Understanding radiative transitions and relaxation pathways in plexcitons

Finkelstein-Shapiro, Daniel; Mante, Pierre‐Adrien; Sarisozen, Sema; Wittenbecher, Lukas; Minda, Iulia; Balci, Sinan; Pullerits, Tõnu; Zigmantas, Donatas

doi:10.1016/j.chempr.2021.02.028

Cited by 35 publications

(59 citation statements)

References 87 publications

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“…However, the stricter criterion for entering strong coupling regime ( ) is not yet realized here, in which the mechanism of plexciton nonlinearity might become different, especially for the so-called ultrastrong coupling regime 58 . Overall, the plexciton nonlinearity in our work is more akin to nonlinear Fano interference-type behaviour than to Rabi splitting-type behaviour 59 – 61 , which is only appliable for the intermediate coupling regime and the very onset of the strong coupling regime.…”

Section: Resultsmentioning

confidence: 97%

Interacting plexcitons for designed ultrafast optical nonlinearity in a monolayer semiconductor

et al. 2022

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Searching for ideal materials with strong effective optical nonlinear responses is a long-term task enabling remarkable breakthroughs in contemporary quantum and nonlinear optics. Polaritons, hybridized light-matter quasiparticles, are an appealing candidate to realize such nonlinearities. Here, we explore a class of peculiar polaritons, named plasmon–exciton polaritons (plexcitons), in a hybrid system composed of silver nanodisk arrays and monolayer tungsten-disulfide (WS2), which shows giant room-temperature nonlinearity due to their deep-subwavelength localized nature. Specifically, comprehensive ultrafast pump–probe measurements reveal that plexciton nonlinearity is dominated by the saturation and higher-order excitation-induced dephasing interactions, rather than the well-known exchange interaction in traditional microcavity polaritons. Furthermore, we demonstrate this giant nonlinearity can be exploited to manipulate the ultrafast nonlinear absorption properties of the solid-state system. Our findings suggest that plexcitons are intrinsically strongly interacting, thereby pioneering new horizons for practical implementations such as energy-efficient ultrafast all-optical switching and information processing.

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Section: Resultsmentioning

confidence: 97%

Interacting plexcitons for designed ultrafast optical nonlinearity in a monolayer semiconductor

et al. 2022

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“…1,3,8 However, plexciton behavior has to be wholly understood and characterized. As an example, the nature of excitations and the mechanisms of energy dissipation in these materials 9 and phenomena as ultrafast coherences (Rabi oscillations), 10 Bose−Einstein condensation, 11 and "induced transparency" (or Fano dip) 12,13 are the object of several ongoing investigations.…”

Section: ■ Introductionmentioning

confidence: 99%

“…These nanomaterials are obtained by combining plasmonic substrates, such as nanostructured surfaces or nanoparticles, with excitonic systems like organic dyes, quantum dots, carbon nanotubes, or 2-dimensional transition-metal dichalcogenides, such as MoS 2 or WS 2 . − The peculiar optical properties of these materials might find application in photovoltaics, sensing, , digital data storage, and in the broad field of photonics as a manner to control light–matter interactions at the nanoscale. ,, However, plexciton behavior has to be wholly understood and characterized. As an example, the nature of excitations and the mechanisms of energy dissipation in these materials and phenomena as ultrafast coherences (Rabi oscillations), Bose–Einstein condensation, and “induced transparency” (or Fano dip) , are the object of several ongoing investigations.…”

Section: Introductionmentioning

confidence: 99%

“…Many works in the literature have investigated the main physicochemical parameters that regulate the plexcitonic coupling strength (see, for example, refs and − ), but the role of the capping layer has never been examined in depth. Among the attractive interactions between the plasmonic and excitonic moieties enabled by the capping layer, electrostatic interactions appear to be the most commonly exploited in nanohybrid preparation. ,, As an example, Mohankumar et al.…”

Section: Introductionmentioning

confidence: 99%

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Plexcitonic Nanohybrids Based on Gold Nanourchins: The Role of the Capping Layer

2021

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Plexcitonic nanohybrids are plasmonic–excitonic novel materials whose peculiar properties are attracting considerable attention in photonics, solar cells, and sensing. These materials can be synthesized and characterized easily by assembling organic or inorganic dyes on plasmonic nanoparticles as support. However, the main factors controlling the assembly process and the occurrence of the plexcitonic coupling are still unclear. To fill this gap, in this work, we studied the plexciton coupling of 12 different dyes with a series of gold nanourchins with various coatings and sizes. Among 24 combinations tested, we observed the formation of plexcitonic hybrids only in five cases. Most of them had cyanine J-aggregates as excitonic counterparts. Stronger plexcitonic couplings were obtained when nanourchins were coated with an exchangeable citrate capping layer rather than a strong ionic thiols capping layer. We propose that the presence of a strongly bound capping layer, as in this latter case, reduces the effective volume available to the dyes.

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“…We now turn our attention to strong and weak light–matter interaction in collection of CDs embedded in the LLC mesophase placed near a metal thin film. In order to study plasmon–exciton coupling 15 in CDs on flat metal surfaces, a well-known Kretschmann configuration, as shown in Figure 5 a, was used. It should be noted that the Kretschmann configuration is commonly used for the excitation of surface plasmons on thin metal films.…”

Section: Methodsmentioning

confidence: 99%

Strong Coupling of Carbon Quantum Dots in Liquid Crystals

Sarisozen

Polat

Balcı

et al. 2022

J. Phys. Chem. Lett.

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Carbon quantum dots (CDs) have recently received a tremendous amount of interest owing to their attractive optical properties. However, CDs have broad absorption and emission spectra limiting their application ranges. We herein, for the first time, show synthesis of water-soluble red emissive CDs with a very narrow line width (∼75 meV) spectral absorbance and hence demonstrate strong coupling of CDs and plasmon polaritons in liquid crystalline mesophases. The excited state dynamics of CDs has been studied by ultrafast transient absorption spectroscopy, and CDs display very stable and strong photoluminescence emission with a quantum yield of 35.4% and a lifetime of ∼2 ns. More importantly, we compare J -aggregate dyes with CDs in terms of their absorption line width, photostability, and ability to do strong coupling, and we conclude that highly fluorescent CDs have a bright future in the mixed light–matter states for emerging applications in future quantum technologies.

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Understanding radiative transitions and relaxation pathways in plexcitons

Cited by 35 publications

References 87 publications

Interacting plexcitons for designed ultrafast optical nonlinearity in a monolayer semiconductor

Interacting plexcitons for designed ultrafast optical nonlinearity in a monolayer semiconductor

Plexcitonic Nanohybrids Based on Gold Nanourchins: The Role of the Capping Layer

Strong Coupling of Carbon Quantum Dots in Liquid Crystals

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