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We investigated the influence of long-range transboundary transport (LRTT) on the aerosol concentrations in the Korean peninsula using the ground- and satellite-based remote sensing with back-trajectory calculations during the Korea-United States Air Quality (KORUS-AQ) campaign. Specifically, aerosol optical depth (AOD) observations from a geostationary satellite can directly provide the progression and evolution of aerosol plume transport. During high pollution cases in western Korea, we found the AOD enhancement over the Yellow Sea and east-central China, at maximum >200% over the pathway of LRTT compared to the mean condition. Particularly, high AOD in the Shandong peninsula appears coincidentally with the high AOD over South Korea in a day, revealing the strong influence of the east-central Chinese emission. Back-trajectory patterns remarkably capture the movement of high AOD bands detected by the geostationary satellite monitoring. LRTT cases through the inside of boundary layer at east-central China usually contribute to the high AOD in Korea, while air-masses above the boundary layer in north China and Mongolia do not much relate to the Korean pollution, showing the importance for both the direction and height of the air-mass movement. Travel speed is another significant factor to describe the LRTT effect. Despite the large effect of LRTT to both urban and rural sites in Korea, sometimes urban sites are more affected by the domestic emission when the air-mass travels shorter than ∼250 km per day, notifying that the effect of Korean domestic emission cannot be negligible as well. Our findings reveal that usage of geostationary satellite observations enables us to better evaluate the influence of LRTT on the local air pollution.

During the Megacity Air Pollution Studies-Seoul (MAPS-Seoul) campaign from May to June 2015, aerosol optical properties in Korea were obtained based on the AERONET sunphotometer measurement at five sites (Anmyon, Gangneung_WNU, Gosan_SNU, Hankuk_UFS, and Yonsei_University). Using this dataset, we examine regional aerosol types by applying a number of known aerosol classification methods. We thoroughly utilize five different methods to categorize the regional aerosol types and evaluate the results from each method by inter-comparison. The differences and similarities among the results are also discussed, contingent upon the usage of AERONET inversion products, such as the single scattering albedo. Despite several small differences, all five methods suggest the same general features in terms of the regionally dominant aerosol type: Fine-mode aerosols with highly absorbing radiative properties dominate at Hankuk_UFS and Yonsei_University; non-absorbing fine-mode particles form a large portion of the aerosol at Gosan_SNU; and coarse-mode particles cause some effects at Anmyon. The analysis of 3-day back-trajectories is also performed to determine the relationship between classified types at each site and the regional transport pattern. In particular, the spatiotemporally short-scale transport appears to have a large influence on the local aerosol properties. As a result, we find that the domestic emission in Korea significantly contributes to the high dominance of radiation-absorbing aerosols in the Seoul metropolitan area and the air-mass transport from China largely affects the western coastal sites, such as Anmyon and Gosan_SNU.

In this study, we present and compare regional correlations between CO total column density (TCD CO ) from the data set of Measurement of Pollution in the Troposphere (MOPITT), and high-absorbing BC dominant aerosol optical depth (AOD BC ) from the retrieval algorithm using Moderate Resolution Imaging Spectroradiometer (MODIS) and Ozone Monitoring Instrument (OMI) (MODIS-OMI algorithm, MOA). TCD CO shows positive relationship to both fine-mode AOD (AOD FM ) and AOD BC in general, but TCD CO better correlates with AOD BC than AOD FM . This enhanced correlation between TCD CO and AOD BC appears more clearly during spring and summer. Correlation between TCD CO and AOD BC is exceptionally poor in Northern Africa where the BC-dominated aerosols are frequently mixed with mineral dust particles from the Sahara. Another issue is also found in Southern Africa; the correlation between AOD BC and TCD CO in this region is not much higher than that between the AOD FM and TCD CO in spite of large occurrence of biomass burning and wildfire. This can be explained by the cloud perturbation near the source regions and dispersion effect due to the typical wind pattern. Correlations between AOD BC and TCD CO increase further when fire detected areas are only considered, but does not change much over the urban area. This difference clarifies the large contribution of burning events to the positive relationship between BC and CO. All findings in this study demonstrate a possible use of satellite CO product in evaluating the BC-dominated aerosol product from satellite remote sensing over the globe.

