Development of an online analyzer of atmospheric H2O2 and several organic hydroperoxides for field campaigns

An online automated instrument was developed for atmospheric measurements of hydroperoxides with separation and quantification of H₂O₂ and several organic hydroperoxides. Samples were trapped in aqueous solutions in a scrubbing glass coil. Analyses were performed on an HPLC column followed by para-hydroxyphenylacetic acid (POPHA) acetic acid and peroxidase derivatization and fluorescence detection. Analytical and sampling tests were performed on different parameters to obtain optimum signal-to-noise ratios, high resolution and collection efficiencies higher than 95% for H₂O₂ and organic hydroperoxides. The obtained performances show large improvements compared to previous studies. The sampling and analytical devices can be coupled providing an online analyzer. The device was used during two field campaigns in the Marseilles area in June 2001 (offline analyzer) and in July 2002 (online analyzer) at rural sites at low and high altitudes, respectively, during the ESCOMPTE and BOND campaigns. During the ESCOMPTE campaign, H₂O₂ was detected occasionally, and no organic hydroperoxides was observed. During the BOND campaign, substantial amounts of H₂O₂ and 1−HEHP+MHP were often detected, and two other organic hydroperoxides were occasionally detected. These observations are discussed.     

Laser depolarization studies of simulated crystallized H2O/H2SO4 clouds

Laboratory experiments were carried out to investigate the linear depolarization ratios (LDRs) of crystallized H₂O/H₂SO₄ acid clouds at angles of 45°, 135° and 157° to the forward direction. LDR is the ratio of the returned energies in the planes of polarization perpendicular and parallel to that of the source (Sassen, 1974). Experiments were carried out for different concentrations of aqueous solution of sulfuric acid. A cloud of supercooled droplets is formed inside an experimental chamber kept in a walk-in cold room by heating an aqueous solution of sulfuric acid, and the ice crystal formation is initiated by momentarily introducing a rod dipped in liquid nitrogen into the cloud. A 2-mW polarized He:Ne laser beam is directed through the cloud and a photomultiplier tube measures the scattered intensity. It is found that the scattered energy is higher in the direction of 157° and 135° than that at 45°. Microscopic examination of the crystals formed from acid concentrations above 50% shows dark fuzzy spots on the surface of the ice crystals suggesting that this could be a film of acid drops. This film also alters the shape of the crystals, and the crystal boundaries are no longer sharp and well defined like that observed for pure water clouds and this is found to influence the LDR.     

Influence of natural and anthropogenic activities on UV Index variations – a study over tropical urban region using ground based observations and satellite data

Measurements of total ozone column and solar UV radiation under different atmospheric conditions are needed to define variations of both UV and ozone and to study the impact of ozone depletion at the Earth’s surface. In this study, spectral and broadband measurements of UV-B irradiance were obtained along with total ozone observations and aerosol optical depth measurements in the tropical urban region of Hyderabad, south India. We specifically used an Ultra-Violet Multifilter Rotating Shadow band Radiometer (UVMFR-SR), to measure UV irradiance in time and space. To assess the aerosol and O₃ effects on ground-reaching UV irradiance, we used measurements from a Microtops II sun photometer in addition to the Tropospheric Ultraviolet Visible radiation (TUV) model. We also assessed the Defense Meteorological Satellite Program – Operational Line Scanner (DMSP-OLS) night time satellite data for inferring biomass burning fires during the study period. Results clearly suggested a negative correlation between the DMSP-OLS satellite derived fire count data and UVMFR-SR data suggesting that aerosols from biomass burning are directly attenuating UV irradiance in the study region. Also, correlation analysis between UV index and ozone measurements from sun photometer and TOMS-Ozone Mapping Instrument (OMI) indicated a clear decrease in ground reaching UV-B irradiance during higher ozone conditions. The higher levels are attributed to photochemical production of O₃ during the oxidation of trace gases emitted from biomass burning. Results also suggested a relatively high attenuation in UV irradiance (~6% higher) from smoke particles than dust. We also found a relatively good agreement between the modeled (TUV) and measured UV irradiance spectra for different atmospheric conditions. Our results highlight the factors affecting UV irradiance in a tropical urban environment, south India.     

