CN101924180A - Antimony-rich Si-Sb-Te sulfur group compound phase-change material for phase change memory - Google Patents

Antimony-rich Si-Sb-Te sulfur group compound phase-change material for phase change memory Download PDF

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CN101924180A
CN101924180A CN 201010172922 CN201010172922A CN101924180A CN 101924180 A CN101924180 A CN 101924180A CN 201010172922 CN201010172922 CN 201010172922 CN 201010172922 A CN201010172922 A CN 201010172922A CN 101924180 A CN101924180 A CN 101924180A
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phase
change material
change
antimony
rich
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周夕淋
吴良才
宋志棠
饶峰
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Shanghai Institute of Microsystem and Information Technology of CAS
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Shanghai Institute of Microsystem and Information Technology of CAS
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Abstract

The invention provides an antimony-rich Si-Sb-Te sulfur group compound phase-change material for a phase change memory, belonging to the technical field of micro-electronics. The phase-change material maintains an atomic ratio of Si to Te of 1:3, the component general formula is SiaSb (100-4a) Te3a, wherein a is more than or equal to 10 and less than or equal to 20; compared with the existing Ge2Sb2Te5, the material features high crystallization temperature, good heat stability and better data retention capacity; moreover, the compound phase-change material in the crystalline state enjoys higher electrical resistivity and small thickness change of the material in crystalline state/amorphous state. With the phase-change material of the invention as the information memory medium, cycle operation times of the memory can be effectively increased, write operation power dissipation can be lowered and device reliability can be improved.