Springtime trans-Pacific transport of Asian air pollutants has been investigated in many ways to figure out its mechanism. Based on the Western Pacific (WP) pattern, one of climate variabilities in the Northern Hemisphere known to be associated with the pattern of atmospheric circulation over the North Pacific Ocean, in this study, we characterize the pattern of springtime trans-Pacific transport using long-term satellite measurements and reanalysis datasets. A positive WP pattern is characterized by intensification of the dipole structure between the northern Aleutian Low and the southern Pacific High over the North Pacific. The TOMS/OMI Aerosol Index (AI) and MOPITT CO show the enhancement of Asian pollutant transport across the Pacific during periods of positive WP pattern, particularly between 40 and 50°N. This enhancement is confirmed by high correlations of WP index with AI and CO between 40 and 50°N. To evaluate the influence of the WP pattern, we examine several cases of trans-Pacific transport reported in previous research. Interestingly, most trans-Pacific transport cases are associated with the positive WP pattern. During the period of negative WP pattern, reinforced cyclonic wave breaking is consistently found over the western North Pacific, which obstructs zonal advection across the North Pacific. However, some cases show the trans-Pacific transport of CO in the period of negative WP pattern, implying that the WP pattern is more influential on the transport of particles mostly emitted near ∼40°N. This study reveals that the WP pattern can be utilized to diagnose the strength of air pollutant transport from East Asia to North America.

Absorption and scattering characteristics of various aerosol events are investigated using 2-years of measurements from a skyradiometer at Yonsei University in Seoul, Korea. Both transported dust and anthropogenic aerosols are observed at distinct geo-location of Seoul, a megacity located a few thousand kilometers away from dust source regions in China. We focus on the wavelength dependence of Angstrom exponent (AE) and single scattering albedo (SSA), showing the characteristics of regional aerosols. The correlation between spectral SSAs and AEs calculated using different wavelength pairs generally indicates relatively weak absorption of fine-mode aerosols (urban pollution and/or biomass burning) and strong absorption of coarse-mode aerosols (desert dust) at this location. AE ratio (AER), a ratio of AEs calculated using wavelength pair between shorter (340–675 nm) and longer wavelength pair (675–1020 nm) correlates differently with SSA according to the dominant size of local aerosols. Correlations between SSA and AER show strong absorption of aerosols for AER 2.0. Based on the seasonal pattern of wavelength dependence of AER and SSA, this correlation difference looks to reveal the separated characteristics of transported dust and anthropogenic particles from urban pollution respectively. The seasonal characteristics of AER and SSAs also show that the skyradiometer measurement with multiple wavelengths may be able to detect the water soluble brown carbon, one of the important secondary organic aerosols in the summertime atmospheric composition.

Quantifying the spectral variation of column aerosol absorption in the ultraviolet (UV) and visible (Vis) wavelengths is required for accurate satellite-based aerosol and trace-gas retrievals. Retrievals of the column-averaged imaginary part of refractive index and single scattering albedo (SSA) in the UV–Vis range have been performed at Yonsei University, Seoul, Korea, since 2016 by combining co-located measurements from the NASA Aerosol Robotic Network (AERONET) Cimel sun-sky photometer, the Ultraviolet Multifilter Rotating Shadowband Radiometer (UV-MFRSR), the SKYNET Prede sky radiometer, and the NASA Pandora sun spectrometer. We investigated the spectral variation of column-averaged imaginary part of refractive index for UV–Vis wavelengths to refine models used in our aerosol retrieval algorithm to process measurements from the upcoming Geostationary Environment Monitoring Satellite (GEMS). The retrieved imaginary part of refractive index for highly absorbing fine pollution particles (BC), dust (DS), and non-absorbing (NA) particles in the selected UV–Vis range (380–440 nm) showed 0–20%, 30%, and 0–40% of spectral dependence, respectively. Retrievals of Ozone Monitoring Instrument (OMI) measurement data using the improved aerosol model showed improved correlation with AERONET data compared to the old algorithm that did not properly account for aerosol absorption effects. These results corroborate the advantage of using local climatology derived from ground-based UV–Vis spectral aerosol absorption measurements for satellite GEMS aerosol retrievals over East Asia. Moreover, this study reveals that spectral variations in the UV column aerosol absorption in East Asia differ from those in other regions.

