On the Correction of Spatial and Statistical Uncertainties in Systematic Measurements of 222Rn for Earthquake Prediction

In earthquake prediction studies, the regional behaviour of accurate ²²²Rn measurements at a set of sites plays a significant role. Here, measurements are obtained using active and passive radon detector systems in an earthquake-active region of Turkey. Two new methods are proposed to explain the spatial behaviours and the statistical uncertainties in the ²²²Rn emission measurements along fault lines in relation to earthquake occurrence. The absolute point cumulative semivariogram (APCSV) and perturbation method (PM) help to depict the spatial distribution patterns of ²²²Rn in addition to the joint effects of the K _dr, the radon distribution coefficient, and the perturbation radon distribution coefficient (PRDC). The K _dr coefficient assists in identifying the spatial distributional behaviour in ²²²Rn concentrations and their migration along the Earth’s surface layers. The PRDC considers not only the arithmetic averages but also the variances (or standard deviations) and the correlation coefficients, in addition to the size of the error among the ²²²Rn measurements. The applications of these methodologies are performed for 13,000 ²²²Rn measurements that are deemed to be sufficient for the characterization of tectonics in the Keban Reservoir along the East Anatolian Fault System (EAFS) in Turkey. The results are evaluated for the ?çme earthquake (M _L 5.4, 5.7 km, 23 June 2011), which occurred in the vicinity of the EAFS.     

Captive balloon measurements of radon 222 and its daughter ions

Summary An instrument for use with a captive balloon has been developed for the investigation of the vertical distribution of²²²Rn and its daughter ions of high mobility. The system consists of a light weight ion collector of the Gerdien type and an automatic air sampler. Simultaneous collections of²²²Rn and its daughter ions having mobilities of known limits makes it possible to determine the concentration of the radioactive ions relative to the ambient concentration of²²²Rn in different atmospheric conditions in the air layer adjacent to the ground where aircraft and tower measurements are not practicable. Vertical profiles taken over a mountain ridge in a well-mixed atmosphere show almost constant concentrations of²²²Rn and its daughter ions with altitude. In some cases a slight increase in the concentrations of²²²Rn and its daughter ions with altitude has been observed. The radioactive ion concentration relative to the ambient concentration of²²²Rn in the boundary layer is of the order of 3%.     

Explicit Modeling of Radon-222 in HydroGeoSphere During Steady State and Dynamic Transient Storage

Transient storage zones (TSZs) are located at the interface of rivers and their abutting aquifers and play an important role in hydrological and biogeochemical functioning of rivers. The natural radioactive tracer ²²²Rn is a particularly well-suited tracer for studying TSZ water exchange and age. Although ²²²Rn measurement techniques have developed rapidly, there has been less progress in modeling ²²²Rn activities. Here, we combine field measurements with the numerical model HydroGeoSphere (HGS) to simulate ²²²Rn emanation, decay and transport during steady state (riffle-pool sequence) and transient (bank storage) conditions. Comparing the HGS mean water ages with the conventional ²²²Rn apparent ages during steady state showed a systemic underestimation of apparent age with increasing dispersion and especially where large concentration gradients exist within the subsurface. A large underestimation of apparent water age was also observed at the advective front during bank storage where regional high ²²²Rn groundwater mixes with newly infiltrated surface water. The explicit modeling of radiogenic tracers such as ²²²Rn offers a physical interpretation of this data as well as a useful way to test simplified apparent age models.     

Release of 222Rn from some soils

Measurements have been made of ²²²Rn release from diverse soils in the region surrounding Malaga, Spain. These flux measurements were carried out by two methods. A direct method using a static chamber technique and another indirect method obtained from concentration profile measurements of ²²²Rn in the soil air. The effects of meteorological variables and other parameters on ²²²Rn flux were studied. The factors that most affected the instantaneous value of ²²²Rn release were humidity and soil thermal gradient. The directly measured ²²²Rn fluxes at investigated sites are higher than ²²²Rn fluxes derived by the indirect method.     

