CN105098065B - A kind of preparation method of storage unit of resistive random access memory (RRAM) and products thereof - Google Patents
A kind of preparation method of storage unit of resistive random access memory (RRAM) and products thereof Download PDFInfo
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Abstract
The invention discloses a kind of preparation method of the storage unit of resistive random access memory (RRAM), step 1, in substrate surface form conductive film as first electrode；Step 2, the first electrode surface obtained in step 1 prepare the ZnO film of argon plasma bombardment processing as intermediate layer；Step 3, the interlayer surfaces obtained in step 2 prepare conductive film as second electrode；Step 4, prepare the device of isolation on the architecture basics that step 3 obtains, and obtains the storage unit of the resistive random access memory (RRAM).The present invention provides a kind of preparation method of the storage unit of resistive random access memory (RRAM), carries out argon plasma bombardment processing to the ZnO film as middle dielectric layer, greatly improves the flatness on ZnO film surface；The memory prepared using the ZnO film of the argon plasma bombardment processing as intermediate layer, initial representation is low resistance state, and electric forming process is not required in the erasable of all devices, and erasable voltage is smaller.
Description
Technical field
The present invention relates to the storage list of technical field of non-volatile, more particularly to a kind of resistive random access memory (RRAM)
Preparation method of member and products thereof.
Background technology
The high-tech rapid development of Contemporary Digital, the requirement of higher, example are proposed to the performance of existing information storage product
Such as：At high speed, high density, long-life, low cost and low-power consumption etc., while the defects of also reveal that existing random storage technology.
One of weakness of dynamic memory and static memory is its volatibility：Information is lost under powering-off state, and easily by electromagnetism spoke
Blackberry lily is disturbed.Then there are the technology barrier such as read or write speed is slow, packing density is low for flash memory.Therefore, there is an urgent need in storage material and skill
Make a breakthrough in terms of art, with the memory technology of exploitation a new generation.
Houston, U.S.A university in 2000 is in metal/Ca titanium ore Mn oxide (PrCaMnO)/this sandwich structure of metal
Middle discovery, application electric pulse can be such that system resistance is switched fast in high low resistance to return between two metal electrodes.Then, people
Find in NiO, ZnO, CuO, ZrO2、TiO2Etc. there is also similar electroluminescent resistance in a variety of Dyadic transition group metallic oxides
Transition effect.Based on the electric resistance changing effect, there has been proposed a kind of new nonvolatile memory concept-resistor-type is random
Memory (RRAM).
The storage unit of RRAM, generally comprises dielectric substrate, and insulated substrate surface sets first electrode, first electrode surface
Upper setting has middle dielectric layer made of resistance transformation characteristic material, and the surface of middle dielectric layer sets second electrode.It is middle
The material of dielectric layer is generally transition metal oxide, such as HfO2、NiO、TiO2、ZrO2、MgO、WO3、Ta2O5、Al2O5、MoOx、
CeOx、La2O3、Pr0.7Ca0.3Mn0.3Deng, and can be doped using the element such as Al, Gd, La, Sr, Ti, intermediate medium
The material of layer can show two stable states, i.e. high-impedance state and low resistance state.
Compared with other species memories, simple, erasable speed is fast, storage density is high and semiconductor with preparing by RRAM
Processing compatibility waits well main advantage.
At present, the overwhelming majority report RRAM devices be required for the higher electric forming of a voltage (electric resistance changing material by
Initial high-resistance state is changed into low resistance state) process.Chinese patent literature such as Publication No. CN102136487B discloses one
The resistance-type ram memory cell of kind based on zinc oxide material and preparation method thereof, using transparent conductive film as hearth electrode, with ZnO
Film is intermediate layer, with the work function such as Pt, Au, Ir higher metal (M) for top electrode, forms the structure of FTO (ITO)/ZnO/M.
The presence of electric forming process is unfavorable to the practical application of memory device.In addition, this electric forming process is deposited
Also it is being unfavorable for RRAM preparation processes and conventional semiconductors CMOS technology compatibility, is constraining the industrialized production of RRAM.
