CN111755600B - Memristor based on composite nanowire network structure - Google Patents
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Abstract
The invention provides a memristor based on a composite nanowire network structure, which sequentially comprises a bottom electrode layer, a composite nanowire network structure layer and a top electrode layer from bottom to top; the method is characterized in that: the composite nanowire network structure layer has the function of serving as a resistance change function layer and comprises an oxygen-doped nitride nanowire and a nanowire coating layer, wherein the bottom end of the oxygen-doped nitride nanowire is connected with one side of a bottom electrode layer; the nanowire coating layer completely coats the top end and the side face of the nanowire, and the nanowire coating layer is connected with the top electrode layer. The advantages are as follows: the structural device shows stable memristor characteristics and learning and forgetting characteristics, and a research path is provided for the research of a memristor in a memristor mechanism and the optimization of device performance. And has high structural stability and excellent electrical properties. The preparation method is simple, low in cost and excellent in performance, is widely applied to the fields of high-density storage calculation, artificial synapse simulation, artificial intelligence and the like, and is favorable for exploring a novel brain-like nerve working mechanism.
Description
Technical Field
The invention relates to a memristor based on a composite nanowire network structure, and the device has the characteristics of stability, low energy consumption, learning and forgetting, and belongs to the technical field of brain-like computing devices.
Background
With the increasing demand of people for computing performance, a new electronic device with brain-like learning and memory functions has become a research hotspot. The emergence of artificial intelligence brings great innovation for the development of new technology. Artificial intelligence is the subject of research that has led computers to simulate certain mental processes and intelligent behaviors of humans (e.g., learning, reasoning, thinking, planning, etc.). The neural network constructed based on the memristor is an important way for realizing artificial intelligence. The memristor has the advantages of nonvolatility, simple structure, low power consumption, high running speed and the like, so that the development of the artificial synapse with high performance is possible. In addition, the memristor has the characteristics of being compatible with COMS devices and the like. Therefore, the memristor based on the neural network has wide application prospects in the aspects of realizing high-density storage calculation, neuromorphic calculation and the like.
At present, memristors based on different materials, different structural types, and different operating mechanisms have been extensively studied. From the aspect of material systems, the material systems are mainly divided into sulfide, oxide, nitride, perovskite, two-dimensional materials, organic thin films and the like; from the aspect of structure types, the memristor is mainly divided into a double-end memristor and a three-end memristor; from the aspect of mechanism types, the mechanism types are mainly divided into a conductive filament mechanism, a boundary migration mechanism, an oxidation-reduction mechanism, a phase change mechanism and the like; from the aspect of material dimension, the method is mainly divided into continuous conductance behavior, quantum conductance behavior and the like. However, the memristor still faces many problems in application, such as unclear resistance change mechanism, difficult performance regulation and the like. For example: based on the conductive filament type memristor, due to the phenomena of random generation, breakage and the like of the conductive filament, the memristor shows great fluctuation in the aspect of stability, and further the application of the memristor in the aspect of artificial synapse is limited; the non-conductive filament type memristor limits further application in the calculation of the neuromorphism at the cost of low on-off ratio and poor low-resistance state retention time. Through research on various structures of the resistive layer, different structures have been found to be effective in improving the instability of the memristor, such as porous materials, layered materials, sheet materials and the like. However, for the memristor made of the one-dimensional nanowire material, the problems that the ion migration path is too long, the migration barrier on the surface or inside of the nanowire is too high, the preparation method is too complex and the like currently limit the further development of the memristor in the field of memristors.
Disclosure of Invention
Aiming at the existing problems of the memristor, the invention provides the memristor based on the composite nanowire network structure by combining the characteristics of the network of the one-dimensional material and according to the principle of the memristor, provides a new path for the research of the memristor mechanism, can improve the electrical performance of the memristor, shows good characteristics in the simulation aspect of artificial synapse, and provides a great application prospect for the calculation of the nerve morphology.
The invention has the difficulty that a top electrode layer and a composite nanowire network structure layer which are formed by a metal nanowire network and a device structure of the memristor which is formed by a substrate serving as a bottom electrode are designed. The layered structure material is combined with the oxygen-doped nitride nanowire, and the memristor characteristic is controlled by controlling the oxygen doping content and the thickness of the layered structure. The invention greatly simplifies the manufacturing cost of the device and the feasibility of large-scale preparation by using a simple preparation method. The invention solves the problems of poor circulation stability and high operating voltage of the one-dimensional material memristor caused by overlong migration path and overlarge migration barrier by using a novel memristor mechanism.
