期刊
NANO LETTERS
卷 18, 期 10, 页码 6248-6254出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.8b02361
关键词
Colloidal synthesis; 2D nanocrystals; halides; photoluminescence; k.p calculations
类别
资金
- MINECO [CTQ2017-83781-P]
- UJI [B2017-59]
- European Union's Horizon 2020 research and innovation program [696656 GrapheneCore1]
- European Research Council (ERC) [714876 PHOCONA]
Current colloidal synthesis methods for CdSe nanoplatelets (NPLs) routinely yield samples that emit, in discrete steps, from 460 to 550 nm. A significant challenge lies with obtaining thicker NPLs, to further widen the emission range. This is at present typically achieved via colloidal atomic layer deposition onto CdSe cores, or by synthesizing NPL core/shell structures. Here, we demonstrate a novel reaction scheme, where we start from 4.5 monolayer (ML) NPLs and increase the thickness in a two-step reaction that switches from 2D to 3D growth. The key feature is the enhancement of the growth rate of basal facets by the addition of CdCl2, resulting in a series of nearly monodisperse CdSe NPLs with thicknesses between 5.5 and 8.5 ML. Optical characterization yielded emission peaks from 554 nm up to 625 nm with a line width (fwhm) of 9-13 nm, making them one of the narrowest colloidal nanocrystal emitters currently available in this spectral range. The NPLs maintained a short emission lifetime of 5-11 ns. Finally, due to the increased red shift of the NPL band edge photoluminescence excitation spectra revealed several high-energy peaks. Calculation of the NPL band structure allowed us to identify these excited-state transitions, and spectral shifts are consistent with a significant mixing of light and split-off hole states. Clearly, chloride ions can add a new degree of freedom to the growth of 2D colloidal nanocrystals, yielding new insights into both the NPL synthesis as well as their optoelectronic properties.
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