The content of the invention
The present invention provides a kind of preparation method of the storage unit of resistive random access memory (RRAM), to as middle dielectric layer
ZnO film carries out argon plasma bombardment processing, greatly improves the flatness on ZnO film surface；Banged with the argon plasma
The memory that the ZnO film of processing is prepared as intermediate layer is hit, initial representation is low resistance state, and the erasable of all devices is not required to
Electric forming process is wanted, and erasable voltage is smaller.
The invention discloses a kind of preparation method of the storage unit of resistive random access memory (RRAM), include the following steps：
Step 1, substrate surface formed conductive film as first electrode；
Step 2, using at least one of common sputtering, magnetron sputtering, collosol and gel, chemical vapor deposition or coating just
Method prepares ZnO film in the first electrode surface that step 1 obtains, then the ZnO film is carried out at argon plasma bombardment
Reason, intermediate layer is used as using the ZnO film after argon plasma bombardment processing；
Step 3, the interlayer surfaces obtained in step 2 prepare conductive film as second electrode；
Step 4, prepare the device of isolation on the architecture basics that step 3 obtains, and obtains the resistor-type random storage
The storage unit of device.
Preferably, the argon plasma bombardment processing process described in step 2 is：
In magnetron sputtering apparatus cavity, argon plasma bombardment processing is carried out to the ZnO film, processing power is
20~1000W, temperature are 20~500 DEG C, and the time is 10s~10h.
Further preferably, the preparation process in the intermediate layer described in step 2 is：
Using the method for magnetron sputtering, using ZnO as sputtering target material, using the gaseous mixture of oxygen and argon gas as sputtering atmosphere,
Prepare ZnO film, then argon plasma bombardment processing is carried out to the ZnO film, processing power is 100~500W, temperature
For 20~50 DEG C, the time is 20min~5h.
Further preferably, the power of the argon plasma bombardment processing is 100W.
Preferably, by the ZnO film for the argon plasma bombardment processing being prepared at 50~500 DEG C, hydrogen,
In the atmosphere such as inert gas (nitrogen, argon gas, helium etc.), anneal 5s~5h.
The substrate can be dielectric substrate, such as glass, thermal oxide silicon chip, ceramics electrically insulating material；Or semiconductive
Substrate, such as Si oxide semiconductor, nitride-based semiconductor semi-conducting material；Or conductive substrates, such as various metals, graphite are led
Electric material.
Preferably, the first electrode is at least one of metal, conductive oxide, conductive nitride, use
It is prepared by sputtering, magnetron sputtering, electron beam evaporation or chemical vapour deposition technique.
Preferably, the second electrode is at least one of metal, conductive oxide, conductive nitride, use
It is prepared by sputtering, magnetron sputtering, electron beam evaporation, chemical vapor deposition, mask plate, photoetching or dry etching method.
The metal is platinum, gold, silver, copper, aluminium etc., and conductive oxide is the doping such as tin-doped indium oxide, aluminium, indium, gallium
Zinc oxide etc., conductive nitride are titanium nitride etc..
The preparation of the device of isolation described in step 4 can use reactive ion etching or inductively coupled plasma etching
Etc. the method for dry etching.
The invention also discloses the storage unit of the resistive random access memory (RRAM) obtained according to the preparation method.
Preferably, the thickness in the intermediate layer is 2~100nm.
Further preferably, the storage unit for the resistive random access memory (RRAM) being prepared：
The substrate is made of monocrystalline silicon with the silica for being grown in monocrystalline silicon surface；
The first electrode is the Titanium and metal platinum being sequentially prepared；
The thickness in the intermediate layer is 20~50nm；
The second electrode is metal platinum and metallic copper.
Compared with prior art, the advantage of the invention is that：
The intermediate layer of the storage unit of resistive random access memory (RRAM) uses the ZnO film of argon plasma bombardment processing, this
The resistive random access memory (RRAM) initial representation of kind structure is low resistance state, and electric forming process is not required in the erasable of all devices,
And erasable voltage is smaller.In addition, comparing with conventional ZnO film, the ZnO film surface of argon plasma bombardment processing is non-
It is often smooth.These characteristics show that the present invention has important application value in Nonvolatile Memory Device field.
