CN114883195A - Preparation method of two-dimensional material semiconductor device for detecting target DNA - Google Patents

Preparation method of two-dimensional material semiconductor device for detecting target DNA Download PDF

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CN114883195A
CN114883195A CN202210347375.XA CN202210347375A CN114883195A CN 114883195 A CN114883195 A CN 114883195A CN 202210347375 A CN202210347375 A CN 202210347375A CN 114883195 A CN114883195 A CN 114883195A
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叶宇
梅继新
陈娇
徐浪浪
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Abstract

The invention discloses a preparation method of a two-dimensional material semiconductor device for detecting target DNA, which comprises the following steps: a back gate electrode and a gate dielectric layer are sequentially prepared on the substrate from bottom to top; transferring the prepared molybdenum disulfide to a gate dielectric layer, preparing a source electrode and a drain electrode on the upper surface of the molybdenum disulfide, and forming a channel region between the source electrode and the drain electrode; pouring the prepared PDMS colloid into a mold, heating and curing to form a PDMS channel, stripping the PDMS channel from the mold, and then hot-pressing the PDMS channel to a channel region; injecting PBS solution containing DNA probes into one end of the PDMS channel, standing for a period of time, continuously injecting pure PBS solution into one end of the PDMS channel after the DNA probes are adsorbed and fixed on the surface of the molybdenum disulfide in the PDMS channel, and simultaneously pumping out the PBS solution from the other end of the PDMS channel by a vacuum pump until the PBS solution in the PDMS channel does not suspend the DNA probes. The invention can realize high specificity and high sensitivity detection of target DNA molecules with lower concentration under the condition of not needing to label a DNA probe.

Description

Preparation method of two-dimensional material semiconductor device for detecting target DNA
Technical Field
The invention belongs to the technical field of semiconductor devices, and particularly relates to a preparation method of a two-dimensional material semiconductor device for detecting target DNA.
Background
DNA molecules are important components of biological genetic materials, carry genetic information necessary for synthesizing RNA and protein, and play an important role in aspects of genetic information storage, life function regulation and the like. In recent years, with the development of life sciences and biotechnology, especially the development of DNA sequencing technology and the completion of human genome project, people are gradually aware that the detection of specific DNA molecular sequences has important application value in the fields of medical treatment, agriculture, environmental monitoring, judicial identification, and the like. Because the content of the target DNA sequence to be detected in an actual sample is low, the sample components are complex, and the interference factors are many, the DNA molecular detection technology is required to have the characteristics of high sensitivity and high specificity.
At present, the commonly used method for detecting the target DNA molecule sequence is to use DNA molecule hybridization technology. Complementary nucleotide sequences can form stable double-stranded DNA molecules through base pairing. Therefore, the target DNA molecule sequence can be captured by specific hybridization using the complementary DNA molecule sequence as a probe. Among them, the DNA probe must be labeled for easy tracing or detection. Usually, the DNA probe molecules are labeled by an isotope labeling method, but in recent years, DNA probes have been labeled with a non-isotope such as a steroid digoxigenin due to the influence of isotope safety. The detection method can realize high-specificity recognition by using hybridization of DNA molecules, but the detection of paired DNA molecules depends on markers, and the used scene and the detection mode need to be considered when designing the DNA probe, so the design and preparation process of the probe of the detection method are more complicated, and in most cases, the concentration of the target DNA molecule has higher requirements.
Disclosure of Invention
In view of the defects of the prior art, the invention aims to provide a preparation method of a two-dimensional material semiconductor device for detecting target DNA, which can realize high-specificity and high-sensitivity detection of target DNA molecules with lower concentration under the condition of not needing a labeled DNA probe.
