黑硅催化反应的化学非微扰SERS检测
Chemically non-perturbing SERS detection of catalytic reaction with black silicon
摘要：
由高折射率纳米材料制成的全介电谐振微纳米结构最近成为一种有前途的SERS平台，可以补充或潜在地取代常规传感测量中的金属基对应物。这些独特的结构将高度可调的光学响应和高场增强与非侵入性相结合，即，化学上不干扰分析物、简单的化学改性和可再循环性。与此同时，用于大规模生产这种结构的具有商业竞争力的制造技术仍然缺失。在这里，我们证明了一个化学惰性的黑硅（b-Si）基板组成的随机排列的尖刺米氏谐振器的一个真正的非侵入性SERS识别的分子指纹在低浓度。基于对氨基苯硫酚到4，4 `二巯基偶氮苯催化转化在裸硅和镀金属的b-Si上的原位SERS跟踪比较，我们证明了无金属的b-Si在低至10^-6 M的浓度水平下用于超灵敏非侵入性SERS检测的适用性。我们进行时域有限差分计算，以揭示在可见光谱范围内的隔离尖峰硅谐振器提供的电磁增强。用化学活性裸黑色氧化铜进行的PATP至DMAB转化的额外比较SERS研究以及在负载有胶体银纳米颗粒的甲醇水溶液中的缓慢日光驱动的PATP至DAMP催化转化的SERS检测证实了全介电结晶b-Si衬底的非侵入性SERS性能。所提出的SERS衬底可以使用简单的可扩展的等离子体蚀刻技术来制造，该技术适用于大的衬底面积，使得这种廉价的全介电衬底有希望用于常规的SERS应用，其中非侵入性是强制性的重要性。
英文摘要：
All-dielectric resonant micro- and nano-structures made of the high-index dielectrics recently emerge as a promising SERS platform which can complement or potentially replace the metal-based counterparts in routine sensing measurements. These unique structures combine the highly-tunable optical response and high field enhancement with the non-invasiveness, i.e., chemically non-perturbing the analyte, simple chemical modification and recyclability. Meanwhile, the commercially competitive fabrication technologies for mass production of such structures are still missing. Here, we attest a chemically inert black silicon (b-Si) substrate consisting of randomly-arranged spiky Mie resonators for a true non-invasive SERS identification of the molecular fingerprints at low concentrations. Based on comparative in-situ SERS tracking of the para-aminothiophenol -to-4,4` dimercaptoazobenzene catalytic conversion on the bare and metal-coated b-Si, we justify applicability of the metal-free b-Si for the ultra-sensitive non-invasive SERS detection at concentration level as low as 10^-6 M. We perform finite-difference time-domain calculations to reveal the electromagnetic enhancement provided by an isolated spiky Si resonator in the visible spectral range. Additional comparative SERS studies of the PATP-to-DMAB conversion performed with a chemically active bare black copper oxide as well as SERS detection of the slow daylight-driven PATP-to-DAMP catalytic conversion in the aqueous methanol solution loaded with colloidal silver nanoparticles confirm the non-invasive SERS performance of the all-dielectric crystalline b-Si substrate. Proposed SERS substrate can be fabricated using simple scalable technology of plasma etching amenable on large substrate areas making such inexpensive all-dielectric substrates promising for routine SERS applications, where the non-invasiveness is of mandatory importance.
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