CN103515535A - Preparing method of phase-changing memory contact electrode and phase-changing memory contact electrode - Google Patents
Preparing method of phase-changing memory contact electrode and phase-changing memory contact electrode Download PDFInfo
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- CN103515535A CN103515535A CN201310471274.4A CN201310471274A CN103515535A CN 103515535 A CN103515535 A CN 103515535A CN 201310471274 A CN201310471274 A CN 201310471274A CN 103515535 A CN103515535 A CN 103515535A
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Abstract
The invention provides a preparing method of a phase-changing memory contact electrode and the phase-changing memory contact electrode. A grapheme layer is deposited on the surface, where metal catalysts are deposited, of a heating electrode, the high flatness of grapheme is effectively used, deposition is only carried out on the surface, covered with the catalysts, of the heating electrode, a further flattening process is of no need, and the technology is simple. Meanwhile, the grapheme is tight in carbon atom array, carbon atoms in a layer are bound through covalent bonds according to sp2 hybridization, strong acting force is achieved, phase-changing storage material atoms can be greatly prevented from being dispersed into the heating electrode, and accordingly the consistency of components and physical property of phase-changing storage materials and the electrode is kept the same. In addition, the thickness of the grapheme is controlled between 0.3nm and 10nm, a high heat conductivity coefficient is achieved, heating electrode efficiency is guaranteed, and the application requirement of a phase-changing memory can be well met.
Description
[technical field]
The present invention relates to semiconductor preparing technical field, relate in particular to a kind of preparation method and phase transition storage contact electrode of phase transition storage contact electrode.
[background technology]
Along with the development of technology, semiconductor memory, as flash memory (FLASH), static random access memory (SRAM) and dynamic random access memory (DRAM) etc., just progressively faces its " technical bottleneck " problem under advanced technologies technology node more.Development of Novel memory technology, the restriction facing to overcome current semiconductor memory technologies, adapts to the application demands such as high power capacity, low-power consumption and fast access and has important research and development value.
In recent years, take the phase transition storage (phase-change memory, PCM) that phase-change material is storage medium is just shown great attention to.Compare with semiconductor memory, PCM belongs to resistor-type memory, there are some obvious advantages, as low cost of manufacture, radioresistance, there is excellent size micro performance and multidigit unit storage capacity to adapt to more high-capacity storage etc., be recognized as at present main flow memory technology of future generation.The PCM conventionally binary based on Ge, Sb and Te element or ternary alloy three-partalloy is core phase-change storage material; yet in the PCM course of work; Ge, Sb and Te atom; especially Te atom fusing point is low; vapour pressure is high; be easy to spread in heating electrode (being generally W); can cause like this component of phase-change storage material and heating electrode and physical property to change; then have a strong impact on the service behaviour of PCM; as after causing repeatedly programming operation there is drift in initial condition; cycle life declines, long term data confining force reduction etc.
For solving this key issue, industry has developed by introduce transition zone between phase-change storage material and contact electrode, as TiN, to alleviate the diffusion of material atom, but still existing the anti-diffusivity of TiN material limited, film thickness, in tens nanometer, has limited the efficiency of heating electrode, meanwhile, because increasing extra flatening process, needs can bring the outstanding problems such as cost increase.
[summary of the invention]
The object of the present invention is to provide a kind of preparation method of phase transition storage contact electrode, its electrical property of phase transition storage contact electrode of preparing by the method is good.
For achieving the above object, the present invention adopts following technical proposals:
A preparation method for phase transition storage contact electrode, comprises the steps:
In heating electrode surface deposition metal catalyst layer, described heating electrode is of a size of 20～150nm;
Depositing the heating electrode surface deposition graphene layer of metal catalyst layer, described Graphene is reduced graphene, and described Graphene thickness is 0.3～10nm; And
Again at the heating electrode surface deposition phase-change storage material layer after above-mentioned steps is processed.
Preferably, described metal catalyst layer is at least one in Ni, Cu, and the thickness of described metal catalyst layer is 5-100nm.
Preferably, in heating electrode surface deposition metal catalyst layer, wherein, the method for described deposition be in thermal evaporation, electron beam evaporation and magnetron sputtering any one or multiple.
