CN102339955A - Resonant tunneling organic light-emitting diode and preparation method thereof - Google Patents
Resonant tunneling organic light-emitting diode and preparation method thereof Download PDFInfo
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Abstract
The invention relates to a resonant tunneling organic light-emitting diode and a preparation method thereof. According to a device structure of an organic light-emitting transistor based on a static induction transistor (SIT), effective overlapping areas formed between an intermediate metal electrode (G electrode), which is sandwiched between two hole transport layers, and an indium tin oxide (ITO) conductive electrode (S electrode) of the resonant tunneling organic light-emitting diode provided by the invention, and between the intermediate metal electrode and an electrode (D electrode) have a certain small mismatch area which forms a current carrier tunneling channel, so a resonant tunneling diode capable of emitting light is formed. Compared with the conventional organic molecule resonant tunneling diode, the resonant tunneling organic light-emitting diode has the advantages that: 1, the structure is simple; 2, the preparation method is simple and convenient, and is easy to operate; and 3, the characteristic of light emitting is provided; and 4, the peak and valley current ratio (PVCR) reaches more than 8.8, and the PVCR increases along with changes of grid voltage (VG).
Description
Technical field
The present invention relates to a kind of resonance tunnel-through Organic Light Emitting Diode and preparation method thereof, belong to electrooptical device and micro-nano photoelectric device technical field.
Background technology
Current solid semiconductor development of integrated circuits has run into many difficult problems and challenge, and the microminiaturization of integrated circuit moves closer to the limit.The live width of integrated circuit has dropped to about 0.1 μ m at present; Though the live width of integrated circuit also might further reduce; But according to quantum theory; When the live width of integrated circuit drops to 0.01 μ m when following, can not work orderly with the flow solid semiconductor electronic device of transmission signals of electronics.This just needs the new science and technology of development to solve this difficult problem.Molecular electronics with good development prospect produces under such condition.
Molecular electronics is to study the new branch of science that individual molecule is played a role as critical component in the computer equipment in future.As far back as the seventies in 20th century, scientists has just progressively proposed the conception of molecular device.Use molecular device not only can make the size of integrated circuit reduce by 5 one magnitude, but also can make speed improve 6 one magnitude, so use molecular device can improve the performance of integrated circuit on the whole greatly.At present scientist generally reaches common understanding, and the molecular electronic engineering is the important directions of electronics development from now on, and prophesy: will be reduced to nanometer scale to the size of left and right sides microelectronic element in recent years, and get into the genuine molecular electronics epoch.
Resonance tunnel-through diode (RTD) is one of nano electron device of succeeding in developing the earliest, RTD is combined to have developed multiple high-speed digital circuit with high migration transistor (HEMT) at present.If can realize organic molecule resonance tunnel-through diode device, will be a kind of very tempting imagination.RTD generally has following characteristics: (1) high-frequency high-speed; (2) low-work voltage, low-power consumption; (3) negative resistance and self-locking (Self-latching) characteristic; (4) just can accomplish multiple logic function with small number of devices.
Through the synthetic organic molecule RTD device that obtains of chemical method; Can the size of RTD be reduced to molecular level; Further improve speed and reduced energy consumption, and the synthesis material wide material sources, with low cost; The particularly important is organic molecule RTD and can carry out MOLECULE DESIGN, directly synthesize various molecular devices with marvellous structure and performance through chemical reaction.
In recent years the research of organic molecule RTD device is obtained paying attention to day by day, people design, synthesize some organic molecule RTD, and on the basis that structure is studied, to the operation principle deep discussion of also contrasting.Organic molecule RTD had both had the solid semiconductor functional characteristic, had the not available good characteristic of solid semiconductor RTD again, can reduce the size of integrated circuit; Raising speed; Cut down the consumption of energy, improve to use the performance of the integrated circuit that RTD processes greatly, and can carry out MOLECULE DESIGN as required; Directly synthesize a series of molecular devices such as three terminal device and gate, further direct synthetic molecules circuit then with specific function.The organic molecule resonance tunnel-through diode that successfully prepares through organic synthesis at present is also few, and main cause is that relatively harshness, synthetic product separation difficulty, yield are low for complex synthetic route, synthesis condition.In addition, the peak-to-valley ratio also smaller (below 4) that present organic molecule resonance tunnel-through diode at room temperature reaches, improving its device performance is one of focus of various countries' researcher research at present.
