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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Precise Q value determinations for forbidden and low energy $\beta $-decays using Penning trap mass spectrometry

Nuclear β-decay provides a laboratory for investigating weak decays occurring inside the nuclear medium. This provides information on the resulting subtle nuclear and atomic effects, and on the underlying interaction and the properties of the particles that are involved, particularly of the neutrino. The Q value of the decay corresponds to the energy equivalent of the mass difference between parent and daughter atoms, and can be precisely and accurately measured using Penning trap mass spectrometry. In this paper we discuss Penning trap Q value measurements for forbidden β-decays of long-lived primordial nuclides, and for a subset of β-unstable nuclides that could potentially undergo a very low energy decay to an excited state in the daughter nucleus. Here we discuss applications of these measurements to tests of systematics in detectors that perform precise β-spectrum measurements, as inputs for theoretical shape factor, electron branching ratio and half-life calculations, and to identify nuclides that could serve as new candidates in direct neutrino mass determination experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Evidence for an isomeric {pi}½{sup +}[411] state in {sup 183}Ta

We report on the identification of a new isomeric state in Ta populated via the ground-state -decay of Hf. The experiment was performed at the KISS setup at RIKEN, where neutron-rich hafnium isotopes were produced via multi-nucleon transfer (MNT) reactions, followed by laser ionization of hafnium atoms, mass separation, and detection using an electron-gamma coincidence system. Isomeric spectroscopy was carried out by gating on different electron-gamma time correlations. A 459.1 keV -ray transition was identified in delayed spectra, and a half-life of μ was extracted through time-distribution fitting. The 459.1 keV state in Ta is known from previous work and has been assigned a Nilsson orbital configuration of , while a proposed new isomeric state above it is interpreted as a configuration that decays to via a low-energy, unobserved E2 transition. This is consistent with the systematic trends in neighbouring odd-A nuclei and transition rate calculations. Similar content being viewed by others

Doshi, S.↗
DOE OSTI2020

Detection prospects for the second-order weak decays of 124 Xe in multi-tonne xenon time projection chambers

We investigate the detection prospects for two-neutrino and neutrinoless second-order weak decays of 124 Xe – double-electron capture (0/2νECEC), electron capture with positron emission (0/2νECβ + ) and double-positron emission (0/2νβ + β + ) – in multi-tonne xenon time projection chambers. We simulate the decays in a liquid xenon medium and develop a reconstruction algorithm which uses the multi-particle coincidence in these decays to separate signal from background. This is used to compute the expected detection efficiencies as a function of position resolution and energy threshold for planned experiments. In addition, we consider an exhaustive list of possible background sources and find that they are either negligible in rate or can be greatly reduced using our topological reconstruction criteria. In particular, we draw two conclusions: First, with a theoretical half-life of $T^{2νECβ^+}_{1/2}$= (1.7 ± 0.6) ∙10 23 year, the 2νECβ + decay of 124 Xe will likely be detected in upcoming Dark Matter experiments (e.g. XENONnT or LZ), and their major background will be γ-rays from detector construction materials. Second, searches for the 0νECβ + decay mode will likely be background-free, and new parameter space may be within reach. To this end we investigate two different scenarios of existing experimental constraints on the effective neutrino mass. The necessary 500 kg-year exposure of 124 Xe could be achieved by the baseline design of the DARWIN observatory, or by extracting and using the 124 Xe from the tailings of the nEXO experiment. We demonstrate how a combination of 124 Xe results with those from 0νβ - β - searches in 136 Xe could help to identify the neutrinoless decay mechanism.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Search for rare alpha and double beta decays of Yb isotopes to excited levels of daughter nuclei

A search for alpha and double beta decays of ytterbium isotopes was performed with an ultra low-background high purity germanium detector at Gran Sasso Underground Laboratory (Italy). A 194.7 g Yb 2 (C 2 O 4 ) 3 powder sample was measured for 11.3 days with a total Yb exposure of 1.25 kg×day. Half-life limits for α-decay modes of 168 Yb, 170 Yb, 171 Yb, 172 Yb, 173 Yb, 174 Yb and 176 Yb into the first excited states have been obtained between 6 × 10 14 years and 2 × 10 16 years. These are the first experimental constraints of these decay modes. Double electron capture of 168 Yb and double beta decay of 176 Yb into the first excited 2 + and 0 + states could be excluded with limits between 1 × 10 14 years to 8 × 10 16 years. This improves the experimental information on some of the decay modes compared to previous constraints.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Performance of novel VUV-sensitive Silicon Photo-Multipliers for nEXO

