CN103236499A - Unipolar memristor and preparation method thereof - Google Patents
Unipolar memristor and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a unipolar nano-film memristor which comprises two electrodes and a Ba (1-x) SrxTiO3-delta nano-film arranged in the two electrodes, wherein x is large than 0 and smaller than 1, and delta is larger than 0 and smaller than 3. The principal crystalline phase of the film is measured to be Ba (1-x) SrxTiO3 through X ray diffraction, and actually is Ba (1-x) SrxTiO3-delta which is rich in oxygen deficiency namely oxygen vacancy; the film adopts a single-layer film structure; and the thickness of the film is 20 to 800 nanometers. The invention also discloses a preparation method of the unipolar nano-film memristor. The unipolar nano-film memristor is particularly applicable to general circuit theoretical research and circuit design, has generality and universality, is low in cost and is easily realized physically.
Description
Technical field
The present invention relates to the nonlinear circuit application, be specifically related to a kind of one pole type memristor and preparation method thereof.
Background technology
As far back as 1971, the theoretical pioneer of international nonlinear circuit and cell neural network, the Leon Chua (Cai Shaotang) in California, USA university Berkeley branch school foretells the existence of the 4th primary element-memristor except resistance, electric capacity, inductance in the circuit theoretically based on Circuit theory integrality in logic.In May, 2008, the researcher of HP Lab has successfully realized first workable memristor prototype in the world, thereby has confirmed the theory of the relevant memristor of Chua, has caused worldwide strong interest.Because memristor has non-volatile, cynapse function and nano-scale structures, at high-density nonvolatile memory, artificial neural net, large scale integrated circuit, reconfigurable logic and FPGA (Field Programmable Gate Array), bioengineering, pattern recognition, fields such as signal processing have great application prospect, will be unlimited for making the storage precision, the non-volatile memory device of superelevation storage density, have the artificial neural net that to regulate synapse power and similar human brain mode and handle with the development of the analog computer of contact details etc. and pave the way, bring revolutionary change for manufacturing and the operational mode of computer.As a kind of new basic circuit elements, the appearance of memristor has increased the variation of circuit element, for Circuit theory research and circuit design provide a kind of brand-new development space.
Along with the discovery of HP memristor, the scientific research institution that is engaged in resistive storage research has more in the world also carried out the research of relevant memristor in kind aspect in succession with the scholar, and new recalling the resistance material and recall resistance body system report constantly arranged.Present research is recalled on the mechanism of resistive energy from realizing, can be divided into based on the boundary migration model, based on the electron spin blocking model, based on Transformation Mechanism, based on the silk conductive mechanism etc.Domestic research to memristor at present is also fewer, lays particular emphasis on mostly in the existing research and recalls resistance circuit and systematic research.Although memristor research has in recent years obtained bigger progress, we will see that also as a basic circuit element, memristor research is just at the early-stage, mainly shows the following aspects:
(1) constantly have in recent years and new recall the resistance material and recall resistance body system report, but the memristor model of physics realization at present also seldom and single relatively (mostly being bipolar device), behavior is described to memristor still not to have the pervasive model of unification.
Bao Dao memristor in kind is mostly used at certain class or is simulated certain function (as high-density nonvolatile memory, Crossbar Latch technology, analog neuron cynapse) and propose in recent years, adopt switch model and the working mechanism with bipolarity resistive behavior (be its resistive behavior with institute making alive polarity relevant) similar with the HP memristor mostly, and complex manufacturing technology, cost height are for research memristor characteristic, recall resistance circuit theory and design of electronic circuits etc. and do not have generality and universality.
(2) as the novel basic circuit elements of a class, memristor with the behavior of unipolarity resistive is irrelevant because of its resistive behavior and institute's making alive polarity, has more generality and universality for memristor specificity analysis and general circuit theoretical research and circuit design.But rarely has one pole type memristor report in kind at present.People are finding to recall the resistance behavior to the research basis of resistance-variable storing device, and resistive research is to recall the experiment basis that resistance is found.And research and physics realization have the memristor in kind of unipolarity resistive behavior, have more generality and universality for memristor specificity analysis and general circuit theoretical research and circuit design, have great importance.Document [T.Driscoll, H.T.Kim, B.G.Chae, et al., Phase-transition driven memristive system.Appl.Phys.Lett, 2009,95 (4): 043505] Bao Dao the VO2 memristor based on Transformation Mechanism, though be one pole type memristor, but since this memristor recall inhibition effect based on metal-insulator phase transition, and phase transition process needs the uniform temperature condition, so this memristor has a fatal defective: only could realize in certain temperature range that it recalls inhibition effect.
