Trace element proxies and stable isotopes used to identify water quality threats to elkhorn coral (Acropora palmata) at two national parks in St. Croix, USVI.

Biological impairments have been documented on reefs at two national parks in St. Croix, USVI. Although several water quality parameters have been out of compliance with USVI criteria, whether these parameters or other pollutants are responsible for coral health impacts is unknown. Trace elements quantified in sediment showed four sites at SARI, which is closer than BUIS to settlements and land-derived anthropogenic outflows, had Cu mass fractions above sediment quality guidelines for invertebrate toxicity. Trace elements were also analyzed in the skeleton of threatened elkhorn coral, Acropora palmata, to evaluate potential exposure. Heavy metals (Pb, Zn) were significantly greater in coral skeleton at SARI than BUIS. Cu, Pb, and Zn may be impacting coral health in these parks. Potential anthropogenic sources of these metals were revealed by the coral tissue stable isotope levels (δ13C and δ15N). These findings provide a framework for determining heavy metal impacts on these invaluable reefs.

Physical and elemental analysis of Middle East sands from recent combat zones.

Objective: The lungs are uniquely exposed to the external environment. Sand and dust exposures in desert regions are common among deployed soldiers. A significant number of Veterans deployed to the Middle East report development of respiratory disorders and diseases.Materials and methods: Sand collected from Fallujah, Iraq and Kandahar, Afghanistan combat zones was analyzed and compared to a sand sample collected from an historic United States (U.S.) battle region (Fort Johnson, James Island, SC, Civil War battle site). Sand samples were analyzed to determine the physical and elemental characteristics that may have the potential to contribute to development of respiratory disease.Results: Using complementary scanning electron microscopy (SEM) imaging and analysis, and inductively coupled plasma mass spectrometry (ICP-MS), it was determined that Iraq sand contained elevated levels of calcium and first row transition metals versus Afghanistan and U.S. sand. Iraq sand particle texture was smooth and round, and particles were considerably smaller than Afghanistan sand. Afghanistan sand was elevated in rare earth metals versus Iraq or U.S. sands and had sharp edge features and larger particle size than Iraq sand.Conclusions: These data demonstrate significant differences in Iraq and Afghanistan sand particle size and characteristics. Middle East sands contained elevated levels of elements that have been associated with respiratory disease versus control site sand, suggesting the potential of sand/dust storm exposure to promote adverse respiratory symptoms. Data also demonstrate the potential for variation based on geographical region or site of exposure. The data generated provide baseline information that will be valuable in designing future exposure studies.

Selenium protein identification and profiling by mass spectrometry: A tool to assess progression of cardiomyopathy in a whale model.

Non-ischemic cardiomyopathy is a leading cause of congestive heart failure and sudden cardiac death in humans and in some cases the etiology of cardiomyopathy can include the downstream effects of an essential element deficiency. Of all mammal species, pygmy sperm whales (Kogia breviceps) present the greatest known prevalence of cardiomyopathy with more than half of examined individuals indicating the presence of cardiomyopathy from gross and histo-pathology. Several factors such as genetics, infectious agents, contaminants, biotoxins, and inappropriate dietary intake (vitamins, selenium, mercury, and pro-oxidants), may contribute to the development of idiopathic cardiomyopathy in K. breviceps. Due to the important role Se can play in antioxidant biochemistry and protein formation, Se protein presence and relative abundance were explored in cardiomyopathy related cases. Selenium proteins were separated and detected by multi-dimension liquid chromatography inductively coupled plasma mass spectrometry (LC-ICP-MS), Se protein identification was performed by liquid chromatography electrospray tandem mass spectrometry (LC-ESI-MS/MS), and Se protein profiles were examined in liver (n=30) and heart tissue (n=5) by SEC/UV/ICP-MS detection. Data collected on selenium proteins was evaluated in the context of individual animal trace element concentration, life history, and histological information. Selenium containing protein peak profiles varied in presence and intensity between animals with no pathological findings of cardiomyopathy and animals exhibiting evidence of cardiomyopathy. In particular, one class of proteins, metallothioneins, was found to be associated with Se and was in greater abundance in animals with cardiomyopathy than those with no pathological findings. Profiling Se species with SEC/ICP-MS proved to be a useful tool to identify Se protein pattern differences between heart disease stages in K. breviceps and an approach similar to this may be applied to other species to study Se protein associations with cardiomyopathy.

