CN106153597B - Dual wavelength multifunctional sensing element, preparation method and application based on antenna auxiliary - Google Patents
Dual wavelength multifunctional sensing element, preparation method and application based on antenna auxiliary Download PDFInfo
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- CN106153597B CN106153597B CN201510188504.5A CN201510188504A CN106153597B CN 106153597 B CN106153597 B CN 106153597B CN 201510188504 A CN201510188504 A CN 201510188504A CN 106153597 B CN106153597 B CN 106153597B
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Abstract
The invention discloses a kind of dual wavelength multifunctional sensing elements based on antenna auxiliary, preparation method and application.Sensing element includes substrate with metallic character, constructs the knot structure of identical material or different materials but same periodic arrangement with metallic character on it.Between adjacent golden collar's knot, micro-nano antenna is constructed, Raman reinforcing effect is further increased to increase the launching efficiency of sub- radiation mode to the capture ability of incident light using the raising of micro-nano antenna.By increasing Antenna Design, this dual wavelength integrated biosensor Raman enhancing enhances one times than the structure of antenna is not added；An order of magnitude is enhanced than single golden collar's junction structure.The present invention solves multiple problems of sensor field by a plasma resonance structure simultaneously.
Description
Technical field
The present invention relates to sensory field more particularly to a kind of dual wavelength multifunctional sensing elements based on antenna auxiliary, system
Preparation Method and application.
Background technique
Biosensor has extensive and important application in fields such as medicine detection, food safety, environmental monitorings.It is raw
Object sensor mainly realizes both sides function --- the examination of unknown molecular and the Concentration Testing of known molecular.Currently used for dividing
The major technique that son is screened is Raman spectral analysis technology.Raman spectrum analysis technology is based on Raman scattering effect, for incidence
The different scattering spectrum of light frequency is analyzed to obtain molecular vibration, rotation aspect information, and is applied to molecular structure and is studied
A kind of analysis method.Therefore different molecule has completely different Raman Scattering Spectra, and also therefore referred to as molecule " refers to
Line ".But the Raman scattering intensities of molecule are usually all very weak, so that directly measuring extremely difficult.On the other hand, for
One of the important means of detection of molecular concentration is to detect the ambient refractive index changed with molecular concentration.Therefore need find out for
The element of local refraction index changing sensitivity.In order to solve both of these problems, the micro-nano structure quilt based on surface plasma body resonant vibration
It has been widely applied in the design of biosensor.Surface plasma body resonant vibration is a kind of conduction electronics in dielectric constant phase
Collective oscillation behavior on anti-two media interface.Plasma resonance on metal micro-nanostructure surface has very strong office
Domain characteristic, because of referred to herein as local surface plasma resonance.This local surface plasma resonance can limit to electromagnetic field
Electric field near the surface of nanostructure, therefore near nanostructured surface is enhanced.The near field of enhancing can be used for increasing
(usual reinforcing effect can achieve 10 for strong Raman scattering6~1012), as Raman sensor.Meanwhile near metal Nano structure
Local fields it is natural for environment sensitive, can be used as index sensor.
Currently, the research of the biosensor based on local surface plasma resonance has had many reports.Wherein, base
In one of the research hotspot of index sensor of local surface plasma resonance be how improve sensor quality because
Son.The definition of quality factor is the ratio of sensitivity (wave length shift caused by unit variations in refractive index) and bandwidth of sensor.
It is not difficult to find out that optimizing two approach of quality factor to improve sensitivity and reducing bandwidth.Pass through the different metal of ingehious design
Nanostructure, quality factor be greatly improved (Lassister, J.B, et al, Nano Letter 10,3184,
2010; Chen, L., et al, Chin. Phys. B 23, 027303, 2014).Detection for Raman sensor
Precision (limit is single-molecule detection), then depend entirely on the field reinforcing effect of the plasma resonance micro-nano structure of design.It draws
The graceful product for enhancing the enhancing for being proportional to exciting light and Raman diffused light enhancing, therefore, for the micro-nano structure singly to resonate, due to
Bandwidth is limited, this reinforcing effect is only effective for shortwave number Raman signal, and long wave number Raman and hyper Raman are increased
Potent fruit can weaken significantly.Crozier et al. has been put forward for the first time the micro-nano structure of dual wavelength plasma resonance, and Raman is enhanced
It is extended to 2000cm-1(Mohamad, et al, ACS Nano 5, 307, 2010; Y.Chu, et al, ACS Nano
4, 2804, 2010)。
We are also it is proposed that adjustable dual wavelength plasma resonance micro-nano structure, further widens Raman enhancing wave number and arrive
3000cm-1(Jiao Lin, et al, Laser & Photon. Rev. 8,610,2014).This range is enough
Almost all of Raman scattering signal is covered, and theoretically there is no limit can continue to expand to long wave number Raman direction.It removes
Solve the problems, such as long wave number Raman and the enhancing of hyper Raman, this dual wavelength plasma resonance micro-nano structure can also
Solve the problems, such as that Raman sensing and refractive index sensing based on plasma resonance are incompatible simultaneously.In this dual wavelength structure
In, we used a sub- radiation modes to be integrated with the folding of high-quality-factor while so that realizing the enhancing of long wave number Raman
Penetrate rate sensing function function.Although the long wave number Raman enhancing of this structure very good solution and Raman sensing and refractive index are passed
The problem of sense integrates, but for realizing single-molecule detection, reinforcing effect still needs to be further increased.
