CN106702320B - Heterogeneous two-dimentional crystalline film material of a kind of superconductor-insulator-metal and preparation method thereof - Google Patents
Heterogeneous two-dimentional crystalline film material of a kind of superconductor-insulator-metal and preparation method thereof Download PDFInfo
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Abstract
It is layer structure the invention discloses a kind of superconductor-insulator-metal heterofilm material, including metal hafnium basal layer, five telluride hafnium membrane structure layers and three telluride hafnium membrane structure layers, the layer structure extend in two-dimensional surface.Preparation method: under vacuum conditions, by appropriate high-purity tellurium hydatogenesis to hafnium transition metal substrate surface；It is made annealing treatment, so that the metal hafnium atom on the tellurium atom and the substrate of deposition interacts to form five telluride hafnium sequential 2 D crystalline state membrane structures；Further annealing, making the surface of the five telluride hafnium sequential 2 D crystalline state membrane structure to be formed, recurring structure changes to form three telluride hafniums again,-five telluride hafnium of three telluride hafniums-metal hafnium two-dimension laminate structure is ultimately formed, superconductor-insulator-metal heterofilm material is obtained.Preparation process is relatively easy, and the heterojunction structure film defects of acquisition are few, and interface is not easy to be contaminated, and improves the quality of heterojunction structure film.
Description
Technical field
The invention belongs to technical field of nano material, and in particular to a kind of heterogeneous two-dimentional crystalline state of superconductor-insulator-metal
Thin-film material and preparation method thereof.
Background technique
Graphene, the classics as two dimensional crystal material represent, due to its unique electronically and physically property, from 2004
It is short to become research hotspot highly visible during the decade since being removed from its parent graphite, cause in world wide to new
The exploration of type two dimensional crystal material and research boom.The two dimensional crystal material of different physical properties is superimposed, it is most likely that generate
Some new material structures and physical property, for example, having observed new object in the heterogeneous laminated construction of graphene-boron nitride
Rationality matter (Hofstadter butterfly --- the excellent parting pattern of description electronics moving situation in magnetic field)；This graphene-
The heterogeneous laminated construction of boron nitride, not a kind of simple material stack, a kind of new two dimensional crystal material, to be used to
Theoretical prediction before confirming 40 years will play great function in electronics and optoelectronic device.Nearest theoretical research shows
It is become attached to the heterogeneous laminated construction of body and (s wave) superconductor by studying topology, it is most likely that observe Maastricht Treaty Rana Fermion,
This particle is expected to form stable quantum bit in quantum calculation, makes it possible efficient topological quantum computer.
This laminated construction is constructed with important scientific value and application prospect.
Five telluride hafniums are theoretically foretold as topological insulator (energy gap of 0.4 electron volts).In addition, three telluride of posture
Hafnium has been reported with superconducting property.The structure of five telluride hafniums and three telluride hafniums is again quite similar, and five telluride hafniums are three telluride hafniums
Got up among prism structures by zigzag tellurium chain link, all there is two-dimensional layer configuration.If can spontaneously form
This five telluride hafnium of different nature and the three heterogeneous laminated construction of telluride hafnium can carry out study on regulation to physical property.For this
The research of a aspect will all have good prospect on basis and application aspect.The application that two-dimentional dissimilar materials is paid, high quality
The preparation of material is its crucial and basis.But the experiment preparation method about five telluride hafnium films, especially atomic-level thickness
The preparation of sample, is not reported so far.About the experiment preparation method of three telluride hafnium blocks, presently mainly with the method for sintering
Preparation, and the preparation of three telluride hafnium samples of atomic-level thickness, are not also reported so far.
As a kind of completely new superconductor-insulator-metal heterofilm material ,-five telluride hafnium of three telluride hafniums-metal hafnium
The acquisition of heterofilm is the premise and condition to its further physical property research and practical application.Common preparation two-dimensional material at present
The method of heterojunction structure is the method that removing transfer stacks, but such a process increases the complexity of preparation process, and obtain
Heterojunction structure film defects are more, and interface is easy to be contaminated, and cause the reduction of its performance.Therefore, a kind of prepare experimentally is found
- five telluride hafnium of three telluride hafnium of high quality-metal hafnium heterofilm material method is particularly important.
