CN109659433B - Memristor with adjustable volatile resistance and nonvolatile resistance conversion behaviors and preparation method thereof - Google Patents

Memristor with adjustable volatile resistance and nonvolatile resistance conversion behaviors and preparation method thereof Download PDF

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CN109659433B
CN109659433B CN201811340222.2A CN201811340222A CN109659433B CN 109659433 B CN109659433 B CN 109659433B CN 201811340222 A CN201811340222 A CN 201811340222A CN 109659433 B CN109659433 B CN 109659433B
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functional layer
memristor
lower electrode
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upper electrode
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CN109659433A (en
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李祎
李灏阳
缪向水
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Huazhong University of Science and Technology
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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 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
    • 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 without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
    • H10N70/011—Manufacture or treatment of multistable switching devices
    • H10N70/021—Formation of the switching material, e.g. layer deposition
    • 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 without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
    • H10N70/801—Constructional details of multistable switching devices
    • H10N70/881—Switching materials

Abstract

The application discloses memristor that volatile and nonvolatile resistance transformation behaviors can be regulated and control and preparation method thereof, including: the device comprises a lower electrode, a functional layer and an upper electrode, wherein the lower electrode is positioned on the surface of a substrate, the upper electrode is positioned on the uppermost layer of the device, and the functional layer is clamped between the upper electrode and the lower electrode to form a sandwich structure. The functional layer is composed of a first functional layer and a second functional layer with different ion mobilities, the first functional layer is in contact with the lower electrode, and the second functional layer is arranged above the first functional layer and in contact with the upper electrode. The technical scheme provided by the application realizes the regulation and control of the transformation behaviors of the device and the nonvolatile resistor by changing the thickness of the functional layer, and changes the structure of the device without changing the material composition of the device, so that the same process can be used when a full memristive neural network is constructed, the difficulty and the complexity of the preparation process are reduced, and meanwhile, the method is compatible with the existing CMOS process, and is favorable for large-scale industrial implementation.

Description

Memristor with adjustable volatile resistance and nonvolatile resistance conversion behaviors and preparation method thereof
Technical Field
The invention belongs to the technical field of microelectronic devices, and particularly relates to a memristor with adjustable volatile and nonvolatile resistance conversion behaviors and a preparation method thereof.
Background
The resistive random access memory is a mature memristor device, and the resistance value of the device is changed by using the change of the conductive property in the functional layer of the device, so that the resistance states with different heights are achieved. The existing resistive random access memory is basically nonvolatile, and can be used for logic calculation or large-scale storage by utilizing the characteristic that the stored information cannot be changed. On the other hand, its unique electrical properties make it suitable for use in synaptic devices as well. Meanwhile, some volatile resistive random access memories also exist, and have a certain application prospect, so that the characteristic that the resistance state of the resistive random access memory is not easy to keep can be utilized as a TS (Threshold switch) for an integrated circuit, and the resistive random access memory can also be used for the composition of a neuron circuit in a neural network. Meanwhile, the characteristics of the volatile device and the nonvolatile device are utilized to construct a neural network with full memristance.
There is much literature on the transition of volatile and non-volatile resistance transition behavior of devices. Document Volatile and Non-Volatile Switching in Cu-SiO2In the Programmmable Metallimationcells, when the device is SiO2When Cu is doped as a functional layer, the device isPresenting volatile having TS characteristics; when the device is SiO without doping2When used as a functional layer, the device exhibits nonvolatile MS (memristive Switch) characteristics. Although the volatility and the non-volatility of the device can be changed by doping and non-doping, the doping mode is complex and involves operations such as annealing, and when a neural network of the full memristor is constructed, the difficulty and the complexity of preparation are increased by two different processes of doping and non-doping. In some other documents, the volatile and nonvolatile resistance transition behavior of the device is changed by changing the limiting current of the device, and at low current limit, the device conductive filament is unstable and volatile, while at high current limit, the device conductive filament is stable and nonvolatile. This method is simple in operation, but it is difficult to achieve different current limiting for different devices, the misoperation may be large, and large-scale operation in an array device is not easy, so that large-scale implementation in industry is impossible. The prior art also adopts a graphene barrier layer, but is not compatible with the existing CMOS process.
