CN104694907B - Radio-frequency discharge vapor deposition method for preparing nickel-nitrogen-doped diamond - Google Patents
Radio-frequency discharge vapor deposition method for preparing nickel-nitrogen-doped diamond Download PDFInfo
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- CN104694907B CN104694907B CN201510097097.7A CN201510097097A CN104694907B CN 104694907 B CN104694907 B CN 104694907B CN 201510097097 A CN201510097097 A CN 201510097097A CN 104694907 B CN104694907 B CN 104694907B
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Abstract
The invention relates to a radio-frequency discharge vapor deposition method for preparing nickel-nitrogen-doped diamond, belonging to the technical field of diamond vapor deposition preparation. Injected radio-frequency discharge plasma is utilized to enhance chemical vapor deposition and implement preparation of the nickel-nitrogen-doped diamond. The plasma excited by radio-frequency discharge is injected onto the substrate, and technical parameters are adjusted to construct the stable plasma boundary layer, thereby implementing controllable-dopant-atom-concentration deposition. The characteristic of mild radio-frequency discharge plasma electric field is utilized to ensure the stability of the polyatomic configuration and keep the completeness of the mask material regular pattern on the substrate, thereby implementing positioned deposition of dopant atoms. The method can satisfy the requirements for polyatomic configuration doping. The method implements regular distribution and growth of the nickel-nitrogen-doped diamond, so that the distribution interval of the doped diamond can achieve 50-mu m regularized distribution.
Description
Technical field
The invention belongs to diamond vapour deposition preparing technical field, in particular, provide one kind and prepare nickel-N doping gold
The radio frequency discharge CVD method of hard rock, strengthens chemical vapor deposition using the rf (discharge) plasma of injection and realizes
Nickel-N doping diamond preparation.
Background technology
With social development, people propose more, faster requirement to information content and processing speed.Entangled using quantum
Twine effect and carry out information transmission and the quantum communication calculating and quantum calculation because its data volume is big, good confidentiality, arithmetic speed
Fast feature is just becoming new communication and calculation, and (straight prestige, Chen Wei, Sun Fangwen, etc. quantum information technology is scanned, section
Learn and circulate a notice of, 57 (17) (2012): 1498-1525).The basis of quantum communication and quantum calculation to coherent superposition or is tangled
[Li Chengzu, etc. " quantum communications and quantum for the quantum information process of quantum state realization coding, transmission and the control calculating and manipulation
Calculate ", publishing house of the National University of Defense technology, Changsha, 2000].Diamond exactly can undertake the preferable material of quantum information process
Material, because when comprising the doped structure of atomic scale in diamond, can show special amount in the presence of external excitation
Sub- effect, such as regulatable single quantum bit and muliti-qubit, the quantum state that can deposit, can be by double amounts of gate operation
Sub- bit, and Entangled State three quantum bit etc. (i.aharonovich, e.neu, diamond nanophotonics,
Advanced optical materials, 2 (2014): 911 928), and these structures have very long electricity at room temperature
Son spin decoherence time, pure spin environment and the hyperfine interaction enriched with nuclear spin around, therefore, this tool
Have the diamond of atomic scale doped structure have broad prospects in quantum information process (f.c.waldermann,
P.olivero, j.nunn etc., creating diamond color centers for quantum optical
Applications, diamond＆related materials, 16 (2007): 1,887 1895).Current sharp in a diamond
Be used for carry out quantum information process doped structure be nitrogen-atoms-room configuration (l.childress, m.v.gurudevdutt,
J.m.taylor, etc. coherent dynamics of coupled electronand nuclear spin qubits in
Diamond, science, 314 (2006): 281-285), since it was reported from 1997 (j.i.cirac, p.zoller,
H.j.kimble, etc. quantum state transfer and entanglement distribution among
, main system distant nodes in a quantum network.phys.rev.lett.78 (1997): 3221-3224)
Standby technology is that (d.p.ertchak, v.g.efimov, v.f.stelmakh, etc. the origin of for ion implantation technique
dominating esr absorption in ion implanted diamond,physica status solidi b-
Basic research, 203 (2) (1997): 529-547), this technology is to introduce using after the nitrogen-atoms ionization of doping is accelerated
To one of diamond material modification method.In addition to ion implantation technique, chemical vapour deposition technique also becomes a kind of
The technology (michl, the julia that prepare nitrogen-atoms-room configuration doped structure of candidate；teraji,tokuyuki；zaiser,
sebastian；Deng perfect alignment and preferential orientation of nitrogen-
vacancy centers during chemical vapor deposition diamond growth on(111)
Surfaces, applied physics letters, 104 (10) (2014): 102407).Chemical vapour deposition technique is will
The atom (or polyatom configuration) of doping imports to reaction zone as the presoma of deposition reaction, agglomerates in deposition process
In the lattice of diamond, form the doped structure of atomic scale.Recently, in diamond, a kind of nickel-nitrogen configuration of atomic scale is mixed
Miscellaneous structure is found in and has many good qualities in quantum performance, be provide the optimal single-photon source of quantum bit (t.gaebel and
J.wrachtrup, stable single-photon source in the near infrared, new journal of
Physics, 6 (2004): 98-104).But, up to the present, an only external seminar reports using microwave legal system
(j.r.rabeau, y.l.chin, s.prawer, etc. fabrication of single nickel- for standby result
Nitrogen defects in diamond by chemical vapor deposition, applied physics
Letters 86 (2005): 131926).
