CN103785492A - Surface enhanced Raman scattering microfluidic system based on PDMS three-dimensional micro-nano antenna - Google Patents
Surface enhanced Raman scattering microfluidic system based on PDMS three-dimensional micro-nano antenna Download PDFInfo
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Abstract
The invention provides a surface enhanced Raman scattering microfluidic system based on PDMS three-dimensional micro-nano antenna, which is used for molecular detection. A PDMS micro-nano antenna structure is adopted as a silver nanoparticle carrier, a layer of graphene covers the silver nanoparticle carrier so as to form a PDMS/silver nanoparticle/graphene-based Raman scattering base with the three-dimensional micro-nano antenna structure, which is taken as a detection area; a laser light source and a spectrograph are connected with an optical fiber and an SERS (Surface-Enhanced Raman Scattering) probe, and irradiate the detection area of a microchannel; the microchannel adopts PDMS materials. According to the system, graphene protects the oxidization of silver nanoparticles on one hand, and brings high chemical reinforcement on the other hand; the PDMS three-dimensional micro-nano antenna structure has a large specific surface area and more Raman enhanced hot points, effectively reinforces the filling effect of the silver nanoparticles, and is beneficial to localized surface plasmon resonance, and the strength of Raman scattering signals is enhanced; according to the system, the PDMS materials and the optical fiber are coupled, the manufacturing process is simple, the cost is low, and portable and on-line detection of molecules can be realized conveniently.
Description
Technical field
The invention belongs to nanophotonics and micro-fluidic field, be specifically related to Surface Enhanced Raman Scattering Spectrum technology.
Background technology
Along with human social development, the disease of manward's health, food pollution, environmental toxin, drugs, and the explosive trace Molecular Detection demand of the national security such as military and national defense is growing, becomes the research topic of chemistry, physics, life science and nanosecond science and technology field rapid growth.Molecule absorbs under different condition or the spectral wavelength launched, intensity, polarization state etc. have intrinsic relation with the architectural feature of this molecule, and therefore, spectrographic technique is considered to survey and the powerful of research trace molecule.Wherein, Raman spectrum is that a kind of photon incides the inelastic collision occurring on molecule, and its frequency shift amount is corresponding with molecule intrinsic vibration energy level, can realize " fingerprint " identification to point subsample, has very high detection accuracy.But common raman scattering cross section is compared very little with fluorescent scattering cross section, make faint Raman signal be submerged in strong fluorescence signal the inside, sensitivity is low, is difficult to realize trace molecular detection.In recent years, the SERS that develops rapidly (surface-enhanced Raman scattering is called for short SERS) spectrum has overcome that the Raman signal that traditional Raman spectrum exists is faint, detection sensitivity is low, be subject to the shortcoming that fluorescence disturbs; Have and do not need the advantage such as pretreatment, non-intruding non-destructive.Become gradually survey trace even unimolecule characteristic, characterize molecular structure effective test analysis instrument, in life science, food security, environmental monitoring, military science etc. and national security and the closely bound up field of people's health, have a wide range of applications.In the gold and silver particle of visible waveband, the SERS Electromagnetic enhancement factor reaches 10
14-10
15magnitude, compares with traditional Raman spectroscopy, and signal increases substantially.
The plurality of advantages of aforementioned SERS technology makes it can be used as the identification probe of molecule, for trace Molecular Detection.Mainly contain 3 kinds of typical way based on SERS molecular detection system at present: the one, metal nanoparticle is injected to photonic crystal fiber, carry out SERS acquisition of signal; The 2nd, adopt the active modes such as extra electric field/magnetic field that metal nanoparticle is adsorbed in microchannel, form SERS microfluidic system; The 3rd, the microchannel mode of employing nanometer bridge joint, adopts passive mode to form SERS microfluidic system.But these SERS systems are used more Nano silver grain, easily oxidation by air; Mostly adopt two-dimentional SERS substrate to be combined with microflow control technique, " focus " strengthening for Raman is limited; How designing, to use more complicated based on laboratory main equipment, when a point subsample is detected, real-time online and convenience are bad.
Summary of the invention
The present invention, in order to solve the shortcoming of the easy oxidation by air of Nano silver grain, proposes to adopt the mode of Graphene, protects on the one hand easily oxidized Nano silver grain, and the chemistry that is expected to obtain on the one hand strengthens; Meanwhile, large, expensive in order to solve SERS detection system volume, be unfavorable for the online shortcoming detecting, the SERS microfluidic system based on coupling fiber is proposed; And, " focus " the limited shortcoming strengthening for Raman for two-dimentional SERS substrate, the three-D micro-nano antenna structure of proposition based on PDMS/ Nano silver grain/Graphene is as Raman scattering substrate.