Preferably, the number of plies of described graphene layer is 1～20 layer.
Preferably, depositing the heating electrode surface deposition graphene layer of metal catalyst layer, comprise the steps:
The heating electrode that deposits metal catalyst layer is placed in to vacuum environment;
Pass into protective gas, and be warming up to 800～1000 ℃, described protective gas is argon gas; And
Pass into successively reaction the first reacting gas and the second reacting gas and fully react, described the first reacting gas is hydrogen, and described the second reacting gas is methane.
Preferably, the vacuum degree of described vacuum environment is 0.1～50mTorr.
Preferably, the flow of described protective gas is 100～500sccm.
Preferably, the flow of described the first reacting gas is 50～300sccm, and the flow of described the second reacting gas is 20～200sccm.
Preferably, the time of described reaction is 1～15min.
Preferably, described phase-change storage material is Ge
2sb
2te
5, N doped with Ge
2sb
2te
5, O doped with Ge
2sb
2te
5, Si doped with Ge
2sb
2te
5, Ge
2sbTe
5, GeTe, Sb
2te
3in any one or multiple.
In addition, the present invention also provides a kind of phase transition storage contact electrode, comprise successively heating electrode, metal catalyst layer, graphene layer and phase-change storage material layer from bottom to top, described heating electrode is of a size of 20～150nm, described Graphene is reduced graphene, and described Graphene thickness is 0.3～10nm.
Adopt technique scheme, beneficial effect of the present invention is:
The preparation method of phase transition storage contact electrode provided by the invention, by in heating electrode surface deposition metal catalyst layer, depositing the heating electrode surface deposition graphene layer of metal catalyst layer, then at the heating electrode surface deposition phase-change storage material layer after above-mentioned steps is processed.Phase transition storage contact electrode provided by the invention, depositing the heating electrode surface deposition graphene layer of metal catalyst layer, effectively utilized the high-flatness of Graphene, and only on the heating electrode surface that is coated with catalyst, deposit, without further flatening process, technique is simple; Simultaneously, Graphene has carbon atom arrangement closely, in layer wherein between carbon atom according to the covalent bonds of sp2 hydridization, there is stronger active force, can greatly suppress phase-change storage material atom and diffuse among heating electrode, thereby guarantee the consistent of the component of phase-change storage material and heating electrode and physical property; In addition, Graphene thickness can be controlled in 0.3～10nm, and has high conductive coefficient, has guaranteed heating electrode efficiency, can meet well the application demand of phase transition storage.
[accompanying drawing explanation]
The preparation method's of the phase transition storage contact electrode that Fig. 1 provides for the embodiment of the present invention flow chart of steps;
Fig. 2 is the flow chart of steps depositing the heating electrode surface deposition graphene layer of metal catalyst layer provided by the invention;
The structural representation of the phase transition storage contact electrode that Fig. 3 provides for the embodiment of the present invention.
[embodiment]
In order to make object of the present invention, technical scheme and advantage clearer, below in conjunction with drawings and the specific embodiments, the present invention is further elaborated.Should be appreciated that specific embodiment described herein, only in order to explain the present invention, is not intended to limit the present invention.
In application documents, relational terms such as the first and second grades is only used for an entity or operation to separate with another entity or operating space, and not necessarily requires or imply and between these entities or operation, have the relation of any this reality or sequentially.And, term " comprises ", " comprising " or its any other variant are intended to contain comprising of nonexcludability, thereby the process, method, article or the equipment that make to comprise a series of key elements not only comprise those key elements, but also comprise other key elements of clearly not listing, or be also included as the intrinsic key element of this process, method, article or equipment.The in the situation that of more restrictions not, the key element being limited by statement " comprising ... ", and be not precluded within process, method, article or the equipment that comprises described key element and also have other identical element.
Refer to Fig. 1, steps flow chart Figure 100 of the preparation method of the phase transition storage contact electrode that Fig. 1 provides for the embodiment of the present invention, as can be seen from Fig. 1, the preparation method 100 of phase transition storage contact electrode comprises the steps:
Step S110: in heating electrode surface deposition metal catalyst layer, wherein, heating electrode is of a size of 20～150nm;
Particularly, heating electrode is placed in to metal depositing device, adopts the method for thermal evaporation, electron beam evaporation or magnetron sputtering at heating electrode surface deposition layer of metal catalyst.
