CN110865110A - Coplanar gate oxide thin film transistor biosensor and preparation method thereof - Google Patents

Coplanar gate oxide thin film transistor biosensor and preparation method thereof Download PDF

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CN110865110A
CN110865110A CN201911128092.0A CN201911128092A CN110865110A CN 110865110 A CN110865110 A CN 110865110A CN 201911128092 A CN201911128092 A CN 201911128092A CN 110865110 A CN110865110 A CN 110865110A
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active layer
electrode
gate
semiconductor active
coplanar
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裴艳丽
杨彭
李亚
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Sun Yat Sen University
National Sun Yat Sen University
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Abstract

The invention discloses a coplanar gate oxide thin film transistor biosensor, which comprises a substrate, an insulating layer, a source electrode, a drain electrode, a gate electrode, a source drain electrode insulating protective layer and a surface biological modified metal oxide semiconductor active layer, wherein the insulating layer is arranged on the substrate; the source electrode, the drain electrode and the gate electrode are made of the same material, and the three electrodes are coplanar. The added gate dielectric layer is liquid electrolyte, the liquid electrolyte covers the semiconductor active layer and part of the gate electrode, and the part of the gate electrode exposed out of the liquid electrolyte is connected with a circuit. The gate electrode, the source electrode and the drain electrode are coplanar, the deposition of the source electrode, the drain electrode and the gate electrode can be completed through one-step process by using the same material, and the ohmic contact with a semiconductor is realized, and meanwhile, the method has the advantages of simple process, integration, low cost and the like; meanwhile, the liquid electrolyte is directly contacted with the semiconductor active layer and the gate electrode, and the double electric layer effect of the liquid electrolyte enables the device to have low working voltage and low power consumption, thereby being beneficial to biomolecule detection.

Description

Coplanar gate oxide thin film transistor biosensor and preparation method thereof
Technical Field
The invention belongs to the technical field of semiconductor electronic devices and sensors, and particularly relates to a coplanar gate oxide thin film transistor biosensor and a preparation method thereof.
Background
With the continuous development of science and technology, the combination of biology and information is tighter and tighter, and the convenient and fast acquisition of biological information is of great importance to the development of modern medical and wearable devices. Biosensors are not only of great significance in the field of medical diagnosis, but also of significance in national security and environmental monitoring. The traditional biomolecule detection method mainly comprises tumor markers, immunological detection, genetic evaluation, blood detection and the like, wherein a biosensor based on a thin film transistor has the advantages of being capable of being miniaturized, low in cost, high in sensitivity, fast in response and the like, and is widely applied to the fields of flat panel display, biochemical sensing, medical diagnosis and the like.
In order to improve the performance of TFT thin film transistor devices, researchers have developed a variety of semiconductor thin film materials that can be used in active layers, mainly including polysilicon, organic materials, oxide semiconductor materials, etc., wherein wide band gap oxide semiconductors have many advantages such as relatively high mobility, visible light transparency, low temperature process, etc., and are widely used in the fields of liquid crystal displays, solar cells, touch panels, flexible displays, etc., and metal oxide semiconductor thin film transistors are also a mature technology applied to next generation active matrix liquid crystal displays and active matrix organic light emitting diode displays (AMOLEDs). In addition, the oxide thin film has good biocompatibility on the surface, and can be widely applied to the research of biosensors by realizing surface modification through chemical treatment.
The traditional TFT device generally adopts an oxide insulating film as a gate dielectric layer, the working voltage of the device is higher, the power consumption of the device is larger, and the device is not beneficial to biological signal detection, so that the application of the device in portable and wearable electronic products is limited.
One key element for TFT biosensors is the gate electrode, which is necessary to adjust the operation of the operating point driver device to obtain high stability and sensitivity. There are several types of gates in conventional transistors, such as Ag/AgCl, conductive substrates, etc. In sensing experiments, the conductive substrate is used as a gate electrode, extra steps and a photolithographic mask are needed for preparation, the process flow is complicated, and the selection of the substrate material is limited. The Ag/AgCl electrode is widely applied to electrochemical experiments as a reference electrode. Integration of such electrodes into conventional fabrication processes is challenging due to limitations in materials suitable for use in microelectronic devices. In addition, the Ag/AgCl electrode is influenced by the ion concentration in the solution in the sensing test, and the working stability of the device is also influenced.
