ALBERT

Description: Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements were performed at Tsukuba, Japan (36.1° N, 140.1° E), in November–December 2006. The measured spectra of scattered sunlight are analyzed by DOAS and optimal estimation methods to retrieve the aerosol optical depth (τ) and the vertical profile of the aerosol extinction coefficient (σ) at 476 nm in the lower troposphere. We characterize these retrieved quantities through comparisons with coincident lidar and sky radiometer measurements. The retrieved σ values for layers of 0–1 and 1–2 km agree with lidar data to within 30% and 60%, respectively, for most cases, including partly cloudy conditions. Results similar to σ at 0–1 km are obtained for the retrieved τ values, demonstrating that MAX-DOAS provides the new, unique aerosol dataset in the lower troposphere.

Description: We developed a new emission inventory for Asia (Regional Emission inventory in ASia (REAS) Version 1.1) for the period 1980–2020. REAS is the first inventory to integrate historical, present, and future emissions in Asia on the basis of a consistent methodology. We present here emissions in 2000, historical emissions for 1980–2003, and projected emissions for 2010 and 2020 of SO2, NOx, CO, NMVOC, black carbon (BC), and organic carbon (OC) from fuel combustion and industrial sources. Total energy consumption in Asia more than doubled between 1980 and 2003, causing a rapid growth in Asian emissions, by 28% for BC, 30% for OC, 64% for CO, 108% for NMVOC, 119% for SO2, and 176% for NOx. In particular, Chinese NOx emissions showed a marked increase of 280% over 1980 levels, and growth in emissions since 2000 has been extremely high. These increases in China were mainly caused by increases in coal combustion in the power plants and industrial sectors. NMVOC emissions also rapidly increased because of growth in the use of automobiles, solvents, and paints. By contrast, BC, OC, and CO emissions in China showed decreasing trends from 1996 to 2000 because of a reduction in the use of biofuels and coal in the domestic and industry sectors. However, since 2000, Chinese emissions of these species have begun to increase. Thus, the emissions of air pollutants in Asian countries (especially China) showed large temporal variations from 1980–2003. Future emissions in 2010 and 2020 in Asian countries were projected by emission scenarios and from emissions in 2000. For China, we developed three emission scenarios: PSC (policy success case), REF (reference case), and PFC (policy failure case). In the 2020 REF scenario, Asian total emissions of SO2, NOx, and NMVOC were projected to increase substantially by 22%, 44%, and 99%, respectively, over 2000 levels. The 2020 REF scenario showed a modest increase in CO (12%), a lesser increase in BC (1%), and a slight decrease in OC (–5%) compared with 2000 levels. However, it should be noted that Asian total emissions are strongly influenced by the emission scenarios for China.

Description: We present vertical profiles of the aerosol extinction coefficient retrieved from ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements at Tsukuba, Japan (36.1° N, 140.1° E), from November 2006 to March 2007. Retrievals utilizing absorption by the oxygen collision complex O4 are first made at two wavelengths, 354 and 476 nm. A robust assessment of the MAX-DOAS aerosol data is made using coincident lidar measurements throughout the period. Agreement between aerosol extinction coefficients measured by MAX-DOAS and the lidar tends to be better at the longer wavelength and at lower altitudes. At 476 nm, the best agreement, to within 30%, is found at altitudes of 0–1 km, confirming results from a literature assessment for a two-month measurement period. These findings are supported by comparisons of the aerosol optical depth by MAX-DOAS and sky radiometer measurements and are further explained by differences in the O4 absorption and the air mass factor profile between 354 and 476 nm. Thus, uncertainty in MAX-DOAS aerosol measurements is well quantified and characterized, providing a basis for quantitative studies using MAX-DOAS measurements.

