Abstract. We use femtosecond time-resolved transmission spectroscopy to study the density and time dependence of transient absorption changes of CdSe nanocrystals. Our data show pronounced absorption saturation up to complete bleaching of the lowest optical transition. At high carrier density the nonlinear spectra show several peaks that can be related to the two lowest quantized electron states. Thetime dependence of the carrier-induced absorption changes indicates an ultrafast relaxation process within the strongly broadened absorption lines. 78.47.+p; 73.20.Dx; 71.35.+z In recent years, there has been a strong interest in lowdimensional semiconductor structures such as quantum wells, quantum wires, and quantum dots. The electronic states in these artificial materials are strongly influenced by size quantization effects, which occur when the dimensions of the structures become comparable to or smaller than the exciton Bohr radius aB. Then, the electronic and optical properties of the structures become determined by their geometry. Thus, the controlled fabrication of low-dimensional semiconductor structures may allow to obtain materials with predefined properties.
PACS:In addition, size quantization has been shown to lead to a significant enhancement of excitonic effects and to strongly enhanced optical nonlinearities in two-dimensional quantum wells, where the carriers are confined in only one dimension [1]. It can be expected that a confinement of carriers in two or three dimensions will lead to a further enhancement of the optical nonlinearities. Therefore, semiconductor quantum dots appear as a promising new material for nonlinear optical applications. It has been found that semiconductor crystallites with radii on the order of a few nanometer, denoted as nanocrystals (NCs), can be rather easily produced in semiconductor-doped glasses (which are commercially available as color-glass filters) or in organic solution [2][3][4]. The linear absorption of such samples generally shows a correlation with the average NC size, as the lowest absorption feature shifts towards higher energies with decreasing size [3,[5][6][7][8][9][10][11]. While this clear sign of size quantization is easily observed, the absorption spectra of semiconductordoped glasses usually fail to show sharp exciton peaks (in contrast with two-dimensional quantum wells) or even wellseparated absorption lines that reflect the expected discrete energy spectrum of a "zero-dimensional" structure. It is commonly accepted that the presence of discrete electronic states is masked in the linear absorption by strong homogeneous and inhomogeneous broadening. The nanocrystals may vary in size, geometry, and chemical composition. These variations cause a strong inhomogeneous broadening of the optical transitions. Variations of the NC size are typically on the order of 25% [12]. This value may be reduced to a few percent by sophisticated preparation techniques, but even then the size distribution has a significant influence on the optical properties [4,10,1...