Bright-Dark Exciton Interplay Evidenced by Spin Polarization in CdSe/CdMnS Nanoplatelets (2404.07014v2)

Abstract: Diluted magnetic semiconductor (DMS) colloidal nanocrystals demonstrate remarkable magneto-optical properties. However, the behavior of circular polarization of their emission in high magnetic fields remains unclear. We measure magneto-optical properties of colloidal CdSe/CdMnS nanoplatelets in high magnetic fields up to 30 T and at cryogenic temperatures. The degree of circular polarization of photoluminescence demonstrates non-monotonous behavior in a magnetic field. In low magnetic fields, the polarization degree is positive, due to an exchange interaction of excitons with localized spins of magnetic Mn ions. The exchange interaction is strong enough to overcome the intrinsic Zeeman splitting, which provides negatively polarized emission in nonmagnetic CdSe/CdS nanoplatelets. After reaching a maximum the polarization degree starts to decrease and reverses the sign to negative in high magnetic fields. The critical magnetic field, in which the sign is reversed, increases when temperature is elevated. We develop a model, which explains this behavior by an interplay of bright and dark exciton recombination.