CN110777436A - Silicon-based group IV alloy material and epitaxial method thereof - Google Patents
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Abstract
A silicon-based IV-group alloy material and an epitaxial method thereof are disclosed, wherein the epitaxial method comprises the following steps: step 1: delivering the substrate into a high-vacuum growth chamber for dehydrogenation and deoxidation treatment; step 2: adjusting the temperature of the substrate; and step 3: and co-depositing at least Ge, Sn and Pb atoms on the substrate to complete the material epitaxy. The germanium tin lead alloy material can realize direct band gap and is compatible with a silicon-based CMOS (complementary metal oxide semiconductor) process; the prepared germanium tin lead alloy material has good crystal quality, and has narrower band gap compared with the germanium tin or germanium lead material with the same component; provides a novel material for manufacturing silicon-based luminescent and detecting devices, and is expected to play an important role in the field of silicon-based photoelectronics.
Description
Technical Field
The invention belongs to the technical field of silicon-based photoelectric materials, and mainly relates to a silicon-based IV-group alloy material and an epitaxial method thereof.
Background
The realization of silicon-based photoelectric integration is an important means for solving the problems of power consumption, time delay, I/O and the like of the traditional electric interconnection. The direct band gap semiconductor material compatible with silicon is searched, and the silicon-based high-efficiency light source is realized, so that the direct band gap semiconductor material has great significance and application value. At present, the photoelectric materials which can realize silicon-based compatibility are mainly group IV materials, and germanium tin and germanium lead alloys can realize direct band gap conversion by adjusting the components of Sn and Pb.
Studies have shown that germanium tin requires more than 8% of the Sn component for conversion to the direct bandgap, while germanium lead requires about 3.4% Pb. In the epitaxy of germanium tin and germanium lead, the following difficulties need to be overcome: 1) sn or Pb has larger lattice mismatch with Ge; 2) lower equilibrium solid solubility of Sn or Pb in Ge; 3) sn or Pb has lower surface free energy and is easy to form surface segregation and segregation phenomena. Therefore, it is difficult to extend high-composition and high-quality germanium tin and germanium lead alloys, and the requirement for manufacturing high-efficiency silicon-based light-emitting devices cannot be met.
Disclosure of Invention
It is therefore an objective of the claimed invention to provide a silicon-based group IV alloy material and an epitaxy method thereof, which are aimed at least partially solving at least one of the above-mentioned problems.
In order to achieve the above object, the present invention provides a method for epitaxy of silicon-based group IV alloy material, comprising the steps of:
step 1: delivering the substrate into a high-vacuum growth chamber for dehydrogenation and deoxidation treatment;
step 2: adjusting the temperature of the substrate;
and step 3: and co-depositing at least Ge, Sn and Pb atoms on the substrate to complete the material epitaxy.
Wherein, step 1 also includes the step of washing before;
and the final step of the cleaning step is to carry out surface treatment by using diluted hydrofluoric acid to realize surface hydrogen passivation.
Wherein, the temperature of the dehydrogenation and deoxidation in the step 1 is between 500 and 1100 ℃, and the time is 5 to 25 min.
Wherein the substrate temperature in the step 2 is 120-350 ℃.
And 2, the substrate in the step 2 is a silicon substrate, a germanium substrate or a germanium dummy substrate on silicon.
Wherein the substrate crystal orientation in step 2 is (100), (110) or (111).
In step 3, Ge, Sn and Pb atoms are co-deposited on the substrate by adopting a physical vapor deposition or chemical vapor deposition method.
A silicon-based group IV alloy material prepared according to the epitaxial method as described above.
The purpose of adjusting the band gap is achieved by regulating and controlling the components of Ge, Sn and Pb atoms which are co-deposited on the substrate in the step 4, and the adjustment range of the band gap is 0-0.66 eV.
Wherein the silicon-based group IV alloy material is a direct bandgap material.
Based on the technical scheme, compared with the prior art, the silicon-based IV-group alloy material and the epitaxial method thereof have at least one of the following beneficial effects:
(1) the germanium tin lead alloy material can realize direct band gap and is compatible with a silicon-based CMOS (complementary metal oxide semiconductor) process;
(2) the prepared germanium tin lead alloy material has good crystal quality, and has narrower band gap compared with the germanium tin or germanium lead material with the same component;
(3) provides a novel material for manufacturing silicon-based luminescent and detecting devices, and is expected to play an important role in the field of silicon-based photoelectronics.
Drawings
FIG. 1 is a schematic diagram of the band transition of germanium tin lead in the present invention;
FIG. 2 shows Rutherford Backscattering (RBS) random spectra of a Ge-Sn-Pb single crystal film with certain epitaxial composition in example 1 of the present invention;
FIG. 3 is an Atomic Force Microscope (AFM) view of a single crystal thin film of germanium tin lead with certain epitaxy composition in example 1 of the present invention;
FIG. 4 is an X-ray diffraction (XRD) pattern of a germanium tin lead single crystal film of certain epitaxial composition in example 1 of the present invention;
fig. 5 is an X-ray diffraction (XRD) pattern of a ge-sn-pb single crystal film of certain epitaxial composition in example 2 of the present invention.
