CN109473547B - Flexible synapse bionic device and preparation method thereof - Google Patents

Flexible synapse bionic device and preparation method thereof Download PDF

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CN109473547B
CN109473547B CN201811265425.XA CN201811265425A CN109473547B CN 109473547 B CN109473547 B CN 109473547B CN 201811265425 A CN201811265425 A CN 201811265425A CN 109473547 B CN109473547 B CN 109473547B
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赵波
张超金
吴莹
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Jiangsu Normal University
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    • H10N70/00Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
    • H10N70/801Constructional details of multistable switching devices
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    • H10N70/00Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
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    • H10N70/00Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
    • H10N70/801Constructional details of multistable switching devices
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Abstract

The invention discloses a flexible synapse bionic device and a preparation method thereof, which sequentially comprise a flexible substrate, a bottom electrode film, an anoxic titanium dioxide film layer, a zinc oxide film layer and a top electrode film from bottom to top, wherein the bottom electrode film and the top electrode film are connected with a power supply through electrode leads; the preparation method comprises the steps of sequentially forming a bottom electrode film, an anoxic titanium dioxide film layer, a zinc oxide film layer and a top electrode film on a flexible substrate, then arranging electrode leads on the bottom electrode film and the top electrode film, and fixing the electrode leads with contact points of the bottom electrode film and the top electrode film by adopting high-frequency ultrasonic waves. The flexible synapse bionic device not only effectively avoids the damage of the flexible substrate caused by the stress generated between the bottom electrode or the top electrode and the flexible substrate due to the mechanical energy or the heat energy generated by the fixed electrode lead, but also can improve the time retentivity and the fatigue resistance of the device and prolong the service life.

Description

Flexible synapse bionic device and preparation method thereof
Technical Field
The invention belongs to the field of microelectronic devices, and particularly relates to a flexible synapse bionic device and a preparation method thereof.
Background
With the further scaling of semiconductor device feature sizes, the traditional integrated circuit technology is facing a serious challenge, and developing brain-like intelligent computers is the direction and target of artificial intelligence development in the future. The neural network of the human brain is a highly parallel information processing system, can efficiently process various information such as vision, hearing and the like, and has important significance for the development of artificial intelligence by simulating the abilities of perception, thinking, judgment, learning and the like of the human brain.
The neural synapse is a basic unit of a brain neural network, and synapse plasticity is the basis of human brain learning and memory, so that the bionic simulation of synapses is an important step for realizing artificial intelligence. In previous researches, a plurality of transistors and corresponding peripheral circuits are needed for simulating a nerve synapse, so that the power consumption is huge and the integration level is seriously influenced. The memristor and the nerve synapse have similar nonlinear electrical properties, have the advantages of simple structure, high integration level and the like, and have great application prospects by utilizing the memristor to simulate the nerve synapse in the neuromorphic circuit.
The flexible electronic device changes the interaction mode of a human body and the digital world, and is expected to realize seamless butt joint of the human body and the digital world. At present, most researches on synapse bionic devices are concentrated on memristors such as silicon-based semiconductors, and few researches on the memristors based on flexible substrates are carried out, because when the flexible substrates are adopted for electrode leads, mechanical energy or heat energy generated by a connection process can be transferred to the flexible substrates and functional materials on the flexible substrates, and the performance of flexible electronic devices is further damaged.
Disclosure of Invention
The purpose of the invention is as follows: the first purpose of the invention is to provide a synapse bionic device adopting a flexible substrate, and the device inhibits the change of an internal microstructure, and improves the time retentivity and the fatigue resistance of a synapse bionic electronic device;
the second purpose of the invention is to provide a preparation method of the flexible synapse bionic device.
The technical scheme is as follows: the flexible synapse bionic device comprises a flexible substrate, a bottom electrode film, an anoxic titanium dioxide film layer, a zinc oxide film layer and a top electrode film from bottom to top in sequence, wherein the bottom electrode film and the top electrode film are connected with a power supply through electrode leads.
