Sources and sinks for nitrous oxide and experimental studies of the source of atmospheric COS, CS-2 and CH-3-Cl

Studies of the air and water chemistry in the Amazon region of Brazil were undertaken. Harvard scientists were invited to participate in several experiments at INPA facilities, at other sites in Brazil, and aboard the RV Calypso of the Cousteau Society. Expeditions and participants are summarized

The chemistry of Antarctic ozone 1960-1987

The factors that influence Antarctic ozone are examined with a view to understanding the observed historical trend. Researchers show that reduced ambient temperatures can dramatically enhance the efficiency of chemical removal processes. Attention is focused on positive feedback between levels of ozone, temperature, and rates of heterogeneous chemical reactions. ClO and its dimer, and high levels of these gases are maintained until the clouds evaporate, on 15 September for the simulation shown here

Agricultural Perturbations of the Nitrogen Cycle and Related Impact on Atmospheric N_2O and Ozone

The available data are employed to identify the fate of agricultural nitrogen in the environment. Best estimates predict denitrification of nearly 50% of fertilizer nitrogen in less than 10 years after application. We also discuss in detail the expected demand curve for agricultural N. If population growth continues at projected levels, between 100 and 200 M tons/yr of agricultural N will be needed by the year 2000. We estimate that as a result, atmospheric N_2O could be more than doubled by 2050, and that perturbations of O_3 at that time could range from 10 to more than 20%. Major uncertainties remain however, and we emphasize the importance of further experimental research into the nitrogen cycle

Reply to “Comment by A. Appleby, D. Lilian and H. B. Singh on ‘Atmospheric halocarbons: A discussion with emphasis on chloroform’”

No abstract

Nitrous oxide in fresh water systems: An estimate for the yield of atmospheric N2O associated with disposal of human waste

The N2O content of waters in the Potomac and Merrimack Rivers was measured on a number of occasions over the period April to July 1977. The concentrations of dissolved N2O exceeded those which would apply in equilibrium with air by factors ranging from about 46 in the Potomac to 1.2 in the Merrimack. Highest concentrations of dissolved N2O were associated with sewage discharges from the vicinity of Washington, D. C., and analysis indicates a relatively high yield, 1.3 to 11%, for prompt conversion of waste nitrogen to N2O. Measurements of dissolved N2O in fresh water ponds near Boston demonstrated that aquatic systems provide both strong sources and sinks for atmospheric N2O

Boreal forest CO2 exchange and evapotranspiration predicted by nine ecosystem process models: Intermodel comparisons and relationships to field measurements

Nine ecosystem process models were used to predict CO2 and water vapor exchanges by a 150-year-old black spruce forest in central Canada during 1994–1996 to evaluate and improve the models. Three models had hourly time steps, five had daily time steps, and one had monthly time steps. Model input included site ecosystem characteristics and meteorology. Model predictions were compared to eddy covariance (EC) measurements of whole-ecosystem CO2exchange and evapotranspiration, to chamber measurements of nighttime moss-surface CO2release, and to ground-based estimates of annual gross primary production, net primary production, net ecosystem production (NEP), plant respiration, and decomposition. Model-model differences were apparent for all variables. Model-measurement agreement was good in some cases but poor in others. Modeled annual NEP ranged from −11 g C m−2 (weak CO2source) to 85 g C m−2 (moderate CO2 sink). The models generally predicted greater annual CO2sink activity than measured by EC, a discrepancy consistent with the fact that model parameterizations represented the more productive fraction of the EC tower “footprint.” At hourly to monthly timescales, predictions bracketed EC measurements so median predictions were similar to measurements, but there were quantitatively important model-measurement discrepancies found for all models at subannual timescales. For these models and input data, hourly time steps (and greater complexity) compared to daily time steps tended to improve model-measurement agreement for daily scale CO2 exchange and evapotranspiration (as judged by root-mean-squared error). Model time step and complexity played only small roles in monthly to annual predictions

Strategies for measurement of atmospheric column means of carbon dioxide from aircraft using discrete sampling

[1] Automated flask sampling aboard small charter aircraft has been proposed as a low-cost, reliable method to greatly increase the density of measurements of CO2 mixing ratios in continental regions in order to provide data for assessment of global and regional CO2 budgets. We use data from the CO2 Budget and Rectification-Airborne 2000 campaign over North America to study the feasibility of using discrete ( flask) sampling to determine column mean CO2 in the lowest 4 km of the atmosphere. To simulate flask sampling, data were selected from profiles of CO2 measured continuously with an onboard ( in situ) analyzer. We find that midday column means can be determined without bias relative to true column means measured by the in situ analyzer to within 0.15 and better than 0.10 ppm by using 10 and 20 instantaneously collected flask samples, respectively. More precise results can be obtained by using a flask sampling strategy that linearly integrates over portions of the air column. Using less than 8 - 10 flasks can lead to significant sampling bias for some common profile shapes. Sampling prior to the breakup of the nocturnal stable layer will generally lead to large sampling bias because of the inability of aircraft to probe large CO2 gradients that often exist very close to the ground at night and during the early morning

