Probing ultrafast energy transfer between excitons and plasmons in the ultrastrong coupling regime

Balci, Sinan; Kocabaş, Coşkun; Küçüköz, Betül; Karatay, Ahmet; Akhüseyin, Elif; Yağlıoğlu, H. Gül; Elmalı, Ayhan

doi:10.1063/1.4892360

Cited by 31 publications

(52 citation statements)

References 33 publications

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“…22,[26][27][28][29][30] It has been demonstrated that the lifetime of the upper hybrid band in exciton-SPPs systems can be much longer than the life of the bare excited molecules. It was suggested that this result can be caused by a trap state observed in the upper band 26,28 or by the block of the vibrational relaxation modes due to the large Rabi splitting. [31][32][33][34] In this work, we report a comprehensive spectroscopic study of a prototypical SPPs-molecule hybrid structure consisting of a gold naonholes array coated with different construction of J-aggregate molecules.…”

Section: Introductionmentioning

confidence: 99%

The role of Rabi splitting tuning in the dynamics of strongly coupled J-aggregates and surface plasmon polaritons in nanohole arrays

et al. 2016

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We have investigated the influence of Rabi splitting tuning on the dynamics of strongly coupled J-aggregate/surface plasmon polariton systems. In particular, the Rabi splitting was tuned by modifying the J-aggregate molecule concentration while a polaritonic system was provided by a nanostructure formed by holes array in a golden layer. From the periodic and concentration changes we have identified, through numerical and experimental steady-state analyses, the best geometrical configuration for maximizing Rabi splitting, which was then used for transient absorption measurements. It was found that in transient absorption spectra, under upper band excitation, two bleaching peaks appear when a nanostructured polaritonic pattern is used. Importantly, their reciprocal distance increases upon increase of J-aggregate concentration, a result confirmed by steady-state analysis. In a similar manner it was also found that the lifetime of the upper band is intimately related to the coupling strength. In particular, we argue that with strong coupling strength, i.e. high J-aggregate concentration, a short lifetime of the upper band has to be expected due to the suppression of the bottleneck effect. This result supports the idea that the dynamics of hybrid systems is profoundly dependent on Rabi splitting.

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Section: Introductionmentioning

confidence: 99%

The role of Rabi splitting tuning in the dynamics of strongly coupled J-aggregates and surface plasmon polaritons in nanohole arrays

et al. 2016

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“…Transient absorption measurements were performed with a femtosecond pump−probe method utilizing a Ti:sapphire laser amplifier-optical parametric amplifier system (Spectra Physics) with a 50 fs pulse duration and 1 kHz repetition rate. 33 A commercial pump−probe experimental setup with a white light continuum probe beam (Spectra Physics) was used. Experiments were performed in transmission geometry at 40 μJ/cm 2 pump fluencies with 100 fs pulse duration.…”

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confidence: 99%

Tunable Plexcitonic Nanoparticles: A Model System for Studying Plasmon–Exciton Interaction from the Weak to the Ultrastrong Coupling Regime

et al. 2016

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Controlling the number of dye molecules on metallic nanoparticles, which in turn affects the magnitude of Rabi splitting energy, is crucial for obtaining hybrid metal core−organic shell nanoparticles with tunable optical properties in the visible spectrum since the magnitude of the Rabi splitting energy directly determines the strength of the coupling between plasmonic nanoparticles and dye molecules. In this work, we present a new method for the synthesis of plexcitonic nanoparticles, and thus we are able to control the number of dye molecules self-assembled on Ag nanoprisms (Ag NPs) by adjusting the concentration of dye molecules used in the synthesis. Indeed, individual dye molecules self-assemble into J-aggregates on Ag NPs. Thus, in the finite-element simulations and experimental data of the hybrid metal organic nanoparticles, we observed a transition from weak coupling to the ultrastrong coupling regime. Besides, ultrafast energy transfer between plasmonic nanoparticles and excitonic aggregated dye molecules has been extensively studied as a function of Rabi splitting energy. We observe that the lifetime of the polariton states increases with the coupling strength and the upper polaritons are short-lived, whereas the lower polaritons are long-lived. Hybrid metal−organic nanoparticles presented in this study (i) have tunable Rabi splitting energies, (ii) are easy to prepare in large quantities in aqueous medium, (iii) can be uniformly assembled on solid substrates, (iv) have resonance frequencies in the visible spectrum, and (v) have small mode volume, thus making them an excellent model system for studying light−matter interaction at nanoscale dimensions from the weak to ultrastrong coupling regime.

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“…In fact, the Ag triangular nanoplate (TNP), which can highly confine electric fields around its sharp tips (23,24), exhibits large electric field enhancements and good optical non-linearity (25,26). Therefore, many significant works have been done based on them (27)(28)(29)(30)(31).…”

Section: Introductionmentioning

confidence: 99%

Surface plasmon-enhanced third-order optical non-linearity of silver triangular nanoplate

Kong

Zhan

et al. 2016

Journal of Modern Optics

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2016):Surface plasmon-enhanced third-order optical non-linearity of silver triangular nanoplate, Journal of Modern Optics, ABSTRACT We have obtained Ag triangular nanoplates with plasmon resonance bands locating from 750 to 950 nm by wet chemical method. The third-order optical non-linear response property of Ag triangular nanoplate is investigated using z-scan technique. The incident wavelength dependence of χ (3) (the third-order susceptibility) shows the third-order nonlinear behaviour of Ag nanoplate is greatly modified by its plasmon resonance property, for the largest value of χ (3) is observed around the wavelength of plasmon resonant peak. Also, we find the maximum value of Ag nanoplate's χ (3) is 7.46 × 10 −11 esu, which is about 1-3 orders of magnitude larger than that of many other nanomaterials including Au nanorod, nanobipyramid and nanocube, as well as Ag nanosphere and nanodisc. This fact indicates the Ag triangular nanoplate is a kind of useful nonlinear material with larger third-order nonlinearity, showing great potentials in the explorations of functional non-linear devices.

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Probing ultrafast energy transfer between excitons and plasmons in the ultrastrong coupling regime

Cited by 31 publications

References 33 publications

The role of Rabi splitting tuning in the dynamics of strongly coupled J-aggregates and surface plasmon polaritons in nanohole arrays

The role of Rabi splitting tuning in the dynamics of strongly coupled J-aggregates and surface plasmon polaritons in nanohole arrays

Tunable Plexcitonic Nanoparticles: A Model System for Studying Plasmon–Exciton Interaction from the Weak to the Ultrastrong Coupling Regime

Surface plasmon-enhanced third-order optical non-linearity of silver triangular nanoplate

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