CN113337887B - Application of laser-assisted MPCVD method in enhancing SiV color center of single crystal diamond and single crystal diamond with SiV color center - Google Patents

Application of laser-assisted MPCVD method in enhancing SiV color center of single crystal diamond and single crystal diamond with SiV color center Download PDF

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CN113337887B
CN113337887B CN202110607629.2A CN202110607629A CN113337887B CN 113337887 B CN113337887 B CN 113337887B CN 202110607629 A CN202110607629 A CN 202110607629A CN 113337887 B CN113337887 B CN 113337887B
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crystal diamond
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siv
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CN113337887A (en
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陶涛
叶煜聪
路鑫宇
殷梓萌
郑凯文
邹幸洁
陈凯
胡文晓
刘斌
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Nanjing University
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    • C—CHEMISTRY; METALLURGY
    • C30—CRYSTAL GROWTH
    • C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
    • C30B25/00—Single-crystal growth by chemical reaction of reactive gases, e.g. chemical vapour-deposition growth
    • C30B25/02—Epitaxial-layer growth
    • C30B25/18—Epitaxial-layer growth characterised by the substrate
    • C30B25/20—Epitaxial-layer growth characterised by the substrate the substrate being of the same materials as the epitaxial layer
    • C—CHEMISTRY; METALLURGY
    • C30—CRYSTAL GROWTH
    • C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
    • C30B25/00—Single-crystal growth by chemical reaction of reactive gases, e.g. chemical vapour-deposition growth
    • C30B25/02—Epitaxial-layer growth
    • C30B25/16—Controlling or regulating
    • C—CHEMISTRY; METALLURGY
    • C30—CRYSTAL GROWTH
    • C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
    • C30B25/00—Single-crystal growth by chemical reaction of reactive gases, e.g. chemical vapour-deposition growth
    • C30B25/02—Epitaxial-layer growth
    • C30B25/18—Epitaxial-layer growth characterised by the substrate
    • C30B25/186—Epitaxial-layer growth characterised by the substrate being specially pre-treated by, e.g. chemical or physical means
    • C—CHEMISTRY; METALLURGY
    • C30—CRYSTAL GROWTH
    • C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
    • C30B29/00—Single crystals or homogeneous polycrystalline material with defined structure characterised by the material or by their shape
    • C30B29/02—Elements
    • C30B29/04—Diamond

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Abstract

The invention discloses application of a laser-assisted MPCVD method in enhancing SiV color centers of a single crystal diamond, and the single crystal diamond with the SiV color centers, which is characterized in that: the SiV color center is formed by growing silicon-doped single crystal diamond on a single crystal diamond substrate by a laser-assisted MPCVD method. The method adopts the laser-assisted MPCVD method to prepare the single crystal diamond, si element enters diamond grains through the assistance of plasma in the preparation process to form an SiV luminescence center, so that the single crystal diamond has strong SiV luminescence characteristics.

Description

Application of laser-assisted MPCVD method in enhancing SiV color center of single crystal diamond and single crystal diamond with SiV color center
Technical Field
The invention relates to application of a laser-assisted MPCVD method in enhancing SiV color centers of a single-crystal diamond and the single-crystal diamond with the SiV color centers.
Background
Single photon emitters are light sources capable of producing photon streams with controllable quantum correlation, and are a fundamental resource of many scalable quantum information technologies. In a solid-state single photon emitter, diamond fluorescent atomic defects have excellent light stability at room temperature, and a solid-state host system combining the excellent optical characteristics of atoms with convenience and expandability can be expected. Research in the field of diamond quantum photonics has made tremendous progress since single NV centres first exhibit single photon emission properties. The SiV centers have narrower luminescence peaks than the NV centers studied most extensively. This means that the SiV center spatial coherence is good and the Zero Phonon Line (ZPL) is stronger, with about 70% of the photons emitted into the ZPL. The emission of the ZPL is very important for photon-mediated entanglement of quantum states in a plurality of emitters, so that the realization of preparing single crystal diamond with SiV central luminescence is an important material basis in the field of quantum information.
