CN102227015B - Phase transition storage material and preparation method thereof - Google Patents

Phase transition storage material and preparation method thereof Download PDF

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CN102227015B
CN102227015B CN201110135885.2A CN201110135885A CN102227015B CN 102227015 B CN102227015 B CN 102227015B CN 201110135885 A CN201110135885 A CN 201110135885A CN 102227015 B CN102227015 B CN 102227015B
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phase
storage material
change storage
phase transition
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CN102227015A (en
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吕业刚
宋三年
宋志棠
刘波
饶峰
吴良才
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Shanghai Institute of Microsystem and Information Technology of CAS
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Abstract

The invention relates to a phase transition material and a preparation method thereof, wherein the phase transition storage material is a gallium-antimony-selenium compound. The chemical component is Ga x SbySez, wherein 4 (*(40, 25 (y (85, 5 (z (70, x + y + z = 100. The gallium-antimony-selenium phase transition thin film material provided in the invention, compared to a common Ge2Sb2Te5 (GST) material, has a better heat stability, a faster phase transition speed and a lower melting point. Meanwhile, the gallium-antimony-selenium phase transition thin film material provided in the invention does not contain element Te, is friendly to environment, does not contaminate semiconductor equipment and brings conveniences for subsequent technology processing. The phase transition memory manufactured of the phase transition storage material possesses advantages such as strong data confining force, low power dissipation, fast operation speed, stable electrics performance and the like.

