CN110923647B - Dirac node sphere semimetal and preparation and application methods thereof - Google Patents

Dirac node sphere semimetal and preparation and application methods thereof Download PDF

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CN110923647B
CN110923647B CN201911191203.2A CN201911191203A CN110923647B CN 110923647 B CN110923647 B CN 110923647B CN 201911191203 A CN201911191203 A CN 201911191203A CN 110923647 B CN110923647 B CN 110923647B
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侯文杰
张学莹
赵巍胜
聂天晓
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Zhizhen Precision Instrument Qingdao Co ltd
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Abstract

The invention relates to a Dirac node sphere semimetal and a preparation method and an application method thereof, and provides X consisting of a VB group transition metal atom X and a V main group atom Y3The Dirac node sphere semimetal formed by the Y alloy material has a drum-shaped topological surface state, a Dirac point in a three-dimensional momentum space forms a spherical shell shape, and the alloy material has larger SHC so as to provide theoretical basis and guidance for subsequent functional nanometer device (such as a spin storage device SOT-MRAM and a magnetic sensor) experiments. The crystal structure of the Dirac nodo sphere semimetal is Cu in an ordered L12 phase3Au is a basic structure, and a face-centered cubic structure (fcc) simulation material X is formed by a VB group transition metal atom X and a V main group atom Y3And Y. Wherein the atoms at the face center are group VB transition metal atoms X (e.g., Nb, Ta), and the atoms at the 8 vertices are group V main atoms Y (e.g., As, Sb, Bi).

Description

Dirac node sphere semimetal and preparation and application methods thereof
Technical Field
The invention provides a novel Dirac node sphere semimetal, and a preparation and analysis process of the Dirac node sphere semimetal is realized by combining simulation design and application analysis, and belongs to the field of metal compound materials.
Background
With the rapid increase of high-speed computing capability and storage demand, attention is being paid to the advanced semiconductor industry such as memory chips. Among them, Magnetic Random Access Memory (MRAM) is a key item developed by both manufacturers and manufacturers because of its low power consumption and fast writing speed. The prior three generations of MRAM all face the problems of low magnetic moment reversal efficiency and the like, and the SOT-MRAM based on Spin Orbit Torque (SOT) of spin orbit coupling interaction can realize efficient electric field control and ferromagnetic layer torque overturning, and generate very large Spin Hall Conductance (SHC). Research shows that SOT-MRAM can be one order of magnitude faster than STT-MRAM, switching energy can be reduced by at least two orders of magnitude, writing speed can be increased by 20 times, bit density can be increased by 10 times, etc. Therefore, the method has important application prospect for the development of high-speed and low-power-consumption information storage and logic operation devices. One of the great obstacles to the fabrication of SOT-MRAM is the choice of device materials. One of the keys to realizing high-efficiency, low-power consumption, mass-producible SOT-MARM devices is to explore a novel material with a large SHC.
It is well known that Spin Hall Conductance (SHC) originates from spin-orbit coupling (SOC) interactions and is closely related to the intrinsic Spin Hall Effect (SHE). Current research on materials with stronger SHE has focused mainly on heavy metals and topological insulators. However, both of the above materials have a problem that the SHC is relatively small in practicality, and finding a novel material having a large SHC among materials having strong SHE is expected to break through this obstacle.
It has been found that materials having the dirac cone band structure have many excellent physical properties, such as Strong Hall Effect (SHE) and extremely high carrier mobility. The dirac semimetal is a novel material with non-trivial topological properties, the energy band of the dirac semimetal meets the dirac equation describing the relativistic particle energy-momentum relationship, a three-dimensional dirac point is arranged near the fermi surface, and the quadruple degeneracy of the energy band structure at the dirac point is generally protected by the lattice symmetry and the time reversal symmetry. Such materials have become hot spots for the research in the field of condensed state and the field of material science recently.