长江三角洲地区净生态系统二氧化碳通量及浓度的数值模拟

净生态系统碳通量(NEE)的计算对于准确模拟区域碳通量和大气CO₂浓度的时空变化至关重要。本文利用中尺度大气-温室气体耦合模式WRF-GHG(Weather Research and Forecasting Model with Greenhouse Gases Module),对2010年7月28日至2010年8月2日期间影响长江三角洲地区大气CO₂浓度及时空分布的各种过程进行了详尽模拟。结果表明,植被光合呼吸模型(VPRM)能模拟不同植被下垫面NEE的日变化;WRF-GHG模拟的大气CO₂浓度日变化与观测相吻合,但低估了大气CO₂浓度5~15 ppm(ppm表示10-6),这可能与人为排放源的低估、VPRM参数的不确定性以及气象场模拟的不准确性有关。太湖和植被覆盖较好的地区如浙江北部山区是该地区的主要碳汇,而城市为CO₂的主要排放源。太湖和陆地生态系统对区域内碳循环起到一定的调节作用,减缓区域大气CO₂浓度的升高。此外,局地气象条件如湖陆风对太湖周边地区大气CO₂浓度有显著影响。     

京津冀周边秸秆燃烧对PM2.5无机组分影响

华北平原是我国主要农作物产区,田间秸秆焚烧现象普遍存在,选取秋收季节（2014年10月）分析了秸秆燃烧的排放特征,利用区域化学传输模型WRF-Chem模拟研究了燃烧排放对气态前体物及其氧化产物的影响,以及最终导致的PM_2.5中硫酸盐、硝酸盐和铵盐的变化。研究表明:2014年秋收季节,河南和山东等省份的秸秆燃烧排放会在东南风的输送作用下影响京津冀地区;秸秆燃烧排放大量挥发性有机物（VOCs）,导致火点源及周边地区大气中主要氧化剂浓度上升,提升了区域大气氧化能力;当携带大量VOCs的秸秆燃烧烟羽与以化石燃料排放为主的城市气团相混合时,大气氧化性增强会加速城市地区人为源排放的NO_x和SO₂等气态前体物的氧化过程,提高硫酸盐和硝酸盐的形成速率、促进二次无机气溶胶的生成。     

0-D-Modelling of Carbonaceous Aerosols over Greater Paris Focusing on the Organic Particle Formation

To improve our understanding of aerosol formation and ageing in urban atmospheres, we have tested the ORISAM 0-D aerosol module (ORganic and Inorganic Spectral Aerosol Model). This module accounts for both types of primary carbonaceous particles (black carbon BC and primary organic carbon OC_p) and also simulates the formation of secondary inorganic and organic particles (sulfates, nitrates, ammonium, water and secondary organic carbon particles OC_sec) by attachment of gas precursors to pre-existing carbonaceous particles. Simulations were performed for surface aerosols over Greater Paris area during the ESQUIF summer 1998 and winter 2000 experiments. Results show that OC_sec formation is highly dependent on temperature and insolation with more intense secondary formation in summer than in winter. Moreover in Summer, when atmospheric conditions shift from warm and humid to hot and dry, the model indicates a decreasing formation of secondary organic aerosols OC_sec as shown by an increase of the OC_p/(OC_p+OC_sec) ratio from 42 to 56%. These results satisfactorily compare with the few experimental available data for BC/(OC_p+OC_sec) ratios increasing from 24 to 37% against modelled values in the range 21–32%. ORISAM module sensitivity to initial size distributions, background concentrations and emissions of gases and primary carbonaceous particles was documented too. One main result is that the formation of secondary organic particles with ORISAM is very sensitive to the concentrations of gaseous precursors. At the present stage of ORISAM development, OC_sec build up appears to be however less sensitive to particulate background concentrations.     

Air pollutant emission rates and concentrations in medieval churches

A series of indoor air quality parameters were determined in two medieval churches, in Cyprus (temperature, relative humidity, total and UV solar radiation, CO₂ indoors and O₃, NO, NO₂ ^*, HNO₃ ^*, HCl, HCOOH, CH₃COOH indoors and outdoors). These data were used as input in a validated indoor air quality model to predict indoor air pollutant source strengths and species concentrations that resulted from dark or photochemical reactions. The NO and NO₂ emission rates due to the burning of incense or candles were estimated. Model results revealed that heterogeneous NO formation takes place simultaneously with the heterogeneous HONO formation. Also, model application has shown that indoor NO_x emissions resulted in decreased free radical concentrations, in contrast to the organic compound emissions, which increased free radical concentrations. This effect of indoor emissions on indoor radicals can partly explain the indoor enhancement/depression of indoor gaseous acid formation.     

