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Manipulating nonlinear emission and cooperative effect of CdSe/ZnS quantum dots by coupling to a silver nanorod complex cavity.

Nan F, Cheng ZQ, Wang YL, Zhang Q, Zhou L, Yang ZJ, Zhong YT, Liang S, Xiong Q, Wang QQ - Sci Rep (2014)

Bottom Line: Power-dependent spectral shifting, narrowing, modulation, and amplification are demonstrated by adjusting longitudinal surface plasmon resonance of silver nanorods, reflectivity and phase shift of silver nanostructured film, and mode spacing of the complex cavity.The underlying physical mechanism of the nonlinear excitation energy transfer and nonlinear emissions are further investigated and discussed by using time-resolved photoluminescence and finite-difference time-domain numerical simulations.Our results suggest effective strategies to design active plasmonic complex cavities for cooperative emission nanodevices based on semiconductor quantum dots.

View Article: PubMed Central - PubMed

Affiliation: 1] Department of Physics, Wuhan University, Wuhan 430072, P. R. China [2].

ABSTRACT
Colloidal semiconductor quantum dots have three-dimensional confined excitons with large optical oscillator strength and gain. The surface plasmons of metallic nanostructures offer an efficient tool to enhance exciton-exciton coupling and excitation energy transfer at appropriate geometric arrangement. Here, we report plasmon-mediated cooperative emissions of approximately one monolayer of ensemble CdSe/ZnS quantum dots coupled with silver nanorod complex cavities at room temperature. Power-dependent spectral shifting, narrowing, modulation, and amplification are demonstrated by adjusting longitudinal surface plasmon resonance of silver nanorods, reflectivity and phase shift of silver nanostructured film, and mode spacing of the complex cavity. The underlying physical mechanism of the nonlinear excitation energy transfer and nonlinear emissions are further investigated and discussed by using time-resolved photoluminescence and finite-difference time-domain numerical simulations. Our results suggest effective strategies to design active plasmonic complex cavities for cooperative emission nanodevices based on semiconductor quantum dots.

No MeSH data available.


Related in: MedlinePlus

Power-dependent multi-mode and few-mode oscillations and amplifications of the SQD/AgNR:AAO/AgNF.(a) Power-dependent PL spectra with multi-mode oscillations (Δνcav ≈ 0.54ΔνQD,0,  ≈ 660 nm, and dAgNF = 10.3 nm). (b) Power-dependences of the normalized peak PL intensity of six cavity modes at the emission wavelengths of 555, 572, 588, 606, 626, and 647 nm. (c) Power-dependent emission spectra with two-mode oscillations (Δνcav ≈ 1.27ΔνSQD,0,  ≈ 610 nm, dAgNF = 10.3 nm). (d) Power dependences of the emission at 575 nm and 615 nm. (e) Differential normalized PL spectrum. The emissions around 575 nm are depressed and the emissions around 615 nm are amplified.
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f3: Power-dependent multi-mode and few-mode oscillations and amplifications of the SQD/AgNR:AAO/AgNF.(a) Power-dependent PL spectra with multi-mode oscillations (Δνcav ≈ 0.54ΔνQD,0, ≈ 660 nm, and dAgNF = 10.3 nm). (b) Power-dependences of the normalized peak PL intensity of six cavity modes at the emission wavelengths of 555, 572, 588, 606, 626, and 647 nm. (c) Power-dependent emission spectra with two-mode oscillations (Δνcav ≈ 1.27ΔνSQD,0, ≈ 610 nm, dAgNF = 10.3 nm). (d) Power dependences of the emission at 575 nm and 615 nm. (e) Differential normalized PL spectrum. The emissions around 575 nm are depressed and the emissions around 615 nm are amplified.

Mentions: The cavity-mode spacing Δνcav is adjusted to about 0.54ΔνSQD,0 to observe the coupling of ensemble SQDs with multi-mode of the cavity. The power-dependent PL spectra of multi-mode oscillations for the SQDs/AgNR:AAO/AgNF cavity (Δνcav = 0.54ΔνSQD,0, = 660 nm, dAgNF = 10.3 nm) is shown in Figure 3a. The energy-level structures of the broaden emission band of the individual SQDs without interaction and the multi-mode of the cavity are illustrated in the inset. One can clearly see multi-mode oscillations of the cavity from the PL spectra. Owing to large reflectivity of the AgNF, the PL spectra of the SQDs around 590 nm are highly modulated. The emissions around 500 nm from the AAO template itself are also modulated by the complex cavity itself. The spectral width (defined as the full width at half maximum) of the emission is directly extracted from the PL spectrum, which reaches as small as 11.5 nm (Figure S10a).


Manipulating nonlinear emission and cooperative effect of CdSe/ZnS quantum dots by coupling to a silver nanorod complex cavity.

