Approaching the strong coupling limit in single plasmonic nanorods interacting with J-aggregates

Zengin, Gülis; Johansson, Göran; Johansson, Peter; Antosiewicz, Tomasz J.; Käll, Mikael; Shegai, Timur

doi:10.1038/srep03074

Cited by 249 publications

(319 citation statements)

References 46 publications

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“…1 a general description of the problem, using Mie theory to model the optical response of silver colloids, and a standard isotropic effective medium [22,25,27,30,31,33,35,36] for the thin coating layer arXiv:1509.07216v1 [physics.optics]…”

Section: Predictions From Electromagnetic Theorymentioning

confidence: 99%

“…Many of these existing and emerging applications are underpinned by the fact that the optical (electronic) absorption of molecules on the surface of metallic NPs is enhanced. But spectral changes induced by molecular adsorption are often ignored because of the experimental challenge of measuring surface absorbance spectra on nanoparticles, despite early attempts more than 30 years ago [21].This question is not directly addressed in the great number of recent studies devoted to the topic of strongcoupling between plasmons and molecules [22][23][24][25][26][27][28][29][30][31][32][33][34][35][36]; in this regime, the plasmon-molecule interaction is evidenced by a typical anti-crossing of the two resonances as a function of detuning [25,33], but in such a strongly interacting system the molecular response cannot be isolated. Moreover, in such studies the dye concentration is often large (typically monolayer coverage and above) to maximize dye/plasmon interactions.…”

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confidence: 99%

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Modified optical absorption of molecules on metallic nanoparticles at sub-monolayer coverage

Darby¹,

Auguié²,

Meyer³

et al. 2015

Nature Photon

139

192

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Enhanced optical absorption of molecules in the vicinity of metallic nanostructures is key to a number of surface-enhanced spectroscopies and of great general interest to the fields of plasmonics and nano-optics. Yet, experimental access to this absorbance has long proven elusive. We here present direct measurements of the intrinsic absorbance of dye-molecules adsorbed onto silver nanospheres, and crucially, at sub-monolayer concentrations where dye-dye interactions become negligible. With a large detuning from the plasmon resonance, distinct shifts and broadening of the molecular resonances reveal the intrinsic properties of the dye in contact with the metal colloid, in contrast to the often studied strong-coupling regime where the optical properties of the dye-molecules cannot be isolated. The observation of these shifts together with the ability to routinely measure them has broad implications in the interpretation of experiments involving resonant molecules on metallic surfaces, such as surface-enhanced spectroscopies and many aspects of molecular plasmonics.Over the last two decades, the optical properties of metallic nanoparticles (NPs) of various sizes and shapes [1] [18][19][20]. Many of these existing and emerging applications are underpinned by the fact that the optical (electronic) absorption of molecules on the surface of metallic NPs is enhanced. But spectral changes induced by molecular adsorption are often ignored because of the experimental challenge of measuring surface absorbance spectra on nanoparticles, despite early attempts more than 30 years ago [21].This question is not directly addressed in the great number of recent studies devoted to the topic of strongcoupling between plasmons and molecules [22][23][24][25][26][27][28][29][30][31][32][33][34][35][36]; in this regime, the plasmon-molecule interaction is evidenced by a typical anti-crossing of the two resonances as a function of detuning [25,33], but in such a strongly interacting system the molecular response cannot be isolated. Moreover, in such studies the dye concentration is often large (typically monolayer coverage and above) to maximize dye/plasmon interactions. Dye-dye interactions cannot therefore be neglected and are expected to induce resonance shifts of the dye layer independently of any plas- * Eric.LeRu@vuw.ac.nz monic effects; in fact many studies specifically work with J-aggregates rather than isolated dyes [22, 25-27, 31, 33]. As a result, the intrinsic effect (chemical and/or electromagnetic) of the NP on an isolated adsorbed molecule cannot be elucidated. To this aim, we will show that it is necessary to measure the absorbance of the dye when the dye and plasmon resonances are detuned (to avoid dye-plasmon interaction effects) and at low surface coverage (to avoid dye-dye interaction effects). This low surface coverage poses a significant experimental challenge because the dye absorbance is then very small and obscured by the large optical response (absorption and scattering) of the NPs.We here propose to measure NP/d...

