Rapid modification of cloud‐nucleating ability of aerosols by biogenic emissions

Ma, Yan; Brooks, Sarah D.; Vidaurre, German; Khalizov, Alexei F.; Wang, Lin; Zhang, Renyi

doi:10.1002/2013gl057895

Cited by 44 publications

(55 citation statements)

References 58 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…As discussed in Sect. 3.2, α-dicarbonyls are likely the most dominant products from the OH-initiated oxidation of m-xylene (Zhao et al, 2005), while organic acids are likely the dominant SOA components derived from ozonolysis of α-pinene (Ma et al, 2013). This is consistent with the higher NOC content in the total SOA mass from the OH oxidation of m-xylene as shown in Fig.…”

Section: Contribution Of Noc To Soasupporting

confidence: 79%

“…The POZ undergoes a unimolecular isomerization to produce Criegee intermediates (CIs), which subsequently yield both gas-phase and particle-phase compounds containing hydroxyl, carbonyl and acidic functional groups Yu et al, 1999). In particular, previous work has found that organic acids are the dominant SOA component (Ma et al, 2013). The OH initialed oxidation mechanism of m-xylene is more complex as described by the Master Chemical Mechanism MCM3.1 (Bloss et al, 2005); however it also leads to particle-phase acids and carbonyls (Loza et al, 2012).…”

Section: Potential Mechanisms Contributing To Observed Nocmentioning

confidence: 99%

“…In these specific experiments (P3, P5), the observed initial reactive uptake coefficients of NH 3 (γ obs,ini ; on an atomic N mass basis) to form the N in NOC were 4.8 ±0.2 × 10 −3 and 1.07 ±0.03 × 10 −3 , respectively. The true uptake coefficients (γ t,ini ) were obtained by performing gas-phase diffusion corrections for NH 3 using a previously reported empirical formula (Fuchs and Sutugin, 1970;Worsnop et al, 2002;Widmann and Davis, 1997) and the diffusion coefficient of NH 3 in air (0.1978 cm 2 s −1 ) (Massman, 1998). The corresponding γ t,ini values for all experiments ranged from 1.23 ±0.04 × 10 −3 to 1.52 ±0.03 × 10 −2 ( Table 2).…”

Section: Reaction Kineticsmentioning

confidence: 99%

See 2 more Smart Citations

Reactive uptake of ammonia to secondary organic aerosols: kinetics of organonitrogen formation

Liu¹,

Liggio²,

Staebler³

et al. 2015

Atmos. Chem. Phys.

View full text Add to dashboard Cite

Abstract. As a class of brown carbon, organonitrogen compounds originating from the heterogeneous uptake of NH 3 by secondary organic aerosol (SOA) have received significant attention recently. In the current work, particulate organonitrogen formation during the ozonolysis of α-pinene and the OH oxidation of m-xylene in the presence of ammonia (34-125 ppb) was studied in a smog chamber equipped with a high resolution time-of-flight aerosol mass spectrometer and a quantum cascade laser instrument. A large diversity of nitrogen-containing organic (NOC) fragments was observed which were consistent with the reactions between ammonia and carbonyl-containing SOA. Ammonia uptake coefficients onto SOA which led to organonitrogen compounds were reported for the first time, and were in the range of ∼ 10 −3 -10 −2 , decreasing significantly to < 10 −5 after 6 h of reaction. At the end of experiments (∼ 6 h) the NOC mass contributed 8.9 ± 1.7 and 31.5 ± 4.4 wt % to the total α-pineneand m-xylene-derived SOA, respectively, and 4-15 wt % of the total nitrogen in the system. Uptake coefficients were also found to be positively correlated with particle acidity and negatively correlated with NH 3 concentration, indicating that heterogeneous reactions were responsible for the observed NOC mass, possibly limited by liquid phase diffusion. Under these conditions, the data also indicate that the formation of NOC can compete kinetically with inorganic acid neutralization. The formation of NOC in this study suggests that a significant portion of the ambient particle associated N may be derived from NH 3 heterogeneous reactions with SOA. NOC from such a mechanism may be an important and unaccounted for source of PM associated nitrogen. This mechanism may also contribute to the medium or long-range transport and wet/dry deposition of atmospheric nitrogen.

show abstract

Section: Contribution Of Noc To Soasupporting

confidence: 79%

Section: Potential Mechanisms Contributing To Observed Nocmentioning

confidence: 99%

Section: Reaction Kineticsmentioning

confidence: 99%

See 1 more Smart Citation

Reactive uptake of ammonia to secondary organic aerosols: kinetics of organonitrogen formation

Liu¹,

Liggio²,

Staebler³

et al. 2015

Atmos. Chem. Phys.