Using new mass balance methods to estimate gross surface water and groundwater exchange with naturally occurring tracer 222Rn in data poor regions: a case study in northwest China

Given that the concentration of ²²²Rn in groundwater is much higher than that in surface water and that its radioactive half‐life (3.83 d) is short, ²²²Rn is an effective tracer of groundwater–surface water interactions. In this study, a new mass balance method is presented, which can be used to estimate specific groundwater–surface water interactions within a river reach. Three possible situations of interaction between groundwater and surface water are considered, and equations based on the mass conservation of ²²²Rn are formulated for judging specific groundwater–surface water interaction processes and for calculating water flux. A case study was conducted for the Nalenggele River, Northwest China, to demonstrate the usefulness of this method. Samples of river water and groundwater containing ²²²Rn were collected from the study area to estimate the interactions between groundwater and surface water. The amount of water exchanged during these interactions was estimated and the results show that transformations between groundwater and surface water are frequent along the stream. The ²²²Rn mass balance method is highly sensitive for studying such interactions, even in areas for which conventional hydrologic data are sparse. Copyright © 2014 John Wiley & Sons, Ltd.     

Network of seismo-geochemical monitoring observatories for earthquake prediction research in India

Present paper deals with a brief review of the research carried out to develop multi-parametric gas-geochemical monitoring facilities dedicated to earthquake prediction research in India by installing a network of seismo-geochemical monitoring observatories at different regions of the country. In an attempt to detect earthquake precursors, the concentrations of helium, argon, nitrogen, methane, radon-222 (²²²Rn), polonium-218 (²¹⁸Po), and polonium-214 (²¹⁴Po) emanating from hydrothermal systems are monitored continuously and round the clock at these observatories. In this paper, we make a cross correlation study of a number of geochemical anomalies recorded at these observatories. With the data received from each of the above observatories we attempt to make a time series analysis to relate magnitude and epicentral distance locations through statistical methods, empirical formulations that relate the area of influence to earthquake scale. Application of the linear and nonlinear statistical techniques in the recorded geochemical data sets reveal a clear signature of long-range correlation in the data sets.     

Evaluating the source and seasonality of submarine groundwater discharge using a radon-222 pore water transport model

Pore water radon (²²²Rn) distributions from Indian River Lagoon, Florida, are characterized by three zones: a lower zone where pore water ²²²Rn and sediment-bound radium (²²⁶Ra) are in equilibrium and concentration gradients are vertical; a middle zone where ²²²Rn is in excess of sediment-bound ²²⁶Ra and concentration gradients are concave-downward; and an upper zone where ²²²Rn concentration gradients are nearly vertical. These ²²²Rn data are simulated in a one-dimensional numerical model including advection, diffusion, and non-local exchange to estimate magnitudes of submarine groundwater discharge components (fresh or marine). The numerical model estimates three parameters, fresh groundwater seepage velocity, irrigation intensity, and irrigation attenuation, using two Monte Carlo (MC) simulations that (1) ensure the minimization algorithm converges on a global minimum of the merit function and the parameter estimates are consistent within this global minimum, and (2) provide 90% confidence intervals on the parameter estimates using the measured ²²²Rn activity variance. Model estimates of seepage velocities and discharge agree with previous estimates obtained from numerical groundwater flow models and seepage meter measurements and show the fresh water component decreases offshore and varies seasonally by a factor of nine or less. Comparison between the discharge estimates and precipitation patterns suggests a mean residence time in unsaturated and saturated zones on the order of 5 to 7 months. Irrigation rates generally decrease offshore for all sampling periods. The mean irrigation rate is approximately three times greater than the mean seepage velocity although the ranges of irrigation rates and seepage velocities are the same. Possible mechanisms for irrigation include density-driven convection, wave pumping, and bio-irrigation. Simulation of both advection and irrigation allows the separation of submarine groundwater discharge into fresh groundwater and (re)circulated lagoon water.     

