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Ultrasensitive Biosensor with Hyperbolic Metamaterials Composed of Silver and Zinc Oxide

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Ultrasensitive Biosensor with Hyperbolic Metamaterials Composed of Silver and Zinc Oxide nanomaterials Article Ultrasensitive Biosensor with Hyperbolic Metamaterials Composed of Silver and Zinc Oxide Shuhan Chen 1,* , Shiqi Hu 2, Yichen Wu 1, Dingnan Deng 1, Yunhan Luo 2,* and Zhe Chen 2 1 School of Physics and Electronic Engineering, Jiaying University, Meizhou 514015, China; [email protected] (Y.W.); [email protected] (D.D.) 2 Key Laboratory of Optoelectronic Information and Sensing Technologies of Guangdong Higher Education Institutes, College of Science and Engineering, Jinan University, Guangzhou 510632, China; [email protected] (S.H.); [email protected] (Z.C.) * Correspondence: [email protected] (S.C.); [email protected] (Y.L.) Abstract: We propose a hyperbolic metamaterial-based surface plasmon resonance (HMM-SPR) sensor by composing a few pairs of alternating silver (Ag) and zinc oxide (ZnO) layers. Aiming to achieve the best design for the sensor, the dependence of the sensitivity on the incidence angle, the thickness of the alternating layer and the metal filling fraction are explored comprehensively. We find that the proposed HMM-SPR sensor achieves an average sensitivity of 34,800 nm per refractive index unit (RIU) and a figure of merit (FOM) of 470.7 RIU−1 in the refractive index ranging from 1.33 to 1.34. Both the sensitivity (S) and the FOM show great enhancement when compared to the conventional silver-based SPR sensor (Ag-SPR). The underlying physical reason for the higher performance is analyzed by numerical simulation using the finite element method. The higher sensitivity could be attributed to the enhanced electric field amplitude and the increased penetration Citation: Chen, S.; Hu, S.; Wu, Y.; depth, which respectively increase the interaction strength and the sensing volume. The proposed Deng, D.; Luo, Y.; Chen, Z. HMM-SPR sensor with greatly improved sensitivity and an improved figure of merit is expected to Ultrasensitive Biosensor with find application in biochemical sensing due to the higher resolution. Hyperbolic Metamaterials Composed of Silver and Zinc Oxide. Nanomaterials Keywords: surface plasmon resonance; hyperbolic metamaterials; silver and zinc oxide; sensitivity; 2021, 11, 2220. https://doi.org/ figure of merit 10.3390/nano11092220 Academic Editor: Andrey B. Evlyukhin 1. Introduction Surface Plasma Resonance (SPR) sensors have become a promising method in the Received: 28 July 2021 field of food safety, drug screening and biological sensors over the last two decades [1–3]. Accepted: 25 August 2021 Published: 28 August 2021 To excite SPR, two configurations have usually been employed, namely Kretschmann configuration and grating coupling configuration [4]. In the Kreschmann configuration, Publisher’s Note: MDPI stays neutral spectral scan and angular scan interrogation are usually employed to measure the reflected with regard to jurisdictional claims in signal [5]. Although the angular scan interrogation is possible to achieve higher signal-to- published maps and institutional affil- noise, the spectral scan has the advantages of low cost, easy fabrication and a compact fiber iations. sensor [6]. Currently, various materials are added to the structure of traditional prism-coupled SPR biosensors to achieve ultra-high detection sensitivity, ultra-high detection accuracy and low detection threshold. For example, metallic nanoparticles and complex nanostructures have been used to enhance the sensitivity of SPR sensors [7,8]. Nanomaterials, such as TiO Copyright: © 2021 by the authors. 2 and graphene, have been deposited to modify the metal for exciting long-range surface Licensee MDPI, Basel, Switzerland. This article is an open access article plasmon [9,10]. distributed under the terms and Recently, hyperbolic metamaterials (HMM), which have been demonstrated to en- conditions of the Creative Commons hance the performance of SPR sensors distinctly, are one of the most concerned metamate- Attribution (CC BY) license (https:// rials with the real part of the permittivity components having opposite signs [11–13]. For creativecommons.org/licenses/by/ instance, the gold/Al2O3 multilayered structure was fabricated as HMM-based sensors to 4.0/). Nanomaterials 2021, 11, 2220. https://doi.org/10.3390/nano11092220 https://www.mdpi.com/journal/nanomaterials Nanomaterials 2021, 11, 2220 2 of 9 Nanomaterials 2021, 11, x FOR PEER REVIEW 2 of 9 −1 achieve a sensitivity of 30,000 nm/RIU and an FOM of 509 RIU [14]. An Ag/TiO2 HMM- based fiber plasmonic sensor was fabricated to achieve a sensitivity of 9000 nm/RIU and −1 −1 anachieve FOM a ofsensitivity 230.8 RIU of 30,000, which nm/RIU has theand advantagean FOM of 509 of miniaturizationRIU [14]. An Ag/TiO and2 integration HMM- [15]. Amongbased fiber a lot plasmonic of semiconductors, sensor was fabricated ZnO as to a wideachieve band a sensitivity gap semiconductor of 9000 nm/RIU was and found