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Wang Wei, Sommer Ephraim, De Sio Antonietta, et al. Field‐level characterization of strong coupling between excitons and surface plasmon polaritons in J‐aggregate/metal hybrid nanostructures[J]. Opto-Electronic Engineering, 2017, 44(2): 202-208. doi: 10.3969/j.issn.1003-501X.2017.02.009
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Field‐level characterization of strong coupling between excitons and surface plasmon polaritons in J‐aggregate/metal hybrid nanostructures
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Abstract
White-light broadband chirp-compensated spectral interferometry is applied to fully probe the optical response of strongly coupled excitons (Xs) and surface plasmon polaritons (SPPs) in J-aggregate/metal hybrid nanostructures at field level. Under impulsive excitation, amplitude and spectral phase of the sample reflectivity are measured with high precision and the time structure of the electric field emitted by the hybrid modes of the nanostructures is accurately reconstructed. Quantitative description of strong X-SPP coupling is precisely obtained by fitting both measured spectra and phases simultaneously to a Fano lineshape model.
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References
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Overview
Abstract: Metallic nanostructures have highly interesting optical properties. When illuminating light on them, surface plasmon polaritons (SPP) can be induced due to the coupling of the electromagnetic fields to collective charge density oscillations near the metal surface. SPPs have recently been used in a variety of new applications due to their abilities to guide light on the scale of nanometer. However, most of these emerging applications are limited by the ultrashort lifetime of SPP and the corresponding short propagation length caused by the strong ohmic loss of metal and radiative damping within the nanostructures. Moreover, SPP is generally a photon-like optical excitation showing intrinsically weak nonlinearities, which hinders active nanoplasmonic device fabrication, such as all-optical switching or information processing.
A promising way to compensate losses and provide missing nonlinearity of SPPs is to couple SPPs to nonlinear optical resonances, such as excitons (Xs) in molecular or semiconducting nanostructures. Consequently, hybrid nanostructures containing J-aggregate molecules and metallic nanostructures have attracted considerable interest. Strong coupling between Xs and SPPs enables an efficient transfer of the strong optical nonlinearities of the excitonic emitters to the passive plasmonic nanostructures on the ultrashort time scale of femtosecond.
Here, we demonstrate a field-level characterization of the optical response of J-aggregate/metal hybrid nanostructures by white-light broadband chirp-compensated spectral interferometry. We show that both the amplitude and spectral phase of the strongly coupled X-SPP system can be measured with high precision by compensating the chirp in both arms of the interferometer. A quantitative description of both the excitonic resonance and the hybrid X-SPP polariton response is obtained by fitting the measured amplitudes and spectral phases simultaneously to a Fano lineshape model. We find that the resonance of the majority of J-aggregated molecules which are not coupled to SPPs is homogeneously broadened. We also demonstrate accurate reconstruction of the time structure of the electric field emitted by the hybrid nanostructures, corresponding to polarization oscillations with short damping time shorter than 100 fs.
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Wang Wei, Sommer Ephraim, De Sio Antonietta, et al. Field‐level characterization of strong coupling between excitons and surface plasmon polaritons in J‐aggregate/metal hybrid nanostructures[J]. Opto-Electronic Engineering, 2017, 44(2): 202-208. doi: 10.3969/j.issn.1003-501X.2017.02.009
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Figure 1.
(a) Schematic of the hybrid nanostructure consisting of a gold nanogroove array with groove period p0=430 nm, depth h0=25 nm and width w0=50 nm, coated with a 50-nm-thick J-aggregate dye film. (b) SEM picture of the uncoated groove array written on a gold film by focus ion beam (FIB).
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Figure 2.
Angle-resolved spectral interferometry setup (BS: beam splitter, τ: variable delay, w: wedge pair).
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Figure 3.
Angle-resolved reflectivity spectra Rx(ω, θ). (a, b) and spectral phase φx(ω, θ). (c, d) of J-aggregate dye coated on planar gold film obtained from SI measurement (a, c) and the fitting (b, d) to Lorentzian oscillator model. The dashed lines mark the dye absorption at around 1.8 eV in (a, b) and the corresponding phase jump in (c, d). (e) Observed (red circles) and fitted (solid black) reflectivity spectra Rx(w), and the corresponding observed (blue circles) and fitted (solid blue) spectral phase φx(ω), measured at the incidence angle of 21°. (f) The corresponding observed normalized reflection coefficient plotted in complex plane (red circles). The solid black curve is the result fitted to a circular function.
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Figure 4.
Observed (a) and modeled (b) angle-resolved reflectivity spectra, R0(ω, θ) and corresponding observed (c) and modeled (d) spectral phase, φ(ω, θ). The black (white) lines mark the coupled (uncoupled) mode dispersions.
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Figure 5.
(a) Experimental (circles) and simulated (solid lines) reflectivity spectra and spectral phases at θ=31°. (b) Time structure of the electric field emitted by the hybrid UP and LP modes at θ=31°, showing distinct polarization beats with frequency ωUP-ωLP.
