CN102011089B - Method for preparing nanocrystalline resistance conversion material - Google Patents
Method for preparing nanocrystalline resistance conversion material Download PDFInfo
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Abstract
The invention discloses a method for preparing a nanocrystalline resistance conversion material and a unit, which comprises the steps of: firstly, depositing an ultrathin resistance conversion storage material film; secondly, forming a uniform nanocrystalline on a base through annealing; thirdly, forming the covering of the nanocrystalline through the deposition of a functional material; fourthly, repeating the three steps to form a uniform nanocrystalline resistance conversion storage material and the unit covered by the functional material. The method for preparing the nanocrystalline resistance conversion storage material can be used in a nanocrystalline resistance conversion storage, and solves the difficulty that the uniform nanocrystalline storage material can not be prepared. The invention can greatly improve the property of the storage and enhance the reliability of elements.
Description
Technical field
The invention belongs to technical field of semiconductors, relate to a kind of nanocrystalline resistance conversion material, relate in particular to a kind of method for preparing nanocrystalline resistance conversion material.
Background technology
Electric resistance transition memory is the candidate of the most very powerful and exceedingly arrogant current nonvolatile semiconductor memory of future generation, has wide market outlook, and has realized the commercial application of short run.Main electric resistance transition memory mainly is divided into two classes, the one, phase transition storage, the 2nd, resistance random access memory now.The former principle be based upon in the device phase change material realize under the effect of electrical signal in the transformation between amorphous and the polycrystalline, the transformation of material crystals structure has caused the change of resistance, and phase transition storage is exactly to utilize the low-resistance difference of this height to realize the storage of logical data.And the latter's principle is to be based upon in the electricity conversion of some strong associated material, also is to utilize the modulation of device resistance to carry out the data storage.In addition, giant magnetoresistive memory also is to be based upon in the change of resistance, also can be described as a kind of of electric resistance transition memory.
In traditional phase transition storage, the phase change material of device inside realizes that storage medium changes uniformly under the effect of electrical signal, and is namely substantially even at the regional composition of phase change material of amorphous that device inside produced and existed and polycrystalline.Chinese invention patent CN201010127277.2 (contriver: Zhang Ting etc., " resistance memory device ") in, a kind of novel nanocrystalline electric resistance transition memory has been proposed, its principle is to be based upon in the change that has a resistance of material internal nanocrystalline material, be with the difference of phase transition storage, when this device carries out logic inversion, in the storage medium, the material component of part or the transformation that particle participates in resistance are only arranged, remaining " functional materials " part then keeps stablizing constant, and what play is the effect of isolation and framework.The principle of this nanocrystalline electric resistance transition memory is obviously also also far from each other with resistance random access memory, be in particular in the process of resistance conversion, there is the material component of at least two different groups always in composite distribution and inhomogeneous in the former, so is a kind of new storage principle.
The difficult point of making nanocrystalline electric resistance transition memory is to prepare the method for uniform nanocrystalline storage medium, nanocrystalline material obviously can significantly promote the performance of storer uniformly, increases device reliability, yet, current, prepare uniform nano-crystal film and remain a difficult problem.
Summary of the invention
Technical problem to be solved by this invention is: a kind of method for preparing nanocrystalline resistance conversion material is provided, has solved the difficult problem that can't prepare the brilliant storage medium of even.
For solving the problems of the technologies described above, the present invention adopts following technical scheme:
A kind of method for preparing nanocrystalline resistance conversion material comprises following steps:
A, deposit thickness are less than the material ultrathin film with resistance transition function of 10nm;
B, employing annealing in vacuum chamber form the nano-crystalline granule that has uniformly memory function by reuniting effect;
C, deposition coating material are coated on the nano-crystalline granule surface with memory function equably;
D, repeating step A until obtain enough thickness, prepare uniform nanocrystalline resistance conversion material to step C.