Preferably, metal catalyst layer is at least one in Ni, Cu.The thickness of metal catalyst layer is 5-100nm.
Preferably, the present invention is by adopting in thermal evaporation, electron beam evaporation and magnetron sputtering at least one method in heating electrode surface deposition metal catalyst layer.
Step S120: depositing the heating electrode surface deposition graphene layer of metal catalyst layer, wherein, Graphene is reduced graphene; Preferably, the number of plies of graphene layer is 1～20 layer.
Be appreciated that Graphene surface has higher evenness, and only on the heating electrode surface that is coated with catalyst, deposit, without further flatening process, simplified technique; In addition, between the interior carbon atom of layer in Graphene, according to the covalent bonds of sp2 hydridization, there is stronger active force, can greatly suppress phase-change storage material atom, diffuse among heating electrode, thereby guaranteed the consistent of the component of phase-change storage material and heating electrode and physical property; In addition, Graphene thickness can be controlled in 0.3～10nm, and has high conductive coefficient (up to 5300W/mK, far above the 19.2W/mK of TiN material), has guaranteed heating electrode efficiency, can meet well the application demand of phase transition storage.
Refer to Fig. 2, for the flow chart of steps depositing the heating electrode surface deposition graphene layer of metal catalyst layer provided by the invention, comprise the steps:
Step S121: the heating electrode that deposits metal catalyst layer is placed in to vacuum environment;
Particularly, the heating electrode that deposits metal catalytic agent film is placed in to vacuum tube furnace, regulating the vacuum degree of vacuum tube furnace is 0.1～50mTorr.
Step S122: pass into protective gas, and be warming up to 800～1000 ℃;
Preferably, protective gas is argon gas, and the flow of protective gas is 100～500sccm.
Step S123: pass into successively reaction the first reacting gas and the second reacting gas and fully react, the first reacting gas is hydrogen, and the second reacting gas is methane;
Preferably, the flow of the first reacting gas is 50～300sccm, and the flow of the second reacting gas is 20～200sccm, and the time of reaction is 1～15min.
Be appreciated that the heating electrode that deposits metal catalyst layer is placed in to vacuum tube furnace, regulate the flow of air pressure, temperature, protective gas and the reacting gas of vacuum tube furnace, thereby at heating electrode surface deposition graphene layer.
Step S130: again at the heating electrode surface deposition phase-change storage material layer after above-mentioned steps is processed.
Particularly, the heating electrode that deposits graphene layer is taken out from vacuum tube furnace, further utilize physical gas-phase deposite method at its surface deposition phase-change storage material.
Preferably, phase-change storage material is Ge
2sb
2te
5, N doped with Ge
2sb
2te
5, O doped with Ge
2sb
2te
5, Si doped with Ge
2sb
2te
5, Ge
2sbTe
5, GeTe, Sb
2te
3in any one or multiple.
Refer to Fig. 3, for the present invention also provides a kind of phase transition storage contact electrode 200, comprise successively heating electrode 210, metal catalyst layer 220, graphene layer 230 and phase-change storage material layer 240 from bottom to top, wherein, heating electrode 210 is of a size of 20～150nm, Graphene is reduced graphene, and Graphene thickness is 0.3～10nm.
The preparation method 100 of phase transition storage contact electrode provided by the invention and phase transition storage contact electrode 200, by in heating electrode 210 surface deposition metal catalyst layer 220, depositing the heating electrode 210 surface deposition graphene layers 230 of metal catalyst layer 220, then at the heating electrode 210 surface deposition phase-change storage material layers 240 after above-mentioned steps is processed.Phase transition storage contact electrode 200 provided by the invention, depositing the heating electrode 210 surface deposition graphene layers 230 of metal catalyst layer 220, effectively utilized the high-flatness of Graphene, and only on heating electrode 210 surfaces that are coated with catalyst, deposit, without further flatening process, technique is simple; Simultaneously, Graphene has carbon atom arrangement closely, in layer wherein between carbon atom according to the covalent bonds of sp2 hydridization, there is stronger active force, can greatly suppress phase-change storage material atom (as Ge, Sb and Te etc.) and diffuse among heating electrode, thereby guarantee the consistent of the component of phase-change storage material and heating electrode and physical property; In addition, Graphene thickness can be controlled in 0.3～10nm, and has high conductive coefficient, has guaranteed heating electrode efficiency, can meet well the application demand of phase transition storage.
