CN117405604B - Graphene biosensor based on double-layer sub-wavelength grating - Google Patents
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 94
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 94
- 238000001514 detection method Methods 0.000 claims abstract description 72
- 239000000126 substance Substances 0.000 claims abstract description 55
- 239000000463 material Substances 0.000 claims abstract description 15
- 239000010410 layer Substances 0.000 claims description 105
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 14
- 229910052709 silver Inorganic materials 0.000 claims description 14
- 239000004332 silver Substances 0.000 claims description 14
- 239000000758 substrate Substances 0.000 claims description 11
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 6
- 239000002355 dual-layer Substances 0.000 claims description 5
- 235000012239 silicon dioxide Nutrition 0.000 claims description 3
- 239000000377 silicon dioxide Substances 0.000 claims description 3
- 230000035945 sensitivity Effects 0.000 abstract description 24
- 238000001228 spectrum Methods 0.000 abstract description 7
- 229910002804 graphite Inorganic materials 0.000 abstract description 4
- 239000010439 graphite Substances 0.000 abstract description 4
- -1 graphite alkene Chemical class 0.000 abstract description 4
- 230000003287 optical effect Effects 0.000 description 18
- 238000010521 absorption reaction Methods 0.000 description 15
- 238000000862 absorption spectrum Methods 0.000 description 9
- 230000008859 change Effects 0.000 description 8
- 239000002356 single layer Substances 0.000 description 8
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Abstract
The invention relates to the technical field of detection and analysis. The graphene biosensor based on the double-layer sub-wavelength grating comprises an upper sub-wavelength grating and a lower sub-wavelength grating; the two sub-wavelength gratings are arranged in mirror symmetry, and an intermediate gap formed by the two sub-wavelength gratings forms a detection material channel; the inner surfaces of the upper sub-wavelength grating and the lower sub-wavelength grating are respectively provided with a graphene layer; the detection substance flows in the horizontal direction through the detection substance channel, and the direction of light rays incident to the upper sub-wavelength grating is not parallel to the direction of the detection substance channel. According to the sensor provided by the invention, on one hand, the detection sensitivity of the biosensor is improved by arranging the detection material channel direction and the incident light direction in a non-parallel manner; on the other hand, through setting up the graphite alkene layer at the internal surface of sub-wavelength grating for the graphite alkene layer can absorb more spectrums, has further improved this biosensor's detection sensitivity.
Description
Technical Field
The invention relates to the technical field of detection and analysis, in particular to a graphene biosensor based on a double-layer sub-wavelength grating.
Background
The sub-wavelength grating structure is quite sensitive to small changes in refractive index of analytes as a typical micro-nano photonic structure, and has been applied as an optical biosensor in fields such as biosensing. Compared with other biosensors, the optical biosensor has wide application in fields such as clinical diagnosis, drug discovery, food sanitation and safety, environmental control and the like due to advantages in terms of electromagnetic interference resistance and cost control. The optical biosensor based on the sub-wavelength grating has the advantages of simple pretreatment, no influence on the property of detection molecules, high sensitivity, robustness, integration and the like, and has excellent application prospect.
The optical biosensor has the advantages of no-mark detection, easy on-chip integration and the like, but the detection sensitivity of the current optical sensor is not high enough.
Disclosure of Invention
The invention provides a graphene biosensor based on a double-layer sub-wavelength grating, which is used for solving the defect that the detection sensitivity of an optical biosensor in the prior art is not high enough.
The invention provides a graphene biosensor based on a double-layer sub-wavelength grating, which comprises the following components:
an upper sub-wavelength grating, a lower sub-wavelength grating; the two sub-wavelength gratings are arranged in mirror symmetry, and an intermediate gap formed by the two sub-wavelength gratings forms a detection material channel;
the inner surfaces of the upper sub-wavelength grating and the lower sub-wavelength grating are respectively provided with a graphene layer;
the detection substance flows in a horizontal direction through the detection substance channel, and the direction of light rays incident to the upper sub-wavelength grating is not parallel to the direction of the detection substance channel.
According to the graphene biosensor based on the double-layer sub-wavelength grating provided by the invention, the upper sub-wavelength grating comprises: the graphene layer is respectively arranged on the upper waveguide layer and the upper grating layer;
the lower sub-wavelength grating includes: the graphene layer is respectively arranged on the lower waveguide layer and the lower grating layers.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the light incident to the upper sub-wavelength grating is perpendicular to the detection material channel.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the silver substrate is arranged on the bottom surface of the outer side of the lower sub-wavelength grating.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the silver substrate is arranged on the bottom surface of the outer side of the lower sub-wavelength grating.
