CN101179108A - Non-volatile organic thin-film transistor memory based on floating gate structure and manufacturing method therefor - Google Patents
Non-volatile organic thin-film transistor memory based on floating gate structure and manufacturing method therefor Download PDFInfo
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- CN101179108A CN101179108A CNA2007101935285A CN200710193528A CN101179108A CN 101179108 A CN101179108 A CN 101179108A CN A2007101935285 A CNA2007101935285 A CN A2007101935285A CN 200710193528 A CN200710193528 A CN 200710193528A CN 101179108 A CN101179108 A CN 101179108A
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Abstract
The invention pertains to organic thin film transistorized memory based on floating gate structure. The manufacturing method adopts the top and bottom gate structures and the matched preparation process art respectively and introduces floating gate into medium layers between floating gate and control gate and realizes the nonvolatile memory of organic thin- film transistor. The invention has the advantages of simple process, low cost, small volume, low power dissipation and well stability.
Description
Technical field
The present invention relates to the non-volatile organic thin-film transistor memory and the manufacture method thereof of floating gate structure.
Background technology
Nonvolatile memory occupies extremely important status in current integrated circuit, field of storage.In all kinds of nonvolatile memories, inorganic transistors memory based on floating gate structure, it is so-called flash memory technology, in making a great contribution for the development of global IC industry over past ten years, also occupy the dominant position of field of storage gradually, be widely used in the stored memory of computer hard disc, portable hard drive, USB flash disk and each electronic product.
Organic electroluminescence device (OLED), OTFT (OTFT) have shown the huge glamour of organic semi-conductor with the invention in succession of organic solar batteries, have that the material range of choice is wide, manufacture craft is simple, cost is low, and easily realize plurality of advantages such as large tracts of land and flexible application, and form an emerging subject---organic electronic is learned.Recent two decades comes, and the continuous lifting of device performance has represented the potential huge commercial application prospect of organic electronic device gradually.At present, the research in organic semiconductor device field has been not limited to academia, nearly all internationally recognizable electronics major company and chemical company all drops into huge manpower and fund enters this research field presents the situation that research, exploitation and industrialization advance side by side.
At present, about the report of non-volatile organic thin-film transistor memory seldom, all be to adopt ferroelectric material to do gate insulation layer, and realize (nature material such as Na Boer, 4 phases, 243 pages stored with its polarization characteristic, 2004, R.C.G.Naber, C.Tanase, P.W.M.Blom.G.H.Gelinck, A.W.Marsman, F.J.Touwslager, S.Setayesh, and D.M.deleeuw, Nat.Mater 4,243 (2004); Si Keluode, this section of the horse rank of nobility, Ge Leier, advanced material, 16 phases, 633 pages,, R.Schroeder, L.A.Majewski and M.Grell.Adv.Mater.16,633 (2004) in 2004); Na Baier, bohr, Bai Lu admires, De Lu, Applied Physics wall bulletin, 87 phases, 203509,2005 years, R.C.G.Naber, B.de Boer, P.W.M.Blomand D.M.de Leeuw, Appl.Phys.Lett.87,203509 (2005)).And in current field of storage, occupy the flash memory technology of main flow, promptly the floating gate structure organic thin-film transistor memory yet there are no patent application and bibliographical information.
Summary of the invention
The present invention provides the non-volatile organic thin-film transistor memory and the manufacture method thereof of floating gate structure.Adopt floating gate structure to realize non-volatile organic thin-film transistor memory first.
OTFT is divided top grid and two kinds of structures of bottom gate, and the present invention is incorporated into the OTFT of these two kinds of structures respectively with floating gate structure, has realized non-volatile organic thin-film transistor memory.Fig. 1 and Fig. 2 implement a kind of structure of the non-volatile organic thin-film transistor memory based on floating gate structure of the present invention, but are not whole structures.
As shown in Figure 1, the top gate non-volatile organic thin-film transistor memory of floating gate structure provided by the invention, it be by: be between substrate 1, source-drain electrode layer 2, source-drain electrode layer 2 electrode that the channel region of device, organic semiconductor layer 3, floating gate dielectric layer 4, floating gate layer 5, control gate dielectric layer 6 and control grid electrode layer 7 constitute; On substrate 1, prepare layer of conductive film, and graphically form the source-drain electrode layer 2 of device, then successively in vacuum chamber evaporation prepare organic semiconductor layer 3, floating gate dielectric layer 4, floating gate layer 5, control gate dielectric layer 6 and control grid electrode layer 7;
Substrate 1 is glass or Merlon flexible substrate;
Source-drain electrode layer 2 adopts tin indium oxide (being called for short ITO), poly-dioxoethyl thiophene: poly-p styrene sulfonic acid (being called for short PEDOT:PSS), gold, silver, nickel, palladium, copper, platinum, aluminium or samarium;
Any in oligomerisation six thiophene that organic semiconductor layer 3 adopts and many benzene, phthalocyanine-like compound, carbon 60, carbon 70, Uniformpoly thiophene, the many benzene of connection, polythiophene, perfluoro metal phthalocyanine, naphthalene glycosides and derivative thereof or perfluoroalkyl replace;
Floating gate dielectric layer 4 adopts any in nylon 6, the poly-bright olefin(e) acid formicester of methyl (being called for short PMMA), Teflon, polyimides and derivative, calcirm-fluoride, lithium fluoride, cesium fluoride, barium fluoride, nickel oxide, aluminium oxide, silica or the titanium oxide insulating material;
Floating gate layer 5 adopts the material of following kind:
1. the metal of nanostructure: any in nickel, silver, aluminium, palladium, copper, gold, platinum or the samarium;
2. have any in the iron of magnetic or nickel and the oxide thereof;
3. Uniformpoly thiophene, and many benzene, join any in the oligomerisation six thiophene organic semiconducting materials that many benzene, polythiophene, phthalocyanine-like compound, carbon 60, carbon 70, perfluoro metal phthalocyanine, naphthalene glycosides and derivative thereof and perfluoroalkyl replace;
4. nano particle: any in calcirm-fluoride, lithium fluoride, cesium fluoride, barium fluoride, nickel oxide or the zinc oxide;
Control gate dielectric layer 6 adopts the insulating material identical with floating gate dielectric layer 4; For improving the composite bed that device performance can also adopt nylon 6/ calcirm-fluoride, nylon 6/ Teflon, calcirm-fluoride/Teflon, PMMA/ Teflon, PMMA/ calcirm-fluoride, nylon 6/ aluminium oxide, the multiple insulating material of PMMA/ aluminium oxide to form;
Control grid electrode layer 7 adopts any in tin indium oxides (being called for short ITO), PEDOT:PSS, gold, silver, nickel, palladium, copper, platinum, aluminium or the samarium.
