Size Matters in the Water Uptake and Hygroscopic Growth of Atmospherically Relevant Multicomponent Aerosol Particles

Laskina, Olga; Morris, Holly S.; Grandquist, Joshua R.; Qin, Zhen; Stone, Elizabeth A.; Tivanski, Alexei V.; Grassian, Vicki H.

doi:10.1021/jp510268p

Cited by 124 publications

(135 citation statements)

References 64 publications

Supporting

Mentioning

124

Contrasting

Order By: Relevance

“…7. The ERH of AS is determined to be 44.3 ± 2.5 % RH, which generally falls into the range from 33 to 52 % RH reported in the literature (Tang and Munkelwitz, 1994a;Cziczo et al, 1997;Dougle et al, 1998;Laskina et al, 2015). The DRH of AS particles is observed to occur at 80.1 ± 1.5 % RH, which agrees well with reported values of 80 % RH by EDB (Tang and Munkelwitz, 1994a) and 82.3 ± 2.5 % RH by micro-Raman spectroscopy (Laskina et al, 2015).…”

Section: Hygroscopic Growth Of Pure and Mixed Componentssupporting

confidence: 88%

“…Similar to OA, succinic acid and adipic acid have a high deliquescence point and low solubility. However, it has been found that the efflorescence point of AS in mixed particles is not elevated even when the content of succinic acid or adipic acid is more than 50 % by mass or mole fraction (Ling and Chan, 2008;Yeung et al, 2009; Laskina et al, 2015). The chemical nature of a solid determines its ability to act as a heterogeneous nucleus (Braban and Abbatt, 2004).…”

Section: Hygroscopic Growth Of Pure and Mixed Componentsmentioning

confidence: 99%

“…Ammonium sulfate (AS) is one of the most abundant inorganic constituents in the atmosphere, the hygroscopicity of which has been widely investigated (Liu et al, 2008;Cziczo et al, 1997;Laskina et al, 2015).…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

et al. 2017

View full text Add to dashboard Cite

Abstract. Although water uptake of aerosol particles plays an important role in the atmospheric environment, the effects of interactions between components on chemical composition and hygroscopicity of particles are still not well constrained. The hygroscopic properties and phase transformation of oxalic acid (OA) and mixed particles composed of ammonium sulfate (AS) and OA with different organic to inorganic molar ratios (OIRs) have been investigated by using confocal Raman spectroscopy. It is found that OA droplets first crystallize to form OA dihydrate at 71 % relative humidity (RH), and further lose crystalline water to convert into anhydrous OA around 5 % RH during the dehydration process. The deliquescence and efflorescence point for AS is determined to be 80.1 ± 1.5 % RH and 44.3 ± 2.5 % RH, respectively. The observed efflorescence relative humidity (ERH) for mixed OA / AS droplets with OIRs of 1 : 3, 1 : 1 and 3 : 1 is 34.4 ± 2.0, 44.3 ± 2.5 and 64.4 ± 3.0 % RH, respectively, indicating the elevated OA content appears to favor the crystallization of mixed systems at higher RH. However, the deliquescence relative humidity (DRH) of AS in mixed OA / AS particles with OIRs of 1 : 3 and 1 : 1 is observed to occur at 81.1 ± 1.5 and 77 ± 1.0 % RH, respectively. The Raman spectra of mixed OA / AS droplets indicate the formation of ammonium hydrogen oxalate (NH 4 HC 2 O 4 ) and ammonium hydrogen sulfate (NH 4 HSO 4 ) from interactions between OA and AS in aerosols during the dehydration process on the time scale of hours, which considerably influence the subsequent deliquescence behavior of internally mixed particles with different OIRs. The mixed OA / AS particles with an OIR of 3 : 1 exhibit no deliquescence transition over the RH range studied due to the considerable transformation of (NH 4 ) 2 SO 4 into NH 4 HC 2 O 4 with a high DRH. Although the hygroscopic growth of mixed OA / AS droplets is comparable to that of AS or OA at high RH during the dehydration process, Raman growth factors of mixed particles after deliquescence are substantially lower than those of mixed OA / AS droplets during the efflorescence process and further decrease with elevated OA content. The discrepancies for Raman growth factors of mixed OA / AS particles between the dehydration and hydration process at high RH can be attributed to the significant formation of NH 4 HC 2 O 4 and residual OA, which remain solid at high RH and thus result in less water uptake of mixed particles. These findings improve the understanding of the role of reactions between dicarboxylic acid and inorganic salt in the chemical and physical properties of aerosol particles, and might have important implications for atmospheric chemistry.

