Persistent spectral hole burning has been observed on the zero-phonon lines of the main site and several perturbed sites of
Eu2+ in CaS:Eu single crystals. Hole burning occurs by two-step photoionization, can be strongly gated with IR irradiation, and takes place by excited-state absorption from the metastable
4f65d excited state to the conduction band followed by electron transport to
Eu3+ centers which are the dominant traps. A complex hole structure consisting of a narrow feature (200 MHz), and broader features ($\ensuremath{\approx}5$ and $\ensuremath{\approx}100\mathrm{GHz}$) is observed. A mechanism is described for the occurrence of these unusually broad features. Time-varying internal electric fields which occur during the hole burning due to photoionization and trapping can lead to burning of holes at frequencies non-resonant with that of the laser. In addition, a mechanism for hole erasure, tunneling between Eu ions, is demonstrated. This mechanism is identified from the frequency dependence of the hole erasure which follows the
Eu2+ absorption, and the linear dependence of the photoconductivity and hole erasure efficiency on irradiation power, both of which indicate erasure in a single-photon process.
Previously we have reported the largest number of photon- gated spectral holes ever burned in a solid. This has interest in their applications in optical storage. However, multiple holeburning in MgS:Eu resulted in noticeable erasure of the previously burned holes. This was attributed to the mechanism of holeburning in this material where both Eu2+ and Eu3+ are stable ions. In gated holeburning, Eu2+ ions are ionized. Eu3+ that form deep traps, capture the electrons generated during the holeburning and are converted to Eu2+. The Zero Phonon Line (ZPL) of these newly formed Eu2+ ions are randomly distributed across the inhomogeneous line causing a partial erasure of the holes burned earlier. This reduces the efficiency of holeburning. Co-doping of MgS:Eu and CaS:Eu with different rare earth (RE) ions has been investigated to provide deep electron traps other than Eu3+. Furthermore, co-doping provides the opportunity to burn holes in multiple ZPLs belonging to different REs, thus increasing the storage density many folds.