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Methylglyoxal is commonly believed to be less reactive than glyoxal because of unreactive methyl substitution, and available laboratory measurements showed negligible aerosol growth from methylglyoxal. Herein, we present experimental results to demonstrate striking oligomerization of small \u03b1-dicarbonyls leading to SOA and BrC formation on sub-micrometer aerosols. Significantly more efficient growth and browning of aerosols occur upon exposure to methylglyoxal than glyoxal under atmospherically relevant concentrations and in the absence\/presence of gas-phase ammonia and formaldehyde, and nonvolatile oligomers and light-absorbing nitrogen-heterocycles are identified as the dominant particle-phase products. The distinct aerosol growth and light absorption are attributed to carbenium ion-mediated nucleophilic addition, interfacial electric field-induced attraction, and synergetic oligomerization involving organic\/inorganic species, leading to surface- or volume-limited reactions that are dependent on the reactivity and gaseous concentrations. Our findings resolve an outstanding discrepancy concerning the multiphase chemistry of small \u03b1-dicarbonyls and unravel a new avenue for SOA and BrC formation from atmospherically abundant, ubiquitous carbonyls and ammonia\/ammonium sulfate.<\/jats:p>","DOI":"10.1021\/acs.est.0c08066","type":"journal-article","created":{"date-parts":[[2021,3,16]],"date-time":"2021-03-16T02:31:33Z","timestamp":1615861893000},"page":"4430-4439","source":"Crossref","is-referenced-by-count":66,"title":["Unexpected\nOligomerization of Small \u03b1\u2011Dicarbonyls\nfor Secondary Organic Aerosol and Brown Carbon Formation"],"prefix":"10.1021","volume":"55","author":[{"given":"Yixin","family":"Li","sequence":"first","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuemeng","family":"Ji","sequence":"additional","affiliation":[{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiayun","family":"Zhao","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuan","family":"Wang","sequence":"additional","affiliation":[{"name":"California Institute of Technology , , , ,","place":["Pasadena, California, United States, 91125"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiuju","family":"Shi","sequence":"additional","affiliation":[{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianfei","family":"Peng","sequence":"additional","affiliation":[{"name":"Nankai University , , ,","place":["Tianjin, China, 300071"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuying","family":"Wang","sequence":"additional","affiliation":[{"name":"Nanjing University of Information Science & Technology , , , ,","place":["Nanjing, Jiangsu, China, 210044"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chunyu","family":"Wang","sequence":"additional","affiliation":[{"name":"University of Science and Technology of China , , , ,","place":["Hefei, Anhui, China, 230022"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fang","family":"Zhang","sequence":"additional","affiliation":[{"name":"Beijing Normal University , , ,","place":["Beijing, China, 100875"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuxuan","family":"Wang","sequence":"additional","affiliation":[{"name":"University of Houston , , , ,","place":["Houston, Texas, United States, 77004"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1344-4068","authenticated-orcid":true,"given":"John H.","family":"Seinfeld","sequence":"additional","affiliation":[{"name":"California Institute of Technology , , , ,","place":["Pasadena, California, United States, 91125"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8708-3862","authenticated-orcid":true,"given":"Renyi","family":"Zhang","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2021,3,16]]},"reference":[{"key":"2026081711182483100_cit1","doi-asserted-by":"publisher","first-page":"3803","DOI":"10.1021\/acs.chemrev.5b00067","article-title":"Formation of Urban\nFine Particulate Matter","volume":"115","author":"Zhang","year":"2015","journal-title":"Chem. 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Contribution of Working Group I to the\nFifth Assessment Report of the Intergovernmental Panel on Climate\nChange","author":"Intergovernmental\nPanel on Climate Change (IPCC)","year":"2013"},{"key":"2026081711182483100_cit4","volume-title":"The Future of Atmospheric Chemistry Research: Remembering Yesterday,\nUnderstanding Today, Anticipating Tomorrow","author":"National\nAcademies of Sciences, Engineering, and Medicine","year":"2016"},{"key":"2026081711182483100_cit5","doi-asserted-by":"publisher","first-page":"1525","DOI":"10.1126\/science.1180353","article-title":"Evolution of Organic Aerosols in the Atmosphere","volume":"326","author":"Jimenez","year":"2009","journal-title":"Science"},{"key":"2026081711182483100_cit6","doi-asserted-by":"publisher","first-page":"17373","DOI":"10.1073\/pnas.1419604111","article-title":"Elucidating\nSevere Urban Haze Formation in China","volume":"111","author":"Guo","year":"2014","journal-title":"Proc.\nNatl. Acad. Sci. 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Technol."},{"key":"2026081711182483100_cit33","doi-asserted-by":"publisher","first-page":"4457","DOI":"10.1021\/jp509916r","article-title":"Heterogeneous Chemistry of Glyoxal\non Acidic Solutions. An Oligomerization Pathway for Secondary Organic\nAerosol Formation","volume":"119","author":"Gomez","year":"2015","journal-title":"J. Phys. Chem. A"},{"key":"2026081711182483100_cit34","doi-asserted-by":"publisher","first-page":"4854","DOI":"10.1021\/acs.jpca.8b00533","article-title":"Methylglyoxal Uptake\nCoefficients on Aqueous Aerosol Surfaces","volume":"122","author":"De\nHaan","year":"2018","journal-title":"J.\nPhys. Chem. A"},{"key":"2026081711182483100_cit35","doi-asserted-by":"publisher","first-page":"984","DOI":"10.1021\/es102933x","article-title":"Formation\nof Nitrogen-Containing Oligomers by Methylglyoxal and Amines in Simulated\nEvaporating Cloud Droplets","volume":"45","author":"De\nHaan","year":"2011","journal-title":"Environ. Sci. 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Phys."},{"key":"2026081711182483100_cit51","doi-asserted-by":"publisher","first-page":"2189","DOI":"10.1021\/acs.est.0c07204","article-title":"Explosive secondary\naerosol formation during severe haze in the North China Plain","volume":"55","author":"Peng","year":"2021","journal-title":"Environ. Sci. Technol."},{"key":"2026081711182483100_cit52","doi-asserted-by":"publisher","first-page":"8835","DOI":"10.1073\/pnas.0904128106","article-title":"Biogenic Carbon\nand Anthropogenic Pollutants Combine to Form a Cooling Haze over the\nSoutheastern United States","volume":"106","author":"Goldstein","year":"2009","journal-title":"Proc. Natl. Acad.\nSci. U.S.A."},{"key":"2026081711182483100_cit53","doi-asserted-by":"publisher","first-page":"3427","DOI":"10.1073\/pnas.1916366117","article-title":"Remarkable\nNucleation and Growth of Ultrafine Particles from Vehicular\nExhaust","volume":"117","author":"Guo","year":"2020","journal-title":"Proc. Natl. Acad. Sci. 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