CN103789204A - Graphene sequencing device and manufacturing method thereof - Google Patents
Graphene sequencing device and manufacturing method thereof Download PDFInfo
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Abstract
The invention discloses a graphene sequencing device. The graphene sequencing device comprises an insulating layer on a substrate; a graphene nanoribbon disposed on the insulating layer and provided with a crystal boundary; a nanopore disposed in the graphene nanoribbon; and metal electrodes disposed in the graphene nanoribbon at the two sides of the nanopore, wherein the nanopore and the crystal boundary form a graphene electrode. According to the graphene sequencing device and a manufacturing method thereof, the manufacturing technology conditions are relatively simple, the two novel semicircle arc electrodes disposed at the two sides of the crystal boundary contribute to reducing influences caused by DNA molecular structure fluctuation and improving test stability and reliability. By utilization of current inhibition by the crystal boundary, the background current can be effectively reduced and the signal to noise ratio is increased. The thickness of a single layer of the graphene is only about 0.35 nm and is lower than the length of a DNA base, thus effectively increasing the NDA sequencing resolution.
Description
Technical field
The present invention relates to a kind of semiconducter device and manufacture method thereof, particularly relate to a kind of Graphene order-checking device and manufacture method thereof that uses polycrystalline graphite alkene crystal boundary.
Background technology
DNA as the medium recording of biometric storage genetic information most information of various biologies, in other words the embodiment of species diversity in molecular level is exactly the diversity of DNA.If first the genetic information that decoding DNA carries just must measure the sequence of DNA.DNA sequencing technology, as one of core technology of modern life science, has obtained development fast since 1977 " chemical cracking method " and " chain termination method " invention, however even to this day fast and accurately DNA sequencing remain a global difficult problem.Quick high-resolution DNA sequencing method develops faster and has vital effect for promotion modern life science.
As DNA tests technology of new generation, nanoporous order-checking is checked order possibility is provided for DNA is quick.Use the DNA sequencing technology of nanoporous mainly to comprise the Strength Changes and two kinds of modes of variation of measuring horizontal tunnelling current that use the ion(ic)current of measuring longitudinal (perpendicular to the direction on nanoporous surface).Relative merits are also obvious separately for these two kinds of modes, use the mode of longitudinal ion(ic)current because the restriction of the nanoporous degree of depth makes resolving power lower, and the method for horizontal tunnelling current is because cause complex process to having relatively high expectations of electrode.
Graphene has just been subject to showing great attention to of numerous scientific research personnel after within 2004, successfully being separated.Graphene is made up of by the carbon atom that is similar to cellular structural arrangement one deck, and thickness is only 0.35 nanometer, has good electric property, machinery and thermal characteristic, thereby be widely studied and be applied to multiple fields.The appearance of the method for CVD (chemical vapour deposition) growing graphene makes Graphene to study on a large scale and to apply.
Summary of the invention
The problems referred to above that order-checking exists for nanopore DNA, for example: low resolution, complicated process of preparation, to having a low resistance of DNA structure fluctuation etc., the present invention proposes a kind of device architecture and basic preparation technology of the DNA sequencing that uses polycrystalline single-layer graphene crystal boundary.
The invention provides a kind of Graphene order-checking device, comprising: be positioned at the insulation layer on substrate; Be positioned at the graphene nanobelt on insulation layer, there is crystal boundary; Be arranged in the nanoporous of graphene nanobelt, wherein nanoporous and crystal boundary form Graphene electrodes jointly; And be positioned at the metal electrode on the graphene nanobelt of nanoporous both sides.
Wherein, substrate comprises body Si, SOI, body germanium, GeOI, SiGe, Si:C, GaN, GaAs, InSb, InP.
Wherein, insulation layer comprises silicon oxide, silicon nitride, silicon oxynitride, quasi-diamond decolorizing carbon (DLC) and combination thereof.
Wherein, nanoporous is positioned at graphene nanobelt center.
Wherein, nanoporous is circle, ellipse, hyperbolical, olive shape, rectangle, fan-shaped, trapezoidal and combination.
Wherein, the crystal boundary direction of graphene nanobelt is different from the bearing of trend of graphene nanobelt.
Wherein, the aperture of nanoporous is 0.1～10nm.
