CN112864252A - DNA sensor based on thin film transistor and preparation method thereof - Google Patents
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- H01L29/772—Field effect transistors
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Abstract
The invention relates to a DNA sensor based on a thin film transistor and a preparation method thereof, wherein the DNA sensor comprises the thin film transistor and a DNA molecular probe, the thin film transistor comprises a substrate, a gate electrode, an insulating layer, a source electrode, a drain electrode and a semiconductor layer, the substrate, the gate electrode and the insulating layer are sequentially arranged from bottom to top, the semiconductor layer is arranged on the insulating layer, the source electrode and the drain electrode are in contact with the semiconductor layer, and the DNA molecular probe is fixed on the source electrode and the drain electrode. Compared with the prior art, the invention adopts the source and drain electrodes as the substrate, and the DNA molecular probe is fixed on the source and drain electrodes, thereby avoiding the influence of physical absorption on the organic semiconductor layer on moisture and certain ions, improving charge injection, enhancing the saturation current and carrier mobility of the sensor, and further improving the stability and sensitivity of the DNA sensor.
Description
Technical Field
The invention belongs to the technical field of DNA sensors, and relates to a DNA sensor based on a thin film transistor and a preparation method thereof.
Background
With the development of technologies such as bioinformatics, internet of things and the like, DNA molecules are regarded as the most basic substances in bioengineering, which attracts attention of extensive research institutes, and the development of DNA detection technology also promotes the continuous progress of research work on DNA structures and functions. At present, the DNA detection technology includes the traditional DNA sequencing technology, DNA chips, biosensors and the like. The DNA biosensor has the characteristics of high detection speed, high sensitivity and the like, and is widely applied to the fields of environmental monitoring, aerospace and the like.
In recent years, research and application of organic transistor devices have been greatly developed, and DNA detection systems have attracted considerable attention in the fields of genotyping, drug discovery, molecular diagnostics, and the like, and the technology has been widely applied to pathogenic and genetic disease diagnostics, and the like. Conventional labeled DNA sensors cannot rapidly monitor probe interactions and also require complex analytical systems, which are expensive, time consuming and cumbersome. In this case, compared with the conventional DNA sensor, the label-free detection method eliminates the labeling process, simplifies the analysis process, and promotes the development of DNA detection.
Thin film transistors, which are transducers for DNA sensors, have certain advantages over existing optical detection techniques and are considered to be the most promising candidates. Previous studies have demonstrated that electrical detection has higher sensitivity than optical detection. In addition, thin film transistor based electrical inspection systems may be a faster inspection process. In recent years, different approaches have been developed to realize thin film transistor-based DNA sensors. However, they are mostly based on the physical absorption of DNA molecules on semiconductors and achieved by changing the electrical characteristics of transistors, but the physical absorption on semiconductors is sensitive to moisture and some ions, which reduces the stability and reproducibility of DNA sensors, thereby reducing their sensitivity.
Disclosure of Invention
The invention aims to provide a DNA sensor based on a thin film transistor and a preparation method thereof.
The purpose of the invention can be realized by the following technical scheme:
a DNA sensor based on a thin film transistor comprises the thin film transistor and a DNA molecular probe, wherein the thin film transistor comprises a substrate, a gate electrode, an insulating layer, a source electrode, a drain electrode and a semiconductor layer, the substrate, the gate electrode and the insulating layer are sequentially arranged from bottom to top, the semiconductor layer is arranged on the insulating layer, the source electrode, the drain electrode and the semiconductor layer are in contact, and the DNA molecular probe is fixed on the source electrode and the drain electrode.
Furthermore, the source and drain electrodes and the semiconductor layer are both arranged on the insulating layer, and the semiconductor layer is positioned in the channel of the source and drain electrodes.
Or, the source and drain electrodes are arranged on the semiconductor layer.
Furthermore, the substrate is made of an insulating material, or a composite material formed by covering a layer of insulating material on the surface of a conductive material. The insulating material is preferably glass or ceramic. If the root mean square roughness of the substrate surface is greater than 1 nm, smoothing with an insulating polymer coating of polymethyl methacrylate or polyvinyl alcohol is required.
