CN101910467B - Metal catalyzed selective deposition of materials including germanium and antimony - Google Patents
Metal catalyzed selective deposition of materials including germanium and antimony Download PDFInfo
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- 239000000463 material Substances 0.000 title claims abstract description 92
- 239000002184 metal Substances 0.000 title claims abstract description 69
- 229910052751 metal Inorganic materials 0.000 title claims abstract description 69
- 229910052732 germanium Inorganic materials 0.000 title claims abstract description 48
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 title claims abstract description 42
- 229910052787 antimony Inorganic materials 0.000 title claims description 52
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 title claims description 38
- 230000008021 deposition Effects 0.000 title claims description 33
- 239000000758 substrate Substances 0.000 claims abstract description 74
- 238000000034 method Methods 0.000 claims abstract description 53
- 238000000151 deposition Methods 0.000 claims abstract description 43
- 238000005229 chemical vapour deposition Methods 0.000 claims abstract description 36
- 239000006023 eutectic alloy Substances 0.000 claims abstract description 10
- 239000002243 precursor Substances 0.000 claims description 67
- 238000006243 chemical reaction Methods 0.000 claims description 38
- 229910000078 germane Inorganic materials 0.000 claims description 18
- 239000011810 insulating material Substances 0.000 claims description 15
- 125000004429 atom Chemical group 0.000 claims description 14
- 150000001875 compounds Chemical class 0.000 claims description 11
- 239000000126 substance Substances 0.000 claims description 11
- 125000004432 carbon atom Chemical group C* 0.000 claims description 9
- -1 antimony amine Chemical class 0.000 claims description 6
- 229910052799 carbon Inorganic materials 0.000 claims description 6
- 229910052737 gold Inorganic materials 0.000 claims description 6
- 229910052782 aluminium Inorganic materials 0.000 claims description 4
- 229910000074 antimony hydride Inorganic materials 0.000 claims description 4
- 230000015572 biosynthetic process Effects 0.000 claims description 4
- OUULRIDHGPHMNQ-UHFFFAOYSA-N stibane Chemical compound [SbH3] OUULRIDHGPHMNQ-UHFFFAOYSA-N 0.000 claims description 4
- 229910052738 indium Inorganic materials 0.000 claims 2
- 229910005872 GeSb Inorganic materials 0.000 abstract description 52
- 239000010410 layer Substances 0.000 description 26
- 239000007789 gas Substances 0.000 description 17
- 239000003989 dielectric material Substances 0.000 description 14
- 239000010931 gold Substances 0.000 description 14
- 239000004065 semiconductor Substances 0.000 description 6
- 239000010408 film Substances 0.000 description 5
- 230000014509 gene expression Effects 0.000 description 5
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- 238000010438 heat treatment Methods 0.000 description 4
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- 125000003118 aryl group Chemical group 0.000 description 3
- 238000003486 chemical etching Methods 0.000 description 3
- 239000004020 conductor Substances 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 150000004767 nitrides Chemical class 0.000 description 3
- 238000000623 plasma-assisted chemical vapour deposition Methods 0.000 description 3
- 239000013074 reference sample Substances 0.000 description 3
- 229910004298 SiO 2 Inorganic materials 0.000 description 2
- 229910000577 Silicon-germanium Inorganic materials 0.000 description 2
- VODLILZKLVZCEA-UHFFFAOYSA-N [Sb].CNC Chemical compound [Sb].CNC VODLILZKLVZCEA-UHFFFAOYSA-N 0.000 description 2
- 125000002915 carbonyl group Chemical group [*:2]C([*:1])=O 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 238000000224 chemical solution deposition Methods 0.000 description 2
- 238000000295 emission spectrum Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 230000008020 evaporation Effects 0.000 description 2
- 238000001704 evaporation Methods 0.000 description 2
- 239000008246 gaseous mixture Substances 0.000 description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000012071 phase Substances 0.000 description 2
- 238000001020 plasma etching Methods 0.000 description 2
- 238000007747 plating Methods 0.000 description 2
- 238000004062 sedimentation Methods 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 238000001228 spectrum Methods 0.000 description 2
- 239000002344 surface layer Substances 0.000 description 2
- 229910001218 Gallium arsenide Inorganic materials 0.000 description 1
- 229910000927 Ge alloy Inorganic materials 0.000 description 1
- 229910000673 Indium arsenide Inorganic materials 0.000 description 1
- 229910003811 SiGeC Inorganic materials 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 239000005864 Sulphur Substances 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 125000000217 alkyl group Chemical group 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000000295 complement effect Effects 0.000 description 1
- 238000005137 deposition process Methods 0.000 description 1
- VXGHASBVNMHGDI-UHFFFAOYSA-N digermane Chemical compound [Ge][Ge] VXGHASBVNMHGDI-UHFFFAOYSA-N 0.000 description 1
- 238000007772 electroless plating Methods 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- RTZKZFJDLAIYFH-UHFFFAOYSA-N ether Substances CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 239000007792 gaseous phase Substances 0.000 description 1
- 238000004050 hot filament vapor deposition Methods 0.000 description 1
- 150000004678 hydrides Chemical class 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- RPQDHPTXJYYUPQ-UHFFFAOYSA-N indium arsenide Chemical compound [In]#[As] RPQDHPTXJYYUPQ-UHFFFAOYSA-N 0.000 description 1
- 239000011229 interlayer Substances 0.000 description 1
- 238000010884 ion-beam technique Methods 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 238000003801 milling Methods 0.000 description 1