Riverine groundwater discharge estimation in a dynamic river corridor using 222Rn

Groundwater discharge flux into rivers (riverine groundwater discharge or RGD) is essential information for the conservation and management of aquatic ecosystems and resources. One way to estimate area-integrated groundwater discharge into surface water bodies is to measure the concentration of a groundwater tracer within the water body. We assessed groundwater discharge using ²²²Rn, a tracer common in many surface water studies, through field measurements, surface water ²²²Rn mass balance model, and groundwater flow simulation, for the seldom studied but ubiquitous setting of a flooding river corridor. The investigation was conducted at the dam-regulated Lower Colorado River (LCR) in Austin, Texas, USA. We found that ²²²Rn in both the river water and groundwater in the river bank changed synchronously over a 12-hour flood cycle. A ²²²Rn mass balance model allowed for estimation of groundwater discharge into a 500-m long reach of the LCR over the flood. The groundwater discharge ranged between negative values (indicating recharge) to 1570 m³/h; groundwater discharge from groundwater flow simulations corroborated these estimates. However, for the dynamic groundwater discharge estimated by the ²²²Rn box model, assuming whether the groundwater ²²²Rn endmember was constant or dynamic led to notably different results. The resultant groundwater discharge estimates are also highly sensitive to river ²²²Rn values. We thus recommend that when using this approach to accurately characterize dynamic groundwater discharge, the ²²²Rn in near-stream groundwater should be monitored at the same frequency as river ²²²Rn. If this is not possible, the ²²²Rn method can still provide reasonable but approximate groundwater discharge given background information on surface water-groundwater exchange time scales.     

Radon-222 in groundwater of the Long Valley caldera,California

In the Long Valley caldera, where seismicity has continued essentially uninterrupted since mid-1980 and uplift is documented, samples of water from hot, warm, and cold springs have been collected since September, 1982, and their²²²Rn concentrations analyzed. Concurrently, rocks encompassing the hydrologic systems feeding the springs were analyzed for their radioelement contents, because their uranium is the ultimate source of the²²²Rn in the water.The²²²Rn concentration in the springs varies inversely with their temperature and specific conductance. High concentrations (1500 to 2500 picocuries per liter) occur in dilute cold springs on the margins of the caldera, while low contents (12 to 25 pCi/l) occur in hot to boiling springs. Springwater radon concentrations also correlate slightly with the uranium content of the encompassing rocks.A continuous monitoring system was installed in August, 1983, at a spring issuing from basalt, to provide hourly records of radon concentration. A gamma detector is submerged in a natural pool, and we have observed that the radioactivity measured in this manner is due almost entirely to the²²²Rn concentration of the water. Initial operation shows diurnal and semidiurnal variations in the²²²Rn concentration of the springwater that are ascribed to earth tides, suggesting that those variations are responding to small changes in stress in the rocks encompassing the hydrologic system.     

Signification de la présence de radon 222 dans les fluides géothermiques

The²²²Rn content of a subterranean fluid depends on the physico-chemical nature of the media through which the fluid passes and on the time spent by the fluid in the various geological formations encountered. Consequently,²²²Rn measurement in a geofluid gives a clue to the subsurface transport conditions of this geofluid. Simple models are proposed for various types of buried structures connected with the surface by a geothermal well; they all lead to the²²²Rn concentration expressed as a function of the flow-rate of the carrier fluid. In real systems, the variations of this concentration with flow-rate would allow the type of structure feading the well to be determined, and, in propitious circumstances, the volume of the possible reservoir to be estimated.     

Natural 222Rn as a tracer of mixing and volatilization in a shallow aquifer during a CO2 injection experiment

