Constraints on ship NOx emissions in Europe using GEOS-Chem and OMI satellite NO2 observations
Vinken, G.C.M. ; Boersma, K.F. ; Donkelaar, A. van; Zhang, W. - \ 2014
Atmospheric Chemistry and Physics 14 (2014). - ISSN 1680-7316 - p. 1353 - 1369.
ozone monitoring instrument - nitrogen-oxide emissions - marine boundary-layer - tropospheric no2 - interannual variability - power-plants - global-model - inventories - retrieval - columns
We present a top-down ship NOx emission inventory for the Baltic Sea, the North Sea, the Bay of Biscay and the Mediterranean Sea based on satellite-observed tropospheric NO2 columns of the Ozone Monitoring Instrument (OMI) for 2005–2006. We improved the representation of ship emissions in the GEOS-Chem chemistry transport model, and compared simulated NO2 columns to consistent satellite observations. Relative differences between simulated and observed NO2 columns have been used to constrain ship emissions in four European seas (the Baltic Sea, the North Sea, the Bay of Biscay and the Mediterranean Sea) using a mass-balance approach, and accounting for nonlinear sensitivities to changing emissions in both model and satellite retrieval. These constraints are applied to 39% of total top-down European ship NOx emissions, which amount to 0.96 TgN for 2005, and 1.0 TgN for 2006 (11–15% lower than the bottom-up EMEP ship emission inventory). Our results indicate that EMEP emissions in the Mediterranean Sea are too high (by 60 %) and misplaced by up to 150 km, which can have important consequences for local air quality simulations. In the North Sea ship track, our top-down emissions amount to 0.05 TgN for 2005 (35% lower than EMEP). Increased top-down emissions were found for the Baltic Sea and the Bay of Biscay ship tracks, with totals in these tracks of 0.05 TgN (131% higher than EMEP) and 0.08 TgN for 2005 (128% higher than EMEP), respectively. Our study explicitly accounts for the (non-linear) sensitivity of satellite retrievals to changes in the a priori NO2 profiles, as satellite observations are never fully independent of model information (i.e. assumptions on vertical NO2 profiles). Our study provides for the first time a space-based, top-down ship NOx emission inventory, and can serve as a framework for future studies to constrain ship emissions using satellite NO2 observations in other seas.
Atmosphere-ocean ozone fluxes during the TexAQS 2006, STRATUS 2006, GOMECC 2007, GasEx 2008, and AMMA 2008 cruises
Helmig, D. ; Lang, E.K. ; Bariteau, L. ; Boylan, P. ; Fairall, C.W. ; Ganzeveld, L.N. ; Hare, J.E. ; Hueber, J. ; Pallandt, M. - \ 2012
Journal of Geophysical Research: Atmospheres 117 (2012). - ISSN 2169-897X - 15 p.
marine boundary-layer - dry deposition - surface - atlantic - iodine - water - coastal - parameterization - enhancement - chemistry
A ship-based eddy covariance ozone flux system was deployed to investigate the magnitude and variability of ozone surface fluxes over the open ocean. The flux experiments were conducted on five cruises on board the NOAA research vessel Ronald Brown during 2006-2008. The cruises covered the Gulf of Mexico, the southern as well as northern Atlantic, the Southern Ocean, and the persistent stratus cloud region off Chile in the eastern Pacific Ocean. These experiments resulted in the first ship-borne open-ocean ozone flux measurement records. The median of 10 min oceanic ozone deposition velocity (v(d)) results from a combined similar to 1700 h of observations ranged from 0.009 to 0.034 cm s(-1). For the Gulf of Mexico cruise (Texas Air Quality Study (TexAQS)) the median v(d) (interquartile range) was 0.034 (0.009-0.065) cm s(-1) (total number of 10 min measurement intervals, N-f = 1953). For the STRATUS cruise off the Chilean coast, the median v(d) was 0.009 (0.004-0.037) cm s(-1) (N-f = 1336). For the cruise from the Gulf of Mexico and up the eastern U. S. coast (Gulf of Mexico and East Coast Carbon cruise (GOMECC)) a combined value of 0.018 (0.006-0.045) cm s(-1) (N-f = 1784) was obtained (from 0.019 (-0.014-0.043) cm s(-1), N-f = 663 in the Gulf of Mexico, and 0.018 (-0.004-0.045) cm s(-1), N-f = 1121 in the North Atlantic region). The Southern Ocean Gas Exchange Experiment (GasEx) and African Monsoon Multidisciplinary Analysis (AMMA), the Southern Ocean and northeastern Atlantic cruises, respectively, resulted in median ozone v(d) of 0.009 (-0.005-0.026) cm s(-1) (N-f = 2745) and 0.020 (-0.003-0.044) cms(-1) (N-f = 1147). These directly measured ozone deposition values are at the lower end of previously reported data in the literature (0.01-0.12 cm s(-1)) for ocean water. Data illustrate a positive correlation (increase) of the oceanic ozone uptake rate with wind speed, albeit the behavior of the relationship appears to differ during these cruises. The encountered wide range of meteorological and ocean biogeochemical conditions is used to investigate fundamental drivers of oceanic O-3 deposition and for the evaluation of a recently developed global oceanic O-3 deposition modeling system.
Atmosphere-Ocean Ozone Exchange – A Global Modeling Study of Biogeochemical, Atmospheric and Water-Side Turbulence Dependencies
Ganzeveld, L.N. ; Helmig, D. ; Fairall, C.W. ; Hare, J. ; Pozzer, A. - \ 2009
Global Biogeochemical Cycles 23 (2009). - ISSN 0886-6236 - 16 p.
general-circulation model - dry deposition parameterization - marine boundary-layer - nonmethane hydrocarbons - iodide distribution - tropospheric ozone - dissolved iodine - aqueous-solution - south atlantic - technical note
The significance of the removal of tropospheric ozone by the oceans, covering ~2/3 of the Earth's surface, has only been addressed in a few studies involving water tank, aircraft, and tower flux measurements. On the basis of results from these few observations of the ozone dry deposition velocity (VdO3), atmospheric chemistry models generally apply an empirical, constant ocean uptake rate of 0.05 cm s-1. This value is substantially smaller than the atmospheric turbulent transport velocity for ozone. On the other hand, the uptake is higher than expected from the solubility of ozone in clean water alone, suggesting that there is an enhancement in oceanic ozone uptake, e.g., through a chemical destruction mechanism. We present an evaluation of a global-scale analysis with a new mechanistic representation of atmosphere-ocean ozone exchange. The applied atmosphere chemistry-climate model includes not only atmospheric but also waterside turbulence and the role of waterside chemical loss processes as a function of oceanic biogeochemistry. The simulations suggest a larger role of biogeochemistry in tropical and subtropical ozone oceanic uptake with a relative small temporal variability, whereas in midlatitude and high-latitude regions, highly variable ozone uptake rates are expected because of the stronger influence of waterside turbulence. Despite a relatively large range in the explicitly calculated ocean uptake rate, there is a surprisingly small sensitivity of simulated Marine Boundary Layer ozone concentrations compared to the sensitivity for the commonly applied constant ocean uptake approach. This small sensitivity points at compensating effects through inclusion of the process-based ocean uptake mechanisms to consider variability in oceanic O3 deposition consistent with that in atmospheric and oceanic physical, chemical, and biological processes