CN115389452A - Light-operated terahertz biosensor, preparation method thereof and detection spectrum system - Google Patents
Light-operated terahertz biosensor, preparation method thereof and detection spectrum system Download PDFInfo
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Abstract
The invention provides a light-operated terahertz biosensor, a preparation method thereof and a detection spectrum system, relating to the field of biomedical detection and comprising the following steps: the device comprises a substrate, and a dielectric material and a super-surface structure which are integrated on the substrate; the terahertz wave super-surface structure comprises a substrate, a dielectric material, a super-surface structure and a cutting wire, wherein the substrate is made of a terahertz wave high-transmittance material, the dielectric material is made of a semiconductor material, and the super-surface structure is an array structure formed by a plurality of metal resonators and the cutting wire; lattice resonance structures are formed among the metal resonators, lorentz resonance structures are formed among the cutting wires, and the lattice resonance structures and the Lorentz resonance structures are coupled to form Lorentz-lattice resonance modes; the dielectric material is integrated between the cutting wires to connect the pair of cutting wires, so that the Lorentz-lattice mode is switched into the EIT mode within a picosecond range by means of the ultrafast carrier excitation and relaxation process of the dielectric material. The invention realizes the high-sensitivity quantitative and qualitative detection of the micro biological substances and has the advantages of portability, high integration degree and the like.
Description
Technical Field
The invention relates to the field of biomedical detection, in particular to a light-operated terahertz biosensor, a preparation method of the light-operated terahertz biosensor and a terahertz detection spectrum system.
Background
The terahertz wave is positioned between a millimeter wave band and an infrared wave band and has the characteristics of photonics and electronics. Terahertz waves are a potential tool in the biomedical field because of the characteristics of non-ionization, no damage, high penetration, high resolution, spectral fingerprints and the like. With the rapid development of the sensor in the field of biological substance detection, terahertz sensing has become a promising technology in biomedical research and substance detection. However, terahertz waves have not been widely used in substance detection due to the lack of a terahertz source having a high radiation intensity and the mismatch between the wavelength of the terahertz wave and the size of an analyte.
Micro-nano photonics hopefully exploits the strong near-field enhancement effect of sub-wavelength resonant structures to break this limitation. The sub-wavelength resonance structure can control the polarization, phase, amplitude and the like of light, and can be used for light emission, detection, modulation, control and amplification of micro-nano scale. Near-field enhancement of the optical field at the microstructure can promote the interaction of light with the substance. Therefore, the terahertz spectrum technology based on the super-surface micro-nano structure becomes a promising method for detecting biochemical substances. However, the conventionally designed super-surface micro-nano structure can only provide a single-mode state with a fixed resonance peak position, and the requirement of ultra-high sensitivity is difficult to meet in the detection and identification of trace biological substances.
The following defects still exist in the prior biological qualitative detection by the technology:
first, qualitative detection is achieved by designing a single microstructure such that its resonance peak position overlaps with a single fingerprint of the analyte. The response of the microstructure is designed according to a certain characteristic fingerprint spectrum known by the analyte, and a single peak position can only be used for detecting a single target. If more substances are to be detected, only the structural parameters of the sensor can be changed, and more sensors can be processed according to the structural parameters. This is far from meeting the development requirements of fast, convenient, small-sized and highly integrated sensor devices, and severely limits the wide application of sensors in practice.
Secondly, designing a single mode microstructure for quantitative detection of trace biological substances. The resonance response of the microstructure has strong dependence on the change of the refractive index of the environment medium, so that the thickness, the density and the like of an analyte can directly influence the response of the microstructure. Therefore, it is now very difficult to detect the frequency shift and amplitude difference of the resonance peak position of different doses of trace species in experimental procedures.
Thirdly, the metamaterial is combined with the detection application of ultrafast optics in the biomedical field. The metamaterial provides a strong local field for detecting micro or trace substances, and enhances the full effect of light and substances; the application of ultrafast optics in the optical field is rapidly developed but the research application in the biomedical field is almost blank.