When between gate electrode layer 7, source-drain electrode layer 2, applying operating voltage, can realize memory property based on the non-volatile organic thin-film transistor memory spare of floating gate structure.
The manufacture method of the top gate non-volatile organic thin-film transistor memory based on floating gate structure of the present invention as shown in Figure 1 is as follows:
Earlier the tin indium oxide on the substrate layer 1, PEDOT:PSS or metal conducting layer 2 are carried out photolithography patterning, prepare source-drain electrode layer 2, be the channel region of device between source-drain electrode layer 2 electrode, clean then, nitrogen dries up, and it is transferred in the vacuum coating system, treats that vacuum degree reaches 1 to 5 * 10
-4During handkerchief, on source-drain electrode layer 2, prepare organic semiconductor layer 3, floating gate dielectric layer 4, floating gate layer 5, control gate dielectric layer 6 and control grid electrode layer 7 successively;
Wherein channel length is 1～150 micron, 50～5000 microns of width; The thickness of organic semiconductor layer 3 is 50～100 nanometers; The thickness of floating gate dielectric layer 4 is 2～40 nanometers; The thickness of floating gate layer 5 is 2～40 nanometers; The thickness of control gate dielectric layer 6 is 100～800 nanometers; The thickness of control grid electrode layer 7 is 80～140 nanometers.
As shown in Figure 2, the bottom gate non-volatile organic thin-film transistor memory of floating gate structure provided by the invention, it is to be made of: substrate 1, control grid electrode layer 7, control gate dielectric layer 6, floating gate layer 5, floating gate dielectric layer 4, organic semiconductor layer 3 and source-drain electrode layer 2; Wherein, on substrate layer 1, prepare one deck conductive layer and carry out photolithography patterning and form control grid electrode layer 7, spin coating prepares control gate dielectric layer 6 on control grid electrode layer 7, evaporation nickel and aluminium film in vacuum chamber then, wherein the nickel film is taken on floating gate layer 5, adopt oxygen plasma technical finesse aluminium film to make its oxidation form floating gate dielectric layer 4, vacuum evaporation organic semiconductor layer 3 and source-drain electrode layer 2 once more are the channel region of device between source-drain electrode layer 2 electrode;
Substrate 1 is glass or Merlon flexible substrate;
Control grid electrode layer 7 adopts any in ITO, PEDOT:PSS, gold, silver, nickel, palladium, copper, platinum, aluminium or the samarium;
Control gate dielectric layer 6 adopts any in nylon 6, the poly-bright olefin(e) acid formicester of methyl, Teflon, polyimides and derivative, calcirm-fluoride, lithium fluoride, cesium fluoride, barium fluoride, nickel oxide, aluminium oxide, silica or the titanium oxide insulating material; For improving the composite bed that device performance can also adopt nylon 6/ calcirm-fluoride, nylon 6/ Teflon, calcirm-fluoride/Teflon, PMMA/ Teflon, PMMA/ calcirm-fluoride, nylon 6/ aluminium oxide, the multiple insulating material of PMMA/ aluminium oxide to form;
Floating gate layer 5 adopts the material of following kind:
1. the metal of nanostructure: any in nickel, silver, aluminium, palladium, copper, gold, platinum or the samarium;
2. have any in the iron of magnetic or nickel and the oxide thereof;
3. Uniformpoly thiophene, and many benzene, join any in the oligomerisation six thiophene organic semiconducting materials that many benzene, polythiophene, phthalocyanine-like compound, carbon 60, carbon 70, perfluoro metal phthalocyanine, naphthalene glycosides and derivative thereof and perfluoroalkyl replace;
4. nano particle: any in calcirm-fluoride, lithium fluoride, cesium fluoride, barium fluoride, nickel oxide or the zinc oxide;
Floating gate dielectric layer 4 adopts the insulating material identical with control gate dielectric layer 6:
Any in oligomerisation six thiophene that organic semiconductor layer 3 adopts and many benzene, phthalocyanine-like compound, carbon 60, carbon 70, Uniformpoly thiophene, the many benzene of connection, polythiophene, perfluoro metal phthalocyanine, naphthalene glycosides and derivative thereof or perfluoroalkyl replace;
Source-drain electrode layer 2 adopts any in ITO, PEDOT:PSS, gold, silver, nickel, palladium, copper, platinum, aluminium, the samarium; The composite bed that also can adopt calcium/aluminium, magnesium/aluminium or lithium fluoride/aluminium to form;
When between gate electrode layer 7, source-drain electrode layer 2, applying operating voltage, can realize memory property based on the bottom gate non-volatile organic thin-film transistor memory spare of floating gate structure.
