA) (12). The CCN activity of the organics was largely unaffected by either ripening or OH oxidation (39).…”

Section: Resultsmentioning

confidence: 96%

“…Volatility (Fig. 3B) showed a consistent temporal pattern in AIDA, PSI, and SAPHIR, responding to ripening and to OH aging (12,13). Volatility measured by the volume fraction remaining at a fixed elevated temperature decreased progressively during ripening, increased sharply with the introduction of OH, and then reverted to a more gradual progressive decrease after roughly 1 h of OH aging.…”

Section: Resultsmentioning

confidence: 96%

“…All experiments included a proton-transfer reaction mass spectrometer (44, 47), a scanning mobility particle sizer , an Aerodyne aerosol mass spectrometer (48,49), and either a thermodenuder (11) or a volatility tandem differential mobility analyzer (12,13). Most experiments measured SOA hygroscopicity, either with tandem differential mobility (12) measurements below 100% RH or with cloud condensation nucleus counting (39, 50) above 100% humidity or both.…”

Section: Methodsmentioning

confidence: 99%

“…This "chamber" SOA is modestly oxidized, with an oxygen to carbon ratio ðO∶CÞ < 0.4 (7). It is unambiguously semivolatile: Yields rise with increasing SOA mass loading (8,9) and decreasing temperature (10), and the SOA evaporates upon heating (11)(12)(13) and after isothermal dilution (14).…”

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confidence: 99%

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Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions

Donahue

Henry

Mentel

et al. 2012

Proc. Natl. Acad. Sci. U.S.A.

273

303

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The Multiple Chamber Aerosol Chemical Aging Study (MUCHA-CHAS) tested the hypothesis that hydroxyl radical (OH) aging significantly increases the concentration of first-generation biogenic secondary organic aerosol (SOA). OH is the dominant atmospheric oxidant, and MUCHACHAS employed environmental chambers of very different designs, using multiple OH sources to explore a range of chemical conditions and potential sources of systematic error. We isolated the effect of OH aging, confirming our hypothesis while observing corresponding changes in SOA properties. The mass increases are consistent with an existing gap between global SOA sources and those predicted in models, and can be described by a mechanism suitable for implementation in those models.atmospheric chemistry | biosphere-atmosphere interactions O rganic aerosol (OA) comprises a large fraction of fine-particle mass (PM 2.5 ) (1). In the developed world, 1-2% of deaths are blamed on inhalation of PM 2.5 (2), and the leading uncertainty in climate forcing is the interplay between the number of fine particles large enough to nucleate cloud droplets and the amount of sunlight reflected by those clouds (3). Oxidation and condensation of organics play a major but uncertain role in both phenomena.Traditional models treat most OA as nonvolatile primary OA (POA), augmented by secondary OA (SOA) (4), and they underpredict OA concentrations by a factor of 3-10 (5). α-Pinene is a major biogenic SOA source, sometimes used to represent all SOA in global models (4, 6). However, less than 20% of the carbon from fresh α-pinene oxidation condenses in chambers at room temperature; (7) the remainder is gaseous (Fig. 1A). This "chamber" SOA is modestly oxidized, with an oxygen to carbon ratio ðO∶CÞ < 0.4 (7). It is unambiguously semivolatile: Yields rise with increasing SOA mass loading (8, 9) and decreasing temperature (10), and the SOA evaporates upon heating (11-13) and after isothermal dilution (14).In contrast, ambient OA is highly oxidized (0.5 ≤ O∶C ≤ 1.0) (1, 15) and not very volatile (16). Ambient SOA is much less volatile than ambient POA (16). Consequently, "chamber" SOA does not represent the atmosphere. Our hypothesis is that homogeneous gas-phase aging by OH is a major missing process connecting chamber studies to the atmosphere. Considerable attention has been paid to heterogeneous uptake of oxidants to particles (17, 18), and recently gas-phase oxidation of semivolatile primary emissions (19), but the degree to which gas-phase oxidation can age chamber SOA is uncertain (1,4,18,20).OA resides in the atmosphere for about one week (21), while the gas-phase lifetimes of major semivolatile SOA constituents are far shorter. Typical α-pinene products pinonaldehyde, cispinonic acid, and pinic acid all have lifetimes of only a few hours for summertime conditions (22). Without question, oxidation of semivolatile SOA vapors will perturb the equilibrium phase partitioning of these constituents. Because almost all of the first-generation products are less volatile than α...

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Section: Resultsmentioning

confidence: 96%

Section: Resultsmentioning

confidence: 96%

Section: Methodsmentioning

confidence: 99%

mentioning

confidence: 99%

See 2 more Smart Citations

Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions

Donahue

Henry

Mentel

et al. 2012

Proc. Natl. Acad. Sci. U.S.A.

273

303

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“…For example, Cappa and Jimenez (2010) found that a large portion of the ambient OA mass in Mexico City was nonvolatile, while Lee et al (2010) discovered that most OA in a remote region near Finokalia in Crete, Greece, was semi-volatile. In chamber studies, Salo et al (2011) found that aerosol ageing took place in the gas phase due to OH oxidation of semi-volatile organic compounds and intermediate-volatility organic compounds rather than by bulk or surface reactions. Furthermore, the effects of particle volatility on CCN number and activity have also been investigated.…”

Section: Introductionmentioning

confidence: 99%

Toward the Determination of Joint Volatility-Hygroscopicity Distributions: Development and Response Characterization for Single-Component Aerosol

Cerully

Hite

McLaughlin

et al. 2014

Aerosol Science and Technology

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This work presents the development and characterization of a thermodenuder for the study and interpretation of aerosol volatility. Thermodenuder measurements are further combined with a continuous-flow streamwise thermal gradient CCN counter to obtain the corresponding aerosol hygroscopicity. The thermodenuder response function is characterized with monodisperse aerosol of variable volatility and hygroscopicity. The measurements are then interpreted with a comprehensive instrument model embedded within an optimization framework to retrieve aerosol properties with constrained uncertainty. Special attention is given to the interpretation of the size distribution of the thermodenuded aerosol, deconvoluting the effects of impurities and multiple charging, and to simplifications on the treatment of thermodenuder geometry, temperature, the cooling section, and the effects of curvature and accommodation coefficient on inferred particle volatility. Retrieved vapor pressures are consistent with published literature and shown to be most sensitive to uncertainty in the accommodation coefficient.

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Chemical characterization of α‐pinene secondary organic aerosol constituents using gas chromatography, liquid chromatography, and paper spray‐based mass spectrometry techniques

Rindelaub

Wiley

Cooper

et al. 2016

Rapid Comm Mass Spectrometry

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The use of HPLC/TOF and paper spray ionization methods to identify previously unobserved α-pinene-derived products helps lower the uncertainty in α-pinene oxidation chemistry and provides new platforms that can be used to identify and quantify important atmospheric compounds that relate to air quality in a complex sample matrix, such as ambient aerosol particles. Additionally, the use of paper spray ionization for direct filter analysis is a fast, relatively inexpensive sample preparation technique that can be used to reduce sample manipulation from solvent-induced reactions. Copyright © 2016 John Wiley & Sons, Ltd.

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Volatility of secondary organic aerosol during OH radical induced ageing

Cited by 66 publications

References 50 publications

Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions

Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions

Toward the Determination of Joint Volatility-Hygroscopicity Distributions: Development and Response Characterization for Single-Component Aerosol

Chemical characterization of α‐pinene secondary organic aerosol constituents using gas chromatography, liquid chromatography, and paper spray‐based mass spectrometry techniques

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