The existing methods for artificially synthesizing diamond include high-temperature high-pressure method, direct-current arc plasma jet method, hot-wire chemical vapor deposition method and microwave plasma chemical vapor deposition method. Because of the advantages of good plasma controllability, high plasma density, no electrode pollution and the like of microwave excitation, a microwave plasma chemical vapor deposition method (MPCVD method) becomes a preferred method for preparing high-quality and even device-level diamond. Therefore, if silicon impurities can be introduced in the MPCVD process, the density of SiV centers in diamond is increased, and the combination of higher crystal quality and strong SiV photoluminescence is expected to be realized. At present, methods for artificially introducing silicon impurities in the growth of diamond include MPCVD on a Si-containing substrate, a silicon ion implantation method and a method of adding Si-containing gas into process gas.
There are studies now proposing a method of producing a high-crystallinity diamond film by Laser microwave plasma chemical vapor deposition (Laser MPCVD). Research has shown that laser light can enhance the precursor reaction process, thereby reducing non-diamond constituents such as graphite and amorphous carbon. Coupling of the laser and plasma with appropriate strength generates more methyl radicals and atomic hydrogen, thereby promoting rapid growth of the diamond crystal. In the existing literature, the LMPCVD method is adopted to prepare the single crystal diamond, the main research focuses on the influence of the process parameters on the grain quality and the morphology structure of the diamond, and the aim is to obtain high-speed growth of the diamond single crystal material; however, the LMPCVD method for preparing the single crystal diamond with SiV luminescence is not reported.
Disclosure of Invention
The invention aims to provide application of a laser-assisted MPCVD method to enhance the SiV color center of a single-crystal diamond, and the single-crystal diamond with stronger SiV luminescence can be obtained.
The technical scheme adopted by the invention is as follows: the application of the laser-assisted MPCVD method in growing the SiV color center of the single crystal diamond refers to providing a C source and a Si source, growing the single crystal diamond by adopting the laser-assisted MPCVD method, and enabling the single crystal diamond to be in the range of direct laser light spots.
The method comprises the following specific steps: and performing surface roughening etching on the single crystal diamond, taking the etched single crystal diamond as a substrate, providing a gaseous C source and a solid Si source, and continuously growing the silicon-doped single crystal diamond by adopting a laser-assisted MPCVD (multi-plasma chemical vapor deposition) method to form the SiV luminous single crystal diamond. The crystal growth direction of the continuously grown single crystal diamond is consistent with that of the substrate single crystal diamond, and the single crystal diamond with SiV luminescence is formed. The etching is typically plasma etching, although other methods commonly used in the art may be used, the purpose of etching is to form rough surface nucleation sites for subsequent diamond attachment growth.
Preferably, the single crystal diamond is subjected to surface cleaning treatment before etching.
Preferably, the laser wavelength is 405-600nm, and the laser power is 10mW-100mW.
Preferably, the specific operation steps are as follows:
(1) Surface pretreatment: acid washing the monocrystal diamond, washing the surface with water, and using N 2 Fully drying with air flow, sequentially placing diamond and silicon wafer in acetone solution, anhydrous alcohol and deionized water, ultrasonic cleaning, and finally N 2 Fully drying the airflow;
(2) Etching: etching at 800-920 deg.C under 2500-3500W microwave power, introducing hydrogen gas at 100-350sccm and 100-260Torr gas pressure, and etching for 10-15min;
(3) And (3) growing: when the laser-assisted MPCVD method is used for growth, the Si source is a silicon wafer, the C source is pure methane gas, the atmosphere of hydrogen is adopted, the growth temperature is 900-1050 ℃, the microwave power is 3000-4000W, the air pressure in the cavity is 200-300Torr, the methane flow is 2-5% of the total gas flow, and the position of the monocrystalline diamond is adjusted to be in a laser direct light spot for growth.
The invention also discloses a single crystal diamond with SiV color center, which is characterized in that: the SiV color center is formed by growing silicon-doped single crystal diamond on a single crystal diamond substrate by a laser-assisted MPCVD method.
Preferably, the emission of the SiV color center has a normalized intensity value of greater than 30.
