Relationship between Oxidation Level and Optical Properties of Secondary Organic Aerosol

Lambe, Andrew T.; Cappa, Christopher D.; Massoli, P.; Onasch, T. B.; Forestieri, Sara D.; Martin, Alexander; Cummings, Molly J.; Croasdale, D. R.; Brune, William H.; Worsnop, Douglas R.; Davidovits, P.

doi:10.1021/es401043j

Cited by 286 publications

(365 citation statements)

References 84 publications

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“…When the fraction of the biomass-burning aqSOA becomes larger, the AAE increases, with values up to 5. This result agrees with measurements of optical properties of aqSOA produced in laboratory experiments from photooxidation and nitration of phenolic compounds (13,17,39). The large AAE indicates that this OA component absorbs radiation efficiently in the near-UV and visible region, possibly contributing to a net positive radiative forcing.…”

Section: Discussionsupporting

confidence: 86%

Direct observation of aqueous secondary organic aerosol from biomass-burning emissions

Gilardoni

Massoli

Paglione

et al. 2016

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

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The mechanisms leading to the formation of secondary organic aerosol (SOA) are an important subject of ongoing research for both air quality and climate. Recent laboratory experiments suggest that reactions taking place in the atmospheric liquid phase represent a potentially significant source of SOA mass. Here, we report direct ambient observations of SOA mass formation from processing of biomass-burning emissions in the aqueous phase. Aqueous SOA (aqSOA) formation is observed both in fog water and in wet aerosol. The aqSOA from biomass burning contributes to the "brown" carbon (BrC) budget and exhibits light absorption wavelength dependence close to the upper bound of the values observed in laboratory experiments for fresh and processed biomass-burning emissions. We estimate that the aqSOA from residential wood combustion can account for up to 0.1-0.5 Tg of organic aerosol (OA) per y in Europe, equivalent to 4-20% of the total OA emissions. Our findings highlight the importance of aqSOA from anthropogenic emissions on air quality and climate.particulate matter | air quality | secondary organic aerosol | biomass burning | aqueous processing

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Section: Discussionsupporting

confidence: 86%

Direct observation of aqueous secondary organic aerosol from biomass-burning emissions

Gilardoni

Massoli

Paglione

et al. 2016

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

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306

275

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“…Figure 9 shows that the real part of the CRI decreases substantially as the O : C of the bulk SOA decreases. This trend is in agreement with the positive correlation between the extinction coefficient at 532 nm wavelength and O : C observed by for the heterogeneous OH oxidation of squalane and aze- (Nakayama et al, 2012) -pinene (Lambe et al 2013) toluene (Nakayama et al, 2013) 1 naphtalene (Lambe et al 2013) guaiacol (Lambe et al 2013) tricyclo[5.2.1.0 2,6 ]decane (Lambe et al 2013) squalane azelaic acid Photooxidation Ozonolysis OH-oxidation laic acid particles. Nakayama et al (2013) reported an increasing real part of the CRI at 532 nm with increasing O : C for SOA generated from the photooxidation of toluene.…”

Section: Dependence Of the Cri And Gf On The Chemical Compositionsupporting

confidence: 90%

“…As a result, atmospheric SOA contains many organic compounds with a large variety of structures, chain lengths, functionalities and degrees of oxidation (Kroll and Seinfeld, 2008;Jimenez et al, 2009). Therefore, SOA possess a wide range of hygroscopic and optical properties (Lambe et al, 2013;Suda et al, 2012).…”

Section: Denjean Et Al: Relating Hygroscopicity and Optical Propementioning

confidence: 99%

“…On the other hand, an opposite trend was observed by Nakayama et al (2012) with a decrease of the real part of the CRI at 532 nm wavelength with increasing O : C for SOA produced from the ozonolysis and photooxidation of α-pinene. Lambe et al (2013) studied SOA formed by OH oxidation of various gas-phase precursors (naphthalene, tricyclo[5.2.1.0 2,6 ]decane, guaiacol and α-pinene) and retrieved a decreasing real part of the CRI with increasing oxidation. These different trends suggest that the change of the real CRI as a function of O : C depends strongly on the organic aerosol source and aging in the atmosphere.…”