The preparation method of the bottom gate non-volatile organic thin-film transistor memory based on floating gate structure of the present invention as shown in Figure 2 is as follows:
Earlier the tin indium oxide on the substrate layer 1, PEDOT:PSS or metal conducting layer 7 are carried out photolithography patterning and form control grid electrode layer 7, clean then, nitrogen dries up, spin coating PMMA prepares control gate dielectric layer 6 on control grid electrode layer 7, evaporation nickel and aluminium film in vacuum chamber then, wherein the nickel film is taken on floating gate layer 5, adopt oxygen plasma technical finesse aluminium film to make its oxidation form floating gate dielectric layer 4, vacuum evaporation organic semiconductor layer 3 and source-drain electrode layer 2 once more are the channel region of device between source-drain electrode layer 2 electrode;
Wherein device channel length is 20～100 microns, 500～2000 microns of width; The thickness of control grid electrode layer 7 is 40～100 nanometers; The thickness of control gate dielectric layer 6 is 200～800 nanometers; The thickness of floating gate layer 5 is 2～15 nanometers; The thickness of floating gate dielectric layer 4 is 2～40 nanometers; The thickness of organic semiconductor layer 3 is 50～100 nanometers; The thickness of source-drain electrode layer 2 is 60～100 nanometers.
Beneficial effect: advantage of the present invention is that floating gate structure is incorporated in the OTFT, makes device have good memory property.At normal temperatures and pressures, the device field-effect mobility of preparation reaches as high as 10
-1Cm
2/ Vs, the pulse of warp-15V writes the pulsed erase voltage of voltage or 10V, and reading under the voltage of-2V, device stores height current ratio is 5～20, calculates that its data hold time can reach 2 hours.
An advantage of the invention is the accurately trench size of control device and the thickness of organic semiconductor layer, floating gate dielectric layer, floating gate layer and control gate dielectric layer, and then can pass through reasonable structural design, reach regulation and control, good industrialization prospect is arranged device operating voltage and memory property.
Another advantage of the present invention be the prepared process of entire device can be in vacuum chamber disposable finishing, compare with the OTFT that great majority have been reported, this makes that device has reduced to help improving device performance because of process environments changes the probability that might cause contamination greatly in preparation process.
Description of drawings
Fig. 1 is based on the generalized section of the top grid organic thin-film transistor memory spare structure of floating gate structure.Fig. 1 also is a Figure of abstract.
Fig. 2 is based on the generalized section of the bottom gate organic thin-film transistor memory spare structure of floating gate structure.
Fig. 3 is the output characteristic curve of embodiment 1 under different gate voltages of the organic thin-film transistor memory spare based on floating gate structure of the present invention.Device has tangible field effect characteristic, and under 20 volts operating voltage, ON state current can reach 3.2 microamperes.
Fig. 4 is the transfer characteristic curve of organic thin-film transistor memory spare embodiment 1 under the different fixing source-drain voltage based on floating gate structure of the present invention.The device operation current on-off ratio can reach 10
3, tangible hesitation is arranged, the threshold voltage difference under the different scanning direction is obvious, and sluggish height current ratio is greater than 10.
Fig. 5 is the storage cycle characteristics curve of the organic thin-film transistor memory spare embodiment 1 based on floating gate structure of the present invention.Write through extra pulse with erasing voltage after, storaging current is than about 10 times, and can keep the long time.
Fig. 6 is of the present invention based on the storage data retention characteristic curve among the organic thin-film transistor memory spare embodiment 1 of floating gate structure.Through about 10 seconds write or erasing voltage after, " 1 " of storage or " 0 " attitude data can keep the long time.
Fig. 7 is the transfer characteristic curve of organic thin-film transistor memory spare embodiment 2 under the different fixing source-drain voltage based on floating gate structure of the present invention.Device operation current on-off ratio～10
2, tangible hesitation is arranged, the threshold voltage difference under the different scanning direction is obvious, about 50 times of sluggish height current ratio.
Fig. 8 is the storage cycle characteristics curve of the organic thin-film transistor memory spare embodiment 2 based on floating gate structure of the present invention.Write through extra pulse with erasing voltage after, storaging current is than about 3 times.
Fig. 9 is of the present invention based on the storage data retention characteristic curve among the organic thin-film transistor memory spare embodiment 1 of floating gate structure.Through about 10 seconds write or erasing voltage after, " 1 " of storage or " 0 " attitude data can keep the long time.Illustration is " 1 " and " 0 " data ratio multiple function in time.
