Cape Grim isotope measurements — A preliminary assessment

Measurements of the stable carbon isotope ratio in atmospheric CO₂ permit a distinction between variations resulting from biospheric and oceanic exchange. In situ extraction of CO₂ from Cape Grim air (41°S) for isotopic analysis commenced in 1977; however difficulties with technique reliability were experienced until 1982. Since 1982, 2.6 years of relatively consistent values have accumulated.For a preliminary assessment of the latter data, estimates of the isotopic behaviour from the global transport and inter-reservoir exchange model of Pearman and Hyson (1985) have been employed. The assessment demonstrates the precision requirements of a carbon isotope monitoring program and the relevance of the isotope measurements as a constraint on parameterization of the model.Clear evidence of the changes due to fossil fuel combustion is seen in the year-to-year differences in ¹³C, with the mean and standard error of the overall trend being –0.025±0.005 yr^-1. A significant seasonal variation in ¹³C is apparent, despite considerable inter-annual variability possibly associated with the 1982/83 ENSO phenomena. The average peak-to-peak amplitude is 0.055±0.014 with a maximum on day 85±15 (approx. 26 March).There is some evidence for a complex seasonal inter-relationship between concentration and isotope ratio, both in the Cape Grim data and in Mook et al. (1983) South Pole data, but with marked differences between the stations, and with both different from the model estimates.In particular, the Cape Grim results suggest that exchange with Southern Hemisphere biosphere is the main contributor to the seasonal variation in isotope ratio at this latitude.     

一次特大暴雨天气的Q*矢量分析

应用修正的Q     

Size distributions of aerosol number concentrations and water-soluble constituents in Toyama, Japan: A comparison of the measurements during Asian dust period with non-dust period

Size-separated aerosol number concentrations and water-soluble constituents were measured in Toyama, the Hokuriku district, near the coast of the Japan Sea, during the spring and summer in 2003. The number concentrations of coarse particles were significantly high in April, which was due to Asian dust events called Kosa in Japanese. Particulate nssCa²⁺, which is mostly present in the coarse-mode particles, was significantly high in April. On the other hand, the concentrations of NH₄⁺ and nssSO₄²⁻, which mainly exist as the accumulation-mode particles were not high in April. The mass-size distributions of water-soluble constituents were compared with the size-separated number concentrations of particles. Backward trajectory analysis was also employed to examine the transport process of the air mass in Toyama.     

Gamma Emitters on Micro-Becquerel Activity Level in Air at Kraków (Poland)

The Petryanov air filters combined into half-year sets were analyzed for the presence of ⁴⁰K, ¹³⁷Cs and ²²Na by means of low-background gamma rays spectrometry. Each sample contains aerosols from more than 1 Mm³ of air. Samples were collected in ground level air at Kraków (Southern Poland) from 1996 to 2002. Activity concentrations of ⁴⁰K are almost constant with the mean of 14.7± 4.5 Bq m^–3. Activity concentrations of ¹³⁷Cs, which are on the level of single Bq m^{– 3} show exponential decrease with effective half-life time of 7.07± 0.77 years. The cosmogenic ²²Na shows a strong seasonal variation with significant different mean values activity concentration between 0.333± 0.095 Bq m^–3 and 0.137± 0.045 Bq m^–3, for summer and winter, respectively. Moreover, the activity ratio for two cosmogenic radionuclides: ²²Na and measured previously ⁷Be show also changes with statistically significant seasonal differences. The lower values were found during winters. The mechanisms which might govern this ratio are discussed. The conclusion is that transport of ²²Na during summer seems to be so much effective, that results in kind of relative depletion of stratosphere of this nuclide.     

Characterization of iron and manganese species in atmospheric aerosols from anthropogenic sources

Electron paramagnetic resonance (EPR) was used to study the chemical form of iron, manganese and other paramagnetic species in airborne particles collected on southern coastal part of the North Sea, located in France. In parallel, chemical analysis was performed to obtain the metal concentrations in samples whereas an individual analysis of particles was provided by scanning electron microscopy coupled to an energy-dispersive X-ray spectrometer (SEM-EDX). EPR spectra have evidenced Fe³⁺ and Mn²⁺ ions in the form of isolated or agglomerated species, as well as carbonaceous products with variable signal intensities according to the wind direction. The monitoring of a signal of isolated Mn²⁺ ions on a distance close to 90 km was proposed as tracer of particles from a Mn local emission source. Fe³⁺ signals are relative to agglomerated species and differences in the type of interaction between these species were evidenced following the wind direction. Fe³⁺ EPR signals parameters revealing antiferromagnetic contribution in Fe-rich particles were found for an industrial origin at Dunkerque.     