Summary of the invention
The purpose of the present invention is to provide a kind of superconductor-insulator-metal heterofilm material and preparation method thereof, systems
Preparation Method is relatively easy, and superconductor-insulator-metal heterofilm material property of preparation is higher.
Concrete scheme of the invention is as follows:
A kind of superconductor-insulator-metal heterofilm material is layer structure, including metal hafnium basal layer, five telluride
Hafnium membrane structure layer and three telluride hafnium membrane structure layers, the five telluride hafnium membrane structure layer are located at the surface of the metal hafnium basal layer,
The three telluride hafnium membrane structure layer is located at the surface of the five telluride hafnium membrane structure layer, which expands in two-dimensional surface
Exhibition.
The invention also discloses a kind of above-mentioned superconductor-insulator-metal heterofilm material preparation methods, including such as
Lower step:
Step 1) under vacuum conditions, by appropriate high-purity tellurium hydatogenesis to hafnium transition metal substrate surface；
Step 2) is made annealing treatment, the shape so that the metal hafnium atom on the tellurium atom and the substrate of deposition interacts
At five telluride hafnium sequential 2 D crystalline state membrane structures；
Step 3) further makes annealing treatment, and makes the surface for the five telluride hafnium sequential 2 D crystalline state membrane structure to be formed again
Secondary recurring structure changes to form three telluride hafniums, ultimately forms-five telluride hafnium of three telluride hafniums-metal hafnium two-dimension laminate structure, obtains
Superconductor-insulator-metal heterofilm the material being made of-five telluride hafnium of three telluride hafniums-metal hafnium.
The high-purity tellurium wherein used is 99.999% or the tellurium of similar purity.Because of the five telluride hafniums this two formed
Tieing up orderly crystalline state membrane structure is insulating material, and the three telluride hafniums that five telluride hafnium surfaces are formed are that a kind of superconduction two dimension has
Sequence crystalline state film, so, finally obtained-five telluride hafnium of three telluride hafnium-metal hafnium two-dimension laminate structure is superconductor-insulator-
Metal heterofilm material.
Further, tellurium used in step 1) is evaporated to the hafnium transition metal base by the method for physical vapour deposition (PVD)
Bottom surface.
Further, annealing temperature section described in step 2) is 450 DEG C~500 DEG C, annealing time 10-20 minutes.It is excellent
Selection of land, the annealing temperature are 500 DEG C, annealing time 15 minutes.
Further, for growing the hafnium transition metal for forming the five telluride hafnium sequential 2 D crystalline state membrane structure
The surface of substrate is (0001) face of metal hafnium.
Further, the forming method in (0001) face of the metal hafnium are as follows: first in vacuum chamber to metal hafnium monocrystalline into
Row argon ion sputtering 3-6 hours, then metal hafnium substrate is heated and maintained at high annealing 5-10 minutes of 900 DEG C, form energy
The periodical superstructure that enough scanned tunnel microscope (STM) is characterized.Preferably, carrying out the argon ion sputtering time is 5 hours,
High annealing 8 minutes of 900 DEG C.
Wherein, the periodical superstructure that the five telluride hafnium crystalline material is formed in (0001) face of hafnium, typical cycle
For 0.34 × 1.09nm, can find to fluctuate with sample temperature.The periodicity superstructure can be scanned tunnel microscope (STM) institute
Characterization.
Further, the Atomic Arrangement of the top of the five telluride hafnium sequential 2 D crystalline state membrane structure can be scanned
Tunnel microscope is characterized.
Further, the energy gap of 0.4 electron volts of the five telluride hafnium crystalline material can be differentiated conductance (dI/dV) spectrum
It is characterized.
Further, the annealing temperature section in step 3) is 500 DEG C~600 DEG C, annealing time 10-20 minutes.
Preferably, which is 560 DEG C, and annealing time is 15 minutes.
Five telluride hafnium surfaces of the three telluride hafnium crystalline material on (0001) face of metal hafnium form periodically super
Structure, typical cycle are 0.38 × 0.47nm, may find to fluctuate with sample temperature, which can be scanned tunnel
Road microscope is characterized.