- 229910003465 moissanite Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 230000006911 nucleation Effects 0.000 description 1
- 238000010899 nucleation Methods 0.000 description 1
- 125000002524 organometallic group Chemical group 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 239000012782 phase change material Substances 0.000 description 1
- 238000001259 photo etching Methods 0.000 description 1
- 229920000412 polyarylene Polymers 0.000 description 1
- 229910021420 polycrystalline silicon Inorganic materials 0.000 description 1
- 229920005591 polysilicon Polymers 0.000 description 1
- 238000005086 pumping Methods 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 239000000523 sample Substances 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 229910021332 silicide Inorganic materials 0.000 description 1
- FVBUAEGBCNSCDD-UHFFFAOYSA-N silicide(4-) Chemical compound [Si-4] FVBUAEGBCNSCDD-UHFFFAOYSA-N 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 239000011232 storage material Substances 0.000 description 1
- 150000003457 sulfones Chemical class 0.000 description 1
- 150000003462 sulfoxides Chemical class 0.000 description 1
- 238000006557 surface reaction Methods 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- ZYTLADNCBYKKJS-UHFFFAOYSA-N tert-butylgermane Chemical compound CC(C)(C)[GeH3] ZYTLADNCBYKKJS-UHFFFAOYSA-N 0.000 description 1
- 229920001187 thermosetting polymer Polymers 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
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- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/44—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating
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- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
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Abstract
A chemical vapor deposition (CVD) method for selectively depositing GeSb materials onto a surface of a substrate is provided in which a metal that is capable of forming an eutectic alloy with germanium is used to catalyze the growth of the GeSb materials. A structure is also provided that includes a GeSb material located on preselected regions of a substrate. In accordance with the present invention, the GeSb material is sandwiched between a lower metal layer used to catalyze the growth of the GeSb and an upper surface metal layer that forms during the growth of the GeSb material.
Description
Technical field
The present invention relates to semiconducter device and semiconducter device manufacturing.More specifically, the present invention relates to for optionally deposit chemical vapour deposition (CVD) method of the material that comprises germanium (Ge) and antimony (Sb) on substrate surface.The invention still further relates to the structure that comprises the material layer that comprises Ge and Sb.
Background technology
The material that can reversibly switch between two structures phases that characterized by different resistivity by suitable temperature variation has the potentiality that are used as phase-change storage material.A kind of such material is the material that comprises germanium (Ge) and antimony (Sb).The material that hereinafter will comprise Ge and Sb is called the GeSb material.
In order to make practical memory device, be necessary deposition GeSb material on the substrate with actual pattern complicacy.Be used for realizing that a kind of possible structure of phase change memory device is circuit and via hole (line-and-via) structure, it is similar to those structures of finding in the interconnection wiring structure.In these structures, the phase change material in narrow via openings will consist of the active parts of memory device.
A kind of promising alternative approach that is used for deposition GeSb material is chemical vapour deposition.In CVD, there are the many Organometallic precursors with suitable vapor pressure (for example carbonyl, alkyl etc.) that are used for a large amount of candidate metals.Part but the useful feature of non-all CVD technique is selectivity.By this selectivity, its expression deposition reaction can be performed as material only is deposited on the specific material that underlies on substrate, and is not deposited on other materials on substrate, even these other materials are exposed to reactant gas under temperature of reaction.The common example of this CVD technique is selective growth Si on Si, and not at the common SiO that exists
2Upper growth Si, the W that grows on Si, but equally not at SiO
2Upper growth W.
The problem that conventional CVD method faces is still to keep required above-mentionedly optionally deposit at enough low temperature (lower than approximately 400 ℃) simultaneously.
Up to now, do not have known being used for deposit the GeSb material and have chemical vapour deposition (CVD) method of required selectional feature on substrate at lower than the temperature of 400 ℃.Therefore, need a kind of chemical gaseous phase depositing process of development, wherein this deposition method has the ability that forms the GeSb material on the selection zone of silicon.
Summary of the invention
The invention provides a kind of chemical vapour deposition (CVD) method for the deposition of selectivity on substrate surface GeSb material.In certain embodiments, method of the present invention has the ability of filling high, aspect ratio openings.Use term " high aspect ratio " to represent that the ratio of its height and the width surpasses the opening of 3: 1 at this.Term " opening " expression can be used circuit/via openings, groove of line opening that chemical etching makes, via openings, combination etc.In other embodiments, the invention provides a kind of CVD method for selectivity deposition GeSb material at least one preliminary election surface of substrate.Described preliminary election surface can be positioned on described substrate or described substrate.
