CN116528656A - Method for regulating and controlling quantized conductance behavior of oxide-based memristor - Google Patents
Method for regulating and controlling quantized conductance behavior of oxide-based memristor Download PDFInfo
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/20—Multistable switching devices, e.g. memristors
- H10N70/24—Multistable switching devices, e.g. memristors based on migration or redistribution of ionic species, e.g. anions, vacancies
- H10N70/245—Multistable switching devices, e.g. memristors based on migration or redistribution of ionic species, e.g. anions, vacancies the species being metal cations, e.g. programmable metallization cells
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/801—Constructional details of multistable switching devices
- H10N70/881—Switching materials
- H10N70/883—Oxides or nitrides
- H10N70/8833—Binary metal oxides, e.g. TaOx
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02D—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN INFORMATION AND COMMUNICATION TECHNOLOGIES [ICT], I.E. INFORMATION AND COMMUNICATION TECHNOLOGIES AIMING AT THE REDUCTION OF THEIR OWN ENERGY USE
- Y02D10/00—Energy efficient computing, e.g. low power processors, power management or thermal management
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Abstract
The invention relates to a method for regulating and controlling the quantized conductance behavior of an oxide-based memristor, which comprises a bottom electrode layer, an alkali metal oxide layer, a functional oxide layer and a top electrode layer in sequence from bottom to top. The method is characterized in that: the functional oxide layer has the functions of storage and limited-domain ion migration, and forms an uneven local gradient electric field under the action of an electric field to limit the domain ion migration. The pulse and direct-current voltage regulation means are combined, so that the controllability and the reproducibility of quantized conductance behaviors are realized. The invention realizes a plurality of quantized states and long retention time, and is expected to be widely applied in the fields of high-density storage, artificial synapse simulation, brain-like calculation and the like.
Description
Technical Field
The invention provides a method for regulating and controlling quantized conductance of an oxide-based memristor, which is characterized in that under the action of an electric field, an uneven local gradient electric field is formed inside the device, and the migration of ions in a limited area is limited, so that the regulation and control of quantized conductance are realized. The device combines pulse and direct-current voltage regulation and control means, realizes controllability and reproducibility of quantized conductance behaviors, has a plurality of quantized conductance states, can realize longer retention time of each quantum state, and belongs to the technical field of brain-like information storage and calculation.
Background
With the advent of the intelligence era, artificial intelligence has become the core driving force leading a new technological revolution and industry revolution. The information storage and processing simulating the human brain thinking mode has become the leading edge and new high point of great competition in countries around the world due to the characteristics of high efficiency, low energy consumption and the like in the artificial intelligence field. The memristor has a simple structure and low energy consumption, the conductance of the memristor can be continuously and reversibly regulated through electric stimulation, the function of human brain synapses can be well simulated, artificial synapses based on the memristor are considered to be one of ideal choices for constructing a neuromorphic computing architecture and realizing brain-like information storage and processing.
As a novel nanoscale component, the memristor has unique advantages in the aspects of ultrahigh data storage, logic operation and neuromorphic calculation. With the intensive research of memristors, a phenomenon of discontinuous conduction, namely quantized conduction behavior, is found in different types of memristors. The current research shows that most memristors apply voltage to drive ion migration to form a nano conductive filament for connecting an anode and a cathode through the coupling action of electrons and ions, and a series of n/2G nano conductive filaments are shown 0 Quantized conductance properties in units. The method is favorable for realizing multi-level storage and neuromorphic calculation. However, the uncontrollable migration of ions in the resistive layer results in a large number of ions migrating randomly, making the quantized conductance behavior poorly controllable and reproducible. How to find proper memristor materials and related regulation and control methods according to requirements to prepare controllable and reproducible quantized conductive devices, and the memristor is realized in ultra-high numberThe application in the aspects of storage and brain-like computation has important significance.
Disclosure of Invention
Aiming at the problems of controllable and poor reproducibility of quantized conductance behavior in the current memristor, the invention aims at constructing an uneven local gradient electric field and a quantum finite field effect by introducing a micro-nano structure into a resistive layer, realizing finite field migration of ions and being beneficial to realizing effective regulation and control of quantized conductance behavior. Provides important application prospect for the development of memristors in multilevel storage and neuromorphic calculation.
The invention adopts the following technical scheme:
the invention relates to a method for regulating and controlling the quantized conductance behavior of an oxide-based memristor, which comprises a bottom electrode layer, an alkali metal oxide layer, a functional oxide layer and a top electrode layer in sequence from bottom to top. The method is characterized in that: the functional oxide layer has the functions of storage and limited-domain ion migration, and forms an uneven local gradient electric field under the action of an electric field to limit the domain ion migration.