The invention adopts the following technical scheme:
the invention relates to a memristor based on a composite nanowire network structure, which sequentially comprises a bottom electrode layer, a composite nanowire network structure layer and a top electrode layer from bottom to top in a basic structure; the method is characterized in that: the composite nanowire network structure layer has the function of serving as a resistance change function layer and comprises an oxygen-doped nitride nanowire and a nanowire coating layer, wherein the bottom end of the oxygen-doped nitride nanowire is connected with one side of a bottom electrode layer; the nanowire coating layer completely coats the top end and the side face of the nanowire and is connected with the top electrode layer.
The oxygen-doped nitride nanowire is 0.5-100 microns in length, 5-1000 nanometers in diameter and comprises one of gallium nitride (GaN), indium nitride (InN), aluminum nitride (AlN), Boron Nitride (BN), indium gallium nitride (InGaN), aluminum gallium nitride (AlGaN) and aluminum indium nitride (AlInN), wherein the oxygen is oxygen element which exists in the nanowire in the form of oxygen ions, oxygen molecules or oxygen atoms;
wherein the nanowire coating layer is a layered structure material with the thickness of 1-50 nanometers, and the layered structure material is molybdenum sulfide (MoS)2) Molybdenum selenide (MoSe), molybdenum selenide sulfide (MoSSe), lithium cobaltate (LiCoO)3) Boron Nitride (BN).
Under the action of an electric field, oxygen elements at the interface of the oxygen-doped nitride nanowire and the nanowire coating layer can be removed/embedded from the nanowire into oxygen ions which enter the nanowire coating layer, and the oxygen ions enter the layers of the layered material to migrate, so that the electrical conductivity of the nanowire coating layer is changed. When oxygen ions enter the nanowire coating layer, the nanowire coating layer is changed from low conductivity to high conductivity; on the contrary, when oxygen ions are removed from the nanowire coating layer, the nanowire coating layer is changed from high conductivity to low conductivity, and the structure of the nanowire coating layer is not obviously changed.
The memristor based on the composite nanowire network structure comprises one of a network structure layer formed by vertical composite nanowires, a network structure layer formed by inclined composite nanowires and a network structure layer formed by bent composite nanowires; wherein the oxygen-doped nitride nanowires constituting the network structure layer are connected to each other or separated from each other.
The top electrode layer is composed of a nanowire network formed by various metal nanowires, specifically is one of networks formed by silver (Ag), gold (Au), copper (Cu) and platinum (Pt) nanowires, wherein the length of each nanowire is 5-100 micrometers, and the diameter of each nanowire is 10-200 nanometers.
The top electrode layer is prepared by a spray coating method, and the specific method comprises the following steps: preparing a solution with the concentration of 5-100 mg/ml by using metal nanowires, wherein the solution comprises water (H)2O), ethanol (C)2H6O), isopropyl alcohol (C)3H8O); placing the prepared solution into a spray gun, placing a mask plate on a substrate with a composite nanowire network structure, and spraying the prepared solution by using the spray gun, wherein the spraying time is 1-120 seconds, and the spraying distance is 5-50 cm; and (4) after the spraying is finished, putting the mixture into an oven, setting the temperature to be 50-200 ℃, and drying for 5-120 minutes. At this time, the top electrode formed by the metal nanowire network is connected with the top end of the composite nanowire structure layer, and the composite nanowire structure layer has good contact characteristics.
The bottom electrode layer mainly comprises a conductor or semiconductor substrate, wherein the conductor or semiconductor substrate comprises the following types: one of carbon (C), nickel (Ni), copper (Cu), silicon (Si) and silicon carbide (SiC), and the thickness of the material is 300-1000 microns.
The preparation method of the nanowire coating layer comprises magnetron sputtering, atomic layer deposition, electron beam deposition, electrochemical deposition, chemical vapor deposition and plasma enhanced chemical vapor deposition.
The oxygen-doped nitride nanowires in the composite nanowire network structure mainly provide support for oxygen ions and the network structure under the action of an external electric field, and the structures of various doped nitride nanowires and the network structure formed by the various doped nitride nanowires do not change obviously under the action of the external electric field.
The nanowire coating layer in the composite nanowire network structure mainly receives and stores oxygen ions under the action of an external electric field, and provides a migration path for the oxygen ions. And the structure of the various doped nitride nanowires does not change obviously under the action of an external electric field.
