CN102646790B - Non-volatile memory - Google Patents
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- CN102646790B CN102646790B CN201110041908.3A CN201110041908A CN102646790B CN 102646790 B CN102646790 B CN 102646790B CN 201110041908 A CN201110041908 A CN 201110041908A CN 102646790 B CN102646790 B CN 102646790B
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- volatility memorizer
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Abstract
The invention discloses a non-volatile memory, which comprises a lower conductive layer, a resistance transition layer arranged on the lower conductive layer, an oxygen-shortage buffer layer arranged on the resistance transition layer and an upper conductive layer arranged on the oxygen-shortage buffer layer.
Description
Technical field
Present invention is directed to a kind of memory component, relate to especially a kind of resistance-type non-volatility memorizer.
Background technology
Non-volatility memorizer is in the market still take flash memory (Flash Memory) as main flow, but it has shortcomings such as operating voltage is large, service speed slow, data keeping quality is poor, will restriction flash memory the development in future.In addition,, under the trend of element micro processing procedure, effect is satisfied in wearing of excessively thin gate pole oxidation layer, will cause data keeping quality not good, is also the problem of current serious.
At present existing many new-type non-volatility memorizer materials and element comprise magnetic memory (MRAM), Ovonics unified memory (OUM) and resistance-type memory (RRAM) etc. in just actively being researched and developed.Wherein resistance-type non-volatility memorizer have that power consumption is low, operating voltage is low, write that the time of erasing is short, durability degree long, memory time long, non-destructive reads, multimode store, element processing procedure simply and the advantage such as micro.The people such as Baek utilize embolism hearth electrode to go to reduce the resistance value variation [I.G.Baek et al., in Tech.Dig.of IEDM (2005)] of two stable states; The people such as Kim utilize resilient coating iridium dioxide (IrO
2) go to improve the resistance value variation of two stable states, and can remove the danger [D.C.Kim et al., Appl.Phys.Lett., 88,232106 (2006)] that writes failure.
Often there is the problems such as transition stability is not good in traditional resistance-type non-volatility memorizer, limits its application at non-volatile memory component.Another aspect, the structure of resistance-type memory has two kinds: a transistor (transistor) and the combination (1T1R) of a resistive element and the combination (1D1R) of a diode (diode) and a resistive element, wherein 1D1R resistance-type memory have can micro to compared with the advantage of small components, but need the resistive element of a kind of monolateral resistance transitions of coupling (unipolar resistive switchingbehavior) just can reach the function of 1D1R resistance-type memory.Therefore, need the non-volatility memorizer of a kind of monolateral resistance transition (unipolar resistive switching behavior) operation, it has high durability degree, high stability, making easily and low cost and other advantages.
Summary of the invention
One embodiment of the invention provide a kind of non-volatility memorizer, comprise a lower conductiving layer; One resistance transition layer, is arranged on above-mentioned lower conductiving layer; One oxygen lacks resilient coating, is arranged on above-mentioned resistance transition layer; And conductive layer on, be arranged at above-mentioned oxygen and lack on resilient coating.
For the present invention can be become apparent, special embodiment below, and coordinate appended graphicly, be described in detail below:
Accompanying drawing explanation
Fig. 1 a is the generalized section of the non-volatility memorizer of the embodiment of the present invention.
Fig. 1 b is the generalized section of the non-volatility memorizer of comparative example.
Fig. 2 a is the electric current and voltage measurement of the non-volatility memorizer of the embodiment of the present invention.
Fig. 2 b is the electric current and voltage measurement of the non-volatility memorizer of comparative example.
Fig. 3 a is the durability degree resolution chart of the non-volatility memorizer of the embodiment of the present invention.
The durability degree resolution chart of the non-volatility memorizer of Fig. 3 b comparative example.
Fig. 4 is the storage power test of the non-volatility memorizer of the embodiment of the present invention.
Fig. 5 is the non-destructive read test of the non-volatility memorizer of the embodiment of the present invention.
Fig. 6 is the potential pulse durability degree resolution chart of the non-volatility memorizer of the embodiment of the present invention.