Preferably, the flexible substrate may be a polyimide, polyethylene terephthalate, polyethylene naphthalate, or polycarbonate film. The thickness of the flexible substrate may be 0.5-2 mm. The bottom electrode film can be a tin-doped indium oxide, aluminum-doped zinc oxide, or fluorine-doped tin oxide film. The thickness of the oxygen-deficient titanium dioxide film layer can be 10-50nm, the thickness of the titanium dioxide film layer can be 100-500nm, and the thickness of the zinc oxide film layer can be 100-1000 nm. The top electrode film may be a copper film, a platinum film or a gold film. The top electrode film may have a thickness of 20-100nm, and the bottom electrode film may have a thickness of 50-1000 nm.
The method for preparing the flexible synapse bionic device comprises the following steps:
(1) sequentially forming a bottom electrode film, an anoxic titanium dioxide film layer, a zinc oxide film layer and a top electrode film on a flexible substrate;
(2) and arranging electrode leads on the bottom electrode film and the top electrode film, and fixing the electrode leads with contact points of the bottom electrode film and the top electrode film by adopting high-frequency ultrasonic waves to prepare the flexible synapse bionic device.
According to the invention, the flexible substrate is adopted, the anoxic titanium dioxide film layer, the titanium dioxide film layer and the zinc oxide film layer are sequentially arranged between the bottom electrode film and the top electrode film, and the high-frequency ultrasonic wave is combined to fix the electrode lead, so that the prepared device has good time retentivity and fatigue resistance, and the service life of the device is prolonged. Firstly, an oxygen-deficient titanium dioxide thin film layer is arranged between a bottom electrode and a top electrode thin film, the atomic ratio of Ti to O in the buffer layer oxygen-deficient titanium dioxide thin film is more than 1:2, the arrangement of the oxygen-deficient titanium dioxide thin film effectively relieves the lattice stress and the interface mismatch between the titanium dioxide thin film and a transparent conductive thin film, and simultaneously provides a nucleation template for the growth of the titanium dioxide thin film, thereby being beneficial to the deposition of titanium dioxide and improving the quality of the titanium dioxide thin film; secondly, high-frequency ultrasonic waves are applied to contact points of the electrode lead, the bottom electrode and the top electrode, ultrasonic energy is transmitted to a contact interface of the lead and the conductive film, metal atoms on the interface generate two-dimensional creeping on the surface of the conductive film within a nanoscale range, and the metal atoms are bonded with the top electrode and the bottom electrode atoms on the interface through diffusion, so that the metal electrode lead is firmly and mechanically connected and efficiently electrically contacted with the surfaces of the two electrodes.
Furthermore, the high-frequency ultrasonic wave is applied to the contact points of the electrode lead wire, the bottom electrode film and the top electrode film through an aluminum oxide ceramic welding head, the end part of the welding head is a plane, and the area is 0.1-3mm2The surface roughness is 0.5-5 μm, and the pressing force applied to the welding head is 0.05-1N. Preferably, the frequency of the high-frequency ultrasonic wave is 80-150kHz, and the energy is 1-5J.
Has the advantages that: compared with the prior art, the invention has the following remarkable advantages: the flexible synapse bionic device firstly breaks through the existing method for preparing the device on the hard substrate, adopts the flexible substrate, and an oxygen-deficient titanium dioxide film layer, a titanium dioxide film layer and a zinc oxide film layer are arranged on the substrate and between the bottom electrode film and the top electrode film, the electrode lead is fixed by combining high-frequency ultrasonic waves, so that the damage of the flexible substrate caused by stress generated between the bottom electrode or the top electrode and the flexible substrate due to mechanical energy or thermal energy generated by fixing the electrode lead is effectively avoided, after the electrode lead is fixed by ultrasonic waves, the intact bottom electrode film and the intact top electrode film are combined with the anoxic titanium dioxide film layer, the titanium dioxide film layer and the zinc oxide film layer, so that the microstructure of the material is not influenced during working, the time retentivity and the fatigue resistance of a device are improved, and the service life is prolonged.
Drawings
FIG. 1 is a schematic structural diagram of a synapse biomimetic device in accordance with the present invention.
