ALBERT

Description: The seasonal variations in background aerosol optical depth (AOD) and aerosol type are investigated over various ecosystems in China based upon three years' worth of meteorological data and data collected by the Chinese Sun Hazemeter Network. In most parts of China, AODs are at a maximum in spring or summer and at a minimum in autumn or winter. Minimum values (0.10~0.20) of annual mean AOD at 500 nm are found in the Qinghai-Tibetan Plateau, which is located in the remote northeast corner of China, the northern forest ecosystems and Hainan Island. Annual mean AOD ranges from 0.25 to 0.30 over desert and oasis areas as well as the desertification grasslands in northern China; the annual mean AOD over the Loess Plateau is moderately high at 0.36. Regions where the highest density of agricultural and industrial activities are located and where anthropogenic sulphate aerosol and soil aerosol emissions are consistently high throughout the whole year (e.g. the central-eastern, southern and eastern coastal regions of China) experience annual mean AODs ranging from 0.50~0.80. Remarkable seasonal changes in the main types of aerosol over northern China (characterized by the Angstrom exponent, α) are seen. Due to biomass and fossil fuel burning from extensive agricultural practices in northern rural areas, concentrations of smoke and soot aerosols rise dramatically during autumn and winter (high α), while the main types of aerosol during spring and summer are dust and soil aerosols (low α). Over southeast Asia, biomass burning during the spring leads to increases in smoke and soot emissions. Over the Tibetan Plateau and Hainan Island where the atmosphere is pristine, the main types of aerosol are dust and sea salt, respectively.

Description: Using a combination of ozonesonde data and numerical simulations of the Chemical Lagrangian Model of the Stratosphere (CLaMS), the trend of tropospheric ozone (O3) during 2002–2010 over Beijing was investigated. Tropospheric ozone over Beijing shows a winter minimum and a broad summer maximum with a clear positive trend in the maximum summer ozone concentration over the last decade. The observed significant trend of tropospheric column ozone is mainly caused by photochemical production (3.1% yr−1 for a mean level of 52 DU). This trend is close to the significant trend of partial column ozone in the lower troposphere (0–3 km) resulting from the enhanced photochemical production during summer (3.0% yr−1 for a mean level of 23 DU). Analysis of the CLaMS simulation shows that transport rather than chemistry drives most of the seasonality of tropospheric ozone. However, dynamical processes alone cannot explain the trend of tropospheric ozone in the observational data. Clearly enhanced ozone values and a negative vertical ozone gradient in the lower troposphere in the observational data emphasize the importance of photochemistry within the troposphere during spring and summer, and suggest that the photochemistry within the troposphere significantly contributes to the tropospheric ozone trend over Beijing during the last decade.

Description: The in situ boundary layer measurement site in Białystok (Poland) has been upgraded with a fully automated observatory for total greenhouse gas column measurements. The automated Fourier Transform Spectrometer (FTS) complements the on-site in situ facilities and FTS solar absorption measurements have been recorded nearly continuously in clear and partially cloudy conditions since March 2009. Here, the FTS measurements are compared with the collocated tall tower data. Additionally, simulations of the Jena CO2 inversion model are evaluated with the Białystok measurement facilities. The simulated seasonal CO2 cycle is slightly overestimated by a mean difference of 1.2 ppm ± 0.9 ppm (1σ) in comparison with the FTS measurements. CO2 concentrations at the surface, measured at the tall tower (5 m, 90 m, 300 m), are slightly underestimated by −1.5 ppm, −1.6 ppm, and −0.7 ppm respectively during the day and by −9.1 ppm, −5.9 ppm, and −1.3 ppm during the night. The comparison of the simulated CO2 profiles with low aircraft profiles shows a slight overestimation of the lower troposphere (by up to 1 ppm) and an underestimation in near-surface heights until 800 m (by up to 2.5 ppm). In an appendix the automated FTS observatory, including the hardware components and the automation software, is described in its basics.

Description: The Zotino Tall Tower Observatory in Central Siberia (ZOTTO, 60°48' N, 89°21' E) is an excellent location to monitor the continental carbon cycle. Since April 2009, a fully automated low maintenance measurement system based on a cavity ring-down spectroscopy (CRDS) analyzer is installed at the site to measure continuously carbon dioxide (CO2) and methane (CH4) from six heights up to 301 m a.g.l. Buffer volumes in each air line remove short term CO2 and CH4 mixing ratio fluctuations associated with turbulence, and allow continuous, near-concurrent measurements from all six tower levels. Instead of drying the air sample, the simultaneously measured water vapor is used to correct the dilution and pressure-broadening effects for the accurate determination of dry air CO2 and CH4 mixing ratios. The stability of the water vapor correction was demonstrated by repeated laboratory and field tests. The effect of molecular adsorption in the wet air lines was shown to be negligible. The low consumption of four calibration tanks that need recalibration only on decadal timescale further reduces maintenance. The measurement precision (accuracy) of 0.04 ppm (0.09 ppm) for CO2 and 0.3 ppb (1.5 ppb) for CH4 is compliant with the WMO recommendations. The data collected during the 2009 vegetation period reveals a seasonal cycle amplitude of 26.4 ppm at the 301 m level.

