CN105529242B - A kind of method for preparing bead string shape monocrystalline silicon nano line - Google Patents
A kind of method for preparing bead string shape monocrystalline silicon nano line Download PDFInfo
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- CN105529242B CN105529242B CN201510504801.6A CN201510504801A CN105529242B CN 105529242 B CN105529242 B CN 105529242B CN 201510504801 A CN201510504801 A CN 201510504801A CN 105529242 B CN105529242 B CN 105529242B
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- H—ELECTRICITY
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- H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
- H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
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- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y40/00—Manufacture or treatment of nanostructures
Abstract
The invention discloses a kind of method for preparing plane bead string shape monocrystalline silicon nano line, 1) on smooth substrate, In, Sn or Bi inducing metal film, the as initial position of nanowire growth is deposited in localization region；2) above-mentioned substrate is put into PECVD system intracavitary, in 500 DEG C of temperature 200 DEG C, hydrogen gas plasma handled sample after 5 30 minutes, metal film various sizes of quasi- nano-catalytic metallic particles between forming a large amount of tens nanometers Dao several microns；3) amorphous silicon layer of one layer of suitable thickness (several nanometers to hundreds of nanometers) in a pecvd system, is covered as presoma dielectric layer；4) anneal in a vacuum or in the non-oxidizing atmosphere such as hydrogen, nitrogen, catalyticing metal particle can be activated, spontaneous absorption non-crystalline silicon, separate out monocrystalline silicon, while diameter generating period changes, and grows bead string shape nano wire.
Description
First, technical field
The invention mainly relates to field of semiconductor devices, particularly single electron quantum device preparation and application field.
2nd, technical background
Semiconductor nano cable architecture is due to its unique optics and electrical properties, in electronic device, photodetection, biology doctor
, sensor etc. have boundless application prospect.Silicon materials be it is most crucial in current semi-conducting material, it is most widely used
Material.In past over half a century, every generation huge advance of microelectronics is carried out around silicon materials.By several
Improve and include many new materials within 10 years, the core technology platform of traditional counting is still based on silicon.Meanwhile with research
Deeply, it is increasingly apparent to firmly believe that what silicon prepare all new generation as a kind of outstanding host material has quantum charge and spin
The device of characteristic.This is included from quantum computer to extensive spintronics application.Silicon materials are due to its weak spin-orbit coupling
Conjunction and the presence of isotope and zero nuclear spin are the ecotopias of spinning electron.Quantum device based on silicon is in Quantum Spin
By with huge application prospect on the basis of the control manufacturing technology consummate with reference to classic computer is had been provided with.
The microelectronics and semiconductor technology of existing industrialization be take developed over half a century it is highly developed from upper and
Under (Top-down) technology, i.e., using fine machining methods such as chemical wet etchings, big material is cut small, forms structure or device,
And integrated with circuit, realize that system is miniaturized.And nanometer and quantum device epoch have been arrived, yardstick is up to hundred nanometers and even several received
Rice, caused technology and Cost Problems are by highly significant therewith.And Bottom-up technologies, it is that molecule, atom package technique are done
Method, i.e., the functional molecular with specific physicochemical property, atom, by molecule, intraatomic active force, subtly form nanometer
Molecular line, film and the other structures of yardstick, then micro-system is integrated into by nanostructured and functional unit.This manufacturing technology reflection
A kind of theory of nanometer technology, i.e., from the level of atom and molecule design, assembled material, device and system, be it is a kind of very
Promising manufacturing technology.
VLS (gas-liquid-solid) growth mechanism is the ripe growth mechanism that nano wire is prepared based on Bottom-up technologies.
The general requirement of VLS growth mechanisms must have the presence of catalyst, and growth material is primarily vaporized into gaseous state, in suitable temperature
Under, catalyst can mutually melt the eutectic for forming liquid with the constituent element of growth material, and the constituent element of growth material constantly obtains from gas phase
, after molten matter constituent element reaches supersaturation in liquid, whisker will separate out along the preferential direction of solid-liquid interface one, grow up to wire crystalline substance
Body.Obviously the size of catalyst grows largely control the size of whisker.Experiment proves this growth mechanism
It can be used for preparing the even more complicated monocrystalline of substantial amounts of simple substance, binary compound, and the monocrystalline of this method growth is substantially
Dislocation-free, the speed of growth are fast.By controlling the size of catalyst to prepare substantial amounts of quasi-one-dimensional nanometer material.