CVD method of the present invention allows to control the GeSb stoichiometry in wide value scope, and method of the present invention carries out under lower than the underlayer temperature of 400 ℃, and this makes method of the present invention and existing interconnection process and material compatibility.According to the present invention, the GeSb material can be formed by basic chemical formula GexSby, and wherein x approximately 2 arrives approximately 98 atom %, and y approximately 98 arrives approximately 2 atom %.
As mentioned above, method of the present invention is selectivity CVD method, and it means that the GeSb material is deposited on the part surface of substrate and is not deposited on other surfaces of substrate.Particularly, to can be applicable at insulating material be selectivity deposition GeSb material on dielectric materials in the present invention.For the manufacturing of the circuit that comprises the GeSb material and via hole (circuit/via hole) structure, this is favourable, because via sidewall is processed without any need for special activation before deposition GeSb material.
Generally speaking, method of the present invention comprises:
Substrate is placed in the chemical vapour deposition reaction chamber, and described substrate comprises the zone that comprises such metal, and this metal can form eutectic alloy (eutectic alloy) with germanium;
The described reaction chamber that will comprise described substrate is evacuated to less than 1.333 * 10
-1Pa is preferably less than 1.333 * 10
-1The pressure of foundation of Pa;
Described substrate is heated to temperature lower than 400 ℃;
Provide to described reaction chamber and contain antimony precursor and contain germanium precursor; And
To comprise the deposition of material of germanium (Ge) and antimony (Sb) from described precursor to the described zone that comprises described metal of described substrate.
In some embodiments of the invention, described substrate is the interconnection dielectric materials with at least one opening, and described opening has the aspect ratio greater than 3: 1, and method of the present invention has the ability of filling described at least one opening with the GeSb material selectivity.In this embodiment of the present invention, describedly can be present in the metal that germanium forms eutectic alloy the bottom of described at least one opening.In other embodiments, described substrate has basically smooth surface, and method of the present invention has the ability of selectivity deposition GeSb material on the preselected area that comprises described metal of described substrate.
Except aforesaid method, the present invention also expects a kind of method, wherein deposits described metal and comprises Ge and the material of Sb in the same reactor in destroying vacuum (breaking vacuum).The party's face of the present invention comprises:
Substrate is placed in the chemical vapour deposition reaction chamber;
The described reaction chamber that will comprise described substrate is evacuated to less than 1.333 * 10
-1Pa is preferably less than 1.333 * 10
-4The pressure of foundation of Pa;
Described substrate is heated to temperature lower than 400 ℃;
Form on a zone of described substrate and can form with germanium the metal of eutectic alloy;
Provide to described reaction chamber and contain antimony precursor and contain germanium precursor; And
To comprise the deposition of material of germanium (Ge) and antimony (Sb) from described precursor to the described zone that comprises described metal of described substrate.
In highly preferred embodiment of the present invention, method of the present invention comprises:
Insulating material is placed in the chemical vapour deposition reaction chamber, and described insulating material comprises the zone that comprises Au;
The described reaction chamber that will comprise described interconnection structure is evacuated to less than 1.333 * 10
-1The pressure of foundation of Pa;
Described interconnection structure is heated to temperature lower than 400 ℃;
Provide to described reaction chamber and contain antimony precursor and contain germanium precursor; And
To comprise the deposition of material of germanium (Ge) and antimony (Sb) from described precursor to the described zone that comprises Au of described insulating material.
Except the CVD method that is used for selectivity deposition GeSb material, the invention still further relates to a kind of semiconductor structure that comprises the GeSb material that utilizes method formation of the present invention.Generally speaking, semiconductor structure of the present invention comprises:
Substrate, it comprises metallic zone; And
The material that comprises Ge and Sb on described metal, wherein said material comprise that its thickness is less than the described metallic surface layer of 5 individual layers.
Use the described metallic surface layer of an atom thick of term " individual layer " expression at this.
According to the present invention, described GeSb material is sandwiched in for the lower metal layer of the growth of catalysis GeSb and between the upper surface metal level that the growing period of described GeSb material forms.If described metal is enough thin before the deposition beginning, described lower metal layer can be so thin for leveling off to as not.
Description of drawings
Fig. 1 is (passing through sectional view) example goes out the original texture that can adopt in the present invention before selective chemical vapour deposition GeSb material diagram;
Fig. 2 is the schematic diagram that selectivity deposits the chemical vapor depsotition equipment of GeSb material that is used for that can use in one embodiment of the invention;
Fig. 3 is the diagram of after selectivity deposition GeSb material on the selection zone that utilizes method of the present invention in structure (passing through sectional view);
Fig. 4 illustrates the X ray light emission spectrum of comparing the GeSb material of growing with the reference sample of Ge (0.15) Sb (0.85) on the Au surface; And
Fig. 5 is the chart that is illustrated in intensity with the relation of combination energy of the various GeSb materials that prepare by method of the present invention under different deposition temperatures.