The existing researches on materials with stronger spin Hall effect are mainly divided into the following two categories: one is heavy metals with strong spin-orbit coupling, such as Ta, W, etc., but their SHC at the fermi level is small. Even if the SHC of platinum Pt exceeds
Figure BDA0002293614590000011
Because Pt is a rare earth noble metal and is expensive, the large-scale production of Pt in practical application is limited; the other is that the ideal material predicted to have a strong spin hall effect, i.e., a topological insulator, is found to be a relatively general metal (resistivity of about 10) through research, even though it exhibits many excellent physical properties1—102μ Ω cm) whose resistivity is generally high (about 10)3—104Mu omega cm), which causes the problem of difficult current injection, and prevents the application of the material in the field of spin electronic devices such as SOT-MRAM. Practice ofIn both of the above two classes, SHC is relatively small, e.g., GaAs-100, WTE2<400,OsO2541, TaAs-781, beta-W-1255, 4d and 5d transition metals
Figure BDA0002293614590000021
Subject to the uncertainty of the current experimental conditions, the discovery of new dirac materials would be a complex and lengthy process. And a novel material can be designed through theoretical calculation, and the novel material with topological characteristics and metal properties, namely the dirac semimetal, can be predicted through simulation calculation and numerical analysis, so that guidance and theoretical basis are provided for experimental research, and blindness in the experimental process can be effectively reduced.
In view of this, the present patent application is specifically proposed.
Disclosure of Invention
The invention discloses a Dirac node sphere semimetal and a preparation and application method thereof, aiming at solving the practical requirements and technical difficulties of the prior art and providing X consisting of a VB group transition metal atom X and a V main group atom Y3The Dirac node ball semimetal formed by the Y alloy material has a drum-shaped topological surface state, a Dirac point in a three-dimensional momentum space forms a spherical shell shape, and the alloy material has larger SHC so as to provide theoretical basis and guidance for subsequent functional nano spin electronic device (such as spin storage device SOT-MRAM and magnetic sensor) experiments.
For the purpose of realizing the design, the crystal structure of the Dirac node sphere semimetal is Cu with an ordered L12 phase3Au is a basic structure, and a face-centered cubic structure (fcc) simulation material X is formed by a VB group transition metal atom X and a V main group atom Y3Y。
Wherein the atoms at the face center are group VB transition metal atoms X (e.g., Nb, Ta), and the atoms at the 8 vertices are group V main atoms Y (e.g., As, Sb, Bi).
X composed of a group VB transition metal atom X and a group V main group atom Y3Y alloy material belongs to a novel Dirac node ball semimetal and is provided withThe drum-shaped topological surface state, the Dirac points in the three-dimensional momentum space form a spherical shell shape;
the Dirac node sphere semimetal has large spin Hall conductance, and the group VB transition metal atom X is preferably Ta, such as Ta3Bi。
The preparation method of the Dirac node ball semi-metal comprises the steps of taking monocrystalline silicon as a substrate and growing X by adopting a multi-source method3Y alloy;
the implementation steps comprise that different numbers of Y metal strips are placed on a pure X metal target for magnetron sputtering; and (3) placing the Y metal strip along the axis of the X metal target in a divergent manner until the ratio of the components of the X metal to the Y metal is 3: 1, finishing the preparation of the Dirac node sphere semimetal alloy.
Specifically, a single crystal silicon having a thickness of about 0.5mm was used as a substrate, and a Ta3Bi alloy was grown by a multi-source method.
The implementation method comprises the following steps: different numbers of Bi strips with the size of 3mm multiplied by 12mm are placed on a pure Ta target for magnetron sputtering, and the more the number of the Bi strips is, the more Bi components in the alloy formed by Ta and Bi are;
the Bi strips were placed divergently along the Ta target axis (only 3Bi strips are shown in fig. 7) until the ratio of Ta and Bi components was 3: 1 hour, finishing the Dirac node ball semimetal Ta3And (3) preparing the Bi alloy.
Further, the application provides that the Dirac node ball half metal is applied to a Magnetic Tunnel Junction (MTJ) element, so that the Dirac node ball half metal is applied to future low-energy-consumption spintronic devices such as SOT-MRAM.
