CN110277493A - A kind of novel multilayered structure having compared with Low dark curient - Google Patents
A kind of novel multilayered structure having compared with Low dark curient Download PDFInfo
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- CN110277493A CN110277493A CN201810207159.9A CN201810207159A CN110277493A CN 110277493 A CN110277493 A CN 110277493A CN 201810207159 A CN201810207159 A CN 201810207159A CN 110277493 A CN110277493 A CN 110277493A
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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 without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/20—Multistable switching devices, e.g. memristors
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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 without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/801—Constructional details of multistable switching devices
- H10N70/881—Switching materials
- H10N70/883—Oxides or nitrides
- H10N70/8836—Complex metal oxides, e.g. perovskites, spinels
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- G—PHYSICS
- G11—INFORMATION STORAGE
- G11C—STATIC STORES
- G11C11/00—Digital stores characterised by the use of particular electric or magnetic storage elements; Storage elements therefor
- G11C11/21—Digital stores characterised by the use of particular electric or magnetic storage elements; Storage elements therefor using electric elements
- G11C11/22—Digital stores characterised by the use of particular electric or magnetic storage elements; Storage elements therefor using electric elements using ferroelectric elements
Abstract
The present invention achievees the purpose that reduce film leakage current by constructing the transition zone of multilayered structure.The multilayered structure basal layer constructed selects Pt piece, buffer layer material Sr2Bi4Ti5O18, film layer material BiFeO3And Sr2Bi4Ti5O18.One side Sr2Bi4Ti5O18Material itself has lesser leakage current characteristic, after forming multilayered structure, has blocked carrier in BiFeO3Film and the interelectrode movement of Pt, so that than being deposited directly to BiFeO on ITO3The leakage current of film is small；Another aspect Sr2Bi4Ti5O18And BiFeO3The special contact condition in the interface of two-phase, also inhibits the movement of film carrier, so that than being deposited directly to BiFeO on ITO3The leakage current of film is small.
Description
Technical field
The invention belongs to technical field of electronic ceramic, and in particular to a kind of for the novel with lower of ferroelectric memory device
Multilayered structure of leakage current and preparation method thereof.
Background technique
BiFeO3A kind of single phase multi-iron material for integrating ferroelectricity and ferromagnetism, at room temperature have ferroelectric order and
Antiferromagnetic order, and there are coupling effects between ferroelectricity and ferromagnetism.BiFeO3Theoretical remanent polarization it is very high, and tie
Brilliant temperature is lower, these make BiFeO3Have in the multifunction devices such as the storage of high temperature information, sensor and MEMS huge
Big application value.
Pure phase BiFeO3Inevitably there is Bi in sintering process in the preparation temperature narrow range of film2O3、Bi2Fe4O9
Equal miscellaneous phases, while Bi element under high temperature is readily volatilized and Fe3+It is easy to appraise at the current rate as Fe2+, this all can cause a large amount of Lacking oxygens to make
BiFeO3The leakage current density of sample is very big.Since leakage current is serious, it is applied to BiFeO3Effective electric field on film will be very
It is small, cause ferroelectric domain that can not overturn, or even material can not show its excellent ferroelectricity with regard to breakdown under very low voltage
Energy.
Improve BiFeO at present3The method of film performance mainly has control thin film alignment, element doping, constructs multilayered structure
Deng.The mismatch very little of selected transition zone and prepared film sample, structure in the existing research for constructing multilayered structure
The thickness of transition zone is larger when building multilayered structure, and reduction is applied to BiFeO by this3Effective electric-field intensity on base film.Therefore,
It needs to find one kind and film leakage current is effectively reduced, construct the buffer layer material of multilayered structure.And Sr2Bi4Ti5O18Material has
Lower leakage current, with BiFeO3Mismatch it is smaller.
Summary of the invention
The purpose of the present invention is to provide a kind of and BiFeO3Mismatch is smaller, and thickness is smaller, can be effectively reduced BiFeO3
The buffer layer material of film electric leakage performance, constructs multilayered structure.