Detailed Description
The technical solution of the present invention will be further described in detail with reference to the following examples.
Example 1
The flexible synapse bionic device comprises a flexible polyimide substrate 1, a bottom electrode tin-doped indium oxide film 2, an oxygen-deficient titanium dioxide film layer 3, a titanium dioxide film layer 4, a zinc oxide film layer 5 and a top electrode copper film 6 in sequence from bottom to top, as shown in figure 1. The thickness of the flexible substrate 1 is 1mm, the thickness of the bottom electrode film 2 is 500nm, the thickness of the anoxic titanium dioxide film 3 is 25nm, the thickness of the titanium dioxide film layer 4 is 500nm, the thickness of the zinc oxide film layer 5 is 1000nm, and the thickness of the top electrode film 6 is 70 nm.
The method for preparing the flexible synapse bionic device comprises the following steps:
(1) preparing a bottom electrode film on a flexible substrate by adopting a magnetron sputtering method: sputtering for 20min at the sputtering power of 150W and the temperature of 50 ℃ by taking tin-doped indium oxide as a sputtering target material and argon as sputtering gas to prepare a bottom electrode thin film layer;
(2) preparing an oxygen-deficient titanium dioxide film layer on the bottom electrode film by adopting a magnetron sputtering method: taking metal titanium as a sputtering target material, taking a mixed gas of oxygen and argon as a sputtering gas (the flow ratio of oxygen to argon is 0.05:1), and sputtering for 15min under the conditions of sputtering power of 100W and temperature of 70 ℃ to prepare an oxygen-deficient titanium dioxide thin film layer;
(3) preparing a titanium dioxide film layer on the oxygen-deficient titanium dioxide film layer by adopting a magnetron sputtering method: sputtering for 20min at the sputtering power of 200W and the temperature of 70 ℃ by taking titanium dioxide as a sputtering target and argon as sputtering gas to prepare a titanium dioxide film layer;
(4) preparing a zinc oxide film layer on the titanium dioxide film layer by adopting a magnetron sputtering method: taking zinc oxide as a sputtering target material and argon as sputtering gas, and sputtering for 40min under the conditions of sputtering power of 250W and temperature of 30 ℃ to prepare a zinc oxide film layer;
(5) preparing a top electrode film on the zinc oxide film layer by adopting a magnetron sputtering method: sputtering for 10min at the sputtering power of 50W and the temperature of 50 ℃ by taking copper as a sputtering target and argon as sputtering gas to prepare a top electrode film layer;
(6) connecting an electrode lead: arranging electrode leads on the bottom electrode film and the top electrode film, applying an aluminum oxide ceramic welding head on contact points of the electrode leads and the bottom electrode film and the top electrode film, and performing ultrasonic reaction to connect the electrode leads under the conditions of frequency of 100kHz and energy of 3J to obtain a flexible synapse bionic device; wherein the end part of the welding head is a plane with an area of 0.1mm2The surface roughness is 0.5 μm, and the pressing force applied to the welding head is 0.05N.
Example 2
The flexible synapse bionic device comprises a flexible polyethylene glycol terephthalate substrate 1, a bottom electrode aluminum-doped zinc oxide film 2, an oxygen-deficient titanium dioxide film layer 3, a titanium dioxide film layer 4, a zinc oxide film layer 5 and a top electrode platinum film 6 from bottom to top in sequence. The thickness of the flexible substrate 1 is 1.5mm, the thickness of the bottom electrode film 2 is 800nm, the thickness of the anoxic titanium dioxide film 3 is 40nm, the thickness of the titanium dioxide film layer 4 is 300nm, the thickness of the zinc oxide film layer 5 is 500nm, and the thickness of the top electrode film 6 is 80 nm.
