ORCID Profile
0000-0002-8283-5014
Current Organisation
University of California, Irvine
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Publisher: Copernicus GmbH
Date: 18-10-2010
Abstract: Abstract. We determine enhancement ratios for NOx, PAN, and other NOy species from boreal biomass burning using aircraft data obtained during the ARCTAS-B c aign and examine the impact of these emissions on tropospheric ozone in the Arctic. We find an initial emission factor for NOx of 1.06 g NO per kg dry matter (DM) burned, much lower than previous observations of boreal plumes, and also one third the value recommended for extratropical fires. Our analysis provides the first observational confirmation of rapid PAN formation in a boreal smoke plume, with 40% of the initial NOx emissions being converted to PAN in the first few hours after emission. We find little clear evidence for ozone formation in the boreal smoke plumes during ARCTAS-B in either aircraft or satellite observations, or in model simulations. Only a third of the smoke plumes observed by the NASA DC8 showed a correlation between ozone and CO, and ozone was depleted in the plumes as often as it was enhanced. Special observations from the Tropospheric Emission Spectrometer (TES) also show little evidence for enhanced ozone in boreal smoke plumes between 15 June and 15 July 2008. Of the 22 plumes observed by TES, only 4 showed ozone increasing within the smoke plumes, and even in those cases it was unclear that the increase was caused by fire emissions. Using the GEOS-Chem atmospheric chemistry model, we show that boreal fires during ARCTAS-B had little impact on the median ozone profile measured over Canada, and had little impact on ozone within the smoke plumes observed by TES.
Publisher: Elsevier BV
Date: 2017
DOI: 10.1016/J.SCITOTENV.2016.09.116
Abstract: Photochemical smog, characterized by high concentrations of ozone (O
Publisher: Springer Science and Business Media LLC
Date: 22-09-2013
DOI: 10.1038/NGEO1955
Publisher: American Geophysical Union (AGU)
Date: 07-03-2019
DOI: 10.1029/2018JD029151
Publisher: Copernicus GmbH
Date: 12-12-2016
Abstract: Abstract. The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr−1, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bottom-up approaches suggest larger global emissions (736 Tg CH4 yr−1, range 596–884) mostly because of larger natural emissions from in idual sources such as inland waters, natural wetlands and geological sources. Considering the atmospheric constraints on the top-down budget, it is likely that some of the in idual emissions reported by the bottom-up approaches are overestimated, leading to too large global emissions. Latitudinal data from top-down emissions indicate a predominance of tropical emissions (∼ 64 % of the global budget, 30° N) as compared to mid (∼ 32 %, 30–60° N) and high northern latitudes (∼ 4 %, 60–90° N). Top-down inversions consistently infer lower emissions in China (∼ 58 Tg CH4 yr−1, range 51–72, −14 %) and higher emissions in Africa (86 Tg CH4 yr−1, range 73–108, +19 %) than bottom-up values used as prior estimates. Overall, uncertainties for anthropogenic emissions appear smaller than those from natural sources, and the uncertainties on source categories appear larger for top-down inversions than for bottom-up inventories and models. The most important source of uncertainty on the methane budget is attributable to emissions from wetland and other inland waters. We show that the wetland extent could contribute 30–40 % on the estimated range for wetland emissions. Other priorities for improving the methane budget include the following: (i) the development of process-based models for inland-water emissions, (ii) the intensification of methane observations at local scale (flux measurements) to constrain bottom-up land surface models, and at regional scale (surface networks and satellites) to constrain top-down inversions, (iii) improvements in the estimation of atmospheric loss by OH, and (iv) improvements of the transport models integrated in top-down inversions. The data presented here can be downloaded from the Carbon Dioxide Information Analysis Center (0.3334/CDIAC/GLOBAL_METHANE_BUDGET_2016_V1.1) and the Global Carbon Project.
