Plasmon-exciton couplings in the MoS2/AuNP plasmonic hybrid structure

Plasmon-exciton couplings in the MoS2/AuNP plasmonic hybrid structure | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Plasmon-exciton couplings in the MoS2/AuNP plasmonic hybrid structure Hyuntae Kim, Jaeseung Im, Sung Jae Yoo, MohammadNavid Haddadnezhad, and 9 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-2249049/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 9 You are reading this latest preprint version Abstract The understanding and engineering of the plasmon-exciton coupling are necessary to control the innovative optoelectronic device platform. In this study, we investigated the intertwined mechanism of each plasmon-exciton couplings in monolayer molybdenum disulfide (MoS 2 ) and plasmonic hybrid structure. The results of absorption, simulation, electrostatics, and emission spectra show that interaction between photoexcited carrier and exciton modes are successfully coupled by energy transfer and exciton recombination processes. Especially, neutral exciton, trion, and biexciton can be selectively enhanced by designing the plasmonic hybrid platform. All of these results imply that there is another degree of freedom to control the individual enhancement of each exciton mode in the development of nano optoelectronic devices. Physical sciences/Nanoscience and technology/Nanoscale devices/Nanophotonics and plasmonics Physical sciences/Optics and photonics/Optical physics/Nanophotonics and plasmonics Physical sciences/Physics/Optical physics/Nanophotonics and plasmonics Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Introduction Optical response in transition metal dichalcogenides (TMDCs) could be engineered by the van der Waals heterostructures, chemical treatment, defect controlling and inducing the local strain, etc 1 – 6 . Among them, the hybrid structure of noble metal nanoparticles with TMDCs has been introduced to enhance the light-matter interaction caused by plasmon-exciton couplings 7 , 8 . The techniques for enhancing the optical response are based on the local electromagnetic (EM) field confinements on a metallic nanostructure that is referred to as the localized surface plasmon resonance (LSPR) 9 . The localized EM field increases the absorption and emission rate in plasmonic hybrid structures. In addition, the orientation of the hotspots of the EM field could be controlled by designing the plasmonic nanoparticles platform, gap distance, and local environment structure 10 – 12 . The molybdenum disulfide (MoS 2 ) is one of the noble candidates for functional optical devices due to its unique physical properties, such as tightly bounded excitons, chemical stability, and visible spectral region of photoluminescence (PL) spectra, bandgap tuning by local induced strain 13 . In the previous studies of MoS 2 /plasmonic hybrid structure, these plasmonic nanoparticles are employed in various structures, such as nano-rings, heterodimers, plates, rods, 3D cubes, and split rings, etc 14 – 16 . The mechanism of plasmon-exciton couplings was explained by hot-electron injection, energy transfer, bandgap funneling, and EM field enhancement 17 – 19 . The exciton dynamics of photogenerated quasiparticles, which are the neutral excitons(X 0 ), trions(X – ), and biexcitons(XX), are electronically excited states consisting of an electron and a hole. The recombination processes of excitons from X 0 to X – and XX are affected by the background carrier concentrations and are also controlled by Fermi level tunning by local doping 20 . The optical response of XX in MoS 2 depends on the optical doping. However, the X 0 and X – do on the electrical doping dependence 21 – 24 . So far as we know, the coupling mechanism of plasmon-exciton has remained vague due to its complex recombination pathways in each exciton mode. In this paper, we investigate the intertwined mechanism of plasmon-exciton couplings in X 0 , X – , and XX modes on the hybrid structure of the monolayer MoS 2 and non-centrosymmetric Au nanoparticle (AuNP). To characterize the optical response, we measured the absorption, Raman, and PL spectra depending on the excitation wavelength, incident power, and polarization. Also, non-centrosymmetric AuNP opens the possibility to control the plasmon-exciton coupling due to the optical response dependence on the polarization. The power-dependent PL spectra of each exciton mode are used to identify the optical doping effect and charge recombination processes in multiexciton modes. Results Figure 1 a shows the optical images of the MoS 2 /plasmonic hybrid structures. The spatial density of the AuNPs is 0.13 particles/µm 2 . The indicated regions are the bare MoS 2 (circle), MoS 2 /AuNP hybrid structure (square), and AuNP particle without MoS 2 (arrow), respectively. The high-resolution scanning electron microscope (SEM) image shows the geometrical shape of AuNP (Fig. 1 b). The AuNPs have an outer radius of ~ 75 nm, an inner radius of ~ 25 nm, and a gap width of ~ 10 nm, respectively (inset of Fig. 1 b). As depicted in Fig. 1 c, the Raman spectra of the monolayer MoS 2 and MoS 2 /AuNP hybrid structure under 532 nm excitations clearly show A 1g and E 1 2g peaks. The frequency difference of Raman modes between the E 1 2g and A 1g in the monolayer MoS 2 was observed as 20.4 cm - 1 , which is consistent with the previous studies 25 , 26 . On the other hand, in the case of the MoS 2 /AuNP hybrid structure, the relative peak intensity ratio between A 1g and E 1 2g modes, A 1g /E 1 2g , was increased. It can be explained as a result of the p-doping effect due to the tensile strain of the MoS 2 surface on the AuNP 27 . Figure 1 d shows the reflectance from Si/SiO 2 , AuNP, MoS 2 , and MoS 2 /AuNP. The Si/SiO 2 was used as a reference surface. AuNP does not show strong resonant absorption feature, but about 5% decreased reflectance in the 550 nm to 800 nm spectral range because of the LSPRs absorption. The MoS 2 and MoS 2 /AuNP show two absorption dips at ~ 651 nm (E A ) and ~ 604 nm (E B ), which correspond to the absorption band of A and B excitons in MoS 2 , respectively 28 , 29 . In the MoS 2 /AuNP hybrid structure, the reflectance was additionally decreased (i.e., absorption increased) at E A and E B by 5% than the bare MoS 2 monolayer. The absorption enhancement originates from the response of LSPRs on the AuNP with the resonant energy transfer 30 . Therefore, the excitation wavelength of 632.8 nm is suitable for enhanced absorption via LSPR. In addition, the absorbance spectrum of the AuNP was calculated by the finite element method (FEM) simulation, as shown in Fig. 1 e-f. The simulated absorbance spectrum has two resonance peaks at 615 nm and 680 nm. In our experiment, two excitation wavelengths of the laser (632.8 nm and 532 nm) were used to compare the on/off resonance characteristics of the MoS 2 /AuNP hybrid structure (Fig. 1 e). The AuNPs have polarization-dependent absorption, which originated from their non-centrosymmetric structure 31 . The absorption can be enhanced only when the polarization and the excitation wavelength of the light are satisfied with the resonance condition of the AuNP (Fig. 1 f). Figure 2 a–d shows the PL spectra with 532 nm and 632.8 nm excitation to investigate the plasmonic response of the hybrid structure, respectively. The peak positions of the PL (denoted as A and B, respectively) are 1.90–1.95 eV and 2.05–2.10 eV, respectively, which are consistent with the previous results for monolayer MoS 2 32 . The peak intensity of the A exciton was enhanced about 1.5 and 2.4 times under 532 nm and 632.8 nm excitation, respectively. The normalized PL spectra with 532 nm excitation are shown in Fig. 2 b. The normalized spectrum barely changed by the AuNPs, owing to the off-resonance excitation of the LSPRs. In contrast, 632.8 nm excited PL spectra showed significant changes with peak positions and line width, as shown in Fig. 2 d. The peak position of the spectrum is red-shifted, and the linewidth of the spectrum is broadened in MoS 2 /AuNP hybrid structure. The observed phenomena can be described by the complex interaction between AuNP and MoS 2 , such as plasmon-exciton coupling, local doping, strain, etc. Discussion We suggest that the exciton-plasmon coupling scheme can explain the exciton recombination mechanism in the MoS 2 /AuNP hybrid structure. As depicted in Fig. 2 e, the energy transfer mechanism was demonstrated considering selective exciton excitation in the MoS 2 /AuNP hybrid structure under the resonant excitation of LSPRs. The recombination of each exciton was followed by excitation, energy transfer, recombination, and EM field enhancement. The first step of the recombination pathways in the MoS 2 /AuNP hybrid structure is the excitation process. The optically excited electron in the AuNP has radiative and nonradiative pathways in the relaxation processes. The nonradiative relaxation of the photoexcited carrier in AuNP, such as carrier-carrier scattering, is much faster than radiative electron-hole recombination 33 . The strength of nonradiative relaxation processes depends on the resonant plasmonic optical response of the AuNP. Also, the resonant energy transfer in nonradiative relaxation processes has to consider the metal-semiconductor energy band alignment in the plasmonic hybrid structure 34 . The condition of resonance energy transfer was estimated through absorption spectra and simulation, as mentioned in Fig. 1 . The second step is the energy transfer between the AuNP and the monolayer MoS 2 . To investigate the energy transfer mechanism, PL emission and electrostatic characteristics were measured. The line width broadening in PL spectra implies the excessive charge density in the excitonic feature of the MoS 2 /AuNP hybrid structure under resonant excitation (Fig. 2 a-d). Figure 3 a-b show the topography and surface potential map of MoS 2 /AuNP plasmonic hybrid structures, respectively. The thickness of the MoS 2 is ~ 0.75 nm on the edge of the monolayer MoS 2 . In addition, monolayer MoS 2 film has wrinkles due to ~ 30 nm of the AuNP particles. Notably, the topography and potential images have different appearances on MoS 2 /AuNP (square) and bare MoS 2 . Besides, the surface, including flat and wrinkled areas without the nanoparticles (circle), does not make a distinct electrical potential difference. As illustrated in Fig. 3 c, the contact potential difference (eV CPD ) on the MoS 2 and hybrid structures is 567.15 meV and 513.61 meV, respectively. The equilibrium state of the Fermi level was p-doped due to the − 55.54 meV Fermi level modulation by contact on the AuNP and MoS 2 . The contact in the MoS 2 /AuNP hybrid structure was estimated as Ohmic contact due to the smaller work function of MoS 2 (5.15 eV) than AuNP in the case of p-doped semiconductors 35 . Notably, the photo-excited carriers in AuNP and plasmonic hot-carriers moved toward the MoS 2 film by the downward energy band bending at the interface 36 . The carrier injection in the interface can modulate the exciton bindings in the MoS 2 film 37 , 38 . Figure 3 d-e show the electrical potential difference on the MoS 2 /AuNP plasmonic hybrid structure with the V CPD distribution and profile. The difference of the eV CPD between the monolayer MoS 2 and Si/SiO 2 substrate is − 5 0 meV. However, the distribution of the eV CPD on the MoS 2 /AuNP structures was decreased to − 5 5.54 meV compared to the flat and wrinkled surface of MoS 2 . The result of the KPFM demonstrates that the monolayer MoS 2 /AuNP hybrid structure was p-doped, as mentioned in Raman spectra (Fig. 1 c). The recombination process in each exciton mode was analyzed from the deconvoluted PL spectra. The energy relaxation in neutral exciton was recombinant to the trion and biexciton mode due to the plasmon-exciton coupling (Fig. 4 ). The interaction between MoS 2 and the AuNP can be explained by introducing plasmonic coupling contributions in the excitation and emission processes of excitons. The majority of the PL enhancement was caused by induced local electric field enhancement at the interface between MoS 2 and AuNP 39 . The total enhancement g(ω) on the plasmonic hybrid structures of the aggregated MoS 2 /AuNP is considered in two independent processes, excitation enhancement g exc (ω exc ) and emission enhancement g em (ω) as following equations as 40 : g(ω) = g exc (ω exc )g em (ω) , (Eq. 1) where ω is the frequency of the EM field, and ω exc is the excitation laser frequency. The enhancement factor (EF) is complex to calculate due to the various exciton dynamics of the radiative/nonradiative decay rates and energy transfer. The energy transfer in the emission process is the response of interband charge transitions in the semiconductor and excited carrier