Main element symbol description:
500～non-volatility memorizer;
200～substrate;
202～insulating barrier;
204～titanium film;
206～platinum film;
207～lower conductiving layer;
208～resistance transition layer;
209～double-deck sull structure;
210～oxygen lacks resilient coating;
212～upper conductive layer;
Embodiment
Embodiment of the present invention system provides a kind of non-volatility memorizer, and it utilizes the change of resistance value to reach storage effect.The non-volatility memorizer system of the embodiment of the present invention adopts noble metal as hearth electrode, and zirconium dioxide (ZrO afterwards grows up
2) film is as resistance transition layer, then the zirconium dioxide (CaO:ZrO of the doping calcium oxide of growing up on resistance transition layer
2) lack resilient coating as oxygen, to form double-deck sull structure; And utilize active metal to change oxygen condition and the distribution thereof of memory film inside as top electrode.Durability degree and the stability of element when the method can significantly promote monolateral operation.
Fig. 1 a is the generalized section of the non-volatility memorizer 500 of one embodiment of the invention.The non-volatility memorizer 500 of one embodiment of the invention is to be arranged on substrate 200.The main element of non-volatility memorizer 500 comprises an insulating barrier 202, is arranged on substrate 200.One lower conductiving layer 207, is arranged on insulating barrier 202.One resistance transition layer 208, is arranged on lower conductiving layer 207.One oxygen lacks resilient coating (oxygen vacancy barrier layer) 210, is arranged on resistance transition layer 208.Conductive layer 212 on one, is located at oxygen and lacks on resilient coating 210.In an embodiment of the present invention, the scarce resilient coating 210 of resistance transition layer 208 and the oxygen on it is the double-deck sull structure 209 of common formation non-volatility memorizer 500.
In one embodiment of this invention, substrate 200 can comprise silicon substrate.Insulating barrier 202 can comprise silica membrane, and its thickness can be between between 100nm to 500nm.Lower conductiving layer 207 can be two metal layers and stacks the composite bed that forms using as hearth electrode, as shown in Figure 1a, lower conductiving layer 207 can comprise a titanium (Titanium of lower floor, Ti) film 204 and upper strata platinum (Platinum, Pt) film 206, the thickness of above-mentioned lower conductiving layer 207 can be between between 10nm to 1000nm.Resistance transition layer 208 can comprise zirconium dioxide (ZrO
2) film, its thickness can be between between 10nm to 1000nm.Oxygen lacks resilient coating 210 and can be the zirconium dioxide film with a metal oxide admixture, and wherein metal oxide admixture comprises calcium oxide (CaO), magnesium oxide (MgO), yittrium oxide (Y
2o
3) or combinations thereof, and the thickness of the scarce resilient coating 210 of oxygen can be between between 1nm to 1000nm.The upper conductive layer 212 that comprises titanium (Ti) film can be used as top electrode, and its thickness can be between between 10nm to 1000nm.
Then the manufacture method of non-volatility memorizer 500 of one embodiment of the invention will be further illustrated.First, provide a substrate 200, a for example silicon substrate, and it is carried out to RCA (Radio Corporation of America) manufacturing process for cleaning.Afterwards, can utilize high temperature furnace pipe processing procedure, the silica membrane of growing up on silicon substrate 200 is as insulating barrier 202, and insulating barrier 202 is for the leakage current between isolated and substrate 200.Then, can utilize electron beam vacuum evaporation (E-beam evaporation) or sputtering method (sputtering), on insulating barrier 202, form one deck titanium film 204.Similarly, utilize another once electron beam vacuum evaporation (E-beam evaporation) or sputtering method (sputtering), on titanium film 204, form one deck platinum film 206, above-mentioned titanium film 204 and platinum film 206 are to form a lower conductiving layer 207 (can be considered hearth electrode 207).Then, can utilize AC magnetic controlled sputtering method (RF magnetron sputtering), a zirconium dioxide (ZrO grows up on platinum film 206
2) film is as resistance transition layer 208.In an embodiment of the present invention, for example for being about 200 ℃, electricity slurry power density, the growth temperature of the resistance transition layer 208 of zirconium dioxide film is about 2.63W/cm
2, operating pressure is about 10mTorr, gas flow is about 18sccm (argon gas (Ar): oxygen (O
2)=12: 6).
