CN114000190B - Method for realizing high-flux film growth by adopting temperature gradient - Google Patents
Method for realizing high-flux film growth by adopting temperature gradient Download PDFInfo
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- CN114000190B CN114000190B CN202111261646.1A CN202111261646A CN114000190B CN 114000190 B CN114000190 B CN 114000190B CN 202111261646 A CN202111261646 A CN 202111261646A CN 114000190 B CN114000190 B CN 114000190B
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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
- C30B23/00—Single-crystal growth by condensing evaporated or sublimed materials
- C30B23/02—Epitaxial-layer growth
- C30B23/025—Epitaxial-layer growth characterised by the substrate
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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
- C30B23/00—Single-crystal growth by condensing evaporated or sublimed materials
- C30B23/02—Epitaxial-layer growth
- C30B23/06—Heating of the deposition chamber, the substrate or the materials to be evaporated
- C30B23/063—Heating of the substrate
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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
- C30B33/00—After-treatment of single crystals or homogeneous polycrystalline material with defined structure
- C30B33/02—Heat treatment
Abstract
The invention discloses a method for realizing high flux film growth by adopting temperature gradient, which is characterized in that on the basis of a heat source capable of uniformly heating a substrate, another auxiliary heat source is introduced, and a sample holder of the fixed substrate and any position of the substrate are heated by adopting the auxiliary heat source to form a local high temperature point, so that the temperature gradient is generated on the surface of the substrate, and the high flux single crystal film with the same elements and different chemical components is grown on the surface of the substrate. The method has simple and flexible process, greatly shortens the growth and research process of the film, and provides powerful technical means for the research and production of films with various properties.
Description
Technical Field
The invention relates to the technical field of semiconductor manufacturing, in particular to a method for realizing high-flux film growth by adopting a temperature gradient.
Background
Substrate epitaxial growth is one of the main methods for material growth, and the molecular beam epitaxial growth film can be used for preparing most of the existing devices, and can also be used for preparing a plurality of new devices, including superlattice structure high electron mobility transistors and multiple quantum well type laser diodes and the like which are difficult to realize by other methods, such as by means of atomic scale film thickness control. The epitaxial growth of the film is carried out in ultrahigh vacuum, the surface of the substrate can be completely clean after being processed, contamination can be avoided in the epitaxial process, the epitaxial film growth process is a physical deposition process, intermediate chemical reaction is not required to be considered, the influence of quality transmission is avoided, the composition and the structural integrity of the epitaxial layer can be monitored at any time, the growth and interruption can be instantaneously controlled by utilizing a shutter, the components and the doping concentration of the film can be rapidly adjusted along with the change of an evaporation source, the epitaxial layer with excellent quality can be grown, and therefore, the epitaxial film is widely used for scientific research work. However, the reaction conditions of the film growth reaction chamber are strict, and a high-vacuum, high-temperature and chemically active growth environment is required. But also determines that the film growth is actually an atomic scale processing technology, the growth efficiency is low, and only one specific film sample can be grown at one time. When different reconstructions of the analytical substrate of the system are required to influence the growth of the film and to study the film properties of different compositions, a great deal of manpower and time are often required.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a method for realizing high-flux film growth by adopting a temperature gradient, which can simultaneously grow high-flux single crystal films with the same elements and different chemical components on the same substrate, thereby greatly improving the film growth efficiency.
The purpose of the invention is realized by the following technical scheme:
a method for realizing high flux film growth by adopting temperature gradient is characterized in that on the basis of a heat source capable of uniformly heating a substrate, another auxiliary heat source is introduced, and the auxiliary heat source is adopted to heat a sample holder for fixing the substrate and any position of the substrate to form a local high temperature point, so that the temperature gradient is generated on the surface of the substrate, and the high flux single crystal film with the same elements and different chemical components is grown on the surface of the substrate.
