CN103311433A - Manufacturing method of resistive random access memory - Google Patents
Manufacturing method of resistive random access memory Download PDFInfo
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- CN103311433A CN103311433A CN2012100586767A CN201210058676A CN103311433A CN 103311433 A CN103311433 A CN 103311433A CN 2012100586767 A CN2012100586767 A CN 2012100586767A CN 201210058676 A CN201210058676 A CN 201210058676A CN 103311433 A CN103311433 A CN 103311433A
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- 238000000034 method Methods 0.000 claims abstract description 47
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- 230000008569 process Effects 0.000 claims abstract description 20
- 238000000137 annealing Methods 0.000 claims abstract description 13
- 239000002243 precursor Substances 0.000 claims description 12
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 11
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical group O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 10
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 10
- 230000015572 biosynthetic process Effects 0.000 claims description 9
- 239000008367 deionised water Substances 0.000 claims description 9
- 229910021641 deionized water Inorganic materials 0.000 claims description 9
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 8
- 229910000449 hafnium oxide Inorganic materials 0.000 claims description 8
- WIHZLLGSGQNAGK-UHFFFAOYSA-N hafnium(4+);oxygen(2-) Chemical group [O-2].[O-2].[Hf+4] WIHZLLGSGQNAGK-UHFFFAOYSA-N 0.000 claims description 8
- 238000000231 atomic layer deposition Methods 0.000 claims description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 6
- 239000001301 oxygen Substances 0.000 claims description 6
- 229910052760 oxygen Inorganic materials 0.000 claims description 6
- 239000010936 titanium Substances 0.000 claims description 6
- 239000000126 substance Substances 0.000 claims description 4
- XJDNKRIXUMDJCW-UHFFFAOYSA-J titanium tetrachloride Chemical compound Cl[Ti](Cl)(Cl)Cl XJDNKRIXUMDJCW-UHFFFAOYSA-J 0.000 claims description 4
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- 239000003595 mist Substances 0.000 claims description 3
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- 230000008859 change Effects 0.000 abstract description 5
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- 229910010413 TiO 2 Inorganic materials 0.000 description 1
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Abstract
A method of manufacturing a resistive random access memory, the method comprising: forming a first electrode; forming a resistance change functional layer on the first electrode, wherein the resistance change functional layer comprises at least one layer of first binary metal oxide and at least one layer of second binary metal oxide, and the first binary metal oxide and the second binary metal oxide are alternately laminated; carrying out a thermal annealing process; and forming a second electrode on the resistance change functional layer. The metal ions of different metal oxides have difference, and are diffused at the interface of the two metal oxides through an annealing process to form a composite dielectric intermediate and form a structural defect, so that the electrical characteristics of the resistance change functional layer are optimized, and the uniformity of the conversion parameters is improved.
Description
Technical field
The present invention relates to semiconductor device and manufacturing technology, more particularly, relate to a kind of manufacture method of resistance-variable storing device.
Background technology
Popular along with the Portable personal device, non-volatility memorizer becomes the research and development emphasis in the semi-conductor industry gradually owing to have and still can keep remember condition and operate advantage such as low-power consumption when non-transformer supply.Non-volatility memorizer in the market is main flow with flash memory (flash) still, but operating voltage is excessive because flash memory exists, service speed is slow, endurance is got well inadequately and owing to shortcomings such as the continuous attenuate of tunnel oxide causes that the retention time falls short of in the device dimensions shrink process, present research and development emphasis has turned to the novel non-volatility memorizer that can replace flash memory gradually.
Resistance-variable storing device (RRAM) since have write operation voltage low, write the erasing time short, the retention time long, non-destructive reads, many-valued storage, simple in structure and storage density advantages of higher, therefore becomes the research emphasis in the present novel non-volatility memorizer spare gradually.The storage principle of resistance-variable storing device is to be based upon on the reversible resistive characteristic of resistive material, that is to say, the resistive material under the signal of telecommunication can high-impedance state (High Resistance State, HRS) and low resistance state (Low Resistance State realizes reversible transformation between LRS).
