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摘要:
表面增强拉曼光谱(Surface-enhanced Raman spectroscopy，SERS)是一种高灵敏度、高分辨率的分子识别技术，在多个领域具有非常重要的应用价值。飞秒激光直写作为一种新兴的低成本、高分辨率、高灵活性的微纳加工方法，在制备SERS基底领域得到了广泛的应用。本文重点概述了四种飞秒激光直写制备SERS基底的加工方法，主要包括飞秒激光双光子还原、飞秒激光切割金属、飞秒激光切割-溅射、飞秒激光3D打印。文章简单介绍了各方法制备SERS基底的性能与应用场景，阐述了飞秒激光直写加工在制备SERS基底中的优势，旨在为今后相关研究提供参考。
Abstract:Surface-enhanced Raman spectroscopy (SERS) technique plays an important role in molecular recognition fields due to its highly sensitive and high-resolution. As an emerging low-cost, high machining accuracy, and high-flexibility processing method, femtosecond laser direct writing processing has been widely used in the field of preparing SERS substrates. This work introduces four methods of preparing SERS substrates by femtosecond laser direct writing, including femtosecond two-photon reduction, femtosecond laser cutting metal, femtosecond laser cutting-sputtering, and femtosecond laser 3D printing. The article introduces the performance and application scenarios of each method in preparing SERS substrates and illustrates the advantages of femtosecond laser direct writing processing in preparing SERS substrates, aiming to provide a reference for future related research.
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Key words:
- SERS /
- femtosecond laser direct writing /
- micro/nano processing /
- SERS substrate
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图 2 SERS原理。 (a) 波纹金属表面上分子的非弹性光散射[33]； (b) 贵金属表面发生等离子体共振现象[36]
Figure 2. SERS principle. (a) Inelastic light scattering of molecules on corrugated metal surfaces[33]; (b) localized surface plasmon resonances (LSPRs) on the surface of precious metals[36]. Figure reproduced with permission from: (a) ref. [33] © American Chemical Society; (b) ref. [36] © The Royal Society of Chemistry
图 3 自上而下微加工和微粒自组装方法制备SERS微结构。 (a) RIE[45]； (b, c) EBL[46-47]； (d~f) 纳米颗粒自组装[48-50]. 比例尺：(e) 20 nm；(f) 200 nm
Figure 3. Preparation of SERS microstructures by top-down micromachining and particle self-assembly. (a) RIE[45]; (b, c) EBL[46-47]; (d-f) Nanoparticle self-assembly[48-50]; Scale bar: (e) 20 nm; (f) 200 nm. Figure reproduced with permission from: (a) ref. [45] © American Chemical Society; (b) ref. [46], (e) ref. [49] and (f) ref. [50] © under a Creative Commons Attribution-NonCommercial-No- Derivatives 4.0 International License; (c) ref. [47] © American Chemical Society; (d) ref. [48] © The American Association for the Advancement of Science
图 4 微柱自组装方法制备SERS微结构。 (a) 金纳米微柱自组装[55]； (b) 聚合物-银微柱自组装[56]；(c) 聚合物-银微柱自组装[57]； (d) 银微柱自组装[58]；(e)聚合物-金微柱自组装[59]
Figure 4. Preparation of SERS microstructure by microcolumn self-assembly methods. (a) Self-assembly of gold nanopillars[55]; (b) Self-assembly of polymer-silver micropillars[56]; (c) Self-assembly of polymer-silver micropillars[57]; (d) Self-assembly of silver micropillars[58]; (e) Self-assembly of polymer-gold micropillars[59]. Figure reproduced with permission from: (a) ref. [55] and (e) ref. [59] © American Chemical Society; (b) ref. [56], (c) ref. [57] and (d) ref. [58] © Wiley
图 5 飞秒双光子金属还原制备SERS基底。(a) 双光子还原原理[70]； (b) 双光子还原银微线[71]；(c~e) 微通道SERS基底[72-74]； 比例尺：(b) 10 µm； (e) 1 µm
