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Ann H. Mullin

Publications and source records attributed to Ann H. Mullin.

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Interpreting and Reporting Radiological Water-Quality Data

This document provides information to U.S. Geological Survey (USGS) Water Science Centers on interpreting and reporting radiological results for samples of environmental matrices, most notably water. The information provided is intended to be broadly useful throughout the United States, but it is recommended that scientists who work at sites containing radioactive hazardous wastes need to consult additional sources for more detailed information. The document is largely based on recognized national standards and guidance documents for radioanalytical sample processing, most notably the Multi-Agency Radiological Laboratory Analytical Protocols Manual (MARLAP), and on documents published by the U.S. Environmental Protection Agency and the American National Standards Institute. It does not include discussion of standard USGS practices including field quality-control sample analysis, interpretive report policies, and related issues, all of which shall always be included in any effort by the Water Science Centers. The use of 'shall' in this report signifies a policy requirement of the USGS Office of Water Quality.

Techniques and Methods

Occurrence of selected radionuclides in ground water used for drinking water in the United States: A reconnaissance survey, 1998

The U.S. Geological Survey, in collaboration with the U.S. Environmental Protection Agency, the American Water Works Association, and the American Water Works Service Company, completed a targeted national reconnaissance survey of selected radionuclides in public ground-water supplies. Radionuclides analyzed included radium-224 (Ra-224), radium-226 (Ra-226), radium-228 (Ra-228), polonium-210 (Po-210) and lead-210 (Pb-210).This U.S. Geological Survey reconnaissance survey focused intentionally on areas with known or suspected elevated concentrations of radium in ground water to determine if Ra-224 was also present in the areas where other isotopes of radium had previously been detected and to determine the co-occurrence characteristics of the three radium isotopes (Ra-224, Ra-226, and Ra-228) in those areas. Ninety-nine raw-water samples (before water treatment) were collected once over a 6-month period in 1998 and 1999 from wells (94 of which are used for public drinking water) in 27 States and 8 physiographic provinces. Twenty-one of the 99 samples exceeded the current U.S. Environmental Protection Agency drinking-water maximum contaminant level of 5 picocuries per liter (pCi/L) for combined radium (Ra-226 + Ra-228). Concentrations of Ra-224 were reported to exceed 1 pCi/L in 30 percent of the samples collected, with a maximum concentration of 73.6 pCi/L measured in water from a nontransient, noncommunity, public-supply well in Maryland. Radium-224 concentrations generally were higher than those of the other isotopes of radium. About 5 percent of the samples contained concentrations of Ra-224 greater than 10 pCi/L, whereas only 2 percent exceeded 10 pCi/L for either Ra-226 or Ra-228. Concentrations of Ra-226 greater than 1 pCi/L were reported in 33 percent of the samples, with a maximum concentration of 16.9 pCi/L measured in water from a public-supply well in Iowa. Concentrations of Ra-228 greater than 1 pCi/L were reported in 22 samples, with a maximum concentration of 72.3 pCi/L measured in water from a non-transient, noncommunity, public-supply well in Maryland.Radium-224, which is a decay product of Ra-228 in the Th-232 decay series, was significantly correlated with Ra-228 (Spearman?s rank correlation coefficient ?r? equals 0.82) and to a lesser degree with Ra-226 (r equals 0.69), which is an isotope in the U-238 decay series. The rank correlation coefficient between Ra-226 and Ra-228 was 0.63. The high correlation between Ra-224 and Ra-228 concentrations and the corresponding isotopic ratios of the two (about 1:1 in 90 percent of the samples) indicates that the two radionuclides occur in approximately equal concentrations in most ground water sampled. Thus, Ra-228 can be considered as a reasonable proxy indicator for the occurrence of Ra-224 in ground water.The maximum concentration of Po-210 was 4.85 pCi/L and exceeded 1 pCi/L in only two samples. The maximum concentration of Pb-210 was 4.14 pCi/L, and about 10 percent of the samples exceeded 1 pCi/L. Areas with known, or suspected, elevated concentrations of polonium and lead were not targeted in this survey.Three major implications are drawn for future radionuclide monitoring on the basis of this information: (1) grossalpha particle analyses of ground water should be done within about 48-72 hours after collection to determine the presence of the short-lived, alpha-particle emitting isotopes, such as Ra-224, which was detected in elevated concentrations in many of the samples collected for this survey; (2) the isotope ratios of Ra-224 to Ra-228 in ground water are variable on a national scale, but the two radioisotopes generally occur in ratios near 1:1, therefore, the more commonly measured Ra-228 can be used as an indicator of Ra-224 occurrence for some general purposes other than compliance; and (3) the isotopic ratios of Ra-226 to Ra-228 were less than 3:2 in many samples. These ratios corroborate results of previous studies that have shown the presence of Ra-228.

Water-Resources Investigations Report

Gross-beta activity in ground water: natural sources and artifacts of sampling and laboratory analysis

Gross-beta activity has been used as an indicator of beta-emitting isotopes in water since at least the early 1950s. Originally designed for detection of radioactive releases from nuclear facilities and weapons tests, analysis of gross-beta activity is widely used in studies of naturally occurring radioactivity in ground water. Analyses of about 800 samples from 5 ground-water regions of the United States provide a basis for evaluating the utility of this measurement. The data suggest that measured gross-beta activities are due to (1) long-lived radionuclides in ground water, and (2) ingrowth of beta-emitting radionuclides during holding times between collection of samples and laboratory measurements. Although 40 K and 228 Ra appear to be the primary sources of beta activity in ground water, the sum of 40 K plus 228 Ra appears to be less than the measured gross-beta activity in most ground-water samples. The difference between the contribution from these radionuclides and gross-beta activity is most pronounced in ground water with gross-beta activities > 10 pCi/L, where these 2 radionuclides account for less than one-half the measured ross-beta activity. One exception is groundwater from the Coastal Plain of New Jersey, where 40 K plus 228 Ra generally contribute most of the gross-beta activity. In contrast, 40 K and 228 Ra generally contribute most of beta activity in ground water with gross-beta activities < 1 pCi/L. The gross-beta technique does not measure all beta activity in ground water. Although 3 H contributes beta activity to some ground water, it is driven from the sample before counting and therefore is not detected by gross-beta measurements. Beta-emitting radionuclides with half-lives shorter than a few days can decay to low values between sampling and counting. Although little is known about concentrations of most short-lived beta-emitting radionuclides in environmental ground water (water unaffected by direct releases from nuclear facilities and weapons tests), their activities are expected to be low. Ingrowth of beta-emitting radionuclides during sample holding times can contribute to gross-beta activity, particularly in ground water with gross-beta activities > 10 pCi/L. Ingrowth of beta-emitting progeny of 238 U, specifically 234 Pa and 234 Th, contributes much of the measured gross-beta activity in ground water from 4 of the 5 areas studied. Consequently, gross-beta activity measurements commonly overestimate the abundance of beta-emitting radionuclides actually present in ground water. Differing sample holding times before analysis lead to differing amounts of ingrowth of the two progeny. Therefore, holding times can affect observed gross-beta measurements, particularly in ground water with 238 U activities that are moderate to high compared with the activity of 40 K plus 228 Ra. Uncertainties associated with counting efficiencies for beta particles with different energies further complicate the interpretation of gross-beta measurements.

Applied Geochemistry