Next be the generation type of describing the scarce resilient coating 210 of oxygen of the non-volatility memorizer 500 of the embodiment of the present invention.Can utilize AC magnetic controlled sputtering method, the oxygen of growing up on resistance transition layer 208 lacks resilient coating 210, and it can comprise the zirconium dioxide film with metal oxide admixture, the zirconium dioxide (CaO:ZrO of the calcium oxide that for example adulterates
2) film.In an embodiment of the present invention, oxygen lacks the growth temperature of resilient coating 210 and is about 200 ℃, electricity slurry power density and is about 2.63W/cm
2, operating pressure is about 10mTorr, gas flow is about 18sccm (argon gas (Ar): oxygen (O
2)=12: 6).In other embodiments of the invention, the metal oxide admixture that oxygen lacks resilient coating 210 can comprise magnesium oxide (MgO), yittrium oxide (Y
2o
3) or combinations thereof.
Finally, can utilize electron beam evaporation plating method area and formation position by metal light shield definition top electrode, to lack on resilient coating 210 and to grow up a platinum/titanium metal thin film as upper conductive layer 212 (can be considered top electrode 212) in oxygen.Through after above-mentioned processing procedure, form the non-volatility memorizer 500 of one embodiment of the invention.
Fig. 1 b is the generalized section of the non-volatility memorizer 600 of comparative example.Not existing together of the non-volatility memorizer 600 of comparative example and the non-volatility memorizer 500 of one embodiment of the invention only do not have the scarce resilient coating 208 of oxygen of the zirconium dioxide film of doping calcium oxide for the non-volatility memorizer 600 of comparative example, therefore, the top electrode 212 of the non-volatility memorizer 600 of comparative example is directly grown up on resistance transition layer 208, and all the other elements are all identical with the non-volatility memorizer 500 of one embodiment of the invention.
Fig. 2 a is the electric current and voltage measurement of the non-volatility memorizer 500 of one embodiment of the invention.As shown in Figure 2 a, in the time that the non-volatility memorizer 500 to the embodiment of the present invention is just applying (bearing) direct current (DC) bias, electric current can increase and increase along with voltage, when Current rise is to cut-off current (5mA), its bias voltage is for forming voltage (forming voltage), conventionally need larger bias voltage, now by reset condition (original state; O-state) be transformed into low resistance state (low resistance state; LRS, or can be described as ON-state).Then, when the non-volatility memorizer 500 of the embodiment of the present invention is bestowed to the voltage of erasing (turn-off voltage) of negative bias, approximately-element current starts to decline when 12V, the rapid current value originally that drops to of electric current in the time of-2V, the now electric current transition of low resistance state is to high resistance state (high resistance state; HRS, or can be described as OFF-state).Then, to the non-volatility memorizer 500 of the embodiment of the present invention bestow negative bias write voltage (turn-onvoltage) time, electric current can increase and increase along with voltage, approximately-arrive Current Limits flow valuve (5mA) when 3V, now high resistance state is converted to low resistance state, and this repeatedly repetitive operation of resistance transfer characteristic.That is we can utilize and control the size of bestowing bias voltage and make conversion that the non-volatility memorizer 500 of the embodiment of the present invention has a resistance to reach storage purpose, under without additional power source supply, high low resistance state all can maintain its storage state, can be used for the application of non-volatility memorizer.It should be noted that, as shown in Figure 2 a, non-volatility memorizer 500 its voltages of erasing (turn-off voltage) of the embodiment of the present invention are about-1.5V, be about-3V and write voltage (turn-on voltage), be negative value voltage, there is the characteristic of monolateral resistance transition (unipolar resistive switching behavior), be applicable to the resistance-type non-volatility memorizer of matched diodes (diode) composition 1D1R.
