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Wang Wei, Zhang Hong. Strong coupling and ultrafast dynamics in organic semiconductor/metal hybrid nanostructures[J]. Opto-Electronic Engineering, 2017, 44(2): 161-171. doi: 10.3969/j.issn.1003-501X.2017.02.004
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Strong coupling and ultrafast dynamics in organic semiconductor/metal hybrid nanostructures
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Abstract
Active plasmonics, as an important branch of Plasmonics, is growing rapidly over the last decades. The main principle of active plasmonics is to combine surface plasmon polaritons (SPPs) with 'active' materials to compenstate intrinsic weak optical nonlinearities and short propagation lengths of SPPs, so that external manipulation and coherent control of SPPs can be realized. Here, we give a brief review of the studies in the area of active plasmonics. In particular, we focus on hybrid J-aggregate/metal nanostructures consisting of J-aggregate excitons and surface plasmon polaritons supported by metallic nanostructures. Two experimental methods: chrip-compensated spectral interferometry and nonlinear pump-probe spectroscopy are introduced. The strong coupling between J-aggregate excitons and SPPs is studied in detail by probing both the static optical properties and ultrasfast dynamics of the strongly coupled X-SPP systems. The results reveal that two different energy transfer channels: a coherent resonant dipole-dipole interaction and an incoherent exchange of photons, are coexisting in the hybrid system. Coherent energy exchange, that is, Rabi oscillations between the excitonic and the SPP systems in real time are also investigated. It is found that coherent X-SPP population transfer induces transient oscillations in exciton density, leading to a periodic modulation of the normal mode splitting and thus optical nonlinearity on a 10 fs timescale. -
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References
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Overview
Abstract: Metallic nanostructures can support the strongly confined interface waves: surface plasmon polaritons (SPPs). SPPs have recently been used in a variety of applications due to their abilities to guide light in the scale of nanometer. Whereas, intrinsic weak optical nonlinearities and short propagation lengths of SPPs hinder their applications in novel active plasmonic devices.
One promising solution 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. In these systems, vacuum field fluctuations lead to a coherent exchange of energy between ensembles of excitons and plasmons and the formation of new hybrid polariton states. 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 give a brief review of our studies in the area of active plasmonics. We focus on hybrid J-aggregate/metal nanostructures consisting of J-aggregate excitons and surface plasmon polaritons supported by metallic nanogroove arrays. We first introduce two experimental methods used in our study: chrip-compensated spectral interferometry and nonlinear pump-probe spectroscopy. The strong coupling between J-aggregate excitons and SPPs is studied in detail by probing both the static optical properties and ultrafast dynamics of the strongly coupled X-SPP systems. We show that two different energy transfer channels: a coherent resonant dipole-dipole interaction and an incoherent exchange of photons, are coexisting in the hybrid system. The interplay between both pathways results in a pronounced modification of the radiative damping due to the formation of super- and subradiant polariton states.
We also investigate the coherent energy exchange, Rabi oscillations between the excitonic and the SPP systems in real time. Using nonlinear pump-probe spectroscopy, coherent polariton dynamics of the hybrid X-SPP systems is studied. It is found that the optical response of the individual resonances is drastically altered by the optical dipole coupling between excitons and SPPs. Coherent X-SPP population transfer induces transient oscillations in exciton density, leading to a periodic modulation of the normal mode splitting and thus optical nonlinearity in a 10 fs timescale.
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Wang Wei, Zhang Hong. Strong coupling and ultrafast dynamics in organic semiconductor/metal hybrid nanostructures[J]. Opto-Electronic Engineering, 2017, 44(2): 161-171. doi: 10.3969/j.issn.1003-501X.2017.02.004
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Figure 1.