According to the graphene biosensor based on the double-layer sub-wavelength grating, which is provided by the invention, the thicknesses d of the upper grating layer and the lower grating layer g All 220nm, width w=357 nm; the thicknesses of the upper waveguide layer and the lower waveguide layer are L=2235 nm; detection material channel width h=2000 nm.
According to the graphene biosensor based on the double-layer sub-wavelength grating, provided by the invention, a single period P=960 nm of the double-layer sub-wavelength grating structure.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the upper grating layer and the lower grating layer are Si with the refractive index of 3.48, and the upper waveguide layer and the lower waveguide layer are silicon dioxide with the refractive index of 1.46.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the thickness of the graphene layer is 0.34nm.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the thickness of the silver substrate is 100nm.
The graphene biosensor based on the double-layer sub-wavelength grating has a simple structure and is convenient to prepare, on one hand, the channel direction of a detection substance and the incident light direction are not arranged in parallel, so that the two channels are distinguished, the mutual interference between the detected substance and the incident light is reduced, and the detection sensitivity of the biosensor is improved; on the other hand, through setting up the graphite alkene layer at the internal surface of sub-wavelength grating for the graphite alkene layer can absorb more spectrums, thereby has further improved this biosensor's detection sensitivity. In addition, the sensor provided by the invention can still maintain higher detection sensitivity in the variation range of the incident angle of the incident light from 0 degree to 20 degrees, and the principle is that: the high surface volume ratio and rich pi conjugated structure of the graphene can enable oblique incident light to be more bound around a substance to be detected, and the characteristic can reduce adverse effects on detection sensitivity of the sensor when light is obliquely incident.
Drawings
In order to more clearly illustrate the invention or the technical solutions of the prior art, the following description will briefly explain the drawings used in the embodiments or the description of the prior art, and it is obvious that the drawings in the following description are some embodiments of the invention, and other drawings can be obtained according to the drawings without inventive effort for a person skilled in the art.
Fig. 1 is a schematic structural diagram of a graphene biosensor based on a double-layer sub-wavelength grating provided by the invention;
FIG. 2 is a graph showing the absorption spectrum of an optical sensor with or without graphene coverage for an incident light ray having an inclination angle of 0, 10, or 20 degrees;
FIG. 3 is a graph showing the absorption spectrum of the resonant peak of the optical sensor when the refractive index of the substance to be measured changes under the condition that the light is fixed to be vertically incident;
fig. 4 is an evolutionary absorption spectrum of a resonance peak of the optical sensor when an incident angle of incident light is changed.
Detailed Description
For the purpose of making the objects, technical solutions and advantages of the present invention more apparent, the technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings, and it is apparent that the described embodiments are some embodiments of the present invention, not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
On one hand, the existing optical biosensor has the problem that incident light is consistent with a detection channel of a molecule to be detected, so that mutual interference is easy to occur, and the detection effect is influenced. According to the invention, the light incident direction of the double-layer sub-wavelength grating and the flowing direction of the substance to be detected are mutually perpendicular, so that the two are not mutually interfered, and the detection sensitivity of the biosensor is improved.
In addition, graphene is used as a two-dimensional material with excellent performance, has a rich pi conjugated structure and a high surface volume ratio, can be used as a biomolecule identifying element to be added into a sub-wavelength grating sensor, and further improves the sensing performance of an optical biosensor. However, because graphene has weak near-infrared light-substance interaction capability (its absorption rate in the near-infrared band is only 2.3%), it may make it difficult to distinguish the absorption peak of the absorption channel of the biosensor, and it is difficult to detect the substance. This has led to the development of graphene optical biosensors with difficulties. According to the invention, graphene is placed in a sub-wavelength grating structure, and the enhancement of the photo-substance interaction capability of the graphene is realized through the resonance of the sub-wavelength grating in a near infrared band. From the electric field distribution, the sub-wavelength grating structure can enable light to be more bound around the graphene layer, so that more detection channels are provided, the absorption efficiency is increased, and finally the detection sensitivity of the sensor is improved.
Fig. 1 is a schematic structural diagram of a graphene biosensor based on a dual-layer sub-wavelength grating, provided by the invention, as shown in fig. 1, and the graphene biosensor based on the dual-layer sub-wavelength grating, provided by the invention, comprises: the two sub-wavelength grating structures are covered with single-layer graphene, an intermediate detection substance channel and a bottom metal substrate. Wherein the intermediate detection substance channel is constituted by a gap between the two sub-wavelength grating structures. The biosensor provided by the invention can form a near perfect resonance peak, has a simple structure, is convenient to process, and can reduce mutual interference by separating a light incidence channel from a middle detection substance channel so as to improve detection sensitivity; and by means of the combined action of the double-layer sub-wavelength grating structure and the graphene, the high-sensitivity detection of the detected substance is realized, and the method has a good application prospect in the aspect of biological sensing in the field of micro-nano optical devices.
