Fabrication of silicon nanowire networks for biological sensing
Introduction
One dimensional nanostructures such as nanowires (NWs) and nanotubes (NTs) with high aspect ratio are quite exciting and promising materials. Due to their high surface to volume ratio, NWs and NTs are considered to be excellent candidates for ultrasensitive biological and chemical sensors [1], [2], [3], [4], [5], [6], [7], [8], [9], [10], [11], [12], [13]. The sensing mechanism of semiconducting nanostructures is based on the binding of charged biological or chemical molecules at the surface of the nanomaterials that causes changes in structural surface properties or in the entire cross-section in the case of the smaller-ones (<Bohr radius). Considering more particularly the biosensors based on target–probe recognition, the usually used planar configuration suffers from limited probe immobilization capacity and inaccessibility of target to probes due to steric hindrances [14], [15]. In contrast, the collective use of high aspect ratio nanostructures increases the immobilization probe concentration and hence the number of available sites for target–probe recognition [16] thereby reducing steric hindrance [17].
Currently, individual nanowires and nanotubes can be integrated into highly sensitive and selective devices for pH measurements [7], chemical species detection [1], biological species sensing [18], [19], [20] and for DNA hybridization detection [3], [21], [22]. However, despite the great potential of such nano-objects, no device based on unique NW has been transferred in all-day-life in the last decade. This is mainly due to the need to interface these nanomaterials with microscale and macroscale platforms. Devices based on a unique nanowire require that an individual nanowire be positioned at a precise location on a substrate [3]. This is time consuming and this requires a complex integration technology, which limits the large scale applications. That is why interest has recently grown on new architectures based on high aspect ratio nanostructure networks. The networks are fabricated by solution-based assembly of the NWs or NTs (for e.g. spray coating [23], [24], Langmuir–Blodgett [25], [26], [27], [28], [29] or vacuum filtration [30], [31]), which enables the fabrication of networks having a wide range of thickness, from sub-monolayer coverage to over 1 μm thick. In the recent years, such carbon NT networks have been studied and integrated into chemical and biological sensors that exhibit high sensitivity to gas or biological molecules [12], [13], [32]. However, to the best of our knowledge, no literature has been reported for SiNW networks for the biological sensing and DNA hybridization detection.
For biological applications, the silicon NWs are particularly attractive due to the fact that their surface is covered with a native oxide which can be easily functionalized for bio-applications [33], [34]. Moreover, with the help of Vapor-Liquid-Solid (VLS) growth of Si NWs, it is possible to precisely control both the dopant concentration and their aspect ratio [35]. Among the solution-based assembly methods for the network fabrication, the vacuum filtration method is highly simple, versatile [12], [30], [36], [37], [38], [39], [40], low cost, and scalable to large areas. The film homogeneity is guaranteed by the process itself. The NW or NT networks fabricated with this method can be easily deposited at room temperature onto various types of substrates: transparent or opaque, conductor or insulating, flexible or rigid.
In this article, we show the steps of the integration of random SiNW networks into DNA biosensors. We report for the first time the fabrication of random networks based on SiNWs: their morphology and the method used to get reproducible, homogeneous and well interconnected networks are presented. Then, we demonstrate the possibility to use such SiNW networks for the detection of DNA hybridization, opening the route to a new type of DNA sensors. Therefore, we report first the functionalization process used for the covalent DNA grafting on the SiNW networks. Second, thanks to the optical detection of DNA hybridization, we demonstrate the DNA immobilization onto the network surface and we evidence an enhanced sensitivity and good selectivity for this new sensor.
Section snippets
Synthesis of the silicon nanowires
In this study, silicon nanowires are grown on silicon 〈1 1 1〉 substrates by reduced pressure chemical vapor deposition (RP-CVD) using the Au catalyzed VLS mechanism [41]. The growth is performed in a CVD furnace Easy Tube™ 3000 from first nano at 650 °C under a pressure of 3 Torr. Silane, SiH4, is used as the silicon precursor with flow of 40 sccm. Hydrogen chloride, HCl, is also added during the growth in order to inhibit the gold diffusion and the lateral growth [42], [43]. Phosphine, PH3, is
Results and discussion
The aim of this work is to demonstrate that integrating SiNWs in a network structure is a possible way for the fabrication of a DNA biosensor device. First, it is necessary to demonstrate the possible elaboration of reproducible and controllable networks. Then, with the help of optical detection of DNA hybridization, the possibility to immobilize DNA onto the network surface is proved.
Conclusions
In this paper we have presented a simple, elegant, versatile and low cost process for creating random silicon nanowire networks. With the vacuum filtration method, adapted for the first time to SiNWs, we have shown the feasibility to achieve homogeneous and reproducible SiNW networks at room temperature. First, we have demonstrated that the network density is readily controlled by both the volume of the solution filtered and the nanowire concentration whose reproducibility is ensured by
Acknowledgements
The authors thank the members of the technical staff of the PTA facilities at Grenoble (France) for their technical support. This work was partly supported by the french RENATECH network. The authors acknowledge funding by the European network Nanofunction. We thank the anonymous referees for their stimulating comments.
Pauline Serre received her engineering diploma in Material science from Grenoble INP, France (2011) after studying one year at Imperial College in London in nanomaterial field. She is currently a Ph.D student at the microelectronics technology laboratory (LTM) in France. Her research interests are semiconducting sensors and characterizations for biological or chemical applications.
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Céline Ternon obtained her PhD at Caen University in 2002 (France). In 2003, she got an associate professor position at Grenoble-INP. Member of FMNT labs (Grenoble, France), she works in the field of nanomaterials and nanotechnologies. In the first years, she works on Si nanoparticles growth and characterization before moving toward Si nanowires study. A year spent as invited researcher at Polytechnique Montreal in 2006 shifts her interest toward the development of universal methods allowing the manipulation and integration of high aspect ratio nanomaterials in 3D architectures and devices.
Valérie Stambouli received her PhD in 1991 in Paris-Sud University (France). Then she moved to E.P.F.L. (Switzerland) where she was involved in physical and chemical characterizations to study the oxidization and tribological behavior of Fe based alloys. Since 1994, she is a full-time researcher of the Center National de la Recherche Scientifique (CNRS). She worked on the elaboration of metallic and dielectric films using P.V.D. techniques for microelectronics and microsystems. In 2002, she joined the LMGP in Grenoble where she initiated an interdisciplinary research program. She focuses on the elaboration and functionalization of thin metal oxide films for label-free biosensing.
Priyanka Periwal received her Masters degree in Nanotechnology from University of Delhi, India and University Joseph Fourier, France (2011) in a sandwich program. She is currently a PhD student at Grenoble University, France. Her current interests include growth and characterization of nanowires for electronic application.
Thierry Baron received his Ph.D. in physics at Grenoble University in 1996. His thesis focused on II–VI semiconductor for optoelectronic applications and his post-doc at the University of Wurzburg (Germany) was on the fabrication and characterization of II-VI LEDs. He joined the CNRS in 1998 to work on the technological platform of CEA-Leti in Grenoble. He developed the elaboration of silicon nanocrystals on insulating substrates, the study of their physical properties and their integration in memory devices. His current research focuses on the CVD growth and the integration of Si/Ge nanowires, and the epitaxy of III-V semiconductor on silicon.