Liquid xenon time projection chambers are promising detectors to search for neutrinoless double beta decay (0νββ), due to their response uniformity, monolithic sensitive volume, scalability to large target masses, and suitability for extremely low background operations. The nEXO collaboration has designed a tonne-scale time projection chamber that aims to search for 0νββ of 136 Xe with projected half-life sensitivity of 1.35 x 10 28 yr. To reach this sensitivity, the design goal for nEXO is ≤1% energy resolution at the decay Q-value (2458.07 ± 0.31 keV). Reaching this resolution requires the efficient collection of both the ionization and scintillation produced in the detector. The nEXO design employs Silicon Photo-Multipliers (SiPMs) to detect the vacuum ultra-violet, 175 nm scintillation light of liquid xenon. This paper reports on the characterization of the newest vacuum ultra-violet sensitive Fondazione Bruno Kessler VUVHD3 SiPMs specifically designed for nEXO, as well as new measurements on new test samples of previously characterised Hamamatsu VUV4 Multi Pixel Photon Counters (MPPCs). Various SiPM and MPPC parameters, such as dark noise, gain, direct crosstalk, correlated avalanches and photon detection efficiency were measured as a function of the applied over voltage and wavelength at liquid xenon temperature (163 K). The results from this study are used to provide updated estimates of the achievable energy resolution at the decay Q-value for the nEXO design.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Searching for beyond the Standard Model physics using the improved description of 100 Mo $2\nu \beta \beta$ decay spectral shape with CUPID-Mo

The current experiments searching for neutrinoless double-β ($0\nu \beta \beta$) decay also collect large statistics of Standard Model allowed two-neutrino double-β ($2\nu \beta \beta$ ) decay events. These can be used to search for Beyond Standard Model (BSM) physics via $2\nu \beta \beta$ decay spectral distortions. 100 Mo has a natural advantage due to its relatively short half-life, allowing higher $2\nu \beta \beta$ decay statistics at equal exposures compared to the other isotopes. We demonstrate the potential of the dual read-out bolometric technique exploiting a 100 Mo exposure of 1.47 kg years, acquired in the CUPID-Mo experiment at the Modane underground laboratory (France). We set limits on $0\nu \beta \beta$ decays with the emission of one or more Majorons, on $2\nu \beta \beta$ decay with Lorentz violation, and $2\nu \beta \beta$ decay with a sterile neutrino emission. In this analysis, we investigate the systematic uncertainty induced by modeling the $2\nu \beta \beta$ decay spectral shape parameterized through an improved model, an effect never considered before. This work motivates searches for BSM processes in the upcoming CUPID experiment, which will collect the largest amount of $2\nu \beta \beta$ decay events among the next-generation experiments.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

CUPID, the Cuore upgrade with particle identification

CUPID, the CUORE Upgrade with Particle Identification, is a next-generation experiment to search for neutrinoless double beta decay (0 νββ ) and other rare events using enriched Li 2 100 MoO 4 scintillating bolometers. It will be hosted by the CUORE cryostat located at the Laboratori Nazionali del Gran Sasso in Italy. The main physics goal of CUPID is to search for 0 νββ of 100 Mo with a discovery sensitivity covering the full neutrino mass regime in the inverted ordering scenario, as well as the portion of the normal ordering regime with lightest neutrino mass larger than 10 meV. With a conservative background index of 10 −4 cts/(keV·kg·yr), 240 kg isotope mass, 5 keV FWHM energy resolution at 3 MeV and 10 live-years of data taking, CUPID will have a 90% C.L. half-life exclusion sensitivity of 1.8 · 10 27 yr, corresponding to an effective Majorana neutrino mass ( m ββ ) sensitivity of 9–15 meV, and a 3σ discovery sensitivity of 1 · 10 27 yr, corresponding to an m ββ range of 12–21 meV.

