CN101958400A - Flexible resistance change memory and manufacturing method thereof - Google Patents
Flexible resistance change memory and manufacturing method thereof Download PDFInfo
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- CN101958400A CN101958400A CN 201010233732 CN201010233732A CN101958400A CN 101958400 A CN101958400 A CN 101958400A CN 201010233732 CN201010233732 CN 201010233732 CN 201010233732 A CN201010233732 A CN 201010233732A CN 101958400 A CN101958400 A CN 101958400A
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Abstract
The invention provides a flexible resistance change memory unit and a manufacturing method thereof. The flexible resistance change memory unit comprises a flexible insulating substrate, a bottom electrode positioned on the flexible insulating substrate, a memory medium layer positioned on the bottom electrode, and a top electrode positioned on the memory medium layer, wherein the memory medium layer is a Zn(1-x)MgxO film, wherein x is more than 0 and less than 1. The flexible resistance change memory can be manufactured at the temperature of below 150 DEG C, and has the advantages of stable resistance change performance and high flexibility.
Description
Technical field
The invention belongs to the resistance-variable storing device field, relate in particular to a kind of flexible resistance-variable storing device and preparation method thereof.
Background technology
Flexible electronic (Flexible Electronics) is the common name of a class technology, comprise plastic electronic (Plastic Electronics), printing electronics (Printed Electronics), organic electronic (Organic Electronics), polymer-electronics (Polymer Electronics) or the like.Flexible electronic can be summarized as the organic electronic device is produced on emerging electronic technology on flexibility/Drawability plastics or the thin metal matrix plate, flexibility/ductility and efficient, low-cost manufacturing process with its uniqueness, has wide application prospect in fields such as information, the energy, medical treatment, national defence, as flexible electronic displays, Organic Light Emitting Diode (OLED), printing radio circuit (RFID), thin-film solar cell panel, electronics surface stickup (Skin Patches) etc.Although develop flexible electronic device at present in succession, also seldom to flexible The Study of Non-Volatile Memory such as flexible wire, flexible PN junction, flexible field effect transistor.
In recent years, domestic and international research personnel have developed a kind of novel memory in a series of oxide materials, be called resistance-variable storing device (RRAM), its principle is: when curtage acts on the sort memory that is made of electrode and described oxide, the change of several magnitudes can take place in the resistance value of this device, and resulting resistance states is under can keeping after the external electric field removal.Utilize this physical characteristic of this types of material can carry out information stores, for example high-impedance state can be used for stored information " 0 ", and low resistance state can be used for stored information " 1 ", and vice versa.With respect to other nonvolatile memory, RRAM has simple, the erasable speed rapidity of preparation, storage density advantages of higher.It has been found that at present multiple transition group metallic oxide material possesses the potentiality of preparation RRAM, as metal-doped manganate, metal-doped titanate, NiO, TiO
2, CuO
x, FeO
x, ZrO
2, CoO, ZnO, MoO
x, MnO
xDeng.Yet, be used for flexible device in order to make these materials, need to be lower than the melting temperature (about 200 ℃) of flexible substrate in the preparation, but when these materials prepare at low temperatures, lost the electric resistance changing effect because of the products therefrom defect density is high.In addition, the fragility of these materials is too high, also can't be competent at flexible demand.
Summary of the invention
Therefore, the objective of the invention is to overcome the defective of above-mentioned prior art, a kind of resistance-variable storing device that steady resistance changes performance and has good flexibility that has when low temperature prepares is provided.
The objective of the invention is to be achieved through the following technical solutions:
According to an aspect of the present invention, provide a kind of flexible resistance-change memory unit, comprising:
The flexible insulation substrate,
Hearth electrode on this flexible insulation substrate,
Storage medium layer on this hearth electrode, and
Top electrode on this storage medium layer,
Wherein, described storage medium layer is Zn
(1-x)Mg
xThe O film, wherein the scope of x is 0＜x＜1.
In said memory cells, described Zn
(1-x)Mg
xThe thickness of O film is 10-1000nm.
In said memory cells, described hearth electrode and top electrode are made by metal material or conductive compound.
In said memory cells, described hearth electrode has the composite construction of conductive compound/metal/conductive compound.
In said memory cells, described Zn
(1-x)Mg
xThe O film is preferably Zn
0.8Mg
0.2The O film.