At present, also have certain dispute at the transformation mechanism of electric resistance changing memory, but the demonstration widely of some mechanism processes has been arranged, solid-state electrolytic solution electric resistance changing memory is exactly wherein a kind of.The basic structure of solid-state electrolytic solution resistance change memory device, as shown in Figure 1, mainly comprise: bottom electrode 11, memory function layer 12 and top electrode 13, it is the metal of inertia that bottom electrode adopts under the electric field action, top electrode adopts the metal of easy oxidation under the electric field action, the material that the memory function layer adopts phase-change material, binary metal oxide material or organic material etc. to have the resistive characteristic.
For the resistance-variable storing device that adopts the binary metal oxide material as the resistive functional layer, industry is interpreted as the mechanism of its electric resistance changing: under the signal of telecommunication, form local conductive filament in the binary metal oxide, conductive filament may be made up of the oxygen room that oxide self decomposes out, also may be formed by the metal ion that electrode is introduced, and the growth course of conductive filament all is at random, and is wayward, therefore causes the discreteness of resistance-variable storing device device transition parameters bigger.
Therefore, improve the discreteness of resistance-variable storing device device transition parameters, improve the uniformity of transition parameters, become the focus of present resistance-variable storing device device research.
Summary of the invention
The embodiment of the invention provides a kind of manufacture method of resistance-variable storing device, optimizes the resistive functional layer, improves the uniformity of transition parameters.
For achieving the above object, the embodiment of the invention provides following technical scheme:
A kind of manufacture method of resistance-variable storing device, described method comprises:
Form first electrode;
Form the resistive functional layer at described first electrode, wherein, described resistive functional layer comprises one deck first binary metal oxide and one deck second binary metal oxide at least at least, and described first binary metal oxide and second binary metal oxide are alternately laminated;
Carry out thermal anneal process;
Form second electrode in described resistive functional layer.
Alternatively, adopt technique for atomic layer deposition to form the resistive functional layer at described first electrode.
Alternatively, described first binary metal oxide is hafnium oxide, and described second binary metal oxide is titanium oxide.
Alternatively, the precursor that adopts in the ald is that unsaturated reaction formation hafnium oxide takes place for TEMAHf and deionized water; The precursor that adopts in the ald is that unsaturated reaction formation titanium oxide takes place for titanium tetrachloride and deionized water.
Alternatively, the chemical dosage ratio that unsaturated reaction forms hafnium oxide taking place is Hf: O=1: 1.5; The chemical dosage ratio that unsaturated reaction formation titanium oxide takes place is Ti: O=1: 1.6.
Alternatively, the gas in the described thermal anneal process is oxygen, nitrogen or their mist.
Alternatively, the annealing region in the described thermal anneal process is 200-1050 ℃, and the scope of annealing time is 30s-30min.
Compared with prior art, technique scheme has the following advantages:
The manufacture method of resistance-variable storing device of the present invention, two kinds of resistive functional layers that binary metal oxide is alternately laminated have been formed, the metal ion of different metal oxides there are differences, as ionic radius with to affinity of oxygen element etc., like this, pass through annealing process, spreading at the interface of two kinds of metal oxides, form compound dielectric intermediate, form fault of construction, thereby optimize the electrology characteristic of resistive functional layer, improve the uniformity of transition parameters.
Description of drawings
Shown in accompanying drawing, above-mentioned and other purpose, feature and advantage of the present invention will be more clear.Reference numeral identical in whole accompanying drawings is indicated identical part.Painstakingly do not draw accompanying drawing by actual size equal proportion convergent-divergent, focus on illustrating purport of the present invention.
Fig. 1 is the basic structure schematic diagram of resistance-variable storing device device;
Fig. 2 is the flow chart of the manufacture method of resistance-variable storing device of the present invention;
Fig. 3-6 is the schematic diagram according to each fabrication stage of the resistance-variable storing device of the embodiment of the invention.
Embodiment
For above-mentioned purpose of the present invention, feature and advantage can be become apparent more, below in conjunction with accompanying drawing the specific embodiment of the present invention is described in detail.
A lot of details have been set forth in the following description so that fully understand the present invention, but the present invention can also adopt other to be different from alternate manner described here and implement, those skilled in the art can do similar popularization under the situation of intension of the present invention, so the present invention is not subjected to the restriction of following public specific embodiment.