Disclosure of Invention
The present invention aims to overcome the defects of the prior art and provide a coplanar gate oxide thin film transistor biosensor, which has the advantages of simple process, integration, low working voltage, high detection sensitivity, etc.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
the coplanar gate oxide thin film transistor biosensor comprises an insulating substrate, a source electrode, a drain electrode, a gate electrode, a source-drain electrode insulating protective layer and a semiconductor active layer; the semiconductor active layer covers the insulating substrate, and the source electrode, the drain electrode and the gate electrode are all arranged on the insulating substrate and protrude out of the semiconductor active layer; the source electrode, the drain electrode and the gate electrode are made of the same material, and the source electrode, the drain electrode and the gate electrode are coplanar; the semiconductor active layer is a metal oxide semiconductor active layer with a biological modified surface, and the metal oxide semiconductor active layer with the biological modified surface is obtained by carrying out surface modification on the metal oxide semiconductor active layer and then continuously modifying biomolecules;
when the coplanar gate oxide thin film transistor biosensor is used, target molecules to be detected are contacted with the surface biologically-modified metal oxide semiconductor active layer, and after a period of reaction, a gate dielectric layer is added; the gate dielectric layer is a liquid electrolyte, the liquid electrolyte covers the semiconductor active layer and part of the gate electrode, and part of the gate electrode exposed out of the liquid electrolyte is connected with a circuit; the source electrode, the drain electrode and the semiconductor active layer form ohmic contact; and the source and drain electrode insulating protective layer isolates the source electrode and the drain electrode from being in contact with the gate dielectric layer.
The gate dielectric layer is liquid electrolyte, covers on the active layer and the gate electrode, and forms an MIS capacitor structure together with the gate electrode, the liquid electrolyte and the oxide semiconductor active layer, so that the MIS capacitor structure has large capacitance based on the double electric layer effect and obtains lower working voltage.
In the structural design of the coplanar gate electrode oxide thin film transistor biosensor, the source and drain electrodes are coplanar with the gate electrode made of the same material, and the source and drain electrodes and the gate electrode can be prepared by a mask, so that the method has the advantages of simple process flow, low cost and easy integration. The metal oxide semiconductor is adopted as a semiconductor active layer, the surface of the metal oxide semiconductor has good biocompatibility, the metal oxide semiconductor active layer is subjected to surface modification through a silane coupling agent, then biomolecules are continuously modified on the surface, and the biomolecules are detected through specific connection. Meanwhile, the liquid electrolyte is used as a gate dielectric layer and is directly contacted with the semiconductor active layer and the gate electrode, and the double electric layer effect of the liquid electrolyte enables the device to have low working voltage and low power consumption and is beneficial to biomolecule detection.
In particular, the preferred insulating substrate of the present invention is SiO-coated2A Si substrate of an insulating layer.
Preferably, the liquid electrolyte is a phosphate buffer solution. However, the present invention is not limited to the kind of liquid electrolyte. Phosphate in the phosphate buffer solution can be used as an electrolyte, and the phosphate buffer solution is used as a buffer solution for common biological research, so that a stable environment is provided for the detection of biological molecules.
Specifically, the surface biological modified metal oxide semiconductor active layer is subjected to surface modification through a silane coupling agent. The surface modification of the metal oxide semiconductor active layer is not limited to silane coupling.
The metal oxide semiconductor active layer is metal oxide semiconductor conventionally used In the art, and specifically, the metal oxide semiconductor active layer is IGZO, IZO, In2O3And ZnO.