Application of Microwave-Induced Combustion and Isotope Dilution Strategies for Quantification of Sulfur in Coals via Sector-Field Inductively Coupled Plasma Mass Spectrometry.

In recent years, microwave-induced combustion (MIC) has proved to be a robust sample preparation technique for difficult-to-digest samples containing high carbon content, especially for determination of halogens and sulfur. National Institute of Standards and Technology (NIST) has applied the MIC methodology in combination with isotope dilution analysis for sulfur determinations, representing the first-reported combination of this robust sample preparation methodology and high-accuracy quantification approach. Medium-resolution mode sector-field inductively coupled plasma mass spectrometry was invoked to avoid spectral interferences on the sulfur isotopes. The sample preparation and instrumental analysis scheme was used for the value assignment of total sulfur in Standard Reference Material (SRM) 2682c Subbituminous Coal (nominal mass fraction 0.5% sulfur). A description of the analytical procedures required is provided, along with metrological results, including an estimation of the overall method uncertainty (<1.5% relative expanded uncertainty) calculated using the IDMS measurement function and a Kragten spreadsheet approach.

Determination of trace sulfur in biodiesel and diesel standard reference materials by isotope dilution sector field inductively coupled plasma mass spectrometry.

A method is described for quantification of sulfur at low concentrations on the order of mgkg(-1) in biodiesel and diesel fuels using isotope dilution and sector field inductively coupled plasma mass spectrometry (ID-SF-ICP-MS). Closed vessel microwave-assisted digestion was employed using a diluted nitric acid and hydrogen peroxide decomposition medium to reduce sample dilution volumes. Medium resolution mode was employed to eliminate isobaric interferences at (32)S and (34)S related to polyatomic phosphorus and oxygen species, and sulfur hydride species. The method outlined yielded respective limits of detection (LOD) and limits of quantification (LOQ) of 0.7 mg kg(-1) S and 2.5 mg kg(-1) S (in the sample). The LOD was constrained by instrument background counts at (32)S but was sufficient to facilitate value assignment of total S mass fraction in NIST SRM 2723b Sulfur in Diesel Fuel Oil at 9.06±0.13 mg kg(-1). No statistically significant difference at a 95% confidence level was observed between the measured and certified values for certified reference materials NIST SRM 2773 B100 Biodiesel (Animal-Based), CENAM DRM 272b and NIST SRM 2723a Sulfur in Diesel Fuel Oil, validating method accuracy.

Development of a Standard Reference Material for metabolomics research.

The National Institute of Standards and Technology (NIST), in collaboration with the National Institutes of Health (NIH), has developed a Standard Reference Material (SRM) to support technology development in metabolomics research. SRM 1950 Metabolites in Human Plasma is intended to have metabolite concentrations that are representative of those found in adult human plasma. The plasma used in the preparation of SRM 1950 was collected from both male and female donors, and donor ethnicity targets were selected based upon the ethnic makeup of the U.S. population. Metabolomics research is diverse in terms of both instrumentation and scientific goals. This SRM was designed to apply broadly to the field, not toward specific applications. Therefore, concentrations of approximately 100 analytes, including amino acids, fatty acids, trace elements, vitamins, hormones, selenoproteins, clinical markers, and perfluorinated compounds (PFCs), were determined. Value assignment measurements were performed by NIST and the Centers for Disease Control and Prevention (CDC). SRM 1950 is the first reference material developed specifically for metabolomics research.

Determination of trace level cadmium in SRM 3280 Multivitamin/Multielement Tablets via isotope dilution inductively coupled plasma mass spectrometry.