Figure 5. Femtosecond two-photon reduction to prepare SERS substrates. (a) Two-photon reduction principle[70]; (b)Two-photon reduced silver microwire[71]; Scale bar: (b) 10 μm; (e) 1 μm. Figure reproduced with permission from: (a) ref. [70], (b) ref. [71], (c) ref. [74] and (e) ref. [71] © Wiley; (d) ref. [72] © The Royal Society of Chemistry
图 6 飞秒激光切割金属制备SERS基底。(a) 飞秒激光直接烧蚀金属表面形成纳米结构机理[80]； (b) Ag周期性表面[91]； (c) 铜表面直接制备超亲水-超疏水图案化基底结构[30]；(d) S-Ag-Ar基底[92]； (e) 钛合金SERS基底[93]
Figure 6. Femtosecond laser cutting metal to prepare SERS substrate. (a) Femtosecond laser directly ablated metal surface forming nanostructure principle [80]; (b) Ag periodic surface[91]; (c) Superhydrophilic - superhydrophobic patterned substrate structures were prepared directly on copper surface [30]; (d) S-Ag-Ar substrate[92]; (e) Titanium alloy SERS substrate[93]. Figure reproduced with permission from: (a) ref. [80] © Elsevier; (b) ref. [91], (c) ref. [30] and (d) ref. [92] © Elsevier; (e) ref. [93] © under a Creative Commons Attribution-NonCommercial-No- Derivatives 4.0 International License
图 7 飞秒激光切割-溅射制备SERS基底。(a) 大面积SERS基底[105]； (b) 柔性透明SERS基底[31]； (c) 玻璃SERS基底[106]； (d) 疏水-超疏水SERS基底[107]； (e) 超疏水-亲水SERS基底[108]
Figure 7. Femtosecond laser cutting-sputtering to prepare a SERS substrate. (a) Large area SERS substrate[105]; (b) Flexible transparent SERS substrate[31]; (c) Glass SERS substrate[106]; (d) Hydrophobic-superhydrophobic SERS substrate[107]; (e) Superhydrophobic-hydrophilic SERS substrate[108] . Figure reproduced with permission from: (a) ref. [108], (b) ref. [31] and (c) ref. [106] © Elsevier; (d) ref. [107] © BioMed Central Ltd unless otherwise stated; (e) ref. [108] © American Chemical Society
图 8 双光子直写结合金属蒸镀。(a, b) 光纤端面三维SERS结构[121-122]
Figure 8. Two-photon direct writing combined metal evaporation. (a, b) 3D SERS structure of fiber surface [121-122]. Figure reproduced with permission from: (a) ref. [121] © under a Creative Commons Attribution-NonCommercial-No-Derivatives 4.0 International License; (b) ref. [122] © Wiley
图 9 飞秒激光加工毛细力自组装制备SERS基底。(a) 毛细力自组装[126]；(b) 基于毛细力自组装微通道的三维SERS结构[7]
Figure 9. Femtosecond laser processing capillary self-assembly to prepare SERS substrate. (a) Capillary force self-assembly[126]; (b) Three-dimensional SERS structure based on capillary force self-assembly microchannels[7]. Figure reproduced with permission from: (a) ref. [126] © American Chemical Society; (b) ref. [7] © Wiley
表 1 四种飞秒激光加工SERS基底各方法对比
Table 1. Comparison of four methods for processing SERS substrates by femtosecond laser
基底类型及维度 微纳结构 分析物 检测浓度下限/mol 增强因子 特殊基底 参考文献 双光子还原金属—-三维 银微花阵列 4-AP 10−10 1×108 封闭微通道 [71] 银钯纳米颗粒 R6G 10−9 2.6×108 封闭微通道 [73] 银纳米颗粒 CV 10−13 / 封闭微通道 [74] 粗糙银纳米结构 R6G 10−9 1×107 光纤端面 [78] 飞秒激光切割金属—二维 金纳米颗粒 R6G 10−9 2.4×108 金板 [94] 铜微粒和粒子团 R6G 10−14 2.09×1014 铜板 [30] 银微粒和粒子团 R6G 10−8 5.3×1014 银板 [92] 钛合金纳米颗粒 R6G 10−11 7.85×105 钛合金 [97] 飞秒激光切割-溅射—二维 金铂纳米颗粒 R6G 10−6 8.46×107 硅 [105] 银纳米颗粒 R6G 10−12 5.6×107 柔性FEP膜 [31] 银纳米颗粒 R6G / 2×105 玻璃 [106] 金纳米颗粒 R6G 10−6 / PTFE [117] 银纳米颗粒 R6G 10−17 5.19×1013 铜箔 [109] 飞秒激光3D打印—三维 金纳米颗粒 水晶紫 10−6 / 光纤端面 [121] 金纳米颗粒 R6G 10−7 3×103 光纤端面 [122] 金纳米颗粒 R6G 10−6 8×107 开放微通道 [7] 
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