show abstract

Section: Hygroscopic Growth Of Pure and Mixed Componentssupporting

confidence: 88%

Section: Hygroscopic Growth Of Pure and Mixed Componentsmentioning

confidence: 99%

See 1 more Smart Citation

Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

et al. 2017

View full text Add to dashboard Cite

show abstract

“…The sample particles were first dried at below 10 % RH and then exposed to 60 % RH during the normal Raman and SERS measurements. Both types of particles are in solid form at 60 % RH (Laskina et al, 2015;Choi and Chan, 2002). There is no difference in the full width at half maximum (FWHM) and the peak position between AS and AS / SA particles (see Table 2), confirming that the presence of SA does not affect the phase state of AS at 60 % RH.…”

Section: Sers Of Laboratory-generated Pmmentioning

confidence: 73%

Electrospray surface-enhanced Raman spectroscopy (ES-SERS) for probing surface chemical compositions of atmospherically relevant particles

Gen

Chan

2017

Atmos. Chem. Phys.

View full text Add to dashboard Cite

Abstract. We present electrospray surface-enhanced Raman spectroscopy (ES-SERS) as a new approach to measuring the surface chemical compositions of atmospherically relevant particles. The surface-sensitive SERS is realized by electrospraying Ag nanoparticle aerosols over analyte particles. Spectral features at v(SO Enhanced spectra of the solid AS and AS / SA particles revealed the formation of surface-adsorbed water on their surfaces at 60 % relative humidity. These observations of surface aqueous sulfate and adsorbed water demonstrate a possible role of surface-adsorbed water in facilitating the dissolution of sulfate from the bulk phase into its water layer(s). Submicron ambient aerosol particles collected in Hong Kong exhibited non-enhanced features of black carbon and enhanced features of sulfate and organic matter (carbonyl group), indicating an enrichment of sulfate and organic matter on the particle surface.

show abstract

“…Spectromicroscopic methods include micro-FTIR, 7,8 micro-Raman, 9-11 69 micro-Raman combined with atomic force microscopy, 12 scanning and transmission electron 70 ray energy is proportional, among other factors, to the mass and composition of the matter in the 139 X-rays' path. Collecting the same image at different X-ray energies spanning across an elemental 140 absorption (referred to collectively as a stack) allows data acquisition for spatially resolved 141 NEXAFS spectroscopy.…”

Section: Introduction 48mentioning

confidence: 99%

Measuring Mass-Based Hygroscopicity of Atmospheric Particles through in Situ Imaging

Piens

Kelly

Harder

et al. 2016

Environ. Sci. Technol.

View full text Add to dashboard Cite

Quantifying how atmospheric particles interact with water vapor is critical for 32 understanding the effects of aerosols on climate. We present a novel method to measure the 33 mass-based hygroscopicity of particles while characterizing their elemental and carbon 34 functional group compositions. Since mass-based hygroscopicity is insensitive to particle 35 geometry, it is advantageous for probing the hygroscopic behavior of atmospheric particles, 36 which can have irregular morphologies. Combining scanning electron microscopy with energy 37 dispersive X-ray analysis (SEM/EDX), scanning transmission X-ray microscopy (STXM) 38 analysis, and in situ STXM humidification experiments, this method was validated using 39 laboratory-generated, atmospherically relevant particles. Then, the hygroscopicity and elemental 40 composition of 15 complex atmospheric particles were analyzed by leveraging quantification of 41 C, N, and O from STXM, and complementary elemental quantification from SEM/EDX. We 42 found three types of hygroscopic responses, and correlated high hygroscopicity with Na and Cl 43 content. The mixing state of 158 other particles from the sample broadly agreed with those of the 44

show abstract

Size Matters in the Water Uptake and Hygroscopic Growth of Atmospherically Relevant Multicomponent Aerosol Particles

Cited by 124 publications

References 64 publications

Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

Electrospray surface-enhanced Raman spectroscopy (ES-SERS) for probing surface chemical compositions of atmospherically relevant particles

Measuring Mass-Based Hygroscopicity of Atmospheric Particles through in Situ Imaging

Contact Info

Product

Resources

About