CN107331771A - A kind of low energy consumption, multi-functional Multilayered Nanowires resistance-variable storing device - Google Patents
A kind of low energy consumption, multi-functional Multilayered Nanowires resistance-variable storing device Download PDFInfo
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- 229910052760 oxygen Inorganic materials 0.000 claims description 2
- 239000001301 oxygen Substances 0.000 claims description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims 2
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- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 6
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- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/20—Multistable switching devices, e.g. memristors
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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
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- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/011—Manufacture or treatment of multistable switching devices
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
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Abstract
The invention provides a kind of low energy consumption, multi-functional Multilayered Nanowires resistive material and its preparation method and application, the material includes the conductive layer and insulating layer arranged along nano wire longitudinal periodicity.The present invention increases the number of defects in insulating barrier by being distributed the magnetic conductive particle of certain amount in its insulating barrier initiatively.When the material of the present invention is used to prepare resistance-variable storing device, these defects contribute to the formation of conductive filament under DC Electric Field, so as to reduce the operating voltage that electroluminescent resistive effect is answered, make its shift voltage as little as 1.2 ± 0.2V from from high-impedance state to low resistance state, shift voltage as little as 0.56 ± 0.14V from low resistance state to high-impedance state, and electric excitation process is not needed before resistive test, energy consumption is effectively reduced.Moreover, before and after electroluminescent resistive, the magnetic of the device also has certain modulation.Therefore, the Multilayered Nanowires are a kind of multifunction devices answered with the electroluminescent resistive effect of low energy consumption and Effective Regulation can be carried out to magnetic.
Description
Technical field
The invention belongs to memory technology field, and in particular to a kind of low energy consumption, multi-functional Multilayered Nanowires resistive are deposited
Reservoir.
Background technology
In recent years, received based on the resistance-variable storing device that electroluminescent resistive effect is answered as a kind of new nonvolatile memory
Academia and the extensive concern of industrial quarters.Electroluminescent resistive phenomenon is present in many binary oxide thin-film materials, phenomenon production
Raw the reason for, is often relevant with the formation and disconnection of conductive filament.Conductive filament in many research discoveries, binary oxide thin-film material
It is randomly formed, so as to cause the electroluminescent change resistance performance of thin-film material unstable, has a strong impact on its application.Moreover, very
Polyoxide, which is required to larger driving voltage, could produce electroluminescent resistive behavior so that surveyed by its obtained resistance-variable storing device
Try and driving voltage must be imposed before to carry out activation manipulation, this adds energy consumption to a certain extent.Therefore, in the urgent need to
Exploitation design low energy consumption, the new material of high stability meet the demand of resistive device practical application.
One-dimensional nano line is transmitted due to electronics in the passage by space constraints, can receive conductive filament local area control
In rice noodles, reduce the randomness of conductive filament formation.Energy when being designed into nanowire array structure applied to electroluminescent resistive device
Enough effectively to solve the problem of electroluminescent change resistance performance is unstable, every nano wire all can be as a memory cell, thus in addition
Storage density will also be increased substantially.However, the operating voltage of traditional nanowire resistance change memory is all higher, and resistive is surveyed
The electric excitation process of a higher voltage is also needed to before examination, binary oxide thin-film material high energy consumption can not be still solved not
Foot.Therefore, technical paper " Using binary resistors to achieve multilevel resistive
switching in multilayer NiO/Pt nanowire arrays(NPG Asia Materials,2014,6:
E85 a kind of preparation method of NiO/Pt Multilayered Nanowires resistance-variable storing device is disclosed in) ", this method uses porous anode
Aluminium, by the way that W metal and Pt metal are carried out into alternating deposit in the template duct, obtains Ni/Pt multi-layer nanos as template
Line, then by Ni complete oxidations, NiO/Pt multi-layer nano linear arrays are obtained, and be made using this nano-wire array as resistive medium
Multilayered Nanowires resistance-variable storing device.Multilayered Nanowires arranged regular in resistance-variable storing device made from above-mentioned technology, and the resistive
The operating voltage of memory is smaller, shift voltage (V from its high-impedance state to low resistance stateSET) as little as 3.24V, and low resistance state is to high resistant
Shift voltage (the V of stateRESET) as little as -1.20V.Unfortunately, the resistance-variable storing device in above-mentioned technology is surveyed in resistive
Still need the process of an electric excitation before examination, and driving voltage is~15V, and this is undoubtedly also increased energy consumption.So,
How resistance-variable storing device when test and use required greater energy consumption is effectively reduced, and being that current this area is urgently to be resolved hurrily asks
Topic.
