CN108281544B - Multi-resistance-state ferroelectric quantum tunnel junction based on ferroelectric coexisting domain and preparation method thereof - Google Patents
Multi-resistance-state ferroelectric quantum tunnel junction based on ferroelectric coexisting domain and preparation method thereof Download PDFInfo
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Abstract
A multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domain and a preparation method thereof belong to the technical field of electronics. The problems of high energy consumption, low read-write speed and low storage density of the conventional magnetic tunnel junction are solved. The invention is a tunnel junction formed by 4 layers of structures which are sequentially arranged from bottom to top, wherein the 4 layers of structures which are sequentially arranged from bottom to top are a single crystal substrate, a bottom electrode, a ferroelectric ultrathin insulating layer and a top electrode respectively; when the thickness of the ferroelectric ultrathin insulating layer is 2nm to 5nm, and the mismatching strain between the ferroelectric ultrathin insulating layer and the single crystal substrate is at the phase boundary of the coexisting phase, a driving voltage is applied to the thickness direction of the ferroelectric ultrathin insulating layer through the bottom electrode and the top electrode, the polarization state of the ferroelectric ultrathin insulating layer is changed by changing the magnitude of the driving voltage, and then the ferroelectric ultrathin insulating layer is driven by different driving voltages to respectively obtain 3 domain structure states with different tunneling resistances. The invention is mainly applied to the memory.
Description
Technical Field
The invention belongs to the technical field of electronics.
Background
With the development of micro-nano devices and integrated circuits and the demand of people for miniaturized portable electronic products, the market demand of nonvolatile memory devices with small size, high density and low power consumption is increasing. The main nonvolatile memories include flash memory (i.e., a common storage scheme in a usb flash disk), ferroelectric memory, phase change memory, and the like. The memories cannot meet future requirements due to the problems of low stability, high power consumption, low integration level and the like. The ferroelectric tunnel junction memory cell developed in recent years has the characteristics of high density, high speed and the like, information can be written by using 6V pulse voltage, and reading is carried out by using 0.6V small voltage, so that the resistance switching ratio of more than 100 is obtained.
However, the ferroelectric thin film with 6V voltage relative to 2nm still has the problems of electric field breakdown and the like. By adopting the ferroelectric film in the multi-domain coexistence state, the switching among different domain structures driven by a small electric field can be realized, and the domain structure size can be greatly reduced, so that the high-density and low-energy-consumption memory device has a great application prospect.
The current tunnel junction is widely made of magnetic materials/insulating layers/magnetic materials, tunneling current is controlled by regulating and controlling the magnetic polarization states of the two magnetic materials through a magnetic field, wherein the insulating layers can be replaced by semiconductor materials to achieve higher resistance switching ratio, but the technologies need higher driving external fields and have lower reading and writing speed, and cannot meet the requirements of rapidness, high density and low energy consumption at present. Ferroelectric tunneling memories were first proposed by l.esaki et al in 1971 [ IBM techn.disc.ball.13, 2,2161(1971) ], but this technology has not been put to practical use due to the immaturity of thin film fabrication technology. With the improvement of the preparation level of the ferroelectric thin film and the deepening of theoretical research, the higher resistance switching effect is obtained in the ferroelectric tunnel junction for the first time until 2009. Although the current ferroelectric tunnel junction breaks through the low speed bottleneck of the magnetic tunnel junction, only the mutual conversion of two resistance states can be realized, and a large driving voltage is required due to the ferroelectric layer clamped by the substrate. Therefore, it is desirable to provide a tunnel junction technology with low driving voltage and fast read/write speed, which can break through the two resistance state limitations to meet the current demands of high density and low power consumption memory devices.
Disclosure of Invention
The invention provides a multi-resistance state ferroelectric quantum tunnel junction based on a ferroelectric coexisting domain and a preparation method thereof, aiming at solving the problems of high energy consumption, low read-write speed and low storage density of the existing magnetic tunnel junction.