The invention has the beneficial effects that:
(1) According to the method, the laser-assisted MPCVD method is adopted to prepare the single crystal diamond, si element enters diamond grains through plasma in the preparation process, and the incident laser enhances the chemical activity in the plasma and increases the chemical activity of the Si element in the plasma. Suitable lasers may enhance the precursor reaction process, reducing the formation of graphitic and amorphous carbon. More methyl free radicals and active Si ions can be generated through the coupling of laser and plasma with proper intensity, so that Si element can be better blended into the growth process of the diamond in the growth process to form an SiV luminescence center, and the single crystal diamond has strong SiV luminescence characteristics;
(2) The surface plasma etching treatment is carried out on the monocrystalline diamond serving as the substrate, so that the surface of the monocrystalline diamond is roughened, and the subsequent growth of the silicon-doped monocrystalline diamond is facilitated;
(3) By controlling parameters such as the air pressure of the reaction chamber, the methane concentration and the like in the growth process, the single crystal diamond with different intensity SiV center luminescence can be prepared, and reference is provided for exploring the influence of laser on the single crystal diamond silicon doping under different conditions;
(4) The SiV luminous intensity of the prepared single crystal diamond is very strong, and the method has very important scientific significance and engineering value for realizing the application of the single crystal diamond in the fields of single photon sources, quantum information processing, biological markers and the like.
Drawings
FIG. 1: schematic diagram of a device for preparing single crystal diamond with SiV color center by adopting laser-assisted MPCVD method.
FIG. 2: raman spectrum of the single crystal diamond prepared in comparative example 1.
FIG. 3: raman spectrum of the single crystal diamond prepared in comparative example 2.
FIG. 4: raman spectrum of the single crystal diamond prepared in example 1.
FIG. 5: raman spectrum of the single crystal diamond prepared in example 2.
FIG. 6: comparative example 1, 2 and example 1 are photoluminescence spectra of single crystal diamonds respectively prepared.
FIG. 7: photoluminescence spectra of single crystal diamonds prepared in examples 1 and 2, respectively.
Wherein: 1. a sample; 2. a sample stage; 3. a cavity; 4. plasma; 5. laser; 6. an external laser; 7. and a transparent observation mirror is arranged at the top of the cavity.
Detailed Description
The technical solutions in the embodiments of the present invention are clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be obtained by a person skilled in the art without any inventive step based on the embodiments of the present invention, are within the scope of the present invention.
Comparative example 1: preparation of single crystal diamond
(1) Cleaning: the Ib type diamond synthesized by a high-temperature high-pressure method (HTHP method) is heated in an acid water bath at 60 ℃ for 40 minutes, and the used acid solution comprises the following components: the nitric acid is 3:1. after the acid washing is finished, the residual acid liquor on the surface is fully cleaned by water, and then N is used 2 The air flow is fully dried. Sequentially placing diamond in acetone solution, anhydrous ethanol and deionized water, ultrasonic cleaning for 5min, and finally performing N 2 And after fully drying the airflow, putting the airflow into a sample table. 4 mm.
(2) Growing: the diamond was placed on a molybdenum (Mo) tray in the center of the sample stage. Vacuum pumping is carried out to 10 -4 And (5) Torr. The sample is etched prior to growth. Etching temperature is 900 deg.C, microwave power is 3000W, flow of introduced hydrogen is 300sccm, pressure in the chamber is 250Torr, and etching time is 15min.
After etching, the conditions in the cavity are adjusted to growth conditions as follows: the growth temperature is 950-970 ℃, the microwave power is 3400W, the flow rates of hydrogen and methane are 576sccm and 24sccm respectively (namely, the methane concentration is 4%), and the pressure in the chamber is 275Torr. The growth was maintained for 5h under this series of conditions.
(3) Removing graphite: putting the diamond into acid solution (nitric acid: sulfuric acid is 1:1) at 220 ℃ to heat in a water bath for 20min, taking out residual acid solution on the surface of the diamond, and drying the diamond.
And (3) testing: observing the components of the single crystal diamond by using Raman spectrum with excitation light wavelength of 514 nm; and testing SiV luminescence property of the single crystal diamond by photoluminescence spectrum.
FIG. 2 is a Raman spectrum of a single crystal diamond grown in this comparative example, the spectrum being shown at 1332cm -1 The characteristic peak of diamond appears, the full width at half maximum FWHM =2.1509cm -1 ；1130cm -1 The nearby absorption peak corresponds to the ib-type nitrogen (mono-substituted nitrogen). The line segment in fig. 6 is the photoluminescence spectrum obtained in this comparative example, and it can be seen that the grown diamond has no significant SiV luminescence peak due to the unintentional doping in the cavity.
