Abstract
We demonstrate the perfect synthesis of terahertz circularly polarized Fano resonant reflecting spectra from hybrid resonator-graphene meta-surfaces for highly sensitive refractive index sensing of the biochemical analyte. Such a hybrid resonator-graphene meta-surface, consisting of periodic multi-node split ring resonators on the top of the grounded polyimide substrate inserted with a monolayer graphene sheet, can perfectly transform the linearly polarized electromagnetic fields into circularly polarized waves. Especially, the greatest polarization purity of the reflecting spectra can readily be obtained at the Fano resonance by tuning the Fermi level of the graphene, thus offering an alternative way to identify the difference between the given test specimens and other analytes with a very close refractive index on the basis of the polarization extinction ratio. The proposed methodology, capable of distinguishing the samples with a difference in the refractive index of ten thousandths, should pave the way for tangible applications of precision detections in biochemical assays with high accuracy.
© 2023 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreement
1. Introduction
Graphene meta-surfaces have demonstrated the great efficiency in generating Fano resonances for high precision detections of dielectrics, possessing the merits of being accurate, fast and harmless to the human body in the biological sensing of proteins, and simultaneously offering the high-quality and cost-effective detection solutions [1–3]. Generally, the sensitivity of the meta-surface based sensors can be determined by observing the frequency shifts of the resonances varied with different refractive index of the analyte. Su et al. proposed a high-performance Fano resonant sensor using two silicon elliptical cylinders with asymmetric minor axis on silica substrate coated graphene [4]. Zhang et al. designed a high-Q, high-sensitivity, all-dielectric four-resonance sensor using periodical asymmetric paired bars in the near-infrared regime [5]. Liu et al. demonstrated a Fano resonance sensor with high modulation depth and polarization insensitive characteristics [6]. Sun et al. presented a Fano resonant sensor that can independently adjust the absorption mode by examining the time domain signal [7]. These researches, using Fano resonant meta-surface sensors as the first choice for biochemical detections, have paved the way for the quest of tangible applications of more advanced sensing technologies.
However, the present proposals often lack the polarization manipulations of the electromagnetic fields at Fano resonances, and testing the polarization purity of the reflected wave should offer an alternative way to identify the difference between the given test specimens and other analytes with very close refractive index on the basis of polarization extinction ratio (PER) [8]. Different from determining the refractive index of the analyte on the basis of the frequency offset, the PER method compares the greatest polarization purity of the given test specimens. As a result, the PER method often depends on the polarization conversion, where the interactions between the incidence and the proposed testing devices will offer multidimensional analysis with much sharper spectra possessing less aliasing effects and huge distinguishability of refractive index, other than solely the shifted frequency. On the other hand, the reconfigurable characteristics of graphene meta-surface also enable the modulations of the polarization states of the reflected waves to achieve the high-purity circularly polarized (CP) fields with efficient linear-to-circular polarization conversions. One can thus use the modulation effect of the graphene layer by tuning the Fermi levels to achieve the maximum polarization purity of the reflections from the given test specimens. Based on these consideration, we demonstrate the high-precision refractive index sensing from dynamically modulated Fano resonances of CP waves using hybrid resonator-graphene meta-surfaces. We will show that the proposed strategy can distinguish the samples with a difference in refractive index of ten thousandths by comparing the greatest polarization purity of the reflecting spectra at Fano resonances.