A multi-resistance state ferroelectric quantum tunnel junction based on a ferroelectric coexisting domain is a tunnel junction formed by 4 layers of structures which are sequentially arranged from bottom to top, wherein the 4 layers of structures which are sequentially arranged from bottom to top are a single crystal substrate, a bottom electrode, a ferroelectric ultrathin insulating layer and a top electrode respectively;
when the thickness of the ferroelectric ultrathin insulating layer is 2nm to 5nm, and the mismatching strain between the ferroelectric ultrathin insulating layer and the single crystal substrate is at the phase boundary of the coexisting phase, a driving voltage is applied to the thickness direction of the ferroelectric ultrathin insulating layer through the bottom electrode and the top electrode, the polarization state of the ferroelectric ultrathin insulating layer is changed by changing the magnitude of the driving voltage, and then the ferroelectric ultrathin insulating layer is driven by different driving voltages to respectively obtain 3 domain structure states with different tunneling resistances.
Preferably, the bottom electrode is a conductive metal oxide, the top electrode is a noble metal, and the ferroelectric ultrathin insulating layer is a perovskite ferroelectric single crystal thin film.
Preferably, the single crystal substrate adopts SmScO3The bottom electrode adopts SrRuO3The ferroelectric ultrathin insulating layer adopts PbTiO3Or BaTiO3And (5) realizing.
Preferably, the ferroelectric ultrathin insulating layer adopts PbTiO3When implemented, PbTiO3The mismatch strain of the coexisting phases of (a) is in the range of 0.2% to 0.8%.
Preferably, the ferroelectric ultrathin insulating layer adopts PbTiO3When implemented, PbTiO3The mismatch strain range of the optimally coexisting phase of (2) was 0.46%.
Preferably, the top electrode is a Pt electrode.
The method for preparing the multi-resistance state ferroelectric quantum tunnel junction based on the ferroelectric coexisting domain comprises the following steps of:
the method comprises the following steps: heating a single crystal substrate to 650-750 ℃, wherein the oxygen pressure atmosphere is in the range of 20-200 mTorr, and depositing a conductive metal oxide on the single crystal substrate by adopting a pulse laser deposition method, wherein the deposition thickness is 10-20 nm, so that a bottom electrode is formed on the single crystal substrate;
step two: heating a single crystal substrate to 650-750 ℃, wherein the oxygen pressure atmosphere is in the range of 20-200 mTorr, depositing a perovskite ferroelectric single crystal film on a bottom electrode by adopting a pulse laser deposition method, and depositing the perovskite ferroelectric single crystal film to the thickness of 2-5 nm so as to form a ferroelectric ultrathin insulating layer on the bottom electrode;
step three: and depositing noble metal on the ferroelectric ultrathin insulating layer by adopting a magnetron sputtering method, and photoetching the ferroelectric ultrathin insulating layer to form an array-shaped top electrode, thereby completing the preparation of the tunnel junction.
Preferably, the array gap of the top electrode is 100nm to 200 nm.
Principle analysis: a film with two coexisting domain structures grows on a certain substrate through a ferroelectric ultrathin insulating layer, and the coexisting state in the film can realize the inversion of the three-polarization state under a small voltage, so that the thickness and the barrier height of the insulating layer are changed, and the tunneling current density and the tunneling resistance state are effectively changed.
The invention relates to a multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domain, which comprises the following components: the device comprises a single crystal substrate, a bottom electrode, a ferroelectric ultrathin insulating layer and a top electrode. Wherein the bottom electrode and the ferroelectric ultrathin insulating layer are epitaxially deposited on a single crystal substrate matched with the ferroelectric single crystal in size by adopting pulse laser. The lattice constant of the single crystal substrate needs to be such that the lattice-size mismatched strain with the ferroelectric layer is near the phase/domain boundary of the corresponding phase diagram, such as PbTiO3The ferroelectric thin film can be selected to have SmScO with 0.486% mismatching strain3A (samarium scandate) single crystal substrate. The domain structure of the ferroelectric ultrathin insulating layer also needs to be controlled by controlling the growth temperature and the oxygen pressure atmosphere, PbTiO3And preparing the ferroelectric film and the bottom electrode.
