Tight-binding g-Factor Calculations of CdSe Nanostructures

TL;DR

This study uses semiempirical tight-binding calculations to analyze the g-factors of CdSe nanostructures, revealing shape-dependent transitions and anisotropy effects that align with experimental observations.

Contribution

It introduces a detailed method for calculating g-factors in CdSe nanocrystals, highlighting the shape dependence and transition phenomena not previously characterized.

Findings

g-factors are size-independent in near-spherical dots

Shape extension causes a transition from anisotropic to isotropic g-factors

Surface details influence g-factor values in small systems

Abstract

The Lande g-factors for CdSe quantum dots and rods are investigated within the framework of the semiempirical tight-binding method. We describe methods for treating both the n-doped and neutral nanostructures, and then apply these to a selection of nanocrystals of variable size and shape, focusing on approximately spherical dots and rods of differing aspect ratio. For the negatively charged n-doped systems, we observe that the g-factors for near-spherical CdSe dots are approximately independent of size, but show strong shape dependence as one axis of the quantum dot is extended to form rod-like structures. In particular, there is a discontinuity in the magnitude of g-factor and a transition from anisotropic to isotropic g-factor tensor at aspect ratio ~1.3. For the neutral systems, we analyze the electron g-factor of both the conduction and valence band electrons. We find that the behavior of the electron g-factor in the neutral nanocrystals is generally similar to that in the n-doped case, showing the same strong shape dependence and discontinuity in magnitude and anisotropy. In smaller systems the g-factor value is dependent on the details of the surface model. Comparison with recent measurements of g-factors for CdSe nanocrystals suggests that the shape dependent transition may be responsible for the observations of anomalous numbers of g-factors at certain nanocrystal sizes.