Alkyl nitrate impacts on the NOx budget: insights from aircraft observations & GEOS-Chem
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1 Alkyl nitrate impacts on the NOx budget: insights from aircraft observations & GEOS-Chem Jenny A. Fisher University of Wollongong Elliot Atlas, University of Miami Don Blake, University of California Irvine Zitely Tzompa, Colorado State University Emily Fischer, Colorado State University Alex Turner, Harvard University th International GEOS-Chem Meeting Harvard University May 17 Thanks to NASA, ARC, NCI for funding & resources
2 Alkyl nitrates (RONO): key player in NOx budget + BVOC 1 α α RONO photolysis, oxidation aerosol uptake N export AVOC BVOC prono hydrolysis HNO 3 N deposition N deposition N deposition Fisher et al., 1
3 Alkyl nitrates (RONO): key player in NOx budget + BVOC 1 α α RONO photolysis, oxidation aerosol uptake N export AVOC BVOC prono hydrolysis HNO 3 N deposition N deposition N deposition Fisher et al., 1
4 Alkyl nitrates (RONO): key player in NOx budget + BVOC 1 α α RONO photolysis, oxidation aerosol uptake N export AVOC BVOC prono hydrolysis HNO 3 N deposition N deposition N deposition Fisher et al., 1 Goal: Quantify impact of RONO production the NOx budget.
5 C1-C3 RONO important in free troposphere Bias in simulated NOx export? isoprene + monoterpene nitrates
6 C1-C3 RONO important in free troposphere Bias in simulated NOx export? methyl + ethyl + propyl nitrates isoprene + monoterpene nitrates
7 C1-C3 RONO important in free troposphere Bias in simulated NOx export? methyl + ethyl + propyl nitrates ~5% of observed RONO above 3 km. Long lifetimes (weeks-months) Missing source of NOx to remote troposphere? isoprene + monoterpene nitrates
8 C1-C3 RONO important in free troposphere Bias in simulated NOx export? methyl + ethyl + propyl nitrates ~5% of observed RONO above 3 km. Long lifetimes (weeks-months) Missing source of NOx to remote troposphere? isoprene + monoterpene nitrates Wealth of historical aircraft data to constrain!
9 New C1-C3 RONO simulation in GEOS-Chem + BVOC 1 α α RONO photolysis, oxidation aeroso up N export Precursors: CH emissions scaled to CH flux inversion (Tzompa et al., 17) C3H emissions scaled to CH globally, NEI11x1 CH surface concentration prescribed from NOAA data Chemical Source: VOC + OH (+O) > RO RO + NO > α RONO (e.g. EtO)** (e.g. EtONO) α =.5 MeNO3; others P-T dependent Flocke et al., 199, Carter & Atkinson, 199 Losses: dry deposition (unreactive), OH, photolysis
10 New C1-C3 RONO simulation in GEOS-Chem + BVOC 1 α α RONO photolysis, oxidation aeroso up N export Precursors: CH emissions scaled to CH flux inversion (Tzompa et al., 17) C3H emissions scaled to CH globally, NEI11x1 CH surface concentration prescribed from NOAA data Chemical Source: VOC + OH (+O) > RO RO + NO > α RONO (e.g. EtO)** (e.g. EtONO) ** not just from ethane! HIPPO N. Pacific α =.5 MeNO3; others P-T dependent Flocke et al., 199, Carter & Atkinson, 199 Losses: dry deposition (unreactive), OH, photolysis
