CN112993157B - Memristor with horizontal structure and uniformity optimization method - Google Patents
Memristor with horizontal structure and uniformity optimization method Download PDFInfo
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- H10N70/00—Solid-state devices without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/20—Multistable switching devices, e.g. memristors
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Abstract
The invention relates to a memristor with a horizontal structure and a uniformity optimization method, which comprises a double-end horizontal electrode, a dielectric material and a substrate; wherein the double-end horizontal electrode has symmetryMetal is used as electrode, perovskite micron rod material is used as dielectric material, and SiO is on surface 2 Silicon wafer, glass plate, polyethylene terephthalate, polyethylene naphthalate, etc. as substrates. The memristor uniformity optimization method obtains a final device by cleaning, drying, UVO hydrophilic treatment, perovskite micron rod preparation, EBL prefabricated horizontal structure electrode, evaporation and dry process transfer of the perovskite micron rod; the optimization method provided by the invention provides the most preferable path for ion migration by utilizing the lower activation energy of metal ion migration on the crystal surface, so that the formation of the CF is limited in the dimension, and the stability and uniformity of the device are improved.
Description
Technical Field
The invention relates to the technical field of electronic materials, in particular to a memristor with a horizontal structure and a uniformity optimization method.
Background
The explosion of Artificial Intelligence (AI) and big data analytics is continuously pushing the revolution of data processing and storage. Facing key technical problems such as storage speed and energy consumption, scientists perform parallel retrieval, processing and storage of mass data information through a novel computing system based on an in-memory computing (in-memory computing) concept. Of these, memristors are receiving increasing attention due to their simple two-terminal structure, as well as excellent memory performance (sub-nanosecond switching time, pico-joule multi-bit programmability, and highly integrated structure). By "SET" (SET) and "RESET" (RESET) operations, the memristor is made to have two or more switchable resistance states. A typical resistance change mechanism is the formation or breaking of one or more Conductive Filaments (CF) with relatively high conductivity based on local defect concentration changes. The defects in the memristor resistive layer may come from the resistive material itself, for example, defects formed by negative ion vacancies in the metal oxide, or defects formed by ion transport from the active metal electrode through the insulating medium. However, due to the randomness of ion/atom migration, the dynamic control of the formation or fracture of the CF on a three-dimensional scale has differences in storage performance (such as SET and RESET voltages, High Resistance State (HRS), Low Resistance State (LRS), and the like) between different devices and between different devices, and these differences greatly affect the reliability of the memristor (such as uncertainty of resistance value, non-uniformity of resistance state, unstable energy consumption value, and the like), thereby hindering further application of the memristor in neuromorphic calculation.
Exploring a strategy of putting a CF (finite frequency) limited domain in a memristor resistance change layer is a key step for solving the reliability problem of the memristor in actual nerve morphology calculation. More recently, Kim et al attempted to form a more stable Ag ion diffusion channel using a top electrode with protrusions designed on p-Si and growing a SiGe barrier layer on the designed electrode (nat. Mater.2018, 17, 335-. Subsequently, the group further prepared memristors based on Ag — Cu alloy electrodes, where preformed Cu pillars could greatly improve the movement channels of silver atoms, improving the stability of the device (nat. nanotechnol.2020, 15, 574-579). In addition, Liu et al also prepared a cation-based memristor, in which the CF size was regulated by the intrinsic ion permeability in graphene with a defect structure (adv. Although the methods realize effective regulation and control of the stability of the memristor, the preparation method is too complex, and is not beneficial to further industrialization of subsequent industrial application.
Disclosure of Invention
The memristor with the horizontal structure and the uniformity optimization method provided by the invention can solve the technical problems of insufficient stability and poor uniformity of the existing memristor device.
