Diurnal variation of CO2 concentration, Δ14C and δ13C in an urban forest: estimate of the anthropogenic and biogenic CO2 contributions

Diurnal variation in the atmospheric CO₂ concentration and the carbon isotopic composition (Δ¹⁴C and δ¹³C) was measured in a forest in an urban area on 9 February 1999. The carbon isotope approach used in the present study differentiated between the quantitative contributions from anthropogenic and biogenic CO₂ sources in the urban atmosphere. The anthropogenic (fossil fuel) and biogenic (soil respiration) contributions was estimated, and they ranged from 1 to 16% and from 2 to 8% of the total atmospheric CO₂. The diurnal variation of the anthropogenic CO₂ was the major cause of the total atmospheric CO₂ variation, while the biogenic CO₂ remained relatively constant throughout the day. Estimating the contribution of soil respired CO₂ provided the mean residence time of soil respired CO₂ within the forest atmosphere.     

Isotopic composition and origin of polar precipitation in present and glacial climate simulations

The Hamburg atmospheric general circulation model (AGCM) ECHAM‐4 is used to identify the main source regions of precipitation falling on Greenland and Antarctica. Both water isotopes H₂¹⁸O and HDO are explicitly built into the water cycle of the AGCM, and in addition the capability to trace water from different source regions was added to the model. Present and LGM climate simulations show that water from the most important source regions has an isotopic signature similar to the mean isotope values of the total precipitation amount. But water from other source regions (with very different isotopic signatures) contributes an additional, non‐negligible part of the total precipitation amount on both Greenland and Antarctica. Analyses of the temperature‐isotope‐relations for both polar regions reveal a solely bias of the glacial isotope signal on Greenland, which is caused by a strong change in the seasonal deposition of precipitation originating from nearby polar seas and the northern Atlantic. Although the performed simulations under LGM boundary conditions show a decrease of the δ ¹⁸O values in precipitation in agreement with ice core measurements, the AGCM fails to reproduce the observed simultaneous decrease of the deuterium excess signal.     

Sulfur (32S, 33S, 34S, 36S) and oxygen (16O,17O,18O) isotopic ratios of primary sulfate produced from combustion processes

The recent discovery of an anomalous enrichment in ¹⁷O isotope in atmospheric sulfate has opened a new way to investigate the oxidation pathways of sulfur in the atmosphere. From laboratory investigations, it has been suggested that the wet oxidation of sulfur in rain droplets was responsible for the excess ¹⁷O. In order to confirm this theory, sulfur and oxygen isotope ratios of different primary sulfates produced during fossil fuel combustion have been investigated and are reported. None of these samples exhibits any anomalous oxygen or sulfur isotopic content, as compared to urban sulfate aerosols. These results, in agreement with the laboratory investigations, reinforce the idea of an aqueous origin for the oxygen-17 anomaly found in tropospheric sulfates.     

Vertical profiles of biospheric and fossil fuel-derived CO2 and fossil fuel CO2 : CO ratios from airborne measurements of Δ14C, CO2 and CO above Colorado, USA

Measurements of  Δ¹⁴C  in atmospheric CO₂ are an effective method of separating CO₂ additions from fossil fuel and biospheric sources or sinks of CO₂. We illustrate this technique with vertical profiles of CO₂ and  Δ¹⁴C  analysed in whole air flask samples collected above Colorado, USA in May and July 2004. Comparison of lower tropospheric composition to cleaner air at higher altitudes (>5 km) revealed considerable additions from respiration in the morning in both urban and rural locations. Afternoon concentrations were mainly governed by fossil fuel emissions and boundary layer depth, also showing net biospheric CO₂ uptake in some cases. We estimate local industrial CO₂:CO emission ratios using in situ measurements of CO concentration. Ratios are found to vary by 100% and average 57 mole CO₂:1 mole CO, higher than expected from emissions inventories. Uncertainty in CO₂ from different sources was ±1.1 to ±4.1 ppm for addition or uptake of −4.6 to 55.8 ppm, limited by  Δ¹⁴C  measurement precision and uncertainty in background  Δ¹⁴C  and CO₂ levels.     