The content of the invention
The technical problems to be solved by the invention are to overcome existing Multilayered Nanowires resistance-variable storing device testing and making
The problem of used time energy consumption is higher, so provide one kind operating voltage can be greatly reduced, do not need electric excitation process and can realize it is electric/
The Multilayered Nanowires resistance-variable storing device of the double store functions of magnetic.
The technical scheme that the present invention is used to achieve the above object is as follows：
A kind of nanowire resistance change material, including the conductive layer and insulating layer arranged along nano wire longitudinal periodicity, it is described exhausted
Edge layer is made up of insulating barrier body and the random magnetic conductive particle being scattered in the insulating barrier body.
The content of magnetic conductive particle is regulated and controled by changing the temperature and time of oxidation in the insulating barrier.
The material of the magnetic conductive particle is the one or more in iron, cobalt, nickel.
The material of the insulating barrier body is one or more oxides in iron, cobalt, nickel.
The thickness of each insulating barrier is 20~100nm.
The arrangement period number of the insulating barrier is 50~300.
The thickness of each conductive layer is 5~30nm.
A kind of method for preparing foregoing nanowire resistance change material, including：
Use electrochemical deposition normal direction that there are in the insulation template of through-hole structure two kinds of conductive materials of alternating deposit with respectively
The precursor of the conductive layer and the insulating barrier is formed, so as to obtain nano-wire array；
Expanding treatment is carried out to the template, incomplete oxidation then is carried out to the nano-wire array in oxygen-containing atmosphere
So that the precursor of the insulating barrier is changed into the insulating barrier, that is, the nanowire resistance change material is made.
By the nano-wire array temperature programming to 300~800 DEG C, 10~20h is incubated under steady temperature, is allowed to incomplete
Oxidation；
It is preferred that, in described program temperature-rise period, insulation operation is carried out at a temperature of each whole hundred；Wherein, at 100 DEG C
During with 200 DEG C, soaking time is 0.5~2h, more than 300 DEG C, and soaking time is 20~80min.
A kind of Multilayered Nanowires resistance-variable storing device, including hearth electrode, top electrode, and positioned at the hearth electrode and the top
Resistive dielectric layer between electrode, the two ends of the resistive dielectric layer are connected with the hearth electrode and the top electrode respectively, institute
Resistive dielectric layer is stated to be made up of foregoing nanowire resistance change material.
The above-mentioned technical proposal of the present invention has advantages below：
1st, nanowire resistance change material of the present invention, the magnetic for being distributed certain amount in its insulating barrier initiatively is led
Electric particle increases the number of defects in insulating barrier, and when applying extra electric field, these magnetic conductive particles can not only be served as leads
The presoma of electrical filament and the migration of oxonium ion is contributed to form conductive filament, so as to significantly reduce the operation electricity of resistance-variable storing device
Pressure, makes shift voltage (V of its high-impedance state to low resistance stateSET) as little as 1.2 ± 0.2V, the shift voltage of low resistance state steering high-impedance state
(VRESET) as little as -0.56 ± 0.14V, and the step of application driving voltage is to carry out activation manipulation can be also omitted, effectively reduce
Energy consumption.
2nd, nanowire resistance change material of the present invention, is controlled in insulating barrier by adjusting the temperature and time of oxidation
Conductive particle content, to ensure substantially to increase number of defects while insulating barrier insulating properties, so as to be more beneficial for reduction resistance
The energy consumption of transition storage.
3rd, nanowire resistance change material of the present invention, selects the material of conductive particle for magnetic metal iron, cobalt, nickel, this
In material its magnetic while electroluminescent resistive effect is answered, which occurs, for sample can also change, and that is to say nanowire resistance change of the present invention
The resistance states and magnetic state of material can simultaneously realize resistance-change memory and magnetic storage by regulating and controlling voltage.Cause
This, the application that the present invention can be further to widen random access memory provides important references.
