CN102169958B - Nanocomposite phase-change material, preparation method and application thereof in phase-change memory - Google Patents
Nanocomposite phase-change material, preparation method and application thereof in phase-change memory Download PDFInfo
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- 239000012782 phase change material Substances 0.000 title claims abstract description 35
- 238000002360 preparation method Methods 0.000 title claims abstract description 16
- 239000000463 material Substances 0.000 claims abstract description 45
- 229910005900 GeTe Inorganic materials 0.000 claims abstract description 36
- 238000003860 storage Methods 0.000 claims abstract description 28
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Abstract
The invention relates to a nanocomposite phase-change material, a preparation method and an application thereof in a phase-change memory, wherein the nanocomposite phase-change material comprises a phase-change material GeTe with a molar percentage of 70-99% and a medium material HfO2 with a molar percentage of 1-30%. The phase-change material GeTe and the medium material HfO2 are uniformly compounded in a nanoscale, so that the crystallization of the phase-change material is suppressed, the thermal stability of the material is enhanced and the data keeping capacity of the material is improved on one hand, and the valid programming volume is reduced due to the participation of the medium material so as to reduce the volume change before and after the crystallization of phase-change unit and decrease the RESET current on the other hand; therefore, the operation stability and the realization of low power consumption of storage apparatus are promoted. In a word, the novel nanocomposite phase-change material is applied to a memory, and is capable of decreasing the RESET voltage of a phase-change storage apparatus and reducing the programming volume, which is beneficial to realizing high-density storage, increasing the heating efficiency of the phase-change memory during programming process, decreasing the power consumption, enhancing data keeping capacity, and the like.
Description
Technical field
The present invention relates to a kind of nano-composite phase-changing material based on tellurium germanium, preparation method, reach the purposes as phase transition storage, relate in particular to a kind of by GeTe and HfO
2The nano-composite phase-changing material that forms and the purposes in phase transition storage thereof.
Background technology
In recent years, the phase transition storage (PCM) that might become nonvolatile memory of future generation has caused the extensive concern of academia and industrial quarters.Compare with present existing multiple semiconductor memory technologies, PCM has that cell size is little, the data confining force strong, has extended cycle life, low in energy consumption, can multistagely store, read at a high speed, high-low temperature resistant (55-125 ℃), anti-irradiation and manufacturing process plurality of advantages such as simple (can and prior integrated circuit process be complementary).It is that the Joule heat that utilizes impressed current to produce makes phase change layer realize reversible transition between amorphous state (high resistant) and crystalline state (low-resistance), and resistance difference (resistance ratio is 10-500 times) huge between binary states can be used for storing and reading data " 0 " and " 1 ".
The operating characteristics of PCM depends primarily on the phase transformation performance of the phase-change storage material of device cell.Phase-change storage material commonly used mainly contains GeTe-Sb
2Te
3, Ag-In-Sb-Te, Si-Sb-Te material system etc., wherein Ge
2Sb
2Te
5(GST) commercial phase change disc and phase transition storage have been widely used in.But also exist some shortcomings, for example power consumption is bigger, is difficult to realize the high density storage, and crystallization temperature is lower, and the data confining force can not get guaranteeing, can not be applied in the special occasions of high temperature storage.In the phase-change material of new research and development, it is fast that GeTe has phase velocity, height resistance difference big (10
5Doubly), the characteristics of crystallization temperature height and Heat stability is good.But because its fusing point higher (720 degree), thereby the RESET electric current is obviously big than GST, so the power consumption of GeTe is bigger, and this has restricted it as the process of commercialization.In addition, in the phase-change material that contains Ge and Te element, repetitious high temperature is write and is wiped the component segregation that operation can cause material internal itself, and Ge or Te be to segregation at the interface, and also is proved to be very big threat to device reliability with phenomenon that active electrode material reacts.Therefore, how to improve thermal stability and the data confining force of phase transition storage, and the reduction power consumption has just become urgent problem.The present invention is evenly compound by GeTe and dielectric material, improves thermal stability and reduces power consumption, to solve the problem that exists in the current phase transition storage.
Nano-composite phase-changing material refers to phase-change material as principal phase, dielectric material is auxilliary phase, and this two-phase is evenly disperseed compound in nanoscale, by composite material two alternate " learning from other's strong points to offset one's weaknesses ", remedy the defective of single phase-change material, thereby reach the purpose of optimizing phase-change material phase transformation performance.At present in phase-change material research, that has reported has a SiO
2With Ge
2Sb
2Te
5Phase-change material compound, but because SiO
2The carrier mobility that less dielectric constant and composite material are lower, SiO
2With Ge
2Sb
2Te
5The threshold voltage of composite phase-change material is higher.For the further performance of boost device, seek a kind of dielectric material that can reduce threshold voltage and RESET voltage simultaneously and seem particularly important.