Secondly, the present invention is described in detail in conjunction with schematic diagram, when the embodiment of the invention is described in detail in detail; for ease of explanation; the profile of expression device architecture can be disobeyed general ratio and be done local the amplification, and described schematic diagram is example, and it should not limit the scope of protection of the invention at this.The three dimensions size that in actual fabrication, should comprise in addition, length, width and the degree of depth.
In order to optimize the electrology characteristic of resistive functional layer, improve the uniformity of resistance-variable storing device transition parameters, as shown in Figure 2, the invention provides a kind of manufacture method of resistance-variable storing device, comprising:
Form first electrode;
Form the resistive functional layer at described first electrode, wherein, described resistive functional layer comprises one deck first binary metal oxide and one deck second binary metal oxide at least at least, and described first binary metal oxide and second binary metal oxide are alternately laminated;
Carry out thermal anneal process;
Form second electrode in described resistive functional layer.
In manufacture method of the present invention, two kinds of resistive functional layers that binary metal oxide is alternately laminated have been formed, the metal ion of different metal oxides there are differences, as ionic radius with to affinity of oxygen element etc., like this, pass through annealing process, spreading at the interface of two kinds of metal oxides, form compound dielectric intermediate, form fault of construction, thereby optimize the electrology characteristic of resistive functional layer, improve the uniformity of transition parameters.
In the present invention, the resistive functional layer is by first binary metal oxide and the alternately laminated structure of second binary metal oxide, and first binary metal oxide is different binary metal oxide materials, for example ZrO with second binary metal oxide
2, HfO
2, TiO
2, SiO
2, WO
x, NiO, CuO
x, ZnO, TaO
x, Y
2O
3Etc..
In the present invention, by thermal anneal process, promote spreading at the interface of these two kinds of metal oxides, form compound dielectric intermediate, form fault of construction, thereby optimize the electrology characteristic of resistive functional layer, improve the uniformity of transition parameters.
In order to understand the present invention better, below with reference to the diagram of each fabrication stage, the manufacture method of above-mentioned resistance-variable storing device embodiment is described in detail.
At first, provide substrate 200, with reference to shown in Figure 3.
In this embodiment, substrate 200 can comprise the Si substrate, can also be formed with SiO on the Si substrate
2Insulating barrier.
In other embodiments, described substrate can also include but not limited to other semiconductors or compound semiconductor, as carborundum, GaAs, indium arsenide or indium phosphide.According to the known designing requirement of prior art (for example p-type substrate or n type substrate), substrate 200 can comprise various doping configurations.In addition, can also comprise other devices in the substrate.
Then, form first electrode 202 at described substrate 200, as shown in Figure 3.
In this embodiment, electron beam evaporation process be can utilize, Ti layer and Pt layer on described substrate 200, formed successively as first electrode 202, bottom electrode just, the thickness of described Ti layer can be 20nm, and the thickness of described Pt layer can be 80nm, and the Ti layer is Pt layer and SiO
2The adhesion layer of insulating barrier.
In other embodiments, described first electrode can also be for comprising the single or multiple lift structure of inert metal, inert metal compound or other suitable metal materials, described inert metal example comprises W, Al, Cu, Au, Ag, Pt, Ru, Ti, Ta, the example of described inert metal compound comprises TiN, TaN, ITO, IZO, can adopt electron beam evaporation, chemical vapour deposition (CVD), pulsed laser deposition, ald, magnetron sputtering or other suitable methods to form.
Then, form resistive functional layer 204 at described first electrode 202, with reference to shown in Figure 4.
In this embodiment, deposit one deck hafnium oxide (HfO by ALD (ald) technology at first electrode 202
2) 204-1, thickness can be 3-10nm, then the thicker titanium oxide (TiO of deposit one deck thereon
2) 204-2, thickness can be 20-30nm, then deposit one deck hafnium oxide (HfO again on titanium oxide
2) 204-3, thickness can be 3-10nm, thereby has formed the resistive functional layer 204 of the stepped construction of being made up of hafnium oxide-titanium oxide-hafnium oxide.