According to another aspect of the present invention, provide a kind of flexible resistance-variable storing device, wherein, comprise flexible resistance-change memory unit according to first aspect present invention.
According to a further aspect of the invention, provide a kind of method of making flexible resistance-change memory unit, comprising:
1) provides the flexible insulation substrate;
2) on this flexible insulation substrate, prepare hearth electrode;
3) on this hearth electrode, prepare Zn
(1-x)Mg
xThe O film, wherein the scope of x is 0＜x＜1, the thickness of film is 10-1000nm;
4) at this Zn
(1-x)Mg
xPrepare top electrode on the O film.
In said method, comprise that in described step 3) the employing pulse laser sediment method prepares Zn
(1-x)Mg
xThe O film, underlayer temperature is between room temperature to 150 ℃.
In said method, described pulse laser sediment method comprises and utilizes Zn
(1-x)Mg
xO target deposition Zn
(1-x)Mg
xThe O film.
In said method, described Zn
(1-x)Mg
xThe O film is preferably Zn
0.8Mg
0.2The O film.
Compared with prior art, the invention has the advantages that:
1. flexible resistance-variable storing device of the present invention can have good processing compatibility in preparation below 150 ℃;
2. flexible resistance-variable storing device of the present invention is at the transformation and the memory characteristic that show under the direct voltage trigger condition of opposed polarity between the good high resistance and low resistance attitude, and its high resistance is than at least 10 times of low-resistance value height;
The operating voltage of flexible resistance-variable storing device of the present invention (make between high-impedance state and the low resistance state to take place change voltage) less than+/-3V, after the memory outage, its resistance states can continue to keep, at least 10
4More than second;
4. flexible resistance-variable storing device of the present invention still keeps good resistance switching performance after through wide-angle bending more than 100 times.
Description of drawings
It is following that embodiments of the present invention is further illustrated with reference to accompanying drawing, wherein:
Fig. 1 be one embodiment of the present of invention based on Zn
(1-x)Mg
xThe structural representation of the flexible resistance-change memory unit of O film;
Fig. 2 is the Zn of one embodiment of the present of invention
0.8Mg
0.2The X-ray diffractogram of O film (XRD);
Fig. 3 is Zn according to an embodiment of the invention
0.8Mg
0.2The scanning electron microscopy of O film surface (SEM) shape appearance figure;
Fig. 4 is the I-V curve of the flexible resistance-change memory unit of one embodiment of the present of invention;
Fig. 5 is the flexible resistance-variable storing device unit schematic diagram of the resistance change under the pulse voltage effect at ambient temperature of one embodiment of the present of invention;
Fig. 6 is the high and low resistance state in the flexible resistance-variable storing device unit of an one embodiment of the present of invention time history plot at room temperature;
Fig. 7 is the height of flexible resistance-variable storing device unit of one embodiment of the present of invention and the low resistance state resistance value variation diagram along with number of bends.
Embodiment
Followingly the present invention is described with reference to specific embodiment.Those skilled in the art will appreciate that these embodiment only are used to purpose of the present invention is described, rather than limit the scope of the invention.
Fig. 1 be one embodiment of the present of invention based on Zn
(1-x)Mg
xThe structural representation of the flexible resistance-change memory unit of O film.This memory cell from top to down comprises top electrode 1, Zn
(1-x)Mg
xO film 2, hearth electrode 3 and substrate 4, wherein the scope of x is 0＜x＜1.In the present embodiment, Zn
(1-x)Mg
xThe thickness of O film can be between 10-1000nm.Top electrode 1 and hearth electrode 3 are made by metal Cu, yet for it will be understood by those skilled in the art that in other embodiments of the invention, top electrode and hearth electrode also can be selected other metal materials except that Cu, for example Ag, Au, Ti for use; Or employing conductive compound, for example ITO, fluorine-doped tin oxide (FTO), zinc oxide aluminum (AZO), stannate (M
2SnO
4, M=Zn, Cd), SnO
2, In
2O
3, Ga doping In
2O
3, cuprous oxide (CuMO
2, M=Al, Ga, Sr), Nb doped Ti O
2,TiN etc.Preferably, hearth electrode 3 adopts the three-layer composite structure of conductive compound/metal/conductive compounds, ITO/Ag/ITO composite construction for example, and purpose is the flexibility that strengthens hearth electrode.Substrate 4 can adopt flexible insulating material, for example polyethersulfone resin (PES), Polyethyleneglycol Terephthalate (PET) or polybutylene terephthalate (PBT) etc.