Summary of the invention
The objective of the invention is to propose a kind of resonance tunnel-through Organic Light Emitting Diode and preparation method thereof in order to overcome the shortcoming that present existing organic molecule resonance tunnel-through diode and preparation method exist.The present invention is according to the device architecture based on the organic light-emitting transistor of SIT; Effective overlapping area of formation has a certain little mismatch area between the ITO conductive electrode (the S utmost point) that makes the resonance tunnel-through Organic Light Emitting Diode that the intermetallic metal electrode that is clipped between the two-layer hole transmission layer and the present invention propose and the electrode (the D utmost point); This little mismatch area forms the charge carrier tunnel channel, forms the resonance tunnel-through diode with luminous behavior.
The objective of the invention is to realize through following technical scheme.
A kind of resonance tunnel-through Organic Light Emitting Diode of the present invention comprises one deck ITO conductive electrode (the S utmost point); On this ITO conductive electrode, prepare one deck organic cavity transmission layer 1 then; On this organic cavity transmission layer 1, prepare one deck intermetallic metal electrode (the G utmost point) then; And then on this intermetallic metal electrode preparation one deck organic cavity transmission layer 2; On this organic cavity transmission layer 2, prepare one deck luminous organic material more afterwards, the preparation of vacuum electrode evaporation (the D utmost point) completion resonance tunnel-through organic light emitting diode device on this organic luminescent material thin-film at last.
When preparation intermetallic metal electrode (the G utmost point); The effective overlapping area that forms between this intermetallic metal electrode and the S utmost point and the D utmost point has a certain little mismatch area; Form the tunnel channel of charge carrier through this mismatch area, thereby make entire device form resonance tunnel-through Organic Light Emitting Diode with luminous behavior.This a certain little mismatch area is far smaller than the effective area that forms between the S utmost point and the D utmost point.
The material of said organic cavity transmission layer 1 and organic cavity transmission layer 2 is preferably α-NPD, or organic hole transferring materials such as NPB and TPD.
Wherein, α-NPD is N, N-Di (naphthalene-1-yl)-N, N`-diphenyl-benzidine;
NPB is N, N '-bis-(1-naphthyl)-N, and N '-diphenyl-1,1 '-biphenyl-4,4 '-diamine;
TPD is N, N '-bis (4-butylphenyl)-N, N '-bis (phenyl) benzidine.
Said organic cavity transmission layer 1 can be with a kind of organic hole transferring material with organic cavity transmission layer 2 used materials, also can be different organic hole transferring materials.
Said organic light emission layer material is preferably Alq
3, green light.Alq
3Be tris (8-quinolinolate) aluminium.
Said electrode (the D utmost point) is layer of metal electrode or double layer of metal electrode or the layer of metal alloy electrode of work function smaller or equal to 4.3eV; Wherein, the layer of metal electrode is preferably the aluminium electrode, and the double layer of metal electrode is preferably the Ca/Al electrode, and metal alloy electrodes is preferably the Mg:Ag alloy.
The preparation method of a kind of resonance tunnel-through Organic Light Emitting Diode of the present invention, concrete steps are:
The 1st step: the method on the ito glass surface that cleans up through thermal evaporation prepares one deck organic hole transferring material film 1 earlier;
Ito thin film thickness on the said ito glass is preferably 120nm.
The 2nd step: the method through thermal evaporation prepares the layer of metal film as the G utmost point on organic hole transferring material film 1 described in the 1st step; It should be noted that; The effective overlapping area that forms between this metallic film and the S utmost point and the D utmost point has a certain little mismatch area; Through the tunnel channel of this little mismatch area formation charge carrier, thereby the resonance tunnel-through Organic Light Emitting Diode that the present invention is proposed has luminous behavior after adding voltage.
Said metallic film (the G utmost point) thickness is preferably 15nm～30nm.
The 3rd step: the method through thermal evaporation goes up preparation one deck organic hole transferring material film 2 at metallic film (the G utmost point) described in the 2nd step;
The thickness of organic hole transferring material film 1 and organic hole transferring material film 2 is preferably 20nm～100nm described in the 1st step and the 3rd step.
The 4th step: the mode through thermal evaporation on organic hole transferring material film 2 described in the 3rd step prepares one deck organic luminous layer;
The thickness of said organic luminous layer is preferably 30nm～100nm.