Summary of the invention
The object of the present invention is to provide a kind of thermal stability height, efficiency of heating surface height, reach the little nano-composite phase-changing material of effective programming volume.
Another object of the present invention is to provide a kind of preparation method of nano-composite phase-changing material.
A further object of the present invention is to provide a kind of low in energy consumption, phase transition storage that data holding ability is strong.
The present invention also has a purpose to be to provide a kind of preparation method of phase transition storage of superior performance.
Reach other purposes in order to achieve the above object, nano-composite phase-changing material provided by the invention comprises: molar percentage is the phase-change material GeTe of 70-99%, and molar percentage is the dielectric material of 1-30%.
Preferable, in the composite material that forms, described phase-change material GeTe and dielectric material HfO
2Evenly distribute.
Preferable, described phase-change material GeTe is the nano-scale particle shape in composite material, for example, the nano-scale particle shape, preferable, maximum gauge is less than 100 nanometers.
Comprise among the preparation method of above-mentioned nano composite material and adopt GeTe alloys target, perhaps simple substance Ge, Te target and HfO
2The step of target sputter simultaneously.
Preferable, during sputter, the base vacuum degree is less than 2 * 10
-4Pa, sputtering pressure are 0.18-0.25Pa, and temperature is room temperature, and the DC power supply that is added on the GeTe alloys target is 10-60 watt, and the direct current power that is added on simple substance Ge target and the Te target is 10-60 watt, is added in HfO
2Radio-frequency power supply on the target is 10-80 watt, and sputtering time is 5-60 minute, and deposit thickness is the 50-300 nanometer.
In addition, phase transition storage provided by the invention comprises that the above-mentioned nano-composite phase-changing material of employing is as the nano-composite phase-changing material layer of storage medium.
The preparation method of above-mentioned phase transition storage comprises step: it is characterized in that comprising step: (1) sputter on Semiconductor substrate prepares bottom electrode, that is: metal electrode layer tungsten and titanium nitride.Spin coating and preceding baking SU8 resist, the recycling electron beam lithography, mark and the electrode structure of making mixed exposure dry by the fire SU8 again and carry out the developing fixing processing, and last etching forms convex electrode part; (2) sputter nanometer dielectric material (HfO
2, SiO
2, TiO
2, Si
3N
4Or Ta
2O
5), spin coating and preceding baking PMMA resist adopt electron beam lithography, and etching is protruded the SiO on the bottom electrode
2, in acetone, soak then, remove the PMMA resist of remained on surface, the lower electrode material surface of exposing protrusion.(3) adopt the GeTe alloys target, perhaps simple substance Ge, Te target, and HfO
2The target magnetic control co-sputtering forms nano-composite phase-changing material film GeTe-HfO
2(4) sputter prepares upper electrode layer on the Semiconductor substrate that is formed with the nano-composite phase-changing material film; (5) the double-deck resist S6809 of spin coating, SU8, the exposure etching forms phase change memory unit structure.
Wherein, described Semiconductor substrate can be the silicon substrate of (100) orientation; The exposure method of the process using of described exposure etching is electron beam exposure, and lithographic method is reactive ion etching.
Description of drawings
Fig. 1 to Fig. 3 is preparation method's flow chart of phase transition storage of the present invention.
Fig. 4 is the XRD figure of nano-composite phase-changing material of the present invention.
Fig. 5 is the XPS figure of nano-composite phase-changing material of the present invention.
Fig. 6 keeps trying hard to for resistance and temperature relation, activation energy and the data of nano-composite phase-changing material of the present invention.
Fig. 7 is the current-voltage correlation figure of phase transition storage of the present invention.
Fig. 8 is the resistance voltage graph of a relation of phase transition storage of the present invention.
Embodiment
The present invention is described in detail below with reference to accompanying drawing.