Excess 210Po in the coastal atmosphere

Many researchers have reported the widespread occurrence of excess ²¹⁰ Po in the global atmosphere and suggested probable sources such as resuspension of top soils, stratospheric aerosols, sea spray of the surface micro‐layer, volcanic emission, and bio‐volatile ²¹⁰Po species from the productive ocean. We have observed excess ²¹⁰Po on aerosols in the coastal atmosphere of the Chesapeake and Delaware Bays. On‐board measurements in the Chesapeake Bay atmosphere show that the increase of this excess ²¹⁰Po is dependent upon wind speed. Simultaneously measured activity ratios of ⁷Be/²¹⁰Pb and ²¹⁰Pb/²²²Rn argue against either higher altitude air or continental soils as the source of this excess. We hypothesize that the excess ²¹⁰Po originates mainly from surface waters either by the sea‐spray of the surface microlayer, or more likely, by gas exchange. We conclude gas exchange as the mechanism since the polonium excess increases linearly with wind speed over a threshold of 3 m s⁻¹(mean) similar to other gases (i.e., CO₂, SF₆ , and DMS). In addition, higher ²¹⁰Po excess with lower ²²²Rn is observed in on‐shore marine air at Lewes, DE. This suggests sea‐air exchange of volatile Po along with other bio‐volatile species (i.e., DMS, DMSe, and MMHg) in the coastal productive ocean during high wind speeds.     

Aerosol modulation of atmospheric and surface solar heating over the tropical Indian Ocean

The major finding of this study is that aerosols over the tropical Indian Ocean enhance clear sky atmospheric solar heating significantly and decrease the surface solar heating by even a larger amount. The results presented here are based on aerosol chemical, microphysical, and optical and radiometric data collected at the island of Kaashidhoo (4.97°N, 73.47°E) during February and March of 1998, as part of the first field phase of the Indian Ocean experiment (INDOEX). The aerosol optical properties were integrated with a multiple scattering Monte Carlo radiative transfer model which was validated at the surface with broadband flux measurements and at the top of the atmosphere (TOA) with the clouds and earth's radiant energy system (CERES) radiation budget measurements. We consider both externally and internally mixed aerosol models with very little difference between the two models in the estimated forcing. For the February–March period, the aerosols increase the monthly mean clear sky atmospheric solar heating by about 12 W/m²(about 15% of the total atmospheric solar heating) and decrease the sea surface clear sky solar heating by about 16 W/m² with a daily range from 5 to 23 W/m². The net aerosol forcing at the top of the atmosphere is about −4 W/m² with a daily range from −2 to −6 W/m². Although the soot contributes only about 10% to the aerosol optical thickness, it contributes more than 50% to the aerosol induced atmospheric solar heating. The fundamental conclusion of this study is that anthropogenic aerosols over the tropical Indian Ocean are altering the clear sky radiation budget of the atmosphere and surface in a major manner.     

The cold event 8200 years ago documented in oxygen isotope records of precipitation in Europe and Greenland

 Stable oxygen isotope ratios of ostracod valves in Late Glacial and Holocene sediments of core AS 92-5 from deep lake Ammersee (southern Germany) reflect variations of mean oxygen isotope ratios in past atmospheric precipitation. The record reconfirms the strong similarity of climate evolution in Europe and Greenland during the last deglaciation. For the first time in Europe, we find a 200-year-long negative δ¹⁸O-excursion, which is contemporaneous with the strongest negative δ¹⁸O-excursion in the Greenland ice around 8.2 ky before present. The 8.2 ky isotopic event on both sides of the North Atlantic ocean is interpreted as a cold period, most probably induced by a perturbation of the North Atlantic thermohaline circulation. We discuss two possible triggering mechanisms: (1) weak forcing (as proposed by Alley et al.), and (2) forcing by a strong and sudden freshwater pulse from the collapse of the Hudson Ice Dome. Received: 27 May 1997 / Accepted: 21 July 1997     

Spring Arctic Oscillation-East Asian summer monsoon connection through circulation changes over the western North Pacific

