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Harnessing the Shape-Induced Optical Anisotropy of a Semiconductor Nanocrystal: A New Type of Intraband Absorption Spectroscopy
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文摘
In recent years there have been active developments of spectroscopic methods for analysis of light absorption by individual nanocrystals. Here we provide a solid theoretical background for one of these methods via developing a uniform theory of anisotropic intraband absorption by a nonspherical semiconductor nanocrystal. The nanocrystal is assumed to be simultaneously excited by the linearly polarized pump and probe fields that are, respectively, resonant to the interband and intraband transitions of the nanocrystal鈥檚 electronic subsystem. Three relative arrangements of the excited electron鈥揾ole pair states are considered, covering all possible types of transition schemes that can occur in experiment. The developed theory is then used to calculate the angular absorption spectra for the most common shapes of the nanocrystals, which essentially lays the foundation of stationary pump鈥損robe polarization spectroscopy based on the shape-induced anisotropy of intraband absorption by a semiconductor nanocrystal. This spectroscopy may serve modern nanotechnology by facilitating characterization of anisotropic nanostructures as it allows one to reliably determine the shapes and orientations of individual nanocrystals and find the symmetry of quantum states involved in the electronic transitions induced by the probe.

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