[1] The radiative impact of the mixing state of black carbon (BC) aerosol is investigated in Asian outflow. The mixing state and size distribution of BC aerosol were measured with a ground-based single-particle soot photometer at a remote island (Fukue) in Japan in spring 2007. The mass concentration of BC in Asian continental air masses reached 0.5 mg m À3 , with a mass median diameter of 200-220 nm. The median value of the shell/core diameter ratio increased to $1.6 in Asian continental and maritime air masses with a core diameter of 200 nm, while in free tropospheric and Japanese air masses it was 1.3-1.4. On the basis of theoretical calculations using the size distribution and mixing state of BC aerosol, scattering and absorption properties of PM 1 aerosols were calculated under both dry and ambient conditions, considering the hygroscopic growth of aerosols. It was estimated that internal mixing enhanced the BC absorption by a factor of 1.5-1.6 compared to external mixing. The calculated absorption coefficient was 2-3 times higher in Asian continental air masses than in clean air. Coatings reduced the single-scattering albedo (SSA) of PM 1 aerosol by 0.01-0.02, which indicates the importance of the mixing state of BC aerosol in evaluating its radiative influence. The SSA was sensitive to changes in air mass type, with a value of $0.98 in Asian continental air masses and $0.95 in Japanese and free tropospheric air masses under ambient conditions.

Many sensors have to be used simultaneously for multipoint carbon dioxide (CO2) observation. All the sensors should be calibrated in advance, but this is a time-consuming process. To seek a simplified calibration method, we used four commercial CO2 sensor models and characterized their output tendencies against ambient temperature and length of use, in addition to offset characteristics. We used four samples of standard gas with different CO2 concentrations (0, 407, 1,110, and 1,810 ppm). The outputs of K30 and AN100 models showed linear relationships with temperature and length of use. Calibration coefficients for sensor models were determined using the data from three individual sensors of the same model to minimize the relative RMS error. When the correction was applied to the sensors, the accuracy of measurements improved significantly in the case of the K30 and AN100 units. In particular, in the case of K30 the relative RMS error decreased from 24% to 4%. Hence, we have chosen K30 for developing a portable CO2 measurement device (10 × 10 × 15 cm, 900 g). Data of CO2 concentration, measurement time and location, temperature, humidity, and atmospheric pressure can be recorded onto a Secure Digital (SD) memory card. The CO2 concentration in a high-school lecture room was monitored with this device. The CO2 data, when corrected for simultaneously measured temperature, water vapor partial pressure, and atmospheric pressure, showed a good agreement with the data measured by a highly accurate CO2 analyzer, LI-6262. This indicates that acceptable accuracy can be realized using the calibration method developed in this study.

[1] We present a regional and seasonal climatology of SHADOZ ozone profiles in the troposphere and tropical tropopause layer (TTL) based on measurements taken during the first five years of Aura, 2005Aura, -2009, when new stations joined the network at Hanoi, Vietnam; Hilo, Hawaii; Alajuela/Heredia, Costa Rica; Cotonou, Benin. In all, 15 stations operated during that period. A west-to-east progression of decreasing convective influence and increasing pollution leads to distinct tropospheric ozone profiles in three regions: (1) western Pacific/eastern Indian Ocean; (2) equatorial Americas (San Cristóbal, Alajuela, Paramaribo); (3) Atlantic and Africa. Comparisons in total ozone column from soundings, the Ozone Monitoring Instrument (OMI, on Aura, 2004-) satellite and ground-based instrumentation are presented. Most stations show better agreement with OMI than they did for EP/TOMS comparisons (1998)(1999)(2000)(2001)(2002)(2003)(2004); Earth-Probe/Total Ozone Mapping Spectrometer), partly due to a revised above-burst ozone climatology. Possible station biases in the stratospheric segment of the ozone measurement noted in the first 7 years of SHADOZ ozone profiles are re-examined. High stratospheric bias observed during the TOMS period appears to persist at one station. Comparisons of SHADOZ tropospheric ozone and the daily Trajectory-enhanced Tropospheric Ozone Residual (TTOR) product (based on OMI/MLS) show that the satellite-derived column amount averages 25% low. Correlations between TTOR and the SHADOZ sondes are quite good (typical r 2 = 0.5-0.8), however, which may account for why some published residual-based OMI products capture tropospheric interannual variability fairly realistically. On the other hand, no clear explanations emerge for why TTOR-sonde discrepancies vary over a wide range at most SHADOZ sites.

