CN116471920A - High-purity graphite doped nano phase change film and application thereof - Google Patents
High-purity graphite doped nano phase change film and application thereof Download PDFInfo
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- 230000008859 change Effects 0.000 title claims abstract description 68
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 27
- 229910002804 graphite Inorganic materials 0.000 title claims abstract description 21
- 239000010439 graphite Substances 0.000 title claims abstract description 21
- 229910052714 tellurium Inorganic materials 0.000 claims abstract description 17
- 229910052787 antimony Inorganic materials 0.000 claims abstract description 8
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229910052732 germanium Inorganic materials 0.000 claims abstract description 8
- PORWMNRCUJJQNO-UHFFFAOYSA-N tellurium atom Chemical compound [Te] PORWMNRCUJJQNO-UHFFFAOYSA-N 0.000 claims abstract description 8
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000000126 substance Substances 0.000 claims abstract description 5
- 239000010408 film Substances 0.000 claims description 66
- 238000010438 heat treatment Methods 0.000 claims description 13
- 239000000758 substrate Substances 0.000 claims description 12
- 239000010409 thin film Substances 0.000 claims description 12
- 238000000034 method Methods 0.000 claims description 10
- 238000004544 sputter deposition Methods 0.000 claims description 10
- 239000004642 Polyimide Substances 0.000 claims description 8
- 239000002184 metal Substances 0.000 claims description 8
- 229920001721 polyimide Polymers 0.000 claims description 8
- 230000002441 reversible effect Effects 0.000 claims description 8
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- 238000001755 magnetron sputter deposition Methods 0.000 claims description 3
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- 229910002056 binary alloy Inorganic materials 0.000 claims description 2
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- 239000000463 material Substances 0.000 description 10
- 238000002360 preparation method Methods 0.000 description 9
- 230000007704 transition Effects 0.000 description 5
- 230000008569 process Effects 0.000 description 4
- 230000009286 beneficial effect Effects 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 238000003860 storage Methods 0.000 description 3
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 238000000605 extraction Methods 0.000 description 2
- 230000002829 reductive effect Effects 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
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Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y10/00—Nanotechnology for information processing, storage or transmission, e.g. quantum computing or single electron logic
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02D—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN INFORMATION AND COMMUNICATION TECHNOLOGIES [ICT], I.E. INFORMATION AND COMMUNICATION TECHNOLOGIES AIMING AT THE REDUCTION OF THEIR OWN ENERGY USE
- Y02D10/00—Energy efficient computing, e.g. low power processors, power management or thermal management
Abstract
The invention discloses a high-purity graphite doped nano phase change film and application thereof. The nano phase-change film comprises graphite and at least one of germanium, antimony and tellurium, and has a chemical formula Gr x (Ge z Sb m Te n ) y Wherein 0 is<x≤0.5，0.5<y is less than or equal to 1, and x+y=1; z is more than or equal to 0 and less than or equal to 1, m is more than or equal to 0 and less than or equal to 1, and n is more than or equal to 0 and less than or equal to 1. Compared with pure Ge-Sb-Te or Sb-Te and Ge-Te, the invention has higher thermal stability, higher phase change speed, stronger data retention and lower density change rate, and particularly has lower resistance drift. By adjusting Gr x (Ge z Sb m Te n ) y The invention can obtain the heat stability, data retention, crystallization speed, density change rate and grain sizeThe nanometer phase change film with more optimized resistance drift characteristics is used for phase change memories and artificial nerve synapses.
Description
Technical Field
The invention relates toAnd a novel nano phase-change film with high speed, high data retention and low resistance drift, and a preparation method and application thereof, in particular to Gr x (Ge z Sb m Te n ) y Nano phase change film based on Gr x (Ge z Sb m Te n ) y A flexible phase change memory device of nano phase change film and a preparation method thereof belong to the technical field of microelectronics.
Background
Phase change memory (Phase Change Memory, PCM) is a new type of nonvolatile semiconductor memory based on resistive memory that is different from existing silicon-based charge memories. Compared with the existing various semiconductor memory technologies, the memory has the advantages of good contractibility, high-speed erasing and writing, low power consumption, high density, simple manufacturing process and the like, is hopeful to become one of the next generation nonvolatile mainstream memory technologies, and has wide application potential and market prospect.