Embodiment
Embodiment 1:
Earlier the tin indium oxide on the indium oxide tin glass is photo-etched into the electrode (being source-drain electrode) of two 10 millimeters long, 1 mm wide (being channel width), spacing between electrodes is 20 microns (being channel length); Clean then, nitrogen dries up.In vacuum degree is 1 to 5 * 10
-4In the coating system of handkerchief, the Teflon of nylon 6,150 nanometer thickness of the nickel of nylon 6,8 nanometer thickness of the pentacene of evaporation 70 nanometer thickness, 25 nanometer thickness, 200 nanometer thickness successively on the tin indium oxide source-drain electrode, and give graphically by mask plate, the width that is 100 nanometer thickness at last is 1 millimeter a aluminum strip, gives graphically by another mask plate.The pentacene thin film growth rate is controlled at 0.05 nanometer per second, and the nickel film growth rate is controlled at 0.02 nanometer per second, and nylon 6 is controlled at 0.1 nanometer per second with the growth rate of Teflon.Accompanying drawing 3 has provided the output characteristic curve of organic thin-film transistor memory spare under different gate voltages based on floating gate structure.Device has tangible field effect characteristic, and under 20 volts operating voltage, ON state current can reach 3.2 microamperes.Accompanying drawing 4 has provided the transfer characteristic curve of organic thin-film transistor memory spare under the different fixing source-drain voltage based on floating gate structure.The device operation current on-off ratio can reach 10
3, tangible hesitation is arranged, the threshold voltage difference under the different scanning direction is obvious, and sluggish height current ratio is greater than 10.The field-effect mobility that calculating can get device is about 10
-2～10
-1Cm
2/ Vs.Accompanying drawing 5 is storage cycle characteristics curves of the organic thin-film transistor memory spare based on floating gate structure of the present invention.Accompanying drawing 6 is based on the storage data retention characteristic curve of the organic thin-film transistor memory spare of floating gate structure.Through after the writing or wipe of different pulse gate voltages, " 1 " of storage or " 0 " attitude data can keep the long time.
Embodiment 2:
Earlier the tin indium oxide on the indium oxide tin glass is photo-etched into the electrode (being source-drain electrode) of two 10 millimeters long, 1 mm wide (being channel width), spacing between electrodes is 100 microns (being channel length); Clean then, nitrogen dries up.In vacuum degree is 1 to 5 * 10
-4In the coating system of handkerchief, the Teflon of nylon 6,150 nanometer thickness of the calcirm-fluoride of nylon 6,15 nanometer thickness of the pentacene of evaporation 70 nanometer thickness, 25 nanometer thickness, 200 nanometer thickness successively on the tin indium oxide source-drain electrode, and give graphically by mask plate, the width that is 100 nanometer thickness at last is 1 millimeter a aluminum strip, gives graphically by another mask plate.The pentacene thin film growth rate is controlled at 0.05 nanometer per second, and the calcium-fluoride thin film growth rate is controlled at 0.05 nanometer per second, and nylon 6 is controlled at 0.1 nanometer per second with the growth rate of Teflon.Device has tangible field effect characteristic, and the device operating voltage can be reduced in 15 volts.Accompanying drawing 7 has provided the transfer characteristic curve of organic thin-film transistor memory spare under the different fixing source-drain voltage based on floating gate structure.Device operation current on-off ratio～10
2, tangible hesitation is arranged, the threshold voltage difference under the different scanning direction is obvious, and sluggish height current ratio reaches 50 times.The field-effect mobility that calculating can get device is about 10
-2～10
-1Cm
2/ Vs.Accompanying drawing 5 is storage cycle characteristics curves of the organic thin-film transistor memory spare based on floating gate structure of the present invention.Accompanying drawing 6 is based on the storage data retention characteristic curve of the organic thin-film transistor memory spare of floating gate structure.Through after the writing or wipe of different pulse gate voltages, " 1 " of storage or " 0 " attitude data can keep the long time.
Embodiment 3:
Earlier the tin indium oxide on the indium oxide tin glass is photo-etched into the electrode (being source-drain electrode) of two 10 millimeters long, 50 microns wide (being channel width), spacing between electrodes is 1 micron (being channel length); Clean then, nitrogen dries up.In vacuum degree is 1 to 5 * 10
-4In the coating system of handkerchief, the Teflon of the nickel of the Teflon of the pentacene of evaporation 50 nanometer thickness, 2 nanometer thickness, 2 nanometer thickness, 100 nanometer thickness successively on the tin indium oxide source-drain electrode, and give graphically by mask plate, the width that is 80 nanometer thickness at last is 1 millimeter a aluminum strip, gives graphically by another mask plate.The pentacene thin film growth rate is controlled at 0.05 nanometer per second, and the nickel film growth rate is controlled at 0.02 nanometer per second, and the growth rate of Teflon is controlled at 0.1 nanometer per second.Device has tangible field effect characteristic, about 10 volts of device operating voltage.Device operation current on-off ratio～10
3, tangible hesitation is arranged, the threshold voltage difference under the different scanning direction is obvious, and sluggish height current ratio reaches 10
2Doubly.The field-effect mobility that calculating can get device is about 10
-2Cm
2/ Vs.Can observe device has tangible storage cycle characteristics curve, " 1 " or " 0 " attitude ratio data～10 of electric current storage
2, and can keep the long time.
Embodiment 4:
Earlier will be on glass substrate the gold thin film layer of vacuum evaporation 40 nanometer thickness, be photo-etched into the electrode (being source-drain electrode) of two 10 millimeters long, 5 mm wides (being channel width) then, spacing between electrodes is 150 microns (they being channel length); Clean then, nitrogen dries up.In vacuum degree is 1 to 5 * 10
-4In the coating system of handkerchief, the Teflon of nylon 6,200 nanometer thickness of the barium fluoride of the PMMA of the pentacene of evaporation 100 nanometer thickness, 40 nanometer thickness, 40 nanometer thickness, 600 nanometer thickness successively on the tin indium oxide source-drain electrode, and give graphically by mask plate, the width that is 140 nanometer thickness at last is 1 millimeter a aluminum strip, gives graphically by another mask plate.The pentacene thin film growth rate is controlled at 0.1 nanometer per second, CaF
2Film growth rate is controlled at 0.1 nanometer per second, and the PMMA growth rate is controlled at 0.1 nanometer per second, and nylon 6 is controlled at 0.5 nanometer per second with the growth rate of Teflon.Device has tangible field effect characteristic, about 30 volts of device operating voltage.Device operation current on-off ratio～10
4, tangible hesitation is arranged, the threshold voltage difference under the different scanning direction is obvious, and sluggish height current ratio reaches 10
2Doubly.The field-effect mobility that calculating can get device is about 10
-1Cm
2/ Vs.Can observe device has tangible storage cycle characteristics curve, " 1 " or " 0 " attitude ratio data～10 of electric current storage
2, and can keep the long time.