Description

The antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage
Technical field
The present invention relates to a kind of phase-change material that is used for phase transition storage, particularly a kind of antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage.
Background technology
Memory occupies critical role in semi-conductor market, and phase transition storage, nonvolatile memory of future generation as tool potentiality, it is to utilize phase change film material to realize information stores as storage medium, become the focus of research (Tech.Dig.-Int.Electron Devices Meet.2001,803) day by day because of having broad application prospects.Phase transition storage is based on memory (the Ovshinsky S R.Reversibleelectrical switching phenomena in discovered structure.Phys.Rev.Lett. of S.R.Ovshinsky in the Ao Fuxinsiji electronic effect of late 1960s proposition, 1968,21 (20): 1450), be that the resistance difference when utilizing phase-change material to produce reversible transition between amorphous state and crystalline state realizes storage.Chalcogenide is a high-impedance state when non crystalline structure, when crystal structure, be low resistance state, use the electricity pulse of programming can make phase-change material between amorphous state and crystalline state, carry out reversible transition, thereby realize that phase change cells is at the high-impedance state of correspondence and the reversible transition between the low resistance state.
The core of phase transition storage is a phase-change material, and the prerequisite key property of phase-change material comprises: between the high-speed phase change of nanosecond order, amorphous state, amorphous state and the crystalline state with long term high temperature thermal stability significantly resistance difference, surpass 10 6Inferior circulation changes ability (Nat.Mater., 6,824-832,2007).Obvious many materials can not satisfy above-mentioned condition, and until now, the typical material that is used for phase transition storage is Ge-Sb-Te, wherein with Ge 2Sb 2Te 5The most outstanding.Though with Ge 2Sb 2Te 5For the memory of storage medium at normal temperatures its data can keep 10 years, but since material from amorphous state to the transition temperature of the crystalline state of cubic structure relatively low (be about 170 degree), still the danger that exists data effectively not keep just becomes problem demanding prompt solution so improve the crystallization temperature of material with thermal stability that improves material and then the data holding ability that strengthens memory.Simultaneously owing to adopt Ge 2Sb 2Te 5Phase transition storage when carrying out write operation, need bigger electric current, therefore be difficult in portable product, be used widely.Have, in the circulation transition process of the amorphous state of phase transition storage and crystalline state, the thickness of phase change material film can change again, if change excessively, will influence the adhesion of phase-change thin film and electrode and other retes, is unfavorable for the long term device steady operation, and Ge 2Sb 2Te 5Also there is this problem in film.
Therefore, provide a kind of thermal stability height, operation is low in energy consumption and phase change film material that can long-term stable operation, has become present technique area research personnel urgent problem.
Summary of the invention
The object of the present invention is to provide a kind of antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage, with the thermal stability that improves phase transition storage, reduce its operation power consumption, and prolong the steady operation time limit.
Reach other purposes in order to achieve the above object, the antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage provided by the invention, the component general formula is Si aSb (100-4a)Te 3a, 10≤a≤20 wherein.
Preferable, preferred ingredient can be Si 10Sb 60Te 30, Si 17.5Sb 30Te 52.5, or Si 20Sb 20Te 60
Preferable, described material can adopt sputtering method, electron-beam vapor deposition method, vapour deposition process, reach a kind of method formation in the atomic layer deposition method.Wherein, can adopt Si, Sb, reach three simple substance target co-sputterings formation of Te, also can adopt Si-Sb alloys target and Te simple substance target co-sputtering to form or employing Si-Te alloys target and the formation of Sb simple substance target co-sputtering or employing Te-Sb alloys target and the formation of Si simple substance target co-sputtering, also can directly adopt the alloys target sputter of Si-Sb-Te to form.
Through experimental study, the antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage of the present invention externally under the effect of energy, is realized the reversible transition between high-resistance state and the low resistance state; It both can reduce write-operation current as the storage medium of phase transition storage the time, can improve the thermal stability of phase transition storage again, can improve the reliability and the cycling number of times of phase transition storage simultaneously.
Description of drawings
Fig. 1 is the SiSb that is used for the antimony-rich Si-Sb-Te sulfur group compound phase-change material of phase transition storage of the present invention 6Te 3, SiSb 1.7Te 3, SiSbTe 3Phase-change material is respectively under noncrystalline state and the X ray diffracting spectrums of 400 degree annealing after 2 minutes.
Fig. 2 is the SiSb that is used for the antimony-rich Si-Sb-Te sulfur group compound phase-change material of phase transition storage of the present invention 6Te 3, SiSb 1.7Te 3, SiSbTe 3The square resistance of phase-change material and the relation curve of annealing temperature.
Fig. 3 is the SiSb that is used for the antimony-rich Si-Sb-Te sulfur group compound phase-change material of phase transition storage of the present invention 6Te 3, SiSb 1.7Te 3, SiSbTe 3The data holding ability match relation curve of phase-change material.
Fig. 4 is the SiSbTe that is used for the antimony-rich Si-Sb-Te sulfur group compound phase-change material of phase transition storage of the present invention 3Phase-change material is under noncrystalline state and the X ray reflection collection of illustrative plates of 250 degree annealing after 2 minutes.
Fig. 5 is the SiSbTe that is used for the antimony-rich Si-Sb-Te sulfur group compound phase-change material of phase transition storage of the present invention 3Phase-change material is applied in the phase transition storage, the relation of formed device cell resistance and the pulse voltage that applied.
Fig. 6 is for adopting the SiSbTe that is used for the antimony-rich Si-Sb-Te sulfur group compound phase-change material of phase transition storage of the present invention 3The formed phase-change memory cell structure schematic diagram of phase-change material.
Embodiment
The antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage of the present invention, its component general formula is Si aSb- (100-4a)Te 3a, 10≤a≤20 wherein, it can adopt several different methods to form, for example, sputtering method, electron-beam vapor deposition method, vapour deposition process, atomic layer deposition method etc.When adopting sputtering method to form, the various elements in the material (be Si, Sb, and Te) can be distinguished corresponding different targets, and by apply the composition that different power can control material on each target, the thickness of material can be controlled by adjusting sputtering time; The chalcogenide alloy target that also can prepare corresponding composition earlier, obtain the film of corresponding composition again by the sputter alloy target material, promptly adopt Si-Sb alloys target and Te simple substance target co-sputtering to form, perhaps adopt Si-Te alloys target and Sb simple substance target co-sputtering to form, perhaps adopt Te-Sb alloys target and Si simple substance target co-sputtering to form; Also can directly adopt the alloys target sputter of Si-Sb-Te to form.Also can pass through in addition Si 2Sb 2Te 6The film intermediate ion injects Sb and forms or the like.
Below will be to Si 10Sb 60Te 30, Si 17.5Sb 30Te 52.5(be SiSb 1.7Te 3), and Si 20Sb 20Te 60(be SiSbTe 3) material is elaborated.
