Yuan Zhaoa,
Guanxiong Chena,
Zhuchen Taoa,
Chunyu Zhangb and
Yanwu Zhu*a
aCAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, P. R. China. E-mail: zhuyanwu@ustc.edu.cn
bSino-French Institute of Nuclear Engineering & Technology, Sun Yat-Sen University, Zhuhai Campus, 519082, Guangdong, P. R. China
First published on 5th June 2014
We propose a structure to excite plasmons in large-area continuous graphene films with insulator-covered sub-wavelength silicon gratings (ICSWSG). By numerical simulations we have demonstrated that, after adding a low-permittivity insulator underneath graphene, the graphene/gratings hybrid structure has a high Q-factor (∼66) and a sharp notch (with the full width at half maximum of ∼122 nm) in the transmission spectra at mid-infrared resonant wavelength. Furthermore, the plasmonic properties, e.g. the resonant wavelength, magnitude and Q-factor, can be tuned over a wide range via structure modulation and/or gating of graphene. The transmission dip is achieved over a wide angle range. Finally we demonstrate that such highly confined graphene plasmons could also be excited in graphene sandwiched between silicon gratings and a SiO2 substrate.
For exciting plasmons in graphene, a key challenge is to efficiently couple to the plasmonic wave, as its wavevector is much larger than that of free-space waves.15,16 Experimentally, excitations of plasmons in graphene have been realized using periodically patterned graphene structures, e.g., one-dimensional (1D) nanoribbons13 or micro-ribbons6 and 2D nanodisks12 or micro-disks.17 Graphene/insulator stacking structures have been investigated to enhance the tunability of the plasmonic resonance magnitude.18 These designs usually suffer a relatively low quality factor (Q-factor) (defined as the ratio of resonant wavelength to the full width at half maximum) which possibly restricts the practical applications, e.g. in sensing. On the other hand, although extremely high carrier mobility, e.g. 230
000 cm2 (V−1 s−1), has been demonstrated in high-quality exfoliated graphene samples,19 the lithography process necessary for fabricating graphene nanostructure or microstructure arrays may severely deteriorate the mobility, thus leading to a big loss and much lower Q-factors.12,20 It will be valuable to have optimized Q-factors, especially in large-area continuous films.
Plasmonic excitations in graphene with sub-wavelength dielectric gratings to compensate wavevector have been proposed to generate a resonance with a Q-factor of ∼40.15,16 In these structures, the dispersion of graphene plasmons splits into bands due to the different dispersions of plasmons on different regions of gratings, which allows the excitation of plasmons in graphene by external incident light.16 Utilizing these structures, plasmonic excitations may be realized without the need of engineering graphene, which may benefit to maintain the excellent electronic property in graphene.21 Moreover, by tuning the period of gratings, the structure can work in mid-infrared, far-infrared or terahertz wavelengths.15 For example, plasmons in a continuous monolayer graphene have been detected in mid-infrared regions with the assistance of sub-wavelength silicon gratings.21 However, the challenges could remain considering the proposed process of experimental preparations and microstructure influences. When compared to flat substrates, the rough gratings may increase the interface scattering and deteriorate the mobility in graphene,12,22–24 thus leading to bigger losses and lower Q-factors in the practical devices.
In this work, a structure with insulator-covered sub-wavelength silicon gratings (ICSWSG) is proposed to excite plasmons in a continuous graphene film. The structure experiences a high Q-factor after a low-permittivity insulator is added underneath graphene. Finite element electromagnetic simulations reveal the strong electric field confinement around the graphene layer at the resonant wavelengths. We demonstrate that the plasmonic properties can be modulated by tuning the insulator layer thickness, grating period, Fermi energy level, carrier mobility and the number of graphene layers. Moreover, the strong resonance has been observed over a wide incident angle of the light. Similar plasmonic resonances and field confinements can also be realized in a graphene layer sandwiched between silicon gratings and a SiO2 substrate. The excellent features of our proposed structures would make high-performance graphene-based plasmonic sensors possible.