By specific embodiment, further set forth the present invention below, these embodiment are only presented for purposes of illustration, do not limit the scope of the invention.
Embodiment mono-
Choose and be of a size of 20nm tungsten heating electrode, be placed on and in thermal evaporation apparatus, deposit 5nm Ni film; Then the heating electrode that deposits Ni film is placed in to vacuum tube furnace; regulate base vacuum degree 0.1mTorr; first pass into 500sccm protective gas argon gas; be warming up to 950 ℃; then pass into 150sccm reacting gas hydrogen and 20sccm reacting gas methane; after 3 minutes, take out, be then placed on and in Pvd equipment-magnetron sputtering coater, deposit Ge
2sb
2te
5.
By Raman spectrometer and atomic force microscope, analyze knownly, use the related parameter of the present embodiment to obtain individual layer reduced graphene on 20nm tungsten heating electrode surface.The phase transition storage contact electrode known by depth resolution X-ray photoelectron spectroscopic analysis, the present embodiment is related, Ge, Sb, Te atom are not found to diffuse in heating electrode within the scope of instrumental resolution; Contrast traditional W electrode and TiN material, can find on heating electrode surface to the distribution of finding Ge, Sb and Te atom in 20nm depth bounds.Further research is found, this patent relate to heating electrode than traditional electrode in the performance boost aspect working life with approximately 80%.
Embodiment bis-
Choose and be of a size of 50nm tungsten heating electrode, be placed on and in thermal evaporation apparatus, deposit 25nm Ni film; Then the heating electrode that deposits Ni film is placed in to vacuum tube furnace; regulate base vacuum degree 30mTorr; first pass into 400sccm protective gas argon gas; be warming up to 800 ℃; then pass into 50sccm reacting gas hydrogen and 20sccm reacting gas methane; after 5 minutes, take out, be then placed on and in Pvd equipment-magnetron sputtering coater, deposit N doped with Ge
2sb
2te
5.
By Raman spectrometer and atomic force microscope, analyze knownly, use the related parameter of the present embodiment to obtain 10 layer graphenes on 50nm tungsten heating electrode surface.The phase transition storage contact electrode known by depth resolution X-ray photoelectron spectroscopic analysis, the present embodiment is related, Ge, Sb, Te atom are not found to diffuse in heating electrode within the scope of instrumental resolution; Contrast traditional W electrode and TiN material, can find on heating electrode surface to the distribution of finding Ge, Sb and Te atom in 15nm depth bounds.Further research is found, this patent relate to heating electrode than traditional electrode in the performance boost aspect working life with approximately 75%.
Embodiment tri-
Choose and be of a size of 150nm tungsten heating electrode, be placed on and in thermal evaporation apparatus, deposit 100nm Ni film; Then the heating electrode that deposits Ni film is placed in to vacuum tube furnace; regulate base vacuum degree 0.1mTorr; first pass into 100sccm protective gas argon gas; be warming up to 1000 ℃; then pass into 300sccm reacting gas hydrogen and 200sccm reacting gas methane; after 1 minute, take out, be then placed on and in Pvd equipment-magnetron sputtering coater, deposit O doped with Ge
2sb
2te
5.
By Raman spectrometer and atomic force microscope, analyze knownly, use the related parameter of the present embodiment to obtain 20 layer graphenes on 150nm tungsten heating electrode surface.The phase transition storage contact electrode known by depth resolution X-ray photoelectron spectroscopic analysis, the present embodiment is related, Ge, Sb, Te atom are not found to diffuse in heating electrode within the scope of instrumental resolution; Contrast traditional W electrode and TiN material, can find on heating electrode surface to the distribution of finding Ge, Sb and Te atom in 15nm depth bounds.
