CN103178062A - Metal nanocrystalline storage - Google Patents
Metal nanocrystalline storage Download PDFInfo
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- CN103178062A CN103178062A CN2011104296082A CN201110429608A CN103178062A CN 103178062 A CN103178062 A CN 103178062A CN 2011104296082 A CN2011104296082 A CN 2011104296082A CN 201110429608 A CN201110429608 A CN 201110429608A CN 103178062 A CN103178062 A CN 103178062A
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Abstract
The invention discloses a metal nanocrystalline storage which comprises a substrate, a source terminal, a drain terminal, a tunneling dielectric layer, a metal nanocrystalline storage layer, a charge blocking layer and a grid electrode, wherein the source terminal and the drain terminal are formed on two sides of a channel region of the substrate, and the tunneling dielectric layer, the metal nanocrystalline storage layer, the charge blocking layer and the grid electrode are sequentially formed on the channel region of the substrate; and the metal nanocrystalline storage layer is formed by depositing metal nanocrystalline colloid on the tunneling medium layer in a spraying method and evaporating solvent in the metal nanocrystalline colloid. The metal nanocrystalline storage is achieved on the basis of a laser etching and spray gun spraying method, and has the advantages of being low in cost, controllable in diameter of the nanometer particles, good in uniformity, free of pollution, excellent in device performance and the like compared with a regularly manufactured nanocrystalline floating gate non-volatile storage.
Description
Technical field
The present invention relates to microelectronic industry memory technology field, relate in particular to a kind of metallic nano crystal memory.
Background technology
Present microelectronic product mainly is divided into logical device and the large class of memory device two, and memory device occupies very important status at microelectronic.Memory device generally can be divided into volatile storage and nonvolatile memory.The main feature of non-volatility memorizer is in the situation that do not power up also and can keep for a long time canned data.The characteristics of its existing read-only memory have again very high access speed, and are easy to wipe and rewrite, and power consumption is less.Along with the needs to large capacity, low-power consumption storage such as multimedia application, mobile communication, non-volatility memorizer, flash memory (Flash) particularly, the market share of shared semiconductor device becomes increasing, also more and more becomes a kind of considerable type of memory.For these memories, how to improve performance and to simplify technique by adjusting structural material, effectively controlling process costs is problem anxious to be resolved.Flash memory take nano-crystal memory as representative namely has the advantage of this respect.
The composition core of traditional flash memory is based on the silica-based non-volatility memorizer of polysilicon membrane floating gate structure.But the polysilicon membrane floating-gate device has, and manufacturing process is more complicated, the write time long, write the shortcomings such as power consumption is larger.And along with the continuous reduction of technology node, the device tunneling medium layer is also more and more thinner, and this makes the charge leakage problem of device be on the rise.This is that the place's defective on tunnel oxide namely can form fatal discharge channel and make component failure because for traditional polysilicon membrane floating gate structure memory.In order to address this problem, charge trapping memory is suggested.Utilize the characteristic of electric charge localization storage in capture layer, charge trapping memory is realized discrete charge storage, and the defective on tunneling medium layer only can cause local charge leakage, makes like this electric charge keep more stable.Wherein nano-crystal memory is owing to possessing the thinner tunnel oxide of use, lower program/erase (P/E) voltage, the advantage of P/E speed, stronger data retention characteristics (retention) etc. has caused scientific circles, the very big concern of industrial circle faster.Introduce simultaneously hafnium and can effectively solve as tunneling medium layer and electric charge barrier layer the compromise problem that data keep and height is erasable.Because employing high-K gate dielectric, under guarantor unit's gate capacitance permanence condition, the physical thickness of gate dielectric layer will be higher than the physical thickness of traditional material (as silicon dioxide, silicon nitride), thereby can effectively solve grid leakage current problem and keep high program erase speed.Adopt the trap of nanocrystalline material to capture the demand that memory can satisfy high-performance memory, obtained research widely.Simultaneously, metallic nano crystal is with Si or Ge is nanocrystalline compares, and has larger advantage, and therefore near as adjustable in work function, the density of states is very high Fermi level, perturbation is little etc. be subject to the extensive concern of industrial circle and scientific research circle.