Detailed Description
The main principle that germanium tin or germanium lead alloy can realize direct band gap conversion is as follows: after Sn or Pb element is introduced into Ge, the descending speed of gamma energy valley (direct band gap) is larger than that of L energy valley (indirect band gap). In view of the same mechanism that germanium tin and germanium lead alloy are converted into direct band gaps, Sn and Pb elements can be simultaneously introduced into Ge, theoretically, Sn and Pb can be simultaneously dissolved in crystal lattices of Ge through a non-equilibrium epitaxial means, a direct band gap material can be formed through the combined action of Sn and Pb atoms, and the formed novel germanium tin lead alloy is expected to become a new generation of silicon-based compatible photoelectric material.
The invention discloses a novel silicon-based IV-group alloy material and a preparation method thereof, wherein the material is germanium tin lead (Ge)
1-x- ySn
xPb
y) The alloy material can realize direct band gap and has the characteristic of silicon-based compatibility. The epitaxial method comprises the following steps: step 1), taking a substrate, cleaning and reserving for later use; step 2) rapidly conveying the substrate into a high-vacuum growth chamber, and then carrying out dehydrogenation and deoxidation treatment; step 3) adjusting the temperature of the substrate; and 4) depositing Ge, Sn and Pb atoms on the substrate together to finish the epitaxial preparation of the material. The germanium tin lead alloy material provided by the invention has great application prospects in the aspects of manufacturing silicon-based light sources, detection devices and the like.
Specifically, the invention provides an epitaxial method of a silicon-based IV-group alloy material, which comprises the following steps:
step 1: delivering the substrate into a high-vacuum growth chamber for dehydrogenation and deoxidation treatment;
step 2: adjusting the temperature of the substrate;
and step 3: and co-depositing at least Ge, Sn and Pb atoms on the substrate to complete the material epitaxy.
Wherein, step 1 also includes the step of washing before;
and the final step of the cleaning step is to carry out surface treatment by using diluted hydrofluoric acid to realize surface hydrogen passivation.
Wherein, the temperature of the dehydrogenation and deoxidation in the step 1 is between 500 and 1100 ℃, and the time is 5 to 25 min.
Wherein the substrate temperature in the step 2 is 120-350 ℃.
And 2, the substrate in the step 2 is a silicon substrate, a germanium substrate or a germanium dummy substrate on silicon.
Wherein the substrate crystal orientation in step 2 is (100), (110) or (111).
In step 3, Ge, Sn and Pb atoms are co-deposited on the substrate by adopting a physical vapor deposition or chemical vapor deposition method.
A silicon-based group IV alloy material prepared according to the epitaxial method as described above.
The purpose of adjusting the band gap is achieved by regulating and controlling the components of Ge, Sn and Pb atoms which are co-deposited on the substrate in the step 4, and the adjustment range of the band gap is 0-0.66 eV.
Wherein the silicon-based group IV alloy material is a direct bandgap material.
In order that the objects, technical solutions and advantages of the present invention will become more apparent, the present invention will be further described in detail with reference to the accompanying drawings in conjunction with the following specific embodiments.
Referring to fig. 1, the present invention provides a novel silicon-based group IV alloy material, named germanium-tin-lead alloy, which can realize direct band gap, is compatible with silicon-based CMOS process, and is expected to play an important role in the field of silicon-based photoelectrons. The principle of achieving a direct bandgap is as follows:
sn and Pb atoms are introduced into Ge, so that the descending speed of a gamma energy valley (direct band gap) is higher than that of an L energy valley (indirect band gap), and the material becomes a direct band gap material.
The invention also provides an epitaxial method of the germanium tin lead alloy material, which comprises the following steps:
step 1: and taking the substrate and cleaning the substrate. The substrate cleaning is carried out by sequentially carrying out ultrasonic cleaning by using acetone, alcohol and deionized water, and finally carrying out surface treatment by using diluted HF (hydrogen fluoride), so that after germanium oxide on the surface is removed, a germanium dangling bond on the surface is bonded with hydrogen, and the surface hydrogen passivation is realized.
Step 2: and (3) rapidly conveying the substrate into a high-vacuum growth chamber, and then carrying out dehydrogenation and deoxidation treatment, wherein the temperature during dehydrogenation and deoxidation is 500-1000 ℃ and the time is 5-25 min. The sample transfer process is fast and uses higher temperatures due to the limited ability of hydrogen passivation to prevent oxidation of the substrate. The purpose of dehydrogenation and deoxidation is to expose a clean substrate surface, which is beneficial to the epitaxial growth of high-quality germanium-tin-lead alloy.
And step 3: the temperature of the substrate is adjusted to be about 120-350 ℃. The substrate temperature is not too high or too low, and the material surface segregation is easily caused by too high temperature; too low will not provide enough kinetic energy to render the epitaxial material amorphous.
And 4, step 4: and (4) co-depositing Ge, Sn and Pb atoms on the substrate to complete material epitaxy. The epitaxial method can adopt molecular beam epitaxy, magnetron sputtering, electron beam evaporation or chemical vapor deposition.