In order to achieve the purpose, the invention adopts the following technical scheme:
comprises a double-end horizontal electrode, a dielectric material and a substrate;
wherein, the double-end horizontal electrode has symmetry, metal is used as the electrode, perovskite micron rod material is used as the dielectric material, and SiO is arranged on the surface 2 Silicon wafer (SiO) 2 Si), glass flake, Polyethylene terephthalate (PET), Polyethylene naphthalate (PEN) as substrates.
Furthermore, the metal of the electrode is one of gold, silver, aluminum and magnesium.
On the other hand, the invention discloses a memristor uniformity optimization method, which comprises the following steps,
the method comprises the following steps: cleaning;
mixing SiO 2 Putting the/Si substrate into a beaker, adding a few drops of Decon cleaning agent and a set amount of ultrapure water, and ultrasonically treating the beaker for 10-20 min; taking out the beaker, adding ultrapure water again to flush the beaker until no foam exists, adding a set amount of ultrapure water again, performing ultrasonic treatment for 5-10min, and repeating the ultrasonic treatment for 2-3 times;
step two: drying;
the cleaned SiO 2 N for/Si substrate 2 Drying with a gun, and oven drying in a vacuum drying oven at 120 deg.C for 30 min;
step three: performing UVO hydrophilization treatment;
mixing SiO 2 Putting the Si substrate into a UVO cleaner for treatment for 20-40 min;
step four: preparing perovskite micron rods;
synthesizing a lead-calcium-titanium halide micron rod on hydrophobic Indium Tin Oxide (ITO) coated glass by adopting a one-step self-assembly method;
step five: EBL prefabricating a horizontal structure electrode;
in SiO 2 Designing a pattern of a Cr/Ag electrode on a/Si substrate by an EBL technology;
step six: evaporation;
in SiO of the designed electrode 2 Depositing a Cr metal layer with the thickness of 2-10nm and an Ag metal layer with the thickness of 20-60nm on the Si substrate by evaporation, and finally obtaining a horizontal metal electrode layer of the device;
step seven: transferring perovskite micron rods by a dry method;
preparing a Polydimethylsiloxane (PDMS) film, and pressing the perovskite micron rod onto an Ag electrode with a double-end horizontal structure by using the PDMS film through a typical dry transfer method to obtain a final device.
Further, the method also comprises the step eight: detecting;
the electrical property of the device is researched by using a semiconductor analyzer, and the resistance state of the device is accurately regulated and controlled by applying an electric field.
Further, the three steps are to prepare SiO 2 SiO when/Si substrate is put into UVO cleaner for treatment 2 The electrodes face upward.
Further, the metal electrode in the sixth step can be replaced by other metals such as gold, silver, aluminum or magnesium.
Further, the lead perovskite micron rod is synthesized on the hydrophobic Indium Tin Oxide (ITO) coated glass by adopting a one-step self-assembly method in the fourth step; the method specifically comprises the following steps:
first, respectively preparing and dissolving CH 3 NH 3 DMF solution of Br and concentration of dissolved PbBr 2 A DMF solution of (1); wherein the concentration of the dimethylformamide solution is the same as that of the DMF solution;
the two solutions are then mixed thoroughly at room temperature in a volume ratio of 1:1 to 1.1:1 to form CH 3 NH 3 Br·PbBr 2 A solution;
coating the ITO glass surface with the obtained solution, and placing the solution on a polytetrafluoroethylene table in a 50 ml beaker;
30-40ml of dichloromethane (CH) 2 Cl 2 ) Putting into a beaker, and sealing with a porous membrane to control the evaporation speed of the solution;
after 48 hours, the perovskite CH was successfully synthesized on the substrate 3 NH 3 PbBr 3 Micron rod crystal for subsequent device preparation.
According to the technical scheme, the memristor with the horizontal structure and the uniformity optimization method provided by the invention have the advantages that the metal ion migration activation energy of the crystal surface is low, and the most preferable path is provided for the ion migration, so that the formation of the domain CF is limited in the dimension, and the stability and uniformity of the device are improved.