The 5th step: at last under vacuum condition in vacuum electrode evaporation (the D utmost point) on the organic luminous layer described in the 4th step, obtain a kind of resonance tunnel-through Organic Light Emitting Diode that the present invention proposes.
Beneficial effect
The resonance tunnel-through Organic Light Emitting Diode that the present invention proposes is compared with existing organic molecule resonance tunnel-through diode and is had the following advantages:
1. simple in structure;
2. the preparation method is easy, easy to operate;
3. has emitting characteristics.
4. its pv curren ratio (PVCR) high (reaching more than 8.8), and this electric current peak-to-valley ratio PVCR increases along with the variation of grid voltage VG.
Description of drawings
Fig. 1 is the resonance tunnel-through organic LED structure sketch map in the embodiments of the invention 1;
Fig. 2 is that resonance tunnel-through organic light emitting diode device in the embodiments of the invention 1 is at grid voltage V
GOutput characteristic curve during=0V;
Fig. 3 is the transfer characteristic curve of resonance tunnel-through organic light emitting diode device under different grid voltages in the embodiments of the invention 1;
The photo that Fig. 4 sees at microscopically for the resonance tunnel-through Organic Light Emitting Diode in the embodiments of the invention 1; Wherein (a) is luminous photo of under dark, seeing; (b) device architecture and the corresponding light-emitting zone thereof for seeing under the illumination.
Fig. 5 is the AFM photo of the Al layer of the 20nm thickness in the embodiments of the invention 1; Wherein Al is plated on the thick α of 60nm-NPD film.
Embodiment
Below in conjunction with accompanying drawing and embodiment the present invention is further specified.
Embodiment 1:
A kind of resonance tunnel-through Organic Light Emitting Diode comprises one deck ITO conductive electrode, ground floor hole transmission layer, intermetallic metal electrode, second layer hole transmission layer, one deck organic luminous layer and one deck electrode.Wherein, the ITO conductive electrode is as the S utmost point; The intermetallic metal electrode is a layer of metal Al electrode, as the G utmost point; Two-layer hole transmission layer is α-NPD material film; Organic luminous layer is Alq
3Electrode is the aluminium electrode, and as the D utmost point, aluminium is stable in the air, and its work function is 4.28eV.
The preparation method of a kind of resonance tunnel-through Organic Light Emitting Diode of the present invention, concrete steps are:
The 1st step: at first use absorbent cotton and washing agent wiping ito glass repeatedly; And dash with deionized water and to clean up; And then used deionized water, acetone and isopropyl alcohol respectively each ultrasonic 15 minutes; All ito glass is dried up before the back ultrasonic cleaning whenever carrying out with nitrogen; After ultrasonic cleaning is intact ito glass is put into the ozone treatment machine and carried out ozone treatment 15 minutes, (wherein transmitance is greater than 85% in visible light and near-ultraviolet range for ito glass, and its square resistance is 10 Ω/) with subsequent use after cooling;
The 2nd step: the method with thermal evaporation on the ito glass that cleans up prepares hole transmission layer α-NPD, thickness 60nm;
The 3rd step: then at the last preparation of α-NPD Al metal electrode (the G utmost point), thickness 30nm;
The 4th step: the mode through thermal evaporation prepares one deck α-NPD film again on Al metal electrode (the G utmost point), and its thickness is 60nm.
The 5th step: then the mode through thermal evaporation prepares one deck organic light emitting film Alq on the α-NPD film described in the 4th step
3, its thickness is 50nm.
The 6th step: at last at Alq
3The aluminium electrode that vapor deposition 100nm is thick under vacuum condition on the thin layer promptly obtains the resonance tunnel-through Organic Light Emitting Diode, and its structure is as shown in Figure 1.