According to the present invention, a kind of method for preparing above-mentioned flexible resistance-change memory unit also is provided, this method may further comprise the steps:
1) provides the flexible insulation substrate.In one embodiment, choose flexible material such as ethylene diester (PET), polyethersulfone resin (PES) or polybutylene terephthalate (PBT) as the flexible insulation substrate.
2) on this flexible insulation substrate, form hearth electrode.In one embodiment, for example can adopt magnetically controlled sputter method deposition hearth electrode film, its thickness can be 50-1000nm, is preferably 300nm, and the hearth electrode square resistance is preferably less than 20 ohm.In yet another embodiment, hearth electrode preferably uses FTO, ITO, AZO, stannate (M
2SnO
4, M=Zn, Cd), SnO
2, In
2O
3, Ga doping In
2O
3, cuprous oxide (CuMO
2, M=Al, Ga, Sr), Nb doped Ti O
2As hearth electrode, also can use metallic film material, for example Ag, Cu, Al etc. Deng polycrystalline or amorphous conductive oxide film.In another embodiment, described hearth electrode adopts the composite construction of ITO/Ag/ITO.
3) in step 2) hearth electrode on form Zn
(1-x)Mg
xThe O film, wherein the scope of x is 0＜x＜1.In one embodiment, can adopt the pulsed laser deposition method to form Zn
0.8Mg
0.2The O film, for example concrete preparation process is as described below: at first in the chamber of laser pulse thin film deposition system with Zn
0.8Mg
0.2The O target is fixed on the target platform, and the flexible substrate that will prepare hearth electrode is fixed on the substrate table; Then this chamber is evacuated down to below the 0.001Pa, in this chamber, charges into oxygen, make oxygen pneumatic remain on about 10Pa; To the substrate heating, make its temperature remain on about 80 ℃ then; Start the KrF excimer laser at last, its operating frequency can be 3HZ, focuses the laser beam into Zn
0.8Mg
0.2On the O target, begin to deposit Zn
0.8Mg
0.2The O film, this Zn
0.8Mg
0.2The O film thickness is about 20-1000nm, is preferably about 300nm.In another embodiment, underlayer temperature is between room temperature to 150 ℃.In addition, for it will be understood by those skilled in the art that about Zn
0.8Mg
0.2The acquisition of O target can form Zn by ZnO and the MgO powder that sintering mixes according to a certain percentage
0.8Mg
0.2The O target, for example ZnO that certain proportion is mixed and MgO powder grind, with ground mixture under air ambient 1000 ℃ of sintering 3 hours; Then the powder behind the sintering is ground once more, and under the static pressure of 30MPa it is pressed into disk, its diameter for example can be 30mm, and thickness for example can be 4mm; And then in electric furnace under air atmosphere at 1000 ℃ of these Zn of sintering
0.8Mg
0.2O disk 10 hours is made Zn thus
0.8Mg
0.2The O target.
4) at the Zn of step 3)
(1-x)Mg
xForm top electrode on the O film.In one embodiment, for example can adopt pulsed laser deposition to deposit and form the top electrode film, its thickness can be 50-1000nm for example, is preferably 500nm.In another embodiment, described top electrode preferably uses ITO, FTO, AZO, stannate (M
2SnO
4, M=Zn, Cd), SnO
2, In
2O
3, Ga doping In
2O
3, cuprous oxide (CuMO
2, M=Al, Ga, Sr), Nb doped Ti O
2Deng polycrystalline or amorphous conductive oxide film as top electrode; Certainly, also can use the flexible metal film material.
Fig. 2 is Zn according to an embodiment of the invention
(1-x)Mg
xThe XRD diffraction pattern of O transparent membrane wherein adopts x=0.2, i.e. Zn
0.8Mg
0.2The O transparent membrane.Observe this diffraction pattern and can know Zn
0.8Mg
0.2The O film is the polycrystal film of weak crystallization.
Fig. 3 is Zn according to an embodiment of the invention
0.8Mg
0.2The scanning electron microscopy of O film surface (SEM) shape appearance figure, as seen from the figure, film is a polycrystalline structure, crystallite dimension is between 50-100nm.