Fig. 2 b is the electric current and voltage measurement of the non-volatility memorizer 600 of comparative example.This element is bestowed to erasing when voltage of negative bias, approximately-element current starts to decline when 14V, the rapid current value originally that drops to of electric current in the time of-2V, the now electric current transition of low resistance state is to high resistance state; To this element bestow negative bias write voltage time, electric current can increase and increase along with voltage, approximately-arrive Current Limits flow valuve (5mA) when 3V, now high resistance state is converted to low resistance state, and this resistance transfer characteristic can repetitive operation.Show that by result the non-volatility memorizer 600 of comparative example and the non-volatility memorizer 500 of the embodiment of the present invention have similar current-voltage characteristic, therefore non-volatility memorizer 600 also has the characteristic of monolateral resistance transition.But show through durability degree test, the non-volatility memorizer 500 with the scarce resilient coating of oxygen has more outstanding durability degree characteristic, and above-mentioned durability degree test result is to be shown in 3a to 6 figure described later and relevant narration.
The non-volatility memorizer 500 of the embodiment of the present invention resistance transition mechanism be as described below.As shown in Figure 1a, it is the double-deck sull structure 209 of common formation that the zirconium dioxide resistance transition layer 208 of the non-volatility memorizer 500 of the embodiment of the present invention and the oxygen on it lack resilient coating 210, wherein the scarce resilient coating 210 of oxygen for example can be the zirconium dioxide film with metal oxide admixture, comprises calcium oxide (CaO), magnesium oxide (MgO), yittrium oxide (Y
2o
3) metal oxide admixture system as the stabilizer (stabilizer) of zirconium dioxide, so that the cubic crystal (cubic) that the crystalline state of zirconium dioxide can maintain high temperature in when cooling does not vary with temperature that generation changes mutually mutually and the variation of volume and produce rhegma, thereby can promote the electric and mechanical property that oxygen lacks resilient coating, on the other hand, these admixture capable of regulating control zirconium dioxide oxygen lack the concentration in room, make it have better ionic conductivity and excellent mechanical strength.For example, for the metal oxide admixture of calcium oxide (CaO) can provide oxygen-containing vacancy (oxygen vacancy), its defect chemistry reaction equation (1) is:
Every doping one mole calcium oxide (CaO), just manufactures a mole oxygen-containing vacancy.Therefore, the oxonium ion that the oxygen of the embodiment of the present invention lacks in resilient coating 210 can spread by above-mentioned oxygen-containing vacancy, thereby can obtain good ionic conductivity.
Fig. 3 a is durability degree test (endurance test) figure of the non-volatility memorizer 500 of the embodiment of the present invention.Above-mentioned durability degree test condition is that the lower conductiving layer 207 that gives bias voltage and non-volatility memorizer 500 to the upper conductive layer 212 of non-volatility memorizer 500 gives ground connection (GND), wherein high resistance state (HRS, be listed as in the drawings OFF-state) and low resistance state (LRS, be listed as in the drawings ON-state) current values under-continuous transition operating condition that 0.3V bias voltage reads all, the non-volatility memorizer 500 of the embodiment of the present invention is under the continuous transition operation exceeding more than 400 times, the resistance ratio of high resistance state and low resistance state is still possessed 100 times, its demonstration has the embodiment of the present invention and has oxygen and lack the non-volatility memorizer 500 of resilient coating and have outstanding durability degree characteristic.
The durability degree resolution chart of the non-volatility memorizer 600 of Fig. 3 b comparative example.Above-mentioned durability degree measuring condition is identical with the described measuring condition of Fig. 3 a.As shown in Figure 3 b, the non-volatility memorizer 600 of comparative example is under the continuous transition operation of 12 times, high resistance state (HRS is listed as OFF-state in the drawings) is still possessed 100 times with the resistance ratio of low resistance state (LRS is listed as ON-state in the drawings).But can obviously be found out by 3a and 3b figure, the transition number of times of the non-volatility memorizer 500 of the embodiment of the present invention has more more than 35 times compared to the non-volatility memorizer 600 of comparative example, can significantly increase durability degree and the stability of monolateral operation so the oxygen of the zirconium dioxide film with doping calcium oxide of the embodiment of the present invention lacks the non-volatility memorizer 500 of resilient coating.
Fig. 4 is the storage power test of the non-volatility memorizer 500 of the embodiment of the present invention, erase voltage and the-3V of its also utilize-1.5V write voltage by non-volatility memorizer 500 respectively transitions to low resistance memory state and high resistance memory state, read low resistance memory state (LRS with-0.3V voltage afterwards, be listed as in the drawings ON-state) and high resistance memory state (HRS, be listed as in the drawings OFF-state) two storage states current value, place 1 × 10
6after second, still Ke Zheng Que Read gets data and without the deteriorated generation of any storage characteristics, and resistance ratio between high resistance memory state and low resistance memory state is all greater than 1000 times.