4th, the preparation method of nanowire resistance change material of the present invention, by controlling oxidizing condition to enter nano-wire array
Row incomplete oxidation, thus just can obtain nanowire resistance change material.The preparation method of the present invention is simple, easily operated, fits very much
In industrial applications with promoting.
Brief description of the drawings
Fig. 1 a are the top view of the scanning electron microscope (SEM) photograph of Ni/Pt multi-layer nano linear arrays in embodiment 1；
Fig. 1 b are the sectional view of the scanning electron microscope (SEM) photograph of Ni/Pt multi-layer nano linear arrays in embodiment 1；
Fig. 2 is Ni/Pt Multilayered Nanowires and NiO in embodiment 1xThe X ray diffracting spectrum of/Pt Multilayered Nanowires；
Fig. 3 is NiO in embodiment 1xThe current -voltage curve figure of/Pt Multilayered Nanowires resistance-variable storing devices；
Fig. 4 is NiO in embodiment 1xThe data retention test design sketch of/Pt Multilayered Nanowires resistance-variable storing devices；
Fig. 5 is NiO in embodiment 1x/ Pt Multilayered Nanowires resistance-variable storing device is under low resistance state (LRS) and high-impedance state (HRS)
Parallel to the hysteresis curve figure in nano wire direction.
Embodiment
Technical scheme is clearly and completely described below in conjunction with accompanying drawing, it is clear that described implementation
Example is a part of embodiment of the invention, rather than whole embodiments.Based on the embodiment in the present invention, ordinary skill
The every other embodiment that personnel are obtained under the premise of creative work is not made, belongs to the scope of protection of the invention.
As long as in addition, technical characteristic involved in invention described below different embodiments does not constitute conflict just each other
It can be combined with each other.
Embodiment 1
Present embodiments provide a kind of NiOxThe preparation method of/Pt Multilayered Nanowires resistance-variable storing devices, comprises the following steps：
(1) porous anodic aluminium oxide (PAA) template is prepared using anodizing twice：
First, by high-purity aluminium flake (99.999%) 4 × 10-4Under Pa vacuum condition, 500 DEG C of annealing 2h；After annealing
PAA templates at 10 DEG C, in the mixed solution (volume ratio 1 of perchloric acid and absolute ethyl alcohol：4) electrobrightening 3min is carried out in；
Again using the aluminium flake after polishing as anode, graphite cake as negative electrode, 0.3mol/L oxalic acid as electrolyte, 5 DEG C, 40V it is constant
Anodic oxidation twice is carried out to aluminium flake under voltage, the time is 5 hours；Then, using saturation copper chloride and hydrochloric acid by volume
4：1 mixed solution reacts with aluminium base, removes aluminium base；Then through hole and reaming, time are carried out with 5wt% phosphoric acid solution again
For 50min, the PAA templates of bilateral are obtained；Finally, led using the method for magnetron sputtering in one layer of Pt of back spatter of PAA templates
Electric layer is 1 × 10 as hearth electrode, operation vacuum-4Pa, power is 20W, and Ar flows are 40scc, and sputtering time is 2000s,
Sputter rate is 0.075nm/s, and hearth electrode thickness is 150nm.
(2) Ni/Pt multi-layer nano linear arrays are prepared：
The obtained PAA templates with hearth electrode of step (1) are bonded at silver conductive adhesive on backing material and are used as work electricity
Pole, Ni/Pt Multilayered Nanowires are deposited using the three-electrode system of electrochemical workstation in template duct, Pt as to electrode,
Saturated calomel electrode is reference electrode, and electroplate liquid is 2mol/L NiSO4·6H2O、3mmol/L H2PtCl4、0.5mol/L
H3BO3Mixed solution.Depositing temperature is 22 DEG C, and deposition Ni potential is -1.3V, and deposition Pt potential is -0.29V, each Pt
The thickness of layer is 10nm, and alternate change deposition potential, deposition cycle is 200, and the Ni/Pt Multilayered Nanowires with hearth electrode are made
Array.
