Gaseous products and secondary organic aerosol formation during long term oxidation of isoprene and methacrolein

Bregonzio-Rozier, L.; Siekmann, F.; Giorio, Chiara; Pangui, Edouard; Morales, Sébastien B.; Temime-Roussel, Brice; Gratien, Aline; Michoud, Vincent; Ravier, Sylvain; Cazaunau, Mathieu; Tapparo, Andrea; Monod, Anne; Doussin, Jean‐François

doi:10.5194/acp-15-2953-2015

Cited by 45 publications

(62 citation statements)

References 58 publications

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“…Caponi et al: Spectral-and The experiments in this work have been performed in the 4.2 m 3 stainless-steel CESAM (Wang et al, 2011). The CE-SAM has been extensively used in recent years to simulate, at sub-and super-saturated conditions, the formation and properties of aerosols at concentration levels comparable to those encountered in the atmosphere (Denjean et al, 2015a, b;Brégonzio-Rozier et al, 2015, 2016Di Biagio et al, 2014, 2017. CESAM is a multi-instrumented platform, equipped with 12 circular flanges to support its analytical environment.…”

Section: Instruments and Methodsmentioning

confidence: 99%

Spectral- and size-resolved mass absorption efficiency of mineral dust aerosols in the shortwave spectrum: a simulation chamber study

et al. 2017

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Abstract. This paper presents new laboratory measurements of the mass absorption efficiency (MAE) between 375 and 850 nm for 12 individual samples of mineral dust from different source areas worldwide and in two size classes: PM 10.6 (mass fraction of particles of aerodynamic diameter lower than 10.6 µm) and PM 2.5 (mass fraction of particles of aerodynamic diameter lower than 2.5 µm). The experiments were performed in the CESAM simulation chamber using mineral dust generated from natural parent soils and included optical and gravimetric analyses.The results show that the MAE values are lower for the PM 10.6 mass fraction (range 37-135 × 10 −3 m 2 g −1 at 375 nm) than for the PM 2.5 (range 95-711 × 10 −3 m 2 g −1 at 375 nm) and decrease with increasing wavelength as λ −AAE , where the Ångström absorption exponent (AAE) averages between 3.3 and 3.5, regardless of size. The size independence of AAE suggests that, for a given size distribution, the dust composition did not vary with size for this set of samples. Because of its high atmospheric concentration, light absorption by mineral dust can be competitive with black and brown carbon even during atmospheric transport over heavy polluted regions, when dust concentrations are significantly lower than at emission. The AAE values of mineral dust are higher than for black carbon (∼ 1) but in the same range as light-absorbing organic (brown) carbon. As a result, depending on the environment, there can be some ambiguity in apportioning the aerosol absorption optical depth (AAOD) based on spectral dependence, which is relevant to the development of remote sensing of light-absorbing aerosols and their assimilation in climate models. We suggest that the sample-to-sample variability in our dataset of MAE values is related to regional differences in the mineralogical composition of the parent soils. Particularly in the PM 2.5 fraction, we found a strong linear correlation between the dust lightPublished by Copernicus Publications on behalf of the European Geosciences Union. 7176 L. Caponi et al.: Spectral-and size-resolved mass absorption efficiency of mineral dust aerosols absorption properties and elemental iron rather than the iron oxide fraction, which could ease the application and the validation of climate models that now start to include the representation of the dust composition, as well as for remote sensing of dust absorption in the UV-vis spectral region.

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Section: Instruments and Methodsmentioning

confidence: 99%

Spectral- and size-resolved mass absorption efficiency of mineral dust aerosols in the shortwave spectrum: a simulation chamber study

et al. 2017

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“…Due to uncertainties with organochloride quantification, the particulate chlorine content was not included in the SOA yield calculation. Only results from neutral seed experiments are used for comparison with other literature values of OH oxidation under low-and high-NO x scenarios (Brégonzio-Rozier et al, 2015;Koo et al, 2014;Liu et al, 2016;Xu et al, 2014) in Fig. 5.…”

Section: Soa Yieldmentioning

confidence: 99%

“…Under atmospheric conditions, the isoprene-to-chlorine ratio will usually be higher than ratios used in these experiments (0.5-1.2). Previous studies on chlorine-initiated SOA formation from toluene (Cai et al, 2008) and limonene (Cai and Griffin, OH, low NO x (CMAQ) OH, low NO x (Xu et al, 2014) OH, low NO x (Liu et al, 2016) OH, high NO x (CMAQ) OH, high NO x (Xu et al, 2014) OH, high NO x (Liu et al, 2016) NO x only (Brégonzio-Rozier et al, 2015) Figure 5. Comparison of observed isoprene-chlorine SOA yield with recent literature values corresponding to low-and high-NO x OH oxidation.…”