transfer from the plasmonic structure. In addition, the local field enhancement depends on the polarization of the incident light according to the plasmonic response. Moreover, the monolayer MoS 2 has a strong absorption rate and PL emission spectra due to the weak dielectric screening and atomically thin spatial confinement of carriers. Neutral excitons (X 0 ) in MoS 2 can be coupled with the bound state of an electron and hole in the presence of residual excessive charge carriers under excitation. The charged neutral exciton of quasiparticles, called trions (X – ), consists of two electrons and one hole. Also, the biexcitons (XX) are the formation of molecular states consisting of two excitons. To estimate the plasmon-exciton coupling for each exciton, Fig. 4 a-c show that the integrated PL intensity map and spectra in the MoS 2 (circle) and MoS 2 /AuNP (square) under 200 µW at 632.8 nm excitations. The PL spectra were deconvoluted by Lorentzian formation for the intensity and center frequency estimation in each exciton mode (Fig. 4 b-f) 21 , 41 , 42 . In Fig. 4 b-c, the total PL peak intensities (gray) are 2.14 times higher in plasmonic hybrid structures than bare MoS 2 film, as same in Fig. 2 c-d. A significant enhancement in the 632.8 nm excitation was caused by the EM field resonance on the AuNP compared to the 532 nm excitation, as mentioned. Also, the change of PL intensity was barely observed on the natural wrinkles in the flake, which is consistent with the result in Fig. 3 b. The linewidth broadening of the total PL spectra on the region of MoS 2 /AuNP can be explained by increasing contributions of the X – and XX states. Figure 4 d shows the hyper spectral image of PL in the MoS 2 /AuNP hybrid structure along the red line in Fig. 4 a. The observed spatially resolved PL intensity shows that the XX peak was clearly enhanced only at the MoS 2 /AuNP hybrid structure. Figure 4 e shows the peak enhancement of each exciton mode, which results using the deconvolution of the PL spectra in the bare MoS 2 and MoS 2 /AuNP hybrid structure. The enhancement of X 0 , X – , and XX is 2.29, 4.96, and 4.90 times, respectively. The intensities of X – and XX are more than two times larger than X 0 due to the large g exc (ω exc ) of plasmon-exciton coupling and energy transfer. Figure 4 f shows the center energy difference in each exciton mode. The peak shift of neutral exciton is − 5.38 meV in MoS 2 /AuNP hybrid structure. Also, the difference of center frequency in X – and XX is 25.68 meV and 44.69 meV, respectively. The peak shifts of X – and XX are significantly larger than X 0 because of the effectively local p-dopping by the AuNP applied local tensile strain and energy transfer in direct contact between nanoparticle and MoS 2 . It is observed that the broadening of the peak (see supplementary information) denotes the increase of the recombination rate, which also supports the existence of the local p-doping effect and the effective charge transfer from metal nanoparticles to the MoS 2 film. The analyzed each exciton mode from PL spectra under 632.8 nm excitation shows the plasmon-exciton coupling and energy transfer mechanism in MoS 2 /AuNP plasmonic hybrid structure 1 , 43 , 44 . The photoexcited carrier in AuNP was coupled with neutral exciton in MoS 2 . Besides, effectively p-doped MoS 2 due to the induced local tensile strain of AuNP creates the hole charge in the MoS 2 semiconductor. Therefore, the enhancement mechanism in X – and XX can be verified by energy transfer and plasmon-exciton coupling in the MoS 2 /AuNP hybrid structure under the excitation of resonance condition of the AuNP. To tell the optical doping and plasmon-exciton coupling, we measured the excitation power-dependent PL spectra in the monolayer MoS 2 /AuNP hybrid structure (Fig. 5 ). To distinguish the optical doping effects and plasmon-exciton coupling, power-dependent PL spectra of MoS 2 without and with AuNP were shown in Fig. 5 a-b, respectively. The observed PL spectra of MoS 2 with/without AuNP were broadened and red-shifted when excitation power was higher than 100 µW. It can be explained by the thermal exciton-phonon coupling and optical doping effect, as reported elsewhere 45 , 46 . The integrated intensity of X 0 , X – , and XX as a function of excitation power is shown in Fig. 5 c-e, respectively. The X 0 is not drastically enhanced, but the integrated intensity of the X – was enhanced about 3.8–7.8 times. Although the peak intensity of the XX was hardly detectable lower than 10 µW excitations in bare MoS 2 , XX peaks appeared on the MoS 2 /AuNP hybrid structure. The EF of each exciton spectra is shown in Fig. 5 f. It was calculated by the following Eq. 4 7 : \(EF=\frac{{I}_{Plasmonic}}{{I}_{Bare}}\times \frac{{A}_{Bare}}{{A}_{Plasmonic}}\) , (Eq. 2) where the \({I}_{Plasmonic}\) and the \({I}_{Bare}\) refer to the exciton peak intensity in plasmonic hybrid structures and the bare MoS 2 film, respectively. The area of A Bare (1 µm 2 ) and A Plasmonic (0.0176 µm 2 ) is determined by the excitation laser spot and EM field enhancement area in the plasmonic structure, respectively. The calculated enhancement factor of the X 0 , X – , and XX is ~ 100, ~300, and over 300, respectively. The enhancement factor can be calculated over 10 µW excitation power due to the absence of the XX signal in bare MoS 2 , as shown in Fig. 5 f (red). The reason is that the high enhancement factor in MoS 2 /AuNP hybrid structure is the result of the strong electric field confinement originating from the LSPR coupling in AuNP. The optical response of the XX is the optical doping dependence excitonic features, as mentioned in the previous papers 21 , 48 . To investigate the role of anisotropy in the optical response of the non-centrosymmetric AuNP and MoS 2 hybrid structure, Fig. 6 a shows the polarization-resolved PL spectra. The sample structure was rotated to avoid any unwanted optical misalignment to control the incident polarization angle θ . The periodic intensity variations of the PL spectra imply that the MoS 2 excitons strongly correlated with polarization-dependent LSPRs coupling in anisotropic resonators. The quantified normalized intensities of each exciton are shown in Fig. 6 b-d. The orientation of maximum optical response in plasmon-exciton coupling was calculated by the function of I 0 + I 1 cos 2 (θ - θ max ) , where I 0 and I 1 are constants of normalized intensity, and θ max is the angle at the maximum intensity by deconvolution of the Lorentzian function. In previous studies, the general bare MoS 2 film does not correlate with the incident angle of linear polarization θ due to high lattice symmetry 49 , 50 . However, the results of the polarization-resolved PL spectra for each exciton in the MoS 2 /AuNP hybrid structure demonstrate anisotropy of the optical response as a function of the incident orientation. The polarizability ( I 1 ) in X 0 and X – are 0.26 and 0.30, respectively, but XX is 0.55. It is the nature of the plasmonic response that local electric field enhancement is relevant not only to excitation polarization but also to emission spectral range. This result agrees with the larger enhancement for XX than X 0 , again confirming that the polarization-sensitive plasmon excitation is responsible for the pronounced XX generation. In conclusion, we investigated the enhanced plasmon-exciton coupling of X 0 , X – , and XX modes on non-centrosymmetric AuNP and monolayer MoS 2 hybrid structure using absorption, Raman, PL spectra depending on the excitation wavelength, incident power, and polarization control. We explained the mechanism of plasmon-exciton coupling in each exciton mode, of which recombination pathways are followed in excitation, energy transfer, recombination, and EM field enhancement. The hybrid structure of specific plasmonic AuNP and TMDCs showed polarization-dependent optical responses and enhancement. Plasmon-biexciton coupling revealed higher polarizabilities than X 0 and X – because of optical doping-dependent excitonic features and plasmonic resonance. We believe that another degree of freedom to control and engineer the excitonic response provides a new pavement toward the development of optoelectronic nanodevices with TMDCs and supports the plasmonic application of innovative optoelectronic technology. Methods Monolayer MoS 2 synthesis Triangular-shaped MoS 2 growth was carried out in an atmospheric pressure chemical vapor deposition. As Mo precursor, 0.3 g of ammonium heptamolybdate (AHM, Sigma-Aldrich, 431346) was dissolved into distilled (DI) water. The AHM solution was again mixed with NaOH solution (0.125 mol) and 0.2 ml of iodixanol solution (Sigma-Aldrich, Opti Prep, D1556) in the ratio of 0.3 : 2 : 0.2. The solution was spin-coated onto O 2 plasma-treated substrate (300 nm oxide Si wafer), forming a uniform Mo-Na-C precursor matrix. Spinning condition and plasma powers are 4000 rpm for 40 s and 30 W for 1 min, respectively. Then, the substrate was cut into 1 × 1 cm 2 , loaded in zone 2 (outlet) with 0.2 g of S (Sigma-Aldrich, 212392) in zone 1 (inlet). For MoS 2 growth, the tube furnace was ramped to 190°C and 780°C for S (zone 1) and Mo (zone 2). 300 sccm of N 2 was injected for the ramping process (12 min), followed by the growth process with an increased flow rate (1000 sccm, 7 min). Plasmonic Structure Synthesis The resulting split Au nano-rings could be obtained, followed by our previous research (Nano Lett. 2020, 20, 10, 7774–7782). 16 Briefly, Au nano-prisms were employed as starting material en route to synthesize split Au nano-rings. First, vertices of Au nano-prisms were etched to thin Au nano-disks (~ 10 ± 1 nm in height) using Au 3+ ion as an etchant. Subsequently, thin Au nano-disks were converted to Au nano-hexagons through depositing Au followed by an etching step, leading to thick Au nano-disks with a height of ~ 25 ± 2 nm. In the selective edge deposition of Pt, Pt atoms were decorated at the periphery of thick Au nano-disks in part aided by the presence of high-index facets that can reduce the activation energy barrier for Pt nucleation leading to Au@Pt disks. In the next step, the core Au domains were etched away by adding Au 3+ ions resulting in the formation of split Pt nano-rings. Eventually, in the Au regrowth step, Au atoms were homogeneously reduced on the entire surface of split Pt nano-rings, leading to split Au nano-rings. Sample Characterizations An absorption hyper spectra map was obtained to analyze the optical response of the nano-ring/MoS 2 structure. The measurement position was controlled with the piezo sample stage (PI, P-611K020 NanoCube) for precise positioning on the commercial inverted microscope (Nikon, ECLIPSE Ti-U). A broadband illumination of light (Nikon, D-LH/LC, color temperature: 3300 K) was used, and the beam was focused on the sample by 100× objective (Nikon, CFI LU PLAN EPI, NA 0.80, WD 3.5 mm). The reflected optical signal was collected and recorded by the spectrometer (Princeton Instruments, SpectraPro 2300i, 150 lpmm, CCD camera) with sample position. The acquisition time for each point was 100 ms. The reference of reflectance spectra was set as on the bare Si/SiO 2 surface under broadband tungsten lamp illumination. The photoluminescence and Raman spectra were excited by 532 nm DPSS laser (Optoelectronicstech, MGL-III-532) and 632.8 nm He-Ne laser (Thorlabs, HNL210LB) with less than 200 µW after objective lens. For tight focusing, the single-mode fiber (Thorlabs, SM450) was used as a spatial mode filter. The polarization dependence experiment was performed by rotating the sample. PL and Raman hyper-spectra map was obtained with each 15-degree clockwise rotation of the sample. The Lorentzian function was adapted to decompose each spectral peak for X 0 , X – , XX, B 0 excitons in PL and E 1 2g , A 1g peak positions in Raman spectra using Python (Ver 3.7.4, Scipy module). To investigate the surface potential dependency, KPFM and topography were acquired simultaneously by using a commercial scanning probe microscope (Parksystems, XE-NSOM) with an Au-coated cantilever (MikroMasch, NSC-14-Cr-Au). Declarations Acknowledgements This research was supported by Nano·Material Technology Development Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT (2020M3A7B4024925 and 2021M3H4A4079146). This work was supported by the Industrial Strategic Technology Development Program funded by the Ministry of Trade, Industry & Energy (Grant No. 20017214). Author contributions H.K. and J.I. contributed equally to optical experiments and write manuscript with support from S.C., M.S.J., J.S.A., D.P., and G.H.H.. S.J.Y., M.H., and S.P. fabricated and provided the asymmetric gold nanoparticles. J.Y.P. and G.H.H. fabricated and offered the 1L-MoS 2 . K.N. conducted the KPFM measurements and analyzed data. W.P., J.S.A., and D.P. calculated optical response of gold nanoparticle by FEM simulation with COMSOL. All authors provided crucial feedback and helped shape the research. Data availability All data generated and the datasets used and analyzed during the current study are available from the corresponding author on reasonable request. Competing interests The authors declare no competing interests. References Zu, S. et al. Active Control of Plasmon–Exciton Coupling in MoS 2 –Ag Hybrid Nanostructures. Adv. Opt. Mater. 