This study aims to evaluate the application of ²²²Rn in groundwater as a tracer for monitoring CO₂ plume migration in a shallow groundwater system, which is important to detect potential CO₂ leakage in the carbon capture and storage (CCS) project. For this research, an artificial CO₂-infused water injection experiment was performed in a shallow aquifer by monitoring hydrogeochemical parameters, including ²²²Rn. Radon in groundwater can be a useful tracer because of its sensitivity to sudden changes in subsurface environment. To monitor the CO₂ plume migration, the data were analysed based on (a) the influence of mixing processes on the distribution of ²²²Rn induced by the artificial injection experiment and (b) the influence of a carrier gas role by CO₂ on the variation of ²²²Rn. The spatio-temporal distributions of radon concentrations were successfully explained in association with horizontal and vertical mixing processes by the CO₂-infused water injection. Additionally, the mixing ratios of each monitoring well were calculated, quantitatively confirming the influence of these mixing processes on the distribution of radon concentrations. Moreover, one monitoring well showed a high positive relationship between ²²²Rn and Total dissolved inorganic carbon (TIC) by the carrier gas effect of CO₂ through volatilization from the CO₂ plume. It indicated the applicability of ²²²Rn as a sensitive tracer to directly monitor CO₂ leakage. When with a little effect of carrier gas, natural ²²²Rn in groundwater can be used to compute mixing ratio of CO₂-infused water indicative of CO₂ migration pathways. CO₂ carrier gas effect can possibly increase ²²²Rn concentration in groundwater and, if fully verified with more field tests, will pose a great potential to be used as a natural tracer for CO₂.     

226Ra and222Rn contents of Galapagos Rift hydrothermal waters —the importance of low-temperature interactions with crustal rocks

Hydrothermal waters collected by “Alvin” from the Galapagos Spreading Center are enriched in²²²Rn by factors of 50–200 over bottom waters. The²²⁶Ra in the same samples, however, is enriched by less than a factor of four over bottom waters. Enrichments of²²²Rn result primarily from α-recoil from rock surfaces while²²⁶Ra enrichments are dominantly produced by high-temperature alteration of cooling ridge volcanics. The abundances of both nuclides exhibit positive correlations with temperature. The data extrapolate to bottom water temperatures and compositions, demonstrating the importance of seawater mixing. Different vents, however, have different mixing lines, and vents with high²²²Rn have low²²⁶Ra. We propose these patterns result from variations in the extent of low-temperature crustal interaction with the hydrothermal fluids. Low-temperature crustal waters can maintain high steady state²²²Rn contents due to the α-recoil additions to the fluids. The²²⁶Ra, however, is strongly adsorbed at low-temperatures resulting in low concentrations of this nuclide in low-temperature crustal waters. Thus, physical mixing of a crustal water component with hydrothermal waters or variable crustal path lengths of the hydrothermal fluids can account for the variable mixing lines and²²²Rn/²²⁶Ra values of the hot springs.The²²²Rn/²²⁶Ra value appears to be a sensitive indicator of low-temperature crustal interaction. Values > 100 have experienced extensive crustal interaction and are indicative of diffuse hydrothermal flow. Values between 1 and 10 are indicative of primary hydrothermal fluids which have not experienced significant interaction with the crust. Values of²²²Rn/²²⁶Ra between 10³ and 10⁴ are indicative of interaction of the hydrothermal fluids with sediments. Such values are observed in water samples from the Galapagos hydrothermal mounds.     

The effect of CO2 on the measurement of 220Rn and 222Rn with instruments utilising electrostatic precipitation

In some volcanic systems, thoron and radon activity and CO₂ flux, in soil and fumaroles, show a relationship between (²²⁰Rn/²²²Rn) and CO₂ efflux. It is theorized that deep, magmatic sources of gas are characterized by high ²²²Rn activity and high CO₂ efflux, whereas shallow sources are indicated by high ²²⁰Rn activity and relatively low CO₂ efflux. In this paper we evaluate whether the observed inverse relationship is a true geochemical signal, or potentially an analytical artifact of high CO₂ concentrations. We report results from a laboratory experiment using the RAD7 radon detector, known ²²²Rn (radon) and ²²⁰Rn (thoron), and a controllable percentage of CO₂ in the carrier gas. Our results show that for every percentage of CO₂, the ²²⁰Rn reading should be multiplied by 1.019, the ²²²Rn radon should be multiplied by 1.003 and the ²²⁰Rn/²²²Rn ratio should be multiplied by 1.016 to correct for the presence of the CO₂.     

