Global simulation of H 2 and HD with GEOS-CHEM Heather Price 1, Lyatt Jaeglé 1, Paul Quay 2, Andrew Rice 2, and Richard Gammon 2 University of Washington, Seattle Departments of 1 Atmospheric Sciences and 2 Oceanography 2 nd GEOS-CHEM Users Meeting 6 Apr 2005
Sinks (Tg/yr) MOZART Novelli GEOS-CHEM OH c Soils c Total Sources (Tg/yr) MOZART a Novelli c GEOS-CHEM d Hauglustaine Fossil Fuel 16 15±10 20 Biomass Burning 13 16±5 10 Biofuel 5 b 4.4 Photochemical Methane Oxidation 26 ± 9 27 BVOC Oxidation 14 ± 7 14 Ocean 5 3 ± 2 ~ N fixation 5 3 ± 1 ~ Total a Hauglustaine et al., 2002; Photochemical production includes Methane(27.5Tg) and nonmethane hydrocarbons (14.2Tg): Isoprene, Acetone, Monoterpenes, and Methanol. b Andreae & Merlet, 2001: bf H 2 /CO = 0.32 per molecule c Novelli, 1999: bb H 2 /CO = 0.29, for fossil fuels Novelli uses global CO source of 500Tg/yr from Logan et al., 1981, Pacnya & Graedel, 1995 and WMO, 1995 Lifetime, years Annual Global Budget of Molecular Hydrogen in the Troposphere
H 2 and HD in the GEOS-CHEM Model Based on the GEOS-CHEM offline CO simulation v Sinks OH d H 2 + OH → H 2 O + H k = 1.5x e -2000/T SoilsUniform Deposition Velocity over land = cm/s Sources H 2 /CO (per molecule) Fossil Fuels 0.59 a Biomass Burning 0.30 c Biofuels 0.32 b Photochemical yield relative to CO Methane Oxidation 0.50 BVOC Oxidation 0.50 a Oliver et al., 1996 CO emission inventory EDGAR H 2 /CO (per molecule) = or 0.042Tg H 2 /CO b Andreae & Merlet, 2001: bf H 2 /CO = 0.32 or 0.023Tg H 2 /CO c Novelli, 1999; bb H 2 /CO= 0.30 or 0.022Tg H 2 /CO d JPL reported average of nine studies detailed in Ravishankara et al., 1981 and in excellent agreement with measurements by Talukdar et al., k
H 2 ppbv GEOS-CHEM Simulation of H 2 Surface (JJA) Surface (DJF)
Validating the GEOS-CHEM H 2 simulation against CMDL H 2 Observations CMDL sites Surface (JJA) CMDL sites H 2 ppbv Surface (DJF) (Novelli, 1999) Climate Monitoring and Diagnostics Laboratory: ftp:// /ccg/h2/flask/
Fall % Bias: R: 0.71 Summer % Bias: 0.71 R: 0.80 Winter % Bias: 1.25 R: 0.67 Spring % Bias: 0.70 R: 0.56 Latitude H 2 ppbv H 2 Interhemispheric Gradient ~40 ppbv gradient GEOS-CHEM H 2 ppbv GEOS-CHEM H 2 simulation vs. CMDL observations GEOS-CHEM model NOAA CMDL observations ( ) CMDL H 2 ppbv Spring Summer Autumn Winter Correlation (r=0.76) model-obs obs Bias: x100 = 0.45%
H 2 Seasonal Cycle Barrow (89-03) Bermuda(91-03) Mauna Loa(89-03) 40.7 S, E Model CMDL observations Ascension (89-03) Cape Grim(91-03) Palmer Station(94-03) Northern Hemisphere Southern Hemisphere H 2 ppbv Month Month S, 14.4 W Month Month Month Month H 2 ppbv N,156.6 W 32.4 N, 64.7 W19.5 N, W 64.9 S, 64.0 W
H 2 Vertical Profiles Nov 2002-Aug 2004 Park Falls, Wisc N,-90.27W H 2 (ppbv) km Poker Flat, Alaska 65.07N, W H 2 (ppbv) Sept Oct Nov March April May Cook Islands S, –159.83W H 2 (ppbv) km Soil Model Observations
Adding hydrogen isotope (HD) to the GEOS-CHEM model 1.Model development based on measured ratios of HD/H 2 for various sources, sinks, and reservoirs 2.Will give additional constraint to the H 2 budget sources and sinks 3.Determine the contributions of sources and sinks to atmospheric D and interhemispheric gradient (Gerst & Quay, 2000, 2001)
Deuterium Source & Sink Signatures Soil, fossil fuel, and biomass burning fractionation: Gerst & Quay, 2001 OH fractionation: Ehhalt et al., 1989 δD of the global Troposphere = 130 % o TermH 2 Tg/yr D% o Fossil Fuels Biomass Burning Biofuels Methane Oxidation28156 BVOC Oxidation14156 OH Sink Soil Sink
JJA D (% 0 ) SMOW H 2 ppbv Annual D Surface H 2 and D
D (% 0 vs SMOW) 1998,2002,2004 Ocean Cruise Observations Barrow Cheeka Peak DJF D Model, Surface & Cruise Observations Biofuels & Fossil Fuels
D vs. Latitude sinks D (atmos) ~40 % 0 gradient D Observational Data from Rice & Quay, 2004 and Gerst, & Quay, Additional enrichment from Stratosphere?
GEOS-CHEM captures well the H 2 and D latitudinal gradient (H 2 ~40ppbv, D~40% o ) and seasonality. Soil Sink uncertainty: incorporate soil moisture, precipitation, to better constrain soil deposition Next, help explain the D observations of stratospheric enrichment (Röckmann et al., 2003; Rahn et al., 2003) Could D measurements be used to constrain Asian biofuel emissions? Summary Biofuel + Fossil Fuel Biomass Burning Fossil Fuels DJF D