4 , 1463–1469 (2016). Kim, J. H. et al. Dielectric Nanowire Hybrids for Plasmon-Enhanced Light-Matter Interaction in 2D Semiconductors. ACS Nano 14 , 11985–11994 (2020). Mangu, V. S., Zamiri, M., Brueck, S. R. J. & Cavallo, F. Strain engineering, efficient excitonic photoluminescence, and exciton funnelling in unmodified MoS 2 nanosheets. Nanoscale 9 , 16602–16606 (2017). Kaviraj, B. & Sahoo, D. Physics of excitons and their transport in two dimensional transition metal dichalcogenide semiconductors. RSC Adv. 9 , 25439–25461 (2019). Wang, Y. et al. Spin-Valley Locking Effect in Defect States of Monolayer MoS 2 . Nano Lett. 20 , 2129–2136 (2020). Yu, Y. et al. Equally efficient interlayer exciton relaxation and improved absorption in epitaxial and nonepitaxial MoS 2 /WS 2 Heterostructures. Nano Lett. 15 , 486–491 (2015). Sun, J. et al. Strong plasmon-exciton coupling in transition metal dichalcogenides and plasmonic nanostructures. Nanoscale 13 , 4408–4419 (2021). Qin, J. et al. Revealing Strong Plasmon-Exciton Coupling between Nanogap Resonators and Two-Dimensional Semiconductors at Ambient Conditions. Phys. Rev. Lett. 124 , 63902 (2020). Zhou, K., Song, J., Lu, L., Luo, Z. & Cheng, Q. Plasmon-enhanced broadband absorption of MoS 2 -based structure using Au nanoparticles . Opt. Express 27 , 2305 (2019). Yang, Y., Pan, R., Tian, S., Gu, C. & Li, J. Plasmonic hybrids of MoS 2 and 10-nm nanogap arrays for photoluminescence enhancement. Micromachines 11 , 1–12 (2020). Kleemann, M. E. et al. Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature. Nat. Commun. 8 , (2017). Sriram, P., Manikandan, A., Chuang, F. C. & Chueh, Y. L. Hybridizing Plasmonic Materials with 2D-Transition Metal Dichalcogenides toward Functional Applications. Small 16 , 1–27 (2020). Mak, K. F., Lee, C., Hone, J., Shan, J. & Heinz, T. F. Atomically thin MoS 2 : A new direct-gap semiconductor. Phys. Rev. Lett. 105 , 2–5 (2010). Chen, H., Deng, S., Jiang, Y., Wang, H. & Wen, S. Resonance coupling in an individual gold nanorod-monolayer WS 2 heterostructure: Photoluminescence enhancement with spectral broadening. ACS Nano 14 , 13841–13851 (2020). Sun, B. et al. Tailoring of silver nanocubes with optimized localized surface plasmon in a gap mode for a flexible MoS 2 photodetector. Adv. Funct. Mater. 29 , 1900541 (2019). Haddadnezhad, M. et al. Synthesis and Surface Plasmonic Characterization of Asymmetric Au Split Nanorings. Nano Lett. 20 , 7774–7782 (2020). Jian, A. et al. Quantitative investigation of plasmonic hot-electron injection by KPFM. Appl. Surf. Sci. 492 , 644–650 (2019). El Kabbash, M. et al. Plasmon-Exciton Resonant Energy Transfer: Across Scales Hybrid Systems. J. Nanomater. 2016 , (2016). Koo, Y. et al. Tip-Induced Nano-Engineering of Strain, Bandgap, and Exciton Funneling in 2D Semiconductors. Adv. Mater. (2021) doi:10.1002/adma.202008234. Singh, A. et al. Trion formation dynamics in monolayer transition metal dichalcogenides. Phys. Rev. B 93 , 1–5 (2016). Lee, H. S., Kim, M. S., Kim, H. & Lee, Y. H. Identifying multiexcitons in MoS 2 monolayers at room temperature. Phys. Rev. B 93 , 1–6 (2016). Pei, J. et al. Exciton and Trion Dynamics in Bilayer MoS 2 . Small 11 , 6384–6390 (2015). Wang, W. et al. Studying of the Biexciton Characteristics in Monolayer MoS 2 . J. Phys. Chem. C 124 , 1749–1754 (2020). Wang, H. et al. Radiative lifetimes of excitons and trions in monolayers of the metal dichalcogenide MoS 2 . Phys. Rev. B 93 , 1–11 (2016). Chakraborty, B., Matte, H. S. S. R., Sood, A. K. & Rao, C. N. R. Layer-dependent resonant Raman scattering of a few layer MoS 2 . J. Raman Spectrosc. 44 , 92–96 (2013). Kukucska, G. & Koltai, J. Theoretical Investigation of Strain and Doping on the Raman Spectra of Monolayer MoS 2 . Phys. Status Solidi Basic Res. 254 , 1–5 (2017). Iqbal, M. W., Shahzad, K., Akbar, R. & Hussain, G. A review on Raman finger prints of doping and strain effect in TMDCs. Microelectron. Eng. 219 , (2020). Luo, X., Zhai, X., Wang, L. & Lin, Q. Enhanced dual-band absorption of molybdenum disulfide using a plasmonic perfect absorber. Opt. Express 26 , 11658 (2018). Sobhani, A. et al. Enhancing the photocurrent and photoluminescence of single crystal monolayer MoS 2 with resonant plasmonic nanoshells. Appl. Phys. Lett. 104 , 1–5 (2014). Bae, H. et al. Light Absorption and Emission Dominated by Trions in the Type-I van der Waals Heterostructures. ACS Photonics 8 , 1972–1978 (2021). Mueller, T. & Malic, E. Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors. npj 2D Mater. Appl. 2 , 1–12 (2018). Golovynskyi, S. et al. Exciton and trion in few-layer MoS 2 : Thickness- and temperature-dependent photoluminescence. Appl. Surf. Sci. 515 , 146033 (2020). Dulkeith, E. et al. Plasmon emission in photoexcited gold nanoparticles. Phys. Rev. B - Condens. Matter Mater. Phys. 70 , 1–4 (2004). Kumar, V., Nisika, N. & Kumar, M. Modified absorption and emission properties leading to intriguing applications in plasmonic–excitonic nanostructures. Adv. Opt. Mater. 9 , 2001150 (2021). Patil, R. A. et al. Size-controllable synthesis of Bi/Bi2O 3 heterojunction nanoparticles using pulsed Nd:YAG laser deposition and metal-semiconductor-heterojunction-assisted photoluminescence. Nanoscale 8 , 3565–3571 (2016). Abid, K. et al. Photoinduced Enhanced Raman Spectroscopy with Hybrid Au@WS 2 Nanosheets. J. Phys. Chem. C 124 , 20350–20358 (2020). Li, Z. et al. Active Light Control of the MoS 2 Monolayer Exciton Binding Energy. ACS Nano 9 , 10158–10164 (2015). Kang, Y. et al. Plasmonic Hot Electron Induced Structural Phase Transition in a MoS 2 Monolayer. Adv. Mater. 26 , 6467–6471 (2014). Jeong, Y., Kook, Y. M., Lee, K. & Koh, W. G. Metal enhanced fluorescence (MEF) for biosensors: General approaches and a review of recent developments. Biosens. Bioelectron. 111 , 102–116 (2018). Ringler, M. et al. Shaping emission spectra of fluorescent molecules with single plasmonic nanoresonators. Phys. Rev. Lett. 100 , 1–4 (2008). Bang, S. et al. Augmented Quantum Yield of a 2D Monolayer Photodetector by Surface Plasmon Coupling. Nano Lett. 18 , 2316–2323 (2018). Pandey, J. & Soni, A. Unraveling biexciton and excitonic excited states from defect bound states in monolayer MoS 2 . Appl. Surf. Sci. 463 , 52–57 (2019). Lee, H. et al. Radiative control of localized excitons at room temperature with an ultracompact tip-enhanced plasmonic nano-cavity. 1–18 (2020). Dong, J., Zhang, Z., Zheng, H. & Sun, M. Recent Progress on Plasmon-Enhanced Fluorescence. Nanophotonics 4 , 472–490 (2015). Poudel, Y. et al. Active Control of Coherent Dynamics in Hybrid Plasmonic MoS 2 Monolayers with Dressed Phonons. ACS Photonics 6 , 1645–1655 (2019). Mueller, T. & Malic, E. Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors. npj 2D Mater. Appl. 2 , 1–12 (2018). Schmid, T., Opilik, L., Blum, C. & Zenobi, R. Nanoscale chemical imaging using tip-enhanced raman spectroscopy: A critical review. Angew. Chemie - Int. Ed. 52 , 5940–5954 (2013). Panasci, S. E. et al. Strain, Doping, and Electronic Transport of Large Area Monolayer MoS 2 Exfoliated on Gold and Transferred to an Insulating Substrate. ACS Appl. Mater. Interfaces 13 , 31248–31259 (2021). Shi, Y. et al. The Polarization Properties of the Reflection Spectra of Single-Layer MoS 2 and ReS 2 on SiO 2 /Si and Quartz Substrates. Nanoscale Res. Lett. 15 , 1–6 (2020). Chen, S. et al. Anisotropic Plasmonic Nanostructure Induced Polarization Photoresponse for MoS 2 -Based Photodetector. Adv. Mater. Interfaces 7 , 2–9 (2020). Additional Declarations No competing interests reported. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-2249049","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":150712119,"identity":"aabe5f49-ad6b-4dc7-b923-0fb451151ad9","order_by":0,"name":"Hyuntae Kim","email":"","orcid":"","institution":"Incheon National University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Hyuntae","middleName":"","lastName":"Kim","suffix":""},{"id":150712120,"identity":"b8e16de7-94dd-4562-979e-ee02bdd5b369","order_by":1,"name":"Jaeseung Im","email":"","orcid":"","institution":"Incheon National University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Jaeseung","middleName":"","lastName":"Im","suffix":""},{"id":150712121,"identity":"fe49b0f2-20d9-49ae-975b-44e7a7a2a740","order_by":2,"name":"Sung Jae Yoo","email":"","orcid":"","institution":"Sungkyunkwan University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Sung","middleName":"Jae","lastName":"Yoo","suffix":""},{"id":150712122,"identity":"ef6deb86-c206-4a5d-8c53-927af21df761","order_by":3,"name":"MohammadNavid Haddadnezhad","email":"","orcid":"","institution":"Sungkyunkwan University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"MohammadNavid","middleName":"","lastName":"Haddadnezhad","suffix":""},{"id":150712124,"identity":"9dc94c68-ba0b-4b2d-93d5-dff7a323b034","order_by":4,"name":"Kiin Nam","email":"","orcid":"","institution":"Incheon National University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Kiin","middleName":"","lastName":"Nam","suffix":""},{"id":150712127,"identity":"d357afd5-8438-46c2-928f-9f42734aa2a7","order_by":5,"name":"Jin Young Park","email":"","orcid":"","institution":"Incheon National University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Jin","middleName":"Young","lastName":"Park","suffix":""},{"id":150712129,"identity":"0e4a1ca7-069d-452f-be62-43af161f70c0","order_by":6,"name":"Woongkyu Park","email":"","orcid":"","institution":"Korea Photonics Technology Institute (KOPTI)","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Woongkyu","middleName":"","lastName":"Park","suffix":""},{"id":150712130,"identity":"1ef33298-a70f-4119-850d-369f349d4c99","order_by":7,"name":"Sungho Park","email":"","orcid":"","institution":"Sungkyunkwan University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Sungho","middleName":"","lastName":"Park","suffix":""},{"id":150712132,"identity":"662fdd14-1536-4e4b-a32a-1028c459bfb9","order_by":8,"name":"Gang Hee Han","email":"","orcid":"","institution":"Incheon National University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Gang","middleName":"Hee","lastName":"Han","suffix":""},{"id":150712134,"identity":"ed1809dc-9921-4fe7-893c-aacc6b3915a2","order_by":9,"name":"Jae Sung Ahn","email":"","orcid":"","institution":"Korea Photonics Technology Institute (KOPTI)","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Jae","middleName":"Sung","lastName":"Ahn","suffix":""},{"id":150712137,"identity":"1de97f1a-6f0a-48c3-b3a1-2ffbe56c588c","order_by":10,"name":"Doojae Park","email":"","orcid":"","institution":"Hallym University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Doojae","middleName":"","lastName":"Park","suffix":""},{"id":150712138,"identity":"b0adaca4-b3c0-43bb-8f4e-f17d1a3b305b","order_by":11,"name":"Mun Seok Jeong","email":"","orcid":"","institution":"Hanyang University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Mun","middleName":"Seok","lastName":"Jeong","suffix":""},{"id":150712139,"identity":"f0d9db17-417b-4c57-b891-98f5112e1e69","order_by":12,"name":"Soobong Choi","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAtElEQVRIiWNgGAWjYDACCQY2BgYDGx4oN4FoLWkka2E4DOMSoUV+dvOzBx8KzsuYSyQwfvjBkJZPUIvBnWPmhjMMbvNYzkhgluxhyLFsIKhFIodNmgeoxeBGAoM0A0OFAWGHzQBrOQfSwvybKC0MN8BaDoC0sAFtySGsBegXM8kZBsk8Bmcetln2GKQR4TBgiEl8+GNnb3A8+fCNHxXJRDgMARgbgJaSomEUjIJRMApGAU4AAOMhMqqaCu6pAAAAAElFTkSuQmCC","orcid":"","institution":"Incheon National University","correspondingAuthor":true,"submittingAuthor":false,"prefix":"","firstName":"Soobong","middleName":"","lastName":"Choi","suffix":""}],"badges":[],"createdAt":"2022-11-08 03:29:13","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-2249049/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-2249049/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":28971365,"identity":"cd6540d5-ae2f-45b4-9897-ec90c3cf2971","added_by":"auto","created_at":"2022-11-11 21:30:30","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":3593007,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eMonolayer MoS\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/sub\u003e\u003cstrong\u003e/AuNP characterization. a\u003c/strong\u003e Optical image of monolayer MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid. The inset is cross-sectional schematics of structure. \u003cstrong\u003eb\u003c/strong\u003e SEM image of non-centrosymmetric AuNP. The inset represents a dimension of AuNP. \u003cstrong\u003ec\u003c/strong\u003e 532 nm excitation Raman scattering spectra. \u003cstrong\u003ed\u003c/strong\u003e The relative reflectance spectra in the 550 ~ 800 nm range. Si/SiO\u003csub\u003e2\u003c/sub\u003e was set as the reference surface. \u003cstrong\u003ee\u003c/strong\u003e Simulation result of absorbance spectrum on the AuNP, which result set the 90 degrees of incident polarization. The red line indicates the resonance excitation wavelength of 632.8 nm. The inset shows the electric field distribution of AuNP. \u003cstrong\u003ef\u003c/strong\u003e FEM simulation result of polarization dependence absorbance strength.