Nano-composite phase-changing material of the present invention is that the phase-change material GeTe of 70-99% and dielectric material that molar percentage is 1-30% are formed by molar percentage.Described dielectric material is HfO
2, SiO
2, TiO
2, Si
3N
4Or Ta
2O
5In one or both and above above-mentioned dielectric material thereof mix altogether.For example, choosing dielectric material is HfO
2, wherein, in described nano-composite phase-changing material, phase-change material GeTe and dielectric material are uniformly dispersed in composite material, and described phase-change material GeTe is the nano-scale particle shape, and maximum gauge is less than 100 nanometers.The preparation method of described nano-composite phase-changing material can adopt semiconductor deposition process preparation, as in sputtering method, chemical vapour deposition technique, pulsed laser deposition method, sol-gel process or the ion implantation any, below to adopt GeTe alloys target and HfO
2It is that example illustrates that target two target magnetic controls spatter the nano combined phase-change thin film of formation altogether.
Clean the silicon substrate of (100) orientation; GeTe alloys target and HfO
2Target two target co-sputtering thin films, in the preparation process, the base vacuum degree is less than 2 * 10
-4Pa, sputtering pressure are 0.21Pa, and temperature is room temperature, and the DC power supply that is added on the GeTe alloys target is 20 watts, is added in HfO
2Radio-frequency power supply on the target is 60 watts, and sputtering time is 15 minutes, and deposit thickness is for being about 200 nanometers, GeTe and HfO
2Molar percentage be respectively 88 and 12mol%.
Phase transition storage of the present invention comprises at least: semiconductor substrate layer, the metal level as bottom electrode, insulating barrier, nano-composite phase-changing material layer and as the metal level of top electrode, wherein, the material of nano-composite phase-changing material layer employing is above-mentioned GeTe-HfO
2Composite material.In described nano-composite phase-changing material layer, phase-change material GeTe and dielectric material are (for example: HfO
2, SiO
2, TiO
2, Si
3N
4Or Ta
2O
5) be evenly distributed, phase-change material is the nano-scale particle shape, and the particle maximum gauge is less than 100 nanometers.
To shown in Figure 3, the preparation method of described phase transition storage is as follows as Fig. 1:
1) cleans the silicon substrate that (100) are orientated, on the silicon substrate 1 with chemical vapour deposition technique (CVD) prepare successively after about 250 nanometers metal level 2 (for example: tungsten, titanium, aluminium) and 20 nanometer transition zones (tantalum nitride or titanium nitride TiN) 3 as bottom electrode, spin coating and preceding baking SU8 resist, the recycling electron beam lithography, mark and the electrode structure of making mixed exposure, the back is dried by the fire SU8 and is carried out developing fixing and handle again, last etching forms convex electrode part, and structure as shown in Figure 1;
2) sputter 100 nanometer dielectric material (HfO
2, SiO
2, TiO
2, Si
3N
4Or Ta
2O
5) 4, preferred SiO
2Spin coating and preceding baking PMMA resist adopt electron beam lithography, and etching is protruded the SiO on the bottom electrode
2(or HfO
2, TiO
2, Si
3N
4Or Ta
2O
5, in acetone, soak then, remove the PMMA resist of remained on surface, the lower electrode material surface of exposing protrusion, structure is as shown in Figure 2.
3) adopt GeTe alloys target and HfO
2The target magnetic control co-sputtering forms nano-composite phase-changing material GeTe-HfO
2Film 5.The DC power supply that is added on the GeTe alloys target is 20 watts, is added in HfO
2Radio-frequency power supply on the target is 60 watts, and sputtering time is 7 minutes, and deposit thickness is for being about 90 nanometers, GeTe and HfO
2Molar percentage be respectively 88 and 12mol%.
4) on the Semiconductor substrate that is formed with the nano-composite phase-changing material film, prepare upper electrode layer successively, comprise the titanium nitride 3 (or tantalum nitride) of 20 nanometer thickness and the tungsten 2 of 300 nanometer thickness (or titanium, aluminium); The double-deck resist S6809 of spin coating, SU8, the exposure etching forms phase change memory unit structure, and the unit component structure is as shown in Figure 3.
The nano combined phase-change thin film that forms on the aforesaid semiconductor substrate and the PCM device of formation have been carried out every test, content measurement has: the XRD figure (Fig. 4) of described nano composite material, x-ray photoelectron general (XPS) figure (Fig. 5), the relation of resistance and temperature, activation energy and data are protected ability (Fig. 6), the electric current of phase change memory device unit and voltage relationship figure (Fig. 7), the graph of a relation of resistance and voltage (Fig. 8).Above-mentioned means of testing is used for the crystallization property of analysis of material, the state of oxidation of element in the phase-change material, the thermal stability of assessment material and data confining force, and the performance of device cell.
