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

Thapa, P., Byrnes, N. K., Denisenko, A. A., Foss, Jr., F. W., Jones, B. J. P., Mao, J. X., Nam, K., Newhouse, C. A., Nygren, D. R., McDonald, A. D., Vuong, T. T., Woodruff, K.

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 $0νββ$.

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