Low Threshold Multiexciton Optical Gain in Colloidal CdSe/CdTe Core/Crown Type-II Nanoplatelet Heterostructures

Colloidal cadmium chalcogenide core/crown type-II nanoplatelet heterostructures, such as CdSe/CdTe, are promising materials for lasing and light-emitting applications. Their rational design and improvement requires the understanding of the nature of single- and multiexciton states. Using pump fluence and wavelength-dependent ultrafast transient absorption spectroscopy, we have identified three spatially and energetically distinct excitons (in the order of increasing energy): interface-localized charge transfer exciton (X_CT, with electron in the CdSe core bound to the hole in the CdTe crown), and CdTe crown-localized X_CdTe and CdSe core-localized X_CdSe excitons. These exciton levels can be filled sequentially, with each accommodating two excitons (due to electron spin degeneracy) to generate one to six exciton states (with lifetimes of ≫1000, 209, 43.5, 11.8, 5.8, and 4.5 ps, respectively). The spatial separation of these excitons prolongs the lifetime of multiexciton states. Optical gain was observed in tri- (XX_CTX_CdTe) and four (XX_CTXX_CdTe) exciton states. Because of the large absorption cross section of nanoplatelets, an optical gain threshold as low as ∼43 μJ/cm² can be achieved at 550 nm excitation for a colloidal solution sample. This low gain threshold and the long triexciton (gain) lifetime suggest potential applications of these 2D type-II heterostructures as low threshold lasing materials.