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Rare earth ions in crystals exhibit narrow spectral features andhyperfine-split ground states with exceptionally long coherence times. Thesefeatures make them ideal platforms for quantum information processing in thesolid state. Recently, we reported on the first high-resolution spectroscopy ofsingle Pr$^{3+}$ ions in yttrium orthosilicate (YSO) nanocrystals. While inthat work we examined the less explored $^3$H$_4$-$^3$P$_0$ transition at awavelength of 488 nm, here we extend our investigations to the$^3$H$_4$-$^1$D$_2$ transition at 606 nm. In addition, we present measurementsof the second-order autocorrelation function, fluorescence lifetime, andemission spectra of single ions as well as their polarization dependencies onboth transitions; these data were not within the reach of the first experimentsreported earlier. Furthermore, we show that by a proper choice of thecrystallite, one can obtain narrower spectral lines and, thus, resolve thehyperfine levels of the excited state. We expect our results to make single-ionspectroscopy accessible to a larger scientific community.

High-resolution spectroscopy of single Pr$^{3+}$ ions on the $^3$H$_4$-$^1$D$_2$ transition