For a continuous monolayer graphene, the dispersion relationship of plasmonic wave is given by14,25
![]() | (1) |
The conductivity of graphene is modeled using Drude model with D (Drude weight) and Γ (scattering width) as two fitting parameters,26
![]() | (2) |
000 cm2 (V−1 s−1)). Here, as the photon energy in the simulated spectral range is always less than 2EF, interband transitions in graphene are forbidden by the Pauli exclusion principle.25–27 Thus the effect of the interband transition has been neglected in the simulations.25
Combining eqn (1) and (2), the wavevector of graphene plasmonic wave can be expressed as
![]() | (3) |
When graphene is placed on a uniform dielectric medium, its plasmonic modes can't be excited directly by mid-infrared light, since the wavevector of graphene plasmonic waves is far larger than that of light in vacuum, as shown in Fig. 2a. However, once the difference is overcomed, the plasmonic wave can be excited in graphene and the electric field is highly confined due to the large differences in wavevector.13,15
Herein, the ICSWSG is used to compensate the wavevector mismatches caused by the difference in the dispersion of graphene plasmons on different regions of ICSWSG,16 which enables the efficient coupling of the incident electromagnetic field and the plasmonic modes in graphene. Introducing a low-permittivity polymer buffer layer between silicon gratings and graphene films may allow a relatively gentle contact for graphene and decrease the resonant wavelength λ0 (eqn (6)), where Q-factors are further improved as decreased value of Re(σ) (real part of the graphene conductivity) in small wavelength range corresponds to low losses (Fig. 2b). Furthermore, it has been claimed that adding a polymer buffer layer underneath graphene may help to minimize the mobility degradation due to the suppression of extrinsic surface phonons and reduction of the impurity concentration.18
For a grating period p, the resonant wavelength λ0 is determined by phase match equation15
![]() | (4) |
For a normal incidence wave, θ = 0, eqn (4) is simplified as
![]() | (5) |
From eqn (5), it can be seen that the plasmonic resonant wavelength λp = 2π/Re(kp) is related to grating period p and η as λp = ηp.
Combining eqn (3) and (5), the resonant wavelength λ0 is given by
![]() | (6) |
Since the optical energy dissipates due to the ohmic loss while the plasmonic wave propagates in the continuous graphene layer, a notch can be observed around the resonant wavelength in the transmission spectrum.15 The simulations were performed in frequency domain using Comsol Multiphysics (COMSOL 4.3a), which implements the finite element method (FEM) to solve Maxwell's equations and is a widely accepted method for modeling optics.28,29 In the simulations, we set the perfectly matched layer (PML) in the vertical direction to achieve absorbing boundary conditions, while in the horizontal directions we used periodic boundary conditions for simulating an infinite silicon grating array (Fig. 1b). The graphene film was modeled as a thin layer with a thickness of 0.5 nm, as in ref. 11 and 15 and dielectric constants of silicon, SiO2 and NFC were taken from ref. 18, 22 and 30. The meshing was done with the program built-in algorithm, which creates a tetrahedral mesh. The mesh maximum element size (MES), which limits the maximum size of the edges of the tetrahedrons, was set to be 0.1 nm in the domain representing the graphene, 1 nm for NFC and 6 nm for all the elements in the air, silicon and SiO2 subdomains. Direct PARDISO solver was used to solve the problem.