The technical solution of the present invention is as follows: a kind of novel multilayered structure having compared with low-leakage current, it includes from the bottom to top
Set gradually basal layer, transition zone, BiFeO3Layer and Sr2Bi4Ti5O18Layer, basal layer select Pt piece, and buffer layer material is
Sr2Bi4Ti5O18, film layer material BiFeO3And Sr2Bi4Ti5O18。
Heretofore described has for the novel of ferroelectric memory device compared in the multilayered structure of low-leakage current
Sr2Bi4Ti5O18The preparation process of transition zone and film layer precursor solution, with bismuth nitrate, strontium acetate, ethylene glycol, acetylacetone,2,4-pentanedione,
Butyl titanate is raw material, is synthesized using sol-gel method, the specific steps are as follows:
(1) solution A: butyl titanate levulinic is prepared according to volume ratio for the ratio of 1:1 with butyl titanate and acetylacetone,2,4-pentanedione
Ketone slowly instills in acetylacetone,2,4-pentanedione solution, and the solution mixed is continued stirring 24 hours, and it is molten to obtain the transparent A of clarification yellowish-brown
Liquid；
(2) 1.2g strontium acetate, 5.9g bismuth nitrate, 18.8ml ethylene glycol are weighed, three is sufficiently mixed, bull magnetic force is placed on and stirs
It mixes and is stirred 24 hours on device, obtain transparent B solution；
(3) B solution is added slowly in solution A, mixed solution is sufficiently stirred 24 hours, flaxen solution is obtained
C；
(4) C solution is stood 24 hours, obtains Sr2Bi4Ti5O18Precursor solution.
Heretofore described has for the novel of ferroelectric memory device compared with BiFeO in the multilayered structure of low-leakage current3
The preparation process of layer precursor solution, with bismuth nitrate, ferric nitrate, glacial acetic acid, acetylacetone,2,4-pentanedione, ethylene glycol is raw material, using colloidal sol-
Gel method synthesis, the specific steps are as follows:
(1) 9.2g bismuth nitrate is weighed first, and measurement 5ml ethylene glycol, 15ml glacial acetic acid are sufficiently mixed as solvent, are placed on bull
It is sufficiently stirred on magnetic stirring apparatus 8 hours, obtains clear solution；
(2) it measures 40ml acetylacetone,2,4-pentanedione to be added in clear solution obtained in (1), weighs 7.4g ferric nitrate and be also added to (1)
Obtained in clear solution.It is stirred 24 hours on bull magnetic stirring apparatus and obtains the translucent BiFeO of kermesinus3Presoma is molten
Liquid；
(3) 24 hours will be stood under precursor solution room temperature.
The heretofore described novel preparation work with the multilayered structure compared with low-leakage current for ferroelectric memory device
Skill, the specific steps are as follows:
(1) by transition zone Sr2Bi4Ti5O18Precursor solution is uniformly spin-coated on Pt/Ti/SiO2/ Si(100) on substrate, then
It is put on 200 DEG C of stainless steel electric hot plates and dries 2-3min；
(2) film sample tentatively dried is placed in quick anneal oven after 350 DEG C of heat preservation 180s and continues to be heated to 700 DEG C of heat preservations
300s；
(3) (1)-(2) are repeated the above steps repeatedly, until obtaining certain thickness transition zone；
(4) by BiFeO3Precursor solution is uniformly spin-coated on transition zone, is then put on 200 DEG C of stainless steel electric hot plates and is dried
2-3min；
(5) film sample tentatively dried is placed in quick anneal oven after 350 DEG C of heat preservation 180s and continues to be heated to 500 DEG C of heat preservations
300s；
(6) (3)-(4) are repeated the above steps repeatedly, until obtaining certain thickness BiFeO3Film layer；
(7) by Sr2Bi4Ti5O18Precursor solution is uniformly spin-coated in BFO film layer, is then put into 200 DEG C of stainless steel electric heating
2-3min is dried on plate；
(8) film sample tentatively dried is placed in quick anneal oven after 350 DEG C of heat preservation 180s and continues to be heated to 700 DEG C of heat preservations
300s；
(9) (7)-(8) are repeated the above steps repeatedly, until obtaining certain thickness Sr2Bi4Ti5O18Film layer.
The novel multilayered structure that has compared with low-leakage current of the present invention for ferroelectric memory device, more existing structure have
Following advantage:
1, the Sr that transition zone is selected2Bi4Ti5O18Material itself has lesser leakage current characteristic, after forming multilayered structure, blocks
Carrier is in BiFeO3Film and the interelectrode movement of Pt, so that than being deposited directly to BiFeO on ITO3The leakage current of film
It is small；
2、Sr2Bi4Ti5O18And BiFeO3The special contact condition in the interface of two-phase, also inhibits the movement of film carrier,
So that than being deposited directly to BiFeO on ITO3The leakage current of film is small.