The principle of the phase change memory is that the nano phase change film is reversibly changed between crystalline state (low resistance) and amorphous state (high resistance) by utilizing the Joule heat generated by electric pulse to realize the writing and erasing of data, and the reading of the data is realized by measuring the state of the resistance. The core of the phase change memory is a phase change memory medium material, and a common nano phase change film system is mainly a Ge-Sb-Te (expressed by abbreviation GST) system material, but the following problems still exist: 1. the crystallization temperature is low, and the danger of data loss is faced, so that the application field is restricted; 2. the grain size is larger, which is not beneficial to reducing the power consumption of the device and inhibiting the drift of the resistance value; 3. the thermal stability is poor, and the data retention is not guaranteed; 4. the volume change before and after phase change is too large, which is unfavorable for the reliability of the device; 5. the phase change speed is to be further improved, and researches show that the electric pulse for realizing stable RESET operation of the phase change memory based on GST is at least 50 nanoseconds, and the requirement of faster speed cannot be met.
Therefore, the novel nano phase change film which has the advantages of high operation speed, good stability, strong data retention, small density change and resistance drift and is compatible with the CMOS technology is sought, and the problem to be solved in the current PCM technical field is solved.
Disclosure of Invention
The technical problems to be solved by the invention are as follows: providing Gr x (Ge z Sb m Te n ) y The nano phase-change film, the phase-change memory device and the preparation method thereof are used for solving the problems of poor stability and data retention, low phase-change speed, large resistance drift, large density change and the like of the nano phase-change film in the prior art.
In order to solve the problems, the invention provides a high-purity Graphite doped nano phase-change film, which comprises a combination of Graphite (Gr) and at least one of three elements of germanium (Ge), antimony (Sb) and tellurium (Te), wherein the chemical formula of the nano phase-change film is Gr x (Ge z Sb m Te n ) y Wherein 0 is<x≤0.5，0.5<y is less than or equal to 1, and x+y=1; z is more than or equal to 0 and less than or equal to 1, m is more than or equal to 0 and less than or equal to 1, and n is more than or equal to 0 and less than or equal to 1.
Preferably, the nano phase-change film has at least two stable resistance states under the action of electric pulse to realize multiple resistance states.
More preferably, in the multi-resistance state, the resistance value of the high-resistance state is 10 5 -10 7 Between ohms, the low resistance state has a resistance value of 10 3 -10 5 Between ohms, when there are more than two stable resistance states, the resistance value of the intermediate resistance state is 10 4 -10 6 Between ohms.
Preferably, the nano phase-change film can realize the rapid and reversible phase change between an amorphous state and a crystalline state under the operation of electric pulse so as to achieve the purpose of mutually converting high and low resistance values and storing information, and the resistance value is kept unchanged under the operation without an electric pulse signal.
Preferably, the thickness of the nano phase-change film is between 2nm and 200 nm.
Preferably, the nano phase-change film is easy to form multi-layer heterogeneous phase-change structures with different periods, wherein the thickness of the sub-layer is between 2nm and 10nm, multi-dimensional limiting crystallization and phase change are realized, the grain size is reduced, the grain size uniformity is improved, and the resistance drift is reduced.
The invention can be prepared by using methods such as multi-target co-sputtering, simple substance alloy target sputtering, magnetron sputtering, pulse laser deposition, electron beam evaporation or atomic layer deposition.
The invention also provides a phase-change memory device, which comprises a heating electrode layer, a top electrode layer and a nano phase-change film layer positioned between the heating electrode layer and the top electrode layer, wherein the nano phase-change film layer comprises the nano phase-change film.
Preferably, the phase change memory device is disposed on a flexible substrate, and the flexible substrate includes at least one of a metal sheet, a metal foil paper, ultra-thin glass, PET, and Polyimide (PI).
The invention also provides a preparation method of the phase-change memory device, which comprises the following steps:
step 1): preparing a heating electrode layer;
step 2): preparing a nano phase-change thin film layer on the heating electrode layer, wherein the nano phase-change thin film layer comprises the nano phase-change thin film according to any one of claims 1 to 6;
step 3): and preparing a top electrode layer on the nano phase-change film layer.
Preferably, in the step 2), the nano phase-change film is prepared by adopting a graphite target and a ternary or any binary alloy target of germanium, antimony and tellurium through co-magnetron sputtering.
