Inverse modeling of long-term CO emission in China with Green s function method and forward sensitivity

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Inverse modeling of long-term CO emission in China with Green s function method and forward sensitivity Keiya YUMIMOTO Meteorological Research Institute (MRI), Japan Meteorological Agency, Japan Itsushi UNO Research Institute for Applied Mechanics, Kyushu University, Japan

1. Introduction Emission Inventory INPUT CTM Kurokawa et al. 2013 statistics and emission factors etc. events and time variations (biomass burning and socioeconomic conditions etc.) Uncertainties ±70% (CO), ±31% (NOx), ±208% (BC), ±258% (OC) Zhang et al. 2009 Inverse Estimate interactive (Top-down) (with observations and model) compensating

2. Inversion Methods Species CO CO2 NOx Methane aerosols Spacial Resolution Time Period (Time Resolution) Observation Method regional Heald et al., 2004 Fotems-Cheiney et al., 2011 Arellano et al., 2004 Wang et al., 2004 gridded Yumimoto and Uno, 2006 Stabrakou and Müller, 2006 Kopacz et al., 2010 month year years Yumimoto and Uno, 2006 Tanimoto et al., 2008 Stabrakou and Müller, 2006 Kopacz et al., 2010 Arellano et al., 2004 Tanimoto et al., 2008 monthly daily diurnal Fotems-Cheiney et al., 2011 in-situ air craft satellite Yumimoto and Uno, 2006 Tanimoto et al., 2008 Forward Wang et al., 2004 Arellano et al., 2004 Heald et al., 2004 Wang et al., 2004 Stabrakou and Müller, 2006 Adjoint (Backward) Yumimoto and Uno, 2006 Tanimoto et al., 2008 Kopacz et al., 2010 Arellano et al., 2004 Fotems-Cheiney et al., 2011 Stabrakou and Müller, 2006 Kopacz et al., 2010 Fotems-Cheiney et al., 2011

2. Inversion Methods Forward Adjoint (Backward) Source Receptor Source Receptor (emission) (observation) (emission) (observation) Forward method calculates sensitivities of sources (emissions) to receptors (measured concentrations). We need ensemble simulation for each source. Backward method calculates sensitivities of receptors (observations) to sources (emissions). We need adjoint of the forward model.

2. Inversion Methods In this study... Green s Function method MOPITT/TERRA CO measurement Information Constraint Forward Sensitivity GEOS-Chem Chemical Transport Model Inversely optimized CO emission China emission Recent 6 years (2005 2010) Vertical profiles Tagged simulation

2. Inversion Methods Species CO CO2 NOx Methane aerosols Spacial Resolution Time Period (Time Resolution) Observation Method regional Heald et al., 2004 Fotems-Cheiney et al., 2011 Arellano et al., 2004 Wang et al., 2004 gridded Yumimoto and Uno, 2006 Stabrakov and Müller, 2006 Kopacz et al., 2010 month year years Yumimoto and Uno, 2006 Tanimoto et al., 2008 Stabrakov and Müller, 2006 Kopacz et al., 2010 Arellano et al., 2004 Tanimoto et al., 2008 monthly daily diurnal Fotems-Cheiney et al., 2011 in-situ air craft satellite Yumimoto and Uno, 2006 Tanimoto et al., 2008 Forward Wang et al., 2004 Arellano et al., 2004 Heald et al., 2004 Wang et al., 2004 Stabrakov and Müller, 2006 Adjoint (Backward) Yumimoto and Uno, 2006 Tanimoto et al., 2008 Kopacz et al., 2010 Arellano et al., 2004 Fotems-Cheiney et al., 2011 Stabrakov and Müller, 2006 Kopacz et al., 2010 Fotems-Cheiney et al., 2011

3. Method (Green s Function Method) Observation Model Menemenlis et al., 2005 Yumimoto and Uno., 2012 y o = Hi[x t ] + ε (1) y o : observation, ε: noise process x t (ti+1) = Mi[x t (ti), η] (2) x t : true state, η: control parameter Convolution y o = G(η) + ε G: convolution of H and M = G(0) + Gη + ε (3) assuming G is linear G: Green s function matrix, forward sensitivity jth column vector of G: g j = G(e j ) G(0) e j miss-fit between observations and model d = y o - G(0) = Gη + ε

