CN106596449A - Intermediate infrared graphene plasmon polariton biochemical sensor - Google Patents
Intermediate infrared graphene plasmon polariton biochemical sensor Download PDFInfo
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- CN106596449A CN106596449A CN201611102441.8A CN201611102441A CN106596449A CN 106596449 A CN106596449 A CN 106596449A CN 201611102441 A CN201611102441 A CN 201611102441A CN 106596449 A CN106596449 A CN 106596449A
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Classifications
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
- G01N21/17—Systems in which incident light is modified in accordance with the properties of the material investigated
- G01N21/25—Colour; Spectral properties, i.e. comparison of effect of material on the light at two or more different wavelengths or wavelength bands
- G01N21/31—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry
- G01N21/35—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry using infrared light
-
- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
- G01N21/17—Systems in which incident light is modified in accordance with the properties of the material investigated
- G01N21/41—Refractivity; Phase-affecting properties, e.g. optical path length
Abstract
The invention discloses an intermediate infrared graphene plasmon polariton biochemical sensor. The intermediate infrared graphene plasmon polariton biochemical sensor comprises an intermediate infrared broad band optical source, a first intermediate infrared lens, a graphene plasmon polariton sensing unit and a second intermediate infrared lens; the graphene plasmon polariton sensing unit comprises a doped silicon substrate, a first grating coupling area, a second grating coupling area, a sensing area, and a graphene layer, wherein the graphene layer covers the first grating coupling area, the second grating coupling area and the sensing area; an intermediate infrared light wave emitted by the broad band optical source is focused in the first grating coupling area through the first intermediate infrared lens so as to be coupled with a graphene plasmon polariton, the produced intermediate infrared graphene plasmon polariton reaches the sensing area through the graphene layer, repeatedly reacts with a biological sample in the sensing area, reaches the second grating coupling area through the graphene layer, is scattered to the far field, and is focused to a fourier infrared spectrometer through the second intermediate infrared lens to implement spectral measurement and analysis. The intermediate infrared graphene plasmon polariton repeatedly reacts with the biological sample in the sensing area, and the detection sensitivity of biomolecules is improved.
Description
Technical field
The present invention relates to optical sensing field, and in particular to a kind of mid-infrared Graphene plasmon biochemical sensor.
Background technology
By special applications on biochemical sensitive, this wave band covers the vibrational energy of molecule to middle-infrared band (3-30 microns)
Level, can be used to the biochemical basic structural unit of identification and analysis life, such as protein, fat, DNA.Mid infrared absorption spectrum
Technology can be absorbed by the fingerprint of molecular resonance, non-intrusion type, the unmarked Biochemical Information for obtaining material.Yet with life
The size (typically smaller than 10 nanometers) and the mismatch of middle infrared wavelength of chemoattractant molecule, the absorption of vibrations that result in molecule is very micro-
Weak, this is very unfavorable for the detection of nanoscale molecule, and in order to overcome weak restriction, locally resonant metal Nano structure are absorbed
Molecular detection is applied to, strengthens molecular detection sensitivity.Although metal nano resonance can strengthen nanoscale molecular detection
Sensitivity, but because metal is in the similar electronics perfection conductor of middle-infrared band, the electron interaction in photon and metal is very
Weak, metal nano resonance technique is still limited by relatively weak optical enhancement and non-tunable narrow-band spectrum.
Graphene is the carbon atom according to cellular two-dimensional arrangements, and because of its remarkable electrical and optical performance, it is described as photon
Learn and the revolutionary material of optoelectronics.Graphene plasmon (graphene plasmons) is photon-driven Graphene
Collective's concussion of middle electronics, is a kind of electromagnetic wave, and compared with the plasmon of traditional metal structure, Graphene plasma swashs
There are three aspect characteristic advantages in unit：
(1) carrier concentration of doped graphene can realize big model at a high speed by the bias of field effect transistor (FET) very little
The modulation enclosed, switch time was shorter than for 1 nanosecond, and this is very crucial for the opto-electronic device for realizing high speed；
(2) the little 1-3 magnitude of wavelength ratio free space optical wavelength of Graphene plasmon, this means that Graphene
Plasmon has very strong restriction effect to mid-infrared light field, can greatly strengthen the interaction of light and material；
(3) Graphene plasmon is recovery time longer, compared with metal plasma excimer, Graphene plasmon
Distance relatively far away from can be transmitted.