(a1) Schematic of the metal-semiconductor hybrid structure consisting of a gold nanoslit grating deposited on a GaAs QW. (a2) Calculated angle-resolved far-field reflectivity spectra of this structure. Dispersion relations for different AM and SM SPP resonances are indicated as dashdotted lines. (b1) Normal incidence absorption spectrum of a CdSe film, ~25 nm in thickness spin coated onto a glass slide. (b2) Reflectivity spectra plotted as a function of the angle of incidence external to the prism (right). Reproduced with permission from Ref. [25-26].
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Figure 2.
(a) Molecular structure of J-aggregated dye. (b) Absorption spectra of monomer molecules (blue) and their corresponding J-aggregate form (red) measured at room temperature. (c) Schematic of gold groove array deposited on glass substrate and (d) the hybrid nanostructure consisting of J-aggregate dye film spin-coated on the gold groove array.
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Figure 3.
(a) Principle of spectral interferometry setup. The broadband laser pulses are split by the first beam splitter (BS1) and sent through the two arms of a Mach-Zehnder interferometer. The one passing through the sample are modulated by its complex response function. The other beam is the undisturbed delayed reference beam with respect to the sample arm. The two beams are then combined after the second beam splitter (BS2) and sent to the detector where the interfering field intensity is recorded. (b) Schematic of angle-resolved spectral interferometry setup.
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Figure 4.
Schematic of a generic setup for pump-probe measurements. An ultrafast laser is split into pump and probe beams. They are both sent to the sample with the probe delayed by a time of τ. The signal of the probe beam is recorded by a detector as a function of delay to monitor the real-time dynamics of the sample.
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Figure 5.
Angle-resolved pump probe setup. The sample is mounted inside a cryostat, which can provide vacuum environment and is cooled with liquid nitrogen or helium. A 6-fs pulse is first compressed using chirped mirrors, a prism compressor and a pulse shaper (not shown) before split into pump and probe. A delay stage is used to delay the probe beam relative to the pump beam. Both beams are modulated using AOMs at different frequencies. The pump beam can be spectrally narrowed by using a short-pass filter. Computer controlled angle tuning platform is used for excitation and detection angle.
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Figure 6.
(a) Schematic of a strongly coupled X-SPP system. The excitonic system is modeled as a three-level system consisting of a ground state, a single exciton state |X〉 and a biexciton state |XX〉. The plasmon system is represented as a photonic mode |P〉. The continuum of vacuum states is denoted as |V〉. The solid arrows denote the incoherent X-SPP coupling through vacuum field. (b) Spectral widths of the UP/LP modes obtained from experiment (circles) and oscillator model (solid lines). (c) Calculated population damping (solid) and pure dephasing (dash-dot) of the UP (blue) and LP (red). Results are taken from Ref. [17].
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Figure 7.
Time-resolved differential reflectivity signal (∆R/R) (a) for UP and LP mode (b) for resonant excitation. (c) ∆R/R dynamics (logarithmic scale) at the X resonance of the bare dye film, and near the LP (1.74 eV) and UP (1.84 eV) resonances of the hybrid structure. (d) Measured polariton population damping term as a function of detuning angle (circles) compared to predictions of the coupled oscillator model (solid). Dashed lines denote the results in the absence of incoherent photon exchange. Green: damping rates of uncoupled X and SPP modes. Results are taken from Ref. [17].
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Figure 8.
Coherent dynamics of X-SPP Rabi oscillations. (a) Measured differential reflectivity map (ΔR/R)(ωpr, τ) for a hybrid structure with p=430 nm, recorded using two nearly collinearly propagating 15 fs pulses with time delay τ at an incidence angle of θ=39°. (b) Comparison between measured (solid line) and simulated (dashed line) differntial spectra. (c) Time evolution of the ΔR/R signal near the LP resonance measured at two different angles. (d), (e) Simulated (ΔR/R)(ωpr, τ) map (d) and pump-induced SPP and exciton population dynamics atθ=39°(e). (f) Comparison between observed (open symbols) and calculated (solid lines, error bars taken as standard deviation of Fouriertransformed ΔR (ωpr, τ) traces) oscillation periods and LP resonance energies. Results are taken from Ref. [39].