Embodiment tetra-
Choose and be of a size of 50nm tungsten heating electrode, be placed on and in thermal evaporation apparatus, deposit 5nm Cu film; Then the heating electrode that deposits Cu film is placed in to vacuum tube furnace; regulate base vacuum degree 0.1mTorr; first pass into 450sccm protective gas argon gas; be warming up to 900 ℃; then pass into 150sccm reacting gas hydrogen and 50sccm reacting gas methane; after 3 minutes, take out, be then placed on and in Pvd equipment-magnetron sputtering coater, deposit Si doped with Ge
2sb
2te
5.
By Raman spectrometer and atomic force microscope, analyze knownly, use the related parameter of the present embodiment to obtain single-layer graphene on 50nm tungsten heating electrode surface.The phase transition storage contact electrode known by depth resolution X-ray photoelectron spectroscopic analysis, the present embodiment is related, Ge, Sb, Te atom are not found to diffuse in heating electrode within the scope of instrumental resolution; Contrast traditional W electrode and TiN material, can find on heating electrode surface to the distribution of finding Ge, Sb and Te atom in 15nm depth bounds.Further research is found, this patent relate to heating electrode than traditional electrode in the performance boost aspect working life with approximately 85%.
Embodiment five
Choose and be of a size of 50nm tungsten heating electrode, be placed on and in electron beam evaporation equipment, deposit 10nm Cu film; Then the heating electrode that deposits Cu film is placed in to vacuum tube furnace; regulate base vacuum degree 50mTorr; first pass into 450sccm protective gas argon gas; be warming up to 900 ℃; then pass into 150sccm reacting gas hydrogen and 50sccm reacting gas methane; after 3 minutes, take out, be then placed on and in Pvd equipment-magnetron sputtering coater, deposit Ge
2sbTe
5.
By Raman spectrometer and atomic force microscope, analyze knownly, use the related parameter of the present embodiment to obtain 5 layer graphenes on 50nm tungsten heating electrode surface.The phase transition storage contact electrode known by depth resolution X-ray photoelectron spectroscopic analysis, the present embodiment is related, Ge, Sb, Te atom are not found to diffuse in heating electrode within the scope of instrumental resolution; Contrast traditional W electrode and TiN material, can find on heating electrode surface to the distribution of finding Ge, Sb and Te atom in 20nm depth bounds.Further research is found, this patent relate to heating electrode than traditional electrode in the performance boost aspect working life with approximately 130%.
Embodiment six
Choose and be of a size of 50nm tungsten heating electrode, be placed on and in magnetron sputtering apparatus, deposit 100nm Cu film; Then the heating electrode that deposits Cu film is placed in to vacuum tube furnace; regulate base vacuum degree 0.1mTorr; first pass into 450sccm protective gas argon gas; be warming up to 900 ℃; then pass into 150sccm reacting gas hydrogen and 50sccm reacting gas methane; after 3 minutes, take out, be then placed on and in Pvd equipment-magnetron sputtering coater, deposit GeTe.
By Raman spectrometer and atomic force microscope, analyze knownly, use the related parameter of the present embodiment to obtain 20 layer graphenes on 50nm tungsten heating electrode surface.The phase transition storage contact electrode known by depth resolution X-ray photoelectron spectroscopic analysis, the present embodiment is related, Ge, Te atom are not found to diffuse in heating electrode within the scope of instrumental resolution; Contrast traditional W electrode and TiN material, can find to 10nm depth bounds, to find that Ge atom distributes, and still finds the distribution of Te atom to 20nm depth bounds on heating electrode surface.Further research is found, this patent relate to heating electrode than traditional electrode in the performance boost aspect working life with approximately 100%.
Embodiment seven
Choose and be of a size of 50nm tungsten heating electrode, be placed on and in thermal evaporation apparatus, deposit 5nm Cu film; Then the heating electrode that deposits Cu film is placed in to vacuum tube furnace; regulate base vacuum degree 0.1mTorr; first pass into 500sccm protective gas argon gas; be warming up to 850 ℃; then pass into 50sccm reacting gas hydrogen and 20sccm reacting gas methane; after 15 minutes, take out, be then placed on and in Pvd equipment-magnetron sputtering coater, deposit Sb
2te
3.
