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Cui, YY, Vijayan A, Falk M, Hsu YK, Yin DZ, Chen XM, Zhao Z, Avise J, Chen YJ, Verhulst K, Duren R, Yadav V, Miller C, Weiss R, Keeling R, Kim J, Iraci LT, Tanaka T, Johnson MS, Kort EA, Bianco L, Fischer ML, Stroud K, Herner J, Croes B.  2019.  A multiplatform inversion estimation of statewide and regional methane emissions in California during 2014-2016. Environmental Science & Technology. 53:9636-9645.   10.1021/acs.est.9b01769   AbstractWebsite

California methane (CH4) emissions are quantified for three years from two tower networks and one aircraft campaign. We used backward trajectory simulations and a mesoscale Bayesian inverse model, Mbring ratios (VI ' initialized by three inventories, to achieve the emission quantification. Results show total statewide CH4 emissions of 2.05 +/- 0.26 (at 95% confidence) Tg/yr, which is 1.14 to 1.47 times greater than the anthropogenic emission estimates by California Air Resource Board (GARB). Some of differences could be biogenic emissions, superemitter point sources, and other episodic emissions which may not be completely included in the CARB inventory. San Joaquin Valley (SJV) has the largest CH4 emissions (0.94 +/- 0.18 Tg/yr), followed by the South Coast Air Basin, the Sacramento Valley, and the San Francisco Bay Area at 0.39 +/- 0.18, 0.21 +/- 0.04, and 0.16 +/- 0.05 Tg/yr, respectively. The dairy and oil/gas production sources in the SJV contribute 0.44 +/- 0.36 and 0.22 +/- 0.23 Tg CH4/yr, respectively. This study has important policy implications for regulatory programs, as it provides a thorough multiyear evaluation of the emissions inventory using independent atmospheric measurements and investigates the utility of a complementary multiplatform approach in understanding the spatial and temporal patterns of CH4 emissions in the state and identifies opportunities for the expansion and applications of the monitoring network.

Nottrott, A, Kleissl J, Keeling R.  2014.  Modeling passive scalar dispersion in the atmospheric boundary layer with WRF large-eddy simulation. Atmospheric Environment. 82:172-182.   10.1016/j.atmosenv.2013.10.026   AbstractWebsite

The ability of the Weather Research and Forecasting, large-eddy simulation model (WRF-LES) to model passive scalar dispersion from continuous sources in convective and neutral atmospheric boundary layers was investigated. WRF-LES accurately modeled mean plume trajectories and concentration fields. WRF-LES statistics of concentration fluctuations in the daytime convective boundary layer were similar to data obtained from laboratory experiments and other LES models. However, poor turbulence resolution near the surface in neutral boundary layer simulations caused under prediction of mean dispersion in the crosswind horizontal direction and over prediction of concentration variance in the neutral surface layer. A gradient in the intermittency factor for concentration fluctuations was observed near the surface, downwind of ground-level sources in the daytime boundary layer. That observation suggests that the intermittency factor is a promising metric for estimating source-sensor distance in source determination applications. (C) 2013 Elsevier Ltd. All rights reserved.

Manning, MR, Edmonds J, Emori S, Grubler A, Hibbard K, Joos F, Kainuma M, Keeling RF, Kram T, Manning AC, Meinshausen M, Moss R, Nakicenovic N, Riahi K, Rose SK, Smith S, Swart R, van Vuuren DP.  2010.  Misrepresentation of the IPCC CO2 emission scenarios. Nature Geoscience. 3:376-377.   10.1038/ngeo880   AbstractWebsite
Keeling, RF, Manning AC, McEvoy EM, Shertz SR.  1998.  Methods for measuring changes in atmospheric O2 concentration and their application in southern hemisphere air. Journal of Geophysical Research-Atmospheres. 103:3381-3397.   10.1029/97jd02537   AbstractWebsite

Methods are described for measuring changes in atmospheric O-2 concentration with emphasis on gas handling procedures. Cryogenically dried air samples are collected in 5 L glass flasks at ambient pressure and analyzed against reference gases derived from high-pressure aluminum tanks. Fractionation effects are minimized by avoiding pressure and flow variations throughout the gas-handling system. The overall external reproducibility is approximately +/-3.3 per meg, with systematic errors associated with collecting samples and with storing them for 1 year reduced to the level of 3 per meg or smaller. The demonstrated short-term reproducibly of air delivered from high-presure tanks is +/-1.5 per meg, with the composition changing by at most 5 per meg by surface desorption reactions as the tank is depleted to below 3500 kPa. A 9-year survey of a suite of six reference gases showed no systematic long-term trends in relative O-2 concentrations to the level of 5 per meg. Results are presented from samples collected at Cape Grim (41 degrees S), Macquarie Island (54 degrees S) and the South Pole Station (90 degrees S). From measurements spanning 1991-1995 it is found that the O-2 concentrations at the South Pole are on average 3.6+/-1.2 per meg higher than at Cape Grim. This result runs contrary to the expectation that the air at high southern latitudes should be depleted in O-2 as a result of O-2 uptake from the Southern Ocean and may require the existence of unknown O-2 sources near Antarctica or unexpected atmospheric transport patterns.

