CN110389110B - Dielectric nanometer light wave antenna sensor based on rod-ring structure and application - Google Patents
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- 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
- G01N21/01—Arrangements or apparatus for facilitating the optical investigation
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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
- G01N21/41—Refractivity; Phase-affecting properties, e.g. optical path length
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Abstract
The invention discloses a rod-ring structure-based dielectric nano lightwave antenna sensor, which takes a material mainly containing silicon dioxide as a substrate, wherein a silicon layer of a rod-ring structure is arranged on the substrate in a periodic array manner, and a peak can be obtained in a transmission/reflection spectral line for incident light with a wavelength range of 600 nm-2500 nm. The invention utilizes the polar resonance characteristic that the dielectric material can be polarized and generate internal displacement current under the irradiation of incident light, can indirectly detect the change of the environmental refractive index, and is further used for detecting water pollutants. And the low-loss characteristic can obtain larger local field enhancement and simultaneously avoid the damage of stronger light thermal effect on the sensing marker molecules, and the composition and the concentration of the protein molecules to be detected can be reversely deduced through resonant wavelength obtained through detection through early calibration and later comparison.
Description
Technical Field
The invention relates to an optical sensing nano device, in particular to a rod-ring structure-based dielectric nano lightwave antenna sensor and application thereof.
Background
In recent years, the problem of water pollution has been increasingly emphasized and emphasized. As for trace pollutants in water, the concentration of the trace pollutants is extremely low, the components of the water in nature are very complex, and a plurality of different complex components easily cause great interference on the detection of a target object, so that the direct detection of the pollutants is difficult.
An effective solution is to use organisms in the water to indirectly detect water pollution. However, this method requires the participation of organisms, and it is difficult to screen suitable biological proteins for indirect detection in the early stage. Taking specific biological marker acetylcholinesterase in fish protein as an example, when a certain amount of pesticide residue exists in the water body, the activity of the acetylcholinesterase changes, and if the acetylcholinesterase can be monitored, the pesticide residue condition in the water body can be obtained.
The other idea is to screen and separate the micro-pollutants to be detected in the polluted water body by a specific means and perform directional detection under the condition of removing other interfering substances in the water body. In the field of optical wave antenna biosensing, a common method is to use local surface plasmon resonance of a metal optical wave antenna, but the resonance is easy to generate strong absorption to light, high temperature is formed in a local area, if biological detection is carried out by combining an antibody antigen, the activity of the antigen antibody protein is easy to damage, the existing activity of the protein is influenced, and most metals have toxicity to the protein.
In summary, no simple, efficient and nontoxic method for directionally monitoring the protein molecules of the trace pollutants to be detected in the polluted water body exists at present.
Disclosure of Invention
Aiming at the defects and shortcomings of the prior art, the invention provides a nano lightwave antenna structure based on a dielectric material by utilizing the polar resonance characteristic that the dielectric material can be polarized and generate internal displacement current under the irradiation of incident light.
The invention also provides a method for detecting protein molecules by using the sensor, and the method has higher sensitivity and better detection precision.
The invention also provides a device for detecting the protein molecules, and the device can be used for conveniently and rapidly detecting the protein molecules.
Meanwhile, the sensor with the structure can indirectly detect the change of the environmental refractive index, and is further used for detecting protein molecules to realize water pollution assessment.
A dielectric nanometer light wave antenna sensor based on a rod-ring structure takes a material mainly containing silicon dioxide as a substrate, a silicon layer of the rod-ring structure is arranged on the substrate in a periodic array mode, and a peak can be obtained in a transmission/reflection spectral line for incident light with the wavelength range of 600 nanometers to 2500 nanometers.
Preferably, the substrate is a quartz plate substrate, and the thickness of the quartz plate substrate is greater than or equal to 100 micrometers.
The technical scheme of the invention is that a quartz plate is used as a substrate, a silicon layer is evaporated on the substrate, and the device is prepared into a periodic array of a rod-ring structure. The device can obtain a relatively sharp peak in the transmission/reflection spectral line under the irradiation of a light source with vertical incidence. The sensor of the present invention can be used to achieve trace biochemical molecule concentrations in a sample (such as a contaminated water source) by shifting the peak wavelength in the transmission/reflection line in the environment.
Preferably, each rod-loop structure comprises an oblong rod structure and a loop structure: the long side of the rectangular rod structure is 300 nanometers to 1 micron, and the short side is 50 nanometers to 200 nanometers along the y direction; the outer circle radius of the ring structure is 100 nanometers to 1 micron, the inner circle radius is 50 nanometers to 150 nanometers, and the inner circle radius is smaller than the outer circle radius; the period of the periodic array of the rod-ring structures in the x direction and the period of the periodic array of the rod-ring structures in the y direction are both 300 nanometers to 1 micron.