The climatology of surface ozone over East Asia was investigated at a wide range of latitudes by integrating continuous measurements from Japanese monitoring networks. Although a spring maximum and a summer minimum were observed at all seven remote stations, significant latitudinal differences in the seasonal cycles were found, particularly in spring. At low latitudes (20–30°N) the spring maximum appears in March, while it appears in April at high latitudes (40–50°N), and in May at middle latitudes (30–40°N). A regional‐scale chemical transport model was applied to examine factors contributing to the latitudinal dependence observed. The model reproduces the latitudinal gradient and the overall seasonal variations well, and suggests that transport patterns of Asian continental outflow coupled with photochemistry result in latitudinal inhomogeneity over East Asia. These results highlight the key role of dynamical processes in modulating the amplitude and phase of the spring maximum in surface ozone.

Temperature sensitivity of soil organic matter (SOM) decomposition may have a significant impact on global warming. Enzyme-kinetic hypothesis suggests that decomposition of low-quality substrate (recalcitrant molecular structure) requires higher activation energy and thus has greater temperature sensitivity than that of high-quality, labile substrate. Supporting evidence, however, relies largely on indirect indices of substrate quality. Furthermore, the enzyme-substrate reactions that drive decomposition may be regulated by microbial physiology and/or constrained by protective effects of soil mineral matrix. We thus tested the kinetic hypothesis by directly assessing the carbon molecular structure of low-density fraction (LF) which represents readily accessible, mineral-free SOM pool. Using five mineral soil samples of contrasting SOM concentrations, we conducted 30-days incubations (15, 25, and 35 °C) to measure microbial respiration and quantified easily soluble C as well as microbial biomass C pools before and after the incubations. Carbon structure of LFs (<1.6 and 1.6-1.8 g cm(-3) ) and bulk soil was measured by solid-state (13) C-NMR. Decomposition Q10 was significantly correlated with the abundance of aromatic plus alkyl-C relative to O-alkyl-C groups in LFs but not in bulk soil fraction or with the indirect C quality indices based on microbial respiration or biomass. The warming did not significantly change the concentration of biomass C or the three types of soluble C despite two- to three-fold increase in respiration. Thus, enhanced microbial maintenance respiration (reduced C-use efficiency) especially in the soils rich in recalcitrant LF might lead to the apparent equilibrium between SOM solubilization and microbial C uptake. Our results showed physical fractionation coupled with direct assessment of molecular structure as an effective approach and supported the enzyme-kinetic interpretation of widely observed C quality-temperature relationship for short-term decomposition. Factors controlling long-term decomposition Q10 are more complex due to protective effect of mineral matrix and thus remain as a central question.

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CO and H 2 uptake by soil was studied as a diffusion process. A diffusion model was used to determine how the surface fluxes (net deposition velocities) were controlled by in-situ microbial uptake rates and soil gas diffusivity calculated from the 3-phase system (solid, liquid, gas) in the soil. Analytical solutions of the diffusion model assuming vertical uniformity of soil properties showed that physical properties such as air-filled porosity and soil gas diffusivity were more important in the uptake process than in the emission process. To incorporate the distribution of in-situ microbial uptake, we used a 2-layer model incorporating ''a microbiologically inactive layer and an active layer'' as suggested from experimental results. By numerical simulation using the 2-layer model, we estimated the effect of several factors on deposition velocities. The variations in soil gas diffusivity due to physical properties, i.e., soil moisture and air-filled porosity, as well as to the depth of the inactive layer and in-situ microbial uptake, were found to be important in controlling deposition velocities. This result shows that the diffusion process in soil is critically important for CO and H 2 uptake by soil, at least in soils with higher in-situ uptake rates and/or with large variation in soil moisture. Similar uptake rates and the difference in deposition velocity between CO and H 2 may be attributable to differences in CO and H 2 molecular diffusivity. The inactive layer is resistant to diffusion and creates uptake limits in CO and H 2 by soil. The coupling of high temperature and a thick inactive layer, common in arid soils, markedly lowers net CO deposition velocity. The temperature for maximum uptake of CO changes with depth of the inactive layer.