Further, the Atomic Arrangement of the three telluride hafnium crystalline material top can be scanned tunnel microscope
(STM) it is characterized.
Further, the superconducting energy gap of the three telluride hafnium crystalline material can be differentiated conductance (dI/dV) and be characterized.
A kind of superconductor provided by the invention-insulator-metal heterofilm material and preparation method thereof, passes through molecular beam
Epitaxy method has grown-five telluride hafnium of three telluride hafniums-metal hafnium crystalline film material of large-area high-quality, has abandoned previous
The method that removing transfer stacks, reduces superconductor-insulator-metal heterofilm material technology complexity, meanwhile, it obtains
Heterojunction structure film defects it is few, interface is not easy to be contaminated, and improves the quality of heterojunction structure film.The thin-film material is superconduction
The newcomer of heterogeneous family has expanded the research field of superconduction heterofilm, in Future Information electronics and device developmental research
Aspect has a wide range of applications potentiality.
Detailed description of the invention
Fig. 1 is in the present invention by high-purity tellurium hydatogenesis to the schematic diagram of hafnium transition metal substrate surface；
Fig. 2 is to form five telluride hafnium membrane structure layers in hafnium transition metal substrate surface after making annealing treatment for the first time in the present invention
Schematic diagram；
Fig. 3 is that five telluride hafnium membrane structure layer surfaces form three telluride hafnium membrane structure layers after second of annealing in the present invention
Schematic diagram；
Fig. 4 is the side view of finally formed-five telluride hafnium of three telluride hafnium-metal hafnium heterofilm material in the present invention；
Fig. 5 is the scanning tunneling microscope of the high coverage tellurium particle deposited in the present invention on (0001) surface of metal hafnium
Image；
Fig. 6 is the scanning tunneling microscopic of the five telluride hafnium film of high quality prepared on (0001) face of metal hafnium in the present invention
Mirror image；
Fig. 7 is the differential conductance spectrum of the five telluride hafnium of high quality prepared on (0001) face of hafnium in the present invention；
Fig. 8 is-five telluride hafnium laminated material of three telluride hafnium of high quality prepared on (0001) face of hafnium in the present invention
Scanning tunneling microscope image；
Fig. 9 is-five telluride hafnium laminated material of three telluride hafnium of high quality prepared on (0001) face of hafnium in the present invention
Differential conductance spectrum.
Specific embodiment
With reference to the accompanying drawing to a kind of superconductor-insulator-metal heterofilm material provided by the invention and its preparation
The specific embodiment of method elaborates.
Fig. 1 is in the present invention by high-purity tellurium hydatogenesis to the schematic diagram of hafnium transition metal substrate surface；Fig. 2 is this hair
The schematic diagram of five telluride hafnium membrane structure layers is formed in hafnium transition metal substrate surface after bright middle first time annealing；Fig. 3 is this
Five telluride hafnium membrane structure layer surfaces form the schematic diagram of three telluride hafnium membrane structure layers after second of annealing in invention；Fig. 4 is
The side view of finally formed-five telluride hafnium of three telluride hafnium-metal hafnium heterofilm material in the present invention.
In superconductor-insulator-metal heterofilm material of hafnium transition metal surface preparation high quality, integrally prepared
Journey effect diagram is as Figure 1-Figure 4, and Fig. 1 is shown in the present invention in the high coverage of (0001) surface room temperature deposition of hafnium
Tellurium particle；Fig. 2 shows the five of the sequential 2 D grown after sample annealing in the present invention on (0001) surface of hafnium
Telluride hafnium membrane material；Fig. 3 shows the sequential 2 D grown after sample annealing on (0001) surface of hafnium in the present invention
- five telluride hafnium lamination membrane material of three telluride hafniums clearly demonstrate-five telluride of three telluride hafniums in the lateral plan of Fig. 4
Hafnium-metal hafnium arrangement, the structure are extended in two-dimensional surface periodically.