The present invention realizes by the following technical solutions:
The present invention is a kind of SERS microfluidic system of the three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene, and described microfluidic system comprises Raman scattering substrate, lasing light emitter, spectrometer, optical fiber and the SERS optical fiber probe of microchannel substrate, microchannel, three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene.Described microchannel substrate is glass plate, as microchannel (adopt PDMS(dimethyl silicone polymer (Polydimethylsiloxane))) supporting body, microchannel adopts PDMS material, closed at both ends, and be respectively equipped with testing molecule incident aperture and testing molecule outgoing aperture at adjacent blind end upside, in microchannel, be provided with the Raman scattering substrate of the three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene as detecting area.
Particularly, the Raman scattering substrate of the described three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene comprises PDMS three-D micro-nano antenna structure, nano grain of silver sublayer and graphene layer; Described nano grain of silver sublayer is to utilize sputter and vacuum annealing method to be modified at PDMS three-D micro-nano antenna structure surface, and described graphene layer is to be attached to nano grain of silver sub-surface by transfer.
Working method: testing molecule is entered by incident aperture, flows through the three-dimensional Raman scattering substrate of detecting area, and testing molecule is adsorbed onto on three-dimensional Raman scattering substrate; Exciting light source is by optical fiber, SERS probe, and irradiating absorption has the three-dimensional Raman scattering substrate of testing molecule, and the scattered signal of testing molecule exports to spectrometer by SERS probe, optical fiber, completes testing molecule Raman signal detection.Can filling liquid molecule in microchannel, also can injecting gas molecule, carry out liquid, gas molecule detects.
Remarkable advantage of the present invention is:
1, adopt Graphene to be combined with nano grain of silver sublayer, protected on the one hand the oxidation of Nano silver grain, can bring on the other hand higher chemistry to strengthen;
2, adopt PDMS three-D micro-nano antenna structure, specific area is large, effectively increase the filling effect of Nano silver grain, there is more Raman and strengthen " focus ", be conducive to local surface plasma resonance effect, Raman scattering signal strength signal intensity increases, and has overcome micro-fluidic two-dimentional SERS substrate Raman enhancing " focus " the few shortcomings that adopt of existing SERS more;
3, microchannel and three-D micro-nano antenna structure all adopt PDMS material, and coupling fiber, and the simple cost of manufacture craft is low, are compared to the shortcoming that existing SERS needs large-scale experiment chamber equipment, are convenient to realize portable, the detection online of molecule.
Visible the present invention theoretically, realize and in feasibility, all the application of effects on surface raman scattering spectrum provided to a kind of portable online test method.
Accompanying drawing explanation
Fig. 1 is the structural representation of the SERS microfluidic system of the three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene of the present invention;
Fig. 2 is the structural representation of the three-D micro-nano antenna structure Raman scattering substrate based on PDMS/ Nano silver grain/Graphene of the present invention;
Fig. 3 is the preparation flow schematic diagram of the three-D micro-nano antenna structure Raman scattering substrate based on PDMS/ Nano silver grain/Graphene of the present invention;
Fig. 4 (a) and Fig. 4 (b) are the schematic diagrames of microchannel of the present invention.
In figure: 1. testing molecule incident aperture, 2. microchannel, the 3. three-D micro-nano antenna structure surface enhanced Raman scattering substrate (as detecting area) based on PDMS/ Nano silver grain/Graphene, 3-1.PDMS three-D micro-nano antenna structure, 3-2. nano grain of silver sublayer, 3-3. graphene layer, 4. testing molecule outgoing aperture, 5. exciting light source, 6. Raman spectrometer, 7. optical fiber, 8.SERS optical fiber probe, 9. microchannel substrate.
The specific embodiment
Below in conjunction with embodiment and accompanying drawing, the present invention is described in further detail, but embodiments of the present invention are not limited to this.
Referring to Fig. 1, the SERS microfluidic system of the three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene the present invention relates to comprises: Raman scattering substrate 3, exciting light source 5, spectrometer 6, optical fiber 7 and the SERS optical fiber probe 8 of microchannel substrate 9, three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene.