\u003c/p\u003e","description":"","filename":"Figure1af.jpg","url":"https://assets-eu.researchsquare.com/files/rs-2249049/v1/d20466ade9b486549995bc3f.jpg"},{"id":28971362,"identity":"d4171ce3-b946-47ee-abe3-ce105e50e700","added_by":"auto","created_at":"2022-11-11 21:30:30","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":3502930,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ePL spectra of 532 nm and 632.8 nm excitation and mechanism of plasmon-exciton coupling. \u003c/strong\u003ePL spectra for \u003cstrong\u003ea\u003c/strong\u003e 532 nm and \u003cstrong\u003ec\u003c/strong\u003e 632.8 nm excitation. Normalized PL spectra for \u003cstrong\u003eb\u003c/strong\u003e 532 nm and \u003cstrong\u003ed\u003c/strong\u003e 632.8 nm excitation. \u003cstrong\u003ee\u003c/strong\u003e Schematics of plasmon-exciton coupling mechanisms of each exciton mode on the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid. (1) excitation process. (2) energy transfer. (3) recombination process. (4) EM field enhancement.\u003c/p\u003e","description":"","filename":"Figure2ae.jpg","url":"https://assets-eu.researchsquare.com/files/rs-2249049/v1/f16a2293b557e603bc1e596e.jpg"},{"id":28971913,"identity":"35ce64fd-7a6c-4de9-97af-c5b0c5702299","added_by":"auto","created_at":"2022-11-11 21:38:30","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":4617693,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eScanning probe microscope results and potential diagram. a\u003c/strong\u003e Topography image and line profile at the white line (inset). \u003cstrong\u003eb\u003c/strong\u003e KPFM result of electrostatic potentials (scale bar : 5 mm). The inset shows the magnification of the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid (size : 700 × 700 nm\u003csup\u003e2\u003c/sup\u003e) \u003cstrong\u003ec\u003c/strong\u003e Schematics of the energy band diagram. \u003cstrong\u003ed\u003c/strong\u003e Distribution of pixels in the KPFM result. \u003cstrong\u003ee\u003c/strong\u003e The line profile of topograph and CPD on the white line in the inset of \u003cstrong\u003eb\u003c/strong\u003e.\u003c/p\u003e","description":"","filename":"Figure3ae.jpg","url":"https://assets-eu.researchsquare.com/files/rs-2249049/v1/d50b80a120f42ba891485893.jpg"},{"id":28971359,"identity":"8727a871-7c1b-4204-ae82-018023eddb42","added_by":"auto","created_at":"2022-11-11 21:30:30","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":3185789,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ePL hyper spectra of 632.8 nm excitation and deconvolution results. a\u003c/strong\u003e Integrated PL intensity mapping image. (Circle) Monolayer bare MoS\u003csub\u003e2\u003c/sub\u003e. (Square) Monolayer MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid. PL spectra and Lorentzian deconvolution results for each exciton in \u003cstrong\u003eb\u003c/strong\u003e the bare MoS\u003csub\u003e2\u003c/sub\u003e and \u003cstrong\u003ec\u003c/strong\u003e the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid. \u003cstrong\u003ed\u003c/strong\u003e The hyperspectral PL image on the red line in \u003cstrong\u003ea\u003c/strong\u003e. \u003cstrong\u003ee\u003c/strong\u003e integrated intensity and \u003cstrong\u003ef\u003c/strong\u003e center energy from the result of deconvoluted PL spectra in \u003cstrong\u003eb\u003c/strong\u003e and \u003cstrong\u003ec\u003c/strong\u003e.\u003c/p\u003e","description":"","filename":"Figure4af.jpg","url":"https://assets-eu.researchsquare.com/files/rs-2249049/v1/2e8f4a44b00c90947626e7a0.jpg"},{"id":28971914,"identity":"fe27e311-8dd8-489c-a24e-77dac7823bbb","added_by":"auto","created_at":"2022-11-11 21:38:30","extension":"jpg","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":3172152,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eFundamental power dependence normalized PL spectra and deconvolution results. \u003c/strong\u003ePower dependence Normalized PL spectra in\u003cstrong\u003e a\u003c/strong\u003e the monolayer bare MoS\u003csub\u003e2\u003c/sub\u003e and \u003cstrong\u003eb\u003c/strong\u003e the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure. The integrated intensity of deconvolution results for \u003cstrong\u003ec\u003c/strong\u003e neutral exciton (X\u003csup\u003e0\u003c/sup\u003e), \u003cstrong\u003ed\u003c/strong\u003e trion (X\u003csup\u003e–\u003c/sup\u003e), and \u003cstrong\u003ee\u003c/strong\u003e biexciton (XX), respectively. \u003cstrong\u003ef\u003c/strong\u003e Calculated enhancement factor of each exciton mode.\u003c/p\u003e","description":"","filename":"Figure5af.jpg","url":"https://assets-eu.researchsquare.com/files/rs-2249049/v1/5c09f5b927c45e591c5c975a.jpg"},{"id":28971364,"identity":"f6001448-566d-44f5-b66f-d1cfe4b99404","added_by":"auto","created_at":"2022-11-11 21:30:30","extension":"jpg","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":3417529,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ePolarization dependency of each exciton mode in the MoS\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/sub\u003e\u003cstrong\u003e/AuNP hybrid. a\u003c/strong\u003e Polarization-dependent hyperspectral PL image in the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid. The normalized intensity of deconvoluted PL spectra depends on the excitation polarization for \u003cstrong\u003eb\u003c/strong\u003e the X\u003csup\u003e0\u003c/sup\u003e, \u003cstrong\u003ec\u003c/strong\u003e X\u003csup\u003e–\u003c/sup\u003e, and \u003cstrong\u003ed\u003c/strong\u003e XX modes.\u003c/p\u003e","description":"","filename":"Figure6ad.jpg","url":"https://assets-eu.researchsquare.com/files/rs-2249049/v1/41daa56ae496bcaac9faf018.jpg"},{"id":28971916,"identity":"3b790508-7e2a-4ae4-b0c4-362920913aec","added_by":"auto","created_at":"2022-11-11 21:38:36","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1364347,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-2249049/v1/74b06813-f50c-411d-bcfd-137cf425f121.pdf"},{"id":28971915,"identity":"b0d844fe-fabd-421e-a4f4-97e7b0597767","added_by":"auto","created_at":"2022-11-11 21:38:30","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":125519,"visible":true,"origin":"","legend":"","description":"","filename":"Supplementaryinformation.pdf","url":"https://assets-eu.researchsquare.com/files/rs-2249049/v1/67e05ef136bdb15ef681df48.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"Plasmon-exciton couplings in the MoS2/AuNP plasmonic hybrid structure","fulltext":[{"header":"Introduction","content":"\u003cp\u003eOptical response in transition metal dichalcogenides (TMDCs) could be engineered by the van der Waals heterostructures, chemical treatment, defect controlling and inducing the local strain, etc\u003csup\u003e\u003cspan additionalcitationids=\"CR2 CR3 CR4 CR5\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e\u003c/sup\u003e. Among them, the hybrid structure of noble metal nanoparticles with TMDCs has been introduced to enhance the light-matter interaction caused by plasmon-exciton couplings\u003csup\u003e\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e,\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e\u003c/sup\u003e. The techniques for enhancing the optical response are based on the local electromagnetic (EM) field confinements on a metallic nanostructure that is referred to as the localized surface plasmon resonance (LSPR)\u003csup\u003e\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e\u003c/sup\u003e. The localized EM field increases the absorption and emission rate in plasmonic hybrid structures. In addition, the orientation of the hotspots of the EM field could be controlled by designing the plasmonic nanoparticles platform, gap distance, and local environment structure\u003csup\u003e\u003cspan additionalcitationids=\"CR11\" citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eThe molybdenum disulfide (MoS\u003csub\u003e2\u003c/sub\u003e) is one of the noble candidates for functional optical devices due to its unique physical properties, such as tightly bounded excitons, chemical stability, and visible spectral region of photoluminescence (PL) spectra, bandgap tuning by local induced strain\u003csup\u003e\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e\u003c/sup\u003e. In the previous studies of MoS\u003csub\u003e2\u003c/sub\u003e/plasmonic hybrid structure, these plasmonic nanoparticles are employed in various structures, such as nano-rings, heterodimers, plates, rods, 3D cubes, and split rings, etc\u003csup\u003e\u003cspan additionalcitationids=\"CR15\" citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e\u003c/sup\u003e. The mechanism of plasmon-exciton couplings was explained by hot-electron injection, energy transfer, bandgap funneling, and EM field enhancement\u003csup\u003e\u003cspan additionalcitationids=\"CR18\" citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eThe exciton dynamics of photogenerated quasiparticles, which are the neutral excitons(X\u003csup\u003e0\u003c/sup\u003e), trions(X\u003csup\u003e\u0026ndash;\u003c/sup\u003e), and biexcitons(XX), are electronically excited states consisting of an electron and a hole. The recombination processes of excitons from X\u003csup\u003e0\u003c/sup\u003e to X\u003csup\u003e\u0026ndash;\u003c/sup\u003e and XX are affected by the background carrier concentrations and are also controlled by Fermi level tunning by local doping\u003csup\u003e\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e\u003c/sup\u003e. The optical response of XX in MoS\u003csub\u003e2\u003c/sub\u003e depends on the optical doping. However, the X\u003csup\u003e0\u003c/sup\u003e and X\u003csup\u003e\u0026ndash;\u003c/sup\u003e do on the electrical doping dependence\u003csup\u003e\u003cspan additionalcitationids=\"CR22 CR23\" citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u003c/sup\u003e. So far as we know, the coupling mechanism of plasmon-exciton has remained vague due to its complex recombination pathways in each exciton mode.\u003c/p\u003e \u003cp\u003eIn this paper, we investigate the intertwined mechanism of plasmon-exciton couplings in X\u003csup\u003e0\u003c/sup\u003e, X\u003csup\u003e\u0026ndash;\u003c/sup\u003e, and XX modes on the hybrid structure of the monolayer MoS\u003csub\u003e2\u003c/sub\u003e and non-centrosymmetric Au nanoparticle (AuNP). To characterize the optical response, we measured the absorption, Raman, and PL spectra depending on the excitation wavelength, incident power, and polarization. Also, non-centrosymmetric AuNP opens the possibility to control the plasmon-exciton coupling due to the optical response dependence on the polarization. The power-dependent PL spectra of each exciton mode are used to identify the optical doping effect and charge recombination processes in multiexciton modes.\u003c/p\u003e"},{"header":"Results","content":"\u003cp\u003eFigure \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ea shows the optical images of the MoS\u003csub\u003e2\u003c/sub\u003e/plasmonic hybrid structures. The spatial density of the AuNPs is 0.13 particles/\u0026micro;m\u003csup\u003e2\u003c/sup\u003e. The indicated regions are the bare MoS\u003csub\u003e2\u003c/sub\u003e (circle), MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure (square), and AuNP particle without MoS\u003csub\u003e2\u003c/sub\u003e (arrow), respectively. The high-resolution scanning electron microscope (SEM) image shows the geometrical shape of AuNP (Fig. \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003eb). The AuNPs have an outer radius of ~\u0026thinsp;75 nm, an inner radius of ~\u0026thinsp;25 nm, and a gap width of ~\u0026thinsp;10 nm, respectively (inset of Fig. \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003eb).