(3) still be unrealized at present and commercially produce.Most researchers is difficult to obtain a real memristor element, when causing Many researchers at the research memristor and recalling resistance circuit, can't carry out the hardware experiments on the real physical meaning in default of the memristor element, more be to rely on the research that experimentizes of emulation or analog circuit.Yet memristor simulation model and analog circuit differ greatly from the memristor characteristic of reality, and the hardware that carries out with analog circuit is realized more considerations also is simulation memristor Mathematical Modeling and ignored the essential physical characteristic of memristor.
Summary of the invention
The technical problem to be solved in the present invention provides and a kind ofly is specially adapted to general circuit theoretical research and circuit design, has generality and universality, cheap and be easy to the one pole type memristor of physics realization.
One pole type nano thin-film memristor of the present invention comprises two electrodes and places Ba between the two
(1-x)Sr
xTiO
3-δNano thin-film, wherein, 0<x<1,0<δ<3.
One pole type nano thin-film memristor of the present invention, wherein to record the principal crystalline phase of described film be Ba to X-ray diffraction
(1-x)Sr
xTiO
3, use ac impedance spectroscopy and disclose its ppm level electrical property microstructure, can find that this film is actual in being rich in the Ba that oxygen defect is the oxygen room
(1-x)Sr
xTiO
3-δ
One pole type nano thin-film memristor of the present invention, wherein said film is the single thin film structure, thickness is the 20-800 nanometer.This memristor is a kind of monofilm memristor based on new model, and it is with the duplicature reported and even multilayer film memristor structure compared and manufacture craft is simple, cost is low, be convenient to industrialization production.Simultaneously, owing to it does not have switching effect for the monofilm memristor, its resistive behavior is the unipolarity resistive behavior irrelevant with institute making alive polarity, has more generality and universality for memristor specificity analysis and general circuit theoretical research and circuit design.
One pole type nano thin-film memristor of the present invention, wherein said memristor is charge carrier with hole and the ionized oxygen ion that produces under bias voltage, under electric field action, rely on the variation of the variation realization device resistance of described hole and described ionized oxygen ion generation, and its resistive behavior and institute's making alive polarity are irrelevant, are the behavior of unipolarity resistive.
A kind of Ba
(1-x)Sr
xTiO
3-δThe preparation method of nano thin-film comprises the steps:
(1) with barium acetate Ba (CH
3COO)
2With strontium acetate Sr (CH
3COO)
2Mixed in molar ratio by (1-x): x is dissolved in glacial acetic acid CH
3COOH stirs 15-30min and obtains compound;
(2) in the compound in final stoicheiometry Ba:Ti=(1-x): 1 ratio adds butyl titanate Ti (OC
4H
9)
4, stir 30-60min, filter;
(3) add glacial acetic acid CH in the solution after filter
3COOH dilutes solution, for the concentration that improves after the solution dilution that plated film efficient and quality select for use is high slightly, is 0.2-0.5mol/L, and it is standby as precursor sol to filter the back;
(4) plated film: with single crystalline Si or Al
2O
3Substrate immerses in the described precursor sol, obtains dissolved glue film, with described dissolved glue film oven dry, makes sol-hydrolysis afterwards, obtains gel film;
(5) behind the repeating step (4) 3-10 time, the gel mould that obtains is at last heat-treated, obtain the film of 20-800 nano thickness.
Ba of the present invention
(1-x)Sr
xTiO
3-δThe preparation method of nano thin-film, wherein the film plating process in the step (4) adopts czochralski method: substrate is immersed in the described precursor sol, and the speed with 0.5-1cm/s behind the 10-60s vertically lifts, horizontal obtains dissolved glue film, afterwards with described dissolved glue film oven dry, make sol-hydrolysis, obtain gel film.