Detailed description of the invention
Attached drawing 1 is to deposit to 130nm thickness Sr in the present invention2Bi4Ti5O18The BiFeO of transition zone3-Sr2Bi4Ti5O18Film and
It is deposited directly to BiFeO on ITO3Film leakage current densogram.
Attached drawing 2 is to deposit to 260nm thickness Sr in the present invention2Bi4Ti5O18The BiFeO of transition zone3-Sr2Bi4Ti5O18Film and
It is deposited directly to BiFeO on ITO3Film leakage current densogram.
Attached drawing 3 is to deposit to 390nm thickness Sr in the present invention2Bi4Ti5O18The BiFeO of transition zone3-Sr2Bi4Ti5O18Film and
It is deposited directly to BiFeO on ITO3Film leakage current densogram.
Specific embodiment
Case study on implementation 1
(1) heretofore described the novel of ferroelectric memory device that be used for has compared in the multilayered structure of low-leakage current
Sr2Bi4Ti5O18The preparation process of transition zone and film layer precursor solution, with bismuth nitrate, strontium acetate, ethylene glycol, acetylacetone,2,4-pentanedione,
Butyl titanate is raw material, is synthesized using sol-gel method, the specific steps are as follows: with butyl titanate and acetylacetone,2,4-pentanedione according to
The ratio that volume ratio is 1:1 prepares solution A: butyl titanate acetylacetone,2,4-pentanedione slowly instills in acetylacetone,2,4-pentanedione solution, will mix
Solution continue stirring 24 hours, obtain the transparent solution A of clarification yellowish-brown；Weigh 1.2g strontium acetate, 5.9g bismuth nitrate,
18.8ml ethylene glycol, three is sufficiently mixed, and is placed on bull magnetic stirring apparatus and is stirred 24 hours, obtains transparent B solution；
B solution is added slowly in solution A, mixed solution is sufficiently stirred 24 hours, flaxen solution C is obtained；C is molten
Liquid stands 24 hours, obtains Sr2Bi4Ti5O18Precursor solution.
(2) heretofore described the novel of ferroelectric memory device that be used for has compared with film in the multilayered structure of low-leakage current
Layer BiFeO3The preparation process of precursor solution, with bismuth nitrate, ferric nitrate, glacial acetic acid, acetylacetone,2,4-pentanedione, ethylene glycol is raw material, is adopted
It is synthesized with sol-gel method, the specific steps are as follows: weighing 9.2g bismuth nitrate first measures 5ml ethylene glycol, 15ml glacial acetic acid is made
It is sufficiently mixed for solvent, is placed on bull magnetic stirring apparatus and is sufficiently stirred 8 hours, obtain clear solution；Measure 40ml acetyl
Acetone be added to above obtained in clear solution, weigh 7.4g ferric nitrate is also added it is above obtained in clear solution.
It is stirred 24 hours on bull magnetic stirring apparatus and obtains the translucent BiFeO of kermesinus3Solution；24 hours will be stood under solution room temperature
Obtain BiFeO3Precursor solution.
(3) the heretofore described novel preparation with the multilayered structure compared with low-leakage current for ferroelectric memory device
Technique, the specific steps are as follows: by Sr2Bi4Ti5O18Transition zone precursor solution is uniformly spin-coated in Pt piece substrate, is then put into
2-3min is dried on 200 DEG C of stainless steel electric hot plates；The film sample tentatively dried is placed on 350 DEG C of heat preservations in quick anneal oven
Continue to be heated to 700 DEG C of heat preservation 300s after 180s, repeats the above steps to obtain the transition zone of 130nm thickness；By BiFeO3Presoma
Solution is uniformly spin-coated on transition zone, is then put on 200 DEG C of stainless steel electric hot plates and is dried 2-3min；It is thin by what is tentatively dried
Membrane sample, which is placed on, to be continued to be heated to 500 DEG C of heat preservation 300s after 350 DEG C of heat preservation 180s in quick anneal oven；It repeats the above steps to obtain
Until obtaining certain thickness BiFeO3Film layer；By Sr2Bi4Ti5O18Film layer precursor solution is uniformly spin-coated on BiFeO3
In film layer, then it is put on 200 DEG C of stainless steel electric hot plates and dries 2-3min；The film sample tentatively dried is placed on and is quickly moved back
Continue to be heated to 700 DEG C of heat preservation 300s after 350 DEG C of heat preservation 180s in stove, repeats the above steps to obtain 1000nm thickness
BiFeO3-Sr2Bi4Ti5O18Film layer.