As shown in fig. 1, the graphene biosensor provided by the present invention includes:
an upper sub-wavelength grating 1 and a lower sub-wavelength grating 2; the two sub-wavelength gratings are arranged in mirror symmetry, and an intermediate gap formed by the two sub-wavelength gratings forms a detection material channel 3;
the inner surfaces of the upper sub-wavelength grating 1 and the lower sub-wavelength grating 2 are respectively provided with a graphene layer 4;
the detection substance flows in the horizontal direction through the detection substance channel, and the direction of the light incident to the upper sub-wavelength grating 1 is not parallel to the direction of the detection substance channel.
Specifically, according to the graphene biosensor provided by the invention, detection substances only flow in the horizontal direction of a detection substance channel, the upper part and the lower part of the biosensor are air, and light enters the sensor from the upper part of the sensor.
The graphene biosensor provided by the invention has the working principle that: after the detected substance flows in the horizontal direction through the detection substance channel, incident light is projected from the upper surface of the upper sub-wavelength grating 1, the incident light sequentially passes through the upper sub-wavelength grating 1, the graphene layer 4 and the detection substance in the detection substance channel, then the graphene layer 4 on the lower sub-wavelength grating 2 absorbs the spectrum of the incident light, then the light after the absorption spectrum is reflected by the lower sub-wavelength grating 2, so that the light is reflected back to the detection substance in the detection substance channel, and finally the light is emitted through the upper sub-wavelength grating 1. Then, the spectrum corresponding to the detected substance can be detected through the spectrum of the incident light and the spectrum of the emergent light, so that the specific type of the detected substance is finally determined, and the high-precision detection of the detected substance is finally realized.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the graphene layers 4 are arranged on the inner surfaces of the upper sub-wavelength grating 1 and the lower sub-wavelength grating 2, so that more light fields in the gratings leak into substances to be detected with low refractive indexes; meanwhile, the graphene is covered on the top of the grating structure and can be fully contacted with a substance to be detected, and more light beams can be bound in a channel where the substance to be detected exists by utilizing the high surface volume ratio of the graphene and the rich pi conjugated structure, so that the detection sensitivity of the biosensor is improved.
The graphene biosensor based on the double-layer sub-wavelength grating has a simple structure and is convenient to prepare, on one hand, the channel direction of a detection substance and the incident light direction are not arranged in parallel, so that the two channels are distinguished, the mutual interference between the detected substance and the incident light is reduced, and the detection sensitivity of the biosensor is improved; on the other hand, through setting up the graphene layer at the internal surface of sub-wavelength grating for more light beams can be bound in the passageway that the material of waiting to examine exists, thereby further improved this biosensor's detection sensitivity.
Further, the upper sub-wavelength grating 1 includes: an upper waveguide layer 11 and a plurality of upper grating layers 12 arranged on the upper waveguide layer 11, wherein the graphene layers 4 are respectively arranged on the upper waveguide layer 11 and the upper grating layers 12;
the lower sub-wavelength grating 2 includes: a lower waveguide layer 22 and several lower grating layers 21 arranged on the lower waveguide layer 22, said graphene layer 4 being arranged on said lower waveguide layer 22 and lower grating layers 21, respectively.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the graphene layers are arranged on the upper waveguide layer 11, the upper grating layer 12, the lower waveguide layer 22 and the lower grating layer 21, so that more light beams are bound in the channel where the substance to be detected exists, and the detection sensitivity of the biosensor is improved.
Further, the light incident on the upper sub-wavelength grating 1 is perpendicular to the detection material channel.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the incident light and the detection substance channel are vertically arranged, so that the mutual interference between the incident light and the detection substance channel is greatly reduced, and the detection sensitivity of the biosensor is further improved.
Further, a silver substrate 5 is provided on the outer bottom surface of the lower sub-wavelength grating 2. The relative dielectric constant of metallic silver is given by Lorentz-Drude model (Lorentz-Drude mode) and the silver substrate thickness l is 100nm.