More preferably, the background vacuum degree is less than 1.0X10 when the nano phase-change film is prepared -4 Pa, the sputtering pressure is between 0.20Pa and 0.25Pa, the sputtering temperature is room temperature, the sputtering power is between 15W and 30W, and the sputtering time is between 5 minutes and 10 minutes.
The preparation method of the nano phase-change film is simple, the graphite purity is high, the price is low, and the process controllability is good. And graphite atoms exist in a solid state form, are not easy to volatilize in the phase change or processing process, so that the technical defects of easy volatilization or phase separation of doping of elements such as O, N, si in the past are overcome, the doping stability and reliability are improved, and the performance of the doped nano phase change film and a device thereof is obviously improved.
The nano phase change film of the invention has good process compatibility, and can be prepared on common inflexible silicon substrates, SOI substrates, quartz substrates and the likeThe substrate can be also used for manufacturing flexible artificial nerve synapse devices on metal sheets, metal foils, metal foil paper, ultrathin glass, PET, polyimide (PI) and any other high-temperature-resistant flexible substrates. Gr (Gr) x (Ge z Sb m Te n ) y Compared with pure Ge-Sb-Te or Sb-Te and Ge-Te, the nano phase-change film has higher thermal stability, higher phase-change speed, stronger data retention and lower density
Compared with other existing nanometer phase-change films, gr based on the invention x (Ge z Sb m Te n ) y The device performance of the nano phase-change film is obviously improved, the reversible phase change of which the storage window reaches two orders of magnitude and the operating voltage is lower than 2.0V can be realized under the action of 5ns electric pulse, and the method is far superior to other existing technical means.
Compared with the prior art, the invention has the following beneficial effects:
1. gr according to the invention x (Ge z Sb m Te n ) y The preparation method of the nano phase-change film is simple and controllable, the purity of graphite is high, and the price is low, so that the performance of the doped nano phase-change film and devices thereof is obviously improved. Gr provided by the invention x (Ge z Sb m Te n ) y The nano phase-change film can realize reversible phase change through external electric pulse, and can realize reversible phase change with a storage window of two orders of magnitude and an operating voltage lower than 2.0V under 5ns electric pulse.
2. The nano phase-change film with different crystallization temperature, melting point, crystallization rate and resistance ratio before and after crystallization can be obtained by adjusting the contents of the three elements. Thus the Gr x (Ge z Sb m Te n ) y The nano phase-change film has very strong adjustability, and is beneficial to optimizing the performances of the nano phase-change film in all aspects. Wherein, graphite, germanium, antimony and tellurium can form stable phases of C-Ge and C-Te, and a part of graphite atoms form C rings or C chains by themselves to inhibit element diffusion, so that the material is stable and is not easy to split phases. Thus, gr according to the invention x (Ge z Sb m Te n ) y NanophaseCompared with pure Ge-Sb-Te or Sb-Te and Ge-Te, the thin film has higher thermal stability, higher phase change speed, stronger data retention, lower density change rate and particularly lower resistance drift.
3. Gr according to the invention x (Ge z Sb m Te n ) y The preparation method of the nano phase-change film is simple and controllable, and graphite atoms exist in a solid state, so that the graphite atoms are not easy to volatilize in the phase change or processing process, the technical defect that the elements such as O, N, si are easy to volatilize or phase-separate in the past is overcome, and the reliability and the electrical property stability of the device are improved.
4. The nano phase-change film provided by the invention is applied to a phase-change memory, and has the advantages of high data retention, high-speed erasing and writing, stable electrical property, low operation voltage and power consumption, small density change before and after phase change, small resistance drift and the like.
Drawings
FIG. 1 shows Gr in example 1 0.4 (Sb 2 Te 1 ) 0.6 And Sb (Sb) 2 Te 1 Resistance-temperature relationship characteristics of (a);
fig. 2 is a schematic structural diagram of a phase-change memory device of embodiment 2;
FIG. 3 is Gr of example 3 0.3 (Sb 2 Te 1 ) 0.7 Reversible erasure performance of phase change memory devices.
Detailed Description
In order to make the invention more comprehensible, preferred embodiments accompanied with figures are described in detail below.
Example 1
The present embodiment provides a Gr 0.4 (Sb 2 Te 1 ) 0.6 Nano phase change film, said Gr 0.4 (Sb 2 Te 1 ) 0.6 The nano phase-change film comprises three elements of graphite, antimony and tellurium, wherein 0<x≤0.5，0.5<y is less than or equal to 1, and x+y=1.