As a preferred embodiment of the present invention, describedly prepare the change that the nanocrystalline resistance conversion material that obtains in the method for nanocrystalline resistance conversion material can be realized in the effect of electrical signal resistivity of material, the nano-crystalline granule that has memory function in the described material needs encapsulated material to separate equably.The resistivity that the nano particle that has uniformly memory function that forms can change under the effect of electrical signal, coating material then under the electrical signal effect resistivity remain unchanged.Nano-crystalline granule with memory function can be the phase change material particle, or resistor random-access storage medium particle, or the stibium containing material particle.
As a preferred embodiment of the present invention, described coating material is insulating material, or is semiconductor material, or is metal-containing material.That adopts is annealed into short annealing, and annealing is carried out in a vacuum.The size of the nano-crystalline granule with memory function that forms is the spheroid of 30nm less than diameter.The method of deposition storage medium and coating material ultrathin film is vapour deposition process, or is the physical deposition method, or is atomic layer deposition method.
A kind of method for preparing nanocrystalline resistance conversion material, comprise following steps: alternating growth storage medium and functional materials thin layer, after thin film deposition is finished, adopt annealing to obtain nanocrystalline storage medium, the thickness of the storage medium thin layer that thin film deposition obtains is less than 20nm, and the functional materials thickness of thin layer is less than 10nm.
As a preferred embodiment of the present invention, the described nanocrystalline resistance conversion material that obtains in the method for nanocrystalline resistance conversion material of preparing can be in the conversion of resistivity between high and low value that realizes material under the effect of electrical signal.Nanocrystalline storage particle can be phase change material, or is the resistor random-access storage medium, or is the stibium containing material material.The conversion phenomena of coating material non-resistance under the effect of electrical signal, these functional materialss are insulating material, or are semiconductor material, or are metal-containing material.The size of the nanometer storing particle that forms is less than 30nm.Can adopt dissimilar resistance transition material and functional materials in the technique, also can deposit resistance transition material and the functional materials of different thickness, can also have multiple resistance transition material and several functions material in the nanocrystalline resistance conversion material that namely prepares at the same time.
A kind of method for preparing nanocrystalline resistance conversion material comprises following steps:
The storage medium ultrathin film that A1, deposition have the resistance transition function, film thickness is less than 15nm;
B1, in the atmosphere of the gas with reaction, anneal, by the acting in conjunction of annealing reaction and reuniting effect, form when having the nano-crystalline granule of memory function, form reactant as coating layer on the surface of nano-crystalline granule;
C1, repeating step A1 until obtain abundant thickness, prepare uniform nanocrystalline resistance conversion material to step B1.
As a preferred embodiment of the present invention, in the described method for preparing nanocrystalline resistance conversion material, nanocrystalline resistance conversion material can be in the conversion of resistivity between high and low value that realizes material under the effect of electrical signal.Nano particle with memory function is the phase change material particle, or is resistor random-access storage medium particle, or is the stibium containing material particle.The conversion phenomena of the coating material that annealing reaction obtains non-resistance under the effect of electrical signal, these materials are insulating material, are semiconductor material, are metal-containing material.That adopts is annealed into short annealing.The size of the nano particle with memory function that forms is the spheroid of 30nm less than diameter.The nano particle with memory function that technique obtains can be in the conversion that is implemented under the effect of electrical signal between the high resistance and low resistance rate.It is to show that nanocrystalline face forms reactant and obtains by annealing that the present invention is coated on nanocrystalline outer coating layer.
Beneficial effect of the present invention is: the processing method of the nanocrystalline resistance conversion storage material of preparation that the present invention proposes, can be used for nanocrystalline electric resistance transition memory, and solution can't prepare the difficult problem of the brilliant storage medium of even.Nanocrystalline being applied in the memory device can significantly promote the performance of storer, increases device reliability, and therefore, the present invention is remarkable for the lifting meaning of memory performance.
Description of drawings
Figure 1A-Fig. 1 G is the schema of preparation nanocrystalline resistance conversion material method.
