Threshold and dose response estimation using the “filter model”

The “filter model” has been developed to explain the biologic effects of radiation and chemicals. We have examined nearly 300 sets of dose response data, of which 50 are presented here. Responses (induced by radiation and chemicals) which have been examined include in vitro survival studies on animal and plant tissues, induction of cellular aberrations and time to tumor or death. Similar data from in vivo studies has also been examined. All of the data appear to fit the model R = a lnD + b(lnD)² + c, where R is the response, a and b are parameters fitted by regression to a particular set of data, and c is the response at zero (or lowest) dose. By writing this model in exponential form, it can be seen that the response R results from multistage filtering (by net amounts a and b) of the initial dose, D. The threshold is obtained from this model as the point, $\text{D}\text{?}{}_{\mathrm{T}}$, at which the second derivative becomes zero. This is given by $\text{D}\text{?}{}_{\mathrm{T}}\text{=}\text{exp}\text{(1 ?}\text{a}\text{2b}\text{)}$ when a and b are oppositelt signed.     

Determination of 99Tc, 63Ni and 121m+126Sn in the marine environment

Four artificially produced radionuclides (${}^{99}\text{Tc, t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 2·15 × 10}{}^5\text{y;}{}^{63}\text{Ni, t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 93 y}$ and ${}^{\mathrm{121m+126}}\text{Sn, t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 55·5 y}$) have been analyzed in sediments and organisms from the marine environment. The samples were obtained from the vicinities of nuclear energy facilities, at sites of nuclear weapon tests and at sites remote from both of these locales. The activities of these nuclides per unit dry weight are remarkably similar at the first two of the above areas but are usually detectable only with difficulty, if at all, in the third area. Techniques for sample treatment and measurement are given.     

Air-to-vegetation transfer rates of natural submicron aerosols

Submicron aerosol deposition to outdoor vegetation was evaluated by measuring vegetation and air concentrations of ²¹²Pb, ²¹⁴Pb, and ⁷Be attached to atmospheric aerosols. A biomass-normalized deposition velocity (V_D), with units of m³ kg^?1 s^?1, was used to compare species and isotopes with respect to air-to-vegetation transfer rates. For ²¹²Pb ($\text{t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 10·64 h}$), higher night-time air concebtrations dominate deposition, while for ²¹⁴Pb ($\text{t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 26·8}\text{min}$), deposition measurements over shorter time periods relative to changing atmospheric conditions were possible. Calculated V_D values were usually higher for ²¹⁴Pb, possibly reflecting wind-enhanced deposition during the afternoon period of sampling. Evergreen species, including pines, were not appreciably different from deciduous species. Most striking was the narrow range of results (factor of 6 for 34 ²¹²Pb measurements of 20 species). Beryllium-7 ($\text{t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 53·3 d}$) was used to evaluate time-integrated deposition by sampling vegetation in California near the end of dry summers. Similar deposition rates were found for this isotope. The results of the study indicated that naturally radioactive atmospheric aerosols can be used to understand the dynamics of submicron aerosol deposition to ecosystems.     

Uptake and loss of technetium-95m in the crab Pachygrapsus marmoratus

The uptake and loss kinetics of ^95mTc in seawater have been investigated in the crab Pachygrapsus marmoratus. Both the uptake and loss kinetics can be represented as the sum of two exponential functions, one short-term ($\text{tb}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 16}\text{d}$) and one long-term ($\text{tb}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 63}\text{d}$), $\text{tb}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}$ being the biological half-time. The predicted steady state concentration factor was estimated to be about 18.No significant linear correlation between Tc uptake rate and animal weight was found during the accumulation phase. At the end of this phase, 77% of the Tc was found to be distributed in the digestive system and particularly in the hepatopancreas (56%); this organ also appeared to lose the radionuclide most quickly. During the loss phase, 90% of the incorporated radioactivity was eliminated in about three months. Therefore P. marmoratus does not appear to be a good bioindicator of Tc in the marine environment nor an important pathway for Tc contamination along marine food chains.     

Nonidentifiability of competing risks

Frequently one is interested in examining the survival experience of a set of individuals exposed to k risks. If W is the time of failure for the individual and J is the indicator variable for cause of death, then the competing risk framework assumes that W = min X_i and J = j if X_j is the minimum, where the X_i's are the survival lifetimes when only risk R_i is operating on the population. To examine the underlying structure of the survival experience one has to know the joint distribution of the $\text{X}{}_{\mathrm{i}}\text{(F}{}_{\mathrm{<mtext>x</mtext>}}\text{)}$. It is shown here that if only W and J are observed, the joint distribution of the $\text{X}{}_{\mathrm{i}}\text{(F}{}_{\mathrm{<mtext>x</mtext>}}\text{)}$ is nonidentifiable.     

Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991-2005

A radioactivity survey was launched in 1991 to determine the background levels of ^239+240Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the ²⁴⁰Pu/²³⁹Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of ^239+240Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the ^239+240Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of ^239+240Pu observed in the bottom water sample at sampling points having greater depth. The ²⁴⁰Pu/²³⁹Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The ²⁴⁰Pu/²³⁹Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing ^239+240Pu concentration and also decreasing the ²⁴⁰Pu/²³⁹Pu atom ratio with sea depth, and further study is required to clarify it.     

Anthropogenic radionuclides in sediment in the Japan Sea: distribution and transport processes of particulate radionuclides

Distributions of anthropogenic radionuclides (⁹⁰Sr, ¹³⁷Cs and ^239+240Pu) in seabed sediment in the Japan Sea were collected during the period 1998–2002. Concentration of ⁹⁰Sr, ¹³⁷Cs and ^239+240Pu in seabed sediment was 0.07–1.6 Bq kg⁻¹, 0.4–9.1 Bq kg⁻¹ and 0.002–1.9 Bq kg⁻¹, respectively. In the northern basin of the sea (Japan Basin), ^239+240Pu/¹³⁷Cs ratios in seabed sediment were higher and their variation was smaller compared to that in the southeastern regions of the sea. The higher ^239+240Pu/¹³⁷Cs ratios throughout the Japan Basin were considered to reflect production of Pu-enriched particles in the surface layer and substantial sinking of particulate materials in this region. In the southern regions of the Japan Sea (<38°N), both inventories and ^239+240Pu/¹³⁷Cs ratios in sediment were larger than those in the other regions. In the southern Japan Sea, observations suggested that supply of particulate radionuclides by the Tsushima Warm Current mainly enhanced accumulation of the radionuclides in this region.     

Comparing computing formulas for estimating concentration ratios

The purpose of this paper is to provide guidance on the choice of computing formulas (estimators) for estimating average concentration ratios and other ratio-type measures of radionuclides and other environmental contaminant transfers between ecosystem components. Mathematical expressions for the expected value of three commonly used estimators (arithmetic mean of ratios, geometric mean of ratios, and the ratio of means) are obtained when the multivariate lognormal distribution is assumed. These expressions are used to explain why these estimators will not in general give the same estimate of the average concentration ratio. They illustrate that the magnitude of the discrepancies depends on the magnitude of measurement biases, and on the variance and correlations associated with spatial heterogeneity and measurement errors. This paper also reports on a computer simulation study that compares the accuracy of eight computing formulas for estimating a ratio relationship that is constant over time and/or space. Statistical models appropriate for both controlled spiking experiments and observational field studies for either normal or lognormal distributions are considered. Our results indicate that for either type of study the geometric mean is generally preferred if the lognormal distribution applies. However, the geometric mean has the disadvantage that its expected value depends on n, the number of measurements taken. Ricker's estimator, $\text{R}\text{?}{}_{\mathrm{rt}}$, appears to perform worse than the other estimators studied when the observations are lognormal. All eight estimators appear to be equally accurate for the controlled spiking study when data are normally distributed. For observational field studies when data are normally distributed the ratio of means or slight modifications thereof are preferred to other estimators investigated. Before one chooses a computing formula for estimating a concentration ratio, thought should be given to what target value needs to be estimated to satisfy study objectives, and to whether the normal or lognormal distribution is a more realistic model. The geometric mean performs well for lognormal distributions, but comparison of geometric means or of a geometric mean with environmental limits can be misleading if n is small. The arithmetic mean of ratios is a conservative choice in that it will always give a larger estimate than will the geometric mean. It may also be severely biased when data are lognormal and the variances of measurement errors are large. The ratio of the means is a reasonable choice if the distribution is normal. The median of the observed ratios, $\text{R}\text{?}{}_{\mathrm{<mtext>md</mtext>}}$, is useful estimate since it is easily obtained and has an easily understood interpretation as the point above which and below which 50% of the observed ratios lie. Also, it is appropriate no matter what the distribution of the observed ratios may be. Confidence limits on the median are also easily obtained. Finally, while this paper emphasizes applications in radionuclide research, our results should be applicable to a wide range of environmental contaminants since many contaminants have approximately lognormal distributions.     

