Sheila Griffin

Large variations of surface ocean radiocarbon: Evidence of circulation changes in the southwestern Pacific

Radiocarbon (Δ14C) and stable isotope (δ18O and δ13C) records are presented for biannual samples from a 323-year banded coral series collected from the southern Great Barrier Reef, Australia. The high-precision Δ14C record contains variations on an interannual timescale, that are particularly large between A.D. 1680 and 1730. By comparison with tree ring Δ14C records [Stuiver and Quay, 1980; M. Stuiver, personal communication, 1992), it is clear that these shifts were not caused by changes in the Δ14C of atmospheric CO2. Changes in vertical mixing and large scale advective changes involving source waters to the western Coral Sea region are likely processes that could account for these large Δ14C variations. Most low Δ14C values for the period A.D. 1635-1875 coincide with El Nino/Southern Oscillation (ENSO) events as reported by Quinn et al. [1987] for the eastern tropical Pacific. However, ENSO does not explain all of the variations, especially during 1875–1920 when Δ14C values remained high. Cross-spectral analysis of the early half of the Δ14C and δ18O records (A.D. 1635–1795) reveals that the 6-year period is coherent; this coherency is not present in the latter half (A.D. 1797–1957) of the isotope records. These data support the concept of century timescale changes in the nature of ENSO, as it is manifest in the southwestern Pacific. Our coral record shows no evidence of a Suess effect, the lowering of Δ14C from late 1800s through 1955 due mainly to CO2 input from fossil fuel burning. This is coincident with the change we observe in the nature of ENSO and is further evidence that a long-term change in mixing of upper waters occurred in this region.

The Keck Carbon Cycle AMS laboratory, University of California, Irvine: Initial operation and a background surprise

A new radiocarbon accelerator mass spectrometry (AMS) laboratory for carbon cycle studies has been established at the University of California, Irvine. The 0.5MV AMS system was installed in mid-2002 and has operated routinely since October of that year. This paper briefly describes the spectrometer and summarizes lessons learned during the first year of operation. In the process of setting up the system, we identified and largely suppressed a previously unreported (super 14) C AMS background: charge exchange tails from (super 14) N beams derived from nitrogen-containing molecular ions produced near the entrance of the accelerator.

Magnesium Perchlorate as an Alternative Water Trap in AMS Graphite Sample Preparation: A Report on Sample Preparation at KCCAMS at the University of California, Irvine

We present a brief discussion of sample preparation procedures at the Keck Carbon Cycle Accelerator Mass Spectrometer (KCCAMS), University of California, Irvine, and a systematic investigation of the use of Mg(ClO (sub 4) ) (sub 2) as an absorptive water trap, replacing the standard dry ice/ethanol cold finger in graphite sample preparation. We compare high-precision AMS measurement results from oxalic acid I and USGS coal samples using Mg(ClO (sub 4) ) (sub 2) under different conditions. The results obtained were also compared with those achieved using the conventional water removal technique. Final results demonstrate that the use of Mg(ClO (sub 4) ) (sub 2) as an alternative water trap seems very convenient and reliable, provided the Mg(ClO (sub 4) ) (sub 2) is replaced frequently.

Seasonal variability of particulate organic radiocarbon in the northeast Pacific Ocean

We present Δ14C measurements of particulate organic carbon (POC) collected on four cruises at our time series site (station M) in the northeast Pacific Ocean. We observe a large gradient with depth in the suspended POC Δ14C values (124–160‰). These profiles display lower Δ14C values (by 20–30‰) in samples between 2500 m and the bottom during June 1992 and July 1993 than those during February and October 1992. Values of Δ14C in sinking POC from deep-moored sediment trap collections suggest a semiannual trend that displays lower overall Δ14C in material collected during periods of high flux. A limited number of Δ14C measurements of small swimmers picked from the trap 650 m above bottom are similar to surface Δ14C measurements of dissolved inorganic carbon (DIC) and suspended POC, indicating a surface carbon source. Overall, we postulate that the major process causing lower Δ14C values of deep suspended and sinking POC is sorption (or biological incorporation) of “old” DOC onto particulate matter. There appears to be a higher ratio of DOC sorbed to sinking particulate matter at times of high flux (late spring and early fall) that can be thought of as a “stripping out” of DOC from the water column. The DIC Δ14C display a small seasonal variation in the surface waters and is not the sole source of the observed seasonality in the POC Δ14C signals.

The radiocarbon signature of microorganisms in the mesopelagic ocean

Several lines of evidence indicate that microorganisms in the meso- and bathypelagic ocean are metabolically active and respiring carbon. In addition, growing evidence suggests that archaea are fixing inorganic carbon in this environment. However, direct quantification of the contribution from deep ocean carbon sources to community production in the dark ocean remains a challenge. In this study, carbon flow through the microbial community at 2 depths in the mesopelagic zone of the North Pacific Subtropical Gyre was examined by exploiting the unique radiocarbon signatures (Δ14C) of the 3 major carbon sources in this environment. The radiocarbon content of nucleic acids, a biomarker for viable cells, isolated from size-fractionated particles (0.2–0.5 μm and >0.5 μm) showed the direct incorporation of carbon delivered by rapidly sinking particles. Most significantly, at the 2 mesopelagic depths examined (670 m and 915 m), carbon derived from in situ autotrophic fixation supported a significant fraction of the free-living microbial community (0.2–0.5 μm size fraction), but the contribution of chemoautotrophy varied markedly between the 2 depths. Results further showed that utilization of the oceans largest reduced carbon reservoir, 14C-depleted, dissolved organic carbon, was negligible in this environment. This isotopic portrait of carbon assimilation by the in situ, free-living microbial community, integrated over >50,000 L of seawater, implies that recent, photosynthetic carbon is not always the major carbon source supporting microbial community production in the mesopelagic realm.

