Abstract

A coupling system is proposed to active control of strong exciton–plasmon–exciton coupling, which consists of a silver nanoprism separated from a monolayer WS2 by J-aggregates. The scattering spectrum of the hybrid system calculated by the finite-difference time-domain (FDTD) method is well reproduced by the coupled oscillator model theory. The calculation results show that strong couplings among WS2 excitons, J-aggregate excitons, and localized surface plasmon resonances (LSPRs) are achieved in the hybrid nanostructure, and result in three plexciton branches. We further analyze the exciton–plasmon–exciton coupling behaviors and obtain the weighting efficiencies of the original modes in three plexciton branches. The strong couplings between two different excitons and LSPRs can be active manipulated by tuning the temperature or the concentration of J-aggregates. The proposed systems make up a simple platform for the dynamic control of exciton–plasmon–exciton couplings and have potential applications in optical modulators at the nanoscale.

© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

1. Introduction

Strong light-matter interactions have attracted intense interest due to their great potentials in single-atom lasers [1], quantum information processing [2–4], and ultrafast single-photon switches [5,6]. When the rate of energy exchange between two individual systems exceeds the damping of either, an extraordinary regime of strong light-matter interactions called strong coupling is achieved [7–15]. Strong coupling between different emitters: excitons in transition metal dichalcogenides (TMDs) or J-aggregated dye molecules and surface plasmon polaritons (SPPs) supported by plasmonic nanocavities has been widely studied [7,16–28]. SPPs are electromagnetic excitations propagating at the interface between dielectric and metal, which can enhance the local field with high field confinement [29]. Thus the strong coupling between excitons and plasmons can be achieved in various plasmonic nanocavities [16–28].

Recently, TMDs and J-aggregated dye molecules have attracted tremendous attention for studying strong coupling between excitons and plasmons. Monolayers of TMDs are semiconductor materials with high optical absorption reaching values of 15% for WS2 at the A exciton resonance around 2 eV [30] and a direct band gap at the Κ (Κ’) points of the Brillouin zone. Because of the reduced dielectric screening, giant excitonic effect dominates the band gap transition in monolayers TMDs, possessing a large transition dipole moment μ that achieves strong coupling [31,32]. Additionally, TMDs are chemically stable at ambient conditions, and the strong coupling between TMDs and plasmonic nanocavities can be active controlled via electrostatic gating [33], temperature control [8,34,35] and femtosecond pumping [36,37]. J-aggregated dye molecules are self-organised molecular crystals which possess narrow, red-shifted absorption bands with high oscillator strength [10,38]. The strong coupling between J-aggregated dye molecules and plasmonic nanocavities can be controlled by varying the concentration of J-aggregates [39,40].

Multimode couplings in hybrid excitonic systems have been studied widely because they have more energy dissipation channels and greater modulation [41–44]. For example, the exciton–plasmon–exciton coupling system which consists of a microcavity containing two different J-aggregated dyes is used to study energy transfer processes [41]. Strong plasmon–exciton–trion interaction between localized surface plasmon resonances (LSPRs) in silver nanoprisms and excitons and trions in monolayer WS2 has been achieved at low temperature, which open up a possibility to exploit electrically charged polaritons at the single nanoparticle level [8]. Plasmon–exciton–plasmon couplings in Ag–J-aggregates–Ag nanostructures have been also studied. Strong couplings among LSPRs, exciton resonances, and SPPs were modulated by varying the original localized surface plasmon resonance mode [44]. However, the strong interaction between LSPRs in silver nanoprisms and excitons in J-aggregated dyes molecules and monolayer WS2 has not been studied. This hybrid system is endowed with a hybrid plexciton state with distinct excitons which provides a potential technological route towards active control of strong exciton–plasmon–exciton coupling by modulating different excitons.

In this paper we investigate WS2 excitons and J-aggregate excitons coupling with LSPRs in the Ag–J-aggregates–WS2 hybrid nanostructure. The strong couplings among the WS2 excitons, J-aggregate excitons, and LSPRs are achieved, resulting in three plexciton branches. Coupled oscillator model is used to calculate scattering spectra of the hybrid nanostructure and analyze the exciton–plasmon–exciton coupling behavior. Weighting efficiencies of original modes in the upper (UPB), middle (MPB) and lower plexciton branches (LPB) states are calculated. The weighting efficiencies are used to analyzing the hybrid modes in the coupling system. In addition, the strong exciton–plasmon–exciton coupling can be modulated by tuning the temperature or the concentration of J-aggregates.

2. Methods

To investigate the strong exciton–plasmon–exciton coupling in the hybrid system, finite-difference time-domain (FDTD) simulations are performed to obtain its optical response. The hybrid nanostructure investigated here composed of a silver nanoprism separated from a monolayer WS2 by J-aggregates, as depicted in Fig. 1. The inset shows the cross section view of the hybrid system. The silver nanoprisms are triangular with side length in the range of 45–65 nm, thickness 10 nm, and corner rounding of 3 nm. The mesh size for the Ag nanoprism is 0.5 nm in the x-, y- and z-directions. The mesh size for the WS2 and J-aggregates layer are 0.5 nm in the x- and y- directions, and 0.1 nm in the z- directions. The permittivities of silver are taken from Johnson and Christy data [45]. The dielectric function of J-aggregates and the monolayer WS2 can be described by the superposition of several Lorentz models [31,46–48]:

ε(E)=εBj=1NfjE0j2E2E0j2+iγ0jE
HereεBrepresents the background permittivity, Eis the photon energy (in unit of eV), E0j, γ0j,andfjare resonance energy, damping rate of the oscillator, and oscillator strength with indexj, respectively. In terms of J-aggregates: we setN=1,εB=2.1,γ0=50meV following that used in [22]. The oscillator strengthfvaries from 0.02 to 0.1, which is consistent with previous experiments [49,50]. In the case of WS2:N=5,εB=1,these parameters applied in the simulation are taken from the data in [46], and the measured transmittance optical spectra of a monolayer WS2 flake on the silica substrate have been well reproduced by using Eq. (1). In our simulation, we use the measured damping rate of the A exciton resonanceγX=28 meV [46]. Both J-aggregates and monolayer WS2 exhibit pure exciton absorption in the hybrid system [51]. Furthermore, temperature dependence of the semiconductor bandgap is conveniently described by the O’Donell model for the temperature dependency of the A excitonic transition energy [8,34,52]:
Eg(T)=Eg(0)Sω{coth[ω2kBT]1},
whereEg(0)is excitonic transition energy at 0 K,Sis a dimensionless coupling constant that represents electron-phonon coupling strength, and ωis the average phonon energy. In our simulation the O’Donnel model gives the following values ofEg(0)=2.07eV, S=1.78,and ω=25meV, which is taken from the data in [8]. Thus, we can get the A exciton resonances of WS2 varies with temperature.

 figure: Fig. 1

Fig. 1 Schematic diagram of the Ag–J-aggregates–WS2 nanostructure. The inset shows the cross section of the hybrid nanostructure with the thickness of Ag nanoprism 10 nm. The thickness of J-aggregates and monolayer WS2 both are 1 nm.

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In order to provide physical insight into the exciton–plasmon–exciton coupling, we further focus on the line shape analysis of the scattering spectra. Hence, we fit the calculation results by using coupled oscillator model [53]. In our hybrid system, the coupled oscillator is composed of an oscillator representing plasmon, an oscillator representing J-aggregates exciton, and an oscillator representing the A exciton resonance of WS2. The equations of motion for the three oscillators are:

x¨PL(t)+γPLx˙PL(t)+ωPL2xPL(t)+gJx˙J(t)+gXx˙X(t)=FPL(t),
x¨J(t)+γJx˙J(t)+ωJ2xJ(t)gJx˙PL(t)=FJ(t),
x¨X(t)+γXx˙X(t)+ωX2xX(t)gXx˙PL(t)=FX(t),
wherexPL,xJ,andxXare the coordinates of plasmon, J-aggregates exciton oscillator, and A exciton oscillator, respectively. γPL,γJ, andγXare the damping rate of plasmon, J-aggregates exciton, and A exciton, respectively. ωPL,ωJ, andωXare the resonance frequencies of plasmon, J-aggregates exciton, and A exciton, respectively. gJis the coupling rate between plasmon and J-aggregates exciton. gXis the coupling rate between plasmon and A exciton. FPL,FJ, andFXrepresent the driving forces because of the external source. We assume that the A exciton and J-aggregates exciton are both entirely driven by the plasmon oscillator, hence, we setFPL(t)=FPLeiωt,whereωis the frequency of the electric field, FJ(t)=0, FX(t)=0.Finally, xPL(t),xJ(t),andxX(t)can be derived from Eq. (3), (4), and (5). In our hybrid nanostructure, the dimensions of the structure are small compared to the optical wavelength, thus the scattering cross-section can be calculated in quasi-limit [54]. In this limit, scattering cross-section is(8π/3)·k4|FPLxPL|2, where k=ωn/cis the wavevector of light. By substitutingxPL(t)into(8π/3)·k4|FPLxPL|2and using incident light energy E replaces the incident light frequencyω,one can obtain the scattering cross-section:
σscat(E)=8π3k4|FPLxPL|2E4|abab(E2EPL2+iEγPL)E2gJ2bE2gX2a|2,
where a=E2EJ2+iEγJ,b=E2EX2+iEγX.