A manufacture method for Graphene order-checking device, comprising: on substrate, form insulation layer; Form substrate opening at substrate back; In insulation layer, form the first nanoporous, expose substrate; On insulation layer, form graphene nano layer; In graphene nano layer, form the second nanoporous, until expose substrate; Patterned Graphene nanometer layer, forms the graphene nanobelt extending along first direction; On the graphene nanobelt of the first and/or second nanoporous both sides, form metal electrode.
Wherein, substrate comprises body Si, SOI, body germanium, GeOI, SiGe, Si:C, GaN, GaAs, InSb, InP.
Wherein, insulation layer comprises silicon oxide, silicon nitride, silicon oxynitride, quasi-diamond decolorizing carbon (DLC) and combination thereof.
Wherein, the first nanoporous is positioned at insulation layer center, and the second nanoporous is positioned at graphene nano layer center, and the second nanoporous is relative with the first nanoporous.
Wherein, nanoporous is semicircle, arc, part ellipse, part hyperbolical, crescent, rectangle, fan-shaped, trapezoidal and combination.
Wherein, the crystal boundary direction of graphene nanobelt is different from the bearing of trend of graphene nanobelt.
Wherein, crystal boundary is manually-injected current blocked border, or the naturally occurring crystal boundary of polycrystalline graphite alkene.
Wherein, adopt dry etching, ionic current impact, TEM high-energy electron to impact and form the first and/or second nanoporous.
Wherein, formation the first nanoporous, graphene nano layer to the processing step that forms the second nanoporous replace with: on substrate, form insulation layer and graphene nano layer; Etching graphene nano layer and insulation layer successively, forms respectively the second nanoporous and the first nanoporous.
Wherein, the aperture of the first nanoporous and/or the second nanoporous is 0.1～10nm.
The step that forms substrate opening further comprises: thinning back side substrate; Anisotropic etch substrate back, forms substrate opening.
According to Graphene order-checking device of the present invention and manufacture method thereof, preparation process condition is relatively simple, two semicircular arc electrodes that are distributed in crystal boundary both sides of exploitation of innovation type contribute to reduce the impact producing due to DNA molecular structural fluctuation, improve stability and the reliability of test.In addition the size of utilizing crystal boundary can effectively reduce background current to the restraining effect of electric current improves signal to noise ratio.The thickness of single-layer graphene is only about the length of 0.35nm lower than a DNA base, can effectively improve the resolving power of DNA sequencing.
Accompanying drawing explanation
Describe technical scheme of the present invention in detail referring to accompanying drawing, wherein:
Figure 1A and Figure 1B have shown respectively top view and the sectional view according to Graphene order-checking device of the present invention; And
Fig. 2 to Fig. 6 is the sectional view according to the each step of Graphene order-checking device making method of the present invention.
Embodiment
Also describe feature and the technique effect thereof of technical solution of the present invention referring to accompanying drawing in conjunction with schematic embodiment in detail, disclose and can effectively improve the stability of NDA order-checking and Graphene order-checking device and the manufacture method thereof of resolving power.It is pointed out that structure like similar Reference numeral representation class, term " first " used in the application, " second ", " on ", D score etc. can be used for modifying various device architectures or processing step.These modify the space, order or the hierarchical relationship that not imply unless stated otherwise institute's modification device architecture or processing step.
Be the top view according to Graphene order-checking device of the present invention as shown in Figure 1A, Figure 1B is the sectional view that Figure 1A edge is parallel to the direction of graphene nanobelt.
Graphene order-checking device comprises the pair of electrodes 5 on the graphene nanobelt 3 of nanoporous 4 in graphene nanobelt 3, the graphene nanobelt 3 (and insulation layer 2) on insulation layer 2, the insulation layer 2 on substrate 1, substrate 1, nanoporous 4 both sides.Wherein, nanoporous 4 through graphene nanobelt 3 and insulation layer 2 until expose substrate 1.Crystal boundary 6 in graphene nanobelt 3 can be along " up and down " direction on paper in Figure 1A, also perpendicular to extension (length) direction of graphene nanobelt 3, can be the second direction that is different from graphene nanobelt 3 bearing of trends in addition, for example crossing with its inclination.Nanoporous 4 and crystal boundary 6 are divided into graphene nanobelt 3 two parts in left and right jointly, and also referred to as Graphene electrodes, its shape is preferably circular arc.
