CN1484278A - Method for contruction of tow-dimension ordered distributing silicon quantum point figurated nano structure - Google Patents
Method for contruction of tow-dimension ordered distributing silicon quantum point figurated nano structure Download PDFInfo
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- CN1484278A CN1484278A CNA031316859A CN03131685A CN1484278A CN 1484278 A CN1484278 A CN 1484278A CN A031316859 A CNA031316859 A CN A031316859A CN 03131685 A CN03131685 A CN 03131685A CN 1484278 A CN1484278 A CN 1484278A
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Abstract
A method for building two-dimension orderly distributed Si quantum spot graphic nanameter structure is to process a phase-shift grating form board on the film of a-Si or a-SiNx: H/a-Si: H/a-SiNx: H then to crystallize it by laser interference, the laser beam arrives at surfaces of a-Si film or a-SiNx: H/a-Si: H/a -SiNx: H via the form board to form beam spots of two dimension periodic distribution of the energy density to make a -Si: H film to realize localized crystallization, that is to form nanometer Si quantum spot array of two-dimension space orderly distributed in the film.
Description
One, technical field:
The present invention proposes a kind of new technology of utilizing quasi-molecule ultra-short pulse laser interference crystallisation to construct the orderly graphical nanostructure of high-density silicon quantum dot that distributes of two-dimensional space from know-why and implementing process two aspects.The graphical distribution nano silicon quantum dots film in order that is provided by this technology is the critical material of studying in the high-tech areas such as nanoelectronic of new generation and nano photoelectronic devices.
Two, background technology:
The nano-electron of based semiconductor quantum structure and photoelectron are integrated to be the core of 21 century new generation of semiconductor device, also is the hardware foundation of modern information technologies.Semiconductor silicon (Si) is the most important material of current preparation microelectronic component, yet whether Si can continue to play an important role in the nanometer electronic device epoch, whether can realize that Si monolithic photoelectricity is integrated, this is the great research topic in present material science and the microelectronics field, also be the international research forward position of this subject, have important basic and applied research meaning.
In recent ten years, many experiments and theoretical research work show, when the size of Si material is reduced to several nanometers (intending with the de Broglie wavelength comparability of electronics), present tangible quantum size effect, particularly its optical characteristics is significantly improved, luminous efficiency improves greatly, and existing report utilizes the quantum size effect of nanometer Si to prepare Si quantum dot single-electron transistor, memory, nanometer Si base luminescent device
[2]L.Pavesi, et.al, Nature
408, 440 (2000) etc., thus worldwide started the upsurge of research Si quantum dot (also claiming nano-silicon nc-Si).In current numerous methods that prepare nanometer Si quantum dot thin-film material, can be summed up as two approach, the first adopts the advanced person but nanofabrication techniques such as the electron beam exposure of cost costliness and reactive ion etching, directly prepare the Si quantum dot, its advantage is that size Control is accurate, but because restriction of the minimum dimension of its etching and surface damage have brought difficulty to practical application.Another approach is to adopt the self-assembled growth technology, forms large-area nanometer Si quantum dot film by atom, molecule or corresponding presoma through growth mechanisms such as nucleation, gathering, growth, phase transformations.But the dimensional controllability and the distribution order (graphically) of the nano-quantum point that is obtained by this approach also exist difficult greatly.
International review points out that nanometer Si quanta point material will really be adopted by industrial quarters and necessarily require (1) quantum dot controllable size, distributes in order; (2) quantum dot blemish attitude is by fine passivation; (3) compatible mutually with current microelectronic technique.Thereby it is compatible mutually to seek a kind of and current microelectronic technique, can prepare the new technology of the graphical film that distributes of nanometer Si quantum dot, and might to be applied to following nanoelectronics and optoelectronics device be starting point of the present invention.
The restricted crystallization technology of having set up at us of ultra-thin amorphous Si (a-Si) layer laser prepares on the research basis of high density nanometer Si
[3]K.J.Chen, X.F.Huang et.al.Appl.Phys.Lett.
612069 (1992)
M.X.Wang，K.J.Chen，et.al.Appl.Phys.Lett.
