CN109883998A - Visible light can be changed penetration depth biosensor and preparation method thereof - Google Patents
Visible light can be changed penetration depth biosensor and preparation method thereof Download PDFInfo
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Abstract
Visible light can be changed penetration depth biosensor and preparation method thereof, including the prism unit set gradually, sensor unit, memristor unit and biomolecule cell factory to be measured, sensor unit includes LRSPR effect sensing unit and CPWR effect sensing unit, memristor unit is for realizing variable dielectric permittivity, including the first nonconductive dielectric layer, metal material layer, the conducting medium layer and power-up pressure device of first nonconductive dielectric layer upper surface are set, it is powered on pressure device difference guide dielectric layer and metal material layer applies positive and negative pole tension, in alive situation, so that electrochemical metallization occurs for the metal electrode of metal material layer, filament is generated in the first nonconductive dielectric layer to change the dielectric constant of medium.Under conditions of memristor unit loads generating positive and negative voltage, sensor unit carries out dynamic transition between LRSPR effect and CPWR effect, to realize the variation of flexible penetration depth.The present invention is suitable for the measurement of different organisms.
Description
Technical field
The invention belongs to surface plasmon resonance biosensor technical field, it is specifically related to a kind of using nano-filaments migration mechanism
Visible light can be changed penetration depth biosensor and preparation method thereof.
Background technique
Surface plasma excimer (SPPs) is the free charge on the interface occurred between dielectric and metal medium
Oscillation.Light can cause the excitation of SPPs.When the wave vector of surface plasma is matched with the wave vector of incident light, institute will occur
Surface plasma body resonant vibration (SPR) phenomenon of meaning, because this wave matching condition is easy to by the small dielectric constant on interface
Variation is destroyed, it is possible to accurately detect the variation of metal surface adsorption layer (cell, bacterium etc.) refractive index.Therefore, base
It is met the tendency of in the various surface plasmon resonance biosensors of decaying total reflection (ATR) method.
In the biosensor classification using the electromagnetism field (EM) enhancing metal film surfaces SPR excitation, it can identify
Four kinds of fundamental types, i.e. tradition SPR, long-range (LRSPR) SPR, coupled plasma Wave guide resonance (CPWR) and waveguide couple SPR
(WCPR)。
(1) tradition SPR surface plasma wave is exponentially decayed along interface normal direction, and Effective depth penetration is only
300nm or so, although this characteristic is very sensitive to the change of refractive index near interface, cannot achieve to virus, bacterium,
Effective detection of the macromoleculars such as protein, and conventional surface plasma resonance technology index reaches bottleneck, it is difficult to it improves.
(2) LRSPR biosensor is that medium buffering is introduced between the prism and metal layer of traditional surface plasmon resonance biosensor
Layer, when the refractive index of dielectric buffer layer and determinand is equal, realizes symmetrical structure, so that SPW (surface plasma wave,
Vibrated and propagated by SPPs) spread length be more than the spread length of routine SPW, and remain the energy of incident beam, advantage
It is the reflectivity that LRSPR device has very sharp (i.e. big depth~width ratio), the disadvantage is that depositing dependent on symmetrical structure
?.
(3) CPWR biosensor is combined with the ducting layer below traditional surface plasmon resonance biosensor surface, in CPWR device
The interference of ducting layer all causes precipitous inclination angle in (TE) mode at longitudinal direction (TM) and laterally, advantage be have preferable depth~
Width ratio and the penetration depth that 2um can be reached, the disadvantage is that bio-sensing surface distance metallic film and the SPW of waveguide bed boundary have
Sizable distance, sensitivity is still than traditional low 10 times of SPR device or so.
(4) WCSPR is made of two metal layers and a ducting layer.SPR and waveguide mode are combined in WCSPR device
The sensitivity of biosensor is not only remained, but also generates steeper reflectivity spectral decline and is lacked to improve measurement accuracy
Point is matching condition harshness.
The film structure of above-mentioned four kinds of SPR types is fixed and invariable, thus their penetration depth is all immutable.
However, current surface plasmon resonance biosensor penetration depth is all fixed and invariable, but for different determinands such as egg
It is white, bacterium, cell dispersion, living cells different sizes, especially to biggish unknown biochemical substances material, fixed penetration depth
Sensor generate ATR decaying evanescent wave can only section senses organism, all information cannot be obtained.And it mutually anticaustic larger penetrates
Depth transducer is come when sensing the small organism of size, the surface plasma wave of resonant check will be deep into across determinand
External environment generates biggish external interference, while resolution ratio can also reduce.It is penetrated accordingly, it is considered to design one kind and can change
The surface plasmon resonance biosensor of depth.