Description

A kind of phase-change storage material and preparation method thereof
Technical field
The invention provides a kind of phase-change storage material and preparation method thereof, particularly a kind of gallium-antimony for phase transition storage-selenium phase-change thin film storage medium.
Background technology
Phase transition storage (PCM) is a kind of non-volatile semiconductor memory of rising in recent years.Compared with current existing multiple semiconductor memory technologies, it has superiority (nanoscale), at a high speed reading, the low-power consumption that device size can contract, the advantages such as high density, manufacturing process are simple, by contenders that industrial quarters is extensively had an optimistic view of in memory, be expected to the main flow memory technology that alternative flash memory (Flash technology) becomes nonvolatile memory of future generation, thus have wide market prospects.
Phase transition storage is that the Joule heat utilizing electricity or light pulse to produce makes phase-change storage material, between crystalline state (low-resistance) and amorphous state (high resistant), reversible transition occur and realizes write and the erasing of data, and the reading of data is then realized by the state of measuring resistance.The core of phase transition storage is phase change memory dielectric material, and conventional phase-change storage material system mainly telluro compound, as Ge-Sb-Te, Si-Sb-Te, Ag-In-Sb-Te etc.Particularly Ge 2sb 2te 5(GST) phase change disc and phase transition storage has been widely used in.But also there are the following problems: one, crystallization temperature is lower, data retention can not be guaranteed, and is faced with the danger of loss of data, constrains its application; Two, power consumption is comparatively large, needs larger drive current (being greater than 1 milliampere).Along with reducing of size, the driving force of transistor or diode is very limited, not easily meets large driven current density, is thus difficult to realize high-density city; Three, phase velocity needs to be improved further, and the phase transition storage that there are some researches show based on GST realizes stablize the electric pulse that RESET operates and was at least for 500 nanoseconds.Dynamic random access memory completes erasable at high speeds, and this needs us to explore to have the storage medium of faster phase velocity.Four, the tellurium all containing easily diffusion in telluro phase-change storage material, make the interfacial instability between phase-change storage material and electrode, phase-change storage material component is easily segregation also, but also easily pollutes semiconductor equipment, to human body and environment also unfavorable, the environmental protection policy advocated with current country is runed counter to.
Therefore, how to provide a kind of Heat stability is good, data retention is strong, low in energy consumption, and phase velocity is fast, environmentally friendly and with the phase change film material of CMOS technology compatibility, be the problem that current techniques field needs to solve.
Summary of the invention
The invention provides a kind of phase-change storage material and preparation method thereof, particularly a kind of gallium-antimony-selenium phase change film material for phase transition storage.The present invention can solve thermal stability that in prior art, phase-change storage material shows and data holding ability is poor, phase velocity is slow, power consumption is higher and the problem of environmental pollution.
For achieving the above object, the present invention adopts following technical scheme: a kind of phase-change storage material, and described phase-change storage material is gallium-antimony-selenium compound.
Preferably, chemical constituent is Ga xsb yse z, wherein 4 < x < 40,25 < y < 85,5 < z < 70, x+y+z=100.
Preferably, chemical constituent is Ga xsb yse z, wherein 10≤x≤20,50≤y≤85,20≤z≤40, x+y+z=100.
Preferably, chemical constituent is Ga xsb yse z, wherein x=8, y=34, z=58.
Preferably, chemical constituent is Ga xsb yse z, wherein x=13, y=32, z=55.
Preferably, chemical constituent is Ga xsb yse z, wherein x=34, y=40, z=26.
Preferably, described gallium-antimony-selenium compound is when film preparation, and composition has certain segregation, and the error of segregation element is within 10%.
Preferably, described gallium-antimony-selenium compound also comprises foreign atom, and the mol ratio of described foreign atom is 0% to 20%.
Preferably, described foreign atom is one of in aluminium, bismuth, nitrogen, oxygen, silver, gold, tin, germanium, silicon or the mixing and doping of above-mentioned several element.
Preferably, described phase-change storage material has the characteristic of reversible transition under outside electric pulse effect.
Preferably, there is 2 and Resistance states stable above in described phase-change storage material under outside electric pulse.
Preferably, described phase-change storage material is at least 4 at the ratio of the resistivity of amorphous state and crystalline state.
Preferably, can there is reversible change in described phase-change storage material its reflectivity under laser pulse effect.
The present invention also comprises a kind of preparation method of phase-change storage material, and described preparation method comprises any one of following method: (1) adopts GaSb alloys target and Sb xse alloys target two target magnetic control co-sputtering, wherein 1 < x < 8; (2) GaSb, Sb is adopted 2se 3with Sb tri-target magnetic control co-sputtering.
Preferably, GaSb alloys target and Sb is adopted 2se 3alloys target two target magnetic control co-sputtering.
Gallium-antimony-selenium phase change film material of the present invention, compared with conventional GST, has better thermal stability, faster crystallization rate, stronger data retention.Simultaneously in this material system not containing poisonous element T e, because of but a kind of eco-friendly material, can not semiconductor equipment be polluted, be convenient to the processing and manufacturing of subsequent technique, compatible better with CMOS technology.
The preparation method of phase-change storage material provided by the invention, technique is simple, is convenient to accurately control material composition and subsequent technique, is conducive to stable components and shortens memory fabrication cycle, cost-saving.
The invention provides phase-change storage material is applied in phase transition storage, makes phase transition storage have strong, the erasable speed of data retention fast, low in energy consumption, the advantages such as stable electrical properties.
Accompanying drawing explanation
Fig. 1 is a phase-change memory cell structure schematic diagram;
Fig. 2 is the resistance-temperature relationship figure of described phase-change storage material Ga-Sb-Se;
Fig. 3 is the activation energy result of calculation figure of described phase-change storage material Ga-Sb-Se;
Fig. 4 is the data holding ability result of calculation figure of described phase-change storage material Ga-Sb-Se;
Fig. 5 is the resistance-voltage relationship figure of Ga-Sb-Se phase transition storage.
Embodiment
Below will be described in detail to invention by specific embodiment.
Embodiment one
Refer to Fig. 1, a kind of phase-change memory cell of vertical stratification, described phase-change memory cell comprise bottom electrode 1, the phase-change storage material layer 2 be positioned on bottom electrode 1, the top electrode 4 that is positioned at the transition zone 3 on phase-change storage material layer 2 and is positioned on transition zone 3; Being surrounded by dielectric 5 of described bottom electrode 1.
Phase-change storage material layer 2 is phase change film materials, and it selects gallium provided by the present invention-antimony-selenium (Ga-Sb-Se) compound.It is as storage medium, is the core in this phase-change memory cell.Wherein, bottom electrode 1 and top electrode 4 can select AL, Ti, W, graphite, TiN, Cu, TiW or other electric conducting materials.Transition zone 3 can select TiN or TaN, and its thickness is about 10-30 nanometer.Be preferably 20 nanometers.Insulating barrier 5 can be SiO 2or Si 3n 4material.
Ga-Sb-Se compound of the present invention, as phase change film material, also can be used in the phase-change memory cell of transversary.
Phase-change storage material Ga-Sb-Se of the present invention can be prepared by the method for More target sputtering together, and its component ratio can obtain by regulating the power that different target is corresponding.Prepared by the methods such as described Ga-Sb-Se also can pass through chemical vapour deposition (CVD), ald (ALD), electron beam evaporation, also can by injecting at Sb-Se film intermediate ion the Ga-Sb-Se material that element Ga obtains required atomic ratio.