By Raman spectrometer and atomic force microscope, analyze knownly, use the related parameter of the present embodiment to obtain 10 layer graphenes on 50nm tungsten heating electrode surface.The phase transition storage contact electrode known by depth resolution X-ray photoelectron spectroscopic analysis, the present embodiment is related, Sb, Te atom are not found to diffuse in heating electrode within the scope of instrumental resolution; Contrast traditional W electrode and TiN material, can find on heating electrode surface to the distribution of finding Sb in 5nm depth bounds, to the distribution of still finding Te atom in 20nm depth bounds.Further research is found, this patent relate to heating electrode than traditional electrode in the performance boost aspect working life with approximately 90%.
The above, it is only preferred embodiment of the present invention, not the present invention is done to any pro forma restriction, although the present invention discloses as above with preferred embodiment, yet not in order to limit the present invention, any those skilled in the art, do not departing within the scope of technical solution of the present invention, when can utilizing the technology contents of above-mentioned announcement to make a little change or being modified to the equivalent embodiment of equivalent variations, in every case be not depart from technical solution of the present invention content, any simple modification of above embodiment being done according to technical spirit of the present invention, equivalent variations and modification, all still belong in the scope of technical solution of the present invention.
Claims (11)
1. a preparation method for phase transition storage contact electrode, is characterized in that, comprises the steps:
In heating electrode surface deposition metal catalyst layer, described heating electrode is of a size of 20～150nm;
Depositing the heating electrode surface deposition graphene layer of metal catalyst layer, described Graphene is reduced graphene, and described Graphene thickness is 0.3～10nm; And
Again at the heating electrode surface deposition phase-change storage material layer after above-mentioned steps is processed.
2. the preparation method of phase transition storage contact electrode according to claim 1, is characterized in that, described metal catalyst layer is at least one in Ni, Cu, and the thickness of described metal catalyst layer is 5-100nm.
3. the preparation method of phase transition storage contact electrode according to claim 1, it is characterized in that, in heating electrode surface deposition metal catalyst layer, wherein, the method for described deposition be in thermal evaporation, electron beam evaporation and magnetron sputtering any one or multiple.
4. the preparation method of phase transition storage contact electrode according to claim 1, is characterized in that, the number of plies of described graphene layer is 1～20 layer.
5. the preparation method of phase transition storage contact electrode according to claim 1, is characterized in that, depositing the heating electrode surface deposition graphene layer of metal catalyst layer, comprises the steps:
The heating electrode that deposits metal catalyst layer is placed in to vacuum environment;
Pass into protective gas, and be warming up to 800～1000 ℃, described protective gas is argon gas; And
Pass into successively reaction the first reacting gas and the second reacting gas and fully react, described the first reacting gas is hydrogen, and described the second reacting gas is methane.
6. the preparation method of phase transition storage contact electrode according to claim 5, is characterized in that, the vacuum degree of described vacuum environment is 0.1～50mTorr.
7. the preparation method of phase transition storage contact electrode according to claim 5, is characterized in that, the flow of described protective gas is 100～500sccm.
8. the preparation method of phase transition storage contact electrode according to claim 5, is characterized in that, the flow of described the first reacting gas is 50～300sccm, and the flow of described the second reacting gas is 20～200sccm.
9. the preparation method of phase transition storage contact electrode according to claim 5, is characterized in that, the time of described reaction is 1～15min.
10. the preparation method of phase transition storage contact electrode according to claim 1, is characterized in that, described phase-change storage material is Ge
2sb
2te
5, N doped with Ge
2sb
2te
5, O doped with Ge
2sb
2te
5, Si doped with Ge
2sb
2te
5, Ge
2sbTe
5, GeTe, Sb
2te
3in any one or multiple.
11. 1 kinds of phase transition storage contact electrodes, it is characterized in that, comprise successively heating electrode, metal catalyst layer, graphene layer and phase-change storage material layer from bottom to top, described heating electrode is of a size of 20～150nm, described Graphene is reduced graphene, and described Graphene thickness is 0.3～10nm.
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| CN109728162A (en) * | 2018-12-28 | 2019-05-07 | 中国科学院上海微***与信息技术研究所 | Phase-change thin film, phase-change memory cell and preparation method thereof and phase transition storage |
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