Characterization of plutonium in deep-sea sediments of the Sulu and South China Seas

Anthropogenic Pu isotopes are important geochemical tracers for sediment studies. Their distributions and sources in the water columns as well as the sediments of the North Pacific have been intensively studied; however, information about Pu in the Southeast Asian seas is limited. To study the isotopic composition of Pu, and thus to identify its sources, we collected sediment core samples in the South China Sea and the Sulu Sea during the KH-96-5 Cruise of the R/V Hakuho Maru. We analysed the activities of ^239+240Pu and the atom ratios of ²⁴⁰Pu/²³⁹Pu using isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The ²⁴⁰Pu/²³⁹Pu atom ratios in the sediments of both areas (inventory weighted mean: 0.251 for the South China Sea and 0.280 for the Sulu Sea) were higher than the global fallout value (0.178 ± 0.019), suggesting the existence of Pu from the Pacific Proving Grounds in the North Pacific. Low inventories of ^239+240Pu in sediments were observed in the South China Sea (3.75 Bq/m²) and the Sulu Sea (1.38 Bq/m²). Most of the Pu input is still present in the water column. Scavenging and benthic mixing processes were considered to be the main processes controlling the distribution of Pu in the deep-sea sediments of both study areas.     

The accumulation of plutonium by the edible winkle (Littorina littorea L.)

Laboratory experiments were carried out to measure the accumulation of ²³⁷Pu by the edible winkle from labelled sea water, food (seaweed), and silt. The equilibrium whole body concentration factor for ²³⁷Pu accumulation from sea water at 10°C was estimated as 34 with a biological half-time of 9 d. After 50 d accumulation, 83% of the measured whole body activity was present on the shell. In the flesh, the major sites for accumulation were the head/foot complex and the digestive gland. Depuration was found to be biphasic with components having half-times of 10 and 193 d respectively. Pu loss, following uptake from labelled Fucus spiralis, was biphasic with half-times of 1 and 69 d for the two components. Assimilation efficiency was tentatively estimated as 7%. Pu accumulation from labelled silt was low with an estimated transfer factor of 0.004; Pu loss was biphasic, with half-times similar to those for the seaweed experiment. Comparison of the laboratory-derived results with those for winkles from the environment showed that the food pathway was the main route for Pu accumulation, with the ingestion of silt playing a critical role in determining the final flesh Pu burden.     

The distribution and inventory of fallout plutonium in sediments of the Ligurian Sea near La Spezia,Italy

Pu concentrations in surface sediments of the Ligurian Sea are about ten times higher than in adjacent river sediments and are highly correlated with sediment porosities. The integrated inventory of ^239,240Pu in a sediment core is calculated to be 3·5 mCi km^?2, nearly twice the average input from fallout at these latitudes, apparently because Pu is removed from seawater by particle scavenging.The sedimentation rate is calculated from the depth of the ^239,240Pu maximum to be 0·52 ± 0·06 cmy^?1.     

Statistical assessment of subsampling procedures

As shown by the examples in this paper, the concentrations in subsamples are not necessarily independently and normally distributed despite vigorous grinding and mixing of the original sample. Studies of the statistical properties of subsample concentrations should test for deviations from independence and normality and, if deviations are found, should model the observed distribution. The tests include an analysis of variance to check for less variation among nearby subsamples than among widely spaced subsamples, as well as the computation of the probability plot correlation coefficient to check for nonnormality. These tests are illustrated with ${}^{239}\text{Pu}\text{+}{}^{240}\text{Pu}$ measurements on subsamples prepared for use as standard reference materials. These materials are used in quality assurance for environmental radioactivity measurements. The material consisting of Human Liver (SRM 4352) exhibits dependence, which may be due to inadequate mixing or to later handling that caused segregation. The material consisting of Human Lung (SRM 4351) and the material consisting of soil from Rocky Flats (SRM 4353) exhibit nonnormality due to the particulate nature of some plutonium-bearing fractions of the material. The lung measurements are modeled with the gamma distribution. The soil measurements are modeled with a combination of the normal distribution and a distribution that models the occurrence of outliers. The use of these models to describe the subsamples involves assessment of the contribution of the measurement error.     

The mass spectrometric determination of fallout 239Pu and 240Pu in marine samples

A thermal ionization mass spectrometric technique is presented for the detection of ²³⁹Pu and ²⁴⁰Pu in sea water, pore water, ocean sediments, sediment trap samples and coral samples. Both sample preparation and purification procedures, as well as the procedure used to detect Pu by mass spectrometry (m.s.), are presented. The m.s. technique proves to be over an order-of-magnitude more sensitive than traditional alpha-counting techniques for the detection of Pu in environmental samples. Also, the ratio of ²⁴⁰Pu/²³⁹Pu is obtained with this technique.     

Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.