Description: Mass concentrations of black carbon (BC) were determined in June 2006 at the top of Mount Tai (36.26° N, 117.11° E, 1534 m a.s.l.), located in the middle of Central East China, using four different instruments: a multi-angle absorption photometer (5012 MAAP, Thermo), a particle soot absorption photometer (PSAP, Radiance Research), an ECOC semi-continuous analyzer (Sunset Laboratory) and an Aethalometer (AE-21, Magee Scientific). High correlation coefficients (R2〉0.88) were obtained between the measurements of the BC mass concentrations by the different instruments. From the range of the slopes of the linear least-square fittings, we concluded that the BC concentrations regionally-representative of the area were measured in a range with a maximum-to-minimum ratio of 1.5 (an exception was that the BC (PM2.5) concentrations derived from MAAP were ~2 times higher than the optical measurements (PM2.5) derived from the ECOC analyzer). This range is significant, but is still sufficiently narrow to better constrain the large and highly uncertain emission rate of BC from China. In detail, two optical instruments (the MAAP instrument and the PSAP instrument equipped with a heated inlet (400°C)) tended to give higher concentrations than the thermal EC concentrations observed by the ECOC analyzer. The ratios of optical BC to thermal EC showed a positive correlation with the OC/EC ratio reported by the ECOC analyzer, suggesting two possibilities. One is that the optical instruments overestimated BC concentrations in spite of careful cancellation of the scattering effect in the MAAP instrument and the expected evaporation of volatile species by heating the inlet of the PSAP instrument. The other is that the determined split points between OC and EC were too late when a large amount of OC underwent charring during the analysis, resulting in an underestimation of EC by the ECOC analyzer. High ratios of optical BC to thermal EC were recorded when the NOx/NOy ratio was low, implying the coating of the particles became thicker in the aged air mass and resulted in the optical instruments overestimating BC concentrations owing to the lensing effect.

Description: The impact of the East Asia monsoon on the seasonal behavior of O3 in the boundary layer of Eastern China and the west Pacific region was analyzed for 2004–2006 by means of full-year nested chemical transport model simulations and continuous observational data obtained from three inland mountain sites in central and eastern China and three oceanic sites in the west Pacific region. The basic common features of O3 seasonal behaviors over all the monitoring sites are the pre- and post-monsoon peaks with a summer trough. Such bimodal seasonal patterns of O3 are predominant over the region with strong summer monsoon penetration, and become weaker or even disappear outside the monsoon region. The seasonal/geographical distribution of the pre-defined Monsoon Index indicated that the East Asia summer monsoon is responsible for the bimodal seasonal O3 pattern, and also partly account for the differences in the O3 seasonal variations between the inland mountain and oceanic sites. Over the inland mountain sites, the O3 concentration increased gradually from the beginning of the year, reached a maximum in June, decreased rapidly to a minimum in July or August, and then peaked in September or October, thereafter decreased gradually again. Over the oceanic sites, O3 abundance showed a similar increasing trend beginning in January, but then decreased gradually from the end of March, followed by a wide trough with the minimum in July and August and a small peak in October or November. A sensitivity analysis performed by setting China-emission to zero revealed that the chemically produced O3 from China-emission contributed more than 40% of total boundary layer O3 during summertime (60–70% in June) and accounted for about 40 ppb of each peak value over the inland region. In contrast, over the oceanic region in the high monsoon index zone, the contribution of China-emission to total O3 was always less than 20% (

Description: A 3-D regional chemical transport model, the Nested Air Quality Prediction Model System (NAQPMS), with an on-line tracer tagging module was applied to study the source of the near-ground (

Description: A challenge for the quantitative analysis of tropospheric nitrogen dioxide (NO2) column data from satellite observations is posed mainly by the lack of satellite-independent observations for validation. We performed such observations of the tropospheric NO2 column using the ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) technique in the North China Plain (NCP) from 29 May to 29 June 2006. Comparisons between tropospheric NO2 columns measured by MAX-DOAS and the Ozone Monitoring Instrument (OMI) onboard the Aura satellite indicate that OMI data (the standard product, version 3) over NCP may have a positive bias of 1.6×1015 molecules cm−2 (20%), where the estimated random error in the OMI data is 0.6×1015 molecules cm−2 or approximately 8%. Combining these results with literature validation results for the US, Europe, and Pacific Ocean suggests that a bias of +20%/–30% is a reasonable estimate, accounting for different regions. Considering the uncertainty estimated here will pave the way for quantitative studies using OMI NO2 data, especially over NCP.

