期刊
NANO LETTERS
卷 19, 期 7, 页码 4297-4305出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b00681
关键词
semiconductor nanocrystals; nanoplatelets; liquid-air interface self-assembly; stacking; energy transfer; dipole orientation
类别
资金
- Singapore National Research Foundation [NRF-NRFI2016-08]
- TUBITAK [115E679]
- TUBA
- TUBITAK through BIDEB program
We proposed and showed strongly orientation-controlled Forster resonance energy transfer (FRET) to highly anisotropic CdSe nanoplatelets (NPLs). For this purpose, we developed a liquidair interface self-assembly technique specific to depositing a complete monolayer of NPLs only in a single desired orientation, either fully stacked (edge-up) or fully nonstacked (face-down), with near-unity surface coverage and across large areas over 20 cm(2). These NPL monolayers were employed as acceptors in an energy transfer working model system to pair with CdZnS/ZnS core/shell quantum dots (QDs) as donors. We found the resulting energy transfer from the QDs to be significantly accelerated (by up to 50%) to the edge-up NPL monolayer compared to the face-down one. We revealed that this acceleration of FRET is accounted for by the enhancement of the dipoledipole interaction factor between a QD-NPL pair (increased from 1/3 to 5/6) as well as the closer packing of NPLs with stacking. Also systematically studying the distance-dependence of FRET between QDs and NPL monolayers via varying their separation (d) with a dielectric spacer, we found out that the FRET rate scales with d(-4) regardless of the specific NPL orientation. Our FRET model, which is based on the original Forster theory, computes the FRET efficiencies in excellent agreement with our experimental results and explains well the enhancement of FRET to NPLs with stacking. These findings indicate that the geometrical orientation of NPLs and thereby their dipole interaction strength can be exploited as an additional degree of freedom to control and tune the energy transfer rate.
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