Fig. 2 A-Fig. 2 B is the schema of another kind of preparation nanocrystalline resistance conversion material method.
Embodiment
Describe the preferred embodiments of the present invention in detail below in conjunction with accompanying drawing.
Embodiment one
The present invention discloses a kind of method for preparing nanocrystalline resistance conversion material, and the method comprises and comprises following steps:
(1) at first pass through PVD sediment phase change material Sb-Te film 2 (shown in Figure 1A) in the substrate 1 with electrode, characteristics are phase change material film thickness ultrathins of deposition, are no more than 10nm, and typical thickness is 1nm, 2nm, 3nm and 5nm etc.Obviously the phase change material Sb-Te film that adopts can be the phase change material of other any type, also can be the resistance conversion storage material of other type, need to point out especially at this.
(2) in a vacuum, carry out short annealing, because the reuniting effect that causes of annealing, can form the nano particle 3 of phase change material Sb-Te on the surface of substrate, its sectional view and vertical view are respectively shown in Figure 1B and 1C.Studies show that phase change material is after annealing under the temperature near temperature of fusion, material can have reunion in substrate, thereby forms nano-crystalline granule.In addition, the selection of substrate is most important for nanocrystalline formation, does not repeat them here.The Sb-Te nano-crystalline granule that forms also possesses the ability of resistance conversion.
(3) adopt PECVD method (perhaps ALD) in another chamber, to deposit Si:H, typical thickness is 1-3nm, surface at above-mentioned nano particle has just coated Si:H thin layer 4, shown in Fig. 1 D, the Si:H thin layer is coating layer in this case, because the restriction of coating layer, the activity meeting of nanocrystal correspondingly is limited in the less scope, and stop nanocrystalline between possible reunion.Be similar to the nanocrystalline difference of the material of Si:H thin layer and Sb-Te and be that these materials do not possess the ability of resistance conversion, are a kind of stable materials, because the coating river of Si:H book layer disperses, make the component of material internal no longer even.
(4) continue sediment phase change material Sb-Te, repeat above-mentioned step (1) to (3) step, can form the structure shown in Fig. 1 E-1G, until obtain enough thickness, formed needed uniform nanocrystalline structure, this material can under the effect of electrical signal, be realized the conversion of material between high resistance and low resistance.
Present embodiment adopts in a vacuum, deposition material across, the reuniting effect that adopts annealing to introduce between the two step deposition process forms nano-crystalline granule, adopt a kind of stable functional materials coating layer to separate the nano particle of phase change material, form equally distributed nanocrystalline storage medium, have great importance for the application of nano-crystal memory spare.Only need two deposition of material cavitys and an anneal chamber in the technique, realize in a vacuum the sample transmission, have very high preparation efficiency, avoid the complicated component alloy target material that adopts cost higher, and obtain more uniform nanocrystalline storage medium, have obvious competitive power.
Embodiment two
Present embodiment discloses a kind of method for preparing nanocrystalline resistance conversion material, and the method comprises and comprises following steps:
(1) sediment phase change material Si-Sb-Te in the substrate with electrode at first.
(2) carry out short annealing, atmosphere is oxygen (or oxygenous atmosphere), under the promotion of annealing, form the nano particle of phase change material Si-Sb-Te on the surface of substrate, in addition because the reason of atmosphere, also can produce oxidizing reaction on the surface of nano particle and form silicon oxide (because silicon has stronger electronegativity, so can preferentially react with oxygen, thereby form thin layer of silicon oxide at particle surface, in the suitable situation of oxidation, Sb and Te can oxidations).
(3) continue sediment phase change material Si-Sb-Te, repeating step (1) is to (2) step, until obtain enough thickness, formed needed uniform nanocrystalline structure, this material can be under the effect of electrical signal, realize the conversion of material between high resistance and low resistance, thereby realize the data storage function.