3rd, the content of the invention
In view of the above-mentioned problems, it is an object of the invention to provide a kind of method for preparing high quality bead string shape silicon nanowires.
The technical scheme is that：A kind of method for preparing bead string shape monocrystalline silicon nano line, using self-positioning growth and collection
Into the method for planar semiconductor nano wire, step is as follows, and 1) on smooth substrate, coordinate photoetching or other pattern generation technologies
Etc. technology, the films such as selected region evaporation inducing metal In, Sn or Bi are accurately controlled in, thickness is in several nanometers to tens
Nanometer；2) above-mentioned substrate is put into PECVD system intracavitary, in 200 DEG C -500 DEG C of temperature, power 2W-50W using hydrogen etc.
Gas ions are handled metallic film, make discrete quasi- nano-catalytic of the diameter between tens nanometers to several microns
Particle；The changes such as different and the temperature of processing, power, time that can be by regulating and controlling thickness of metal film are controllable to form catalytic gold
The size of metal particles；3) in a pecvd system, one layer of suitable thickness (several nanometers to tens nanometers) of covering on substrate
Amorphous silicon layer；4) anneal (temperature is at 350 DEG C -400 DEG C), swashed in a vacuum or in the non-oxidizing atmosphere such as hydrogen, nitrogen
Catalyticing metal particle meeting spontaneous absorption non-crystalline silicon living, separates out crystalline silicon, while diameter generating period changes, and grows bead string shape
Nano wire.
The present invention program can be by adjusting growth course plasma processing time power and temperature, covering non-crystalline silicon
The parameters such as the thickness and temperature conditionss of growth, annealing temperature and time regulate and control the growth of bead string shape nano wire, obtain diameter, week
The adjustable silicon nanowires such as phase length.
Selected inducing metal both can be Sn, Bi or In or other can induce plane nano line to grow
Metal.
Further, the bead string shape nano wire of planar growth both can be that the semiconductors such as silicon nanowires or germanium are received
Rice noodles, nano wire can be intrinsic nano wire or be doped nanowire.
The positioning of inducing metal can both use mask plate, photoetching technique, nanometer embossing can also be utilized to obtain.
The substrate of growth bead string shape silicon nanowires is planar semiconductor substrate, or organic resistance to 350 DEG C of high-temperature material substrates.
The plane solid-liquid that the present invention uses-(Gu IP-SLS) growth mechanism is similar to VLS mechanism, the difference with VLS mechanism
It is, in VLS mechanism growth courses, required raw material are provided by gas phase；And in SLS mechanism growth courses, it is required
Raw material is provided from the non-crystalline material of solid-state, in general, in the method is commonly used low-melting-point metal (such as In, Sn or Bi) and is made
For cosolvent, equivalent to the catalyst in VLS mechanism.
Beneficial effects of the present invention, the present invention grow bead string shape semiconductor using IP-SLS methods and received in a pecvd system
Rice noodles.The advantage of IP-SLS methods is, it is possible to achieve the self-positioning nano-wire array of primary reconstruction, the life of bead string shape silicon nanowires
Long technology is to be based on IP-SLS methods, by regulating and controlling the thickness of metal catalytic drop and non-crystalline silicon, by metal catalytic drop with receiving
Inherent interaction between rice noodles, autonomous growth in situ go out the nano wire of diameter mechanical periodicity, and transmission electron microscope characterizes
After prove, it only has diameter to change, and nano wire keeps high quality single crystal in itself.With reference to the technological orientation catalysed particulate such as photoetching
Position, it is possible to obtain the self-positioning plane high quality bead string shape silicon nanowire array of self assembly.Because such nano wire is given birth to
Length is unrelated with the selection of substrate, and in addition to common nano wire transfer techniques, it still can be real on the high temperature-resistant liner bottom of part
Existing primary reconstruction is self-positioning.Again due to itself being exactly monocrystalline silicon, it can easily blend, be easy to existing silicon technology
Integra-tion application.Special coulomb island structure possessed by the nano wire grown due to the present invention, will be to realizing that single electron transports
Regulation and control, preparing single-electron device has revolutionary break through., can again because its growth is determined by the position of catalysis inducing metal completely
The self-positioning array growth of self assembly is realized, will there is huge applications prospect at the integrated aspect of single electron quantum device.This item
Technology is prepared and integrated for the self-positioning single electron quantum device of self assembly based on (Button-up) technology from bottom to top and provides
Key technology basis.Therefore, self-positioning prepare of IPSLS growth mechanism self assemblies that the present invention takes grows bead string shape silicon nanowires
Technology prepared in single electron quantum device and integrated aspect has broad application prospects.