The invention has the advantages that the invention breaks through the limitation of the two resistance states of the existing tunnel junction, and the three resistance states can be realized only by changing the domain structure of the ferroelectric layer; and the write voltage of the tunnel junction is reduced to be below 1V, the read voltage is below 500mV, the read-write energy consumption is greatly reduced, the energy consumption is reduced by more than 20%, the read-write speed is improved by more than 50%, and the low storage density is improved.
Drawings
FIG. 1 is a schematic structural diagram of a multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domains according to the present invention;
FIG. 2 is a top view of FIG. 1;
FIG. 3 is a schematic diagram of polarization states in an ultra-thin ferroelectric insulating layer of a multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domains according to the present invention; wherein-P3Represents a single domain polarization down state; p1/P2Representing a set of in-plane polarization statesState; p3Represents a single domain polarization up state;
FIG. 4 is a waveform diagram of driving voltages required for the resistance states corresponding to each polarization state in FIG. 3;
FIG. 5 is a graph of applied voltage versus current density for each resistance state;
FIG. 6 is a schematic flow chart of a photolithography method for preparing an array electrode;
FIG. 7 shows a ferroelectric ultrathin insulating layer of PbTiO3Its energy density phase diagram; wherein a/c represents the energy density curve of a multi-domain state, c represents the energy density curve of a single-domain polarization state, a1/a2An energy density curve representing a set of in-plane polarization states.
Detailed Description
The first embodiment is as follows: referring to fig. 1 to 5, the present embodiment is described, wherein the multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domains in the present embodiment is a tunnel junction formed by 4 layers of structures arranged in sequence from bottom to top, and the 4 layers of structures arranged in sequence from bottom to top are a single crystal substrate 1, a bottom electrode 2, a ferroelectric ultrathin insulating layer 3 and a top electrode 4 respectively;
when the thickness of the ferroelectric ultrathin insulating layer 3 is 2nm to 5nm, and the mismatch strain between the ferroelectric ultrathin insulating layer 3 and the single crystal substrate 1 is at the phase boundary of the coexisting phase, a driving voltage is applied to the ferroelectric ultrathin insulating layer 3 in the thickness direction through the bottom electrode 2 and the top electrode 4, the polarization state of the ferroelectric ultrathin insulating layer 3 is changed by changing the magnitude of the driving voltage, and then the ferroelectric ultrathin insulating layer 3 is driven by different driving voltages to respectively obtain 3 domain structure states with different tunneling resistances.
In this embodiment, the lattice matching state between the single crystal substrate 1 and the ultra-thin ferroelectric insulating layer 3 is designed to make the ultra-thin ferroelectric insulating layer 3 in a coexisting phase state, and then the domain structure state of the ultra-thin ferroelectric insulating layer 3 is changed by changing the magnitude of the driving voltage applied to the ultra-thin ferroelectric insulating layer 3, so as to obtain 3 different tunneling resistances, that is, the tunnel junctions realize the mutual conversion of 3 resistance states at different driving voltages.
The ferroelectric ultrathin insulating layer 3 grows a film with a multi-domain coexistence state on a certain substrate, and the domain structures can be turned over under a smaller voltage, so that the thickness and the barrier height of the insulating layer are changed, and the tunneling current density and the tunneling resistance state are effectively changed.
The second embodiment is as follows: referring to fig. 1 to 7, the present embodiment is described, and the difference between the present embodiment and the multi-resistance state ferroelectric quantum tunnel junction based on the ferroelectric coexisting domain in the first embodiment is that the bottom electrode 2 is a conductive metal oxide, the top electrode 4 is a noble metal, and the ferroelectric ultrathin insulating layer 3 is a perovskite ferroelectric single crystal thin film.
In this embodiment, BaTiO is generally used as the perovskite ferroelectric single crystal thin film3、PbTiO3And Pb (ZrTi) O3And the like.
The third concrete implementation mode: referring to fig. 1 to 7, the present embodiment is described, and the present embodiment is different from the second embodiment in that the single crystal substrate 1 employs SmScO as the material of the multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domain3The bottom electrode 2 adopts SrRuO3The ferroelectric ultrathin insulating layer 3 adopts PbTiO3Or BaTiO3And (5) realizing.