The memristor device based on the horizontal structure of the low-dimensional crystal material has the advantages of simple manufacturing process, large on-off ratio, high storage density, high stability and the like, so that the memristor device has a good application prospect and can be widely applied to multiple fields in life.
Drawings
FIG. 1 is a schematic diagram of a top view structure of a perovskite nanorod based memristor device;
FIG. 2 is a schematic diagram of a side view structure of a perovskite nanorod based memristor device;
FIG. 3 is a temperature dependent Arrhenius plot reflecting the difference in ion conductivity activation energies of Ag/perovskite nanorods/Ag and Ag/perovskite films/Ag;
FIG. 4 is a formation process of a conductive filament of a memristor device based on different materials, the memristor device based on low-dimensional crystalline materials having a limited-domain effect on the formation and fracture process of the conductive filament, as the stability and uniformity of the device may be improved;
FIG. 5 is a current-voltage curve of a memristor with 5 different Ag/perovskite microrod/Ag structures under the action of an electric field, and the device shows stable storage characteristics;
FIG. 6 is a current-voltage curve of a memristor of the same Ag/perovskite nanorod/Ag structure under the action of an electric field in a 100-cycle test, and the device shows stable storage characteristics.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are some, but not all, embodiments of the present invention.
Perovskite CH 3 NH 3 PbBr 3 The micron rod crystal material is a novel low-dimensional crystal material, is prepared by a one-step self-assembly method, is simple in preparation method, has excellent physical and chemical properties, and has wide application prospects in many fields.
Resistance state switching of memristor taking Ag or Cu as active metal electrodeOften an electrochemical process accompanied by atomic/ionic transport. The metal ion migration is considered to be an important factor influencing the switching performance of different resistance states of the memristor. Therefore, the present embodiment first evaluates the activation barrier for Ag ion migration in the active material. FIG. 2 depicts the conductivities of the different devices Ag/perovskite microrod/Ag (see FIG. 1 for structure) and Ag/perovskite thin film/Ag devices at subthreshold voltage pulses (pulse voltage: 5V; pulse width: 8 seconds) calculated by Arrhenius plot method (Arrhenius plot). It can be seen from the temperature-dependent arrhenius diagram that the migration activation energy of Ag ions in the perovskite nanorods having a good crystal structure is 0.25eV, whereas the migration activation energy of Ag ions in the perovskite thin film prepared by thermal evaporation is 0.35 eV. In addition, the migration activation energy value of Ag ions in the memristor device based on the perovskite micron rod is obviously lower than that of Ag in SiO 2 Upper mobility value (0.47-1.24 eV). These results indicate that perovskite nanorods can provide preferential migration paths for reactive metal ions. Accordingly, embodiments of the present invention construct a memristor element in a horizontal structure using perovskite nanorods to address the issues of stability and uniformity of storage.
As shown in fig. 1, the memristor with the horizontal structure of the present embodiment includes a double-ended horizontal electrode, a dielectric material, and a substrate;
wherein, the double-end horizontal electrode has symmetry, and can be made of metal (gold, silver, aluminum, magnesium, etc.) as electrode, perovskite micron rod material as dielectric material, and SiO on the surface 2 Silicon wafer (SiO) 2 Si), glass flake, Polyethylene terephthalate (PET), Polyethylene naphthalate (PEN), and the like as a substrate.
In the invention, a perovskite micron rod material is prepared mainly by adopting a one-step self-assembly method. The preparation of the memristor device is realized by combining dry transfer with Electron Beam Lithography (EBL), wherein the horizontal metal electrode is completed by controlling temperature and time in the thermal evaporation process. And the influence of the different top electrodes on the device performance is explored through evaporation.