4th, illustrate
Fig. 1:A kind of manufacturing flow chart of high quality bead string shape monocrystalline silicon nano line provided by the invention.
(a) is the SEM shape appearance figures of bead string shape monocrystalline silicon nano line in Fig. 2.(b)-(d) is the TEM image of nano wire, wherein
(b) it is low power TEM image, (c) and (d) is the high-resolution TEM image of A and B points (region) in (b).
Fig. 3 (a) are under Coulomb blockade effect, and bead string shape nano wire realizes the schematic diagram that single electron transports, and (b) is single electricity
Sub- quantum device prepares schematic diagram.
5th, embodiment
For the object, technical solutions and advantages of the present invention are more clearly understood, below in conjunction with specific embodiment, to this hair
Bright further description.
Embodiment 1, Sn (tin) induced growth diameters are in the periodically variable bead string shape monocrystalline silicon nanometers of about 100nm/300nm
Line
1) using the n-type heavy doping monocrystalline of the silicon dioxide layer of 500 μm of general thickness and front with 300nm dry-oxygen oxidations
Silicon chip is as experiment substrate.And using RCA standard cleanings method cleaning substrate, obtain clean smooth substrate.
2) conventional lithographic techniques are used, stripe array pattern are produced on substrate, the width of bar shaped is 10 μm, spacing
100μm.100nm inducing metal Sn is deposited on the substrate with photoengraving pattern using the method for thermal evaporation.Removed with acetone
After photoresist, metal Sn stripe array pattern is left.
3) sample is put into PECVD system, after vacuumizing, at 320 DEG C of temperature, pressure 80Pa atmosphere of hydrogen, opened
The radio frequency of PECVD system is opened, power 20W, sample 10min is handled using the hydrogen gas plasma of formation, forms 500-800nm
The metal Sn drops of left and right.
4) 120 DEG C are cooled in a pecvd system, pumps the hydrogen in system, are passed through silane, pressure maintains 18Pa,
Under radio-frequency power 2W, one layer of about 60nm amorphous silicon membrane is covered on substrate.
5) PECVD system is warming up to 400 DEG C, and anneal 30min in 130Pa atmosphere of hydrogen.The Sn drops being activated are just
The amorphous silicon of surrounding can be absorbed, autonomous induction grows diameter in the periodically variable bead string shape monocrystalline of about 100nm/300nm
Silicon nanowires.
Embodiment 2, Sn (tin) induced growth diameters are in the periodically variable bead string shape monocrystalline silicon nano lines of about 30nm/80nm
1) using the n-type heavy doping monocrystalline of the silicon dioxide layer of 500 μm of general thickness and front with 300nm dry-oxygen oxidations
Silicon chip is as experiment substrate.And using RCA standard cleanings method cleaning substrate, obtain clean smooth substrate.
2) conventional lithographic techniques are used, stripe array pattern are produced on substrate, the width of bar shaped is 10 μm, spacing
100μm.100nm inducing metal Sn is deposited on the substrate with photoengraving pattern using the method for thermal evaporation.Removed with acetone
After photoresist, metal Sn stripe array pattern is left.
3) sample is put into PECVD system, after vacuumizing, at 320 DEG C of temperature, pressure 80Pa atmosphere of hydrogen, opened
The radio frequency of PECVD system is opened, power 20W, sample 10min is handled using the hydrogen gas plasma of formation, forms 500-800nm
The metal Sn drops of left and right.
4) 120 DEG C are cooled in a pecvd system, pumps the hydrogen in system, are passed through silane, pressure maintains 18Pa,
Under radio-frequency power 2W, one layer of about 30nm amorphous silicon membrane is covered on substrate.
5) PECVD system is warming up to 400 DEG C, and anneal 30min in 130Pa atmosphere of hydrogen.The Sn drops being activated are just
The amorphous silicon of surrounding can be absorbed, autonomous induction grows diameter in the periodically variable bead string shape monocrystalline silicon of about 30nm/80nm
Nano wire.