Embodiment 5:
Earlier the vacuum evaporation thickness on glass substrate is the silver-colored thin layer of 50 nanometers, is photo-etched into the electrode (being source-drain electrode) of two 10 millimeters long, 1 mm wide then, and spacing between electrodes is 50 microns; Clean then, nitrogen dries up.In vacuum degree is 1 to 5 * 10
-4In the coating system of handkerchief, the Teflon of nylon 6,150 nanometer thickness of the silver of nylon 6,5 nanometer thickness of ten hexafluoro CuPcs of evaporation 70 nanometer thickness, 25 nanometer thickness, 200 nanometer thickness successively on the tin indium oxide source-drain electrode, and give graphically by mask plate, the width that is 100 nanometer thickness at last is 1 millimeter a aluminum strip, gives graphically by another mask plate.Ten hexafluoro phthalocyanine copper film growth rates are controlled at 0.05 nanometer per second, and silver-colored film growth rate is controlled at 0.1 nanometer per second, and nylon 6 is controlled at 0.1 nanometer per second with the growth rate of Teflon.Device has tangible field effect characteristic, and the device operating voltage can be low to moderate 10 volts.The transfer characteristic curve of device under the stationary source drain voltage has tangible hesitation, and the threshold voltage difference under the different scanning direction is obvious, 30～80 times of sluggish height current ratios.Test its storage cycle characteristics, " 1 " or " 0 " attitude data read current difference is obvious, and can keep one long period.
Embodiment 6:
Earlier the tin indium oxide on the indium oxide tin glass is photo-etched into the electrode (being source-drain electrode) of two 10 millimeters long, 1 mm wide (being channel width), spacing between electrodes is 50 microns (being channel length); Clean then, nitrogen dries up.In vacuum degree is 1 to 5 * 10
-4In the coating system of handkerchief, the aluminium of the calcirm-fluoride of nylon 6,15 nanometer thickness of the pentacene of evaporation 70 nanometer thickness, 25 nanometer thickness, 10 nanometer thickness (speed of growth is controlled at 0.1 nanometer per second), the calcirm-fluoride of 150 nanometer thickness, the Teflon of 150 nanometer thickness successively on the tin indium oxide source-drain electrode, and give graphically by mask plate, the width that is 100 nanometer thickness at last is 1 millimeter a aluminum strip, gives graphically by another mask plate.The pentacene thin film growth rate is controlled at 0.1 nanometer per second, and the calcirm-fluoride growth rate is controlled at 0.2 nanometer per second, and the growth rate of Teflon is controlled at 0.1 nanometer per second.Device has tangible field effect characteristic, and the device operating voltage can be low to moderate 10 volts.The transfer characteristic curve of device under the stationary source drain voltage has tangible hesitation, and the threshold voltage difference under the different scanning direction is obvious, 50～100 times of sluggish height current ratios.Test its storage cycle characteristics, " 1 " or " 0 " attitude data read current difference is obvious, and can keep one long period.
Embodiment 7:
Earlier the tin indium oxide on the indium oxide tin glass is photo-etched into the electrode (being source-drain electrode) of two 10 millimeters long, 1 mm wide (being channel width), spacing between electrodes is 50 microns (being channel length); Clean then, nitrogen dries up.In vacuum degree is 1 to 5 * 10
-4In the coating system of handkerchief, the pentacene of evaporation 70 nanometer thickness successively on the tin indium oxide source-drain electrode, growth rate is controlled at 0.1 nanometer per second; The nylon 6 of 25 nanometer thickness, growth rate are controlled at 0.1 nanometer per second; The calcirm-fluoride of 15 nanometer thickness, growth rate are controlled at 0.1 nanometer per second; The calcirm-fluoride of 150 nanometer thickness, growth rate are controlled at 0.2 nanometer per second; The Teflon of 150 nanometer thickness, growth rate are controlled at 0.1 nanometer per second; And give graphically by mask plate.Be that 100 nanometer thickness, width are 1 millimeter aluminum strip at last, give graphically by another mask plate.Device has tangible field effect characteristic, and the device operating voltage can be low to moderate 10 volts.The transfer characteristic curve of device under the stationary source drain voltage has tangible hesitation, and the threshold voltage difference under the different scanning direction is obvious, sluggish height current ratio～10
2Doubly.Test its storage cycle characteristics, " 1 " or " 0 " attitude data read current is than about 10
2, and can keep one long period.