Embodiment two
Phase-change storage material gallium-antimony-selenium (Ga-Sb-Se) compound provided by the invention, its chemical constituent is Ga xsb yse z, wherein 4 < x < 40,25 < y < 85,5 < z < 70, x+y+z=100.
Its in the phase-change memory cell of vertical stratification time, bottom electrode 1 and top electrode 4 can select AL, Ti, W, graphite, TiN, Cu, TiW or other electric conducting materials.Transition zone 3 can select TiN or TaN, and its thickness is about 10-30 nanometer.Be preferably 20 nanometers.Insulating barrier 5 can be SiO 2or Si 3n 4material.
Phase-change storage material Ga-Sb-Se of the present invention can be prepared by the method for More target sputtering together.Adopt GaSb alloys target and Sb 2se 3(or Sb xse, 1 < x < 8) technological parameter of alloys target two target magnetic control co-sputtering comprises: background vacuum is less than 2 × 10 -4pascal, sputtering pressure is 0.18 Pascal to 0.25 Pascal, and sputter gas is argon, and temperature is room temperature, the radio-frequency power supply power be applied in GaSb alloys target be 10 watts to 45 watts, be applied to Sb 2se 3(or Sb xse, 1 < x < 8) radio-frequency power supply power on target is 8 watts to 40 watts, sputtering time is 20 minutes to 60 minutes, and deposited film thickness is 50 nanometer to 200 nanometers.
Embodiment three
Preferably, phase-change storage material gallium-antimony-selenium (Ga-Sb-Se) compound provided by the invention, its chemical constituent is Ga xsb yse z, wherein, 10≤x≤20,50≤y≤85,20≤z≤40, x+y+z=100.
The present invention also comprises a kind of preparation method of phase-change storage material, and described preparation method comprises any one of following method: (1) adopts GaSb alloys target and Sb xse alloys target two target magnetic control co-sputtering, wherein 1 < x < 8; (2) GaSb, Sb is adopted 2se 3with Sb tri-target magnetic control co-sputtering.
Embodiment four
Preferably, the invention provides the described concrete component of phase-change storage material Ga-Sb-Se is Ga 8sb 34se 58, Ga 13sb 32se 55or Ga 34sb 40se 26.
Preferably, the present invention adopts GaSb alloys target and Sb 2se 3alloys target two target magnetic control co-sputtering.
In addition, in the process of the described phase-change storage material of preparation, also comprise foreign atom in its gallium-antimony-selenium compound, the mol ratio of described foreign atom is 0% to 20%.Particularly, described foreign atom is one of in aluminium, bismuth, nitrogen, oxygen, silver, gold, tin, germanium, silicon or the mixing and doping of above-mentioned several element.
The compound of described phase-change storage material gallium-antimony has the characteristic of reversible transition under outside electric pulse or light pulse effect, and its ratio in the resistivity of amorphous state and crystalline state is for being at least 4.
Alternatively, there is 2 and Resistance states stable above in described phase-change storage material under outside electric pulse.
The preparation method of phase-change storage material provided by the invention, technique is simple, is convenient to accurately control material composition and subsequent technique.
Ga-Sb-Se phase change film material provided by the present invention is not limited to the phase change memory structure shown in Fig. 1, every various cellular constructions (as transversary) for phase transition storage can use, and comprise and utilize the resistance difference between the crystalline state of Ga-Sb-Se phase change film material provided by the invention and amorphous state to realize other function elements stored.
To described phase change memory film Ga-Sb-Se prepared by Semiconductor substrate and use Ga-Sb-Se of the present invention to carry out every test as the phase-change memory cell of storage medium, to assess the phase-change characteristic of phase-change storage material, comprise crystallization temperature, thermal stability, data holding ability, and the performance of phase transition storage.
Fig. 2 is the resistance-temperature relationship figure of described phase-change storage material Ga-Sb-Se.As can be seen from the figure, the crystallization temperature of phase-change storage material Ga-Sb-Se is between 230-310 DEG C, and comparatively GST (about 140 DEG C) is high.When antimony content one timing, the crystallization temperature of phase-change storage material increases along with the increase of gallium selenium ratio.Thus the crystallization temperature by regulating the ratio of gallium Se content conveniently can control phase-change storage material Ga-Sb-Se.
As shown in Figure 3, the activation energy of described phase-change storage material Ga-Sb-Se is obtained by the resistance-temperature relationship under different heating rate.Described phase-change storage material Ga-Sb-Se activation energy increases along with the increase of gallium selenium ratio, and scope is 4.06 to 5.52eV, obviously high than GST (2.20eV).High crystallization temperature and activation energy absolutely prove that the thermal stability of described phase-change storage material Ga-Sb-Se is better than GST, thus can avoid problem in GST memory, the problem includes: problems such as crosstalks.The 10 annual data confining forces of described phase-change storage material Ga-Sb-Se also increase along with the increase of gallium selenium ratio.
As shown in Figure 4.10 annual datas keep temperature range between 159 to 230 DEG C, at least exceeding 70 more spend than GST (88 DEG C).Strong data holding ability can make described phase-change storage material Ga-Sb-Se be applied in the special occasions of high temperature, such as automotive electronics, embedded storage etc.Described phase-change storage material Ga-Sb-Se is prepared into memory cell as shown in Figure 1, obtains the resistance-voltage relationship of this phase transition storage after tested.
As shown in Figure 5.Under applying electric pulse, described phase transition storage realizes reversible transition, and RESET voltage (turning back to the voltage corresponding to high resistant by low-resistance) is lower, and thus device power consumption is lower.Such as under the electric pulse of 200 nanoseconds, phase transition storage can be obtained and realize " wiping " (resistance of high resistant step-down) and " writing " (low-resistance uprises resistance) operation in 1.4 and 3V respectively.The RESET voltage of described phase transition storage, comparatively GST low (500 nanosecond 3.5V), shows that described phase transition storage has lower power consumption.And in phase velocity, this phase transition storage can make phase transition storage complete " erasable window " under the electric pulse of 50 nanoseconds, far below " the erasable window " of 500 nanoseconds that GST phase transition storage is reported usually.Therefore, described phase transition storage has obvious advantage than GST phase transition storage in power consumption and speed.
In sum, compared with general storage medium, phase-change storage material Ga-Sb-Se compound provided by the invention, wherein 4 < x < 40,25 < y < 85,5 < z < 70, x+y+z=100, Heat stability is good, data holding ability is strong, and physical property is adjustable; In addition, described phase-change storage material Ga-Sb-Se is not containing easy pollution element Te, environmentally friendly, not easily pollutes semiconductor manufacturing equipment, is convenient to following process.
The preparation method of phase-change storage material provided by the invention, technique is simple, is convenient to accurately control material composition and subsequent technique.
The phase transition storage using described phase-change storage material Ga-Sb-Se to be prepared into, has the advantages such as low in energy consumption, service speed is fast, stable electrical properties.
Be understandable that, although the present invention with preferred embodiment disclose as above, but above-described embodiment and be not used to limit the present invention.For any those of ordinary skill in the art, do not departing under technical solution of the present invention ambit, the technology contents of above-mentioned announcement all can be utilized to make many possible variations and modification to technical solution of the present invention, or be revised as the Equivalent embodiments of equivalent variations.Therefore, every content not departing from technical solution of the present invention, according to technical spirit of the present invention to any simple modification made for any of the above embodiments, equivalent variations and modification, all still belongs in the scope of technical solution of the present invention protection.