2. Modeling and simulation results
Figure 1 schematically demonstrates interactions between the electromagnetic fields and the proposed hybrid resonator-graphene meta-surfaces, where the biochemical analyte can be loaded over the meta-surface. Such a hybrid resonator-graphene meta-surface consists of periodic multi-node split ring resonators (SRRs) on the top of the grounded polyimide ($\varepsilon _{r}$ = 3+0.05j) substrate inserted with a monolayer graphene sheet. The detailed geometric parameters are h = 5 $\mu$m, P = 36 $\mu$m, w = 1.25 $\mu$m, g = 1.25 $\mu$m, L = 20 $\mu$m, ${d}_{1}$ = 5 $\mu$m, ${d}_{2}$ = 4 $\mu$m. When the x-polarized wave is casting over the meta-surface, Fano resonant reflecting spectrum will be created by the multi-node-SRR array. In the meanwhile, the chirality of the resonators also enables the polarization conversion of the reflected waves [9,10], transforming x-polarized incidence into the CP reflections. The greatest polarization purity of the reflecting spectra can readily be obtained at the Fano resonance though tuning the Fermi level of the graphene. The permittivity ($\varepsilon _g$) of graphene is depending on the surface conductivity function ($\sigma _g$):
where $\varepsilon _0$ is the vacuum permittivity and $\Delta$ = 1 nm is the thickness of the mono-layer graphene sheet. Graphene conductivity can be obtained from the Kubo formula [11–13]The relationship between the incidence and reflected fields of hybrid resonator-graphene meta-surfaces can thus be represented using the Jones matrix with
Full-wave simulations (CST Studio Suite) are carried out to verify the proposed hybrid resonator-graphene meta-surfaces with an x-polarized incidence along the -z direction. Figure 2 demonstrates the reflections and the PER of the proposed hybrid resonator-graphene meta-surfaces, where we mimic the interactions between the electromagnetic fields and the proposed hybrid resonator-graphene meta-surface using the Floquet mode analysis as shown in Fig. 2(a) with boundary conditions virtually repeating the modeled structure periodically in x and y directions. The reflection spectra of the meta-surface and phase difference ($\Delta \varphi =\Phi _{yx} -\Phi _{xx}$) of the co- and cross- components are shown in Fig. 2(b) with 0.49 eV Fermi energy imposed over the graphene sheet. It can be found that the $\Delta \varphi$ is around $\pm 90^{\circ }$ between 4 THz and 6 THz, performing the linear-to-circular polarization conversion. We use the ellipticity $\chi$ derived from Stokes Parameters to qualify the polarization purity of the reflected wave [14,15].
Figures 2(e) to (g) continue to demonstrate the multipole analysis of the interaction between the hybrid resonator-graphene meta-surface and the x-polarized incidence by demonstrating the distribution of the normalized electric field $E_{z}$ on the x-y plane and also the current over the multi-node SRR array, as well as the magnetic field on the x-z plane. For the comparison purpose, we choose three points of $P_{1}$ = 4.2 THz dominated by electric dipole, $P_{2}$ = 4.698 THz at the PER peak, and $P_{3}$ = 4.96 THz dominated by toroidal mode for the demonstration. It can be seen from the x-z plane that the magnetic field directions at the intermediate gap of the multi-node SRR at $P_{1}$ are all in the -y direction, and the current over the multi-node SRR can thus be equivalent to an electric dipole when other modes are weaker. However, the partial ring current on the multi-node SRR at $P_{2}$ will lead to the generation of magnetic fields in $\pm z$ directions at the gap. The magnetic field is confined inside the multi-node SRR gap, with the magnetic ring near the center in the x-z plane creating the toroidal mode. On the other hand, the opposite current on the multi-node SRR is more pronounced at $P_{3}$, while the magnetic fields in the x-z plane distribute almost linearly oriented along the z axis with opposite directions as the distinct feature of the toroidal mode [20–22].
The meta-surface can be regarded as a multi-layer cascaded structure as shown in Fig. 3(a), where each layer is equivalent to a generalized two-port network. The layer-1 is composed of multi-node SRR array and a half-layer-thick polyimide substrate. The layer-2 refers to a mono-layer graphene sheet embedded in the middle of the polyimide to control the electromagnetic fields between the multi-node SRR array and the ground. The layer-3 is another half-layer substrate and the ground. Using generalized signal flow analysis, the reflection matrix of the proposed hybrid graphene-meta-surface can be expressed as follows
The scattering matrix of Layer-2 for a mono-layer graphene sheet sandwiched in a polyimide substrate can be expressed as
The layer-3 of the ground is equivalent to a short circuit terminal in the transmission line with the reflection coefficient of
The theoretical values from Eq. (12) in Fig. 3(g) of the amplitude and phase of the scattering spectrum are basically agree with the full-wave simulation, and we can conclude that the layer-1 and layer-3 only depend on their structural composition, and the response of the entire system can be manipulated through the dynamic modulation of the Fermi level so as to achieve the high polarization purity with efficient linear-to-circular conversion.