Ba of the present invention
(1-x)Sr
xTiO
3-δThe preparation method of nano thin-film, wherein the film plating process in the step (4) adopts spin-coating method: at first substrate is fixed on the sol evenning machine, the precursor sol rotation is coated on the substrate again, rotating speed is 3000-8000r/min, and time 30-60s obtains dissolved glue film; With described dissolved glue film oven dry, make sol-hydrolysis afterwards, obtain gel film.
Ba of the present invention
(1-x)Sr
xTiO
3-δThe preparation method of nano thin-film wherein, in order to prevent having solute to separate out behind the solution left standstill, also comprises in the step (1) adding acetylacetone,2,4-pentanedione CH before stirring
3COCH
2COCH
3Used as stabilizers, addition are the 5%-20% of quality of acetic acid.
Ba of the present invention
(1-x)Sr
xTiO
3-δThe preparation method of nano thin-film, wherein, in the step (4) described dissolved glue film is dried 10-20min down at 100-150 ℃, under this bake out temperature temperature retention time condition, both guaranteed that dissolved glue film was transformed into efficient and the quality of gel mould, and avoided the too high or overlong time of temperature to cause gel mould to damage again; In the step (5), described gel mould is at 700-800 ℃ of heat treatment 10-30min, under this heat treatment temperature and temperature retention time condition, efficient and the quality of gel mould dense sintering had both been guaranteed, avoid temperature to cross low and the densification inadequately of the too short film of temperature retention time again, the perhaps too high and long damage distortion that causes film and electrode of temperature retention time of temperature.
A kind of preparation method of one pole type nano thin-film memristor comprises the steps: at first at single crystalline Si or Al
2O
3Plate one deck electrode on the substrate, then by Ba of the present invention
(1-x)Sr
xTiO
3-δThe preparation method of nano thin-film plates Ba at electrode
(1-x)Sr
xTiO
3-δNano thin-film is at last at Ba
(1-x)Sr
xTiO
3-δPlate one deck electrode on the nano thin-film again.Wherein, thickness of electrode is pressed actual needs between 50nm-50um, and electrode material is Au, Ag, In-Ga or Pt.
Provided by the invention based on Ba
(1-x)Sr
xTiO
3-δThe memristor of nano thin-film, it recalls resistance mechanism and Mathematical Modeling is specially:
This memristor is by being sandwiched in two individual layer Ba between the electrode
(1-x)Sr
xTiO
3-δNano thin-film constitutes.When a voltage or electric current were added on this device, because film thickness is nanoscale, very little voltage will produce huge electric field, Ba
(1-x)Sr
xTiO
3-δO can take place with airborne oxygen in the surface that contacts with air under bias effect
2+ 4e
--→ 2O
2-Reaction produces the hole and make in the film.Simultaneously, influenced by bias effect O takes place
2--→ e
-+ O
-, hole and ionized oxygen ion (O
-) directed mobile under electric field action as main charge carrier, along with hole and ionized oxygen ion (O
-) variation of generation can cause the resistance variations between two electrodes, corresponding film presents minimum (R with it
Min) or maximum (R
Max) two kinds of different resistance, this is Ba
(1-x)Sr
xTiO
3-δRepresent the mechanism of recalling the resistance characteristic.Now use a certain moment Ba of O (t) expression
(1-x)Sr
xTiO
3-δThe hole that under bias effect, produces amount, M represents the maximum void amount that produces under the bias effect, v represents to produce under the bias effect speed in hole.Because hole and ionized oxygen ion (O
-) generation relevant with size of current and duration (be electric charge accumulation) thereof by it:
, that is:
Therefore, film resistor is it by the function of electric charge: work as R
Min<<R
MaxThe time,
Because bias voltage (electric current) interrupts not having the electric field of driving in the rear film, and motions such as each ion, electronics, hole are inactive at normal temperatures, hole and ionized oxygen ion (O in the film
-) amount can't return the preceding state of biasing (electric current by), therefore has memory effect and resistance when keeping bias voltage (electric current) to interrupt.
