CN112382721A - Conductive filament type memristor, preparation method and storage mode regulation and control method - Google Patents
Conductive filament type memristor, preparation method and storage mode regulation and control method Download PDFInfo
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Abstract
The invention discloses a conductive filament type memristor, a preparation method thereof and a regulation and control method of a storage mode. The conductive filament-type memristor includes: the quantum dot structure comprises a bottom electrode, a core-shell quantum dot layer formed on the bottom electrode and a top electrode formed on the core-shell quantum dot layer. According to the conductive filament type memristor, the core-shell quantum dot layer is used as the dielectric layer of the memristor, the core-shell quantum dot photoresponse is utilized to realize the switching of the optical control memristor between the volatile storage mode and the non-volatile storage mode, and the conductive filament type memristor has the advantages of being capable of being remotely controlled, non-damaging, simple and easy to operate and the like.
Description
Technical Field
The invention relates to the technical field of electronic information, in particular to a conductive filament type memristor, a preparation method thereof and a regulation and control method of a storage mode.
Background
The advent of the big data era has placed ever higher demands on modern computer information processing technology, and the development of digital computers of traditional architecture has been stranded due to the failure of von neumann bottlenecks and moore's law. An innovative strategy is to apply a brain-like storage and computation integration mode, that is, storage and operation are located in the same unit. The two-terminal memristor is a memory cell perfectly matched with the brain computing architecture.
Compared with the traditional silicon-based fast memory, the memristor has the advantages of easiness in miniaturization, low cost, simple structure, high operation speed and the like. The memristor adopts a sandwich structure, namely metal-dielectric layer-metal, and the external power supply stimulation can drive ions of the dielectric layer to move and then realize the structural change of the material, thereby causing the resistance value of the device to change. The movement of ions in the memristor just simulates the function of biological synapses, and the controllable resistance value can represent the weight of the synapses. The hardware neural network circuit based on the memristor has high operational parallelism, and people think that the hardware neural network circuit can be applied to the fields of future on-chip operational storage, storage and calculation integration, biological simulation calculation and the like.
The research on the memristor plays a crucial role in the development of the future electronic information field. The nonvolatile memory and the volatile memory can be classified according to whether data recorded in the memory device is lost. The nonvolatile memory means that the recorded resistance value is not changed after an external power supply is removed; volatile memory means that data recorded by the device is lost as the external power supply is removed. Generally, the movement of ions in the memristor forms conductive filaments connecting two electrodes, and the number, shape and size of the conductive filaments determine the conductance value of the device; the conductive filament in the nonvolatile memristor can stably exist after the power supply is removed, and the conductive filament of the volatile memristor spontaneously diffuses and dissolves after the power supply is removed due to factors such as surface energy minimization and space repulsion. To date, many international research teams have applied non-volatile memristors to build logic gates, oscillators, hardware neural network circuits, while volatile memristors are applied to build high sub-threshold slope transistors, selectors in cross-structure arrays, true random number generation circuits, and biological neuron circuits. Different storage modes depend on specific material systems, and the stable and controllable switching between the volatile storage mode and the nonvolatile storage mode in a single memristor is a research target which is actively explored all the time, and the multifunctional memristor device is an essential unit for innovative circuit development.
Currently, there are many reported methods for achieving coexistence of two modes in a single device, such as doping, changing annealing or voltage scanning conditions, and applying different limiting currents. Among them, applying different limiting currents during electrical scanning is the most common implementation. When a small limiting current is applied, the conductive filaments formed in the memristor are thin and small in quantity, the filaments can break spontaneously after the power supply is removed, and the conductance returns to the initial state; when a larger limiting current is applied, the conductive filament allowed to grow in the memristor will be thicker and more numerous, and the filament will survive even after the power supply is removed. However, the mode adjustment and control means switches the set limiting current in the circuit, which may cause an additional adjustment module to be added in the circuit design process, and even affect the signal of the back-end circuit. The other regulation and control means can cause irreversible influence on the material system of the memristor, and further influences the service life of the device. Therefore, how to simply and nondestructively regulate the storage mode of the device becomes a key problem for preparing the multifunctional memristor.
Accordingly, the prior art is yet to be improved and developed.