Fourthly, the single-mode resonance structure is used for data processing after biological detection, and actually measured information needs to be subjected to Fourier transform processing. In the conventional application of the prior art, ideal data can be obtained by performing Fourier transform on substance detection information from a time-domain signal and performing complex data processing. The complex processing procedure greatly limits the application of biosensors to the detection of bulk materials.
Therefore, how to further improve the existing terahertz detection system to realize ultra-sensitive detection of the tiny biological substances becomes a technical problem to be solved.
Disclosure of Invention
The invention aims to at least solve one of the technical problems in the prior art or the related technology, and provides a light-operated terahertz biosensor, a preparation method thereof and a detection spectrum system.
A first aspect of the present invention provides an optically controlled terahertz biosensor, including: the device comprises a substrate, and a dielectric material and a super-surface structure which are integrated on the substrate; the terahertz wave super-surface structure comprises a substrate, a dielectric material, a super-surface structure and a cutting wire, wherein the substrate is made of a terahertz wave high-transmittance material, the dielectric material is made of a semiconductor material, and the super-surface structure is an array structure formed by a plurality of metal resonators and the cutting wire; lattice resonance structures are formed among the metal resonators, lorentz resonance structures are formed among the cutting wires, and the lattice resonance structures and the Lorentz resonance structures are coupled to form Lorentz-lattice resonance modes; the dielectric material is arranged between the cutting wires to connect the pair of cutting wires, so that the Lorentz-lattice mode is switched into an EIT (Electromagnetic Induced Transparency) mode in a picosecond range by means of an ultrafast carrier excitation and relaxation process of the dielectric material.
According to the light-operated terahertz biosensor provided by the invention, preferably, the super-surface structure is a plurality of unit structures which are periodically arranged, and each unit structure comprises two pairs of metal resonators and a pair of cutting wires; the metal resonator is a square opening resonator; the openings of the two metal resonators are oppositely arranged to form a pair of metal resonators; two pairs of metal resonators arranged up and down in the same plane are separated by a pair of cutting wires.
According to the light-operated terahertz biosensor provided by the invention, the cutting wires are preferably connected through a silicon bridge.
According to the light-operated terahertz biosensor provided by the invention, preferably, the metal resonator is made of any one of gold, silver or aluminum.
According to the light-operated terahertz biosensor provided by the invention, preferably, the dielectric material is silicon or germanium.
The second aspect of the invention provides a preparation method of a light-operated terahertz biosensor, which comprises the following steps: cleaning the sapphire substrate silicon by using acetone and isopropanol; preparing a metal super-surface structure; constructing a silicon pattern by combining an alignment lithography technology and a silicon deep etching technology to complete secondary pattern transfer; wherein, the super surface structure of metal is a plurality of unit structures of periodic arrangement, and every unit structure includes: two pairs of open square resonators, and two cut wires connected by a semiconductor material.
In the technical scheme, the specific layout of the metal super-surface structure comprises: each unit structure comprises two pairs of metal resonators and a pair of cutting wires; the metal resonator is a square opening resonator; the openings of the two metal resonators are oppositely arranged to form a pair of metal resonators; two pairs of metal resonators which are arranged up and down in the same plane are separated by a pair of cutting wires; the semiconductor material is integrated between the two cutting wires to form a pair of cutting wires.
According to the preparation method of the light-operated terahertz biosensor provided by the invention, preferably, the sapphire substrate silicon specifically comprises an epitaxial silicon layer with the thickness of 600nm and a sapphire substrate with the thickness of 460 nm.
According to the preparation method of the light-operated terahertz biosensor, preferably, a metal super-surface structure is prepared on the titanium and the gold film by adopting a step photoetching method and an ion beam etching method, and specifically, the thickness of the titanium is 10nm, and the thickness of the gold film is 160nm.
A third aspect of the present invention provides a terahertz detection spectroscopy system, including: the optical control terahertz biosensor comprises a femtosecond laser, a beam splitter and the optical control terahertz biosensor disclosed by any one of the technical schemes; wherein the femtosecond laser is used for generating femtosecond laser; the beam splitter is used for splitting the femtosecond laser to form terahertz light, terahertz detection light and pumping light; the pump light is used for realizing the excitation of photo-carriers; the terahertz detection light is used for testing and recording transmission spectral lines of the front and rear super surfaces into which the pump light is incident.