72722(1998)
X.F.Huang, K.J.Chen et.al.J.Non.Cryst.,
266(2000) 1015, the new technology of constructing the graphical nanostructure of sequential 2 D distribution silicon quantum dot that we propose is to utilize quasi-molecule ultra-short pulse laser interfering beams and ultra-thin a-Si film (thickness is less than 10nm) mutual effect, distribute the in order nanometer silica quantum dot array of (graphically) of self assembly formation two-dimensional space.Referring to D.C.Glattli, Nature,
393516 (1998)
Three, summary of the invention:
Show by domestic and international result of study in recent years: make nano silicon quantum dots walk out the laboratory, really can be adopted by industrial quarters, both required to control the size of quantum dot, requirement can be carried out passivation to the surface of silicon quantum dot again, and is also compatible mutually with current microelectronic process engineering simultaneously.
Purpose of the present invention is exactly the requirement at above three aspects, propose to construct the graphically new technology principle of the nanostructure of distribution of Si quantum dot in conjunction with the laser crystallization technology, design and provide a kind of new technical method experimentally with the moving phase grating masterplate of particular design.Utilize this method both compatible mutually with current microelectronic process engineering, avoid the hyperfine process technology of use cost costliness again, when obtaining the graphical high density nano silicon quantum dots that distributes, can carry out effective passivation with the reduction defect state density to the nanocrystal surface again, thereby can show the quantum effect that causes owing to change in size.Reach the purpose of regulation and control orderly architecture of low-dimensional and performance.The quantum device of preparing based on this technology will become devices field that great application prospect and value are arranged with the nano photoelectric subclass at the nanoelectronic in future.
The present invention is achieved in that the method for constructing the graphical nanostructure of sequential 2 D distribution silicon quantum dot, it is characterized in that ultra-thin amorphous silicon (a-Si) film or a-SiN
X: H/a-Si:H/a-SiN
X: make the moving phase grating masterplate on the H structural membrane earlier, then with the laser interference crystallization: laser beam arrives a-Si film or a-SiN through two-dimentional moving phase grating masterplate
X: H/a-Si:H/a-SiN
X: form the bundle spot that the energy density two-dimension periodic distributes on the H structural membrane surface, make the a-Si:H film realize selective crystallization, promptly in film, form distribute the in order nanometer silica quantum dot array of (graphically) of two-dimensional space.
The advantage of the technology of the present invention:
1. graphical quantum dot film can be produced in batches: the two-dimentional moving phase grating masterplate of design in advance is placed in the light path of laser crystallization, under suitable laser energy density irradiation, makes the a-Si film or the a-SiN that wait for selective crystallization
X: H/a-Si:H/a-SiN
X: H structural membrane selective crystallization forms and corresponding to figure of moving phase grating masterplate cycle, thereby realizes that in film quantum dot graphically distributes.Change the masterplate design according to requirement on devices, can carry out graphical quantum dot film and produce in batches.
2. can control the formation and the size of silicon quantum dot effectively.The size of silicon quantum dot is relevant with the thickness of film.Because the thickness of a-Si:H sublayer can manually design in the membrane structure, precision can reach 0.5nm, and controllability is strong, thereby makes the last nc-Si quantum dot size that forms also can manually design and control.
3. the surface of nano silicon quantum dots is by the hydrogen atom passivation: utilize nc-Si quantum dot surface that the technical program obtains because hydrogen atom and a-SiN
X: the existence of H deielectric-coating can obtain effective passivation protection, reduces interface state density, makes it be highly suitable for constructing following nano-device.
4. last, the formation of quantum dot is to utilize the laser crystallization technology in the technical program, has avoided the high-temperature process in the conventional thermal annealing technology, and this point is particularly conducive to and from now on this technology is used for receiving photoelectron and nano-electron integrated device.
The technology of the present invention also is applicable to the preparation of other semi-conducting material quantum dot.
Four, description of drawings:
Fig. 1 a laser crystallization device of the present invention schematic diagram: 1, laser; 2, diaphragm; 3, focus on quartz lens; 4, speculum; 5, moving phase grating masterplate; 6, sample; 7, X-Y loading mobile platform;
Fig. 1 b the present invention interferes back arrival sample surfaces schematic diagram by the laser beam of two-dimentional moving phase grating masterplate.