The composite nanowire network structure has good oxygen ion storage and migration performance.
The method for realizing the memristor effect by applying the memristor of the invention comprises the following steps:
step one, a writing process, wherein the bottom electrode layer is grounded, and continuous forward voltage is applied to the top electrode layer; under the action of an electric field, oxygen ions at the interface of the oxygen-doped nitride nanowire in the composite nanowire and the nanowire coating layer are separated from the nanowire, enter the nanowire coating layer, namely the layered structure material, undergo redox reaction with the layered structure material, fill up an electron trap generated by a vacancy in the layered structure, provide external electrons, and change the resistance state of the device into a low resistance state;
step two, erasing, namely continuously applying a continuous negative voltage to the top electrode layer; under the action of an electric field, oxygen ions in the nanowire coating layer, namely the layered material, are separated from the nanowire coating layer and enter the nanowire under the action of the electric field, so that the total number of electrons in the layered structure on the surface of the composite nanowire is reduced, electron traps are generated again, and the device is changed into a high-resistance state.
Compared with the prior art, the memristor based on the composite nanowire network structure combines the characteristic that the top nanowire network electrode and the composite nanowire network are mutually communicated, so that the structural device has lower manufacturing cost and large-scale preparation potential, and has the following advantages in terms of device functions:
1. compared with the existing one-dimensional material memristor, the composite nanowire network structure can change the original migration of the ion migration path in the whole nanowire into the migration on the surface of the short-distance nanowire, thereby being beneficial to improving the stability of the device and reducing the power consumption of the device;
2. under the action of an electric field, the nanowire coating layer, namely the layered structure material, provides a channel for transporting ions, reduces an ion migration potential barrier and fixes an ion migration path, and improves the stability of the device;
3. the external electric field is removed, and the nanowire coating layer, namely the interlayer in the layered structure material, can effectively store oxygen ions;
4. the memristive effect is generated based on the migration of oxygen ions in the oxygen-doped nanowire and the nanowire coating layer, namely the layered structure material.
5. In the memristor based on the composite nanowire network structure, the top electrode layer formed by the metal nanowire network is mutually connected with the composite nanowire network structure layer at multiple points, the effect of facilitating the composite nanowire under the top electrode is generated under the action of a continuous electric field, and the learning and forgetting phenomena of the memristor are observed.
Drawings
Fig. 1 is a structural schematic diagram of a memristor based on a composite nanowire network structure.
FIG. 2 is a schematic diagram of a single composite nanowire structure in a memristor based on a composite nanowire network structure.
FIG. 3 is a preparation technology roadmap for a composite nanowire network structure in a memristor based on the composite nanowire network structure.
Fig. 4a is a sectional FE-SEM image of a composite nanowire network structure, which is composed of tilted nanowires and bent nanowires, wherein the individual nanowires are connected or separated from each other.
Figure 4b is a view of the layered structure HR-TEM of the nanowire cladding in the composite nanowire.
FIG. 4c is a surface FE-SEM image of the top electrode layer metal electrode network.
FIG. 5 is an electrical measurement diagram of memristors of a composite nanowire network structure.
FIG. 6a is a voltage-current curve diagram with a voltage sweep range of 0V to-1.5V with continuous negative voltage applied.
FIG. 6b is a continuous scanning graph of forward voltage and voltage-current curve, wherein the voltage scanning range is 0V-1.5V.
Fig. 6c is a current-time, voltage-time diagram corresponding to the application of 7 negative-going triangular wave voltages to the device, i.e. the development of voltage-current in the time domain.
Fig. 6d is a current-time, voltage-time diagram corresponding to the application of 7 forward triangular wave voltages to the device, i.e. the development of voltage-current in the time domain.
FIG. 7 is a graph of continuous pulse measurement of a memristor of a composite nanowire network structure with a forward pulse number of 50, a pulse width of 5 milliseconds, an amplitude of 1V, and a duty cycle of 50%; the number of negative-going pulses is 50, the pulse width is 5 milliseconds, the amplitude is-1V, and the duty ratio is 50%.
The specific reference numbers in the figures are as follows:
201-a top electrode layer; 101-a composite nanowire network structure layer;
202-a bottom electrode layer; 103-nanowire cladding; 102-oxygen doped nitride nanowires.