Publisher: Elsevier BV
Date: 11-2004
Publisher: American Geophysical Union (AGU)
Date: 04-2020
DOI: 10.1029/2019MS001882
Publisher: American Geophysical Union (AGU)
Date: 07-2023
DOI: 10.1029/2022MS003458
Abstract: Model intercomparison studies often report a large spread in simulation results, but quantifying the causes of these differences is hindered by the fact that several processes contribute to the model spread simultaneously. Here we use the Multi‐Scale Infrastructure for Chemistry and Aerosols (MUSICA) version 0 to investigate the model resolution dependencies of simulated chemical species, with a focus on the differences between global uniform grid and regional refinement grid simulations with the same modeling framework. We construct two global (ne30 [∼112 km] and ne60 [∼56 km]) and two regional refinement grids over Korea (ne30x8 [∼14 km] and ne30x16 [∼7 km]). The grid resolution can change chemical concentrations by an order of magnitude in the boundary layer, and the importance increases as the species' reactivity increases (e.g., up to 50% and 1,000% changes for ethane and xylenes, respectively). The diurnal cycle of oxidants (OH, O 3 , and NO 3 ) also varies with the grid resolution, which leads to different oxidation pathways of volatile organic compounds (e.g., the fraction of monoterpenes reacting with NO 3 in Seoul around midnight is 90% for ne30, but 65% for ne30x16). The models with high‐resolution grids usually do a better job at reproducing aircraft observations during the KORUS‐AQ c aign, but not always, implying compensating errors in the coarse grid simulations. For ex le, ozone is better reproduced by the coarse grid due to the artificial mixing of NO x . When developing new chemical mechanisms and evaluating models over urban areas, the uncertainties associated with model resolution should be considered.
Publisher: Elsevier BV
Date: 10-2007
Publisher: Copernicus GmbH
Date: 12-09-2018
DOI: 10.5194/ACP-17-11135-2017
Abstract: Abstract. Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4) budget over 2000–2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000–2012, but this increase is not linear over the 13 years. Despite differences between in idual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000–2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008–2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16–32] Tg CH4 yr−1 higher methane emissions over the period 2008–2012 compared to 2002–2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002–2006 and 2008–2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for in idual studies based on five emission sectors and find that for six in idual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13CH4. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.
Publisher: Copernicus GmbH
Date: 15-09-2017
DOI: 10.5194/ACP-17-10919-2017
Abstract: Abstract. Over the past 10 years (2005–2014), ground-level O3 in Hong Kong has consistently increased in all seasons except winter, despite the yearly reduction of its precursors, i.e. nitrogen oxides (NOx = NO + NO2), total volatile organic compounds (TVOCs), and carbon monoxide (CO). To explain the contradictory phenomena, an observation-based box model (OBM) coupled with CB05 mechanism was applied in order to understand the influence of both locally produced O3 and regional transport. The simulation of locally produced O3 showed an increasing trend in spring, a decreasing trend in autumn, and no changes in summer and winter. The O3 increase in spring was caused by the net effect of more rapid decrease in NO titration and unchanged TVOC reactivity despite decreased TVOC mixing ratios, while the decreased local O3 formation in autumn was mainly due to the reduction of aromatic VOC mixing ratios and the TVOC reactivity and much slower decrease in NO titration. However, the decreased in situ O3 formation in autumn was overridden by the regional contribution, resulting in elevated O3 observations. Furthermore, the OBM-derived relative incremental reactivity indicated that the O3 formation was VOC-limited in all seasons, and that the long-term O3 formation was more sensitive to VOCs and less to NOx and CO in the past 10 years. In addition, the OBM results found that the contributions of aromatics to O3 formation decreased in all seasons of these years, particularly in autumn, probably due to the effective control of solvent-related sources. In contrast, the contributions of alkenes increased, suggesting a continuing need to reduce traffic emissions. The findings provide updated information on photochemical pollution and its impact in Hong Kong.
No related grants have been discovered for Donald Blake.