Aqueous Oxidation of Sulfur(IV) Catalyzed by Manganese(II): A Generalized Simple Kinetic Model

The reaction kinetics of S(IV) autoxidation catalyzed by Mn(II) in the pH range 3–5 typical for atmospheric liquid water, was investigated. For reactions with pH maintained constant during the reaction course, the predictions obtained by a simple integral approach cover kinetic results only for concentrations of HSO ₃ ⁻ up to 0.2 mM at pH 4.5. Thus, a generalized simple kinetic model, which can be used for predicting the reaction kinetics in wider concentration, pH and temperature ranges, was derived. This model is based on the assumption that the reaction rate is proportional to the concentration of a transient manganese-sulfito complex formed in the initial step of a radical chain mechanism. In the proposed power law rate equation

A Study Of The Atmospheric Boundary Layer Using Radon And Air Pollutants As Tracers

Concentrations of radon ²²²Rn andair pollutants, meteorological parametersnear the surface and vertical profiles of meteorological elements were measured atUchio (Okayama City, Okayama Prefecture, Japan) 12 km north from the coast ofthe Inland Sea of Japan. In the nighttime, the ²²²Rn concentration increased in the case of weak winds, but did not increase as much in the case of moderate or strong winds, as had been expected. In the daytime, the ²²²Rn concentrationheld at a slightly higher than average level for the period from sunrise to about 1100 JST. It is considered that this phenomenon is due to a period of morning calm, that is, a transition period from land breeze to sea breeze.NO, which is sensitive to traffic volume,brought information concerning advection.Oxidant concentrations,which reflect the availability of sunlight,acted in the reverse manner to ²²²Rnconcentrations. Thus, a set of ²²²Rn and air pollutants could provide useful information regarding the local conditions of the atmospheric boundary layer.     

Concentrations of 222 Rn, Its Short-Lived Daughters And 212 Pb And Their Ratios Under Complex Atmospheric Conditions And Topography

Atmospheric activity concentrations of ²¹²Pb and short-lived ²²²Rndaughters, together with meteorological elements, have been observed continuously atthree sites at Kamisaibara Village in Japan. In addition, atmospheric activity concentrationof ²²²Rn, equilibrium-equivalent concentration of ²²²Rn and conditionsof the lower atmosphere were observed for three intensive observation periods at Akawase,one of the three sites in Kamisaibara Village. The equilibrium-equivalent concentration of²²²Rn is almost the same as the atmospheric activity concentration of short-lived²²²Rn daughters.The activity concentrations of ²¹²Pb and the short-lived ²²²Rn daughtersand their ratio were low in the daytime owing to convective mixing, and high at nightowing to the surface-based inversion during periods of no precipitation. Their variationshave several patterns corresponding to the scale of the drainage wind or weak mixing.Mechanical mixing due to strong winds through both day and night during the first andsecond observation periods made the atmospheric activity concentrations of ²¹²Pb and the short-lived ²²²Rn daughters continuously low. However, their ratios werecontinuously high during the first period yet continuously low during the second period.This difference can be explained by the effect ofextraction of ²²⁰Rn and ²²²Rndue to strong winds and snow cover. There were also cases in which the ratio of theatmospheric activity concentration of ²¹²Pb to that of the short-lived ²²²Rndaughters at night was equal to or less than the ratio in the daytime. Thisinverse trend, asin the periods of no precipitation mentioned above, is considered to be due to near-neutralconditions on these nights.We find a difference in the ratio of the equilibrium-equivalent concentration of²²²Rn (the activity concentration of short-lived ²²²Rn daughters) tothe activity concentration of ²²²Rn during the first observation period and thatduring the second. The difference can be explained by snow cover on the ground. Wealso find differences among the ratios of the activity concentration of the short-lived²²²Rn daughters to that of ²²²Rn during the three observation periods.These differences can be explained by the submergence of paddy fields.     