Metal nano filament migration mechanism structure under bias is usually metal~medium~metal (or conducting medium)
Sandwich shape, principle be with voltage drive metal ion occur electrochemical metallization (ECM), form metal in the dielectric layer
Nano-filaments, the filament have modulating action to light propagation, are the dielectric constant for changing medium on microcosmic.Therefore, it is based on
The technology considers that design visible light can be changed penetration depth biosensor.
Summary of the invention
The technical problem to be solved by the present invention is to the disadvantages mentioned above in order to overcome the prior art, providing a kind of visible light can
Become penetration depth biosensor and preparation method thereof.
The technical solution adopted by the present invention to solve the technical problems is: visible light can be changed penetration depth biosensor,
Including prism unit, sensor unit, memristor unit and the biomolecule cell factory to be measured set gradually, sensor unit
Including LRSPR effect sensing unit and CPWR effect sensing unit,
Prism unit is for generating ATR decaying evanescent wave；
For LRSPR effect sensing unit for realizing LRSPR effect, first successively including auxiliary realization LRSPR effect is non-
Conducting medium layer, metal material layer and the second nonconductive dielectric layer, metal material layer and are arranged in the first non-of its surface
Conducting medium layer forms CPWR effect sensing unit, and when LRSPR effect resonance condition is by broken ring, CPWR effect sensing unit is real
Existing CPWR effect；
Memristor unit is for realizing variable dielectric permittivity, including the first nonconductive dielectric layer, metal material layer, setting
Conducting medium layer and power-up pressure device in the first nonconductive dielectric layer upper surface, power-up pressure device distinguish guide dielectric layer
And metal material layer applies positive and negative pole tension, in alive situation, so that electrification occurs for the metal electrode of metal material layer
Metallization is learned, generates filament in the first nonconductive dielectric layer to change the dielectric constant of medium.
Specifically, the first nonconductive dielectric layer is SiO2Layer, thickness range are 350~375nm, metal material layer Ag
Layer, thickness range are 35~42nm, and the second nonconductive dielectric layer is SiO2Layer, thickness range are 350~375nm；Conducting medium
The ITO ranges of indices of refraction of layer is 1.45~1.60, and thickness range is 40~60nm.Preferably, metal material layer and conducting medium
Layer forms orthogonal CROSSBAR structure, and the CROSSBAR line width and spacing range are 0.2~1mm.
Specifically, prism unit is semi- cylindrical glass lens, sensor unit is set on its rectangle face.
Preferably, the material of prism unit is SF11 or BK7.
Another technical solution adopted by the present invention to solve the technical problem thereof is that: preparing above-mentioned visible light can be changed penetration depth
The method of biosensor, comprising the following steps:
In the first nonconductive dielectric layer of prism side sputtering sedimentation；
In the first non-conductive medium layer surface sputtering sedimentation metal material layer, to metal material layer gluing and figure dissolves slot
Body forms top electrode, and light excitation generates surface plasma body resonant vibration；
In metal material layer surface the second nonconductive dielectric layer of sputtering sedimentation；
In the second non-conductive medium layer surface sputtering sedimentation conducting medium layer, to its gluing and figure dissolves groove body and forms bottom
Electrode, and CROSSBAR structure is constituted with metal material layer.
Specifically, using radio frequency magnetron mode sputtering sedimentation nonconductive dielectric layer, using Deposited By Dc Magnetron Sputtering metal
Material layer.
The beneficial effects of the present invention are: compared to the prior art, which can load positive and negative in memristor unit
Under conditions of voltage, sensor unit carries out dynamic transition between LRSPR effect and CPWR effect, is flexibly penetrated with realizing
The variation of depth can significantly improve its resolution ratio when detecting unknown material organism, be widely used in different determinands.This
Invention is suitable for the measurement of different organisms.
Detailed description of the invention
Fig. 1 is structural schematic diagram of the invention；
Fig. 2 is the structural schematic diagram of memristor unit of the invention；
Fig. 3 is the simulation result diagram of Finite-Difference Time-Domain Method of the invention；
Wherein, 10 be biosensor, and 11 be prism unit, and 12 be LRSPR effect sensor unit, and 13 be CPWR effect
Sensing unit, 14 be memristor unit, and 15 be biomolecule cell factory to be measured, and 121 be the first nonconductive dielectric layer, and 122 be gold
Belong to material layer, 123 be the second nonconductive dielectric layer, and 141 be conducting medium layer, and 142 be power-up pressure device.
