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Single molecule fluorescence detection of barium is investigated forenhancing the sensitivity and robustness of a neutrinoless double beta decay($0\nu\beta\beta$) search in $^{136}$Xe, the discovery of which would alter ourunderstanding of the nature of neutrinos and the early history of the Universe.A key developmental step is the synthesis of barium-selective chemosensorscapable of incorporation into ongoing experiments in high-pressure $^{136}$Xegas. Here we report turn-on fluorescent naphthalimide chemosensors containingmonoaza- and diaza-crown ethers as agents for single Ba$^{2+}$ detection.Monoaza-18-crown-6 ether naphthalimide sensors showed sensitivity primarily toBa$^{2+}$ and Hg$^{2+}$, whereas two diaza-18-crown-6 ether naphthalimidesrevealed a desirable selectivity toward Ba$^{2+}$. Solution-phase fluorescenceand NMR experiments support a photoinduced electron transfer mechanism enablingturn-on fluorescence sensing in the presence of barium ions. Changes inion-receptor interactions enable effective selectivity between competitivebarium, mercury, and potassium ions, with detailed calculations correctlypredicting fluorescence responses. With these molecules, dry-phase singleBa$^{2+}$ ion imaging with turn-on fluorescence is realized using oil-freemicroscopy techniques. This represents a significant advance toward a practicalmethod of single Ba$^{2+}$ detection within large volumes of $^{136}$Xe,plausibly enabling a background-free technique to search for the hypotheticalprocess of $0\nu\beta\beta$.

Barium Selective Chemosensing by Diazacrown Ether Naphthalimide Turn-on Fluorophores for Single Ion Barium Tagging