Comparative example 2: preparation of single crystal diamond with SiV luminescence center
(1) Cleaning: the Ib type diamond synthesized by a high-temperature high-pressure method (HTHP method) is heated in an acid water bath at 60 ℃ for 40 minutes, and the used acid solution comprises the following components: the nitric acid is 3:1. after the acid washing is finished, the residual acid liquor on the surface is fully cleaned by water, and then N is used 2 The air flow is fully dried. Sequentially placing diamond and silicon wafer in acetone solution, anhydrous ethanol and deionized water, ultrasonic cleaning for 5min, and finally N 2 And after fully drying the airflow, putting the airflow into a sample table. The wafer size was 1 inch by 1 inch.
(2) Growing: the silicon wafer is placed on a molybdenum (Mo) tray in the center of the sample table, and the diamond is placed in the center of the silicon wafer. Vacuum pumping is carried out to 10 -4 And (5) Torr. The sample is etched prior to growth. Etching temperature is 900 deg.C, microwave power is 3000W, flow of introduced hydrogen is 300sccm, pressure in the chamber is 250Torr, and etching time is 15min. After etching, the conditions in the cavity are adjusted to growth conditions as follows: the growth temperature is 950-970 deg.C, and the microwave powerAt 3400W, the flow rates of hydrogen and methane were 576sccm and 24sccm, respectively (i.e., the methane concentration was 4%), and the pressure in the chamber was 275Torr. The growth is carried out for 5h by keeping the condition parameter.
(3) Removing graphite: putting the diamond into 220 ℃ acid solution (nitric acid: sulfuric acid is 1:1) to be heated in a water bath for 20min, taking out residual acid solution on the surface of the diamond, and drying the diamond.
And (3) testing: observing the components of the single crystal diamond by using Raman spectrum with excitation light wavelength of 514 nm; and testing SiV luminescence property of the single crystal diamond by photoluminescence spectrum.
FIG. 3 is a Raman spectrum of a single crystal diamond grown according to the comparative example, the spectrum being shown at 1332cm -1 The characteristic peak of diamond appears, the full width at half height FWHM =2.1514cm -1 ；1130cm -1 The nearby absorption peak corresponds to the ib-type nitrogen (mono-substituted nitrogen). The broken line segment in FIG. 6 is the photoluminescence spectrum obtained in this comparative example, and it can be seen that the sample has a SiV luminescence peak at 738nm, the full width at half maximum FWHM =4.9457cm -1 . And (3) making a ratio of the intensity of the SiV luminescence peak at 738nm to the intensity of the Raman signal peak at 552.5nm to obtain a normalized intensity value of SiV luminescence of the sample. The normalized intensity value for SiV luminescence for this comparative example was calculated to be 18.12. This indicates that we prepared single crystal diamond with SiV luminescent centers due to the silicon doping introduced by the plasma in the silicon wafer.
Example 1: laser-assisted MPCVD method for preparing single crystal diamond with SiV luminescence center
(1) Cleaning: the Ib type diamond synthesized by a high-temperature high-pressure method (HTHP method) is heated in an acid water bath at 60 ℃ for 40 minutes, and the used acid solution comprises the following components: the nitric acid is 3:1. after the acid washing is finished, the residual acid liquor on the surface is fully cleaned by water, and then N is used 2 The air flow is fully dried. Sequentially placing diamond and silicon wafer in acetone solution, anhydrous alcohol and deionized water, ultrasonic cleaning for 5min, and finally N 2 And after fully drying the airflow, putting the airflow into a sample table. The wafer size was 1 inch by 1 inch.
(2) Growing: the silicon wafer is placed on a molybdenum (Mo) tray in the center of the sample table, and the diamond is placed in the center of the silicon wafer. Vacuum pumping is carried out to 10 -4 And (5) Torr. Before growth, firstly toAnd etching the sample, turning on laser, wherein the laser wavelength is 514nm, the power is adjusted to be 60mW, and the laser directly irradiates the size of a circular spot to uniformly cover the molybdenum tray, the silicon wafer and the diamond. Etching temperature is 900 deg.C, microwave power is 3000W, flow of introduced hydrogen is 300sccm, pressure in the chamber is 250Torr, and etching time is 15min.
