JOURNAL ARTICLE
RESEARCH SUPPORT, U.S. GOV'T, NON-P.H.S.
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Low Threshold Multiexciton Optical Gain in Colloidal CdSe/CdTe Core/Crown Type-II Nanoplatelet Heterostructures.

ACS Nano 2017 March 29
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 (XCT , with electron in the CdSe core bound to the hole in the CdTe crown), and CdTe crown-localized XCdTe and CdSe core-localized XCdSe 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- (XXCT XCdTe ) and four (XXCT XXCdTe ) 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.

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