In order to achieve the above object, in a first aspect, the present invention provides a method for manufacturing a two-dimensional material semiconductor device for detecting a target DNA, comprising the steps of:
(1) preparing a back gate electrode on a substrate, and depositing a gate dielectric layer on the back gate electrode;
(2) transferring the prepared molybdenum disulfide to the gate dielectric layer, preparing a source electrode and a drain electrode on the upper surface of the molybdenum disulfide through a photoetching process and electron beam evaporation, and forming a channel region between the source electrode and the drain electrode;
(3) pouring the prepared PDMS colloid into a mold, heating and curing to form a PDMS channel, peeling the PDMS channel from the mold, and then hot-pressing the PDMS channel to a channel region to form a two-dimensional material semiconductor device to be biologically modified;
(4) injecting PBS solution containing DNA probes into one end of the PDMS channel, standing for a period of time, continuously injecting pure PBS solution into one end of the PDMS channel after the DNA probes are adsorbed and fixed on the surface of the molybdenum disulfide in the PDMS channel, and simultaneously pumping out the PBS solution from the other end of the PDMS channel by a vacuum pump until the PBS solution in the PDMS channel does not suspend the DNA probes.
According to the preparation method of the two-dimensional material semiconductor device for detecting the target DNA, provided by the invention, the molybdenum disulfide is formed on the gate dielectric layer when the semiconductor device is prepared, the DNA probe and the semiconductor device are combined together by utilizing the material characteristics of the molybdenum disulfide, and on the basis of realizing high-specificity detection on target DNA molecules by utilizing the DNA probe, the high-sensitivity detection on the target DNA molecules is realized by combining the excellent electrical properties of the two-dimensional material semiconductor device, namely, obvious electrical response can be generated under the target DNA molecules with lower concentration. The DNA probe used in the invention does not need a marker, the design of the probe molecule is simpler, the test does not depend on a complex instrument, whether the target DNA exists can be directly judged through the change of the source-drain current of the two-dimensional material semiconductor device, and the DNA molecule and the DNA probe can be degraded by DNA enzyme and removed by PBS buffer solution after the use, so that the device can be reused.
In one embodiment, in step (2), the chemical vapor deposition-grown molybdenum disulfide is transferred onto the gate dielectric layer by using a wet transfer process, or the mechanically stripped molybdenum disulfide is transferred onto the gate dielectric layer from the polydimethylsiloxane by using a dry transfer process.
In one embodiment, before step (3), further comprising:
and respectively spin-coating covering photoresist on the surfaces of the source electrode and the drain electrode, and patterning by adopting a photoetching process to reserve a part of channel regions.
In one embodiment, before step (4), further comprising:
and carrying out thermal annealing treatment on the two-dimensional material semiconductor device to be biologically modified.
In one embodiment, in the step (4), the step of pouring the prepared PDMS colloid into the mold and heating and curing the PDMS colloid to form the PDMS channel includes:
mixing a PDMS reagent and a curing agent in a mass ratio of 10: 1 to form a mixture;
uniformly stirring the mixture, and pouring the uniformly stirred mixture into a culture dish;
placing the culture dish in a vacuum cabinet, and vacuumizing to remove gas in the mixture to obtain a prepared PDMS colloid;
spin-coating photoresist on a silicon wafer with silicon oxide, patterning by photoetching, and etching by using a sodium hydroxide solution to obtain a mold;
removing the residual photoresist by using acetone or dimethylformamide solution, then pouring the prepared PDMS colloid onto a mould, and then putting the mould into a hot substrate or an oven for drying, shaping and curing to form the PDMS channel.
In one embodiment, in step (4), the step of hot pressing the PDMS channel onto the partial channel region after being peeled off from the mold comprises:
peeling the PDMS channels off the mold;
processing the stripped PDMS channel by oxygen plasma;
and transferring and hot-pressing the stripped PDMS channel on the partial channel region by using a thermal bonding and dry transfer process.
In one embodiment, the oxygen plasma treatment time of the stripped PDMS channels is controlled within 10 minutes.
In one embodiment, step (1) comprises:
spin-coating photoresist on a silicon wafer with silicon oxide, and evaporating by utilizing a photoetching process and an electron beam process to obtain a patterned back gate electrode;
and depositing a layer of aluminum oxide on the back gate electrode by utilizing an atomic layer deposition process to serve as a gate dielectric layer.