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Section: Predictions From Electromagnetic Theorymentioning

confidence: 99%

mentioning

confidence: 99%

Modified optical absorption of molecules on metallic nanoparticles at sub-monolayer coverage

Darby¹,

Auguié²,

Meyer³

et al. 2015

Nature Photon

139

192

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“…In a strong exciton-plasmon coupling regime, a coherent coupling between LSPs and excitons overwhelms all losses and results in two new mixed states of light. Hence, matter is separated energetically by a Rabi splitting that exhibits a characteristic anticrossing behavior of the exciton-LSP energy tuning [32][33][34]. In this regime, a new quasi-particle (plexciton) forms with distinct properties possessed by neither original particle.…”

Section: Introductionmentioning

confidence: 99%

Exciton-plasmon coupling interactions: from principle to applications

et al. 2017

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Abstract:The interaction of exciton-plasmon coupling and the conversion of exciton-plasmon-photon have been widely investigated experimentally and theoretically. In this review, we introduce the exciton-plasmon interaction from basic principle to applications. There are two kinds of exciton-plasmon coupling, which demonstrate different optical properties. The strong exciton-plasmon coupling results in two new mixed states of light and matter separated energetically by a Rabi splitting that exhibits a characteristic anticrossing behavior of the exciton-LSP energy tuning. Compared to strong coupling, such as surface-enhanced Raman scattering, surface plasmon (SP)-enhanced absorption, enhanced fluorescence, or fluorescence quenching, there is no perturbation between wave functions; the interaction here is called the weak coupling. SP resonance (SPR) arises from the collective oscillation induced by the electromagnetic field of light and can be used for investigating the interaction between light and matter beyond the diffraction limit. The study on the interaction between SPR and exaction has drawn wide attention since its discovery not only due to its contribution in deepening and broadening the understanding of SPR but also its contribution to its application in light-emitting diodes, solar cells, low threshold laser, biomedical detection, quantum information processing, and so on.

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“…Recently several groups have moved to a much smaller scale, investigating strong interaction of molecular excitons with individual plasmonic resonators, such as metallic nanospheres [27,28], nanorods [29][30][31], nanoprisms [15] and nanodisk dimers [13]. This greatly enlarges the freedom to observe and control the strong coupling process at the nanoscale, significantly deepening our understanding of relevant phenomena.…”

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confidence: 99%

Mode Modification of Plasmonic Gap Resonances Induced by Strong Coupling with Molecular Excitons

Chen

Qin

et al. 2017

Nano Lett.

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Plasmonic cavities can be used to control the atom-photon coupling process at the nanoscale, since they provide ultrahigh density of optical states in an exceptionally small mode volume. Here we demonstrate strong coupling between molecular excitons and plasmonic resonances (so-called plexcitonic coupling) in a film-coupled nanocube cavity, which can induce profound and significant spectral and spatial modifications to the plasmonic gap modes. Within the spectral span of a single gap mode in the nanotube-film cavity with a 3-nm wide gap, the introduction of narrow-band J-aggregate dye molecules not only enables an anti-crossing behavior in the spectral response, but also splits the single spatial mode into two distinct modes that are easily identified by their far-field scattering profiles. Simulation results confirm the experimental findings and the sensitivity of the plexcitonic coupling is explored using digital control of the gap spacing. Our work opens up a new perspective to study the strong coupling process, greatly extending the functionality of nanophotonic systems, with the potential to be applied in cavity quantum electrodynamic systems. † These authors contributed equally to this work 2 Strong light-matter interactions build upon fast energy exchange [1] between excitonic quantum emitters and electromagnetic (EM) modes in a cavity, which leads to cavity-exciton mode hybridization, manifesting as a split in the cavity spectral response, known as vacuum Rabi splitting.Understanding these phenomena is very important for cavity quantum electrodynamics applications [2,3]; for example, quantum computing requires repeated manipulation of excitonic states with photons before atomic or molecular excitons lose their coherence. On the other hand, once strongly coupled to a resonant cavity, electronic states of molecules can be greatly reshaped [4] from those in free space, enabling a variety of extraordinary effects, such as modification of molecular thermodynamics [5] and chemical landscape [6], mediation of energy transfer between multiple molecules [7] and even alternation of photosynthetic processes in bacteria [8].Strong coupling (SC) requires a high atomic cooperativity (, where g is the coupling strength, γ and κ are the spectral width of the excitonic transition of emitters and EM modes respectively. To achieve high C, traditional investigations [9][10][11][12] have used cavities with high Q performance (quality factor κ ω / = Q , where ω is the oscillation frequency of the cavity).Another solution is to reduce the cavity mode volume V, sincewhere N is the number of excitons contributing to the coupling process. In this context, plasmonic cavities have been proposed to investigate strong coupling, because these cavities can concentrate light energy within deep subwavelength volumes, and thus are capable of providing high cooperativity by compensating their moderate Q values with ultra-small V [13][14][15]. Specifically, plasmonic cavities are specially designed metallic nanostructures, in w...

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Approaching the strong coupling limit in single plasmonic nanorods interacting with J-aggregates

Cited by 249 publications

References 46 publications

Modified optical absorption of molecules on metallic nanoparticles at sub-monolayer coverage

Modified optical absorption of molecules on metallic nanoparticles at sub-monolayer coverage

Exciton-plasmon coupling interactions: from principle to applications

Mode Modification of Plasmonic Gap Resonances Induced by Strong Coupling with Molecular Excitons

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