The method for preparing the flexible synapse bionic device comprises the following steps:
(1) preparing a bottom electrode film on a flexible substrate by adopting a magnetron sputtering method: sputtering for 15min at the sputtering power of 200W and the temperature of 50 ℃ by taking aluminum-doped zinc oxide as a sputtering target material and argon gas as a sputtering gas to prepare a bottom electrode film layer;
(2) preparing an oxygen-deficient titanium dioxide film layer on the bottom electrode film by adopting a magnetron sputtering method: taking metal titanium as a sputtering target material, taking a mixed gas of argon and oxygen as a sputtering gas (the flow ratio of oxygen to argon is 0.08:1), and sputtering for 20min under the conditions of sputtering power of 100W and temperature of 70 ℃ to prepare an oxygen-deficient titanium dioxide thin film layer;
(3) preparing a titanium dioxide film layer on the oxygen-deficient titanium dioxide film layer by adopting a magnetron sputtering method: sputtering for 15min at the sputtering power of 250W and the temperature of 70 ℃ by taking titanium dioxide as a sputtering target and argon gas as sputtering gas to prepare a titanium dioxide film layer;
(4) preparing a zinc oxide film layer on the titanium dioxide film layer by adopting a magnetron sputtering method: taking zinc oxide as a sputtering target material and argon as sputtering gas, and sputtering for 30min under the conditions of sputtering power of 250W and temperature of 30 ℃ to prepare a zinc oxide film layer;
(5) preparing a top electrode film on the zinc oxide film layer by adopting a magnetron sputtering method: sputtering for 10min at the sputtering power of 150W and the temperature of 50 ℃ by taking platinum as a sputtering target and argon as a sputtering gas to prepare a top electrode film layer;
(6) connecting an electrode lead: arranging electrode leads on the bottom electrode film and the top electrode film, applying an aluminum oxide ceramic welding head on contact points of the electrode leads and the bottom electrode film and the top electrode film, and performing ultrasonic reaction under the conditions of frequency of 120kHz and energy of 2J to connect the electrode leads to obtain a flexible synapse bionic device; wherein the end part of the welding head is a plane with an area of 1mm2The surface roughness was 1 μm, and the pressing force applied to the horn was 0.08N.
Example 3
The flexible synapse bionic device comprises a flexible polyethylene naphthalate substrate 1, a bottom electrode fluorine-doped tin oxide film 2, an oxygen-deficient titanium dioxide film layer 3, a titanium dioxide film layer 4, a zinc oxide film layer 5 and a top electrode gold film 6 from bottom to top in sequence. The thickness of the flexible substrate 1 is 0.5mm, the thickness of the bottom electrode film 2 is 50nm, the thickness of the anoxic titanium dioxide film 3 is 10nm, the thickness of the titanium dioxide film layer 4 is 100nm, the thickness of the zinc oxide film layer 5 is 200nm, and the thickness of the top electrode film 6 is 20 nm.
The method for preparing the flexible synapse bionic device comprises the following steps:
(1) preparing a bottom electrode film on a flexible substrate by adopting a magnetron sputtering method: sputtering for 10min at the sputtering power of 100W and the temperature of 60 ℃ by taking fluorine-doped tin oxide as a sputtering target and argon as sputtering gas to prepare a bottom electrode film layer;
(2) preparing an oxygen-deficient titanium dioxide film layer on the bottom electrode film by adopting a pulse laser deposition method: taking metal titanium as a sputtering target material, taking a mixed gas of argon and oxygen as a sputtering gas (the flow ratio of oxygen to argon is 0.05:1), and sputtering for 10min under the conditions of sputtering power of 100W and temperature of 50 ℃ to prepare an oxygen-deficient titanium dioxide thin film layer;
(3) preparing a titanium dioxide film layer on the oxygen-deficient titanium dioxide film layer by adopting a magnetron sputtering method: sputtering for 15min at the sputtering power of 100W and the temperature of 70 ℃ by taking titanium dioxide as a sputtering target material, argon as sputtering gas and argon as sputtering gas to prepare a titanium dioxide film layer;
(4) preparing a zinc oxide film layer on the titanium dioxide film layer by adopting a magnetron sputtering method: taking zinc oxide as a sputtering target material and argon as sputtering gas, and sputtering for 10min under the conditions of sputtering power of 200W and temperature of 50 ℃ to prepare a zinc oxide film layer;
(5) preparing a top electrode film on the zinc oxide film layer by adopting a magnetron sputtering method: sputtering for 5min under the conditions of sputtering power of 150W and temperature of 50 ℃ by taking gold as a sputtering target and argon as sputtering gas to prepare a top electrode film layer;
(6) connecting an electrode lead: arranging electrode leads on the bottom electrode film and the top electrode film, applying an aluminum oxide ceramic welding head on contact points of the electrode leads and the bottom electrode film and the top electrode film, and performing ultrasonic reaction to connect the electrode leads under the conditions of frequency of 80kHz and energy of 1J to obtain a flexible synapse bionic device; wherein the end part of the welding head is a plane with an area of 2mm2Surface roughness of 3 μm, weldingThe pressing force of the head is 1N.