Claims (8)

1. a phase-change storage material, is characterized in that, described phase-change storage material is gallium-antimony-selenium compound;
Its chemical constituent is Ga xsb yse z, wherein x=34, y=40, z=26.
2. phase-change storage material as claimed in claim 1, it is characterized in that, described gallium-antimony-selenium compound is when film preparation, and composition has certain segregation, and the error of segregation element is within 10%.
3. phase-change storage material as claimed in claim 1, it is characterized in that, described gallium-antimony-selenium compound also comprises foreign atom, and the mol ratio of described foreign atom is 0% to 20%.
4. phase-change storage material as claimed in claim 3, is characterized in that, described foreign atom is one of in aluminium, bismuth, nitrogen, oxygen, silver, gold, tin, germanium, silicon or the mixing and doping of above-mentioned several element.
5. phase-change storage material as claimed in claim 1, it is characterized in that, described phase-change storage material has the characteristic of reversible transition under outside electric pulse effect.
6. phase-change storage material as claimed in claim 1, it is characterized in that, there is 2 and Resistance states stable above in described phase-change storage material under outside electric pulse.
7. phase-change storage material as claimed in claim 1, is characterized in that, described phase-change storage material is at least 4 at the ratio of the resistivity of amorphous state and crystalline state.
8. phase-change storage material as claimed in claim 1, it is characterized in that, can there is reversible change in described phase-change storage material its reflectivity under laser pulse effect.
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