The preparation nano-crystal memory, wherein critical process is the preparation of nano-crystal film.Its preparation method is varied, mainly comprises following several: the method for (1) Implantation forms nano-crystalline granule; (2) method of rapid thermal annealing forms nano-crystalline granule; (3) method of CVD direct growth prepares nano-crystalline granule.
In realizing process of the present invention, the applicant recognizes that there is following technological deficiency in prior art metallic nano crystal memory spare: the metallic nano crystal particle diameter is larger, and lack of homogeneity has a strong impact on the memory property of floating-gate memory.
Summary of the invention
The technical problem that (one) will solve
For solving above-mentioned one or more problems, the invention provides a kind of preparation method of metallic nano crystal memory, to improve the quality of metal nano crystal layer, reduce process complexity and the cost of preparation metallic nano crystal memory.
(2) technical scheme
According to an aspect of the present invention, provide a kind of metallic nano crystal memory.This metallic nano crystal memory comprises: substrate; Be formed at source and the drain terminal of substrate channel region both sides; Reach the tunneling medium layer, metallic nano crystal accumulation layer, electric charge barrier layer and the gate electrode that are formed at successively the substrate channel region top; Wherein, this metallic nano crystal accumulation layer by the metallic nano crystal colloid through spraying method be deposited on tunneling medium layer and the nanocrystalline colloid of evaporated metal in solvent form.
(3) beneficial effect
As shown from the above technical solution, metallic nano crystal memory of the present invention has following beneficial effect:
(1) nano-crystal memory of the present invention combines nanocrystalline electric charge localization storage characteristics and the anti-leak characteristic of high-K gate dielectric;
(2) metallic nano crystal memory of the present invention, the method that is based on laser ablation, spray gun spraying realizes, with the preparation nanocrystalline floating gate non-vaporability memory of routine relatively, have with low cost, the nano particle diameter is controlled, good uniformity, the plurality of advantages such as pollution-free, device performance is good.
Description of drawings
Figure 1A is the generalized section of embodiment of the present invention metallic nano crystal memory;
Figure 1B is the three-dimensional structure schematic diagram of embodiment of the present invention nano-crystal memory;
Fig. 2 A is the schematic diagram of the NOR type array that is made of embodiment of the present invention nano-crystal memory;
Fig. 2 B is the schematic diagram of the array direction of NOR type shown in Fig. 2 A;
Fig. 3 A carries out after shallow isolating trough structural representation along A-A ' direction to substrate in embodiment of the present invention metallic nano crystal memory preparation method;
Fig. 3 B carries out after shallow isolating trough structural representation along B-B ' direction to substrate in embodiment of the present invention metallic nano crystal memory preparation method;
Fig. 4 A be in embodiment of the present invention metallic nano crystal memory preparation method after the high K tunneling medium layer of deposit along the structural representation of A-A ' direction;
Fig. 4 B be in embodiment of the present invention metallic nano crystal memory preparation method after the high K tunneling medium layer of deposit along the structural representation of B-B ' direction;
Fig. 5 A is the schematic diagram that in embodiment of the present invention metallic nano crystal memory preparation method, laser ablation method prepares metallic nano crystal colloid device;
Fig. 5 B is the schematic diagram of the nanocrystalline colloid of plated metal spray gun used in embodiment of the present invention metallic nano crystal memory preparation method;
Fig. 6 A is the structural representation that forms in embodiment of the present invention metallic nano crystal memory preparation method after the metallic nano crystal accumulation layer along A-A ' direction;
Fig. 6 B is the structural representation that forms in embodiment of the present invention metallic nano crystal memory preparation method after the metallic nano crystal accumulation layer along B-B ' direction;
Fig. 7 A be in embodiment of the present invention metallic nano crystal memory preparation method after the deposit electric charge barrier layer along the structural representation of A-A ' direction;
Fig. 7 B be in embodiment of the present invention metallic nano crystal memory preparation method after the deposit electric charge barrier layer along the structural representation of B-B ' direction;
Fig. 8 is the structural representation of A-A ' direction after over etching in embodiment of the present invention metallic nano crystal memory preparation method;
Fig. 9 A be in embodiment of the present invention metallic nano crystal memory preparation method after the deposition grid along the structural representation of A-A ' direction;
Fig. 9 B be in embodiment of the present invention metallic nano crystal memory preparation method after the deposition grid along the structural representation of B-B ' direction;
Figure 10 carries out after etching structural representation along B-B ' direction along B-B ' direction in embodiment of the present invention metallic nano crystal memory preparation method;
Figure 11 is the structural representation that forms in embodiment of the present invention metallic nano crystal memory preparation method after source and drain terminal along B-B ' direction.