Description: In September/October 2009, six European ground-based Fourier Transform Spectrometers (FTS) of the Total Carbon Column Observation Network (TCCON) were calibrated for the first time using aircraft measurements. The campaign was part of the Infrastructure for Measurement of the European Carbon Cycle (IMECC) project. During this campaign, altitude profiles of several trace gases and meteorological parameters were taken close to the FTS sites (typically within 1–2 km distance for flight altitudes below 5000 m). Profiles of CO2, CH4, CO and H2O were measured continuously. N2O, H2, and SF6 were later derived from flask measurements. The aircraft data had a vertical coverage ranging from approximately 300 to 13 000 m, corresponding to ~80% of the total atmospheric column seen by the FTS. This study summarizes the calibration results for CH4. The resulting calibration factor of 0.978 ± 0.002 (±1 σ) from the IMECC campaign agreed very well with the results that Wunch et al. (2010) had derived for TCCON instruments in North America, Australia, New Zealand, and Japan using similar methods. By combining our results with the data of Wunch et al. (2010), the uncertainty of the calibration factor could be reduced by a factor of three (compared to using only IMECC or only Wunch et al. (2010) data). A careful analysis of the calibration method used by Wunch et al. (2010) revealed that the incomplete vertical coverage of the aircraft profiles can lead to a bias in the calibration factor. This bias can be compensated with a new iterative approach that we developed. Using this improved method, we derived a significantly lower calibration factor of 0.974 ± 0.002 (±1 σ). This corresponds to a correction of all TCCON CH4 measurements by roughly −7 ppb.

Description: The Total Carbon Column Observing Network (TCCON) is a ground-based network of Fourier Transform Spectrometer (FTS) sites around the globe, where the column abundances of CO2, CH4, N2O, CO and O2 are measured. CO2 is constrained with a precision better than 0.25% (1-σ). To achieve a similarly high accuracy, calibration to World Meteorological Organization (WMO) standards is required. This paper introduces the first aircraft calibration campaign of five European TCCON sites and a mobile FTS instrument. A series of WMO standards in-situ profiles were obtained over European TCCON sites via aircraft and compared with retrievals of CO2 column amounts from the TCCON instruments. The results of the campaign show that the FTS measurements are consistently biased 1.1% ± 0.2% low with respect to WMO standards, in agreement with previous TCCON calibration campaigns. The standard a priori profile for the TCCON FTS retrievals is shown to not add a bias. The same calibration factor is generated using aircraft profiles as a priori and with the TCCON standard a priori. With a calibration to WMO standards, the highly precise TCCON CO2 measurements of total column concentrations provide a suitable database for the calibration and validation of nadir-viewing satellites.

Description: High-resolution mapping of fuel combustion and CO2 emission provides valuable information for modeling pollutant transport, developing mitigation policy, and for inverse modeling of CO2 fluxes. Previous global emission maps included only few fuel types, and emissions were estimated on a grid by distributing national fuel data on an equal per capita basis, using population density maps. This process distorts the geographical distribution of emissions within countries. In this study, a sub-national disaggregation method (SDM) of fuel data is applied to establish a global 0.1° × 0.1° geo-referenced inventory of fuel combustion (PKU-FUEL) and corresponding CO2 emissions (PKU-CO2) based upon 64 fuel sub-types for the year 2007. Uncertainties of the emission maps are evaluated using a Monte Carlo method. It is estimated that CO2 emission from combustion sources including fossil fuel, biomass, and solid wastes in 2007 was 11.2 Pg C yr−1 (9.1 Pg C yr−1 and 13.3 Pg C yr−1 as 5th and 95th percentiles). Of this, emission from fossil fuel combustion is 7.83 Pg C yr−1, which is very close to the estimate of the International Energy Agency (7.87 Pg C yr−1). By replacing national data disaggregation with sub-national data in this study, the average 95th minus 5th percentile ranges of CO2 emission for all grid points can be reduced from 417 to 68.2 Mg km−2 yr−1. The spread is reduced because the uneven distribution of per capita fuel consumptions within countries is better taken into account by using sub-national fuel consumption data directly. Significant difference in per capita CO2 emissions between urban and rural areas was found in developing countries (2.08 vs. 0.598 Mg C/(cap. × yr)), but not in developed countries (3.55 vs. 3.41 Mg C/(cap. × yr)). This implies that rapid urbanization of developing countries is very likely to drive up their emissions in the future.

