Revealing the Exciton Fine Structure of PbSe Nanocrystal Quantum Dots Using Optical Spectroscopy in High Magnetic Fields

Abstract

We measure the photoluminescence lifetime τ of excitons in colloidal PbSe nanocrystals (NCs) at low temperatures to 270 mK and in high magnetic fields to 15 T. For all NCs, τ increases sharply below 10 K but saturates by 500 mK. In contrast to the usual picture of well-separated "bright" and "dark" exciton states (found, e.g., in CdSe NCs), these dynamics fit remarkably well to a system having two exciton states with comparable--but small--oscillator strengths that are separated by only 300-900 μeV depending on NC size. Importantly, magnetic fields reduce τ below 10 K, consistent with field-induced mixing between the two states. Magnetic-circular dichroism studies reveal exciton g factors from 2-5, and magnetophotoluminescence shows >10% circularly polarized emission.