This investigation examines aerosol dynamics during major fine mode aerosol transboundary pollution events in South Korea primarily during the KORUS-AQ campaign from May 1 – June 10, 2016, particularly when cloud fraction was high and/or fog was present to quantify the change in aerosol characteristics due to near-cloud or fog interaction. We analyze the new AERONET Version 3 data that have significant changes to cloud screening algorithms, allowing many more fine-mode observations in the near vicinity of clouds or fog. Case studies for detailed investigation include May 25–26, 2016 when cloud fraction was high over much of the peninsula, associated with a weak frontal passage and advection of pollution from China. These cloud-influenced Chinese transport dates also had the highest aerosol optical depth (AOD), surface PM2.5 concentrations and fine mode particle sizes of the entire campaign. Another likewise cloud/high relative humidity (RH) case is June 9 and 10, 2016 when fog was present over the Yellow Sea that appears to have affected aerosol properties well downwind over the Korean peninsula. In comparison we also investigated aerosol properties on air stagnation days with very low cloud cover and relatively low RH (May 17 & 18, 2016), when local Korean emissions dominated. Aerosol volume size distributions show marked differences between the transport days (with high RH and cloud influences) and the local pollution stagnation days, with total column-integrated particle fine mode volume being an order of magnitude greater on the pollution transport dates. The PM2.5 over central Seoul were significantly greater than for coastal sites on the transboundary transport days yet not on stagnation days, suggesting additional particle formation from gaseous urban emissions in cloud/fog droplets and/or in the high RH humidified aerosol environment. Many days had KORUS-AQ research aircraft flights that provided observations of aerosol absorption, particle chemistry and vertical profiles of extinction. AERONET retrievals and aircraft in situ measurements both showed high single scattering albedo (weak absorption) on the cloudy or cloud influenced days, plus aircraft profile in situ measurements showed large AOD enhancements (versus dried aerosol) at ambient relative humidity (RH) on the pollution transport days, consistent with the significantly larger fine mode particle radii and weak absorption.

We investigate the effects of aerosol peak height (APH) and various parameters on the air mass factor (AMF) for SO2 retrieval. Increasing aerosol optical depth (AOD) leads to multiple scattering within the planetary boundary layer (PBL) and an increase in PBL SO2 AMF. However, under high AOD conditions, aerosol shielding effects dominate, which causes the PBL SO2 AMF to decrease with increasing AOD. The height of the SO2 layer and the APH are found to significantly influence the PBL SO2 AMF under high AOD conditions. When the SO2 and aerosol layers are of the same height, aerosol multiple scattering occurs dominantly within the PBL, which leads to an increase in the PBL SO2 AMF. When the APH is greater than the SO2 layer height, aerosol shielding effects dominate, which decreases the PBL SO2 AMF. When the SO2 and aerosol layers are of the same height under low AOD and solar zenith angle (SZA) conditions, increased surface reflectance is found to significantly increase the PBL SO2 AMF. However, high AOD dominates the surface reflectance contribution to PBL SO2 AMF. Under high SZA conditions, Rayleigh scattering contributes to a reduction in the light path length and PBL SO2 AMF. For volcanic SO2 AMF, high SZA enhances the light path length within the volcanic SO2 layer, as well as the volcanic SO2 AMF, because of the negligible photon loss by Rayleigh scattering at high altitudes. High aerosol loading and an APH that is greater than the SO2 peak height lead to aerosol shielding effects, which reduce the volcanic SO2 AMF. The SO2 AMF errors are also quantified as a function of uncertainty in the input data of AOD, APH, and surface reflectance. The SO2 AMF sensitivities and error analysis provided here can be used to develop effective error reduction strategies for satellite-based SO2 retrievals.

The Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) instrument is an airborne hyperspectral spectrometer measuring backscattered solar radiation in the ultraviolet (290–400 nm) and visible (415–695 nm) wavelength regions. This paper presents high-resolution sulfur dioxide (SO2) maps over the Korean Peninsula, produced by SO2 retrievals from GeoTASO measurements during the Korea–United States Air Quality Field Study (KORUS-AQ) from May to June 2016. The highly sensitive GeoTASO instrument with a spatial resolution of ~250 m × 250 m can detect point emission sources of SO2 within its fields of view, even without merging multiple overlapping observations. To retrieve SO2 vertical columns from the GeoTASO measurements, we apply an algorithm based on principal component analysis (PCA), which is effective in suppressing noise and biases in SO2 retrievals. The retrievals successfully capture SO2 plumes and various point sources such as power plants, a petrochemical complex, and a steel mill, located in South Chungcheong Province, some of which are not detected by a ground-based in situ measurement network. Spatial distributions of SO2 from GeoTASO observations in source areas are consistent with those from the Stack Tele-Monitoring System reports and airborne in situ SO2 measurements. Comparisons of SO2 retrievals from GeoTASO and existing satellite sensors demonstrate the significance of high-resolution SO2 observations, by indicating that GeoTASO detects small SO2 emission sources that are not precisely resolved by single overpasses of satellites. To assess future geostationary SO2 observations having a higher spatial resolution, we upscale the GeoTASO SO2 retrievals to a spatial resolution of the Geostationary Environment Monitoring Spectrometer (GEMS). Since the upscaled GeoTASO retrievals also detect SO2 plumes clearly, we expect from GEMS to identify even small SO2 emission sources over Asia.

Analysis of sun photometer measured and satellite retrieved aerosol optical depth (AOD) data has shown that major aerosol pollution events with very high fine mode AOD (>1.0 in mid-visible) in the China/Korea/Japan region are often observed to be associated with significant cloud cover. This makes remote sensing of these events difficult even for high temporal resolution sun photometer measurements. Possible physical mechanisms for these events that have high AOD include a combination of aerosol humidification, cloud processing, and meteorological co-variation with atmospheric stability and convergence. The new development of Aerosol Robotic network (AERONET) Version 3 Level 2 AOD with improved cloud screening algorithms now allow for unprecedented ability to monitor these extreme fine mode pollution events. Further, the Spectral Deconvolution Algorithm (SDA) applied to Level 1 data (L1; no cloud screening) provides an even more comprehensive assessment of fine mode AOD than L2 in current and previous data versions. Studying the 2012 winter-summer period, comparisons of AERONET L1 SDA daily average fine mode AOD data showed that Moderate Resolution Imaging Spectroradiometer (MODIS) satellite remote sensing of AOD often did not retrieve and/or identify some of the highest fine mode AOD events in this region. Also, compared to models that include data assimilation of satellite retrieved AOD, the L1 SDA fine mode AOD was significantly higher in magnitude, particularly for the highest AOD events that were often associated with significant cloudiness.

Quantifying the aerosol absorption at ultraviolet (UV) wavelengths is important for monitoring air pollution using current (e.g., Aura/OMI) and future (e.g., TROPOMI, TEMPO, GEMS, and Sentinel-4) satellite measurements. Measurements of column atmospheric aerosol absorption (i.e., column effective imaginary refractive index (k), single scattering albedo (SSA), and aerosol absorption optical depth (AAOD)) are performed on the ground by the NASA AERONET in the visible (VIS) and near-infrared (NIR) wavelengths and in the UV-VIS-NIR by the SKYNET networks. Previous comparison studies have focused on visible and NIR wavelengths due to the lack of co-incident measurements of aerosol and gaseous absorption properties in the UV. This study compares the SKYNET-retrieved SSA in the UV with the SSA derived from a combination of AERONET, MFRSR, and Pandora (AMP) retrievals in Seoul, South Korea in spring and summer of 2016. The results show that the spectrally invariant surface albedo assumed in the SKYNET SSA retrievals leads to underestimated SSA compared to AMP values at near UV wavelengths. Re-processed SKYNET inversions using spectrally varying surface albedo, consistent with the AERONET retrieval improves agreement with AMP SSA. The combined AMP inversions allow for separating aerosol and gaseous (NO2 and O3) absorption and provides aerosol retrievals from the shortest UVB (305 nm) through visible to NIR wavelengths (870 nm).

