Time- and Polarization-Resolved Optical Spectroscopy of Colloidal CdSe Nanocrystal Quantum Dots in High Magnetic Fields

Abstract: In an effort to elucidate the spin (rather than charge) degrees of freedom in colloidal semiconductor nanocrystal quantum dots, we report on a series of static and time-resolved photoluminescence measurements of colloidal CdSe quantum dots in ultra-high magnetic fields up to 45 Tesla. At low temperatures (1.5 K - 40 K), the steady-state photoluminescence (PL) develops a high degree of circular polarization with applied magnetic field, indicating the presence of spin-polarized excitons. Time-resolved PL studies reveal a marked decrease in radiative exciton lifetime with increasing magnetic field and temperature. Except for an initial burst of unpolarized PL immediately following photoexcitation, high-field time-resolved PL measurements reveal a constant degree of circular polarization throughout the entire exciton lifetime, even in the presence of pronounced exciton transfer via Forster energy transfer processes.