We present an update on the development of techniques to adapt Single Molecule Fluorescent Imaging for the tagging of individual barium ions in high pressure xenon gas detectors, with the goal of realizing a background-free neutrinoless double beta decay technology. Previously reported progress is reviewed, including the recent demonstration of single barium dication sensitivity using SMFI. We then describe two important advances: 1) the development of a new class of custom barium sensing fluorescent dyes, which exhibit a significantly stronger response to barium than commercial calcium sensing compounds in aqueous solution; 2) the first demonstration of a dry-phase chemosensor for barium ions. This proceeding documents work presented at the 9th Symposium on Large TPCs for Rare Event Detection in Paris, France.
The search for neutrinoless double beta decay probes the fundamental properties of neutrinos, including whether or not the neutrino and antineutrino are distinct. Double beta detectors are large and expensive, so background reduction is essential for extracting the highest sensitivity. The identification, or 'tagging', of the $^{136}$Ba daughter atom from double beta decay of $^{136}$Xe provides a technique for eliminating backgrounds in the nEXO neutrinoless double beta decay experiment. The tagging scheme studied in this work utilizes a cryogenic probe to trap the barium atom in solid xenon,…
The clustering and drift properties of barium ions in xenon gas are explored theoretically, using density functional theory and computational ion mobility theory, with the goal of better understanding barium ion transport for neutrinoless double beta decay. We derive the equilibrium conformations, energies and entropies of molecular ions in the Ba$^{+}$-Xe and Ba$^{++}$-Xe systems, which yield a predictive model of cluster formation in high pressure gas. We calculate ion-neutral interaction potential curves for these species and use them to predict effective molecular ion mobilities. Our calcu…
The search for neutrinoless double beta decay requires increasingly advanced methods of background reduction. A bold approach to solving this problem, in experiments using Xe-136, is to extract and identify the daughter Ba-136 ion produced by double beta decay. Tagging events in this manner allows for a virtually background-free verification of double beta decay signals. Various approaches are being pursued by the nEXO collaboration to achieve Ba-tagging. A Multi-Reflection Time-of-Flight Mass Spectrometer (MR TOF) has been designed and optimized as one of the ion-identification methods, where…
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…
In the search for neutrinoless double beta decay, understanding and reducing backgrounds is crucial for success. An advance that could drive backgrounds to negligible levels would be the ability to efficiently detect the barium daughter in $^{136}$Xe to $^{136}$Ba double beta decay, since no conventional radioactive process can produce barium ions or atoms in xenon at significant rates. In xenon gas, the barium daughter most likely survives as a dication. An approach under development by the NEXT collaboration involves transporting this ion from the active medium onto a coated transparent plan…
Progress on a method of barium tagging for the nEXO double beta decay experiment is reported. Absorption and emission spectra for deposits of barium atoms and ions in solid xenon matrices are presented. Excitation spectra for prominent emission lines, temperature dependence and bleaching of the fluorescence reveal the existence of different matrix sites. A regular series of sharp lines observed in Ba$^+$ deposits is identified with some type of barium hydride molecule. Lower limits for the fluorescence quantum efficiency of the principal Ba emission transition are reported. Under current condi…
Single molecule fluorescence detection of barium is investigated for enhancing the sensitivity and robustness of a neutrinoless double beta decay ($0νββ$) search in $^{136}$Xe, the discovery of which would alter our understanding of the nature of neutrinos and the early history of the Universe. A key developmental step is the synthesis of barium-selective chemosensors capable of incorporation into ongoing experiments in high-pressure $^{136}$Xe gas. Here we report turn-on fluorescent naphthalimide chemosensors containing monoaza- and diaza-crown ethers as agents for single Ba$^{2+}$ detection.…
Background rejection is key to success for future neutrinoless double beta decay experiments. To achieve sensitivity to effective Majorana lifetimes of $\sim10^{28}$ years, backgrounds must be controlled to better than 0.1 count per ton per year, beyond the reach of any present technology. In this paper we propose a new method to identify the birth of the barium daughter ion in the neutrinoless double beta decay of $^{136}$Xe. The method adapts Single Molecule Fluorescent Imaging, a technique from biochemistry research with demonstrated single ion sensitivity. We explore possible SMFI dyes sui…