In addition, there is " band when realizing Raman enhancing and two functions of refractive index sensing at the same time for single resonant structure
It is wide " contradiction --- i.e. Raman enhancing needs bandwidth is wide as far as possible can enhance exciting light simultaneously and scatter Raman signal, and based on etc.
The index sensor of ion resonance body then pursues narrower bandwidth, realizes higher quality factor.
Summary of the invention
The purpose of the present invention is in view of the deficiencies of the prior art, provided for molecular detection system a kind of based on antenna auxiliary
Dual wavelength multifunctional sensing element, preparation method and application.
Dual wavelength multifunctional sensing element proposed by the present invention based on antenna auxiliary, including with metallic character material
Substrate and the knot structure of the period with metallic character constructed on it arrangement, between adjacent knot, building is improved
The micro-nano antenna for capturing incident light ability reaches two by adjusting knot, the size of antenna and the period of knot, antenna element
Kind plasma resonance mode, i.e., the mode of resonance that a kind of electric dipole in the structural plane of the knot combines are another
Kind is then the sub- radiative collision dipole photon mode being present between knot and substrate, adjusts both plasma resonance moulds
Formula, so that resonance wavelength and Raman excitation and Raman scattering is Wavelength matched.
Described to adjust knot, antenna size and the period of arrangement specific as follows: passing through setting knot triangular apex
To the height on bottom edge, the position for adjusting the first formant is matched with exciting light length；Thickness by the way that knot is arranged adjusts the second resonance
The position at peak and the Raman signal of detection are Wavelength matched；By the way that knot arrangement period is arranged, the electric field of the first formant is adjusted, is led to
The frequency for crossing the width adjusting resonance of setting micro-nano antenna, reaches two kinds of plasma resonance moulds by above-mentioned parameter setting
Formula.
Described there is metallic character material requirements negative permittivity, including metal material to be presented in required frequency range
The dielectric material of material and metallic character, the metal material include but is not limited to gold, silver, copper, aluminium, the metallic character
Dielectric material includes the carbofrax material in middle infrared band.
The knot uses identical material or different materials.
Further enhancing of the present invention suitable for long wave number Raman and hyper Raman.
Nano-antenna in the sensing element is identical as the thickness of knot.
A kind of preparation method of the sensing element: 0.2um metallic character material is sputtered in any planar substrates and is made
For substrate, the spin coating 0.18um positive photoresist PMMA950K in metallic character material substrate, the thickness of photoresist and substrate
Thickness exposes knot-micro-nano antenna structure in 3:1, with electron beam lithography on a photoresist, and after development, exposed portion is washed
Fall, leave knot-micro-nano antenna pit, the metallic character material of directionality vapor deposition 0.055um, will remain in these pits
Glue wash, then leave knot-micro-nano antenna period arrangement on substrate.
Sensing element of the invention can be applied to bio-sensing.
A kind of sensor using the sensing element.
The beneficial effect comprise that
(1) present invention enhances Raman enhancing than single golden collar's structure in metal substrate by periodical knot structure
An order of magnitude.
(2) it is periodically designed by nano-antenna and knot, Raman enhancing is doubled, and enhances the capture to incident light
Ability substantially increases Raman reinforcing effect to improve the launching efficiency of sub- radiation mode.Meanwhile increasing gold bar structure
Do not increase process complexity, can be prepared by electron beam lithography, also can use nanometer embossing and realize big face
The processing of droning of product.
(3) present invention can be long wave number Raman (3000cm-1) and hyper Raman offer 108Above electric field increases
By force, the refractive index sensing based on local plasmon resonance body that quality factor reaches 25.8 is realized.
(4) spectral response of structure of the invention at most can provide three enhancing peaks, and the resonance wavelength at three peaks is adjusted
The position for matching excitation, stokes and anti-stokes respectively, can enhance stokes and anti-stokes signal simultaneously.
