CN102194995A - Zinc-oxide-based polarity-controlled resistive random-access memory (RRAM) and manufacturing method thereof - Google Patents
Zinc-oxide-based polarity-controlled resistive random-access memory (RRAM) and manufacturing method thereof Download PDFInfo
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Abstract
The invention discloses a zinc-oxide-based polarity-controlled resistive random-access memory (RRAM) based on which is composed of a SiO2/Si substrate, an adhesive layer, a lower electrode, a zinc oxide thin film with a resistance conversion characteristic, an upper electrode and a protective layer, wherein, the thickness of the adhesive layer is 5-20nm, the thickness of the lower electrode is 5-100nm, the thickness of the zinc oxide thin film with characteristics of conversion is 5-200nm, the thickness of the upper electrode is 5-100nm, and the thickness of the protective layer is 5-100nm. The polarity-controlled RRAM provided by the invention has the advantages that the influence of the characteristics of resistance conversion based on a zinc oxide thin film resistance changing device is shown into unipolarity, bipolarity and nonpolarity through depositing different upper electrode materials; according to the characteristics of different polarity resistance changing properties, the application prospects of the RRAM can be expanded, the importance of academics and practical application of the RRAM is highlighted; and a polarity-controlled resistance changing device can be prepared through preparing different upper electrodes of the resistance changing device, thus the RRAM has great significance in the aspects of mass production and actual promotion of the RRAM production process.
Description
Technical field
The invention belongs to technical field of semiconductors, particularly a kind of preparation method of the controlled resistance-variable storing device of polarity based on zinc oxide.
Background technology
Modern society's main flow memory all adopts flash memory (flash) memory based on floating gate structure, because constantly dwindling of integrated level and device size, the influence that floating gate structure itself is crosstalked, almost reached dimension limit, when the tunnel oxide layer thickness more and more hour, the leakage of electric charge become more and more serious (gate medium electric leakage); And in view of the contradiction between erasable speed and the reliability with and higher operating voltage, complicated restrictions such as circuit structure, particularly after the technology node enters below the 32nm, can't further improve integration density in the flash memory, make non-volatility memorizer of new generation more and more attract people's eyeball, also more and more urgent for the demand of jumbo nonvolatile memory.Resistance-variable storing device (Resistive Random Access Memory, RRAM), ferroelectric memory (FeRAM), phase transition storage (PcRAM), magnetic memory (MRAM) etc. arise at the historic moment, all has very big application potential, and all in constantly exploring, and RRAM with its low-power consumption, non-volatile, preparation is simple, size is little and it is integrated to be easy to, storage density is high, operating voltage is low, good with the traditional cmos process compatibility, favored by most of people.
Resistance-variable storing device is a kind ofly to send a telegraph the device of resistance transition effect based on electricity, is a kind of novel non-volatility memorizer, is described as the strongest competitor of non-volatility memorizer of future generation with himself powerful advantage.The resistive material of resistance-variable storing device mainly contains perovskite, organic substance, binary metal oxide etc. as its resistive conversion layer, because Dyadic transition metal oxide (Transition Metal Oxide, TMO) the more excellent electrology characteristic of thin-film material self, preparation is simple, processes expend is lower, characteristics compatible good with the traditional handicraft line, becomes everybody research focus.And zinc oxide is the high material of a kind of chemical stability, the broad stopband direct gap semiconductor, and stability is very high under the atmospheric pressure, and the inner oxygen room and the electric resistance changing characteristic of zinc gap affects zinc-oxide film oxide.Resistance-variable storing device based on zinc oxide has lower Reset electric current and set voltage, draws materials conveniently, has very big prospect in practical application.
The basic structure of RRAM device, the sandwich structure that tradition adopts top electrode-resistive conversion layer-bottom electrode to constitute.Present stage, though RRAM still has a lot of problems to need solution badly, for example material system is numerous, and which kind of material system memory property is the most superior still indeterminate; Further reduce power problems and be still emphasis as non-volatility memorizer of future generation; The concrete physical mechanism of resistive mechanism is still not exclusively clear and definite, has the electric charge capture of conductive filament model, space charge limited current model, defect level and release, Schottky model, pul-flange to restrain model etc.And the earth terminal of bottom electrode during generally as applied voltage.In sum, the research emphasis of resistance-variable storing device, key are the influence of top electrode to change resistance performance.By depositing of the influence of different top electrodes to the electric resistance changing characteristic, form resistive device with opposed polarity, very big application prospect is arranged in actual process.