Specific embodiment
With reference to the accompanying drawings and embodiments, technical scheme in the embodiment of the invention is clearly and completely described, shows
So, described embodiment is only a part of the embodiments of the present invention, instead of all the embodiments.Below at least one
The description only actually of exemplary embodiment be it is illustrative, never as to the present invention and its application or any limit used
System.Based on the embodiments of the present invention, obtained by those of ordinary skill in the art without making creative efforts
Every other embodiment, shall fall within the protection scope of the present invention.Non-elaborated part of the present invention belongs to techniques well known.
Technology, method and apparatus known to person of ordinary skill in the relevant may be not discussed in detail, but suitable
In the case of, the technology, method and apparatus should be considered as authorizing part of specification.
As shown in Figure 1, it includes for generating ATR decaying suddenly that visible light of the invention, which can be changed penetration depth biosensor 10,
Die the prism unit 11 of wave, for realizing the sensor unit 12/13 of LRSPR effect or CPWR effect, for realizing variable Jie
The memristor unit 14 of matter dielectric constant and biomolecule cell factory 15 to be measured.
Prism unit 11 includes the biggish prism of refractive index to meet light wave total reflection condition, in visible light incident excitation
Under, ATR decaying evanescent wave can be generated, based on cost and realizes that effect considers, prism unit semi- cylindrical glass lens, at it
Sensor unit is set on rectangle face, and material is preferably SF11 or BK7.
Sensor unit includes for realizing the LRSPR effect sensing unit 12 of LRSPR effect and for realizing CPWR effect
The CPWR effect sensing unit 13 answered, LRSPR effect sensing unit 12 successively include that auxiliary realizes that the first of LRSPR effect non-leads
Dielectric layer 121, metal material layer 122 and the second nonconductive dielectric layer 123 for constituting symmetrical structure, the symmetrical junction
Structure i.e. the second non-conductive medium 123 and the first non-conductive medium 121 are formed symmetrically about metal material layer 122, and second is non-conductive
Medium 123 is identical or approximately uniform with the refractive index of the first non-conductive medium 121, the SPR generated under light wave excitation in this way
Effect is also essentially identical, therefore the SPR effect under two antisymmetry could be made to form LRSPR effect；Based on effect and cost
Comprehensively consider, metal material layer is preferably Ag layers, this is because metal Ag, in the case where biasing holds electric field action, Ag electrode will generate electricity
Chemical metallization effect provides Ag nano-filaments, and the high sensitivity that resonates, and resonance depth is big；And since Ag nano-filaments are easy to
In SiO2Electrochemical metallization effect occurs in dielectric layer, realizes the growth and resolution of nano-filaments, that is, is easy to nano-filaments and moves
It moves and generates SPR effect, therefore that the first nonconductive dielectric layer 121 and the second nonconductive dielectric layer 123 is preferably SiO2Layer；In order to
Reach preferably variable penetration depth variation, Ag layers with a thickness of 35~42nm, SiO2Layer with a thickness of 350~375nm, wherein
The thickness of first nonconductive dielectric layer 121 and the second nonconductive dielectric layer 123 can be identical according to practical adjustments, can also not
Together, but require the refractive index of the two as identical as possible；.Metal material layer 122 and it is disposed thereon the first non-conductive of surface
Dielectric layer 121 forms CPWR effect sensing unit (13), and when LRSPR effect resonance condition is by broken ring, CPWR effect sensing is single
First (13) realize CPWR effect.
As shown in Fig. 2, memristor unit (14) is for realizing variable dielectric permittivity, including the first nonconductive dielectric layer
121, metal material layer 122, be arranged in 121 upper surface of the first nonconductive dielectric layer conducting medium layer 141 and power-up press fitting
Set 142, in order to reach preferably variable penetration depth variation, conducting medium layer 141 be preferably refractive index be 1.45~1.60, it is thick
Degree is the ITO layer of 40~60nm, and to guarantee that ohmic contact resistance is sufficiently small, metal material layer and conducting medium layer are formed and mutually hung down
Straight CROSSBAR structure, the CROSSBAR line width and spacing range are 0.2~1mm.Pressure device is powered on to be situated between to conduction respectively
Matter layer 141 and metal material layer 122 apply positive and negative pole tension, in alive situation, so that the metal of metal material layer 122
Electrochemical metallization (ECM) occurs for electrode, generates filament in the first nonconductive dielectric layer 121 to change the dielectric of medium
Constant.Under conditions of memristor unit loads generating positive and negative voltage, sensor unit is moved between LRSPR effect and CPWR effect
State transformation, to realize the variation of flexible penetration depth.