Figures 4(a) and (b) demonstrates the variations of PER curve with different Fermi levels imposed over the graphene sheet. We can clearly observe that Fermi level is not only manifested in the blue shift of the PER spectrum, the polarization purity of the linear-to-circular polarization conversion is also significantly changed. The sharpest PER curve at 0.49 eV with the highest polarization purity paves the way for high-precision refractive index sensing. The equivalent circuit model of the SRR is inserted in Fig. 4(b) [24]. $C_{analyte}$ represents the equivalent analyte capacitance and will become larger with the increase of the refractive index. $L_{SRR1}$, $L_{SRR2}$ are controlled by the branches of SRR and their values will gradually increase with the width and the length of the branch. $C_{SRR}$ is determined by the two gaps of the SRR, and the narrower gap will lead to more charge accumulation, resulting in an increase in $C_{SRR}$. The total impact of $L_{SRR1}$, $L_{SRR2}$ can be described by $L_{SRR}$ and as long as any branch becomes wider or longer, $L_{SRR}$ will definitely increase. Figures 4(c) to (f) show the influences of different structural parameters L, ${d}_{1}$, g, w of the multi-node SRR on the PER curve, respectively. As we can observed, the PER peak will have red-shifts with the increase of L and ${d}_{1}$ because $L_{SRR}$ increases due to the elongation of the SRR main arms and broadening of the wide branches along the x direction. On the other hand, it will experience blue-shifts as g becomes bigger because the gaps become wider and the strong electric field in the gap weakens, leading to a decrease in $C_{SRR}$. In addition, the variation of w will not significantly influence the operating frequency of the PER peak, the reason is that the widening of the main branches of SRR lead to the increase of ${L_{SRR}}$, the charge aggregation at the gap is simultaneously weakened because the gap is also widened, ${C_{SRR}}$ is almost inversely proportional to ${L_{SRR}}$. As a result, we selected L = 20 $\mu$m, ${d}_{1}$ = 5 $\mu$m, g = 1.25 $\mu$m and w = 1.25 $\mu$m from all geometric parameters to ensure the maximum polarization purity for the precise sensing purpose.
3. Sensing applications
When loaded a superstrate of the analyte with thickness of ${h}_{1}$ as shown in Fig. 5(a), the proposed hybrid resonator-graphene meta-surface can readily start the applications. The temperature and other conventional variables, such as Polyimide substrate thickness and SRR geometry parameters, are kept constantly when performing the test. Clearly, different ${h}_{1}$ will lead to the variations of sensitivity ($S=\Delta f/\Delta n$) from the reflection spectrum as illustrated in Fig. 5(b). We can observe the sensitivity increases continuously as the ${h}_{1}$ increases, but the uptrend of the curve is gradually slowing down. As a result, we take ${h}_{1}$ = 3 $\mu$m in the following two specific examples of biochemical detections to verify the great detection accuracy of our proposed hybrid resonator-graphene meta-surface, where a micropipette is required to control the total volume of the analyte and keeps ${h}_{1}$ at 3 $\mu$m with the assistance of an optical 3D surface profiler.
Case-1: Anhydrous alcohol has important applications in solvents, cosmetics, and fuels nowadays. However, distinguishing anhydrous ethanol from ultra-high-concentration ethanol often needs very precision sensing with a 1/10,000 refractive index discrimination capacity. The alcohol’s refractive index is 1.3604 with 97$\%$ concentration, 1.3599 with 98$\%$ concentration, and 1.3593 for anhydrous ethanol with more than 99.5$\%$ concentration [25]. In this way, we can adjust the graphene Fermi level imposed over the graphene meta-surface to 0.635 eV so that the PER curve of anhydrous ethanol reached the sharpest peak as shown in Fig. 5(c). On the contrary, if we still depend on the method of observing the frequency shift of the resonance peak, we will fail to tell the difference as the reflection spectra overlap in a wide range as shown in Fig. 5(d).