Present studies show that, it is inner or in that top electrode-the resistive conversion layer at the interface that the electric resistance changing characteristic mainly occurs in the resistive conversion layer.Occur in the interface of top electrode-resistive conversion layer for the electric resistance changing characteristic, the resistive conversion layer adopts zinc-oxide film, so top electrode has direct influence for the resistive transfer characteristic.The people such as Wan-Gee Kim of Korea S in 2009 have studied based in top electrode/titanium dioxide/platinum electrode structure, for the top electrode with different work contents, such as Pt, Au, Ag, Ni, Al etc., for the influence of electric resistance changing characteristic.Different metal electrode and TiO
2The difference of work content between the film, the inherent barrier height that is caused is for the effect of resistive characteristic important influence, with Pt and Au during as top electrode, when adding current limliting (Compliance Current, CC) time, stable unipolarity and bipolarity can occur and change; When being top electrode, when not adding current limliting, can only find that bipolarity changes this moment with Ag; Ni and Al electrode have similar work content to Ag, under very low current limliting, can find that unsettled bipolarity and unipolarity change, and are because at the chemical reaction that takes place at the interface; For the Ti electrode, do not find the resistive process, because the work content of Ti compares TiO
2Little with TiO work content mutually.In March, 2011 Taiwan Chun-Chieh Lin, people such as Yi-Peng Chang have studied a kind of based on new material CaCu
3Ti
4O
12(CCTO) resistive characteristic, mainly characterized top electrode in the CCTO material system for the resistive characteristic influence.The work content that has shown top electrode has very important significance for the resistive characteristic.Observing of success when powering on very Ni, the resistive conversion of the opposed polarity when Pd and Pt.
For this reason, at in the resistive device, by depositing different top electrodes to influence based on zinc oxide resistive device performance, prepare the controlled resistance-variable storing device of polarity, and the characteristics by performance opposed polarity resistive device will have important and practical meanings and potential huge commercial value in semiconductor technology is used.
Summary of the invention
The objective of the invention is at above-mentioned technical Analysis, a kind of preparation method based on the controlled resistance-variable storing device of the polarity of zinc oxide is provided, this method is by the different top electrode of deposition, realize preparation, bring into play the application prospect of opposed polarity resistive device in actual applications based on the resistance-variable storing device of zinc oxide resistive material opposed polarity.
Technical scheme of the present invention:
The controlled resistance-variable storing device of a kind of polarity based on zinc oxide is by SiO
2/ Si substrate, adhesion layer, bottom electrode, the zinc-oxide film with electric resistance changing characteristic, top electrode and protective layer constitute, and adhesion layer thickness is that 5-20nm, bottom electrode thickness are 5-100nm, thickness with zinc-oxide film of electric resistance changing characteristic is 5-200nm, top electrode thickness is that the thickness of 5-100nm, protective layer is 5-100nm.
Described adhesion layer is Titanium or tin indium oxide.
Described bottom electrode is metal Cu, Pt or Al.
Described upper electrode material is pure conducting metal, combination metal material or conductive metallic compound, and metal material is Ta, Cu, Au, Ag, W, Ni or Pt; Metal alloy compositions is Pt/Ti, Ta/Ti, Cu/Ti, Cu/Au, Cu/Al or Au/Zr; Conductive metallic compound is TiN or ITO.
Described zinc-oxide film with electric resistance changing characteristic is the binary metal oxide zinc-oxide film.
Described protective layer is copper Au or conductive metallic compound ITO.
A kind of preparation method of the described controlled resistance-variable storing device of polarity based on zinc oxide, step is as follows:
1) at first at SiO
2Deposition of adhesion on the/Si substrate base;
2) on the adhesion layer for preparing, deposit bottom electrode, as the exit or the ground connection of device applied voltage negative electrode;
3) zinc-oxide film that deposition has the electric resistance changing characteristic on the bottom electrode for preparing;
4) on zinc-oxide film, prepare top electrode with electric resistance changing characteristic;
5) layer protective layer of on top electrode, growing.；
The deposition process of described adhesion layer is magnetic control method, ion beam method, chemical vapour deposition technique, physical vaporous deposition, evaporation deposition method or atomic layer deposition method.