With Ta3For example, the material of the metal mask layer is preferably a single layer or a stack of a plurality of materials of titanium (Ti) and ruthenium (Ru).
The thickness of the metal mask layer can be slightly larger than that of the MTJ element layer Ta3A Bi alloy.
The residual photoresist can be removed by a photoresist removing process such as oxygen plasma, chemical cleaning, and the like, and finally the isolated metal mask layer with the cylindrical structure is formed.
Using techniques such as Ion Beam Etching (IBE), inductively coupled plasma etching (ICP),A Reactive Ion Etching (RIE) process or processes suitable for the formation of the Ta of the semiconductor from the Dirac node sphere3And the MTJ element layer is made of Bi alloy and has an independent cylindrical structure.
The dielectric region may be comprised of any suitable dielectric material such as silicon dioxide, aluminum oxide, and the like.
In summary, the dirac node sphere semimetal and the preparation and application method thereof have the advantages that a novel three-dimensional dirac node sphere semimetal material is designed by adopting theoretical simulation and calculation, model construction, stability test, energy band calculation, accurate fitting and topological characteristic analysis, and on one hand, the understanding and comprehension of the topological material are enriched; on the other hand, Ta is found by calculation3The Y alloy has large Spin Hall Conductance (SHC) and can provide a valuable theoretical basis for subsequent experiments on nano devices such as SOT-MRAM. The method for simulating calculation has the advantages of low cost, high accuracy and good repeatability, and can continuously excavate other excellent characteristics of the material so as to be applied to more frontier fields.
Drawings
FIG. 1 is the present application X3A semi-metal structure schematic diagram of a Y Dirac node sphere;
FIG. 2 is a diagram showing the calculated results of phonon spectra obtained by performing a crystal structure stability test;
FIGS. 3a and 3b are Ta in the topological feature analysis, respectively3A schematic diagram of Bi alloy energy band and tight binding potential model fitting energy bands;
FIG. 4a and FIG. 4b are schematic diagrams of a momentum space node sphere and a topological surface state, respectively, obtained by topological characteristic analysis;
FIG. 5 is a schematic illustration of a Dirac half-metal of a plurality of materials of the same family;
FIG. 6 is a Dirac node sphere semimetal X3Spin Hall Conductance (SHC) diagram of Y;
FIG. 7 is a schematic diagram of the preparation of a Dirac nodo sphere semimetal;
FIG. 8 is Ta3The Bi alloy is used as a structural schematic of the MTJ element.
Detailed Description
The invention is described in further detail below with reference to the figures and the examples of embodiment.
In the embodiment 1, theoretical simulation and calculation are adopted, model construction and stability test are carried out, energy band calculation and accurate fitting are carried out, and topological characteristic simulation analysis is carried out, so that a novel Dirac node sphere semimetal and a preparation method thereof are provided.
As shown in FIG. 1, the crystal structure of the Dirac nodulus semimetal is Cu in an ordered L12 phase3Au is a basic structure, and a face-centered cubic structure (fcc) simulation material X is formed by a VB group transition metal atom X (Nb, Ta) and a V main group atom Y (As, Sb, Bi)3Y。
Wherein the atoms at the face center are group VB transition metal atoms X (e.g., Nb, Ta), and the atoms at the 8 vertices are group V main atoms Y (e.g., As, Sb, Bi).
X composed of a group VB transition metal atom X and a group V main group atom Y3The Y alloy material belongs to a novel Dirac node sphere semimetal, and has a drum-shaped topological surface state, and Dirac points in a three-dimensional momentum space form a spherical shell shape;
the Dirac node sphere semimetal has larger spin Hall conductance, and the VB group transition metal atom X is preferably Ta. Such as Ta3Bi having a maximum SHC value at Fermi energy of about
Figure BDA0002293614590000041
Is higher than other materials found at present except for noble metal Pt, but Pt belongs to noble metals and has no popularization prospect of wide application.
As shown in fig. 1, the crystal structure was optimized as follows using vasop software.