Alfonso, K. [Virginia Polytechnic Institute and St↗
DOE OSTI2025

The XLZD Design Book: towards the next-generation liquid xenon observatory for dark matter and neutrino physics

This report describes the experimental strategy and technologies for XLZD, the next-generation xenon observatory sensitive to dark matter and neutrino physics. In the baseline design, the detector will have an active liquid xenon target of 60 tonnes, which could be increased to 80 tonnes if the market conditions for xenon are favorable. It is based on the mature liquid xenon time projection chamber technology used in current-generation experiments, LZ and XENONnT. The report discusses the baseline design and opportunities for further optimization of the individual detector components. The experiment envisaged here has the capability to explore parameter space for Weakly Interacting Massive Particle (WIMP) dark matter down to the neutrino fog, with a 3σ evidence potential for WIMP-nucleon cross sections as low as 3 x 10 –49 cm 2 (at 40 GeV/c 2 WIMP mass). The observatory will also have leading sensitivity to a wide range of alternative dark matter models. It is projected to have a 3σ observation potential of neutrinoless double beta decay of 136 Xe at a half-life of up to 5.7 x 10 27 years. Additionally, it is sensitive to astrophysical neutrinos from the sun and galactic supernovae.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Radioactive decay of $\mathrm {{}^{90}Sr}$ in cement: a non-equilibrium first-principles investigation

Cement is an inexpensive and relatively easily manageable material that is used as a last barrier for nuclear waste disposal. Under these conditions, the cement is in contact with low radiation doses, but there is a distinct possibility of being contaminated with radioactive products. Of particular concern is the medium lived half-life product 90 Sr (28.8 years) due to its ability to replace Ca. 90 Sr undergoes β-decay to 90 Y which, in turn, β-decays to stable 90 Zr. In this work, we discuss systematically the chain of non-equilibrium processes that result as a consequence of β-decay events in cement. We first use density functional-based methods to study the consequences of the sudden increase of the nuclear charge from Z to Z+1, a possible induced ionization and the perturbation of the surrounding electronic charge. Secondly, we use molecular dynamics simulations to study the recoil of the daughter nucleus. Finally, we discuss the damage caused by the ionization cascade produced during the propagation of the β-electron and the resulting chemical and structural perturbation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Status and results from the CUORE experiment

The Cryogenic Underground Observatory for Rare Events (CUORE) is a tonne-scale cryogenic experiment located at the Laboratori Nazionali del Gran Sasso that exploits bolometric technique to search for neutrinoless double beta decay [0$vββ$] of 130 Te. The detector consists of a segmented array of 988 natural TeO 2 cubic crystals arranged in a cylindrical compact structure of 19 towers. The detector construction was completed in August 2016 and data taking started in Spring 2017. Here, we present a brief description of the bolometric technique for rare events search and the CUORE detector, then we concentrate on the data analysis results. In this respect, we focus on the procedure for data processing and on the first 0$vββ$ results we obtained from a total TeO 2 exposure of 86.3 kg · yr. Next, we illustrate the main background sources and the CUORE background model, from which we obtain the most precise measurement of 130 Te 2$vββ$ half-life to date. Finally, we discuss the improvements achieved with 2018 and 2019 detector optimization campaigns and the current perspectives of our experiment.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Radionuclide-specific Parameters Dataset

The radionuclide-specific parameters dataset is searchable for radiological information for multiple isotopes simultaneously. After selecting radionuclides of interest and the desired parameters, the RAIS will generate a table containing the values, chosen according to an established hierarchy. Results can be downloaded in Excel format. 50 parameters are available, including atomic number, soil to animal transfer coefficients, plant uptake coefficients, half-life, specific activity, and water solubility. Seven primary sources are used to populate the dataset of radiological-specific parameters. These values should be used in cancer risk assessments for the calculation of preliminary remediation goals (PRGs), hazard characterization, and transport modeling. Users can select up to 1000 radionuclides per query. The dataset supports environmental risk assessments, regulatory decision-making, and environmental planning with tools for benchmarking against risk-based standards. This structured approach ensures a robust evaluation of environmental risks tailored to regulatory needs.

Manning, Karessa [Oak Ridge National Laboratory (O↗
DOE OSTI2021

Lasofoxifene as a potential treatment for therapy-resistant ER-positive metastatic breast cancer