Described bottom electrode, the deposition process of top electrode and protective layer are magnetic control or ion beam sputtering, chemical vapour deposition technique, physical vaporous deposition, evaporation deposition method or atomic layer deposition method, and preparation technology is: base vacuum degree＜10
-4Pa, underlayer temperature are that room temperature, operating air pressure are that 0.5-2Pa, sputtering time are 1-10min, and 5-50sccm under the Ar atmosphere, sputtering power are 50-250W.
Described deposition process with zinc-oxide film of resistive characteristic is magnetic control or ion beam sputtering, chemical vapour deposition technique, physical vaporous deposition, evaporation deposition method, atomic layer deposition method or sol-gal process, and preparation technology is:: base vacuum degree＜10
-4Pa, underlayer temperature are that room temperature-300 ℃, operating air pressure are that 0.5-2Pa, sputtering time are 1-60min, at O
2With partial pressure of oxygen in the Ar mist be that 5%-30%, sputtering power are 50-250W.Electrode and protective layer be prepared as base vacuum degree＜10
-4Pa, underlayer temperature are that room temperature, operating air pressure are that 0.5-2Pa, sputtering time are 1-10min, and 5-50sccm under the Ar atmosphere, sputtering power are 50-250W.
Technical Analysis of the present invention:
By depositing different top electrodes, characterize it to the influence based on the electric resistance changing characteristic of zinc oxide resistance-variable storing device, unipolarity, bipolarity, nonpolarity.Different electrodes have different work functions, and work function is exactly the E0(electron energy) and the Ef(Fermi level) energy poor, be exactly that electronics escapes into the energy that needs outside the medium in medium inside.Briefly be exactly that the metal-semiconductor work function difference has caused them in the electrical potential difference that contacts rear interface, when applied voltage, this electrical potential difference can influence the electric resistance changing characteristic of device.And because the work content difference between different top electrodes and the resistive conversion layer, meeting directly influence the resistive characteristic of device, unipolarity, bipolarity, nonpolarity occur.Characteristics are: because unipolarity is meant that in the electric resistance changing process, needed applied voltage polarity is identical, and it is very fast to write (Set) speed, lower Set voltage, because it is polarity of voltage is identical, just enough by the applied voltage that applies single direction in actual applications.Bipolarity is under different applied voltage polarity, and reversible electric resistance changing could take place, and electric resistance changing speed is fast, has smaller operating voltage, and very low Reset electric current and homogeneity preferably because applied voltage polarity is opposite, have anti-interference.Nonpolarity electric resistance changing process and the applied voltage polarity of being meant has nothing to do, but is applicable to when resistive device generation resistance inverse conversion, does not need clear and definite voltage direction.And, in semicon industry, when the prepared resistance-variable storing device,, should avoid forming the device that the resistive conversion can not take place in order to keep the yield of device finished product.Because the application prospect difference of opposed polarity resistive device, and self-characteristic has notable difference, demand to the resistive device property also is different in actual applications, therefore for resistance-variable storing device, the resistive characteristic that characterizes opposed polarity is very important, and has potential practical significance.
The operating characteristic of this resistance-variable storing device is: 1) when adding Forming voltage, under the applied voltage situation, with hole conduction mechanism or interfacial state reaction, form conductive filament, thereby make device become low resistance state from high-impedance state in the zinc oxide change resistance layer.2) when the Reset process, add Vreset voltage, the Joule heat that formed Reset electric current the is produced conductive filament that will fuse is finished the electric resistance changing of low resistance state to high-impedance state.Set and Reset process are reversible processes.
Superiority of the present invention is: by depositing different upper electrode materials, be unipolarity, bipolarity and nonpolarity to the influence based on zinc-oxide film resistive device resistance conversion characteristic.According to the characteristics of opposed polarity resistive characteristic, can expand the application prospect of RRAM.Because opposed polarity resistive device will highlight its importance academic and practical application.By the preparation of the different top electrodes of resistive device, prepare the controlled resistive device of polarity, be significant aspect the volume production of RRAM production technology and the actual popularization.