For the ease of testing every performance of above-mentioned resistance-change memory unit, adopting photoetching technique is a series of rectangular shape with top electrode film etching, and the size of each rectangular block for example can be 100 μ m * 100 μ m.Fig. 4-7 shows based on Zn
0.8Mg
0.2The performance of the flexible resistance-change memory unit of O film.
Fig. 4 is according to an embodiment of the invention based on Zn
0.8Mg
0.2The I-V curve of the flexible resistance-change memory unit of O film, wherein X-axis is that voltage, Y-axis are electric current.Top electrode is applied positive voltage is example, shows the I-V curve in the bias voltage scope of+2V at-2V.As shown in the figure, when 0V began to apply voltage, memory cell showed the high resistant characteristic.When voltage reached the 0.5V left and right sides, electric current increase rapidly reached capacity, and memory cell is converted to low resistance state.When voltage be applied to-during 0.5V, electric current reduces gradually.The resistance that shows memory cell raises, and transforms back into high resistance state.Except the mode of I-V scanning, can come erasable this memory with the mode of pulse voltage.The electric resistance changing voltage of this memory cell is very little, is fit to very much the application to the low-power consumption memory device.
Fig. 5 is according to an embodiment of the invention based on Zn
0.8Mg
0.2The flexible resistance-change memory unit variation of the resistance value under the pulse voltage effect at ambient temperature of O film, wherein X-axis is a pulse number, Y-axis is a resistance value.As shown in the figure, at ambient temperature, alternately applying+3V and-3V, when length is the pulse voltage of 1ms, the resistance value of memory cell about 1k Ω (low resistance state, LRS) and approximately 10k Ω (high resistance state, HRS) between alternate.Still good, illustrate that resistance-variable storing device of the present invention has good fatigue resistance through resistance switching performance after 1000 pulses.
Fig. 6 is for when reading of 0.1V read according to the present invention above-mentioned flexible resistance-change memory unit under the voltage, and its resistance states is time history plot at room temperature respectively, and wherein X-axis is the time, and Y-axis is a resistance value.As can be seen from the figure, at ambient temperature, the height of memory cell and low resistance state still keep at least 10 times ratio in for example 10000s long-time.This has illustrated that resistance-variable storing device of the present invention has the function of non-volatile memory.
Fig. 7 is that flexible resistance-change memory of the present invention unit is under high resistance state and low resistance state, through 100 bendings (changes in resistance during minimum profile curvature radius＜4mm).X-axis is a number of bends, and Y-axis is a resistance.As seen from the figure, no matter be high resistance state and low resistance state, its resistance changes along with number of bends hardly.
Above behavioral illustrations flexible resistance-variable storing device of the present invention adapt to potential application fully in field of storage and flexible circuit field.Therefore, according to the present invention, also provide a kind of resistance-variable storing device based on above-mentioned resistance-change memory unit, this resistance-variable storing device comprises the memory cell array based on above-mentioned resistance-change memory unit.According to of the present invention based on Zn
(1-x)Mg
xThe resistance-variable storing device of O film has good readwrite performance and fatigue resistance, has good data retentivity under the state of bending.
For it should be understood by one skilled in the art that, the concrete data value of mentioning among the above embodiment all is schematic, those skilled in the art requires also can adopt other data value according to specific design, therefore above-mentioned data value should be interpreted as limitation of the present invention.The present invention does not describe the concrete process conditions and the process of making top electrode and hearth electrode in detail, this is because can adopt technology well known in the art to make top electrode and hearth electrode, for example sputter, pulsed laser deposition, chemical vapour deposition (CVD), sol-gel process or electron-beam vapor deposition method.Adopt laser deposition to prepare Zn
(1-x)Mg
xThe O film also only is schematically, can also utilize sputter, chemical vapour deposition (CVD), sol-gel process or thermal oxidation method etc.
Although the present invention is made specific descriptions with reference to the above embodiments, but for the person of ordinary skill of the art, should be appreciated that and to make amendment based on content disclosed by the invention within spirit of the present invention and the scope or improve not breaking away from, these modifications and improving all within spirit of the present invention and scope.
Claims (10)
1. flexible resistance-change memory unit comprises:
The flexible insulation substrate,
Hearth electrode on this flexible insulation substrate,
Storage medium layer on this hearth electrode, and
Top electrode on this storage medium layer,
It is characterized in that described storage medium layer is Zn
(1-x)Mg
xThe O film, wherein the scope of x is 0＜x＜1.