XRD collection of illustrative plates as shown in Figure 4, the crystallization temperature of GeTe are about about 190 degree, spend sufficient crystallising 250.With 5mol%HfO
2After compound, the crystallization temperature of film is improved: crystallization temperature is between 220 to 250 degree.HfO
2Content when increasing to 12mol%, the crystallization temperature of composite material is brought up between 250 to 280 degree.This shows GeTe and HfO
2After forming composite material, the stability of film be improved significantly.Because HfO
2Contain oxygen element in the target, element Ge and Te that may the oxidation phase-change material may cause the solute segregation of phase-change material like this.
Adopt XPS analysis, as shown in Figure 5, the oxidized peak of Ge and Te do not occur, this shows that Ge and Te can be not oxidized in preparation process.As shown in Figure 6, along with HfO
2The increase of content, the crystallization activation energy of composite material are increased to 4.69eV from 2.36, and 10 annual data confining forces are increased to 187 degree from 108.This has proved absolutely phase-change material GeTe and dielectric material HfO
2Carry out compound after, its thermal stability and data holding ability be improved significantly.HfO particularly
2Content is the GeTe-HfO of 12mol%
2, its 10 annual data keeps temperature to exceed 100 degree than the GST of present extensive use.10 annual datas of this superelevation keep temperature, make this material can be applied in the special occasions of high temperature storage, for example the memory of onboard system.
It can also be seen that GeTe-HfO from Fig. 6
2The crystalline resistance of composite material is along with HfO
2The increase of content and increasing.The increase of crystalline resistance is conducive to reducing of RESET electric current, and then helps the reduction of device power consumption.As shown in Figure 7 device cell electric current and voltage relationship, when electric current was increased to threshold current, the voltage at device cell two ends sharply reduced, and the threshold value upset has namely taken place.This illustrates GeTe-HfO
2The memory device of Composite Preparation possesses the phase change memory ability.
Fig. 8 is composite material GeTe-HfO
2Concern comparison diagram with the resistance voltage of GST.GeTe-HfO as can be seen
2Can realize under 20 nanoseconds that " wiping " " write " operation, but crystalline resistance is bigger, this is because there is not complete crystallization.Under 100 nanoseconds, can realize stablizing " wiping " and " write " operation.And GST also can realize that " wiping " " write " 100 nanoseconds, but if stable operation, the required voltage pulse duration was at least for 500 nanoseconds.Therefore, composite material GeTe-HfO
2It is littler than GST to realize that stable " wiping " " writes " the required minimum pulse width of operation, thereby phase velocity is faster than GST.It can also be seen that GST is little for the RESET voltage ratio, thereby power consumption is littler than GST.
Composite phase-change material GeTe-HfO of the present invention
2, by dielectric material HfO
2The nanometer frame structure that forms helps to improve the thermal stability of material and reduces power consumption.One, suppress to be evenly distributed on the crystallization of the phase-change material GeTe of this frame structure, improved the crystallization temperature of material, improved thermal stability.Its two because HfO
2Obstruction, make grain growth be restricted, crystal grain diminishes.A large amount of crystal boundaries of Yin Ruing make the thermal conductivity of composite material reduce thus, and thermal loss reduces in the device operation process, is conducive to the reduction of device power consumption.Three, HfO
2Introducing improved dielectric constant and the crystalline resistance of material, be conducive to the further reduction with power consumption of reducing of device threshold voltage.Four, because dielectric material HfO
2Participation, make effective programming volume to reduce, thereby reduced the change in volume before and after the phase change cells crystallization and reduced the RESET electric current that this helps the stability of memory device operation and realizes low-power consumption.In a word, this novel nano composite phase-change film is applied in the memory, and the RESET voltage of phase change memory device is reduced, programming volume reduces, and is conducive to realize the high density storage, the efficiency of heating surface in the programming process of raising phase transition storage, reduce its power consumption, promote data holding ability etc.
In sum, nano-composite phase-changing material of the present invention is by with GeTe phase-change material and HfO
2Compound, can improve thermal stability and the data holding ability of material.By its phase transition storage that constitutes, performances such as the power consumption of device, operational stability, document properties and program speed are all promoted.
Above-described embodiment just lists expressivity principle of the present invention and effect is described, but not is used for restriction the present invention.Any personnel that are familiar with this technology all can make amendment to above-described embodiment under spirit of the present invention and scope.Therefore, the scope of the present invention should be listed as claims.