Embodiment
For making the purpose, technical solutions and advantages of the present invention clearer, below in conjunction with specific embodiment, and with reference to accompanying drawing, the present invention is described in more detail.Although this paper can provide the demonstration of the parameter that comprises particular value, should be appreciated that, parameter need not definitely to equal corresponding value, but can be similar to described value in acceptable error margin or design constraint.
In one exemplary embodiment of the present invention, provide a kind of metallic nano crystal memory.Figure 1A is the generalized section of embodiment of the present invention metallic nano crystal memory.Figure 1B is the three-dimensional structure schematic diagram of embodiment of the present invention nano-crystal memory.As shown in Figure 1A and Figure 1B, the present embodiment metallic nano crystal memory comprises: substrate 101; Be formed at source 102 and the drain terminal 103 of substrate channel region both sides; Be formed at the tunneling medium layer 104 of substrate channel region top; Be formed at the metallic nano crystal accumulation layer 105 of tunneling medium layer 104 tops; Be formed at the electric charge barrier layer 106 of metallic nano crystal accumulation layer 105 tops; And be formed at the gate electrode 107 of electric charge barrier layer 106 tops.Wherein, this metallic nano crystal accumulation layer be by the metallic nano crystal colloid through spraying method be deposited on tunneling medium layer 104 and the nanocrystalline colloid of evaporated metal in solvent after remaining metal nanoparticle form.And this metallic nano crystal colloid is that the mode by laser ablation produces.
In the present embodiment, metallic nano crystal accumulation layer 105 is preferably individual layer, and its granular size (is decided by process conditions) between 2～15nm, and material has the metal material of larger work function for gold (Au), silver (Ag), platinum (Pt) etc.
In the present embodiment, the material of gate electrode can be chosen precious metal platinum (Pt), silver (Ag), palladium (Pd); Tungsten (W), titanium (Ti), aluminium (Al), the copper (Cu) commonly used in CMOS technique; Metal oxide ITO (tin indium oxide), IZO (indium zinc oxide) etc. and polycrystalline silicon material.
In the present embodiment, tunneling medium layer and electric charge barrier layer are all hafnium, namely have the material of high-k, and its dielectric constant is generally higher than silicon nitride (Si
3N
4), as hafnium oxide (HfO
2), aluminium oxide (Al
2O
3) or other have the material of similarity or stacking (as HfO by multilayer material
2/ Al
2O
3Double-deck).
In the present embodiment, metallic nano crystal memory has fully utilized the electric charge localization storage characteristics of metallic nano crystal and the anti-leak characteristic of high-K gate dielectric, can greatly promote the memory property of metallic nano crystal memory.Especially, in the present embodiment, the metallic nano crystal accumulation layer is deposited on tunneling medium layer through spraying method by the metallic nano crystal colloid, its nano particle diameter is controlled, good uniformity without chemical contamination, can further promote the performance of metallic nano crystal memory.
In another exemplary embodiment of the present invention, also provide a kind of method for preparing above-mentioned metallic nano crystal memory.For convenience of explanation, at first the direction on substrate is stipulated.
Fig. 2 A is the schematic diagram of the NOR type array that is made of embodiment of the present invention nano-crystal memory.As shown in Fig. 2 A, be connected to bit line with the drain terminal of the nano-crystal memory of delegation; The grid end of the nano-crystal memory of same row is connected to the word line, and its source is connected to source electrode line (SL).Need to prove, the NOR type array structure shown in Fig. 2 A is identical with NOR array structure of the prior art, is not described in detail herein.