Description: Black carbon (BC) is an important atmospheric constituent as an air pollutant and as a climate forcer. To our knowledge, field measurements of BC have not been reported over the South China Sea. Observations of light-absorption coefficients (σabs) and BC concentrations by Aethalometer were conducted on Yongxing Island in the South China Sea and at five continental sites in the Pearl River delta (PRD) region, South China, in two periods: 16 May–20 June 2008 in the rainy season and 12 December 2008–8 January 2009 in the dry season. At the oceanic site, the daily average BC concentrations varied from 0.28 to 2.14 μg m−3 and variations of BC were small between the two periods (0.67 in the dry season sampling period and 0.54 μg m−3 in the rainy season sampling period). Similarly, little difference in BC level was found at a rural site in PRD between the two sampling periods (2.88 and 2.62 μg m–3). At the PRD urban sites, the daily average concentration of BC ranged from 1.56 to 37.9 μg m−3, higher in the dry season sampling period (12.31 μg m–3) and lower in the rainy season sampling period (6.17 μg m–3). The observed average σabs values in rainy vs. dry season sampling periods are 119 vs. 62 Mm−1 at the PRD urban sites, 29 vs. 26 Mm−1 at the PRD background site, and 8.4 vs. 7.2 Mm−1 at the marine site. At urban/suburban PRD sites, BC was observed to have a diurnal pattern of higher concentrations at night and at the urban sites a small peak in the early morning rush hour.

Description: Characteristics of the chemical and optical properties of aerosols in urban Shanghai and their relationship were studied over a three-day period in October 2011. A suite of real-time instruments, including an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS), a Monitor for AeRosols and GAses (MARGA), a Cavity Ring Down Spectrometer (CRDS), a nephelometer and a Scanning Mobility Particle Sizer (SMPS), was employed to follow the quick changes of the aerosol properties within the 72 h sampling period. The origin of the air mass arriving in Shanghai during this period shifted from the East China Sea to the northwest area of China, offering a unique opportunity to observe the evolution of aerosols influenced by regional transport from the most polluted areas in China. According to the meteorological conditions and temporal characterizations of the chemical and optical properties, the sampling period was divided into three periods. During Period 1 (00:00–23:00 LT, 13 October), the aerosols in urban Shanghai were mainly fresh and the single scattering albedo varied negatively with the emission of elemental carbon, indicating that local sources dominated. Period 2 (23:00 LT on 13 October to 10:00 LT on 15 October) was impacted by regionally transported pollutants and had the highest particulate matter (PM) mass loading and the lowest particle acidity, characterized by large fractions of aged particles and high secondary ion (nitrate, sulfate and ammonium) mass concentrations. Comparison between ATOFMS particle acidity and quantitative particle acidity by MARGA indicated the significance of semi-quantitative calculation in ATOFMS. Two sub-periods were identified in Period 2 based on the scattering efficiency of PM1 mass. Period 3 (from 10:00 LT on 15 October to 00:00 LT on 16 October) had a low PM1/PM10 ratio and a new particle formation event. The comparison of these sub-periods highlights the influence of particle mixing state on aerosol optical properties. We directly observed the influence of regionally transported pollutants on local aerosol properties and demonstrate that the PM mass extinction efficiency is largely determined by the mixing states of the aerosol.

Description: Characteristics of the chemical and optical properties of aerosols in urban Shanghai and their relationship were studied over a three-day period in October 2011. A suite of real-time instruments, including an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS), a Monitor for AeRosols and GAses (MARGA), a Cavity Ring Down Spectrometer (CRDS), a nephelometer and a Scanning Mobility Particle Sizer (SMPS), was employed to follow the quick changes of the aerosol properties within the 72-h sampling period. The origin of the air mass arriving in Shanghai during this period shifted from the East China Sea to the northwest area of China, offering a unique opportunity to observe the evolution of aerosols influenced by regional transport from the most polluted areas in China. According to the meteorological conditions and temporal characterizations of the chemical and optical properties, the sampling period was divided into three periods. During Period 1 (00:00–23:00, 13 October), the aerosols in urban Shanghai were mainly fresh and the single scattering albedo varied negatively with the emission of elemental carbon, indicating that local sources dominated. Period 2 (23:00 on 13 October to 10:00 on 15 October) was impacted by regionally transported pollutants and had the highest particulate matter (PM) mass loading and the lowest particle acidity, characterized by large fractions of aged particles and high secondary ion (nitrate, sulfate and ammonium) mass concentrations. Two sub-periods were identified in Period 2 based on the scattering efficiency of PM1 mass. The comparison of these sub-periods highlights the influence of particle mixing state on aerosol optical properties. Period 3 (from 10:00 on 15 October to 00:00 on 16 October) had a low PM1/PM10 ratio and a new particle formation event. We directly observed the influence of regionally transported pollutants on local aerosol properties and demonstrate that the PM mass extinction efficiency is largely determined by the chemical components and mixing states of the aerosol.