CN105428527B - A kind of based on amorphous state LaMnO3resistance-variable storing device of thin film and preparation method thereof - Google Patents
A kind of based on amorphous state LaMnO3resistance-variable storing device of thin film and preparation method thereof Download PDFInfo
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- 239000010409 thin film Substances 0.000 title claims abstract description 71
- 238000002360 preparation method Methods 0.000 title claims abstract description 21
- 229910002328 LaMnO3 Inorganic materials 0.000 claims abstract description 47
- 238000000034 method Methods 0.000 claims abstract description 46
- 238000001755 magnetron sputter deposition Methods 0.000 claims abstract description 23
- 239000000758 substrate Substances 0.000 claims abstract description 16
- 239000002346 layers by function Substances 0.000 claims abstract description 14
- 229910052751 metal Inorganic materials 0.000 claims abstract description 9
- 239000002184 metal Substances 0.000 claims abstract description 9
- 238000010276 construction Methods 0.000 claims abstract description 5
- 230000008569 process Effects 0.000 claims description 23
- 238000004544 sputter deposition Methods 0.000 claims description 23
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 18
- 239000007789 gas Substances 0.000 claims description 11
- 229910052786 argon Inorganic materials 0.000 claims description 9
- 238000005477 sputtering target Methods 0.000 claims description 8
- 239000013077 target material Substances 0.000 claims description 8
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 5
- 239000001301 oxygen Substances 0.000 claims description 5
- 229910052760 oxygen Inorganic materials 0.000 claims description 5
- 239000000919 ceramic Substances 0.000 claims description 4
- 238000005516 engineering process Methods 0.000 abstract description 12
- 238000005265 energy consumption Methods 0.000 abstract description 8
- 239000010408 film Substances 0.000 abstract description 7
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- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 5
- 229910052710 silicon Inorganic materials 0.000 description 5
- 239000010703 silicon Substances 0.000 description 5
- 238000009826 distribution Methods 0.000 description 4
- 238000003860 storage Methods 0.000 description 4
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- 229910052906 cristobalite Inorganic materials 0.000 description 3
- 239000000377 silicon dioxide Substances 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 3
- 229910052682 stishovite Inorganic materials 0.000 description 3
- 229910052905 tridymite Inorganic materials 0.000 description 3
- 125000004122 cyclic group Chemical group 0.000 description 2
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- 238000004377 microelectronic Methods 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
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- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
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- 239000004332 silver Substances 0.000 description 1
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
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Abstract
The invention discloses a kind of based on amorphous state LaMnO3The resistance-variable storing device of thin film, substrate, hearth electrode, top electrode and the functional layer between hearth electrode and top electrode the laminated construction formed, functional layer is amorphous state LaMnO3Thin film, amorphous state LaMnO3Film thickness is 20nm～40nm.The preparation method of the present invention, comprises the following steps: (1) prepares hearth electrode on substrate；(2) on described hearth electrode, functional layer amorphous state LaMnO is prepared by radio frequency magnetron sputtering method3Thin film；(3) in described amorphous state LaMnO3Top electrode is prepared by metal mask plate DC magnetron sputtering method on thin film.The resistance-variable storing device of the present invention, has the operation advantage that voltage is low, change resistance performance is good, and its preparation technology is not related to any high-temperature technology, the most just can realize, reduce energy consumption, save preparation time, be conducive to completely compatible with other techniques and actual application.
Description
Technical field
The invention belongs to microelectronics technology, be specifically related to a kind of amorphous state LaMnO3Resistance-variable storing device of thin film and preparation method thereof.
Background technology
In the information age, the mass memory of the information of explosive growth is seemed particularly important with quickly processing.Improve rapidly along with microelectronic chip integrated level and performance follow Moore's Law, conventional storage technologies based on CMOS technology moves closer to its physics limit, the Computer Storage wall problem that between processor and memorizer, speed difference causes also becomes increasingly severe, and these the most seriously hamper the further development of computer.Resistance-variable storing device is that two or more the different Resistance states utilizing some thin-film material to show under the effect of extra electric field store to realize data, is near during the last ten years by the one novel nonvolatile memory concept of academia and industrial quarters extensive concern.Resistance-variable storing device has that erasable speed is fast, memory density is high, the many merits such as high, multilevel storage and three-dimensional storage potentiality that repeats erasable number of times, the resistance-variable storing device with these excellent properties is the contenders of novel non-volatile storage technologies, is also the most promising a kind of technology alleviated and even solve Computer Storage wall problem.