In a second aspect, the invention provides a two-dimensional material semiconductor device, which is prepared by the preparation method of the two-dimensional material semiconductor device for detecting the target DNA.
According to the two-dimensional material semiconductor device for detecting the target DNA, provided by the invention, the molybdenum disulfide is formed on the grid dielectric layer, the DNA probe and the semiconductor device are combined together by utilizing the material characteristics of the molybdenum disulfide, and on the basis of realizing high-specificity detection on the target DNA molecules by utilizing the DNA probe, the high-sensitivity detection on the target DNA molecules is realized by combining the excellent electrical properties of the two-dimensional material semiconductor device, namely, the obvious electrical response can be generated under the target DNA molecules with lower concentration. The DNA probe used in the invention does not need a marker, the design of the probe molecule is simpler, the test does not depend on a complex instrument, whether the target DNA exists can be directly judged through the change of the source-drain current of the two-dimensional material semiconductor device, and the DNA molecule and the DNA probe can be degraded by DNA enzyme and removed by PBS buffer solution after the use, so that the device can be reused.
In a third aspect, the invention provides a two-dimensional material field effect transistor array, which includes a plurality of two-dimensional material semiconductor devices for detecting target DNA, wherein each two-dimensional material semiconductor device is arranged in an array, PDMS channels in each two-dimensional material semiconductor device are arranged in an isolated manner, and different DNA probes are adsorbed and fixed on the surfaces of molybdenum disulfide in the PDMS channels in each two-dimensional material semiconductor device.
The two-dimensional material field effect transistor array provided by the invention comprises a two-dimensional material semiconductor device for detecting target DNA, which is prepared by a two-dimensional material semiconductor device preparation method, and on the basis of realizing high-specificity detection on DNA molecules to be detected by using a DNA probe, the two-dimensional material field effect transistor array combines the excellent electrical properties of the two-dimensional material semiconductor device to realize high-sensitivity detection on the DNA molecules to be detected, namely, the two-dimensional material field effect transistor array can generate obvious electrical response under the condition of lower-concentration DNA molecules to be detected. The DNA probe used in the invention does not need a marker, the design of probe molecules is simpler, the test does not depend on complex instruments, whether the DNA to be tested exists or not can be directly judged through the change of source-drain current of the two-dimensional material semiconductor device, and after the use is finished, the DNA molecules to be tested and the DNA probe can be degraded through DNA enzyme and removed by PBS buffer solution, so that the device can be reused.
Drawings
FIG. 1 is a flowchart of a method for manufacturing a two-dimensional material semiconductor device for detecting a target DNA in one embodiment;
FIG. 2 is a schematic structural view of a two-dimensional material semiconductor device in which a target DNA is detected by the method of manufacturing a two-dimensional material semiconductor device in FIG. 1;
FIG. 3 is a flow chart illustrating the preparation of PDMS channels in one embodiment;
FIG. 4 is a flowchart of step S40 in one embodiment.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
The traditional method for detecting the target DNA molecule sequence adopts a complementary DNA molecule sequence as a probe, and utilizes the principle of a DNA molecule hybridization technology to realize the high specificity detection of the target DNA molecule. However, the traditional target DNA detection method requires labeling of the DNA probe, and has high requirements for the concentration of the target DNA molecule to be detected.
In order to solve the above problems, the present invention provides a method for preparing a two-dimensional material semiconductor device for detecting a target DNA, as shown in fig. 1 and 2, the method for preparing a two-dimensional material semiconductor device includes a semiconductor device preparation step, a PDMS channel preparation and transfer step, and a two-dimensional material surface biological modification step.
The semiconductor device manufacturing steps provided by the present embodiment include steps S10 and S20, which are detailed as follows:
s10, sequentially preparing the back gate electrode 10 and the gate dielectric layer 20 from bottom to top on the substrate, that is, firstly preparing the back gate electrode 10 on the substrate, and then depositing the gate dielectric layer 20 on the back gate electrode.