Radio-frequency (RF) carpets with ultra-fine pitches are examined for ion transport in gases at atmospheric pressures and above. We develop new analytic and computational methods for modeling RF ion transport at densities where dynamics are strongly influenced by buffer gas collisions. An analytic description of levitating and sweeping forces from phased arrays is obtained, then thermodynamic and kinetic principles are used to calculate ion loss rates in the presence of collisions. This methodology is validated against detailed microscopic SIMION simulations. We then explore a parameter space …
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$2~nm), and detected with a statistical significance of 12.9~$σ$ over backgrounds. This lays the foundation for a new and potentially background-free neutrinoless double beta decay technology, based on SMFI co…
Motivated by the possibility of guiding daughter ions from double beta decay events to single-ion sensors for barium tagging, the NEXT collaboration is developing a program of R&D to test radio frequency (RF) carpets for ion transport in high pressure xenon gas. This would require carpet functionality in regimes at higher pressures than have been previously reported, implying correspondingly larger electrode voltages than in existing systems. This mode of operation appears plausible for contemporary RF-carpet geometries due to the higher predicted breakdown strength of high pressure xenon rela…
Experimental updates on development of accelerator-driven ion source at TRIUMF to benchmark Ba-tagging techniques for future neutrinoless double beta decay searches
TRIUMF（特柳姆夫国家粒子加速器中心）；Department of Physics and Astronomy, McMaster University（麦克马斯特大学物理与天文系）；Department of Physics and Physical Oceanography, University of North Carolina at Wilmington（北卡罗来纳大学威尔明顿分校物理与物理海洋学系）；Department of Physics, McGill University（麦吉尔大学物理系）；Department of Physics and Astronomy, University of Victoria（维多利亚大学物理与天文系）
We describe a system to transport and identify barium ions produced in liquid xenon, as part of R&D towards the second phase of a double beta decay experiment, nEXO. The goal is to identify the Ba ion resulting from an extremely rare nuclear decay of the isotope $^{136}$Xe, hence providing a confirmation of the occurrence of the decay. This is achieved through Resonance Ionization Spectroscopy (RIS). In the test setup described here, Ba ions can be produced in liquid xenon or vacuum and collected on a clean substrate. This substrate is then removed to an analysis chamber under vacuum, where la…
\Xe{136} is used as the target medium for many experiments searching for \bbnonu. Despite underground operation, cosmic muons that reach the laboratory can produce spallation neutrons causing activation of detector materials. A potential background that is difficult to veto using muon tagging comes in the form of \Xe{137} created by the capture of neutrons on \Xe{136}. This isotope decays via beta decay with a half-life of 3.8 minutes and a \Qb\ of $\sim$4.16 MeV. This work proposes and explores the concept of adding a small percentage of \He{3} to xenon as a means to capture thermal neutrons …
We introduce a novel particle detection concept for large-volume, fine granularity particle detection: The Ion Fluorescence Chamber (IFC). In electronegative gases such as SF$_6$ and SeF$_6$, ionizing particles create ensembles of positive and negative ions. In the IFC, positive ions are drifted to a chemically active cathode where they react with a custom organic turn-on fluorescent monolayer encoding a long-lived 2D image. The negative ions are sensed electrically with course resolution at the anode, inducing an optical microscope to travel to and scan the corresponding cathode location for …
We describe a source capable of producing single barium ions through nuclear recoils in radioactive decay. The source is fabricated by electroplating 148Gd onto a silicon α-particle detector and vapor depositing a layer of BaF2 over it. 144Sm recoils from the alpha decay of 148Gd are used to dislodge Ba+ ions from the BaF2 layer and emit them in the surrounding environment. The simultaneous detection of an α particle in the substrate detector allows for tagging of the nuclear decay and of the Ba+ emission. The source is simple, durable, and can be manipulated and used in different environments…
An RF ion-funnel technique has been developed to extract ions from a high-pressure (10 bar) noble-gas environment into vacuum ($10^{-6}$ mbar). Detailed simulations have been performed and a prototype has been developed for the purpose of extracting $^{136}$Ba ions from Xe gas with high efficiency. With this prototype, ions have been extracted for the first time from high-pressure xenon gas and argon gas. Systematic studies have been carried out and compared to the simulations. This demonstration of extraction of ions with mass comparable to that of the gas generating the high-pressure into va…