Fig. 2 B is the schematic diagram of the array direction of NOR type shown in Fig. 2 A.As shown in Fig. 2 B, the word-line direction (WL) of the corresponding NOR type of A-A ' direction array, the bit line direction of the corresponding NOR type of B-B ' direction array.Direction below in conjunction with Fig. 2 B defined is elaborated to the present embodiment.Embodiment of the present invention metallic nano crystal memory is the preparation method comprise:
Step S302 carries out Implantation and short annealing (being used for adjusting the doping concentration distribution of substrate) to substrate; Deposited sacrificial oxide layer (for the injury of the injection effects on surface that prevents next step), and carry out threshold value adjustment injection and prevent the break-through injection after deposited oxide layer on described substrate.
In this step, substrate is preferably silicon substrate, can also be the germanium substrate.Implantation is the step that all will carry out except the place of shallow isolating trough substrate surface, after Implantation, also to carry out short annealing, its objective is to make uniform ion be entrained in substrate surface, the temperature of short annealing is roughly 500～1000 ℃ and does not wait, and is relevant with the Implantation metering.
Step S304: form shallow isolating trough (Shallow Trench Isolation is called for short STI) on substrate, as shown in Fig. 3 A and Fig. 3 B;
Wherein, Fig. 3 A carries out after shallow isolating trough structural representation along A-A ' direction to substrate in embodiment of the present invention metallic nano crystal memory preparation method.Fig. 3 B carries out after shallow isolating trough structural representation along B-B ' direction to substrate in embodiment of the present invention metallic nano crystal memory preparation method.In Fig. 3 A and Fig. 3 B, 301 is shallow isolating trough, and 303 and 302 are respectively the threshold value adjustment injects and prevents the break-through injection, and 304 is sacrificial oxide layer.
Step S306: remove sacrificial oxide layer 304, the high K tunneling medium layer 104 of deposit is as shown in Fig. 4 A and Fig. 4 B;
Wherein, Fig. 4 A be in embodiment of the present invention metallic nano crystal memory preparation method after the high K tunneling medium layer of deposit along the structural representation of A-A ' direction.Fig. 4 B be in embodiment of the present invention metallic nano crystal memory preparation method after the high K tunneling medium layer of deposit along the structural representation of B-B ' direction.
In this step, tunneling medium layer and electric charge barrier layer are all hafnium, namely have the material of high-k, and its dielectric constant is generally higher than silicon nitride Si
3N
4, as hafnium oxide (HfO
2), aluminium oxide (Al
2O
3), titanium oxide, zirconia, hafnium alumina, hafnium oxynitride or other have the material of similarity or stacking (as HfO by multilayer material
2/ Al
2O
3Bilayer) has the structure of similarity.
Step S308, utilize spray gun with metallic nano crystal colloid jet deposition on tunneling medium layer;
In this step, in the metallic nano crystal colloid, metal material has the metal material of larger work function for gold (Au), silver (Ag), platinum (Pt) etc.The granular size of metal material is between 2～15nm.
Fig. 5 A is the ablation index path that in embodiment of the present invention metallic nano crystal memory preparation method, laser ablation method prepares the metallic nano crystal colloid.This ablation light path comprises: laser b01, attenuator b02, power detector b03, convex lens b04, total reflective mirror b05; Cuvette b06.Laser power detector b03 and attenuator b02 are set in the ablation light path, are used for the power of monitoring and adjusting laser.Cuvette b06 is used for placing aqueous solvent and metal targets.Particularly, metal targets b07 and solvent b08 all are placed in cuvette b06, laser is radiated in metal targets in cuvette by completely reflecting mirror after by convex lens focus again, metallic atom or atomic group effusion metal targets surface formation nano-crystalline granule, this metallic nano crystal forms colloid in solvent b08.
Herein, the present embodiment solvent b08 adopts aqueous solvent, add therein lauryl sodium sulfate (SDS) or to four-(4-N-picoline) porphyrin (H2TMPyP) as activating agent.Certainly, solvent b08 also can take organic solvent, such as acetonitrile (CH3CN) etc., in the situation that adopt organic solvent, has not just needed activating agent.In addition, specific metal may need different surfactants, but more than the metal material with larger work function carried can meet the demands fully with aqueous solvent and SDS activating agent, and adopt the aqueous solution also to have advantages of conveniently to shift, the saving cost.Adopt the laser ablation preparation nanocrystalline to have uniform particles good, without advantages such as chemical contaminations, in addition, in specific operation process, can regulate speed and the size that nano particle produces by power and the wavelength of adjusting laser.