To reveal the underlying exciton–plasmon–exciton coupling behaviors in the hybrid nanostructure, we use the classic coupled oscillator model to study the multimode coupling. In order to simplify the oscillator model, the damping losses are not taken into account [41,42,44]. The exciton–plasmon–exciton system can be modeled as three coupled harmonic oscillators:

[EPLgXgJgXEX0gJ0EJ][α1α2α3]=E[α1α2α3],
whereEPL,EX,andEJare the energies of plasmon, A exciton, and J-aggregates exciton, respectively. gXis the interaction constant betweenEPLandEXmodes. gJis the interaction constant betweenEPLandEJmodes. The interaction constant betweenEXandEJmodes is zero. α1,α2,andα3are the eigenvector components (Hopfield coefficients), the corresponding|α1|2,|α2|2,and|α3|2 represent the weighting efficiencies and satisfy|α1|2+|α2|2+|α3|2=1.

3. Results and discussion

We investigate the optical properties of the Ag nanoprism at first. Figure 2(a) presents the simulated scattering spectra of the Ag nanoprisms, showing the LSPRs at 1.93 eV, 1.99 eV, and 2.03 eV, respectively. The resonance spectral width (γPL=80meV) hardly varies with the plasmon resonance. Figure 2(b) gives the simulated transmission spectrum Tof the monolayer WS2. We can get the A exciton resonance atEX=2.02eV with the resonance spectral widthγX=28meV, which is consistent with the experimental result [46]. Figure 2(c) shows the electric field distribution of the Ag nanoprism at 624 nm and polarization along the x-direction axis, the maximum field enhancement occurs at the tips of the Ag nanoprism. The corresponding charge distributions revealed dipole mode and surface charge distribution of the Ag nanoprism at 624 nm as shown in Fig. 2(d).

 figure: Fig. 2

Fig. 2 (a) Scattering spectra of the Ag nanoprisms. The corresponding LSPRs energies are 1.93 eV, 1.99 eV, and 2.03 eV, respectively. (b) Simulated transmission spectrum of the monolayer WS2 flake. (c) The electric field distribution of the Ag nanoprism at wavelength of 624 nm (1.99 eV). (d) The corresponding charge distributions of the Ag nanoprism at 624 nm wavelength.

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Then, we study the strong coupling between J-aggregates and Ag nanoprisms, and strong coupling between WS2 and Ag nanoprisms, respectively. Figure 3(a) shows the resulting successive scattering spectra of J-aggregates coupled with Ag nanoprisms. The color scale represents the scattering efficiency. The “energy” axis of the horizontal represents plasmon resonance energy of Ag nanoprisms (plasmon resonance energy varies with the size of Ag nanoprisms). The “energy” axis of the vertical represents the incident light wavelength (“wavelength” is converted into “energy”).The solid white lines are fit to the coupled oscillator model [10]:

[EPLiγPL2ggEtiγt2][αβ]=E[αβ],
here, EPLis various with the size of Ag nanoprism, γPL=80 meV, t{J,X},EJ=1.94eV, EX=2.02eV, γJ=50meV,γX=28meV. The energy of the UPB and LPB exhibits a clear anticrossing behavior which indicates the strong coupling between J-aggregates exciton and LSPR mode. The Rabi splitting is extracted as the minimal splitting between the two polariton branches. A vacuum Rabi splitting ofΩ=140meV is obtained at zero detuning (Δ=EPLEJ=0eV). It rigorously satisfies the criteria for strong couplingΩ>γPL>(γPL+γJ)/2. Fig. 3(b) shows weighting efficiencies for LSPR mode and J-aggregates exciton contributions to UPB and LPB states as a function of plasmon resonance. This displays a standard plasmon-exciton intermixing behavior, whose weighting efficiencies vary monotonically with the plasmon–exciton detuning. A zero detuning (EPL=EJ=1.94eV) corresponds to two polaritons with identical excitonic and plasmonic fractions. A negative detuning (Δ<0) corresponds to the larger excitonic fraction in UPB and smaller excitonic fraction in LPB. A positive detuning (Δ>0) corresponds to the larger plasmonic fraction in UPB and smaller plasmonic fraction in LPB. In our system, the detuning is modulated by LSPRs. The strong coupling between WS2 and Ag nanoprism is similar to strong coupling between J-aggregates and Ag nanoprism. Figure 3(c) shows the resulting successive scattering spectra of WS2 coupled with Ag nanoprisms. A vacuum Rabi splitting ofΩ=148meV is obtained at zero detuning and Ω>γPL>(γPL+γX)/2 satisfies the strong coupling criteria. The weighting efficiencies for LSPR mode and the A exciton contributions to UPB and LPB states are shown in Fig. 3(d).

 figure: Fig. 3

Fig. 3 (a) Successive scattering spectra of J-aggregates coupled with Ag nanoprisms. The black scattered-diamonds and scattered-triangles represent simulated upper and lower plexciton branches as a function of plasmon resonance position extracted from scattering the spectrum of individual Ag–J-aggregates hybrids of various sizes. The solid white lines are fit to the coupled oscillator model, giving a splitting of 140 meV. The dashed diagonal line and horizontal line correspond to uncoupled LSPR mode and exciton resonance, respectively. The color scale represents the scattering efficiency. The “energy” axis of the horizontal represents plasmon resonance energy of Ag nanoprisms (plasmon resonance energy varies with the size of Ag nanoprisms). The “energy” axis of the vertical represents the incident light wavelength (“wavelength” is converted into “energy”). (b) Weighting efficiencies for LSPR mode and J-aggregates exciton contributions to UPB and LPB states as a function of plasmon resonance. (c) Successive scattering spectra of WS2 coupled with Ag nanoprisms. (d) Weighting efficiencies for LSPR mode and the A exciton contributions to UPB and LPB states as a function of plasmon resonance.

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Let us now turn our attention to the exciton–plasmon–exciton coupling in Ag–J-aggregates–WS2 hybrid nanostructures. Figure 4(a) shows scattering cross sections spectra of the hybrids nanostructure. We suppose that there is no directly interaction between the A exciton and J-aggregates exciton. Therefore, the interaction constant between the A exciton and J-aggregates exciton is zero and the exciton–plasmon–exciton coupling can be investigated through three-oscillator model with Eq. (7). The solid white lines in Fig. 4(a) indicate three anticrossed bands corresponding to UPB, MPB and LPB based on Eq. (7). The solid white lines match well with the numerical simulation results (black scattered-diamonds, scattered-circles and scattered-triangles in Fig. 4(a)). The couplings of the plasmon mode with the A exciton and J-aggregates exciton mode result in two anticrossings at aroundEX=2.02 eV and EJ=1.94eV, respectively. The corresponding coupling strength aregX=65meV andgJ=85meV, respectively. Therefore, the splitting extracted at the zero detuning between the UPB and MPB is ΩUPBMPB=130meV, and the splitting extracted at the zero detuning between MPB and LPB isΩMPBLPB=170meV. Note that the damping losses were not taken into account, since the calculated Rabi splittings are slightly larger than the actual results. Both of them satisfy a simplified strong coupling criterion asΩUPBMPB>γPL>(γPL+γX)/2=54meV andΩMPBLPB>γPL>(γPL+γJ)/2=65meV. Moreover, the minimal splitting between the upper and lower polariton branches is around ΩUPBLPB=227meV, and this satisfies a simplified strong coupling condition asΩUPBLPB>(γPL+γX+γJ)/2=79meV. Figure 4(b) depicts normalized scattering spectrum of J-aggregates and WS2 coupled with Ag nanoprism simulated by FDTD method (red solid line) and calculated by the three-oscillator model based on Eq. (6) (blue circle). The calculated scattering spectrum by the coupled oscillator model matches well with the simulated one, despite there is a little different between amplitude of the scattering spectrum. The coupled oscillator model further reveals the complicated spectral changes as strong coupling. Figure 4(c) shows the weighting efficiencies for LSPR mode, the A exciton of WS2 and J-aggregates exciton contributions to three polariton branches (UPB, MPB and LPB) as a function of plasmon resonance. For simplicity, we discuss the J-aggregates exciton fractions in three polariton branches states. The J-aggregates excitonic fraction is nearly zero in UPB. However, it decreases monotonically with plasmon resonance energies in MPB and increases monotonically with plasmon resonance energies in LPB.

