Optical conductivity-based ultrasensitive mid-infrared biosensing on a hybrid metasurface.
Optical conductivity-based ultrasensitive mid-infrared biosensing on a hybrid metasurface.
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DOI：
10.1038/s41377-018-0066-1
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发表时间：
2018
期刊：
影响因子：
--
通讯作者：
Lin Q
中科院分区：
文献类型：
--
作者：
Zhu Y;Li Z;Hao Z;DiMarco C;Maturavongsadit P;Hao Y;Lu M;Stein A;Wang Q;Hone J;Yu N;Lin Q
光学器件对于生物传感具有高度吸引力，因为它们不仅可以实现分析物的定量测量，而且还可以提供关于分子结构的信息。不幸的是，典型的基于折射率的光学传感器不具有足够的灵敏度来探测低分子量分析物的结合。场效应晶体管等非光学器件可能更敏感，但不提供光学器件的一些重要特征，特别是分子指纹。我们提出了基于光学电导率的中红外（中红外）生物传感器，允许灵敏和定量测量的低分子量的分析物，以及光谱指纹的增强。该传感器采用由单层石墨烯和金属纳米天线组成的混合超颖表面，并联合收割机结合了等离子体、电子和光谱方法的各自优势。首先，混合超颖表面传感器可以光学检测目标分子诱导的载流子掺杂到石墨烯，允许高灵敏度检测低分子量分析物，尽管它们的小尺寸。其次，由石墨烯光学电导率的变化引起的共振位移是石墨烯载流子密度的明确定义的函数，从而允许量化分子的结合。第三，由于其对石墨烯载流子迁移率降低的不敏感性，传感器性能高度稳定和一致。最后，传感器还可以作为表面增强红外光谱的基底。我们展示了亚纳米大小的分子或颗粒的单层的测量和基于亲和结合的定量检测葡萄糖低至200 pM（36 pg/mL）。我们还展示了微量葡萄糖和聚合物分子的增强指纹。一种高灵敏度的葡萄糖传感器已被构建从功能化的石墨烯-金属混合超颖表面。由哥伦比亚大学，南卡罗来纳州大学，布鲁克海文国家实验室和南京大学的中美合作开创的该设备通过检测石墨烯光学电导率的变化，通过其等离子体共振波长的微小偏移，能够超灵敏地检测葡萄糖浓度，小至200 pM，然后测量。重要的是，新的传感原理克服了由分子量或局部折射率变化定义的检测极限，这在很长一段时间内阻碍了更灵敏的光学生物传感器的发展。该器件由单层石墨烯覆盖金纳米棒阵列组成，顶部是铂-二氧化硅-铂三明治，用作光学腔。当石墨烯用用作葡萄糖结合剂的硼酸官能化时，可以看到器件的波长响应随着葡萄糖浓度的增加而明显红移。实验表明，测量的动态范围超过6个数量级，从2nM到10 mM。
Optical devices are highly attractive for biosensing as they can not only enable quantitative measurements of analytes but also provide information on molecular structures. Unfortunately, typical refractive index-based optical sensors do not have sufficient sensitivity to probe the binding of low-molecular-weight analytes. Non-optical devices such as field-effect transistors can be more sensitive but do not offer some of the significant features of optical devices, particularly molecular fingerprinting. We present optical conductivity-based mid-infrared (mid-IR) biosensors that allow for sensitive and quantitative measurements of low-molecular-weight analytes as well as the enhancement of spectral fingerprints. The sensors employ a hybrid metasurface consisting of monolayer graphene and metallic nano-antennas and combine individual advantages of plasmonic, electronic and spectroscopic approaches. First, the hybrid metasurface sensors can optically detect target molecule-induced carrier doping to graphene, allowing highly sensitive detection of low-molecular-weight analytes despite their small sizes. Second, the resonance shifts caused by changes in graphene optical conductivity is a well-defined function of graphene carrier density, thereby allowing for quantification of the binding of molecules. Third, the sensor performance is highly stable and consistent thanks to its insensitivity to graphene carrier mobility degradation. Finally, the sensors can also act as substrates for surface-enhanced infrared spectroscopy. We demonstrated the measurement of monolayers of sub-nanometer-sized molecules or particles and affinity binding-based quantitative detection of glucose down to 200 pM (36 pg/mL). We also demonstrated enhanced fingerprinting of minute quantities of glucose and polymer molecules. A highly sensitive glucose sensor has been constructed from a functionalized graphene-metallic hybrid metasurface. Pioneered by a US-Chinese collaboration from Columbia University, University of South Carolina, Brookhaven National Laboratory and Nanjing University the device by detecting the changes in graphene optical conductivity, enables ultrasensitive detection of glucose concentrations as small as 200 pM via a small shift in its plasmonic resonant wavelength which is then measured. Importantly, the new sensing principle overcomes the detection limit defined by the molecular weight or the changes in local refractive index, which for a long time has impeded the development of more sensitive optical biosensors. The device consists of a monolayer of graphene covering an array of gold nanorods, atop a platinum-silicon dioxide-platinum sandwich that serves as an optical cavity. When the graphene is functionalized with boronic acid which serves as a glucose binding agent, the device’s wavelength response was seen to clearly red shift with increasingly glucose concentration. Experiments indicate a dynamic range of measurement of over 6 orders of magnitude from 2nM to 10mM.
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