Background: Endocrine therapy remains the mainstay of treatment for estrogen receptor-positive (ER+) breast cancer. Constitutively active mutations in the ligand binding domain of ERα render tumors resistant to endocrine agents. Breast cancers with the two most common ERα mutations, Y537S and D538G, have low sensitivity to fulvestrant inhibition, a typical second-line endocrine therapy. Lasofoxifene is a selective estrogen receptor modulator with benefits on bone health and breast cancer prevention potential. This study investigated the anti-tumor activity of lasofoxifene in breast cancer xenografts expressing Y537S and D538G ERα mutants. The combination of lasofoxifene with palbociclib, a CDK4/6 inhibitor, was also evaluated. Methods: Luciferase-GFP tagged MCF7 cells bearing wild-type, Y537S, or D538G ERα were injected into the mammary ducts of NSG mice (MIND model), which were subsequently treated with lasofoxifene or fulvestrant as single agents or in combination with palbociclib. Tumor growth and metastasis were monitored with in vivo and ex vivo luminescence imaging, terminal tumor weight measurements, and histological analysis. Results: As a monotherapy, lasofoxifene was more effective than fulvestrant at inhibiting primary tumor growth and reducing metastases. Adding palbociclib improved the effectiveness of both lasofoxifene and fulvestrant for tumor suppression and metastasis prevention at four distal sites (lung, liver, bone, and brain), with the combination of lasofoxifene/palbociclib being generally more potent than that of fulvestrant/palbociclib. X-ray crystallography of the ERα ligand binding domain (LBD) shows that lasofoxifene stabilizes an antagonist conformation of both wild-type and Y537S LBD. The ability of lasofoxifene to promote an antagonist conformation of Y537S, combined with its long half-life and bioavailability, likely contributes to the observed potent inhibition of primary tumor growth and metastasis of MCF7 Y537S cells. Conclusions: We report for the first time the anti-tumor activity of lasofoxifene in mouse models of endocrine therapy-resistant breast cancer. The results demonstrate the potential of using lasofoxifene as an effective therapy for women with advanced or metastatic ER+ breast cancers expressing the most common constitutively active ERα mutations.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2025

Establishing Pb-203 production from electrodeposited Tl targets at Brookhaven National Laboratory

Background: Promising developments in Pb-212 radiopharmaceutical therapies have increased demand for Pb-203 diagnostic agents. Building on previous work from various isotope production facilities, this study optimized Pb-203 production from electrodeposited Tl targets at Brookhaven National Laboratory (BNL). The additional supply of Pb-203 may help meet growing preclinical and clinical demands. Results: Two Tl targets were irradiated at the Brookhaven Linac Isotope Producer facility with 30 ± 1 MeV protons, measured using previously published cross section data. Distribution coefficients for Pb Resin in acetate media were investigated for both Na + and K + cations, where potassium acetate was ~ 4 times more effective at stripping Pb from the Pb Resin. The Tl electrodeposition was optimized to deposit 350 mg of Tl (~ 60 mg/cm 2 ) on Au backing in under 6 h. The proposed separation process was completed in < 1.5 h and achieved > 98% and 92 ± 3% recovery of Tl and Pb, respectively, with an overall Tl-Pb separation factor of 6 × 10 5 . The experimentally measured half-life of Pb-203 was 52.4 ± 0.7 h, agreeing with 51.93 ± 0.02 h reported by the National Nuclear Data Center. The radioisotopic purity of the Pb fraction at 24 h post end of bombardment (EOB) from a 24 h irradiation was 66% Pb-203, 28% Pb-201, and 6% Pb-200. Following chemical separation, the Pb-203 produced in this work (21 MBq Pb-203 EOB) achieved apparent molar activities of 10 ± 5 and 0.9 ± 0.5 GBq/µmol for [ 203 Pb]Pb-DOTAM and [ 203 Pb]Pb-DO3A, respectively, decay corrected to EOB. Data derived from this work suggests BNL can produce > 10’s GBq Pb-203 with > 99% radiochemical and radioisotopic purity from Tl-205 for worldwide distribution. Conclusions: The production and separation of Pb-203 from natural Tl target material was successfully demonstrated at BNL. Existing methods were adapted and optimized for the facilities at BNL. Results from this work will guide future large-scale Pb-203 production opportunities at BNL for clinical applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Evaluation of residue management practices on barley residue decomposition

