Most alkali halides crystallize in the fcc sodium chloride structure. In contrast, with the exception of CsF, the Cs-halides form the simple cubic cesium chloride (CsCl) structure at ambient conditions and they have a substantially different electronic structure than other alkali halides; in particular, they have several nearly degenerate electronic levels near the Brillouin zone center. Highly resolved Three-Photon Spectroscopy (TPS) measurements allow direct observation of the near band edge structure and, in the case of CsI, probe more states than one-photon techniques. A number of interesting phenomena, among them level repulsion (Fermi resonance), occur as these levels are tuned through one another by application of hydrostatic pressure. To the best of our knowledge, this has been
Unusual phenomena occurring under hydrostatic compression in the near-band-edge structure of CsI crystals were examined using the nonlinear optical technique of three-photon excitation. The lowest one-photon allowed transition to the exciton-polariton A of gamma-4 symmetry redshifts, while the one-photon forbidden paraexciton C of gamma-5 symmetry blueshifts to a crossing of energies at 4.4 kbar. During this process, the A level exhibits strong spectral line narrowing by more than a factor of 10, while the C level intensity increases by about the same factor. We believe this is the first reported observation of pressure induced line narrowing of deep UV electronic states in solids.
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