ALBERT

Description: Being the largest contributor to the global source of fossil-fuel CO2 emissions, China's emissions need to be accurately quantified and well understood. Previous studies have usually focused on the amount of national emissions and rarely discussed their spatiotemporal distributions, which are also crucial for both carbon flux and carbon management. In this study, we calculated China's CO2 emissions from fossil fuel use and industrial processes using provincial statistics and then mapped those emissions at 0.25° resolution on a monthly basis. Several key steps have been implemented to gain a better understanding of the spatiotemporal distributions, including (1) development and application of China's CO2 emission inventories using provincial statistics; (2) separate calculations of emissions from large point sources and accurate identification of their geographical locations; (3) development of 1 km × 1 km gridded population and GDP (gross domestic product) data for China from 2000 to 2009 and application of them as dynamic spatial proxies to allocate emissions; and (4) monthly variation curves of CO2 emissions from various sectors that were developed for each province and applied to our inventory. China's total CO2 emission from fossil fuels and industrial processes has increased from 3.6 billion tons in 2000 to 8.6 billion tons in 2009, which may be off by 14–18% and is enough to skew global totals. The resulting spatiotemporal distributions of our inventories also differed greatly in several ways from those derived using a national statistics and population-based approach for the various economic development levels, industrial and energy structures, and even large point emission sources within China and each province.

Description: Being the largest contributor to the global source of fossil-fuel CO2 emissions, China's emissions need to be accurately quantified and well understood. Previous studies have usually focused on the amount of national emissions and rarely discussed their spatiotemporal distributions, which are also crucial for both carbon flux and carbon management. In this study, we calculated China's CO2 emissions from fossil fuel use and industrial processes using provincial statistics and then mapped those emissions at 0.25° resolution on monthly basis. Several key steps have been implemented to gain a better understanding of the spatiotemporal distributions, including (1) development and application of China's CO2 emission inventories using provincial statistics; (2) separate calculations of emissions from large point sources and accurate identification of their geographical locations; (3) development of 1 km×1 km gridded population and GDP data for China from 2000 to 2009 and application of them as dynamic spatial proxies to allocate emissions; and (4) monthly variation curves of CO2 emissions from various sectors were developed for each province and applied to our inventory. China's total CO2 emission from fossil fuel and industrial process have increased from 3.6 billion tons in 2000 to 8.6 billion tons in 2009, which may be off by 14–18% and are enough to skew global totals. And the resulting spatiotemporal distributions of our inventories also differed greatly in several ways from those derived using national statistics and population-based approach for the various economic development levels, industrial and energy structures, and even large point emissions sources within China and each province.

Description: Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (137Cs) and xenon-133 (133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τe, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τe lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol (137Cs) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.

Description: We use the stratospheric/tropospheric chemical transport model MOZART-3 to study the distribution and transport of stratospheric O3 during the exceptionally intense stratospheric sudden warming event observed in January 2004 in the Northern polar region. A comparison between observations by the MIPAS instrument on board the ENVISAT spacecraft and model simulations shows that the evolution of the polar vortex and of planetary waves during the warming event plays an important role in controlling the spatial distribution of stratospheric ozone and the downward ozone flux in the lower stratospheric and upper tropospheric regions. Compared to the situation during the winter of 2002–2003, lower ozone concentrations were transported from the polar regions (polar vortex) to mid-latitudes, leading to exceptional large areas of low ozone concentrations outside the polar vortex and "low-ozone pockets" in the middle stratosphere. The unusually long-lasting stratospheric westward winds (easterlies) during the 2003–2004 event greatly restricted the upward propagation of planetary waves, causing the weak transport of ozone-rich air originated from low latitudes to the middle polar stratosphere (10 hPa). The restricted wave activities led to a reduced downward ozone flux from the lower stratosphere (LS) to the upper troposphere (UT), especially in East Asia. Consequently, in this region during wintertime (December and January), the column ozone between 100 and 300 hPa was about 10% lower during the 2003–2004 event compared to the situation in 2002–2003.