PARSIVEL2对降雪测量的订正方法及误差计算

为了获得更加准确的冬季降水数据,针对PARSIVEL2（Particle Size and Velocity）测量降雪时近地面水平风的影响进行了订正及误差计算。订正结果表明:一定风速下,不考虑风的影响会造成小粒子直径的明显低估,而对于同一粒径段的粒子,风速越大,计算过程中对于粒子直径的低估越明显。风速不超过2 m s?1时,其降雪粒子下落末速度计算误差在3%左右,直径计算误差在7%以内（水平偏转角度45°）。在对2018年1月4日南京一次降雪过程中获取的真实雪花谱的分析中可以看出,忽略风的影响会导致雪花谱峰值的偏移和谱的缩窄,这会造成小粒子数浓度的高估和大粒子数浓度的低估,进而影响微物理量的计算。具体表现在雷达反射率因子Z和降雪强度I的低估,及Z–I关系拟合系数a值的实际数值会大于计算值,b值则偏小。但当风速较大时,近地面流场比较复杂,垂直向湍流运动不可忽略,此种订正方法很可能不再适用。建议在以后的业务观测中增设防风圈或在后续的数据处理中增加针对风的订正,以排除风对降雪测量的影响。     

S2MP结构分析

S²MP是SGI刚刚推出的新一代体系结构,既具有MPP的可扩展性,又具有SMP的可编程性,将两者的优势集于一身。将S²MP与历史上曾经出现的两种多机结构进行比较,指出了S²MP结构的特点。分析结果认为,S²MP是当代MIMD机器最具代表性的结构。     

Nitrate in the atmospheric boundary layer of the tropical South Pacific: Implications regarding sources and transport

Weekly bulk aerosol samples collected at Funafuti, Tuvalu (8°30S, 179°12E), American Samoa (14°15S, 170°35W), and Rarotonga (21°15S, 159°45W), from 1983 through most of 1987 have been analyzed for nitrate and other constituents. The mean nitrate concentration is about 0.11 g m^–3 at each of these stations: 0.107±0.011 g m^–3 at Funafuti; 0.116±0.008 at American Samoa; and 0.117±0.010 at Rarotonga. Previous measurements of mineral aerosol and trace metal concentrations at American Samoa are among the lowest ever recorded for the near-surface troposphere and indicate that this region is minimally affected by transport of soil material and pollutants from the continents. Consequently, the nitrate concentration of 0.11 g m^–3 can be regarded as the natural level for the remote marine boundary layer of the tropical South Pacific Ocean. In contrast, over the tropical North Pacific which is significantly impacted by the transport of material from Asia and North America, the mean nitrate concentrations are about three times higher, 0.29 and 0.36 g m^–3 at Midway and Oahu, respectively. The major sources of the nitrate over the tropical South Pacific are still very uncertain. A very significant correlation between the nitrate concentrations at American Samoa and the concentrations of ²¹⁰Pb suggests that transport from continental sources might be important. This continental source could be lightning, which occurs most frequently over the tropical continents. A near-zero correlation with ⁷Be indicates that the stratosphere and upper troposphere are probably not the major sources. A significant biogenic source would be consistent with the higher mean nitrate concentrations, 0.16 to 0.17 g m^–3, found over the equatorial Pacific at Fanning Island (3°55N, 159°20W) and Nauru (0°32S, 166°57E). The lack of correlation between nitrate and nss sulfate at American Samoa does not necessarily preclude an important role for marine biogenic sources.     

Beryllium-7 Deposition and Its Relation to Sulfate Deposition

Deposition of ⁷Be, a cosmogenic radionuclide, was observed at the Meteorological Research Institute in Tsukuba, Japan from 1986 to 1993 and compared with those of several chemical species observed in Tsukuba over the same period. We found a correlation between the monthly depositions of ⁷ Be and SO ₄ ² -, a major acidic species. The correlation was especially strong for late spring and fall, when both species had high depositional fluxes. This correlation was also observed in precipitation samples collected daily in 1992 at the same site. The cause of this correlation is discussed in connection with the fact that the stratospheric aerosol is composed largely of SO ₄ ² -. ⁷ Be is produced in the upper atmosphere, and detection of ⁷Be, especially in spring and fall in Japan, can be regarded as detection of stratospheric aerosol. However, we conclude that the bulk of the SO ₄ ² - observed did not have a stratospheric or an upper tropospheric origin. The correlation, therefore, may present a new question regarding acidic deposition: Why does the deposition of stratospheric aerosol in Japan coincide with that of nss-SO ₄ ² - originally from anthropogenic sources on the Earth's surface?     