In this embodiment, the ferroelectric ultrathin insulating layer 3 is made of PbTiO3Realization of PbTiO3The energy density phase diagram of (1) is shown in FIG. 7, and in FIG. 7, PbTiO is selected and used in combination with PbTiO3SmScO with lattice matching strain of 0.48%3The single crystal serves as a substrate. And when the mismatching strain of the ferroelectric ultrathin insulating layer 3 is near 0.46%, the a/c domain and the a1/a2The domains coexist. Specifically, SmScO is selected3The single crystal is PbTiO3The film substrate, the bottom electrode 2 can adopt SrRuO with similar lattice parameter3And (5) realizing.
Since multiple domains coexist and the energy densities of the respective domains are close, as in fig. 7, the respective domain states compete with each other, and thus a finer domain structure can be formed. The domain size can now be reduced to 20nm, greatly increasing the information storage density based on such materials.
The fourth concrete implementation mode: the present embodiment will be described with reference to fig. 1 to 7The difference between the mode of the multi-resistance state ferroelectric quantum tunnel junction based on the ferroelectric coexisting domain and the embodiment three is that the ferroelectric ultrathin insulating layer 3 adopts PbTiO3When implemented, PbTiO3The mismatch strain of the coexisting phases of (a) is in the range of 0.2% to 0.8%.
The fifth concrete implementation mode: referring to fig. 1 to 7, the present embodiment is described, and the present embodiment is different from the fourth embodiment in that the ferroelectric ultra-thin insulating layer 3 employs PbTiO as the ferroelectric co-existing domain based multi-resistance state ferroelectric quantum tunnel junction3When implemented, PbTiO3The mismatch strain range of the optimally coexisting phase of (2) was 0.46%.
The sixth specific implementation mode: referring to fig. 1 to 7, the present embodiment is described, and the present embodiment is different from the second embodiment in that the top electrode 4 is a Pt electrode.
The seventh embodiment: referring to fig. 1 to 5 to illustrate the present embodiment, a method for preparing a multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domains, the method comprising the steps of:
the method comprises the following steps: heating a single crystal substrate 1 to 650 ℃ to 750 ℃, and depositing a conductive metal oxide on the single crystal substrate 1 to a deposition thickness of 10nm to 20nm by a pulsed laser deposition method in an oxygen pressure atmosphere in a range of 20mTorr to 200mTorr, thereby forming a bottom electrode 2 on the single crystal substrate 1;
step two: heating a single crystal substrate 1 to 650-750 ℃, wherein the oxygen pressure atmosphere is in the range of 20 mTorr-200 mTorr, depositing a perovskite ferroelectric single crystal thin film on a bottom electrode 2 by adopting a pulse laser deposition method, and the deposition thickness is 2 nm-5 nm, so that a ferroelectric ultrathin insulating layer 3 is formed on the bottom electrode 2;
step three: noble metal is deposited on the ferroelectric ultrathin insulating layer 3 by adopting a magnetron sputtering method, so that array-shaped top electrodes 4 are formed on the ferroelectric ultrathin insulating layer 3 by photoetching, and the preparation of the tunnel junction is completed.
In this embodiment, a noble metal such as platinum Pt is deposited by a magnetron sputtering method, and an electrode array is obtained by a photolithography method, as shown in fig. 6.
The specific implementation mode is eight: referring to fig. 1 to 5, the present embodiment is illustrated, and the present embodiment is different from the method for fabricating a multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domains described in the seventh embodiment in that the array gap of the top electrode 4 is 100nm to 200 nm.
The structure of the multi-resistance state ferroelectric quantum tunnel junction based on the ferroelectric coexisting domain according to the present invention is not limited to the specific structure described in the above embodiments, and may be a reasonable combination of the technical features described in the above embodiments.