Obviously the reaction atmosphere that adopts also can be the reactant gases of nitrogen or other any type, and source material also is not limited to Si-Sb-Te, does not just particularly point out at this.The benefit of this method is, only needs a kind of deposition of material, and follow-up coating layer obtains by annealing reaction, and technique is more simple.
Embodiment three
Present embodiment discloses a kind of method for preparing nanocrystalline resistance conversion material, and the method comprises and comprises following steps:
(1) the metal Ni film of depositing ultrathin in substrate at first, thickness is 3nm, typical thickness can also be 0.5nm in addition, 1nm and 4.5nm etc.
(2) carry out short annealing, atmosphere is oxygen, because the effect of annealing and reaction forms the NiO nano particle on the surface of substrate, these nano particles can be realized the counter-rotating of resistance under the effect of electrical signal.
(3) adopt physical deposition method deposited amorphous Si in another chamber, just coated amorphous Si thin layer on the surface of above-mentioned nano particle.
(4) continue metal refining Ni, repeating step (1) goes on foot to (3), until obtain enough thickness, and formed uniform nanocrystalline structure.
The coating layer amorphous Si of deposition obviously also can be other dielectric material, such as silicon oxide and silicon nitride etc., only require that these isolated materials do not possess the ability that realizes the resistance conversion under the electrical signal effect, yet, through peroxidation, Ni has formed NiO, and the nano particles such as NiO then can be implemented in the conversion between the high resistance and low resistance under the effect of electrical signal, and the principle of the data storage of storer is also originally in this.Obviously, described NiO also can replace with other the materials such as metal oxide as storage media, and for example Tungsten oxide 99.999 and cupric oxide are the metal oxide of representative, needn't give unnecessary details at this.
Embodiment four
Present embodiment discloses a kind of method for preparing nanocrystalline resistance conversion material, and the method comprises and comprises following steps:
(1) deposit thickness is the Si of 2nm in the substrate with electrode.
(2) deposit thickness is the Sb of 5nm.
(3) repeating step (1) is to (2) step, until obtain enough thickness.
(4) annealing, atmosphere are to anneal in the protective atmosphere of high pure nitrogen, obtain nanocrystalline material, and nanocrystalline material mainly relies on the non-crystalline silicon between Sb and the Sb to separate, and possess the storage capacity of resistance conversion.
Demonstrating a kind of successive sedimentation film at last by the together growth of annealing realization nano-crystal film at this, it may be noted that at this this scheme is not limited to Si and Sb, is can be the material of other any type.After thin film deposition and annealing, the inside of film will form the nano particle that is coated by certain material, possesses the ability of resistive memory.
Embodiment five
See also Fig. 2 A, Fig. 2 B, present embodiment discloses a kind of method for preparing nanocrystalline resistance conversion material, and the method comprises and comprises following steps:
(1) with reference to figure 2A, deposit thickness is the Si layer 11 of 3nm in the substrate having.
(2) deposit thickness is the Sb-Te layer 12 of 3nm.
(3) continuing deposit thickness is the Si layer 13 of 5nm.
(4) deposit thickness is the Sb-Te layer 14 of 5nm.
(5) deposit thickness is the Si layer 15 of 2nm.
(6) deposit thickness is the Sb-Te layer 16 of 8nm.
(7) deposit thickness is the Si layer 17 of 3nm.
(8) deposit thickness is the Sb-Te layer 18 of 7nm.
(9) deposit thickness is the Si layer 19 of 4nm.
(10) annealing, atmosphere is nitrogen atmosphere protection, obtains nanocrystalline material; shown in Fig. 2 B, annealed after, corresponding amorphous silicon layer remains unchanged substantially; and between the Sb-Te layer, formed nanocrystallinely 20, separated by the coating zone 21 of formation after diffusion between nanocrystalline.
Present case will illustrate, in the multilayered structure, can adopt isolated material and the nanocrystalline material of different sorts and different thickness, and the thickness that adopts between each layer does not need identical.