Further, the method comprises the steps of:
step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 Uniformly heating the sample holder by adopting a heat source in an ultra-vacuum environment of mbar, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: adjusting the substrate temperature obtained in the step S2 to the film growth temperature, heating the substrate surface by adopting an auxiliary heat source after the temperature is stable, maintaining the temperature gradient of the substrate surface as a fixed value together, and then controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
and step S4: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
Further, when the growth of the single crystal thin film requires pretreatment, the S3 is replaced by:
controlling the temperature of the substrate obtained in the step S2 within a pre-annealing temperature range of film growth, heating any position of the surface of the substrate by adopting an auxiliary heat source to realize that the temperature difference of different positions of the surface of the substrate is more than or equal to 50 ℃, and maintaining the two heat sources together for a period of time to realize a pre-annealing process with a temperature gradient on the surface of the substrate;
and adjusting the surface temperature of the substrate to the film growth temperature, adopting an evaporation source after the temperature is stable, and controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source.
Further, when the growth of the single crystal thin film requires a post-treatment, the S3 is replaced with:
adjusting the surface temperature of the substrate to the film growth temperature, adopting an evaporation source after the temperature is stable, and controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
the temperature of the substrate with the film is controlled within the post-annealing temperature range of the growth of different film samples, then an auxiliary heat source is adopted to heat the surface of the substrate or any position of a sample holder, the temperature difference of different positions of the surface of the substrate is more than or equal to 50 ℃, and the two heat sources are jointly maintained for a period of time, so that the post-annealing process of the surface temperature gradient of the sample is realized.
Further, when the growth of the single crystal film requires pretreatment and post-treatment at the same time, after the growth thickness of the film on the substrate is controlled, the temperature of the substrate on which the film is grown is controlled within the post-annealing temperature range for the growth of different film samples, then an auxiliary heat source is adopted to heat the substrate surface or any position of the sample holder, the temperature difference of different positions of the substrate surface is larger than or equal to 50 ℃, and the two heat sources are maintained together for a period of time, so that the post-annealing process for the temperature gradient of the sample surface is realized.
Further, the substrate with the atomic-scale step surface is fixed on the sample holder by adopting a mechanical mode or a glue fixing mode.
Further, the evaporation source is selected from any one of a resistance heating type thermal evaporation source, an electron gun heating evaporation source, and electron beam heating.
Further, the auxiliary heat source is selected from any one of laser heating, resistance heating, electron beam heating, and infrared heating.
The invention has the following beneficial effects:
1. the invention firstly proposes that an auxiliary heat source is introduced to realize the temperature gradient of the surface of the substrate and obtain a film sample with continuously changed components on the same substrate;
2. the invention can realize the preparation of film samples with different components on the same substrate, and shortens the research and development period and development.
3. In the pre-treatment stage: by introducing an auxiliary heat source, different pre-annealing temperatures can be realized on the same substrate, which is beneficial to forming different surface reconstructions, such as reconstruction of 4 × 1, 3 × 1, 2 × 1 and the like on the same SrTiO3 substrate, thereby obtaining films with different structures, such as hexagonal and tetragonal films grown on the same substrate. The traditional method can only obtain reconstruction and film of one structure, annealing before gradient obtains different structures, and continuous change of the structures along with temperature can be observed at the same time.
4. And (3) growth stage: and an auxiliary heat source is introduced, so that the temperature gradient in the growth stage can be realized. In MBE growth, the growth temperature determines the film quality, different growth temperatures and different film quality, the traditional heating needs a large amount of time to search for a proper growth temperature, and the gradient temperature growth also obtains at least 3 temperature points in one experiment, thereby greatly shortening the research and development time. In addition, some elements reaching the substrate surface in the form of molecular clusters, such as chalcogen Se, are often distilled out in the form of Se4 or Se8, and the elements can be decomposed and react with other elements to form a thin film only by a certain temperature, and the gradient growth temperature can be used for conveniently and quickly searching the temperature point, and simultaneously, the expense for upgrading from a k-cell source to a cracking source is saved.