One pole type nano thin-film memristor of the present invention and preparation method thereof difference from prior art is that the present invention proposes and physics realization one class manufacture craft is simple, cost is low, be easy to realize and have more the novel passive of generality and universality and do not have the one pole type memristor element of rectifying effect, adopts based on Ba
(1-x)Sr
xTiO
3-δThe single-layer membrane structure of material, is recalled the unique novel features of resistance mechanism and Mathematical Modeling at the behavior of unipolarity resistive; The present invention has simplified the manufacture craft of nanometer memristor element, reduces manufacturing cost, is specially adapted to general circuit theoretical research and circuit design, specifically has the following advantages:
Based on Ba
(1-x)Sr
xTiO
3-δThe memristor of material, its working mechanism and Mathematical Modeling novelty, and have the behavior of unipolarity resistive and have more generality and universality.Ba of the present invention
(1-x)Sr
xTiO
3-δMemristor be a class based under bias effect with hole and ionized oxygen ion (O
-) the solid electrolyte memristor that conducts electricity for charge carrier.Such memristor has been abandoned TiO
2Memristor, WO
3Memristor, Ag/Ag
2The rectified action of S memristor and Ag/Si memristor, be not at computer memory system or human mind system and research and develop, no special purpose or application background, be a kind ofly to change with the sub-generation of bias voltage download stream, and cause the passive electric circuit element (being that its resistive behavior and institute's making alive polarity have nothing to do) of the unipolarity resistive behavior that its resistance changes.As a kind of basic passive electric circuit element, one pole type memristor for research memristor characteristic, recall resistance circuit theory and design of electronic circuits etc. and have more generality and universality.
Ba of the present invention
(1-x)Sr
xTiO
3-δThe memristor manufacture craft is simple, cost is low, is easy to carry out physics realization, and described memristor belongs to single-layer membrane structure, and the employing combination of sol-gel lifts or the spin-coating method plated film is realized Ba
(1-x)Sr
xTiO
3-δThe making of nano thin-film.In whole process of preparation, only need colloidal sol preparation, plated film, three steps of gel can realize the preparation of nano thin-film, simplified manufacture craft greatly; Secondly, film preparation only needs collosol and gel platform and thermostatic drying chamber to finish, and equipment is extremely simple; Simultaneously, the required raw material of preparation film are common chemical agent, and are cheap.Therefore, the Ba of invention
(1-x)Sr
xTiO
3-δIt is simple that memristor and the memristor of having reported are at present compared manufacture craft, and manufacturing cost is greatly diminished, and is easy to physics realization.
Below in conjunction with accompanying drawing to Ba of the present invention
(1-x)Sr
xTiO
3-δMemristor is described further.
Description of drawings
Fig. 1 is the one pole type nano thin-film memristor structural representation under one embodiment of the present invention;
Fig. 2 is the Mathematical Modeling of one pole type nano thin-film memristor M of the present invention (q);
Embodiment
As shown in Figure 1, one pole type nano thin-film memristor of the present invention comprises two electrodes 1 and the nano thin-film structure 2 that is placed in one, and Fig. 2 is the Mathematical Modeling of one pole type nano thin-film memristor M of the present invention (q), and the preparation method of described nano thin-film structure 2 is as follows:
(1) with barium acetate Ba (CH
3COO)
2With strontium acetate Sr (CH
3COO)
2Press the mixed in molar ratio of 9:1, be dissolved in acetic acid CH
3COOH adds an amount of acetylacetone,2,4-pentanedione CH
3COCH
2COCH
3Used as stabilizers stirs 15min and obtains compound;
(2) again in the compound in the ratio of final stoicheiometry Ba:Ti=9:10, add butyl titanate Ti (OC
4H
9)
4, stir 30min, filter;
(3) add an amount of glacial acetic acid CH in the solution after filter
3COOH is diluted to 0.3mol/L, and is standby as presoma after filtering;
(4) substrate is immersed in the precursor sol, the speed with 1cm/s behind the 30s vertically lifts, and horizontal obtains dissolved glue film, and dissolved glue film is dried 15min down at 120 ℃, makes sol-hydrolysis, obtains gel film;
(5) step (4) is repeated 10 times after, the gel mould that obtains at last at 700-750 ℃ of heat treatment 10-30min, is obtained the product that thickness is the 20-800 nanometer.