Case-2: DNA amplification method has been recognized as an alternative to polymerase chain reaction for virus detection nowadays [26–28]. Microcavity inline Mach-Zehnder interferometer ($\mathrm {\mu }$IMZI) offers a direct, real-time and label-free isothermal DNA amplification monitoring method with the advantages of high sensitivity and high linearity in a short time [29]. However, the detection principle of the DNA amplification method is actually the change of the refractive index of the solution induced by the synthesis of new DNA strands. Figure 5(e) demonstrates the process of the DNA amplification, where the refractive index of the solution changes from 1.3333 to 1.3343 with the synthesis of new DNA strands. Given 0.640 eV Fermi energy imposed over the graphene, the polarization purity reaches the peak with the refractive index of 1.3333. It can be seen that the peak value of PER decreases continuously as the refractive index increases, and the corresponding frequency of the peak is red-shifted compared with the peak frequency corresponding to n =1.3333. Compared with $\mathrm {\mu }$IMZI sensing in Fig. 5(f), graphene-modulated PER sensing is more sensitive and accurate when the refractive indices are very close.
In fact, the proposed hybrid graphene meta-surface has excellent performance not only in the refractive index range of 1.3-1.4 given in the above two examples, but can also satisfy the detection accuracy over the refractive index range of 1-1.6 by setting the proper Fermi level of graphene. A refractive index distinguishability of 1/10,000 can be achieved when PER < −50 dB. Table 1 demonstrates when the refractive index is changed from 1 to 1.6 in 0.1 intervals, the maximum polarization purity can always be found to meet the 1/10,000 refractive index distinguishability requirement through the change of graphene Fermi level. This refractive index range includes many common biochemical solutions, which makes our proposal universal.
Table 2 presents a detailed comparison between the previous studies on meta-surface sensors and our proposed design. Reference [8] proposed highly sensitive graphene plasmonic meta-surfaces to characterize refractive index of viruses by detecting the polarization state of the reflected electric fields spectrum at 1-2 THz in the refractive index range of 1-1.5 with a 1/1,000 distinguishability. Reference [30] proposed a graphene meta-surface-based cross polarization converter operating for detecting biomolecules such as SARS-CoV-2 virus at 1-3.5 THz in the refractive index range of 1.29-1.37 with a 1/100 distinguishability. Reference [31] investigated a chiral meta-surface sensor filled with ferromagnetic nanofluids for LHCP and RHCP sensing of nanoparticle concentration at 0.5-1 THz in the refractive index range of 1-1.9 with a 1/100 distinguishability. Based on coupled mode theory, Ref. [32] proposed a graphene meta-surface composed of a continuous graphene strip and a truncated graphene strip for sensing at 3-7 THz in the refractive index range of 1-1.62 with a 1/100 distinguishability. Reference [33] proposed a metallic toroidal dipole meta-surface for sensing applications at 2.5-5 THz in the refractive index range of 1-2 with a 1/100 distinguishability. Reference [34] demonstrated high-Q Fano terahertz resonance in all-dielectric meta-surface for refractive-index sensing at 1.65-1.95 THz in the refractive index range of 1-2 with a 1/10 distinguishability. Reference [35] proposed a plasmon induced tunable meta-surface for multiband superabsorption and terahertz sensing at 1.25-1.75 THz in the refractive index range of 1-2 with a 1/10 distinguishability. Different from the present sensors above achieving the highly sensing characteristics on the basis of observing the frequency shifts of the resonances varied with different refractive index of the analyte, our proposal employs the Fano resonances induced high-purity CP spectra for high-precision refractive index sensing on the basis of PER analysis. Compared with these literatures, our design should achieve much more accurate sensing applications with the great capacity of refractive index distinguishability of 1/10,000 in refractive index range of 1-1.6.
4. Conclusions
In conclusion, we have demonstrated the high-precision refractive index sensing through Fano resonances induced high-purity CP spectra using hybrid resonator-graphene meta-surfaces. The greatest polarization purity of the reflecting spectra with linear-to-circular polarization conversion can readily be obtained at the Fano resonance though tuning the Fermi level of the graphene, and two cases of biochemical detections have validated the advantages our proposal of using the PER peak variations compared with the observations of the frequency shifts of the resonances, thus should offer promising prospects in the high-precision detection of biochemical solutions.
Funding
National Natural Science Foundation of China (61301072, 61671344).
Disclosures
The authors declare no conflicts of interest.
Data availability
Data underlying the results presented in this paper are not publicly available at this time but may be obtained from the authors upon reasonable request.
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