5. And (3) in a post-treatment stage: and introducing an auxiliary heat source to realize different post-annealing temperatures of the same substrate. For some special material growth, the post-annealing temperature also determines the film quality, for example, the growth of FeSe can be realized, high-quality FeSe can be formed only by post-annealing above a certain temperature, the temperature interval is very small, the high temperature can be decomposed, a large amount of time and a substrate are required for searching the temperature interval in the traditional heating, the temperature interval can be quickly found by gradient post-annealing realized by auxiliary heating, the research and development period is shortened, and the use cost is reduced.
Drawings
For a better understanding of the description and/or illustration of embodiments and/or examples of those applications disclosed herein, reference may be made to one or more of the drawings. The additional details or examples used to describe the figures should not be considered limiting of the scope of any of the disclosed applications, the presently described embodiments and/or examples, and the presently understood best mode of such applications.
FIG. 1 is a flow chart of the steps performed by the present invention;
FIG. 2 is a schematic diagram of a temperature gradient high-throughput thin film growth apparatus provided in an embodiment of the present invention;
FIG. 3 is a schematic diagram of the temperature gradient on the surface of the sample in FIG. 2.
Detailed Description
The present invention will be described in detail below with reference to the accompanying drawings and preferred embodiments, and the objects and effects of the present invention will become more apparent, it being understood that the specific embodiments described herein are merely illustrative of the present invention and are not intended to limit the present invention.
Referring to fig. 1, the method for realizing high-flux film growth by using temperature gradient according to the present invention includes the following steps:
step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
the fixing mode of fixing the substrate on the sample holder comprises the following steps: mechanical fixation or colloidal fixation. Wherein, mechanical fastening includes: fixing modes such as pressing sheets and spot welding; the glue used for fixing the glue comprises: carbon glue, platinum glue, silver glue, etc.
The sample support can be made of copper (Cu), stainless steel (Inconel), molybdenum (Mu), silicon carbide (SiC) and the like, has excellent heat conducting property, is beneficial to more uniform temperature of the surface of the substrate, and reduces the temperature outwards along the heating point serving as the circle center under the heating condition of the auxiliary heating equipment.
The sample support is unfixed in form and thickness and can be a flat plate support or a support with steps.
Step S2: the sample holder with the substrate fixed is placed at less than 1e10 -9 In an ultra-high vacuum system with mbar, a heat source is adopted to uniformly heat the sample holder, so that the temperature of the substrate is raised to remove impurities on the surface of the substrate;
and step S3: adjusting the substrate temperature obtained in the step (S2) to the film growth temperature, heating the substrate surface by adopting an auxiliary heat source after the temperature is stable, maintaining the temperature gradient of the substrate surface as a fixed value, and then controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
here, for different single crystal films, the introduction of the auxiliary heat source may run through the whole process of sample generation, or only in the process that the sample needs pre-treatment or post-treatment or sample growth, so that the two heat sources jointly implement a pre-annealing process in which the sample surface has a temperature gradient, or the two heat sources jointly maintain the substrate surface temperature gradient as a fixed value to control the growth thickness of the film on the substrate, or the two heat sources jointly implement a post-annealing process in which the sample surface has a temperature gradient.
The purpose of pre-annealing the substrate is to eliminate and improve the tissue defects and internal stress left by the previous heat treatment process, and simultaneously form reconstruction types required by the growth of different types of single crystal films, and the temperature gradient of the substrate surface can realize the reconstruction types of the substrate surface along with the temperature change. Then, different film materials can be obtained at different positions on the surface of the substrate through film growth.
The post annealing after the film sample grows on the surface of the substrate is to improve the crystallinity of the film and supplement the oxygen content to the film in time, and the film component which is compact and has continuous change can be obtained after the post annealing.
The heating stage and the auxiliary heating device can be one of the following devices, including: laser heating, resistance heating, electron beam heating, infrared heating.
The evaporation source includes a resistance heating type thermal evaporation source, an electron gun heating evaporation source, or electron beam heating.
The heating position of the auxiliary heating device can be any position of the substrate or the sample holder, and the heating positions shown in fig. 2 and 3 are only one of the preferred embodiments.