Large seasonal changes in the recharge of seawater in a subterranean estuary revealed by a radon tracer

Activities of radon (²²²Rn) in groundwater were continuously monitored in a saline aquifer from September 2010 to July 2011. The activities of ²²²Rn ranged from 200 to 4300 Bq m^?3, with a large seasonal variation. Because the activity of ²²²Rn in seawater is low, ²²²Rn in saline groundwater must be produced in the aquifer from radium (²²⁶Ra) in rocks and sediments. The ²²²Rn activities were higher in the warm‐dry seasons (September–November 2010 and April–May 2011) when the saline aquifer was stable. In contrast, the lowest ²²²Rn activities were observed in the cold‐dry season (December 2010 and January–March 2011), because of the effective exchange between groundwater and seawater. In addition, sudden decreases of ²²²Rn activities coincided with episodic drops in groundwater temperatures. These results reveal that lower seawater temperature in winter may result in density‐driven seawater intrusion. During the wet season (June–July 2011), ²²²Rn activities were more clearly affected by semi‐monthly and diurnal tidal pumping, showing higher ²²²Rn activities during low and spring tides. Such a tidal effect was not clearly observed during the warm‐dry and cold‐dry seasons. This result implies that the residence time of SGD in coastal zones is significantly affected by seasonal changes in driving forces such as tidal pumping and seawater intrusion. Copyright © 2016 John Wiley & Sons, Ltd.     

A multi‐tracer approach to quantifying groundwater inflows to an upland river; assessing the influence of variable groundwater chemistry

Understanding the behaviour and variability of environmental tracers is important for their use in estimating groundwater discharge to rivers. This study utilizes a multi‐tracer approach to quantify groundwater discharge into a 27 km upland reach of the Gellibrand River in southwest Victoria, Australia. Ten sampling campaigns were conducted between March 2011 and June 2012, and the distribution of ²²²Rn activities, Cl and ³H concentrations imply the river receives substantial groundwater inflows. Mass balances based on ²²²Rn, Cl and ³H yield estimates of groundwater inflows that agree to within ± 12%, with cumulative inflows in individual campaigns ranging from 24 346 to 88 467 m³/day along the studied river section. Groundwater discharge accounts for between 10 and 50% of river flow dependent on the time of year, with a high proportion (>40 %) of groundwater sustaining summer flows. Groundwater inflow is largely governed by regional groundwater flowpaths; between 50 and 90% of total groundwater inflows occur along a narrow 5–10 km section where the river intersects the Eastern View Formation, a major regional aquifer. Groundwater ²²²Rn activities over the 16 month period were spatially heterogeneous across the catchment, ranging between 2000 Bq/m³ and 16 175 Bq/m³. Although groundwater ²²²Rn activities display temporal variation, spatial variation in groundwater ²²²Rn is a key control on ²²²Rn mass balances in river catchments where groundwater and river ²²²Rn activities are within an order of magnitude of each other. Calculated groundwater discharges vary from 8.4 to 15 m³/m/day when groundwater ²²²Rn activities are varied by ± 1 σ. Copyright © 2013 John Wiley & Sons, Ltd.     

The calculation of the statistical counting error for 222Rn scintillation counting

The calculation of the statistical counting error for alpha-scintillation counting of²²²Rn is complicated by the fact that two of the short-lived daughter products of²²²Rn are alpha emitters. All observed daughter-product counts attributable to parent decays that have already been detected must be excluded in the calculation of this error. An equation is derived which takes this into consideration.     

Tracer Method to Determine Residence Time in a Permeable Reactive Barrier

A method is presented to evaluate ground water residence time in a zero‐valent iron (ZVI) permeable reactive barrier (PRB) using radon‐222 (²²²Rn) as a radioactive tracer. Residence time is a useful indicator of PRB hydraulic performance, with application to estimating the volumetric rate of ground water flow through a PRB, identifying flow heterogeneity, and characterizing flow conditions over time as a PRB matures. The tracer method relies on monitoring the decay of naturally occurring aqueous ²²²Rn as ground water flows through a PRB. Application of the method at a PRB site near Monticello, Utah, shows that after 8 years of operation, residence times in the ZVI range from 80 to 486 h and correlate well with chemical parameters (pH, Ca, SO₄, and Fe) that indicate the relative residence time. Residence times in this case study are determined directly from the first‐order decay equation because we show no significant emanation of ²²²Rn within the PRB and no measurable loss of ²²²Rn other than by radioactive decay.     