Disclosure of Invention
In view of the foregoing defects in the prior art, an object of the present invention is to provide a conductive filament type memristor, a method for manufacturing the same, and a method for regulating a memory mode, so as to solve the problem that a signal of a back-end circuit is affected due to the need of adding an additional adjusting module to the existing memristor.
A conductive filament-type memristor, comprising:
the quantum dot structure comprises a bottom electrode, a core-shell quantum dot layer formed on the bottom electrode and a top electrode formed on the core-shell quantum dot layer.
The conductive filament-type memristor, wherein the bottom electrode comprises a plurality of strip-shaped bottom electrodes, and the top electrode comprises a plurality of strip-shaped top electrodes;
the strip-shaped bottom electrodes are transversely and parallelly arranged on the lower side face of the core-shell quantum dot layer, and the strip-shaped top electrodes are longitudinally and parallelly arranged on the upper side face of the core-shell quantum dot layer.
The conductive filament memristor is characterized in that the core-shell quantum dot layer is one selected from an indium phosphide-zinc sulfide core-shell quantum dot layer, an indium phosphide-zinc selenide core-shell quantum dot layer, a chromium selenide-zinc sulfide core-shell quantum dot layer and a lead selenide-lead sulfide core-shell quantum dot layer.
The conductive filament type memristor, wherein the bottom electrode is an ITO bottom electrode.
The conductive filament memristor, wherein the top electrode is a silver top electrode.
A method of making a conductive filament memristor as described above, comprising:
forming a bottom electrode on a substrate;
forming a core-shell quantum dot layer on the bottom electrode;
and forming a top electrode on the core-shell quantum dot layer.
The preparation method of the conductive filament type memristor comprises the following steps of:
and depositing an ITO material on the substrate by a magnetron sputtering method to form a bottom electrode.
The preparation method of the conductive filament type memristor comprises the following steps of:
and spin-coating the core-shell quantum dot solution on the bottom electrode, and annealing to form a core-shell quantum dot layer.
The preparation method of the conductive filament type memristor comprises the following steps of:
and depositing a top electrode material on the core-shell quantum dot layer by a thermal evaporation method to form the top electrode.
A regulating and controlling method of a storage mode of a conductive filament type memristor is characterized in that the storage mode of the conductive filament type memristor is converted by irradiating the conductive filament type memristor with light;
the storage mode includes a volatile storage mode and a non-volatile storage mode.
Has the advantages that: according to the conductive filament type memristor, the core-shell quantum dot layer is used as the dielectric layer of the memristor, the core-shell quantum dot photoresponse is utilized to realize the switching of the optical control memristor between the volatile storage mode and the non-volatile storage mode, and the conductive filament type memristor has the advantages of being capable of being remotely controlled, non-damaging, simple and easy to operate and the like.
Drawings
FIG. 1 is an I-V plot of a typical volatile memristor.
FIG. 2 is an I-V plot of a typical non-volatile memristor.
Fig. 3 is a core-shell energy level diagram of different types of core-shell quantum dots.
Fig. 4 is a schematic view of the type I core-shell quantum dot in fig. 3 in carrier distribution under optical excitation.
FIG. 5 is a schematic diagram of a structure of a conductive filament memristor in accordance with the present disclosure.
Fig. 6 is a synthesis flow chart of the core-shell quantum dot.
FIG. 7 is a flow chart of the present invention for fabricating the conductive filament type memristor.
Detailed Description
The invention provides a conductive filament type memristor, a preparation method thereof and a regulation and control method of a storage mode, and the invention is further described in detail below in order to make the purpose, technical scheme and effect of the invention clearer and more clear. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
Data of a volatile memory automatically disappears when power is off, a nonvolatile memory can store data when power is off, so-called resistive random access memories are all default nonvolatile memories, but actually, volatile resistive random access memories exist, are widely reported and are used for neuron circuits, selectors and the like, and fig. 1 shows an I-V curve of a typical volatile memristor. FIG. 2 shows an I-V curve for a typical non-volatile memristor. As shown in FIG. 2, after the set process, the voltage flyback to 0V of the non-volatile memristor can keep the low resistance state all the time, but the volatile memristor has a process of sharp current drop before the voltage flyback to 0V, which indicates that the device returns to the high resistance state again, i.e., the device cannot keep the data (cannot maintain the low resistance state) after the power is cut off.