The memristor uniformity optimization method of the embodiment specifically operates as follows:
step one (cleaning): mixing SiO 2 Putting the/Si substrate into a beaker, adding a few drops of Decon cleaning agent and a proper amount of ultrapure water, and ultrasonically treating the beaker for 10 min. Taking out the beaker, adding ultrapure water again to wash until no foam exists, adding an appropriate amount of ultrapure water, performing ultrasonic treatment for 5min, and repeating for 2-3 times.
Step two (drying): the cleaned SiO 2 N for/Si substrate 2 Drying with a gun, and oven drying in a vacuum drying oven at 120 deg.C for 30 min.
Step three (UVO hydrophilization treatment): mixing SiO 2 the/Si substrate is placed in a UVO cleaner (SiO) 2 Electrode up) for 30 min.
Step four (preparation of perovskite micron rods): the lead halide perovskite micron rod is synthesized on hydrophobic Indium Tin Oxide (ITO) coated glass by adopting a one-step self-assembly method.
Step five (EBL prefabricated horizontal structure electrode): in SiO 2 And designing a Cr/Ag electrode pattern on the/Si substrate by using an EBL technology.
Step six (evaporation): in SiO with designed electrode 2 Depositing a Cr metal layer with the thickness of 10nm and an Ag metal layer with the thickness of 60nm on the/Si substrate by evaporation (the metal electrode can be replaced by other metals such as gold, silver, aluminum, magnesium and the like) to finally obtain the horizontal metal electrode layer of the device.
Step seven (dry transfer of perovskite micro-rods): preparing a Polydimethylsiloxane (PDMS) film, and pressing the perovskite micron rod onto an Ag electrode with a double-end horizontal structure by using the PDMS film through a typical dry transfer method to obtain a final device.
Step eight (detection): the electrical property of the device is researched by using a semiconductor analyzer, and the resistance state of the device is accurately regulated and controlled by applying an electric field.
The preparation method of the memristor device based on the perovskite micron rod comprises the following steps:
the lead halide perovskite micron rod is synthesized on hydrophobic Indium Tin Oxide (ITO) coated glass by adopting a one-step self-assembly method. First, dissolved CH was prepared at a concentration of 0.1M 3 NH 3 Of BrDimethylformamide (DMF) solution and 0.1M concentration of dissolved PbBr 2 In DMF. The two solutions were then mixed well at room temperature in a volume ratio of 1.05:1 to form CH 3 NH 3 Br·PbBr 2 Solution (0.02M). The solution obtained was coated on the ITO glass surface and placed on a teflon table in a 50 ml beaker. 35ml of dichloromethane (CH) 2 Cl 2 ) Put into a beaker and sealed with a 3M porous membrane to control the evaporation rate of the solution. After 48 hours, the perovskite CH is successfully synthesized on the substrate 3 NH 3 PbBr 3 Micron rod crystal. For subsequent device fabrication.
In summary, the present invention provides an optimization method for solving the stability and uniformity problems of memristor devices through low-dimensional crystalline materials, the memory comprising: horizontal metal electrode, dielectric material, substrate. The innovation point of the invention is that the dielectric layer of the device is prepared by using the method of using the low-dimensional crystal material as the dielectric layer of the memristor.
1. The perovskite nanowires of the present patent are intended to be illustrative of the present invention only and are not intended to be limiting. Memristors fabricated from other low-dimensional materials, such as crystalline materials like nanowires, microwires, two-dimensional materials, etc., and used for achieving device uniformity performance optimization, shall also fall within the scope of the appended claims.
2. The Cr/Ag symmetrical electrode of the present invention is only for explaining the present invention and is not intended to limit the present invention. The invention also belongs to the protection scope of the appended claims, wherein the memristors are prepared by using other active electrode combinations, such as Cr/Cu, Cr/Ni and the like, asymmetric electrodes, such as Cr/Cu-Cr/Au, Cr/Ag-Cr/Au, Cr/Ni-Cr/Au and the like, and are combined with low-dimensional dielectric layer materials for realizing the optimization of the uniformity performance of the device.