Between two electrodes 5, add a DC offset voltage, in the time that a DNA molecular strand (not shown) passes through nanoporous 4, change because the structure difference of different bases causes the electric current of 5, two electrode, thus the sequence of reading DNA.
Fig. 2 to Fig. 6 is according to the sectional view of the each step of Graphene order-checking device making method of the present invention, wherein analyses and observe along the direction that is parallel to graphene nanobelt in Figure 1A.
As shown in Figure 2, on substrate 1, form insulation layer 2.Substrate 1 is provided, and its material can be various conventional semiconducter substrate 1 materials such as body Si, SOI, body germanium, GeOI, SiGe, Si:C, GaN, GaAs, InSb, InP.Preferably, for reduce manufacturing cost and with main flow IC manufacturing process compatibility, adopt single crystal Si or SOI as substrate 1.Preferably, substrate 1 for example has the crystal orientation of (100), is also that the upper and lower surface of substrate 1 is (100) crystal face.The upper insulation layer 2 that forms in the front of substrate 1 (upper surface), its material is for example silicon oxide, silicon nitride, silicon oxynitride, quasi-diamond decolorizing carbon (DLC) etc. and combination thereof, array mode comprises and mixing, stacked, block etc.According to material difference, the technology mode that forms insulation layer 2 can comprise LPCVD, PECVD, HDPCVD, MBE, ALD, thermooxidizing, chemical oxidation (for example immersing in deionized water ozoniferous), evaporation, sputter.Need according to electrology characteristic, the thickness of insulation layer 2 is for example 1～100nm, and preferred 10nm.
Preferably, as shown in Figure 3, the back side of attenuate substrate 1.Can adopt cmp planarization processing, or wet etching, from thinning back side substrate 1, make its thickness reach making order-checking device required.Further preferably, after attenuate substrate, carry out anisotropic corrosion for substrate 1 back side, make the crystal orientation at substrate 1 back side be different from front.For example, for the substrate of Si material, adopt Tetramethylammonium hydroxide (TMAH) corrosion substrate 1 back side, because TMAH erosion rate in (111) crystal plane direction is low, final etch stops at (111) crystal face, and the back side that is also substrate 1 is (111) crystal face.Now, control etching process and mask position, can make substrate 1 back side centre portions form opening 1A, its shape can be rectangle, trapezoidal, inverted trapezoidal, V-type etc. and combination thereof, and preferably up-narrow and down-wide trapezoidal.The size of opening 1A needn't be as shown in FIG., can be greater than the nanoporous 4 that will form after a while, is also that width can be 1～1000nm, preferably 1～100nm.
As shown in Figure 4, in insulation layer 2, form the first nanoporous 4A.Adopt the techniques such as dry etching, ionic current impact, the impact of TEM high-energy electron, in insulation layer 2, form the first nanoporous 4A, expose the front of substrate 1.The aperture of the first nanoporous 4A is 0.1～10nm.Although nanoporous shown in figure is only one and is positioned at insulation layer center (1 backside openings 1A is relative with substrate), but in fact nanoporous can be to be distributed in insulation layer center neighbouring multiple nanoporouss, nanohole array, to be applicable to different DNA (and possible RNA) order-checking needs.
As shown in Figure 5, on insulation layer 2, form graphene nanobelt 3, and form nanoporous 4.By CVD technique, for example LPCVD, PECVD, HDPCVD, MOCVD, UHVCVD etc. deposit graphene nano layer 3 on insulation layer 2, and for example 0.35nm only of its thickness, has good electric property, machinery and thermal characteristic.Graphene nano layer after deposition has covered insulation layer 2 (and first nanoporous 4A) completely.It should be noted that the parameter that can select depositing operation, making graphene nano layer is polycrystalline structure or the microlitic structure having along the crystal boundary of first direction.