Particular embodiments described above, the purpose of the present invention, technical scheme and beneficial effect are carried out further in detail
Describe in detail it is bright, should be understood that the foregoing is only the present invention specific embodiment, be not intended to limit the invention, it is all
Within the spirit and principles in the present invention, any modification, equivalent substitution and improvements done etc., it should be included in the guarantor of the present invention
Within the scope of shield.
Claims (9)
- A kind of 1. method for preparing plane bead string shape monocrystalline silicon nano line, it is characterised in that step is as follows, and 1）In smooth substrate On, coordinate photoetching or other pattern generation technologies, In, Sn or Bi inducing metal film are deposited in localization region, as nano wire is given birth to Long initial position, thickness of metal film is in several nanometers to tens nanometers；2）Above-mentioned substrate is put into PECVD system intracavitary, In 200 DEG C -500 DEG C of temperature, after hydrogen gas plasma processing sample 5-30 minutes, metal film can form a large amount of tens nanometers to several Various sizes of quasi- nano-catalytic metallic particles between micron；3）In a pecvd system, one layer several nanometers to hundreds of nanometers are covered The amorphous silicon layer of thickness is as presoma dielectric layer；4）In a vacuum or including hydrogen, nitrogen non-oxidizing atmosphere in move back Fire, temperature are at 350-400 DEG C, and catalyticing metal particle can be activated, spontaneous absorption non-crystalline silicon, separate out monocrystalline silicon, while diameter is sent out Raw cyclically-varying, grows bead string shape nano wire.
- 2. according to the method for claim 1, it is characterised in that：Step 2）Middle plasma power is 2-20W.
- 3. according to the method for claim 1, it is characterised in that：Step 4）In a vacuum or including hydrogen, nitrogen it is non- Annealing time is 30-60min in oxidizing atmosphere.
- 4. according to the method for claim 1, it is characterised in that：By adjust growth course plasma processing time, Temperature conditionss, annealing temperature and the time parameter of power and temperature, covering amorphous silicon thickness and growth regulates and controls bead string shape nanometer The growth of line, obtain diameter, cycle and length-adjustable silicon nanowires.
- 5. according to the method for claim 1, it is characterised in that the adjusting and controlling growth of the size of bead string shape nano wire refers to pass through Regulate and control the size of metal catalytic drop, amorphous silicon thickness, annealing temperature and time parameter are realized.
- 6. according to the method for claim 1, it is characterised in that the inducing metal is Sn, Bi or In, or other can be lured Lead the metal of growth plane nano wire.
- 7. according to the method for claim 1, it is characterised in that the bead string shape nano wire of planar growth is silicon nanowires or germanium Semiconductor nanowires, the nano wire are intrinsic nano wire or doped nanowire.
- 8. according to the method for claim 1, it is characterised in that the positioning mask plate or utilization photoetching technique of inducing metal, Nanometer embossing.
- 9. according to the method for claim 1, it is characterised in that the substrate of growth bead string shape silicon nanowires is planar semiconductor Substrate or resistance to 350 DEG C of high temperature organic material substrate.
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| CN107640741B (en) * | 2017-03-15 | 2019-11-15 | 南京大学 | A method of plane germanium silicon and related nanowire growth pattern and component regulation based on the supply of heterogeneous lamination noncrystal membrane |
| CN108231542A (en) * | 2018-01-09 | 2018-06-29 | 南京大学 | A kind of plane germanium silicon based on heterogeneous lamination noncrystal membrane and related nanowire growth method |
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| CN101798089A (en) * | 2010-01-21 | 2010-08-11 | 复旦大学 | Silicon oxide nanowire growing by catalysis of germanium and preparation method thereof |
| CN101891145A (en) * | 2009-05-22 | 2010-11-24 | 熊长宏 | Silicon nanowire preparation by gas-liquid-solid phase method |
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| CN101891145A (en) * | 2009-05-22 | 2010-11-24 | 熊长宏 | Silicon nanowire preparation by gas-liquid-solid phase method |
| CN101798089A (en) * | 2010-01-21 | 2010-08-11 | 复旦大学 | Silicon oxide nanowire growing by catalysis of germanium and preparation method thereof |
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