Complex refractive indices in the near-ultraviolet spectral region of biogenic secondary organic aerosol aged with ammonia

JM Flores, RA Washenfelder, G Adler, HJ Lee, Lior Segev, J Laskin, A Laskin, SA Nizkorodov, SS Brown, Yinon Rudich

פרסום מחקרי: פרסום בכתב עתמאמרביקורת עמיתים

תקציר

Atmospheric absorption by brown carbon aerosol may play an important role in global radiative forcing. Brown carbon arises from both primary and secondary sources, but the mechanisms and reactions of the latter are highly uncertain. One proposed mechanism is the reaction of ammonia or amino acids with carbonyl products in secondary organic aerosol (SOA). We generated SOA in situ by reacting biogenic alkenes (alpha-pinene, limonene, and alpha-humulene) with excess ozone, humidifying the resulting aerosol, and reacting the humidified aerosol with gaseous ammonia. We determined the complex refractive indices (RI) in the 360-420 nm range for these aerosols using broadband cavity enhanced spectroscopy (BBCES). The average real part (n) of the measured spectral range of the NH3-aged alpha-pinene SOA increased from n = 1.50 (+/- 0.01) for the unreacted SOA to n = 1.57 (+/- 0.01) after 1.5 h of exposure to 1.9 ppm NH3, whereas the imaginary component (k) remained below k <0.001 ((+0.002)(-0.001)) For the limonene and alpha-humulene SOA the real part did not change significantly, and we observed a small change in the imaginary component of the RI. The imaginary component increased from k = 0.000 to an average k = 0.029 (+/- 0.021) for alpha-humulene SOA, and from k <0.001((+0.002)(-0.001)) to an average k = 0.032 (+/- 0.019) for limonene SOA after 1.5 h of exposure to 1.3 and 1.9 ppm of NH3, respectively. Collected filter samples of the aged and unreacted alpha-pinene SOA and limonene SOA were analyzed off-line by nanospray desorption electrospray ionization high resolution mass spectrometry (nano-DESI/HR-MS), and in situ using a Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS), confirming that the SOA reacted and that various nitrogen-containing reaction products formed. If we assume that NH3 aging reactions scale linearly with time and concentration, which will not necessarily be the case in the atmosphere, then a 1.5 h reaction with 1 ppm NH3 in the laboratory is e
שפה מקוריתאנגלית
עמודים (מ-עד)10629-10642
מספר עמודים14
כתב עתPhysical Chemistry Chemical Physics
כרך16
מספר גיליון22
מזהי עצם דיגיטלי (DOIs)
סטטוס פרסוםפורסם - 2014

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