Utilize subsequently mask to carry out photoetching/etching, above the first nanoporous 4A, (also corresponding to the position of graphene nano layer middle part, central authorities) forms the second nanoporous 4B, jointly forms the nanoporous 4 that exposes substrate 1 front.The second nanoporous 4B is the same with the first nanoporous 4A, can be also the array that multiple nanoporouss form, and is positioned at the center of layer 3.The aperture of the second nanoporous 4B can be less than or equal to the first nanoporous 4A, for example, be 0.2～4nm.The technique of etching the second nanoporous 4B is dry etching, and for example plasma etching, reactive ion etching can also be that ionic current impacts or TEM high-energy electron impacts.According to the material behavior of Graphene, preferably adopt oxygen plasma etching.In erosion process at the moment, the graphene nano layer of microlitic structure may polycrystallization, or the crystal boundary of the graphene nano layer of polycrystalline may expand, and improves signal to noise ratio thereby can suppress noise.
After this, adopt mask lithography/etching, form along the graphene nanobelt 3 of second direction, wherein second direction is different from first direction, can be vertical (direction that for example, in the top view of Fig. 1 graphene nanobelt 3 extends), also can be tilt crossing.Because the bearing of trend of graphene nanobelt 3 is different from crystal boundary 6, improve signal to noise ratio thereby therefore can utilize crystal boundary to suppress noise.
Now, nanoporous 4 and crystal boundary 6 are divided into graphene nanobelt 3 two of left and right part 3A and 3B jointly, in fact also can be called Graphene electrodes.Nanoporous 4 (4A and/or 4B) preferably has illustrated circle to make isotropy, can be also ellipse, hyperbolical, olive shape (regions between two bending in opposite directions arcs), rectangle, fan-shaped, trapezoidal etc. and combination in addition.Therefore, therefore the junction surface of Graphene electrodes also has corresponding circle or above-mentioned other shapes, and electric current is uniformly distributed as far as possible.
In addition, thereby improving signal to noise ratio in order to utilize crystal boundary to suppress noise, also can artificially introduce current blocked border 6, for example, is that Selective implantation adulterates to change distribution of current or local plasma bombardment processes to increase current blocked structure.
It should be noted that, although Fig. 4, 5 show be the first nanoporous 4A first forming in insulation layer 2, then form the second nanoporous 4B in graphene nanobelt 3, in fact also can form simultaneously, also: formation of deposits insulation layer 2 successively on substrate 1, graphene nanobelt 3, then etching or impact form nanoporous 4, etching process can be the nanoporous 4 that a step etching/impact forms upper and lower consistent size, also can be to adjust the processing parameter of etching/impact to make the upper and lower size of nanoporous inconsistent and form equally first nanoporous 4A/ the second nanoporous 4B.
As shown in Figure 6, on the graphene nanobelt 3 of nanoporous 4 both sides, form pair of electrodes 5.By methods such as evaporation, sputter, MOCVD, MBE, ALD, form electrode 5, its material is for example metal simple-substance or the alloy of these metals and the nitride of these metals such as Co, Ni, Cu, Al, Pd, Pt, Ru, Re, Mo, Ta, Ti, Hf, Zr, W, Ir, Eu, Nd, Er, La.Wherein, preferably shape, measure-alike and about nanoporous 4 symmetries of left and right electrode.
According to Graphene order-checking device of the present invention and manufacture method thereof, preparation process condition is relatively simple, two semicircular arc electrodes that are distributed in crystal boundary both sides of exploitation of innovation type contribute to reduce the impact producing due to DNA molecular structural fluctuation, improve stability and the reliability of test.In addition the size of utilizing crystal boundary can effectively reduce background current to the restraining effect of electric current improves signal to noise ratio.The thickness of single-layer graphene is only about the length of 0.35nm lower than a DNA base, can effectively improve the resolving power of DNA sequencing.
Although with reference to one or more exemplary embodiments explanation the present invention, those skilled in the art can know without departing from the scope of the invention device architecture and/or technical process are made to various suitable changes and equivalents.In addition, can make and manyly may be suitable for the modification of particular condition or material and not depart from the scope of the invention by disclosed instruction.Therefore, object of the present invention does not lie in and is limited to as the disclosed specific embodiment for realizing preferred forms of the present invention, and disclosed device architecture and manufacture method thereof will comprise all embodiment that fall in the scope of the invention.