Characteristics of ionic components in precipitation in Kitakyushu City,Japan

Precipitation samples were collected by filtrating bulk sampler in Kitakyushu City, Japan, from January 1988 to December 1990. Volume weighted annual mean of pH was 4.93, but the pH distribution indicated that most probable value lay in the range pH 6.0–6.4. Volume weighted annual mean concentrations of major ionic components were as follows; SO ₄ ^2– : 84.2, NO ₃ ^– : 28.1, Cl^–: 86.3, NH ₄ ⁺ : 45.5, Ca²⁺: 63.3, Mg²⁺: 27.0, K⁺: 3.4, Na⁺: 69.0 µ eq l^–1. The highest concentrations of these ionic components were observed in winter and the lowest occurred in the rainy season. The ratio of ex-SO ₄ ^2– /NO ₃ ^– exhibited the lowest ratio in summer, and the highest ratio in winter. Good correlations were obtained between Cl^– and Na⁺, ex-SO ₄ ²⁺ and ex-Ca²⁺, NO ₃ ^– and ex-Ca²⁺, and NH ₄ ⁺ and ex-SO ₄ ^2– , respectively. However, no correlation between Cl^– and Na⁺ with Ca²⁺ was observed. The relationship of H⁺ with (ex-SO ₄ ^2– + NO ₃ ^– ) - (ex-Ca²⁺ + NH ₄ ⁺ ) indicated positive correlation.     

Free tropospheric reservoir of natural sulfate

¹⁰Be is used as a spike of the natural background atmospheric aerosol to calculate the global flux of sulfur (F_S) into the free troposphere. The sulfate and¹⁰Be concentrations determined in polar snow are compared. On the basis of an annual¹⁰Be production rate of 1.21 10⁶ at.cm^-2, a very low figure of 2.9 Tg S a^-1 is calculated for F_S, which suggests that most of the sulfur emitted at ground level remains in the boundary layer. The role of OCS in the upper tropospheric sulfur budget is reviewed. It is also shown that cataclysmic volcanic eruptions may disturb considerably for 1–2 years this vast background tropospheric sulfur reservoir.     

Measurements of stratospheric HO2 and NO2 by matrix isolation and ESR spectroscopy

Vertical profiles of stratospheric HO₂ and NO₂ concentrations were determined using matrix isolation and ESR. Up to 10 different samples per flight were collected in situ by a balloon borne cryosampler. Free radicals and trace constituents which are condensable at 68 K are trapped in a polycristalline H₂O or D₂O matrix. After collection, the samples are stored at a temperature below 83 K until they are analysed in the laboratory by X-band ESR spectroscopy at 4 K. The HO₂ and NO₂ were identified and calibrated by comparison with standard samples collected in the laboratory under typical stratospheric sampling conditions. From several flights over Southern France (44°N) we obtained two profiles of the stratospheric NO₂ mixing ratio. One, from 21 October 1982, agrees well with previous measurements. The other, from 8 October 1981, is lower by one order of magnitude. The few HO₂ data obtained around 35 km altitude agree with previous measurements. An isolated measurement at 17 km altitude is one order of magnitude higher than the model predicted HO₂ concentration.     

Vikings and virtues: a decade of CO2 taxation

Abstract

Experience with implementation of CO² taxes spans almost a decade in the Nordic countries, and time is ripe for an evaluation of their performance. In contrast to ex-ante forecasts, empirical research can show the extent to which such taxes deliver on the assumptions of economic theory. A survey of the existing literature shows that there are currently 20 ex-post studies of the full or partial effects of CO² taxes. Evaluations are complicated by frequent changes in tax rates, widespread exemptions and the ‘too many variables’ problem. Attempts have been made to deal with these problems by using a variety of approaches and research techniques, some more advanced than others. On balance the studies appear to show that emissions have been curbed when compared to businessas-usual forecasts, while absolute CO² reduction remains the exception. Among the Nordic countries, Denmark's scheme, which combines taxes with subsidies for energy efficiency, seems to have attained the most marked results, although the achieved reductions also reflect the higher carbon content of the Danish energy sector. The evaluations differ considerably in scope, approach and methodology. Methodological issues connected with expost evaluation are considered. An adequate evaluation of the impact of the CO² taxes, in both environmental and economic terms, will require the establishment of comprehensive panel databases of energy consumers.     