Embodiment six
Present embodiment discloses a kind of method for preparing nanocrystalline resistance conversion material, and the method comprises and comprises following steps:
(1) deposit thickness is the Si of 1nm in the substrate with electrode.
(2) deposit thickness is the Sb-Te of 2nm.
(3) deposit thickness is the Si of 2nm in the substrate with electrode.
(4) deposit thickness is the Ge-Sb-Te of 3nm.
(5) deposit thickness is the SiO of 2nm in the substrate with electrode
2
(6) deposit thickness is the SiSb of 3nm.
(7) continue metal refining Ni, repeating step (1) is to (6) step, until obtain enough thickness.
(8) annealing, atmosphere is nitrogen atmosphere protection, obtains nanocrystalline material.
Present embodiment will illustrate, in the multilayered structure, can adopt isolated material and the nanocrystalline material of different sorts and different thickness, and the thickness or even the material that adopt between each layer do not need identical.
In sum, the processing method of the nanocrystalline resistance conversion storage material of preparation that the present invention proposes can be used for nanocrystalline electric resistance transition memory, and solution can't prepare the difficult problem of the brilliant storage medium of even.If the present invention is applied in electric resistance transition memory, the storer that manufacturing obtains can significantly promote the performance of storer than current memory device, increases device reliability.
Here description of the invention and application is illustrative, is not to want with scope restriction of the present invention in the above-described embodiments.Here the distortion of disclosed embodiment and change is possible, and the various parts of the replacement of embodiment and equivalence are known for those those of ordinary skill in the art.Those skilled in the art are noted that in the situation that does not break away from spirit of the present invention or essential characteristic, and the present invention can be with other form, structure, layout, ratio, and realize with other assembly, material and parts.In the situation that does not break away from the scope of the invention and spirit, can carry out other distortion and change to disclosed embodiment here.
Claims (16)
1. a method for preparing nanocrystalline resistance conversion material is characterized in that, described method comprises the steps:
A, deposit thickness be less than the ultrathin film with resistance converting function material of 10nm, i.e. sediment phase change material film in the substrate with electrode at first, and the phase change material film thickness of deposition is no more than 10nm;
B, in vacuum chamber, adopt annealing, form the nano-crystalline granule that has uniformly memory function by reuniting effect, namely in a vacuum, carry out short annealing, because the reuniting effect that annealing causes, can form the nano particle of phase change material on the surface of substrate; The nano particle that forms possesses the ability of resistance conversion;
C, deposition coating material are coated on the nano grain surface with memory function equably, namely deposit coating material, and the thickness of coating material is 0.2-5nm, has just coated the coating material thin layer on the surface of above-mentioned nano particle; Described coating material thin layer is coating layer because the restriction of coating layer, in the activity meeting of nano particle correspondingly is limited among a small circle, and stop nanocrystalline between possible reunion;
D, repeating step A until obtain enough thickness, have formed needed uniform nanocrystalline structure to step C, and this material can under the effect of electrical signal, be realized the conversion of material between high resistance and low resistance.
2. the method for preparing nanocrystalline resistance conversion material according to claim 1 is characterized in that:
Described nanocrystalline resistance conversion material can be realized in the effect of electrical signal the change of resistivity.
3. the method for preparing nanocrystalline resistance conversion material according to claim 1 is characterized in that:
The nano particle encapsulated material that has memory function in the described resistance transition material is separated equably.
4. the method for preparing nanocrystalline resistance conversion material according to claim 1 is characterized in that:
Described nano particle with memory function can change nanocrystalline resistivity under the effect of electrical signal.
5. the method for preparing nanocrystalline resistance conversion material according to claim 1 is characterized in that:
Described nano particle with memory function is the phase change material particle, or is resistor random-access storage medium particle, or is the stibium containing material particle.
