Exciton Spin Dynamics and Photoluminescence Polarization of CdSe/CdS Dot-in-Rod Nanocrystals in High Magnetic Fields
Benjamin Siebers a, Louis Biadala a, Dmitri Yakovlev a b, Manfred Bayer a b, Anna Rodina b, Zeger Hens c, Tangi Aubert c
a TU-Dortmund, Experimentelle Physik 2 Technische Universität Dortmund Otto-Hahn-Straße 4, Dortmund, 0, Germany
b Ioffe Institute, Ioffe Institute,St. Petersburg, Russian Federation
c Physics and Chemistry of Nanostructures, Krijgslaan 281 - building S3, Ghent
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe September Meeting 2015 (NFM15)
Santiago de Compostela, Spain, 2015 September 6th - 15th
Oral, Louis Biadala, presentation 008
Publication date: 8th June 2015

Understanding spin relaxation mechanisms is important to design spin preserving environments for future spin-based devices for information storage. Colloidal NCs, due to their high versatility regarding synthesis and processing as well as due to their unique and widely tunable optical properties are suitable candidates for such applications. Thus, comprehensive knowledge about the linkage between NC size, shape and material properties and exciton spin dynamics is highly desirable. We report on how spin dynamics between the dark exciton ground states split by the magnetic field are affected by the size and shape of the CdS shell. Interestingly we find, that the core/shell interface strongly affects the spin relaxation rate, whereas the shell shape and size have only slight impact. These results highlight the crucial role of the core/shell interface for the optical properties of NCs, especially for the relaxation and recombination dynamics of dark excitons. We also study the impact of the shell shape on magnetic field induced PL circular polarization. Our results indicate, that the saturation level of the Degree of Circular Polarization (DCP) in NCs depends on the aspect ratio of the shell. We elaborate a theoretical approach for analyzing and predicting polarization properties of NCs in the presence of an external magnetic field, which includes a dielectric enhancement effect resulting from an anisotropic shell as well as phonon-mediated coupling of the dark exciton ground state to bright exciton states with radiative transitions parallel and perpendicular to the hexagonal axis. Besides explaining the discrepancy existing in literature regarding DCP values [1-4], our model suggests, that, at low temperatures and in the presence of magnetic fields the PL can be polarized perpendicular to the hexagonal axis in contrast to what has been observed at room temperature [5]. This striking result highlights a new mechanism in the radiative recombination of the dark exciton. 



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