In this embodiment, step S10 can be prepared by a preparation process commonly used in the art, such as: firstly, photoresist is spin-coated on a silicon wafer with silicon oxide, then a patterned back gate electrode is obtained by utilizing a photoetching process and electron beam evaporation, namely, the photoresist is patterned by the photoetching process, then a metal electrode is evaporated on a silicon substrate by utilizing an Electron Beam Evaporation (EBE) process, and finally the silicon wafer is soaked in acetone or dimethyl formamide (DMF) solution to remove the photoresist, so that a back gate electrode 10 is obtained; and then depositing a layer of aluminum oxide on the back gate electrode 10 by using an atomic layer deposition process to serve as a gate dielectric layer 20.
S20, transferring the prepared molybdenum disulfide 30 onto the gate dielectric layer 20, and preparing source and drain electrodes on the upper surface of the molybdenum disulfide 30 by photolithography and electron beam evaporation, and forming a channel region between the source electrode 40a and the drain electrode 40 b. Specifically, the preparation process of the source electrode and the drain electrode mentioned in this embodiment may refer to the detailed description of the preparation process of the back gate electrode 10, and is not described again in this embodiment.
The molybdenum disulfide 30 formed on the gate dielectric layer 20 in this embodiment has the following advantages: 1) the molybdenum disulfide is an n-type semiconductor material, is a channel material for preparing a semiconductor device, has excellent electrical properties, is small in size, is only several atomic layers thick, is 0.65nm thick in a single layer, is compatible with a silicon-based CMOS (complementary metal oxide semiconductor) process, and can be used for preparing a large-scale array device; 2) the surface of the molybdenum disulfide lacks oxygen-containing functional groups, so that the molybdenum disulfide material is relatively stable in an electrolyte solution and is insensitive to a PH value, and further the electrical property of the prepared semiconductor device is more stable; 3) the molybdenum disulfide 30 can also adsorb and fix DNA probes used in the subsequent two-dimensional material surface modification step through deoxyribonucleic acid base and Van der Waals force action of DNA.
Specifically, in this embodiment, the manner of transferring the prepared molybdenum disulfide 30 onto the gate dielectric layer 20 may be: formed by chemical vapor deposition and then transferred to the gate dielectric layer 20 by a wet transfer process. Firstly, growing molybdenum disulfide on a metal matrix through chemical vapor deposition, then spin-coating a polymethyl methacrylate (PMMA) film on the surface of the molybdenum disulfide by using a spin coater, and heating to cure the film; then placing the metal substrate into an etching solution, etching the metal substrate and drying the metal substrate; finally, the composite of molybdenum disulfide and the PMMA film is placed on the gate dielectric layer 20 provided in this embodiment, and the PMMA film is removed by cleaning with acetone, thereby completing the transfer step. In this embodiment, the PMMA film can play a role in protecting molybdenum disulfide at this time as a transfer medium, and large-scale transfer of molybdenum disulfide can be completed by using this transfer method, which is suitable for producing semiconductor devices of arrays.
Of course, it is also possible to transfer the mechanically exfoliated molybdenum disulfide from the Polydimethylsiloxane (PDMS) onto the gate dielectric layer 20 by a dry transfer process (e.g., a transfer platform) in a more straightforward manner. The transfer mode mainly comprises the steps of directly pasting molybdenum disulfide on PDMS by utilizing the viscoelasticity of PDMS, then overturning the PDMS, accurately aligning by utilizing a transfer platform, attaching the molybdenum disulfide on the PDMS to the gate dielectric layer 20 provided by the embodiment, and finally slowly lifting the PDMS to complete transfer.
The PDMS channel 60 provided in this example was prepared and transferred by the following steps:
and S30, pouring the prepared PDMS colloid into a mold, heating and curing to form the PDMS channel 60, peeling the PDMS channel 60 from the mold, and then hot-pressing to the channel region to form the two-dimensional material semiconductor device to be biologically modified.
In this embodiment, the PDMS channel 60 functions as a microfluidic channel, one end of which can be injected with liquid and the other end of which can be pumped out by a vacuum pump, thereby facilitating subsequent biological modification and directional flow of liquid.