 figure: Fig. 4

Fig. 4 (a) Scattering cross sections spectra of J-aggregates and WS2 coupled with Ag nanoprisms. The black scattered-diamonds, scattered-circles and scattered-triangles represent simulated upper, middle and lower plexciton branches as a function of plasmon resonance position extracted from the scattering spectrum of individual Ag–J-aggregates–WS2 hybrid nanostructure of various sizes. The solid white lines are fit to the coupled oscillator model. The dashed diagonal line and horizontal line correspond to uncoupled LSPR mode and two different exciton resonances, respectively. (b) Normalized scattering spectrum of J-aggregates and WS2 coupled with Ag nanoprism simulated by FDTD solution (red solid line) and calculated by the coupled oscillator model (blue circle). (c) Weighting efficiencies for LSPR mode, the A exciton of WS2 and J-aggregates exciton contributions to UPB, MPB and LPB states as a function of plasmon resonance.

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Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for the thickness of Ag nanoprism in the range of 8-13 nm are shown in Fig. 5(a). With increasing the thickness of Ag nanoprism, the plasmon resonance energy will show a blue-shift and moves through two exciton modes one after another. As a result, the scattering spectra of strong coupling system have a blue-shift with increasing the thickness of Ag nanoprism as shown in Fig. 5(a). Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for the thickness of J-aggregates layer in the range of 1-8 nm are shown in Fig. 5(b). When the thickness of the J-aggregates layer increases from 1 nm to 7 nm, the coupling strength between J-aggregates exciton and plasmon resonance is increased, resulting in increased Rabi splitting. This phenomenon can be explained by the fact that the coupled J-aggregates excitons are increase with thickness of the J-aggregates layer. When the thickness of J-aggregates layer is increased to 8 nm, the normalized scattering spectrum of the hybrid system hardly changes, which can be attributed to the saturation of coupled J-aggregates excitons. In addition, as the thickness of the J-aggregates layer increases, the coupling strength of WS2 and plasmon decrease. As a result, three plexciton branches of scattering spectra become two plexciton branches. Therefore, when the middle plexciton branches disappear, there is a maximum thickness of J-aggregates layer to observe strong coupling among J-aggregates excitons, WS2 excitons and plasmon resonances.

 figure: Fig. 5

Fig. 5 (a) Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for the thickness of Ag nanoprism in the range of 8-13 nm. The dashed vertical line correspond to uncoupled J-aggregates exciton and WS2 exciton modes, respectively. (b) Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for the thickness of J-aggregates layer in the range of 1-8 nm.

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Finally, we discuss the modulation of strong couplings in the Ag–J-aggregates–WS2 hybrid nanostructures. Figure 6(a) shows normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for the temperature range from 220K to 380K. The red dash line in Fig. 6(a) indicates that low energy peak positions (ELPB220K=1.884eV, ELPB380K=1.880eV) of scattering spectra hardly change with increase of the temperature. This phenomenon is due to the little contribution of WS2 excitons to the LPB for temperature range from 220K to 380K as shown in Fig. 4(c). The blue dash line shows middle energy peak positions (EMPB220K=2.004eV,EMPB380K=1.972eV) of scattering spectra have a red-shift with increase of temperature, and the green dash line shows high energy peak positions (EUPB220K=2.127eV, EUPB380K=2.110eV) of scattering spectra have a red-shift with increase of temperature. However, the splitting (Δ220K=EUPB220KEMPB220K=123meV, Δ380K=EUPB380KEMPB380K=138meV) between high energy and middle energy increases with increase of temperature. This can be explained by the fact that the A exciton resonances of WS2 have a red-shift with increase of temperature, effectively tuning WS2 excitons close to LSPR, the coupling strength increase result in the increase of the Rabi splitting. Figure 6(b) depicts normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for oscillator strength of J-aggregates range from 0.02 to 0.1. It is obvious that the splitting (Δ0.02=EMPB0.02ELPB0.02=64meV, Δ0.1=EMPB0.1ELPB0.1=124meV) between middle energy and low energy increases with increase of oscillator strength. However, the splitting (Δ0.02=EUPB0.02EMPB0.02=138meV, Δ0.1=EUPB0.1EMPB0.1=118meV) between high energy and middle energy decreases with increase of oscillator strength, because that the coupling between plasmon and the A excitons is suppressed by the coupling between plasmon and J-aggregate excitons. Therefore, the strong couplings in the Ag–J-aggregates–WS2 hybrid nanostructures could be modulated by adjusting WS2 excitons or J-aggregate excitons individually.

 figure: Fig. 6

Fig. 6 (a) Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for different temperature. (b) Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for different oscillator strength of J-aggregates.

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4. Conclusions

In summary, we investigated the exciton–plasmon–exciton couplings in the Ag–J-aggregates–WS2 hybrid nanostructures based on the FDTD method and the coupled oscillator model. The scattering spectrum computed by the FDTD is consistent with scattering spectrum calculated by the coupled oscillator model. The strong couplings among the LSPR, J-aggregates exciton, and the A exciton modes leads to three plexciton branches (UPB, MPB, LPB). We further analyzed the exciton–plasmon–exciton coupling behaviors using classic oscillator models and obtained the weighting efficiencies of the original modes in three plexciton branches. It is found that WS2 excitons have little contribution to the LPB, thus we could modulate the strong couplings in the Ag–J-aggregates–WS2 hybrid nanostructures by adjusting WS2 excitons through temperature control without change LPB. Furthermore, the coupling between plasmon and the A excitons is suppressed by the coupling between plasmon and J-aggregates with the increase of J-aggregate excitons oscillator strength, thus we could modulate the strong couplings in the Ag–J-aggregates–WS2 hybrid nanostructures by adjusting J-aggregate excitons through control concentration of J-aggregates.

Funding

Ministry of Science and Technology of the People's Republic of China (2016YFA0301300); National Natural Science Foundation of China (NSFC) (11574035, 11374041, 11604020); State Key Laboratory of Information Photonics and Optical Communications.

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23. B. Lee, W. Liu, C. H. Naylor, J. Park, S. C. Malek, J. S. Berger, A. T. C. Johnson, and R. Agarwal, “Electrical tuning of exciton–plasmon polariton coupling in monolayer MoS2 integrated with plasmonic nanoantenna lattice,” Nano Lett. 17(7), 4541–4547 (2017). [CrossRef]   [PubMed]  

24. W. Liu, B. Lee, C. H. Naylor, H.-S. Ee, J. Park, A. T. Johnson, and R. Agarwal, “Strong exciton–plasmon coupling in MoS2 coupled with plasmonic lattice,” Nano Lett. 16(2), 1262–1269 (2016). [CrossRef]   [PubMed]  

25. J. Sun, H. Hu, D. Zheng, D. Zhang, Q. Deng, S. Zhang, and H. Xu, “Light-Emitting Plexciton: Exploiting Plasmon-Exciton Interaction in the Intermediate Coupling Regime,” ACS Nano 12(10), 10393–10402 (2018). [CrossRef]   [PubMed]  

26. M. E. Kleemann, R. Chikkaraddy, E. M. Alexeev, D. Kos, C. Carnegie, W. Deacon, A. C. de Pury, C. Große, B. de Nijs, J. Mertens, A. I. Tartakovskii, and J. J. Baumberg, “Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature,” Nat. Commun. 8(1), 1296 (2017). [CrossRef]   [PubMed]  