The invention aims to provide a memory for realizing the conversion of volatile and nonvolatile memory types, and a device based on core-shell quantum dots has the potential of realizing the conversion of two memory types.
In the research process, the memory based on the mononuclear quantum dots is found to have difficult stable light modulation and control storage characteristics, because the surface of the mononuclear quantum dots is not provided with a shell protection layer, defects are easily formed, so that the behavior of photon-generated carriers becomes complex, and photon-generated electron hole pairs are not easy to separate, can be rapidly compounded or captured by a surface defect state, and cannot be distributed in a medium layer to influence the stability of a conductive filament.
However, the photogenerated electron-hole pairs in the core-shell quantum dot material are spatially separated due to the energy barrier difference between the core and the shell material, and the barriers restrict the recombination of carriers, so that one of the carriers, a hole or an electron, can move to an external medium.
As shown in fig. 3, the core-shell quantum dots can be classified into three types, i.e., I type, II type, and I type inversion, according to the difference of energy level structures. The distribution of carriers of different types of core-shell quantum dots is different under different response wavelengths, fig. 4 is a simplified distribution diagram of carriers of I type of core-shell quantum dots under optical excitation, it can be seen that holes are limited in the core, and electrons have a very large probability of moving to the edge of the shell to reach an external medium. The stability of the conductive filament in the memristor can be influenced by the distribution of the light-operated current carriers, and the expected device performance can be realized from various aspects of the type, the size and the structure of the core-shell quantum dot.
As shown in FIG. 5, the present invention provides a conductive filament type memristor, comprising:
the quantum dot structure comprises a bottom electrode 2, a core-shell quantum dot layer 3 formed on the bottom electrode 2, and a top electrode 4 formed on the core-shell quantum dot layer.
According to the conductive filament type memristor, the core-shell quantum dots are used as the dielectric layer of the memristor, the core-shell quantum dot photoresponse is utilized to realize the switching between the volatile storage mode and the nonvolatile storage mode of the optical control memristor, and the conductive filament type memristor has the advantages of remote control, no damage, simplicity and the like.
In the conductive thin-wire memristor, a top electrode 4 and a bottom electrode 2 form a cross shape, and each intersection point is a memristor device (memristor unit). Specifically, the projections of the top electrode 4 and the bottom electrode 2 on the plane where the core-shell quantum dot layer 3 is located are overlapped, and further, the top electrode 4 and the bottom electrode 2 are both strip-shaped and respectively located in two perpendicular directions, so that the projections form a cross shape. In one embodiment of the present invention, the bottom electrode 2 comprises at least 1 strip-shaped bottom electrode 2, and the top electrode 4 comprises at least 1 strip-shaped top electrode 4; the bottom electrodes 2 are arranged transversely, and the top electrodes 4 are arranged longitudinally.
In one embodiment of the present invention, the bottom electrode 2 comprises a plurality of strip-shaped bottom electrodes, and the top electrode 4 comprises a plurality of strip-shaped top electrodes; the strip-shaped bottom electrodes are transversely and parallelly arranged on the lower side face of the core-shell quantum dot layer 3, and the strip-shaped top electrodes are longitudinally and parallelly arranged on the upper side face of the core-shell quantum dot layer 3. That is, the bottom electrode 2 is a plurality of strip-shaped bottom electrodes arranged in parallel in the transverse direction on the lower side surface of the core-shell quantum dot layer 3; the top electrode 4 is a plurality of strip-shaped top electrodes longitudinally arranged in parallel on the upper side surface of the core-shell quantum dot layer 3.
Specifically, the top electrode 4 is composed of a plurality of strip-shaped fixed electrodes, and is transversely arranged on one side of the core-shell quantum dot layer 3 in parallel; the bottom electrode 2 is composed of a plurality of strip-shaped bottom electrodes 2, the strip-shaped bottom electrodes are longitudinally arranged on the other side of the core-shell quantum dot layer 3 in parallel, a memristor unit is formed at the intersection point, the memristor unit can independently complete the function of a memristor, and the memristor unit is equivalent to the memristor. As can be seen, a plurality of cross areas are formed by the plurality of strip top electrodes 4 and the plurality of strip bottom electrodes 2, and each cross area is a memristive cell. In other words, a plurality of the memristive cells constitute the conductive filament type memristor in the present invention.