Description: The impact of open crop residual burning on O3, CO, Black Carbons (BC), and Organic Carbons (OC) concentrations over Central Eastern China (CEC) during the Mount Tai Experiment 2006 (MTX2006) was evaluated using the regional chemical transport model, the Models-3 Community Multiscale Air Quality Modeling System (CMAQ). To investigate these pollutants during the MTX2006 period in June, daily gridded emissions from open crop residual burning were developed based on a bottom-up methodology and using land cover and hotspot information from satellites. This model system which involves daily emissions from open biomass burning, captured monthly-averaged observed concentrations and day-to-day variations in the patterns of O3, CO, BC, and OC with good correlation coefficients between models and observations, ranging from 0.54 to 0.66. These results were significantly improved from those using annual emissions. For monthly-averaged O3, the simulated concentration of 81.5 ppbv was close to the observed concentration (82.5 ppbv). The period of MTX2006 was roughly divided into two parts: 1) polluted days with heavy open crop residual burning in the first half of June; 2) cleaner days with negligible field burning in the latter half of June. Additionally, the first half of June was defined by two high pollution episodes during 5–7 and 12–13 June, and a relatively cleaner episode during 8–10 June between these two high pollution episodes. In the first polluted episode, this model captured high O3, CO, BC, and OC concentrations at the summit of Mount Tai which were affected by open crop residual burning in the south of CEC and northward transport. For this episode, the impacts from open crop residual burning were 12% for O3, 35% for CO, 56% for BC, and 80% for OC over CEC. The daily emissions from open crop residual burning were an essential factor to evaluate the pollutants during the MTX2006. These emissions have a large impact not only on primary pollutants but also on secondly pollutions, such as O3, in the first half of June over northeastern Asia. On the other hand, this model did not capture the second polluted episode and underestimated observed CO and BC. Improvements of both anthropogenic and open burning emissions and CO inflow from model boundary are necessary to improve both anthropogenic and open burning emissions and CO inflow to evaluate the pollutants using this model.

Description: Atmospheric nanoparticles (NPs) are important intermediates in the transition from gas-phase molecules to new aerosols that can activate into cloud droplets. Through increases in the emissions of sulfur-containing gases, human activities have likely increased the number of NPs produced in the atmosphere. To have significant impacts, however, sulfur pollution must be transported away from the surface, where NP formation is inefficient, to higher altitudes. To characterize this anthropogenic influence, tagged tracers are implemented in a global atmospheric transport model. The tagged tracers are used to track the contributions of sulfur from five sources (anthropogenic, oceanic, volcanic, aircraft, and stratospheric) to the gas-phase burdens of SO2 and H2SO4(g), and the rates of forming atmospheric NPs. Because NPs may be produced by a variety of mechanisms, three different aerosol nucleation schemes (binary, ternary and ion-induced) are used in the model calculations. Of the SO2 in the global troposphere, the tagged tracers indicate that about 69% originates from anthropogenic surface emissions, 20% from the oceans and 10% from de-gassing volcanoes. The same sources contribute about 56%, 24% and 19%, respectively, to the global tropospheric H2SO4(g) burden. The anthropogenic contribution for H2SO4(g) is reduced because anthropogenic SO2 produces H2SO4(g) less efficiently than oceanic and volcanic sulfur. Regardless of the underlying nucleation assumptions, the simulations show a pronounced influence of anthropogenic sulfur on atmospheric NP formation, particularly in the Northern Hemisphere. Utilizing the tagged H2SO4(g) contributions, anthropogenic sulfur is estimated to account for roughly 69% of the NP formation in the Northern Hemisphere, 31% in the Southern Hemisphere and 56% across the global troposphere. In the key region of the upper troposphere, anthropogenic and oceanic sulfur both make sizeable contributions to NP formation (54% and 37%, respectively). The tagged tracer contributions suggest that human activities have probably more than doubled the NP production rate in the atmosphere from preindustrial to modern times.

Description: The Indian summer monsoon rainfall (ISMR), which has a strong connection to agricultural food production, has been less predictable by conventional models in recent times. Two distinct years 2002 and 2003 with lower and higher July rainfall, respectively, are selected to help understand the natural and anthropogenic influences on ISMR. We show that heating gradients along the meridional monsoon circulation are reduced due to aerosol radiative forcing and the Indian Ocean Dipole in 2002. An increase in the dust and biomass-burning component of the aerosols through the zonal monsoon circulation resulted in reduction of cloud droplet growth in July 2002. These conditions were opposite to those in July 2003 which led to an above average ISMR. In this study, we have utilized NCEP/NCAR reanalyses for meteorological data (e.g. sea-surface temperature, horizontal winds, and precipitable water), NOAA interpolated outgoing long-wave radiation, IITM constructed all-India rainfall amounts, aerosol parameters as observed from the TOMS and MODIS satellites, and ATSR fire count maps. Based on this analysis, we suggest that monsoon rainfall prediction models should include synoptic as well as interannual variability in both atmospheric dynamics and chemical composition.