In sum, we can replace metal plasma excimer with Graphene plasmon, using middle infrared absorption
Spectral technique and Graphene plasmon characteristic superiority, strengthen the absorption of vibrations to nanoscale biomolecule, so as to realize
The high-acruracy survey that super-small chip absorbs to the refractive index and vibration fingerprint of different classes of biomolecule.
The content of the invention
The technical problem to be solved is special using mid infrared absorption spectrum technology and Graphene plasmon
Advantage is levied, strengthens the absorption of vibrations to nanoscale biomolecule, so as to realize super-small chip to different classes of biological point
The problem of the high-acruracy survey that the refractive index and vibration fingerprint of son absorbs.
In order to solve above-mentioned technical problem, the technical solution adopted in the present invention be to provide a kind of mid-infrared Graphene etc. from
Sub- excimer biochemical sensor, including wide spectrum light source, the first mid-infrared lens, the Graphene plasmon sensing unit of mid-infrared
With the second mid-infrared lens；
The Graphene plasmon sensing unit includes doped silicon substrate, is laid in the doped silicon substrate two respectively
The first grating coupled zone and the second grating coupled zone at end, the sensing unit being laid in the middle of the doped silicon substrate, and cover
Graphene layer above the first grating coupled zone, sensing unit and the second grating coupled zone；
The mid-infrared light wave that the mid-infrared wide spectrum light source sends is by first mid-infrared lens focuss described
One grating coupled zone, couples with Graphene plasmon, produces mid-infrared Graphene plasmon；The mid-infrared graphite
Alkene plasmon reaches the sensing unit by the graphene layer, with the biological sample being placed on the sensing unit repeatedly
Reaction；Again the second grating coupled zone is reached via the graphene layer, and scatter to far field；It is saturating by second mid-infrared
Mirror is focused on and carry out in infrared spectrometer spectral measurement analysis.
In such scheme, screen periods length Λ of the first grating coupled zone and the second grating coupled zone is：
Λ=λ0/neff；
Wherein, λ0It is free space mid-infrared light wavelength；neffIt is effective refraction of mid-infrared Graphene plasmon
Rate.
In such scheme, the sensing unit is optical microcavity structure, is served as a contrast including the doped silicon is laid in laterally side by side
Two identical Bragg reflectors on bottom；
Each described Bragg reflector includes M air ducting layer and doped silicon ducting layer, and by first air ducting layer
Afterwards the order of doped silicon ducting layer is transversely alternately arranged, 8 >=M >=4；
By an air grooves connection in the middle of two Bragg reflectors, one optical resonator of formation, two
The Bragg reflector makes mid-infrared Graphene plasmon height local in the air grooves, described with being filled in
The biological sample of air grooves repeated reaction.
In such scheme, the grating of the first grating coupled zone and the second grating coupled zone is by the doping
Etch linear groove on silicon substrate to realize；
The air ducting layer and the air grooves of the Bragg reflector is by the doped silicon substrate
Linear pair of Prague emitting structural groove of etching is realized.
In such scheme, lateral length d1 and the doped silicon ducting layer of the air ducting layer of the Bragg reflector
Lateral length d2 is determined that physical relationship is by Bragg condition：
d1×Real(neff1)+d2×Real(neff2)=m λb/2；
Wherein, λbIt is the centre wavelength in Prague；M is the exponent number in Prague；Real(neff1) for mid-infrared Graphene etc. from
Effective refractive index of the sub- excimer in air ducting layer；Real(neff2) for mid-infrared Graphene plasmon in doped silicon waveguide
The effective refractive index of layer.