Resistive material is the basis preparing resistance-variable storing device, the resistance-variable storing device reported at present has covered multiple material type, mainly includes binary oxide, solid electrolyte, simple substance class material, nitride, organic and polymeric material, perofskite type oxide etc..Wherein perofskite type oxide LaMnO3Belonging to the strong related system that the degree of freedom such as electric charge, track, lattice, spin intercouples, there is the interaction of Various Complex in inside, is the class functional material with specific physical properties and chemical property.At present for research LaMnO3Film characteristics, prepares crystalline state LaMnO frequently with laser molecular beam epitaxy, magnetron sputtering method3Thin film.This crystalline state LaMnO3The preparation temperature of thin film is the highest (more than 450 DEG C), and also needing to of having is annealed under high-temperature oxygen atmosphere, and this is unfavorable for and other process compatible and actual application.Additionally, crystalline state LaMnO3Thin film generation resistive effect answers that action required voltage is big, film thickness big, these be difficult to meet high density, at high speed, the requirement of low energy consumption non-volatile memory.
Summary of the invention
The technical problem to be solved in the present invention is to overcome the deficiencies in the prior art, it is provided that a kind of based on amorphous state LaMnO3Resistance-variable storing device of thin film and preparation method thereof, this amorphous state LaMnO3Film preparation temperature is low, can be with other process compatibles, based on this amorphous state LaMnO3Thin film resistance-variable storing device operation voltage is low, change resistance performance good, it is easy to meet high density, at high speed, the requirement of low energy consumption non-volatile memory.
For solving above-mentioned technical problem, the technical scheme that the present invention proposes is:
A kind of based on amorphous state LaMnO3The resistance-variable storing device of thin film, for the laminated construction formed by substrate, hearth electrode, top electrode and the functional layer between hearth electrode and top electrode, described functional layer is amorphous state LaMnO3Thin film, described amorphous state LaMnO3The thickness of thin film is 20 nm～40nm.
Above-mentioned resistance-variable storing device, it is preferred that described amorphous state LaMnO3Thin film uses radio frequency magnetron sputtering method to prepare, and the sputter temperature of rf magnetron sputtering is 20 DEG C～100 DEG C.
Above-mentioned resistance-variable storing device, it is preferred that described hearth electrode is Pt thin film, the thickness of described Pt thin film is 100 nm～300nm；Described top electrode is Ag thin film, and the thickness of described Ag thin film is 50 nm～200nm.
As a total inventive concept, the present invention also provides for the preparation method of a kind of above-mentioned resistance-variable storing device, comprises the following steps:
(1) on substrate, hearth electrode is prepared；
(2) on described hearth electrode, amorphous state LaMnO is prepared by radio frequency magnetron sputtering method3Thin layer；
(3) in described amorphous state LaMnO3Prepare top electrode by metal mask plate DC magnetron sputtering method on thin layer, i.e. obtain described resistance-variable storing device.
Above-mentioned preparation method, it is preferred that in described step (2), the process conditions of rf magnetron sputtering are with LaMnO3Ceramic target is sputtering target material, and chamber pressure is less than 5 × 10-4Pa(reduces the interference that in sputtering chamber, change resistance layer film preparation is brought by other molecules as far as possible), sputter temperature is 20 DEG C～100 DEG C, sputtering pressure is 0.8Pa～1.5Pa, sputtering power is 50W～100W, in sputter gas, argon flow amount is 20sccm～40sccm, and it is 10%～30% that oxygen volume accounts for the volume fraction of sputter gas.Microstructure and the final performance of resistance-variable storing device for assurance function layer, the present invention have selected suitable sputtering pressure (0.8Pa～1.5Pa): when sputtering pressure is less than 0.8 Pa, sputtered atom is few with the collision frequency of argon, energy is bigger, the thin film formed is fine and close, and resistance-variable storing device operation voltage so can be caused to increase；When sputtering pressure is higher than 1.5Pa, the mean free path of sputtered atom strongly reduces, and incides the kinetic energy of atom on substrate and significantly reduces, and the thin film formed can become again loose.In the present invention, thin film functional layer thickness is 20nm～40nm, and thickness is thin, adds open structure, easily lead to film breakdown, for ensureing the performance of resistance-variable storing device in the present invention, through research many times and checking, final sputtering pressure have selected 0.8Pa～1.5Pa.