Fig. 2: (a) scanning electron microscopy of two-dimentional moving phase grating masterplate (SEM) photo
(b) the equally distributed outgoing laser beam of energy density arrives a-Si film or a-SiN through two-dimentional moving phase grating masterplate
X: H/a-Si:H/a-SiN
X: form the bundle spot that the energy density two-dimension periodic distributes on the H film surface.Figure is that laser energy density is along sample surfaces x direction distribution relation.
Fig. 3 a, scanning electron microscopy (SEM) photo of a-Si:H film after KrF quasi-molecule ultra-short pulse laser is interfered crystallization.The two-dimensional space nanometer silica quantum dot array of (graphically) that distributes in order as can be seen from FIG..
3b, cross section transmission electron microscopy mirror (x-TEM) photo of a-Si:H film after KrF quasi-molecule ultra-short pulse laser is interfered crystallization.The a-Si:H layer thickness is 10nm.From figure, can clearly see the graphical nanostructure of silicon quantum dot that forms in the a-Si:H film after crystallization.The size of quantum dot is about 10nm, and in the zone of about 200nm, the repetition period is 2 μ m by localization for they.
Five, embodiment:
1, ultra-thin amorphous silicon (a-Si) film preparation: utilize plasma reinforced chemical vapor deposition (PECVD) technology to prepare the a-Si:H film.The a-Si:H layer thickness can accurately be controlled in the 1.0-10nm scope; Wish behind the laser crystallization that the quantum dot size that obtains conforms to substantially with the a-Si:H layer thickness.Similarly, we also can prepare (a-SiN
X: H/a-Si:H/a-SiN
X: H) three-layer sandwich structure, this structure have on nano electron device widely to be used.
A-Si:H film and a-SiN
X: H/a-Si:H/a-SiN
X: the preparation of H three-layer sandwich structural membrane:
Utilize computer-controlled plasma reinforced chemical vapor deposition (PECVD) technology, adopt silane (SiH
4), ammonia (NH
3) and argon gas (Ar) as reactant gas source; Deposit a-Si:H film or a-SiN on monocrystalline silicon piece and two throwing vitreosil or optical glass substrate
X: H/a-Si:H/a-SiN
X: H three-decker film.Concrete process conditions during preparation are as follows:
Power source frequency: 13.56MHz; Power density: 0.2-0.3W/cm
2
Reaction chamber pressure: 33-40Pa; Underlayer temperature: 250 ℃
When deposition of amorphous silicon (a-Si:H) sublayer, by SiH
4+ Ar forms by the aura decomposition reaction, wherein SiH
4Flow is 8sccm (a per minute standard cubic centimeter), and deposition rate is 0.10nm/s; And amorphous silicon nitride (a-SiN:H) sublayer is by SiH
4+ NH
3+ Ar mixed gas reaction forms, NH during reaction
3/ SiH
4Gas flow ratio is 5, and the optical band gap of the a-SiN:H film of Huo Deing is about 3.0eV like this, and deposition rate is 0.11nm/s.A-Si:H and a-SiN
X: H sublayer thickness can design as requested.In our example, a-Si:H sublayer thickness is 10nm, a-SiN
X: H sublayer thickness is 30nm.Key problem in technology is to utilize the switch of computer control gas valve and the speed of exhaust faster to make that gas can quick exchange when the different sublayer of deposit in the reaction chamber in the deposition process.
2, moving phase grating stamp fabrication: the two throwing of general employing vitreosils are base material, prepare repetition period 1-3 μ m with microelectronic process engineerinies such as evaporation, photoetching, electron beam exposure, reactive ion beam etching (RIBE)s, commonly used is two kinds of two-dimentional moving phase grating masterplates of 1 μ m and 2 μ m.