Claims (8)
1. A multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domains is a tunnel junction formed by 4 layers of structures which are sequentially arranged from bottom to top, and is characterized in that the 4 layers of structures which are sequentially arranged from bottom to top are a single crystal substrate (1), a bottom electrode (2), a ferroelectric ultrathin insulating layer (3) and a top electrode (4) respectively;
when the thickness of the ferroelectric ultrathin insulating layer (3) is 2nm to 5nm, and the mismatch strain between the ferroelectric ultrathin insulating layer (3) and the single crystal substrate (1) is at the phase boundary of the coexisting phase, a driving voltage is applied to the thickness direction of the ferroelectric ultrathin insulating layer (3) through the bottom electrode (2) and the top electrode (4), the polarization state of the ferroelectric ultrathin insulating layer (3) is changed by changing the magnitude of the driving voltage, and then the ferroelectric ultrathin insulating layer (3) respectively obtains 3 domain structure states with different tunneling resistances under the driving of different driving voltages.
2. The multi-resistance state ferroelectric quantum tunnel junction based on the ferroelectric coexisting domain as claimed in claim 1, wherein the bottom electrode (2) is a conductive metal oxide, the top electrode (4) is a noble metal, and the ferroelectric ultra-thin insulating layer (3) is a perovskite ferroelectric single crystal thin film.
3. The multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domain as claimed in claim 1, wherein said single crystalline substrate (1) is SmScO3The bottom electrode (2) adopts SrRuO3The ferroelectric ultrathin insulating layer (3) adopts PbTiO3Or BaTiO3And (5) realizing.
4. A multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domain as claimed in claim 3, wherein the ferroelectric ultra-thin insulating layer (3) is made of PbTiO3When implemented, PbTiO3The mismatch strain of the coexisting phases of (a) is in the range of 0.2% to 0.8%.
5. The multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domain as claimed in claim 4, wherein the ferroelectric ultra-thin insulating layer (3) is made of PbTiO3When implemented, PbTiO3The mismatch strain range of the optimally coexisting phase of (2) was 0.46%.
6. A ferroelectric quantum tunnel junction in a multi-resistance state based on ferroelectric coexisting domains as in claim 2, characterized in that the top electrode (4) is a Pt electrode.
7. The method for preparing the multi-resistance state ferroelectric quantum tunnel junction based on the ferroelectric coexisting domain is characterized by comprising the following steps of:
the method comprises the following steps: heating a single crystal substrate (1) to 650 ℃ to 750 ℃, and depositing a conductive metal oxide on the single crystal substrate (1) to a thickness of 10nm to 20nm by a pulsed laser deposition method in an oxygen pressure atmosphere in a range of 20mTorr to 200mTorr, thereby forming a bottom electrode (2) on the single crystal substrate (1);
step two: heating a single crystal substrate (1) to 650-750 ℃, and depositing a perovskite ferroelectric single crystal thin film on a bottom electrode (2) by a pulse laser deposition method with the deposition thickness of 2-5 nm in the oxygen pressure atmosphere of 20-200 mTorr, thereby forming a ferroelectric ultrathin insulating layer (3) on the bottom electrode (2);
step three: and (3) depositing noble metal on the ferroelectric ultrathin insulating layer (3) by adopting a magnetron sputtering method, and photoetching on the ferroelectric ultrathin insulating layer (3) to form an array-shaped top electrode (4), thereby completing the preparation of the tunnel junction.
8. The method for preparing a multi-resistance state ferroelectric quantum tunnel junction based on ferroelectric coexisting domains as claimed in claim 7, wherein the array gap of the top electrode (4) is in the range of 100nm to 200 nm.
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| GB2576174B (en) * | 2018-08-07 | 2021-06-16 | Ip2Ipo Innovations Ltd | Memory |
| CN110429085B (en) * | 2019-07-31 | 2022-07-15 | 复旦大学 | Ferroelectric three-bit memory, preparation method and operation method thereof |
| US11087791B1 (en) * | 2020-05-05 | 2021-08-10 | Western Digital Technologies, Inc. | Data storage device with voltage-assisted magnetic recording (VAMR) for high density magnetic recording |
| CN112382719B (en) * | 2020-10-10 | 2023-10-10 | 清华大学 | Device structure for improving ferroelectric tunneling junction performance and preparation method thereof |
| CN113707806A (en) * | 2021-08-26 | 2021-11-26 | 山东大学 | Long-range plasticity ferroelectric tunnel junction nerve synapse device with high symmetry and high linearity as well as preparation method and application thereof |
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