27. P. Peng, Y. C. Liu, D. Xu, Q. T. Cao, G. Lu, Q. Gong, and Y. F. Xiao, “Enhancing Coherent Light-Matter Interactions through Microcavity-Engineered Plasmonic Resonances,” Phys. Rev. Lett. 119(23), 233901 (2017). [CrossRef]   [PubMed]  

28. T. Song, Z. Chen, W. Zhang, L. Lin, Y. Bao, L. Wu, and Z. K. Zhou, “Compounding Plasmon-Exciton Strong Coupling System with Gold Nanofilm to Boost Rabi Splitting,” Nanomaterials (Basel) 9(4), 564(2019). [CrossRef]  

29. S. A. Maier, Plasmonics: fundamentals and applications (Springer Science & Business Media, 2007).

30. Y. Li, A. Chernikov, X. Zhang, A. Rigosi, H. M. Hill, A. M. van der Zande, D. A. Chenet, E.-M. Shih, J. Hone, and T. F. Heinz, “Measurement of the optical dielectric function of monolayer transition-metal dichalcogenides: MoS2, MoSe2, WS2, and WSe2,” Phys. Rev. B Condens. Matter Mater. Phys. 90(20), 205422 (2014). [CrossRef]  

31. K. He, N. Kumar, L. Zhao, Z. Wang, K. F. Mak, H. Zhao, and J. Shan, “Tightly bound excitons in monolayer WSe(2).,” Phys. Rev. Lett. 113(2), 026803 (2014). [CrossRef]   [PubMed]  

32. M. M. Ugeda, A. J. Bradley, S.-F. Shi, F. H. da Jornada, Y. Zhang, D. Y. Qiu, W. Ruan, S.-K. Mo, Z. Hussain, Z.-X. Shen, F. Wang, S. G. Louie, and M. F. Crommie, “Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor,” Nat. Mater. 13(12), 1091–1095 (2014). [CrossRef]   [PubMed]  

33. L. C. Flatten, D. M. Coles, Z. He, D. G. Lidzey, R. A. Taylor, J. H. Warner, and J. M. Smith, “Electrically tunable organic-inorganic hybrid polaritons with monolayer WS2,” Nat. Commun. 8(1), 14097 (2017). [CrossRef]   [PubMed]  

34. I. Abid, W. Chen, J. Yuan, A. Bohloul, S. Najmaei, C. Avendano, R. Péchou, A. Mlayah, and J. Lou, “Temperature-dependent plasmon–exciton interactions in hybrid Au/MoSe2 nanostructures,” ACS Photonics 4(7), 1653–1660 (2017). [CrossRef]  

35. J. Wen, H. Wang, W. Wang, Z. Deng, C. Zhuang, Y. Zhang, F. Liu, J. She, J. Chen, H. Chen, S. Deng, and N. Xu, “Room-temperature strong light–matter interaction with active control in single plasmonic nanorod coupled with two-dimensional atomic crystals,” Nano Lett. 17(8), 4689–4697 (2017). [CrossRef]   [PubMed]  

36. P. Vasa, R. Pomraenke, G. Cirmi, E. De Re, W. Wang, S. Schwieger, D. Leipold, E. Runge, G. Cerullo, and C. Lienau, “Ultrafast manipulation of strong coupling in metal-molecular aggregate hybrid nanostructures,” ACS Nano 4(12), 7559–7565 (2010). [CrossRef]   [PubMed]  

37. P. Vasa, W. Wang, R. Pomraenke, M. Lammers, M. Maiuri, C. Manzoni, G. Cerullo, and C. Lienau, “Real-time observation of ultrafast Rabi oscillations between excitons and plasmons in metal nanostructures with J-aggregates,” Nat. Photonics 7(2), 128–132 (2013). [CrossRef]  

38. T. Kobayashi, J-aggregates (World Scientific, 2012).

39. S. Balci, C. Kocabas, S. Ates, E. Karademir, O. Salihoglu, and A. Aydinli, “Tuning surface plasmon-exciton coupling via thickness dependent plasmon damping,” Phys. Rev. B Condens. Matter Mater. Phys. 86(23), 235402 (2012). [CrossRef]  

40. I. Pockrand, A. Brillante, and D. Möbius, “Exciton–surface plasmon coupling: An experimental investigation,” J. Chern. Phys. 77(12), 6289–6295 (1982). [CrossRef]  

41. D. M. Coles, N. Somaschi, P. Michetti, C. Clark, P. G. Lagoudakis, P. G. Savvidis, and D. G. Lidzey, “Polariton-mediated energy transfer between organic dyes in a strongly coupled optical microcavity,” Nat. Mater. 13(7), 712–719 (2014). [CrossRef]   [PubMed]  

42. K. Zhang, W.-B. Shi, D. Wang, Y. Xu, R.-W. Peng, R.-H. Fan, Q.-J. Wang, and M. Wang, “Couple molecular excitons to surface plasmon polaritons in an organic-dye-doped nanostructured cavity,” Appl. Phys. Lett. 108(19), 193111 (2016). [CrossRef]  

43. M. Balasubrahmaniyam, D. Kar, P. Sen, P. B. Bisht, and S. Kasiviswanathan, “Observation of subwavelength localization of cavity plasmons induced by ultra-strong exciton coupling,” Appl. Phys. Lett. 110(17), 171101 (2017). [CrossRef]  

44. H. Yang, J. Yao, X.-W. Wu, D.-J. Wu, and X.-J. Liu, “Strong Plasmon–Exciton–Plasmon Multimode Couplings in Three-Layered Ag–J-Aggregates–Ag Nanostructures,” J. Phys. Chem. C 121(45), 25455–25462 (2017). [CrossRef]  

45. P. B. Johnson and R.-W. Christy, “Optical constants of the noble metals,” Phys. Rev. B 6(12), 4370–4379 (1972). [CrossRef]  

46. S. Wang, S. Li, T. Chervy, A. Shalabney, S. Azzini, E. Orgiu, J. A. Hutchison, C. Genet, P. Samorì, and T. W. Ebbesen, “Coherent coupling of WS2 monolayers with metallic photonic nanostructures at room temperature,” Nano Lett. 16(7), 4368–4374 (2016). [CrossRef]   [PubMed]  

47. A. Shalabney, J. George, J. Hutchison, G. Pupillo, C. Genet, and T. W. Ebbesen, “Coherent coupling of molecular resonators with a microcavity mode,” Nat. Commun. 6(1), 5981 (2015). [CrossRef]   [PubMed]  

48. S. Zhang, H. Zhang, T. Xu, W. Wang, Y. Zhu, D. Li, Z. Zhang, J. Yi, and W. Wang, “Coherent and incoherent damping pathways mediated by strong coupling of two-dimensional atomic crystals with metallic nanogrooves,” Phys. Rev. B 97(23), 235401 (2018). [CrossRef]  

49. N. T. Fofang, T.-H. Park, O. Neumann, N. A. Mirin, P. Nordlander, and N. J. Halas, “Plexcitonic nanoparticles: plasmon-exciton coupling in nanoshell-J-aggregate complexes,” Nano Lett. 8(10), 3481–3487 (2008). [CrossRef]   [PubMed]  

50. A. E. Schlather, N. Large, A. S. Urban, P. Nordlander, and N. J. Halas, “Near-field mediated plexcitonic coupling and giant Rabi splitting in individual metallic dimers,” Nano Lett. 13(7), 3281–3286 (2013). [CrossRef]   [PubMed]  

51. M. J. Gentile, S. Núñez-Sánchez, and W. L. Barnes, “Optical field-enhancement and subwavelength field-confinement using excitonic nanostructures,” Nano Lett. 14(5), 2339–2344 (2014). [CrossRef]   [PubMed]  

52. K. O’Donnell and X. Chen, “Temperature dependence of semiconductor band gaps,” Appl. Phys. Lett. 58(25), 2924–2926 (1991). [CrossRef]  

53. X. Wu, S. K. Gray, and M. Pelton, “Quantum-dot-induced transparency in a nanoscale plasmonic resonator,” Opt. Express 18(23), 23633–23645 (2010). [CrossRef]   [PubMed]  

54. C. F. Bohren and D. R. Huffman, Absorption and scattering of light by small particles (John Wiley & Sons, 2008).

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  50. A. E. Schlather, N. Large, A. S. Urban, P. Nordlander, and N. J. Halas, “Near-field mediated plexcitonic coupling and giant Rabi splitting in individual metallic dimers,” Nano Lett. 13(7), 3281–3286 (2013).
    [Crossref] [PubMed]
  51. M. J. Gentile, S. Núñez-Sánchez, and W. L. Barnes, “Optical field-enhancement and subwavelength field-confinement using excitonic nanostructures,” Nano Lett. 14(5), 2339–2344 (2014).
    [Crossref] [PubMed]
  52. K. O’Donnell and X. Chen, “Temperature dependence of semiconductor band gaps,” Appl. Phys. Lett. 58(25), 2924–2926 (1991).
    [Crossref]
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    [Crossref] [PubMed]
  54. C. F. Bohren and D. R. Huffman, Absorption and scattering of light by small particles (John Wiley & Sons, 2008).