Size-Resolved Aerosol Characterization for a Polluted Episode at the IfT Research Station Melpitz in Autumn 1997

Inorganic ions, organic carbon (OC), elemental carbon (EC) and a variety of organic single species in airborne particles have been determined at the research station of the Leibniz – Institut für Troposphärenforschung (IfT) in Melpitz (Germany) in autumn 1997.Samples of eight selected measurement events were divided in two groups in order to investigate differences in the chemical composition of particles originating from southwesterly (SW – developed EU countries) or from easterly directions (E – less developed eastern countries). Differences between these two groups were tested statistically by Student's t-test.Five stage cascade impactor samples show nitrate as most abundant in the accumulation mode in the SW group. EC and sulphate show the most abundant mass fractions in the E group. That can be considered as a consequence of domestic coal heating and coal-fired power plant emissions in the region of westerly Poland, northern Czech Republic and easterly Germany. Higher nitrate concentrations in the SW group can be explained by stronger NO _x emissions caused by the leeward plume of the conurbation of Leipzig, as well as by the still higher traffic density in western Germany.The methane sulphonic acid (MSA) mass fraction was higher for SW air masses in accumulation mode particles, probably indicating marine origin. Succinic acid also showed higher mass fractions for the SW group. This could be caused by primary emission in automobile exhaust gases and photochemical formation during transport from SW. Indeed, during SW sampling, solar radiation intensity was higher than during E sampling.The observed differences in the particle composition are an expression of the still existing technology gradient in Europe. Future campaigns could show the development to a joint economy with smaller differences in anthropogenic emissions.     

H2释放扰动电离层的数值模拟

由于电离层中分子性离子与电子的复合要比氧离子与电子的复合快得多,因此H₂在电离层高度释放可有效地引起电子的消耗。本文基于一个包括中性气体扩散方程和离子化学反应方程的二维动力学模型,对H₂在电离层高度释放过程进行了数值模拟研究,并分析了不同释放条件下的电子扰动特性。结果表明:1)500 mol H₂释放后,迅速向周围空间扩散,释放中心处的电子密度30 s内下降了近4%,F₂层临界频率下降了1%左右;2)在不同高度处释放H₂时,最大的电子密度相对变化率并不是在峰值高度附近处释放时出现的;3)释放化学物质的量越多,电子密度的扰动幅度也越大,但两者之间并不存在线性关系;4)相同量的H₂在电离层峰值高度处释放,白天的电子密度扰动幅度要大于夜间的扰动幅度。     

Atmospheric variability and binary homogeneous nucleation: A parametrisation and conditions required for a significant effect

The binary water–sulphuric acid nucleation has long been considered an important path for new particle formation in the atmosphere. The formation rate depends nonlinearly on temperature and vapour concentrations. We aim to find out if atmospheric small scale and mesoscale spatial and temporal variability can increase the nucleation rate significantly. Simultaneous and separate effects of variation in temperature, humidity and sulphuric acid concentration on the mean nucleation rate have been modelled. We have assumed that the distributions of variables are Gaussian and compare the mean of simulated nucleation rates with the nucleation rate in mean conditions without variation. According to our studies the atmospheric variability can increase the mean nucleation rate by orders of magnitude but the significant effect is limited to specific conditions. The effect seems to be more important in the lower troposphere than in the upper troposphere, where temperature and sulphuric acid concentrations are lower. In addition, our model simulations indicate that the atmospheric variability can only explain part of the difference between measured and theoretically required sulphuric acid concentrations in conditions where particle formation has been observed. We have parametrised the effect of atmospheric variability as a simple correction factor for the effect of temperature and humidity variation.     

A Perspective on the Evolution of Atmospheric Blocking Theories: From Eddy-Mean flow Interaction to Nonlinear Multiscale Interaction

In this paper, we first review the research advancements in blocking dynamics and highlight the merits and drawbacks of the previous theories of atmospheric blocking. Then, the dynamical mechanisms of atmospheric blocking are presented based on a nonlinear multi-scale interaction(NMI) model. Previous studies suggested that the eddy deformation(e.g., eddy straining, wave breaking, and eddy merging) might lead to the formation and maintenance of atmospheric blocking.However, the results were specu...     