Optimizing barley (hordeum vulgare L.) production in Idaho and other parts of the Pacific Northwest (PNW) should focus on farm resource management. The effect of post-harvest residue management on barley residue decomposition has not been adequately studied. Thus, the objective of this study was to determine the effect of residue placement (surface vs. incorporated), residue size (chopped vs. ground-sieved) and soil type (sand and sandy loam) on barley residue decomposition. A 50-day(d) laboratory incubation experiment was conducted at a temperature of 25°C at the Aberdeen Research and Extension Center, Aberdeen, Idaho, USA. Following the study, a Markov-Chain Monte Carlo (MCMC) modeling approach was applied to investigate the first-order decay kinetics of barley residue. An accelerated initial flush of residue carbon(C)-mineralization was measured for the sieved (Day 1) compared to chopped (Day 3 to 5) residues for both surface incorporated applications. The highest evolution of carbon dioxide (CO 2 )-C of 8.3 g kg -1 dry residue was observed on Day 1 from the incorporated-sieved application for both soils. The highest and lowest amount of cumulative CO 2 -C released and percentage residue decomposed over 50-d was observed for surface-chopped (107 g kg -1 dry residue and 27%, respectively) and incorporated-sieved (69 g kg -1 dry residue and 18%, respectively) residues, respectively. There were no significant differences in C-mineralization from barley residue based on soil type or its interactions with residue placement and size (p >0.05). The largest decay constant k of 0.0083 d -1 was calculated for surface-chopped residue where the predicted half-life was 80 d, which did not differ from surface sieved or incorporated chopped. In contrast, incorporated-sieved treatments only resulted in a k of 0.0054 d -1 and would need an additional 48 d to decompose 50% of the residue. Future residue decomposition studies under field conditions are warranted to verify the residue C-mineralization and its impact on residue management.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Status and prospects of discovery of 0νββ decay with the CUORE detector

In this contribution we present the achievements of the CUORE experiment so far. It is the first tonne-scale bolometric detector and it is in stable data taking since 2018. We reached to collect about 1800 kg×yr of exposure of which more than 1 ton×year have been analysed. The CUORE detector is meant to search for the neutrinoless double β decay (0νββ) of the 130 Te isotope. This is a beyond Standard Model process which could establish the nature of the neutrino to be Dirac or a Majorana particle. It is an alternative mode of the two-neutrinos double β decay, a rare decay which have been precisely measured by CUORE in the 130 Te. We found no evidence of the 0νββ and we set a Bayesian lower limit of 2.2 ×10 25 yr on its half-life. The expertise achieved by CUORE set a milestone for any future bolometric detector, including CUPID, which is the planned next generation experiment searching for 0νββ with scintillating bolometers.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Evaluated Nuclear Structure Data File (ENSDF)

Contains recommended nuclear structure and decay data for all the known nuclides, which are obtained following a critical review of all available experimental data, supplemented with systematic trend studies and theoretical models. ENSDF data include (i) nuclear level properties, such as observation source, energy, half-life, decay modes, spin and parity; (ii) gamma ray energies, intensities, multipolarities, mixing ratios and conversion coefficients; (iii) nuclear radiation energy and intensity as well as radiation-specific data for different radiation types, such as such as gammas, alphas, betas and neutrons. Data for about 220 nuclides are fully evaluated each year; additionally, many datasets are partially updated each year. Nearly all the evaluation work is supported by the US Nuclear Data Program. The National Nuclear Data Center at Brookhaven National Laboratory is responsible for coordinating the evaluation effort as well as its web and journal dissemination.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Experimental Unevaluated Nuclear Data List (XUNDL)

Contains nuclear structure and decay data from published articles. Data include nuclear level properties, such as energy, half-life, decay modes, spin and parity, as well as energy and intensity for radiation types such as gammas, alphas, betas and neutrons. For articles published in Physical Review C and the European Physical Journal, compilation takes place during the article submission process. Data from approximately 250 articles are added per year. All the compilation effort is supported by the US Nuclear Data Program and coordinated by the National Nuclear Data Center at Brookhaven National Laboratory, which is also responsible for its web dissemination.

Basic Nuclear Research, nuclear structure and deca↗
DOE OSTI2020

Collaborative Research: Natural Organic Matter and Microbial Controls on Mobilization/Immobilization of I and Pu in Soils and Waters Affected by Radionuclide Releases in USA and Japan