The core-shell quantum dot layer 3 has photoresponse, specifically, a photon-generated electron hole pair in the core-shell quantum dot material is spatially separated due to the energy level barrier difference between the core and the shell material, and the barrier limits the recombination of current carriers, so that one of the hole or the electron can move to an external medium, the stability of a conductive filament in a memristor can be influenced by the distribution of light-controlled current carriers, and the switching of the storage mode of the conductive filament type memristor is further realized. The core-shell quantum dots are any one of I type, II type and I type inversion. In one embodiment of the present invention, the core-shell quantum dot layer is selected from one of an indium phosphide-zinc sulfide core-shell quantum dot layer, an indium phosphide-zinc selenide core-shell quantum dot layer, a chromium selenide-zinc sulfide core-shell quantum dot layer, a lead selenide-lead sulfide core-shell quantum dot layer, a cadmium sulfide-lead sulfide core-shell quantum dot layer, and an indium phosphide-zinc selenide-zinc sulfide core-shell quantum dot layer.
It is understood that the material of the indium phosphide-zinc sulfide core-shell quantum dot layer 3 is indium phosphide-zinc sulfide (InP/ZnS), the material of the indium phosphide-zinc selenide core-shell quantum dot layer 3 is indium phosphide-zinc selenide (InP/ZnSe), the material of the chromium selenide-zinc sulfide core-shell quantum dot layer 3 is chromium selenide-zinc sulfide (CdSe/ZnS), and the material of the lead selenide-lead sulfide core-shell quantum dot layer 3 is lead selenide-lead sulfide (PbSe/PbS). The simplified synthesis steps of the core-shell quantum dots are shown in fig. 6, and include: synthesizing and purifying the nuclear quantum dots, preparing the shell and the like.
The conductive filament type memristor is a memristor with a sandwich structure and comprises a bottom electrode 2, a dielectric layer and a fixed electrode, wherein the dielectric layer is the core-shell quantum dot layer 3. In one embodiment of the present invention, the bottom electrode 2 is an ITO bottom electrode 2, and the top electrode 4 is a silver top electrode 4.
Wherein, the ITO bottom electrode 2 is an indium tin oxide bottom electrode 2, and the material thereof is indium (III) oxide (In)2O3) And tin (group IV) oxides (SnO)2) A mixture of (a). The ITO bottom electrode 2 has good light transmittance. The silver top electrode 4 is a metal electrodeOne of the most conductive metal electrodes.
Optionally, the thickness of the ITO bottom electrode 2 is 50-150 nm; the thickness of the silver top electrode 4 is 10-80 nm.
As shown in fig. 7, the present invention further provides a method for preparing the conductive filament memristor, which includes:
forming a bottom electrode 2 on a substrate 1;
forming a core-shell quantum dot layer 3 on the bottom electrode 2;
the top electrode 4 is formed on the core-shell quantum dot layer.
The preparation method can prepare the conductive filament type memristor with photoresponse, and can influence the stability of the conductive filament in the memristor by utilizing the distribution of light-controlled carriers, so that the switching of the storage mode of the conductive filament type memristor is realized. The memristor based on the core-shell quantum dots is prepared by applying a solution spin-coating method, and has a simple preparation process on one hand, so that the cost can be reduced; on the other hand, innovation and optimization functions can be realized by adjusting the type, size and structure of the core-shell quantum dots.
The substrate 1 of the present invention is used as a carrier for forming the bottom electrode 2 in the manufacturing process, and the substrate 1 (base) is a transparent substrate 1, such as a glass substrate 1.
In one embodiment of the present invention, the forming of the bottom electrode 2 on the substrate 1 includes: an ITO material is deposited on the substrate 1 by magnetron sputtering, forming a bottom electrode 2.