Claims (4)
1. nano-composite phase-changing material is characterized in that comprising:
Molar percentage is the phase-change material GeTe of 70-99%, and molar percentage is the dielectric material HfO of 1-30%
2Described phase-change material GeTe and dielectric material HfO
2In the nanoscale scope, evenly disperse, and HfO
2In the element of oxygen in can oxidation GeTe; Described phase-change material GeTe is the nano-scale particle shape in this composite phase-change material, the largest particles diameter is less than 100 nanometers.
2. the preparation method of a nano-composite phase-changing material is characterized in that, adopts GeTe alloys target and HfO
2Target two target magnetic controls spatter altogether or adopt simple substance Ge target, Te target and HfO
2The method that three target magnetic controls spatter altogether;
During sputter, the base vacuum degree is less than 2 * 10
-4Pa, sputtering pressure are 0.18-0.25Pa, and temperature is room temperature, and the DC power supply that is added on the GeTe alloys target is 10-60 watt, and the direct current power that is added on simple substance Ge target and the Te target is 10-60 watt, is added in HfO
2Radio-frequency power supply on the target is 10-80 watt, and sputtering time is 5-60 minute, and deposit thickness is the 50-300 nanometer.
3. method for preparing phase transition storage is characterized in that comprising step:
I. on Semiconductor substrate successively sputter prepare bottom electrode, described bottom electrode comprises metal electrode layer and is positioned at transition zone on the metal electrode layer that etching forms convex electrode part;
Ii. the dielectric material of sputter nanometer then, etching protrudes from the nanometer dielectric material on the bottom electrode;
Iii. adopt the GeTe alloys target, perhaps simple substance Ge, Te target and HfO
2The target magnetic control co-sputtering forms nano-composite phase-changing material film GeTe-HfO
2, described nano-composite phase-changing material is that molar percentage is the phase-change material GeTe of 70-99% and the dielectric material HfO that molar percentage is 1-30%
2Form;
Iv. step (iii) on the nano-composite phase-changing material film on the Semiconductor substrate that obtains of back successively sputter prepare upper electrode layer; Described top electrode comprises metal electrode layer and the transition zone that is positioned on the metal electrode layer;
V. last, the exposure etching forms phase change memory unit structure.
4. the method for preparing phase transition storage as claimed in claim 3, it is characterized in that: the exposure method of the process using of described exposure etching is electron beam exposure, lithographic method is reactive ion etching.
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| CN101106176A (en) * | 2006-07-12 | 2008-01-16 | 旺宏电子股份有限公司 | Method for making a pillar-type phase change memory element |
| CN101276617A (en) * | 2007-03-26 | 2008-10-01 | 光洋应用材料科技股份有限公司 | Composite type phase variation recording thin film as well as target material and method for manufacturing the thin film |
| CN101660118A (en) * | 2009-09-10 | 2010-03-03 | 中国科学院上海微系统与信息技术研究所 | Nanometer composite phase-change material, preparation and application thereof |
| CN101752497A (en) * | 2009-12-15 | 2010-06-23 | 中国科学院上海微系统与信息技术研究所 | Phase-change storage unit with low power consumption and high stability and preparation method thereof |
| CN101783391A (en) * | 2010-02-04 | 2010-07-21 | 中国科学院上海微系统与信息技术研究所 | Nano-composite phase change material, preparation method thereof and application thereof as phase change memory |
| CN101818294A (en) * | 2010-04-28 | 2010-09-01 | 中国科学院上海微系统与信息技术研究所 | Nanometer composite phase-change material, preparation method and optimization method |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101106176A (en) * | 2006-07-12 | 2008-01-16 | 旺宏电子股份有限公司 | Method for making a pillar-type phase change memory element |
| CN101276617A (en) * | 2007-03-26 | 2008-10-01 | 光洋应用材料科技股份有限公司 | Composite type phase variation recording thin film as well as target material and method for manufacturing the thin film |
| CN101660118A (en) * | 2009-09-10 | 2010-03-03 | 中国科学院上海微系统与信息技术研究所 | Nanometer composite phase-change material, preparation and application thereof |
| CN101752497A (en) * | 2009-12-15 | 2010-06-23 | 中国科学院上海微系统与信息技术研究所 | Phase-change storage unit with low power consumption and high stability and preparation method thereof |
| CN101783391A (en) * | 2010-02-04 | 2010-07-21 | 中国科学院上海微系统与信息技术研究所 | Nano-composite phase change material, preparation method thereof and application thereof as phase change memory |
| CN101818294A (en) * | 2010-04-28 | 2010-09-01 | 中国科学院上海微系统与信息技术研究所 | Nanometer composite phase-change material, preparation method and optimization method |
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