And step S4: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
SrTiO of rectangle 5 x 2.5mm below 3 (100) The substrate is illustrated as an example. The substrate is fixed on a molybdenum sample support with steps by platinum glue, the heating table is heated by resistance wires, the auxiliary heating equipment adopts infrared laser, and the laser heating position is positioned at the edge of the short side of the rectangle, as shown in figure 3.
Example 1
The embodiment comprises pretreatment, sample growth and post-treatment, and auxiliary heating equipment is adopted in the pretreatment.
Step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample with the substrate fixed is held in a holder of less than 1X 10 -9 In an ultra-vacuum environment of mbar, uniformly heating the sample holder by using a heating table, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 400-700 ℃, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: pre-treating;
further heating the substrate after removing impurities at high temperature by using a heating table, measuring the temperature of the surface of a sample by using an infrared thermometer to obtain the surface temperature of the substrate of 800-1100 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the surface temperature of the sample is stable, so that the surface of the sample has a temperature gradient of more than 100 ℃, the surface temperature of the substrate ranges from 850 ℃ to 1250 ℃, the temperature is gradually reduced from a laser heating point to the outside, two heat sources are maintained for a period of time together, and the two heating modes jointly realize a pre-annealing process that the surface of the sample has the temperature gradient;
and step S4: growing a sample;
reducing the heating temperature of the sample stage by the substrate subjected to temperature gradient pre-annealing, and turning off the infrared auxiliary heating to ensure that the surface temperature of the substrate obtained by using an infrared thermometer ranges from 700 ℃ to 850 ℃, namely, the surface temperature of the substrate is adjusted to the film growth temperature; after the temperature is stable, an evaporation source is adopted, the beam current of the evaporation source is measured by using a crystal oscillator, and the thickness of the film evaporated on the surface of the substrate is obtained by calculating the evaporation time; controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
step S5: post-treatment;
after the growth of the film on the surface of the substrate is finished, adjusting the heating temperature of the sample stage, and utilizing the temperature of the surface of the substrate obtained by the infrared thermometer to enable the temperature range of the surface of the substrate to be 700-850 ℃, namely achieving the post-annealing temperature range of the growth of the film sample, and maintaining the temperature for a certain time to realize the post-annealing process of the surface of the substrate;
step S6: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
The substrate surface obtained through the step S3 has different reconstructions, and different film materials can be obtained at different positions of the substrate surface through the film growth in the step S4.
Example 2
The embodiment comprises pretreatment, sample growth and post-treatment, and auxiliary heating equipment is adopted in the sample growth stage.
Step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 In an ultra-vacuum environment of mbar, uniformly heating the sample holder by using a heating table, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 400-700 ℃, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: pre-treating;
further heating the substrate after removing impurities at high temperature by using a heating table, measuring the temperature of the surface of a sample by using an infrared thermometer to obtain the surface temperature of the substrate of 800-1100 ℃, and maintaining for 0.5-8 hours to realize pre-annealing of the film;
and step S4: growing a sample;
reducing the heating temperature of the sample stage by the substrate subjected to pre-annealing to ensure that the surface temperature range of the substrate obtained by an infrared thermometer is 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the temperature is stable to ensure that the surface of the sample has a fixed temperature gradient of more than 100 ℃, ensuring that the surface temperature range of the substrate is 850-1100 ℃, and gradually reducing the temperature from a laser heating point outwards, wherein the two heating modes jointly realize the film growth temperature of the surface of the sample with the temperature gradient;
after the temperature is stable, an evaporation source is adopted, the beam current of the evaporation source is measured by using a crystal oscillator, and the thickness of the film evaporated on the surface of the substrate is obtained by calculating the evaporation time; controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
step S5: post-treatment;
after the growth of the film on the surface of the substrate is finished, adjusting the heating temperature of the sample stage, and utilizing the substrate surface temperature obtained by an infrared thermometer to enable the substrate surface temperature range to be 700-850 ℃, namely achieving the post-annealing temperature range of the film sample growth, and maintaining the temperature for a certain time to realize the post-annealing process of the substrate surface;
step S6: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
Example 3
The embodiment comprises pretreatment, sample growth and post-treatment, and auxiliary heating equipment is adopted in the post-treatment.