Embodiment 8:
Earlier the tin indium oxide on the indium oxide tin glass is photo-etched into the electrode (being source-drain electrode) of two 10 millimeters long, 1 mm wide (being channel width), spacing between electrodes is 50 microns (being channel length); Clean then, nitrogen dries up.In vacuum degree is 1-5 * 10
-4In the coating system of handkerchief, the CuPc of evaporation 70 nanometer thickness successively on the tin indium oxide source-drain electrode, growth rate is controlled at 0.05 nanometer per second; The nylon 6 of 25 nanometer thickness, growth rate are controlled at 0.1 nanometer per second; The calcirm-fluoride of 15 nanometer thickness, growth rate are controlled at 0.1 nanometer per second; The calcirm-fluoride of 150 nanometer thickness, growth rate are controlled at 0.2 nanometer per second; The Teflon of 150 nanometer thickness, growth rate are controlled at 0.1 nanometer per second; And give graphically by mask plate.Be that 100 nanometer thickness, width are 1 millimeter aluminum strip at last, give graphically by another mask plate.Device has tangible field effect characteristic, and the device operating voltage can be low to moderate 10 volts.The transfer characteristic curve of device under the stationary source drain voltage has tangible hesitation, and the threshold voltage difference under the different scanning direction is obvious, 20～50 times of sluggish height current ratios.Test its storage cycle characteristics, " 1 " or " 0 " attitude data read current is than about 10～30, and can keep one long period.
Embodiment 9:
Earlier the tin indium oxide on the indium oxide tin glass is photo-etched into the electrode of 20 millimeters long, 1 mm wide, cleans then, nitrogen dries up.Prepare the PMMA film with spin coating proceeding, and in 100 ℃ of annealing down, improve film performance, wherein solution concentration is 1.5%, and solvent is a chloroform.By regulating rotating speed, can control the film thickness scope is 200～800 nanometers, and then the operating voltage range of device is 20～100 volts.Transferring to then in the vacuum system, is～4 * 10 in vacuum degree
-4During handkerchief, the nickel film of hot successively evaporation 2 nanometers, the aluminium film of 2 nanometers.With oxygen plasma it is handled then, make that the aluminium film surface is oxidized, form the aluminium oxide floating gate dielectric layer.Once more it being transferred to vacuum system, is～4 * 10 in vacuum degree
-4During handkerchief, the pentacene of evaporation 50 nanometer thickness on nickel oxide film, growth rate is controlled at 0.1 nanometer per second.The gold of 60 nanometer thickness of growing is at last done source-drain electrode, gives graphically by mask plate, and channel length is 20 microns, and width is 500 microns.Device has tangible field effect characteristic, the about 0.3cm of device mobility
2/ Vs.Transfer characteristic curve under the stationary source drain voltage has tangible hesitation, and the threshold voltage difference under the different scanning direction is obvious, sluggish height current ratio～10
3Doubly.Test its storage cycle characteristics, " 1 " or " 0 " attitude data read current ratio is higher than 500, and can keep one long period.
Embodiment 10:
The aluminium of heat growth 100 nanometer thickness, 20 millimeters long, 1 mm wide is made gate electrode on the Merlon flexible substrate.Prepare the PMMA film with spin coating proceeding, and in 100 ℃ of annealing, improve film performance, wherein solution concentration is 1.5%, and solvent is a chloroform.By regulating rotating speed, can control the film thickness scope is 200～800 nanometers, and then the operating voltage range of device is 20～100 volts.Spin coating nano-silver water solution then, about 15 nanometers of the film thickness of preparation.Once more it being transferred to vacuum system, is～4 * 10 in vacuum degree
-4During handkerchief, the pentacene of nylon 6,1000 nanometer thickness of hot successively evaporation 40 nanometer thickness, the gold of 60 nanometer thickness are taken on the floating gate dielectric layer of device, active layer, source-drain electrode layer respectively, give graphically by mask plate.Channel length is 100 microns, and width is 2000 microns.Device has tangible field effect characteristic, the about 0.1cm of device mobility
2/ Vs.Transfer characteristic curve under the stationary source drain voltage has tangible hesitation, and the threshold voltage difference under the different scanning direction is obvious, sluggish height current ratio～10
2Doubly.Test its storage cycle characteristics, " 1 " or " 0 " attitude data read current ratio is higher than 50～100, and can keep one long period.
Embodiment 11:
The aluminium of heat growth 100 nanometer thickness, 20 millimeters long, 1 mm wide is made gate electrode on the Merlon flexible substrate.Prepare the PMMA-GMA film with spin coating proceeding, and in 100 ℃ of annealing down, improve film performance, wherein solution concentration is 1.5%, and solvent is a chloroform.By regulating rotating speed, can control the film thickness scope is 200～800 nanometers, and then the operating voltage range of device is 20～100 volts.Transferring to then in the vacuum system, is～4 * 10 in vacuum degree
-4During handkerchief, the nickel film of hot successively evaporation 10 nanometers, the aluminium film of 10 nanometers.With oxygen plasma it is handled then, make that the aluminium film surface is oxidized, form the aluminium oxide floating gate dielectric layer.Once more it being transferred to vacuum system, is～4 * 10 in vacuum degree
-4During handkerchief, the carbon 60 of evaporation 60 nanometer thickness on nickel oxide film, growth rate 0.1 nanometer per second.The lithium fluoride of 1 nanometer of growing at last and the aluminium composite bed of 100 nanometer thickness are done source-drain electrode, give graphically by mask plate, and channel length is 50 microns, and width is 1000 microns.Device has tangible field effect characteristic, device mobility～10
-1Cm
2/ Vs.Transfer characteristic curve under the stationary source drain voltage has tangible hesitation, and the threshold voltage difference under the different scanning direction is obvious, sluggish height current ratio～10
2Doubly.Test its storage cycle characteristics, " 1 " or " 0 " attitude data read current ratio is higher than 20～50, and can keep one long period.