Preferably, the metal oxide semiconductor active layer is In2O3
Preferably, the source and drain electrode insulating protective layer is made of SU-8 photoresist. The source and drain electrode insulating protective layer completely covers the source electrode and the drain electrode, so that the liquid electrolyte cannot contact the source electrode and the drain electrode.
Specifically, the source electrode, the drain electrode and the gate electrode are all made of Ti/Au.
Preferably, the biomolecule modified on the surface of the metal oxide semiconductor active layer is streptavidin, and the streptavidin is used as a receptor molecule for quantitatively detecting the target molecule biotin. However, the present invention is not limited to the kinds of biomolecules. The streptavidin-biotin system becomes a new technology for qualitative and quantitative detection and positioning observation and research of trace antigens and antibodies at present due to the advantages of the streptavidin-biotin system on specificity and stability. The streptavidin molecules are fixed on the surface of the semiconductor active layer through modifying the surface of the oxide to be used as receptor molecules for detecting target molecule biotin, so that the content of biotin in the solution can be quantitatively analyzed.
Furthermore, the metal oxide semiconductor active layer selects In2O3Indium oxide is an oxide per se, and the related literature reports that the surface of indium oxide is rich in hydroxyl groups. Surface treatment of In with silane coupling agent gamma-aminopropyltriethoxysilane APTES2O3And reacting glutaraldehyde solution GA with coupling agent APTES to make the surface of the metal oxide semiconductor active layer be aldehyde-group-converted, and connecting the functional group with aldehyde group with amino group of streptavidin so as to make the streptavidin be fixed on the surface of the metal oxide semiconductor active layer.
The preparation method of the coplanar gate oxide thin film transistor biosensor comprises the following steps:
s1, preparing an insulating substrate;
s2, preparing a metal oxide semiconductor active layer;
s3, patterning the active layer of the metal oxide semiconductor;
s4, preparing and patterning a source electrode, a drain electrode and a gate electrode;
s5, isolating the source electrode and the drain electrode, and exposing the active layer, the gate electrode and the lead part of the source electrode and the drain electrode;
s6, biologically modifying the surface of the metal oxide semiconductor active layer.
The use method of the coplanar grid oxide thin film transistor biosensor comprises the following steps:
s1, dripping a target molecule to be detected on the surface of a biologically modified metal oxide semiconductor active layer in a liquid form, washing with deionized water after reacting for a period of time, and then drying with nitrogen;
s2, liquid electrolyte is dripped on the surfaces of the semiconductor active layer and the gate electrode to serve as gate dielectrics, the dripped amount of the liquid electrolyte covers the semiconductor active layer and part of the gate electrode, and part of the gate electrode exposed out of the liquid electrolyte is connected with a circuit;
and S3, carrying out test analysis by using a semiconductor parameter tester.
Specifically, the method for detecting biotin by using the coplanar gate oxide thin film transistor biosensor comprises the following steps:
s1, enabling a biomolecule modified on the surface of a metal oxide semiconductor active layer to be streptavidin, then dropping biotin (N-hydroxysuccinimide ester) solutions with different concentrations on the surface of the metal oxide semiconductor active layer fixed with the streptavidin, washing the surface with deionized water after half an hour in a dark room temperature environment, and drying the surface with a nitrogen gun;
s2, dropping a phosphate buffer solution on the surfaces of the semiconductor active layer and the gate electrode to serve as a gate dielectric, wherein the dropping amount of the phosphate buffer solution covers the semiconductor active layer and part of the gate electrode, and the part of the gate electrode exposed out of the phosphate buffer solution is connected with a circuit;
and S3, carrying out test analysis by using a semiconductor parameter tester.
Compared with the prior art, the invention has the beneficial effects that:
the coplanar gate oxide thin film transistor biosensor completes the deposition of the source electrode, the drain electrode and the gate electrode through one-step process, realizes ohmic contact with a semiconductor, and has the advantages of simple process, integration, low cost and the like(ii) a The gate dielectric layer is made of liquid electrolyte and is directly contacted with the semiconductor channel layer, and the working voltage is low (V) through the double electric layer characteristic of the gate dielectric materialGS<0.8V,VDS0.05V) to facilitate the testing of biomolecule signals. The invention adopts a streptavidin-biotin system to realize the quantitative detection of biotin, the sensitivity is as high as 200nA/Dec, and the minimum detection limit is 50 pg/mL. The invention provides a device foundation for the field of high-sensitivity biosensors and has important significance in the fields of medical diagnosis, environmental monitoring and the like.
