Quantum crystallites and nonlinear optics

  • Brus L
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This is a review and analysis of the optical properties of quantum crystallites, with principal emphasis on the electro-optic Stark effect and all optical third order nonlinearity. There are also introductory discussions on physical size regimes, crystallite synthesis, quantum confinement theory, and linear optical properties. The experiments describe CdSe crystallites, exhibiting strong confinement of electrons and holes, and CuCl crystallites, exhibiting weak confinement of the exciton center of mass. In the CdSe system, neither the Stark effect nor the third order nonlinearity is well understood. The Stark shifts appear to be smaller than calculated, and field inducted broadening also occurs. The third order nonlinearity is only modestly stronger than in bulk material, despite theoretical prediction. Unexpectedly large homogeneous widths, due to surface carrier trapping, in the nominally discrete crystallite excited states appear to be involved. The CuCl system shows far narrower spectroscopic homogeneous widths, and corresponds more closely to an ideal quantum dot in the weak confinement limit. CuCl also exhibits exciton superradiance at low temperature. Surface chemistry and crystallite encapsulation are critical in achieving the predicted large Stark and third order optical effects in II-VI and III-V crystallites.

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  • L. Brus

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