%0 Journal Article %1 Laskin:2010p3387 %A Laskin, Julia %A Laskin, Alexander %A Roach, Patrick J %A Slysz, Gordon W %A Anderson, Gordon A %A Nizkorodov, Sergey A %A Bones, David L %A Nguyen, Lucas Q %D 2010 %J Analytical Chemistry %K Aerosol, Aerosols, Ambient Analysis Atmospheric Biomass Burning Characterization, Conditions, Identification, Molecular Oligomers, Package, Particles, Rapid Samples, Software %N 5 %P 2048--2058 %R 10.1021/ac902801f %T High-Resolution Desorption Electrospray Ionization Mass Spectrometry for Chemical Characterization of Organic Aerosols %U http://pubs.acs.org/doi/abs/10.1021/ac902801f %V 82 %X Characterization of the chemical composition and chemical transformations of secondary organic aerosol (SOA) is both a major challenge and the area of greatest uncertainty in current aerosol research. This study presents the first application of desorption electrospray ionization combined with high-resolution mass spectrometry (DESI-MS) for detailed chemical characterization and studies of chemical aging of organic aerosol (OA) samples collected on Teflon substrates. DESI-MS offers unique advantages both for detailed characterization of chemically labile components in OA that cannot be detected using traditional electrospray ionization mass spectrometry (ESI-MS) and for studying chemical aging of OA. DESI-MS enables rapid characterization of OA samples collected oil substrates by eliminating the sample preparation stage. In addition, it enables detection and structural characterization of chemically labile molecules in OA samples by minimizing the residence time of analyte in the solvent In this study, DESI-MS and tandem mass spectrometry experiments (MS/MS) were used to examine chemical aging of SOA produced by the ozonolysis of limonene (LSOA) in the presence of gaseous ammonia. Exposure of LSOA to ammonia resulted in measurable changes in the optical properties of the sample observed using ultraviolet (UV)-visible spectroscopy. High-resolution DESI-MS analysis demonstrated that chemical aging results in formation of highly conjugated nitrogen-containing species that are most likely responsible for light-absorbing properties of the aged LSOA Detailed analysis of the experimental data allowed us to identify several key aging reactions, including the transformation of carbonyls to imines, intramolecular dimerization of imines with other carbonyl compounds in SOA, and intermolecular cyclization of imines. This study presents all important step toward understanding the formation of light-absorbing OA (brown carbon) in the atmosphere.

@article{Laskin:2010p3387, abstract = {Characterization of the chemical composition and chemical transformations of secondary organic aerosol (SOA) is both a major challenge and the area of greatest uncertainty in current aerosol research. This study presents the first application of desorption electrospray ionization combined with high-resolution mass spectrometry (DESI-MS) for detailed chemical characterization and studies of chemical aging of organic aerosol (OA) samples collected on Teflon substrates. DESI-MS offers unique advantages both for detailed characterization of chemically labile components in OA that cannot be detected using traditional electrospray ionization mass spectrometry (ESI-MS) and for studying chemical aging of OA. DESI-MS enables rapid characterization of OA samples collected oil substrates by eliminating the sample preparation stage. In addition, it enables detection and structural characterization of chemically labile molecules in OA samples by minimizing the residence time of analyte in the solvent In this study, DESI-MS and tandem mass spectrometry experiments (MS/MS) were used to examine chemical aging of SOA produced by the ozonolysis of limonene (LSOA) in the presence of gaseous ammonia. Exposure of LSOA to ammonia resulted in measurable changes in the optical properties of the sample observed using ultraviolet (UV)-visible spectroscopy. High-resolution DESI-MS analysis demonstrated that chemical aging results in formation of highly conjugated nitrogen-containing species that are most likely responsible for light-absorbing properties of the aged LSOA Detailed analysis of the experimental data allowed us to identify several key aging reactions, including the transformation of carbonyls to imines, intramolecular dimerization of imines with other carbonyl compounds in SOA, and intermolecular cyclization of imines. This study presents all important step toward understanding the formation of light-absorbing OA (brown carbon) in the atmosphere.}, added-at = {2010-06-22T19:38:37.000+0200}, affiliation = {Pacific NW Natl Lab, Div Chem {\&} Mat Sci, Richland, WA 99352 USA}, author = {Laskin, Julia and Laskin, Alexander and Roach, Patrick J and Slysz, Gordon W and Anderson, Gordon A and Nizkorodov, Sergey A and Bones, David L and Nguyen, Lucas Q}, biburl = {https://www.bibsonomy.org/bibtex/2344a12e9a160ff93ece7f04541547204/gsmith}, date-added = {2010-05-04 15:06:31 -0400}, date-modified = {2010-06-10 10:21:09 -0400}, doi = {10.1021/ac902801f}, interhash = {a5d2445ecec733cb98ab2902679395af}, intrahash = {344a12e9a160ff93ece7f04541547204}, journal = {Analytical Chemistry}, keywords = {Aerosol, Aerosols, Ambient Analysis Atmospheric Biomass Burning Characterization, Conditions, Identification, Molecular Oligomers, Package, Particles, Rapid Samples, Software}, language = {English}, local-url = {file://localhost/Users/geoffreysmith/Documents/Papers/Analytical%20Chemistry/2010/Analytical%20Chemistry,%2082,%202048-2058%202010.pdf}, month = Jan, number = 5, pages = {2048--2058}, pmid = {000274841300067}, rating = {0}, read = {Yes}, timestamp = {2010-06-22T19:39:26.000+0200}, title = {High-Resolution Desorption Electrospray Ionization Mass Spectrometry for Chemical Characterization of Organic Aerosols}, uri = {papers://E88B624E-D406-46FF-9D95-BB9C1AAE3FDC/Paper/p3387}, url = {http://pubs.acs.org/doi/abs/10.1021/ac902801f}, volume = 82, year = 2010 }