Description: Atmospheric hydrogen peroxide (H2O2) and organic hydroperoxides were measured from 18 to 30 July in 2006 during the PRIDE-PRD'06 campaign at Backgarden, a rural site located 48 km north of Guangzhou, a mega-city in southern China. A ground-based instrument was used as a scrubbing coil collector to sample ambient air, followed by on-site analysis by high-performance liquid chromatography (HPLC) coupled with post-column derivatization and fluorescence detection. The H2O2 mixing ratio over the 13 days ranged from below the detection limit to a maximum of 4.6 ppbv, with a mean (and standard deviation) of (1.26±1.24) ppbv during the daytime (08:00–20:00 LT). Methyl hydroperoxide (MHP), with a maximum of 0.8 ppbv and a mean (and standard deviation) of (0.28±0.10) ppbv during the daytime, was the dominant organic hydroperoxide. Other organic peroxides, including bis-hydroxymethyl hydroperoxide (BHMP), peroxyacetic acid (PAA), hydroxymethyl hydroperoxide (HMHP), 1-hydroxy-ethyl hydroperoxide (1-HEHP) and ethyl hydroperoxide (EHP), were detected occasionally. The concentration of H2O2 exhibited a pronounced diurnal variation on sunny days, with a peak mixing ratio in the afternoon (12:00–18:00 LT), but lacked an explicit diurnal cycle on cloudy days. Sometimes a second peak mixing ratio of H2O2 was observed during the evening, suggesting that H2O2 was produced by the ozonolysis of alkenes. The diurnal variation profile of MHP was, in general, consistent with that of H2O2. The estimation indicated that in the morning the H2O2 detected was formed mostly through local photochemical activity, with the rest probably attributable to vertical transport. It is notable that relatively high levels of H2O2 and MHP were found in polluted air. The unexpectedly high level of HO2 radicals detected in this region can account for the production of hydroperoxides, while the high level of NOx suppressed the formation of hydroperoxides significantly. High concentrations of hydroperoxides were detected in samples of rainwater collected in a heavy shower on 25 July when a typhoon passed through, indicating that a considerable mixing ratio of hydroperoxides, particularly MHP, resided above the upper boundary layer, which might be transported on a regional scale and further influence the redistribution of HOx and ROx radicals. It was found that hydroperoxides, in particular H2O2, play an important role in the formation of secondary sulfate in the aerosol phase, where the heterogeneous reaction might contribute substantially. A negative correlation between hydroperoxides and water-soluble organic compounds (WSOC), a considerable fraction of the secondary organic aerosol (SOA), was observed, providing field evidence for the importance of hydroperoxides in the formation of SOA found in previous laboratory studies. We suggest that hydroperoxides act as an important link between sulfate and organic aerosols, which needs further study and should be considered in current atmospheric models.

Description: Regional trans-boundary air pollution has become an important issue in the field of air pollution modeling. This paper presents the results of the implementation of the MM5-CMAQ modeling system in the Yangtze River Delta (YRD) for the months of January and July of 2004. The meteorological parameters are obtained by using the MM5 model. A new regional emission inventory with spatial and temporal allocations based on local statistical data has been developed to provide input emissions data to the MM5-CMAQ modeling system. The pollutant concentrations obtained from the MM5-CMAQ modeling system have been compared with observational data from the national air pollution monitoring network. It is found that air quality in winter in the YRD is generally worse than in summer, due mainly to unfavorable meteorological dispersion conditions. In winter the pollution transport from Northern China to the YRD reinforces the pollution caused by large local emissions. The monthly average concentration of SO2 in the YRD is 0.026 ± 0.011 mg m−3 in January and 0.017 ± 0.009 mg m−3 in July. Monthly average concentrations of NO2 in the YRD in January and July are 0.021 ± 0.009 mg m−3, and 0.014 ± 0.008 mg m−3 respectively. Visibility is also a problem, with average deciview values of 26.4 ± 2.95 dcv in winter and 17.6 ± 3.3 dcv in summer. The ozone concentration in the downtown area of a city like Zhoushan can be very high, with the highest simulated value reaching 107 ppb. Our results show that ozone and haze have become extremely important issues in the regional air quality. Thus, regional air pollution control is urgently needed to improve air quality in the YRD.

Description: Inverse modeling of CO2 satellite observations to better quantify carbon surface fluxes requires a forward model such as a chemical transport model (CTM) to relate the fluxes to the observed column concentrations. Model transport error is an important source of observational error. We investigate the potential of using CO satellite observations as additional constraints in a joint CO2–CO inversion to improve CO2 flux estimates, by exploiting the CTM transport error correlations between CO2 and CO. We estimate the error correlation globally and for different seasons by a paired-model method (comparing CTM simulations of CO2 and CO columns using different assimilated meteorological data sets for the same meteorological year) and a paired-forecast method (comparing 48- vs. 24-h CTM forecasts of CO2 and CO columns for the same forecast time). We find strong positive and negative error correlations (r2〉0.5) between CO2 and CO columns over much of the world throughout the year, and strong consistency between different methods to estimate the error correlation. Application of the averaging kernels used in the retrieval for thermal IR CO measurements weakens the correlation coefficients by 15% on average (mostly due to variability in the averaging kernels) but preserves the large-scale correlation structure. Results from a testbed inverse modeling application show that CO2–CO error correlations can indeed significantly reduce uncertainty on surface carbon fluxes in a joint CO2–CO inversion vs. a CO2–only inversion.