Disclosure of Invention
Aiming at the defects or improvement requirements of the prior art, the invention provides a memristor with adjustable volatile resistance and nonvolatile resistance conversion behaviors and a preparation method thereof, and aims to change the structure of a device without changing the material composition of the device, use the same process when constructing a full memristor neural network, avoid adding process difficulty and complexity, have simple adjustment and control operation, be compatible with the existing CMOS process and be beneficial to large-scale industrial implementation.
The invention utilizes the CBRAM (Conductive bridge random access memory) principle, the functional layer is composed of a first functional layer and a second functional layer with different ion mobility, and the metal ions of the upper electrode are transferred to the second functional layer with low ion mobility through the first functional layer with high ion mobility and finally reach the lower electrode. When voltage is applied, the diffusion rate of active metal ions in the material with high ion mobility is high, and a large number of metal ions are reduced into metal particles at the lower end to form the conductive wire with a trapezoid structure with a narrow upper part and a wide lower part; in the low ion mobility material, the mobility rate of active metal ions is low, a large number of metal ions are reduced at a position close to the upper side, and only a small number of metal ions can reach the lower electrode, so that the conductive wire formed by the reduced metal particles is in a trapezoidal structure with a wide upper part and a narrow lower part. When the thickness of the low ion migration rate material is thickened, less metal ions can reach the lower electrode, the stability of the conductive wire is poor, and when the external voltage is lost, the metal particles form separated metal particle clusters and are changed into a high configuration. Therefore, by using the mode and adopting the double-layer structure of the first functional layer and the second functional layer, the active metal ions form the stable conductive wire through the high-ion-mobility material so as to enhance the stability of the device, and meanwhile, the stability of the conductive wire of the device is regulated and controlled by changing the thickness of the low-ion-mobility material so as to respectively obtain the devices with volatile and nonvolatile characteristics.
To achieve the above objects, according to one aspect of the present invention, the exemplary embodiments described herein provide a memristor with controllable volatile and non-volatile resistance transition behaviors, including a lower electrode, a functional layer, and an upper electrode;
the lower electrode is positioned on the surface of the substrate, the upper electrode is positioned on the uppermost layer of the device, and the functional layer is clamped between the upper electrode and the lower electrode to form a sandwich structure.
The functional layer is composed of a first functional layer and a second functional layer with different ion mobility, wherein the first functional layer adopts Al2O3、HfO2、TiO2、SiO2、Ta2O5、ZrO2、Y2O or Si3N4Plasma low-ion mobility material in contact with the lower electrode, and GeTe, GeSe, CuI and Cu as the second functional layer2HgI4、Cu2Se (copper ion conductor), RbAg4I5α -AgI, AgX or Ag2And a material with high ion mobility such as S (silver ion conductor) is arranged above the first functional layer and is in contact with the upper electrode. The ion mobility of the first functional layer is lower than that of the second functional layer, whether the memristor can form a stable conductive wire similar to a cone is determined by changing the thickness of the low ion mobility material functional layer,if the thickness of the first functional layer is less than the first critical thickness L of the low ion mobility materialn，LnThe range is 3 nm-4 nm, the functional layer forms stable conductive filaments, the device is non-volatile, and if the thickness of the first functional layer is larger than the second critical thickness L of the low ion mobility materialm，LmThe range is 4 nm-8 nm, the functional layer can not form stable conductive wires, and the device is volatile.
Preferably, the thickness of the second functional layer is 10nm to 100nm.
Preferably, the thickness of the first functional layer is 1 nm-4 nm, which is smaller than the first critical thickness of the low ion mobility material, so as to form a stable conductive wire, and the device is nonvolatile; the thickness of the first functional layer is 4 nm-10 nm and is larger than the second critical thickness of the low ion mobility material, so that a stable conductive wire cannot be formed, and the device is nonvolatile.
