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The Excited-state Absorption-spectra Of Doped Inorganic Crystals And Glasses By Double Optical Resonance.

James Hunter Thirtle

Published Jan 1, 1974• 0 citations
Publisher
DOI
10.7302/21209

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European Quantum Electronics Conference (EQEC)•Jan 1, 2003•0 citations
Excited-state absorption spectra of erbium and thulium doped gallium lanthanum sulfide glasses reveal transitions whose final 4f4f4f states do not appear in the ground state absorption spectra due to resonance with the fundamental absorption of the glass host. The results give direct evidence for the model of isolated rare-earth ions with highly shielded 4f4f4f levels showing no noticeable interaction with the host material despite resonance. Only the energy splitting of the 4f4f4f levels is relevant for energy transfer processes between rare-earth ions and the host material, whereas the absolute energetic position is unimportant.
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.
The paper reports on the experimental realization on the possibility of isolating ions in a selected frequency channel. In the scheme, this interaction is mediated by the change in permanent dipole moment experienced by the rare-earth ions when they are optically excited from the ground state to an excited state. The change in dipole moment changes the electric field experienced by ions situated close to the excited ion, thus their absorption frequencies are changed. The important aspect, in order to use this frequency shift for controlled logic, is that the shift is large enough for ions, originally resonant with a certain laser frequency, to be shifted out of resonance with this laser field. Excitation induced frequency shifts are experimentally observed, which opens the way for the realisation of the first quantum gate in this type of solid state materials.