Specifically, step S30 provided in this embodiment may be: referring to fig. 3, after photoresist is spin-coated on another silicon wafer with silicon oxide and patterned by photolithography, a mold is obtained by etching with a sodium hydroxide (NaOH) solution; removing the photoresist by using acetone or DMF solution, pouring the prepared PDMS colloid on a mold, then putting the mold into a hot substrate or an oven for drying, shaping and curing to form a PDMS channel, and preferably putting the mold carrying the PDMS colloid into the hot substrate or the oven for drying at 65 ℃ for about 2 hours for shaping and curing; and finally, peeling the cured PDMS channel, transferring the PDMS channel to a channel region by using a thermal bonding and dry transfer process, and carrying out hot pressing on the PDMS channel.
In this embodiment, the prepared PDMS colloid is cast on a mold prepared by photolithography, so that a PDMS microfluidic channel with a very small size (micron order) can be obtained, and the PDMS channel can be accurately transferred to a channel region through thermal bonding and a transfer platform after being peeled off, so that the PDMS channel formed on the channel region is more suitable for microfluidics of a two-dimensional material-based nanoelectronic device. In addition, the PDMS colloid is nearly transparent after being cured, is suitable for experimental observation, and does not have great influence on the lattice interface of the nanoscale two-dimensional material in the preparation process.
Further, in order to solidify the liquid PDMS reagent into the PDMS channel that can be used for microfluidics, the mass ratio of the PDMS colloid provided in this embodiment may be (8-12): 1, specifically, the ratio can be designed according to actual conditions, and in this embodiment, a mixture of 10: 1 PDMS reagent and curing agent ratio PDMS colloids were prepared. In this embodiment, the curing agent is used to cure the PDMS agent, and specifically, dow corning DC184 silicone rubber can be used.
Considering that the bubbles generated during the mixing of the PDMS reagent and the curing agent may affect the preparation of the PDMS channels, the preparation steps of the PDMS colloid provided in this embodiment may be: referring to fig. 4, the mass ratio of PDMS reagent to curing agent is 10: 1 to form a mixture; and then stirring the mixture for 5-10 minutes by using a glass rod to uniformly mix the mixture, pouring the uniformly stirred mixture into a culture dish, standing for 1-2 hours until bubbles are discharged, and if the bubbles exist, puncturing the bubbles by using tweezers. In order to discharge air bubbles in the mixture more quickly, the culture dish loaded with the mixture can be placed in a vacuum cabinet to be vacuumized so as to remove air in the mixture.
The two-dimensional material surface biological modification steps provided by the embodiment are as follows:
s40, injecting Phosphate Buffered Saline (PBS) solution containing the DNA probe 70 into one end of the PDMS channel 60, standing for a period of time, after the DNA probe 70 is adsorbed and immobilized on the surface of the molybdenum disulfide in the PDMS channel 60, continuously injecting pure PBS solution into one end of the PDMS channel 60, and simultaneously pumping out the PBS solution from the other end of the PDMS channel 60 by a vacuum pump until the PBS solution in the PDMS channel 60 has no DNA probe suspended.
The PBS solution provided by this embodiment is mainly used to maintain the biological activity of the DNA molecules (DNA probes and target DNA), and in order to optimize the biological activity of the DNA molecules, the PBS solution provided by this embodiment can be 0.1 × PBS solution.
Specifically, step S40 provided in this embodiment may be: injecting a PBS solution containing the DNA probe from one end of the PDMS channel 60 by adopting a needle injection mode, standing for 16 hours, and fixing the DNA probe through physical adsorption on the surface of molybdenum disulfide in the PDMS channel 60; then, pure PBS solution is continuously injected into one end of the PDMS channel 60 to remove the remaining DNA probes and connect unstable DNA probes to prevent the DNA probes from being adsorbed on the surface of the channel again, which interferes with the results of the subsequent experimental tests, and the PBS solution is pumped out at the other end of the PDMS channel 60 by a vacuum pump until the PBS solution in the PDMS channel 60 has no DNA probes suspended.