Satellite Measurements of Tropospheric Column O<Subscript>3</Subscript> and NO<Subscript>2</Subscript> in Eastern and Southeastern Asia: Comparison with a Global Model (MOZART-2)

Satellite measurements of tropospheric column O₃ and NO₂ in eastern and southeastern Asia are analyzed to study the spatial and seasonal characteristics of pollution in these regions. Tropospheric column O₃ is derived from differential measurements of total column ozone from Total Ozone Mapping Spectrometer (TOMS), and stratospheric column ozone from the Microwave Limb Sounder (MLS) instrument on the Upper Atmosphere Research Satellite (UARS). The tropospheric column NO₂ is measured by Global Ozone Monitoring Experiment (GOME). A global chemical and transport model (Model of Ozone and Related Chemical Tracers, version 2; MOZART-2) is applied to analyze and interpret the satellite measurements. The study, which is based on spring, summer, and fall months of 1997 shows generally good agreement between the model and satellite data with respect to seasonal and spatial characteristics of O₃ and NO₂ fields. The analysis of the model results show that the industrial emission of NO_x (NO + NO₂) contributes about 50%–80% to tropospheric column NO₂ in eastern Asia and about 20%–50% in southeastern Asia. The contribution of industrial emission of NO_x to tropospheric column O₃ ranges from 10% to 30% in eastern Asia. Biomass burning and lightning NO_x emissions have a small effect on tropospheric O₃ in central and eastern Asia, but they have a significant impact in southeastern Asia. The varying effects of NO_x on tropospheric column ozone are attributed to differences in relative abundance of volatile organic compounds (VOCs) with respect to total nitrogen in the two regions.     

Determination of carbon balances for smog chamber terpene oxidation experiments using a 14C tracer technique

In the last decade, numerous studies of monoterpene hydrocarbons in the presence of ozone and oxides of nitrogen have been completed. Although insights about the reactivity of terpenes have been gained, and several products have been identified in the gas and aerosol phases, carbon balances have been generally poor. This paper describes a radiotracer technique which accounts for carbon-containing compounds in a smog chamber at the conclusion of a photooxidation or ozonolysis reaction. Instead of attempting to identify individual products, gas-phase compounds were separated from aerosols, and each phase was analyzed by a liquid scintillation counter. A carbon balance of 79 to 97% was obtained with ¹⁴C--pinene and ozone using this technique. The significance of the results are discussed in terms of the ¹⁴C--pinene concentrations used in this study, which were lower than concentrations used previously by one to four orders of magnitude. In spite of the lower concentrations, the gaseous and aerosol fractions observed in the present investigation are comparable to those observed by others. Possible reaction products are discussed with respect to likely mechanisms for -pinene oxidation.     

天目山柳杉树轮δ13C对华东地区降水序列的重建

对采自天目山的柳杉树轮进行交叉定年后,得到树轮的δ¹³C年序列。将δ¹³C年序列去除大气CO₂的影响,保留其高频振荡部分。利用华东地区部分气象站的降水资料,通过主成份分析,分析了降水与树轮δ¹³C之间的关系。考虑滞后效应,利用回归方法重建了过去一百多年来的华东地区不同时段的降水序列,并分析其变化特征。     

冰芯中所记录的气候异常与ENSO事件

通过对３００ＢＰ以来记录于中国古里雅冰芯中的降水和δ１８Ｏ等环境气候信息记录及ＥＮ－ＳＯ事件的分析,发现ＥＮＳＯ的发生与古里雅降水异常显著相关。在厄尔尼诺年,古里雅冰芯中的降水与δ１８Ｏ均负异常,即ＥＮＳＯ与古里雅的降水偏少,温度偏低相联系。