The beneficial effects obtained by the invention at least comprise: the application of the ultrafast optics can provide possibility for the ultrafast surface micro-nano structure to complete the fast switching of the resonance peak position in the ultrafast time so as to realize the bimodal or even multimodal detection, and further can greatly improve the detection sensitivity, specifically, when a detected substance moves to an ultrafast surface interface to cause the tiny dielectric constant of a medium layer to change, the coupling state of resonance is changed according to the difference of the sensitivities of two resonance structures, the obvious change can be found and recorded through a terahertz time-domain signal in the experimental process, compared with the mode that the final result can be obtained only by carrying out complicated data processing such as Fourier transform and the like in the prior art, the light-operated terahertz sensor has the advantages of more sensitive detection result, more convenient and simpler use, avoiding the follow-up complicated data processing such as Fourier transform and the like, and providing a new method for the high-sensitivity detection.
Drawings
Fig. 1 shows a schematic structural diagram of an optically controlled terahertz biosensor according to an embodiment of the invention.
Fig. 2 shows transmission spectra of a light-controlled terahertz biosensor according to an embodiment of the present invention at different pump energies.
Fig. 3 shows transmission spectra of a light-controlled terahertz biosensor according to an embodiment of the present invention with different silicon conductivities.
Fig. 4 shows a transmission spectrum of the light-controlled terahertz biosensor according to an embodiment of the present invention with a pump light detection time delay between-2 ps to 32 ps.
Fig. 5 shows a transmission spectrum of the light-controlled terahertz biosensor according to an embodiment of the present invention with a pump light detection time delay between 32ps and 162 ps.
FIG. 6 shows a schematic optical path diagram of a terahertz detection spectroscopy system according to an embodiment of the invention.
FIG. 7 is a schematic diagram illustrating a cell structure of a super-surface structure according to an embodiment of the present invention.
Detailed Description
In order that the above objects, features and advantages of the present invention can be more clearly understood, a more particular description of the invention, taken in conjunction with the accompanying drawings and detailed description, is set forth below. To simplify the disclosure of the present invention, the components and arrangements of specific examples are described below. Moreover, the present disclosure may repeat reference numerals and/or letters in the various examples. This repetition is for the purpose of simplicity and clarity and does not in itself dictate a relationship between the various embodiments and/or configurations discussed. It should be noted that the components illustrated in the figures are not necessarily drawn to scale. Descriptions of well-known components and processing techniques and processes are omitted so as to not unnecessarily limit the invention.
As shown in fig. 1, according to an embodiment of the present invention, there is disclosed an optically controlled terahertz biosensor, including: a substrate 1, and a dielectric material 2 and a super-surface structure integrated on the substrate; the terahertz wave super-surface structure comprises a substrate, a dielectric material, a plurality of metal resonators 3 and cutting wires 4, wherein the substrate is made of a terahertz wave high-transmittance material, the dielectric material is made of a semiconductor material, and the super-surface structure is an array structure formed by the metal resonators 3 and the cutting wires 4; lattice resonance structures are formed among the metal resonators, lorentz resonance structures are formed among the cutting wires, and the lattice resonance structures and the Lorentz resonance structures are coupled to form Lorentz-lattice resonance modes; the dielectric material is integrated between the cutting wires to connect the pair of cutting wires, so that the Lorentz-lattice mode is switched into the EIT mode within picoseconds by means of the ultrafast carrier excitation and relaxation process of the dielectric material.