Description of drawings
Fig. 1 is the structural representation based on the controlled resistance-variable storing device of the polarity of zinc oxide.
Fig. 2 is the I-V resolution chart based on Pt top electrode zinc-oxide film resistance-variable storing device.
Fig. 3 is the I-V resolution chart based on Au top electrode zinc-oxide film resistance-variable storing device.
Fig. 4 is the I-V resolution chart based on Ag top electrode zinc-oxide film resistance-variable storing device.
Embodiment
Further illustrate substantive distinguishing features of the present invention and marked improvement by following examples.But the present invention only is confined to following examples by no means.
Embodiment 1:
The controlled resistance-variable storing device of a kind of polarity based on zinc oxide is by SiO
2/ Si substrate, adhesion layer, bottom electrode, the zinc-oxide film with electric resistance changing characteristic, top electrode and protective layer constitute, and as shown in Figure 1, concrete preparation technology is as follows:
1) by ion beam sputtering at SiO
2Preparation adhesion layer Ti film on the/Si substrate, the thickness of described Ti film is 5nm;
2) on described adhesion layer, prepare bottom electrode Cu, base vacuum degree: 1 * 10 by direct current magnetron sputtering process
-4Pa, underlayer temperature: room temperature, operating air pressure: 1.5Pa, Ar=30sccm, sputtering power: 85W; Film thickness 20nm;
3) on described bottom electrode, prepare the zinc-oxide film with resistive characteristic, base vacuum degree: 1 * 10 by rf magnetron sputtering
-4Pa, underlayer temperature: 250 ℃, operating air pressure: 1.0Pa, O in the sputter
2=8sccm, Ar=32sccm, sputtering power: 100W; Film thickness 100nm;
4) adopt direct current magnetron sputtering process on zinc-oxide film, to prepare top electrode Pt, film thickness 20nm;
5) adopt direct current magnetron sputtering process on described top electrode, to deposit protective layer.
Test its I-V characteristic by analyzing parameters of semiconductor instrument B1500, Fig. 2 is the I-V resolution chart based on Pt top electrode zinc-oxide film resistance-variable storing device.The result shows: Set under the applying bias, Reset on the identical voltage direction, unipolarity resistance reversible transition.
Embodiment 2:
The controlled resistance-variable storing device of a kind of polarity based on zinc oxide is by SiO
2/ Si substrate, adhesion layer, bottom electrode, the zinc-oxide film with electric resistance changing characteristic, top electrode and protective layer constitute, and concrete preparation technology is as follows:
1) prepare adhesion layer Ti film by ion beam sputtering on the SiO2/Si substrate, the thickness of described Ti film is 5nm;
2) on described Ti film, prepare bottom electrode Cu, base vacuum degree: 1 * 10 by direct current magnetron sputtering process
-4Pa, underlayer temperature: room temperature, operating air pressure: 1.5Pa, Ar=30sccm, sputtering power: 85W; Film thickness 20nm;
3) on described bottom electrode, prepare the zinc-oxide film with resistive characteristic, base vacuum degree: 1 * 10 by rf magnetron sputtering
-4Pa, underlayer temperature: 250 ℃, operating air pressure: 1.0Pa, O in the sputter
2=8sccm, Ar=32sccm, sputtering power: 100W; Film thickness 100nm;
4) adopt direct current magnetron sputtering process on described zinc-oxide film, to prepare top electrode Au, film thickness 20nm;
5) adopt direct current magnetron sputtering process on top electrode, to deposit protective layer.
Test its I-V characteristic by analyzing parameters of semiconductor instrument B1500, Fig. 3 is the I-V resolution chart based on Au top electrode zinc-oxide film resistance-variable storing device.The result shows: Set under the positive bias, Reset under the back bias voltage, the bipolarity resistance reversible transition of standard.