When adopting the ALD technology to deposit, generally include step:
S1, the substrate that will have first electrode places reaction chamber, vacuumizes and heats, and reaches the preparation condition of required technology;
S2 feeds first kind of precursor, and under the air-flow effect, precursor is realized saturated, irreversible chemisorbed at substrate surface;
S3 feeds inert gas, purges substrate surface, under the air-flow effect, with the byproduct of reaction of excessive precursor and the chemisorbed reaction chamber that blows off;
S4 feeds second kind of reaction precursor, in substrate surface generation chemisorbed, thereby with step S2 in be adsorbed on substrate surface first kind of precursor generation chemical reaction form solid-state film;
S5 feeds inert gas at this, purges substrate surface, removes excessive second kind and reacts precursor and byproduct of reaction;
S6, repeating step S2-S5 is up to forming required film thickness.
In order to guarantee the saturated absorption of first kind of reaction precursor, S2-S3 can be repeated repeatedly, and in order to guarantee the saturated absorption of reaction precursor in second, also S4-S5 can be repeated repeatedly.
In the present embodiment, adopt ALD deposition techniques hafnium oxide (HfO
2) time, the presoma of employing is tetramethyl ethyl ester-metal hafnium amine salt (TEMAHf), another kind of presoma adopts deionized water (H
2O).Wherein deionized water adopts and feeds reaction chamber from the volatilization mode, and the volatilization pressure under the TEMAHf normal temperature is less, adopts the method for heating, and heating-up temperature is 100 ℃.Inert gas adopts nitrogen (N
2).On concrete technological parameter, preferable reaction temperature is 250 ℃ in the experiment; Reaction pressure control is below 2mBar; Inert gas flow control is at 200sccm; The reactant service time, TEMAHf control is at 550ms, deionized water control is at 500ms, the time control of inert gas purge is at 2000ms, under such process conditions, by control reduce slightly the dosage of reactants water and faster reaction cycle time realize unsaturated reaction, the stoichiometric proportion of the hafnia film of formation is about Hf: O=1: 1.5.
In the present embodiment, adopt ALD deposition techniques titanium oxide (TiO
2) time, the presoma of employing is titanium tetrachloride (TiCl
4), another kind of presoma adopts deionized water (H
2O).Both all adopt from the volatilization mode and feed reaction chamber, and inert gas adopts nitrogen (N
2).On concrete technological parameter, select 250 ℃ of reaction temperatures in the experiment according to qualifications; Reaction pressure control is below 2mBar; Inert gas flow control is at 200sccm; The reactant service time, titanium tetrachloride control is at 200ms, deionized water control is at 250ms, the time control of inert gas purge is at 1500ms, under such process conditions, by control reduce slightly the dosage of reactants water and faster reaction cycle time realize unsaturated reaction, the stoichiometric proportion of the thin film of titanium oxide of formation is about Ti: O=1: 1.6.
Structure, material and the preparation technology of above resistive functional layer only are example, in other embodiments, can also adopt other materials, other technological parameters to form the resistive functional layer of other structures.
Then, carry out thermal anneal process.
In the present embodiment, the gas of thermal anneal process can be oxygen, nitrogen or their mist etc., and flow can be 0-15L/min; preferably, can be 2L/min, annealing region can be 200-1050 ℃; preferably, can be 400-850 ℃, annealing time can be 30s-30min; preferably can be 30s-20min; after the annealing, stop heating, keep Annealing Protection atmosphere; take out wafer after naturally cooling to low temperature, generally in the time of 200 ℃, take out.By annealing process, spreading at the interface of two kinds of metal oxides, as shown in Figure 5, form compound dielectric intermediate 204-4, form fault of construction, thereby optimize the electrology characteristic of resistive functional layer, improve the uniformity of transition parameters.
At last, form second electrode 206 in resistive functional layer 204, as shown in Figure 6.
In the present embodiment, can utilize the method for electron beam evaporation, deposit Cu and carry out photoetching in described resistive functional layer 204, adopt stripping technology to form second electrode 206, top electrode just, thickness can be 50nm, thereby forms the typical storage devices structure of metal-oxide-metal.In other embodiments, can also adopt other suitable methods to form second electrode of material requested.
The above only is preferred embodiment of the present invention, is not the present invention is done any pro forma restriction.