It is very crucial as bombardment source using argon plasma in the present invention, defect in ZnO film can be significantly increased
Concentration, reduces film initial resistance, so as to eliminate electric forming process.If bombarding ZnO film using oxygen plasma, can drop
Low film defects concentration, causes film initial resistance to increase, it is necessary to the larger electric forming process of a voltage.
Brief description of the drawings
Fig. 1 is the structure diagram of the storage unit of the resistive random access memory (RRAM) of the present invention；
Fig. 2 is the transmission electron microscope photo of ZnO film before and after argon plasma bombardment processing in embodiment 1；
Fig. 3 is initial current-voltage curve of resistive random access memory (RRAM) storage unit prepared by embodiment 1；
Fig. 4 is normal current-voltage curve of resistive random access memory (RRAM) storage unit prepared by embodiment 1；
Fig. 5 is initial current-voltage curve of resistive random access memory (RRAM) storage unit prepared by embodiment 2；
Fig. 6 is normal current-voltage curve of resistive random access memory (RRAM) storage unit prepared by embodiment 2；
Fig. 7 is the resistor-type random storage based on the ZnO film without argon plasma bombardment processing prepared by comparative example 1
The current -voltage curve of device storage unit；
Fig. 8 is that the resistive random access memory (RRAM) of the ZnO film based on oxygen plasma bombardment processing prepared by comparative example 2 is deposited
The current -voltage curve of storage unit.
Embodiment
The present invention is described in further detail below in conjunction with attached drawing embodiment.
Fig. 1 be the present invention resistive random access memory (RRAM) storage unit structure diagram, the storage unit from
Under supreme be followed successively by substrate, first electrode, intermediate layer and second electrode.
Embodiment 1
The storage unit of resistive random access memory (RRAM) manufactured in the present embodiment, including dielectric substrate, dielectric substrate is by monocrystalline
Silicon is formed with the silica spacer medium layer for being grown in monocrystalline silicon surface, and the first electricity is set on silica spacer medium layer
Pole, first electrode are made of the titanium of 20nm thickness and the platinum of 150nm thickness；Argon plasma bombardment processing is set in first electrode surface
ZnO film intermediate layer, intermediate layer thickness 20nm, the surface in intermediate layer sets second electrode made of platinum, second electrode
Thickness is 50nm.
The preparation method of the storage unit of above-mentioned resistive random access memory (RRAM) is：
Step 1, using thermal oxide method by silica spacer medium layer growth dielectric substrate is made on the monosilicon；
Step 2, be sequentially prepared the titanium of 20nm thickness and the platinum of 150nm thickness is used as first by the use of sputtering method in insulated substrate surface
Electrode；
Step 3, the method using magnetron sputtering, using ZnO as sputtering target material, using the mixed gas of oxygen and argon gas as
Sputtering atmosphere, underlayer temperature are room temperature, prepare ZnO film, the thickness of prepared ZnO film is 35nm.Then in magnetron sputtering
In equipment cavity, at a temperature of 25 DEG C, power 100W, to ZnO film argon plasma bombardment processing 60min, obtains argon
The ZnO film of plasma bombardment processing, processing rear film thickness is 20nm.
Step 4, made using the method for electron beam evaporation combination mask plate on the ZnO film of argon plasma bombardment processing
It is 50nm to make second electrode, second electrode thickness made of platinum；
Step 5, the device that isolation is prepared using the method for reactive ion etching on the acquired architecture basics of step 4
Structure.
Fig. 2 is the transmission electron microscope photo of plasma bombardment ZnO film before and after the processing, as seen from the figure, ZnO film after processing
The flatness on surface greatly improves.
The I-E characteristic of device manufactured in the present embodiment is tested using analyzing parameters of semiconductor tester.In electricity
Press the I-E characteristic that the device is tested under continuous scan pattern.Scan bias voltage is added in second electrode and first electrode.