The Q-factor of the plasmonic spectra is determined by the optical loss in graphene and can be calculated from relaxation time τ of charge carriers in graphene at resonance wavelength λ0. Theoretically, the Q-factor is expressed as25
![]() | (7) |
![]() | ||
Fig. 4 (a) Simulated normal-incidence transmission spectra with various carrier mobilities of graphene when EF = 0.6 eV, p = 200 nm, T1 = 500 nm and T2 = 10 nm. The real part of graphene conductivity and Q-factor with varying carrier mobilities at resonant wavelength λ0 = 8.08 μm are shown in the inset. The dots are simulated data and the lines are calculated from eqn (2) or (7). (b) Transmission spectra with buffer layer thickness of 5, 10, 20, 30 or 50 nm, respectively when EF = 0.6 eV, μ = 10 000 cm2 (V−1 s−1), p = 200 nm and T1 = 500 nm. | ||
In the proposed structure, another factor affecting FWHM and Q-factor is the thickness of buffer layer, which influences the effective dielectric constants of εr2. Fig. 4b shows the simulated transmission spectra with different thicknesses of buffer layers. It can be seen that the resonant wavelength blue-shifts as increasing the thickness of buffer layer due to the additional decrease in the effective permittivity εr2. Thus FWHM decreases and Q-factor increases due to the low loss at smaller resonant wavelength. However, if the thickness of buffer layer is too large, the transmission notch is too shallow to ensure enough detection (it is 100 nm in our case); 10 nm was used in the following discussions.
Furthermore, our simulations (Fig. 5) show that the deep transmission dip can be realized over a wide angle range. Such a result is explained by the existence of flat graphene plasmon bands above the light line at mid-infrared regions, which is attributed to the deep sub-wavelength nature of graphene plasmons and effects of Bragg scattering at the Brillouin zone center.16
![]() | ||
Fig. 5 The simulated angular dispersions of the transmittance for TM configurations when EF = 0.6 eV, μ = 10 000 cm2 (V−1 s−1), p = 200 nm, T1 = 500 nm and T2 = 10 nm. | ||
The Q-factor can be tuned by the Fermi energy level EF in graphene relative to the Dirac points via gate voltage or electrostatic doping and period p of silicon gratings. From the simulation results shown in Fig. 6a, it can be seen that the transmission spectra can be effectively tuned with varying Fermi energy level EF of graphene. The resonant wavelength and Q-factor with respect to the Fermi energy level EF agree well with eqn (6) or (7) (η = 1.50), as shown in Fig. 6b. Recent studies suggested that, adding a buffer layer before transferring additional graphene layers could help to distribute carriers into multiple graphene layers and make the structure have a broader tunability.18 Fig. 6c shows the transmission spectra in the multilayer graphene/insulator structures. It can be seen that the resonant properties can be tuned in a broader range via changing the number of multilayer structures. It is worth noticing that the contribution of the buffer layer to the total conductivity has been ignored since the buffer layer is thin (10 nm) and non-conducting.18 In the calculations of multilayer graphene, we considered each graphene layer has the same Fermi energy level, mobility and relaxation time. The total conductivity still has the Drude form, σtotal = iDtotal/π(ω + iΓ), where the sum of the Drude weights for N layer graphene Dtotal = N1/2e2EF/ħ.18,26 The resonant wavelength and Q-factor with respect to the number of graphene layers agree well with theoretical values (substituting N1/2EF for EF in eqn (6) or (7)), as shown in Fig. 6d. Thus, multilayer graphene films (e.g. by sequentially transferring monolayer) could be used to further improve the tunability of such devices.
