[1] We use the nearly ideal tracer 14 CO 2 to estimate the fossil fuel CO 2 enhancement in boundary layer air at two sites in New England and Colorado. Improved D 14 C measurement precision of 1.6-2.6% provides fossil fuel CO 2 detection capability of 0.8-1.5 ppm. Using the indirect tracers CO and SF 6 , we obtain two additional independent estimates of the fossil fuel CO 2 component, and we assess the biases in these methods with respect to the 14 CO 2 -based estimates. The SF 6 -based estimates vary considerably from the 14 CO 2 -based estimates, and are at times implausibly large. The CO-based estimates are less variable, but show seasonally coherent biases with respect to the 14 CO 2 method.

We develop a high precision Δ14CO2 measurement capability in 2‐5 L samples of whole air for implementation within existing greenhouse gas flask sampling networks. The long‐term repeatability of the measurement is 1.8‰ (1‐sigma), as determined from repeated analyses of quality control standards and replicate extraction and measurement of authentic field samples. In a parallel effort, we have begun a Δ14CO2 measurement series from NOAA/ESRL’s (formerly NOAA/CMDL) surface flask sampling site at Niwot Ridge, Colorado, USA (40.05°N, 105.58°W, 3475 masl) in order to monitor the isotopic composition of carbon dioxide in relatively clean air over the North American continent. Δ14CO2 at Niwot Ridge decreased by 5.7‰/yr from 2004 to 2006, with a seasonal amplitude of 3‐5‰. A comparison with measurements from the free troposphere above New England, USA (41°N, 72°W) indicates that the Δ14CO2 series at the two sites are statistically similar at timescales longer than a few days to weeks (i.e., those of synoptic scale variations in transport), suggesting that the Niwot Ridge measurements can be used as a proxy for North American free tropospheric air in future carbon cycle studies.

4C measured in trace gases in clean air helps to determine the sources of such gases, their long-range transport in the atmosphere, and their exchange with other carbon cycle reservoirs. In order to separate sources, transport and exchange, it is necessary to interpret measurements using models of these processes. We present atmospheric ' 4C02 measurements made in New Zealand since 1954 and at various Pacific Ocean sites for shorter periods. We analyze these for latitudinal and seasonal variation, the latter being consistent with a seasonally varying exchange rate between the stratosphere and troposphere. The observed seasonal cycle does not agree with that predicted by a zonally averaged global circulation model. We discuss recent accelerator mass spectrometry measurements of atmospheric 14CH4 and the problems involved in determining the fossil fuel methane source. Current data imply a fossil carbon contribution of ca 25%, and the major sources of uncertainty in this number are the uncertainty in the nuclear power source of 14CH4, and in the measured value for S'4C in atmospheric methane.

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The 2,500‐km Kermadec‐Tonga arc is the longest submarine arc on the planet. Here, we report on the second of a series of cruises designed to investigate large‐scale controls on active hydrothermal venting on this arc. The 2002 NZAPLUME II cruise surveyed 12 submarine volcanic centers along ∼580 km of the middle Kermadec arc (MKA), extending a 1999 cruise that surveyed 260 km of the southern Kermadec arc (SKA). Average spacing between volcanic centers increases northward from 30 km on backarc crust along the SKA, to 45 km on backarc crust along the southern MKA, to 58 km where the MKA joins the Kermadec Ridge. Volcanic cones dominate in the backarc, and calderas dominate the Kermadec Ridge. The incidence of venting is higher along the MKA (83%, 10 of 12 volcanic centers) than the SKA (67%, 8 of 12), but the relative intensity of venting, as given by plume thickness, areal extent, and concentration of dissolved gases and ionic species, is generally weaker in the MKA. This pattern may reflect subduction of the ∼17‐km‐thick oceanic Hikurangi Plateau beneath the SKA. Subduction of this basaltic mass should greatly increase fluid loss from the downgoing slab, initiating extensive melting in the upper mantle wedge and invigorating the hydrothermal systems of the SKA. Conversely, volcanic centers in the southern MKA are starved of magma replenishment and so their hydrothermal systems are waning. Farther north, where the MKA centers merge with the Kermadec Ridge, fewer but larger magma bodies accumulate in the thicker (older) crust, ensuring more widely separated, caldera‐dominated volcanic centers.