2019 (2)

A. Bisht, J. Cuadra, M. Wersäll, A. Canales, T. J. Antosiewicz, and T. Shegai, “Collective strong light-matter coupling in hierarchical microcavity-plasmon-exciton systems,” Nano Lett. 19(1), 189–196 (2019).
[Crossref] [PubMed]

T. Song, Z. Chen, W. Zhang, L. Lin, Y. Bao, L. Wu, and Z. K. Zhou, “Compounding Plasmon-Exciton Strong Coupling System with Gold Nanofilm to Boost Rabi Splitting,” Nanomaterials (Basel) 9(4), 564(2019).
[Crossref]

2018 (10)

J. Sun, H. Hu, D. Zheng, D. Zhang, Q. Deng, S. Zhang, and H. Xu, “Light-Emitting Plexciton: Exploiting Plasmon-Exciton Interaction in the Intermediate Coupling Regime,” ACS Nano 12(10), 10393–10402 (2018).
[Crossref] [PubMed]

D. G. Baranov, M. Wersäll, J. Cuadra, T. J. Antosiewicz, and T. Shegai, “Novel nanostructures and materials for strong light–matter interactions,” ACS Photonics 5(1), 24–42 (2018).
[Crossref]

J. Cuadra, D. G. Baranov, M. Wersäll, R. Verre, T. J. Antosiewicz, and T. Shegai, “Observation of tunable charged exciton polaritons in hybrid monolayer WS2– plasmonic nanoantenna system,” Nano Lett. 18(3), 1777–1785 (2018).
[Crossref] [PubMed]

P. Vasa and C. Lienau, “Strong light–matter interaction in quantum emitter/metal hybrid nanostructures,” ACS Photonics 5(1), 2–23 (2018).
[Crossref]

J. Flick, N. Rivera, and P. Narang, “Strong light-matter coupling in quantum chemistry and quantum photonics,” Nanophotonics 7(9), 1479–1501 (2018).
[Crossref]

K. L. Koshelev, S. K. Sychev, Z. F. Sadrieva, A. A. Bogdanov, and I. V. Iorsh, “Strong coupling between excitons in transition metal dichalcogenides and optical bound states in the continuum,” Phys. Rev. B 98(16), 161113 (2018).
[Crossref]

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X. Han, K. Wang, X. Xing, M. Wang, and P. Lu, “Rabi Splitting in a Plasmonic Nanocavity Coupled to a WS2 Monolayer at Room Temperature,” ACS Photonics 5(10), 3970–3976 (2018).
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M. Stührenberg, B. Munkhbat, D. G. Baranov, J. Cuadra, A. B. Yankovich, T. J. Antosiewicz, E. Olsson, and T. Shegai, “Strong Light-Matter Coupling between Plasmons in Individual Gold Bi-pyramids and Excitons in Mono- and Multilayer WSe2,” Nano Lett. 18(9), 5938–5945 (2018).
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S. Zhang, H. Zhang, T. Xu, W. Wang, Y. Zhu, D. Li, Z. Zhang, J. Yi, and W. Wang, “Coherent and incoherent damping pathways mediated by strong coupling of two-dimensional atomic crystals with metallic nanogrooves,” Phys. Rev. B 97(23), 235401 (2018).
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2017 (10)

M. Balasubrahmaniyam, D. Kar, P. Sen, P. B. Bisht, and S. Kasiviswanathan, “Observation of subwavelength localization of cavity plasmons induced by ultra-strong exciton coupling,” Appl. Phys. Lett. 110(17), 171101 (2017).
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H. Yang, J. Yao, X.-W. Wu, D.-J. Wu, and X.-J. Liu, “Strong Plasmon–Exciton–Plasmon Multimode Couplings in Three-Layered Ag–J-Aggregates–Ag Nanostructures,” J. Phys. Chem. C 121(45), 25455–25462 (2017).
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D. Zheng, S. Zhang, Q. Deng, M. Kang, P. Nordlander, and H. Xu, “Manipulating coherent plasmon–exciton interaction in a single silver nanorod on monolayer WSe2,” Nano Lett. 17(6), 3809–3814 (2017).
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R. Liu, Z.-K. Zhou, Y.-C. Yu, T. Zhang, H. Wang, G. Liu, Y. Wei, H. Chen, and X.-H. Wang, “Strong light-matter interactions in single open plasmonic nanocavities at the quantum optics limit,” Phys. Rev. Lett. 118(23), 237401 (2017).
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M. E. Kleemann, R. Chikkaraddy, E. M. Alexeev, D. Kos, C. Carnegie, W. Deacon, A. C. de Pury, C. Große, B. de Nijs, J. Mertens, A. I. Tartakovskii, and J. J. Baumberg, “Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature,” Nat. Commun. 8(1), 1296 (2017).
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P. Peng, Y. C. Liu, D. Xu, Q. T. Cao, G. Lu, Q. Gong, and Y. F. Xiao, “Enhancing Coherent Light-Matter Interactions through Microcavity-Engineered Plasmonic Resonances,” Phys. Rev. Lett. 119(23), 233901 (2017).
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B. Lee, W. Liu, C. H. Naylor, J. Park, S. C. Malek, J. S. Berger, A. T. C. Johnson, and R. Agarwal, “Electrical tuning of exciton–plasmon polariton coupling in monolayer MoS2 integrated with plasmonic nanoantenna lattice,” Nano Lett. 17(7), 4541–4547 (2017).
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L. C. Flatten, D. M. Coles, Z. He, D. G. Lidzey, R. A. Taylor, J. H. Warner, and J. M. Smith, “Electrically tunable organic-inorganic hybrid polaritons with monolayer WS2,” Nat. Commun. 8(1), 14097 (2017).
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I. Abid, W. Chen, J. Yuan, A. Bohloul, S. Najmaei, C. Avendano, R. Péchou, A. Mlayah, and J. Lou, “Temperature-dependent plasmon–exciton interactions in hybrid Au/MoSe2 nanostructures,” ACS Photonics 4(7), 1653–1660 (2017).
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J. Wen, H. Wang, W. Wang, Z. Deng, C. Zhuang, Y. Zhang, F. Liu, J. She, J. Chen, H. Chen, S. Deng, and N. Xu, “Room-temperature strong light–matter interaction with active control in single plasmonic nanorod coupled with two-dimensional atomic crystals,” Nano Lett. 17(8), 4689–4697 (2017).
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2016 (3)

K. Zhang, W.-B. Shi, D. Wang, Y. Xu, R.-W. Peng, R.-H. Fan, Q.-J. Wang, and M. Wang, “Couple molecular excitons to surface plasmon polaritons in an organic-dye-doped nanostructured cavity,” Appl. Phys. Lett. 108(19), 193111 (2016).
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W. Liu, B. Lee, C. H. Naylor, H.-S. Ee, J. Park, A. T. Johnson, and R. Agarwal, “Strong exciton–plasmon coupling in MoS2 coupled with plasmonic lattice,” Nano Lett. 16(2), 1262–1269 (2016).
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S. Wang, S. Li, T. Chervy, A. Shalabney, S. Azzini, E. Orgiu, J. A. Hutchison, C. Genet, P. Samorì, and T. W. Ebbesen, “Coherent coupling of WS2 monolayers with metallic photonic nanostructures at room temperature,” Nano Lett. 16(7), 4368–4374 (2016).
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2015 (2)