The optimization setting is that Perew-Burke-Ernzehof (PBE) pseudopotential is adopted, the exchange-correlation functional adopts Generalized Gradient Approximation (GGA) to describe the exchange-correlation functional, and Brillouin zone k-point sampling adopts a Monkhorst-pack (MK) scheme.
The main parameters in the structural optimization are as follows: the plane wave cut-off energy is 340eV, the convergence precision is 10 < -6 >, and the k point of the Brillouin zone is selected to be 15 multiplied by 15.
Ta with predicted maximum SHC3For example, Bi, the optimized three-dimensional dirac simulation material has the structural parameters:
space group
Figure BDA0002293614590000042
(No.221)
Lattice constant
Figure BDA0002293614590000051
Direct coordinates of atoms
Figure BDA0002293614590000052
The parameters are obtained after structure optimization, and the uniqueness of the three-dimensional Dirac simulation material can be determined.
As shown in fig. 2, a test was performed to prove the stability of the crystal structure of the dirac node sphere semi-metallic material.
And based on a finite displacement method, a PHONOPYY program is adopted to carry out stability test on the phonon spectrum of the crystal structure of the node sphere. With Ta3Taking Bi as an example, Ta3The phonon spectrum was calculated after the original cells of Bi were expanded to 5X 7 supercells. The calculation result shows that no virtual frequency exists, which indicates that the crystal structure of the Dirac semimetal material exists stably.
Computational analysis on energy band and topological properties is as follows.
Using QUANTUM ESPRESSO in combination with the programs Wannier90 and Wannier tools, the Hamilton values were determined by using a tightly bound potential model (TB model): h (k) ═ dx(k)σx+dy(k)σy+dz(k)σz+d0I
Under the condition of fully considering Spin Orbit Coupling (SOC), the energy band of the system is subjected to simulation calculation, accurate fitting and topological characteristic analysis.
The main parameters are set as follows: the atomic force precision is
Figure BDA0002293614590000053
The truncated charge density of the plane wave is 850Ry, and the truncated energy parameter is 70 Ry.
With Ta3For Bi as an example, the calculation and fitting results are shown in fig. 3a and 3 b.
This illustrates the above X3Y is a novel three-dimensional Dirac node sphere semi-metal material, which presents the topological characteristics of the Dirac node sphere in a three-dimensional momentum space and shows the tympanic membrane topology surface states on (010), (001) surfaces and the like, as shown in FIGS. 4a and 4 b.
According to the design principle and the structure test, on the basis of the same three-dimensional node sphere structure, the Dirac semimetal material is found to be not only Ta but also by replacing other materials in the same family3Bi alloy, family X3The Y-class materials are all dirac semimetals, as shown in fig. 5.
The Spin Hall Conductance (SHC) was calculated as follows.
Based on the above X3The Y material was calculated from a Spin Hall Conductance (SHC) study by maximum localization of the Wannier function and the Wannier90 program (the exact reliability of which has been confirmed and published in phys. rev. b 2018,98, 214402). A dense K-point grid is selected in the calculation process, and the parameters are set to be 100 multiplied by 100.
As shown in FIG. 6, a three-dimensional Dirac semimetal X is shown3Spin hall conductance of Y. Visible, Ta3The Y material has a very large SHC. Therefore, the problems of low practical efficiency of noble metals such as Pt and the like, high resistivity faced by topological insulators and the like can be solved, and a theoretical basis and a guiding function are provided for material selection of nano-functional devices such as spin electronic devices (such as SOT-MRAM).
The metals Pt and beta-W in the prior art have larger spin Hall conductance. However, the metal Pt is a rare earth noble metal, and is very expensive and not suitable for mass production; the thermal stability of β -W is poor and it is difficult to realize MTJ devices with stable β -W/ferromagnetic layers.
The preparation method of the Dirac node sphere semimetal is to realize the structure that Bi is doped in metal element TaDirac node sphere semimetal (chemical formula Ta)3Bi) as a material for the fabrication of MTJ elements.
Specifically, a single crystal silicon having a thickness of about 0.5mm was used as a substrate, and Ta was grown by a multi-source (multi-source) method3A Bi alloy.