Mass fluxes and isofluxes of methane (CH4) at a New Hampshire fen measured by a continuous wave quantum cascade laser spectrometer

We have developed a mid‐infrared continuous‐wave quantum cascade laser direct‐absorption spectrometer (QCLS) capable of high frequency (≥1 Hz) measurements of 12CH4 and 13CH4 isotopologues of methane (CH4) with in situ 1‐s RMS image precision of 1.5 ‰ and Allan‐minimum precision of 0.2 ‰. We deployed this QCLS in a well‐studied New Hampshire fen to compare measurements of CH4 isoflux by eddy covariance (EC) to Keeling regressions of data from automated flux chamber sampling. Mean CH4 fluxes of 6.5 ± 0.7 mg CH4 m−2 hr−1 over two days of EC sampling in July, 2009 were indistinguishable from mean autochamber CH4 fluxes (6.6 ± 0.8 mgCH4 m−2 hr−1) over the same period. Mean image composition of emitted CH4 calculated using EC isoflux methods was −71 ± 8 ‰ (95% C.I.) while Keeling regressions of 332 chamber closing events over 8 days yielded a corresponding value of −64.5 ± 0.8 ‰. Ebullitive fluxes, representing ∼10% of total CH4 fluxes at this site, were on average 1.2 ‰ enriched in 13C compared to diffusive fluxes. CH4 isoflux time series have the potential to improve process‐based understanding of methanogenesis, fully characterize source isotopic distributions, and serve as additional constraints for both regional and global CH4 modeling analysis

What can tracer observations in the continental boundary layer tell us about surface-atmosphere fluxes?

International audienceWe analyze the potential for inferring spatially resolved surface fluxes from atmospheric tracer observations within the mixed layer, such as from monitoring towers, using a receptor oriented transport model (Stochastic Time-Inverted Lagrangian Transport model ? STILT) coupled to a simple biosphere in which CO2 fluxes are represented as functional responses to environmental drivers (radiation and temperature). Transport and biospheric fluxes are coupled on a dynamic grid using a polar projection with high horizontal resolution (~20 km) in near field, and low resolution far away (as coarse as 2000 km), reducing the number of surface pixels without significant loss of information. To test the system, and to evaluate the errors associated with the retrieval of fluxes from atmospheric observations, a pseudo data experiment was performed. A large number of realizations of measurements (pseudo data) and a priori fluxes were generated, and for each case spatially resolved fluxes were retrieved. Results indicate strong potential for high resolution retrievals based on a network of tall towers, subject to the requirement of correctly specifying the a priori uncertainty covariance, especially the off diagonal elements that control spatial correlations. False assumptions about the degree to which the uncertainties in the a priori fluxes are spatially correlated may lead to a strong underestimation of uncertainties in the retrieved fluxes, or, equivalently, to biased retrievals. The framework presented here, however, allows a conservative choice of the off diagonal elements that avoids biasing the retrievals

Comparing Global Atmospheric CO2 Flux and Transport Models with Remote Sensing (and Other) Observations

We report recent progress derived from comparison of global CO2 flux and transport models with new remote sensing and other sources of CO2 data including those from satellite. The overall objective of this activity is to improve the process models that represent our understanding of the workings of the atmospheric carbon cycle. Model estimates of CO2 surface flux and atmospheric transport processes are required for initial constraints on inverse analyses, to connect atmospheric observations to the location of surface sources and sinks, to provide the basic framework for carbon data assimilation, and ultimately for future projections of carbon-climate interactions. Models can also be used to test consistency within and between CO2 data sets under varying geophysical states. Here we focus on simulated CO2 fluxes from terrestrial vegetation and atmospheric transport mutually constrained by analyzed meteorological fields from the Goddard Modeling and Assimilation Office for the period 2000 through 2009. Use of assimilated meteorological data enables direct model comparison to observations across a wide range of scales of variability. The biospheric fluxes are produced by the CASA model at 1x1 degrees on a monthly mean basis, modulated hourly with analyzed temperature and sunlight. Both physiological and biomass burning fluxes are derived using satellite observations of vegetation, burned area (as in GFED-3), and analyzed meteorology. For the purposes of comparison to CO2 data, fossil fuel and ocean fluxes are also included in the transport simulations. In this presentation we evaluate the model's ability to simulate CO2 flux and mixing ratio variability in comparison to remote sensing observations from TCCON, GOSAT, and AIRS as well as relevant in situ observations. Examples of the influence of key process representations are shown from both forward and inverse model comparisons. We find that the model can resolve much of the synoptic, seasonal, and interannual variability in the observations, although reasons for persistent discrepancies in northern hemisphere vegetation uptake are examined. At this time, we do not find any serious shortcomings in the model transport representation, but this is still the subject of close scrutiny. In general, the fidelity of these simulations leads us to anticipate incorporation of real-time, highly resolved remote sensing and other observations into quantitative analyses that will reduce uncertainty in CO2 fluxes and revolutionize our understanding of the key processes controlling atmospheric CO2 and its evolution with time