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تسجيل مستخدم جديدBarium Selective Chemosensing by Diazacrown Ether Naphthalimide Turn-on Fluorophores for Single Ion Barium Tagging
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Single molecule fluorescence detection of barium is investigated for enhancing the sensitivity and robustness of a neutrinoless double beta decay ($0 ubetabeta$) 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. Monoaza-18-crown-6 ether naphthalimide sensors showed sensitivity primarily to Ba$^{2+}$ and Hg$^{2+}$, whereas two diaza-18-crown-6 ether naphthalimides revealed a desirable selectivity toward Ba$^{2+}$. Solution-phase fluorescence and NMR experiments support a photoinduced electron transfer mechanism enabling turn-on fluorescence sensing in the presence of barium ions. Changes in ion-receptor interactions enable effective selectivity between competitive barium, mercury, and potassium ions, with detailed calculations correctly predicting fluorescence responses. With these molecules, dry-phase single Ba$^{2+}$ ion imaging with turn-on fluorescence is realized using oil-free microscopy techniques. This represents a significant advance toward a practical method of single Ba$^{2+}$ detection within large volumes of $^{136}$Xe, plausibly enabling a background-free technique to search for the hypothetical process of $0 ubetabeta$.
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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 bee
n 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.
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, where the barium atom is tagged via fluorescence imaging in the solid xenon matrix. Here we demonstrate imaging and counting of individual atoms of barium in solid xenon by scanning a focused laser across a solid xenon matrix deposited on a sapphire window. When the laser sits on an individual atom, the fluorescence persists for $sim$30~s before dropping abruptly to the background level, a clear confirmation of one-atom imaging. No barium fluorescence persists following evaporation of a barium deposit to a limit of $leq$0.16%. This is the first time that single atoms have been imaged in solid noble element. It establishes the basic principle of a barium tagging technique for nEXO.
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, beyo
nd 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 suitable for the problem of barium ion detection in high pressure xenon gas, and develop a fiber-coupled sensing system with which we can detect the presence of bulk Ba$^{++}$ ions remotely. We show that our sensor produces signal-to-background ratios as high as 85 in response to Ba$^{++}$ ions when operated in aqueous solution. We then describe the next stage of this R&D program, which will be to demonstrate chelation and fluorescence in xenon gas. If a successful barium ion tag can be developed using SMFI adapted for high pressure xenon gas detectors, the first essentially zero background, ton-scale neutrinoless double beta decay technology could be realized.
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 d
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