期刊
NANO LETTERS
卷 14, 期 12, 页码 6799-6810出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl502237f
关键词
Chiral assemblies; supraparticles; nanoscale chirality; hybrid electronic states; polarization rotation; circular dichroism
类别
资金
- Center for Photonic and Multiscale Nanomaterials (C-PHOM) - National Science Foundation Materials Research Science and Engineering Center program [DMR 1120923]
- National Science Foundation [CHE-1252322]
- Center for Solar and Thermal Energy Conversion, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0000957]
- NSF [DMR-0315633]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1252322] Funding Source: National Science Foundation
- Directorate For Engineering [1403777] Funding Source: National Science Foundation
- Div Of Chem, Bioeng, Env, & Transp Sys [1403777] Funding Source: National Science Foundation
Chiral nanostructures exhibit strong coupling to the spin angular momentum of incident photons. The integration of metal nanostructures with semiconductor nanoparticles (NPs) to form hybrid plasmonexciton nanoscale assemblies can potentially lead to plasmon-induced optical activity and unusual chiroptical properties of plasmonexciton states. Here we investigate such effects in supraparticles (SPs) spontaneously formed from gold nanorods (NRs) and chiral CdTe NPs. The geometry of this new type of self-limited nanoscale superstructures depends on the molar ratio between NRs and NPs. NR dimers surrounded by CdTe NPs were obtained for the ratio NR/NP = 1:15, whereas increasing the NP content to a ratio of NR/NP = 1:180 leads to single NRs in a shell of NPs. The SPs based on NR dimers exhibit strong optical rotatory activity associated in large part with their twisted scissor-like geometry. The preference for a specific nanoscale enantiomer is attributed to the chiral interactions between CdTe NP in the shell. The SPs based on single NRs also yield surprising chiroptical activity at the frequency of the longitudinal mode of NRs. Numerical simulations reveal that the origin of this chiroptical band is the cross talk between the longitudinal and the transverse plasmon modes, which makes both of them coupled with the NP excitonic state. The chiral SP NRNP assemblies combine the optical properties of excitons and plasmons that are essential for chiral sensing, chiroptical memory, and chiral catalysis.
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