A. Shalabney, J. George, J. Hutchison, G. Pupillo, C. Genet, and T. W. Ebbesen, “Coherent coupling of molecular resonators with a microcavity mode,” Nat. Commun. 6(1), 5981 (2015).
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P. Törmä and W. L. Barnes, “Strong coupling between surface plasmon polaritons and emitters: a review,” Rep. Prog. Phys. 78(1), 013901 (2015).
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2014 (7)

S. Smolka, W. Wuester, F. Haupt, S. Faelt, W. Wegscheider, and A. Imamoglu, “Cavity quantum electrodynamics with many-body states of a two-dimensional electron gas,” Science 346(6207), 332–335 (2014).
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M. J. Holmes, K. Choi, S. Kako, M. Arita, and Y. Arakawa, “Room-temperature triggered single photon emission from a III-nitride site-controlled nanowire quantum dot,” Nano Lett. 14(2), 982–986 (2014).
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Y. Li, A. Chernikov, X. Zhang, A. Rigosi, H. M. Hill, A. M. van der Zande, D. A. Chenet, E.-M. Shih, J. Hone, and T. F. Heinz, “Measurement of the optical dielectric function of monolayer transition-metal dichalcogenides: MoS2, MoSe2, WS2, and WSe2,” Phys. Rev. B Condens. Matter Mater. Phys. 90(20), 205422 (2014).
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K. He, N. Kumar, L. Zhao, Z. Wang, K. F. Mak, H. Zhao, and J. Shan, “Tightly bound excitons in monolayer WSe(2).,” Phys. Rev. Lett. 113(2), 026803 (2014).
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M. M. Ugeda, A. J. Bradley, S.-F. Shi, F. H. da Jornada, Y. Zhang, D. Y. Qiu, W. Ruan, S.-K. Mo, Z. Hussain, Z.-X. Shen, F. Wang, S. G. Louie, and M. F. Crommie, “Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor,” Nat. Mater. 13(12), 1091–1095 (2014).
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D. M. Coles, N. Somaschi, P. Michetti, C. Clark, P. G. Lagoudakis, P. G. Savvidis, and D. G. Lidzey, “Polariton-mediated energy transfer between organic dyes in a strongly coupled optical microcavity,” Nat. Mater. 13(7), 712–719 (2014).
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M. J. Gentile, S. Núñez-Sánchez, and W. L. Barnes, “Optical field-enhancement and subwavelength field-confinement using excitonic nanostructures,” Nano Lett. 14(5), 2339–2344 (2014).
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2013 (3)

A. E. Schlather, N. Large, A. S. Urban, P. Nordlander, and N. J. Halas, “Near-field mediated plexcitonic coupling and giant Rabi splitting in individual metallic dimers,” Nano Lett. 13(7), 3281–3286 (2013).
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P. Vasa, W. Wang, R. Pomraenke, M. Lammers, M. Maiuri, C. Manzoni, G. Cerullo, and C. Lienau, “Real-time observation of ultrafast Rabi oscillations between excitons and plasmons in metal nanostructures with J-aggregates,” Nat. Photonics 7(2), 128–132 (2013).
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W. Chen, K. M. Beck, R. Bücker, M. Gullans, M. D. Lukin, H. Tanji-Suzuki, and V. Vuletić, “All-optical switch and transistor gated by one stored photon,” Science 341(6147), 768–770 (2013).
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2012 (2)

T. Volz, A. Reinhard, M. Winger, A. Badolato, K. J. Hennessy, E. L. Hu, and A. Imamoğlu, “Ultrafast all-optical switching by single photons,” Nat. Photonics 6(9), 605–609 (2012).
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S. Balci, C. Kocabas, S. Ates, E. Karademir, O. Salihoglu, and A. Aydinli, “Tuning surface plasmon-exciton coupling via thickness dependent plasmon damping,” Phys. Rev. B Condens. Matter Mater. Phys. 86(23), 235402 (2012).
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2010 (3)

P. Vasa, R. Pomraenke, G. Cirmi, E. De Re, W. Wang, S. Schwieger, D. Leipold, E. Runge, G. Cerullo, and C. Lienau, “Ultrafast manipulation of strong coupling in metal-molecular aggregate hybrid nanostructures,” ACS Nano 4(12), 7559–7565 (2010).
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T. M. Babinec, B. J. Hausmann, M. Khan, Y. Zhang, J. R. Maze, P. R. Hemmer, and M. Lončar, “A diamond nanowire single-photon source,” Nat. Nanotechnol. 5(3), 195–199 (2010).
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X. Wu, S. K. Gray, and M. Pelton, “Quantum-dot-induced transparency in a nanoscale plasmonic resonator,” Opt. Express 18(23), 23633–23645 (2010).
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2008 (2)

N. T. Fofang, T.-H. Park, O. Neumann, N. A. Mirin, P. Nordlander, and N. J. Halas, “Plexcitonic nanoparticles: plasmon-exciton coupling in nanoshell-J-aggregate complexes,” Nano Lett. 8(10), 3481–3487 (2008).
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P. Vasa, R. Pomraenke, S. Schwieger, Y. I. Mazur, V. Kunets, P. Srinivasan, E. Johnson, J. E. Kihm, D. S. Kim, E. Runge, G. Salamo, and C. Lienau, “Coherent exciton-surface-plasmon-polariton interaction in hybrid metal-semiconductor nanostructures,” Phys. Rev. Lett. 101(11), 116801 (2008).
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2006 (1)

Y. Sugawara, T. A. Kelf, J. J. Baumberg, M. E. Abdelsalam, and P. N. Bartlett, “Strong coupling between localized plasmons and organic excitons in metal nanovoids,” Phys. Rev. Lett. 97(26), 266808 (2006).
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2004 (1)

A. Wallraff, D. I. Schuster, A. Blais, L. Frunzio, R. Huang, J. Majer, S. Kumar, S. M. Girvin, and R. J. Schoelkopf, “Strong coupling of a single photon to a superconducting qubit using circuit quantum electrodynamics,” Nature 431(7005), 162–167 (2004).
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2003 (1)

J. McKeever, A. Boca, A. D. Boozer, J. R. Buck, and H. J. Kimble, “Experimental realization of a one-atom laser in the regime of strong coupling,” Nature 425(6955), 268–271 (2003).
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1991 (1)

K. O’Donnell and X. Chen, “Temperature dependence of semiconductor band gaps,” Appl. Phys. Lett. 58(25), 2924–2926 (1991).
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1982 (1)

I. Pockrand, A. Brillante, and D. Möbius, “Exciton–surface plasmon coupling: An experimental investigation,” J. Chern. Phys. 77(12), 6289–6295 (1982).
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1972 (1)

P. B. Johnson and R.-W. Christy, “Optical constants of the noble metals,” Phys. Rev. B 6(12), 4370–4379 (1972).
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Abdelsalam, M. E.

Y. Sugawara, T. A. Kelf, J. J. Baumberg, M. E. Abdelsalam, and P. N. Bartlett, “Strong coupling between localized plasmons and organic excitons in metal nanovoids,” Phys. Rev. Lett. 97(26), 266808 (2006).
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Abid, I.

I. Abid, W. Chen, J. Yuan, A. Bohloul, S. Najmaei, C. Avendano, R. Péchou, A. Mlayah, and J. Lou, “Temperature-dependent plasmon–exciton interactions in hybrid Au/MoSe2 nanostructures,” ACS Photonics 4(7), 1653–1660 (2017).
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Agarwal, R.

B. Lee, W. Liu, C. H. Naylor, J. Park, S. C. Malek, J. S. Berger, A. T. C. Johnson, and R. Agarwal, “Electrical tuning of exciton–plasmon polariton coupling in monolayer MoS2 integrated with plasmonic nanoantenna lattice,” Nano Lett. 17(7), 4541–4547 (2017).
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W. Liu, B. Lee, C. H. Naylor, H.-S. Ee, J. Park, A. T. Johnson, and R. Agarwal, “Strong exciton–plasmon coupling in MoS2 coupled with plasmonic lattice,” Nano Lett. 16(2), 1262–1269 (2016).
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Aizpurua, J.

J. J. Baumberg, J. Aizpurua, M. H. Mikkelsen, and D. R. Smith, “Extreme nanophotonics from ultrathin metallic gaps,” Nat. Mater. (2019).

Alexeev, E. M.