(5) present invention solves three problems of sensor field simultaneously: first is that passing through dual wavelength plasma resonance knot
Structure solves the problems, such as the enhancing of long wave number and hyper Raman；Second is that by introducing a sub- radiation mode for high-quality-factor
Refractive index sensing element is integrated into Raman sensor, realizes multifunctional bio sensing, and convenient biological detection is also dropped significantly
Low cost；Third is that Raman reinforcing effect is further improved by the introducing of nano-antenna, to realize that single-molecule detection provides
Possibility.
To sum up, structure of the invention design is very flexible, being total to flexible modulation dual wavelength by changing structural parameters
The position at vibration peak, to be suitable for the different Raman scattering signal of different excitaton source and detection.
Detailed description of the invention
The structural schematic diagram of the one embodiment for the dual wavelength multifunctional sensing element that Fig. 1 is assisted based on antenna, the right side are three
It ties up structural schematic diagram (Unit 5 × 3), upper left lower-left is respectively that side view and top view (in order to compare conveniently, are placed on a figure
In)；Substrate material is gold, constructs golden collar's knot-gold bar composition periodic array of identical material in substrate, gold bar is (micro-
Receive antenna) between adjacent golden collar knot, direction is perpendicular to knot long axis direction.
Fig. 2 is an electric-field enhancing of the dual wavelength multifunctional sensing element based on antenna auxiliary that numerical simulation obtains
Spectrum.The spectrometry be knot upper surface center electric-field enhancing.Two dotted lines respectively indicate excitation and Raman signal
Position.
Fig. 3 is the curve of the drift of two resonant positions shown in Fig. 2 under conditions of ambient refractive index changes.
Specific embodiment
Present invention will be further explained below with reference to the attached drawings and examples.
As shown in Figure 1, the dual wavelength multifunctional sensing element based on antenna auxiliary includes golden substrate and structure on it
Golden collar's knot-gold bar the structure for the period arrangement built, gold bar, that is, micro-nano antenna.Gold bar is between adjacent golden collar's junction structure, direction
Perpendicular to the long axis direction of golden collar's knot.
Based on the dual wavelength multifunctional sensing element of antenna auxiliary, including substrate with metallic character, construct on it
The knot structure of identical material or different materials but same periodic arrangement with metallic character.It is tied in adjacent golden collar
Between, micro-nano antenna is constructed, improves the capture ability to incident light using micro-nano antenna, to increase the excitation effect of sub- radiation mode
Rate further increases Raman reinforcing effect.
Further, the material requirements with metallic character is that negative dielectric is presented in the frequency range of research is normal
Number, therefore either gold, silver, copper, aluminium, are also possible to dielectric material with metallic character, such as in middle infrared band
Carbofrax material.
Still further, Raman enhancing enhances one than single golden collar's junction structure in metal substrate by optimizing cycle
A order of magnitude；By optimizing Antenna Design, Raman enhancing is doubled.
Further, the dual wavelength multifunctional sensing element based on antenna auxiliary, can be long wave number Raman
(3000cm-1) and hyper Raman offer 108Above electric-field enhancing.This high-performance dual wavelength multifunctional sensing element branch
Hold two kinds of plasma resonance modes.One is the modes of resonance that the electric dipole in knot structural plane combines；It is another then
It is the sub- radiative collision dipole photon mode being present between knot and substrate.Both plasma resonance modes can be free
It adjusts, so that resonance wavelength and Raman excitation and Raman scattering is Wavelength matched, for long wave number Raman and hyper Raman
Enhance extremely advantageous.
For a kind of above-mentioned sub- radiative collision dipole photon mode, spectral band width.Therefore quality factor is high, is fine
Refractive index sensing element.Realize the refractive index sensing based on local plasmon resonance body that quality factor reaches 25.8.
It is integrated with the function of refractive index sensing on the basis of Raman enhances and senses, realizes multifunctional sensing.
Embodiment 1
A specific embodiment of the invention is given below.The golden substrate of setting is sufficiently thick, and no light can penetrate；It is tied along golden collar
Long axis, short-axis direction period be respectively 0.6um and 0.4um；Golden collar's knot and gold bar are contour, are 0.055nm；Gold bar width is
0.1um；A height of 0.14um of two isosceles triangles of golden collar's knot is formed, apex angle is 50 °, and the gap between apex angle is
0.01um.The present embodiment design is directed to 0.633um laser excitation, detection 0.78um(3000cm-1) neighbouring Raman dissipates
Penetrate signal.Adjust height of a pair of of the isosceles Golden Triangle shape vertex of composition golden collar's knot to bottom edge, the position of adjustable first formant
It sets, is allowed to match with excitation wavelength.The position for adjusting adjustable second formant of height of golden collar's knot, is allowed to and needs to visit
The Raman signal of survey it is Wavelength matched.Fig. 2 gives the electricity that the golden collar that numerical simulation is calculated ties centre of surface point position
Field enhancing.Regulating cycle, so that the electric-field enhancing of the first formant is most strong, the frequency for adjusting its resonance that the width of gold bar makes is connect
Nearly Asia radiation mode, to greatly improve the electric filed enhanced effect of sub- radiation mode.Raman enhancing approximation can be reached with following table
Formula obtains:
Wherein EF represents independent variable as the function of the electric-field enhancing of wavelength.Golden collar, which is obtained, according to this expression formula ties surface
The Raman enhancing of central point is approximately 108。
The drift of the corresponding two resonance peak frequencies of Fig. 2 when Fig. 3 gives ambient refractive index and changes is obtained,
It is respectively 23.1 and 25.8 that the first formant and the corresponding quality factor of the second formant, which can therefrom be calculated,.