Ion implantation technique is only limitted to make the nitrogen-atoms-room doping in diamond at present, adulterates but for polyatom
Difficult to realize, such as carry out the preparation just not success of nickel-N doping using this technology.The reason analyze its failure, former from it
It can be seen that the process of ion implanting is using ion exposure (injection) Buddha's warrior attendant through acceleration, atom to be adulterated in reason
Shi Zhong, thus form a superficial layer (implanted layer) with special nature in selected (being injected into) region.So
The speciality of this technology is by monoatomic doping, is difficult to carry out polyatomic doping, the limitation of this exactly this technology.Compare it
Under, chemical vapour deposition technique is relatively suitable for carrying out polyatomic doping in a diamond, but, currently used chemical gaseous phase
Deposition technique is all chemical vapor deposition using microwave plasma enhanced it is impossible to ensure the regular distribution life of doped diamond
Long, it is unsatisfactory for carrying out the requirement that the quantum information of next step is processed；And because microwave plasma ionization level is higher, it is difficult to protect
The realization of card polyatom configuration doping.In order to expand the preparation species of doped diamond, meet the requirement of polyatom configuration doping,
It is badly in need of providing new technology of preparing.
Content of the invention
It is an object of the invention to provide a kind of radio frequency discharge CVD method preparing nickel-N doping diamond, profit
Strengthen chemical vapor deposition with the rf (discharge) plasma of injection, realize nickel-N doping diamond preparation.By radio frequency discharge
The plasma exciting graze substrate in the way of spraying, constructs stable plasma boundary by adjusting process parameter
Layer, realizes the controllable deposition of concentration of dopant atoms；On the other hand, using the feature that rf (discharge) plasma electric field is gentle, come
Ensure the stability of polyatom configuration configuration and the integrality keeping mask material rule style on substrate, thus realizing adulterating
The pin deposition of atom.This method can meet the requirement of polyatom configuration doping.
Nickel of the present invention-N doping diamond is to carry out in rf (discharge) plasma injection chemical gas-phase deposition system
's.Radio frequency inductive coupled discharge exciting method is wherein adopted to produce plasma, it is former that the composition of plasma contains excitation state carbon
The nickle atom of son, hydrocarbon molecules, hydrogen atom and doping and nitrogen-atoms, the electron temperature of plasma is in 0.7-2ev.Plasma
The spout geometry of body is circle, and area is 3-20 centimetre2.The axis of movement of plasma is parallel to horizontal direction, Reynolds
Number is 1200-2400, the angle graze substrate surface that plasma is 60 °～90 ° with axis of movement and substrate normal angle.Lining
Bottom is single-crystal diamond, and its surface has the mask being formed by refractory metal, and the crystal face that exposes to the open air of substrate is (100) crystal face, with machine
Tool is inlayed or the mode of vacuum brazing is fixed on the refractory metal substrate bracket with water cooling function, and the size of substrate is 1
～6 centimetres2, the distance away from plasma jet for the substrate be 0.5～1.5 centimetre, underlayer temperature is between 650 DEG C～1300 DEG C.
Reaction chamber pressure is between 6000～18000pa.
Advantages of the present invention and good effect:
Process provides an injection in addition to microwave method, that nickel-N doping diamond preparation can be achieved
Rf (discharge) plasma strengthens chemical vapour deposition technique approach it is achieved that the regular distribution of nickel-N doping diamond grows,
Make doped diamond distribution spacing reach 50 μm regularization distribution.
Brief description
Fig. 1 is the schematic diagram of rf (discharge) plasma jet deposition system, wherein, quartz ampoule 1, radio-frequency coil 2, deposition
Chamber 3, plasma 4, the substrate of water-cooled and bearing 5, vacuum pump group 6.
Fig. 2 is the result of variations with graze distance for the composition of plasma.
Fig. 3 is the electron scanning micrograph of substrate surface au mask.