The method for preparing the sensor, which comprises the following steps:
A. the second nonconductive dielectric layer of radio frequency magnetron mode sputtering sedimentation 123, second non-conductive Jie are used in prism side
Matter layer 123 is preferably the SiO with a thickness of 350~375nmd2Layer, by taking semi- cylindrical glass lens as an example, herein side be its four
Face where the shape of side；
B. magnetron sputtering deposited metal material layer 122 is flowed on 121 surface of the first nonconductive dielectric layer, metal material layer is preferred
For with a thickness of the Ag of 35~42nm layer, to 122 gluing of metal material layer and figure dissolves groove body and forms top electrode, and light excitation produces
Raw surface plasma body resonant vibration；
C. the second nonconductive dielectric layer 123, first non-conductive Jie are deposited in 122 surface radio frequency magnetron sputtering of metal material layer
Matter layer is preferably the SiO with a thickness of 350~375nm2Layer,
D. conducting medium layer 141, conducting medium layer are deposited in 123 surface radio frequency magnetron sputtering of the second nonconductive dielectric layer
141 preferably with a thickness of the ITO layer of 40~60nm, and to its gluing and figure dissolves groove body and forms hearth electrode, and and metal material
Layer 122 constitutes the channel CROSSBAR.
On adding bias voltage, electrochemical metallization (ECM) can occur for metal material layer 122, and metal material layer 122 passes through
Redox grows metal nano filament in the first nonconductive dielectric layer 121, changes original first non-conductive Jie
The dielectric constant of 121 film regional area of matter layer.
The workflow of the sensor is as follows:
In the biasing of 14 no-voltage of memristor unit, surface plasmon resonance biosensor uses angle mode, it will be seen that hot spot alignment
The channel CROSSBAR, shown in resonance angle such as Fig. 3 (a), principle are as follows: for prism unit 11 under the excitation of visible light incidence, first is non-
The sandwich structure (121/122/123) of 121/ metal material layer of conducting medium layer, 122/ second nonconductive dielectric layer 123 can shape
LRSPR at LRSPR effect (long-range plasma resonance) and at this time has high sensitivity, has overlength penetration depth.
In memristor unit 14 plus positive voltage bias, which still uses angle mode, incident in visible light
Under excitation, resonance angle is adjusted to such as Fig. 3 (b), and under positive bias-voltage, 122/ first nonconductive dielectric layer 121/ of metal material layer is led
Electrochemical metallization (ECM) occurs for the metal material layer 122 in the sandwich structure (122/121/141) of dielectric layer 141, gold
Belong to material layer 122 and metal nano filament is grown into 121 medium of the first nonconductive dielectric layer by redox, entirely
10 structure of biosensor becomes 11/ first nonconductive dielectric layer of prism unit, 121/ metal material layer 122/ containing filament
First nonconductive dielectric layer, 121/ conducting medium layer 141/ biomolecule cell factory 15 to be measured, the at this time filament containing metal nano
Compared to original first nonconductive dielectric layer 121, dielectric constant changes first nonconductive dielectric layer 121, destroys original
There is the symmetrical structure of device refractive index, also destroys the condition of LRSPR formation, device architecture is because of memristor mechanism to restructural
For CPWR structure, and penetrating for CPWR effect reduces compared to LRSPR penetration depth.
In memristor unit 14 plus negative voltage bias, 122/ first nonconductive dielectric layer of metal material layer, 121/ conducting medium
Electrochemical metallization (ECM) occurs for the metal material layer 122 of the sandwich structure (122/121/141) of layer 141.In this case,
The metal nano filament of first nonconductive dielectric layer 121 migrates back silver electrode under reversed electric field effect, it will be seen that hot spot alignment
The channel CROSSBAR, under the excitation of visible light incidence, entire 10 structure of biosensor has become again again biases feelings without making alive
Condition, the LRSPR effect formed at this time have the characteristic of overlength penetration depth again.
Fig. 3 is biosensor FDTD (Finite-Difference Time-Domain Method) simulation result, and surface plasmon resonance biosensor is tuned into angle mould
Formula.