Case study on implementation 2
(1) heretofore described the novel of ferroelectric memory device that be used for has compared in the multilayered structure of low-leakage current
Sr2Bi4Ti5O18The preparation process of transition zone and film layer precursor solution, with bismuth nitrate, strontium acetate, ethylene glycol, acetylacetone,2,4-pentanedione,
Butyl titanate is raw material, is synthesized using sol-gel method, the specific steps are as follows: with butyl titanate and acetylacetone,2,4-pentanedione according to
The ratio that volume ratio is 1:1 prepares solution A: butyl titanate acetylacetone,2,4-pentanedione slowly instills in acetylacetone,2,4-pentanedione solution, will mix
Solution continue stirring 24 hours, obtain the transparent solution A of clarification yellowish-brown；Weigh 1.2g strontium acetate, 5.9g bismuth nitrate,
18.8ml ethylene glycol, three is sufficiently mixed, and is placed on bull magnetic stirring apparatus and is stirred 24 hours, obtains transparent B solution；
B solution is added slowly in solution A, mixed solution is sufficiently stirred 24 hours, flaxen solution C is obtained；C is molten
Liquid stands 24 hours, obtains Sr2Bi4Ti5O18Precursor solution.
(2) heretofore described the novel of ferroelectric memory device that be used for has compared in the multilayered structure of low-leakage current
BiFeO3The preparation process of film layer precursor solution, with bismuth nitrate, ferric nitrate, glacial acetic acid, acetylacetone,2,4-pentanedione, ethylene glycol is original
Material, is synthesized using sol-gel method, the specific steps are as follows: weighing 9.2g bismuth nitrate first measures 5ml ethylene glycol, 15ml ice second
Acid is sufficiently mixed as solvent, is placed on bull magnetic stirring apparatus and is sufficiently stirred 8 hours, obtains clear solution；Measure 40ml
Acetylacetone,2,4-pentanedione be added to above obtained in clear solution, weigh 7.4g ferric nitrate is also added it is above obtained in clear solution
In.It is stirred 24 hours on bull magnetic stirring apparatus and obtains the translucent BiFeO of kermesinus3Solution；24 will be stood under solution room temperature
Hour obtains BiFeO3Precursor solution.
(3) the heretofore described novel preparation with the multilayered structure compared with low-leakage current for ferroelectric memory device
Technique, the specific steps are as follows: by Sr2Bi4Ti5O18Transition zone precursor solution is uniformly spin-coated in Pt piece substrate, is then put into
2-3min is dried on 200 DEG C of stainless steel electric hot plates；The film sample tentatively dried is placed on 350 DEG C of heat preservations in quick anneal oven
Continue to be heated to 700 DEG C of heat preservation 300s after 180s, repeats the above steps to obtain the transition zone of 260nm thickness；By BiFeO3Presoma
Solution is uniformly spin-coated on transition zone, is then put on 200 DEG C of stainless steel electric hot plates and is dried 2-3min；It is thin by what is tentatively dried
Membrane sample, which is placed on, to be continued to be heated to 500 DEG C of heat preservation 300s after 350 DEG C of heat preservation 180s in quick anneal oven；It repeats the above steps to obtain
Until obtaining certain thickness BiFeO3Film layer；By Sr2Bi4Ti5O18Film layer precursor solution is uniformly spin-coated on BiFeO3
In film layer, then it is put on 200 DEG C of stainless steel electric hot plates and dries 2-3min；The film sample tentatively dried is placed on and is quickly moved back
Continue to be heated to 700 DEG C of heat preservation 300s after 350 DEG C of heat preservation 180s in stove, repeats the above steps to obtain 1000nm thickness
BiFeO3-Sr2Bi4Ti5O18Film layer.
Case study on implementation 3
(1) heretofore described the novel of ferroelectric memory device that be used for has compared in the multilayered structure of low-leakage current
Sr2Bi4Ti5O18The preparation process of transition zone and film layer precursor solution, with bismuth nitrate, strontium acetate, ethylene glycol, acetylacetone,2,4-pentanedione,
Butyl titanate is raw material, is synthesized using sol-gel method, the specific steps are as follows: with butyl titanate and acetylacetone,2,4-pentanedione according to
The ratio that volume ratio is 1:1 prepares solution A: butyl titanate acetylacetone,2,4-pentanedione slowly instills in acetylacetone,2,4-pentanedione solution, will mix
Solution continue stirring 24 hours, obtain the transparent solution A of clarification yellowish-brown；Weigh 1.2g strontium acetate, 5.9g bismuth nitrate,
18.8ml ethylene glycol, three is sufficiently mixed, and is placed on bull magnetic stirring apparatus and is stirred 24 hours, obtains transparent B solution；
B solution is added slowly in solution A, mixed solution is sufficiently stirred 24 hours, flaxen solution C is obtained；C is molten
Liquid stands 24 hours, obtains Sr2Bi4Ti5O18Precursor solution.