Drawings
FIG. 1 is a cross-sectional view of the structure of a coplanar gate oxide thin film transistor biosensor in accordance with the present invention.
Fig. 2 is a source-drain current variation curve of the oxide thin film transistor biosensor device according to embodiment 1 of the present invention, as the concentration of detected biomolecules increases.
The reference numerals in fig. 1 illustrate:
1. si substrate, 2, SiO2The device comprises an insulating layer, 3, an indium oxide active layer, 4, a source drain electrode, 5, a gate electrode, 6, an SU-8 glue isolation barrier layer, 7 and a liquid gate dielectric layer.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail below with reference to specific embodiments and the accompanying drawings, but the scope of the present invention is not limited to the embodiments.
Example 1:
the preparation method of the coplanar gate oxide thin film transistor biosensor (surface modified streptavidin) comprises the following steps:
s1, sputtering In with the thickness of 45nm on a heavily doped silicon substrate grown with thermal oxidation silicon dioxide2O3An active layer;
s2, for In2O3Photoetching and wet etching are carried out on the active layer to finish the patterning process of the active layer;
s3, photoetching, evaporating source, drain and gate electrodes, removing photoresist and stripping to form a required electrode pattern;
s4, isolating an electrode by using SU-8 glue, and exposing an active layer, a contact part of a grid electrode and a grid medium layer and an electrode lead part;
s5, surface modification of streptavidin: soaking the device in 15% ethanol solution of gamma-Aminopropyltriethoxysilane (APTES) for 12h in dark room temperature, washing with ethanol under shaking, washing with deionized water, and blow-drying with nitrogen gun; placing the device in 25% glutaraldehyde solution (GA) for 2 hours in dark room temperature environment, then washing with deionized water and drying with a nitrogen gun; mu.L of streptavidin solution (600. mu.g/mL) was titrated onto the surface of the indium oxide active layer, and after one hour in the dark room temperature environment, the device surface was rinsed with deionized water and blown dry with a nitrogen gun.
The biosensor prepared above was used to detect different concentrations of biotin: 10 mu L of biotin (N-hydroxysuccinimide ester) solutions with different concentrations are respectively dripped on the surface of the streptavidin-immobilized indium oxide active layer, the surface of the device is washed by deionized water after being in a dark room temperature environment for half an hour, and the device is dried by a nitrogen gun. And dropping 2 mu L of phosphate buffer solution on the surfaces of the indium oxide active layer and the grid electrode to be used as grid dielectric layers, and carrying out test analysis by using a semiconductor parameter tester.
The structure of the above-described coplanar gate oxide thin film transistor biosensor is shown in fig. 1.
FIG. 2 is a graph showing the time-dependent change of the current at the biotin concentration of 50fg/mL to 500ng/mL in this example, and the gate voltage V at the time of the testGS=0V,VDSThe lowest detection limit is 50pg/mL and the detection sensitivity is about 200nA/Dec when the detection voltage is 0.05V.
The above shows that the coplanar gate electrode thin film transistor sensor of the invention has the advantages of simple structure, easy preparation and integration, low working voltage, high sensitivity, low detection limit and the like.
Variations and modifications to the above-described embodiments may occur to those skilled in the art, which fall within the scope and spirit of the above description. Therefore, the present invention is not limited to the specific embodiments disclosed and described above, and some modifications and variations of the present invention should fall within the scope of the claims of the present invention. In addition, although specific terms are employed herein, they are used in a generic and descriptive sense only and not for purposes of limitation.

