Department of Atmospheric Sciences, University of Washington

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Department of Atmospheric Sciences, University of Washington Wintertime emissions and chemistry over the N.E. US: Role of oxidants and heterogeneous chemistry Lyatt Jaeglé, Viral Shah, Joel Thornton, Felipe Lopez-Hilfiker, Ben Lee Department of Atmospheric Sciences, University of Washington S. Brown (NOAA), J. Jimenez (U Colorado), J. Dibb (U New Hampshire), R. Cohen (UC Berkeley), R. Weber (Georgia Tech), A. Weinheimer, T. Campos, E. Apel (NCAR), G. Wolfe (UMBC), J. DiGangi (NASA Langley), T. Hanisco (NASA GSFC) How well do we understand wintertime emissions of pollutants? How important are nocturnal & multiphase processes? What factors control aerosol formation and aerosol/gas partitioning?  Viral Shah (talk); Jessica Haskins, Kelsey Larson (posters) on Tuesday

NSF/NCAR C-130 aircraft flight tracks WINTER: Feb 3 - Mar 13 2015 NSF/NCAR C-130 aircraft flight tracks Measurements Gas-phase: NO2, NO, HNO3, N2O5, ∑PANs, ∑ANs, HONO, NOy, ClNO2, HCl, Cl2, CO, O3, SO2, NH3, CH2O, alkanes, alkenes, alkynes, CFCs, halons Aerosol composition (ToF-AMS, PILS, Filter): organic aerosol, SO42-, NH3+, NO3-, Cl-, Na+, Mg2+, Ca2+ Aerosol size distribution, actinic flux, meteorological parameters 50% of flight hours at night 71% within 1 km of the surface (3,000 feet) 13 flights SZA GEOS-Chem Model Nested grid (0.5ºx0.625º). v10-01 Scale EPA NEI 2011 to 2015: 20% reduction in NOx (2015 CEMS + 7%/yr decrease in transportation) 32% reduction in SO2 (2015 CEMS) day 50% of flights hours at night 71% within 1 km of the surface

Vertical profiles over land Anthropogenic emissions NOx HCHO 50 40 30 20 10 5 4 3 2 1 NOx emissions 58% transportation 29% stationary FF 13% industry HCHO emissions 60% transportation 28% stationary FF 12% industry change (%) ∆HO2 Impact on oxidants 5xHCHO + ClNO2 chemistry 40-80% increase in HOx 10-20% increase in SO4= & OA 1010 atoms cm-2 s-1 Vertical profiles over land NOy HCHO observations model model 5xNEI observations model NOy within 10% of observations, but HCHO too low by x2 Increase NEI HCHO emissions by x5 (cold-start OVOC emissions?)

NOy partitioning during WINTER NOy partitioning (<1km) Nighttime NOz (NOy-NOx) PNs ANs N2O5 HNO3 ClNO2 HONO Obs Model means for all flights HNO3 N2O5 ANs PNs NOx Obs Model ANs = RONO2 PNs = RO2NO2 Model HNO3 too high x4 [Zhang et al., 2012; Heald et al, 2012] Model N2O5 too low by x4  Problem with ɣ(N2O5)? GEOS-Chem [Evans & Jacob, 2005]: ɣ(N2O5) = f(RH, aerosol, T)~0.02

Update ɣ(N2O5) to more recent lab obs ɣ(N2O5) – inhibited by nitrate and organics SO4=-NO3--NH4+ aerosol ɣ = f(H2O, NO3-, Cl-) [Bertram & Thornton, 2009] Organic aerosol ɣ = 0.0001 (RH<50%), 0.001 (RH>50%) [Badger et al., 2006] ClNO2 yield, 𝝓 SO4=-NO3--NH4+ aerosol 𝝓 = f(H2O, Cl-) [Bertram & Thornton, 2009] Sea salt 𝝓=1, other aerosol 𝝓=0 New ɣ(N2O5) New 𝝓(ClNO2) ɣ(N2O5)<0.01 𝝓 <0.2 ɣ(N2O5)>0.02 𝝓 =1 Feb-Mar surface

Improved NOy partitioning HNO3 + pNO3 Nighttime NOz (NOy-NOx) (<1 km) observations model model, new ɣN2O5 HNO3 model, new ɣN2O5+𝑣d HONO ClNO2 N2O5 ANs PNs Obs Model Updated model (new ɣN2O5+𝑣d) O3 observations model model, new 𝑣d New ɣ(N2O5) + Update dry deposition Surface resistance (Rc) ↑ at cold temp ~ exp(-T-4) [Wesely, 1989] Set Rc(HNO3)=0 [Wesely and Hicks, 2000]  𝑣d(HNO3)~1-4 cm s-1 Other species: limit Rc increase by x2  𝑣d(O3) increases by 40%

Summary ClNO2 NOx HNO3 Org nit. 15% 75% 10% Oxidative capacity of wintertime polluted air controlled by regional anthropogenic emissions and multiphase chemistry Nitrate + OA suppression of ɣ(N2O5) + corrected dry dep  helps address long-standing winter HNO3/nitrate overestimate problem GEOS-Chem budget (NE US 0-1km) 15% ClNO2 ClNO2 Org nit. NO2+OH 44% 75% NOx HNO3 NOx N2O5+aer 55% NOx 𝜏 =1.2d HNO3 NO3+VOC 10% Org nit.