Excited states of barium 136 and barium 134
Barium 134 and barium 136 excitation by proton irradiation
Fessler, T. E.↗
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Nuclear Data Sheets for A=136☆
Spectroscopic data for all nuclei with mass number A=136 have been evaluated and the corresponding level schemes from radioactive decay and reaction studies are presented. No excited states are known in {sup 136}In, {sup 136}Eu, or {sup 136}Gd and {sup 136}Tb remains unidentified. Discrepancies between experiments on isomeric decays in {sup 136}Sb and {sup 136}La suggest the need for futher experimental investigation. The decay of {sup 136}Eu has only been observed in a mixed source. The energy of the 17.5 s isomer in {sup 136}Cs was determined since the last evaluation, however, the branching ratio remains unknown. This work supersedes the earlier full evaluation of A=136 by A.A. Sonzogni (2002So05), and benefited tremendously from all previous evaluations of A=136.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Barium Chemosensors with Dry-Phase Fluorescence for Neutrinoless Double Beta Decay
The nature of the neutrino is one of the major open questions in experimental nuclear and particle physics. The most sensitive known method to establish the Majorana nature of the neutrino is detection of the ultra-rare process of neutrinoless double beta decay. However, identification of one or a handful of decay events within a large mass of candidate isotope, without obfuscation by backgrounds is a formidable experimental challenge. One hypothetical method for achieving ultra- low-background neutrinoless double beta decay sensitivity is the detection of single 136 Ba ions produced in the decay of 136 Xe (“barium tagging”). To implement such a method, a single-ion-sensitive barium detector must be developed and demonstrated in bulk liquid or dry gaseous xenon. This paper reports on the development of two families of dry-phase barium chemosensor molecules for use in high pressure xenon gas detectors, synthesized specifically for this purpose. One particularly promising candidate, an anthracene substituted aza-18-crown-6 ether, is shown to respond in the dry phase with almost no intrinsic background from the unchelated state, and to be amenable to barium sensing through fluorescence microscopy. This interdisciplinary advance, paired with earlier work demonstrating sensitivity to single barium ions in solution, opens a new path toward single ion detection in high pressure xenon gas.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
CORRELATED STRONTIUM AND BARIUM ISOTOPIC COMPOSITIONS OF ACID-CLEANED SINGLE MAINSTREAM SILICON CARBIDES FROM MURCHISON
We present strontium, barium, carbon, and silicon isotopic compositions of 61 acid-cleaned presolar SiC grains from Murchison. Comparison with previous data shows that acid washing is highly effective in removing both strontium and barium contamination. For the first time, by using correlated {sup 88}Sr/{sup 86}Sr and {sup 138}Ba/{sup 136}Ba ratios in mainstream SiC grains, we are able to resolve the effect of {sup 13}C concentration from that of {sup 13}C-pocket mass on s-process nucleosynthesis, which points toward the existence of large {sup 13}C pockets with low {sup 13}C concentrations in asymptotic giant branch stars. The presence of such large {sup 13}C pockets with a variety of relatively low {sup 13}C concentrations seems to require multiple mixing processes in parent asymptotic giant branch stars of mainstream SiC grains.
79 ASTRONOMY AND ASTROPHYSICS↗
Demonstration of Single-Barium-Ion Sensitivity for Neutrinoless Double-Beta Decay Using Single-Molecule Fluorescence Imaging
Here, a new method to tag the barium daughter in the double beta decay of $^{136}$Xe is reported. Using the technique of single molecule fluorescent imaging (SMFI), individual barium dication (Ba$^{++}$) resolution at a transparent scanning surface has been demonstrated. A single-step photo-bleach confirms the single ion interpretation. Individual ions are localized with super-resolution ($\sim$2~nm), and detected with a statistical significance of 12.9~$\sigma$ over backgrounds. This lays the foundation for a new and potentially background-free neutrinoless double beta decay technology, based on SMFI coupled to high pressure xenon gas time projection chambers.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Isotopic excesses of proton-rich nuclei related to space weathering observed in a gas-rich meteorite Kapoeta
The idea that solar system materials were irradiated by solar cosmic rays from the early Sun has long been suggested, but is still questionable. In this study, Sr, Ba, Ce, Nd, Sm, and Gd isotopic compositions of sequential acid leachates from the Kapoeta meteorite (howardite) were determined to find systematic and correlated variations in their isotopic abundances of proton-rich nuclei, leading to an understanding of the irradiation condition by cosmic rays. Significantly large excesses of proton-rich isotopes (p-isotopes), {sup 84}Sr, {sup 130}Ba, {sup 132}Ba, {sup 136}Ce, {sup 138}Ce, and {sup 144}Sm, were observed, particularly in the first chemical separate, which possibly leached out of the very shallow layer within a few μm from the surface of regolith grains in the sample. The results reveal the production of p-isotopes through the interaction of solar cosmic rays with the superficial region of the regolith grains before the formation of the Kapoeta meteorite parent body, suggesting strong activity in the early Sun.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Fluorescence imaging of individual ions and molecules in pressurized noble gases for barium tagging in 136Xe