After etching, the conditions in the cavity are adjusted to growth conditions as follows: the growth temperature is 950-970 ℃, the microwave power is 3400W, the flow rates of the hydrogen and the methane are 576sccm and 24sccm respectively (namely, the methane concentration is 4%), and the air pressure in the chamber is 275Torr. The growth was maintained for 5h under this series of conditions.
(3) Removing graphite: to remove the graphite phase, the diamond was placed in an acid solution (nitric acid: sulfuric acid: 1:1) at 220 ℃ and heated in a water bath for 20min, and the residual acid solution on the surface was taken out and washed and then dried.
And (3) testing: observing the components of the single crystal diamond by using Raman spectrum with excitation light wavelength of 514 nm; and testing SiV luminescence property of the single crystal diamond by photoluminescence spectrum.
FIG. 4 is a Raman spectrum of a single crystal diamond grown in this example, the spectrum being at 1332cm -1 The characteristic peak of diamond appears, the full width at half height FWHM =2.3909cm -1 ；1130cm -1 The nearby absorption peak corresponds to the ib-type nitrogen (mono-substituted nitrogen). The solid line segment in FIG. 6 is the photoluminescence spectrum obtained for this example and it can be seen that the sample has a SiV luminescence peak at 738nm, which has a full width at half maximum FWHM =5.0223cm -1 . The SiV luminescence peak for this example is stronger compared to the dashed line segment of comparative example 2. And (3) making a ratio of the intensity of the SiV luminescence peak at 738nm to the intensity of the Raman signal peak at 552.5nm to obtain a normalized intensity value of SiV luminescence of the sample. Through calculation, the normalized intensity value of SiV luminescence in this embodiment is 32.48. This indicates that the laser promotes silicon doping during diamond deposition due to the silicon doping introduced by the wafer via the plasma, in which case the resulting single crystal diamond has a stronger SiV luminescence peak.
Example 2: laser-assisted MPCVD method for preparing single crystal diamond with SiV luminescence center
(1) Cleaning: using diamond type Ib synthesized by high-temperature high-pressure method (HTHP method)Heating the stone in an acid liquor water bath at 60 ℃ for 40 minutes, wherein the used acid liquor comprises the following components: the nitric acid is 3:1. after the acid washing is finished, the residual acid liquor on the surface is fully cleaned by water, and then N is used 2 The air flow is fully dried. Sequentially placing diamond and silicon wafer in acetone solution, anhydrous alcohol and deionized water, ultrasonic cleaning for 5min, and finally N 2 And after fully drying the airflow, putting the airflow into a sample table. The wafer size was 1 inch by 1 inch.
(2) Growing: the silicon wafer is placed on a molybdenum (Mo) tray in the center of the sample table, and the diamond is placed in the center of the silicon wafer. Vacuum pumping is carried out to 10 -4 And (5) Torr. The sample is etched prior to growth. Etching temperature is 900 deg.C, microwave power is 3000W, flow of introduced hydrogen is 300sccm, pressure in the chamber is 250Torr, and etching time is 15min.
After etching, the conditions in the cavity are adjusted to growth conditions as follows: and (3) turning on laser, wherein the laser wavelength is 514nm, the power is adjusted to be 60mW, and the size of a laser circular spot can uniformly cover the molybdenum tray, the silicon wafer and the diamond. The growth temperature is 950-970 ℃, the microwave power is 3400W, the flow rates of hydrogen and methane are 576sccm and 24sccm respectively (namely, the methane concentration is 4%), and the pressure in the chamber is 275Torr. The growth was maintained for 5h under this series of conditions.
(3) Removing graphite: to remove the graphite phase, the diamond was placed in an acid solution (nitric acid: sulfuric acid: 1:1) at 220 ℃ and heated in a water bath for 20min, and the residual acid solution on the surface was taken out and washed and then dried.
And (3) testing: observing the components of the single crystal diamond by using Raman spectrum with excitation light wavelength of 514 nm; and testing SiV luminescence property of the single crystal diamond by photoluminescence spectrum.