人为大气污染物对一次冬季浓雾形成发展的影响研究

基于WRF/Chem模式和雾的观测资料,开展了包含和不包含人为污染排放源两种大气背景条件下的数值模拟对比试验,在此基础上探讨了人为污染物对2009年12月1日发生在我国华北和华东地区的一次浓雾天气过程的影响机理.结果表明,在考虑污染排放源时,模式模拟的雾的空间分布和强度变化与卫星、能见度仪和微波辐射计的观测更为接近.污...     

Atmospheric variability and binary homogeneous nucleation: A parametrisation and conditions required for a significant effect

The binary water–sulphuric acid nucleation has long been considered an important path for new particle formation in the atmosphere. The formation rate depends nonlinearly on temperature and vapour concentrations. We aim to find out if atmospheric small scale and mesoscale spatial and temporal variability can increase the nucleation rate significantly. Simultaneous and separate effects of variation in temperature, humidity and sulphuric acid concentration on the mean nucleation rate have been modelled. We have assumed that the distributions of variables are Gaussian and compare the mean of simulated nucleation rates with the nucleation rate in mean conditions without variation. According to our studies the atmospheric variability can increase the mean nucleation rate by orders of magnitude but the significant effect is limited to specific conditions. The effect seems to be more important in the lower troposphere than in the upper troposphere, where temperature and sulphuric acid concentrations are lower. In addition, our model simulations indicate that the atmospheric variability can only explain part of the difference between measured and theoretically required sulphuric acid concentrations in conditions where particle formation has been observed. We have parametrised the effect of atmospheric variability as a simple correction factor for the effect of temperature and humidity variation.     

Long-term effects of anthropogenic CO<Subscript>2</Subscript> emissions simulated with a complex earth system model

A new complex earth system model consisting of an atmospheric general circulation model, an ocean general circulation model, a three-dimensional ice sheet model, a marine biogeochemistry model, and a dynamic vegetation model was used to study the long-term response to anthropogenic carbon emissions. The prescribed emissions follow estimates of past emissions for the period 1751–2000 and standard IPCC emission scenarios up to the year 2100. After 2100, an exponential decrease of the emissions was assumed. For each of the scenarios, a small ensemble of simulations was carried out. The North Atlantic overturning collapsed in the high emission scenario (A2) simulations. In the low emission scenario (B1), only a temporary weakening of the deep water formation in the North Atlantic is predicted. The moderate emission scenario (A1B) brings the system close to its bifurcation point, with three out of five runs leading to a collapsed North Atlantic overturning circulation. The atmospheric moisture transport predominantly contributes to the collapse of the deep water formation. In the simulations with collapsed deep water formation in the North Atlantic a substantial cooling over parts of the North Atlantic is simulated. Anthropogenic climate change substantially reduces the ability of land and ocean to sequester anthropogenic carbon. The simulated effect of a collapse of the deep water formation in the North Atlantic on the atmospheric CO₂ concentration turned out to be relatively small. The volume of the Greenland ice sheet is reduced, but its contribution to global mean sea level is almost counterbalanced by the growth of the Antarctic ice sheet due to enhanced snowfall. The modifications of the high latitude freshwater input due to the simulated changes in mass balance of the ice sheet are one order of magnitude smaller than the changes due to atmospheric moisture transport. After the year 3000, the global mean surface temperature is predicted to be almost constant due to the compensating effects of decreasing atmospheric CO₂ concentrations due to oceanic uptake and delayed response to increasing atmospheric CO₂ concentrations before.     

Biogenic hydrogen sulphide emissions and non-sea sulfate aerosols over the Indian Sundarban mangrove forest

Temporal variations in atmospheric hydrogen sulphide concentrations and its biosphere-atmosphere exchanges were studied in the World’s largest mangrove ecosystem, Sundarbans, India. The results were used to understand the possible contribution of H₂S fluxes in the formation of atmospheric aerosol of different size classes (e.g. accumulation, nucleation and coarse mode). The mixing ratio of hydrogen sulphide (H₂S) over the Sundarban mangrove atmosphere was found maximum during the post-monsoon season (October to January) with a mean value of 0.59?±?0.02 ppb and the minimum during pre-monsoon (February to May) with a mean value of 0.26?±?0.01 ppb. This forest acted as a perennial source of H₂S and the sediment-air emission flux ranged between 1213?±?276 μg S m^?2 d^?1(December) and 457?±?114 μg S m^?2 d^?1 (August) with an annual mean of 768?±?240 μg S m^?2d^?1. The total annual emissions of H₂S from the Indian Sundarban were estimated to be 1.2?±?0.6 Tg S. The accumulation mode of aerosols was found to be more enriched with non-sea salt sulfate with an average loading of 5.74 μg m^?3 followed by the coarse mode (5.18 μg m^?3) and nucleation mode (1.18 μg m^?3). However, the relative contribution of Non-sea salt sulfate aerosol to total sulfate aerosol was highest in the nucleation mode (83%) followed by the accumulation (73%) and coarse mode (58%). Significant positive relations between H₂S flux and different modes of NSS indicated the likely link between H₂S, a dominant precursor for the non-sea salt sulfate, and non-sea sulfate aerosol particles. An increase in H₂S emissions from the mangrove could result in an increase in enhanced NSS in aerosol and associated cloud albedo, and a decrease in the amount of incoming solar radiation reaching the Sundarban mangrove forest.     