The bottom electrode layer is one of (100) high doped silicon, tungsten foil and molybdenum foil.
The functional oxide layer is one of silicon oxide, tungsten oxide, molybdenum oxide and hafnium oxide.
The preparation method of the functional oxide layer is one of electrochemical anodic oxidation, radio frequency magnetron sputtering and electron beam deposition.
The method for functionalizing the functionalized oxide layer is one of micro-nano structure construction and quantum dot modification.
The functional oxide layer adopts a quantum dot modification method; wherein, the quantum dots are induced to generate nonuniform local gradient electric fields; the quantum dots comprise one of silicon quantum dots, molybdenum disulfide quantum dots, tungsten disulfide quantum dots and graphene quantum dots.
The alkali metal oxide layer is a layered material for providing ions, and is respectively lithium cobalt oxide (LiCoO) 2 ) Sodium cobaltate (NaCoO) 2 ) Potassium cobaltate (KCoO) 2 ) One of them has a thickness of 20-60nm。
The preparation method of the alkali metal oxide layer comprises one of radio frequency magnetron sputtering, electron beam deposition, pulse laser deposition and sol-gel method.
The oxide-based memristor tests the quantized conductance behavior of the oxide-based memristor by using two modes of direct current scanning and pulse scanning; the quantized conductivity can be regulated and controlled by two modes of direct current scanning and pulse scanning; the DC regulation means is divided into limiting current I cc Cut-off voltage V stop The method comprises the steps of carrying out a first treatment on the surface of the The pulse regulation and control can regulate and control the quantized conductance state of the oxide-based memristor based on different pulse intervals, different pulse widths, different pulse amplitudes and different pulse numbers; and discontinuous quantized conductance behavior occurs for both positive and negative sweeps during the application of both direct and pulsed voltage sweeps.
The method for realizing quantized conductance behavior by using the oxide-based memristor comprises the following steps:
step one, a writing process, in which a bottom electrode is grounded, a forward DC and a pulse voltage are applied to a top electrode, li + 、Na + 、K + The quantum conducting material is separated from the alkali metal oxide layer, enters the functionalized oxide layer and undergoes electrochemical reaction, and a conducting channel is formed in the oxide memristor, so that the stepped quantum conducting behavior is realized in the process of switching the device from a high-resistance state to a low-resistance state.
Step two, the erasing process is continued to apply negative direct current or pulse voltage to the top electrode, metal ions are separated from the functionalized oxide layer and are embedded back into the alkali metal oxide, the transition of the device from a low-resistance state to a high-resistance state is completed, and the device shows a stepped quantum conductivity behavior in the transition process; the functionalized silicon oxide layer is hardly changed in the process of de-embedding, so that the cycling stability of the device is improved.
The alkali metal oxide layer mainly provides alkali metal ions under the action of an external electric field, and hardly changes under the action of the external electric field.
The functional oxide layer mainly receives and stores alkali metal ions under the action of an external electric field, and the micro-nano structure induces formation of an uneven local gradient electric field, so that a migration path is provided for alkali metal, and the functional oxide layer is a key layer for realizing quantized conductivity behavior.
Compared with the prior art, the method for regulating and controlling the quantized conductance behavior of the oxide-based memristor has the advantages of simplicity, low manufacturing cost, large-area preparation and device function:
1. under the action of an electric field, the functionalized oxide layer induces a local nonuniform gradient electric field to limit ion transport; the ion gradient capturing and releasing are realized, and the quantized conductance behavior is more facilitated.
2. The external electric field is removed, the functional oxide layer can effectively store metal ions, and each quantum state is more than 10 4 s retention time.
3. Based on the functionalized oxide layer nanostructure-based memristor, under the condition of pulse voltage application, different pulse amplitudes and pulse widths are found to have synaptic plasticity behavior similar to continuous learning of brain, and conditions are provided for application of neuromorphic calculation.
Drawings
FIG. 1 is a schematic diagram of a structure of an oxide-based memristor.
Fig. 2a is an SEM image of a functionalized oxide layer.
Fig. 2b is a HRTEM image of a functionalized oxide layer.
Fig. 2c is a diagram of the lattice structure of modified quantum dots in a functionalized oxide.
FIG. 3 is a flow chart of a method of fabricating an oxide-based memristor.
FIG. 4a is an electrical measurement of a DC voltage sweep of an oxide-based memristor.