Claims (10)

1. The coplanar gate oxide thin film transistor biosensor is characterized by comprising an insulating substrate, a source electrode, a drain electrode, a gate electrode, a source drain electrode insulating protective layer and a semiconductor active layer; the semiconductor active layer covers the insulating substrate, and the source electrode, the drain electrode and the gate electrode are all arranged on the insulating substrate and protrude out of the semiconductor active layer; the source electrode, the drain electrode and the gate electrode are made of the same material, and the source electrode, the drain electrode and the gate electrode are coplanar; the semiconductor active layer is a metal oxide semiconductor active layer with a biological modified surface, and the metal oxide semiconductor active layer with the biological modified surface is obtained by carrying out surface modification on the metal oxide semiconductor active layer and then continuously modifying biomolecules;
when the coplanar gate oxide thin film transistor biosensor is used, target molecules to be detected are contacted with the surface biologically-modified metal oxide semiconductor active layer, and after a period of reaction, a gate dielectric layer is added; the gate dielectric layer is a liquid electrolyte, the liquid electrolyte covers the semiconductor active layer and part of the gate electrode, and part of the gate electrode exposed out of the liquid electrolyte is connected with a circuit; the source electrode, the drain electrode and the semiconductor active layer form ohmic contact; and the source and drain electrode insulating protective layer isolates the source electrode and the drain electrode from being in contact with the gate dielectric layer.
2. The coplanar gate oxide thin film transistor biosensor as set forth in claim 1, wherein the insulating substrate is SiO-coated2A Si substrate of an insulating layer.
3. The coplanar gate oxide thin film transistor biosensor as set forth in claim 1, wherein the metal oxide is selected from the group consisting of copper, nickel, and copperThe semiconductor active layer is IGZO, IZO, In2O3And ZnO.
4. The coplanar gate oxide thin film transistor biosensor as claimed in claim 1, wherein the surface-biologically modified metal oxide semiconductor active layer is surface-modified with a silane coupling agent.
5. The coplanar gate oxide thin film transistor biosensor as claimed in claim 1, wherein the source-drain electrode insulating protective layer is SU-8 photoresist.
6. The coplanar gate oxide thin film transistor biosensor as set forth in claim 1 wherein the source, drain and gate electrodes are each of Ti/Au.
7. The coplanar gate oxide thin film transistor biosensor as claimed in claim 1, wherein the biomolecule modified on the surface of the metal oxide semiconductor active layer is streptavidin, and the streptavidin is used as a receptor molecule for quantitatively detecting the target molecule biotin.
8. The coplanar gate oxide thin film transistor biosensor as set forth in claim 1 wherein the liquid electrolyte is a phosphate buffer solution.
9. The method of making a coplanar gate oxide thin film transistor biosensor as claimed in any one of claims 1-8, comprising the steps of:
s1, preparing an insulating substrate;
s2, preparing a metal oxide semiconductor active layer;
s3, patterning the active layer of the metal oxide semiconductor;
s4, preparing and patterning a source electrode, a drain electrode and a gate electrode;
s5, isolating the source electrode and the drain electrode, and exposing the active layer, the gate electrode and the lead part of the source electrode and the drain electrode;
s6, biologically modifying the surface of the metal oxide semiconductor active layer.
10. The method of using a coplanar gate oxide thin film transistor biosensor as claimed in any one of claims 1-8, comprising the steps of:
s1, dripping a target molecule to be detected on the surface of a biologically modified metal oxide semiconductor active layer in a liquid form, washing with deionized water after reacting for a period of time, and then drying with nitrogen;
s2, liquid electrolyte is dripped on the surfaces of the semiconductor active layer and the gate electrode to serve as gate dielectrics, the dripped amount of the liquid electrolyte covers the semiconductor active layer and part of the gate electrode, and part of the gate electrode exposed out of the liquid electrolyte is connected with a circuit;
and S3, carrying out test analysis by using a semiconductor parameter tester.
CN201911128092.0A 2019-11-18 2019-11-18 Coplanar gate oxide thin film transistor biosensor and preparation method thereof Pending CN110865110A (en)

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