When the two-dimensional material semiconductor device prepared by the preparation method of the two-dimensional material semiconductor device provided by the embodiment is used for detecting target DNA molecules (specific DNA molecules), a voltage needs to be applied between the back gate electrode 10 and the source electrode 40a of the semiconductor device; then injecting a PBS solution containing the target DNA to be detected into the PDMS channel 60 through one end of the PDMS channel 60; the detection of the target DNA can be realized by detecting the current change of the source electrode 40a and the drain electrode 40b in the semiconductor device in real time.
The detection principle is as follows: in the process of biologically modifying the surface of the two-dimensional material, when the DNA probe 70 is adsorbed on the surface of the molybdenum disulfide 30, the current is reduced due to the electrostatic doping of the DNA probe 70 to the channel; and after the target DNA molecule is hybridized with the DNA probe, the DNA probe is desorbed, and the current rises, so that after the biological modification of the molybdenum disulfide surface is finished, if the current is increased, the target DNA molecule can be judged to be hybridized with the DNA probe, and the detection of the target DNA is realized. Specific examples are: when the target DNA molecules with the concentration of 100fm are introduced under the back gate voltage of 5V and the source-drain bias voltage of 0.1V, the source-drain current rises from about 1 microampere to 2 microampere.
According to the preparation method of the two-dimensional material semiconductor device for detecting the target DNA, the molybdenum disulfide 30 is formed on the gate dielectric layer 20 when the semiconductor device is prepared, the material characteristics of the molybdenum disulfide 30 are utilized to combine the DNA probe and the semiconductor device, and on the basis of realizing high-specificity detection of target DNA molecules by utilizing the DNA probe, the high-sensitivity detection of the target DNA molecules is realized by combining the excellent electrical properties of the two-dimensional material semiconductor device, namely, obvious electrical response can be generated under the target DNA molecules with lower concentration. The DNA probe used in the embodiment does not need a marker, the design of the probe molecule is simpler, the test does not depend on a complex instrument, whether the target DNA exists can be directly judged through the change of source-drain current of the two-dimensional material semiconductor device, the DNA molecule and the DNA probe can be degraded through DNA enzyme and removed by PBS buffer solution after the use is finished, and the device can be reused.
In one embodiment, before performing the biological modification on the two-dimensional material device, that is, before performing step S40 provided in the foregoing embodiment, a thermal annealing process may be performed on the two-dimensional material semiconductor device to be subjected to the biological modification, so as to improve the contact between the source/drain electrodes and the channel.
In one embodiment, when the PDMS channel 60 is transferred to the channel region within 10 minutes after the oxygen plasma treatment, the weak bonding of the PDMS channel 60 can be prevented from causing leakage of the injected PBS solution in the PDMS channel 60.
Further, in order to prevent the PBS solution injected into the PDMS channel 60 from penetrating into the source and drain electrodes of the semiconductor device, a layer of photoresist 50 may be spin-coated on the source and drain electrodes to isolate the liquid before the PDMS channel 60 is transferred to the channel region, and a part of the channel region is reserved by using photolithography patterning, and then the prepared PDMS channel 60 is transferred to the part of the channel region, thereby completing the preparation of the two-dimensional material semiconductor device to be biologically modified.
In one embodiment, the back gate electrode 10, the source electrode 40a and the drain electrode 40b provided by the present embodiment may use 10nm/60nmCr/Au, and use Cr/Au may improve contact resistance, and the thickness is selected for good adhesion. The thickness of the aluminum oxide in the gate dielectric layer 20 can be set to 30nm, wherein the aluminum oxide is a high-K gate dielectric, and the aluminum oxide is used as the gate dielectric layer, so that the thickness of the oxide layer can be reduced, and the applied gate voltage can be reduced.
As shown in FIG. 2, the invention provides a two-dimensional material semiconductor device for detecting target DNA, which is prepared by the preparation method of the two-dimensional material semiconductor device for detecting target DNA.