Cadmium was quantified at 80.15±0.86 ng/g (mean±95% expanded uncertainty) in NIST SRM 3280 Multivitamin/Multielement Tablets, using isotope dilution mass spectrometry. The method described utilized various precipitation and solid-phase extraction separation methodologies to isolate Cd from Sn and Mo, present respectively, at 11.1±0.9 mg/kg and 70.7±4.5 mg/kg in the tablet matrix. This allowed for measurement of (111)Cd/(113)Cd and (111)Cd/(114)Cd isotope ratios using both quadrupole collision cell technology inductively coupled plasma mass spectrometry (Q-CCT-ICP-MS) and sector field (SF)-ICP-MS equipped with a desolvating nebulizer system to mitigate the MoO(+) and MoOH(+) molecular ion interferences that typically affect the envelope of Cd isotopes.

Certification of elements in and use of standard reference material 3280 multivitamin/multielement tablets.

Standard Reference Material 3280 Multivitamin/ Multielement Tablets was issued by the National Institute of Standards and Technology in 2009, and has certified and reference mass fraction values for 13 vitamins, 26 elements, and two carotenoids. Elements were measured using two or more analytical methods at NIST with additional data contributed by collaborating laboratories. This reference material is expected to serve a dual purpose: to provide quality assurance in support of a database of dietary supplement products and to provide a means for analysts, dietary supplement manufacturers, and researchers to assess the appropriateness and validity of their analytical methods and the accuracy of their results.

Influence of mercury and selenium chemistries on the progression of cardiomyopathy in pygmy sperm whales, Kogia breviceps.

More than half of pygmy sperm whales (Kogia breviceps) that strand exhibit signs of cardiomyopathy (CMP). Many factors may contribute to the development of idiopathic CMP in K. breviceps, including genetics, infectious agents, contaminants, biotoxins, and dietary intake (e.g. selenium, mercury, and pro-oxidants). This study assessed trace elements in K. breviceps at various stages of CMP progression using fresh frozen liver and heart samples collected from individuals that stranded along US Atlantic and Gulf coasts between 1993 and 2007. Standard addition calibration and collision cell inductively coupled plasma mass spectrometry (ICP-MS) were employed for total Se analysis and pyrolysis atomic absorption (AA) was utilized for total Hg analysis to examine if the Se/Hg detoxification pathway inhibits the bioavailability of Se. Double spike speciated isotope dilution gas chromatography ICP-MS was utilized to measure methyl Hg and inorganic Hg. Immunoblot detection and colorimetric assays were used to assess protein oxidation status. Data collected on trace elements, selenoproteins, and oxidative status were evaluated in the context of animal life history and other complementary histological information to gain insight into the biochemical pathways contributing to the development of CMP in K. breviceps. Cardiomyopathy was only observed in adult pygmy sperm whales, predominantly in male animals. Both Hg:Se molar ratios and overall protein oxidation were greater in males than females and increased with progression of CMP.

Preliminary evaluation of a microwave-assisted metal-labeling strategy for quantification of peptides via RPLC-ICP-MS and the method of standard additions.

NIST has performed preliminary research on applying a calibration methodology based on the method of standard additions to the quantification of peptides via reverse-phase liquid chromatography coupled to inductively coupled plasma mass spectrometry (RPLC-ICP-MS). A microwave-assisted lanthanide labeling procedure was developed and applied to derivatize peptides using the macrocyclic bifunctional chemical chelator DOTA (1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid), which significantly improved the lanthanide labeling yield and reduced reaction times compared to benchtop labeling procedures. Biomolecular MS technologies of matrix-assisted laser desorption ionization (MALDI)-MS and electrospray ionization (ESI)-MS/MS were used in concert with ICP-MS to confirm the results of microwave labeling, sample cleanup and standard additions experiments for several test peptides. The calibration scheme is outlined in detail and contextualized against complementary high accuracy calibration strategies currently employed for ICP-MS detection of biomolecules. Standard additions experiments using native, non-isotopic peptide calibrants confirm the simplicity of the scheme and the potential of applying a blending (recombined sample and spike) procedure, facilitating calibration via co-elution of lanthanide labeled peptides. Ways to improve and fully leverage the analytical methodology are highlighted.