In such scheme, the lateral length L for connecting the air grooves of two Bragg reflectors is：
L=Λ r/ [neff·2]；
Wherein, Λ r are resonant wavelength；neffIt is the effective refractive index of resonant wavelength waveguide.
In such scheme, the Graphene plasmon sensing unit also includes dielectric layer, and the dielectric layer is arranged
Between the graphene layer and the doped silicon substrate, field-effect tube structure is formed；
The graphene layer is provided with metal electrode, the metal electrode ground connection；
When the doped silicon substrate connects electricity, field-effect tube structure conducting, is the graphene layer applied voltage；
Regulation is applied to the size of voltage on the graphene layer, adjusts the fermi level size of Graphene, Graphene
Fermi level size changes resonance spectrum and is moved.
In such scheme, the dielectric layer is Al2O3。
The present invention utilizes mid-infrared Graphene plasmon the characteristics of optical resonator and biological specimen react repeatedly,
Strengthen absorption of vibrations to nanoscale biomolecule, realize super-small chip to the refractive index of different classes of biomolecule and
High-acruracy survey while vibration fingerprint absorbs, improves the sensitivity of biomolecule detection and the integrated level of sensor.
Description of the drawings
A kind of structural representation of mid-infrared Graphene plasmon biochemical sensor that Fig. 1 is provided for the present invention；
Fig. 2 is the structural representation of Graphene plasmon sensing unit in the present invention；
Fig. 3 is illustrated for the spectrum test result obtained using the mid-infrared plasmon biochemical sensor for providing of the invention
Figure.
Specific embodiment
The present invention utilizes the superpower light field containment of Graphene plasmon and tunable characteristic, in highly integrated core
Complex refractivity index and spectrum to the micro biochemical material such as protein high precision test simultaneously is realized on piece.
The present invention is described in detail with reference to Figure of description and specific embodiment.
As shown in figure 1, a kind of mid-infrared Graphene plasmon biochemical sensor that the present invention is provided, including mid-infrared
The mid-infrared lens 20 of wide spectrum light source (globar) 10, first, Graphene plasmon sensing unit 30 and the second mid-infrared
Lens 40；Graphene plasmon sensing unit 30 includes doped silicon substrate 35, is laid in the two ends of doped silicon substrate 35 respectively
The first grating coupled zone 31 and the second grating coupled zone 34, the sensing unit 33 that is laid in the middle of doped silicon substrate 35, and cover
The graphene layer 32 in the first grating coupled zone 31, the top of 33 and second grating coupled zone of sensing unit 34 is covered, in the present invention, the
First, the second grating coupled zone is made up of diffraction grating；
The free space mid-infrared light wave that mid-infrared wide spectrum light source 10 sends focuses on stone by the first mid-infrared lens 20
On first grating coupled zone 31 of black alkene plasmon sensing unit 30, couple with Graphene plasmon, it is red in generation
Outer Graphene plasmon；Mid-infrared Graphene plasmon reaches sensing unit 33 by waveguide media graphene layer 32,
After reacting repeatedly with the biological sample (such as protein) being placed on sensing unit 33, via graphene layer 32 the second grating is reached
Coupled zone 34, and scatter to far field；Focus on Fourier transform infrared spectrometer 50 (FTIR) by the second mid-infrared lens 40 again
In carry out spectral measurement analysis.