Claims (18)
1. a Graphene order-checking device, comprising:
Be positioned at the insulation layer on substrate;
Be positioned at the graphene nanobelt on insulation layer, there is crystal boundary;
Be arranged in the nanoporous of graphene nanobelt, wherein nanoporous and crystal boundary form Graphene electrodes jointly; And
Be positioned at the metal electrode on the graphene nanobelt of nanoporous both sides.
2. Graphene order-checking device as claimed in claim 1, wherein, substrate comprises body Si, SOI, body germanium, GeOI, SiGe, Si:C, GaN, GaAs, InSb, InP.
3. Graphene order-checking device as claimed in claim 1, wherein, insulation layer comprises silicon oxide, silicon nitride, silicon oxynitride, quasi-diamond decolorizing carbon (DLC) and combination thereof.
4. Graphene order-checking device as claimed in claim 1, wherein, nanoporous is positioned at graphene nanobelt center.
5. Graphene order-checking device as claimed in claim 1, wherein, nanoporous is circle, ellipse, hyperbolical, olive shape, rectangle, fan-shaped, trapezoidal and combination.
6. Graphene order-checking device as claimed in claim 1, wherein, the crystal boundary direction of graphene nanobelt is different from the bearing of trend of graphene nanobelt.
7. Graphene order-checking device as claimed in claim 1, wherein, the aperture of nanoporous is 0.1～10nm.
8. a manufacture method for Graphene order-checking device, comprising:
On substrate, form insulation layer;
Form substrate opening at substrate back;
In insulation layer, form the first nanoporous, expose substrate;
On insulation layer, form graphene nano layer;
In graphene nano layer, form the second nanoporous, until expose substrate;
Patterned Graphene nanometer layer, forms the graphene nanobelt extending along first direction;
On the graphene nanobelt of the first and/or second nanoporous both sides, form metal electrode.
9. the manufacture method of Graphene order-checking device as claimed in claim 8, wherein, substrate comprises body Si, SOI, body germanium, GeOI, SiGe, Si:C, GaN, GaAs, InSb, InP.
10. the manufacture method of Graphene order-checking device as claimed in claim 8, wherein, insulation layer comprises silicon oxide, silicon nitride, silicon oxynitride, quasi-diamond decolorizing carbon (DLC) and combination thereof.
The manufacture method of 11. Graphene order-checking devices as claimed in claim 8, wherein, the first nanoporous is positioned at insulation layer center, and the second nanoporous is positioned at graphene nano layer center, and the second nanoporous is relative with the first nanoporous.
The manufacture method of 12. Graphene order-checking devices as claimed in claim 8, wherein, nanoporous is circle, ellipse, hyperbolical, olive shape, rectangle, fan-shaped, trapezoidal and combination.
The manufacture method of 13. Graphene order-checking devices as claimed in claim 8, wherein, the crystal boundary direction of graphene nanobelt is different from the bearing of trend of graphene nanobelt.
The manufacture method of 14. order-checking of the Graphene as claim 13 devices, wherein, crystal boundary is manually-injected current blocked border, or the naturally occurring crystal boundary of polycrystalline graphite alkene.
The manufacture method of 15. Graphene order-checking devices as claimed in claim 8, wherein, adopts dry etching, ionic current impact, TEM high-energy electron to impact and forms the first and/or second nanoporous.
The manufacture method of 16. Graphene order-checking devices as claimed in claim 8, wherein, formation the first nanoporous, graphene nano layer to the processing step that forms the second nanoporous replace with: on substrate, form insulation layer and graphene nano layer; Etching graphene nano layer and insulation layer successively, forms respectively the second nanoporous and the first nanoporous.
The manufacture method of 17. Graphene order-checking devices as claimed in claim 8, wherein, the aperture of the first nanoporous and/or the second nanoporous is 0.1～10nm.
The manufacture method of 18. Graphene order-checking devices as claimed in claim 8, wherein, the step that forms substrate opening further comprises: thinning back side substrate; Anisotropic etch substrate back, forms substrate opening.
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| CN112041261B (en) * | 2018-05-08 | 2024-07-09 | 罗伯特·博世有限公司 | Method for producing a sequencing unit for sequencing biochemical material and sequencing unit |
| CN114262660A (en) * | 2021-12-21 | 2022-04-01 | 上海天马微电子有限公司 | Gene sequencing panel and manufacturing method thereof |
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