Fig. 4 is the electron scanning micrograph of qd-1 sample.
Fig. 5 is the electron scanning micrograph of qd-2 sample.
Fig. 6 is the power spectrum result of qd-1 sample.
Fig. 7 is the power spectrum result of qd-2 sample.
Fig. 8 is the Raman spectrum result of qd-1 sample.
Fig. 9 is the Raman spectrum result of qd-2 sample.
Specific embodiment
In injection rf (discharge) plasma depositing system shown in Fig. 1, test plasma using light emission spectrum
Composition with the situation of change of graze distance, obtained the result of Fig. 2, therefrom visible plasma composition be mainly carbon, hydrogen,
Argon, nickel and nitrogen, each excited atom and atomic configuration concentration in the growth district of diamond is stable.In (100), crystal face is
Expose the single-crystal diamond surface of crystal face to the open air, au mask is prepared for using photoetching technique and magnetron sputtering technique, obtain the knot of Fig. 3
Really, the circular deposition hole that spacing is 50 μm of having arranged can be seen from result on mask.It is doped the heavy of diamond preparation
Long-pending technological parameter is shown in Table 1, the obtained electron microscopic pattern of doped diamond, power spectrum composition and with Raman (raman) spectrum
Result is shown in Fig. 4 to Fig. 9 respectively.
The deposition parameter of doped diamond prepared by table 1.
The deposition parameter of doped diamond prepared by table 1.
Claims (1)
1. a kind of radio frequency discharge CVD method preparing nickel-N doping diamond is it is characterised in that nickel-N doping Buddha's warrior attendant
Stone is carried out in rf (discharge) plasma injection chemical gas-phase deposition system；Radio frequency inductive coupled discharge is wherein adopted to swash
Forwarding method produces plasma, and the composition of plasma contains the nickel of excitation state carbon atom, hydrocarbon molecules, hydrogen atom and doping
Atom and nitrogen-atoms, the electron temperature of plasma is in 0.7-2ev；The spout geometry of plasma is circle, and area is
3-20 centimetre2；The axis of movement of plasma is 1200-2400 parallel to horizontal direction, Reynolds number, and plasma is with kinematic axis
Line and substrate normal angle are 60 °～90 ° of angle graze substrate surface；Substrate is single-crystal diamond, and its surface has by difficulty
The mask that molten metal is formed, the crystal face that exposes to the open air of substrate is (100) crystal face, is fixed in the way of cast setting or vacuum brazing
Have on the refractory metal substrate bracket of water cooling function, the size of substrate is 1～6 centimetre2, substrate away from plasma jet away from
From for 0.5～1.5 centimetre, between 650 DEG C～1300 DEG C, reaction chamber pressure is between 6000～18000pa for underlayer temperature.
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| CN201510097097.7A CN104694907B (en) | 2015-03-04 | 2015-03-04 | Radio-frequency discharge vapor deposition method for preparing nickel-nitrogen-doped diamond |
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| CN201510097097.7A CN104694907B (en) | 2015-03-04 | 2015-03-04 | Radio-frequency discharge vapor deposition method for preparing nickel-nitrogen-doped diamond |
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| CN104694907B true CN104694907B (en) | 2017-01-25 |
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Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109518159B (en) * | 2018-11-21 | 2020-12-04 | 中国科学院大学 | Method for growing diamond by codoping transition metal elements and nitrogen |
| CN110835741B (en) * | 2019-10-28 | 2020-09-18 | 北京科技大学 | Method for preparing diamond nitrogen-nickel composite color center through ion implantation |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5174983A (en) * | 1990-09-24 | 1992-12-29 | The United States Of America, As Represented By The Secretary Of The Navy | Flame or plasma synthesis of diamond under turbulent and transition flow conditions |
| CN103370765A (en) * | 2010-12-23 | 2013-10-23 | 六号元素有限公司 | Controlling doping of synthetic diamond material |
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2015
- 2015-03-04 CN CN201510097097.7A patent/CN104694907B/en not_active Expired - Fee Related
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5174983A (en) * | 1990-09-24 | 1992-12-29 | The United States Of America, As Represented By The Secretary Of The Navy | Flame or plasma synthesis of diamond under turbulent and transition flow conditions |
| CN103370765A (en) * | 2010-12-23 | 2013-10-23 | 六号元素有限公司 | Controlling doping of synthetic diamond material |
Non-Patent Citations (1)
| Title |
|---|
| "Fabrication of single nickel-nitrogen defects in diamond by chemical vapor deposition";J.R. Rabeau et al.;《APPLIED PHYSICS LETTERS》;20051231;第86卷;第131926-1页右栏第2-4段 * |
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