Because the transmission wave vector of mid-infrared Graphene plasmon is measured than big 1-2 of free space mid-infrared light wave
, there is great wave vector between them and mismatch in level, it is impossible to directly by free space mid-infrared light wave be coupled to Graphene etc. from
Sub- excimer, conversion generates mid-infrared Graphene plasmon, therefore, the present invention adopts grating (first, second light of sub-wavelength
The grating of grid coupled zone) compensating the mismatch of wave vector.Screen periods length Λ of first, second grating coupled zone of the invention
For：
Λ=λ0/neff；
Wherein, λ0It is free space mid-infrared light wavelength, in the present invention, we use wideband light source, λ0Take wherein
Cardiac wave is long, still can keep very big coupling efficiency；neffIt is the effective refractive index of mid-infrared Graphene plasmon.
As shown in Fig. 2 in the present invention, sensing unit 33 is optical microcavity structure, including laterally (by the first grating coupled zone
The direction of the 31 to the second grating coupled zone 34) two identical Bragg reflectors being laid in side by side in doped silicon substrate 35
331, each Bragg reflector 331 includes M air ducting layer 3311 and doped silicon ducting layer 3312, and by first air waveguide
The order of layer 3311 and rear doped silicon ducting layer 3312 is transversely alternately arranged, and M >=4, M is bigger, and certainty of measurement is higher, while by
In the restriction of the exciting unit's transmission range of Graphene plasma, M values are no more than 8；Pass through in the middle of two Bragg reflectors 331
One air grooves 332 connects, and forms an optical resonator；The grating of the first, second grating coupled zone of the present invention is logical
Cross and linear groove realization is etched in doped silicon substrate 35, the air ducting layer 3311 of Bragg reflector 331 and air are recessed
Groove 332 is realized by etching double Prague emitting structural grooves in doped silicon substrate 35.
Two Bragg reflectors 331 make mid-infrared Graphene plasmon height local in the (optics of air grooves 332
Resonator cavity) in, reaction is repeated with the biological sample for being filled in air grooves 332, measure biological sample so as to high-precision
The infrared spectrum of molecule and the drift of formant.
In the present invention, lateral length d1 (the mid-infrared Graphene plasmas of the air ducting layer of Bragg reflector 331
Conveying length of the excimer in air waveguide) with lateral length d2 (the mid-infrared Graphene plasmons of doped silicon ducting layer
In the conveying length of doped silicon ducting layer) determined by Bragg condition, i.e.,：
d1×Real(neff1)+d2×Real(neff2)=m λb/2；
Wherein, λbIt is the centre wavelength in Prague；M is the exponent number in Prague；Real(neff1) for mid-infrared Graphene etc. from
Effective refractive index of the sub- excimer in air ducting layer；Real(neff2) for mid-infrared Graphene plasmon in doped silicon waveguide
The effective refractive index of layer.
Long L (the air grooves in chamber of the optical resonator that the air grooves 332 of two Bragg reflectors 331 of connection are formed
Lateral length) be：
L=Λ r/ [neff·2]；
Wherein, Λ r are resonant wavelength；neffIt is the effective refractive index of resonant wavelength waveguide, it is Graphene fermi level Ef
Function, Graphene fermi level can pass through to adjust the voltage that be applied on Graphene and.
In the present invention, Graphene plasmon sensing unit 30 also includes dielectric layer 36, and dielectric layer 36 is arranged on stone
Between black alkene layer 32 and doped silicon substrate 35, field-effect tube structure is formed；Present media layer 36 is Al2O3, in Al2O3In, in
Infrared Graphene plasmon loss is little.
In the present invention, metal electrode 37 is provided with graphene layer 32, metal electrode 37 is grounded, and doped silicon substrate 35 connects
Electricity, field-effect tube structure conducting realizes that the mode that back electrode is powered up is the applied voltage of graphene layer 32, and by adjusting stone is applied to
Voltage swing on black alkene layer 32, regulation and control are the fermi level sizes of Graphene, and resonance spectrum is big with the fermi level of Graphene
Little change is moved；When resonance spectrum is moved, formant will be in different wavelength regions, so as to realize to not jljl
The measurement of the absworption peak of matter, thus can measure different biological specimens on a biochemical sensor.