Abstract The imaging of individual Ba 2+ ions in high pressure xenon gas is one possible way to attain background-free sensitivity to neutrinoless double beta decay and hence establish the Majorana nature of the neutrino. In this paper we demonstrate selective single Ba 2+ ion imaging inside a high-pressure xenon gas environment. Ba 2+ ions chelated with molecular chemosensors are resolved at the gas-solid interface using a diffraction-limited imaging system with scan area of 1 × 1 cm 2 located inside 10 bar of xenon gas. This form of microscopy represents key ingredient in the development of barium tagging for neutrinoless double beta decay searches in 136 Xe. This also provides a new tool for studying the photophysics of fluorescent molecules and chemosensors at the solid-gas interface to enable bottom-up design of catalysts and sensors.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Early Career Award: Single Molecule Fluorescence Imaging for a Background-Free Neutrinoless Double Beta Decay Search
This project aimed to develop a suite of novel technologies targeted at detecting individual barium ions produced in neutrinoless double beta decays of 136 Xe, as part of the NEXT program of gaseous xenon detectors. We realized novel molecules which could sense Ba 2+ ions in dry conditions; new microscopy techniques operable in dry noble gases, including the required operating conditions of xenon at 10 bar pressure; and new radiofrequency ion transport methods (developed both theoretically and experimentally) that can transport ions in dense xenon gas. Together, these developments represent a major advance toward a background-free neutrinoless double beta decay experiment based on single molecule fluorescence imaging of Ba 2+ daughter ions.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
New Technique for Barium Daughter Ion Identification in a Liquid Xe-136 Double Beta Decay Experiment
This work addresses long-standing issues of fundamental interest in elementary particle physics. The most important outcome of this work is a new limit on neutrinoless double beta decay. This is an extremely rare and long-sought-after type of radioactive decay. If discovered, it would require changes in the standard model of the elementary constituents of matter, and would prove that neutrinos and antineutrinos are the same, a revolutionary concept in particle physics. Neutrinos are major components of the matter in the universe that are so small and so weakly interacting with other matter that their masses have not yet been discovered. A discovery of neutrinoless double beta decay could help determine the neutrino masses. An important outcome of the work on this project was the Colorado State University role in operating the EXO-200 neutrinoless double beta decay experiment and in analysis of the data from this experiment. One type of double beta decay of the isotope 136 Xe, the two-neutrino variety, was discovered in this work. Although the other type of double beta decay, the neutrinoless variety, was not yet discovered in this work, a world’s best sensitivity of 1.9x10 25 year half-life was obtained. This result rules out a previous claim of a positive result in a different isotope. This work also establishes that the masses of the neutrinos are less than one millionth of that of electrons. A unique EXO-200 analysis, in which the CSU group had a leading role, has established for the first time ever in a liquid noble gas the fraction of daughter atoms from alpha and beta decay that are ionized. This result has important impact on other pending studies, including nucleon decay and barium tagging. Novel additional discoveries include multiphoton ionization of liquid xenon with UV pulsed lasers, which may find application in calibration of future noble liquid detectors, and studies of association and dissociation reactions of Ba + ions in gaseous xenon. Through this project, we are substantially closer to demonstrating “barium tagging”, i.e., detection of single daughter 136 Ba atoms from 136 Xe double beta decay. Milestones achieved include obtaining spectra of small numbers of Ba atoms and cryoprobe advances toward trapping single 136 Ba atoms in solid xenon and probe extraction for detection. One of the other benefits to society is the training of six Ph.D. students in a variety of state-of-the-art technologies, half under primary support of this grant and half with partial support, with four finishing their Ph.D. degrees and two well on their way.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Barium isotopic composition of mainstream silicon carbides from Murchison: Constraints for s-process nucleosynthesis in asymptotic giant branch stars
We present barium, carbon, and silicon isotopic compositions of 38 acid-cleaned presolar SiC grains from Murchison. Comparison with previous data shows that acid washing is highly effective in removing barium contamination. Strong depletions in δ({sup 138}Ba/{sup 136}Ba) values are found, down to –400‰, which can only be modeled with a flatter {sup 13}C profile within the {sup 13}C pocket than is normally used. The dependence of δ({sup 138}Ba/{sup 136}Ba) predictions on the distribution of {sup 13}C within the pocket in asymptotic giant branch (AGB) models allows us to probe the {sup 13}C profile within the {sup 13}C pocket and the pocket mass in AGB stars. In addition, we provide constraints on the {sup 22}Ne(α, n){sup 25}Mg rate in the stellar temperature regime relevant to AGB stars, based on δ({sup 134}Ba/{sup 136}Ba) values of mainstream grains. We found two nominally mainstream grains with strongly negative δ({sup 134}Ba/{sup 136}Ba) values that cannot be explained by any of the current AGB model calculations. Instead, such negative values are consistent with the intermediate neutron capture process (i process), which is activated by the very late thermal pulse during the post-AGB phase and characterized by a neutron density much higher than the s process. These two grains may have condensed around post-AGB stars. Finally, we report abundances of two p-process isotopes, {sup 130}Ba and {sup 132}Ba, in single SiC grains. These isotopes are destroyed in the s process in AGB stars. By comparing their abundances with respect to that of {sup 135}Ba, we conclude that there is no measurable decay of {sup 135}Cs (t {sub 1/2} = 2.3 Ma) to {sup 135}Ba in individual SiC grains, indicating condensation of barium, but not cesium into SiC grains before {sup 135}Cs decayed.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Decay of super 136 La and super 134 La.