It should be noted that; When the 3rd step preparation Al metal electrode; The effective overlapping area that forms between the Al metallic film and the S utmost point and the D utmost point has a certain little mismatch area; Through the tunnel channel of this little mismatch area formation charge carrier, zone shown in dash area among Fig. 1, thereby resonance tunnel-through organic light emitting diode device ITO/ α-NPD (60nm)/α-NPD (60nm)/Alq that the present invention is proposed
3(50nm)/Al has luminous behavior under electric field action.Fig. 2 is that the resonance tunnel-through Organic Light Emitting Diode is at grid voltage V
GOutput characteristic curve during=0V, visible this device has tangible differential negative resistance effect, has typical resonance tunnel-through diode characteristic.Fig. 3 is the transfer characteristic curve of resonance tunnel-through organic light emitting diode device under different grid voltages, shows that this device has characteristics of transistor.Fig. 4 is the luminous photo of resonance tunnel-through Organic Light Emitting Diode of the present invention, wherein (a) luminous photo under dark, seeing; (b) device architecture and the corresponding light-emitting zone thereof for seeing under the illumination.It is thus clear that the light-emitting zone of this device is very tiny, this is that effective overlapping area of forming between intermetallic metal electrode (the G utmost point) and the device S utmost point and the D utmost point has a certain little mismatch area and causes.Fig. 5 is the AFM photo that is plated in the thick Al metal level of 20nm on the thick α of 60nm-NPD film; Wherein the evaporation rate of Al film is 0.4nm/s, and the evaporation rate of α-NPD film is 0.2nm/s, and the roughness on Al surface is 6.1nm.Organic material α-NPD and Alq
3The thermal evaporation vacuum condition be 3-5 * 10
-7Mbar, the vapor deposition condition of metal A l is 6 * 10
-6Mbar.
Embodiment 2:
A kind of resonance tunnel-through Organic Light Emitting Diode comprises one deck ITO conductive electrode, one deck hole transmission layer, intermetallic metal electrode, second layer hole transmission layer, one deck organic luminous layer and one deck electrode.Wherein the ITO conductive electrode is as the S utmost point; The intermetallic metal electrode is a layer of metal Al electrode, as the G utmost point; Two-layer hole transmission layer is TPD; Organic luminous layer is Alq
3Electrode is the aluminium electrode, and as the D utmost point, aluminium is stable in the air, and its work function is 4.28eV.
A kind of preparation method of resonance tunnel-through Organic Light Emitting Diode, concrete steps are:
The 1st step: at first use absorbent cotton and washing agent wiping ito glass repeatedly; And dash with deionized water and to clean up; And then used deionized water, acetone and isopropyl alcohol respectively each ultrasonic 15 minutes; All ito glass is dried up before the back ultrasonic cleaning whenever carrying out with nitrogen; After ultrasonic cleaning is intact ito glass is put into the ozone treatment machine and carried out ozone treatment 5 minutes, (wherein transmitance is greater than 85% in visible light and near-ultraviolet range for ito glass, and its square resistance is 10 Ω/) with subsequent use after cooling;
The 2nd step: the method with thermal evaporation prepares hole transmission layer TPD on the ito glass that cleans up then, thickness 60nm;
The 3rd step: then on TPD, prepare Al metal electrode (the G utmost point), thickness 30nm;
The 4th step: the mode through thermal evaporation prepares one deck TPD film again on Al metal electrode (the G utmost point), and its thickness is 60nm.
The 5th step: then the mode through thermal evaporation prepares one deck organic light emitting film Alq on the TPD film described in the 4th step
3, its thickness is 50nm.
The 6th step: at last at Alq
3The aluminium electrode that vapor deposition 100nm is thick under vacuum condition on the thin layer promptly obtains the resonance tunnel-through Organic Light Emitting Diode.
Wherein the evaporation rate of organic material and metal electrode all is
Organic material TPD and Alq
3The thermal evaporation vacuum condition be 3-5 * 10
-7Mbar, the vapor deposition condition of metal A l is 6 * 10
-6Mbar.
What deserves to be mentioned is that the hole transmission layer in specific embodiment 1 and the specific embodiment 2 all is an identical materials, for the hole transmission layer 1 and hole transmission layer 2 that are not identical organic hole material, like device architecture ITO/TPD/Al/ α-NPD/Alq
3/ Al and ITO/TPD/Al/ α-NPD/Alq
3/ Al is fine.
More than combine 2 specific embodiments that technical scheme of the present invention is described; But these explanations can not be understood that to have limited scope of the present invention; Protection scope of the present invention is limited the claims of enclosing, and any change on claim of the present invention basis all is protection scope of the present invention.