The bottom electrode 2 is made of an electrochemical inert electrode material, the upper electrode layer is made of an electrochemical active electrode material, and one of the bottom electrode 2 or the top electrode 4 is required to be a metal with high light transmittance, such as ITO (indium tin oxide), because the subsequent light regulation and control operation requires that light energy is transmitted through the electrode and is incident into the core-shell quantum dot film.
Optionally, the parameters of the ITO film magnetron sputtering coating process are as follows: sputtering power of pulse direct current power supply: 1000w, working air pressure: constant pressure control 3mTorr, working gas: ar (purity 99.99%) 50sccm, O2(purity 99.999%) 1sccm, substrate 1 temperatureDegree: at 300 ℃.
In one embodiment of the present invention, the forming of the core-shell quantum dot layer 3 on the bottom electrode 2 includes: and spin-coating the core-shell quantum dot solution on the bottom electrode 2, and annealing to form a core-shell quantum dot layer 3.
In the spin coating process, the film forming property of the core-shell quantum dot solution can be influenced by the concentration of the core-shell quantum dot solution and the spin coating condition, so that the performance of the memristor is influenced. If the concentration is too low or the spin-coating rotation speed is too high, the thickness of the obtained film is thin and sparse, and when the top electrode 4 is subjected to vapor deposition, metal easily permeates into the film and even directly contacts with the bottom electrode 2, so that the off-state resistance value of the device is reduced or the device is in a conducting state. If the concentration is too high or the spin-coating speed is too low, the obtained thin film is dense but has too large thickness, and the operating voltage of the device is affected. Optionally, the concentration of the core-shell quantum dot solution is 4-5 [ mu ] mol/L; the spin speed was 2000rpm and the spin time was 40 s.
Optionally, the temperature of the annealing treatment is 80-150 ℃.
In the present invention, the solvent in the core-shell quantum dot solution may be water, and further, the solvent is deionized water.
In the preparation process, after spin coating of the core-shell quantum dot solution to form a film, annealing at a specific temperature overnight, wherein the specific value depends on the volatilization temperature of the solvent, so that the solvent component is completely removed, otherwise, the residual solvent can influence the performance of the final resistance change device; for example, some residual solvents may cause defect states to form on the surface of the quantum dots, which affects the carrier transport performance of the quantum dots during device operation, so that the memristor exhibits unexpected properties, possibly a negative differential resistance effect. Moreover, some solvents may also serve as a resistance change layer of the memristive device, the residual solvents complicate the whole physical system, subsequent mechanism analysis is difficult to perform, and optimization of device performance is not facilitated.
The size and the structure of the core-shell quantum dot determine the optical performance and the energy band structure of the core-shell quantum dot, and the size and the structure of the core-shell quantum dot influence the carrier transmission performance and the light responsiveness of the film. If CdS/PbS core-shell quantum dots with different shell thicknesses can influence the on-off ratio of the memristor, InP/ZnSe/ZnS core-shell quantum dots can enable the performance of the memristor to be better and more stable than InP/ZnSe core-shell quantum dots, and the multi-stage storage of the memristor can be realized by designing the energy band structure of the quantum dots.
In one embodiment of the present invention, the forming of the top electrode 4 on the core-shell quantum dot layer 3 includes:
the top electrode 4 is formed by depositing a material for the top electrode 4 on the core-shell quantum dot layer 3 by a thermal evaporation method.
Alternatively, the degree of vacuum for the thermal evaporation method for preparing the silver top electrode 4 may be 1 × 10-4Pa。
The invention also provides a regulation and control method of the storage mode of the conductive filament type memristor, wherein the storage mode of the conductive filament type memristor is converted by irradiating the conductive filament type memristor with light;
the storage modes are a volatile storage mode and a non-volatile storage mode.
The conductive filament type memristor is based on the core-shell quantum dots, regulation and control of current carriers in a dielectric layer can be achieved according to the photoresponsive performance of the memristor, the stability of a conductive filament formed in the memristor can be affected by the distribution of the internal current carriers, the storage performance of a device is further affected, and the multifunctional photoregulating memristor is achieved. Compared with the traditional storage mode control mode, the light control method has the advantages of remote control, no damage, simplicity and the like.