11 New C1-C3 RONO simulation in GEOS-Chem + BVOC 1 α α RONO photolysis, oxidation aeroso up N export Precursors: CH emissions scaled to CH flux inversion (Tzompa et al., 17) C3H emissions scaled to CH globally, NEI11x1 CH surface concentration prescribed from NOAA data Chemical Source: VOC + OH (+O) > RO RO + NO > α RONO (e.g. EtO)** (e.g. EtONO) α =.5 MeNO3; others P-T dependent Flocke et al., 199, Carter & Atkinson, 199 MeNO3 in the surface ocean (pm) Losses: dry deposition (unreactive), OH, photolysis Ocean exchange for MeNO3, EtNO3 3
12 Small low bias in some source regions Southeast U.S. (SEAC RS) 1 1 (AC5 (T13 (AC MeNO3 EtNO3 PrNO3 AOtitude (Nm) (13 (SSt) Central U.S. (DC3) 1 1 DC3 ( (T13 (SSt) DC3 (T (SSt) DC MeNO3 EtNO3 PrNO3 AOtitude (Nm) (13 (ppt) (T13 (ppt) (ppt)
13 General agreement in North Pacific North Pacific (HIPPO, -5N) all months, HI33_13ac ( HI33_13ac (T HI33_13ac 3513 MeNO3 EtNO3 PrNO (13 (ppt) (T13 (ppt) (ppt)
14 General agreement in North Pacific but low bias in South Pacific North Pacific (HIPPO, -5N) all months, HI33_13ac ( HI33_13ac (T HI33_13ac 3513 MeNO3 EtNO3 PrNO (13 (ppt) (T13 (ppt) South Pacific (HIPPO, -5S) all months, HI33_3ac ( (ppt) HI33_3ac 3513 MeNO3 EtNO3 PrNO (13 (SSt) (T13 (SSt) 3513 (SSt)
15 New global distributions: -5 km Methyl Nitrate (MeNO3) Ethyl Nitrate (EtNO3) Propyl Nitrate (PrNO3)
16 Implications for NOx budget? -5 km [percent] 5- km [percent] x, % x, % Ocean alkyl nitrate source: increased NOx in tropics
17 Implications for NOx budget? -5 km [percent] 5- km [percent] x, % x, % Ocean alkyl nitrate source: increased NOx in tropics Continental export: decreased NOx in outflow (below ~5 km)
18 PAN suppression due to RONO formation PAN, - km [percent] 1 1 PA1, %
19 PAN suppression due to RONO formation with mixed impacts on ozone PAN, - km [percent] O3, - km [percent] 1 1 PA1, % , % Direct RONO source from ocean increases O3 in tropical free troposphere, but RONO from continents decreases O3 in mid-latitudes export due to competition with PAN.
20
21 Airborne datasets included / planned
22 New simulation: small low bias in source regions Colorado (FRAPPE) 1 1 )5A33( (T13 )5A33( 3513 MeNO3 EtNO3 PrNO3 AOtitude (NP) (13 (ppt) (T13 (ppt) 3513 (ppt)
23 New simulation: general agreement in North Pacific North Pacific (HIPPO, -5N) all months, HI33_13ac ( HI33_13ac (T HI33_13ac 3513 MeNO3 EtNO3 PrNO (13 (ppt) (T13 (ppt) North Pacific (TRACE-P, 15-5N) NH spring, T5AC(_3 ( T5AC(_3 (T (ppt) T(XA 3513 MeNO3 EtNO3 PrNO3 AOtitude (NP) AOtitude (NP) AOtitXde (NP) (13 (ppt) (T13 (ppt) (SSt)
24 MeNO3 perhaps too low in Eq. Pacific Equatorial Pacific (HIPPO, S-N) all months, HI33_(q3ac ( HI33_(T3ac (T HI33_(q3ac 3513 MeNO3 EtNO3 PrNO (13 (ppt) (T13 (ppt) Equatorial Pacific (PEM-Tropics-B, 35S-35N) March-April (BT53ICBB ( (BT53ICBB (T (ppt) 1 1 3(BT53ICBB 3513 MeNO3 EtNO3 PrNO3 AOtitude (NP) AOtitude (NP) AOtitude (NP) (13 (SSt) (T13 (SSt) 3513 (SSt)
25 MeNO3, EtNO3 much too low in South Pacific South Pacific (HIPPO, -5S) all months, HI33_3ac ( HI33_3ac 3513 MeNO3 EtNO3 PrNO (13 (SSt) (T13 (SSt) 3513 (SSt) South Pacific (PEM-Tropics A, -7S) SH spring (_T53IC_A ( (_T53IC_A (T (_T53IC_A 3513 MeNO3 EtNO3 PrNO3 AOtitude (NP) AOtitude (NP) AOtitude (NP) (13 (SSt) (T13 (SSt) 3513 (SSt)
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