Preferably, the lower electrode is made of an inert metal material, such as TaN, TiN, TiAlN, TiW, Pt, TiN or TiW, with a thickness of 100nm.
Preferably, the upper electrode is made of an active metal material, such as Cu, Ag or Ni, with a thickness of 100nm.
To achieve the object of the present invention, according to another aspect of the present invention, there is provided a method for preparing a memristor with controllable volatile and nonvolatile resistance transition behaviors, including:
forming a lower electrode on the surface of the substrate;
forming a first functional layer positioned on the surface of the lower electrode according to a preset first process flow, wherein the first process flow comprises atomic layer deposition and the like;
forming a second functional layer positioned on the surface of the first functional layer according to a preset second process flow, wherein the second process flow comprises magnetron sputtering and the like;
and forming an upper electrode on the surface of the second functional layer.
The ion mobility of the first functional layer formed by the first process flow is lower than that of the second functional layer formed by the second process flow.
Compared with the prior art, the memristor with adjustable volatile resistance and nonvolatile resistance conversion behaviors and the preparation method thereof provided by the invention can obtain the following beneficial effects:
1. the functional layer of the device is formed by a double-layer structure of a first functional layer and a second functional layer with different ion mobility, and a stable conductive wire is formed by a high-ion-mobility material of the first functional layer so as to enhance the stability of the device; meanwhile, the stability of the conductive wire is regulated and controlled by changing the thickness of the low-ion-mobility material of the second functional layer, so that the volatility and the non-volatility of the device are changed, and the regulation and control of the conversion behavior of the volatile resistance and the non-volatile resistance of the device are realized.
2. The structure of the device is changed without changing the material composition of the device, so that the preparation method has process identity, and the difficulty and complexity of the preparation process are reduced;
3. the volatile and nonvolatile resistance transition behaviors of the device are not influenced by the current limiting height, the misoperation is possibly small, and the large-scale operation of the device in the array is easy.
4. The preparation process is compatible with the existing CMOS process and can be realized industrially in large scale.
Drawings
FIG. 1 is a schematic diagram of a structure of a memristor with adjustable volatile and nonvolatile resistance transition behaviors, according to an embodiment of the present disclosure;
fig. 2 is a schematic diagram of a volatile and nonvolatile structure of a memristor with adjustable volatile and nonvolatile resistance transition behaviors, according to an embodiment of the present invention;
FIG. 3 is a graph of ideal current-voltage relationships for volatile and non-volatile applications, according to an embodiment of the present invention;
fig. 4 is a schematic diagram of a principle of a memristor with a switchable volatile and nonvolatile resistance transition behavior according to an embodiment of the present invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
Fig. 1 is a schematic structural diagram of a memristor with adjustable volatile and nonvolatile resistance transition behaviors, which is provided in an embodiment of the present invention, and referring to fig. 1, the embodiment provides a memristor with adjustable volatile and nonvolatile resistance transition behaviors, specifically, the memristor includes a lower electrode, a functional layer, and an upper electrode, the lower electrode is located on a substrate surface, the upper electrode is located on an uppermost layer of a device, and the functional layer is sandwiched between the upper electrode and the lower electrode to form a sandwich structure.
The functional layer is composed of a first functional layer and a second functional layer with different ion mobilities, and the first functional layer in contact with the lower electrode can be Al2O3、HfO2、TiO2、SiO2、Ta2O5、ZrO2、Y2O or Si3N4A low ion mobility material, more specifically, Al in this example2O3The second functional layer in contact with the upper electrode may be GeTe, GeSe, CuI, Cu2HgI4、Cu2Se、RbAg4I5α -AgI, AgX or Ag2The thickness of the first functional layer of the present invention has a critical thickness that determines the device' S performance to be volatile and non-volatile, i.e., the critical thickness of the low ion mobility material, which has a first critical thickness of LnAnd a second critical thickness LmFirst critical thickness LnIn the range of 3nm to 4nm, and a second critical thickness of LnIn the range of 4nm to 8nm, as shown in FIG. 2, if the thickness of the first functional layer is less than the first critical thickness L of the low ion mobility materialnIf the thickness of the first functional layer is larger than the critical thickness L of the second material of the low ion mobility materialmThe functional layer cannot form stable conductive wires, and the device is volatile.