Embodiment
Describe in more detail the present invention referring now to following discussion and accompanying drawing of the present invention, the invention provides for the metal catalytic CVD method of selectivity deposition GeSb material and the structure that forms by the method.Note, the application's accompanying drawing provides for the purpose of example, and therefore, accompanying drawing may not be drawn in proportion.
At first with reference to figure 1, its example goes out the illustrative substrate 10 that can adopt in the present invention.Particularly, this illustrative substrate 10 is insulating material, that is, dielectric materials, its have comprise alternatively in the middle of the smooth surface basically of adhesion layer 12.In an illustrated embodiment, metal 14 is arranged on the top of middle adhesion layer 12.In other embodiments, when not having middle adhesion layer 12, can directly form metal 14 on substrate 10.
In another embodiment, substrate 10 is interconnection structures, and it is included at least one opening that forms in dielectric materials.According to the present invention, described at least one opening has the aspect ratio greater than 3: 1.Described at least one opening can comprise circuit/via structure of via hole, circuit, groove, combination etc.
Although not shown, substrate 10 can typically be arranged on the second substrate.Unshowned the second substrate comprises semiconductive material, insulating material, electro-conductive material or its any combination.When the second substrate is made of semiconductive material, can use any semi-conductor, for example Si, SiGe, SiGeC, SiC, Ge alloy, GaAs, InAs, InP and other III/V or II/VI compound semiconductor.Except the semiconductive material type that these are listed, the present invention also expects such situation, and wherein semiconducter substrate is stacked semiconductor, for example, and Si/SiGe, Si/SiC, silicon-on-insulator (SOI) or sige-on-insulator (SGOI).
When the second substrate was insulating material, this insulating material can be organic insulator, inorganic insulator or its combination that comprises multilayer.When the second substrate was electro-conductive material, for example, the second substrate can comprise alloy, metal silicide, the metal nitride of polysilicon, metal element, metal element or comprise its combination of multilayer.When the second substrate comprises semiconductive material, can make one or more semiconducter device thereon, for example, complementary metal oxide semiconductor (CMOS) device.When the second substrate comprised the combination of insulating material and electro-conductive material, this substrate can represent the first interconnection layer of multilayer interconnect structure.
When forming at least one opening in substrate 10, typically utilize chemical etching to form described opening.Photoetching process is included on the top of the hard mask material (for example, oxide compound and/or nitride) on the top that typically is arranged at substrate 10 and forms photo-resist, photo-resist is exposed to the hope figure of radiation, and the resist that develops and be exposed.Etch process comprises wet chemical etch and/or dry chemical etch.These types the time carving technology in the middle of, preferred dry chemical etch technique, for example reactive ion etching, ion beam milling or plasma etching.In the situation that circuit/via structure, circuit technique thereof after the first via hole of employing routine.Alternately, also expect in the present invention via hole technique after first circuit.
As mentioned above, substrate 10 can comprise optional middle adhesion layer 12.In the middle of optional, adhesion layer 12 comprises metal or metal nitride.The example that is used for the suitable metal of optional middle adhesion layer includes but not limited to: Ti, Ta, Ru and W.
Can utilize conventional depositing operation to form optional adhesion layer 12, for example, this routine depositing operation comprises chemical vapour deposition (CVD), plasma enhanced chemical vapor deposition (PECVD), evaporation, sputter, plating, metal organic deposit and chemical solution deposition.In some embodiments of the invention, can form middle adhesion layer 12 in the reaction chamber identical with the GeSb material and not destroy vacuum between deposition.
When existing, optional in the middle of adhesion layer 12 typically have approximately 1 to the about thickness of 6nm, wherein approximately 2 to about 4nm thickness is more typical.
In the embodiment in figure 1, metal 14 is set on the top of middle adhesion layer 12.In other embodiments, when not having middle adhesion layer, can directly form metal 14 on the top of substrate 10.No matter adopt which kind of embodiment, metal 14 comprises can form with germanium any metal of eutectic alloy.Can include but not limited to the illustrative examples that germanium forms this metal of eutectic alloy: Au, Al and Sn.Preferably, adopt Au or Al as metal 14.More preferably, adopt Au as metal 14.
Can optionally form metal 14 on the preselected area (or pre-selected zone) that wherein will form subsequently the Gesb material of substrate 10.In exemplified embodiment, stride across the structural integrity ground formation metal 14 that comprises middle adhesion layer 12 and substrate 10.In other other embodiment, metal 14 can be set on the specific region of the structure that comprises substrate 10 or in described specific region.
In certain embodiments, can form metal 14 before deposition is as the dielectric materials of substrate 10 on the second substrate.In such embodiments, metal 14 will intactly be present under dielectric materials, and when forming opening in dielectric materials, the part of metal 14 exposes.