3. Method (Green s Function Method) miss-fit between observations and model d = y o - G(0) = Gη + ε (4) Menemenlis et al., 2005, MWR Cost function (to be minimized) J = η T Q -1 η + ε T R -1 ε (5) Solution η a = (Q + G T R -1 G) -1 G T R -1 d (6) We set η as scaling factor for emissions E a = (1 + η a )E f (7) a posteriori a priori

4. Experiment Setting Model (Chemical Transport Model; CTM) GEOS-Chem v9-01-01 GEOS5 Met. fields a priori (base) emission FF (Fossil Fuel): EDGAR (2005) BF (Bio-Fuel) : Yevich and Logan (2003) BB (Biomass Burning): Duncan et al. (2003) = 117.8 Tg/year from China Tagged CO simulation calculate Green s function matrix by one integration 11 geographical tagged region 4 tags (regions) in China emissions from the 11 geographical regions are inversely optimized

4. Experiment Setting Observation (Constraint) MOPITT CO profile (V4) on board TERRA satellite 10:30 Local Time over 10-year continuous observation (2-month lack in Aug. and Sep. 2009) 200501 @ surface 200501 @ 700hPa Monthly-averaged CO distribution from MOPITT

4. Experiment Setting Observation (Constraint) MOPITT CO profile (V4) on board TERRA satellite 10:30 Local Time over 10-year continuous observation (2-month lack in Aug. and Sep. 2009) the highest sensitivity at 700 hpa Example of averaging kernels of 1000, 900, 800, 700 and 600 hpa.

4. Experiment Setting Observation (Constraint) MOPITT CO profile (V4) on board TERRA satellite 10:30 Local Time over 10-year continuous observation (2-month lack in Aug. and Sep. 2009) the highest sensitivity at 700 hpa We use MOPITT measurements monthly-averaged measured at 4 vertical levels (surface, 900, 800, 700 hpa) corrected assuming 5% positive bias (Kopacz et al., 2009) through averaging kernel (H includes operation of AK) 25,000 30,000 data/month used in the inversion MOPITT data region used in the inversion

4. Experiment Setting Global 2x2.5 11 regional tags a priori = EDGAR MOPITT V4 TIR Only Thermal Infrared Only Product the highest sensitivity around 700 hpa lower 4 vertical levels (Surface 900, 800, 700) through averaging kernel ~30,000 data/month used Yumimoto and Uno, 2012 China Nest 0.5x0.667 MOPITT V5 TIR/NIR Thermal Infrared + Near Infrared Product additional sensitivity near surface finer China tags REAS V2 Yumimoto et al., in prep.

5. Inversion Results vs. MOPITT (ppbv, 2D-distribution, season) CO mixing ratio (ppbv) at 700 hpa from MOPITT, a priori, and a posteriori A posteriori successfully re-produce CO outflows from China to Japan

5. Inversion Results vs. MOPITT (ppbv, 2D-distribution, season) CO mixing ratio (ppbv) at 700 hpa from MOPITT, a priori, and a posteriori

5. Inversion Results vs. MOPITT (Time-Series, Statistics) ca. 20~60% 0.69~0.95 Time series of (a) monthly-averaged CO concentration and (b) statistics

5. Inversion Results vs. in-situ measurements (independent validation) Scatter plots of in-situ measurements vs. model

A posteriori emission and increment between a posteriori an d a priori Emission in central eastern China is increased. 5. Inversion Results a posteriori emission (2D-distribution, season)

5. Inversion Results a posteriori emission (2D-distribution, season) A posteriori emission and increment between a posteriori an d a priori

5. Inversion Results a posteriori emission (seasonal cycle)

5. Inversion Results a posteriori emission (seasonal cycle) Kopacz et al. 2010(Figure 2) China + Japan + Korea + part of Indea Fortems-Cheiney et al. 2011 China + Japan + Korea + south eastern Asia

5. Inversion Results a posteriori emission (annual variation)

5. Inversion Results a posteriori emission (annual variation)

6. Summary In this study, CO emissions in China are inversely optimized with Green s function method, MOPITT vertical profiles, and GEOS-Chem for the recent 6 years. We found that a posteriori emissions successfully reproduce (1) CO outflows from China to East China Sea and the Japanese archipelago in winter and spring. (2) high CO over the central eastern China region. a posteriori emissions exhibit significant variation (peak in winter- spring, bottom in summer) a posteriori Chinese CO sources range from 156.1 to 180.8 Tg/year, representing inter-annual variations due to socioeconomic conditions