Example 4
The flexible synapse bionic device comprises a flexible polycarbonate substrate 1, a bottom electrode aluminum-doped zinc oxide film 2, an oxygen-deficient titanium dioxide film layer 3, a titanium dioxide film layer 4, a zinc oxide film layer 5 and a top electrode platinum film 6 from bottom to top in sequence. The thickness of the flexible substrate 1 is 2mm, the thickness of the bottom electrode film 2 is 1000nm, the thickness of the anoxic titanium dioxide film 3 is 50nm, the thickness of the titanium dioxide film layer 4 is 100nm, the thickness of the zinc oxide film layer 5 is 100nm, and the thickness of the top electrode film 6 is 100 nm.
The method for preparing the flexible synapse bionic device comprises the following steps:
(1) preparing a bottom electrode film on a flexible substrate by adopting a magnetron sputtering method: sputtering for 25min at the sputtering power of 200W and the temperature of 70 ℃ by taking aluminum-doped zinc oxide as a sputtering target and argon as sputtering gas to prepare a bottom electrode film layer;
(2) preparing an oxygen-deficient titanium dioxide film layer on the bottom electrode film by adopting a magnetron sputtering method: taking metal titanium as a sputtering target material, taking a mixed gas of argon and oxygen as a sputtering gas (the flow ratio of oxygen to argon is 0.08:1), and sputtering for 15min under the conditions of sputtering power of 150W and temperature of 70 ℃ to prepare an oxygen-deficient titanium dioxide thin film layer;
(3) preparing a titanium dioxide film layer on the anoxic titanium dioxide film layer by adopting pulse laser deposition: sputtering for 15min at the sputtering power of 100W and the temperature of 70 ℃ by taking titanium dioxide as a sputtering target and argon as sputtering gas to prepare a titanium dioxide film layer;
(4) preparing a zinc oxide film layer on the titanium dioxide film layer by adopting a magnetron sputtering method: taking zinc oxide as a sputtering target material and argon as sputtering gas, and sputtering for 20min under the conditions of sputtering power of 150W and temperature of 50 ℃ to prepare a zinc oxide film layer;
(5) preparing a top electrode film on the zinc oxide film layer by adopting a magnetron sputtering method: sputtering for 15min at the sputtering power of 150W and the temperature of 50 ℃ by taking platinum as a sputtering target and argon as sputtering gas to prepare a top electrode film layer;
(6) connecting an electrode lead: arranging electrode leads on the bottom electrode film and the top electrode film, applying an aluminum oxide ceramic welding head on contact points of the electrode leads and the bottom electrode film and the top electrode film, and performing ultrasonic reaction to connect the electrode leads under the conditions of frequency of 150kHz and energy of 5J to obtain a flexible synapse bionic device; wherein the end part of the welding head is a plane with an area of 3mm2The surface roughness is 5 μm, and the pressing force applied to the welding head is 1N.
The flexible synapse bionic device prepared in the embodiments 1-4 is detected, and found that the device can simulate the experience learning and memory capability of synapses, and can still work after continuously switching a plurality of resistance states of the device for more than 1000 times; when the device is placed in the air for 1 year, the state of the device still does not change obviously, and the flexible substrate is not damaged. Therefore, the flexible synapse bionic device prepared by the method has good time retentivity and fatigue resistance.