3. The invention uses Cr/Ag metal material as electrode material to prepare memristor device, which is only used for explaining the invention and is not used for limiting the invention. Memristor devices based on low-dimensional crystal materials and prepared by using electrodes (gold, silver, aluminum, magnesium and the like) prepared by other metal materials, and realizing uniformity control by using the memristor devices also belong to the protection scope of the appended claims.
The above examples are only intended to illustrate the technical solution of the present invention, and not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some technical features may be equivalently replaced; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions of the embodiments of the present invention.
Claims (3)
1. A memristor homogeneity optimization method of a horizontal structure is provided, wherein the memristor of the horizontal structure comprises a double-end horizontal electrode, a dielectric material and a substrate; the double-end horizontal electrode has symmetry, adopts metal as electrode, perovskite micron rod material as dielectric material and SiO on the surface 2 The silicon chip, the glass sheet, the polyethylene terephthalate and the polyethylene naphthalate are used as substrates; the method is characterized in that: the memristor uniformity optimization method comprises the following steps:
comprises the following steps of (a) carrying out,
the method comprises the following steps: cleaning;
mixing SiO 2 Putting the/Si substrate into a beaker, adding a few drops of Decon cleaning agent and a set amount of ultrapure water, and ultrasonically treating the beaker for 10-20 min; taking out the beaker, adding ultrapure water again to flush the beaker until no foam exists, adding a set amount of ultrapure water again, performing ultrasonic treatment for 5-10min, and repeating the ultrasonic treatment for 2-3 times;
step two: drying;
the cleaned SiO 2 N for/Si substrate 2 Drying with a gun, and drying in a vacuum drying oven at 120 deg.C for 30 min;
step three: performing UVO hydrophilization treatment;
mixing SiO 2 Putting the Si substrate into a UVO cleaner for treatment for 20-40 min;
step four: preparing perovskite micron rods;
the lead-calcium-titanium halide micron rod is synthesized on hydrophobic indium tin oxide coated glass by adopting a one-step self-assembly method, and specifically comprises the following steps:
first, respectively preparing and dissolving CH 3 NH 3 Dimethylformamide solution of Br and dissolved PbBr 2 A DMF solution of (1); wherein the concentration of the dimethylformamide solution is the same as that of the DMF solution;
then the two solutions are mixed thoroughly at room temperature in a volume ratio of 1:1 to 1.1:1 to form CH 3 NH 3 Br∙PbBr 2 A solution;
coating the ITO glass surface with the obtained solution, and placing the solution on a polytetrafluoroethylene table in a 50 ml beaker;
putting 30-40ml of dichloromethane into a beaker, and sealing the beaker by using a porous membrane to control the evaporation speed of the solution;
after 48 hours, perovskite CH is successfully synthesized on the ITO glass surface 3 NH 3 PbBr 3 Micron rod crystals for subsequent device fabrication
Step five: EBL prefabricating a horizontal structure electrode;
in SiO 2 Designing a pattern of a Cr/Ag electrode on a Si substrate by an EBL technology;
step six: evaporation;
in SiO of the designed electrode 2 Depositing a Cr metal layer with the thickness of 2-10nm and an Ag metal layer with the thickness of 20-60nm on the Si substrate by evaporation to finally obtain a horizontal metal electrode layer of the device;
step seven: transferring the perovskite micron rod by a dry method;
preparing a polydimethylsiloxane film, and pressing perovskite microrods onto an Ag electrode with a double-end horizontal structure by using the film through a typical dry transfer method to obtain a final device.
2. The memristor uniformity optimization method of claim 1, wherein: the metal of the electrode is one of gold, silver, aluminum and magnesium.
3. The memristor uniformity optimization method according to claim 1, characterized in that: further comprises the following steps: detecting;
the electrical property of the device is researched by using a semiconductor analyzer, and the resistance state of the device is accurately regulated and controlled by applying an electric field.
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