See also Fig. 1, it through the thickness on the silicon substrate of thermal oxidation is being SiSb about 200nm for preparation 1.7Te 3, Si1Sb 6Te 3-, SiSbTe 3The X ray diffracting spectrum of phase-change material sample before and after annealing in process; wherein; each material is cycle annealing 2 minutes under the temperature of 400 degree; whole annealing process is carried out under the protection of high pure nitrogen atmosphere; subgraph (a) is the X ray diffracting spectrum under the noncrystalline state, and subgraph (b) is the X ray diffracting spectrums of 400 degree annealing after 2 minutes.As seen from the figure, SiSb 6Te 3, SiSb 1.7Te 3, SiSbTe 3Phase-change material is typical non crystalline structure, the amorphous state that corresponding resistance value is higher in the deposition attitude; After the process annealing in process of higher temperature, these three kinds of phase-change materials have all taken place from non crystalline structure to the transformation with low-resistance polycrystalline structure, there is transformation behavior, simultaneously, along with the increase of antimony element atomic percent in the phase-change material, it is big that the X-ray diffraction intensity of phase-change material correspondence becomes, the half-breadth height reduces, illustrate that phase-change material crystal grain has the trend of increase, help to promote the stability of memory, prevent the inefficacy of device in crystalline state.
See also Fig. 2 again, it is the square resistance of the antimony-rich Si-Sb-Te sulfur group compound phase-change material of the different Si content that use add in-place thermal vacuum system and record and the relation curve of annealing temperature.When annealing temperature is lower than 180 when spending, all phase-change materials all are in the amorphous state of high resistant, and along with the further increase of temperature, the square resistance of all phase-change materials begins to occur significantly to descend to change the polycrystalline attitude that is in low-resistance into until phase-change material.This process can heat phase-change thin film and realizes in phase transition storage by applying external energies such as electric pulse, can realize the reversible transition of phase-change thin film between amorphous state and crystalline state by applying different electric pulses simultaneously.As seen from the figure, SiSb 6Te 3, SiSb 1.7Te 3, SiSbTe 3The crystallization temperature of phase change film material all is higher than Ge commonly used 2Sb 2Te 5Film, so this series material has better thermal stability and stronger data holding ability.
See also Fig. 3 again, along with the increase of Si content, the data holding ability of antimony-rich Si-Sb-Te sulfur group compound phase-change material strengthens gradually, wherein SiSbTe as seen from Figure 3 3Phase-change material is during as storage medium, and the maximum temperature that the data of storage keep can bear in 10 years has surpassed 130 degree, is better than the Ge that uses always greatly 2Sb 2Te 5Phase-change material (can not surpass 110 degree usually).The antimony-rich Si-Sb-Te sulfur group compound phase-change material of adopt optimizing keeps performance as the data that the storage medium of phase transition storage helps to promote memory, improves the reliability that data keep.
" writing " " wiping " of phase transition storage operation is the process that storage medium wherein circulates at high-impedance state and low resistance state, and promptly phase-change material experiences the reversible transition of amorphous state and crystalline state repeatedly, and the thickness of phase-change material can change in this process.Subgraph among Fig. 4 (a) and (b) be depicted as the SiSbTe for preparing on the silicon substrate 3Phase-change material is respectively at the X ray reflection collection of illustrative plates of amorphous state and crystalline state (i.e. the forms of 250 degree annealing after 2 minutes).Can obtain amorphous and thickness crystalline state of phase-change material by the match to curve among the figure and be respectively 91.673nm and 88.605nm, its thickness change is 3.35%, less than Ge commonly used 2Sb 2Te 5Phase change medium material (6.5%).Adopt the less phase-change thin film of varied in thickness to help to improve stability and the cycle characteristics of memory in operating process.
The square resistance of antimony-rich Si-Sb-Te sulfur group compound phase-change material polycrystalline attitude is higher than Ge commonly used as seen from Figure 2 2Sb 2Te 5Phase-change material, higher crystalline resistance help energy more effective transmission in " writing " operating process of memory, thereby reach the purpose that the operation power consumption " is write " in reduction.Simultaneously because its amorphous state square resistance also has bigger increase, so the antimony-rich Si-Sb-Te sulfur group compound phase-change material still has higher amorphous state/crystalline resistance rate of change, guaranteed the accuracy rate of data read in the operating process.
Figure 5 shows that SiSbTe 3Phase-change material is applied in the phase transition storage, and formed device resistance is with the situation of change of the electric pulse that applies, wherein, the phase-change memory cell structure of described phase transition storage as shown in Figure 6, phase-change memory cell comprises top electrode 1, SiSbTe 3Phase-change material 2, dielectric material are (as SiO 2) 3, and bottom electrode 4.Device is 40ns in pulse duration as shown in the figure, and amplitude is just to have realized under the pulse voltage effect about 2V from the polycrystalline attitude being lower than Ge commonly used to amorphous transformation 2Sb 2Te 5Phase change memory device; And the difference between its high value and the low resistance surpasses 2 orders of magnitude, can guarantee effectively reading of data.Therefore the antimony-rich Si-Sb-Te sulfur group compound phase-change material is a kind of material that low power consumption phase changing memory uses that is suitable for.
Need to prove that the antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage of the present invention is not only to be applied in above-mentioned phase-change memory cell structure, and can use at the various cellular constructions that are phase transition storage.In fact, just can constitute phase-change memory cell as long as between specific upper/lower electrode, fill antimony-rich Si-Sb-Te sulfur group compound phase-change material provided by the present invention.The upper/lower electrode material can adopt W, Ti, TiW, TiN, TiAlN, Al, graphite or other electric conducting material.The structure of phase-change memory cell also is not limited to structure shown in Figure 6, and in different structures, the structure of electrode can be different with size, and the geometry of key storage medium also can be different with size.Dielectric material in the phase-change memory cell is (as SiO 2) can adopt method preparations such as PECVD, electron beam evaporation as electricity and calorifics separator.This phase-change memory cell can prepare separately, also can same MOS, triode, the integrated formation array of diode or memory.
In sum, the advantage that is used for the antimony-rich Si-Sb-Te sulfur group compound phase-change material of phase transition storage of the present invention shows following aspect:
1, externally under the effect of energy, can realize the reversible transition between high-resistance state and the low resistance state, corresponding high low resistance state can be carried out storage before and after utilizing reversible transition, the ratio of the resistance of its high-impedance state and low resistance state resistance is 2 between the several magnitude, and described external energy can drive for heat, electron beam drives, electric pulse drives or laser pulse one or more in driving.
2, as the storage medium of phase transition storage the time, both can reduce write-operation current, can improve the thermal stability of phase transition storage again, and can improve the reliability and the cycling number of times of phase transition storage simultaneously.
3, phase-change material crystalline resistance rate of the present invention is Ge commonly used at present 2Sb 2Te 52 to 100 times of phase-change material can help effectively to reduce the write operation power consumption, and simultaneously, its thermal stability also is better than Ge 2Sb 2Te 5Therefore phase-change material is more suitable for the application under the adverse circumstances such as high temperature, also have, its antimony-rich Si-Sb-Te sulfur group compound phase change film material from amorphous state to the crystalline state transition process, varied in thickness is also less than Ge 2Sb 2Te 5Phase-change material, less varied in thickness can help to improve the stability and the cycling number of times of storage operation.
What 4, can be applicable to adopt various type of drive carries out the memory of storage based on Transformation Principle, comprises phase transition storage that phase change disc that laser pulse drives or electric pulse drive etc.
The foregoing description just lists expressivity principle of the present invention and effect is described, but not is used to limit the present invention.Any personnel that are familiar with this technology all can make amendment to the foregoing description under spirit of the present invention and scope.Therefore, the scope of the present invention should be listed as claims.