The implementation method comprises the following steps: different numbers of Bi strips with the size of 3mm multiplied by 12mm are placed on a pure Ta target for magnetron sputtering, and the more the number of the Bi strips is, the more Bi components in the alloy formed by Ta and Bi are;
the Bi strips were placed divergently along the Ta target axis (only 3Bi strips are shown in fig. 7) until the ratio of Ta and Bi components was 3: 1 hour, finishing the Dirac node ball semimetal Ta3And (3) preparing the Bi alloy.
Since the dirac noddle semimetal is a novel material with non-trivial topological properties, the energy band of the dirac noddle semimetal meets the dirac equation describing the relativistic particle energy-momentum relationship, a three-dimensional dirac point is arranged near the fermi surface, and the quadruple degeneracy of the energy band structure at the dirac point is generally protected by the combination of lattice symmetry and time-reversal symmetry. The materials exhibit a plurality of excellent physical properties such as very high carrier mobility, large spin Hall conductance and the like, and can be well applied to Magnetic Tunnel Junction (MTJ) elements, so that the materials can be applied to future low-energy-consumption spintronic devices such as SOT-MRAM and the like.
As shown in FIG. 8, Ta3The Bi alloy is used as a structural schematic of the MTJ element.
The metal mask layer is preferably formed from a single layer or a stack of multiple materials, preferably titanium (Ti), ruthenium (Ru), using a suitable deposition process, such as Physical Vapor Deposition (PVD), Plasma Enhanced Chemical Vapor Deposition (PECVD), or the like. The thickness of the metal mask layer can be slightly larger than that of the MTJ element layer Ta3Bi alloy, specifically controlled to be between 1nm and 200nm, and the metal mask layer is formed by adopting a standard patterning technology. After the metal mask layer is formed, a photoresist removing process such as oxygen plasma, chemical cleaning and the like can be adopted to remove residual photoresist, and finally the metal mask layer with an isolated cylindrical structure is formed, wherein the minimum size is determined by the design size of the cylindrical MTJ element.
In this embodiment, the minimum size of the metal mask layer cylinder may be 10nm to 100 nm. Forming the semi-metal Ta of the Dirac node ball by adopting one or more proper etching processes such as Ion Beam Etching (IBE), inductively coupled plasma etching (ICP), Reactive Ion Etching (RIE) and the like3And the MTJ element layer is made of Bi alloy and has an independent cylindrical structure. The dielectric region may be comprised of any suitable dielectric material such as silicon dioxide, aluminum oxide, and the like.
It will be understood that modifications and variations can be made by persons skilled in the art in light of the above teachings and all such modifications and variations are intended to be included within the scope of the invention as defined in the appended claims.

Claims (4)

1. A dirac node ball semimetal which characterized in that: the crystal structure is Cu in an ordered L12 phase3Au as basic structure, and forming a face-centered cubic (fcc) structure (X) by using group VB transition metal atoms X and group V main group atoms Y3Y；
The atoms at the face center are group VB transition metals, and the atoms at the 8 vertices are group V main metals;
the Dirac node sphere semimetal has a drum-shaped topological surface state, and Dirac points in a three-dimensional momentum space form a spherical shell shape.
2. The dirac node sphere semimetal of claim 1, wherein: the dierac semimetal material is Ta3Bi。
3. A method of preparing a dirac nodel ball semimetal of any one of claims 1 or 2, characterized in that: taking monocrystalline silicon as a substrate, growing X by a multi-source method3Y alloy;
the implementation steps comprise that different numbers of Y metal strips are placed on a pure X metal target for magnetron sputtering;
and (3) placing the Y metal strip along the axis of the X metal target in a divergent manner until the ratio of the components of the X metal to the Y metal is 3: 1, finishing the preparation of the Dirac node sphere semimetal alloy.
4. A method of applying the dirac node ball semimetal of any one of claims 1 or 2 or the dirac node ball semimetal prepared by the preparation method of claim 3 to a Magnetic Tunnel Junction (MTJ) element.
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