Graven, HD, Guilderson TP, Keeling RF.  2007.  Methods for high-precision 14C AMS measurement of atmospheric CO2 at LLNL. Radiocarbon. 49:349-356. AbstractWebsite

Development of radiocarbon analysis with precision better than 2%omicron has the potential to expand the utility of (CO2)-C-14 measurements for carbon cycle investigations as atmospheric gradients currently approach the typical measurement precision of 2-5%omicron. The accelerator mass spectrometer at Lawrence Livermore National Laboratory (LLNL) produces high and stable beam currents that enable efficient acquisition times for large numbers of C-14 counts. One million C-14 atoms can be detected in approximately 25 min, suggesting that near 1%omicron counting precision is economically feasible at LLNL. The overall uncertainty in measured values is ultimately determined by the variation between measured ratios in several sputtering periods of the same sample and by the reproducibility of replicate samples. Experiments on the collection of 1 million counts on replicate samples of CO2 extracted from a whole air cylinder show a standard deviation of 1.7%omicron in 36 samples measured over several wheels. This precision may be limited by the reproducibility of oxalic acid I standard samples, which is considerably poorer. We outline the procedures for high-precision sample handling and analysis that have enabled reproducibility in the cylinder extraction samples at the <2%omicron level and describe future directions to continue increasing measurement precision at LLNL.

Keeling, RF.  1991.  Mechanisms for stabilization and destabilization of a simple biosphere: catastrophe on Daisyworld. Scientists on Gaia. ( Schneider S, Boston PJ, Eds.).:118-120., Cambridge, Mass.: MIT Press Abstract
Keeling, RF.  1988.  Measuring correlations between atmospheric oxygen and carbon dioxide mole fractions: A preliminary study in urban air. Journal of Atmospheric Chemistry. 7:153-176.   10.1007/bf00048044   AbstractWebsite

On 25 and 26 October 1986 the air in Cambridge, Massachusetts was monitored for O2 and CO2 mole fraction. O2 concentrations were detected from changes in the relative refractivity of dried air between two lines of 198Hg at 2537.269 and 4359.562 Å using dual-wavelength interferometry. Changes in oxygen mole fraction were resolved with two-minute time resolution to a precision of ±2.0 ppm. Changes in O2 were shown to be strongly anticorrelated with changes in CO2 as expected for combustion processes. The demonstrated instrumental capabilities are appropriate for measuring changes in O2 mole fraction in background air which could be of importance to a broad range of biogeochemical studies.

Petrenko, VV, Severinghaus JP, Schaefer H, Smith AM, Kuhl T, Baggenstos D, Hua Q, Brook EJ, Rose P, Kulin R, Bauska T, Harth C, Buizert C, Orsi A, Emanuele G, Lee JE, Brailsford G, Keeling R, Weiss RF.  2016.  Measurements of 14C in ancient ice from Taylor Glacier, Antarctica constrain in situ cosmogenic 14CH4 and 14CO production rates. Geochimica et Cosmochimica Acta. 177:62-77.   10.1016/j.gca.2016.01.004   Abstract

Carbon-14 (14C) is incorporated into glacial ice by trapping of atmospheric gases as well as direct near-surface in situ cosmogenic production. 14C of trapped methane (14CH4) is a powerful tracer for past CH4 emissions from “old” carbon sources such as permafrost and marine CH4 clathrates. 14C in trapped carbon dioxide (14CO2) can be used for absolute dating of ice cores. In situ produced cosmogenic 14C in carbon monoxide (14CO) can potentially be used to reconstruct the past cosmic ray flux and past solar activity. Unfortunately, the trapped atmospheric and in situ cosmogenic components of 14C in glacial ice are difficult to disentangle and a thorough understanding of the in situ cosmogenic component is needed in order to extract useful information from ice core 14C. We analyzed very large (≈1000 kg) ice samples in the 2.26–19.53 m depth range from the ablation zone of Taylor Glacier, Antarctica, to study in situ cosmogenic production of 14CH4 and 14CO. All sampled ice is >50 ka in age, allowing for the assumption that most of the measured 14C originates from recent in situ cosmogenic production as ancient ice is brought to the surface via ablation. Our results place the first constraints on cosmogenic 14CH4 production rates and improve on prior estimates of 14CO production rates in ice. We find a constant 14CH4/14CO production ratio (0.0076 ± 0.0003) for samples deeper than 3 m, which allows the use of 14CO for correcting the 14CH4 signals for the in situ cosmogenic component. Our results also provide the first unambiguous confirmation of 14C production by fast muons in a natural setting (ice or rock) and suggest that the 14C production rates in ice commonly used in the literature may be too high.