In the embodiment, after pump light is injected into the light-controlled terahertz biosensor, due to the ultrafast carrier excitation and relaxation processes of the dielectric material, the physical interval between the two cutting wires is opened, so that the resonance mode of the super surface is switched from a Lorentz-lattice mode to an Electromagnetic Induced resonance (EIT) mode within a picosecond range, the detection application of two tunable modes on the basis of the same structure under the light-controlled condition is realized, the single-mode microstructure designed on the traditional super surface is broken, and the light-controlled terahertz biosensor has the advantages of high sensitivity, strong portability, high integration degree and the like. The sensing mode and the function are quickly switched, so that the ultra-sensitive and quick detection of the double-mode state of the biological substance is realized. The respective frequency spectrum positions of the two modes are mainly related to the respective sizes of the two pairs of open square resonators, the two cutting wires and the dielectric material, the distance between the three and the distance between the unit array structures; and the conversion time of the two modes depends on the property of ultrafast carrier excitation and relaxation of the medium material. The ultrafast carrier excitation and relaxation characteristics of the dielectric material provide a foundation for ultrafast switching under the light control condition, and meanwhile, the miniaturization of the light-controlled terahertz biosensor is greatly promoted. Pumping light is utilized to drive in and then along with the excitation of the ultrafast current carrier of the dielectric material, a physical gap between two parting lines connected with the dielectric material is opened, so that the resonance mode of the super-surface structure is rapidly switched within a picosecond range. Meanwhile, the two tunable modes can be rapidly switched under the light control condition on the basis of the same structure, the detection efficiency is greatly improved by dual-mode detection, and a new thought is provided for the miniaturization and integration design of the super-surface micro-nano structure.
According to the above embodiment, preferably, the super-surface structure is a plurality of unit structures arranged periodically, each unit structure including two pairs of metal resonators and one pair of cut wires; the metal resonator is a square opening resonator; the openings of the two metal resonators are oppositely arranged to form a pair of metal resonators; two pairs of metal resonators arranged up and down in the same plane are separated by a pair of cutting wires.
In this embodiment, coupling a Lorentz mode composed of a plurality of two dividing line (cut wire) array structures and a lattice mode composed of a plurality of two pairs of split square resonator array structures realizes a Lorentz-lattice resonance mode. When a detected substance moves to a super-surface interface to cause the change of a tiny dielectric constant of a dielectric layer, the change of a resonance coupling state is caused according to the difference of the sensitivities of two resonance structures, obvious changes can be found and recorded through a terahertz time-domain signal in an experimental process, subsequent complex data processing such as Fourier transform and the like is omitted, and a new method is provided for high-sensitivity detection.
According to the above embodiments, it is preferable that a silicon bridge connection is used between the dicing wires.
According to the above embodiments, preferably, the metal resonator is made of any one of gold, silver, or aluminum.
According to the above embodiment, preferably, the dielectric material is silicon or germanium.
According to the above embodiment, preferably, fig. 7 shows that one implementation manner of specific parameters of each unit structure in the super-surface structure is as follows: a =10 μm, b =18 μm, c =26 μm, d =32.5 μm, e =9 μm, and P =83 μm, and the above parameters are the optimal schemes for satisfying the fast switching between the Lorentz-lattice resonance mode and the electronically Induced resonance (EIT) resonance mode after repeated simulation and calculation.
According to another embodiment of the invention, a preparation method of the light-controlled terahertz biosensor corresponding to the embodiment is disclosed:
1) And cleaning the sapphire substrate silicon by using acetone and isopropanol to remove surface dust. Wherein the sapphire substrate silicon includes: a 600nm epitaxial silicon layer and a 460nm sapphire substrate.
2) A metal superstructure (metal super-surface structure) is prepared. The superstructure is a plurality of unit structures (shown in fig. 1) arranged periodically. The unit structure includes: two pairs of open square resonators with the openings of the square resonators facing each other, and two dicing wires connected by a semiconductor material. The cut wires are connected using a silicon bridge (dielectric material).
In this step, a metal superstructure is prepared on the titanium and gold films using step lithography and ion beam etching. The thickness of the metallic titanium is 10nm; the thickness of the gold film was 160nm.
3) And (3) constructing a silicon pattern by combining an alignment lithography technology with a silicon deep etching technology to finish secondary pattern transfer. According to the observation result of a microscope, the transverse etching precision is +/-0.5 mu m, and the longitudinal etching precision is +10%.
