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摘要:
表面增强拉曼散射(SERS)传感器在诸多领域拥有重要的应用潜力。为实现高精度SERS检测，增加热点密度和热点区域中分析物分子数量成为当前研究的重点。超快激光可快速在材料表面构筑大面积的微纳米结构，对于高性能SERS基底的商业化制备具有重要的意义。本文从热点密度和检测区域中分析物分子浓度两个方面，总结了近年来超快激光制造高性能SERS基底的工艺方法。超快激光既能“自下而上”，也能“自上而下”加工出具有局域场增强效应的微纳米结构。其中，超快激光制备的超疏水表面是目前实现待测分子富集的有效方法之一。最后展望了激光制备SERS基底的应用前景。
Abstract:Surface-enhanced Raman scattering (SERS) provides important applications in diverse fields. In order to achieve high-precision SERS detection of trace molecules, current research focuses on how to increase the density of hot spots and the number of analyte molecules in the detection area. An ultrafast laser can rapidly construct large-area micro/nano-structures on material surfaces. It is important for the commercial preparation of high-performance SERS sensors. In this paper, the ultrafast laser preparation of high-performance SERS sensors is introduced from the aspect of the density of hot spots and the number of analyte molecules in the detection region. Ultrafast lasers enable both "bottom-up" and "top-down" processing. In particular, the superhydrophobic surface prepared by the ultrafast laser is one of the most effective methods to achieve the enrichment of analyte molecules. Finally, a prospect for the development of laser-prepared SERS substrates is provided.
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图 2 (a) 飞秒激光诱导银/钯合金还原示意图 [31]； (b) 两步飞秒激光诱导银离子还原形成的纳米结构 [32]；(c) 固液界面等离子体增强还原银离子示意图 [33]； (d) 激光诱导正向转移制备SERS基片示意图 [35]；(e) 脉冲激光沉积形成的金属纳米结构 [37]
Figure 2. (a) Schematic diagram of femtosecond laser-induced reduction of silver/palladium alloy [31]; (b) Nanostructures formed by two-step femtosecond laser-induced reduction of silver ions [32]; (c) Schematic diagram of the plasma-enhanced reduction of silver ionsat the solid-liquid interface [33]; (d) Schematic diagram of SERS substrates prepared by laser-induced forward transfer [35]; (e) Metal nanostructures formed by pulsed laser deposition [37]
图 3 (a)飞秒激光在空气中制备银基SERS基底 [42]； (b) 飞秒激光在氩气氛围中制备银基SERS基底(S-Ag-Ar) [44]；(c) 飞秒激光制备金基SERS基底 [47]
Figure 3. (a) Femtosecond laser preparation of silver-based SERS substrates in air [42]; (b) Femtosecond laser preparation of silver-based SERS substrates (S-Ag-Ar) in an argon atmosphere [44]; (c) Femtosecond laser preparation of gold-based SERS substrates [47]
图 7 (a) 超敏感SERS基底的制造示意图 [74]； (b) 混合超亲水/超疏水基底的制造示意图 [75]； (c) 混合型超亲水/超疏水微孔SERS基底的示意图 [27]
Figure 7. (a) Schematic of the fabrication strategy of ultrasensitive SERS substrates [74]; (b) Schematic of the fabrication strategy of hybrid superhydrophilic/superhydrophobic substrates [75]; (c) Schematic of hybrid superhydrophilic/superhydrophobic microporous SERS substrates [27]
表 1 基于超快激光制备的各种类型SERS传感器的性能对比
Table 1. Performance comparison among various types of SERS sensors prepared by the ultrafast laser
基底材料 活性热点 加工方式 表面润湿性 分析物 检测极限/(mol/L) 增强因子 参考文献 活性热点的增加 微通道 银纳米颗粒 飞秒激光 / 对氨基苯硫酚 10−10 4 × 108 [22] 微通道 银/钯合金纳米颗粒 飞秒激光 / R6G 10−9 2.62 × 108 [31] 硅 银纳米颗粒 飞秒激光 亲水 R6G 10−12 / [33] 银 银纳米颗粒 飞秒激光 / R6G 10−8 1.2 × 106 [42] 银 银纳米颗粒 飞秒激光 / R6G 10−8 5.6 × 106 [44] 金 金纳米颗粒 飞秒激光 / DPA 10−15 / [47] 硅 金纳米颗粒 飞秒激光 / R6G / 4.3 × 107 [62] 钛 银纳米颗粒 飞秒激光/水热法 / R6G 10−14 1.2 × 109 [61] 铜 银纳米颗粒 纳秒激光/热氧化 / 4-甲苯硫酚 / 1.44 × 105 [60] 目标分子的富集 硅 银纳米颗粒 飞秒激光 超疏水 R6G 10−14 6 × 106 [72] 铜 铜纳米颗粒 飞秒激光 超疏水 R6G 10−13 1.2 × 105 [71] 不锈钢 银纳米颗粒 飞秒激光 超疏水/疏水 R6G 10−14 5.7 × 108 [68] 硅/PDMS 金纳米颗粒 飞秒激光 超疏水/超亲水 R6G 10−16 / [35] 聚四氟乙烯基 银纳米颗粒 飞秒激光 超疏水/超亲水 R6G 10−12 1 × 107 [74] 铜 纳米金星 飞秒激光 超疏水/超亲水 R6G 10−18 1.09 × 1014 [75] 铜 银纳米颗粒 飞秒激光 超疏水/超亲水/微孔 R6G 10−17 5.19 × 1013 [27] 
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