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中国物理学会期刊

InSb光栅耦合的太赫兹表面等离子体共振生化传感方法的实验研究

Experimental Study of InSb Grating-Coupled Terahertz Surface Plasmon Resonance Biochemical Sensing Method

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  • 锑化铟是一种窄禁带半导体,在太赫兹(THz)波段具有表面等离子体共振(SPR)效应,它为实验研究被长期忽视的THz-SPR生化传感方法创造了条件。本文首先对锑化铟光栅耦合的THz-SPR机理和特性进行了仿真分析,在此基础上设计制备了不同周期的锑化铟光栅,利用THz时域光谱仪测试了干燥空气中的锑化铟光栅在入射角为30°时的p-偏振THz反射频谱,观测到尖锐的THz-SPR吸收峰,获得了共振频率与光栅周期的关系曲线,系统测试了周期为130 μm的锑化铟光栅的THz-SPR生化传感特性,测得其在入射角30°下对液体折射率的灵敏度为0.665 THz/RIU;基于碳酸钙沉积反应,实现了锑化铟光栅THz-SPR传感芯片对水溶液中钙离子的识别探测,实验结果表明,在1-10 mmol/L 范围内THz-SPR共振频率随钙离子浓度增加线性升高,灵敏度为 0.0032 THz/(mmol/L),对1 mmol/L的钙离子探测结果具有重复性。进一步利用锑化铟光栅表面的碳酸钙沉积反应,实现了胎牛血清样品中的游离钙浓度探测,通过与第三方利用ICP-MS方法测得的结果比较,验证了探测结果合理可信。本文取得的实验结果填补了我国在THz-SPR生化检测领域的研究空白,为太赫兹生化传感器的片上集成和实际应用奠定了实验基础。

    Indium antimonide (InSb) is a narrow-bandgap semiconductor that supports intrinsic surface plasmon resonance (SPR) effects in the terahertz (THz) frequency range. By avoiding the manufacturing complexities and low quality factors associated with artificial spoof surface plasmon polaritons (SSPPs), it provides favorable conditions for experimental investigations of THz-SPR-based biochemical sensing methods that have long been overlooked. In this work, the InSb grating-coupled THz-SPR mechanism and properties were first analyzed through numerical simulations using the Drude-Lorentz material model. Based on these theoretical results, which optimized the grating ridge height to 7 μm and the duty cycle to 0.5, periodic InSb gratings with varying periods ranging from 100 to 160 μm were designed and fabricated. The fabrication utilized standard semiconductor processes on a heavily Te-doped InSb wafer, including deep reactive ion etching (DRIE) and inductively coupled plasma (ICP) etching. Using a custom-built reflection-mode measurement module integrated with a THz time-domain spectrometer (THz-TDS), the p-polarized THz reflection spectra of the InSb gratings in dry air were measured at a fixed incident angle of 30°. High-resolution frequency spectra were acquired by applying zero-padding and fast Fourier transform (FFT) to the time-domain signals, revealing extremely sharp intrinsic THz-SPR absorption peaks. The experimentally measured relationship between the resonance frequency and the grating period matched the theoretical calculations excellently. Subsequently, the THz-SPR biochemical sensing performance of an optimized InSb grating with a period of 130 μm was systematically investigated. In the unloaded state, this sensing chip exhibited a distinct resonance frequency of 1.540 THz, a narrow full width at half maximum (FWHM) of 8.20 GHz, and a high quality factor of 188. By utilizing glycerol-ethanol mixed solutions with varying volume fractions as the dielectric media, a high refractive-index sensitivity of 0.665 THz/RIU for liquids was achieved at an incident angle of 30°, significantly outperforming most reported metasurface-based THz-SSPP sensors. Furthermore, to overcome the severe interference caused by the strong THz absorption of liquid water, a specific detection method based on a calcium carbonate deposition reaction was introduced. Through the selective combination and sedimentation of target ions using a saturated sodium carbonate solution, the quantitative detection of calcium ions in aqueous solutions was realized using the InSb grating THz-SPR sensing chip. The experimental results show that, within the concentration range of 1-10 mmol/L, the THz-SPR resonance frequency increases linearly with increasing calcium ion concentration, demonstrating a high sensitivity of 0.0032 THz/(mmol/L) and excellent measurement consistency. Good repeatability was also demonstrated for the detection of 1 mmol/L calcium ions by restoring the initial resonance frequency after cleaning. Furthermore, by exploiting the calcium carbonate deposition reaction on the surface of the InSb grating, the concentration of free calcium ions in fetal bovine serum samples was measured. The sensing chip detected an ionized calcium concentration of 2.08 mmol/L. Comparison with total calcium concentration results obtained by a third party using inductively coupled plasma mass spectrometry (ICP-MS) verified the reliability and validity of the proposed method, as the measured free calcium closely matches the standard proportion of ionized calcium in serum. The experimental results reported in this paper fill a research gap in the field of THz-SPR biochemical detection in China. By demonstrating a structurally simple, highly tunable, and semiconductor-process-compatible platform, this work highlights the unique advantages of intrinsic THz-SPR in achieving high-Q biomolecular detection, laying a robust experimental foundation for the on-chip integration and practical application of terahertz biochemical sensors.

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