The specific design of moving phase grating masterplate and making: the grating cycle of the two-dimentional moving phase grating masterplate that this example uses is d=2 μ m, grating depth of groove
H is 248nm, h=λ/2 (n-1)
λ is a KrF optical maser wavelength in the formula, and n is quartzy refractive index.Concrete manufacturing process is as follows: the preparation of (1), two throwing vitreosil; (2), the quartz surfaces evaporation of aluminum, the aluminium film thickness is about 1 μ m; (3), on the surface of aluminium film, apply photoresist; (4), adopt the electron beam lithography technology in photoresist, to form the two-dimensional grating figure of design; (5), with chemical corrosion method graph copying to the aluminium film; (6), utilize reactive ion etching technology, make mask with the aluminium film quartz carried out etching, raster graphic is copied on the quartz plate, thereby control etch period control grating depth of groove is made the moving phase grating masterplate.
3, the quasi-molecule ultra-short pulse laser is interfered crystallization: use optical maser wavelength to make LASER Light Source as the KrF excimer pulse laser of 248nm.The even emitting laser bundle of energy density arrives a-Si film or a-SiN through two-dimentional moving phase grating masterplate
X: H/a-Si:H/a-SiN
X: form the bundle spot that the energy density two-dimension periodic distributes on the H structural membrane surface, make the a-Si:H film realize selective crystallization, promptly in film, form distribute the in order nanometer silica quantum dot array of (graphically) of two-dimensional space.
Concrete KrF excimer pulsed laser crystallization process:
Utilize the laser irradiating device shown in Fig. 1 (a), adopt the KrF excimer pulsed laser a-Si:H film or a-SiN
X: H/a-Si:H/a-SiN
X: samples such as H three-decker carry out crystallization to be handled, and makes a-Si:H layer selective crystallization.The wavelength of used KrF excimer pulsed laser is 248nm, pulse duration 30ns.In our concrete instance, utilize the laser interference bundle to the a-Si:H layer crystalization, localization forms quantum dot in the a-Si:H of original deposit layer.The size of quantum dot is about 10nm, and in the zone of about 200nm, the repetition period is 2 μ m (seeing Fig. 3 (b)) by localization for they.Concrete process conditions are:
Laser irradiation area: 6 * 5mm
2
Laser irradiation density: 500-800mJ/cm
2
Behind laser scanning irradiation, the a-Si:H sublayer has formed nano silicon quantum dots through the nucleating growth process, has been formed the quantum dot of silicon really in former amorphous silicon sublayer by the section electron microscope examination.By changing a-Si:H sublayer thickness, utilize this method can obtain to be of a size of the silicon quantum dot of 1-10nm.
The present invention also is suitable for other laser, for example: excimer pulse lasers such as ArF, XeCl.As long as correspondingly change the grating etching depth according to optical maser wavelength.
Claims (6)
1, constructs the method for the graphical nanostructure of sequential 2 D distribution silicon quantum dot, it is characterized in that ultra-thin amorphous silicon (a-Si) film or a-SiN
X: H/a-Si:H/a-SiN
X: make the moving phase grating masterplate on the H structural membrane earlier, then with the laser interference crystallization: laser beam arrives a-Si film or a-SiN through two-dimentional moving phase grating masterplate
X: H/a-Si:H/a-SiN
X: form the bundle spot that the energy density two-dimension periodic distributes on the H structural membrane surface, make the a-Si:H film realize selective crystallization, promptly in film, form distribute the in order nanometer silica quantum dot array of (graphically) of two-dimensional space.
2, by the described method of constructing the graphical nanostructure of sequential 2 D distribution silicon quantum dot of claim 1, the two throwing of the employing vitreosil that it is characterized in that the moving phase grating masterplate is a base material, prepares the two-dimentional moving phase grating masterplate that the repetition period is 1 μ m to 3 μ m with microelectronic process engineerinies such as evaporation, photoetching, electron beam exposure, reactive ion beam etching (RIBE)s.
3, by the described method of constructing the graphical nanostructure of sequential 2 D distribution silicon quantum dot of claim 1, it is characterized in that the moving phase grating masterplate grating cycle is d=2 μ m, grating depth of groove h is 248nm, h=λ/2 (n-1), λ is a KrF optical maser wavelength in the formula, and n is quartzy refractive index.
