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Bright-Dark Exciton Interplay Evidenced by Spin Polarization in CdSe/CdMnS Nanoplatelets for Spin-Optronics
Diluted magnetic semiconductor (DMS) colloidal nanocrystals demonstrate remarkable magneto-optical properties. The ability to control their magnetization and, consequently, the circular polarization of exciton emission holds significant potential for spintronic applications. However, the interplay between bright and dark exciton recombination and its impact on the polarization of emission are not yet fully understood. We measure the magneto-optical properties of colloidal CdSe/CdMnS nanoplatelets at cryogenic temperatures in high magnetic fields up to 30 T. The degree of circular polarization of photoluminescence demonstrates nonmonotonous 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 Mn2+ ions. After reaching a maximum, the polarization degree starts to decrease and reverses the sign to negative in high magnetic fields, which is unusual in DMSs. The critical magnetic field, in which the sign is reversed, increases when the temperature is elevated. We develop a model that explains this behavior by an interplay of bright and dark exciton recombination. In high magnetic fields, the dark exciton radiative recombination rate accelerates due to mixing with the bright state, and the intrinsic Zeeman splitting of dark exciton overcomes the exchange with Mn2+ ions. As a result, the lowest |−2⟩ exciton energy level dominates in emission, providing negatively polarized photoluminescence.