6. the method for preparing nanocrystalline resistance conversion material according to claim 1 is characterized in that:
Coating material among the described step C is the non-resistance conversion phenomena under the effect of electrical signal.
7. it is characterized in that according to claim 1 or the 6 described methods that prepare nanocrystalline resistance conversion material:
Described coating material is insulating material, or is semiconductor material, or is metal-containing material.
8. the method for preparing nanocrystalline resistance conversion material according to claim 1 is characterized in that:
The nano particle with memory function that forms among the described step B is that diameter is less than the spheroid of 30nm.
9. the method for preparing nanocrystalline resistance conversion material according to claim 1 is characterized in that:
The method of deposition coating material and storage medium is vapour deposition process among the described step C, or is the physical deposition method, or is atomic layer deposition method.
10. method for preparing nanocrystalline resistance conversion material comprises following steps:
A1, at the storage medium ultrathin film that the substrate deposition with electrode has the resistance transition function, film thickness is less than 15nm;
B1, be short annealing in the oxygen in atmosphere, by the acting in conjunction of annealing reaction and reuniting effect, the surface of substrate form have the nano particle of memory function in, form reactant as coating layer on the surface of nano particle;
C1, repeating step A1 until obtain enough thickness, have formed needed uniform nanocrystalline structure to step B1, and this material can be realized the conversion of material between high resistance and low resistance under the effect of electrical signal, thereby realizes the data storage function.
11. the method for preparing nanocrystalline resistance conversion material according to claim 10 is characterized in that:
Described nanocrystalline resistance conversion material can be in the conversion of resistivity between high and low value that realizes material under the effect of electrical signal.
12. the method for preparing nanocrystalline resistance conversion material according to claim 10 is characterized in that:
Described nano particle with memory function is the phase change material particle, or is resistor random-access storage medium particle, or is the stibium containing material particle.
13. the method for preparing nanocrystalline resistance conversion material according to claim 10 is characterized in that:
The conversion phenomena of the coating material that described annealing reaction obtains non-resistance under the effect of electrical signal.
14. the method for preparing nanocrystalline resistance conversion material according to claim 10 is characterized in that:
Described coating material is insulating material, or is semiconductor material, or is metal-containing material.
15. the method for preparing nanocrystalline resistance conversion material according to claim 10 is characterized in that:
The nano particle with memory function of described formation is that diameter is less than the spheroid of 30nm.
16. the method for preparing nanocrystalline resistance conversion material according to claim 10 is characterized in that:
The nano particle with memory function that described method obtains can be in the conversion that is implemented under the effect of electrical signal between the high resistance and low resistance rate.
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| CN103022346B (en) * | 2011-09-27 | 2014-09-10 | 华邦电子股份有限公司 | Resistance-type memorizer |
| CN103996790B (en) * | 2014-05-28 | 2016-10-05 | 河北大学 | A kind of nanoscale tri-state resistance-variable storing device and preparation method thereof |
| CN108682739A (en) * | 2018-05-03 | 2018-10-19 | 五邑大学 | A kind of metal quantum point enhancing ZnO resistive memories and preparation method thereof |
| CN111142304B (en) * | 2019-12-25 | 2022-10-14 | 宁波祢若电子科技有限公司 | All-solid-state electrochromic device and manufacturing method thereof |
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| CN1327581A (en) * | 1999-10-04 | 2001-12-19 | 皇家菲利浦电子有限公司 | Optical recording medium comprising a gesbte recording layer |
| CN101299453A (en) * | 2008-06-13 | 2008-11-05 | 中国科学院上海微系统与信息技术研究所 | Nano composite phase-changing material and preparation method thereof |
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| CN1327581A (en) * | 1999-10-04 | 2001-12-19 | 皇家菲利浦电子有限公司 | Optical recording medium comprising a gesbte recording layer |
| CN101299453A (en) * | 2008-06-13 | 2008-11-05 | 中国科学院上海微系统与信息技术研究所 | Nano composite phase-changing material and preparation method thereof |
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