As an example, the Gr 0.4 (Sb 2 Te 1 ) 0.6 The nano phase-change film can be operated by an electric pulse signalThe reversible conversion of the high resistance and the low resistance can be realized, and the resistance is kept unchanged under the operation without an electric pulse signal.
As an example, the Gr 0.4 (Sb 2 Te 1 ) 0.6 The nano phase-change film has at least two stable resistance states under the action of electric pulse.
As an example, the Gr 0.4 (Sb 2 Te 1 ) 0.6 Is a phase-change film material, the Gr 0.4 (Sb 2 Te 1 ) 0.6 The thickness of the nano phase-change film is about 150nm.
Gr according to the invention 0.4 (Sb 2 Te 1 ) 0.6 Compared with the common Ge-Sb-Te or Sb-Te, ge-Te or O, N, si and other element doped nano phase-change film, the phase-change film material has higher thermal stability, higher phase-change speed, stronger data retention and lower density change rate, and particularly has lower resistance drift.
Example 2
The embodiment provides a method for preparing a phase-change memory device on a Polyimide (PI) flexible substrate, which mainly comprises the following process steps:
(1) Firstly, preparing an insulating medium layer with the thickness of 300nm on a PI flexible substrate;
(2) Opening holes in the insulating medium layer, filling metal W, and polishing to prepare a heating electrode with the diameter of 190nm;
(3) Preparation of Gr on heating electrode 0.4 (Sb 2 Te 1 ) 0.6 A nano phase change film layer with the thickness of 100nm;
(4) Preparing a transition layer on the nano phase-change film, wherein the thickness of the transition layer is 10nm;
(5) Finally, a top electrode layer was prepared on the transition layer, with a thickness of 400nm.
The nano phase-change film layer comprises Gr provided by the invention x (Ge z Sb m Te n ) y The nano phase-change film, namely the high-purity graphite doped nano phase-change film comprises graphite (Gr) and any combination of one, two or three elements of germanium (Ge), antimony (Sb) and tellurium (Te), wherein the material is prepared fromThe chemical general formula of the material is Gr x (Ge z Sb m Te n ) y Wherein 0 is<x≤0.5，0.5<y is less than or equal to 1, and x+y=1; z is more than or equal to 0 and less than or equal to 1, m is more than or equal to 0 and less than or equal to 1, and n is more than or equal to 0 and less than or equal to 1.
Gr in example 1 0.4 (Sb 2 Te 1 ) 0.6 The phase-change film material can be used for phase-change memory devices with vertical structures and phase-change memory devices with horizontal or transverse structures. Embodiment 2 is a phase-change memory device for a vertical structure, the phase-change memory device 1 is fabricated on a flexible substrate 2 as shown in FIG. 2, the phase-change memory device 1 includes a heating electrode layer 11 having an electrode diameter of 190nm, an insulating dielectric layer 12, a thickness of 300nm, gr 0.4 (Sb 2 Te 1 ) 0.6 The nano phase-change film layer 13 has a thickness of 100nm, the transition layer 14 has a thickness of 10nm and the top electrode layer 15 has a thickness of 400nm. Gr provided in the present embodiment 0.4 (Sb 2 Te 1 ) 0.6 The nano phase-change thin film layer 13 is used as a storage medium and is the core of the phase-change memory device. The heating electrode layer 11 may be made of W, tiN, tiW or other conductive materials with higher resistivity; the top electrode layer 15 may be made of Al, ti, cu or other materials with better conductivity. The transition layer 14 may be TiN, taN, etc. with a thickness of 2-10nm. The insulating dielectric layer 12 may be SiO 2 、Si 3 N 4 Materials, etc., with a thickness of 300-600 nm.
It should be emphasized that Gr provided by the present invention x (Ge z Sb m Te n ) y The nano phase-change film is not limited to be used in the vertical phase-change memory structure shown in fig. 2, and any device structure (such as a lateral structure) for a phase-change memory can be used, including Gr provided by the invention x (Ge z Sb m Te n ) y The difference in resistance between the crystalline and amorphous states of the nano-phase change film enables the electronic device of any other structure to be stored.