Section: Soa Yieldmentioning

confidence: 99%

“…7 were among the earliest oxidation products, which were further oxidized to produce SOA. MVK and MACR are also key intermediary products in OH-isoprene reactions from NO + RO 2 and RO 2 + RO 2 reaction pathways, where MACR is a known SOA precursor (Brégonzio-Rozier et al, 2015;Kroll et al, 2006;Surratt et al, 2006;Xu et al, 2014), which could contribute to some similarities between OH-isoprene and chlorine-isoprene SOA. Multiple generations of chlorinated C 5 compounds were observed in the gas phase, as shown in Fig.…”

Section: Soa Yieldmentioning

confidence: 99%

“…The majority of SOA originates from oxidation of biogenic volatile organic compounds (BVOCs), which account for ∼ 90% of annual non-methane hydrocarbon emissions (Goldstein and Galbally, 2007;Guenther et al, 2012), among which isoprene has the highest emission rate at ∼ 600 Tg yr −1 (Guenther et al, 2006). Isoprene SOA formation initiated by ozone (O 3 ), nitrate (NO 3 ), and hydroxyl (OH) radicals has been studied extensively and is estimated to account for 6-30 Tg yr −1 of the global aerosol budget (Brégonzio-Rozier et al, 2015;Claeys, 2004;Guenther et al, 2006;Kroll et al, 2006;Surratt et al, 2006Zhao et al, 2015), but the importance of isoprene SOA formation within the marine boundary layer (MBL) remains highly disputed in the literature (Arnold et al, 2009;Bikkina et al, 2014;Fu et al, 2011Fu et al, , 2013Gantt et al, 2010Gantt et al, , 2015Hu et al, 2013;Luo and Yu, 2010;O'Dowd and de Leeuw, 2007). Although the production of reactive chlorine species such as Cl 2 and HOCl has been observed within the MBL (Lawler et al, 2011), little is known about SOA from chlorine-initiated oxidation of isoprene.…”

Section: Introductionmentioning

confidence: 99%

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Secondary organic aerosol from chlorine-initiated oxidation of isoprene

Wang

Ruiz

2017

Atmos. Chem. Phys.

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Abstract. Recent studies have found concentrations of reactive chlorine species to be higher than expected, suggesting that atmospheric chlorine chemistry is more extensive than previously thought. Chlorine radicals can interact with hydroperoxy (HO x ) radicals and nitrogen oxides (NO x ) to alter the oxidative capacity of the atmosphere. They are known to rapidly oxidize a wide range of volatile organic compounds (VOCs) found in the atmosphere, yet little is known about secondary organic aerosol (SOA) formation from chlorineinitiated photooxidation and its atmospheric implications. Environmental chamber experiments were carried out under low-NO x conditions with isoprene and chlorine as primary VOC and oxidant sources. Upon complete isoprene consumption, observed SOA yields ranged from 7 to 36 %, decreasing with extended photooxidation and SOA aging. Formation of particulate organochloride was observed. A highresolution time-of-flight chemical ionization mass spectrometer was used to determine the molecular composition of gasphase species using iodide-water and hydronium-water cluster ionization. Multi-generational chemistry was observed, including ions consistent with hydroperoxides, chloroalkyl hydroperoxides, isoprene-derived epoxydiol (IEPOX), and hypochlorous acid (HOCl), evident of secondary OH production and resulting chemistry from Cl-initiated reactions. This is the first reported study of SOA formation from chlorineinitiated oxidation of isoprene. Results suggest that tropospheric chlorine chemistry could contribute significantly to organic aerosol loading.

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Recent advances in understanding secondary organic aerosol: Implications for global climate forcing

Shrivastava

Cappa

Fan

et al. 2017

Reviews of Geophysics

723

668

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Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron‐sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This review summarizes some of the important developments during the past decade in understanding SOA formation. We highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid‐catalyzed multiphase chemistry of isoprene epoxydiols, particle‐phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global models neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process‐related interactions, so that these processes can be accurately represented in atmospheric chemistry‐climate models.

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Gaseous products and secondary organic aerosol formation during long term oxidation of isoprene and methacrolein

Cited by 45 publications

References 58 publications

Spectral- and size-resolved mass absorption efficiency of mineral dust aerosols in the shortwave spectrum: a simulation chamber study

Spectral- and size-resolved mass absorption efficiency of mineral dust aerosols in the shortwave spectrum: a simulation chamber study

Secondary organic aerosol from chlorine-initiated oxidation of isoprene

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing

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