Referring to Fig. 4 (a) and Fig. 4 (b), microchannel substrate 9 adopts glass plate, and microchannel 2 arranges thereon, and microchannel is adopt soft lithographic method to make and obtain materials'use PDMS.The closed at both ends of microchannel 2, and adjacent blind end upside is processed with respectively testing molecule incident aperture 1 and testing molecule outgoing aperture 4, the Raman scattering substrate 3 of the three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene is bonded in microchannel 2, as detecting area.Exciting light source 5 is connected SERS optical fiber probe 8 by optical fiber 7 respectively with spectrometer 6, and SERS optical fiber probe is positioned at detecting area top.Time prepared by microchannel: first prepare microchannel base section, be detecting area part based on PDMS/ Nano silver grain/Graphene ground three-D micro-nano antenna structure, prepare again microchannel sidewall and upside with entrance and exit part, then these two parts are bonded on glass substrate.
Referring to Fig. 2, three-D micro-nano antenna structure surface enhanced Raman scattering substrate based on PDMS/ Nano silver grain/Graphene of the present invention comprises: PDMS three-D micro-nano antenna structure 3-1, nano grain of silver sublayer 3-2, graphene layer 3-3, its preparation method is referring to Fig. 3: first adopt nano-imprinting method to prepare PDMS three-D micro-nano antenna structure; Recycling sputter and vacuum annealing method are being modified at Nano silver grain on PDMS three-D micro-nano antenna structure surface; Again Graphene is transferred on Nano silver grain, thereby formed the three-D micro-nano antenna structure surface enhanced Raman scattering substrate based on PDMS/ Nano silver grain/Graphene.
When Molecular Detection, testing molecule enters microchannel 2 by testing molecule incident aperture 1, flow through the three-D micro-nano antenna structure surface enhanced Raman scattering substrate 3 based on PDMS/ Nano silver grain/Graphene of search coverage, testing molecule is adsorbed on three-dimensional Raman scattering substrate 3, exciting light source 5 incides search coverage by optical fiber 7 and SERS optical fiber probe 8, due to the surface plasma resonance characteristic of Nano silver grain 3-2, the Raman scattering signal of testing molecule exports to spectrometer 6 by SERS optical fiber probe 8 and optical fiber 7, testing molecule in passage is after three-dimensional surface strengthens Raman scattering substrate 3, flowed out by testing molecule outgoing aperture 4, complete Molecular Detection.
The present invention is not limited to above-mentioned embodiment, if the various changes to invention or distortion do not depart from the spirit and scope of the present invention, if within these changes and distortion belong to claim of the present invention and equivalent technologies scope, the present invention is also intended to comprise these changes and distortion.
Claims (2)
1. the SERS microfluidic system based on PDMS three-D micro-nano antenna, is characterized in that: described microfluidic system comprises Raman scattering substrate, lasing light emitter, spectrometer, optical fiber and the SERS optical fiber probe of microchannel substrate, microchannel, three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene; Described microchannel is positioned on the substrate of microchannel, microchannel adopts PDMS material, its closed at both ends, and adjacent blind end upside is established respectively testing molecule incident aperture and testing molecule outgoing aperture, the Raman scattering substrate of the three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene is arranged in microchannel, and as detecting area, described lasing light emitter is connected SERS probe by optical fiber respectively with spectrometer, SERS probe is positioned at detecting area top, and is irradiated to the detecting area of microchannel;
The Raman scattering substrate of the described three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene comprises PDMS three-D micro-nano antenna structure, nano grain of silver sublayer and graphene layer; Described nano grain of silver sublayer is to utilize sputter and vacuum annealing method to be modified at PDMS three-D micro-nano antenna structure surface, and described graphene layer is to be attached to nano grain of silver sub-surface by transfer;
Testing molecule is entered by incident aperture, flow through the Raman scattering substrate of detecting area, testing molecule is adsorbed onto on Raman scattering substrate, exciting light source is by optical fiber, SERS probe, irradiate the Raman scattering substrate that absorption has testing molecule, the scattered signal of testing molecule exports to spectrometer by SERS probe, optical fiber, completes testing molecule Raman signal detection.
2. the SERS microfluidic system based on PDMS three-D micro-nano antenna according to claim 1, is characterized in that: the preparation method of the three-D micro-nano antenna structure based on PDMS/ Nano silver grain/Graphene is first to adopt nano-imprinting method to prepare PDMS three-D micro-nano antenna structure; Recycling sputter and vacuum annealing method are being modified at Nano silver grain on PDMS three-D micro-nano antenna structure surface; Again Graphene is transferred on Nano silver grain, thereby formed the three-D micro-nano antenna structure surface enhanced Raman scattering substrate based on PDMS/ Nano silver grain/Graphene.
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