Nan F, Cheng ZQ, Wang YL, Zhang Q, Zhou L, Yang ZJ, Zhong YT, Liang S, Xiong Q, Wang QQ - Sci Rep (2014)

Power-dependent multi-mode and few-mode oscillations and amplifications of the SQD/AgNR:AAO/AgNF.(a) Power-dependent PL spectra with multi-mode oscillations (Δνcav ≈ 0.54ΔνQD,0,  ≈ 660 nm, and dAgNF = 10.3 nm). (b) Power-dependences of the normalized peak PL intensity of six cavity modes at the emission wavelengths of 555, 572, 588, 606, 626, and 647 nm. (c) Power-dependent emission spectra with two-mode oscillations (Δνcav ≈ 1.27ΔνSQD,0,  ≈ 610 nm, dAgNF = 10.3 nm). (d) Power dependences of the emission at 575 nm and 615 nm. (e) Differential normalized PL spectrum. The emissions around 575 nm are depressed and the emissions around 615 nm are amplified.
© Copyright Policy - open-access
Related In: Results  -  Collection

License
Show All Figures
getmorefigures.php?uid=PMC4007083&req=5

f3: Power-dependent multi-mode and few-mode oscillations and amplifications of the SQD/AgNR:AAO/AgNF.(a) Power-dependent PL spectra with multi-mode oscillations (Δνcav ≈ 0.54ΔνQD,0, ≈ 660 nm, and dAgNF = 10.3 nm). (b) Power-dependences of the normalized peak PL intensity of six cavity modes at the emission wavelengths of 555, 572, 588, 606, 626, and 647 nm. (c) Power-dependent emission spectra with two-mode oscillations (Δνcav ≈ 1.27ΔνSQD,0, ≈ 610 nm, dAgNF = 10.3 nm). (d) Power dependences of the emission at 575 nm and 615 nm. (e) Differential normalized PL spectrum. The emissions around 575 nm are depressed and the emissions around 615 nm are amplified.
Mentions: The cavity-mode spacing Δνcav is adjusted to about 0.54ΔνSQD,0 to observe the coupling of ensemble SQDs with multi-mode of the cavity. The power-dependent PL spectra of multi-mode oscillations for the SQDs/AgNR:AAO/AgNF cavity (Δνcav = 0.54ΔνSQD,0, = 660 nm, dAgNF = 10.3 nm) is shown in Figure 3a. The energy-level structures of the broaden emission band of the individual SQDs without interaction and the multi-mode of the cavity are illustrated in the inset. One can clearly see multi-mode oscillations of the cavity from the PL spectra. Owing to large reflectivity of the AgNF, the PL spectra of the SQDs around 590 nm are highly modulated. The emissions around 500 nm from the AAO template itself are also modulated by the complex cavity itself. The spectral width (defined as the full width at half maximum) of the emission is directly extracted from the PL spectrum, which reaches as small as 11.5 nm (Figure S10a).

Bottom Line: Power-dependent spectral shifting, narrowing, modulation, and amplification are demonstrated by adjusting longitudinal surface plasmon resonance of silver nanorods, reflectivity and phase shift of silver nanostructured film, and mode spacing of the complex cavity.The underlying physical mechanism of the nonlinear excitation energy transfer and nonlinear emissions are further investigated and discussed by using time-resolved photoluminescence and finite-difference time-domain numerical simulations.Our results suggest effective strategies to design active plasmonic complex cavities for cooperative emission nanodevices based on semiconductor quantum dots.

View Article: PubMed Central - PubMed

Affiliation: 1] Department of Physics, Wuhan University, Wuhan 430072, P. R. China [2].

ABSTRACT
Colloidal semiconductor quantum dots have three-dimensional confined excitons with large optical oscillator strength and gain. The surface plasmons of metallic nanostructures offer an efficient tool to enhance exciton-exciton coupling and excitation energy transfer at appropriate geometric arrangement. Here, we report plasmon-mediated cooperative emissions of approximately one monolayer of ensemble CdSe/ZnS quantum dots coupled with silver nanorod complex cavities at room temperature. Power-dependent spectral shifting, narrowing, modulation, and amplification are demonstrated by adjusting longitudinal surface plasmon resonance of silver nanorods, reflectivity and phase shift of silver nanostructured film, and mode spacing of the complex cavity. The underlying physical mechanism of the nonlinear excitation energy transfer and nonlinear emissions are further investigated and discussed by using time-resolved photoluminescence and finite-difference time-domain numerical simulations. Our results suggest effective strategies to design active plasmonic complex cavities for cooperative emission nanodevices based on semiconductor quantum dots.

No MeSH data available.


Related in: MedlinePlus