Though the present invention discloses as above with preferred embodiment, yet is not in order to limit the present invention.Any those of ordinary skill in the art, do not breaking away under the technical solution of the present invention scope situation, all can utilize method and the technology contents of above-mentioned announcement that technical solution of the present invention is made many possible changes and modification, or be revised as the equivalent embodiment of equivalent variations.Therefore, every content that does not break away from technical solution of the present invention according to any simple modification, equivalent variations and the modification that technical spirit of the present invention is done above embodiment, all still belongs in the scope of technical solution of the present invention protection.
Claims (7)
1. the manufacture method of a resistance-variable storing device is characterized in that, described method comprises:
Form first electrode;
Form the resistive functional layer at described first electrode, wherein, described resistive functional layer comprises one deck first binary metal oxide and one deck second binary metal oxide at least at least, and described first binary metal oxide and second binary metal oxide are alternately laminated;
Carry out thermal anneal process;
Form second electrode in described resistive functional layer.
2. manufacture method according to claim 1 is characterized in that, adopts technique for atomic layer deposition to form the resistive functional layer at described first electrode.
3. manufacture method according to claim 2 is characterized in that, described first binary metal oxide is hafnium oxide, and described second binary metal oxide is titanium oxide.
4. manufacture method according to claim 3 is characterized in that, the precursor that adopts in the ald is that unsaturated reaction formation hafnium oxide takes place for TEMAHf and deionized water; The precursor that adopts in the ald is that unsaturated reaction formation titanium oxide takes place for titanium tetrachloride and deionized water.
5. manufacture method according to claim 4 is characterized in that, the chemical dosage ratio that unsaturated reaction formation hafnium oxide takes place is Hf: O=1: 1.5; The chemical dosage ratio that unsaturated reaction formation titanium oxide takes place is Ti: O=1: 1.6.
6. manufacture method according to claim 1 is characterized in that, the gas in the described thermal anneal process is oxygen, nitrogen or their mist.
7. manufacture method according to claim 1 is characterized in that, the annealing region in the described thermal anneal process is 200-1050 ℃, and the scope of annealing time is 30s-30min.
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| CN105140391A (en) * | 2015-07-02 | 2015-12-09 | 河北大学 | Double-charge injection trap memory and preparation method thereof |
| CN105575991A (en) * | 2014-09-04 | 2016-05-11 | 财团法人交大思源基金会 | Memory structure and method of forming the same |
| WO2017157074A1 (en) * | 2016-03-18 | 2017-09-21 | 中国科学院微电子研究所 | Selector for use in bipolar resistive memory and manufacturing method for selector |
| CN110828658A (en) * | 2018-08-08 | 2020-02-21 | 北京北方华创微电子装备有限公司 | Preparation method of resistive random access memory device and resistive random access memory device |
| CN111009609A (en) * | 2019-12-24 | 2020-04-14 | 华中科技大学 | Superlattice memristor functional layer material, memristor unit and preparation method of superlattice memristor functional layer material |
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| CN105140391B (en) * | 2015-07-02 | 2017-12-08 | 河北大学 | A kind of Double-charge implantation capture memory and preparation method thereof |
| WO2017157074A1 (en) * | 2016-03-18 | 2017-09-21 | 中国科学院微电子研究所 | Selector for use in bipolar resistive memory and manufacturing method for selector |
| CN110828658A (en) * | 2018-08-08 | 2020-02-21 | 北京北方华创微电子装备有限公司 | Preparation method of resistive random access memory device and resistive random access memory device |
| CN111009609A (en) * | 2019-12-24 | 2020-04-14 | 华中科技大学 | Superlattice memristor functional layer material, memristor unit and preparation method of superlattice memristor functional layer material |
| WO2021128994A1 (en) * | 2019-12-24 | 2021-07-01 | 华中科技大学 | Superlattice memristor functional layer material, and memristor unit and preparation method therefor |
| CN114068808A (en) * | 2021-11-03 | 2022-02-18 | 厦门半导体工业技术研发有限公司 | Semiconductor integrated circuit device and method for manufacturing the same |
| CN116507195A (en) * | 2023-06-21 | 2023-07-28 | 武汉大学 | Based on WO x /YO y Preparation method of double-heterojunction structure analog memristor |
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