FIG. 4b is the quantized conductivity state corresponding to the 50 th turn of an oxide-based memristor.
FIG. 5 is a graph of oxide-based memristor multi-quantum conductivity state retention times.
FIG. 6 is a conductance-time electrical diagram of a pulse voltage of an oxide-based memristor to achieve quantized conductance.
FIG. 7 is a continuous learning behavior of an oxide-based memristor pulse test.
FIG. 8 is a flow chart of preparation and measurement of oxide-based memristor-modulated quantized conductance behavior and continuous learning behavior.
Specific reference numerals in the drawings are as follows:
201-a top electrode layer; a 101-alkali metal oxide layer;
202-a bottom electrode layer; 102-a functionalized oxide layer.
Detailed Description
The invention will be described in further detail with reference to fig. 1-8, which are intended to facilitate an understanding of the invention, and specific structural and functional details thereof are merely representative for purposes of describing example embodiments and are not intended to be limiting. Thus, the present invention may be embodied in many alternate forms and should not be construed as limited to only the example embodiments set forth herein, but rather, should cover all changes, equivalents, and alternatives falling within the scope of the present invention.
In this embodiment, the structure is based on a "top electrode layer/alkali metal oxide layer/functionalized oxide layer/bottom electrode layer" structure, which has a top electrode layer 201, an alkali metal oxide layer 101, a functionalized oxide layer 102, and a bottom electrode layer 202 from top to bottom as shown in fig. 1.
The structure adopts a silicon wafer as a bottom electrode, and adopts methods of electrochemical anodic oxidation, magnetron sputtering and the like to prepare the structure layer by layer on a substrate from bottom to top, as shown in figure 3. An example oxide-based memristor flow chart is shown in fig. 8, and specific preparation and testing steps are as follows:
step one, preparing a substrate:
cutting P-type (100) high doped silicon into 1X 1cm 2 Respectively and sequentially using acetone, absolute ethyl alcohol and deionized water to ultrasonically clean the silicon wafers for 15 minutes, wherein the ultrasonic power is 100W, and drying the silicon wafers by high-purity nitrogen after cleaning.
Step two, preparing a functional oxide layer:
1. p-type (100) highly doped silicon is selected as a bottom electrode layer 202, and is used as an anode, and electrolyte with volume fraction of 15% hydrofluoric acid and 6.25% hydrogen peroxide is prepared by taking the volume ratio of ethanol to deionized water of 1:1 as a solvent; the Pt sheet is used as a cathode, the P type (100) high silicon doped is used as an anode, and the distance between the cathode and the anode is fixed to be 0.5 cm.
2. Opening an electrochemical workstation, and setting the corrosion current to 75 milliamperes; and the size is 1X 1cm 2 The P-type (100) silicon wafer is completely soaked in electrolyte, and the etching time is 5 minutes.
3. And ultrasonically cleaning the silicon wafer subjected to electrochemical anodic oxidation in absolute ethyl alcohol for 5 minutes, sufficiently removing the residual electrolyte on the surface, and drying the silicon wafer by high-purity nitrogen to prepare for the subsequent work.
Step three, micro-nano structure characterization:
SEM and HRTEM micro-nano structural characterization of the electrochemically anodized samples was performed as shown in fig. 2a, 2b and 2 c.
Step four, preparing an oxide-based memristor:
depositing a layer of LiCoO on the prepared sample surface by using radio frequency magnetron sputtering 2 The film was sputtered for 30 minutes. And then depositing a layer of Pt as a top electrode by using direct current magnetron sputtering, wherein the sputtering time is 3 minutes, and obtaining the oxide-based memristor.
Fifthly, quantized conductivity behavior characterization:
1. d.c. electrical behavior test: during the test, the bottom electrode layer is grounded, and a negative and a positive dc scan voltages are applied to the top electrode layer Pt, as shown in fig. 4 a. Under the action of an electric field, lithium ions migrate into the quantum dot modified silicon oxide layer, the resistance state of the device is changed, and the stepped quantum conductivity behavior is realized as shown in fig. 4 b; performing a hold time test on each quantum state, each quantum state achieving greater than 10 4 The holding time of s is shown in fig. 5.
2. Pulse voltage test: an incremental voltage of 4V-8.5V was applied with a voltage increment interval of 0.5V, a pulse interval of 50 ms, a pulse width of 5 ms, and a read voltage of 0.5V, as shown in fig. 6.