Example 1
The invention provides an epitaxial method of a GeSnPb alloy material, which comprises the following steps:
step 1: a silicon germanium dummy substrate is taken and cleaned, the crystal face of the dummy substrate is (100), and the dummy substrate is prepared by a molecular beam epitaxy method. And ultrasonically cleaning the germanium virtual substrate by acetone, alcohol and deionized water for 10min respectively, finally soaking the germanium virtual substrate by 10% HF for 30s, then immersing and washing the germanium virtual substrate by deionized water for 6min, and after removing germanium oxide on the surface, realizing surface hydrogen passivation.
Step 2: and blowing the germanium virtual substrate by using a nitrogen gun, quickly conveying the germanium virtual substrate into a high-vacuum growth chamber, and carrying out dehydrogenation and deoxidation treatment at the temperature of 800 ℃ for 25 min.
And step 3: the substrate temperature was adjusted to 135 ℃.
And 4, step 4: ge, Sn and Pb atoms are co-deposited on the substrate by a magnetron sputtering method, and the deposition thickness is 60nm (refer to figures 2-4).
The Rutherford Backscattering (RBS) random spectrum of fig. 2 shows that Sn, Pb atoms have successfully incorporated into the lattice of Ge and GeSnPb alloys have been successfully epitaxial. The Atomic Force Microscopy (AFM) image of fig. 3 shows that the epitaxial GeSnPb alloy has a flat surface morphology with no surface segregation of Sn or Pb. The X-ray diffraction (XRD) pattern of fig. 4 indicates that the GeSnPb alloy crystal is of good quality, with Sn and Pb atoms occupying substitutional tetrahedral lattice sites.
Example 2
The preparation method is the same as that of example 1, and only differs in that the sputtering external time delay is adopted, so that the sputtering power of the Sn target and the Pb target is increased, and the ratio of Sn atoms to Pb atoms in the GeSnPb alloy is increased (see figure 5).
The X-ray diffraction (XRD) pattern of fig. 5 shows that the prepared GeSnPb alloy has good crystal quality and a higher ratio of Sn and Pb atoms in the GeSnPb alloy and a larger lattice constant than in example 1.
The above-mentioned embodiments are intended to illustrate the objects, technical solutions and advantages of the present invention in further detail, and it should be understood that the above-mentioned embodiments are only exemplary embodiments of the present invention and are not intended to limit the present invention, and any modifications, equivalents, improvements and the like made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. A method for epitaxy of silicon-based group IV alloy materials, comprising the steps of:
step 1: delivering the substrate into a high-vacuum growth chamber for dehydrogenation and deoxidation treatment;
step 2: adjusting the temperature of the substrate;
and step 3: and co-depositing at least Ge, Sn and Pb atoms on the substrate to complete the material epitaxy.
2. Epitaxy method according to claim 1, characterised in that step 1 is preceded by a step of washing;
and the final step of the cleaning step is to carry out surface treatment by using diluted hydrofluoric acid to realize surface hydrogen passivation.
3. Epitaxial method according to claim 1, characterized in that the temperature of the dehydrodeoxygenation in step 1 is between 500 ℃ and 1100 ℃ for a time comprised between 5 and 25 min.
4. Epitaxial method according to claim 2, characterized in that the substrate temperature in step 2 is between 120 ℃ and 350 ℃.
5. The epitaxy method according to claim 1, characterised in that in step 2 the substrate is a silicon substrate, a germanium substrate or a germanium dummy substrate on silicon.
6. The epitaxy method according to claim 1, characterised in that the substrate crystal orientation in step 2 is (100), (110) or (111).
7. Epitaxy method according to claim 1, characterised in that in step 3, the Ge, Sn, Pb atoms are co-deposited on the substrate by physical vapour deposition or chemical vapour deposition.
8. A silicon-based group IV alloy material prepared by the epitaxial method of any one of claims 1 to 7.
9. The silicon-based group IV alloy material according to claim 8, wherein the band gap is adjusted in the range of 0-0.66eV by adjusting the composition of Ge, Sn, Pb atoms co-deposited on the substrate in step 4.
10. The silicon-based group IV alloy material of claim 8, wherein the silicon-based group IV alloy material is a direct bandgap material.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111312807A (en) * | 2020-03-05 | 2020-06-19 | 中国科学院半导体研究所 | Silicon-based IV group alloy strip and preparation method thereof |
| CN113113512A (en) * | 2021-04-15 | 2021-07-13 | 中国科学院半导体研究所 | Directional heteroepitaxy method and silicon-based germanium-tin alloy material |
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| CN111312807A (en) * | 2020-03-05 | 2020-06-19 | 中国科学院半导体研究所 | Silicon-based IV group alloy strip and preparation method thereof |
| CN111312807B (en) * | 2020-03-05 | 2021-10-15 | 中国科学院半导体研究所 | Silicon-based IV group alloy strip and preparation method thereof |
| CN113113512A (en) * | 2021-04-15 | 2021-07-13 | 中国科学院半导体研究所 | Directional heteroepitaxy method and silicon-based germanium-tin alloy material |
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Application publication date: 20200211 |