Example 1
This embodiment prepares a conductive filament type memristor of sandwich structure, includes: the quantum dot structure comprises a substrate 1, a bottom electrode 2 formed on the substrate 1, a core-shell quantum dot layer 3 formed on the bottom electrode 2, and a top electrode 4 formed on the core-shell quantum dot layer 3.
The preparation process of the conductive filament type memristor comprises the following steps: the memristor is prepared on a transparent substrate 1 such as glass, and 100-nanometer-thick ITO is deposited on the substrate 1 through magnetron sputtering and is used as a bottom electrode 2; forming 100 μ L of a 10mg/mL InP/ZnS core-shell quantum dot solution on the bottom electrode 2 by spin coating, and annealing overnight at 100 degrees celsius to completely remove the solvent (toluene) component in the solution; and finally, depositing a 30-nanometer patterned silver top electrode 4 on the core-shell quantum dot film by a thermal evaporation method, wherein the top electrode 4 and the bottom electrode 2 form a cross shape, and each intersection point is a memristor.
The invention utilizes the light responsiveness of the core-shell quantum dots to realize the mode conversion of the light-regulated memory, simplifies the operation process and ensures that the regulation and control of the device are more efficient and have stronger controllability. The device provided by the invention has a simple structure, the controllability of the core-shell quantum dot material layer is strong, and the performance of the device can be optimized by adjusting the type, size and structure of the core-shell quantum dots.
It is to be understood that the invention is not limited to the examples described above, but that modifications and variations may be effected thereto by those of ordinary skill in the art in light of the foregoing description, and that all such modifications and variations are intended to be within the scope of the invention as defined by the appended claims.
Claims (10)
1. A conductive filament-type memristor, comprising:
the quantum dot structure comprises a bottom electrode, a core-shell quantum dot layer formed on the bottom electrode and a top electrode formed on the core-shell quantum dot layer.
2. The electrically conductive filament-type memristor of claim 1, wherein the bottom electrode comprises a plurality of strip-shaped bottom electrodes, the top electrode comprises a plurality of strip-shaped top electrodes;
the strip-shaped bottom electrodes are transversely and parallelly arranged on the lower side face of the core-shell quantum dot layer, and the strip-shaped top electrodes are longitudinally and parallelly arranged on the upper side face of the core-shell quantum dot layer.
3. The conductive filament-type memristor of claim 1, wherein the core-shell quantum dot layer is selected from one of an indium phosphide-zinc sulfide core-shell quantum dot layer, an indium phosphide-zinc selenide core-shell quantum dot layer, a chromium selenide-zinc sulfide core-shell quantum dot layer, a lead selenide-lead sulfide core-shell quantum dot layer, a cadmium sulfide-lead sulfide core-shell quantum dot layer.
4. The conductive filament-type memristor of claim 1, wherein the bottom electrode is an ITO bottom electrode.
5. The conductive filament-type memristor of claim 1, wherein the top electrode is a silver top electrode.
6. A method of making the conductive filament-type memristor of claim 1, comprising:
forming a bottom electrode on a substrate;
forming a core-shell quantum dot layer on the bottom electrode;
and forming a top electrode on the core-shell quantum dot layer.
7. The method of fabricating a conductive filament-type memristor according to claim 6, wherein the forming of the bottom electrode on the substrate comprises:
and depositing an ITO material on the substrate by a magnetron sputtering method to form a bottom electrode.
8. The method of fabricating a conductive filament-type memristor according to claim 6, wherein the forming of the core-shell quantum dot layer on the bottom electrode comprises:
and spin-coating the core-shell quantum dot solution on the bottom electrode, and annealing to form a core-shell quantum dot layer.
9. The method of making a conductive filament-type memristor according to claim 6, wherein the forming of the top electrode on the core-shell quantum dot layer comprises:
and depositing a top electrode material on the core-shell quantum dot layer by a thermal evaporation method to form the top electrode.
10. A regulation and control method for a storage mode of a conductive filament type memristor is characterized in that the storage mode of the conductive filament type memristor is converted by irradiating the conductive filament type memristor according to any one of claims 1 to 5 with light;
the storage mode includes a volatile storage mode and a non-volatile storage mode.
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