Further, the gate electrode is made of one or more of gold (Au), aluminum (Al), copper (Cu), titanium (Ti), silver (Ag), or heavily doped silicon.
Further, the material of the insulating layer includes one or more of silicon dioxide, silicon nitride, aluminum oxide, titanium oxide, or polyvinyl alcohol. The insulating layer is mainly made of an insulating material with a high dielectric constant.
Further, the source/drain electrode may be made of one or more of gold (Au), silver (Ag), copper (Cu), aluminum (Al), magnesium (Mg), aluminum (Al), titanium (Ti), lead (Pd), or platinum (Pt).
Furthermore, the material of the semiconductor layer is graphene, black phosphorus, silicon alkene, metal oxide, MoS2、WS2、MoSe2、WSe2、MoTe2、WTe2、ZrS2、ZrSe2、NbSe2、NbS2、TaS2、NiSe2、GaSe、GaTe、InSe、ReTe2、TiTe2、NbTe2Or SnTe2. The metal oxide is preferably TiOx、NbOx、MnOx、VaOxOr TaO3. The semiconductor layer is made of two-dimensional material.
Further, the DNA molecular probe is an ssDNA molecular probe or a dsDNA molecular probe.
A preparation method of a DNA sensor based on a thin film transistor comprises the following steps:
1) preparing a gate electrode on the surface of the substrate by adopting an evaporation or sputtering method;
2) manufacturing an insulating layer on the gate electrode by adopting an evaporation method;
3) depositing a source-drain electrode and a semiconductor layer, and fixing a DNA molecular probe on the surface of the source-drain electrode by a physical adsorption, bonding or self-assembly method.
When the source-drain electrode and the semiconductor layer are both arranged on the insulating layer and the semiconductor layer is positioned in a channel of the source-drain electrode, in the step 3), firstly, the position of the source-drain electrode is determined above the insulating layer by using a mask plate, and the source-drain electrode is deposited on the semiconductor layer by adopting a vacuum metal deposition method; and preparing a semiconductor layer by adopting a vacuum evaporation, solution spin coating or film spinning method and depositing the semiconductor layer on the insulating layer of the channel region between the source electrode and the drain electrode to form the DNA sensor with the bottom-gate bottom contact structure.
When the source and drain electrodes are disposed on the semiconductor layer, in step 3), the semiconductor layer is first deposited on the insulating layer, and then the source and drain electrodes are deposited on the semiconductor layer.
Wherein the background vacuum degree is not less than 10-4Pa, metal electrodeThe deposition rate was 20 nm/min and the other material deposition rate was 0.03 nm/min.
The invention provides a DNA sensor based on a thin film transistor, which records and analyzes the characteristics of a target object based on various physicochemical signal changes caused by the interaction of DNA molecules, thereby realizing the detection and monitoring of the target object. The DNA sensor is composed of a recognition element and a transducer, the thin film transistor is used as the transducer, and the signal sensed by the recognition element is converted into other recordable signals, such as mass change, frequency change, magnetic signals, fluorescent signals, electric signals, sound wave signals and the like; the recognition element is a DNA molecular probe and is fixed on the source and drain electrodes by means of adsorption, bonding, self-assembly and the like. By applying voltage on the source electrode and the drain electrode of the DNA sensor, charge injection is improved, and the saturation current and the carrier mobility of the sensor are enhanced, so that the sensitivity of the DNA sensor is improved.
Compared with the prior art, the invention has the following characteristics:
1) according to the invention, the source and drain electrodes are used as the substrate, and the DNA molecular probe is fixed on the source and drain electrodes, so that the influence of physical absorption on moisture and certain ions on the organic semiconductor layer is avoided, the charge injection is improved, the saturation current and the carrier mobility of the sensor are enhanced, and the stability and the sensitivity of the DNA sensor are improved;
2) the traditional DNA sensor has the problems of high cost, time consumption and complexity, and the label-free detection method of the DNA sensor based on the thin film transistor omits the label process, simplifies the analysis process, improves the DNA detection efficiency and promotes the development of DNA detection.