Preferably, the rectangular rods in each rod-ring structure have a center located at a distance of 300 to 450nm from the center of the ring.
As a further preference, each rod-ring structure comprises an oblong rod and ring: the long side of the rectangular rod is 650-800 nm, and the short side is 100-200 nm along the y direction; the outer circle radius of the ring is 150 nm-300 nm, and the inner circle radius is 90 nm-130 nm; the period of the bar-ring structure in the x direction and the period of the bar-ring structure in the y direction are both 650-850 nm, and the distance from the center of the rectangular bar to the center of the ring is 350-400 nm.
As a specific preferred scheme, the long side of the rectangular rod structure in each rod-ring structure is 720 nm, and the short side along the y direction is 150 nm; the outer circle radius of the ring structure is 225 nanometers, and the inner circle radius is 110 nanometers; the periodic array of rod-ring structures has a period of 750 nanometers in both the x-direction and the y-direction. That is, a plurality of rod-ring structures are uniformly spaced along a distance of 750 nanometers in the x-direction and the y-direction. The rectangular rod structure center in each rod-ring structure was 380 nm from the ring structure center.
Preferably, the basic structure material of the quartz plate substrate is silicon dioxide, the thickness of the silicon dioxide is more than or equal to 100 micrometers, and preferably, the thickness of the substrate is 200-1000 micrometers; the structure height of the upper silicon layer is 50 nanometers to 1 micron.
In the invention, the incident light source is a wide-spectrum light source, and the wavelength range is 600 nm-2500 nm. The signal light of the transmission/reflection spectral line is received by a spectrometer, and the working waveband of the spectrometer is 600-2500 nm.
The sensor can be used for detecting protein molecules, such as common acetylcholinesterase in water pollutants, and can evaluate the water quality through the concentration measurement of the acetylcholinesterase. The sensor of the invention can be used in the field of monitoring water body pollution mainly through the light response change after being combined with protein. It is also possible to respond to such as serum proteins, antibody proteins, etc. for high-precision measurement in the biomedical field.
A method for detecting protein molecules by using the rod-ring structure-based dielectric nano lightwave antenna sensor is characterized in that a sample containing protein molecules is dripped on a periodic array silicon layer of the rod-ring structure, incident light with the wavelength range of 600 nm-2500 nm is vertically incident, the wavelength of a target measurement peak in a transmission/reflection spectral line is determined, the wavelength moving distance between the target measurement peak and a target measurement peak corresponding to a standard reference substance is calculated, and a detection result is obtained.
Preferably, the concentration of the protein molecules in the sample to be detected is 5% to 15%.
The principle of the concentration detection process is that the dielectric nano antenna can generate electromagnetic resonance under the irradiation and excitation of a light source, the periodic array of the rod-ring structure is based on the Fano resonance design, electric resonance and magnetic resonance can be simultaneously excited, and a relatively sharp peak can be obtained in a transmission/reflection spectral line after the electric resonance and the magnetic resonance interact with each other. The peak wavelength of the detection peak is sensitive to the change of the environmental refractive index, and the change of the environmental refractive index caused by concentration can be converted into visible peak wavelength movement by placing the device in environments with different concentrations. The concentration can be obtained according to the difference of the moving distance. Before detection, the relationship between the concentration of a certain component and the change in wavelength (wavelength shift) can be generally calibrated, and the relationship between the two can be predetermined. And the relation is prestored in a detection system, and the concentration value can be directly obtained by using the obtained wavelength shift value during detection. Preferably, before detection, a plurality of standard reference substances with known concentrations are calibrated in advance, the relationship between the mass percentage concentration of the protein molecules and the moving distance data of the target measurement peak is determined, and after the moving distance data is obtained in actual detection, the mass percentage concentration of the protein molecules in the sample to be detected is directly obtained by using the relationship between the mass percentage concentration of the protein molecules and the moving data of the target measurement peak.
The rod-ring structure dielectric nanometer lightwave antenna provided by the invention is mainly applied to two aspects: (1) the advantages of high-quality resonance, low local temperature increase during strong field enhancement and strong biological and process compatibility of the dielectric nano antenna can realize high-precision detection of trace protein molecules. (2) Through the calibration in the early stage and the comparison in the later stage, the composition and the concentration of the protein molecules to be detected can be reversely deduced through the resonance wavelength obtained through detection.
The device for detecting protein molecules comprises an incident light emitter, a receiver, a sensor for detecting samples and a spectrometer, wherein the sensor is a rod-ring structured dielectric nanometer light wave antenna sensor in any technical scheme.