Prepare the superconductor-insulator-metal heterofilm material specific steps:
Embodiment 1:
Hafnium monocrystalline is carried out multiple argon ion sputtering nearly 5 hours in vacuum chamber, then by heating metal hafnium substrate
And it is maintained at 900 DEG C of high annealings 8 minutes, obtain clean smooth (0001) crystal face.Under vacuum conditions, by appropriate high-purity
Tellurium is by silica crucible evaporation source, by metallic tellurium uniform deposition in hafnium substrate (0001) table that is clean smooth and remaining room temperature
Face.Tellurium particle as shown in Figure 1 will be deposited as shown in the scanning tunneling microscope image of Fig. 5 in substrate surface in random distribution
There is the sample of tellurium particle to anneal 15 minutes at 500 DEG C, so that being covered on the tellurium atom and substrate hafnium on hafnium substrate (0001) surface
Atom interacts, and five telluride hafnium membrane materials is formed, as shown in fig. 6, the membrane material is can be scanned tunnel microscope
The periodical superstructure characterized, this is but also the tellurium particle for being deposited on hafnium substrate (0001) surface originally disappears.Fig. 7's is micro-
Point conductance spectrum shows that the energy gap of the structure has (shown in arrow), belongs to insulating material.By above-mentioned sample into one at 560 DEG C
Step annealing 15 minutes, so that the five telluride hafniums in top react, three telluride hafnium membrane materials are formed, as shown in figure 8, shape
At three telluride hafnium membrane materials tunnel microscope can be scanned by periodic structure characterize.The differential conductance spectrum of Fig. 9 shows
There is (shown in arrow) in the superconducting energy gap of the structure, belong to superconductor material.So finally obtaining by-five telluride of three telluride hafniums
Superconductor-insulator-metal heterofilm material that hafnium-metal hafnium is constituted.
Embodiment 2:
Hafnium monocrystalline is carried out multiple argon ion sputtering nearly 3 hours in vacuum chamber, then by heating metal hafnium substrate
And it is maintained at 900 DEG C of high annealings 5 minutes, obtain clean smooth (0001) crystal face.Under vacuum conditions, by appropriate high-purity
Tellurium is by silica crucible evaporation source, by metallic tellurium uniform deposition in hafnium substrate (0001) table that is clean smooth and remaining room temperature
Face.Tellurium particle is in random distribution in substrate surface, and the sample for being deposited with tellurium particle is annealed 10 minutes at 450 DEG C, so that
The tellurium atom and substrate hafnium atom for being covered on hafnium substrate (0001) surface interact, and form five telluride hafnium membrane materials, should
Membrane material is the periodical superstructure that can be scanned tunnel microscope and be characterized, this but also be deposited on hafnium substrate originally
(0001) the tellurium particle on surface disappears.Show that the energy gap of the structure exists through differential conductance spectrum, belongs to insulating material.It will be upper
It states sample further to anneal at 600 DEG C 20 minutes, so that the five telluride hafniums in top react, forms three telluride hafniums
Membrane material, three telluride hafnium membrane materials of formation can be scanned tunnel microscope by periodic structure and characterize.Through differential conductance
Spectrum shows that the superconducting energy gap of the structure exists, and belongs to superconductor material.So finally obtaining by-five telluride hafnium of three telluride hafniums-gold
Belong to superconductor-insulator-metal heterofilm material that hafnium is constituted.
Embodiment 3:
Hafnium monocrystalline is carried out multiple argon ion sputtering nearly 6 hours in vacuum chamber, then by heating metal hafnium substrate
And it is maintained at 900 DEG C of high annealings 10 minutes, obtain clean smooth (0001) crystal face.It under vacuum conditions, will be appropriate high-purity
Tellurium is spent by silica crucible evaporation source, by metallic tellurium uniform deposition in hafnium substrate (0001) table that is clean smooth and remaining room temperature
Face.Tellurium particle is in random distribution in substrate surface, and the sample for being deposited with tellurium particle is annealed 10 minutes at 500 DEG C, so that
The tellurium atom and substrate hafnium atom for being covered on hafnium substrate (0001) surface interact, and form five telluride hafnium membrane materials, should
Membrane material is the periodical superstructure that can be scanned tunnel microscope and be characterized, this but also be deposited on hafnium substrate originally
(0001) the tellurium particle on surface disappears.Show that the energy gap of the structure exists through differential conductance spectrum, belongs to insulating material.It will be upper
It states sample further to anneal at 500 DEG C 10 minutes, so that the five telluride hafniums in top react, forms three telluride hafniums
Membrane material, three telluride hafnium membrane materials of formation can be scanned tunnel microscope by periodic structure and characterize.Through differential conductance
Spectrum shows that the superconducting energy gap of the structure exists, and belongs to superconductor material.So finally obtaining by-five telluride hafnium of three telluride hafniums-gold
Belong to superconductor-insulator-metal heterofilm material that hafnium is constituted.