2. memory cell according to claim 1 is characterized in that, described Zn
(1-x)Mg
xThe thickness of O film is 10-1000nm.
3. memory cell according to claim 1 is characterized in that described hearth electrode and top electrode are made by metal material or conductive compound.
4. memory cell according to claim 1 is characterized in that described hearth electrode has the composite construction of conductive compound/metal/conductive compound.
5. memory cell according to claim 1 is characterized in that, described Zn
(1-x)Mg
xThe O film is Zn
0.8Mg
0.2The O film.
6. a flexible resistance-variable storing device is characterized in that, comprises the flexible resistance-change memory unit of one of claim 1 to 5.
7. the manufacture method of a flexible resistance-change memory unit comprises:
1) provides the flexible insulation substrate;
2) on this flexible insulation substrate, prepare hearth electrode;
3) on this hearth electrode, prepare Zn
(1-x)Mg
xThe O film, wherein the scope of x is 0＜x＜1, the thickness of film is 10-1000nm;
4) at this Zn
(1-x)Mg
xPrepare top electrode on the O film.
8. method according to claim 7 is characterized in that, comprises in described step 3) and adopts pulse laser sediment method to prepare Zn
(1-x)Mg
xThe O film, underlayer temperature is between room temperature to 150 ℃.
9. method according to claim 8 is characterized in that, described pulse laser sediment method comprises and utilizes Zn
(1-x)Mg
xO target deposition Zn
(1-x)Mg
xThe O film.
10. method according to claim 7 is characterized in that, described Zn
(1-x)Mg
xThe O film is Zn
0.8Mg
0.2The O film.
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|---|---|---|---|---|
| CN102280578A (en) * | 2011-08-22 | 2011-12-14 | 东北师范大学 | Flexible resistive nonvolatile memory based on amorphous multi-element metal oxide |
| CN102881822A (en) * | 2011-07-13 | 2013-01-16 | 北京大学 | Transparent flexible resistance random access memory and manufacturing method therefor |
| CN109980082A (en) * | 2019-03-06 | 2019-07-05 | 电子科技大学 | A kind of resistance-variable storing device and preparation method thereof based on ZnMgO |
| CN110197874A (en) * | 2019-05-29 | 2019-09-03 | 中国科学院宁波材料技术与工程研究所 | Stretchable elastic resistive random access memory of one kind and preparation method thereof |
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| CN101533890A (en) * | 2009-04-03 | 2009-09-16 | 中国科学院上海硅酸盐研究所 | Transparent RRAM component with zinc oxide based homogeneous structure and manufacture method thereof |
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| CN101257089A (en) * | 2007-01-04 | 2008-09-03 | 三星电子株式会社 | Resistive random access memory and manufacturing method for the same |
| CN101452994A (en) * | 2008-10-14 | 2009-06-10 | 中山大学 | Non-volatile memory element and preparation method thereof |
| CN101533890A (en) * | 2009-04-03 | 2009-09-16 | 中国科学院上海硅酸盐研究所 | Transparent RRAM component with zinc oxide based homogeneous structure and manufacture method thereof |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102881822A (en) * | 2011-07-13 | 2013-01-16 | 北京大学 | Transparent flexible resistance random access memory and manufacturing method therefor |
| WO2013007113A1 (en) * | 2011-07-13 | 2013-01-17 | 北京大学 | Transparent and flexible organic resistive random access memory and method for manufacturing same |
| US20140145139A1 (en) * | 2011-07-13 | 2014-05-29 | Ru Huang | Transparent flexible resistive memory and fabrication method thereof |
| CN102280578A (en) * | 2011-08-22 | 2011-12-14 | 东北师范大学 | Flexible resistive nonvolatile memory based on amorphous multi-element metal oxide |
| CN109980082A (en) * | 2019-03-06 | 2019-07-05 | 电子科技大学 | A kind of resistance-variable storing device and preparation method thereof based on ZnMgO |
| CN110197874A (en) * | 2019-05-29 | 2019-09-03 | 中国科学院宁波材料技术与工程研究所 | Stretchable elastic resistive random access memory of one kind and preparation method thereof |
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Application publication date: 20110126 |