Embodiment 3:
The controlled resistance-variable storing device of a kind of polarity based on zinc oxide is by SiO
2/ Si substrate, adhesion layer, bottom electrode, the zinc-oxide film with electric resistance changing characteristic, top electrode and protective layer constitute, and concrete preparation technology is as follows:
1) prepare adhesion layer Ti film by ion beam sputtering on the SiO2/Si substrate, the thickness of described Ti film is 5nm;
2) on described adhesion layer, prepare bottom electrode Cu, base vacuum degree: 1 * 10 by direct current magnetron sputtering process
-4Pa, underlayer temperature: room temperature, operating air pressure: 1.5Pa, Ar=30sccm, sputtering power: 85W; Film thickness 20nm;
3) adopt radio frequency sputtering method to prepare zinc-oxide film on described bottom electrode, partial pressure of oxygen is 25% in the sputter, sputtering power is 250W, film thickness 100nm;
4) adopt direct current magnetron sputtering process on described zinc-oxide film, to prepare top electrode Ag, film thickness 20nm;
5) adopt direct current magnetron sputtering process on described top electrode, to deposit protective layer.
Test its I-V characteristic by analyzing parameters of semiconductor instrument B1500, Fig. 4 is the I-V resolution chart based on Ag top electrode zinc-oxide film resistance-variable storing device.The result shows: Set under the positive bias, Reset under the back bias voltage, bipolarity resistance reversible transition.
Claims (9)
1. the controlled resistance-variable storing device of the polarity based on zinc oxide is characterized in that: by SiO
2/ Si substrate, adhesion layer, bottom electrode, the zinc-oxide film with electric resistance changing characteristic, top electrode and protective layer constitute, and adhesion layer thickness is that 5-20nm, bottom electrode thickness are 5-100nm, thickness with zinc-oxide film of electric resistance changing characteristic is 5-200nm, top electrode thickness is that the thickness of 5-100nm, protective layer is 5-100nm.
2. according to the controlled resistance-variable storing device of the described polarity based on zinc oxide of claim 1, it is characterized in that: described adhesion layer is Titanium or tin indium oxide.
3. according to the controlled resistance-variable storing device of the described polarity based on zinc oxide of claim 1, it is characterized in that: described bottom electrode is metal Cu, Pt or Al.
4. according to the controlled resistance-variable storing device of the described polarity based on zinc oxide of claim 1, it is characterized in that: described upper electrode material is pure conducting metal, combination metal material or conductive metallic compound, and metal material is Ta, Cu, Au, Ag, W, Ni or Pt; Metal alloy compositions is Pt/Ti, Ta/Ti, Cu/Ti, Cu/Au, Cu/Al or Au/Zr; Conductive metallic compound is TiN or ITO.
5. according to the controlled resistance-variable storing device of the described polarity based on zinc oxide of claim 1, it is characterized in that: described zinc-oxide film with electric resistance changing characteristic is the binary metal oxide zinc-oxide film, and described protective layer is golden Au or conductive metallic compound ITO.
6. one kind according to claim 1 based on the preparation method of the controlled resistance-variable storing device of polarity of zinc oxide, it is characterized in that step is as follows:
1) at first at SiO
2Deposition of adhesion on the/Si substrate base;
2) on the adhesion layer for preparing, deposit bottom electrode, as the exit or the ground connection of device applied voltage negative electrode;
3) zinc-oxide film that deposition has the electric resistance changing characteristic on the bottom electrode for preparing;
4) on zinc-oxide film, prepare top electrode with electric resistance changing characteristic;
5) layer protective layer of on top electrode, growing.
7. according to the preparation method of the described controlled resistance-variable storing device of polarity based on zinc oxide of claim 6, it is characterized in that: the deposition process of described adhesion layer is magnetic control method, ion beam method, chemical vapour deposition technique, physical vaporous deposition, evaporation deposition method or atomic layer deposition method.
8. according to the preparation method of the described controlled resistance-variable storing device of polarity based on zinc oxide of claim 6; it is characterized in that: described bottom electrode; the deposition process of top electrode and protective layer is magnetic control or ion beam sputtering, chemical vapour deposition technique, physical vaporous deposition, evaporation deposition method or atomic layer deposition method, and preparation technology is: base vacuum degree＜10
-4Pa, underlayer temperature are that room temperature, operating air pressure are that 0.5-2Pa, sputtering time are 1-10min, and 5-50sccm under the Ar atmosphere, sputtering power are 50-250W.