\u003c/p\u003e\n\u003cp\u003eAs depicted in Fig. \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ec, the Raman spectra of the monolayer MoS\u003csub\u003e2\u003c/sub\u003e and MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure under 532 nm excitations clearly show A\u003csub\u003e1g\u003c/sub\u003e and E\u003csup\u003e1\u003c/sup\u003e\u003csub\u003e2g\u003c/sub\u003e peaks. The frequency difference of Raman modes between the E\u003csup\u003e1\u003c/sup\u003e\u003csub\u003e2g\u003c/sub\u003e and A\u003csub\u003e1g\u003c/sub\u003e in the monolayer MoS\u003csub\u003e2\u003c/sub\u003e was observed as 20.4 cm\u003csup\u003e-\u003cspan class=\"CitationRef\"\u003e1\u003c/span\u003e\u003c/sup\u003e, which is consistent with the previous studies\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e25\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e26\u003c/span\u003e\u003c/sup\u003e. On the other hand, in the case of the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure, the relative peak intensity ratio between A\u003csub\u003e1g\u003c/sub\u003e and E\u003csup\u003e1\u003c/sup\u003e\u003csub\u003e2g\u003c/sub\u003e modes, A\u003csub\u003e1g\u003c/sub\u003e/E\u003csup\u003e1\u003c/sup\u003e\u003csub\u003e2g\u003c/sub\u003e, was increased. It can be explained as a result of the p-doping effect due to the tensile strain of the MoS\u003csub\u003e2\u003c/sub\u003e surface on the AuNP\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e27\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e\n\u003cp\u003eFigure \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ed shows the reflectance from Si/SiO\u003csub\u003e2\u003c/sub\u003e, AuNP, MoS\u003csub\u003e2\u003c/sub\u003e, and MoS\u003csub\u003e2\u003c/sub\u003e/AuNP. The Si/SiO\u003csub\u003e2\u003c/sub\u003e was used as a reference surface. AuNP does not show strong resonant absorption feature, but about 5% decreased reflectance in the 550 nm to 800 nm spectral range because of the LSPRs absorption. The MoS\u003csub\u003e2\u003c/sub\u003e and MoS\u003csub\u003e2\u003c/sub\u003e/AuNP show two absorption dips at ~\u0026thinsp;651 nm (E\u003csub\u003eA\u003c/sub\u003e) and ~\u0026thinsp;604 nm (E\u003csub\u003eB\u003c/sub\u003e), which correspond to the absorption band of A and B excitons in MoS\u003csub\u003e2\u003c/sub\u003e, respectively\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e28\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e29\u003c/span\u003e\u003c/sup\u003e. In the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure, the reflectance was additionally decreased (i.e., absorption increased) at E\u003csub\u003eA\u003c/sub\u003e and E\u003csub\u003eB\u003c/sub\u003e by 5% than the bare MoS\u003csub\u003e2\u003c/sub\u003e monolayer. The absorption enhancement originates from the response of LSPRs on the AuNP with the resonant energy transfer\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e30\u003c/span\u003e\u003c/sup\u003e. Therefore, the excitation wavelength of 632.8 nm is suitable for enhanced absorption via LSPR.\u003c/p\u003e\n\u003cp\u003eIn addition, the absorbance spectrum of the AuNP was calculated by the finite element method (FEM) simulation, as shown in Fig. \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ee-f. The simulated absorbance spectrum has two resonance peaks at 615 nm and 680 nm. In our experiment, two excitation wavelengths of the laser (632.8 nm and 532 nm) were used to compare the on/off resonance characteristics of the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure (Fig. \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ee). The AuNPs have polarization-dependent absorption, which originated from their non-centrosymmetric structure\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e31\u003c/span\u003e\u003c/sup\u003e. The absorption can be enhanced only when the polarization and the excitation wavelength of the light are satisfied with the resonance condition of the AuNP (Fig. \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ef).\u003c/p\u003e\n\u003cp\u003eFigure \u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003ea\u0026ndash;d shows the PL spectra with 532 nm and 632.8 nm excitation to investigate the plasmonic response of the hybrid structure, respectively. The peak positions of the PL (denoted as A and B, respectively) are 1.90\u0026ndash;1.95 eV and 2.05\u0026ndash;2.10 eV, respectively, which are consistent with the previous results for monolayer MoS\u003csub\u003e2\u003c/sub\u003e\u003csup\u003e32\u003c/sup\u003e.\u003c/p\u003e\n\u003cp\u003eThe peak intensity of the A exciton was enhanced about 1.5 and 2.4 times under 532 nm and 632.8 nm excitation, respectively. The normalized PL spectra with 532 nm excitation are shown in Fig. \u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003eb. The normalized spectrum barely changed by the AuNPs, owing to the off-resonance excitation of the LSPRs.\u003c/p\u003e\n\u003cp\u003eIn contrast, 632.8 nm excited PL spectra showed significant changes with peak positions and line width, as shown in Fig. \u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003ed. The peak position of the spectrum is red-shifted, and the linewidth of the spectrum is broadened in MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure. The observed phenomena can be described by the complex interaction between AuNP and MoS\u003csub\u003e2\u003c/sub\u003e, such as plasmon-exciton coupling, local doping, strain, etc.\u003c/p\u003e"},{"header":"Discussion","content":"\u003cp\u003eWe suggest that the exciton-plasmon coupling scheme can explain the exciton recombination mechanism in the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure. As depicted in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee, the energy transfer mechanism was demonstrated considering selective exciton excitation in the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure under the resonant excitation of LSPRs. The recombination of each exciton was followed by excitation, energy transfer, recombination, and EM field enhancement.\u003c/p\u003e \u003cp\u003eThe first step of the recombination pathways in the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure is the excitation process. The optically excited electron in the AuNP has radiative and nonradiative pathways in the relaxation processes. The nonradiative relaxation of the photoexcited carrier in AuNP, such as carrier-carrier scattering, is much faster than radiative electron-hole recombination\u003csup\u003e\u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e\u003c/sup\u003e. The strength of nonradiative relaxation processes depends on the resonant plasmonic optical response of the AuNP. Also, the resonant energy transfer in nonradiative relaxation processes has to consider the metal-semiconductor energy band alignment in the plasmonic hybrid structure\u003csup\u003e\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e\u003c/sup\u003e. The condition of resonance energy transfer was estimated through absorption spectra and simulation, as mentioned in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e.\u003c/p\u003e \u003cp\u003eThe second step is the energy transfer between the AuNP and the monolayer MoS\u003csub\u003e2\u003c/sub\u003e. To investigate the energy transfer mechanism, PL emission and electrostatic characteristics were measured. The line width broadening in PL spectra implies the excessive charge density in the excitonic feature of the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure under resonant excitation (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea-d). Figure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea-b show the topography and surface potential map of MoS\u003csub\u003e2\u003c/sub\u003e/AuNP plasmonic hybrid structures, respectively. The thickness of the MoS\u003csub\u003e2\u003c/sub\u003e is ~\u0026thinsp;0.75 nm on the edge of the monolayer MoS\u003csub\u003e2\u003c/sub\u003e. In addition, monolayer MoS\u003csub\u003e2\u003c/sub\u003e film has wrinkles due to ~\u0026thinsp;30 nm of the AuNP particles. Notably, the topography and potential images have different appearances on MoS\u003csub\u003e2\u003c/sub\u003e/AuNP (square) and bare MoS\u003csub\u003e2\u003c/sub\u003e. Besides, the surface, including flat and wrinkled areas without the nanoparticles (circle), does not make a distinct electrical potential difference.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAs illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec, the contact potential difference (eV\u003csub\u003eCPD\u003c/sub\u003e) on the MoS\u003csub\u003e2\u003c/sub\u003e and hybrid structures is 567.15 meV and 513.61 meV, respectively. The equilibrium state of the Fermi level was p-doped due to the \u0026minus;\u0026thinsp;55.54 meV Fermi level modulation by contact on the AuNP and MoS\u003csub\u003e2\u003c/sub\u003e. The contact in the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure was estimated as Ohmic contact due to the smaller work function of MoS\u003csub\u003e2\u003c/sub\u003e (5.15 eV) than AuNP in the case of p-doped semiconductors\u003csup\u003e\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e\u003c/sup\u003e. Notably, the photo-excited carriers in AuNP and plasmonic hot-carriers moved toward the MoS\u003csub\u003e2\u003c/sub\u003e film by the downward energy band bending at the interface\u003csup\u003e\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e\u003c/sup\u003e. The carrier injection in the interface can modulate the exciton bindings in the MoS\u003csub\u003e2\u003c/sub\u003e film\u003csup\u003e\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e,\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed-e show the electrical potential difference on the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP plasmonic hybrid structure with the V\u003csub\u003eCPD\u003c/sub\u003e distribution and profile. The difference of the eV\u003csub\u003eCPD\u003c/sub\u003e between the monolayer MoS\u003csub\u003e2\u003c/sub\u003e and Si/SiO\u003csub\u003e2\u003c/sub\u003e substrate is \u003cb\u003e\u0026minus;\u0026thinsp;5\u003c/b\u003e0 meV. However, the distribution of the eV\u003csub\u003eCPD\u003c/sub\u003e on the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP structures was decreased to \u003cb\u003e\u0026minus;\u0026thinsp;5\u003c/b\u003e5.54 meV compared to the flat and wrinkled surface of MoS\u003csub\u003e2\u003c/sub\u003e. The result of the KPFM demonstrates that the monolayer MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure was p-doped, as mentioned in Raman spectra (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ec).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe recombination process in each exciton mode was analyzed from the deconvoluted PL spectra. The energy relaxation in neutral exciton was recombinant to the trion and biexciton mode due to the plasmon-exciton coupling (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e). The interaction between MoS\u003csub\u003e2\u003c/sub\u003e and the AuNP can be explained by introducing plasmonic coupling contributions in the excitation and emission processes of excitons. The majority of the PL enhancement was caused by induced local electric field enhancement at the interface between MoS\u003csub\u003e2\u003c/sub\u003e and AuNP\u003csup\u003e\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e\u003c/sup\u003e. The total enhancement \u003cem\u003eg(ω)\u003c/em\u003e on the plasmonic hybrid structures of the aggregated MoS\u003csub\u003e2\u003c/sub\u003e/AuNP is considered in two independent processes, excitation enhancement \u003cem\u003eg\u003c/em\u003e\u003csub\u003e\u003cem\u003eexc\u003c/em\u003e\u003c/sub\u003e\u003cem\u003e(ω\u003c/em\u003e\u003csub\u003e\u003cem\u003eexc\u003c/em\u003e\u003c/sub\u003e\u003cem\u003e)\u003c/em\u003e and emission enhancement \u003cem\u003eg\u003c/em\u003e\u003csub\u003e\u003cem\u003eem\u003c/em\u003e\u003c/sub\u003e\u003cem\u003e(ω)\u003c/em\u003e as following equations as\u003csup\u003e\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e\u003c/sup\u003e:\u003c/p\u003e \u003cp\u003e \u003cem\u003eg(ω)\u0026thinsp;=\u0026thinsp;g\u003c/em\u003e \u003csub\u003e \u003cem\u003eexc\u003c/em\u003e \u003c/sub\u003e \u003cem\u003e(ω\u003c/em\u003e \u003csub\u003e \u003cem\u003eexc\u003c/em\u003e \u003c/sub\u003e \u003cem\u003e)g\u003c/em\u003e \u003csub\u003e \u003cem\u003eem\u003c/em\u003e \u003c/sub\u003e \u003cem\u003e(ω)\u003c/em\u003e, (Eq.\u0026nbsp;1)\u003c/p\u003e \u003cp\u003ewhere ω is the frequency of the EM field, and \u003cem\u003eω\u003c/em\u003e\u003csub\u003e\u003cem\u003eexc\u003c/em\u003e\u003c/sub\u003e is the excitation laser frequency. The enhancement factor (EF) is complex to calculate due to the various exciton dynamics of the radiative/nonradiative decay rates and energy transfer. The energy transfer in the emission process is the response of interband charge transitions in the semiconductor and excited carrier transfer from the plasmonic structure. In addition, the local field enhancement depends on the polarization of the incident light according to the plasmonic response.