Drawings
FIG. 1 is a schematic view showing the structure of a DNA sensor based on a thin film transistor in example 1;
FIG. 2 is an electrical schematic diagram of the thin film transistor-based DNA sensor in example 1 with voltage applied at the source and drain electrodes;
FIG. 3 is a graph showing output characteristics of organic field effect transistors in example 1 without immobilized DNA (a) and with an Au surface treated with SH-ssDNA (b);
FIG. 4 is a graph showing transfer characteristics of the organic field effect transistor of example 1 without immobilized DNA and with an SH-ssDNA-treated Au surface;
FIG. 5 is a schematic view showing the structure of a DNA sensor based on a thin film transistor in example 2;
FIG. 6 is a schematic view showing the structure of a DNA sensor based on a thin film transistor in a comparative example;
the notation in the figure is:
1-substrate, 2-gate electrode, 3-insulating layer, 4-source drain electrode, 5-semiconductor layer and 6-DNA molecular probe.
Detailed Description
The invention is described in detail below with reference to the figures and specific embodiments. The present embodiment is implemented on the premise of the technical solution of the present invention, and a detailed implementation manner and a specific operation process are given, but the scope of the present invention is not limited to the following embodiments.
In the following examples, SH-ssDNA (5 '-SH-TATA CGGT TCGCGC-3') was synthesized by Shanghai Santong Biotech Co., Ltd.
Example 1:
a structure of a DNA sensor based on a thin film transistor is shown in figure 1, the DNA sensor is composed of a recognition element and a transducer, a DNA molecular probe 6 is used as the recognition element, and the DNA molecular probe 6 is solidified on the surface of a source electrode and a drain electrode 4 through adsorption, bonding, self-assembly and other modes; the transducer is a thin film transistor, and the transducer is used for converting a signal sensed by the identification element into other recordable signals, such as mass change, frequency change, magnetic signals, fluorescent signals, electric signals, sound wave signals and the like. The DNA sensor is formed by sequentially connecting a substrate 1, a gate electrode 2 and an insulating layer 3, then preparing a source-drain electrode 4 on the insulating layer 3, fixing a DNA molecular probe 6 on the source-drain electrode 4, and finally evaporating and depositing a semiconductor layer 5 on the upper surface of the insulating layer 3 in a channel region between the source-drain electrode 4 to form the bottom-gate bottom-contact DNA sensor.
The specific preparation method of each structural layer of the DNA sensor of this example is as follows:
1) selecting heavily doped silicon wafers as a substrate 1 and a gate electrode 2, wherein the conductivity of the silicon wafers is 0.01-0.15 omega cm, ultrasonically cleaning the substrate 1 with acetone and ethanol for fifteen minutes, and washing with a corresponding solvent when the substrate is taken out after ultrasonic cleaning to remove adhered debris;
2) thermally oxidizing a layer of silicon dioxide with the thickness of 300nm on a silicon wafer to be used as an insulating layer 3 of a transistor;
3) washing the silicon wafer with deionized water, and baking in a vacuum oven at 120 ℃; and after the silicon wafer is cooled, putting the silicon wafer into vacuum evaporation equipment. Using a mask method to rapidly evaporate a gold electrode as a source electrode and a drain electrode 4 of the transistor, and determining that the length of a channel is 180 mu m and the width is 2700 mu m;
4) preparing Phosphate Buffer Solution (PBS) containing Na as main ingredient2HPO4、NaH2PO4NaCl, KCl, pH 7.4, and the ssDNA probe used was dissolved in Phosphate Buffer Solution (PBS). Dripping PBS solution containing ssDNA onto the source and drain electrodes 4, namely gold electrodes, to realize the immobilization of the ssDNA molecular probe 6;
5) washing with deionized water, flushing residual water with high pressure, and placing the device in vacuum chamber until vacuum pressure reaches 10%-4Pa, the semiconductor layer 5 was slowly heated to 110 ℃ to start evaporation, and the evaporation was carried out at an evaporation rate of 0.03nm/s on the upper surface of the insulating layer 3 in the channel region between the source and drain electrodes 4.