9. according to the preparation method of the described controlled resistance-variable storing device of polarity based on zinc oxide of claim 6, it is characterized in that: described deposition process with zinc-oxide film of resistive characteristic is magnetic control or ion beam sputtering, chemical vapour deposition technique, physical vaporous deposition, evaporation deposition method, atomic layer deposition method or sol-gal process, and preparation technology is:: base vacuum degree＜10
-4Pa, underlayer temperature are that room temperature-300 ℃, operating air pressure are that 0.5-2Pa, sputtering time are 1-60min, at O
2With partial pressure of oxygen in the Ar mist be that 5%-30%, sputtering power are 50-250W; Electrode and protective layer be prepared as base vacuum degree＜10
-4Pa, underlayer temperature are that room temperature, operating air pressure are that 0.5-2Pa, sputtering time are 1-10min, and 5-50sccm under the Ar atmosphere, sputtering power are 50-250W.
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| CN102694121A (en) * | 2012-05-17 | 2012-09-26 | 中国科学院物理研究所 | Method for manufacturing resistance memory device and product and application thereof |
| CN103606625A (en) * | 2013-11-28 | 2014-02-26 | 北京大学 | High-uniformity low-power-dissipation resistive random access memory and preparation method thereof |
| CN105552220A (en) * | 2015-12-15 | 2016-05-04 | 中国人民解放军国防科学技术大学 | Silicon oxide thin film based low power consumption resistive random access memory and preparation method therefor |
| CN105742492A (en) * | 2016-04-13 | 2016-07-06 | 上海大学 | Carbon-based material resistance storage unit having unilateral resistance characteristic and preparation method thereof |
| CN105810817A (en) * | 2016-05-31 | 2016-07-27 | 天津理工大学 | Resistive device of two-dimensional nanosheet-layer MoS2 vertical structure |
| CN105870321A (en) * | 2016-03-28 | 2016-08-17 | 北京大学 | Nonlinear self-rectifying resistive random access memory and preparation method therefor |
| CN108140665A (en) * | 2015-09-30 | 2018-06-08 | Arm有限公司 | More impedances are associated with electronic switch structure |
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| CN111029341A (en) * | 2019-11-14 | 2020-04-17 | 天津大学 | Flexible bottom gate flash memory device with calcium copper titanate gate dielectric layer and manufacturing method thereof |
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| US9525133B2 (en) | 2013-11-28 | 2016-12-20 | Peking University | Resistive random access memory with high uniformity and low power consumption and method for fabricating the same |
| CN103606625A (en) * | 2013-11-28 | 2014-02-26 | 北京大学 | High-uniformity low-power-dissipation resistive random access memory and preparation method thereof |
| WO2015078120A1 (en) * | 2013-11-28 | 2015-06-04 | 北京大学 | High consistency and low power consumption resistive memory and preparation method thereof |
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| CN105870321B (en) * | 2016-03-28 | 2019-03-08 | 北京大学 | A kind of non-linear self-rectifying resistance-variable storing device and preparation method thereof |
| CN105742492A (en) * | 2016-04-13 | 2016-07-06 | 上海大学 | Carbon-based material resistance storage unit having unilateral resistance characteristic and preparation method thereof |
| CN105742492B (en) * | 2016-04-13 | 2018-08-17 | 上海大学 | Carbon-based material variable-resistance memory unit and preparation method thereof with unilateral resistive characteristic |
| CN105810817A (en) * | 2016-05-31 | 2016-07-27 | 天津理工大学 | Resistive device of two-dimensional nanosheet-layer MoS2 vertical structure |
| CN110071215A (en) * | 2018-04-03 | 2019-07-30 | 东北师范大学 | A kind of bipolarity/nonpolarity reversible mutual transition resistance-variable storing device and preparation method thereof |
| CN110071215B (en) * | 2018-04-03 | 2022-08-09 | 东北师范大学 | Bipolar/non-polar reversible mutual transformation type resistive random access memory and preparation method thereof |
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Application publication date: 20110921 |