Detailed Description
The present invention is further described in detail in conjunction with the accompanying fig. 1-7, which are intended to facilitate an understanding of the present invention, and the specific structural and functional details thereof are merely representative to illustrate exemplary embodiments and are not intended to be limiting. Thus, the invention may be embodied in many different forms and should not be construed as limited to the exemplary embodiments set forth herein, but rather should be construed to cover all modifications, equivalents, and alternatives falling within the scope of the invention.
In this embodiment, based on the "top electrode/composite nanowire network structure layer/bottom electrode" structure, as shown in fig. 1, the structure includes a top electrode layer 201, a composite nanowire network structure layer 101, and a bottom electrode layer 202 from top to bottom, where the composite nanowire network structure layer 101 is composed of a plurality of nanowires having nanowire structures shown in fig. 2, including the oxygen-doped nitride nanowires 102 and the nanowire cladding layer 103.
The structure is prepared on a substrate layer by layer from bottom to top by adopting methods of plasma-assisted chemical vapor deposition, magnetron sputtering, spraying and the like. As shown in fig. 3, the specific preparation process is as follows:
step one, selecting highly doped n-type (100) Si as a bottom electrode layer 202, sputtering a 15-nanometer gold (Au) film by magnetron sputtering, and vertically placing gallium oxide (Ga) 3g in the film2O3) Mixed powder of activated carbon (C) and Ga in a molar ratio2O3: c is 1: and 12, putting the crucible into a plasma chemical vapor deposition system.
And secondly, growing a layer of gallium nitride (GaN) nanowire on the surface of the Si through plasma chemical vapor deposition, wherein the single structure is 102.
Thirdly, growing a layer of molybdenum sulfide (MoS) on the surface of the gallium nitride nanowire with the structure of 102 layers by utilizing the magnetron sputtering technology2) The thin film is used as a nanowire coating layer, the coating layer structure of a single nanowire is 103, the composite nanowire network structure layer is manufactured to be 101, the section FE-SEM image is shown in figure 4a, and the HR-TEM image of the coating layer layered structure is shown in figure 4 b.
Covering an electrode mask on a Si sheet with a composite nanowire network structure on the structure 101 by using a spraying technology, and preparing an ethanol solution with the concentration of 20mg/ml by using silver (Ag) nanowires; putting the prepared solution into a spray gun, and spraying the prepared solution by using the spray gun, wherein the spraying time is 20 seconds, and the spraying distance is 15 centimeters; and (4) after the spraying is finished, putting the mixture into an oven, setting the temperature to be 150 ℃, and drying the mixture for 90 minutes, wherein an FE-SEM image is shown in figure 4 c.
The above devices are shown in fig. 6a, 6b, 6c and 6d using a semiconductor parametric analyzer tester. In the test process, the bottom electrode layer is grounded, and negative and positive voltages are applied to the top electrode layer silver nanowire network. Under the action of the electric field, oxygen ions migrate or migrate back to the nanowire coating layer, namely the layered molybdenum sulfide, and the resistance state of the device is changed, as shown in fig. 5.
In the learning ability test, continuous negative voltage is applied to the top electrode layer silver nanowire network, under the action of an electric field, oxygen ions in the nanowires under the top electrode can migrate to the nanowire coating layer, the number of composite nanowire structures of the nanowire coating layer rich in the oxygen ions is gradually increased, the resistance state of the device is gradually reduced, and finally a stable resistance state is formed, so that the device has the learning ability due to the easy effect, as shown in fig. 6 a.
In the forgetting capability test, continuous forward voltage is applied to the top electrode layer silver nanowire network, under the action of an electric field, oxygen ions in the nanowire coating layer below the top electrode can migrate to the nanowires, the number of composite nanowire structures of the nanowire coating layer rich in the oxygen ions is gradually reduced, the resistance state of the device is gradually increased, and finally a stable resistance state is formed, so that the device has the forgetting capability due to the easy effect, as shown in fig. 6 b.
FIGS. 6c and 6d are plots of the voltage-current cycle of FIGS. 6a and 6b, respectively, developed over time, with the solid black line representing applied voltage, the solid gray line representing the responsive current, and the abscissa time representing the maximum responsive current increasing with time under successive pulse signals, as shown in FIG. 6 c; or the maximum response current gradually decreases with time as shown in fig. 6 d.
In learning and forgetting capability tests, the device test is carried out by using a pulse signal generator and an ammeter. 50 continuous negative pulses with the pulse width of 5 milliseconds, the amplitude of-1V and the duty ratio of 50 percent are applied, 50 continuous positive pulses with the pulse width of 5 milliseconds, the amplitude of 1V and the duty ratio of 50 percent are subsequently applied, the change relation of the conductance and the pulse number is obtained, and the device shows obvious learning and forgetting capabilities as shown in figure 7.