According to another embodiment of the invention, a terahertz detection spectrum system for detecting by adopting the light-operated terahertz biosensor is also disclosed. The terahertz detection spectrum system comprises: the device comprises a femtosecond laser, a beam splitter and a light-operated terahertz biosensor. The femtosecond laser is used for generating femtosecond laser; the beam splitter is used for splitting the femtosecond laser to form terahertz light, terahertz detection light and pumping light; the pump light is used for exciting photo-carriers; the terahertz detection light is used for testing and recording transmission spectral lines of the front and rear super surfaces into which the pump light is incident.
As shown in fig. 6, the terahertz detection spectroscopy system specifically includes: the high-power optical fiber laser comprises a reflector (M), a beam splitter 1 (BS 1), a beam splitter 2 (BS 2), a half-wave plate (HWP), a Thin Film Polarizer (TFP), indium tin oxide transparent conductive thin film glass (ITO), off-axis parabolic mirrors (OPM 1, OPM2, OPM3 and OPM 4), a high-resistance silicon wafer (HR Si), a quarter-wave plate (QW), a Wollaston Prism (WP), a balanced diode (BPD) and a zinc telluride crystal (ZnTe). The process of detecting the biological substances by using the terahertz detection spectrum system comprises the following steps:
first, laser light (800nm, 100fs) emitted from a femtosecond laser is divided into three paths by a beam splitter. One path of light is used for generating terahertz waves, the other path of light is used for terahertz detection light, and the other path of light is used for pumping light to excite silicon carriers. Generating terahertz and detecting light for testing, and recording transmission spectral lines of front and rear super-surface structures of pumping light;
secondly, the biological substance to be tested is treated, for example: samples of different types and concentrations of cellular or macromolecular biological substances are taken. And then, moving the sample to the surface of the super-surface structure, testing the transmission spectral lines before and after the pumping light is injected again, and recording the frequency shift and amplitude change spectral lines of each test.
Since the electric and magnetic field energy of the resonant metal structure is mainly localized at the metal/media interface, the interaction of light and substance is favoured in the near field. Therefore, after different kinds and concentrations of cells or macromolecular biological substances are moved, the resonance structure can be shifted in frequency or amplitude due to the difference of dielectric constant and conductivity of the cells or the coupling between the vibration of the biological macromolecules and the enhanced magnetic field around the resonator.
Finally, qualitative or quantitative analysis is carried out on the substances by comparing changes of frequency spectrum information (such as frequency shift and amplitude shift) before and after different types and concentrations of cell or macromolecular biological substances are placed and before and after pumping light is injected.
Furthermore, the biosensor can perform qualitative analysis on the resonance coupling of a certain characteristic peak position of a biomacromolecule and a resonance peak position in one mode, and can perform verification by utilizing ultra-fast conversion to another mode. The scheme for distinguishing substances by single characteristic absorption lines, which may cause false positives, is optimized. The application of two or even multiple modes can realize accurate detection of multiple characteristic spectral lines of a single substance or multiple mixed substances. Meanwhile, quantitative analysis can be carried out according to the frequency shift and amplitude shift changes of the biomacromolecules with different doses.
Fig. 2 to 5 show the transmission lines under different conditions. Fig. 2 shows transmission spectra of the light-controlled terahertz biosensor under different pumping energies in the present invention; FIG. 3 shows transmission spectra of a light-controlled terahertz biosensor according to the present invention with different silicon conductivities; FIG. 4 shows a transmission spectrum of the light-controlled terahertz biosensor in the invention with a pump light detection time delay of-2 ps to 32 ps; fig. 5 shows a transmission spectrum of the light-controlled terahertz biosensor in the invention when the pump light detection time delay is between 32ps and 162 ps.
