Showing papers by "Yutaka Matsumi published in 2006"

Seasonal variation of carbon monoxide in northern Japan: Fourier transform IR measurements and source-labeled model calculations

Abstract: [ 1] Tropospheric carbon monoxide ( CO) was measured throughout 2001 using groundbased Fourier transform IR ( FTIR) spectrometers at Moshiri (44.4 degrees N) and Rikubetsu (43.5 degrees N) observatories in northern Japan, which are separated by 150 km. Seasonal and day-to-day variations of CO are studied using these data, and contributions from various CO sources are evaluated using three-dimensional global chemistry transport model (GEOS-CHEM) calculations. Seasonal maximum and minimum FTIR-derived tropospheric CO amounts occurred in April and September, respectively. The ratio of partial column amounts between the 0 - 4 and 0 - 12 km altitude ranges is found to be slightly greater in early spring. The GEOS-CHEM model calculations generally reproduce these observed features. Source-labeled CO model calculations suggest that the observed seasonal variation is caused by seasonal contributions from various sources, in addition to a seasonal change in chemical CO loss by OH. Changes in meteorological fields largely control the relative importance of various source contributions. The contributions from fossil fuel (FF) combustion in Asia and photochemical CO production have the greatest yearly averaged contribution at 1 km among the CO sources (31% each). The Asian FF contribution increases from winter to summer, because weak southwesterly wind in summer brings more Asian pollutants to the observation sites. The seasonal variation from photochemical CO production is small ( +/- 17% at 1 km), likely because of concurrent increases ( decreases) of photochemical production and loss rates in summer ( winter), with the largest contribution between August and December. The contribution from intercontinental transport of European FF combustion CO is found to be comparable to that of Asian FF sources in winter. Northwesterly wind around the Siberian high in this season brings pollutants from Europe directly to Japan, in addition to southward transport of accumulated pollution from higher latitudes. The influences are generally greater at lower altitudes, resulting in a vertical gradient in the CO profile during winter. The model underestimates total CO by 12 - 14% between March and June. Satellite-derived fire-count data and the relationship between FTIR-derived HCN and CO amounts are generally consistent with biomass burning influences, which could have been underestimated by the model calculations.

Scavenging of pollutant acid substances by Asian mineral dust particles

Abstract: [1] Uptakes of sulfate and nitrate onto Asian dust particles during transport from the Asian continent to the Pacific Ocean were analyzed by using a single-particle time-of-flight mass spectrometer. Observation was conducted at Tsukuba in Japan in the springtime of 2004. Sulfate-rich dust particles made their largest contribution during the ‘dust event’ in the middle of April 2004. As a result of detailed analysis including backward trajectory calculations, it was confirmed that sulfate components originating from coal combustion in the continent were internally mixed with dust particles. Even in the downstream of the outflow far from the continental coastline, significant contribution of Asian dust to sulfate was observed. Asian dust plays critical roles as the carrier of sulfate over the Pacific Ocean.

Laboratory Study of O(1S) Formation Process in the Photolysis of O3 and its Atmospheric Implications

Abstract: A high-sensitive technique to detect O(1S) atoms using vacuum ultraviolet laser-induced fluorescence (VUV-LIF) spectroscopy has been applied to study the O(1S) production process from the UV photodissociation of O3, N2O, and H2O2. The quantum yields for O(1S) formation from O3 photolysis at 215 and 220 nm are determined to be (1.4 ± 0.4) × 10−4 and (5 ± 3) × 10−5, respectively. Based on thermochemical considerations, the O(1S) formation from O3 photolysis at 215 and 220 nm is attributed to a spin-forbidden process of O(1S)+O2(X3Σg −). Analysis of the Doppler profile of O(1S) produced from O3 photolysis at 193 nm also indicates that the O(1S) atoms are produced from the spin-forbidden process. In the photolysis of N2O and H2O2 at 193 nm, no discernible signal of O(1S) atoms has been detected. The upper limit values of the quantum yields for O(1S) production from N2O and H2O2 photolysis at 193 nm are estimated to be 8 × 10−5 and 3 × 10−5, respectively. Using the experimental results, the impact of the O(1S) formation from O3 photolysis on the atmospheric OH radical formation through the reaction of O(1S)+H2O has been estimated. The calculated results show that the contribution of the O(1S)+H2O reaction to the OH production rate is ∼2% of that of the O(1D)+H2O reaction at 30 km altitude in mid-latitude. Implications of the present laboratory experimental results for the terrestrial airglow of O(1S) at 557.7 nm have also been discussed.

New Kinetic and Spectroscopic Measurements in the CF3Ox + NOx System

Abstract: CF3Ox radicals are present in the atmosphere as oxidized species of a series of CFCs, HFCs and HCFCs. They react with NOx species. In particular, the reaction between CF3O2 and NO which shows two reaction channels,