Step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 In an ultra-vacuum environment of mbar, uniformly heating the sample holder by using a heating table, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 400-700 ℃, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: pre-treating;
further heating the substrate after removing impurities at high temperature by using a heating table, measuring the temperature of the surface of a sample by using an infrared thermometer to obtain the surface temperature of the substrate of 800-1100 ℃, and maintaining for 0.5-8 hours to realize pre-annealing of the film;
and step S4: growing a sample;
reducing the heating temperature of the sample stage of the substrate subjected to pre-annealing, and turning off the infrared auxiliary heating to ensure that the surface temperature of the substrate obtained by using an infrared thermometer ranges from 700 ℃ to 850 ℃, namely, the surface temperature of the substrate is adjusted to the growth temperature of the film; after the temperature is stable, an evaporation source is adopted, the beam current of the evaporation source is measured by using a crystal oscillator, and the thickness of the film evaporated on the surface of the substrate is obtained by calculating the evaporation time; controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
step S5: post-treatment;
after the growth of the film on the surface of the substrate is finished, adjusting the heating temperature of the sample stage, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the surface temperature of the sample is stable, so that the surface of the sample has a temperature gradient of more than 100 ℃, the surface temperature of the substrate ranges from 800 ℃ to 1000 ℃, the temperature is gradually reduced outwards from a laser heating point, and the two heating modes jointly realize the post annealing process that the surface of the sample has the temperature gradient;
step S6: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
Example 4
The embodiment comprises pretreatment, sample growth and post-treatment, and auxiliary heating equipment is adopted in the pretreatment and the sample growth stages.
Step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 In an ultra-vacuum environment of mbar, uniformly heating the sample holder by using a heating table, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 400-700 ℃, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: pretreatment;
further heating the substrate after removing impurities at high temperature by using a heating table, measuring the temperature of the surface of a sample by using an infrared thermometer to obtain the surface temperature of the substrate of 800-1100 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the surface temperature of the sample is stable, so that the surface of the sample has a temperature gradient of more than 100 ℃, the surface temperature of the substrate ranges from 850 ℃ to 1250 ℃, the temperature is gradually reduced from a laser heating point to the outside, two heat sources are maintained for a period of time together, and the two heating modes jointly realize a pre-annealing process that the surface of the sample has the temperature gradient;
and step S4: growing a sample;
reducing the heating temperature of the sample stage by the substrate annealed before the temperature gradient, so that the surface temperature range of the substrate obtained by using an infrared thermometer is 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the temperature is stable, so that the surface of the sample has a fixed temperature gradient of more than 100 ℃, the surface temperature range of the substrate is 850-1100 ℃, the temperature is gradually reduced from a laser heating point outwards, and the two heating modes jointly realize the film growth temperature of the surface of the sample with the temperature gradient;
after the temperature is stable, an evaporation source is adopted, the beam current of the evaporation source is measured by using a crystal oscillator, and the thickness of the film evaporated on the surface of the substrate is obtained by calculating the evaporation time; controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
step S5: post-treatment;
after the growth of the film on the surface of the substrate is finished, adjusting the heating temperature of the sample stage, and utilizing the temperature of the surface of the substrate obtained by the infrared thermometer to enable the temperature range of the surface of the substrate to be 700-850 ℃, namely achieving the post-annealing temperature range of the growth of the film sample, and maintaining the temperature for a certain time to realize the post-annealing process of the surface of the substrate;
step S6: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
Example 5
The embodiment comprises pretreatment, sample growth and post-treatment, and auxiliary heating equipment is adopted in the sample growth stage and the post-treatment.