Above-mentioned preparation method, it is preferred that in described step (3), the process conditions of magnetically controlled DC sputtering are with metal Ag target as sputtering target material, and chamber pressure is less than 1 × 10-3Pa, sputter temperature is 20 DEG C～50 DEG C, and sputtering pressure is 1.0Pa～2.0Pa, and sputtering power is 10W～20W, and sputter gas argon flow amount is 20sccm～40sccm.
Compared with prior art, it is an advantage of the current invention that:
The present invention based on amorphous state LaMnO3The resistance-variable storing device of thin film, uses amorphous state LaMnO3Thin film is compared with crystalline film, and depositing temperature is low, the range of choice width of composition, there is not crystal boundary, isotropism, amorphous state LaMnO3The ionic conductance of thin film is than crystalline state LaMnO3Want height；Amorphous state LaMnO3Thin film belongs to the decoupled system that ionic conductance relaxation separates with structural relaxation, can realize single-ion conductor, the separately control to change resistance layer thickness (20nm～40nm) wherein, advantageously in formation and the disconnection of silver conductive filament.Therefore, the present invention based on amorphous state LaMnO3The resistance-variable storing device of thin film has operation voltage is low, change resistance performance is good advantage, it is easy to meet high density, at high speed, the requirement of low energy consumption non-volatile memory.The one that the present invention provides is based on amorphous state LaMnO3The resistance-variable storing device of thin film, its functional layer thickness is only 20 nm～40nm, and resistance-variable storing device can be overcome to be difficult to meet high speed, the requirement of low energy consumption non-volatile memory.
The one that the present invention provides is based on amorphous state LaMnO3The resistance-variable storing device of thin film, its preparation technology is not related to any high-temperature technology, the most at low temperatures it is achieved that reduce energy consumption, saves preparation time, is conducive to completely compatible with other techniques and actual application.
Accompanying drawing explanation
Fig. 1 is that the present invention is based on amorphous state LaMnO3The resistance variation memory structure schematic diagram of thin film.
Fig. 2 be the embodiment of the present invention 1 based on amorphous state LaMnO3The resistance-variable storing device typical current-voltage characteristics curve of thin film.
Fig. 3 is based on amorphous state LaMnO in the embodiment of the present invention 13The SET voltage of continuous 30 the resistance switch processes of resistance-variable storing device of thin film and RESET voltage scattergram.
Fig. 4 be the embodiment of the present invention 2 based on amorphous state LaMnO3The resistance-variable storing device typical current-voltage characteristics curve of thin film.
Fig. 5 is based on amorphous state LaMnO in the embodiment of the present invention 23The SET voltage of continuous 30 the resistance switch processes of resistance-variable storing device of thin film and RESET voltage scattergram.
Marginal data: 1, silicon substrate；2、SiO2Insulating barrier；3, Ti adhesion layer；4, hearth electrode；5, amorphous state LaMnO3Thin film；6, top electrode.
Detailed description of the invention
For the ease of understanding the present invention, below in conjunction with Figure of description and preferred embodiment, the present invention is made more comprehensively, describes meticulously, but protection scope of the present invention is not limited to embodiment in detail below.
Unless otherwise defined, the implication that all technical term used hereinafter is generally understood that with those skilled in the art is identical.Technical term used herein is intended merely to describe the purpose of specific embodiment, is not intended to limit the scope of the invention.
Except there being special instruction, the various reagent used in the present invention, raw material are can commodity commercially or can be by the prepared product of known method.
Embodiment
1
:
A kind of present invention based on amorphous state LaMnO3The resistance-variable storing device of thin film, its structure is as it is shown in figure 1, be that (substrate is by silicon substrate 1, SiO by substrate2Insulating barrier 2 and Ti adhesion layer 3 forms), the laminated construction that formed of hearth electrode 4, top electrode 6 and the functional layer between hearth electrode 4 and top electrode 6, functional layer be thickness be amorphous state LaMnO of 20 nm3Thin film 5；Amorphous state LaMnO3Thin film 5 uses radio frequency magnetron sputtering method to prepare；Hearth electrode 4 is the Pt thin film that thickness is 100nm, and top electrode 6 is the Ag thin film that 50 nm are thick.