FIG. 5 is a Raman spectrum of a single crystal diamond grown in this example, the spectrum being at 1332cm -1 The characteristic peak of diamond appears, the full width at half height FWHM =2.3760cm -1 ；1130cm -1 The nearby absorption peak corresponds to the ib-type nitrogen (mono-substituted nitrogen). The broken line segment in fig. 7 is the photoluminescence spectrum obtained in this example. (Note: the solid line segment in FIG. 7 is the photoluminescence spectrum of example 1, which is consistent with the solid line segment in FIG. 6, where the curve is separately highlighted in FIG. 7 for simplicity of illustration and comparison with this example). It can be seen that the sample is at 738nmHas SiV luminescence peak with full width at half maximum FWHM =5.0765cm -1 . And (3) making a ratio of the intensity of the SiV luminescence peak at 738nm to the intensity of the Raman signal peak at 552.5nm to obtain a normalized intensity value of SiV luminescence of the sample. The normalized intensity value of SiV luminescence for this example was calculated to be 30.92.
The used device structure comprises a sample table 2, a cavity 3, a laser 5, an external laser 6 and a transparent observation mirror 7 at the top of the cavity. A sample 1 is placed on a sample table 2, the sample table 2 is located in a cavity 3, plasma 4 is excited in the cavity to etch and grow the sample 1, and an external laser 6 emits laser to cover the plasma 4 and the sample 1.
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such changes, modifications, substitutions, combinations, and simplifications are intended to be included in the scope of the present invention.

Claims (5)

1. The application of the laser-assisted MPCVD method in the growth of the SiV color center of the single crystal diamond is characterized in that: the method comprises the following specific steps: the surface of the single crystal diamond is coarsened and etched, the etched single crystal diamond is used as a substrate, a gaseous C source and a solid Si source are provided, the silicon-doped single crystal diamond continues to grow by adopting a laser-assisted MPCVD method, the single crystal diamond is positioned in the range of direct laser spots, the laser wavelength is 405-600nm, and the laser power is 10mW-100mW, so that the single crystal diamond with SiV luminescence is formed.
2. Use according to claim 1, characterized in that: before etching, the single crystal diamond is firstly subjected to surface cleaning treatment.
3. The application according to claim 2, characterized by the specific operating steps of:
(1) Surface pretreatment: acid washing the monocrystal diamond, washing the surface with water, and using N 2 Fully drying by airflow to obtain diamond and silicon waferSequentially placing in acetone solution, anhydrous alcohol and deionized water, ultrasonic cleaning, and finally N-washing 2 Fully drying the airflow;
(2) Etching: etching at 800-920 deg.C under 2500-3500W microwave power, introducing hydrogen gas at 100-350sccm and 100-260Torr gas pressure, and etching for 10-15min;
(3) Growing: when the laser-assisted MPCVD method is used for growing, the Si source is a silicon wafer, the C source is pure methane gas, the atmosphere of hydrogen is adopted, the growth temperature is 900-1050 ℃, the microwave power is 3000-4000W, the air pressure in the cavity is 200-300Torr, the methane flow is 2-5% of the total gas flow, and the position of the monocrystalline diamond is adjusted to be in a laser direct-injection light spot for growing.
4. A single crystal diamond having an SiV color center, characterized by: the SiV color center is formed by growing silicon-doped monocrystalline diamond on a monocrystalline diamond substrate by adopting a laser-assisted MPCVD method, and the method comprises the following specific steps: the surface of the single crystal diamond is coarsened and etched, the etched single crystal diamond is used as a substrate, a gaseous C source and a solid Si source are provided, the silicon-doped single crystal diamond continues to grow by adopting a laser-assisted MPCVD method, the single crystal diamond is positioned in the range of direct laser spots, the laser wavelength is 405-600nm, and the laser power is 10mW-100mW, so that the single crystal diamond with SiV luminescence is formed.
5. The single crystal diamond having an SiV color center according to claim 4, wherein: the normalized intensity value of the light emission of the SiV color center is greater than 30.
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CN107419329B (en) * 2017-05-22 2019-08-27 北京科技大学 The preparation method of the full carbon structure of single-crystal diamond surface in situ n-type semiconductorization
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