Step six, continuously learning behavior simulation:
continuous learning behavior test of device using pulse voltage, and during continuous learning capability test, the top electrode layer Pt is connectedApplying pulse sequence (pulse voltage 6V, pulse interval 5 ms, pulse width 5 ms, learning times 3 times, learning pulse number 20 each time, reading pulse number 500, reading pulse voltage 0.5V, liCoO under the action of electric field) three times 2 The lithium ions in the layer gradually migrate into the quantum dot modified silicon oxide layer, exhibiting good learning ability, as shown in fig. 7.
In summary, oxide-based memristors exhibit pronounced memristive properties, exhibit quantized conductance behavior of discontinuous conductance during both direct voltage and pulse voltage sweeps, and exhibit continuous learning capabilities.
Claims (10)
1. An oxide-based memristor, wherein the overall structure of the oxide-based memristor sequentially comprises a bottom electrode layer/an alkali metal oxide layer/a functional oxide layer/a top electrode layer from bottom to top; the method is characterized in that: the functional oxide layer has the functions of storage and limited-area ion migration, and forms an uneven local gradient electric field under the action of an electric field to limit the area ion migration, so that the effective regulation and control of the quantized conductance behavior are realized.
2. The oxide-based memristor of claim 1, wherein: the bottom electrode layer is one of (100) high silicon-doped, tungsten foil and molybdenum foil.
3. The oxide-based memristor of claim 1, wherein: the functional oxide layer is one of silicon oxide, tungsten oxide, molybdenum oxide and hafnium oxide.
4. The oxide-based memristor of claim 1, wherein: the preparation method of the functional oxide layer is one of electrochemical anodic oxidation, radio frequency magnetron sputtering and electron beam deposition.
5. The oxide-based memristor of claim 1, wherein: the functionalization method of the functionalized oxide layer is one of micro-nano structure construction and quantum dot modification; wherein, the quantum dots are induced to generate nonuniform local gradient electric fields; the quantum dots comprise one of silicon quantum dots, molybdenum disulfide quantum dots, tungsten disulfide quantum dots and graphene quantum dots.
6. The oxide-based memristor of claim 1, wherein: the alkali metal oxide layer is a layered material providing ions, respectively lithium cobalt oxide (LiCoO) 2 ) Sodium cobaltate (NaCoO) 2 ) Potassium cobaltate (KCoO) 2 ) The thickness of the material is 20-60nm.
7. The oxide-based memristor of claim 1, wherein: the preparation method of the alkali metal oxide layer comprises one of radio frequency magnetron sputtering, electron beam deposition, pulse laser deposition and sol-gel method.
8. The oxide-based memristor of claim 1, wherein: the oxide-based memristor tests the quantized conductance behavior of the oxide-based memristor by using two modes of direct current scanning and pulse scanning; the DC regulation means is divided into limiting current I cc Cut-off voltage V stop The method comprises the steps of carrying out a first treatment on the surface of the The pulse regulation and control is based on different pulse intervals, different pulse widths, different pulse amplitudes and different pulse numbers to regulate and control the quantized conductance states of the oxide-based memristor; and discontinuous quantized conductance behavior occurs for both positive and negative sweeps during the application of both direct and pulsed voltage sweeps.
9. A method for regulating and controlling quantized conductance behavior of an oxide-based memristor based on any of claims 1-8, characterized by: the method comprises the following steps:
step one, a writing process, in which a bottom electrode is grounded, a forward DC and a pulse voltage are applied to a top electrode, li + 、Na + 、K + Is separated from the alkali metal oxide layer, enters the functionalized oxide layer and generates electrochemical reaction to form conduction in the oxide memristorThe channel is used for realizing the stepped quantum conductivity behavior of the device in the process of converting from a high-resistance state to a low-resistance state;
step two, the erasing process is continued to apply negative direct current or pulse voltage to the top electrode, metal ions are separated from the functionalized oxide layer and are embedded back into the alkali metal oxide, the transition of the device from a low-resistance state to a high-resistance state is completed, and the device shows a stepped quantum conductivity behavior in the transition process; the functionalized silicon oxide layer is hardly changed in the process of de-embedding, so that the cycling stability of the device is improved.
10. The method for regulating and controlling the quantized conductance behavior of the oxide-based memristor according to claim 9, wherein the method comprises the following steps: the alkali metal oxide layer provides alkali metal ions under the action of an external electric field, and hardly changes under the action of the external electric field; the functional oxide layer receives and stores alkali metal ions under the action of an external electric field, and the micro-nano structure induces formation of an uneven local gradient electric field to provide a migration path for alkali metal, so that effective regulation and control of quantized conductance behavior are realized.
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