Claims (6)

1. antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage, it is characterized in that: the general formula of material component is Si aSb (100-4a)Te 3a, 10≤a≤20 wherein.
2. the antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage as claimed in claim 1 is characterized in that: preferred ingredient is Si 10Sb 60Te 30, Si 17.5Sb 30Te 52.5, and Si 20Sb 20Te 60In a kind of.
3. the antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage as claimed in claim 1 is characterized in that: described material adopts sputtering method, electron-beam vapor deposition method, vapour deposition process, reaches a kind of method formation in the atomic layer deposition method.
4. the antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage as claimed in claim 1 is characterized in that: described material adopts Si, Sb, reaches three simple substance target co-sputterings formation of Te.
5. the antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage as claimed in claim 1, it is characterized in that: described material adopts Si-Sb alloys target and Te simple substance target co-sputtering to form, perhaps adopt Si-Te alloys target and Sb simple substance target co-sputtering to form, perhaps adopt Te-Sb alloys target and Si simple substance target co-sputtering to form.
6. the antimony-rich Si-Sb-Te sulfur group compound phase-change material that is used for phase transition storage as claimed in claim 1 is characterized in that: described material directly adopts the alloys target sputter of Si-Sb-Te to form.
CN 201010172922 2010-05-13 2010-05-13 Antimony-rich Si-Sb-Te sulfur group compound phase-change material for phase change memory Pending CN101924180A (en)

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CN102130298A (en) * 2011-01-19 2011-07-20 中国科学院上海微系统与信息技术研究所 Si-Sb-Te phase change material for phase change storage
CN102185106A (en) * 2011-04-22 2011-09-14 中国科学院上海微系统与信息技术研究所 Phase change memory material and preparation method thereof
CN102610745A (en) * 2011-01-19 2012-07-25 中国科学院上海微系统与信息技术研究所 Si-Sb-Te based sulfur group compound phase-change material for phase change memory
CN110061131A (en) * 2019-04-23 2019-07-26 中国科学院上海微系统与信息技术研究所 A kind of phase-change material, phase-change memory cell and preparation method thereof

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CN101488557A (en) * 2009-02-23 2009-07-22 中国科学院上海微系统与信息技术研究所 Si-Sb-Se phase changing thin-film material used for phase changing memory

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CN101101965A (en) * 2005-08-11 2008-01-09 上海交通大学 Phase change film material of silicon-adulterated sulfur series for phase change memory
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CN102130298A (en) * 2011-01-19 2011-07-20 中国科学院上海微系统与信息技术研究所 Si-Sb-Te phase change material for phase change storage
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CN110061131A (en) * 2019-04-23 2019-07-26 中国科学院上海微系统与信息技术研究所 A kind of phase-change material, phase-change memory cell and preparation method thereof

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Application publication date: 20101222