The invention relates to a rod-ring structure-based dielectric nanometer lightwave antenna sensor, which belongs to the field of lightwave antenna biosensing. The invention utilizes the polar resonance characteristic that the dielectric material can be polarized and generate internal displacement current under the irradiation of incident light, can indirectly detect the change of the environmental refractive index, and is further used for detecting water pollutants. And the low-loss characteristic can obtain larger local field enhancement and simultaneously avoid the damage of stronger light thermal effect on the sensing marker molecules, and the composition and the concentration of the protein molecules to be detected can be reversely deduced through resonant wavelength obtained through detection through early calibration and later comparison.
The invention has the advantages that: the dielectric nano antenna has extremely low loss, and can realize high-quality factor resonance, thereby improving the sensing sensitivity. The low loss characteristic can obtain larger local field enhancement and simultaneously avoid the damage of stronger photothermal effect on the sensing marker molecules. The control of the radiation direction can be realized by regulating and controlling the electric resonance and the magnetic resonance coupling of the antenna, and the collection efficiency is favorably improved so as to improve the sensing sensitivity. The dielectric nano antenna is usually based on silicon, has excellent biocompatibility, is compatible with a microelectronic complementary metal oxide semiconductor process in preparation, and can be prepared in a large area and at low cost. According to the preliminary study of the surface, the local refractive index change in the molecule combination process is detected by adopting the electromagnetic resonance of the dielectric nano antenna, and the sensitivity of the sensor can be improved by at least one order of magnitude compared with a sensor based on metal surface plasma resonance.
Drawings
FIG. 1(a) is a schematic perspective view of a rod-ring structure-based dielectric nanoantenna sensor according to the present invention;
FIG. 1(b) is a front view of the sensor of FIG. 1 (a);
FIG. 2 is a scanning electron microscope image of the rod-ring structure based dielectric nano-antenna sensor according to the embodiment;
fig. 3 is a reflection simulation curve of the rod-ring structure based dielectric nano-antenna sensor according to the embodiment.
Fig. 4 is a graph of the detection result of the rod-loop structure-based dielectric nano-antenna sensor for different concentrations of serum protein molecules.
Detailed Description
The following detailed description of embodiments of the invention refers to the accompanying drawings in which: the present embodiment is premised on the rod-ring structure dielectric nano antenna proposed in the present invention, but the scope of the present invention is not limited to the following embodiments and examples.
As shown in fig. 1(a) and 1(b), a rod-ring structure based dielectric nano lightwave antenna sensor comprises a substrate, a plurality of rod-ring structures arranged in a periodic array on the top surface of the substrate, wherein each unit of the rod-ring structures is composed of a rectangular rod and a circular ring, the rectangular rod plays a role of exciting a 'bright mode' (i.e. electric resonance) and the circular ring plays a role of exciting a 'dark mode' (i.e. magnetic resonance).
In this example, the long side of the rectangular rod structure in each rod-ring structure is 720 nm, along the y-direction, and the short side is 150 nm, along the x-direction; the outer circle radius of the ring structure is 225 nanometers, and the inner circle radius is 110 nanometers; the periodic array of rod-ring structures has a period of 750 nanometers in both the x-direction and the y-direction. That is, a plurality of rod-ring structures are uniformly spaced along a distance of 750 nanometers in the x-direction and the y-direction. The rectangular rod structure center in each rod-ring structure was 380 nm from the ring structure center.
In this embodiment, the basic structural material of the quartz substrate is silicon dioxide, the thickness is greater than 100 micrometers, the thickness in this embodiment is 500 micrometers, the structural height of the upper silicon layer is 50 nanometers to 1 micrometer, and the height of the upper silicon layer is 220 nanometers.
Under the irradiation of a light source with vertical incidence, the sensor in the embodiment can obtain a relatively sharp peak in the transmission/reflection spectral line. The concentration of trace protein molecules in the contaminated water source is obtained by shifting the peak wavelength in the transmission/reflection line in the environment.
The light source in this embodiment is a broad spectrum light source with a wavelength range of 600 nm to 2500 nm. The signal light of the transmission/reflection spectral line is received by a spectrometer, and the working waveband of the spectrometer is 600-2500 nm.
When the polarization direction of incident light is parallel to the long side of the rectangular rod and the wavelength of the incident light is in a specific wavelength region (i.e., in the vicinity of twice the optical length of the long side of the rectangular rod), the incident light forms electrical resonance in the rectangular rod. Due to the inherent field enhancement characteristic of the electrical resonance, a near field with a large electric field strength is generated around the rectangular rod. A ring-shaped structure is placed within the near-field active region of the rod, and a ring-shaped magnetic resonance is induced in the disk-shaped structure by the near-field generated by the rod. Because the magnetic resonance is caused by the near field of the rectangular rod, the vibration direction of the electric field of the rectangular rod is inconsistent with the direction of the incident electromagnetic field, so the interaction between the resonance in the disk and the outside is small, the coupling loss is small, and the disk can be used as a 'dark mode'. The 'bright mode' generated in the rod and the 'dark mode' generated in the ring interact with each other, and the sharp spectral line of the Fano resonance can be obtained. When the rod-ring structures are arranged periodically, the characteristic peak of the final Fano resonance spectrum is further enhanced.
