Environmental Chemistry Commons^™

Glyoxal’S Impact On Dry Ammonium Salts: Fast And Reversible Surface Aerosol Browning (Raw Data), David O. De Haan Phd, Lelia N. Hawkins Phd, Margaret A. Tolbert Phd, Jean-François Doussin

Chemistry and Biochemistry: Faculty Scholarship

Alpha-dicarbonyl compounds are believed to form brown carbon in the atmosphere via reactions with ammonium sulfate (AS) in cloud droplets and aqueous aerosol particles. In this work, brown carbon formation in AS and other aerosol particles was quantified as a function of relative humidity (RH) during exposure to gas-phase glyoxal (GX) in chamber experiments. Under dry conditions (RH < 5%), solid AS, AS/glycine, and methylammonium sulfate aerosol particles brown within minutes upon exposure to GX, while sodium sulfate particles do not. When GX concentrations decline, browning goes away, demonstrating that this dry browning process is reversible. Declines in aerosol albedo are found to be a function of [GX]2, and are consistent between AS and AS/glycine aerosol. Dry methylammonium sulfate aerosol browns 4´ more than dry AS aerosol, but deliquesced AS aerosol browns much less than dry AS aerosol. Optical measurements at 405, 450, and 530 nm provide an estimated Ångstrom absorbance coefficient of -16 ±4. This coefficient and the empirical relationship between GX and albedo are used to estimate an upper limit to global radiative forcing by brown carbon formed by 70 ppt GX reacting with AS (+7.6 ´10-5 W/m2). This quantity is < 1% of the total radiative forcing by secondary brown carbon, but occurs almost entirely in the ultraviolet range.

The zipped data files are in the following formats: Igor experiments (.pxp), Word documents (.docx), Excel spreadsheets (.xlsx), organized by experiment number. “Optical” files contain cavity attenuated phase shift (CAPS) extinction, scattering and albedo data; PILS/waveguide data (experiments 1,2, and 5 only); …

Glyoxal’S Impact On Dry Ammonium Salts: Fast And Reversible Surface Aerosol Browning, David O. De Haan Phd, Lelia N. Hawkins Phd, Kevin Jansen, Hannah G. Welsh, Raunak Pednekar, Alexia De Loera, Natalie G. Jimenez, Margaret A. Tolbert Phd, Mathieu Cazaunau Phd, Aline Gratien, Antonin Bergé, Edouard Pangui, Paola Formenti, Jean-François Doussin

Chemistry and Biochemistry: Faculty Scholarship

Alpha-dicarbonyl compounds are believed to form brown carbon in the atmosphere via reactions with ammonium sulfate (AS) in cloud droplets and aqueous aerosol particles. In this work, brown carbon formation in AS and other aerosol particles was quantified as a function of relative humidity (RH) during exposure to gas-phase glyoxal (GX) in chamber experiments. Under dry conditions (RH < 5%), solid AS, AS/glycine, and methylammonium sulfate aerosol particles brown within minutes upon exposure to GX, while sodium sulfate particles do not. When GX concentrations decline, browning goes away, demonstrating that this dry browning process is reversible. Declines in aerosol albedo are found to be a function of [GX]², and are consistent between AS and AS/glycine aerosol. Dry methylammonium sulfate aerosol browns 4´ more than dry AS aerosol, but deliquesced AS aerosol browns much less than dry AS aerosol. Optical measurements at 405, 450, and 530 nm provide an …

Brown Carbon Production By Aqueous-Phase Interactions Of Glyoxal And So2, David O. De Haan, Kevin Jansen, Alec D. Rynaski, W. Ryan P. Sueme, Ashley K. Torkelson, Eric T. Czer, Alexander K. Kim, Michael A. Rafla, Audrey C. De Haan, Margaret A. Tolbert

Chemistry and Biochemistry: Faculty Scholarship

Oxalic acid and sulfate salts are major components of aerosol particles. Here, we explore the potential for their respective precursor species, glyoxal and SO₂, to form atmospheric brown carbon via aqueous-phase reactions in a series of bulk aqueous and flow chamber aerosol experiments. In bulk aqueous solutions, UV- and visible-light-absorbing products are observed at pH 3–4 and 5–6, respectively, with small but detectable yields of hydroxyquinone and polyketone products formed, especially at pH 6. Hydroxymethanesulfonate (HMS), C₂, and C₃ sulfonates are major products detected by electrospray ionization mass spectrometry (ESI-MS) at pH 5. Past studies …