According to the graphene biosensor based on the double-layer sub-wavelength grating, the silver substrate 5 is arranged on the bottom surface of the outer side of the lower sub-wavelength grating 2, so that incident light can be reflected to a detected substance, and the detection sensitivity of the biosensor is further improved. By controlling the thickness of the silver substrate to be 100nm, the biosensor has more sensitive detection degree, and the principle is that: the silver substrate acts as a metal mirror to re-reflect light leaking from the sub-wavelength grating structure into the sub-wavelength grating structure to enhance absorption. The choice of too small a thickness of silver may result in incomplete reflection, impact absorption, and too thick silver may increase cost. In a comprehensive view, the invention selects the silver with the thickness of 100nm to realize the function of total reflection while controlling the cost.
Further, the thicknesses d of the upper grating layer 12 and the lower grating layer 21 g All 220nm, width w=357 nm; the thickness l=2235 nm of the upper waveguide layer 11 and the lower waveguide layer 22; detecting material channel width h=2000 nm; a single period p=960 nm of the dual layer sub-wavelength grating structure.
According to the graphene biosensor based on the double-layer sub-wavelength grating, through the limitation of the data, the resonance intensity can be increased to a greater extent, and the wide detection material channel (H=2000 nm) can contain more substances to be detected, so that a light field can be more localized in the detection channel, and the detection sensitivity is further improved.
Further, in the embodiment of the present invention, the upper grating layer 12 and the lower grating layer 21 are Si with a refractive index of 3.48, and the upper waveguide layer 11 and the lower waveguide layer 22 are silicon dioxide with a refractive index of 1.46.
The graphene biosensor based on the double-layer sub-wavelength grating provided by the invention has more sensitive detection degree by limiting the data, and the principle is that: a high refractive index difference grating (HCG) structure is a sub-wavelength grating structure that is simple and easy to implement for high sensitivity grating sensors. Using Si of high refractive index (refractive index 3.48) and lowSiO of refractive index 2 (refractive index 1.46) materials as the grating layer and the waveguide layer, respectively, enable the construction of a high refractive index difference grating, so that the biosensor has high sensitivity.
Further, the thickness d of the graphene layer h 0.34nm.
Specifically, the graphene layer is a single-layer graphene, and the thickness of the single-layer graphene is 0.34nm, namely the thickness of one carbon atom, and the single-layer graphene can absorb more light because the surface conductivity of the single-layer graphene layer is composed of inter-band conductivity and in-band conductivity and has high strength and electron mobility.
The graphene biosensor based on the double-layer sub-wavelength grating provided by the invention has the advantages that the thickness d of the graphene layer is as follows h The single-layer graphene is 0.34nm, so that more light can be absorbed, the refractive index sensing of the sub-wavelength grating is converted into absorption sensing, and the light can be more bound in a channel in which a substance to be detected exists by utilizing the high surface volume ratio and rich pi conjugated structure of the graphene, so that the detection sensitivity of the biosensor is further improved.
Fig. 2 is a graph showing the absorption spectrum of an optical sensor with or without graphene coverage in the case where the incident light is inclined at 0 degrees, 10 degrees, and 20 degrees. As shown in fig. 2, when no graphene is present in the sensor, the absorption intensity of the entire sensor is very low, but the resonance position is substantially the same as when the sensor has graphene. In general, the presence or absence of graphene has little influence on the resonance position in the absorption spectrum, but the presence of graphene has a very important influence on the absorption intensity of the absorption spectrum, especially at the right resonance peak position, the absorption intensity is improved from 54.1% to 99.3%. Therefore, although the single-layer graphene has low absorption in the near infrared band, the combined action of the single-layer graphene and the sub-wavelength grating can obviously improve the absorption intensity, so that the detection sensitivity of the sensor is finally improved. Meanwhile, when the incident angle of light is changed from 0 to 20 degrees, the resonance peak change amplitude of the sensor with graphene is significantly smaller than that of the sensor without graphene, which means that the sensor with graphene can maintain a high absorptivity more than the sensor without graphene when the incident angle is changed from 0 to 20 degrees.
Fig. 3 is an absorption spectrum diagram of the resonant peak of the optical sensor when the refractive index of the substance to be measured changes under the condition that the light is fixed to be vertically incident, and the refractive indexes of the corresponding detection substances are 1.331, 1.336, 1.341, 1.346 and 1.361. As can be seen from fig. 3, the change of the refractive index of the detection material causes a shift of the center wavelength of the output spectrum of the sensor, i.e. the center wavelengths of the resonance peaks corresponding to the substances to be detected with different refractive indexes are different. As can be clearly seen from fig. 3, the center wavelengths of resonance peaks corresponding to the substances to be detected with refractive indexes of 1.331, 1.336, 1.341, 1.346 and 1.361 are obviously different, so that the optical detection of the substances to be detected can be realized, and the optical absorption rate sensing can be realized. The resonance peak sensitivity was calculated to be 320nm/RIU.