Description: As increasing urbanization has become a national policy priority for economic growth in China, cities have become important players in efforts to reduce carbon emissions. However, their efforts have been hampered by the lack of specific and comparable carbon emission inventories. Comprehensive carbon emission inventories for twelve Chinese cities, which present both a relatively current snapshot and also show how emissions have changed over the past several years, were developed using a bottom-up approach. Carbon emissions in most Chinese cities rose along with economic growth from 2004 to 2008. Yet per capita carbon emissions varied between the highest and lowest emitting cities by a factor of nearly 7. Average contributions of sectors to per capita emissions for all Chinese cities were 65.1% for industrial energy consumption, 10.1% for industrial processes, 10.4% for transportation, 7.7% for household energy consumption, 4.2% for commercial energy consumption and 2.5% for waste processing. However, these shares are characterized by considerable variability due to city-specific factors. The levels of per capita carbon emissions in China's cities were higher than we anticipated before comparing them with the average of ten cities in other parts of the world. This is mainly due to the major contribution of the industry sector in Chinese cities.

Description: Terrestrial carbon dioxide (CO2) flux estimates in China using atmospheric inversion method are beset with considerable uncertainties because very few atmospheric CO2 concentration measurements are available. In order to improve these estimates, nested atmospheric CO2 inversion during 2002–2008 is performed in this study using passenger aircraft-based CO2 measurements over Eurasia from the Comprehensive Observation Network for Trace gases by Airliner (CONTRAIL) project. The inversion system includes 43 regions with a focus on China, and is based on the Bayesian synthesis approach and the TM5 transport model. The terrestrial ecosystem carbon flux modeled by the Boreal Ecosystems Productivity Simulator (BEPS) model and the ocean exchange simulated by the OPA-PISCES-T model are considered as the prior fluxes. The impacts of CONTRAIL CO2 data on inverted China terrestrial carbon fluxes are quantified, the improvement of the inverted fluxes after adding CONTRAIL CO2 data are rationed against climate factors and evaluated by comparing the simulated atmospheric CO2 concentrations with three independent surface CO2 measurements in China. Results show that with the addition of CONTRAIL CO2 data, the inverted carbon sink in China increases while those in South and Southeast Asia decrease. Meanwhile, the posterior uncertainties over these regions are all reduced (2–12%). CONTRAIL CO2 data also have a large effect on the inter-annual variation of carbon sinks in China, leading to a better correlation between the carbon sink and the annual mean climate factors. Evaluations against the CO2 measurements at three sites in China also show that the CONTRAIL CO2 measurements may have improved the inversion results.

Description: Chemical and aerosol processes in the transition from closed- to open-cell circulation in the remote, cloudy marine boundary layer are explored. It has previously been shown that precipitation can initiate a transition from the closed- to the open-cellular state, but that the boundary layer cannot maintain this open-cell state without a resupply of cloud condensation nuclei (CCN). Potential sources of CCN include wind-driven production of sea salt from the ocean, nucleation from the gas phase, and entrainment from the free troposphere. In order to investigate CCN sources in the marine boundary layer and their role in supplying new particles, we have coupled in detail chemical, aerosol, and cloud processes in the WRF/Chem model, and added state-of-the-art representations of sea salt emissions and aerosol nucleation. We conduct numerical simulations of the marine boundary layer in the transition from a closed- to an open-cell state. Results are compared with observations in the Southeast Pacific boundary layer during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). The transition from the closed- to the open-cell state generates conditions that are conducive to nucleation by forming a cloud-scavenged, ultra-clean layer below the inversion base. Open cell updrafts loft dimethyl sulfide from the ocean surface into the ultra-clean layer, where it is oxidized during daytime to SO2 and subsequently to H2SO4. Low H2SO4 condensation sink values in the ultra-clean layer allow H2SO4 to rise to concentrations at which aerosol nucleation produces new aerosol in significant numbers. The existence of the ultra-clean layer is confirmed by observations. We find that the observed DMS flux from the ocean in the VOCALS-REx region can support a nucleation source of aerosol in open cells that exceeds sea salt emissions in terms of the number of particles produced. The freshly nucleated, nanometer-sized aerosol particles need, however, time to grow to sizes large enough to act as CCN. In contrast, mechanical production of particles from the ocean surface by near-surface winds provides a steady source of larger particles that are effective CCN at a rate exceeding a threshold for maintenance of open-cell circulation. Entrainment of aerosol from the free troposphere contributes significantly to boundary layer aerosol for the considered VOCALS-REx case, but less than sea salt aerosol emissions.