M. E. Kleemann, R. Chikkaraddy, E. M. Alexeev, D. Kos, C. Carnegie, W. Deacon, A. C. de Pury, C. Große, B. de Nijs, J. Mertens, A. I. Tartakovskii, and J. J. Baumberg, “Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature,” Nat. Commun. 8(1), 1296 (2017).
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Antosiewicz, T. J.

A. Bisht, J. Cuadra, M. Wersäll, A. Canales, T. J. Antosiewicz, and T. Shegai, “Collective strong light-matter coupling in hierarchical microcavity-plasmon-exciton systems,” Nano Lett. 19(1), 189–196 (2019).
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M. Stührenberg, B. Munkhbat, D. G. Baranov, J. Cuadra, A. B. Yankovich, T. J. Antosiewicz, E. Olsson, and T. Shegai, “Strong Light-Matter Coupling between Plasmons in Individual Gold Bi-pyramids and Excitons in Mono- and Multilayer WSe2,” Nano Lett. 18(9), 5938–5945 (2018).
[Crossref] [PubMed]

D. G. Baranov, M. Wersäll, J. Cuadra, T. J. Antosiewicz, and T. Shegai, “Novel nanostructures and materials for strong light–matter interactions,” ACS Photonics 5(1), 24–42 (2018).
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J. Cuadra, D. G. Baranov, M. Wersäll, R. Verre, T. J. Antosiewicz, and T. Shegai, “Observation of tunable charged exciton polaritons in hybrid monolayer WS2– plasmonic nanoantenna system,” Nano Lett. 18(3), 1777–1785 (2018).
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Arakawa, Y.

M. J. Holmes, K. Choi, S. Kako, M. Arita, and Y. Arakawa, “Room-temperature triggered single photon emission from a III-nitride site-controlled nanowire quantum dot,” Nano Lett. 14(2), 982–986 (2014).
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Arita, M.

M. J. Holmes, K. Choi, S. Kako, M. Arita, and Y. Arakawa, “Room-temperature triggered single photon emission from a III-nitride site-controlled nanowire quantum dot,” Nano Lett. 14(2), 982–986 (2014).
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Ates, S.

S. Balci, C. Kocabas, S. Ates, E. Karademir, O. Salihoglu, and A. Aydinli, “Tuning surface plasmon-exciton coupling via thickness dependent plasmon damping,” Phys. Rev. B Condens. Matter Mater. Phys. 86(23), 235402 (2012).
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Avendano, C.

I. Abid, W. Chen, J. Yuan, A. Bohloul, S. Najmaei, C. Avendano, R. Péchou, A. Mlayah, and J. Lou, “Temperature-dependent plasmon–exciton interactions in hybrid Au/MoSe2 nanostructures,” ACS Photonics 4(7), 1653–1660 (2017).
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Aydinli, A.

S. Balci, C. Kocabas, S. Ates, E. Karademir, O. Salihoglu, and A. Aydinli, “Tuning surface plasmon-exciton coupling via thickness dependent plasmon damping,” Phys. Rev. B Condens. Matter Mater. Phys. 86(23), 235402 (2012).
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Azzini, S.

S. Wang, S. Li, T. Chervy, A. Shalabney, S. Azzini, E. Orgiu, J. A. Hutchison, C. Genet, P. Samorì, and T. W. Ebbesen, “Coherent coupling of WS2 monolayers with metallic photonic nanostructures at room temperature,” Nano Lett. 16(7), 4368–4374 (2016).
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Babinec, T. M.

T. M. Babinec, B. J. Hausmann, M. Khan, Y. Zhang, J. R. Maze, P. R. Hemmer, and M. Lončar, “A diamond nanowire single-photon source,” Nat. Nanotechnol. 5(3), 195–199 (2010).
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Badolato, A.

T. Volz, A. Reinhard, M. Winger, A. Badolato, K. J. Hennessy, E. L. Hu, and A. Imamoğlu, “Ultrafast all-optical switching by single photons,” Nat. Photonics 6(9), 605–609 (2012).
[Crossref]

Balasubrahmaniyam, M.

M. Balasubrahmaniyam, D. Kar, P. Sen, P. B. Bisht, and S. Kasiviswanathan, “Observation of subwavelength localization of cavity plasmons induced by ultra-strong exciton coupling,” Appl. Phys. Lett. 110(17), 171101 (2017).
[Crossref]

Balci, S.

S. Balci, C. Kocabas, S. Ates, E. Karademir, O. Salihoglu, and A. Aydinli, “Tuning surface plasmon-exciton coupling via thickness dependent plasmon damping,” Phys. Rev. B Condens. Matter Mater. Phys. 86(23), 235402 (2012).
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Bao, Y.

T. Song, Z. Chen, W. Zhang, L. Lin, Y. Bao, L. Wu, and Z. K. Zhou, “Compounding Plasmon-Exciton Strong Coupling System with Gold Nanofilm to Boost Rabi Splitting,” Nanomaterials (Basel) 9(4), 564(2019).
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Baranov, D. G.

J. Cuadra, D. G. Baranov, M. Wersäll, R. Verre, T. J. Antosiewicz, and T. Shegai, “Observation of tunable charged exciton polaritons in hybrid monolayer WS2– plasmonic nanoantenna system,” Nano Lett. 18(3), 1777–1785 (2018).
[Crossref] [PubMed]

D. G. Baranov, M. Wersäll, J. Cuadra, T. J. Antosiewicz, and T. Shegai, “Novel nanostructures and materials for strong light–matter interactions,” ACS Photonics 5(1), 24–42 (2018).
[Crossref]

M. Stührenberg, B. Munkhbat, D. G. Baranov, J. Cuadra, A. B. Yankovich, T. J. Antosiewicz, E. Olsson, and T. Shegai, “Strong Light-Matter Coupling between Plasmons in Individual Gold Bi-pyramids and Excitons in Mono- and Multilayer WSe2,” Nano Lett. 18(9), 5938–5945 (2018).
[Crossref] [PubMed]

Barnes, W. L.

P. Törmä and W. L. Barnes, “Strong coupling between surface plasmon polaritons and emitters: a review,” Rep. Prog. Phys. 78(1), 013901 (2015).
[Crossref] [PubMed]

M. J. Gentile, S. Núñez-Sánchez, and W. L. Barnes, “Optical field-enhancement and subwavelength field-confinement using excitonic nanostructures,” Nano Lett. 14(5), 2339–2344 (2014).
[Crossref] [PubMed]

Bartlett, P. N.

Y. Sugawara, T. A. Kelf, J. J. Baumberg, M. E. Abdelsalam, and P. N. Bartlett, “Strong coupling between localized plasmons and organic excitons in metal nanovoids,” Phys. Rev. Lett. 97(26), 266808 (2006).
[Crossref] [PubMed]

Baumberg, J. J.

M. E. Kleemann, R. Chikkaraddy, E. M. Alexeev, D. Kos, C. Carnegie, W. Deacon, A. C. de Pury, C. Große, B. de Nijs, J. Mertens, A. I. Tartakovskii, and J. J. Baumberg, “Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature,” Nat. Commun. 8(1), 1296 (2017).
[Crossref] [PubMed]

Y. Sugawara, T. A. Kelf, J. J. Baumberg, M. E. Abdelsalam, and P. N. Bartlett, “Strong coupling between localized plasmons and organic excitons in metal nanovoids,” Phys. Rev. Lett. 97(26), 266808 (2006).
[Crossref] [PubMed]

J. J. Baumberg, J. Aizpurua, M. H. Mikkelsen, and D. R. Smith, “Extreme nanophotonics from ultrathin metallic gaps,” Nat. Mater. (2019).

Beck, K. M.

W. Chen, K. M. Beck, R. Bücker, M. Gullans, M. D. Lukin, H. Tanji-Suzuki, and V. Vuletić, “All-optical switch and transistor gated by one stored photon,” Science 341(6147), 768–770 (2013).
[Crossref] [PubMed]

Berger, J. S.

B. Lee, W. Liu, C. H. Naylor, J. Park, S. C. Malek, J. S. Berger, A. T. C. Johnson, and R. Agarwal, “Electrical tuning of exciton–plasmon polariton coupling in monolayer MoS2 integrated with plasmonic nanoantenna lattice,” Nano Lett. 17(7), 4541–4547 (2017).
[Crossref] [PubMed]

Bisht, A.