Claims (8)
1. based on the non-volatile organic thin-film transistor memory of floating gate structure, it is characterized in that it is by constituting for the channel region of device, organic semiconductor layer 3, floating gate dielectric layer 4, floating gate layer 5, control gate dielectric layer 6 and control grid electrode layer 7 between substrate 1, source-drain electrode layer 2, source-drain electrode layer 2 electrode; On substrate 1, prepare layer of conductive film, and graphically form the source-drain electrode layer 2 of device, then successively in vacuum chamber evaporation prepare organic semiconductor layer 3, floating gate dielectric layer 4, floating gate layer 5, control gate dielectric layer 6 and control grid electrode layer 7;
Substrate 1 is glass or Merlon flexible substrate;
Source-drain electrode layer 2 adopts tin indium oxide, poly-dioxoethyl thiophene: poly-p styrene sulfonic acid, gold, silver, nickel, palladium, copper, platinum, aluminium or samarium;
Any in oligomerisation six thiophene that organic semiconductor layer 3 adopts and many benzene, phthalocyanine-like compound, carbon 60, carbon 70, Uniformpoly thiophene, the many benzene of connection, polythiophene, perfluoro metal phthalocyanine, naphthalene glycosides and derivative thereof or perfluoroalkyl replace;
Floating gate dielectric layer 4 adopts any in nylon 6, the poly-bright olefin(e) acid formicester of methyl, Teflon, polyimides and derivative, calcirm-fluoride, lithium fluoride, cesium fluoride, barium fluoride, nickel oxide, aluminium oxide, silica or the titanium oxide insulating material;
Floating gate layer 5 adopts the material of following kind:
1. the metal of nanostructure: any in nickel, silver, aluminium, palladium, copper, gold, platinum or the samarium;
2. have any in the iron of magnetic or nickel and the oxide thereof;
3. Uniformpoly thiophene, and many benzene, join any in the oligomerisation six thiophene organic semiconducting materials that many benzene, polythiophene, phthalocyanine-like compound, carbon 60, carbon 70, perfluoro metal phthalocyanine, naphthalene glycosides and derivative thereof and perfluoroalkyl replace;
4. nano particle: any in calcirm-fluoride, lithium fluoride, cesium fluoride, barium fluoride, nickel oxide or the zinc oxide;
Control gate dielectric layer 6 adopts the insulating material identical with floating gate dielectric layer 4; For improving the composite bed that device performance can also adopt nylon 6/ calcirm-fluoride, nylon 6/ Teflon, calcirm-fluoride/Teflon, the poly-bright olefin(e) acid of methyl formicester/Teflon, the poly-bright olefin(e) acid formicester/calcirm-fluoride of methyl, nylon 6/ aluminium oxide, the multiple insulating material of the poly-bright olefin(e) acid formicester/aluminium oxide of methyl to form;
Control grid electrode layer 7 adopts any in tin indium oxide oxides, poly-p styrene sulfonic acid, gold, silver, nickel, palladium, copper, platinum, aluminium or the samarium.
2. the non-volatile organic thin-film transistor memory based on floating gate structure as claimed in claim 1 is characterized in that, 1～150 micron of described channel length, 50～5000 microns of width; The thickness of organic semiconductor layer 3 is 50～100 nanometers; The thickness of floating gate dielectric layer 4 is 2～40 nanometers; The thickness of floating gate layer 5 is 2～40 nanometers; The thickness of control gate dielectric layer 6 is 100～800 nanometers; The thickness of control grid electrode layer 7 is 80～140 nanometers.
3. the manufacture method of the non-volatile organic thin-film transistor memory based on floating gate structure as claimed in claim 1, it is characterized in that, step and condition are as follows: earlier the indium tin oxide on the substrate layer 1, poly-p styrene sulfonic acid or metal conducting layer 2 are carried out photolithography patterning, preparation source-drain electrode layer 2, be the channel region of device between source-drain electrode layer 2 electrode, clean then, nitrogen dries up, it is transferred in the vacuum coating system, treat that vacuum degree reaches 1 to 5 * 10
-4During handkerchief, on source-drain electrode layer 2, prepare organic semiconductor layer 3, floating gate dielectric layer 4, floating gate layer 5, control gate dielectric layer 6 and control grid electrode layer 7 successively.
4. the manufacture method of the non-volatile organic thin-film transistor memory based on floating gate structure as claimed in claim 2, it is characterized in that, step and condition are as follows: earlier the tin indium oxide thing on the substrate layer 1, poly-p styrene sulfonic acid or metal conducting layer 2 are carried out photolithography patterning, preparation source-drain electrode layer 2, be the channel region of device between source-drain electrode layer 2 electrode, clean then, nitrogen dries up, it is transferred in the vacuum coating system, treat that vacuum degree reaches 1 to 5 * 10
-4During handkerchief, on source-drain electrode layer 2, prepare organic semiconductor layer 3, floating gate dielectric layer 4, floating gate layer 5, control gate dielectric layer 6 and control grid electrode layer 7 successively; 1～150 micron of described channel length, 50～5000 microns of width; The thickness of organic semiconductor layer 3 is 50～100 nanometers; The thickness of floating gate dielectric layer 4 is 2～40 nanometers; The thickness of floating gate layer 5 is 2～40 nanometers; The thickness of control gate dielectric layer 6 is 100～800 nanometers; The thickness of control grid electrode layer 7 is 80～140 nanometers.