\u003c/p\u003e \u003cp\u003eMoreover, the monolayer MoS\u003csub\u003e2\u003c/sub\u003e has a strong absorption rate and PL emission spectra due to the weak dielectric screening and atomically thin spatial confinement of carriers. Neutral excitons (X\u003csup\u003e0\u003c/sup\u003e) in MoS\u003csub\u003e2\u003c/sub\u003e can be coupled with the bound state of an electron and hole in the presence of residual excessive charge carriers under excitation. The charged neutral exciton of quasiparticles, called trions (X\u003csup\u003e\u0026ndash;\u003c/sup\u003e), consists of two electrons and one hole. Also, the biexcitons (XX) are the formation of molecular states consisting of two excitons.\u003c/p\u003e \u003cp\u003eTo estimate the plasmon-exciton coupling for each exciton, Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea-c show that the integrated PL intensity map and spectra in the MoS\u003csub\u003e2\u003c/sub\u003e (circle) and MoS\u003csub\u003e2\u003c/sub\u003e/AuNP (square) under 200 \u0026micro;W at 632.8 nm excitations. The PL spectra were deconvoluted by Lorentzian formation for the intensity and center frequency estimation in each exciton mode (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb-f) \u003csup\u003e\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e,\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e,\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e\u003c/sup\u003e. In Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb-c, the total PL peak intensities (gray) are 2.14 times higher in plasmonic hybrid structures than bare MoS\u003csub\u003e2\u003c/sub\u003e film, as same in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec-d. A significant enhancement in the 632.8 nm excitation was caused by the EM field resonance on the AuNP compared to the 532 nm excitation, as mentioned. Also, the change of PL intensity was barely observed on the natural wrinkles in the flake, which is consistent with the result in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb. The linewidth broadening of the total PL spectra on the region of MoS\u003csub\u003e2\u003c/sub\u003e/AuNP can be explained by increasing contributions of the X\u003csup\u003e\u0026ndash;\u003c/sup\u003e and XX states.\u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed shows the hyper spectral image of PL in the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure along the red line in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea. The observed spatially resolved PL intensity shows that the XX peak was clearly enhanced only at the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee shows the peak enhancement of each exciton mode, which results using the deconvolution of the PL spectra in the bare MoS\u003csub\u003e2\u003c/sub\u003e and MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure. The enhancement of X\u003csup\u003e0\u003c/sup\u003e, X\u003csup\u003e\u0026ndash;\u003c/sup\u003e, and XX is 2.29, 4.96, and 4.90 times, respectively. The intensities of X\u003csup\u003e\u0026ndash;\u003c/sup\u003e and XX are more than two times larger than X\u003csup\u003e0\u003c/sup\u003e due to the large \u003cem\u003eg\u003c/em\u003e\u003csub\u003e\u003cem\u003eexc\u003c/em\u003e\u003c/sub\u003e\u003cem\u003e(ω\u003c/em\u003e\u003csub\u003e\u003cem\u003eexc\u003c/em\u003e\u003c/sub\u003e\u003cem\u003e)\u003c/em\u003e of plasmon-exciton coupling and energy transfer.\u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ef shows the center energy difference in each exciton mode. The peak shift of neutral exciton is \u0026minus;\u0026thinsp;5.38 meV in MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure. Also, the difference of center frequency in X\u003csup\u003e\u0026ndash;\u003c/sup\u003e and XX is 25.68 meV and 44.69 meV, respectively. The peak shifts of X\u003csup\u003e\u0026ndash;\u003c/sup\u003e and XX are significantly larger than X\u003csup\u003e0\u003c/sup\u003e because of the effectively local p-dopping by the AuNP applied local tensile strain and energy transfer in direct contact between nanoparticle and MoS\u003csub\u003e2\u003c/sub\u003e. It is observed that the broadening of the peak (see supplementary information) denotes the increase of the recombination rate, which also supports the existence of the local p-doping effect and the effective charge transfer from metal nanoparticles to the MoS\u003csub\u003e2\u003c/sub\u003e film.\u003c/p\u003e \u003cp\u003eThe analyzed each exciton mode from PL spectra under 632.8 nm excitation shows the plasmon-exciton coupling and energy transfer mechanism in MoS\u003csub\u003e2\u003c/sub\u003e/AuNP plasmonic hybrid structure\u003csup\u003e\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e,\u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e,\u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e\u003c/sup\u003e. The photoexcited carrier in AuNP was coupled with neutral exciton in MoS\u003csub\u003e2\u003c/sub\u003e. Besides, effectively p-doped MoS\u003csub\u003e2\u003c/sub\u003e due to the induced local tensile strain of AuNP creates the hole charge in the MoS\u003csub\u003e2\u003c/sub\u003e semiconductor. Therefore, the enhancement mechanism in X\u003csup\u003e\u0026ndash;\u003c/sup\u003e and XX can be verified by energy transfer and plasmon-exciton coupling in the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure under the excitation of resonance condition of the AuNP.\u003c/p\u003e \u003cp\u003eTo tell the optical doping and plasmon-exciton coupling, we measured the excitation power-dependent PL spectra in the monolayer MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e). To distinguish the optical doping effects and plasmon-exciton coupling, power-dependent PL spectra of MoS\u003csub\u003e2\u003c/sub\u003e without and with AuNP were shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea-b, respectively. The observed PL spectra of MoS\u003csub\u003e2\u003c/sub\u003e with/without AuNP were broadened and red-shifted when excitation power was higher than 100 \u0026micro;W. It can be explained by the thermal exciton-phonon coupling and optical doping effect, as reported elsewhere\u003csup\u003e\u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e45\u003c/span\u003e,\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eThe integrated intensity of X\u003csup\u003e0\u003c/sup\u003e, X\u003csup\u003e\u0026ndash;\u003c/sup\u003e, and XX as a function of excitation power is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ec-e, respectively. The X\u003csup\u003e0\u003c/sup\u003e is not drastically enhanced, but the integrated intensity of the X\u003csup\u003e\u0026ndash;\u003c/sup\u003e was enhanced about 3.8\u0026ndash;7.8 times. Although the peak intensity of the XX was hardly detectable lower than 10 \u0026micro;W excitations in bare MoS\u003csub\u003e2\u003c/sub\u003e, XX peaks appeared on the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure.\u003c/p\u003e \u003cp\u003eThe EF of each exciton spectra is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ef. It was calculated by the following Eq.\u0026nbsp;4\u003csup\u003e7\u003c/sup\u003e :\u003c/p\u003e \u003cp\u003e \u003cspan class=\"InlineEquation\"\u003e \u003cspan class=\"mathinline\"\u003e\\(EF=\\frac{{I}_{Plasmonic}}{{I}_{Bare}}\\times \\frac{{A}_{Bare}}{{A}_{Plasmonic}}\\)\u003c/span\u003e \u003c/span\u003e, (Eq.\u0026nbsp;2)\u003c/p\u003e \u003cp\u003ewhere the \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({I}_{Plasmonic}\\)\u003c/span\u003e\u003c/span\u003e and the \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({I}_{Bare}\\)\u003c/span\u003e\u003c/span\u003e refer to the exciton peak intensity in plasmonic hybrid structures and the bare MoS\u003csub\u003e2\u003c/sub\u003e film, respectively. The area of \u003cem\u003eA\u003c/em\u003e\u003csub\u003e\u003cem\u003eBare\u003c/em\u003e\u003c/sub\u003e (1 \u0026micro;m\u003csup\u003e\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u003c/sup\u003e) and \u003cem\u003eA\u003c/em\u003e\u003csub\u003e\u003cem\u003ePlasmonic\u003c/em\u003e\u003c/sub\u003e (0.0176 \u0026micro;m\u003csup\u003e\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u003c/sup\u003e) is determined by the excitation laser spot and EM field enhancement area in the plasmonic structure, respectively.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe calculated enhancement factor of the X\u003csup\u003e0\u003c/sup\u003e, X\u003csup\u003e\u0026ndash;\u003c/sup\u003e, and XX is ~\u0026thinsp;100, ~300, and over 300, respectively. The enhancement factor can be calculated over 10 \u0026micro;W excitation power due to the absence of the XX signal in bare MoS\u003csub\u003e2\u003c/sub\u003e, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ef (red). The reason is that the high enhancement factor in MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure is the result of the strong electric field confinement originating from the LSPR coupling in AuNP. The optical response of the XX is the optical doping dependence excitonic features, as mentioned in the previous papers\u003csup\u003e\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e,\u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eTo investigate the role of anisotropy in the optical response of the non-centrosymmetric AuNP and MoS\u003csub\u003e2\u003c/sub\u003e hybrid structure, Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ea shows the polarization-resolved PL spectra. The sample structure was rotated to avoid any unwanted optical misalignment to control the incident polarization angle \u003cem\u003eθ\u003c/em\u003e. The periodic intensity variations of the PL spectra imply that the MoS\u003csub\u003e2\u003c/sub\u003e excitons strongly correlated with polarization-dependent LSPRs coupling in anisotropic resonators.\u003c/p\u003e \u003cp\u003eThe quantified normalized intensities of each exciton are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eb-d. The orientation of maximum optical response in plasmon-exciton coupling was calculated by the function of \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e0\u003c/em\u003e\u003c/sub\u003e\u0026thinsp;\u003cem\u003e+\u0026thinsp;I\u003c/em\u003e\u003csub\u003e\u003cem\u003e1\u003c/em\u003e\u003c/sub\u003e \u003cem\u003ecos\u003c/em\u003e\u003csup\u003e\u003cem\u003e\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u003c/em\u003e\u003c/sup\u003e \u003cem\u003e(θ - θ\u003c/em\u003e\u003csub\u003e\u003cem\u003emax\u003c/em\u003e\u003c/sub\u003e\u003cem\u003e)\u003c/em\u003e, where \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e0\u003c/em\u003e\u003c/sub\u003e and \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e1\u003c/em\u003e\u003c/sub\u003e are constants of normalized intensity, and \u003cem\u003eθ\u003c/em\u003e\u003csub\u003e\u003cem\u003emax\u003c/em\u003e\u003c/sub\u003e is the angle at the maximum intensity by deconvolution of the Lorentzian function.\u003c/p\u003e \u003cp\u003eIn previous studies, the general bare MoS\u003csub\u003e2\u003c/sub\u003e film does not correlate with the incident angle of linear polarization \u003cem\u003eθ\u003c/em\u003e due to high lattice symmetry\u003csup\u003e\u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e,\u003cspan citationid=\"CR50\" class=\"CitationRef\"\u003e50\u003c/span\u003e\u003c/sup\u003e. However, the results of the polarization-resolved PL spectra for each exciton in the MoS\u003csub\u003e2\u003c/sub\u003e/AuNP hybrid structure demonstrate anisotropy of the optical response as a function of the incident orientation. The polarizability (\u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e1\u003c/em\u003e\u003c/sub\u003e) in X\u003csup\u003e0\u003c/sup\u003e and X\u003csup\u003e\u0026ndash;\u003c/sup\u003e are 0.26 and 0.30, respectively, but XX is 0.55. It is the nature of the plasmonic response that local electric field enhancement is relevant not only to excitation polarization but also to emission spectral range. This result agrees with the larger enhancement for XX than X\u003csup\u003e0\u003c/sup\u003e, again confirming that the polarization-sensitive plasmon excitation is responsible for the pronounced XX generation.