In this example, ssDNA molecular probes were physically immobilized on the source and drain electrodes 4 of a thin film transistor device, formed by gathering ssDNA molecules together by van der waals forces, and a bias voltage was applied between the source and gate electrodes, as shown in fig. 2, and the electrical properties were measured using a test device.
Performance analysis of the DNA sensor of this example:
the output characteristic curves of the organic field effect transistor in which the source-drain electrodes 4, i.e., the Au surface, had no dna immobilized (a) and the Au surface was treated with SH-ssDNA (b) are shown in fig. 3. It can be seen that after DNA was immobilized, the drain current was significantly increased, improving device performance.
The transfer characteristic curve of the organic field effect transistor in which no DNA was immobilized on the source-drain electrode 4, i.e., the Au surface, and the Au surface was treated with SH-ssDNA at a gate voltage of-50V is shown in FIG. 4. It can be seen that the threshold voltage of the two samples is significantly enhanced, and that of the untreated sample of gold electrode is-17V. After the source and drain electrodes 4 are modified by SH-ssDNA, the threshold voltage is reduced to-10V due to the reduction of the injection barrier between the metal electrode and the organic active layer. Studies have shown that phosphate groups on the DNA backbone create a net negative charge in the DNA molecule, thereby attracting holes on the semiconductor, increasing the tunneling probability of charge injection. Therefore, the SH-ssDNA is fixed on the source and drain electrodes 4, so that the injection characteristic can be improved, the saturation current and the carrier mobility of the sensor can be enhanced, and the sensitivity of the DNA sensor can be improved.
Example 2:
the structure of the DNA sensor in this example is substantially the same as that of example 1, except that:
in this embodiment, referring to fig. 5, a substrate 1, a gate electrode 2, an insulating layer 3, and a semiconductor layer 5 are sequentially connected, then a source/drain electrode 4 is fabricated on the semiconductor layer 5 to form a bottom-gate top contact structure, and finally a DNA molecular probe is fixed on the source/drain electrode 4.
The specific preparation method of each structural layer of the thin film transistor in this embodiment is as follows:
1) selecting heavily doped silicon wafers as a substrate 1 and a gate electrode 2, wherein the conductivity of the silicon wafers is 0.01-0.15 omega cm, and ultrasonically cleaning the substrate 1 with acetone and ethanol for fifteen minutes; after the ultrasonic treatment, the ultrasonic wave is taken out and washed by a corresponding solvent to remove adhered debris;
2) thermally oxidizing a layer of silicon dioxide with the thickness of 300nm on a silicon wafer to be used as an insulating layer 3 of a transistor; washing the silicon wafer with deionized water, and baking in a vacuum oven at 90 ℃;
3) and after the silicon wafer is cooled, putting the silicon wafer into vacuum evaporation equipment. When the vacuum pressure reaches 10-4Pa slowly heats the semiconductor layer 5 to 110 deg.C to start evaporation, and the evaporation speed is 0.05nm/s to evaporate on the silicon wafer. The substrate temperature for deposition of the semiconductor layer 5 is maintained at 70 ℃;
4) after the film temperature is cooled to room temperature, a gold electrode is quickly evaporated by using a mask method to be used as a source electrode and a drain electrode 4 of the transistor, and the length of a channel is determined to be 180 mu m and the width is determined to be 3800 mu m;
5) preparing PBS buffer solution containing Na as main ingredient2HPO4、NaH2PO4NaCl, KCl, pH 7.4, and the ssDNA probe used was dissolved in PBS buffer solution. Dripping PBS solution containing ssDNA onto the source and drain electrodes 4 to realize the fixation of the ssDNA molecular probe 6;
6) and washing the thin film transistor by adopting a large amount of deionized water, removing residual ions in the solution, finally placing the thin film transistor device into a vacuum cavity, and naturally drying for 8 hours.