The thickness of metal 14 that is used for the selectivity deposition of " catalysis " GeSb material can depend on the depositing operation of the material that uses and use when it forms and change.Typically, metal 14 has approximately 1 to the about thickness of 50nm, and wherein approximately 3 to about 10nm thickness is more typical.
With reference now to Fig. 2,, its example goes out typical chemical vapour deposition (CVD) reactor 50 that is used for deposition GeSb material on the zone of substrate 10 or in it that can adopt in the present invention.Note, although with reference to the exemplified CVD (Chemical Vapor Deposition) reactor 50 of figure 2, the invention is not restricted to utilize only such reactor.But can also utilize the CVD (Chemical Vapor Deposition) reactor that well known to a person skilled in the art other types to carry out the present invention.Below, be described in further detail the reactor of the other types that can adopt in the present invention here.
Again with reference to CVD reactor 50, CVD reactor 50 comprises reaction chamber 52, and wherein original texture is placed in this reaction chamber 52.Reaction chamber 52 typically is vacuum-sealing, and it comprises substrate holder 54, be connected to the shower nozzle 56 of suction manifold 58 and the vacuum pump 60 (for example turbomolecular pump) that can be opened or closed by valve 62.
According to the present invention, all original textures that comprises substrate 10 as shown in Figure 1 are held in place on the surface of the substrate holder 54 in CVD reaction chamber 52.Original texture and shower nozzle 56 typically separate approximately 10 to the about distance of 80mm.Although mention particularly this distance, the invention is not restricted to cited distance.
Under condition in original texture is placed on reaction chamber 52, the pressure in reaction chamber 52 is evacuated to less than 1.333 * 10
-1The pressure of foundation of Pa wherein is more preferably less than 1.333 * 10
-4The pressure of foundation of Pa.Valve 62 by being opened to vacuum pump 60 is implemented to finding time of this pressure of foundation.
In some embodiments of the invention, substrate holder 54 typically comprises heating unit, and this heating unit can contain in deposition subsequently the Ge precursor and contain Sb precursor heating original texture.According to the present invention, this heating unit can be heated to original texture the temperature lower than 400 ℃, wherein approximately 250 ℃ to approximately the temperature of 375 ℃ is more typical.
Then will contain the Ge precursor and contain the Sb precursor by shower nozzle 56 and be incorporated into heated structure.According to shown specific embodiment, be introduced as the precursor of gaseous mixture to shower nozzle 56 by suction manifold 58.Air-flow by utilizing quality controller 64 to allow to contain the Ge precursor from the source 63 typically but do not enter rare gas element not essentially, and by utilizing mass flow controller 68 to make rare gas element 66 flow through and comprise the bubbler 70 that contains the Sb precursor from the source, form precursor gas mixture.Preferably, containing the Ge precursor is the pure Ge of containing precursor, that is, it does not comprise rare gas element.Use in this application term " rare gas element " expression not participate in the gas of the formation of GeSb material.The example of such rare gas element comprises Ar, Ne, N
2, H
2, and He, the preferred Ar of its camber.
According to the present invention, contain the Ge precursor and comprise any compound or the complex compound that comprises Ge.The example that contains the Ge precursor comprises germane (for example first germane, digermane, the third germane and higher germane), comprise 1 to approximately germane base, germane hydride and other organic germanes of 16 carbon atoms.Preferably, contain the Ge precursor and be for example germane or comprise 1 to the about germane base of 6 carbon atoms, for example, the tert-butyl germane.
The Sb precursor that contains that can adopt in the present invention comprises any compound or the complex compound that comprises Sb.The illustrative examples of such precursor comprises that comprising 1 arrives approximately antimony alkyl, antimony amine, antimony hydride and other organic antimony containing compounds of 16 carbon atoms.In a preferred embodiment of the invention, containing the Sb precursor is three (dimethylamine) antimony.
The flow of two kinds of precursor gases that adopt in the present invention can depend on the expection stoichiometry of the GeSb material that produces and change.According to the present invention, the flow that contains the Ge precursor that does not have rare gas element is approximately 1 to about 1000sccm, adopts simultaneously approximately 10 to the about flow that comprises the rare gas element that contains the Sb precursor of 300sccm.When containing the Ge precursor and coexist, the flow that contains the Ge precursor is typically greater than the above-mentioned flow for the pure Ge of containing precursor when rare gas element.In a preferred embodiment of the invention, the flow of the pure Ge of containing precursor gases is approximately 2 to about 150sccm, adopts simultaneously approximately 15 to the about flow that comprises the rare gas element that contains the Sb precursor of 50sccm.In highly preferred embodiment, adopt approximately 20% germane of 5sccm, adopt simultaneously the Ar that comprises 20ml three (dimethylamine) antimony of 20sccm.Should be understood that the particular reactor that above-mentioned flow is applicable to adopt.If adopt another kind of reactor, for example, have the reactor that different volumes is derived spool and pumping speed, preferred flow can depart from the flow that provides above significantly.