In the present study the links between spring Arctic Oscillation (AO) and East Asian summer monsoon (EASM) was investigated with focus on the importance of the North Pacific atmospheric circulation and sea surface temperature (SST). To reduce the statistical uncertainty, we analyzed high-pass filtered data with the inter-annual time scales, and excluded the El Ni?o/Southern Oscillation signals in the climate fields using a linear fitting method. The significant relationship between spring AO and EASM are supported by the changes of multi-monsoon components, including monsoon indices, precipitation, and three-dimensional atmospheric circulations. Following a stronger positive spring AO, an anomalous cyclonic circulation at 850?hPa appears in southeastern Asia and the western North Pacific in summer, with the easterly anomalies spanning from the Pacific to Asian continent along 25°N?C30°N and the westerly anomalies south of 15°N. At the same time, the summer western North Pacific subtropical high becomes weaker. Consistently, the positive precipitation anomalies are developed over a broad region south of 30°N stretching from southern China to the western Pacific and the negative precipitation anomalies appear in the lower valley of the Yangtze River and southern Japan. The anomalous cyclone in the western North Pacific persisting from spring to summer plays a key role in modulating EASM and monsoon precipitation by a positive air-sea feedback mechanism. During spring the AO-associated atmospheric circulation change produces warmer SSTs between 150°E?C180° near the equator. The anomalous sensible and latent heating, in turn, intensifies the cyclone through a Gill-type response of the atmosphere. Through this positive feedback, the tropical atmosphere and SST patterns sustain their strength from spring to summer, that consequently modifies the monsoon trough and the western North Pacific subtropical high and eventually the EASM precipitation. Moreover, the SST response to AO-circulation is supported by the numerical simulations of an ocean model, and the anomalous atmospheric circulation over the western North Pacific is also reproduced by the dedicated numerical simulations using the coupled atmosphere?Cocean model. The observation evidence and numerical simulations suggest the spring AO can impact the EASM via triggering tropical air-sea feedback over the western North Pacific.     

Potential impact of climate change on marine dimethyl sulfide emissions

Dimethyl sulfide (DMS) is a biogenic compound produced in sea-surface water and outgased to the atmosphere. Once in the atmosphere, DMS is a significant source of cloud condensation nuclei in the unpolluted marine atmosphere. It has been postulated that climate may be partly modulated by variations in DMS production through a DMS-cloud condensation nuclei-albedo feedback. We present here a modelled estimation of the response of DMS sea-water concentrations and DMS fluxes to climate change, following previous work on marine DMS modeling ( Aumont et al., 2002 ) and on the global warming impact on marine biology ( Bopp et al., 2001 ). An atmosphere–ocean general circulation model (GCM) was coupled to a marine biogeochemical scheme and used without flux correction to simulate climate response to increased greenhouse gases (a 1% increase per year in atmospheric CO₂ until it has doubled). The predicted global distribution of DMS at  1 × CO₂  compares reasonably well with observations; however, in the high latitudes, very elevated concentrations of DMS due to spring and summer blooms of Phaeocystis can not be reproduced. At  2 × CO₂  , the model estimates a small increase of global DMS flux to the atmosphere (+2%) but with large spatial heterogeneities (from −15% to +30% for the zonal mean). Mechanisms affecting DMS fluxes are changes in (1) marine biological productivity, (2) relative abundance of phytoplankton species and (3) wind intensity. The mean DMS flux perturbation we simulate represents a small negative feedback on global warming; however, the large regional changes may significantly impact regional temperature and precipitation patterns.     

Seasonal variations in the isotopic composition of near-surface water vapour in the eastern Mediterranean

Although the isotopic composition of precipitation is widely used in global climate change studies, use of water vapour isotopes is considerably more limited. Here we present the results from 9 yr of atmospheric vapour measurements in the Eastern Mediterranean, at a site in Israel. The measurements show a strong mean seasonal cycle of about 4‰ in ¹⁸O (peaking around July). This seasonality could not be adequately explained by changes in surface interactions or in air mass trajectories, as usually invoked for variations in local precipitation. We could explain this cycle only as a combination of three components: (1) rainout effects; (2) temperature and relative humidity control of the initial vapour and (3) seasonal variations in the vertical mixing across the top of the planetary boundary layer. This last component is emphasized in the current study, and it was shown to be a significant factor in the seasonal cycle features. The measurements were also compared with an isotope-enabled GCM (CAM2) run, which exhibited a markedly different seasonal cycle. Such comparisons with vapour isotopes data could help in constraining models better.     

In situ produced 14C by cosmic ray muons in ablating Antarctic ice

Samples of a core (52 m) of ablating Antarctic ice were analysed for ¹⁴CO and ¹⁴CO₂ by accelerator mass spectrometry. The data were compared with a ¹⁴C in situ production model that includes muon capture in addition to oxygen spallation by neutrons. The analysis reveals significant in situ ¹⁴C at depths below 10 m, which we attribute to ¹⁴C production by cosmic ray muons. The age of the ice was determined as 9.3±0.4 ¹⁴C ka BP.     