Gerardia: Bristlecone pine of the deep-sea?

We measured carbon isotope abundances in the layered, proteinaceous skeleton of a zoanthid Gerardia collected from 620 m depth off the Little Bahama Bank (27°N, 79°W). The δ 14C values decreased from −76% in the outer growth edge to an average of −267% in the center of three portions of the skeleton. These δ 14C data suggest an age for this living organism of 1800 ± 300 years. The possibility that the large decrease in δ 14C reflects the gradual input of bomb 14C over the entire growth of the organism is inconsistent with the post-bomb δ 14C values obtained for the most recent growth tips. If the age estimate of two millennia is correct, it may be the longest-lived animal yet observed in the ocean. Gerardia may serve as a long-lived recorder of ocean chemistry, similar to the Bristlecone pine tree that has served as a millennial-timescale recorder for atmospheric 14CO2 (Suess, 1980) and climate. In particular, there is potential for Gerardia to serve as a millennial-scale integrator of upper ocean particle flux, and possibly reveal past changes in the productivity of the surface ocean.

Variability of surface ocean radiocarbon and stable isotopes in the southwestern Pacific

We present high-precision radiocarbon (Δ14C) results and stable isotope (δ18O and δ13C) records for a coral from Heron Island (23°S, 152°E) and new stable isotope (δ18O and δ13C) records for annual coral bands from Abraham Reef (22°S, 153°E) in the southern Great Barrier Reef studied earlier [Druffel and Griffin, 1993]. These tracers provide unique information on the regional water mass history, and together these data allow us to constrain the variability of circulation in the upper Pacific over the past four centuries. First, we observe decreases in δ18O of coral from Abraham Reef and Heron Island, indicating an increase in sea surface temperature and/or a decrease in surface salinity since 1850. Second, the small Suess effect value (Δ14C decrease from 1880 to 1955, due mostly to fossil fuel CO2) observed previously at Abraham Reef[Druffel and Griffin, 1993] is confirmed in the measurements reported here from the Heron Island coral. This value is low compared to those observed in other areas of the ocean [Druffel, 1997; Druffel and Linick, 1978; Nozaki et al., 1978] between 1880 and 1955. Third, we report alterations in the correlation between El Nino events and the occurrence of low Δ14C, which is indicative of long-term change(s) in circulation in the SW Pacific. The Δ14C shifts reported here are not large, but even small temporal changes in prebomb Δ14C suggest that important changes in the large-scale state of the ocean have occurred, such as a temporal change in circulation.

Radiocarbon in dissolved organic and inorganic carbon from the central North Pacific

Author(s): Druffel, ER; Druffel, ER; Williams, PM; Robertson, KL; Griffin, S; Jull, AJ; Donahue, D | Abstract: Radiocarbon measurements are reported for dissolved organic carbon (DOC) and inorganic carbon (DIC) from seawater samples collected from the Alcyone-5 cruise in the central North Pacific Ocean in 1985. Differences between the UV-radiation techniques used here and those reported by Williams, Oeschger and Kinney (1969) to oxidize and recover the DOC from sea water are presented. UV unoxldizable DOC in these samples is discussed in a separate publication (Druffel, Williams a Suzuki,1989). We briefly discuss the penetration of the bomb 14C signal into the DOC and DIC pools. The temporal variability of z14C in DIC in surface samples taken every 2-3 days is presented. Concentrations of total dissolved free (FAA) plus combined (hydrolyzable) amino acids (THAA) and total dissolved carbohydrates TCHO) measured in the same water samples are also reported. Our main aim is to present the chemical and isotopic data from samples collected during the Alcyone-5 cruise. Detailed interpretation is published elsewhere.

AMS 14C Sample Preparation at the KCCAMS/UCI Facility: Status Report and Performance of Small Samples

We present an overview of accelerator mass spectrometry (AMS) radiocarbon sample preparation and measurements, describing the technical upgrades that now allow us to routinely obtain 0.2-0.3% precision for 1-mg carbon samples. A precision of ~1% on samples with 100 g of carbon can also be achieved. We have also developed graphitization techniques and AMS procedures for ultra-small samples (down to 0.002 mg of carbon). Detailed time series are presented for large and small aliquots of standards such as NIST OX-I and OX-II; FIRI-C and -D; IAEA-C6, -C7 and -C8; and 14C-free samples.

Distribution of particulate organic carbon and radiocarbon in the water column from the upper slope to the abyssal NE Pacific Ocean

We report profiles of concentrations and radiocarbon contents of suspended particulate organic carbon (POCsusp) and sedimentary organic carbon from an abyssal site (Stn M) in the northeast (NE) Pacific collected in September 1994 (a period of very high flux of particulate carbon in the deep sea) and June 1995, as well as from stations on the continental rise and slope off the coast of California in June 1995. We show that during a period of anomalously high sinking POC flux to the deep sea (September 1994), Δ14C of suspended POC did not decrease detectably between 85 and 1600 m depth. This is in contrast to depth profiles during low and moderate fluxes of sinking POC at this station where Δ14C-POCsusp decreased 50–60‰ in this depth range. One explanation for the constant Δ14C values of POCsusp between 85 and 1600 m is that large quantities of sinking POC could continuously release labile, 14C-enriched POCsusp during biological and chemical alteration of the sinking POC. The radiocarbon evidence further suggests that resuspension of organic carbon from the sediment surface, either locally or laterally transported from the slope to the deep sea, is likely, but is probably limited to depths within a few hundred meters of the bottom. Sorption of ‘old’ DOC by suspended particulate matter in the water column is also possible, especially at shallower depths (<3500 m), though proof of this mechanism cannot be demonstrated at this time.