Section: Dependence Of the Cri And Gf On The Chemical Compositionmentioning

confidence: 99%

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Relating hygroscopicity and optical properties to chemical composition and structure of secondary organic aerosol particles generated from the ozonolysis of α-pinene

et al. 2015

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Abstract. Secondary organic aerosol (SOA) were generated from the ozonolysis of α-pinene in the CESAM (French acronym for Experimental Multiphasic Atmospheric Simulation Chamber) simulation chamber. The SOA formation and aging were studied by following their optical, hygroscopic and chemical properties. The optical properties were investigated by determining the particle complex refractive index (CRI). The hygroscopicity was quantified by measuring the effect of relative humidity (RH) on the particle size (size growth factor, GF) and on the scattering coefficient (scattering growth factor, f (RH)). The oxygen to carbon atomic ratios (O : C) of the particle surface and bulk were used as a sensitive parameter to correlate the changes in hygroscopic and optical properties of the SOA composition during their formation and aging in CESAM.The real CRI at 525 nm wavelength decreased from 1.43-1.60 (±0.02) to 1.32-1.38 (±0.02) during the SOA formation. The decrease in the real CRI correlated to the O : C decrease from 0.68 (±0.20) to 0.55 (±0.16). In contrast, the GF remained roughly constant over the reaction time, with values of 1.02-1.07 (±0.02) at 90 % (±4.2 %) RH. Simultaneous measurements of O : C of the particle surface revealed that the SOA was not composed of a homogeneous mixture, but contained less oxidised species at the surface which may limit water absorption. In addition, an apparent change in both mobility diameter and scattering coefficient with increasing RH from 0 to 30 % was observed for SOA after 14 h of reaction. We postulate that this change could be due to a change in the viscosity of the SOA from a predominantly glassy state to a predominantly liquid state.

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“…H C H O , H C O O H , C H 3 N O 2 , CH 3 N  C H 2 a n d (CH 3 ) 2 NCHO were confirmed as the major products by both FTIR and PTR-MS. Heterogeneous oxidation usually leads to increases in oxygen-containing species, 69,70 O/C ratio 71 and structure modifications of aerosol particles, 72 subsequently, may alter its hygroscopicity 73 and optical properties. 74 Although most of these products are volatile from ozone oxidation of particulate TMA, a portion of these compounds are in the particle phase. Thus, heterogeneous oxidation might have influence on the hygroscopic and optical properties of particulate amines, while further studies are required in the future.…”

Section: ■ Atmospheric Implicationsmentioning

confidence: 99%

Ozonolysis of Trimethylamine Exchanged with Typical Ammonium Salts in the Particle Phase

Chu

et al. 2016

Environ. Sci. Technol.

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Alkylamines contribute to both new particle formation and brown carbon. The toxicity of particle-phase amines is of great concern in the atmospheric chemistry community. Degradation of particulate amines may lead to secondary products in the particle phase, which are associated with changes in the adverse health impacts of aerosols. In this study, O 3 oxidation of particulate trimethylamine (TMA) formed via heterogeneous uptake of TMA by (NH 4 ) 2 SO 4 , NH 4 HSO 4 , NH 4 NO 3 and NH 4 Cl, was investigated with in situ attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and proton transfer reaction mass spectrometry (PTR-MS). HCOOH, HCHO, CH 3 NCH 2 , (CH 3 ) 2 NCHO, CH 3 NO 2 , CH 3 N(OH)CHO, CH 3 NHOH and H 2 O were identified as products on all the substrates based upon IR (one-dimensional IR and two-dimensional correlation infrared spectroscopy), quantum chemical calculation and PTR-MS results. A reaction mechanism was proposed to explain the observed products. This work demonstrates that oxidation might be a degradation pathway of particulate amines in the atmosphere. This will aid in understanding the fate of particulate amines formed by nucleation and heterogeneous uptake and their potential health impacts during atmospheric aging.

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Relationship between Oxidation Level and Optical Properties of Secondary Organic Aerosol

Cited by 286 publications

References 84 publications

Direct observation of aqueous secondary organic aerosol from biomass-burning emissions

Direct observation of aqueous secondary organic aerosol from biomass-burning emissions

Relating hygroscopicity and optical properties to chemical composition and structure of secondary organic aerosol particles generated from the ozonolysis of α-pinene

Ozonolysis of Trimethylamine Exchanged with Typical Ammonium Salts in the Particle Phase

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