More than, although the description of several embodiments of the invention, but these embodiments are intended only as example proposition
, it is not intended to limit the scope of the present invention.For these new embodiments, can be implemented with various other ways,
In the range of not departing from the gist of the invention, it is able to carry out various omissions, displacement and change.These embodiments and its change
Shape while being contained in scope and spirit of the present invention, is also contained in the invention recorded in claims and its impartial model
In enclosing.
Claims (10)
1. a kind of superconductor-insulator-metal heterofilm material, which is characterized in that be layer structure, including metal hafnium substrate
Layer, five telluride hafnium membrane structure layers and three telluride hafnium membrane structure layers, the five telluride hafnium membrane structure layer are located at the metal hafnium substrate
The surface of layer, the three telluride hafnium membrane structure layer are located at the surface of the five telluride hafnium membrane structure layer, and the layer structure is in two dimension
Extension in plane.
2. a kind of superconductor-insulator-metal heterofilm material preparation method, which comprises the steps of:
Step 1) under vacuum conditions, by appropriate high-purity tellurium hydatogenesis to hafnium transition metal substrate surface；
Step 2) is made annealing treatment, so that the metal hafnium atom on the tellurium atom and the substrate of deposition interacts to form five
Telluride hafnium sequential 2 D crystalline state membrane structure；
Step 3) further makes annealing treatment, and sends out the surface for the five telluride hafnium sequential 2 D crystalline state membrane structure to be formed again
Raw structure change forms three telluride hafniums, ultimately forms-five telluride hafnium of three telluride hafniums-metal hafnium two-dimension laminate structure, obtains by three
Superconductor-insulator-metal heterofilm material that-five telluride hafnium of telluride hafnium-metal hafnium is constituted.
3. preparation method according to claim 2, which is characterized in that tellurium used in step 1) passes through physical vapour deposition (PVD)
Method be evaporated to the hafnium transition metal substrate surface.
4. preparation method according to claim 2, which is characterized in that annealing temperature section described in step 2) is 450 DEG C
~500 DEG C, annealing time 10-20 minutes.
5. according to the described in any item preparation methods of claim 2-4, which is characterized in that form the five telluride hafnium for growing
The surface of the hafnium transition metal substrate of sequential 2 D crystalline state membrane structure is (0001) face of metal hafnium.
6. preparation method according to claim 5, which is characterized in that the forming method in (0001) face of the metal hafnium
Are as follows: first metal hafnium monocrystalline is carried out argon ion sputtering 3-6 hours in vacuum chamber, then metal hafnium substrate is heated and maintained at
900 DEG C of high annealing 5-10 minutes, formation can be scanned the periodical superstructure that tunnel microscope is characterized.
7. preparation method according to claim 6, which is characterized in that the five telluride hafnium sequential 2 D crystalline state membrane structure
The Atomic Arrangement of top can be scanned tunnel microscope and characterized.
8. preparation method according to claim 7, which is characterized in that 0.4 electron volts of the five telluride hafnium crystalline material
Energy gap can be differentiated conductance spectrum characterized.
9. preparation method according to claim 2, which is characterized in that the annealing temperature section in step 3) is 500
DEG C~600 DEG C, annealing time 10-20 minutes.
10. preparation method according to claim 2, which is characterized in that the original of the three telluride hafnium crystalline material top
Son arrangement can be scanned tunnel microscope and be characterized, and the superconducting energy gap of the three telluride hafnium crystalline material can be differentiated
Conductance spectrum is characterized.
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