This review is concerned with quantum confinement effects in low-dimensional semiconductor systems. The emphasis is on the optical properties, including luminescence, of nanometre-sized microcrysta...

Low-dimensional systems: quantum size effects and electronic properties of semiconductor microcrystallites (zero-dimensional systems) and some quasi-two-dimensional systems

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.

Quantum crystallites and nonlinear optics

We analyze theoretically the optical properties of ideal semiconductor crystallites so small that they show quantum confinement in all three dimensions [quantum dots (QD's)]. In the limit of a QD much smaller than the bulk exciton size, the linear spectrum will be a series of lines, and we consider the phonon broadening of these lines. The lowest interband transition will saturate like a two-level system, without exchange and Coulomb screening. Depending on the broadening, the absorption and the changes in absorption and refractive index resulting from saturation can become very large, and the local-field effects can become so strong as to give optical bistability without external feedback. The small QD limit is more readily achieved with narrow-band-gap semiconductors.

Theory of the linear and nonlinear optical properties of semiconductor microcrystallites

We have observed a darkening effect and the formation of permanent volume gratings in CdSSe semiconductor-doped glasses, both phenomena being certainly due to the same photochemical mechanism. This allowed us to reconcile contradictory results concerning the speed of their nonlinear response. We also studied the frequency dependence of X (3) below the gap and the intensity dependence of the reflectivity of these phase-conjugate mirrors. Our results can be interpreted in terms of the band-filling model with Boltzmann statistics. Finally, frequency- and. time-resolved luminescence measurements helped us to interpret various results.

New results on optical phase conjugation in semiconductor-doped glasses

Excitons in Quantum Dots

Using a “pump-and-probe” technique, the absorption changes of CuCl microcrystallites embedded in a glass matrix are studied. A blue shift of the resonance and a bleaching of the absorption at photon energies lower than the photon energy of the pump, is observed accompanied by an increase of absorption at higher photon energies.



Nous etudions les variations induites d'absorption de microcristallites de CuCl dispersees dans du verre, en utilisant une technique „pompe et test”. Nous observons un deplacement vers le bleu de la resonance excitonique, une diminution de l'absorption a des energies de photon inferieures a celle de la pompe, ainsi qu'une augmentation de l'absorption a des energies superieures.

M. Robino

Papers

Laser Induced Absorption of CuCl Microcrystallites in a Glass Matrix