For a memory device, the important characteristics of volatility and non-volatility are that the existing state of the device can be maintained after the applied voltage is lost, orWhether the saved information will disappear. The ideal current-voltage relationship diagram of the memristor in the volatile and nonvolatile states is shown in fig. 3, and IV curves obtained by testing memristor devices with different properties are shown in the diagram respectively. Under the non-volatile condition, in the cyclic scanning process that the voltage of the device returns to 0 from 0 to Vset, the device is changed from high configuration to low configuration at the Vset point, and then is changed from 0 to Vreset to 0 when negative scanning is carried out, and the low resistance state of the device is changed to high configuration at the Vreset point; for a volatile device, the main difference is that after a positive scan from 0 to Vset, the device will change from the high configuration to the low resistance state at the Vset point, but when the applied voltage returns to 0, the state will automatically return to the high configuration, and during the negative scan, the device does not exhibit the low resistance state but remains in the high resistance state. In the present embodiment, the first functional layer Al is changed2O3To control the amount of metal ions that migrate into the functional layer and thereby control the volatile to non-volatile transition of the device. In the first functional layer Al2O3When the thickness of (2) is 3nm, metal ions are in Al due to the thin material thickness2O3More diffusion can reach the lower electrode, so that a conductive wire is easy to form, and the device is nonvolatile; when Al is present2O3When the thickness of (2) is 5nm, the metal ion cannot be in Al2O3When the voltage is not applied any more, the conductive wire formed by the metal ions is unstable and is easy to break, so that the device is volatile. Referring to the schematic diagram of the principle of the memristor with adjustable volatile and nonvolatile resistance transition behaviors shown in fig. 4, the diffusion behavior of metal ions is embodied.
The lower electrode is made of an inert metal such as TaN, TiN, TiAlN, TiW, Pt, TiN or TiW, and more specifically, Pt in this embodiment.
The upper electrode is made of an active metal such as Cu, Ag or Ni, and more specifically, Cu in the present embodiment.
The embodiment of the application further provides a preparation method of the memristor with adjustable volatile resistance and nonvolatile resistance conversion behaviors. The method comprises the following steps:
forming a lower electrode on the surface of the substrate;
forming a first functional layer positioned on the surface of the lower electrode according to a preset first process flow;
forming a second functional layer positioned on the surface of the first functional layer according to a preset second process flow;
and forming an upper electrode on the surface of the second functional layer.
In practical applications, the preparation method of the memristor embodiment is explained in detail.
S1, cleaning a substrate, which specifically comprises the following steps:
s101, acetone cleaning: will grow SiO2Immersing the Si substrate of the insulating layer into an acetone solution, and carrying out ultrasonic cleaning;
s102, absolute ethyl alcohol cleaning: immersing the sample soaked and cleaned in the step S101 into absolute ethyl alcohol, and carrying out ultrasonic cleaning;
s103, deionized water cleaning: washing and drying the cleaning sample in the step S102 by using deionized water;
s2, forming a lower electrode on the surface of the substrate, and specifically comprising the following steps:
s201, forming an adhesion layer on the surface of the substrate through magnetron sputtering, wherein the adhesion layer can be Ti specifically and has the thickness of 100nm. The magnetron sputtering process conditions can be as follows: under Ar gas atmosphere, the background vacuum is 5 x 10-5Pa, working pressure of 0.5Pa, direct current sputtering power of 100W and sputtering time of 500 s;
s202, forming a lower electrode positioned on the surface of the adhesion layer through magnetron sputtering, wherein the lower electrode can be Pt specifically, the thickness is 100nm, and the process conditions of the magnetron sputtering can be as follows: ar gas atmosphere, background vacuum 5 x 10-5Pa, working pressure of 0.5Pa, direct-current sputtering power of 35W and sputtering time of 700 s;
s3, forming a first functional layer positioned on the surface of the lower electrode according to a preset first process flow, wherein the first functional layer can be specifically Al2O3. When Al is present2O3When the thickness is 1 nm-4 nm,the device will appear non-volatile; when Al is present2O3With a thickness of 4nm to 10nm, the device will appear volatile.