As shown in fig. 2, which is a scanning electron microscope image of the dielectric nano antenna sensor based on the rod-ring structure in this embodiment, the rod-ring structure needs to etch a surface silicon layer in the preparation process, so that the requirement for etching is high, the rod-ring structure can be etched by using the existing reactive ion etching process, after etching, the disc structure in the effective region is a silicon layer, and the rest surfaces are silicon oxide layers.
As shown in fig. 3, the rod-ring structure in this embodiment has a plurality of curve peaks (shown in (a)) near 1080 nm, near 1225 nm, near 1275 nm, near 1430 nm, and near 1475 nm in the near infrared band, and each of the curve peaks is shifted to a certain degree in red as the ambient refractive index changes from 1.332 to 1.352 (shown in (b)). And considering the quality factor, the difference value of the peak and the valley value and the red shift speed generated along with the change of the environmental refractive index, and selecting the peak near 1475 nanometers as the target measurement peak of the structure.
As shown in FIG. 4, the reflection spectra of the rod-loop structure in the present example were obtained in the serum protein solutions with 0%, 5%, 10% and 15% by weight, respectively, of air as a blank. It can be seen that the reflection spectrum moves towards the direction of lengthening the wavelength along with the increase of the concentration of serum protein in the solution, and the mass fraction change of one percent can generate the spectrum movement of 10nm through measurement and calculation, so that the precision is higher.
During actual detection, a sample with standard mass concentration can be calibrated in advance, the position of a detection peak is determined, the relation between mass fraction change and detection peak movement data is established, and then during actual detection, the mass percentage content of the component to be detected in the sample can be directly obtained by using the obtained detection peak movement data and the established relation between mass fraction change and detection peak movement data.
Claims (8)
1. A dielectric nanometer light wave antenna sensor based on a rod-ring structure is characterized in that a material mainly containing silicon dioxide is used as a substrate, a silicon layer of the rod-ring structure is arranged on the substrate in a periodic array mode, and a peak can be obtained in a transmission/reflection spectral line for incident light with the wavelength range of 600 nm-2500 nm;
each rod-ring structure comprises a rectangular rod and ring: the long side of the rectangular rod is 650-800 nm, and the short side is 100-200 nm along the y direction; the outer circle radius of the ring is 150 nm-300 nm, and the inner circle radius is 90 nm-130 nm; the period of the bar-ring structure in the x direction and the period of the bar-ring structure in the y direction are both 650-850 nm, and the distance from the center of the rectangular bar to the center of the ring is 300-450 nm.
2. The rod-ring structure based dielectric nano lightwave antenna sensor according to claim 1, wherein the distance from the center of the rectangular rod to the center of the ring is 350 to 400 nm.
3. The rod-ring structure based dielectric nano lightwave antenna sensor of claim 1, wherein the silicon layer has a height of 50nm to 1 μm.
4. The rod-ring structure based dielectric nano lightwave antenna sensor as claimed in claim 1, wherein the substrate is a quartz plate substrate with a thickness of 100 μm or more.
5. A method for detecting the concentration of protein molecules by using the sensor as claimed in any one of claims 1 to 4, wherein a sample to be detected containing protein molecules is dripped on the periodic array silicon layer of the rod-ring structure, the incident light with the vertical incident wavelength range of 600 nm to 2500 nm is used, the wavelength of a target measurement peak in a transmission/reflection spectral line is determined, and the moving distance data of the wavelength between the target measurement peak and a target measurement peak corresponding to a standard reference substance is calculated to obtain a detection result.
6. The method for detecting the concentration of the protein molecules by using the sensor as claimed in claim 5, wherein the concentration of the protein molecules in the sample to be detected is 5% -15%.
7. The method for detecting the concentration of protein molecules by using the sensor as claimed in claim 5, wherein before detection, a plurality of standard reference substances with known concentrations are calibrated in advance to determine the relationship between the mass percentage concentration of the protein molecules and the moving distance data of the target measurement peak, and during actual detection, after the moving distance data is obtained, the mass percentage concentration of the protein molecules in the sample to be detected is directly obtained by using the relationship between the mass percentage concentration of the protein molecules and the moving data of the target measurement peak.
8. A device for detecting the concentration of protein molecules, which comprises an incident light emitter, a receiver, a sensor for detecting a sample and a spectrometer, and is characterized in that the sensor is a rod-ring structured dielectric nanometer light wave antenna sensor as claimed in any one of claims 1 to 4.
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