Autler-Townes splitting and linear dichroism in colloidal CdSe nanoplatelets driven by near-infrared pulses.

Abstract

Coherent interaction between light fields and matter has led to many exotic physical phenomena, one of which is the Autler-Townes splitting originating from the optical Stark effect of a three-level system. It has been well documented for atoms, molecules, and low-dimensional, epitaxial-grown semiconductors but rarely for solution-processed samples. Here, we report on Autler-Townes splitting observed in CdSe nanoplatelets. The strong intersubband transition of these nanoplatelets situated in the near-infrared allows us to coherently drive it with femtosecond near-infrared pulses, and meanwhile, their strong interband transition in the visible records the resultant spectral changes. The splitting is most prominent with cross-polarized, linear pump-probe pulses, consistent with the orthogonal polarizations of interband and intersubband transition dipoles. When the nanoplatelets are driven from tilted incident angles, we observe anomalous spectral lineshapes arising from a competition between interband and intersubband drivings, which are nevertheless quantitatively captured by our dressed-state model simulation.