Fig. 5 is that the non-Po Huai Read of the non-volatility memorizer 500 of the embodiment of the present invention gets test, first utilize the voltage of erasing of utilizations-1.5V, with the potential pulse that writes of-3V, non-volatility memorizer 500 is distinguished to transitions to low resistance and high resistance memory state, read continuously low resistance memory state (LRS with the voltage of-0.3V afterwards, be listed as in the drawings ON-state) and high resistance memory state (HRS, be listed as in the drawings OFF-state) the resistance value of two shape storage states, no matter be under room temperature (being listed as in the drawings RT) or the hot conditions of 150 ℃, get exceed 10000 seconds in the situation that at Even Xu Read, the low resistance of the non-volatility memorizer 500 of the embodiment of the present invention and high resistance memory state still maintain 800 times of above degrees of discrimination, without any the deteriorated generation of storage characteristics.
Fig. 6 is the potential pulse durability degree resolution chart of the non-volatility memorizer 500 of the embodiment of the present invention, and it is in order to test the durability degree of non-volatility memorizer under high speed (short pulse time) operation.The test condition of pulse durability degree is the top electrode of non-volatility memorizer 500 to be bestowed to one write potential pulse, its pulse duration be highly respectively 50ns and-6V, therefore, the store status of non-volatility memorizer 500 is converted to low resistance state by high resistance state (HRS is listed as OFF-state in the drawings).Then, then the top electrode of non-volatility memorizer 500 is bestowed to an application of erase voltage pulses, its pulse duration be highly respectively 50ns and-4V, meaning is converted to high resistance state by the store status of non-volatility memorizer 500 by low resistance state.Process is as shown in Figure 6 above-mentioned write with application of erase voltage pulses condition under durability degree test result show, the non-volatility memorizer 500 of the embodiment of the present invention can continued operation exceed 200 times, and has the resistance transition characteristic of (50ns) at a high speed.
As previously mentioned, the metal oxide admixture that the oxygen of the embodiment of the present invention lacks resilient coating 210 is as stabilizer (stabilizer) and oxygen-containing vacancy is provided, and the solubility that metal oxide admixture lacks in resilient coating 210 at oxygen is relevant to temperature and pressure.With regard to improving the position of ionic conductivity, stabilizer can dissolve completely, and produces low concentration defect (oxygen vacancy), between defect, is unlikely in interactional scope, and oxygen-containing vacancy concentration is higher, and ionic conductivity better.Therefore, oxygen lacks the ionic conductivity that the content of metal oxide admixture in resilient coating 210 can change itself, thereby can affect the reliability of non-volatility memorizer 500.
The oxygen of the content with different metal oxides admixture of the 1st table embodiment of the present invention lacks the reliability test result of the non-volatility memorizer 500 of resilient coating 210.
The non-volatility memorizer 500 showing at the 1st tabular is the zirconium dioxide (CaO:ZrO that uses doping calcium oxide
2) film as oxygen lack resilient coating 210.As shown in the 1st table result, the durability degree that the oxygen of the content of metal oxide admixture between mole concentration 1 to 2mol% lacks resilient coating 210 is all better than existing non-volatility memorizer (0mol%).And have mole concentration be 2.8mol% metal oxide admixture oxygen lack resilient coating 210 be as a comparative example.
