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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

New Host Lattices for Optical Hole Burning: Materials of Low Nuclear Spin Densities

A. Caprez, P. Meyer, J. Hulliger

Published Jan 1, 1996• 0 citations
Publisher
DOI
10.1109/cleoe.1996.562182

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New Host Lattices for Optical Hole Burning: Materials of Low Nuclear Spin Densities

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Optical hole burning (OHB) on rare earth ions has so far been performed mainly on single crystals which have been developed as a laser host material. However, an essential drawback of most of these lattices is the high nuclear spin density s of the constituting ions, giving rise to a broadening of the homogeneous width of the absorption of individual rare earth ions [1]. As a result of a limited number of elements providing a high natural abundance of isotopes with zero nuclear spin I or small nuclear momentum µ, there are not too many existing or possible new host lattices to work on. Further restrictions arise in the case of heterogeneous doping as well as from a given site symmetry.

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Laser induced hole burning in optical absorption bands of low temperature solids has been investigated with emphasis on mechanisms for population hole burning, the interactions with the environment which limit the hole widths and the use of hole burning for ultra high resolution spectroscopy. Hole burning was observed in a wide range of solids including organic and organometallic molecules in crystals and rare earth ions in crystals and glasses. The mechanisms for hole burning also varied widely and a new mechanism involving optically induced nuclear spin flips of near neighbor nuclei was discovered. Examples of hole burning in new classes of materials are presented here for the first time, namely inorganic glasses (silicate glasses containing Nd(3+), Pr(3+) or Eu(3+)) and undoped stoichiometric compounds (e.g., EuP5O14). Hole recovery was used to determine nuclear spin lattice relaxation rates in praseodymium doped crystals. For allowed optical transitions (e.g., singlet states of zinc porphyrin, dibromoindigo and color centers in alkali halides) the hole widths at 2K are limited by population decay to approximately 50 MHz. For longer lived optical levels in crystalline materials, e.g., those containing rare earth ions, the hole widths are narrower (less than 10 MHz) and are limited by dynamical interactions with surrounding nuclei. In amorphous materials such as europium doped silicate glass, hole widths are much broader, being limited by low frequency tunneling motions. Hole burning measurements were complemented by time domain coherent transient (photon echo, and optical free decay) measurements of homogeneous linewidths which enabled us to measure optical resonances as narrow as 760 Hz in Eu(3+):Y2O3.

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Spectroscopic investigations of Pr3+:CaWO4 at liquid-helium temperatures

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Rare-earth ions doped into low nuclear-spin density host crystals provide a promising platform for quantum information storage and processing. Calcium tungstate $({\mathrm{CaWO}}_{4})$ is an attractive host crystal because it can be isotopically enriched to provide a nuclear spin free environment. Here, we report a spectroscopic investigation of the optical transitions and hyperfine transitions of praseodymium $(^{141}\mathrm{Pr}^{3+})$ doped in ${\mathrm{CaWO}}_{4}$ at liquid-helium temperatures. The hyperfine structures of the ${}^{3}{H}_{4}$(0) and ${}^{1}{D}_{2}$(0) states are determined by spectral hole burning. The results indicate that ${\mathrm{Pr}}^{3+}$:${\mathrm{CaWO}}_{4}$ is an appealing candidate for quantum memory in quantum information processing.

Physical Review A•Feb 6, 2023•4 citations
Optical hole burning (OHB) on rare earth ions has so far been performed mainly on single crystals which have been developed as a laser host material. However, an essential drawback of most of these lattices is the high nuclear spin density s of the constituting ions, giving rise to a broadening of the homogeneous width of the absorption of individual rare earth ions [1]. As a result of a limited number of elements providing a high natural abundance of isotopes with zero nuclear spin I or small nuclear momentum µ, there are not too many existing or possible new host lattices to work on. Further restrictions arise in the case of heterogeneous doping as well as from a given site symmetry.
Laser induced hole burning in optical absorption bands of low temperature solids has been investigated with emphasis on mechanisms for population hole burning, the interactions with the environment which limit the hole widths and the use of hole burning for ultra high resolution spectroscopy. Hole burning was observed in a wide range of solids including organic and organometallic molecules in crystals and rare earth ions in crystals and glasses. The mechanisms for hole burning also varied widely and a new mechanism involving optically induced nuclear spin flips of near neighbor nuclei was discovered. Examples of hole burning in new classes of materials are presented here for the first time, namely inorganic glasses (silicate glasses containing Nd(3+), Pr(3+) or Eu(3+)) and undoped stoichiometric compounds (e.g., EuP5O14). Hole recovery was used to determine nuclear spin lattice relaxation rates in praseodymium doped crystals. For allowed optical transitions (e.g., singlet states of zinc porphyrin, dibromoindigo and color centers in alkali halides) the hole widths at 2K are limited by population decay to approximately 50 MHz. For longer lived optical levels in crystalline materials, e.g., those containing rare earth ions, the hole widths are narrower (less than 10 MHz) and are limited by dynamical interactions with surrounding nuclei. In amorphous materials such as europium doped silicate glass, hole widths are much broader, being limited by low frequency tunneling motions. Hole burning measurements were complemented by time domain coherent transient (photon echo, and optical free decay) measurements of homogeneous linewidths which enabled us to measure optical resonances as narrow as 760 Hz in Eu(3+):Y2O3.
Rare-earth ions doped into low nuclear-spin density host crystals provide a promising platform for quantum information storage and processing. Calcium tungstate (CaWO4)({\mathrm{CaWO}}_{4})(CaWO4​) is an attractive host crystal because it can be isotopically enriched to provide a nuclear spin free environment. Here, we report a spectroscopic investigation of the optical transitions and hyperfine transitions of praseodymium (141Pr3+)(^{141}\mathrm{Pr}^{3+})(141Pr3+) doped in CaWO4{\mathrm{CaWO}}_{4}CaWO4​ at liquid-helium temperatures. The hyperfine structures of the 3H4{}^{3}{H}_{4}3H4​(0) and 1D2{}^{1}{D}_{2}1D2​(0) states are determined by spectral hole burning. The results indicate that Pr3+{\mathrm{Pr}}^{3+}Pr3+:CaWO4{\mathrm{CaWO}}_{4}CaWO4​ is an appealing candidate for quantum memory in quantum information processing.