A. Bisht, J. Cuadra, M. Wersäll, A. Canales, T. J. Antosiewicz, and T. Shegai, “Collective strong light-matter coupling in hierarchical microcavity-plasmon-exciton systems,” Nano Lett. 19(1), 189–196 (2019).
[Crossref] [PubMed]

Bisht, P. B.

M. Balasubrahmaniyam, D. Kar, P. Sen, P. B. Bisht, and S. Kasiviswanathan, “Observation of subwavelength localization of cavity plasmons induced by ultra-strong exciton coupling,” Appl. Phys. Lett. 110(17), 171101 (2017).
[Crossref]

Blais, A.

A. Wallraff, D. I. Schuster, A. Blais, L. Frunzio, R. Huang, J. Majer, S. Kumar, S. M. Girvin, and R. J. Schoelkopf, “Strong coupling of a single photon to a superconducting qubit using circuit quantum electrodynamics,” Nature 431(7005), 162–167 (2004).
[Crossref] [PubMed]

Boca, A.

J. McKeever, A. Boca, A. D. Boozer, J. R. Buck, and H. J. Kimble, “Experimental realization of a one-atom laser in the regime of strong coupling,” Nature 425(6955), 268–271 (2003).
[Crossref] [PubMed]

Bogdanov, A. A.

K. L. Koshelev, S. K. Sychev, Z. F. Sadrieva, A. A. Bogdanov, and I. V. Iorsh, “Strong coupling between excitons in transition metal dichalcogenides and optical bound states in the continuum,” Phys. Rev. B 98(16), 161113 (2018).
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Bohloul, A.

I. Abid, W. Chen, J. Yuan, A. Bohloul, S. Najmaei, C. Avendano, R. Péchou, A. Mlayah, and J. Lou, “Temperature-dependent plasmon–exciton interactions in hybrid Au/MoSe2 nanostructures,” ACS Photonics 4(7), 1653–1660 (2017).
[Crossref]

Boozer, A. D.

J. McKeever, A. Boca, A. D. Boozer, J. R. Buck, and H. J. Kimble, “Experimental realization of a one-atom laser in the regime of strong coupling,” Nature 425(6955), 268–271 (2003).
[Crossref] [PubMed]

Bradley, A. J.

M. M. Ugeda, A. J. Bradley, S.-F. Shi, F. H. da Jornada, Y. Zhang, D. Y. Qiu, W. Ruan, S.-K. Mo, Z. Hussain, Z.-X. Shen, F. Wang, S. G. Louie, and M. F. Crommie, “Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor,” Nat. Mater. 13(12), 1091–1095 (2014).
[Crossref] [PubMed]

Brillante, A.

I. Pockrand, A. Brillante, and D. Möbius, “Exciton–surface plasmon coupling: An experimental investigation,” J. Chern. Phys. 77(12), 6289–6295 (1982).
[Crossref]

Buck, J. R.

J. McKeever, A. Boca, A. D. Boozer, J. R. Buck, and H. J. Kimble, “Experimental realization of a one-atom laser in the regime of strong coupling,” Nature 425(6955), 268–271 (2003).
[Crossref] [PubMed]

Bücker, R.

W. Chen, K. M. Beck, R. Bücker, M. Gullans, M. D. Lukin, H. Tanji-Suzuki, and V. Vuletić, “All-optical switch and transistor gated by one stored photon,” Science 341(6147), 768–770 (2013).
[Crossref] [PubMed]

Canales, A.

A. Bisht, J. Cuadra, M. Wersäll, A. Canales, T. J. Antosiewicz, and T. Shegai, “Collective strong light-matter coupling in hierarchical microcavity-plasmon-exciton systems,” Nano Lett. 19(1), 189–196 (2019).
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Cao, Q. T.

P. Peng, Y. C. Liu, D. Xu, Q. T. Cao, G. Lu, Q. Gong, and Y. F. Xiao, “Enhancing Coherent Light-Matter Interactions through Microcavity-Engineered Plasmonic Resonances,” Phys. Rev. Lett. 119(23), 233901 (2017).
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Figures (6)

Fig. 1
Fig. 1 Schematic diagram of the Ag–J-aggregates–WS2 nanostructure. The inset shows the cross section of the hybrid nanostructure with the thickness of Ag nanoprism 10 nm. The thickness of J-aggregates and monolayer WS2 both are 1 nm.
Fig. 2
Fig. 2 (a) Scattering spectra of the Ag nanoprisms. The corresponding LSPRs energies are 1.93 eV, 1.99 eV, and 2.03 eV, respectively. (b) Simulated transmission spectrum of the monolayer WS2 flake. (c) The electric field distribution of the Ag nanoprism at wavelength of 624 nm (1.99 eV). (d) The corresponding charge distributions of the Ag nanoprism at 624 nm wavelength.
Fig. 3
Fig. 3 (a) Successive scattering spectra of J-aggregates coupled with Ag nanoprisms. The black scattered-diamonds and scattered-triangles represent simulated upper and lower plexciton branches as a function of plasmon resonance position extracted from scattering the spectrum of individual Ag–J-aggregates hybrids of various sizes. The solid white lines are fit to the coupled oscillator model, giving a splitting of 140 meV. The dashed diagonal line and horizontal line correspond to uncoupled LSPR mode and exciton resonance, respectively. The color scale represents the scattering efficiency. The “energy” axis of the horizontal represents plasmon resonance energy of Ag nanoprisms (plasmon resonance energy varies with the size of Ag nanoprisms). The “energy” axis of the vertical represents the incident light wavelength (“wavelength” is converted into “energy”). (b) Weighting efficiencies for LSPR mode and J-aggregates exciton contributions to UPB and LPB states as a function of plasmon resonance. (c) Successive scattering spectra of WS2 coupled with Ag nanoprisms. (d) Weighting efficiencies for LSPR mode and the A exciton contributions to UPB and LPB states as a function of plasmon resonance.
Fig. 4
Fig. 4 (a) Scattering cross sections spectra of J-aggregates and WS2 coupled with Ag nanoprisms. The black scattered-diamonds, scattered-circles and scattered-triangles represent simulated upper, middle and lower plexciton branches as a function of plasmon resonance position extracted from the scattering spectrum of individual Ag–J-aggregates–WS2 hybrid nanostructure of various sizes. The solid white lines are fit to the coupled oscillator model. The dashed diagonal line and horizontal line correspond to uncoupled LSPR mode and two different exciton resonances, respectively. (b) Normalized scattering spectrum of J-aggregates and WS2 coupled with Ag nanoprism simulated by FDTD solution (red solid line) and calculated by the coupled oscillator model (blue circle). (c) Weighting efficiencies for LSPR mode, the A exciton of WS2 and J-aggregates exciton contributions to UPB, MPB and LPB states as a function of plasmon resonance.
Fig. 5
Fig. 5 (a) Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for the thickness of Ag nanoprism in the range of 8-13 nm. The dashed vertical line correspond to uncoupled J-aggregates exciton and WS2 exciton modes, respectively. (b) Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for the thickness of J-aggregates layer in the range of 1-8 nm.
Fig. 6
Fig. 6 (a) Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for different temperature. (b) Normalized scattering spectra of J-aggregates and WS2 coupled with Ag nanoprism for different oscillator strength of J-aggregates.

Equations (8)

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ε(E)= ε B j=1 N f j E 0j 2 E 2 E 0j 2 +i γ 0j E
E g (T)= E g (0)S ω { coth[ ω 2 k B T ]1 },
x ¨ PL (t)+ γ PL x ˙ PL (t)+ ω PL 2 x PL (t)+ g J x ˙ J (t)+ g X x ˙ X (t)= F PL (t),
x ¨ J (t)+ γ J x ˙ J (t)+ ω J 2 x J (t) g J x ˙ PL (t)= F J (t),
x ¨ X (t)+ γ X x ˙ X (t)+ ω X 2 x X (t) g X x ˙ PL (t)= F X (t),
σ scat (E)= 8π 3 k 4 | F PL x PL | 2 E 4 | ab ab( E 2 E PL 2 +iE γ PL ) E 2 g J 2 b E 2 g X 2 a | 2 ,
[ E PL g X g J g X E X 0 g J 0 E J ][ α 1 α 2 α 3 ]=E[ α 1 α 2 α 3 ],
[ E PL i γ PL 2 g g E t i γ t 2 ][ α β ]=E[ α β ],

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