Battle, M, Bender M, Hendricks MB, Ho DT, Mika R, McKinley G, Fan SM, Blaine T, Keeling RF.  2003.  Measurements and models of the atmospheric Ar/N2 ratio. Geophysical Research Letters. 30   10.1029/2003gl017411   AbstractWebsite

[1] The Ar/N-2 ratio of air measured at 6 globally distributed sites shows annual cycles with amplitudes of 12 to 37 parts in 10(6). Summertime maxima reflect the atmospheric Ar enrichment driven by seasonal warming and degassing of the oceans. Paired models of air-sea heat fluxes and atmospheric tracer transport predict seasonal cycles in the Ar/N-2 ratio that agree with observations, within uncertainties.

Keeling, RF, Blaine T, Paplawsky B, Katz L, Atwood C, Brockwell T.  2004.  Measurement of changes in atmospheric Ar/N2 ratio using a rapid-switching, single-capillary mass spectrometer system. Tellus Series B-Chemical and Physical Meteorology. 56:322-338.   10.1111/j.1600-0889.2004.00117.x   AbstractWebsite

The atmospheric Ar/N-2 ratio is expected to undergo very slight variations due to exchanges of Ar and N-2 across the air-sea interface, driven by ocean solubility changes. Observations of these variations may provide useful constraints on large-scale fluxes of heat across the air-sea interface. A mass spectrometer system is described that incorporates a magnet with a wide exit face, allowing a large mass spread, and incorporates an inlet with rapid (5 s) switching of sources gases through a single capillary, thus achieving high precision in the comparison of sample and reference gases. The system allows simultaneous measurement of Ar/N-2, O-2/N, and CO2/N-2 ratios. The system achieves a short-term precision in Ar/N-2 of 10 per meg for a 10 s integration, which can be averaged to achieve an internal precision of a few per meg in the comparison of reference gases. Results for Ar/N-2 are reported from flasks samples collected from nine stations in a north-to-south global network over about a 1 yr period. The imprecision on an individual flask, as estimated from replicate agreement, is 11 per meg. This imprecision is dominated by real variability between samples at the time of analysis. Seasonal cycles are marginally resolved at the extra-tropical stations with amplitudes of 5 to 15 per meg. Annual-mean values are constant between stations to within 5 per meg. The results are compared with a numerical simulation of the cycles and gradients in Ar/N-2 based on the TM2 tracer transport model in combination with air-sea Ar and N-2 fluxes derived from climatological air-sea heat fluxes. The possibility is suggested that Ar/N-2 ratios may be detectably enriched near the ground by gravimetric or thermal fractionation under conditions of strong surface inversions.

Keeling, RF, Blaine T, Paplawsky B, Katz L, Atwood C, Brockwell T.  2006.  Measurement of changes in atmospheric Ar/N2 ratio using a rapid-switching, single-capillary mass spectrometer system (vol 56B, pg 322, 2006). Tellus Series B-Chemical and Physical Meteorology. 58:255-255.   10.1111/j.1600-0889.2006.00190.x   AbstractWebsite
Najjar, RG, Keeling RF.  2000.  Mean annual cycle of the air-sea oxygen flux: A global view. Global Biogeochemical Cycles. 14:573-584.   10.1029/1999gb900086   AbstractWebsite

A global monthly-mean climatology of the air-sea oxygen flux is presented and discussed. The climatology is based on the ocean oxygen climatology of Najjar and Keeling [1997] and wind speeds derived from a meteorological analysis center. Seasonal variations are characterized by outgassing of oxygen during spring and summer and ingassing of oxygen during fall and winter, a pattern consistent with thermal and biological forcing of the air-sea oxygen flux. The annual mean flux pattern is characterized by ingassing at high latitudes and the tropics and outgassing in middle latitudes. The air-sea oxygen flux is shown to exhibit patterns that agree well with patterns seen in a marine primary productivity climatology, in model generated air-sea O-2 fluxes, in estimates of remineralization in the shallow aphotic zone based on seasonal oxygen variations, in observed seasonal nutrient-temperature relationships, and in independent estimates of meridional oxygen transport in the Atlantic ocean. We also find that extratropical mixed layer new production during the spring-summer period, computed from biological seasonal net outgassing of oxygen, is equivalent to the production of 4.5-5.6 Gt C, much lower than previous estimates based on atmospheric O-2/N-2 measurements.

Sundquist, ET, Keeling RF.  2009.  The Mauna Loa carbon dioxide record: lessons for long-term earth observations. Carbon sequestration and its role in the global carbon cycle. ( McPherson BJ, Sundquist ET, Eds.).:27-35., Washington, DC: American Geophysical Union Abstract

"For carbon sequestration, the issues of monitoring, assessment and verification of carbon content and storage efficacy are perhaps the most uncertain yet most critical issues facing the broader context of climate change in relation to carbon sequestration. As a result, this book presents current perspectives and research that combine four major areas: verification and assessment of global carbon sources and sinks; potential capacity and temporal/spatial scales of terrestrial, oceanic, and geologic carbon storage; assessing risks and benefits associated with terrestrial, oceanic, and geologic carbon storage; and predicting, monitoring, and verifying effectiveness of terrestrial, oceanic and geologic carbon storage. This volume is based on a Chapman conference and will appeal to the rapidly growing group of scientists and engineers in examining methods for deliberate carbon sequestration through storage in plants, soils, the oceans, and geological repositories."--Publisher's description.