It should be noted that during deposition process, the pressure in reaction chamber 52 is maintained at about 1 arrives the approximately deposition pressures of 10 holders.Typically, the deposition pressure in reactor is maintained at about 6 during depositing operation and arrives the approximately values of 8 holders.
Should also be noted that, substituting makes two kinds of precursor gases mix in single input manifold as mentioned above and as shown in Figure 2, method of the present invention works under these circumstances equally, wherein independent manifold is used for every kind of precursor and can shower nozzle itself or in the space between shower nozzle and original texture the mixing of two kinds of precursor gases of generation.The latter is called as and mixes rear system.
Typically with precursor as gaseous mixture, that is, side by side, be provided to original texture 10.Although typically preferably contact simultaneously, the present invention also can be used at first utilizing and contain the Ge precursor and the Ge layer is provided and then provides and contain the Sb precursor.
According to the present invention, can realize comprising Ge and Sb material approximately 10 to the about sedimentation rate of 1000nm/min, wherein more preferably from about 20 to the about sedimentation rate of 150nm/min.
Under above-mentioned details, the present invention forms the material that comprises Ge and Sb that optionally is deposited on metal 14, produces structure shown in Figure 3.In Fig. 3, reference number 20 expressions comprise the material of Ge and Sb.According to the present invention, GeSb material 20 has chemical formula Ge
xSb
y, wherein x approximately 2 arrives the approximately Ge of 98 atom %, and y approximately 98 arrives the approximately Sb of 2 atom %.More preferably, the GeSb material 20 that provides in the present invention is such material, and wherein the atomic percent x of Ge approximately 10 arrives approximately 20 atom %, and the atomic percent y of Sb approximately 90 arrives approximately 80 atom %.
Except forming GeSb material 20, form surface metal-layer 22 on GeSb material 20.According to the present invention, surface metal-layer 22 comprises the metal identical with metal level 14, and metal level 14 also is present in structure shown in Figure 3.Surface metal-layer 22 has the thickness less than 5 single monolayer thick, wherein preferably approximately 1 arrives the approximately thickness of 3 individual layers.Growing period at layer 20 forms surface metal-layer 22 on the surface of GeSb material 20.
Following instance example the present invention in more detail.
Example
In this example, utilization can form the metal conduct of eutectic alloy for the catalyzer of selectivity deposition with Ge, deposits the GeSb materials 360 ℃ of lower selectivity on the surface of dielectric materials.It should be noted that when growth GeSb material on dielectric materials, observe insignificant film growth under the condition of using in this example.When at first depositing Au on dielectric materials, the GeSb material is to surpass the growth velocity deposition of 10nm/min.Fig. 4 illustrates the X ray light emission spectrum of comparing the GeSb material (sample of the present invention) of growing with the reference sample of Ge (0.15) Sb (0.85) on the Au surface.Ge feature in the spectrum of the film that deposits and the intensity of Sb feature show that the composition of the composition that obtains and reference sample is roughly the same.Supplementary features of this spectrum are the appearance at the peak that caused by Au 4f level.This peak is not the gold that results from the film below, swims in the lip-deep gold thin film of film and make to result from growing period.Believe that above-mentioned phenomenon is very important for deposition method of the present invention.
At the temperature that adopts, the Ge precursor be not simply with dielectric surface reaction, or with GeSb material id reaction.Therefore, when being dielectric medium, substrate do not deposit the Ge of significant quantity.When there is no the Ge deposition, Sb is difficult to nucleation in time, so net result is the not growth on dielectric surface.Yet the Ge precursor is stronger with the reaction of Au under growth temperature.This allows the beginning deposition reaction.Yet, for Ge, the conditional solubleness of Au tool, so it swims on the surface of this film, allows to keep growth.
Fig. 5 shows that the little variation (line A-370 ℃, line B-360 ℃, line C-350 ℃) of growth temperature allows to adjust the stoichiometry of GeSb material in wide region.This can also realize by the appropriate variation of precursor gas mixture.
Above example shows, can utilize method of the present invention selectivity deposition GeSb material at lower than the temperature of 400 ℃.For such selectivity deposition occurs, form the metal such as Au on the specific region that will form the GeSb material of substrate.Then form GeSb on the zone that comprises this metal of substrate.
Although illustrate particularly and described the present invention about the preferred embodiments of the present invention, it will be understood by those skilled in the art that can carry out in the form and details above and other changes and do not break away from the spirit and scope of the present invention.Therefore, the present invention is intended to be not limited to definite form and the details of describe and example, but falls within the scope of the appended claims.