Add in the composition of raw materials, barium acetate: strontium acetate: butyl titanate=8:2:10(mol ratio), other are with embodiment 1.
Embodiment 3
Add in the composition of raw materials, barium acetate: strontium acetate: butyl titanate=7:3:10(mol ratio), the mixing time in the step (1) is 30min; The acetylacetone,2,4-pentanedione addition is 5% of quality of acetic acid; Mixing time in the step (2) is 40min; Glacial acetic acid concentration in the step (3) is 0.5mol/L; In the step (4), substrate is immersed in the precursor sol, the speed with 0.5cm/s behind the 60s vertically lifts, and described dissolved glue film is dried 10min down at 100 ℃, and number of repetition is 3 in the step (5), and gel mould is at 700 ℃ of heat treatment 10min, and other are with embodiment 1.
Embodiment 4
Add in the composition of raw materials, barium acetate: strontium acetate: butyl titanate=6:4:10(mol ratio), the mixing time in the step (1) is 20min; The acetylacetone,2,4-pentanedione addition is 20% of quality of acetic acid; Mixing time in the step (2) is 60min; Glacial acetic acid concentration in the step (3) is 0.2mol/L; Film plating process in the step (4) adopts the spin-coating method plated film: at first substrate is fixed on the sol evenning machine, again the precursor solution rotation is coated on the substrate, rotating speed is 3000r/min, time 60s, obtain dissolved glue film, described dissolved glue film is dried 20min down at 150 ℃, and number of repetition is 5 in the step (5), gel mould is at 800 ℃ of heat treatment 30min, and other are with embodiment 1.
Embodiment 5
Add in the composition of raw materials, barium acetate: strontium acetate: butyl titanate=5:5:10(mol ratio), the mixing time in the step (1) is 25min; The acetylacetone,2,4-pentanedione addition is 15% of quality of acetic acid; Mixing time in the step (2) is 50min; Glacial acetic acid concentration in the step (3) is 0.4mol/L; Film plating process in the step (4) adopts the spin-coating method plated film: at first substrate is fixed on the sol evenning machine, again the precursor solution rotation is coated on the substrate, rotating speed is 8000r/min, time 30s, obtain dissolved glue film, described dissolved glue film is dried 10min down at 100 ℃, and number of repetition is 8 in the step (5), gel mould is at 750 ℃ of heat treatment 20min, and other are with embodiment 1.
Embodiment 6
Add in the composition of raw materials, barium acetate: strontium acetate: butyl titanate=4:6:10(mol ratio), other are with embodiment 1.
Embodiment 7
Add in the composition of raw materials, barium acetate: strontium acetate: butyl titanate=3:7:10(mol ratio), other are with embodiment 1.
Embodiment 8
Add in the composition of raw materials, barium acetate: strontium acetate: butyl titanate=2:8:10(mol ratio), other are with embodiment 1.
Embodiment 9
Add in the composition of raw materials, barium acetate: strontium acetate: butyl titanate=1:9:10(mol ratio), other are with embodiment 1.
A kind of preparation method of one pole type nano thin-film memristor comprises the steps: at first at single crystalline Si or Al
2O
3Plate one deck electrode on the substrate, then by Ba of the present invention
(1-x)Sr
xTiO
3-δThe preparation method of nano thin-film plates Ba at electrode
(1-x)Sr
xTiO
3-δNano thin-film is at last at Ba
(1-x)Sr
xTiO
3-δPlate one deck electrode on the nano thin-film again.Wherein, thickness of electrode is pressed actual needs between 50nm-50um, and electrode material is Au, Ag, In-Ga or Pt.
Embodiment 10~15 is Ba
(1-x)Sr
xTiO
3-δThe top electrode of nano thin-film is handled, and all adopts the prescription of example 2, and the technological parameter in the preparation process of example 10~15 is as shown in table 1.