The present embodiment based on amorphous state LaMnO3The preparation method of the resistance-variable storing device of thin film, comprises the following steps:
(1) first on silicon substrate 1, SiO is prepared2Insulating barrier 2, then at SiO2Insulating barrier 2 prepares Ti adhesion layer 3, then prepares the Pt thin film (hearth electrode 4) that thickness is 100nm on Ti adhesion layer 3；
(2) on hearth electrode 4, thick amorphous state LaMnO of 20nm is prepared by radio frequency magnetron sputtering method3Thin film 5, wherein rf magnetron sputtering process conditions are: with diameter 60mm, the LaMnO of thickness 4mm3Ceramic target is sputtering target material, and chamber pressure is less than 5 × 10-4Pa, sputter temperature is 20 DEG C, and sputtering pressure is 0.8Pa, and sputtering power is 50W, and in sputter gas, argon flow amount is 20sccm, and it is 10% that oxygen accounts for the volume fraction of sputter gas；
(3) in amorphous state LaMnO3DC magnetron sputtering method is used to prepare Ag thin film thick for 200nm as top electrode 6 by metal mask plate on thin film 5, i.e. obtain resistance-variable storing device, wherein DC magnetron sputtering process condition is: with diameter 60mm, thickness 4mm metal Ag target as sputtering target material, chamber pressure be less than 1 × 10-3Pa, sputter temperature is 20 DEG C, and sputtering pressure is 1.0Pa, and sputtering power is 10W, and sputter gas argon flow amount is 20sccm.
Semiconductor Parameter Analyzer is utilized to study the resistance switch characteristic of resistance-variable storing device prepared by this enforcement, as shown in Figure 2, the resistance switch characteristic of resistance-variable storing device needs an electric forming process to excite, increase along with the forward voltage put on Ag electrode, when about 0.77V, electric current increases suddenly, device transfers rapidly low resistance state to from high-impedance state, and this process is referred to as electric forming process；Continuing to backward voltage, device comes back to high-impedance state from low resistance state again in left and right；This completes an electric forming I-V circulation, excite amorphous state LaMnO3The resistive characteristic of thin film.Fig. 3 is SET voltage and the RESET voltage distribution of continuous 30 the resistance switch processes of the present embodiment resistance-variable storing device.As it is shown on figure 3, SET voltage and RESET voltage narrow distribution in 30 cyclic processes, show that this resistance-variable storing device has a relatively stable SET and RESET process, the meansigma methods of SET voltage and RESET voltage be respectively 0.75 V and.
Embodiment
2
:
A kind of present invention based on amorphous state LaMnO3The resistance-variable storing device of thin film, its structure is as it is shown in figure 1, be that (substrate is by silicon substrate 1, SiO by substrate2Insulating barrier 2 and Ti adhesion layer 3 forms), the laminated construction that formed of hearth electrode 4, top electrode 6 and the functional layer between hearth electrode 4 and top electrode 6, functional layer be thickness be amorphous state LaMnO of 40 nm3Thin film 5；Amorphous state LaMnO3Thin film 5 uses radio frequency magnetron sputtering method to prepare；Hearth electrode 4 is the Pt thin film that thickness is 300nm, and top electrode 6 is the Ag thin film that 200 nm are thick.
The present embodiment based on amorphous state LaMnO3The preparation method of the resistance-variable storing device of thin film, comprises the following steps:
(1) first on silicon substrate 1, SiO is prepared2Insulating barrier 2, then at SiO2Prepare Ti adhesion layer 3 on insulating barrier 2, then on Ti adhesion layer 3, prepare the Pt thin film (hearth electrode 4) that thickness is 300nm；
(2) on hearth electrode 4, thick amorphous state LaMnO of 40nm is prepared by radio frequency magnetron sputtering method3Thin film 5, wherein rf magnetron sputtering process conditions are: with diameter 60mm, the LaMnO of thickness 4mm3Ceramic target is sputtering target material, and chamber pressure is less than 5 × 10-4Pa, sputter temperature is 100 DEG C, and sputtering pressure is 1.5Pa, and sputtering power is 100W, and in sputter gas, argon flow amount is 40sccm, and it is 30% that oxygen accounts for sputter gas volume fraction；
(3) in amorphous state LaMnO3Use DC magnetron sputtering method to prepare Ag thin film thick for 400nm as top electrode 6 by metal mask plate on thin film 5, i.e. obtain resistance-variable storing device；Wherein DC magnetron sputtering process condition is: with diameter 60mm, thickness 4mm metal Ag target as sputtering target material, chamber pressure be less than 1 × 10-3Pa, sputter temperature is 20 DEG C, and sputtering pressure is 2.0Pa, and sputtering power is 20W, and sputter gas argon flow amount is 40sccm.