Arctic ozone depletion events (ODEs) are caused by halogen catalyzed ozone loss. In situ chemistry, advection of ozone-poor air mass, and vertical mixing in the lower troposphere are important factors affecting ODEs. To better characterize the ODEs, we analyze the combined set of surface, ozonesonde, and aircraft in situ measurements of ozone and bromine compounds during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS), the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC), and the Arctic Intensive Ozonesonde Network Study (ARCIONS) experiments (April 2008). Tropospheric BrO columns retrieved from satellite measurements and back trajectory calculations are also used to investigate the characteristics of observed ODEs. In situ observations from these field experiments are inadequate to validate tropospheric BrO columns derived from satellite measurements. In view of this difficulty, we construct an ensemble of tropospheric column BrO estimates from two satellite (OMI and GOME-2) measurements and with three independent methods of calculating stratospheric BrO columns. Furthermore, we select analysis methods that do not depend on the absolute magnitude of column BrO, such as time-lagged correlation analysis of ozone and tropospheric column BrO, to understand characteristics of ODEs. Time-lagged correlation analysis between in situ (surface and ozonesonde) measurements of ozone and satellite derived tropospheric BrO columns indicates that the ODEs are due to either local halogen-driven ozone loss or short-range (∼1 day) transport from nearby regions with ozone depletion. The effect of in situ ozone loss is also evident in the diurnal variation difference between low (10th and 25th percentiles) and higher percentiles of surface ozone concentrations at Alert, Canada. Aircraft observations indicate low-ozone air mass transported from adjacent high-BrO regions. Correlation analyses of ozone with potential temperature and time-lagged tropospheric BrO column show that the vertical extent of local ozone loss is surprisingly deep (1–2 km) at Resolute and Churchill, Canada. The unstable boundary layer during ODEs at Churchill could potentially provide a source of free-tropospheric BrO through convective transport and explain the significant negative correlation between free-tropospheric ozone and tropospheric BrO column at this site.

As a part of the IGAC (International Global Atmospheric Chemistry) Mega-cities program, aerosol physical and optical properties were continuously measured from March 2007 to March 2008 at an urban site (37.57° N, 126.94° E) in Seoul, Korea. Spectral optical properties of long-range transported Asian dust and pollution aerosols have been investigated based on the year long measurement data. Optically measured black carbon/thermally measured elemental carbon (BC/EC) ratio showed clear monthly variation with high values in summer and low values in winter mainly due to the enhancement of light attenuation by the internal mixing of EC. Novel approach has been suggested to retrieve the spectral light absorption coefficient (babs) from Aethalometer raw data by using BC/EC ratio. Mass absorption efficiency, σabs (=babs/EC) at 550 nm was determined to be 9.0±1.3, 8.9±1.5, 9.5±2.0, and 10.3±1.7 m2 g−1 in spring, summer, fall, and winter, respectively with an annual mean of 9.4±1.8 m2 g−1. Threshold values to classify severe haze events were suggested in this study. Increasing trend of aerosol single scattering albedo (SSA) with wavelength was observed during Asian dust events while little spectral dependence of SSA was observed during long-range transport pollution (LTP) events. Satellite aerosol optical thickness (AOT) and Hysplit air mass backward trajectory analyses as well as chemical analysis were performed to characterize the dependence of spectral optical properties on aerosol type. Results from this study can provide useful information for studies on regional air quality and aerosol's effects on climate change.

In this study, wavelength dependency of aerosol was investigated using the correlation between Single scattering albedo (SSA) and Angstrom exponent (AE), the time series of SSA difference in accordance with wavelength, and the relationship between SSA and AE ratio which defined AE at longer wavelength pair over AE at shorter wavelength pair. All used data in this study are daily mean values. The positive correlation between SSA and AE becomes clear as the wavelength pair of AE becomes longer, however negative correlation with AE at shorter wavelength pair also cannot be neglected. Accordingly, the correlation is well negative between SSA at longer wavelength (LW‐SSA) and AE at shorter wavelength pair (SW‐AE), opposite to the well positive correlation between SSA at shorter wavelength (SW‐SSA) and AE at longer wavelength pair (LW‐AE). SSA also shows the interesting relationship with AE ratio. In this study, AE ratio is defined as AE at 675–1020 nm over AE at 340–675 nm. Their relation shows the quadratic correlated shape, and the part of this relationship can be distributed distinctly by the size of aerosol. Time series of SSA difference between two wavelengths can show the properties of dominant related to the information of aerosol size or type.