View full text Add to dashboard Cite

show abstract

“…Not accounting for non-ideal interactions between particle components (i.e., assuming equilibrium partitioning to an ideal solution under circumstances in which this assumption is not valid) can result in a 10-40 % overprediction of cloud droplet number, depending on aerosol loading (Nenes et al, 2001). On the other hand, the presence of surface-active organic components can contribute to enhancements in CCN activity by reducing the surface tension of the particle surface-air interface (Ma et al, 2013;Sareen et al, 2013;Woo et al, 2013). In addition, simultaneous condensation of semivolatile organic vapors and water onto aerosol particles may enhance water uptake by increasing the availability of soluble material (Topping and McFiggans, 2012;Topping et al, 2013).…”

Section: Introductionmentioning

confidence: 99%

Discontinuities in hygroscopic growth below and above water saturation for laboratory surrogates of oligomers in organic atmospheric aerosols

et al. 2016

View full text Add to dashboard Cite

Abstract. Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. However, uncertainty remains regarding the factors that contribute to observations of low hygroscopic growth below water saturation but enhanced cloud condensation nuclei (CCN) activity for a given aerosol population. Utilizing laboratory surrogates for oligomers in atmospheric aerosols, we explore the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors. Measurements of hygroscopic growth under subsaturated conditions and the CCN activity of aerosols comprised of polyethylene glycol (PEG) with average molecular masses ranging from 200 to 10 000 g mol −1 and mixtures of PEG with ammonium sulfate (AS) were conducted. Experimental results are compared to calculations of hygroscopic growth at thermodynamic equilibrium conducted with the Aerosol Inorganic Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model, and the potential influence of kinetic limitations on observed water uptake was further explored through estimations of water diffusivity in the PEG oligomers. Particle-phase behavior, including the prevalence of liquid-liquid phase separation (LLPS), was also modeled with AIOMFAC. Under subsaturated relative humidity (RH) conditions, we observed little variability in hygroscopic growth across PEG systems with different molecular masses; however, an increase in CCN activity with increasing PEG molecular mass was observed. This effect is most pronounced for PEG-AS mixtures, and, in fact, an enhancement in CCN activity was observed for the PEG10000-AS mixture as compared to pure AS, as evidenced by a 15 % reduction in critical activation diameter at a supersaturation of 0.8 %. We also observed a marked increase in apparent hygroscopicity for mixtures of higher molecular mass PEG and AS under supersaturated conditions as compared to subsaturated hygroscopic growth. AIOMFAC-based predictions and estimations of water diffusivity in PEG suggest that such discontinuities in apparent hygroscopicity above and below water saturation can be attributed, at least in part, to differences in the sensitivity of water uptake behavior to surface tension effects. There is no evidence that kinetic limitations to water uptake due to the presence of viscous aerosol components influenced hygroscopic growth. For the systems that display an enhancement in apparent hygroscopicity above water saturation, LLPS is predicted to persist to high RH. This indicates a miscibilityPublished by Copernicus Publications on behalf of the European Geosciences Union. 12768 N. Hodas et al.: Discontinuities in the hygroscopicity of oligomers gap and is likely to influence bulk-to-surface partitioning of PEG at high RH, impacting droplet surface tension and CCN activity....

show abstract

“…This implies that the influence that a high content of sulfur in fuel, particularly in China, exalts on soot properties may significantly affect the resulting atmospheric impacts and the further transformation of soot. Although the cloudforming potential of soot particles is mainly determined by their atmospheric aging Ma et al, 2013b), lean flame soot particles generated from high sulfur content fuel are coated with more sulfate species, which will increase the hygroscopicity and to some extent enhance the cloud-forming potential of soot particles . Sulfate species coating and the subsequently enhanced hygroscopicity of soot particles increase the light absorption and scattering of soot particles , and then deteriorate the visibility and the local air quality.…”

Section: Discussionmentioning

confidence: 99%

Influence of sulfur in fuel on the properties of diffusion flame soot

Zhao

2016

Atmospheric Environment

View full text Add to dashboard Cite

h i g h l i g h t sLean flame soot was influenced more by sulfur in fuel than rich flame soot. Sulfate species were mainly formed on the surface of soot. The diameter of primary lean flame soot from high sulfur content fuel increased. The hygroscopicity of lean flame soot from high sulfur content fuel increased. a r t i c l e i n f o a b s t r a c tPrevious studies indicate that sulfur in fuel affects the hygroscopicity of soot. However, the issue of the effect of sulfur in fuel on soot properties is not fully understood. Here, the properties of soot prepared from fuel with a variable sulfur content were investigated under lean and rich flame conditions. Lean flame soot was influenced more by sulfur in fuel than rich flame soot. The majority of sulfur in fuel in lean flame was converted to gaseous SO 2 , while a small fraction appeared as sulfate and bisulfate (referred to as sulfate species) in soot. As the sulfur content in fuel increased, sulfate species in lean flame soot increased nonlinearly, while sulfate species on the surface of lean flame soot increased linearly. The hygroscopicity of lean flame soot from sulfur-containing fuel was enhanced mainly due to sulfate species. Meanwhile, more alkynes were formed in lean flame. The diameter of primary lean flame soot particles increased and accumulation mode particle number concentrations of lean flame soot from sulfurcontaining fuel increased as a result of more alkynes. Because the potential effects of soot particles on air pollution development greatly depend on the soot properties, which are related to both chemical aging and combustion conditions, this work will aid in understanding the impacts of soot on air quality and climate.

show abstract

Rapid modification of cloud‐nucleating ability of aerosols by biogenic emissions

Cited by 44 publications

References 58 publications

Reactive uptake of ammonia to secondary organic aerosols: kinetics of organonitrogen formation

Reactive uptake of ammonia to secondary organic aerosols: kinetics of organonitrogen formation

Discontinuities in hygroscopic growth below and above water saturation for laboratory surrogates of oligomers in organic atmospheric aerosols

Influence of sulfur in fuel on the properties of diffusion flame soot

Contact Info

Product

Resources

About