Semiconductor Parameter Analyzer is utilized to study the resistance switch characteristic of resistance-variable storing device prepared by this enforcement, as shown in Figure 4, the resistance switch characteristic of resistance-variable storing device needs an electric forming process to excite, increase along with the forward voltage put on Ag electrode, when about 0.67V, electric current increases suddenly, device transfers rapidly low resistance state to from high-impedance state, and this process is referred to as electric forming process；Continuing to backward voltage, device comes back to high-impedance state from low resistance state again in left and right；This completes an electric forming I-V circulation, excite amorphous state LaMnO3The resistive characteristic of thin film.Fig. 5 is SET voltage and the RESET voltage distribution of continuous 30 the resistance switch processes of this resistance-variable storing device.As it is shown in figure 5, SET voltage and RESET voltage narrow distribution in 30 cyclic processes, show that this resistance-variable storing device has a relatively stable SET and RESET process, the meansigma methods of SET voltage and RESET voltage be respectively 0.7 V and.
The present invention use magnetron sputtering method to be prepared for amorphous state LaMnO that a kind of thickness is 20nm～40nm3Thin film, its preparation technology is not related to any high-temperature technology, the most at low temperatures it is achieved that reduce energy consumption, saves preparation time, is conducive to completely compatible with other techniques and actual application, and, based on amorphous state LaMnO3The resistance-variable storing device of thin film has operation voltage is low, change resistance performance is good advantage, it is easy to meet high density, at high speed, the requirement of low energy consumption non-volatile memory.
Claims (4)
1. one kind based on amorphous state LaMnO3The resistance-variable storing device of thin film, for by substrate, hearth electrode, top electrode and be positioned at the end
The laminated construction that functional layer between electrode and top electrode is formed, it is characterised in that described functional layer is amorphous state LaMnO3Thin
Film, described amorphous state LaMnO3The thickness of thin film is 20nm～40nm；Described top electrode is Ag thin film, described Ag thin film
Thickness be 50nm～200nm；Described amorphous state LaMnO3Thin film uses radio frequency magnetron sputtering method to prepare；
The process conditions of described rf magnetron sputtering are: with LaMnO3Ceramic target is sputtering target material, chamber pressure less than 5 ×
10-4Pa, sputter temperature is 20 DEG C～100 DEG C, and sputtering pressure is 0.8Pa～1.5Pa, and sputtering power is 50W～100W；Spatter
Argon flow amount in body of emanating is 20sccm～40sccm, and it is 10%～30% that oxygen volume accounts for the volume fraction of sputter gas.
2. resistance-variable storing device as claimed in claim 1, it is characterised in that described hearth electrode is Pt thin film, described Pt thin film
Thickness be 100nm～300nm.
3. the preparation method of the resistance-variable storing device as described in any one of claim 1～2, it is characterised in that include following
Step:
(1) on substrate, hearth electrode is prepared；
(2) on described hearth electrode, functional layer amorphous state LaMnO is prepared by radio frequency magnetron sputtering method3Thin film；
(3) in described amorphous state LaMnO3Top electrode is prepared by metal mask plate DC magnetron sputtering method, i.e. on thin film
Obtain described resistance-variable storing device.
4. preparation method as claimed in claim 3, it is characterised in that in described step (3), the technique of magnetically controlled DC sputtering
Condition is: with metal Ag target as sputtering target material, and chamber pressure is less than 1 × 10-3Pa, sputter temperature is 20 DEG C～50 DEG C, sputtering
Pressure is 1.0Pa～2.0Pa, and sputtering power is 10W～20W, and sputter gas argon flow amount is 20sccm～40sccm.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN1977337A (en) * | 2004-05-03 | 2007-06-06 | 统一半导体公司 | Non-volatile programmable memory |
| CN101527349A (en) * | 2009-04-08 | 2009-09-09 | 南京大学 | Amorphous indium and tin oxide film and application thereof in manufacturing resistive memory element |
| CN103280525A (en) * | 2013-05-27 | 2013-09-04 | 河北大学 | Transparent resistance random access memory and manufacturing method thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1977337A (en) * | 2004-05-03 | 2007-06-06 | 统一半导体公司 | Non-volatile programmable memory |
| CN101527349A (en) * | 2009-04-08 | 2009-09-09 | 南京大学 | Amorphous indium and tin oxide film and application thereof in manufacturing resistive memory element |
| CN103280525A (en) * | 2013-05-27 | 2013-09-04 | 河北大学 | Transparent resistance random access memory and manufacturing method thereof |
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