The non-volatility memorizer 500 of the embodiment of the present invention is to utilize noble metal as bottom electrode, follow-up growth zirconium dioxide film is as resistance transition layer, and utilize the zirconium dioxide film of doping calcium oxide (CaO) to lack resilient coating (oxygenvacancy barrier layer), the zirconium dioxide (CaO:ZrO of the calcium oxide that wherein adulterates as oxygen
2) oxygen that forms of film lacks content that resilient coating can mat calcium oxide and regulate and control the concentration of its oxygen-containing vacancy (oxygen vacancy) (the defect chemistry reaction equation of the zirconium dioxide of doping calcium oxide is
except regulating and controlling, interpolation calcium oxide also can add magnesium oxide (MgO) or yittrium oxide (Y
2o
3) reach.And utilize active metal titanium to be used as top electrode, because titanium is easily captured oxygen (oxygen getter) in oxide and can change oxygen condition and the distribution thereof of memory film inside, component resistance transition characteristic can be confined to oxygen and lack near resilient coating, and the variation that carrys out control operation parameter (operational parameters) is in extremely narrow scope.The method, compared to the resistance-type non-volatile memory component that uses other kind of structure, can significantly promote durability degree and the stability of monolateral operation, can make this kind of double-deck stacking structure be more suitable in the application of resistance-type non-volatility memorizer.
Though the present invention discloses as above with various embodiment; so it is not in order to limit scope of the present invention; any person of ordinary skill in the field; without departing from the spirit and scope of the present invention; when doing a little change and retouching, therefore protection scope of the present invention when with the claims in the present invention scope the person of being defined be as the criterion.
Claims (8)
1. a non-volatility memorizer, is characterized in that, described non-volatility memorizer comprises:
One lower conductiving layer;
One resistance transition layer, is arranged on described lower conductiving layer;
One oxygen lacks resilient coating, is arranged on described resistance transition layer; And
Conductive layer on one, is arranged at described oxygen and lacks on resilient coating; Wherein,
Described oxygen lacks resilient coating and comprises the zirconium dioxide film with a metal oxide admixture, and described metal oxide admixture comprises calcium oxide, magnesium oxide, yittrium oxide or combinations thereof.
2. non-volatility memorizer as claimed in claim 1, is characterized in that, described non-volatility memorizer more comprises:
One substrate, the below of the lower conductiving layer described in being arranged at; And
One insulating barrier, between the lower conductiving layer described in being arranged at and described substrate.
3. non-volatility memorizer as claimed in claim 1, is characterized in that, described lower conductiving layer is platinum.
4. non-volatility memorizer as claimed in claim 1, is characterized in that, described upper conductive layer comprises titanium, titanium nitride or combinations thereof.
5. non-volatility memorizer as claimed in claim 2, is characterized in that, described insulating barrier is silica membrane.
6. non-volatility memorizer as claimed in claim 1, is characterized in that, described resistance transition layer is zirconium dioxide film.
7. non-volatility memorizer as claimed in claim 1, is characterized in that, the content of described metal oxide admixture is between between 1mol% to 2mol%.
8. non-volatility memorizer as claimed in claim 1, it is characterized in that, when described non-volatility memorizer is applied to a formation voltage, can in described resistance transition layer, form a conductive path, make described non-volatility memorizer be transformed into a low resistance state from a reset condition, and wherein erase voltage during in described non-volatility memorizer when applying one, can interrupt the described conductive path of described resistance transition layer, make described non-volatility memorizer be transformed into a high resistance state from described low resistance state, wherein said formation voltage and the described voltage of erasing are all negative value, belong to monolateral resistance transition.
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| CN103904212B (en) * | 2012-12-26 | 2016-08-10 | 华邦电子股份有限公司 | Non-volatility memorizer |
| CN106098932B (en) * | 2016-06-16 | 2019-01-15 | 北京大学 | A kind of linearly gradual memristor and preparation method thereof |
| CN109920908B (en) * | 2017-12-13 | 2023-07-11 | 有研工程技术研究院有限公司 | Resistive random access memory with ultrathin conversion function layer and preparation method thereof |
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| CN101075629A (en) * | 2006-05-19 | 2007-11-21 | 三星电子株式会社 | Nonvolatile memory device using oxygen-deficient metal oxide layer and method of manufacturing the same |
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Non-Patent Citations (2)
| Title |
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| B. Sun et al..Highly uniform resistive switching characteristics of TiN/ZrO2/Pt memory devices.《JOURNAL OF APPLIED PHYSICS》.2009,第105卷(第6期), |
| Highly uniform resistive switching characteristics of TiN/ZrO2/Pt memory devices;B. Sun et al.;《JOURNAL OF APPLIED PHYSICS》;20090316;第105卷(第6期);第061630-1页左栏第1行~第061630-3页末行、附图1 * |
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