Comparative example 1
The basic procedure was the same as in example 1 except that the oxygen deficient titanium dioxide thin film layer was not provided. The preparation method is basically the same as that of example 1.
The flexible synapse bionic device prepared by the comparative example is detected, and the device can not work normally and is seriously damaged after being placed for 1 year when a plurality of resistance states of the device are continuously switched for more than 1000 times. Therefore, the oxygen-deficient titanium dioxide thin film layer is arranged below the titanium dioxide thin film layer, so that the lattice stress and the interface mismatch between the titanium dioxide thin film and the bottom electrode thin film can be effectively relieved, the quality of the titanium dioxide thin film is improved, and the service life of a device is further prolonged.
Comparative example 2
The basic procedure is the same as in example 1, except that the electrode leads are connected using a conventional connection method, such as a conductive silver paste bonding method. The preparation method is basically the same as that of example 1.
The flexible synapse bionic device prepared by the comparative example is detected, and the device can not work normally when a plurality of resistance states of the device are continuously switched for more than 1000 times, and after the device is placed for 1 year, the welding spot of the substrate is seriously damaged. Therefore, the electrode lead is connected by adopting high-frequency ultrasonic waves, so that firm mechanical connection and efficient electrical contact of the metal electrode lead on the surfaces of the two electrodes can be realized on the top electrode film and the bottom electrode film, the damage to the flexible substrate is effectively avoided, and the service life of the device is prolonged.

Claims (10)

1. A flexible synapse biomimetic device, comprising: the device sequentially comprises a flexible substrate (1), a bottom electrode film (2), an anoxic titanium dioxide film layer (3), a titanium dioxide film layer (4), a zinc oxide film layer (5) and a top electrode film (6) from bottom to top, wherein the bottom electrode film (2) and the top electrode film (6) are connected with a power supply (8) through electrode leads (7).
2. The flexible synapse biomimetic device of claim 1, wherein: the flexible substrate (1) is a polyimide film, a polyethylene terephthalate film, a polyethylene naphthalate film or a polycarbonate film.
3. The flexible synapse biomimetic device of claim 1, wherein: the thickness of the flexible substrate (1) is 0.5-2 mm.
4. The flexible synapse biomimetic device of claim 1, wherein: the bottom electrode film (2) is a tin-doped indium oxide film, an aluminum-doped zinc oxide film or a fluorine-doped tin oxide film.
5. The flexible synapse biomimetic device of claim 1, wherein: the thickness of the oxygen-deficient titanium dioxide film layer (3) is 10-50nm, the thickness of the titanium dioxide film layer (4) is 100-500nm, and the thickness of the zinc oxide film layer (5) is 100-1000 nm.
6. The flexible synapse biomimetic device of claim 1, wherein: the top electrode film (6) is a copper film, a platinum film or a gold film.
7. The flexible synapse biomimetic device of claim 1, wherein: the thickness of the top electrode film (6) is 20-100nm, and the thickness of the bottom electrode film (2) is 50-1000 nm.
8. A method of making the flexible synapse biomimetic device of claim 1, comprising the steps of:
(1) sequentially forming a bottom electrode film (2), an anoxic titanium dioxide film layer (3), a titanium dioxide film layer (4), a zinc oxide film layer (5) and a top electrode film (6) on a flexible substrate (1);
(2) and arranging electrode leads (7) on the bottom electrode film (2) and the top electrode film (6), and fixing the electrode leads (7) with contact points of the bottom electrode film (2) and the top electrode film (6) by adopting high-frequency ultrasonic waves to obtain the flexible synapse bionic device.
9. The method of claim 8, wherein: the high-frequency ultrasonic wave is applied to the contact points of the electrode lead (7), the bottom electrode film (2) and the top electrode film (6) through an aluminum oxide ceramic welding head, the end part of the welding head is a plane, and the area is 0.1-3mm2The surface roughness is 0.5-5 μm, and the pressing force applied to the welding head is 0.05-1N.
10. The method of claim 8, wherein: the frequency of the high-frequency ultrasonic wave is 80-150kHz, and the energy is 1-5J.
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