(2) heretofore described the novel of ferroelectric memory device that be used for has compared with film in the multilayered structure of low-leakage current
Layer BiFeO3The preparation process of precursor solution, with bismuth nitrate, ferric nitrate, glacial acetic acid, acetylacetone,2,4-pentanedione, ethylene glycol is raw material, is adopted
It is synthesized with sol-gel method, the specific steps are as follows: weighing 9.2g bismuth nitrate first measures 5ml ethylene glycol, 15ml glacial acetic acid is made
It is sufficiently mixed for solvent, is placed on bull magnetic stirring apparatus and is sufficiently stirred 8 hours, obtain clear solution；Measure 40ml acetyl
Acetone be added to above obtained in clear solution, weigh 7.4g ferric nitrate is also added it is above obtained in clear solution.
It is stirred 24 hours on bull magnetic stirring apparatus and obtains the translucent BiFeO of kermesinus3Solution；24 hours will be stood under solution room temperature
Obtain BiFeO3Precursor solution.
(3) the heretofore described novel preparation with the multilayered structure compared with low-leakage current for ferroelectric memory device
Technique, the specific steps are as follows: by Sr2Bi4Ti5O18Transition zone precursor solution is uniformly spin-coated in Pt piece substrate, is then put into
2-3min is dried on 200 DEG C of stainless steel electric hot plates；The film sample tentatively dried is placed on 350 DEG C of heat preservations in quick anneal oven
Continue to be heated to 700 DEG C of heat preservation 300s after 180s, repeats the above steps to obtain the transition zone of 390nm thickness；By BiFeO3Film layer
Precursor solution is uniformly spin-coated on transition zone, is then put on 200 DEG C of stainless steel electric hot plates and is dried 2-3min；It will tentatively dry
Dry film sample, which is placed on, to be continued to be heated to 500 DEG C of heat preservation 300s after 350 DEG C of heat preservation 180s in quick anneal oven；Repeat above-mentioned step
Suddenly it obtains until obtaining certain thickness BiFeO3Film layer；By Sr2Bi4Ti5O18Film layer precursor solution is uniformly spin-coated on
BiFeO3In film layer, then it is put on 200 DEG C of stainless steel electric hot plates and dries 2-3min；The film sample tentatively dried is placed on
Continue to be heated to 700 DEG C of heat preservation 300s after 350 DEG C of heat preservation 180s in quick anneal oven, repeats the above steps to obtain 1000nm thickness
BiFeO3-Sr2Bi4Ti5O18Film layer.
Due to using above structure scheme, the present invention is for the novel with more compared with low-leakage current of ferroelectric memory device
Layer structure, compares existing structure and has the advantage that
1, the Sr that transition zone is selected2Bi4Ti5O18Material itself has lesser leakage current characteristic, after forming multilayered structure, blocks
Carrier is in BiFeO3Film and the interelectrode movement of Pt, so that than being deposited directly to BiFeO on ITO3The leakage current of film
It is small；
2、Sr2Bi4Ti5O18And BiFeO3The special contact condition in the interface of two-phase, also inhibits the movement of film carrier,
So that than being deposited directly to BiFeO on ITO3The leakage current of film is small.
Claims (3)
1. a kind of novel multilayered structure having compared with Low dark curient for ferroelectric memory device, it is characterised in that: it includes under
Supreme to set gradually substrate layer (1), transition zone (2), film layer (3), transition zone (2) material is Sr2Bi4Ti5O18, described
Film layer (3) material be BiFeO3And Sr2Bi4Ti5O18。
2. the novel multilayered structure having compared with Low dark curient according to claim 1 for ferroelectric memory device, special
Sign is: substrate layer (1) material is Pt/Ti/SiO2/ Si(100).
3. the novel multilayered structure having compared with Low dark curient according to claim 1 for ferroelectric memory device, special
Sign is: transition zone (2) material is Sr2Bi4Ti5O18；Material have lower leakage current, lower coercive field strength, more by force
Fatigue resistance the advantages that.
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