Establishing baseline levels of trace elements in blood and skin of bottlenose dolphins in Sarasota Bay, Florida: implications for non-invasive monitoring.

Several major unusual mortality events occurring in recent years have increased the level of concern for the health of bottlenose dolphin populations along the United States Atlantic and Gulf of Mexico coasts. Trace element concentrations were examined in a population of free-ranging dolphins in Sarasota Bay, Florida, in order to develop a benchmark for future comparisons within and between populations. Whole blood (n=51) and skin (n=40) samples were collected through capture and release health assessment events during 2002-2004. Samples were analyzed for Al, V, Cr, Mn, Cu, Zn, As, Se, Rb, Sr, Mo, Cd, and Pb by inductively coupled plasma mass spectrometry (ICPMS) and Hg via atomic fluorescence spectrometry (AFS). Trace element concentrations (wet mass) in skin were 2 to 45 times greater than blood, except Cu was approximately 1.5 times higher in blood. Statistically strong correlations (p<0.05) were found for V, As, Se, Rb, Sr, and Hg between blood and skin demonstrating that these tissues can be used as effective non-lethal monitoring tools. The strongest correlation was established for Hg (r=0.9689) and concentrations in both blood and skin were above the threshold at which detrimental effects are observed in other vertebrate species. Female dolphins had significantly greater Hg concentrations in blood and skin and Pb concentrations in skin, relative to males. Calves exhibited significantly lower V, As, and Hg concentrations in blood and V and Hg concentrations in skin, relative to other age classes. Rubidium and Cu concentrations in skin were greatest in subadults and calves, respectively. In blood, V, Zn, and As concentrations were significantly greater in winter, relative to summer, and the opposite trend was observed for Rb and Sr concentrations. In skin, Cu and Zn concentrations were significantly greater in winter, relative to summer, and the opposite trend was observed for Mn, Rb, Cd, and Pb concentrations. The baseline concentrations and trends established in this study will serve as a benchmark for comparison and aid in sampling design for future monitoring of this population and other coastal bottlenose dolphin populations.

Diamondback terrapins, Malaclemys terrapin, as a sentinel species for monitoring mercury pollution of estuarine systems in South Carolina and Georgia, USA.

Total mercury concentrations were measured in diamondback terrapin blood and scutes collected from four sites in South Carolina, USA, and at a superfund site in Brunswick, Georgia, USA. There was a strong correlation between mercury concentrations in the two terrapin body compartments (Kendall's tau = 0.79, p < 0.001). Mercury concentrations in terrapin scute and blood and in salt marsh periwinkles, Littoraria irrorata, were significantly higher in Brunswick (scute x = 3810.2 ng/g, blood x = 746.2 ng/g) than from all other sites (scute x = 309.5 ng/g, blood x = 43.2 ng/g, p < 0.001). Seasonal fluctuations of total mercury in the blood and scutes of terrapins collected in the Ashley River, South Carolina, were significantly lower in August than in April, June, or October in blood (p < 0.001); however, scute concentrations did not vary seasonally. Overall, we found higher concentrations of mercury in the scutes of females than males (n = 32, p < 0.05). Larger females may preferentially prey on larger food items, like large periwinkles, which had significantly higher mercury levels in their body tissues than smaller periwinkles (p < 0.001). Methylmercury levels in terrapin scutes were measured, revealing that 90% of the total mercury stored in this compartment was in the organic form. A methylmercury biomagnification factor of 173.5 was calculated from snails to terrapin scutes, and we found that mercury levels in scutes were representative of the mercury levels in other compartments of the ecosystem. These findings show that terrapin scutes are good predictors of mercury pollution and that this species could be used as a bioindicator for assessing mercury contamination of estuarine systems.