Embodiment 2
Following steps preparation can be used in dual wavelength multifunctional sensing element based on antenna auxiliary of the invention: arbitrarily flat
0.2um gold is sputtered in the substrate of face as substrate, which is enough to prevent light from penetrating.The spin coating 0.18um positive-tone photo on golden substrate
Glue PMMA950K, the thickness of photoresist and the thickness of building material guarantee subsequent stripping technology feasibility about in 3:1.Electricity consumption
Beamlet exposure technique exposes knot-elongate configuration on a photoresist.After development, exposed portion is washed off, and leaves knot-strip
Pit, the gold of directionality vapor deposition 0.055um in these pits.Remaining glue is washed, then leaves golden collar's knot-on substrate
Gold bar period arrangement.
By designing different structure, two peak structure of the invention can be adapted for different excitation and scattering Raman signal.
Meanwhile the size of golden collar's knot is carefully selected, it at most can provide three enhancing peaks, while enhancing stokes and anti-stokes letter
Number.
Claims (8)
1. a kind of dual wavelength multifunctional sensing element based on antenna auxiliary, it is characterised in that: including with metallic character material
Substrate and construct on it period with metallic character arrangement knot structure, between adjacent knot, building is mentioned
The micro-nano antenna of height capture incident light ability, is reached by adjusting knot, the size of antenna and the period of knot, antenna element
Two kinds of plasma resonance mode electric field enhancings, i.e., the resonance that a kind of electric dipole in the structural plane of the knot combines
Mode, it is another then be the sub- radiative collision dipole photon mode being present between knot and substrate, adjust both plasmas
Resonance body mode, so that resonance wavelength and Raman excitation and Raman scattering is Wavelength matched；The ruler for adjusting knot, antenna
Very little and knot, the period of antenna element are specific as follows: by the height of setting knot triangular apex to bottom edge, it is total to adjust first
The position at vibration peak is matched with exciting light length；Thickness by the way that knot is arranged adjusts the position of the second formant and the Raman of detection is believed
It is number Wavelength matched；By the way that knot arrangement period is arranged, the electric field strength of the first formant is adjusted, by the width that micro-nano antenna is arranged
Degree adjusts the frequency of resonance, adjusts the electric field strength of the second formant, reaches two kinds of plasmas by above-mentioned parameter setting
The most strong enhancement mode of resonance electric field.
2. sensing element as described in claim 1, which is characterized in that described has metallic character material requirements required
Negative permittivity, the dielectric material including metal material and metallic character are presented in frequency range, the metal material includes
But it is not limited to gold, silver, copper or aluminium, the dielectric material of the metallic character includes the carbofrax material in middle infrared band.
3. sensing element as described in claim 1, it is characterised in that: the knot uses identical material or different materials.
4. sensing element as described in claim 1, it is characterised in that: the increasing suitable for long wave number Raman and hyper Raman
By force.
5. sensing element as described in claim 1, it is characterised in that: micro-nano antenna and knot in the sensing element
Thickness is identical, perpendicular to the long axis direction of knot.
6. a kind of preparation method of sensing element as described in claim 1, it is characterised in that be carried out as follows: in office
Sputtering 0.2um metallic character material is as substrate in planar substrates of anticipating, the spin coating 0.18um positivity in metallic character material substrate
Photoresist PMMA950K, the thickness of photoresist and the thickness of substrate expose neck with electron beam lithography in 3:1 on a photoresist
Knot-micro-nano antenna structure, after development, exposed portion is washed off, and leaves knot-micro-nano antenna pit, the side in these pits
The metallic character material of 0.055um is deposited in tropism, and remaining glue is washed, then leaves knot-micro-nano antenna week on substrate
Phase arrangement.
7. a kind of application of sensing element as described in claim 1, which is characterized in that be applied to bio-sensing.
8. a kind of sensor using sensing element as described in claim 1.
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