To quantify radiative forcing of aerosol and to investigate the dependence of the horizontal UV, visible and NIR on total optical depth (TOD) and cloudiness, narrowband surface solar irradiances were measured and analyzed for direct and diffuse component. A MFRSR (Multifilter Rotating Shadowband Ratiometer) was used to measure the global, direct and diffuse solar irradiances atone broadband of 391–955 nm and 6 narrowband channels of 412.8, 495.2, 611.9, 672.2, 869, 936.6 nm for a year from Jan. to Dec. in 2006 at Yonsei University in Seoul and a UV‐MFRSR was used to measure irradiance at 7 narrowband channels of 299.1, 304.5, 310.7, 317.1, 323.8, 331.3, 367.4 nm in UV range during 7 months at the same location with the MFRSR.

The contributions of long range transported aerosol in East Asia to carbonaceous aerosol and particulate matter (PM) concentrations in Seoul, Korea were estimated with potential source contribution function (PSCF) calculations. Carbonaceous aerosol (organic carbon (OC) and elemental carbon (EC)), PM(2.5), and PM(10) concentrations were measured from April 2007 to March 2008 in Seoul, Korea. The PSCF and concentration weighted trajectory (CWT) receptor models were used to identify the spatial source distributions of OC, EC, PM(2.5), and coarse particles. Heavily industrialized areas in Northeast China such as Harbin and Changchun and East China including the Pearl River Delta region, the Yangtze River Delta region, and the Beijing-Tianjin region were identified as high OC, EC and PM(2.5) source areas. The conditional PSCF analysis was introduced so as to distinguish the influence of aerosol transported from heavily polluted source areas on a receptor site from that transported from relatively clean areas. The source contributions estimated using the conditional PSCF analysis account for not only the aerosol concentrations of long range transported aerosols but also the number of transport days effective on the measurement site. Based on the proposed algorithm, the condition of airmass pathways was classified into two types: one condition where airmass passed over the source region (PS) and another condition where airmass did not pass over the source region (NPS). For most of the seasons during the measurement period, 249.5-366.2% higher OC, EC, PM(2.5), and coarse particle concentrations were observed at the measurement site under PS conditions than under NPS conditions. Seasonal variations in the concentrations of OC, EC, PM(2.5), and coarse particles under PS, NPS, and background aerosol conditions were quantified. The contributions of long range transported aerosols on the OC, EC, PM(2.5), and coarse particle concentrations during several Asian dust events were also estimated. We also investigated the performance of the PSCF results obtained from combining highly time resolved measurement data and backward trajectory calculations via comparison with those from data in low resolutions. Reduced tailing effects and the larger coverage over the area of interest were observed in the PSCF results obtained from using the highly time resolved data and trajectories.

Recently, temporal changes in Aerosol Optical Thickness (AOT) have been investigated based on model simulations, satellite and ground-based observations. Most AOT trend studies used monthly or annual arithmetic means that discard details of the generally right-skewed AOT distributions. Potentially, such results can be biased by extreme values (including outliers). This study additionally uses percentiles (i.e., the lowest 5%, 25%, 50%, 75% and 95% of the monthly cumulative distributions fitted to Aerosol Robotic Network (AERONET)-observed and ECHAM/MESSy Atmospheric Chemistry (EMAC)-model simulated AOTs) that are less affected by outliers caused by measurement error, cloud contamination and occasional extreme aerosol events. Since the limited statistical representativeness of monthly percentiles and means can lead to bias, this study adopts the number of observations as a weighting factor, which improves the statistical robustness of trend estimates. By analyzing the aerosol composition of AERONET-observed and EMAC-simulated AOTs in selected regions of interest, we distinguish the dominant aerosol types and investigate the causes of regional AOT trends. The simulated and observed trends are generally consistent with a high correlation coefficient (R = 0.89) and small bias (slope±2σ = 0.75 ± 0.19). A significant decrease in EMAC-decomposed AOTs by water-soluble compounds and black carbon is found over the USA and the EU due to environmental regulation. In particular, a clear reversal in the AERONET AOT trend percentiles is found over the USA, probably related to the AOT diurnal cycle and the frequency of wildfires. In most of the selected regions of interest, EMAC-simulated trends are mainly attributed to the significant changes of the dominant aerosols; e.g., significant decrease in sea salt and water soluble compounds over Central America, increase in dust over Northern Africa and Middle East, and decrease in black carbon and organic carbon over Australia.