Simultaneous determination of inorganic mercury, methylmercury, and total mercury concentrations in cryogenic fresh-frozen and freeze-dried biological reference materials.

Two speciated isotope dilution (SID) approaches consisting of a single-spike (SS) method and a double-spike (DS) method including a reaction/transformation model for the correction of inadvertent transformations affecting mercury species were compared in terms of accuracy, method performance, and robustness for the simultaneous determination of methylmercury (MeHg), inorganic mercury (iHg), and total mercury (HgT) concentrations in five biological Standard Reference Materials (SRMs). The SRMs consisted of oyster and mussel tissue materials displaying different mercury species concentration levels and different textural/matrix properties including freeze-dried (FD) materials (SRMs 1566b, 2976, and 2977) and cryogenically prepared and stored fresh-frozen (FF) materials (SRMs 1974a, 1974b). Each sample was spiked with (201)iHg (Oak Ridge National Laboratory, ORNL) and Me(202)Hg (Institute for Reference Materials and Measurements. IRMM-670) solutions and analyzed using alkaline microwave digestion, ethylation, and gas chromatography inductively coupled plasma mass spectrometry (GC/ICP-MS). The results obtained by the SS-SID method suggested that FF and FD materials are not always commutable for the simultaneous determination of iHg, MeHg, and HgT, due to potential transformation reactions resulting probably from the methodology and/or from the textural/matrix properties of the materials. These transformations can occasionally significantly affect mercury species concentration results obtained by SS-SID, depending on the species investigated and the materials considered. The results obtained by the DS-SID method indicated that the two classes of materials were commutable. The simultaneous and corrected concentrations of iHg, MeHg, and HgT obtained by this technique were not found to be statistically different form the certified and reference concentration together with their expanded uncertainty budgets for the five SRMs investigated, exemplifying the robustness, the accuracy, and the improved commutability of this method compared to SS-SID measurements.

Metal complexes and free radical toxins produced by Pfiesteria piscicida.

Metal-containing organic toxins produced by Pfiesteria piscicida were characterized, for the first time, by corroborating data obtained from five distinct instrumental methods: nuclear magnetic resonance spectroscopy (NMR), inductively coupled plasma mass spectrometry (ICP-MS), liquid chromatography particle beam glow discharge mass spectrometry (LC/PB-G DMS), electron paramagnetic resonance spectroscopy (EPR), and X-ray absorption spectroscopy (XAS). The high toxicity of the metal-containing toxins is due to metal-mediated free radical production. This mode of activity explains the toxicity of Pfiesteria, as well as previously reported difficulty in observing the molecular target, due to the ephemeral nature of radical species. The toxins are highly labile in purified form, maintaining activity for only 2-5 days before all activity is lost. The multiple toxin congeners in active extracts are also susceptible to decomposition in the presence of white light, pH variations, and prolonged heat. These findings represent the first formal isolation and characterization of a radical forming toxic organic-ligated metal complex isolated from estuarine/marine dinoflagellates. These findings add to an increased understanding regarding the active role of metals interacting with biological systems in the estuarine environment, as well as their links and implications to human health.

Standard reference materials for foods and dietary supplements.