Fig. 3 is illustrated for the spectrum test result obtained using the mid-infrared plasmon biochemical sensor for providing of the invention
Figure, mid-infrared plasmon biochemical sensor predominantly detects two physical quantitys of absorption of the movement of formant and formant.By
In the enhanced characteristic of mid-infrared Plasmon Resonance, (in Fig. 3, it is applied on Graphene by the wavelength amount of movement of formant
Voltage when being V1, the wavelength amount of movement of formant is Δ λ 1；When the voltage being applied on Graphene is V2, the wavelength of formant
Amount of movement is Δ λ 2), the refractive index that biomolecule can be obtained with high sensitivity, being absorbed by formant to be given birth in high precision
The fingerprint of thing molecule absorbs information, and (when the voltage being applied in Fig. 3 on Graphene is V1, formant is absorbed as absworption peak 1；Apply
When voltage on Graphene is V2, formant is absorbed as absworption peak 2；), it is important so as to judge protein types and degeneration etc.
Biometric information.Using the characteristic of the fermi level electric tunable of Graphene, the voltage being applied on Graphene is adjusted from V1
V2 is saved, the formant dynamic of Graphene different positions can be continuously regulated to, to measure the refraction of different biological molecules
Rate and fingerprint absorption spectrum.
In the present invention, the processing technology of Graphene plasmon sensing unit comprises the steps：
The first step, device of the present invention are using the conventional lightly doped silicon chip (1-10 Ω cm) of semiconductor technology as graphite
The substrate of alkene plasmon sensing unit, draws the doped silicon wafer for taking 1cm*1cm as doped silicon substrate 10.
Second step, PMMA (poly methyl methacrylate) photoresist is uniformly spin-coated in doped silicon substrate 10
Face, after drying, in being put into electron beam exposure instrument, design configuration is transferred in doped silicon substrate 10.
3rd step, will be photo-etched using reactive ion light beam etching machine (reactive ion etching RIE) glue guarantor
The silicon dry etching in shield region falls 20nm.Then the doped silicon substrate 10 after etching is put in acetone soln, thoroughly removes and cover
Cover the PMMA photoresists on surface.
4th step, using thermal evaporation instrument under conditions of fine vacuum low rate, slowly three oxidations of one layer of 30nm of evaporation
Two aluminum (Al2O3) as the dielectric layer for applying dorsad voltage (back electrode).
The commercial chemical vapour deposition technique (chemical vapor deposition CVD) of 5th step, employing is in copper film
Graphene is laid on substrate.Before transfer grapheme two-dimension material, first by uniform spin coating one above the graphene layer of copper film
Layer PMMA layers, then put it in iron chloride (ferric chloride) environment and soak 12 hours, make the substrate of copper completely molten
Take off；The graphene film for being suspended in corrosive liquid surface and being stamped PMMA is got and is put in distilled water repeatedly rinsing until corrosion
Till residue is cleaned out；Then the Graphene sample insertion after etching pattern is floated over and is coated with PMMA layer graphene thin film
Below, carefully scoop up, allow the uniform unfolded of graphene film is layered on Graphene sample area of the pattern in doped silicon substrate 10；Deng
After Graphene sample drying, it is put in acetone soln and isopropanol and removes on PMMA layers.
The Graphene sample for having shifted is again passed by after electron beam exposure, the titanium and 100nm for being deposited with 5nm is golden, Ran Hou
Stripping is carried out in acetone soln and forms electrode 13, so far, whole Graphene plasmon sensing unit is prepared and finished.
Obviously, those skilled in the art can carry out the essence of various changes and modification without deviating from the present invention to the present invention
God and scope.So, if these modifications of the present invention and modification belong to the scope of the claims in the present invention and its equivalent technologies
Within, then the present invention is also intended to comprising these changes and modification.