The technological parameter of table 1 example 10~15
Example number | Electrode material | The top electrode mode | Heat treatment temperature (℃) |
Embodiment 10 | Au | Printing | 800 |
Embodiment 11 | Au | Deposition | Room temperature |
Embodiment 12 | Ag | Printing | 600 |
Embodiment 13 | In-Ga | Printing | Room temperature |
Embodiment 14 | Pt | Printing | 900 |
Embodiment 15 | Pt | Deposition | Room temperature |
Above-described embodiment is described preferred implementation of the present invention; be not that scope of the present invention is limited; design under the prerequisite of spirit not breaking away from the present invention; various distortion and improvement that those of ordinary skills make technical scheme of the present invention all should fall in the definite protection range of claims of the present invention.
Claims (10)
1. one pole type nano thin-film memristor is characterized in that: comprise two electrodes and place Ba between the two
(1-x)Sr
xTiO
3-δNano thin-film, wherein, 0<x<1,0<δ<3.
2. one pole type nano thin-film memristor according to claim 1, it is characterized in that: the principal crystalline phase that X-ray diffraction records described film is Ba
(1-x)Sr
xTiO
3, actual in being rich in the Ba that oxygen defect is the oxygen room
(1-x)Sr
xTiO
3-δ
3. one pole type nano thin-film memristor according to claim 2, it is characterized in that: described film is the single thin film structure, thickness is the 20-800 nanometer.
4. according to claim 1 or 2 or 3 described one pole type nano thin-film memristors, it is characterized in that: described memristor is charge carrier with hole and the ionized oxygen ion that produces under bias voltage, under electric field action, rely on the variation of the variation realization device resistance of described hole and described ionized oxygen ion generation, and its resistive behavior and institute's making alive polarity are irrelevant, are the behavior of unipolarity resistive.
5. described Ba of above-mentioned any claim
(1-x)Sr
xTiO
3-δThe preparation method of nano thin-film is characterized in that, comprises the steps:
(1) with barium acetate and the strontium acetate mixed in molar ratio by (1-x): x, is dissolved in glacial acetic acid, stirs 15-30min and obtain compound;
(2) in the compound in final stoicheiometry Ba:Ti=(1-x): 1 ratio adds butyl titanate, stirs 30-60min, filters;
(3) add glacial acetic acid in the solution after filter solution is diluted to 0.2-0.5mol/L, it is standby as precursor sol to filter the back;
(4) plated film: with single crystalline Si or Al
2O
3Substrate immerses in the described precursor sol, obtains dissolved glue film, with described dissolved glue film oven dry, makes sol-hydrolysis afterwards, obtains gel film;
(5) behind the repeating step (4) 3-10 time, the gel mould that obtains is at last heat-treated, obtain the film of 20-800 nano thickness.
6. preparation method according to claim 5, it is characterized in that: the film plating process in the step (4) adopts czochralski method: substrate is immersed in the described precursor sol, speed with 0.5-1cm/s behind the 10-60s vertically lifts, horizontal, obtain dissolved glue film, with described dissolved glue film oven dry, make sol-hydrolysis afterwards, obtain gel film.
7. preparation method according to claim 5, it is characterized in that: the film plating process in the step (4) adopts spin-coating method: at first substrate is fixed on the sol evenning machine, again the precursor sol rotation is coated on the substrate, rotating speed is 3000-8000r/min, time 30-60s obtains dissolved glue film, afterwards with described dissolved glue film oven dry, make sol-hydrolysis, obtain gel film.
8. according to claim 6 or 7 described preparation methods, it is characterized in that: also comprise in the step (1) adding the acetylacetone,2,4-pentanedione used as stabilizers before stirring, addition is the 5%-20% of quality of acetic acid.
9. preparation method according to claim 8 is characterized in that: in the step (4), described dissolved glue film is dried 10-20min down at 100-150 ℃; In the step (5), described gel mould is at 700-800 ℃ of heat treatment 10-30min.
10. the preparation method of an one pole type nano thin-film memristor is characterized in that: comprise the steps:
At first at single crystalline Si or Al
2O
3Plate one deck electrode on the substrate, plate Ba by the mode of claim 5 at electrode afterwards
(1-x)Sr
xTiO
3-δNano thin-film is at last at Ba
(1-x)Sr
xTiO
3-δPlate one deck electrode on the nano thin-film again; Wherein, described thickness of electrode is pressed actual needs between 50nm-50um, and electrode material is Au, Ag, In-Ga or Pt.
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