Step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 In an ultra-vacuum environment of mbar, uniformly heating the sample holder by using a heating table, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 400-700 ℃, and heating the substrate to remove impurities on the surface of the substrate;
and step S4: growing a sample;
reducing the heating temperature of the sample stage by the substrate subjected to pre-annealing to ensure that the surface temperature range of the substrate obtained by an infrared thermometer is 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the temperature is stable to ensure that the surface of the sample has a fixed temperature gradient of more than 100 ℃, ensuring that the surface temperature range of the substrate is 850-1100 ℃, and gradually reducing the temperature from a laser heating point outwards, wherein the two heating modes jointly realize the film growth temperature of the surface of the sample with the temperature gradient;
after the temperature is stable, an evaporation source is adopted, the beam current of the evaporation source is measured by using a crystal oscillator, and the thickness of the film evaporated on the surface of the substrate is obtained by calculating the evaporation time; controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
step S5: post-treatment;
after the growth of the film on the surface of the substrate is finished, adjusting the heating temperature of the sample stage, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the surface temperature of the sample is stable, so that the surface of the sample has a temperature gradient of more than 100 ℃, the surface temperature of the substrate ranges from 800 ℃ to 1000 ℃, the temperature is gradually reduced outwards from a laser heating point, and the two heating modes jointly realize the post annealing process that the surface of the sample has the temperature gradient;
step S6: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
Example 6
The embodiment comprises pretreatment, sample growth and post-treatment, and auxiliary heating equipment is adopted in the sample growth stage and the post-treatment.
Step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 In an ultra-vacuum environment of mbar, uniformly heating the sample holder by using a heating table, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 400-700 ℃, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: pretreatment;
further heating the substrate after removing impurities at high temperature by using a heating table, measuring the temperature of the surface of a sample by using an infrared thermometer to obtain the surface temperature of the substrate of 800-1100 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the surface temperature of the sample is stable, so that the surface of the sample has a temperature gradient of more than 100 ℃, the surface temperature of the substrate ranges from 850 ℃ to 1250 ℃, the temperature is gradually reduced from a laser heating point to the outside, two heat sources are maintained for a period of time together, and the two heating modes jointly realize a pre-annealing process that the surface of the sample has the temperature gradient;
and step S4: growing a sample;
reducing the heating temperature of the sample stage by the substrate annealed before the temperature gradient, so that the temperature range of the surface of the substrate obtained by using an infrared thermometer is 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the temperature is stable, so that the surface of the sample has a fixed temperature gradient of more than 100 ℃, the temperature range of the surface of the substrate is 850-1100 ℃, the temperature is gradually reduced from a laser heating point outwards, and the two heating modes jointly realize the film growth temperature of the surface of the sample with the temperature gradient;
after the temperature is stable, an evaporation source is adopted, the beam current of the evaporation source is measured by using a crystal oscillator, and the thickness of the film evaporated on the surface of the substrate is obtained by calculating the evaporation time; controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
step S5: post-treatment;
after the growth of the film on the surface of the substrate is finished, adjusting the heating temperature of the sample stage, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the surface temperature of the sample is stable, so that the surface of the sample has a temperature gradient of more than 100 ℃, the surface temperature of the substrate ranges from 800 ℃ to 1000 ℃, the temperature is gradually reduced outwards from a laser heating point, and the two heating modes jointly realize the post annealing process that the surface of the sample has the temperature gradient;
step S6: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
Example 7
This embodiment includes pre-treatment and sample growth, and employs auxiliary heating equipment in both the pre-treatment and sample growth stages.