Claims (8)
1. a kind of mid-infrared Graphene plasmon biochemical sensor, it is characterised in that wide spectrum light source including mid-infrared,
One mid-infrared lens, Graphene plasmon sensing unit and the second mid-infrared lens；
The Graphene plasmon sensing unit includes doped silicon substrate, is laid in the doped silicon substrate two ends respectively
First grating coupled zone and the second grating coupled zone, the sensing unit being laid in the middle of the doped silicon substrate, and it is covered in institute
State the graphene layer above the first grating coupled zone, sensing unit and the second grating coupled zone；
The mid-infrared light wave that the mid-infrared wide spectrum light source sends is by first mid-infrared lens focuss in first light
Grid coupled zone, couples with Graphene plasmon, produces mid-infrared Graphene plasmon；Described mid-infrared Graphene etc.
Ion excimer reaches the sensing unit by the graphene layer, repeatedly anti-with the biological sample being placed on the sensing unit
Should；Again the second grating coupled zone is reached via the graphene layer, and scatter to far field；By the second mid-infrared lens
Focus on and carry out in infrared spectrometer spectral measurement analysis.
2. sensor as claimed in claim 1, it is characterised in that the first grating coupled zone and the second grating coupled zone
Screen periods length Λ is：
Λ=λ0/neff；
Wherein, λ0It is free space mid-infrared light wavelength；neffIt is the effective refractive index of mid-infrared Graphene plasmon.
3. sensor as claimed in claim 1, it is characterised in that the sensing unit is optical microcavity structure, including laterally simultaneously
Arrangement is located at two identical Bragg reflectors in the doped silicon substrate；
Each described Bragg reflector includes M air ducting layer and doped silicon ducting layer, and by mixing after first air ducting layer
The order of miscellaneous silicon ducting layer is transversely alternately arranged, 8 >=M >=4；
By an air grooves connection in the middle of two Bragg reflectors, an optical resonator is formed, described in two
Bragg reflector makes mid-infrared Graphene plasmon height local in the air grooves, and is filled in the air
The biological sample of groove repeated reaction.
4. sensor as claimed in claim 3, it is characterised in that the first grating coupled zone and the second grating coupled zone
Grating is realized by etching linear groove in the doped silicon substrate；
The air ducting layer and the air grooves of the Bragg reflector is by etching in the doped silicon substrate
Linear pair of Prague emitting structural groove is realized.
5. sensor as claimed in claim 3, it is characterised in that the horizontal length of the air ducting layer of the Bragg reflector
Degree d1 is determined that physical relationship is by Bragg condition with the lateral length d2 of doped silicon ducting layer：
d1×Real(neff1)+d2×Real(neff2)=m λb/2；
Wherein, λbIt is the centre wavelength in Prague；M is the exponent number in Prague；Real(neff1) swash for mid-infrared Graphene plasma
Effective refractive index of the unit in air ducting layer；Real(neff2) for mid-infrared Graphene plasmon in doped silicon ducting layer
Effective refractive index.
6. sensor as claimed in claim 3, it is characterised in that the air grooves of two Bragg reflectors of connection
Lateral length L is：
L=Λ r/ [neff·2]；
Wherein, Λ r are resonant wavelength；neffIt is the effective refractive index of resonant wavelength waveguide.
7. sensor as claimed in claim 1, it is characterised in that the Graphene plasmon sensing unit also includes being situated between
Matter layer, the dielectric layer is arranged between the graphene layer and the doped silicon substrate, forms field-effect tube structure；
The graphene layer is provided with metal electrode, the metal electrode ground connection；
When the doped silicon substrate connects electricity, field-effect tube structure conducting, is the graphene layer applied voltage；
Regulation is applied to the size of voltage on the graphene layer, adjusts the fermi level size of Graphene, the Fermi of Graphene
Energy level size changes resonance spectrum and is moved.
8. sensor as claimed in claim 7, it is characterised in that the dielectric layer is Al2O3。
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