In the biasing of 14 no-voltage of memristor unit, device architecture forms LRSPR effect, and it is anti-that Fig. 3 (a) shows normalization
It penetrates and composes existing double resonance peak, tested organism is sensed with low-angle formant under antisymmetry, simulates penetrating for its LRSPR
Depth such as Fig. 3 (c) is shown in solid, up to 2.5um or more；
When memristor unit 14 plus when positive voltage bias, shown in normalization reflectance spectrum such as Fig. 3 (b), at this time device architecture because
The symmetrical structure of original dielectric layer dielectric constant is destroyed for metal nano filament, so that CPWR effect is formed, corresponding diagram 3
(c) penetration depth shown in dotted line is only 1um or so；
When memristor unit 14 plus negative voltage bias, the metal nano filament in dielectric layer migrates under reversed electric field effect
Silver electrode is returned, entire biosensor structure changes back to no-voltage biasing again, and the LRSPR formed at this time again there is overlength to penetrate depth
The characteristic of degree.
Claims (7)
1. visible light can be changed penetration depth biosensor, which is characterized in that including prism unit (11), the sensing set gradually
Device unit, memristor unit (14) and biomolecule cell factory to be measured (15), sensor unit include that LRSPR effect sensing is single
First (12) and CPWR effect sensing unit (13),
Prism unit (11) is for generating ATR decaying evanescent wave；
For LRSPR effect sensing unit (12) for realizing LRSPR effect, first successively including auxiliary realization LRSPR effect is non-
Conducting medium layer (121), metal material layer (122) and the second nonconductive dielectric layer (123), the second non-conductive medium and first
Non-conductive medium constitutes symmetrical structure；
Metal material layer (122) and the second nonconductive dielectric layer (123) for being disposed thereon surface form CPWR effect sensing
Unit (13), when LRSPR effect resonance condition is by broken ring, CPWR effect sensing unit (13) realizes CPWR effect；
Memristor unit (14) is for realizing variable dielectric permittivity, including the first nonconductive dielectric layer (121), metal material layer
(122), the conducting medium layer (141) in the first nonconductive dielectric layer (121) upper surface and power-up pressure device (142) are set,
It is powered on pressure device difference guide dielectric layer (141) and metal material layer (122) applies positive and negative pole tension, in alive situation
Under, so that electrochemical metallization occurs for the metal electrode of metal material layer (122), produced in the first nonconductive dielectric layer (121)
Filament is given birth to change the dielectric constant of medium；
Under conditions of memristor unit loads generating positive and negative voltage, sensor unit is moved between LRSPR effect and CPWR effect
State transformation, to realize the variation of flexible penetration depth.
2. sensor as described in claim 1, which is characterized in that the first nonconductive dielectric layer (121) is SiO2Layer, thickness model
It encloses for 350~375nm, metal material layer is Ag layer, and thickness range is 35~42nm, and the second nonconductive dielectric layer is SiO2Layer,
Thickness range is 350~375nm；The ITO ranges of indices of refraction of conducting medium layer be 1.45~1.60, thickness range be 40~
60nm。
3. sensor as described in claim 1, which is characterized in that metal material layer forms orthogonal with conducting medium layer
CROSSBAR structure, the line width of the CROSSBAR and the value range of spacing are 0.2~1mm.
4. sensor as described in claim 1, which is characterized in that prism unit (11) is semi- cylindrical glass lens, at it
Sensor unit is arranged on face in rectangle.
5. sensor as claimed in claim 4, which is characterized in that the material of prism unit is SF11 or BK7.
6. the method that the visible light of preparation such as 1~5 any claim can be changed penetration depth biosensor, which is characterized in that
The following steps are included:
In the first nonconductive dielectric layer of prism side sputtering sedimentation (121)；
In the first nonconductive dielectric layer (121) surface sputtering sedimentation metal material layer (122), to metal material layer (122) gluing
And figure dissolves groove body and forms top electrode, and light excitation generates surface plasma body resonant vibration；
In metal material layer (122) surface the second nonconductive dielectric layer of sputtering sedimentation (123),
In the second nonconductive dielectric layer (123) surface sputtering sedimentation conducting medium layer (141), to its gluing and figure dissolves groove body
Hearth electrode is formed, and constitutes CROSSBAR structure with metal material layer (122).
7. method as claimed in claim 6, which is characterized in that using radio frequency magnetron mode sputtering sedimentation nonconductive dielectric layer and
Conducting medium layer, using Deposited By Dc Magnetron Sputtering metal material layer.
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| CN111812908A (en) * | 2020-07-23 | 2020-10-23 | 电子科技大学 | Fabry-Perot cavity filter and method for dynamic color regulation |
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