Real-time observation of ultrafast Rabi oscillations between excitons and plasmons in metal nanostructures with J-aggregates

Vasa, Parinda; Wang, Wei; Pomraenke, R.; Lammers, Melanie; Maiuri, Margherita; Manzoni, Cristian; Cerullo, Giulio; Lienau, Christoph

doi:10.1038/nphoton.2012.340

Cited by 398 publications

(495 citation statements)

References 32 publications

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“…PACS numbers: 05.60. Gg, 42.50.Pq, 74.40.Gh, The study of strong light-matter interactions [1][2][3][4] is playing an increasingly crucial role in understanding as well as engineering new states of matter with relevance to the fields of quantum optics [5][6][7][8][9][10][11][12][13][14][15][16][17][18], solid state physics [19][20][21][22][23][24][25][26][27][28][29][30][31], as well as quantum chemistry [32][33][34][35][36] and material science [37][38][39][40][41][42][43][44][45][46][47][48][49][...…”

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confidence: 99%

Cavity-Enhanced Transport of Charge

et al. 2017

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We theoretically investigate charge transport through electronic bands of a mesoscopic onedimensional system, where inter-band transitions are coupled to a confined cavity mode, initially prepared close to its vacuum. This coupling leads to light-matter hybridization where the dressed fermionic bands interact via absorption and emission of dressed cavity-photons. Using a selfconsistent non-equilibrium Green's function method, we compute electronic transmissions and cavity photon spectra and demonstrate how light-matter coupling can lead to an enhancement of charge conductivity in the steady-state. We find that depending on cavity loss rate, electronic bandwidth, and coupling strength, the dynamics involves either an individual or a collective response of Bloch states, and explain how this affects the current enhancement. We show that the charge conductivity enhancement can reach orders of magnitudes under experimentally relevant conditions. PACS numbers: 05.60. Gg, 42.50.Pq, 74.40.Gh, The study of strong light-matter interactions [1][2][3][4] is playing an increasingly crucial role in understanding as well as engineering new states of matter with relevance to the fields of quantum optics [5][6][7][8][9][10][11][12][13][14][15][16][17][18], solid state physics [19][20][21][22][23][24][25][26][27][28][29][30][31], as well as quantum chemistry [32][33][34][35][36] and material science [37][38][39][40][41][42][43][44][45][46][47][48][49][50][51][52][53]. An emerging topic of interest is the modification of material properties using either external electro-magnetic radiation [54][55][56] or spatially confined modes such as in cavity quantum electrodynamics [57][58][59][60][61][62][63]. Recent experiments with organic semiconductors have demonstrated a dramatic enhancement of charge conductivity when molecules interact strongly with a surface plasmon mode [64]. In principle, this can open up exciting new opportunities both for basic science and applications of organic electronics [65]. The microscopic mechanisms leading to charge conductivity enhancement, however, remain today largely unexplained. In this work, we propose a proof-of-principle model that sheds light on the physical mechanisms behind current enhancement due to the interaction with a confined bosonic mode. We show that our model can lead to a dramatic current enhancement by orders of magnitude for certain conditions that can be relevant to typical experiments across fields.The setup we consider [see Fig. 1(a)] consists of a mesoscopic chain of N sites with two orbitals of energy ω 1 and ω 2 ( = 1) in a 1D geometry, forming two bands in a tight-binding picture. The edges of the chain are connected to a source and a drain with a bias voltage across, respectively inserting and removing (spin-less) electrons in the two orbitals at rates Γ 1 and Γ 2 . The on-site interband transitions with energy ω 21 = ω 2 −ω 1 are resonantly coupled to a cavity mode with coupling strength g and loss rate κ. Initially, we only allow electrons in the upper band to hop with a ...

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Cavity-Enhanced Transport of Charge

et al. 2017

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“…Recently, delocalized electromagnetic modes supported by metal surfaces (surface plasmon polaritons) or periodic arrays of metallic nanoparticles [surface lattice resonances (SLRs) [8][9][10][11]] have been shown to strongly couple with localized emitters [12][13][14][15][16][17][18][19]. The strong coupling in these plasmonic systems involves a large number N of emitters.…”

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Spatial Coherence Properties of Organic Molecules Coupled to Plasmonic Surface Lattice Resonances in the Weak and Strong Coupling Regimes

et al. 2014

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We study spatial coherence properties of a system composed of periodic silver nanoparticle arrays covered with a fluorescent organic molecule (DiD) film. The evolution of spatial coherence of this composite structure from the weak to the strong coupling regime is investigated by systematically varying the coupling strength between the localized DiD excitons and the collective, delocalized modes of the nanoparticle array known as surface lattice resonances. A gradual evolution of coherence from the weak to the strong coupling regime is observed, with the strong coupling features clearly visible in interference fringes. A high degree of spatial coherence is demonstrated in the strong coupling regime, even when the mode is very excitonlike (80 %), in contrast to the purely localized nature of molecular excitons. We show that coherence appears in proportion to the weight of the plasmonic component of the mode throughout the weak-to-strong coupling crossover, providing evidence for the hybrid nature of the normal modes.

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“…kinetics) has been suggested based on several earlier experiments where bulk properties were modified by strong coupling, such as the work-function and the ground-state energy (Vasa et al, 2013). However, changing the energy landscape and energy transfer pathways via strong coupling remains a challenge.…”

Section: Controlling and Probing Molecular Energy Transfer Pathways Vmentioning

confidence: 99%

Quantum Information and Computation for Chemistry

Kais

2014

Advances in Chemical Physics

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Real-time observation of ultrafast Rabi oscillations between excitons and plasmons in metal nanostructures with J-aggregates

Cited by 398 publications

References 32 publications

Cavity-Enhanced Transport of Charge

Cavity-Enhanced Transport of Charge

Spatial Coherence Properties of Organic Molecules Coupled to Plasmonic Surface Lattice Resonances in the Weak and Strong Coupling Regimes

Quantum Information and Computation for Chemistry

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