Step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 In an ultra-vacuum environment of mbar, uniformly heating the sample holder by using a heating table, measuring the temperature of the sample surface by using an infrared thermometer to obtain the surface temperature of the substrate of 400-700 ℃, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: pretreatment;
further heating the substrate after removing impurities at high temperature by using a heating table, measuring the temperature of the surface of a sample by using an infrared thermometer to obtain the surface temperature of the substrate of 800-1100 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the surface temperature of the sample is stable, so that the surface of the sample has a temperature gradient of more than 100 ℃, the surface temperature of the substrate ranges from 850 ℃ to 1250 ℃, the temperature is gradually reduced from a laser heating point to the outside, two heat sources are maintained for a period of time together, and the two heating modes jointly realize a pre-annealing process that the surface of the sample has the temperature gradient;
and step S4: growing a sample;
reducing the heating temperature of the sample stage by the substrate subjected to pre-annealing to ensure that the surface temperature range of the substrate obtained by an infrared thermometer is 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the temperature is stable to ensure that the surface of the sample has a fixed temperature gradient of more than 100 ℃, ensuring that the surface temperature range of the substrate is 850-1100 ℃, and gradually reducing the temperature from a laser heating point outwards, wherein the two heating modes jointly realize the film growth temperature of the surface of the sample with the temperature gradient;
after the temperature is stable, an evaporation source is adopted, the beam current of the evaporation source is measured by using a crystal oscillator, and the thickness of the film evaporated on the surface of the substrate is obtained by calculating the evaporation time; controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
step S5: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
Example 8
This embodiment includes sample growth and post-processing, and auxiliary heating devices are employed in both sample growth and post-processing.
Step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 In an ultra-vacuum environment of mbar, uniformly heating the sample holder by using a heating table, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 400-700 ℃, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: growing a sample;
reducing the heating temperature of the sample stage by the substrate subjected to pre-annealing to ensure that the surface temperature range of the substrate obtained by an infrared thermometer is 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the temperature is stable to ensure that the surface of the sample has a fixed temperature gradient of more than 100 ℃, ensuring that the surface temperature range of the substrate is 850-1100 ℃, and gradually reducing the temperature from a laser heating point outwards, wherein the two heating modes jointly realize the film growth temperature of the surface of the sample with the temperature gradient;
after the temperature is stable, an evaporation source is adopted, the beam current of the evaporation source is measured by using a crystal oscillator, and the thickness of the film evaporated on the surface of the substrate is obtained by calculating the evaporation time; controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
and step S4: post-treatment;
after the growth of the film on the surface of the substrate is finished, adjusting the heating temperature of the sample stage, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 700-850 ℃, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate after the surface temperature of the sample is stable, so that the surface of the sample has a temperature gradient of more than 100 ℃, the surface temperature of the substrate ranges from 800 ℃ to 1000 ℃, the temperature is gradually reduced outwards from a laser heating point, and the two heating modes jointly realize the post annealing process that the surface of the sample has the temperature gradient;
step S5: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
Example 9
This embodiment includes only the sample growth stage, and an auxiliary heating device is employed during the sample growth stage.
Step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 In an ultra-vacuum environment of mbar, uniformly heating the sample holder by using a heating table, measuring the temperature of the surface of the sample by using an infrared thermometer to obtain the surface temperature of the substrate of 400-700 ℃, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: growing a sample;
further heating the substrate by using a heating table, wherein the temperature range of the surface of the substrate obtained by using an infrared thermometer is 700-850 ℃, after the temperature is stabilized, introducing infrared laser auxiliary heating equipment to heat the edge of the surface of the substrate, so that the surface of the sample has a fixed temperature gradient higher than 100 ℃, the temperature range of the surface of the substrate is 850-1100 ℃, the temperature is gradually reduced from a laser heating point outwards, and the two heating modes jointly realize the film growth temperature of the surface of the sample with the temperature gradient;
after the temperature is stable, an evaporation source is adopted, the beam current of the evaporation source is measured by using a crystal oscillator, and the thickness of the film evaporation on the surface of the substrate is obtained by calculating the evaporation time; controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
step S6: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
The above examples of the method of the present invention for implementing temperature gradient to realize high-throughput thin film growth are intended to further illustrate the design concept and embodiments of the present invention, but the present invention is not limited to all kinds of thin film samples for molecular beam epitaxial growth. The method is also applicable to other devices for growing the film sample, such as laser deposition technology and the like.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and although the invention has been described in detail with reference to the foregoing examples, it will be apparent to those skilled in the art that various changes in the form and details of the embodiments may be made and equivalents may be substituted for elements thereof. All modifications, equivalents and the like which come within the spirit and principle of the invention are intended to be included within the scope of the invention.