to havean FOM high of 230.8 thermal RIU and−1, which chemical has the stability, advantage and of mini thusaturization it is an ideal and materialintegration to [15]. protect the metallicAmong a layer lot of from semiconductors, oxidation [ 16ZnO]. as a wide band gap semiconductor was found to haveIn high this thermal study, and an HMM-SPR chemical stability, sensor and composed thus it is of an alternating ideal material Ag/ZnO to protect layers the is investi- metallic layer from oxidation [16]. gated. The ZnO layer is used to protect the Ag layer from oxidation. The HMM structure In this study, an HMM-SPR sensor composed of alternating Ag/ZnO layers is inves- composedtigated. The of ZnO Ag/ZnO layer is used multi-layers to protect is th demonstratede Ag layer from tooxidation. greatly The improve HMM thestructure sensitivity of thecomposed SPR sensor. of Ag/ZnO The effectsmulti-layers of the is incidencedemonstrated angle, to greatly alternating improve layer the thicknesssensitivity andof metal fillingthe SPR factor sensor. on The the effects sensitivity of the of incidence the sensor angle, are alternating studied using layer thethickness transfer and matrix metal method (TMM)filling factor [17]. on The the underlying sensitivity of physical the sensor reason are studied for the using higher the transfer performance matrix method is analyzed by using(TMM) finite [17]. elementThe underlying method physical [18]. The reason improvement for the higher is attributedperformance to is the analyzed enhanced by electric fieldusing amplitude finite element and method the increased [18]. The penetrationimprovement depth,is attributed which to respectivelythe enhanced increaseelectric the in- teractionfield amplitude strength and and the increa the sensingsed penetration volume. depth, With which optimized respectively parameters, increase the the average in- S of 34,800teraction nm/RIU strength and and FOMthe sensing of 470.7 volume. RIU− 1Wiareth achievedoptimized inparameters, the range the of 1.33average to 1.34S of RIU. 34,800 nm/RIU and FOM of 470.7 RIU−1 are achieved in the range of 1.33 to 1.34 RIU. 2. Model and Theory 2. Model and Theory In the proposed structure, the SPR sensor based on HMM composed of Ag/ZnO is shownIn inthe Figure proposed1. The structure, Kretschmann the SPR sensor configuration based on is HMM used composed to excite theof Ag/ZnO surface is plasmon shown in Figure 1. The Kretschmann configuration is used to excite the surface plasmon wave, where a BK7 prism is used as the coupling element. The Ag/ZnO bilayer in the wave, where a BK7 prism is used as the coupling element. The Ag/ZnO bilayer in the structurestructure has has aa thickness thickness approximate approximate 30 nm, 30 nm,which which is much is muchsmaller smaller than the than exciting the exciting wavelengthwavelength (500–2000 (500–2000 nm). nm). Therefore, Therefore, the thealternating alternating Ag/ZnO Ag/ZnO layers layerscan be assumed can be assumed to to bebe a uniform medium. medium. FigureFigure 1. SchematicSchematic diagram diagram of ofthe the proposed proposed SPR SPR sensor sensor with withhyperbolic hyperbolic metamaterial metamaterial composed composed of of Ag/ZnO. Ag/ZnO. The effective effective medium medium theory theory (EMT) (EMT) is used is used to evaluate to evaluate the parallel the parallel and perpendicu- and perpendicular lar component of equivalent dielectric tensors of the HMM [19] with the following formu- component of equivalent dielectric tensors of the HMM [19] with the following formulas: las: dAg#Ag + dZnO#ZnO (1) #x = (1) dAg + dZnO (2) /dAg +d/ZnO # = (2) z + where and denote the thickness,dAg/# Agwhiled ZnO /and#ZnO denote the dielectric permittivity of the Ag and ZnO layer, respectively. The is obtained according to Ref. where dAg and dZnO denote the thickness, while #Ag and #ZnO denote the dielectric permit- [20]. The is obtained according to Ref. [21], using the following formula: tivity of the Ag and ZnO layer, respectively. The #Ag is obtained according to Ref. [20]. The #ZnO is obtained according to Ref. [21], using the following formula: 0.87968l2 n2 = 2.81418 + − 0.00711l2 (3) l2 − 0.30422 Nanomaterials 2021, 11, 2220 3 of 9 where l denotes the wavelength. The refractive index of the sensing medium is set as ns = 1.33. The refractive index of BK7 prism (np) is obtained according to the formula as follows: Nanomaterials 2021, 11, x FOR PEER REVIEW 2 2 3 of2 9 2 1.03961212l 0.231792344l 1.01046945l np − 1= + + (4) l2 − 0.006000698672 l2 − 0.02001791442 l2 − 103.5606532 To solve the proposed multilayer0.87968 systems, the transfer matrix method is employed 2.81418 0.00711 (3) due to its simplicity and flexibility. For the 0.3042N-layer model in this study, the propagation characteristicwhere denotes is describedthe wavelength. by transfer The refractive matrix Sindexm [22 of], i.e.,the sensing medium is set as 1.33. The refractive index of BK7 prism () is obtained according to the formula as N ! follows: S11 S12 S = = ∏ I(m−1)m Lm ·IN(N+1) (5) .S21 S22 . 1= m=1 (4) .
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