In this project, the relationship between natural organic matter (NOM) and two radioactive elements that are relevant to nuclear waste disposal were studied: Plutonium (Pu) and Iodine. The human and environmental risks associated with Pu stem mainly from the very long half-lives of several of its isotopes ( 238 Pu, 88 yr; 239 Pu, 24,100 yr; 240 Pu, 6560 yr) and its radiotoxicity. Understanding Pu biogeochemical behavior in both near-field (>10-11M) and far-field scales (<10-11M) is imperative to the development of approaches for reprocessing Pu, remediation of Pu contamination and accurate assessment of risks posed by disposal practices for Pu-bearing wastes. The environmental mobility of Pu can be affected by redox potential, pH, adsorption, precipitation, complexation, colloid formation, and microbial activity, of which the first characteristic has the most profound influence. Numerous studies have shown high affinity of Pu towards NOM, as well as to mineral phases. NOM is ubiquitous in the environment, e.g., both fulvic and humic acids are able to reduce Pu(V,VI) to Pu(IV) and the redox potential of NOM is positively related to the abundance of phenolic/acidic OH groups. NOM can either facilitate or limit actinide migration, depending on specific biogeochemical conditions including pH, mineral and organic matter characteristics, etc. The other radionuclide of interest is radioiodine ( 129 I). 129I is a major by-product of nuclear fission and of serious concern to the Department of Energy (DOE) as it is among the top risk drivers at existing and potential radiowaste-contaminated sites. The risk of 129 I stems largely from its high bioconcentration factor (90% of the body’s iodine is accumulated in the thyroid), a high inventory at source terms, a very long-half life (16M years), and rapid mobility in the subsurface environment. As a consequence, 129 I has the lowest drinking water standard (1 pCi/L) among all radionuclides in the Federal Register. With a novel and sensitive gas chromatography-mass spectrometry (GC-MS) method developed in our lab, it is possible to quickly and simultaneously determine the distribution of 129 I and stable 127 I forms in environments, as low as 2 pCi/L for 129 I. This method was subsequently validated using accelerator mass spectroscopy, AMS. IO 3 - and organo-I were determined as major species in the groundwater of SRS and the Hanford Site, contrary to thermodynamic predictions that I- should be the dominant species at these sites. Mobility of 129 I was also demonstrated to depend greatly on the I species and its concentration, sediment pH, and redox state, with times to achieve equilibrium taking up to 12 weeks. Along the groundwater pathway in the F-Area of SRS, 129 I- supplied from the seepage basins was transformed to 129 IO 3 - and organo- 129 I with increasing iodine sediment sorption, causing the lower total 127 I and 129 I concentrations along the gradient transect of the waste plume. By contrast, groundwater 129 I concentrations in the wetlands (as high as 1617.3 pCi/L) were greatly elevated with respect to the source term (159.3 pCi/L). While the NOM promoted the uptake of 129 I to the wetland sediment, it also promoted the formation of soluble organic fraction. A small fraction of NOM that is bound to iodine can behave as a mobile organo-I source. Iodide was enzymatically incorporated into NOM, whereas both iodide and iodate were abiotically bound to NOM, under certain conditions. Iodate removal from the mobile aqueous phase can also occur through incorporation into carbonate (e.g., at the Hanford Site, USA). Thus immobilization and re-mobilization of iodine species were influenced by pH, Eh and the presence of NOM and metal oxides, which adds to the complexity of site remediation action. A ground-breaking result was to elucidate the products (i.e. organo-iodine moieties formed via enzymatic and non-enzymatic processes) at the molecular level by nuclear magnetic resonance (NMR) and electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICRMS). We found that iodine-NOM interactions may be influenced by NOM hydrophobic aliphatic moieties. From the perspective of ESI-FTICRMS, organo-iodine formulas were ascribed to the groups of unsaturated hydrocarbons, lignins and proteins. Iodate is likely abiotically reduced to reactive iodine species by lignin- and tannin-like compounds or carboxylic-rich alicyclic molecules (CRAM). We also investigated microbial mechanisms in iodine incorporation into NOM. We established that soil bacteria isolated from F-Area of SRS did not accumulate significant amounts of I- (0.2-2%). Intracellular uptake of I- decreases with increasing pH when pH ranged from 4 to 6. In contrast, 44 out of 84 strains isolated from the F-Area of SRS can transform I- to IO 3 - and organo-iodine. In some cases, oxidation was facilitated in the presence of H 2 O 2 . Microbes can also excrete organic acids that enhance I- oxidation by lowering the ambient pH and reacting with H 2 O 2 to form peroxy carboxylic acids. At lower pH values (≤5), H 2 O 2 hydrolysis was the driving force for iodide-oxidation; whereas, at pH ≥ 6, spontaneous decomposition of peroxy carboxylic acids, originating from H 2 O 2 and organic acids were the primary cause of iodide oxidation. Lastly, it was determined that microbial processes involved in Mn (II) are capable of directly oxidizing I- via enzymatic catalysis (i.e., multicopper oxidases), or indirectly through the formation of reactive oxygen species (ROS) and/or biogenic manganese oxides. ROS-mediated oxidation of I- was found to predominate at pH >5, whereas the enzymatic and Mn oxide pathways were more active at pH < 5. Together, this project has resulted in 9 publications in high-impact journals, and the training of 1 Ph.D and 4 undergraduate students.

54 ENVIRONMENTAL SCIENCES↗