In this embodiment, ssDNA molecular probes 6 are physically immobilized on the source and drain electrodes 4 of the thin film transistor device, formed by gathering ssDNA molecules together by van der waals force, and a bias voltage is applied between the source and drain electrodes while the ssDNA is immobilized, and the electrical properties of the ssDNA are measured using a test device.
Comparative example:
referring to the method of embodiment 2, a DNA sensor based on a thin film transistor shown in fig. 6 is prepared, where the DNA sensor includes a thin film transistor and a DNA molecular probe 6, the thin film transistor includes a substrate 1, a gate electrode 2, an insulating layer 3, source and drain electrodes 4 and a semiconductor layer 5, the substrate 1, the gate electrode 2 and the insulating layer 3 are sequentially disposed from bottom to top, the semiconductor layer 5 is disposed on the insulating layer 3, the source and drain electrodes 4 are in contact with the semiconductor layer 5, and the DNA molecular probe 6 is fixed on the semiconductor layer 5.
Table 1 shows device parameters of the DNA sensor based on the bottom-gate top contact structure with the source-drain electrode 4 as the substrate and the DNA sensor based on the semiconductor layer 5 as the substrate, which are prepared by using the above-described examples and comparative examples and under the given conditions of table 1.
TABLE 1
As can be seen from table 1, there is a significant variation in threshold voltage among the key parameters in the bottom contact: the threshold voltage was reduced to-10V before the immobilization of ssDNA, and the mobility did not change much when the ssDNA was immobilized, and the saturation current reached 46.74. mu.A with SH-ssDNA modification, which was twice that of the untreated sample. The changes of the parameters are generated after the ssDNA is fixed on the Au electrode, and the SH-ssDNA is fixed on the source electrode and the drain electrode to play a role in improving the charge injection characteristic, so that the sensitivity of the DNA sensor is improved. Furthermore, when the Au electrodes were treated with SH-ssDNA, the field effect mobility generated by the bottom-gate bottom contact was comparable to the level of the bottom-gate top-contact sensor fabricated with untreated source and drain electrodes at room temperature. The saturation current and mobility of the semiconductor layer-based DNA sensor are lower than those of the source-drain electrode-based sensor, and physical absorption on the semiconductor layer is sensitive to moisture and certain ions, which reduces the stability and repeatability of the DNA sensor, thereby reducing its sensitivity.
Example 3:
the DNA sensor comprises a thin film transistor and a DNA molecular probe 6, wherein the thin film transistor comprises a substrate 1, a gate electrode 2, an insulating layer 3, a source electrode, a drain electrode 4 and a semiconductor layer 5, the substrate 1, the gate electrode 2 and the insulating layer 3 are sequentially arranged from bottom to top, the semiconductor layer 5 is arranged on the insulating layer 3, the source electrode, the drain electrode 4 and the semiconductor layer 5 are in contact, and the DNA molecular probe 6 is fixed on the source electrode, the drain electrode 4.
Wherein, the source-drain electrode 4 and the semiconductor layer 5 are both arranged on the insulating layer 3, and the semiconductor layer 5 is positioned in the channel of the source-drain electrode 4.
The substrate 1 is made of an insulating material or a composite material formed by covering a layer of insulating material on the surface of a conductive material.
The gate electrode 2 is made of one or more of gold, aluminum, copper, titanium, silver, or heavily doped silicon.
The material of the insulating layer 3 includes one or more of silicon dioxide, silicon nitride, aluminum oxide, titanium oxide, or polyvinyl alcohol.
The source-drain electrode 4 is made of one or more of gold, silver, copper, aluminum, magnesium, aluminum, titanium, lead, or platinum.
The material of the semiconductor layer 5 is graphene, black phosphorus, silicon alkene, metal oxide, MoS2、WS2、MoSe2、WSe2、MoTe2、WTe2、ZrS2、ZrSe2、NbSe2、NbS2、TaS2、NiSe2、GaSe、GaTe、InSe、ReTe2、TiTe2、NbTe2Or SnTe2。
The DNA molecular probe 6 is a ssDNA molecular probe or a dsDNA molecular probe.