Variations of atmospheric nitrous oxide concentration in the northern and western Pacific

Atmospheric N₂O concentration was observed in the Pacific for the period 1991–2006, using commercial container ships sailing between Japan and North America and between Japan and Australia or New Zealand. The N₂O concentration showed a secular increase and interannual variations at all sampling locations, but a seasonal cycle was detectable only at northern high latitudes. The annual mean N₂O concentration showed little longitudinal variations (within ± 0.3 ppb) in the northern Pacific, but showed a clear north-south gradient of about 0.8 ppb, with higher values in the Northern Hemisphere. The annual mean N₂O was also characterized by especially high values at 30°N due to strong local N₂O emissions and by a steep latitudinal decrease from the equator to 20°S due to the suppression of interhemispheric exchange of air by the South Pacific Convergence Zone. The N₂O growth rate showed an interannual variation with a period of about 3 yr (high-values in 1999 and 2000), with a delayed eastward and poleward phase propagation in the northern and western Pacific, respectively. The interannual variations of the N₂O growth rate and soil water showed a good correlation, suggesting that the N₂O emission from soils have an important causative role in the atmospheric N₂O variation.     

Wet‐only sequential deposition in a rural area in north‐eastern Spain

The present work summarises the results of a 2‐year study of wet‐only sequential deposition in 2 rural areas (Alcan¯iz and Morella) located at different distances from a large coal‐fired power station. Precipitation chemistry was characterised by relatively high , Ca²⁺ and average concentrations. Sequential study of single precipitation events showed that concentrations of most of the ions studied decreased exponentially throughout single precipitation events, with a sharper decrease in concentrations at the beginning of the event. Usually, 40 to 80% of the wet‐only deposition of major ions occurred in the first 2 mm. pH measurements, ranging from 5.6 to 8.1, showed a decrease in the pH values throughout a precipitation event. Deposition levels of Ca²⁺ and accounted for the neutralisation of major acidic species in the precipitation events except in 5 rain episodes sampled at Morella. The sequential study of the evolution of the ratio during a single precipitation allowed us to identify potential acidic rainfall fractions after an initial volume of precipitation, after most of the Ca²⁺ in atmospheric particles had been scavenged. A higher neutralisation capacity was deduced for Alcan¯iz owing to the higher atmospheric levels of natural carbonates and .     

东亚-北太平洋副热带海气耦合模态及其对降水的影响

利用53年的NCEP/NCAR再分析资料和英国气象局Hadley气候预测和研究中心的海表面温度资料,使用SVD方法研究了东亚-北太平洋地区表层海温(SST)异常与大气环流异常间的主要耦合模态.分析结果表明,中纬度北太平洋地区存在两种主要的海-气耦合模态,第一模态是海温异常分布的纬向型,第二模态主要表现为经向海温差异分布.两种空间耦合模态共同反映出中纬度北太平洋地区大气和海洋的异常中心有很强的局地耦合性.在第一模态的正(负)异常年,东亚-北太平洋地区主要为负(正)的降水异常,在第二模态的正(负)异常年,东亚和北太平洋的大部分地区出现降水正(负)异常,北美西岸及以西的部分区域出现降水的负(正)异常.两个模态所对应的降水差异显示,海气耦合模态的循环变化有利于形成我国降水分布南北差异的改变.     

Feedback mechanisms and sensitivities of ocean carbon uptake under global warming

Global warming simulations are performed with a coupled climate model of reduced complexity to investigate global warming–marine carbon cycle feedbacks. The model is forced by emissions of CO₂ and other greenhouse agents from scenarios recently developed by the Intergovernmental Panel on Climate Change and by CO₂ stabilization profiles. The uptake of atmospheric CO₂ by the ocean is reduced between 7 to 10% by year 2100 compared to simulations without global warming. The reduction is of similar size in the Southern Ocean and in low‐latitude regions (32.5°S‐32.5°N) until 2100, whereas low‐latitude regions dominate on longer time scales. In the North Atlantic the CO₂ uptake is enhanced, unless the Atlantic thermohaline circulation completely collapses. At high latitudes, biologically mediated changes enhance ocean CO₂ uptake, whereas in low‐latitude regions the situation is reversed. Different implementations of the marine biosphere yield a range of 5 to 16% for the total reduction in oceanic CO₂ uptake until year 2100. Modeled oceanic O₂ inventories are significantly reduced in global warming simulations. This suggests that the terrestrial carbon sink deduced from atmospheric O₂/N₂ observations is potentially overestimated if the oceanic loss of O₂ to the atmosphere is not considered.     