Claims (7)
1. A method for realizing high flux film growth by adopting temperature gradient is characterized in that on the basis of a heat source capable of uniformly heating a substrate, another auxiliary heat source is introduced, the auxiliary heat source is adopted to heat and fix a sample holder of the substrate and any position of the substrate to form a local high temperature point, so that the temperature gradient is generated on the surface of the substrate, and the high flux single crystal film with the same elements and different chemical components is grown on the surface of the substrate;
the method comprises the following steps:
step S1: fixing a substrate with an atomic-scale step surface on a sample holder;
step S2: the sample holder with the substrate fixed is placed at less than 1 x 10 -9 Uniformly heating the sample holder by adopting a heat source in an ultra-vacuum environment of mbar, and heating the substrate to remove impurities on the surface of the substrate;
and step S3: adjusting the substrate temperature obtained in the step S2 to the film growth temperature, heating the substrate surface by adopting an auxiliary heat source after the temperature is stable, maintaining the temperature gradient of the substrate surface as a fixed value together, and then controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
and step S4: and cooling the substrate to obtain the high-flux single crystal film with the same elements and different chemical components growing on the surface of the substrate.
2. The method for realizing the growth of the high-flux thin film by adopting the temperature gradient as claimed in claim 1, wherein when the growth of the single crystal thin film needs pretreatment, the S3 is replaced by:
controlling the temperature of the substrate obtained in the step S2 within a pre-annealing temperature range of film growth, heating any position of the surface of the substrate by adopting an auxiliary heat source to realize that the temperature difference of different positions of the surface of the substrate is more than or equal to 50 ℃, and maintaining the two heat sources together for a period of time to realize a pre-annealing process with a temperature gradient on the surface of the substrate;
and adjusting the surface temperature of the substrate to the film growth temperature, adopting an evaporation source after the temperature is stable, and controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source.
3. The method for realizing high-flux film growth by using temperature gradient according to claim 1, wherein when the growth of the single crystal film requires post-treatment, the S3 is replaced by:
adjusting the surface temperature of the substrate to the film growth temperature, adopting an evaporation source after the temperature is stable, and controlling the growth thickness of the film on the substrate by regulating and controlling the growth beam current and the growth time of the evaporation source;
the temperature of the substrate with the film is controlled within the post-annealing temperature range of the growth of different film samples, then an auxiliary heat source is adopted to heat the surface of the substrate or any position of a sample holder, the temperature difference of different positions of the surface of the substrate is more than or equal to 50 ℃, and the two heat sources are jointly maintained for a period of time, so that the post-annealing process of the surface temperature gradient of the sample is realized.
4. The method for realizing the growth of the high-flux film by adopting the temperature gradient as claimed in claim 2, wherein when the growth of the single crystal film requires pretreatment and post-treatment at the same time, after the growth thickness of the film on the substrate is controlled, the temperature of the substrate on which the film is grown is controlled within a post-annealing temperature range for the growth of different film samples, then an auxiliary heat source is adopted to heat the surface of the substrate or any position of a sample holder, the temperature difference of different positions of the surface of the substrate is more than or equal to 50 ℃, and the two heat sources are maintained for a period of time together, so that the post-annealing process of the temperature gradient of the surface of the sample is realized.
5. The method for realizing the growth of the high-flux thin film by using the temperature gradient as claimed in claim 1, wherein the substrate with the atomic-scale step surface is fixed on the sample holder by using a mechanical method or a glue fixing method.
6. The method for growing a thin film with high flux using temperature gradient according to claim 1, wherein the evaporation source is selected from any one of a resistance heating type thermal evaporation source, an electron gun heating evaporation source, and an electron beam heating.
7. The method for growing a thin film with high flux according to claim 1, wherein the auxiliary heat source is selected from any one of laser heating, resistance heating, electron beam heating and infrared heating.
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