Comparison of PM2.5 and CO2 Concentrations in Large Cities of China during the COVID-19 Lockdown

Estimating the impacts on PM_2.5pollution and CO₂emissions by human activities in different urban regions is important for developing efficient policies.In early 2020,China implemented a lockdown policy to contain the spread of COVID-19,resulting in a significant reduction of human activities.This event presents a convenient opportunity to study the impact of human activities in the transportation and industrial sectors on air pollution.Here,we investigate the variations in air quality attributed to the COVID-19 lockdown policy in the megacities of China by combining in-situ environmental and meteorological datasets,the Suomi-NPP/VIIRS and the CO₂emissions from the Carbon Monitor project.Our study shows that PM_2.5concentrations in the spring of 2020 decreased by 41.87%in the Yangtze River Delta(YRD)and 43.30%in the Pearl River Delta(PRD),respectively,owing to the significant shutdown of traffic and manufacturing industries.However,PM_2.5concentrations in the Beijing-Tianjin-Hebei(BTH)region only decreased by 2.01%because the energy and steel industries were not fully paused.In addition,unfavorable weather conditions contributed to further increases in the PM_2.5concentration.Furthermore,CO₂concentrations were not significantly affected in China during the short-term emission reduction,despite a 19.52%reduction in CO₂emissions compared to the same period in 2019.Our results suggest that concerted efforts from different emission sectors and effective long-term emission reduction strategies are necessary to control air pollution and CO₂emissions.     

RESPONSES OF A GLOBAL CGCM TO CO2 INCREASE

The responses of the climate system to increase of atmospheric carbon dioxide(CO₂)arestudied by using a new version of the Bureau of Meteorological Research Centre(BMRC)globalcoupled general circulation model(CGCM).Two simulations are run:one with atmospheric CO₂concentration held constant at 330 ppm,the other with a tripling of atmospheric CO₂(990 ppm).Results from the 41-year control coupled integration are applied to analyze the mean state,seasonal cycle and interannual variability in the model.Comparisons between the greenhouseexperiment and the control experiment then provide estimations of the influence of increased CO₂on climate changes and climate variability.Especially discussed is the question on whether theclimate changes concerned with CO₂ inerease will impact interannual variability in tropical Pacific,such as ENSO.     

A Model to Estimate Global Radiation in Complex Terrain

Global radiation is an important parameter necessary for most ecological models. However, in situ data barely meets the needs of modelling mountainous ecosystems since most field stations are located in flat areas. Consequently, it is usually necessary to extrapolate radiation measurements obtained from an adjacent flat area to the complex terrain of concern. The distribution of radiation in complex terrain depends upon two factors: the local atmospheric conditions, which determine the radiation potentially available to a supposed flat surface in a given location, and the topographic effects on this possible radiation. The latter have been included in detail in most radiation models for complex terrain, but the former are often only simply treated as constant or estimated by over-simplified empirical algorithms. In this paper we propose a novel model that uses a parametric atmospheric model to calculate the potential radiation for a supposed flat surface in a given location, and then account for topographic effects. Direct radiation, diffuse radiation and reflected radiation are calculated separately in the model due to the distinctive characteristics of and the effects by topography. Based on the parametric model, this paper has investigated the relationship between radiation transmittance, clearness indices and altitude under a series of water vapour content and turbidity conditions. This combines three ratios, R _b, R _d, and R _r, defined as the direct radiation, diffuse radiation and reflected radiation received by the arbitrary surface, respectively, to their counterparts in the horizontal surface, to estimate the global radiation for any given location. The model has been validated with data from measurements in National Park Berchtesgaden, Germany, where six measurement sites with various altitudes and topographic characteristics have been deployed. The r ² of modelled and measured hourly global radiation are greater than 0.90 in all six sites, with RMSE varies from 16 to 100 W m⁻². Sensitivity analysis revealed that the model was not sensitive to change in water vapour content, which suggests the possibility to use an exponential algorithm of water vapour content when there is no in situ water vapour content information in complex terrains. The NRMSE was only reduced by 0.04, on average, in five of the six sites when water vapour content information was calculated from the in situ air temperature and relative humidity measurements.     