Well-characterized certified reference materials are needed by laboratories in the food testing, dietary supplement, and nutrition communities to facilitate compliance with labeling laws and improve the accuracy of information provided on product labels, so that consumers can make good choices. As a result of the enactment of the Nutrition Labeling and Education Act of 1990 and the Infant Formula Act of 1980, the National Institute of Standards and Technology (NIST) worked to develop a series of food-matrix standard reference materials (SRMs) characterized for nutrient concentrations. These include SRM 1544 Fatty Acids and Cholesterol in a Frozen Diet Composite, SRM 1546 Meat Homogenate, SRM 1548a Typical Diet, SRM 1566b Oyster Tissue, SRM 1846 Infant Formula, SRM 1946 Lake Superior Fish Tissue, SRM 1947 Lake Michigan Fish Tissue, SRM 2383 Baby Food Composite, SRM 2384 Baking Chocolate, SRM 2385 Slurried Spinach, and SRM 2387 Peanut Butter. With the enactment of the Dietary Supplement Health and Education Act of 1994, NIST has been working to develop suites of dietary supplement SRMs characterized for active and marker compounds and for toxic elements and pesticides, where appropriate. An updated SRM 1588b Organics in Cod Liver Oil, a suite of ephedra-containing materials (SRMs 3240-3245), a carrot extract in oil (SRM 3276), and a suite of ginkgo-containing materials (SRMs 3246-3248) are available. Several other materials are currently in preparation. Dietary supplements are sometimes provided in forms that are food-like; for these, values may also be assigned for nutrients, for example SRM 3244 Ephedra-Containing Protein Powder. Both the food-matrix and dietary supplement reference materials are intended primarily for validation of analytical methods. They may also be used as "primary control materials" in assignment of values to in-house (secondary) control materials to confirm accuracy and to establish measurement traceability to NIST.

Development and application of an ultratrace method for speciation of organotin compounds in cryogenically archived and homogenized biological materials.

An accurate, ultra-sensitive and robust method for speciation of mono, di, and tributyltin (MBT, DBT, and TBT) by speciated isotope-dilution gas chromatography-inductively coupled plasma-mass spectrometry (SID-GC-ICPMS) has been developed for quantification of butyltin concentrations in cryogenic biological materials maintained in an uninterrupted cryo-chain from storage conditions through homogenization and bottling. The method significantly reduces the detection limits, to the low pg g(-1) level (as Sn), and was validated by using the European reference material (ERM) CE477, mussel tissue, produced by the Institute for Reference Materials and Measurements. It was applied to three different cryogenic biological materials-a fresh-frozen mussel tissue (SRM 1974b) together with complex materials, a protein-rich material (whale liver control material, QC03LH03), and a lipid-rich material (whale blubber, SRM 1945) containing up to 72% lipids. The commutability between frozen and freeze-dried materials with regard to spike equilibration/interaction, extraction efficiency, and the absence of detectable transformations was carefully investigated by applying complementary methods and by varying extraction conditions and spiking strategies. The inter-method results enabled assignment of reference concentrations of butyltins in cryogenic SRMs and control materials for the first time. The reference concentrations of MBT, DBT, and TBT in SRM 1974b were 0.92 +/- 0.06, 2.7 +/- 0.4, and 6.58 +/- 0.19 ng g(-1) as Sn (wet-mass), respectively; in SRM 1945 they were 0.38 +/- 0.06, 1.19 +/- 0.26, and 3.55 +/- 0.44 ng g(-1), respectively, as Sn (wet-mass). In QC03LH03, DBT and TBT concentrations were 30.0 +/- 2.7 and 2.26 +/- 0.38 ng g(-1) as Sn (wet-mass). The concentration range of butyltins in these materials is one to three orders of magnitude lower than in ERM CE477. This study demonstrated that cryogenically processed and stored biological materials are a promising alternative to conventional freeze-dried materials for organotin speciation analysis, because these are, at present, the best conditions for minimizing degradation of thermolabile species and for long-term archival. Finally, the potential of the analytical method was illustrated by analysis of polar bear (Ursus maritimus) and beluga whale (Delphinapterus leuca) liver samples that had been collected in the Arctic and archived at the Marine Environmental Specimen Bank. Significant concentrations of butyltin compounds were found in the samples and provide the first evidence of the presence of this class of contaminant in the Arctic marine ecosystem. Figure Eye catch image.

Murre eggs (Uria aalge and Uria lomvia) as indicators of mercury contamination in the Alaskan marine environment.