The initial current of device-voltage characteristic test result is shown in that (numeral 1,2,3,4 in figure shows that voltage scanning is suitable to Fig. 3
Sequence), device is in low resistance state at the beginning, therefore need not extra larger electric forming voltage.When voltage from 0V scan to
When near 0.6V, device is maintained at low resistance state, and it is non-volatile to show low resistance state, in 0.6V (resetting voltage), device
Be changed into high-impedance state suddenly from low resistance state, when voltage is scanned to 0V from 0.6V, and continue from 0V scan to 1.7V when, device
Part is maintained at high-impedance state, and the high resistance state for showing device is also non-volatile, and at 1.7V (set voltage), device is from high resistant
State is changed into low resistance state suddenly.
The normal current of device-voltage characteristic test result is shown in that (numeral 1,2,3,4 in figure shows that voltage scanning is suitable to Fig. 4
Sequence), device is resetted in 0.6V, is changed into high-impedance state from low resistance state, and set occurs in 1.4V, is changed into low-resistance from high-impedance state
State.The resistance mean difference of high and low resistance state is more than 1000 times, and the transition process of the high low resistance state can repeat.
Embodiment 2
The storage unit of resistive random access memory (RRAM) manufactured in the present embodiment, including dielectric substrate, dielectric substrate is by monocrystalline
Silicon is formed with the silica spacer medium layer for being grown in monocrystalline silicon surface, and the first electricity is set on silica spacer medium layer
Pole, first electrode are made of the titanium of 20nm thickness and the platinum of 150nm thickness；Argon plasma bombardment processing is set in first electrode surface
ZnO film intermediate layer, intermediate layer thickness 21nm, the surface in intermediate layer sets second electrode made of copper, second electrode
Thickness is 50nm.
The preparation method of the storage unit of above-mentioned resistive random access memory (RRAM) is：
Step 1, using thermal oxide method by silica spacer medium layer growth dielectric substrate is made on the monosilicon；
Step 2, be sequentially prepared the titanium of 20nm thickness and the platinum of 150nm thickness is used as first by the use of sputtering method in insulated substrate surface
Electrode；
Step 3, the method using magnetron sputtering, using ZnO as sputtering target material, using the mixed gas of oxygen and argon gas as
Sputtering atmosphere, underlayer temperature are room temperature, prepare ZnO film, the thickness of prepared ZnO film is 25nm.Then in magnetron sputtering
In equipment cavity, at a temperature of 50 DEG C, power 500W, to ZnO film argon plasma bombardment processing 10min, obtains argon
The ZnO film of plasma bombardment processing, processing rear film thickness is 21nm；
Step 4, made using the method for electron beam evaporation combination mask plate on the ZnO film of argon plasma bombardment processing
Make the second electrode being made of copper, second electrode thickness is 50nm；
Step 5, using inductively coupled plasma etching method prepare isolation on the acquired architecture basics of step 4
Device architecture.
The I-E characteristic of device manufactured in the present embodiment is tested using analyzing parameters of semiconductor tester.In electricity
Press the I-E characteristic that the device is tested under continuous scan pattern.Scan bias voltage is added in second electrode and first electrode.
The initial current of device-voltage characteristic test result is shown in that (numeral 1,2,3,4 in figure shows that voltage scanning is suitable to Fig. 5
Sequence), device is in low resistance state at the beginning, therefore need not extra larger electric forming voltage.When voltage from 0V scan to-
During 0.4V, device is maintained at low resistance state, and it is non-volatile to show low resistance state, continues to scan from -0.4V (resetting voltage)
To -0.8V, the resistance of device constantly increases, and is finally changed into high-impedance state, when voltage is scanned to 0V from -1V, device
Part is maintained at high-impedance state, and the high resistance state for showing device is also non-volatile, when continuing forward voltage scanning, in+0.7V
(set voltage), device is changed into low resistance state suddenly from high-impedance state.