The application scenario of the two-dimensional material semiconductor device for detecting the target DNA provided by the embodiment is as follows: 1) in the judicial identification process, residual DNA sequences on the testimony can be used for designing DNA probes and screening matchers on a large scale to confirm criminal suspects; 2) the early detection and diagnosis of diseases and the like according to tumor genes are suitable for early screening of diseases; 3) the method is applied to food safety detection work, can effectively detect a specific DNA sequence, and particularly can powerfully guarantee the accuracy in the aspects of denaturation, renaturation, basic group and the like. For example, in the detection of Escherichia coli, Salmonella, Staphylococcus aureus, etc. in food, it is possible to design a complementary sequence probe of a target DNA based on the fact that the DNA is a main genetic material of bacteria, and then to determine whether or not food contains a large amount of Escherichia coli, Salmonella, etc. in accordance with a DNA sequence specific to a microorganism to be detected.
According to the two-dimensional material semiconductor device for detecting the target DNA, the molybdenum disulfide 30 is formed on the gate dielectric layer 20, the DNA probe and the semiconductor device are combined together by utilizing the material characteristics of the molybdenum disulfide 30, and on the basis of realizing high-specificity detection on the target DNA molecules by utilizing the DNA probe, the high-sensitivity detection on the target DNA molecules is realized by combining the excellent electrical properties of the two-dimensional material semiconductor device, namely, obvious electrical response can be generated under the target DNA molecules with lower concentration. The DNA probe used in the embodiment does not need a marker, the design of the probe molecule is simpler, the test does not depend on a complex instrument, whether the target DNA exists can be directly judged through the change of source-drain current of the two-dimensional material semiconductor device, the DNA molecule and the DNA probe can be degraded through DNA enzyme and removed by PBS buffer solution after the use is finished, and the device can be reused.
Based on the same inventive concept, the invention also provides a two-dimensional material field effect transistor array which can realize the detection of different DNA molecules to be detected, the two-dimensional material field effect transistor array comprises a plurality of two-dimensional material semiconductor devices for detecting the target DNA, the two-dimensional material semiconductor devices are prepared by the preparation method of the two-dimensional material semiconductor devices for detecting the target DNA, the two-dimensional material semiconductor devices are arranged in an array manner, PDMS channels in the two-dimensional material semiconductor devices are arranged in an isolated manner, and different DNA probes are adsorbed and fixed on the surfaces of molybdenum disulfide in the PDMS channels in the two-dimensional material semiconductor devices.
The two-dimensional material field effect transistor array provided by the embodiment comprises a two-dimensional material semiconductor device for detecting target DNA, which is prepared by a two-dimensional material semiconductor device preparation method, and on the basis of realizing high-specificity detection on DNA molecules to be detected by using a DNA probe, high-sensitivity detection on the DNA molecules to be detected is realized by combining the excellent electrical properties of the two-dimensional material semiconductor device, namely, obvious electrical response can be generated under the condition of lower-concentration DNA molecules to be detected. The DNA probe used in the embodiment does not need a marker, the design of probe molecules is simpler, the test does not depend on a complex instrument, whether the DNA to be tested exists or not can be directly judged through the change of source-drain current of the two-dimensional material semiconductor device, after the use is finished, the DNA molecules to be tested and the DNA probe can be degraded through DNA enzyme and removed by PBS buffer solution, and the device can be reused.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.

Claims (10)

1. A preparation method of a two-dimensional material semiconductor device for detecting target DNA is characterized by comprising the following steps:
(1) preparing a back gate electrode on a substrate, and depositing a gate dielectric layer on the back gate electrode;
(2) transferring the prepared molybdenum disulfide to the gate dielectric layer, preparing a source electrode and a drain electrode on the upper surface of the molybdenum disulfide through a photoetching process and electron beam evaporation, and forming a channel region between the source electrode and the drain electrode;
(3) pouring the prepared PDMS colloid into a mold, heating and curing to form a PDMS channel, peeling the PDMS channel from the mold, and then hot-pressing the PDMS channel to a channel region to form a two-dimensional material semiconductor device to be biologically modified;
(4) injecting PBS solution containing DNA probes into one end of the PDMS channel, standing for a period of time, continuously injecting pure PBS solution into one end of the PDMS channel after the DNA probes are adsorbed and fixed on the surface of the molybdenum disulfide in the PDMS channel, and simultaneously pumping out the PBS solution from the other end of the PDMS channel by a vacuum pump until the PBS solution in the PDMS channel does not suspend the DNA probes.