东亚地区二氧化碳体积分数变化特征

利用2004年以来东亚地区10个本底观测站大气φ(CO₂)观测资料,分析了各站大气φ(CO₂)的变化特征及其各站之间的差异,讨论了下垫面特征、源汇作用等对φ(CO₂)变化的影响.结果表明:10个本底站大气月均φ(CO₂)有明显的季节变化,高值多出现在冬春等寒冷季节,而低值则多出现在6—9月,属于北半球的夏季;大气φ(CO₂)日变化趋势较为一致,15时(当地时间)前后达到全天最低,随后φ(CO₂)升高,并在日落后继续积累,至清晨7时(当地时间)前后达到全天最高,之后φ(CO₂)随着太阳辐射的增强而逐渐降低,且平均φ(CO₂)水平与下垫面植被量成反比,φ(CO₂)日变化的幅度与下垫面植被量成反比.作为全球基准站之一的瓦里关山站,2004—2008年φ(CO₂)年均值逐年增加,年增长率为2.28×10^-6/a.     

Managing atmospheric CO2

A coupled carbon cycle-climate model is used to compute global atmospheric CO₂ and temperature variation that would result from several future CO₂ emission scenarios. The model includes temperature and CO₂ feedbacks on the terrestrial biosphere, and temperature feedback on the oceanic uptake of CO₂. The scenarios used include cases in which fossil fuel CO₂ emissions are held constant at the 1986 value or increase by 1% yr^–1 until either 2000 or 2020, followed by a gradual transition to a rate of decrease of 1 or 2% yr^–1. The climatic effect of increases in non-CO₂ trace gases is included, and scenarios are considered in which these gases increase until 2075 or are stabilized once CO₂ emission reductions begin. Low and high deforestation scenarios are also considered. In all cases, results are computed for equilibrium climatic sensitivities to CO₂ doubling of 2.0 and 4.0 °C.Peak atmospheric CO₂ concentrations of 400–500 ppmv and global mean warming after 1980 of 0.6–3.2 °C occur, with maximum rates of global mean warming of 0.2–0.3 °C decade^–1. The peak CO₂ concentrations in these scenarios are significantly below that commonly regarded as unavoidable; further sensitivity analyses suggest that limiting atmospheric CO₂ to as little as 400 ppmv is a credible option.Two factors in the model are important in limiting atmospheric CO₂: (1) the airborne fraction falls rapidly once emissions begin to decrease, so that total emissions (fossil fuel + land use-induced) need initially fall to only about half their present value in order to stabilize atmospheric CO₂, and (2) changes in rates of deforestation have an immediate and proportional effect on gross emissions from the biosphere, whereas the CO₂ sink due to regrowth of forests responds more slowly, so that decreases in the rate of deforestation have a disproportionately large effect on net emission.If fossil fuel emissions were to decrease at 1–2% yr^–1 beginning early in the next century, emissions could decrease to the rate of CO₂ uptake by the predominantly oceanic sink within 50–100 yrs. Simulation results suggest that if subsequent emission reductions were tied to the rate of CO₂ uptake by natural CO₂ sinks, these reductions could proceed more slowly than initially while preventing further CO₂ increases, since the natural CO₂ sink strength decreases on time scales of one to several centuries. The model used here does not account for the possible effect on atmospheric CO₂ concentration of possible changes in oceanic circulation. Based on past rates of atmospheric CO₂ variation determined from polar ice cores, it appears that the largest plausible perturbation in ocean-air CO₂ flux due to changes of oceanic circulation is substantially smaller than the permitted fossil fuel CO₂ emissions under the above strategy, so tieing fossil fuel emissions to the total sink strength could provide adequate flexibility for responding to unexpected changes in oceanic CO₂ uptake caused by climatic warming-induced changes of oceanic circulation.