\u003c/p\u003e \u003cp\u003eIn conclusion, we investigated the enhanced plasmon-exciton coupling of X\u003csup\u003e0\u003c/sup\u003e, X\u003csup\u003e\u0026ndash;\u003c/sup\u003e, and XX modes on non-centrosymmetric AuNP and monolayer MoS\u003csub\u003e2\u003c/sub\u003e hybrid structure using absorption, Raman, PL spectra depending on the excitation wavelength, incident power, and polarization control. We explained the mechanism of plasmon-exciton coupling in each exciton mode, of which recombination pathways are followed in excitation, energy transfer, recombination, and EM field enhancement. The hybrid structure of specific plasmonic AuNP and TMDCs showed polarization-dependent optical responses and enhancement. Plasmon-biexciton coupling revealed higher polarizabilities than X\u003csup\u003e0\u003c/sup\u003e and X\u003csup\u003e\u0026ndash;\u003c/sup\u003e because of optical doping-dependent excitonic features and plasmonic resonance. We believe that another degree of freedom to control and engineer the excitonic response provides a new pavement toward the development of optoelectronic nanodevices with TMDCs and supports the plasmonic application of innovative optoelectronic technology.\u003c/p\u003e"},{"header":"Methods","content":"\u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003eMonolayer MoS\u003csub\u003e2\u003c/sub\u003e synthesis\u003c/h2\u003e \u003cp\u003eTriangular-shaped MoS\u003csub\u003e2\u003c/sub\u003e growth was carried out in an atmospheric pressure chemical vapor deposition. As Mo precursor, 0.3 g of ammonium heptamolybdate (AHM, Sigma-Aldrich, 431346) was dissolved into distilled (DI) water. The AHM solution was again mixed with NaOH solution (0.125 mol) and 0.2 ml of iodixanol solution (Sigma-Aldrich, Opti Prep, D1556) in the ratio of 0.3 : 2 : 0.2. The solution was spin-coated onto O\u003csub\u003e2\u003c/sub\u003e plasma-treated substrate (300 nm oxide Si wafer), forming a uniform Mo-Na-C precursor matrix. Spinning condition and plasma powers are 4000 rpm for 40 s and 30 W for 1 min, respectively. Then, the substrate was cut into 1 \u0026times; 1 cm\u003csup\u003e\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u003c/sup\u003e, loaded in zone 2 (outlet) with 0.2 g of S (Sigma-Aldrich, 212392) in zone 1 (inlet). For MoS\u003csub\u003e2\u003c/sub\u003e growth, the tube furnace was ramped to 190\u0026deg;C and 780\u0026deg;C for S (zone 1) and Mo (zone 2). 300 sccm of N\u003csub\u003e2\u003c/sub\u003e was injected for the ramping process (12 min), followed by the growth process with an increased flow rate (1000 sccm, 7 min).\u003c/p\u003e \u003c/div\u003e\n\u003ch3\u003ePlasmonic Structure Synthesis\u003c/h3\u003e\n\u003cp\u003eThe resulting split Au nano-rings could be obtained, followed by our previous research (Nano Lett. 2020, 20, 10, 7774\u0026ndash;7782).\u003csup\u003e\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e\u003c/sup\u003e Briefly, Au nano-prisms were employed as starting material en route to synthesize split Au nano-rings. First, vertices of Au nano-prisms were etched to thin Au nano-disks (~\u0026thinsp;10\u0026thinsp;\u0026plusmn;\u0026thinsp;1 nm in height) using Au\u003csup\u003e3+\u003c/sup\u003e ion as an etchant. Subsequently, thin Au nano-disks were converted to Au nano-hexagons through depositing Au followed by an etching step, leading to thick Au nano-disks with a height of ~\u0026thinsp;25\u0026thinsp;\u0026plusmn;\u0026thinsp;2 nm. In the selective edge deposition of Pt, Pt atoms were decorated at the periphery of thick Au nano-disks in part aided by the presence of high-index facets that can reduce the activation energy barrier for Pt nucleation leading to Au@Pt disks. In the next step, the core Au domains were etched away by adding Au\u003csup\u003e3+\u003c/sup\u003e ions resulting in the formation of split Pt nano-rings. Eventually, in the Au regrowth step, Au atoms were homogeneously reduced on the entire surface of split Pt nano-rings, leading to split Au nano-rings.\u003c/p\u003e\n\u003ch3\u003eSample Characterizations\u003c/h3\u003e\n\u003cp\u003eAn absorption hyper spectra map was obtained to analyze the optical response of the nano-ring/MoS\u003csub\u003e2\u003c/sub\u003e structure. The measurement position was controlled with the piezo sample stage (PI, P-611K020 NanoCube) for precise positioning on the commercial inverted microscope (Nikon, ECLIPSE Ti-U). A broadband illumination of light (Nikon, D-LH/LC, color temperature: 3300 K) was used, and the beam was focused on the sample by 100\u0026times; objective (Nikon, CFI LU PLAN EPI, NA 0.80, WD 3.5 mm). The reflected optical signal was collected and recorded by the spectrometer (Princeton Instruments, SpectraPro 2300i, 150 lpmm, CCD camera) with sample position. The acquisition time for each point was 100 ms. The reference of reflectance spectra was set as on the bare Si/SiO\u003csub\u003e2\u003c/sub\u003e surface under broadband tungsten lamp illumination.\u003c/p\u003e \u003cp\u003eThe photoluminescence and Raman spectra were excited by 532 nm DPSS laser (Optoelectronicstech, MGL-III-532) and 632.8 nm He-Ne laser (Thorlabs, HNL210LB) with less than 200 \u0026micro;W after objective lens. For tight focusing, the single-mode fiber (Thorlabs, SM450) was used as a spatial mode filter. The polarization dependence experiment was performed by rotating the sample. PL and Raman hyper-spectra map was obtained with each 15-degree clockwise rotation of the sample.\u003c/p\u003e \u003cp\u003eThe Lorentzian function was adapted to decompose each spectral peak for X\u003csup\u003e0\u003c/sup\u003e, X\u003csup\u003e\u0026ndash;\u003c/sup\u003e, XX, B\u003csup\u003e0\u003c/sup\u003e excitons in PL and E\u003csup\u003e1\u003c/sup\u003e\u003csub\u003e2g\u003c/sub\u003e, A\u003csub\u003e1g\u003c/sub\u003e peak positions in Raman spectra using Python (Ver 3.7.4, Scipy module). To investigate the surface potential dependency, KPFM and topography were acquired simultaneously by using a commercial scanning probe microscope (Parksystems, XE-NSOM) with an Au-coated cantilever (MikroMasch, NSC-14-Cr-Au).\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eAcknowledgements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis research was supported by Nano\u0026middot;Material Technology Development Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT (2020M3A7B4024925 and 2021M3H4A4079146). This work was supported by the Industrial Strategic Technology Development Program funded by the Ministry of Trade, Industry \u0026amp; Energy (Grant No. 20017214).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthor contributions\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eH.K. and J.I. contributed equally to optical experiments and write manuscript with support from S.C., M.S.J., J.S.A., D.P., and G.H.H.. S.J.Y., M.H., and S.P. fabricated and provided the asymmetric gold nanoparticles. J.Y.P. and G.H.H. fabricated and offered the 1L-MoS\u003csub\u003e2\u003c/sub\u003e.\u003csub\u003e\u0026nbsp;\u003c/sub\u003eK.N. conducted the KPFM measurements and analyzed data. W.P., J.S.A., and D.P. calculated optical response of gold nanoparticle by FEM simulation with COMSOL. All authors provided crucial feedback and helped shape the research.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData availability\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eAll data generated and the datasets used and analyzed during the current study are available from the corresponding author on reasonable request.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCompeting interests\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors declare no competing interests.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eZu, S. \u003cem\u003eet al.\u003c/em\u003e Active Control of Plasmon\u0026ndash;Exciton Coupling in MoS\u003csub\u003e2\u003c/sub\u003e\u0026ndash;Ag Hybrid Nanostructures. \u003cem\u003eAdv. Opt. Mater.\u003c/em\u003e \u003cstrong\u003e4\u003c/strong\u003e, 1463\u0026ndash;1469 (2016).\u003c/li\u003e\n\u003cli\u003eKim, J. H. \u003cem\u003eet al.\u003c/em\u003e Dielectric Nanowire Hybrids for Plasmon-Enhanced Light-Matter Interaction in 2D Semiconductors. \u003cem\u003eACS Nano\u003c/em\u003e \u003cstrong\u003e14\u003c/strong\u003e, 11985\u0026ndash;11994 (2020).\u003c/li\u003e\n\u003cli\u003eMangu, V. S., Zamiri, M., Brueck, S. R. J. \u0026amp; Cavallo, F. Strain engineering, efficient excitonic photoluminescence, and exciton funnelling in unmodified MoS\u003csub\u003e2\u003c/sub\u003e nanosheets. \u003cem\u003eNanoscale\u003c/em\u003e \u003cstrong\u003e9\u003c/strong\u003e, 16602\u0026ndash;16606 (2017).\u003c/li\u003e\n\u003cli\u003eKaviraj, B. \u0026amp; Sahoo, D. Physics of excitons and their transport in two dimensional transition metal dichalcogenide semiconductors. \u003cem\u003eRSC Adv.\u003c/em\u003e \u003cstrong\u003e9\u003c/strong\u003e, 25439\u0026ndash;25461 (2019).\u003c/li\u003e\n\u003cli\u003eWang, Y. \u003cem\u003eet al.\u003c/em\u003e Spin-Valley Locking Effect in Defect States of Monolayer MoS\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003eNano Lett.\u003c/em\u003e \u003cstrong\u003e20\u003c/strong\u003e, 2129\u0026ndash;2136 (2020).\u003c/li\u003e\n\u003cli\u003eYu, Y. \u003cem\u003eet al.\u003c/em\u003e Equally efficient interlayer exciton relaxation and improved absorption in epitaxial and nonepitaxial MoS\u003csub\u003e2\u003c/sub\u003e/WS\u003csub\u003e2\u003c/sub\u003e Heterostructures. \u003cem\u003eNano Lett.\u003c/em\u003e \u003cstrong\u003e15\u003c/strong\u003e, 486\u0026ndash;491 (2015).\u003c/li\u003e\n\u003cli\u003eSun, J. \u003cem\u003eet al.\u003c/em\u003e Strong plasmon-exciton coupling in transition metal dichalcogenides and plasmonic nanostructures. \u003cem\u003eNanoscale\u003c/em\u003e \u003cstrong\u003e13\u003c/strong\u003e, 4408\u0026ndash;4419 (2021).\u003c/li\u003e\n\u003cli\u003eQin, J. \u003cem\u003eet al.\u003c/em\u003e Revealing Strong Plasmon-Exciton Coupling between Nanogap Resonators and Two-Dimensional Semiconductors at Ambient Conditions. \u003cem\u003ePhys. Rev. Lett.\u003c/em\u003e \u003cstrong\u003e124\u003c/strong\u003e, 63902 (2020).\u003c/li\u003e\n\u003cli\u003eZhou, K., Song, J., Lu, L., Luo, Z. \u0026amp; Cheng, Q. Plasmon-enhanced broadband absorption of MoS\u003csub\u003e2\u003c/sub\u003e -based structure using Au nanoparticles . \u003cem\u003eOpt. Express\u003c/em\u003e \u003cstrong\u003e27\u003c/strong\u003e, 2305 (2019).\u003c/li\u003e\n\u003cli\u003eYang, Y., Pan, R., Tian, S., Gu, C. \u0026amp; Li, J. Plasmonic hybrids of MoS\u003csub\u003e2\u003c/sub\u003e and 10-nm nanogap arrays for photoluminescence enhancement. \u003cem\u003eMicromachines\u003c/em\u003e \u003cstrong\u003e11\u003c/strong\u003e, 1\u0026ndash;12 (2020).\u003c/li\u003e\n\u003cli\u003eKleemann, M. E. \u003cem\u003eet al.\u003c/em\u003e Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature. \u003cem\u003eNat. Commun.\u003c/em\u003e \u003cstrong\u003e8\u003c/strong\u003e, (2017).\u003c/li\u003e\n\u003cli\u003eSriram, P., Manikandan, A., Chuang, F. C. \u0026amp; Chueh, Y. L. Hybridizing Plasmonic Materials with 2D-Transition Metal Dichalcogenides toward Functional Applications. \u003cem\u003eSmall\u003c/em\u003e \u003cstrong\u003e16\u003c/strong\u003e, 1\u0026ndash;27 (2020).\u003c/li\u003e\n\u003cli\u003eMak, K. F., Lee, C., Hone, J., Shan, J. \u0026amp; Heinz, T. F. Atomically thin MoS\u003csub\u003e2\u003c/sub\u003e: A new direct-gap semiconductor. \u003cem\u003ePhys. Rev. Lett.\u003c/em\u003e \u003cstrong\u003e105\u003c/strong\u003e, 2\u0026ndash;5 (2010).\u003c/li\u003e\n\u003cli\u003eChen, H., Deng, S., Jiang, Y., Wang, H. \u0026amp; Wen, S. Resonance coupling in an individual gold nanorod-monolayer WS\u003csub\u003e2\u003c/sub\u003e heterostructure: Photoluminescence enhancement with spectral broadening. \u003cem\u003eACS Nano\u003c/em\u003e \u003cstrong\u003e14\u003c/strong\u003e, 13841\u0026ndash;13851 (2020).\u003c/li\u003e\n\u003cli\u003eSun, B. \u003cem\u003eet al.\u003c/em\u003e Tailoring of silver nanocubes with optimized localized surface plasmon in a gap mode for a flexible MoS\u003csub\u003e2\u003c/sub\u003e photodetector. \u003cem\u003eAdv. Funct. Mater.\u003c/em\u003e \u003cstrong\u003e29\u003c/strong\u003e, 1900541 (2019).\u003c/li\u003e\n\u003cli\u003eHaddadnezhad, M. \u003cem\u003eet al.\u003c/em\u003e Synthesis and Surface Plasmonic Characterization of Asymmetric Au Split Nanorings. \u003cem\u003eNano Lett.\u003c/em\u003e \u003cstrong\u003e20\u003c/strong\u003e, 7774\u0026ndash;7782 (2020).\u003c/li\u003e\n\u003cli\u003eJian, A. \u003cem\u003eet al.\u003c/em\u003e Quantitative investigation of plasmonic hot-electron injection by KPFM. \u003cem\u003eAppl. Surf. Sci.\u003c/em\u003e \u003cstrong\u003e492\u003c/strong\u003e, 644\u0026ndash;650 (2019).\u003c/li\u003e\n\u003cli\u003eEl Kabbash, M. \u003cem\u003eet al.\u003c/em\u003e Plasmon-Exciton Resonant Energy Transfer: Across Scales Hybrid Systems. \u003cem\u003eJ. Nanomater.\u003c/em\u003e \u003cstrong\u003e2016\u003c/strong\u003e, (2016).\u003c/li\u003e\n\u003cli\u003eKoo, Y. \u003cem\u003eet al.\u003c/em\u003e Tip-Induced Nano-Engineering of Strain, Bandgap, and Exciton Funneling in 2D Semiconductors. \u003cem\u003eAdv. Mater.\u003c/em\u003e (2021) doi:10.1002/adma.202008234.