Combining isotopic tracers (222Rn and δ13C) for improved modelling of groundwater discharge to small rivers

In regions where aquifers sustain rivers, the location and quantification of groundwater discharge to surface water are important to prevent pollution hazards, to quantify and predict low flows and to manage water supplies. ²²²Rn is commonly used to determine groundwater discharge to rivers. However, using this isotopic tracer is challenging because of the high diffusion capacity of ²²²Rn in open water. This study illustrates how a combination of isotopic tracers can contribute to an enhanced understanding of groundwater discharge patterns in small rivers. The aim of this paper is to combine ²²²Rn and δ¹³C_DIC to better constrain the physical parameters related to the degassing process of these tracers in rivers. The Hallue River (northern France) was targeted for this study because it is sustained almost exclusively by a fractured chalk aquifer. The isotopes ²²²Rn, δ¹³C_DIC, δ²H and δ¹⁸O were analysed along with other natural geochemical tracers. A mass balance model was used to simulate ²²²Rn and δ¹³C_DIC. The results of δ²H and δ¹⁸O analyses prove that evaporation did not occur in the river. The calibration of a numerical model to reproduce ²²²Rn and δ¹³C_DIC provides a best‐fit diffusive layer thickness of 3.21 × 10^?5 m. This approach is particularly useful for small rivers flowing over carbonate aquifers with high groundwater DIC where the evolution of river DIC reflects the competing processes of groundwater inflow and CO₂ degassing. This approach provides a means to evaluate groundwater discharge in small ungauged rivers. Copyright © 2014 John Wiley & Sons, Ltd.     

Natural Radioactivity at the Sin Quyen Iron-Oxide-Copper-Gold Deposit in North Vietnam

The field radiometric and laboratory measurements were performed at the Sin Quyen copper deposit in North Vietnam. The field gamma-ray spectrometry indicated the concentration of uranium ranging from 5.5 to 87 ppm, thorium from 5.6 to 33.2 ppm, and potassium from 0.3 to 4.7%. The measured dose rates ranged from 115 to 582 nGy/h, the highest doses being at the copper ore. Concentrations in the solid samples were in the range of 20–1700 Bq/kg for uranium, 20–92.7 Bq/kg for thorium, and 7–1345 Bq/kg for potassium. The calculated doses were from 22 to 896 nGy/h; both measured and calculated dose rates are mostly related to uranium. Concentrations of radium in water samples were below 0.17 Bq/L. Uranium in water samples was significantly higher than the hydrogeological background; the maximum of 13 Bq/L was at the waste zone pool, but neither radium nor uranium were present in tap water. Radon concentration in the dwelling air was from 42 to 278 Bq/m³ for ²²²Rn and from 8 to 193 Bq/m³ for ²²⁰Rn. The estimated committed dose rates were principally related to ²²²Rn concentration and ranged from 1.1 to 8.1 mSv/y.     

Radon emanation as an indicator of current activity of the moon

An interpretation of previously reported measurements of the Apollo 15/16 alpha-particle spectrometer on the distribution of ²²²Rn and ²¹⁰Po across the lunar surface suggests that continuation of these measurements is a method of monitoring current activity on the moon. Since the two isotopes are relatively short-lived with effective half-lives of 3 days and 21 years, respectively, the activity detected has had to have been released during this current epoch. Changes in the rate of lunar emanation can be measured on three different time scales: (1) of a few days or less by detecting ²²²Rn at discrete sites such as the crater Aristarchus; (2) of a month by measuring ²²²Rn activity at the sunrise terminator; (3) of a few years by measuring ²¹⁰Po activity at various locations. These observations could be carried out very effectively from a lunar polar orbiting satellite.