Lanthanum isotopes beta decay, analyzing excitation of near spherical daughter nuclei of barium isotopes
Fessler, T. E.↗
Overcoming photobleaching in imaging of single barium atoms in a solid xenon matrix
Neutrinoless double beta decay is one of the most sensitive probes for new physics beyond the Standard Model of particle physics. One of the isotopes under investigation is 136 Xe, which would double beta decay into 136 Ba. Detecting the single 136 Ba daughter provides a sort of ultimate tool in the discrimination against backgrounds. Previous work demonstrated the ability to perform single atom imaging of Ba atoms in a single-vacancy site of a solid xenon matrix. In this paper, the effort to identify signal from individual barium atoms is extended to Ba atoms in a hexa-vacancy site in the matrix and is achieved despite increased photobleaching in this site. Abrupt fluorescence turn-off of a single Ba atom is also observed. Significant recovery of fluorescence signal lost through photobleaching is demonstrated upon annealing of Ba deposits in the Xe ice. Following annealing, it is observed that Ba atoms in the hexa-vacancy site exhibit antibleaching while Ba atoms in the tetra-vacancy site exhibit bleaching. This may be evidence for a matrix site transfer upon laser excitation. Our findings offer a path of continued research toward tagging of Ba daughters in all significant sites in solid xenon.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Demonstration of Selective Single-Barium Ion Detection with Dry Diazacrown Ether Naphthalimide Turn-on Chemosensors
Single-molecule fluorescence imaging (SMFI) of gas-phase ions has been proposed for “barium tagging,” a burgeoning area of research in particle physics to detect individual barium daughter ions. This has potential to significantly enhance the sensitivity of searches for neutrinoless double-beta decay (0νββ) that is obscured by background radiation events. The chemistry required to make such sensitive detection of Ba 2+ by SMFI in dry Xe gas at solid interfaces has implications for solid-phase detection methods but has not been demonstrated. Here, we synthesized simple, robust, and effective Ba 2+ -selective chemosensors capable of function within ultrapure high-pressure 136 Xe gas. Turn-on fluorescent naphthalimide-(di)azacrown ether chemosensors were Ba 2+ -selective and achieved SMFI in a polyacrylamide matrix. Here, fluorescence and NMR experiments supported a photoinduced electron transfer mechanism for turn-on sensing. Ba 2+ selectivity was achieved with computational calculations correctly predicting the fluorescence responses of sensors to barium, mercury, and potassium ions. With these molecules, dry-phase single-Ba 2+ ion imaging with turn-on fluorescence was realized using an oil-free microscopy technique for the first time—a significant advance toward single-Ba 2+ ion detection within large volumes of 136 Xe, plausibly enabling a background-independent technique to search for the hypothetical process of 0νββ.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Barium and neodymium isotopic anomalies in the Allende meteorite
The discovery of Ba and Nd isotopic anomalies in two inclusions from the Allende meteorite is reported. The inclusions are Ca-Al-rich objects typical of the type considered as high-temperature condensation products in the solar nebula and contain distinctive Mg and O isotopic anomalies of the FUN (mass Fractionation, Unknown Nuclear processes) type. Mass-spectrometry results are discussed which show that inclusion C1 has anomalies in Ba at masses 134 and 136, while inclusion EK1-4-1 exhibits large marked negative anomalies at 130, 132, 134, and 136, as well as a positive anomaly at 137. It is also found that inclusion EK1-4-1 shows marked negative anomalies in Nd at masses 142, 146, 148, and 150, in addition to a positive anomaly at 145. These isotopic shifts are attributed to addition of r-process nuclei rather than mass fractionation. It is suggested that an onion-shell supernova explosion followed by injection into the solar nebula is the most likely generic model that may explain the observations.
Mcculloch, M. T.↗
Method for estimating ionicities of oxides using O1s photoelectron spectra
The average valence, V{sub alO}, of the oxygen anions in the perovskite oxide BaTiO{sub 3}, was found using O1s photoelectron spectra to be −1.55. This experimental result is close to the theoretical value for BaTiO{sub 3} (−1.63) calculated by Cohen [Nature 358, 136 (1992)] using density functional theory. Using the same approach, we obtained values of V{sub alO} for several monoxides, and investigated the dependence of V{sub alO} and the ionicity on the second ionization energy, V(M{sup 2+}), of the metal cation. We found that the dependence of the ionicity on V(M{sup 2+}) in this work is close to that reported by Phillips [Rev. Mod. Phys. 42, 317 (1970)]. We therefore suggest that O1s photoelectron spectrum measurements should be accepted as a general experimental method for estimating the ionicity and average valence of oxygen anions.
36 MATERIALS SCIENCE↗