![]() | ||
Fig. 6 (a) Simulated normal-incidence transmission spectra with different Fermi energy level EF in graphene when μ = 10 000 cm2 (V−1 s−1), p = 200 nm, T1 = 500 nm and T2 = 10 nm. (b) Scaling rule of the resonant wavelength λ0 and Q-factor with respect to EF. The dots are simulated results and the lines are calculated from eqn (6) or (7). (c) Transmission spectra with different number of graphene/insulator multilayer structure when EF = 0.6 eV, μ = 10 000 cm2 (V−1 s−1), p = 200 nm, T1 = 500 nm and T2 = 10 nm. (d) Scaling rule of the resonant wavelength λ0 and Q-factor versus the number of multilayer structure. The dots are simulated results and the lines are calculated from eqn (6) or (7) when substituting N1/2EF for EF. (e) Transmission spectra with different period p of silicon gratings when EF = 0.6 eV, μ = 10 000 cm2 (V−1 s−1), w = 0.5p, T1 = 500 nm and T2 = 10 nm. (f) Scaling rule of the resonant wavelength λ0 and Q-factor with respect to p. The dots are simulated results and the lines are calculated from eqn (6) or (7). | ||
The effects of the period of silicon gratings were studied by fixing the ratio of grating width w and period p (w/p) to be 1/2. It can be seen from Fig. 6e that the transmission spectra are largely tuned with varying periods. The resonant wavelength and Q-factor with respect to the period agree well with eqn (6) or (7), as shown in Fig. 6f. Specially, when the period of silicon gratings is reduced to 50 nm, the Q-factor can be as high as 155. For large period, the notches at the higher frequencies are caused by higher order modes.
Finally, the dependence of the resonant wavelength to the refractive index (RI) of dielectric environment above graphene (n1 = εr11/2) has been considered for possible applications of the graphene/ICSWSG hybrid structure as sensors since graphene has strong bio-compatibility and adsorption to biomolecules due to the π-stacking interactions and the high surface to volume ratio of graphene.31,33–37 Fig. 7 shows the transmission spectra with a 20 nm-thick sensing medium on graphene films and corresponding sensitivity calculated (defined as the ratio of the shift of resonant wavelength δλ0 to the change of RI of the sensing medium δn1, δλ0/δn1), with or without buffer layer. The sensitivity improves 45.13% and figure of merit (FOM, defined as the ratio of sensitivity to FWHM) increases ∼190% (from ∼3.84 to ∼11.38) after a thin buffer layer is present underneath the graphene. The increase in the sensitivity and in the FOM is due to the decrease in the effective permittivity εr2 and minimization of the loss at smaller resonant wavelength.25 Furthermore, the sensitivity is related to the thickness of sensing medium since the characteristic decay length of graphene plasmons is as high as ∼100 nm.25 Fig. 8a shows the transmission spectra with sensing medium RI n1 = 1.31 and thickness of 1, 2, 5, 10, 20, 50, 100 and 200 nm above graphene films, respectively when EF = 0.6 eV, μ = 10
000 cm2 (V−1 s−1), p = 200 nm, T1 = 500 nm and T2 = 10 nm. It can be seen that the resonant wavelength red-shifts with increasing film thickness, and saturation of the shift is observed when the thickness exceeds 100 nm (Fig. 8b), where the sensing is close to the bulk RI sensitivity. For bulk medium, the RI sensitivity can be as high as 1923 nm per RIU, as can be deduced using eqn (6),
![]() | (8) |
From eqn (8), we can see that the bulk RI sensitivity is related to period, permittivity of material beneath graphene and Fermi energy of graphene. By decreasing the Fermi energy of graphene to 0.2 eV, the bulk sensitivity can be up to 3328 nm per RIU (Fig. 8c and d).
To further demonstrate the flexibility of the dielectric environment surrounding graphene in the hybrid structure, we show that setting sub-wavelength silicon gratings above graphene films can also be used for compensating wavevector differences and exciting graphene plasmons (Fig. 9). Similarly, adding a buffer layer underneath (and/or above) graphene is beneficial to decrease FWHM and to increase Q-factor in the transmission spectra around the resonant wavelength. From the simulated transmission spectra and the side-view electric field profiles, it can be seen that the transmission spectra vary similarly to those for placing sub-wavelength silicon gratings beneath. Moreover, the fundamental mode and second-mode are detected simultaneously for the structure either with or without a buffer layer beneath graphene. When adding buffer layers both on the top and beneath graphene films, the resonant wavelength blue-shifts and FWHM decreases due to the further decrease in the effective permittivity εr1 above graphene, and the second mode is too shallow to be detected. The structure provides an alternative to excite plasmons in continuous graphene films.
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