Claims (22)
- One kind optionally deposition comprise the method for material (20) of germanium and antimony, comprise the following steps:Substrate is placed in chemical vapour deposition reaction chamber (52), and described substrate comprises the zone (14) that comprises such metal, and described metal can form eutectic alloy with germanium;The described reaction chamber (52) that will comprise described substrate is evacuated to the pressure of foundation less than 0.1333Pa;Described substrate is heated to temperature lower than 400 ℃;Provide to described reaction chamber (52) and contain antimony precursor and contain germanium precursor; AndThe material (20) that will comprise germanium (Ge) and antimony (Sb) from described precursor deposits on the described zone (14) that comprises described metal of described substrate, wherein at the growing period of the described material (20) that comprises germanium and antimony, described metallic surface metal level (22) swims on the surface of the described material (20) that comprises germanium and antimony, and the wherein said material (20) that comprises germanium (Ge) and antimony (Sb) has chemical formula Ge xSb y, wherein x is the Ge of 2 to 98 atom %, y is the Sb of 98 to 2 atom %.
- 2. according to claim 1 method, wherein said metal comprises Au, Al, Ge and In.
- 3. according to claim 2 method, wherein said metal comprises Au.
- 4. according to claim 1 method, the described zone (14) that comprises described metal of wherein said substrate are the diapires that has greater than at least one opening of the aspect ratio of 3: 1.
- 5. according to claim 1 method, wherein simultaneously provide described precursor to described reaction chamber (52).
- 6. at first according to claim 1 method, wherein provide the described germanium precursor that contains to form the Ge layer to described reaction chamber (52), and the described antimony precursor that contains is provided subsequently.
- 7. according to claim 1 method wherein saidly contains organic germane that germanium precursor comprises germane or comprises the germane base of 1 to 16 carbon atom.
- 8. according to claim 1 method, the wherein said antimony precursor that contains is antimony amine, antimony hydride or the organic antimony containing compounds that comprises the antimony alkyl of 1 to 16 carbon atom.
- 9. one kind optionally deposits the method that comprises germanium (Ge) and antimony (Sb), comprises the following steps:Substrate is placed in chemical vapour deposition reaction chamber (52);The described reaction chamber (52) that will comprise described substrate is evacuated to the pressure of foundation less than 0.1333Pa;Described substrate is heated to temperature lower than 400 ℃;Upper formation can form with germanium the metal of eutectic alloy in the zone (14) of described substrate;Provide to described reaction chamber (52) and contain antimony precursor and contain germanium precursor; AndThe material (20) that will comprise germanium (Ge) and antimony (Sb) from described precursor deposits on the described zone (14) that comprises described metal of described substrate, wherein at the growing period of the described material (20) that comprises germanium and antimony, described metallic surface metal level (22) swims on the surface of the described material (20) that comprises germanium and antimony, and the wherein said material (20) that comprises germanium (Ge) and antimony (Sb) has chemical formula Ge xSb y, wherein x is the Ge of 2 to 98 atom %, y is the Sb of 98 to 2 atom %.
- 10. according to claim 9 method, wherein said metal comprises Au, Al, Ge and In.
- 11. method according to claim 10, wherein said metal comprises Au.
- 12. method according to claim 9, the described zone (14) that comprises described metal of wherein said substrate are the diapires that has greater than at least one opening of the aspect ratio of 3: 1.
- 13. method according to claim 9 wherein simultaneously provides described precursor to described reaction chamber (52).
- 14. at first method according to claim 9 wherein provides the described germanium precursor that contains to form the Ge layer to described reaction chamber (52), and the described antimony precursor that contains is provided subsequently.
- 15. method according to claim 9 wherein saidly contains organic germane that germanium precursor comprises germane or comprises the germane base of 1 to 16 carbon atom.
- 16. method according to claim 9, the wherein said antimony precursor that contains is antimony amine, antimony hydride or the organic antimony containing compounds that comprises the antimony alkyl of 1 to 16 carbon atom.
- 17. a method that optionally deposits the material (20) that comprises germanium (Ge) and antimony (Sb) comprises the following steps:Insulating material is placed in chemical vapour deposition reaction chamber (52), and described insulating material comprises the zone (14) that comprises Au;The described reaction chamber (52) that will comprise interconnection structure is evacuated to the pressure of foundation less than 0.1333Pa;Described interconnection structure is heated to temperature lower than 400 ℃;Provide to described reaction chamber (52) and contain antimony precursor and contain germanium precursor; AndThe material (20) that will comprise germanium (Ge) and antimony (Sb) from described precursor deposits on the described zone (14) that comprises Au of described insulating material, wherein comprising described material (20 the growing period of germanium and antimony, the surface metal-layer of described Au (22) swims on the surface of the described material (20) that comprises germanium and antimony, and the wherein said material (20) that comprises germanium (Ge) and antimony (Sb) has chemical formula Ge xSb y, wherein x is the Ge of 2 to 98 atom %, y is the Sb of 98 to 2 atom %.
- 18. method according to claim 17, the described zone (14) that comprises described Au of wherein said insulating material are the diapires that has greater than at least one opening of the aspect ratio of 3: 1.
- 19. method according to claim 17 wherein simultaneously provides described precursor to described reaction chamber (52).
- 20. at first method according to claim 17 wherein provides the described germanium precursor that contains to form the Ge layer to described reaction chamber (52), and the described antimony precursor that contains is provided subsequently.