The normal current of device-voltage characteristic test result is shown in that (numeral 1,2,3,4 in figure shows that voltage scanning is suitable to Fig. 6
Sequence), device is resetted in -0.3~-1V, is changed into high-impedance state from low resistance state, and set occurs in+1V, is changed into from high-impedance state
Low resistance state.More than 100 times, the transition process of the high low resistance state can repeat the resistance mean difference of high and low resistance state.
Comparative example 1
The storage unit of resistive random access memory (RRAM) prepared by this comparative example, including dielectric substrate, dielectric substrate is by monocrystalline
Silicon is formed with the silica spacer medium layer for being grown in monocrystalline silicon surface, and the first electricity is set on silica spacer medium layer
Pole, first electrode are made of the titanium of 20nm thickness and the platinum of 150nm thickness；Set in first electrode surface and bombarded without argon plasma
The intermediate layer of the ZnO film of processing, intermediate layer thickness 35nm, second electrode made of the surface setting platinum in intermediate layer, second
Thickness of electrode is 50nm.
The preparation method of the storage unit of above-mentioned resistive random access memory (RRAM) is：
Step 1, using thermal oxide method by silica spacer medium layer growth dielectric substrate is made on the monosilicon；
Step 2, be sequentially prepared the titanium of 20nm thickness and the platinum of 150nm thickness is used as first by the use of sputtering method in insulated substrate surface
Electrode；
Step 3, the method using magnetron sputtering, using ZnO as sputtering target material, using the mixed gas of oxygen and argon gas as
Sputtering atmosphere, underlayer temperature are room temperature, prepare ZnO film, the thickness of prepared ZnO film is 35nm；
Step 4, made using the method for electron beam evaporation combination mask plate on the ZnO film of argon plasma bombardment processing
It is 50nm to make second electrode, second electrode thickness made of platinum；
Step 5, using inductively coupled plasma etching method prepare isolation on the acquired architecture basics of step 4
Device architecture.
The I-E characteristic of device manufactured in the present embodiment is tested using analyzing parameters of semiconductor tester.In electricity
Press the I-E characteristic that the device is tested under continuous scan pattern.Scan bias voltage is added in second electrode and first electrode.
The I-E characteristic test result of device is shown in Fig. 7 (numeral 1,2,3 in figure shows voltage scanning order), device
Part is in high resistance state at the beginning, it is necessary to which the larger electric forming process (3V) of a voltage, makes device from initial high-resistance state
It is changed into low resistance state.When voltage continues to scan to 1V from 0V, device current declines suddenly, and high resistant is transformed back into from low resistance state
State, that is, occur reseting procedure.When voltage is scanned to 1.3V from 0V again, device sports low resistance state from high-impedance state again, and occurs
Set process.The transition process of the high low resistance state can repeat.
Comparative example 2
The storage unit of resistive random access memory (RRAM) prepared by this comparative example, including dielectric substrate, dielectric substrate is by monocrystalline
Silicon is formed with the silica spacer medium layer for being grown in monocrystalline silicon surface, and the first electricity is set on silica spacer medium layer
Pole, first electrode are made of the titanium of 20nm thickness and the platinum of 150nm thickness；Oxygen plasma bombardment processing is set in first electrode surface
ZnO film intermediate layer, intermediate layer thickness 40nm, the surface in intermediate layer sets second electrode made of copper, second electrode
Thickness is 50nm.
The preparation method of the storage unit of above-mentioned resistive random access memory (RRAM) is：
Step 1, using thermal oxide method by silica spacer medium layer growth dielectric substrate is made on the monosilicon；
Step 2, be sequentially prepared the titanium of 20nm thickness and the platinum of 150nm thickness is used as first by the use of sputtering method in insulated substrate surface
Electrode；
Step 3, the method using magnetron sputtering, using ZnO as sputtering target material, using the mixed gas of oxygen and argon gas as
Sputtering atmosphere, underlayer temperature are room temperature, prepare ZnO film, the thickness of prepared ZnO film is 42nm.Then in magnetron sputtering
In equipment cavity, at room temperature, power 100W, to ZnO film oxygen plasma bombardment processing 60min, obtains oxygen plasma
The ZnO film of body bombardment processing, processing rear film thickness is 40nm；
Step 4, made using the method for electron beam evaporation combination mask plate on the ZnO film of argon plasma bombardment processing
Make the second electrode being made of copper, second electrode thickness is 50nm；
Step 5, using inductively coupled plasma etching method prepare isolation on the acquired architecture basics of step 4
Device architecture.
