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DOI | 10.5194/acp-19-1491-2019 |
Viscosities, diffusion coefficients, and mixing times of intrinsic fluorescent organic molecules in brown limonene secondary organic aerosol and tests of the Stokes-Einstein equation | |
Ullmann, Dagny A.1; Hinks, Mallory L.2; Maclean, Adrian M.1; Butenhoff, Christopher L.3; Grayson, James W.1; Barsanti, Kelley6,7; Jimenez, Jose L.4,5; Nizkorodov, Sergey A.2; Kamal, Saeid1; Bertram, Allan K.1 | |
2019-02-04 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2019 |
卷号 | 19期号:3页码:1491-1503 |
文章类型 | Article |
语种 | 英语 |
国家 | Canada; USA |
英文摘要 | Viscosities and diffusion rates of organics within secondary organic aerosol (SOA) remain uncertain. Using the bead-mobility technique, we measured viscosities as a function of water activity (a(w)) of SOA generated by the ozonolysis of limonene followed by browning by exposure to NH3 (referred to as brown limonene SOA or brown LSOA). These measurements together with viscosity measurements reported in the literature show that the viscosity of brown LSOA increases by 3-5 orders of magnitude as the a w decreases from 0.9 to approximately 0.05. In addition, we measured diffusion coefficients of intrinsic fluorescent organic molecules within brown LSOA matrices using rectangular area fluorescence recovery after photobleaching. Based on the diffusion measurements, as the a w decreases from 0.9 to 0.33, the average diffusion coefficient of the intrinsic fluorescent organic molecules decreases from 5.5 +/- 10(9) to 7.1 +/- 10(13) cm(2) s(1) and the mixing times of intrinsic fluorescent organic molecules within 200 nm brown LSOA particles increases from 0.002 to 14 s. These results suggest that the mixing times of large organics in the brown LSOA studied here are short (< 1 h) for a(w) and temperatures often found in the planetary boundary layer (PBL). Since the diffusion coefficients and mixing times reported here correspond to SOA generated using a high mass loading (similar to 1000 mu gm(3)), biogenic SOA particles found in the atmosphere with mass loadings similar to 10 mu gm(3) are likely to have higher viscosities and longer mixing times (possibly 3 orders of magnitude longer). These new measurements of viscosity and diffusion were used to test the accuracy of the Stokes-Einstein relation for predicting diffusion rates of organics within brown LSOA matrices. The results show that the Stokes-Einstein equation gives accurate predictions of diffusion coefficients of large organics within brown LSOA matrices when the viscosity of the matrix is as high as 10(2) to 10(4) Pa s. These results have important implications for predicting diffusion and mixing within SOA particles in the atmosphere. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000457698000001 |
WOS关键词 | SIZE DISTRIBUTION DYNAMICS ; LONG-RANGE TRANSPORT ; ALPHA-PINENE ; PHASE STATE ; TRANSLATIONAL DIFFUSION ; ATMOSPHERIC AEROSOLS ; GLASS-TRANSITION ; REACTIVE UPTAKE ; SMALL VOLUMES ; PARTICLES |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/29513 |
专题 | 地球科学 |
作者单位 | 1.Univ British Columbia, Dept Chem, Vancouver, BC V6T 1Z1, Canada; 2.Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA; 3.Portland State Univ, Dept Phys, Portland, OR 97207 USA; 4.Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA; 5.Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA; 6.Univ Calif Riverside, Dept Chem & Environm Engn, Riverside, CA 92521 USA; 7.Univ Calif Riverside, Ctr Environm Res & Technol, Riverside, CA 92521 USA |
推荐引用方式 GB/T 7714 | Ullmann, Dagny A.,Hinks, Mallory L.,Maclean, Adrian M.,et al. Viscosities, diffusion coefficients, and mixing times of intrinsic fluorescent organic molecules in brown limonene secondary organic aerosol and tests of the Stokes-Einstein equation[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(3):1491-1503. |
APA | Ullmann, Dagny A..,Hinks, Mallory L..,Maclean, Adrian M..,Butenhoff, Christopher L..,Grayson, James W..,...&Bertram, Allan K..(2019).Viscosities, diffusion coefficients, and mixing times of intrinsic fluorescent organic molecules in brown limonene secondary organic aerosol and tests of the Stokes-Einstein equation.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(3),1491-1503. |
MLA | Ullmann, Dagny A.,et al."Viscosities, diffusion coefficients, and mixing times of intrinsic fluorescent organic molecules in brown limonene secondary organic aerosol and tests of the Stokes-Einstein equation".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.3(2019):1491-1503. |
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