(3) corrosion and reaming of template in the Ni/Pt multi-layer nano linear arrays of hearth electrode are carried：
Above-mentioned Ni/Pt multi-layer nanos linear array is immersed in the mixing of 30 DEG C of 6.0wt% phosphoric acid and 1.8wt% chromic acid
Corrode 90min in solution, remove the part that wherein PAA templates do not deposit Ni/Pt Multilayered Nanowires；Then 30 DEG C are immersed in
6.0wt% phosphoric acid,diluteds in PAA templates carry out reaming 15min, make occur one between Ni/Pt Multilayered Nanowires and template hole wall
Fixed gap.
(4) Ni/Pt multi-layer nanos linear array is subjected to incomplete oxidation and NiO is madex/ Pt multi-layer nano linear arrays：
The Ni/Pt multi-layer nano linear arrays for completing reaming are put into the tube furnace of air atmosphere, temperature programming is carried out, risen
Warm speed is 5 DEG C/min, is incubated 2h at 100 DEG C, 200 DEG C respectively, 1.5h, 600 DEG C are incubated at 300 DEG C, 400 DEG C, 500 DEG C
Steady temperature under aoxidize 10h, obtain NiOx/ Pt multi-layer nano linear arrays, wherein each NiOxThe thickness of layer is 40nm.
(5) in NiOx/ Pt Multilayered Nanowires array top sets top electrode：
The NiO that step (4) is obtainedx/ Pt multi-layer nano linear arrays bottom is viscous on a si substrate, utilizes Ar Ion Beam Etching
Technology at the top of nano wire to performing etching 3min, and then covering diameter is 500 μm of mask plate at the top of it, utilizes magnetron sputtering
Technology deposits Pt top electrodes, and top electrode thickness is 40nm, obtains NiOx/ Pt Multilayered Nanowires array memories.
Respectively to Ni/Pt Multilayered Nanowires obtained above and NiOx/ Pt Multilayered Nanowires have carried out XRD tests, and it is surveyed
Test result is as shown in Fig. 2 NiOxIn/Pt Multilayered Nanowires in addition to the presence for having NiO, also a small amount of Ni simple substance is present.
To NiO obtained abovex/ Pt Multilayered Nanowires array memory carries out electroluminescent change resistance performance test, and hearth electrode connects
Ground, tests top electrode making alive its current-voltage (I-V) curve, and has carried out stability test, and test result is respectively as schemed
Shown in 3 and Fig. 4, according to Fig. 3 and Fig. 4, NiO made from the present embodimentxThe electroluminescent resistive of/Pt Multilayered Nanowires array memories
Can be as follows：
(1)VSETFor 1.2 ± 0.2V, VRESETFor -0.56 ± 0.14V；
(2) NiO obtained byx/ Pt Multilayered Nanowires array memory does not need electric excitation process, is reached first in voltage
Transformation of the high-impedance state (HRS) to low resistance state (LRS) is observed during 1.2V；
(3) on-off ratio is about 1 × 103；
The above results show that the memory that the present embodiment is provided, the presence of Ni simple substance adds lacking for resistive dielectric layer
Number is fallen into, resistive is not needed electric excitation process before testing, electroluminescent resistance can occur when external voltage reaches 1.2V first
Change effect.
The present embodiment is also to NiO obtained abovexThe HRS and LRS of/Pt Multilayered Nanowires array memories are carried out respectively
Magnetic Test, as a result the hysteresis curve obtained on parallel to its nano wire direction as shown in figure 5, show：
Before and after electroluminescent resistive, the magnetic of the memory is also changed.Saturation magnetization (Ms) and coercivity under LRS
(Hc) it is both greater than the value under HRS.
Embodiment 2
The FeO that the present embodiment is providedxThe preparation method of/Au Multilayered Nanowires resistance-variable storing devices is similar to Example 1, different
Part is that electrochemical deposition is metallic iron, is by the condition of its incomplete oxidation：Programmed rate is 10 DEG C/min,
Respectively in 100 DEG C, 200 DEG C of each insulation 0.5h, 20h is incubated at 300 DEG C, that is, obtains FeOx/ Au Multilayered Nanowires resistance-variable storing devices.