The preparation method of the DNA sensor based on the thin film transistor comprises the following steps:
1) preparing a gate electrode 2 on the surface of a substrate 1 by adopting an evaporation or sputtering method;
2) manufacturing an insulating layer 3 on the gate electrode 2 by adopting an evaporation method;
3) depositing a source drain electrode 4 and a semiconductor layer 5, and fixing a DNA molecular probe 6 on the surface of the source drain electrode 4 by a physical adsorption, bonding or self-assembly method.
Example 4:
in this embodiment, the source-drain electrodes 4 are provided on the semiconductor layer 5, which is otherwise the same as embodiment 4.
The embodiments described above are described to facilitate an understanding and use of the invention by those skilled in the art. It will be readily apparent to those skilled in the art that various modifications to these embodiments may be made, and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above embodiments, and those skilled in the art should make improvements and modifications within the scope of the present invention based on the disclosure of the present invention.
Claims (10)
1. The DNA sensor based on the thin film transistor is characterized by comprising the thin film transistor and a DNA molecular probe (6), wherein the thin film transistor comprises a substrate (1), a gate electrode (2), an insulating layer (3), a source drain electrode (4) and a semiconductor layer (5), the substrate (1), the gate electrode (2) and the insulating layer (3) are sequentially arranged from bottom to top, the semiconductor layer (5) is arranged on the insulating layer (3), the source drain electrode (4) is in contact with the semiconductor layer (5), and the DNA molecular probe (6) is fixed on the source drain electrode (4).
2. The thin film transistor-based DNA sensor according to claim 1, wherein the source and drain electrodes (4) and the semiconductor layer (5) are both disposed on the insulating layer (3), and the semiconductor layer (5) is located in the channel of the source and drain electrodes (4).
3. The thin film transistor-based DNA sensor according to claim 1, wherein the source and drain electrodes (4) are disposed on the semiconductor layer (5).
4. The thin film transistor-based DNA sensor according to claim 1, wherein the substrate (1) is made of an insulating material or a composite material formed by covering a layer of insulating material on the surface of a conductive material.
5. The thin film transistor-based DNA sensor of claim 1, wherein the gate electrode (2) comprises one or more of gold, aluminum, copper, titanium, silver or heavily doped silicon.
6. The thin film transistor-based DNA sensor according to claim 1, wherein the insulating layer (3) is made of one or more materials selected from silicon dioxide, silicon nitride, aluminum oxide, titanium oxide and polyvinyl alcohol.
7. The thin film transistor-based DNA sensor according to claim 1, wherein the source and drain electrodes (4) are made of one or more of gold, silver, copper, aluminum, magnesium, aluminum, titanium, lead or platinum.
8. The thin film transistor-based DNA sensor according to claim 1, wherein the semiconductor layer (5) is made of stoneGraphene, black phosphorus, silylene, metal oxide, MoS2、WS2、MoSe2、WSe2、MoTe2、WTe2、ZrS2、ZrSe2、NbSe2、NbS2、TaS2、NiSe2、GaSe、GaTe、InSe、ReTe2、TiTe2、NbTe2Or SnTe2。
9. The thin film transistor-based DNA sensor of claim 1, wherein the DNA molecular probes (6) are ssDNA molecular probes or dsDNA molecular probes.
10. A method for preparing a thin film transistor-based DNA sensor according to any one of claims 1 to 9, comprising the steps of:
1) preparing a gate electrode (2) on the surface of a substrate (1) by adopting an evaporation or sputtering method;
2) manufacturing an insulating layer (3) on the gate electrode (2) by adopting an evaporation method;
3) depositing a source drain electrode (4) and a semiconductor layer (5), and fixing a DNA molecular probe (6) on the surface of the source drain electrode (4) by a physical adsorption, bonding or self-assembly method.
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