- 21. method according to claim 17 wherein saidly contains organic germane that germanium precursor comprises germane or covers the germane base of 16 carbon atoms.
- 22. method according to claim 17, the wherein said antimony precursor that contains is antimony amine, antimony hydride or the organic antimony containing compounds that comprises the antimony alkyl of 1 to 16 carbon atom.
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| PCT/US2008/000967 WO2009093994A1 (en) | 2008-01-25 | 2008-01-25 | Metal catalyzed selective deposition of materials including germanium and antimony |
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|---|---|
| CN101910467A CN101910467A (en) | 2010-12-08 |
| CN101910467B true CN101910467B (en) | 2013-05-15 |
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|---|---|
| JP (1) | JP5341107B2 (en) |
| KR (1) | KR20100119756A (en) |
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| KR101771173B1 (en) | 2015-04-22 | 2017-08-24 | 충남대학교산학협력단 | Method of forming germanide and semiconductor device including the germanide |
| CN106756869B (en) * | 2016-12-09 | 2019-03-01 | 中国科学院上海微系统与信息技术研究所 | A method of no adhesion metal Mi Dui grows graphene |
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| US3200490A (en) * | 1962-12-07 | 1965-08-17 | Philco Corp | Method of forming ohmic bonds to a germanium-coated silicon body with eutectic alloyforming materials |
| DE2930789A1 (en) * | 1978-07-28 | 1980-02-07 | Tokyo Shibaura Electric Co | Contact layer for semiconductor chip - consists of nickel or alloy layer and gold-germanium alloy layer for soldering, giving firm bond |
| EP1039448A2 (en) * | 1999-03-26 | 2000-09-27 | Matsushita Electric Industrial Co., Ltd. | Phase change recording with crystallization improving layer |
| CN1763987A (en) * | 2004-09-08 | 2006-04-26 | 三星电子株式会社 | Antimony precursor, the phase change memory device that uses this antimony precursor and manufacture method thereof |
| CN1953229A (en) * | 2006-10-31 | 2007-04-25 | 中国科学院上海微系统与信息技术研究所 | Germanium-titanium base memory material for phase transition memory and its manufacture method |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| DE2359640C2 (en) * | 1973-11-30 | 1983-09-15 | Licentia Patent-Verwaltungs-Gmbh, 6000 Frankfurt | Electrical connection contact to a semiconductor body and use |
| KR100717286B1 (en) * | 2006-04-21 | 2007-05-15 | 삼성전자주식회사 | Methods of forming a phase change material layer and method of forming phase change memory device using the same and phase change memory device formed from using the same |
| KR100763916B1 (en) * | 2006-06-21 | 2007-10-05 | 삼성전자주식회사 | Method of manufacturing gesbte thin film and method of manufacturing phase change random access memory using the same |
| KR100780865B1 (en) * | 2006-07-19 | 2007-11-30 | 삼성전자주식회사 | Methods of forming a semiconductor device including a phase-change layer |
| KR100896180B1 (en) * | 2007-01-23 | 2009-05-12 | 삼성전자주식회사 | Phase change Random Access Memory comprising phase change material layer formed by selective growth method and method of manufacturing the same |
-
2008
- 2008-01-25 CN CN200880124687.2A patent/CN101910467B/en active Active
- 2008-01-25 JP JP2010544276A patent/JP5341107B2/en not_active Expired - Fee Related
- 2008-01-25 WO PCT/US2008/000967 patent/WO2009093994A1/en active Application Filing
- 2008-01-25 KR KR1020107016879A patent/KR20100119756A/en not_active Application Discontinuation
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3200490A (en) * | 1962-12-07 | 1965-08-17 | Philco Corp | Method of forming ohmic bonds to a germanium-coated silicon body with eutectic alloyforming materials |
| DE2930789A1 (en) * | 1978-07-28 | 1980-02-07 | Tokyo Shibaura Electric Co | Contact layer for semiconductor chip - consists of nickel or alloy layer and gold-germanium alloy layer for soldering, giving firm bond |
| EP1039448A2 (en) * | 1999-03-26 | 2000-09-27 | Matsushita Electric Industrial Co., Ltd. | Phase change recording with crystallization improving layer |
| CN1763987A (en) * | 2004-09-08 | 2006-04-26 | 三星电子株式会社 | Antimony precursor, the phase change memory device that uses this antimony precursor and manufacture method thereof |
| CN1953229A (en) * | 2006-10-31 | 2007-04-25 | 中国科学院上海微系统与信息技术研究所 | Germanium-titanium base memory material for phase transition memory and its manufacture method |
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| Publication number | Publication date |
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| KR20100119756A (en) | 2010-11-10 |
| WO2009093994A1 (en) | 2009-07-30 |
| JP5341107B2 (en) | 2013-11-13 |
| CN101910467A (en) | 2010-12-08 |
| JP2011512456A (en) | 2011-04-21 |
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