Sixty common murre (Uria aalge) and 27 thick-billed murre (Uria lomvia) eggs collected by the Seabird Tissue Archival and Monitoring Project (STAMP) in 1999-2001 from two Gulf of Alaska and three Bering Sea nesting colonies were analyzed for total mercury (Hg) using isotope dilution cold vapor inductively coupled mass spectrometry. Hg concentrations (wet mass) ranged from 0.011 microg/g to 0.357 microg/g (relative standard deviation = 76%), while conspecifics from the same colonies and years had an average relative standard deviation of 33%. Hg levels in eggs from the Gulf of Alaska (0.166 microg/g +/- 0.011 microg/g) were significantly higher (p < 0.0001) than in the Bering Sea (0.047 microg/g +/- 0.004 microg/g). Within the Bering Sea, Hg was significantly higher (p = 0.0007) in eggs from Little Diomede Island near the arctic than at the two more southern colonies. Although thick-billed and common murres are ecologicallysimilar,there were significant species differences in egg Hg concentrations within each region (p < 0.0001). In the Bering Sea, eggs from thick-billed murres had higher Hg concentrations than eggs from common murres, while in the Gulf of Alaska, common murre eggs had higher concentrations than those of thick-billed murres. A separate one-way analysis of variance on the only time-trend data currently available for a colony (St. Lazaria Island in the Gulf of Alaska) found significantly lower Hg concentrations in common murre eggs collected in 2001 compared to 1999 (p = 0.017). Results from this study indicate that murre eggs may be effective monitoring units for detecting geographic, species, and temporal patterns of Hg contamination in marine food webs. The relatively small intracolony variation in egg Hg levels and the ability to consistently obtain adequate sample sizes both within and among colonies over a large geographic range means that monitoring efforts using murre eggs will have suitable statistical power for detecting environmental patterns of Hg contamination. The potential influences of trophic effects, physical transport patterns, and biogeochemical processes on these monitoring efforts are discussed, and future plans to investigate the sources of the observed variability are presented.

Monitoring mercury in the loggerhead sea turtle, Caretta caretta.

The validity of using blood samples and keratinized scutes for nonlethal routine monitoring of mercury (Hg) in loggerhead sea turtles, Caretta caretta, is evaluated in the context of how effectively these matrixes predict internal tissue Hg burdens and the different temporal scales of exposure they represent. Total Hg (THg) was measured in blood and scutes collected from live captures (n = 34) and liver, kidney, muscle, spinal cord, blood, and scutes collected from freshly stranded loggerhead turtles (n = 6) along the coast of the southeastern United States. Linear regressions between monitoring compartments and internal tissues from stranded animals were all statistically significant (r2 > 0.805, p < 0.015) but varied in their utility as a predictive tool depending on which tissues were paired. Blood was an effective predictor of THg in muscle (r2 = 0.988, p < 0.0001) and spinal cord (r2 = 0.988, p < 0.0001), while scute was the most accurate predictor of THg in liver (r2 = 0.948, p = 0.0010). The strength of the relationship between tissues types is believed to reflect the similarity in the temporal scales they represent and the variability in the fraction of methylmercury present. The stability of Hg in the scute matrix makes this tissue preferable for approximating long-term exposure, while blood Hg levels can be affected by recent changes in Hg intake. THg levels in blood and scutes from live captures were highly correlated (linear regression r2 = 0.926, p < 0.0001) and increased significantly with body mass (r2 = 0.173, p = 0.016 and r2 = 0.187, p = 0.012 respectively), further supporting thatthere is a component reflecting long-term accumulation of Hg in these matrixes. We also present a novel technique using the residuals from the blood-scute regression as an index of recent exposure (IRE). The interpretation of this value is derived from the comparison between the most recent Hg intake (which contributes to the Hg measured in the blood) relative to the average past intake (which is recorded in the scute). A stepwise multiple regression revealed a significant positive relationship between the IRE and the proximity of the capture site to the nearest major industrial river mouth (p = 0.0102). This suggests that there is an elevation of bioavailable Hg in nearshore habitats where terrestrial influences and anthropogenic impacts are high. Seasonal foraging site fidelity and the variability in environmental Hg may explain the high intraspecific variability and occasional highly contaminated turtle seen in this and previous studies.