In practical applications, the first process flow may be implemented by atomic layer deposition. The conditions of the atomic layer deposition process may be: the nitrogen flow rate is 0.5sccm, the pressure of the reaction chamber is 100-2O。
And S4, forming a second functional layer positioned on the surface of the first functional layer according to a preset second process flow, wherein the second functional layer can be specifically GeTe and has the thickness of 20 nm.
In practical applications, the second process flow may be implemented by magnetron sputtering. The conditions of the magnetron sputtering process can be as follows: under Ar gas atmosphere, the background vacuum is 5 x 10-5Pa, working pressure of 0.5Pa and sputtering power of 60W.
And S5, forming an upper electrode positioned on the surface of the second functional layer through magnetron sputtering, wherein the upper electrode can be Cu, and the thickness of the upper electrode is 100nm. The magnetron sputtering process conditions can be as follows: under Ar gas atmosphere, the background vacuum is 5 x 10-5Pa, working pressure of 0.5Pa, direct current sputtering power of 60W and sputtering time of 600 s.
The above description is only a preferred embodiment of the present application, but the scope of the present application is not limited thereto, and any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present application should be covered within the scope of the present application. Therefore, the protection scope of the present application shall be subject to the protection scope of the claims.

Claims (5)

1. A memristor with adjustable volatile and non-volatile resistance transition behavior, the memristor comprising: a lower electrode, a functional layer and an upper electrode, wherein the lower electrode is positioned on the surface of the substrate, the upper electrode is positioned on the uppermost layer of the device, the functional layer is clamped between the upper electrode and the lower electrode to form a sandwich structure,
the functional layer is composed of a first functional layer and a second functional layer with different ion mobilities, the first functional layer is in contact with the lower electrode, and the second functional layer is arranged above the first functional layer and is in contact with the upper electrode; the first functional layer has a lower ion mobility than the second functional layer; the first functional layer is made of Al2O3、HfO2、TiO2、SiO2、Ta2O5、ZrO2、Y2O or Si3N4The second functional layer is made of GeTe, GeSe, CuI and Cu2HgI4、Cu2Se、RbAg4I5α -AgI, AgX or Ag2S；
When the thickness of the first functional layer is less than the first critical thickness LnWhen the memristor is used, a stable conductive wire is formed by the memristor, and a nonvolatile behavior is presented;
when the thickness of the first functional layer is larger than the second critical thickness LmWhen the memristor is used, the memristor cannot form a stable conductive wire and presents a volatile behavior;
second critical thickness LmGreater than the first critical thickness Ln。
2. The memristor of claim 1, wherein the first critical thickness LnIn the range of 3nm to 4nm, and a second critical thickness of LmThe range is 4nm to 8 nm.
3. The memristor of claim 1, wherein a lower electrode of the memristor employs an inert metal material.
4. The memristor of claim 1, wherein an upper electrode of the memristor employs an active metal material.
5. A preparation method of a memristor with adjustable volatile resistance and nonvolatile resistance conversion behaviors is characterized by comprising the following steps:
forming a lower electrode on the surface of the substrate;
forming a first functional layer positioned on the surface of the lower electrode according to a preset first process flow;
forming a second functional layer positioned on the surface of the first functional layer according to a preset second process flow; the ion mobility of the first functional layer formed by the first process flow is lower than that of the second functional layer formed by the second process flow; the first functional layer is made of Al2O3、HfO2、TiO2、SiO2、Ta2O5、ZrO2、Y2O or Si3N4The second functional layer is made of GeTe, GeSe, CuI and Cu2HgI4、Cu2Se、RbAg4I5α -AgI, AgX or Ag2S；
And forming an upper electrode on the surface of the second functional layer.
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