The I-E characteristic of device manufactured in the present embodiment is tested using analyzing parameters of semiconductor tester.In electricity
Press the I-E characteristic that the device is tested under continuous scan pattern.Scan bias voltage is added in second electrode and first electrode.
The initial current of device-voltage characteristic test result is shown in that (numeral 1,2,3 in figure shows that voltage scanning is suitable to Fig. 8
Sequence), device is in high resistance state at the beginning, it is necessary to the larger electric forming process (3.1V) of a voltage, makes device from initial
High-resistance state is changed into low resistance state.When voltage is scanned to -0.4V from 0V, device is maintained at low resistance state, continues from -0.4V
During (resetting voltage) scanning extremely -0.6V, the resistance of device constantly increases, and is finally changed into high-impedance state.When voltage continues
When scanning from 0V to 1.9V, device current increases suddenly, is changed into low resistance state from high-impedance state, that is, set process occurs.The height
The transition process of resistance state can repeat.
Claims (7)
1. a kind of preparation method of the storage unit of resistive random access memory (RRAM), it is characterised in that include the following steps：
Step 1, substrate surface formed conductive film as first electrode；
Step 2, existed using at least one of common sputtering, magnetron sputtering, collosol and gel, chemical vapor deposition or coating method
The first electrode surface that step 1 obtains prepares ZnO film, then carries out argon plasma bombardment processing to the ZnO film, with
ZnO film after argon plasma bombardment processing is as intermediate layer；
The argon plasma bombardment processing process is：
In magnetron sputtering apparatus cavity, carry out argon plasma bombardment processing to the ZnO film, processing power for 20~
1000W, temperature are 20~50 DEG C, and the time is 10s~10h；
Step 3, the interlayer surfaces obtained in step 2 prepare conductive film as second electrode；
Step 4, prepare the device of isolation on the architecture basics that step 3 obtains, and obtains the resistive random access memory (RRAM)
Storage unit.
2. preparation method according to claim 1, it is characterised in that the preparation process in the intermediate layer described in step 2 is：
Using the method for magnetron sputtering, using ZnO as sputtering target material, using the gaseous mixture of oxygen and argon gas as sputtering atmosphere, prepare
ZnO film, then argon plasma bombardment processing is carried out to the ZnO film, processing power are 100~500W, temperature 20
~50 DEG C, the time is 20min~5h.
3. preparation method according to claim 2, it is characterised in that the power of the argon plasma bombardment processing is
100W。
4. preparation method according to claim 1, it is characterised in that the first electrode and second electrode is independently selected
From at least one of metal, conductive oxide, conductive nitride.
5. the resistive random access memory (RRAM) that a kind of preparation method according to Claims 1 to 4 any claim obtains
Storage unit.
6. the storage unit of resistive random access memory (RRAM) according to claim 5, it is characterised in that the thickness in the intermediate layer
Spend for 2~100nm.
7. the storage unit of the resistive random access memory (RRAM) according to claim 5 or 6, it is characterised in that the substrate
It is made of monocrystalline silicon and the silica for being grown in monocrystalline silicon surface；
The first electrode is the Titanium and metal platinum being sequentially prepared；
The thickness in the intermediate layer is 20~50nm；
The second electrode is metal platinum and metallic copper.
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| CN102136487B (en) * | 2010-12-31 | 2013-09-18 | 中国科学院上海硅酸盐研究所 | Resistance-type RAM (Random Access Memory) memory unit based on zinc oxide material and preparation method thereof |
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