The role of ocean dynamics in producing decadal climate variability in the North Pacific

 Decadal time scale climate variability in the North Pacific has implications for climate both locally and over North America. A crucial question is the degree to which this variability arises from coupled ocean/atmosphere interactions over the North Pacific that involve ocean dynamics, as opposed to either purely thermodynamic effects of the oceanic mixed layer integrating in situ the stochastic atmospheric forcing, or the teleconnected response to tropical variability. The part of the variability that is coming from local coupled ocean/atmosphere interactions involving ocean dynamics is potentially predictable by an ocean/atmosphere general circulation model (O/A GCM), and such predictions could (depending on the achievable lead time) have distinct societal benefits. This question is examined using the results of fully coupled O/A GCMs, as well as targeted numerical experiments with stand-alone ocean and atmosphere models individually. It is found that coupled ocean/atmosphere interactions that involve ocean dynamics are important to determining the strength and frequency of a decadal-time scale peak in the spectra of several oceanic variables in the Kuroshio extension region off Japan. Local stochastic atmospheric heat flux forcing, integrated by the oceanic mixed layer into a red spectrum, provides a noise background from which the signal must be extracted. Although teleconnected ENSO responses influence the North Pacific in the 2–7 years/cycle frequency band, it is shown that some decadal-time scale processes in the North Pacific proceed without ENSO. Likewise, although the effects of stochastic atmospheric forcing on ocean dynamics are discernible, a feedback path from the ocean to the atmosphere is suggested by the results. Received: 23 January 2000 / Accepted: 10 January 2001     

An intimate coupling of ocean–atmospheric interaction over the extratropical North Atlantic and Pacific

The inter-basin teleconnection between the North Atlantic and the North Pacific ocean–atmosphere interaction is studied using a coupled ocean–atmosphere general circulation model. In the model, an idealized oceanic temperature anomaly is initiated over the Kuroshio and the Gulf Stream extension region to track the coupled evolution of ocean and atmosphere interaction, respectively. The experiments explicitly demonstrate that both the North Pacific and the North Atlantic ocean–atmosphere interactions are intimately coupled through an inter-basin atmospheric teleconnection. This fast inter-basin communication can transmit oceanic variability between the North Atlantic and the North Pacific through local ocean-to-atmosphere feedbacks. The leading mode of the extratropical atmospheric internal variability plays a dominant role in shaping the hemispheric-scale response forced by oceanic variability over the North Atlantic and Pacific. Modeling results also suggest that a century (two centuries) long observations are necessary for the detection of Pacific response to Atlantic forcings (Atlantic response to Pacific forcing).     

Vertical distributions of sulfur species simulated by large scale atmospheric models in COSAM: Comparison with observations

A comparison of large‐scale models simulating atmospheric sulfate aerosols (COSAM) was conducted to increase our understanding of global distributions of sulfate aerosols and precursors. Earlier model comparisons focused on wet deposition measurements and sulfate aerosol concentrations in source regions at the surface. They found that different models simulated the observed sulfate surface concentrations mostly within a factor of two, but that the simulated column burdens and vertical profiles were very different amongst different models. In the COSAM exercise, one aspect is the comparison of sulfate aerosol and precursor gases above the surface. Vertical profiles of SO₂, SO²⁻₄, oxidants and cloud properties were measured by aircraft during the North Atlantic Regional Experiment (NARE) experiment in August/September 1993 off the coast of Nova Scotia and during the Second Eulerian Model Evaluation Field Study (EMEFSII), in central Ontario in March/April 1990. While no single model stands out as being best or worst, the general tendency is that those models simulating the full oxidant chemistry tend to agree best with observations although differences in transport and treatment of clouds are important as well.     

Latitudinal distribution of radon-222 flux from continents

Global atmospheric transport models are frequently tested by using ²²²Rn as a tracer. Generally this tracer is assumed to be emitted at a uniform rate (1 atom cm⁻² s⁻¹) from all ice-free land surfaces. The analysis of published data suggests a strong decrease from 30°N northwards to 0.2 atom cm⁻² s⁻¹ at 70°N. This could be a result of increasing water tables and proportions of organic soils as indicated by larger proportions of wetlands in northern latitudes.