论文标题
钡选择性化学(通过二重乙醚萘)的荧光团进行单离子钡标记的荧光团
Barium Selective Chemosensing by Diazacrown Ether Naphthalimide Turn-on Fluorophores for Single Ion Barium Tagging
论文作者
论文摘要
研究了钡的单分子荧光检测,以增强中准双β衰变($0νββ$)搜索的敏感性和鲁棒性,$^{136} $ XE,这些发现将改变我们对中子性质和宇宙早期历史的理解。一个关键的发展步骤是合成能够掺入高压$^{136} $ XE气体中的钡选择性化学传感器。在这里,我们将含有单核和迪亚扎 - 克罗恩醚的荧光萘化学传感器报告为单个BA $^{2+} $检测的代理。 Monoaza-18-Crown-6 Ether Naphthalimide传感器主要对Ba $^{2+} $和HG $^{2+} $显示敏感性,而两种Diaza-18-Crown-6 Ether-6 Ether Naphthalimides显示出对BA $^{2+} $的理想选择。溶液期荧光和NMR实验支持光诱导的电子转移机制,可在存在钡离子的情况下进行转式荧光感应。离子受体相互作用的变化可在竞争性钡,汞和钾离子之间有效选择性,并通过详细的计算正确预测了荧光响应。使用这些分子,使用无油显微镜技术实现了干燥相单BA $^{2+} $ ion成像。这代表着在$^{136} $ Xe中进行单个BA $^{2+} $检测的实用方法的重大进展,可说明了一种无背景的技术来搜索假设的$0νββ$。
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. 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 $0νββ$.