4, by the described method of constructing the graphical nanostructure of sequential 2 D distribution silicon quantum dot of claim 1, it is characterized in that the method for making the moving phase grating masterplate is: quartz surfaces evaporation of aluminum, aluminium film thickness are about 1 μ m; On the surface of aluminium film, apply photoresist; Adopt the electron beam lithography technology in photoresist, to form the two-dimensional grating figure of design; With chemical corrosion method graph copying to the aluminium film; Utilize reactive ion etching technology, make mask with the aluminium film quartz is carried out etching, raster graphic is copied on the quartz plate, thereby control etch period control grating depth of groove is made the moving phase grating masterplate.
5, by the described method of constructing the graphical nanostructure of sequential 2 D distribution silicon quantum dot of claim 1, the method that it is characterized in that the laser interference crystallization is: the quasi-molecule ultra-short pulse laser is interfered crystallization: use optical maser wavelength is that the KrF excimer pulse laser of 248 nm is made LASER Light Source, and the even emitting laser bundle of energy density arrives a-Si film or a-SiN through two-dimentional moving phase grating masterplate
X: H/a-Si:H/a-SiN
X: form the bundle spot that the energy density two-dimension periodic distributes on the H structural membrane surface, make the a-Si:H film realize selective crystallization, promptly in film, form distribute the in order nanometer silica quantum dot array of (graphically) of two-dimensional space.
6, by the described method of constructing the graphical nanostructure of sequential 2 D distribution silicon quantum dot of claim 5, the method that it is characterized in that the laser interference crystallization is: the wavelength of KrF excimer pulsed laser is 248nm, pulse duration 30ns, utilize the laser interference bundle to the a-Si:H layer crystalization, localization forms quantum dot in the a-Si:H of original deposit layer, the size of quantum dot is about 10nm, and in the zone of about 200nm, the repetition period is 2 μ m by localization for they.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1299327C (en) * | 2004-10-21 | 2007-02-07 | 上海交通大学 | Method for preparing large-area and height ordered nanometer silica quantum dot array |
| CN100376467C (en) * | 2005-10-14 | 2008-03-26 | 江苏大学 | Method and apparatus for laser interference coupling preparation of nono-material |
| CN100395565C (en) * | 2004-12-16 | 2008-06-18 | 中国工程物理研究院激光聚变研究中心 | Quantum lattice diffracting rasters |
| CN101928914A (en) * | 2010-09-02 | 2010-12-29 | 南京大学 | Method for preparing large-area two-dimensional super-structure material |
| CN103972079A (en) * | 2014-04-01 | 2014-08-06 | 三峡大学 | Preparation method for ordered silicon quantum dots in three-dimensional space |
| CN106115681A (en) * | 2016-07-11 | 2016-11-16 | 浙江工业大学 | One realizes the patterned method of two-dimensional material |
Families Citing this family (1)
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|---|---|---|---|---|
| CN100446290C (en) * | 2007-02-09 | 2008-12-24 | 南京大学 | Oxygen silicon base doped nitride film yellow green wave band LED and its preparing method |
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2003
- 2003-06-06 CN CN 03131685 patent/CN1242454C/en not_active Expired - Fee Related
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1299327C (en) * | 2004-10-21 | 2007-02-07 | 上海交通大学 | Method for preparing large-area and height ordered nanometer silica quantum dot array |
| CN100395565C (en) * | 2004-12-16 | 2008-06-18 | 中国工程物理研究院激光聚变研究中心 | Quantum lattice diffracting rasters |
| CN100376467C (en) * | 2005-10-14 | 2008-03-26 | 江苏大学 | Method and apparatus for laser interference coupling preparation of nono-material |
| CN101928914A (en) * | 2010-09-02 | 2010-12-29 | 南京大学 | Method for preparing large-area two-dimensional super-structure material |
| CN101928914B (en) * | 2010-09-02 | 2011-12-21 | 南京大学 | Method for preparing large-area two-dimensional super-structure material |
| CN103972079A (en) * | 2014-04-01 | 2014-08-06 | 三峡大学 | Preparation method for ordered silicon quantum dots in three-dimensional space |
| CN103972079B (en) * | 2014-04-01 | 2016-06-01 | 三峡大学 | The preparation method of the orderly silicon quantum dot of a kind of three-dimensional spatial distribution |
| CN106115681A (en) * | 2016-07-11 | 2016-11-16 | 浙江工业大学 | One realizes the patterned method of two-dimensional material |
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