Take preparation silver nanoparticle crystalline substance as example, the frequency doubled light 532nm that uses the Nd:YAG laser to produce, pulsewidth 10ns, repetition rate 10Hz.Be used for monitoring power by attenuator to regulate light intensity and to tell 40%.The ablation light beam focuses on the metallic target that is immersed in the aqueous solution through the 150mm quartz lens; Laser ablation out silver nano-grain, will be melted in the aqueous solution and to form the brilliant colloid of silver nanoparticle.
Metallic nano crystal colloid in cuvette b06 is transferred in the sample cavity c01 of above-mentioned spray gun by glue head dropper or little measuring cup.
Fig. 5 B is the schematic diagram of the nanocrystalline colloid of plated metal spray gun used in embodiment of the present invention metallic nano crystal memory preparation method.The spray gun that adopts in the present embodiment is the Richpen 112B type spray gun of Japanese Fuso Seiki Co., Ltd..The process of the nanocrystalline colloid of plated metal comprises: the sample cavity c01 that at first the metallic nano crystal colloid of preparation packed into is positioned over the substrate that deposits tunneling medium layer on heating station c05; Passing into nitrogen (or inert gas) as protective gas by nitrogen inlet c02 and c03, is to complete under the protection atmosphere to guarantee whole process; Lance head c04 is injected in the nanocrystalline colloid in sample cavity c01 on the high temperature substrate that is positioned on heating station c05.For different materials, the parameter that spray gun arranges is different, take the brilliant colloid of silver nanoparticle as example, the temperature of heating station is 190 degrees centigrade, nitrogen pressure is 2bar, control last thickness by the flow button adjust flux on spray gun, preferred, the thickness of nanocrystalline accumulation layer is that one deck is nanocrystalline.
Step S210 makes the solvent evaporates in the metallic nano crystal colloid, and residual metallic is nanocrystalline in described tunneling medium layer surface formation metallic nano crystal accumulation layer 105, as shown in Fig. 6 A and Fig. 6 B;
Fig. 6 A is the structural representation that forms in embodiment of the present invention metallic nano crystal memory preparation method after the metallic nano crystal accumulation layer along A-A ' direction.Fig. 6 B is the structural representation that forms in embodiment of the present invention metallic nano crystal memory preparation method after the metallic nano crystal accumulation layer along B-B ' direction.
In this step, the moisture of metallic nano crystal colloid can be dried naturally, also the substrate of described spray deposited metallic nano crystal colloid under 190 degree, under blanket of nitrogen, can be dried 180 minutes in drying baker.Adopt drying baker, can save time, and the moisture little residue, be conducive to the realization of later steps.
Step S212, the electric charge barrier layer 106 of deposit high K dielectric on the metallic nano crystal accumulation layer is as shown in Fig. 7 A and Fig. 7 B;
Fig. 7 A be in embodiment of the present invention metallic nano crystal memory preparation method after the deposit electric charge barrier layer along the structural representation of A-A ' direction.Fig. 7 B be in embodiment of the present invention metallic nano crystal memory preparation method after the deposit electric charge barrier layer along the structural representation of B-B ' direction.
In this step, the material of electric charge barrier layer is similar to the material of above-mentioned tunneling medium layer, is not described in detail herein.
Step S212 along A-A ' direction etching, falls tunnel layer, nanocrystalline accumulation layer and barrier etch above shallow-trench isolation;
Fig. 8 is the structural representation of A-A ' direction after over etching in embodiment of the present invention metallic nano crystal memory preparation method.
Step S214, on the substrate after carrying out etching, deposition of gate material 107, as shown in Fig. 9 A and 9B;
Fig. 9 A be in embodiment of the present invention metallic nano crystal memory preparation method after the deposition grid along the structural representation of A-A ' direction.Fig. 9 B be in embodiment of the present invention metallic nano crystal memory preparation method after the deposition grid along the structural representation of B-B ' direction.
In this step, wherein grid is polysilicon, metal, metal silicide or by the stacking structure with similarity of multilayer material.
Step S216 carries out etching along B-B ' direction on the substrate after the deposition grid, etch away tunnel layer, nanocrystalline accumulation layer, barrier layer and the gate material layers of substrate top, forms grid 107, as shown in figure 10;
Figure 10 carries out after etching structural representation along B-B ' direction along B-B ' direction in embodiment of the present invention metallic nano crystal memory preparation method.