In summary, the device exhibits significant memristive behavior and exhibits learning and forgetting capabilities.
Claims (9)
1. A memristor based on a composite nanowire network structure sequentially comprises a bottom electrode layer, a composite nanowire network structure layer and a top electrode layer from bottom to top; the method is characterized in that: the above-mentionedThe composite nanowire network structure layer has the function of serving as a resistance change function layer and comprises an oxygen-doped nitride nanowire and a nanowire coating layer, wherein the bottom end of the oxygen-doped nitride nanowire is connected with one side of a bottom electrode layer; the nanowire coating layer completely coats the top end and the side surface of the nanowire, and the nanowire coating layer is connected with the top electrode layer; the nanowire coating layer is made of a layered structure material and has the thickness of 1-50 nanometers; wherein the material with a layered structure is molybdenum sulfide (MoS)2) Molybdenum selenide (MoSe), molybdenum selenide sulfide (MoSSe), lithium cobaltate (LiCoO)3) Boron Nitride (BN).
2. The memristor based on the composite nanowire network structure, in which: the oxygen-doped nitride nanowire is 0.5-100 microns in length, 5-1000 nanometers in diameter and comprises one of gallium nitride (GaN), indium nitride (InN), aluminum nitride (AlN), Boron Nitride (BN), indium gallium nitride (InGaN), aluminum gallium nitride (AlGaN) and aluminum indium nitride (AlInN); wherein the oxygen is oxygen element which exists in the inside of the nanowire in the form of oxygen ions, oxygen molecules or oxygen atoms.
3. The memristor based on the composite nanowire network structure, in which: the composite nanowire network structure layer comprises a network structure layer formed by vertical nanowires, the inclined nanowires form the network structure layer or one of the network structure layers formed by bent nanowires, and the oxygen-doped nitride nanowires forming the network structure layer are mutually connected or mutually separated.
4. The memristor based on the composite nanowire network structure, in which: the top electrode layer is composed of a nanowire network formed by various metal nanowires, specifically is one of networks formed by silver (Ag), gold (Au), copper (Cu) and platinum (Pt) nanowires, wherein the length of each nanowire is 5-100 micrometers, and the diameter of each nanowire is 10-200 nanometers.
5. The memristor based on the composite nanowire network structure, wherein the memristor comprises: the top electrode layer is prepared by a spray coating method, and the specific method comprises the following steps: preparing a solution with the concentration of 5-100 mg/ml by using metal nanowires, wherein the solution comprises water (H)2O), ethanol (C)2H6O), isopropyl alcohol (C)3H8O); placing the prepared solution into a spray gun, placing a mask plate on a substrate with a composite nanowire network structure, and spraying the prepared solution by using the spray gun, wherein the spraying time is 1-120 seconds, and the spraying distance is 5-50 cm; after the spraying is finished, putting the mixture into an oven, setting the temperature to be 50-200 ℃, and drying for 5-120 minutes; at this time, the top electrode formed by the metal nanowire network and the top end of the composite nanowire structure layer are connected with each other, and have a contact characteristic.
6. The memristor based on the composite nanowire network structure, in which: the bottom electrode layer comprises a conductor or semiconductor substrate, wherein the conductor or semiconductor substrate comprises the following types: one of carbon (C), nickel (Ni), copper (Cu), silicon (Si) and silicon carbide (SiC), and the thickness of the material is 300-1000 microns.
7. The memristor based on the composite nanowire network structure, in which: the nanowire coating is made by one of magnetron sputtering, atomic layer deposition, electron beam deposition, electrochemical deposition, chemical vapor deposition and plasma enhanced chemical vapor deposition.
8. The memristor based on the composite nanowire network structure, wherein the memristor is characterized in that: the oxygen-doped nitride nanowires in the composite nanowire network structure provide support for oxygen ions and the network structure under the action of an external electric field, and the structures of various doped nitride nanowires and the network structure formed by the doped nitride nanowires are not changed under the action of the external electric field.
9. The memristor based on the composite nanowire network structure, wherein: the nanowire coating layer in the composite nanowire network structure receives and stores oxygen ions under the action of an external electric field and provides a migration path for the oxygen ions; and the structure of various doped nitride nanowires is not changed under the action of an external electric field.
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