5. based on the non-volatile organic thin-film transistor memory of floating gate structure, it is characterized in that it is to be made of substrate 1, control grid electrode layer 7, control gate dielectric layer 6, floating gate layer 5, floating gate dielectric layer 4, organic semiconductor layer 3 and source-drain electrode layer 2; Wherein, on substrate layer 1, prepare one deck conductive layer and carry out photolithography patterning and form control grid electrode layer 7, spin coating prepares control gate dielectric layer 6 on control grid electrode layer 7, evaporation nickel and aluminium film in vacuum chamber then, wherein the nickel film is taken on floating gate layer 5, adopt oxygen plasma technical finesse aluminium film to make its oxidation form floating gate dielectric layer 4, vacuum evaporation organic semiconductor layer 3 and source-drain electrode layer 2 once more are the channel region of device between source-drain electrode layer 2 electrode;
Substrate 1 is glass or Merlon flexible substrate;
Control grid electrode layer 7 adopts any in indium tin oxides, poly-p styrene sulfonic acid, gold, silver, nickel, palladium, copper, platinum, aluminium or the samarium;
Control gate dielectric layer 6 adopts any in nylon 6, the poly-bright olefin(e) acid formicester of methyl, Teflon, polyimides and derivative, calcirm-fluoride, lithium fluoride, cesium fluoride, barium fluoride, nickel oxide, aluminium oxide, silica or the titanium oxide insulating material; For improving the composite bed that device performance can also adopt nylon 6/ calcirm-fluoride, nylon 6/ Teflon, calcirm-fluoride/Teflon, the poly-bright olefin(e) acid of methyl formicester/Teflon, the poly-bright olefin(e) acid formicester/calcirm-fluoride of methyl, nylon 6/ aluminium oxide, the multiple insulating material of the poly-bright olefin(e) acid formicester/aluminium oxide of methyl to form;
Floating gate layer 5 adopts the material of following kind:
1. the metal of nanostructure: any in nickel, silver, aluminium, palladium, copper, gold, platinum or the samarium;
2. have any in the iron of magnetic or nickel and the oxide thereof;
3. Uniformpoly thiophene, and many benzene, join any in the oligomerisation six thiophene organic semiconducting materials that many benzene, polythiophene, phthalocyanine-like compound, carbon 60, carbon 70, perfluoro metal phthalocyanine, naphthalene glycosides and derivative thereof and perfluoroalkyl replace;
4. nano particle: any in calcirm-fluoride, lithium fluoride, cesium fluoride, barium fluoride, nickel oxide or the zinc oxide;
Floating gate dielectric layer 4 adopts the insulating material identical with control gate dielectric layer 6:
Any in oligomerisation six thiophene that organic semiconductor layer 3 adopts and many benzene, phthalocyanine-like compound, carbon 60, carbon 70, Uniformpoly thiophene, the many benzene of connection, polythiophene, perfluoro metal phthalocyanine, naphthalene glycosides and derivative thereof or perfluoroalkyl replace;
Source-drain electrode layer 2 adopts any in indium tin oxides, poly-p styrene sulfonic acid, gold, silver, nickel, palladium, copper, platinum, aluminium, the samarium; The composite bed that also can adopt calcium/aluminium, magnesium/aluminium or lithium fluoride/aluminium to form;
6. the non-volatile organic thin-film transistor memory based on floating gate structure as claimed in claim 5 is characterized in that, 20～100 microns of described device channel length, 500～2000 microns of width; The thickness of control grid electrode layer 7 is 40～100 nanometers; The thickness of control gate dielectric layer 6 is 200～800 nanometers; The thickness of floating gate layer 5 is 2～15 nanometers; The thickness of floating gate dielectric layer 4 is 2～40 nanometers; The thickness of organic semiconductor layer 3 is 50～100 nanometers; The thickness of source-drain electrode layer 2 is 60～100 nanometers.
7. the manufacture method of the non-volatile organic thin-film transistor memory based on floating gate structure as claimed in claim 5, it is characterized in that, step and condition are as follows: earlier to the tin indium oxide on the substrate layer 1, poly-p styrene sulfonic acid or metal conducting layer 7 carry out photolithography patterning and form control grid electrode layer 7, clean then, nitrogen dries up, the poly-bright olefin(e) acid formicester of methyl of spin coating prepares control gate dielectric layer 6 on control grid electrode layer 7, evaporation nickel and aluminium film in vacuum chamber then, wherein the nickel film is taken on floating gate layer 5, adopt oxygen plasma technical finesse aluminium film to make its oxidation form floating gate dielectric layer 4, vacuum evaporation organic semiconductor layer 3 and source-drain electrode layer 2 once more are the channel region of device between source-drain electrode layer 2 electrode.
8. the manufacture method of the non-volatile organic thin-film transistor memory based on floating gate structure as claimed in claim 6, it is characterized in that, earlier to the tin indium oxide oxide on the substrate layer 1, poly-p styrene sulfonic acid or metal conducting layer 7 carry out photolithography patterning and form control grid electrode layer 7, clean then, nitrogen dries up, the poly-bright olefin(e) acid formicester of methyl of spin coating prepares control gate dielectric layer 6 on control grid electrode layer 7, evaporation nickel and aluminium film in vacuum chamber then, wherein the nickel film is taken on floating gate layer 5, adopt oxygen plasma technical finesse aluminium film to make its oxidation form floating gate dielectric layer 4, vacuum evaporation organic semiconductor layer 3 and source-drain electrode layer 2 once more are the channel region of device between source-drain electrode layer 2 electrode; 20～100 microns of described device channel length, 500～2000 microns of width; The thickness of control grid electrode layer 7 is 40～100 nanometers; The thickness of control gate dielectric layer 6 is 200～800 nanometers; The thickness of floating gate layer 5 is 2～15 nanometers; The thickness of floating gate dielectric layer 4 is 2～40 nanometers; The thickness of organic semiconductor layer 3 is 50～100 nanometers; The thickness of source-drain electrode layer 2 is 60～100 nanometers.
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