\u003c/li\u003e\n\u003cli\u003eSingh, A. \u003cem\u003eet al.\u003c/em\u003e Trion formation dynamics in monolayer transition metal dichalcogenides. \u003cem\u003ePhys. Rev. B\u003c/em\u003e \u003cstrong\u003e93\u003c/strong\u003e, 1\u0026ndash;5 (2016).\u003c/li\u003e\n\u003cli\u003eLee, H. S., Kim, M. S., Kim, H. \u0026amp; Lee, Y. H. Identifying multiexcitons in MoS\u003csub\u003e2\u003c/sub\u003e monolayers at room temperature. \u003cem\u003ePhys. Rev. B\u003c/em\u003e \u003cstrong\u003e93\u003c/strong\u003e, 1\u0026ndash;6 (2016).\u003c/li\u003e\n\u003cli\u003ePei, J. \u003cem\u003eet al.\u003c/em\u003e Exciton and Trion Dynamics in Bilayer MoS\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003eSmall\u003c/em\u003e \u003cstrong\u003e11\u003c/strong\u003e, 6384\u0026ndash;6390 (2015).\u003c/li\u003e\n\u003cli\u003eWang, W. \u003cem\u003eet al.\u003c/em\u003e Studying of the Biexciton Characteristics in Monolayer MoS\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003eJ. Phys. Chem. C\u003c/em\u003e \u003cstrong\u003e124\u003c/strong\u003e, 1749\u0026ndash;1754 (2020).\u003c/li\u003e\n\u003cli\u003eWang, H. \u003cem\u003eet al.\u003c/em\u003e Radiative lifetimes of excitons and trions in monolayers of the metal dichalcogenide MoS\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003ePhys. Rev. B\u003c/em\u003e \u003cstrong\u003e93\u003c/strong\u003e, 1\u0026ndash;11 (2016).\u003c/li\u003e\n\u003cli\u003eChakraborty, B., Matte, H. S. S. R., Sood, A. K. \u0026amp; Rao, C. N. R. Layer-dependent resonant Raman scattering of a few layer MoS\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003eJ. Raman Spectrosc.\u003c/em\u003e \u003cstrong\u003e44\u003c/strong\u003e, 92\u0026ndash;96 (2013).\u003c/li\u003e\n\u003cli\u003eKukucska, G. \u0026amp; Koltai, J. Theoretical Investigation of Strain and Doping on the Raman Spectra of Monolayer MoS\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003ePhys. Status Solidi Basic Res.\u003c/em\u003e \u003cstrong\u003e254\u003c/strong\u003e, 1\u0026ndash;5 (2017).\u003c/li\u003e\n\u003cli\u003eIqbal, M. W., Shahzad, K., Akbar, R. \u0026amp; Hussain, G. A review on Raman finger prints of doping and strain effect in TMDCs. \u003cem\u003eMicroelectron. Eng.\u003c/em\u003e \u003cstrong\u003e219\u003c/strong\u003e, (2020).\u003c/li\u003e\n\u003cli\u003eLuo, X., Zhai, X., Wang, L. \u0026amp; Lin, Q. Enhanced dual-band absorption of molybdenum disulfide using a plasmonic perfect absorber. \u003cem\u003eOpt. Express\u003c/em\u003e \u003cstrong\u003e26\u003c/strong\u003e, 11658 (2018).\u003c/li\u003e\n\u003cli\u003eSobhani, A. \u003cem\u003eet al.\u003c/em\u003e Enhancing the photocurrent and photoluminescence of single crystal monolayer MoS\u003csub\u003e2\u003c/sub\u003e with resonant plasmonic nanoshells. \u003cem\u003eAppl. Phys. Lett.\u003c/em\u003e \u003cstrong\u003e104\u003c/strong\u003e, 1\u0026ndash;5 (2014).\u003c/li\u003e\n\u003cli\u003eBae, H. \u003cem\u003eet al.\u003c/em\u003e Light Absorption and Emission Dominated by Trions in the Type-I van der Waals Heterostructures. \u003cem\u003eACS Photonics\u003c/em\u003e \u003cstrong\u003e8\u003c/strong\u003e, 1972\u0026ndash;1978 (2021).\u003c/li\u003e\n\u003cli\u003eMueller, T. \u0026amp; Malic, E. Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors. \u003cem\u003enpj 2D Mater. Appl.\u003c/em\u003e \u003cstrong\u003e2\u003c/strong\u003e, 1\u0026ndash;12 (2018).\u003c/li\u003e\n\u003cli\u003eGolovynskyi, S. \u003cem\u003eet al.\u003c/em\u003e Exciton and trion in few-layer MoS\u003csub\u003e2\u003c/sub\u003e: Thickness- and temperature-dependent photoluminescence. \u003cem\u003eAppl. Surf. Sci.\u003c/em\u003e \u003cstrong\u003e515\u003c/strong\u003e, 146033 (2020).\u003c/li\u003e\n\u003cli\u003eDulkeith, E. \u003cem\u003eet al.\u003c/em\u003e Plasmon emission in photoexcited gold nanoparticles. \u003cem\u003ePhys. Rev. B - Condens. Matter Mater. Phys.\u003c/em\u003e \u003cstrong\u003e70\u003c/strong\u003e, 1\u0026ndash;4 (2004).\u003c/li\u003e\n\u003cli\u003eKumar, V., Nisika, N. \u0026amp; Kumar, M. Modified absorption and emission properties leading to intriguing applications in plasmonic\u0026ndash;excitonic nanostructures. \u003cem\u003eAdv. Opt. Mater.\u003c/em\u003e \u003cstrong\u003e9\u003c/strong\u003e, 2001150 (2021).\u003c/li\u003e\n\u003cli\u003ePatil, R. A. \u003cem\u003eet al.\u003c/em\u003e Size-controllable synthesis of Bi/Bi2O\u003csub\u003e3\u003c/sub\u003e heterojunction nanoparticles using pulsed Nd:YAG laser deposition and metal-semiconductor-heterojunction-assisted photoluminescence. \u003cem\u003eNanoscale\u003c/em\u003e \u003cstrong\u003e8\u003c/strong\u003e, 3565\u0026ndash;3571 (2016).\u003c/li\u003e\n\u003cli\u003eAbid, K. \u003cem\u003eet al.\u003c/em\u003e Photoinduced Enhanced Raman Spectroscopy with Hybrid Au@WS\u003csub\u003e2\u003c/sub\u003eNanosheets. \u003cem\u003eJ. Phys. Chem. C\u003c/em\u003e \u003cstrong\u003e124\u003c/strong\u003e, 20350\u0026ndash;20358 (2020).\u003c/li\u003e\n\u003cli\u003eLi, Z. \u003cem\u003eet al.\u003c/em\u003e Active Light Control of the MoS\u003csub\u003e2\u003c/sub\u003e Monolayer Exciton Binding Energy. \u003cem\u003eACS Nano\u003c/em\u003e \u003cstrong\u003e9\u003c/strong\u003e, 10158\u0026ndash;10164 (2015).\u003c/li\u003e\n\u003cli\u003eKang, Y. \u003cem\u003eet al.\u003c/em\u003e Plasmonic Hot Electron Induced Structural Phase Transition in a MoS\u003csub\u003e2\u003c/sub\u003e Monolayer. \u003cem\u003eAdv. Mater.\u003c/em\u003e \u003cstrong\u003e26\u003c/strong\u003e, 6467\u0026ndash;6471 (2014).\u003c/li\u003e\n\u003cli\u003eJeong, Y., Kook, Y. M., Lee, K. \u0026amp; Koh, W. G. Metal enhanced fluorescence (MEF) for biosensors: General approaches and a review of recent developments. \u003cem\u003eBiosens. Bioelectron.\u003c/em\u003e \u003cstrong\u003e111\u003c/strong\u003e, 102\u0026ndash;116 (2018).\u003c/li\u003e\n\u003cli\u003eRingler, M. \u003cem\u003eet al.\u003c/em\u003e Shaping emission spectra of fluorescent molecules with single plasmonic nanoresonators. \u003cem\u003ePhys. Rev. Lett.\u003c/em\u003e \u003cstrong\u003e100\u003c/strong\u003e, 1\u0026ndash;4 (2008).\u003c/li\u003e\n\u003cli\u003eBang, S. \u003cem\u003eet al.\u003c/em\u003e Augmented Quantum Yield of a 2D Monolayer Photodetector by Surface Plasmon Coupling. \u003cem\u003eNano Lett.\u003c/em\u003e \u003cstrong\u003e18\u003c/strong\u003e, 2316\u0026ndash;2323 (2018).\u003c/li\u003e\n\u003cli\u003ePandey, J. \u0026amp; Soni, A. Unraveling biexciton and excitonic excited states from defect bound states in monolayer MoS\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003eAppl. Surf. Sci.\u003c/em\u003e \u003cstrong\u003e463\u003c/strong\u003e, 52\u0026ndash;57 (2019).\u003c/li\u003e\n\u003cli\u003eLee, H. \u003cem\u003eet al.\u003c/em\u003e Radiative control of localized excitons at room temperature with an ultracompact tip-enhanced plasmonic nano-cavity. 1\u0026ndash;18 (2020).\u003c/li\u003e\n\u003cli\u003eDong, J., Zhang, Z., Zheng, H. \u0026amp; Sun, M. Recent Progress on Plasmon-Enhanced Fluorescence. \u003cem\u003eNanophotonics\u003c/em\u003e \u003cstrong\u003e4\u003c/strong\u003e, 472\u0026ndash;490 (2015).\u003c/li\u003e\n\u003cli\u003ePoudel, Y. \u003cem\u003eet al.\u003c/em\u003e Active Control of Coherent Dynamics in Hybrid Plasmonic MoS\u003csub\u003e2\u003c/sub\u003e Monolayers with Dressed Phonons. \u003cem\u003eACS Photonics\u003c/em\u003e \u003cstrong\u003e6\u003c/strong\u003e, 1645\u0026ndash;1655 (2019).\u003c/li\u003e\n\u003cli\u003eMueller, T. \u0026amp; Malic, E. Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors. \u003cem\u003enpj 2D Mater. Appl.\u003c/em\u003e \u003cstrong\u003e2\u003c/strong\u003e, 1\u0026ndash;12 (2018).\u003c/li\u003e\n\u003cli\u003eSchmid, T., Opilik, L., Blum, C. \u0026amp; Zenobi, R. Nanoscale chemical imaging using tip-enhanced raman spectroscopy: A critical review. \u003cem\u003eAngew. Chemie - Int. Ed.\u003c/em\u003e \u003cstrong\u003e52\u003c/strong\u003e, 5940\u0026ndash;5954 (2013).\u003c/li\u003e\n\u003cli\u003ePanasci, S. E. \u003cem\u003eet al.\u003c/em\u003e Strain, Doping, and Electronic Transport of Large Area Monolayer MoS\u003csub\u003e2\u003c/sub\u003e Exfoliated on Gold and Transferred to an Insulating Substrate. \u003cem\u003eACS Appl. Mater. Interfaces\u003c/em\u003e \u003cstrong\u003e13\u003c/strong\u003e, 31248\u0026ndash;31259 (2021).\u003c/li\u003e\n\u003cli\u003eShi, Y. \u003cem\u003eet al.\u003c/em\u003e The Polarization Properties of the Reflection Spectra of Single-Layer MoS\u003csub\u003e2\u003c/sub\u003e and ReS\u003csub\u003e2\u003c/sub\u003e on SiO\u003csub\u003e2\u003c/sub\u003e/Si and Quartz Substrates. \u003cem\u003eNanoscale Res. Lett.\u003c/em\u003e \u003cstrong\u003e15\u003c/strong\u003e, 1\u0026ndash;6 (2020).\u003c/li\u003e\n\u003cli\u003eChen, S. \u003cem\u003eet al.\u003c/em\u003e Anisotropic Plasmonic Nanostructure Induced Polarization Photoresponse for MoS\u003csub\u003e2\u003c/sub\u003e-Based Photodetector. \u003cem\u003eAdv. Mater. Interfaces\u003c/em\u003e \u003cstrong\u003e7\u003c/strong\u003e, 2\u0026ndash;9 (2020).\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"scientific-reports","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"scirep","sideBox":"Learn more about [Scientific Reports](http://www.nature.com/srep/)","snPcode":"","submissionUrl":"","title":"Scientific Reports","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Scientific Reports","inReviewEnabled":true,"inReviewRevisionsEnabled":true},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-2249049/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-2249049/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThe understanding and engineering of the plasmon-exciton coupling are necessary to control the innovative optoelectronic device platform. In this study, we investigated the intertwined mechanism of each plasmon-exciton couplings in monolayer molybdenum disulfide (MoS\u003csub\u003e2\u003c/sub\u003e) and plasmonic hybrid structure. The results of absorption, simulation, electrostatics, and emission spectra show that interaction between photoexcited carrier and exciton modes are successfully coupled by energy transfer and exciton recombination processes. Especially, neutral exciton, trion, and biexciton can be selectively enhanced by designing the plasmonic hybrid platform. All of these results imply that there is another degree of freedom to control the individual enhancement of each exciton mode in the development of nano optoelectronic devices.\u003c/p\u003e","manuscriptTitle":"Plasmon-exciton couplings in the MoS2/AuNP plasmonic hybrid structure","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2022-11-11 21:30:24","doi":"10.21203/rs.3.rs-2249049/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Major revision","date":"2022-11-17T08:30:32+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2022-11-16T11:57:29+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"59e44ef5-898c-4699-8317-ff819a844292","date":"2022-11-09T11:38:21+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"7b098eb8-9d0c-410a-9bb6-2a70c504fab7","date":"2022-11-09T11:35:27+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2022-11-09T11:31:45+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2022-11-09T11:16:49+00:00","index":"","fulltext":""},{"type":"editorInvited","content":"","date":"2022-11-09T11:05:55+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2022-11-09T11:02:05+00:00","index":"","fulltext":""},{"type":"submitted","content":"Scientific Reports","date":"2022-11-08T03:21:54+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"scientific-reports","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"scirep","sideBox":"Learn more about [Scientific Reports](http://www.nature.com/srep/)","snPcode":"","submissionUrl":"","title":"Scientific Reports","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Scientific Reports","inReviewEnabled":true,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"a8c9f63e-94f1-45aa-a621-a451b5294f3d","owner":[],"postedDate":"November 11th, 2022","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":16837810,"name":"Physical sciences/Nanoscience and technology/Nanoscale devices/Nanophotonics and plasmonics"},{"id":16837811,"name":"Physical sciences/Optics and photonics/Optical physics/Nanophotonics and plasmonics"},{"id":16837812,"name":"Physical sciences/Physics/Optical physics/Nanophotonics and plasmonics"}],"tags":[],"updatedAt":"2022-12-15T06:29:24+00:00","versionOfRecord":[],"versionCreatedAt":"2022-11-11 21:30:24","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-2249049","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-2249049","identity":"rs-2249049","version":["v1"]},"buildId":"WrCJVZZCHTDjtuVLN7oU0","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}