In addition, an extraction electrode is formed on the top electrode layer 15, and the top electrode layer, the heating electrode layer, and a control switch, a driving circuit, and a peripheral circuit of the device can be integrated through the extraction electrode.
Example 3
Preparation of 150nm Gr-based on a typical Si substrate 0.3 (Sb 2 Te 1 ) 0.7 The resistance-voltage relationship of the phase change memory is obtained through testing of the memory device of the nano phase change film, and is shown in fig. 3. Under the application of an electrical pulse, the phase change memory achieves reversible phase change, and the RESET voltage (the voltage corresponding to return from low resistance to high resistance) is low. Under an electric pulse of 5 nanoseconds, the operation of erasing (high resistance to low resistance) and writing (low resistance to high resistance) can be realized, which is far faster than the operation of erasing and writing of 50 nanoseconds of GST phase change memory devices. In terms of operation voltage, the "erasing" and "writing" voltages of the phase change memory device under an electric pulse of 5 nanoseconds are about 1.0V and 2.0V respectively, which are far lower than the operation voltage of the existing GST phase change memory device under a pulse of 50 nanoseconds. Therefore, the phase change memory device has remarkable technical breakthroughs in the aspects of operation speed, operation voltage, power consumption and the like.
In summary, the present invention effectively overcomes various disadvantages in the prior art and has high industrial utility value.
Claims (11)
1. A high-purity graphite doped nano phase-change film is characterized by comprising a combination of graphite and at least one of germanium, antimony and tellurium, wherein the chemical formula of the nano phase-change film is Gr x (Ge z Sb m Te n ) y Wherein 0 is<x≤0.5，0.5<y is less than or equal to 1, and x+y=1; z is more than or equal to 0 and less than or equal to 1, m is more than or equal to 0 and less than or equal to 1, and n is more than or equal to 0 and less than or equal to 1.
2. The high purity graphite doped nanophase change film of claim 1, wherein the nanophase change film has at least two stable resistance states under the action of an electrical pulse to achieve multiple resistance states.
3. The high purity graphite doped nano phase change film according to claim 2, wherein the high resistance state has a resistance value of 10 5 -10 7 Between ohms, low resistance stateResistance value is 10 3 -10 5 Between ohms, when there are more than two stable resistance states, the resistance value of the intermediate resistance state is 10 4 -10 6 Between ohms.
4. The high purity graphite doped nano phase change film according to claim 1, wherein the nano phase change film can realize rapid reversible phase change between amorphous and crystalline states under the operation of electric pulse, so as to achieve the purpose of mutually converting high and low resistance values to store information, and the resistance value is kept unchanged under the operation without electric pulse signals.
5. The high purity graphite doped nano phase change film according to claim 1, wherein the thickness of the nano phase change film is between 2nm and 200 nm.
6. The high purity graphite doped nano phase change film according to claim 1, wherein the nano phase change film is easy to form multi-layer heterogeneous phase change structures with different periods, wherein the thickness of the sub-layer is between 2nm and 10nm.
7. A phase change memory device comprising a heating electrode layer, a top electrode layer, and a nano phase change thin film layer between the heating electrode layer and the top electrode layer, the nano phase change thin film layer comprising the nano phase change thin film of any one of claims 1-6.
8. The phase-change memory device of claim 7, wherein the phase-change memory device is disposed on a flexible substrate comprising at least one of a metal sheet, a metal foil paper, ultra-thin glass, PET, polyimide.
9. A method of manufacturing a phase change memory device according to claim 7 or 8, comprising the steps of:
step 1): preparing a heating electrode layer;
step 2): preparing a nano phase-change thin film layer on the heating electrode layer, wherein the nano phase-change thin film layer comprises the nano phase-change thin film according to any one of claims 1 to 6;
step 3): and preparing a top electrode layer on the nano phase-change film layer.
10. The method for fabricating a phase-change memory device according to claim 9, wherein in the step 2), the nano phase-change thin film is fabricated by co-magnetron sputtering using a graphite target and a ternary or arbitrary binary alloy target of germanium, antimony, tellurium.
11. The method for fabricating a phase-change memory device according to claim 10, wherein the nano phase-change film has a background vacuum degree of less than 1.0X10 when fabricated -4 Pa, the sputtering pressure is between 0.20Pa and 0.25Pa, the sputtering temperature is room temperature, the sputtering power is between 15W and 30W, and the sputtering time is between 5 minutes and 10 minutes.
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