2. The method for manufacturing a two-dimensional material semiconductor device according to claim 1, wherein in the step (2), the chemical vapor deposition-grown molybdenum disulfide is transferred onto the gate dielectric layer by using a wet transfer process, or the mechanically stripped molybdenum disulfide is transferred onto the gate dielectric layer from the polydimethylsiloxane by using a dry transfer process.
3. The method for manufacturing a two-dimensional material semiconductor device for detecting a target DNA according to claim 1, further comprising, before the step (3):
and respectively spin-coating covering photoresist on the surfaces of the source electrode and the drain electrode, and patterning by adopting a photoetching process to reserve a part of channel regions.
4. The method for preparing a two-dimensional material semiconductor device for detecting target DNA according to claim 1, wherein before the step (4), the method further comprises:
and carrying out thermal annealing treatment on the two-dimensional material semiconductor device to be biologically modified.
5. The method for preparing a two-dimensional material semiconductor device for detecting target DNA according to claim 1, wherein in the step (3), the step of pouring the prepared PDMS colloid into a mold and heating for curing to form the PDMS channel comprises:
the method comprises the following steps of (1) mixing a PDMS reagent and a curing agent in a mass ratio of (8-12): 1 to form a mixture;
uniformly stirring the mixture, and pouring the uniformly stirred mixture into a culture dish;
placing the culture dish in a vacuum cabinet, and vacuumizing to remove gas in the mixture to obtain a prepared PDMS colloid;
spin-coating photoresist on a silicon wafer with silicon oxide, patterning by photoetching, and etching by using a sodium hydroxide solution to obtain a mold;
removing the residual photoresist by using acetone or dimethylformamide solution, then pouring the prepared PDMS colloid onto a mould, and then putting the mould into a hot substrate or an oven for drying, shaping and curing to form the PDMS channel.
6. The method for preparing a two-dimensional material semiconductor device for detecting target DNA according to claim 3, wherein in the step (3), the step of hot-pressing the PDMS channels onto the partial channel regions after being stripped from the mold comprises:
peeling the PDMS channels off the mold;
processing the stripped PDMS channel by oxygen plasma;
and transferring and hot-pressing the stripped PDMS channel on the partial channel region by using a thermal bonding and dry transfer process.
7. The method for preparing a two-dimensional material semiconductor device for detecting target DNA according to claim 6, wherein the time for processing the stripped PDMS channel by the oxygen plasma is controlled within 10 minutes.
8. The method for preparing a two-dimensional material semiconductor device for detecting target DNA according to claim 1, wherein the step (1) is implemented by the following steps:
spin-coating photoresist on a silicon wafer with silicon oxide, and evaporating by utilizing a photoetching process and an electron beam process to obtain a patterned back gate electrode;
and depositing a layer of aluminum oxide on the back gate electrode by utilizing an atomic layer deposition process to serve as a gate dielectric layer.
9. A two-dimensional material semiconductor device for detecting a target DNA, characterized by being prepared by the method for preparing a two-dimensional material semiconductor device for detecting a target DNA according to any one of claims 1 to 8.
10. A two-dimensional material field effect transistor array, comprising a plurality of two-dimensional material semiconductor devices for detecting target DNA as claimed in claim 9, wherein each of the two-dimensional material semiconductor devices is arranged in an array, PDMS channels in each of the two-dimensional material semiconductor devices are isolated, and different DNA probes are adsorbed and fixed on the surface of molybdenum disulfide in the PDMS channels in each of the two-dimensional material semiconductor devices.
CN202210347375.XA 2022-04-03 2022-04-03 Preparation method of two-dimensional material semiconductor device for detecting target DNA Pending CN114883195A (en)

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