Step S218, and on the silicon substrate that etching is exposed (B-B ' direction) enter to form source and drain terminal, as shown in figure 11;
Figure 11 is the structural representation that forms in embodiment of the present invention metallic nano crystal memory preparation method after source and drain terminal along B-B ' direction.In Figure 11,102 is the drain doping region opposite with the channel region doping type, and 103 is the source doping region opposite with the channel region doping type, and source electrode is public communicating along A-A ' direction, form common source (common source) structure, a03 is anti-break-through injection region, and a04 is side wall.
Step S220 makes metal electrode, draws bit line and word line by drain doping region and gate regions respectively, forms the nonvolatile memory array.Wherein, electrode material can be metal, polysilicon, metallicity oxide, the materials such as silicide.
In sum, nano-crystal memory of the present invention has fully utilized nanocrystalline electric charge localization storage characteristics and the anti-leak characteristic of high-K gate dielectric, and the comprehensive memory property of metallic nano crystal memory can be provided.Further, nano-crystal memory provided by the invention, the method that is based on laser ablation, spray gun spraying realizes, compare with the preparation nanocrystalline floating gate non-vaporability memory of routine, have with low cost, the nano particle diameter is controlled, good uniformity, the plurality of advantages such as pollution-free, device performance is good.
Above-described specific embodiment; purpose of the present invention, technical scheme and beneficial effect are further described; institute is understood that; the above is only specific embodiments of the invention; be not limited to the present invention; within the spirit and principles in the present invention all, any modification of making, be equal to replacement, improvement etc., within all should being included in protection scope of the present invention.
Claims (8)
1. a metallic nano crystal memory, is characterized in that, comprising:
Substrate;
Be formed at source and the drain terminal of substrate channel region both sides; And
Be formed at successively tunneling medium layer, metallic nano crystal accumulation layer, electric charge barrier layer and the gate electrode of substrate channel region top;
Wherein, described metallic nano crystal accumulation layer by the metallic nano crystal colloid through spraying method be deposited on described tunneling medium layer and the nanocrystalline colloid of evaporated metal in solvent form.
2. nano-crystal memory according to claim 1, is characterized in that, described metal nano colloid is to utilize the laser ablation method preparation.
3. nano-crystal memory according to claim 1, is characterized in that, described metallic nano crystal accumulation layer is the single-layer metal nano-crystalline granule, and its granular size is between 2～15nm.
4. nano-crystal memory according to claim 3, is characterized in that, the material of described metallic nano crystal accumulation layer is the metal material of large work function.
5. nano-crystal memory according to claim 4, is characterized in that, the metal material of described large work function is gold, silver or platinum.
6. the described nano-crystal memory of any one according to claim 1 to 5, is characterized in that, it is characterized in that, the material of described tunneling medium layer and electric charge barrier layer is high dielectric constant material.
7. nano-crystal memory according to claim 6, is characterized in that, described high dielectric constant material is hafnium oxide, aluminium oxide or hafnium oxide/aluminium oxide double stacked.
8. the described nano-crystal memory of any one according to claim 1 to 5, is characterized in that, the material of described gate electrode is platinum, silver, palladium, tungsten, titanium, aluminium, copper, ITO, IZO or polycrystalline silicon material.
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| US20100196192A1 (en) * | 2009-01-30 | 2010-08-05 | Imra America, Inc. | Production of metal and metal-alloy nanoparticles with high repetition rate ultrafast pulsed laser ablation in liquids |
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| CN101512754A (en) * | 2006-07-28 | 2009-08-19 | 奈米系统股份有限公司 | Methods and devices for forming nanostructure monolayers and devices including such monolayers |
| CN200984643Y (en) * | 2006-12-19 | 2007-12-05 | 浙江工业大学 | Device for preparing metal nanometer particle colloid with pulse laser ablation in liquid phase |
| CN101020999A (en) * | 2007-03-23 | 2007-08-22 | 沈阳航空工业学院 | Planar reciprocating process and apparatus for spraying to deposit multilayer composite material |
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Application publication date: 20130626 |