FeO made from the present embodimentxIn/Au Multilayered Nanowires resistance-variable storing devices, each FeOxThe thickness of insulating barrier is
100nm, the thickness of each Au conductive layers is 30nm, FeOx/ Au arrangement period number is 50.
Embodiment 3
The CoO that the present embodiment is providedxThe preparation method of/Pt Multilayered Nanowires resistance-variable storing devices is similar to Example 1, different
Part is that electrochemical deposition is metallic cobalt, is by the condition of its incomplete oxidation：Programmed rate is 10 DEG C/min,
Respectively in 100 DEG C, 200 DEG C of each insulation 1h, 1h, 800 DEG C of insulations are incubated respectively in 300 DEG C, 400 DEG C, 500 DEG C, 600 DEG C, 700 DEG C
15h, that is, obtain CoOx/ Pt Multilayered Nanowires resistance-variable storing devices.
CoO made from the present embodimentxIn/Pt Multilayered Nanowires resistance-variable storing devices, each CoOxThe thickness of insulating barrier is
20nm, the thickness of each Pt conductive layers is 5nm, CoOx/ Pt arrangement period number is 300.
Obviously, above-described embodiment is only intended to clearly illustrate example, and the not restriction to embodiment.It is right
For those of ordinary skill in the art, can also make on the basis of the above description it is other it is various forms of change or
Change.There is no necessity and possibility to exhaust all the enbodiments.And the obvious change thus extended out or
Among changing still in protection scope of the present invention.
Claims (10)
1. a kind of nanowire resistance change material, including the conductive layer and insulating layer arranged along nano wire longitudinal periodicity, its feature exist
In the insulating barrier is made up of insulating barrier body and the random magnetic conductive particle being scattered in the insulating barrier body.
2. nanowire resistance change material according to claim 1, it is characterised in that magnetic conductive particle in the insulating barrier
Content is by controlling the temperature and time of oxidation to be regulated and controled.
3. nanowire resistance change material according to claim 1 or 2, it is characterised in that the material of the magnetic conductive particle
For the one or more in iron, cobalt, nickel.
4. the nanowire resistance change material according to claim any one of 1-3, it is characterised in that the material of the insulating barrier body
Matter is one or more oxides in iron, cobalt, nickel.
5. the nanowire resistance change material according to claim any one of 1-4, it is characterised in that the thickness of each insulating barrier
Degree is 20~100nm.
6. the nanowire resistance change material according to claim any one of 1-5, it is characterised in that the arrangement week of the insulating barrier
Issue is 50~300.
7. the nanowire resistance change material according to claim any one of 1-6, it is characterised in that the material of the conductive layer is
Gold or platinum, the thickness of each conductive layer is 5~30nm.
8. a kind of method for preparing the nanowire resistance change material described in claim any one of 1-7, including：
Use electrochemical deposition normal direction that there are in the insulation template of through-hole structure two kinds of conductive materials of alternating deposit to be formed respectively
The precursor of the conductive layer and the insulating barrier, so as to obtain nano-wire array；
To the template carry out expanding treatment, then in oxygen-containing atmosphere to the nano-wire array carry out incomplete oxidation so that
The precursor of the insulating barrier is changed into the insulating barrier, that is, the nanowire resistance change material is made.
9. preparation method according to claim 8, it is characterised in that by the nano-wire array temperature programming to 300~
800 DEG C, 10~20h is incubated under steady temperature, incomplete oxidation is allowed to；
It is preferred that, in described program temperature-rise period, insulation operation is carried out at a temperature of each whole hundred；Wherein, at 100 DEG C and
At 200 DEG C, soaking time is 0.5~2h, more than 300 DEG C, and soaking time is 20~80min.
10. a kind of Multilayered Nanowires resistance-variable storing device, including hearth electrode, top electrode, and positioned at the hearth electrode and the top
Resistive dielectric layer between electrode, the two ends of the resistive dielectric layer are connected with the hearth electrode and the top electrode respectively, its
It is characterised by：The resistive dielectric layer is made up of the nanowire resistance change material described in claim any one of 1-7.
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