Biogenic secondary organic aerosols (SOAs) contribute to a large fraction of fine aerosols globally, impacting air quality and climate. The formation of biogenic SOA depends on not only emissions of biogenic volatile organic compounds (BVOCs) but also anthropogenic pollutants including primary organic aerosol, sulfur dioxide (SO2), and nitrogen oxides (NOx). However, the anthropogenic impact on biogenic SOA production (AIBS) remains unclear. Here we use the decadal trend and variability in observed organic aerosol (OA) in the southeast US, combined with a global chemistry-climate model, to better constrain AIBS. We show that the reduction in SO2 emissions can only explain 40 % of the decreasing decadal trend of OA in this region, constrained by the low summertime month-to-month variability in surface OA. We hypothesize that the rest of the OA decreasing trend is largely due to a reduction in NOx emissions. By implementing a scheme for monoterpene SOA with enhanced sensitivity to NOx, our model can reproduce the decadal trend and variability in OA in this region. Extending to a centennial scale, our model shows that global SOA production increases by 36 % despite BVOC reductions from the preindustrial period to the present day, largely amplified by AIBS. Our work suggests a strong coupling between anthropogenic and biogenic emissions in biogenic SOA production that is missing from current climate models.
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Univ Calif Berkeley, Dept Civil & Environm Engn, Berkeley, CA 94720 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Franklin, Emily B.
Amiri, Sarah
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Univ Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Amiri, Sarah
Crocker, Daniel
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Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Crocker, Daniel
Morris, Clare
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Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Morris, Clare
Mayer, Kathryn
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Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Mayer, Kathryn
Sauer, Jonathan S.
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Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Sauer, Jonathan S.
Weber, Robert J.
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Univ Calif Berkeley, Dept Environm Sci Policy & Management, Berkeley, CA 94720 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Weber, Robert J.
Lee, Christopher
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Univ Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Lee, Christopher
Malfatti, Francesca
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Univ Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Univ Trieste, Dept Life Sci, I-34100 Trieste, ItalyUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Malfatti, Francesca
Cappa, Christopher D.
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Univ Calif Davis, Dept Civil & Environm Engn, Davis, CA 95616 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Cappa, Christopher D.
Bertram, Timothy H.
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Univ Wisconsin, Dept Chem, Madison, WI 53706 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Bertram, Timothy H.
Prather, Kimberly A.
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Univ Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
Prather, Kimberly A.
Goldstein, Allen H.
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Univ Calif Berkeley, Dept Environm Sci Policy & Management, Berkeley, CA 94720 USA
Univ Calif Berkeley, Dept Civil & Environm Engn, Berkeley, CA 94720 USAUniv Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA
机构:
US EPA, Natl Exposure Res Lab, Human Exposure Atmospher Sci Div, Res Triangle Pk, NC 27711 USAUS EPA, Natl Exposure Res Lab, Human Exposure Atmospher Sci Div, Res Triangle Pk, NC 27711 USA
Offenberg, John H.
Lewandowski, Michael
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US EPA, Natl Exposure Res Lab, Human Exposure Atmospher Sci Div, Res Triangle Pk, NC 27711 USAUS EPA, Natl Exposure Res Lab, Human Exposure Atmospher Sci Div, Res Triangle Pk, NC 27711 USA
Lewandowski, Michael
Edney, Edward O.
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US EPA, Natl Exposure Res Lab, Human Exposure Atmospher Sci Div, Res Triangle Pk, NC 27711 USAUS EPA, Natl Exposure Res Lab, Human Exposure Atmospher Sci Div, Res Triangle Pk, NC 27711 USA
Edney, Edward O.
Kleindienst, Tadeusz E.
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US EPA, Natl Exposure Res Lab, Human Exposure Atmospher Sci Div, Res Triangle Pk, NC 27711 USAUS EPA, Natl Exposure Res Lab, Human Exposure Atmospher Sci Div, Res Triangle Pk, NC 27711 USA
Kleindienst, Tadeusz E.
Jaoui, Mohammed
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Alion Sci & Technol, Res Triangle Pk, NC 27709 USAUS EPA, Natl Exposure Res Lab, Human Exposure Atmospher Sci Div, Res Triangle Pk, NC 27711 USA