Fig. 4 is an evolutionary absorption spectrum of a resonance peak of the optical sensor when an incident angle of incident light is changed. In a practical use environment, there may be difficulties in accurately controlling the angle of incidence of light, which requires the angular insensitivity of the sensor. With reference to fig. 2 and 4, the presence or absence of the graphene layer has an important effect on the resonance intensity, and when the light incidence angle is changed from 0 degrees to 20 degrees, the change amplitude of the sensor with graphene is significantly smaller than that of the sensor without graphene. This means that the graphene biosensor provided by the invention has a linear change in absorption intensity while maintaining a high absorption rate in the process of changing the whole angle from 0 degrees to 20 degrees. As can be seen from fig. 4, the graphene biosensor provided by the present invention still maintains 95% absorptivity when incident light is obliquely incident at an incident angle of 20 degrees.
In summary, the graphene biosensor based on the double-layer sub-wavelength grating provided by the invention has the technical advantages that:
(1) The graphene biosensor provided by the invention combines the advantages of the sub-wavelength grating and graphene, and realizes high-sensitivity detection of detection substances;
(2) According to the invention, the detection channel and the light incidence channel are separated and are vertically arranged, so that the interference between light and detection substances is effectively reduced, the substances to be detected cannot directly contact the laser, the possible reaction is avoided, and the anti-interference performance of the sensor is improved;
(3) The graphene biosensor provided by the invention can detect the refractive index change of a substance through the drift change of the resonance peak, so that the liquid or gas absorptivity is sensed.
(4) The graphene biosensor provided by the invention can also maintain 95% of light absorptivity at an incident angle of 20 degrees, and the light absorptivity maintains high absorptivity and change linearity in the change process of the incident angle from 0 degrees to 20 degrees. Even if the incident light is inclined to 20 degrees, the sensor can still have better absorptivity for the incident light. This means that the sensor requires little light incidence angle in practical use.
Finally, it should be noted that: the above embodiments are only for illustrating the technical solution of the present invention, and are not limiting; although the invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical scheme described in the foregoing embodiments can be modified or some technical features thereof can be replaced by equivalents; such modifications and substitutions do not depart from the spirit and scope of the technical solutions of the embodiments of the present invention.
Claims (5)
1. Graphene biosensor based on double-layer sub-wavelength grating, which is characterized by comprising:
an upper sub-wavelength grating (1) and a lower sub-wavelength grating (2); the two sub-wavelength gratings are arranged in mirror symmetry, and an intermediate gap formed by the two sub-wavelength gratings forms a detection material channel (3);
the inner surfaces of the upper sub-wavelength grating (1) and the lower sub-wavelength grating (2) are respectively provided with a graphene layer (4);
the detection substance flows in a horizontal direction through the detection substance channel (3), and the direction of light rays incident to the upper sub-wavelength grating (1) is perpendicular to the direction of the detection substance channel (3);
the upper sub-wavelength grating (1) comprises: the graphene layer (4) is respectively arranged on the upper waveguide layer (11) and the upper grating layers (12);
the lower sub-wavelength grating (2) comprises: a lower waveguide layer (22) and a plurality of lower grating layers (21) arranged on the lower waveguide layer (22), wherein the graphene layers (4) are respectively arranged on the lower waveguide layer (22) and the lower grating layers (21);
a silver substrate (5) is arranged on the bottom surface of the outer side of the lower sub-wavelength grating (2);
the thickness of the upper grating layer (12) and the lower grating layer (21)d g All 220nm in widthW=357 nm; the thicknesses of the upper waveguide layer (11) and the lower waveguide layer (22) are respectivelyL=2235 nm; width of detecting material channel (3)H=2000nm。
2. The dual-layer sub-wavelength grating-based graphene biosensor of claim 1, wherein a single period of the dual-layer sub-wavelength grating structureP=960nm。
3. The graphene biosensor based on double-layer sub-wavelength gratings according to claim 1, wherein the upper grating layer (12) and the lower grating layer (21) are Si with a refractive index of 3.48, and the upper waveguide layer (11) and the lower waveguide layer (22) are silicon dioxide with a refractive index of 1.46.
4. The graphene biosensor based on a bilayer sub-wavelength grating according to claim 1, wherein the graphene layer (4) has a thickness of 0.34nm.
5. The graphene biosensor based on double-layer sub-wavelength gratings according to claim 1, wherein the thickness of the silver substrate (5) is 100nm.
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