In order to achieve the best detection effect, the optical control terahertz biosensor claimed by the invention is used in the spectral system. In order to prepare a high-precision biosensor, firstly, the parameters of the super-surface micro-nano structure are calculated, simulated and adjusted, and the conversion of the resonance mode before and after pumping light is injected is simulated. The design structure is converted from the coupling state which is in Lorentz and lattice modes before pumping light is injected into the sensing mode after the pumping light is injected into the sensing mode into the EIT mode. The coupled mode provides an ultrasensitive feature for the detection of biological substances. In order to improve the simulation accuracy, FDTD software may be preferably used for the calculation simulation. And then, according to the parameters of the super-surface structure, integrating a silicon material and a super-structure on a substrate to manufacture the light-operated terahertz biosensor with the ultra-fast switch sensing function.
According to the invention, through designing and adjusting the structural parameters, the resonance mode can be rapidly switched under the condition of pumping light and no pumping light, so that the rapid detection of the biological substances in a dual-mode state is completed. Finally, the qualitative and quantitative detection of the object to be detected, which is more accurate, sensitive and portable, is realized.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. An optically controlled terahertz biosensor, comprising: the device comprises a substrate, and a dielectric material and a super-surface structure which are integrated on the substrate; the terahertz wave super-surface structure comprises a substrate, a dielectric material, a super-surface structure and a plurality of metal resonators, wherein the substrate is a terahertz wave high-transmittance material, the dielectric material is a semiconductor material, and the super-surface structure is an array structure formed by a plurality of metal resonators and cutting wires;
a lattice resonant structure is formed among the plurality of metal resonators, a Lorentz resonant structure is formed among the plurality of cutting wires, and the lattice resonant structure and the Lorentz resonant structure are coupled to form a Lorentz-lattice resonant mode;
the dielectric material is integrated between the cutting wires to connect the pair of cutting wires, so that the Lorentz-lattice mode is switched into the EIT mode in a picosecond range by means of the ultrafast carrier excitation and relaxation process of the dielectric material.
2. The optically controlled terahertz biosensor according to claim 1, wherein the super-surface structure is a plurality of unit structures arranged periodically, each unit structure comprising two pairs of metal resonators and one pair of cutting wires; the metal resonator is a square opening resonator; the openings of the two metal resonators are oppositely arranged to form a pair of metal resonators; two pairs of metal resonators arranged up and down in the same plane are separated by a pair of cutting wires.
3. The light-operated terahertz biosensor as claimed in claim 1, wherein the cutting wires are connected with each other by a silicon bridge.
4. The light-controlled terahertz biosensor according to any one of claims 1 to 3, wherein the metal resonator is made of any one of gold, silver or aluminum.
5. The light-controlled terahertz biosensor according to any one of claims 1 to 3, wherein the dielectric material is silicon or germanium.
6. A preparation method of the light-controlled terahertz biosensor, which is used for preparing the light-controlled terahertz biosensor as claimed in any one of claims 1 to 5, and comprises the following steps:
cleaning the sapphire substrate silicon by using acetone and isopropanol;
preparing a metal super-surface structure;
constructing a silicon pattern by combining an alignment lithography technology and a silicon deep etching technology to complete secondary pattern transfer;
the metal super-surface structure is a plurality of unit structures which are periodically arranged, and each unit structure comprises: two pairs of open square resonators, and two dicing wires connected by a semiconductor material.
7. The light-controlled terahertz biosensor as claimed in claim 6, wherein the sapphire substrate silicon specifically comprises an epitaxial silicon layer with a thickness of 600nm and a sapphire substrate with a thickness of 460 nm.
8. The light-operated terahertz biosensor as claimed in claim 6, wherein the metal super-surface structure is prepared on the titanium and gold film by a step photolithography method and an ion beam etching method.
9. The light-controlled terahertz biosensor as claimed in claim 8, wherein the titanium is 10nm thick, and the gold film is 160nm thick.
10. A terahertz detection spectroscopy system, comprising: a femtosecond laser, a beam splitter, and the light-controlled terahertz biosensor of any one of claims 1 to 5; wherein
The femtosecond laser is used for generating femtosecond laser;
the beam splitter is used for splitting the femtosecond laser to form terahertz light, terahertz detection light and pumping light;
the pump light is used for realizing the excitation of photo-carriers;
the terahertz detection light is used for testing and recording the transmission spectral line of the pumping light which is irradiated into the front and rear super surfaces.
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