Claims (10)
1. a resonance tunnel-through Organic Light Emitting Diode is characterized in that: comprise one deck ITO conductive electrode, i.e. the S utmost point; On this ITO conductive electrode, prepare one deck organic cavity transmission layer 1 then; Then preparation one deck intermetallic metal electrode on this organic cavity transmission layer 1, i.e. the G utmost point, and then on this intermetallic metal electrode preparation one deck organic cavity transmission layer 2; On this organic cavity transmission layer 2, prepare one deck luminous organic material more afterwards; Vacuum electrode evaporation on this organic luminescent material thin-film at last, promptly the D utmost point is accomplished the preparation of resonance tunnel-through organic light emitting diode device;
When preparation intermetallic metal electrode; The effective overlapping area that forms between this intermetallic metal electrode G utmost point and the S utmost point and the D utmost point has a certain little mismatch area; Form the tunnel channel of charge carrier through this mismatch area, thereby make entire device form resonance tunnel-through Organic Light Emitting Diode with luminous behavior; This a certain little mismatch area is far smaller than the effective overlapping area that forms between the S utmost point and the D utmost point.
2. a kind of resonance tunnel-through Organic Light Emitting Diode as claimed in claim 1 is characterized in that: the material of said organic cavity transmission layer 1 and organic cavity transmission layer 2 is preferably α-NPD, or organic hole transferring materials such as NPB and TPD;
Wherein, α-NPD is N, N-Di (naphthalene-1-yl)-N, N`-diphenyl-benzidine;
NPB is N, N '-bis-(1-naphthyl)-N, and N '-diphenyl-1,1 '-biphenyl-4,4 '-diamine;
TPD is N, N '-bis (4-butylphenyl)-N, N '-bis (phenyl) benzidine.
3. according to claim 1 or claim 2 a kind of resonance tunnel-through Organic Light Emitting Diode is characterized in that:
Said organic cavity transmission layer 1 can be with a kind of organic hole transferring material with organic cavity transmission layer 2 used materials, also can be different organic hole transferring materials.
4. like the described a kind of resonance tunnel-through Organic Light Emitting Diode of one of claim 1 to 3, it is characterized in that:
Said organic light emission layer material is preferably Alq
3, green light; Alq
3Be tris (8-quinolinolate) aluminium.
5. like the described a kind of resonance tunnel-through Organic Light Emitting Diode of one of claim 1 to 4, it is characterized in that:
Said electrode, promptly the D utmost point is layer of metal electrode or double layer of metal electrode or the layer of metal alloy electrode of work function smaller or equal to 4.3eV; Wherein, the layer of metal electrode is preferably the aluminium electrode, and the double layer of metal electrode is preferably the Ca/Al electrode, and the double layer of metal alloy electrode is preferably the Mg/Ag alloy.
6. the preparation method of a resonance tunnel-through Organic Light Emitting Diode, it is characterized in that: its concrete preparation process is:
The 1st step: the method on the ito glass surface that cleans up through thermal evaporation prepares one deck organic hole transferring material film 1 earlier;
The 2nd step: the method through thermal evaporation prepares the layer of metal film as the G utmost point on organic hole transferring material film 1 described in the 1st step; It should be noted that; The effective overlapping area that forms between this metallic film and the S utmost point and the D utmost point has a certain little mismatch area; Through the tunnel channel of this little mismatch area formation charge carrier, thereby the resonance tunnel-through Organic Light Emitting Diode that the present invention is proposed has luminous behavior after adding voltage;
The 3rd step: through method preparation one deck organic hole transferring material film 2 on metallic film described in the 2nd step of thermal evaporation;
The 4th step: the mode through thermal evaporation on organic hole transferring material film 2 described in the 3rd step prepares one deck organic luminous layer;
The 5th step: at last under vacuum condition in vacuum electrode evaporation on the organic luminous layer described in the 4th step, promptly the D utmost point obtains a kind of resonance tunnel-through Organic Light Emitting Diode that the present invention proposes.
7. the preparation method of a kind of resonance tunnel-through Organic Light Emitting Diode as claimed in claim 6 is characterized in that: the ito thin film thickness described in the 1st step on the ito glass is preferably 120nm.
8. like the preparation method of claim 6 or 7 described a kind of resonance tunnel-through Organic Light Emitting Diodes, it is characterized in that: the thickness of metallic film is preferably 15nm～30nm described in the 2nd step.
9. like the preparation method of the described a kind of resonance tunnel-through Organic Light Emitting Diode of one of claim 6 to 8, it is characterized in that: the thickness of organic hole transferring material film 1 and organic hole transferring material film 2 is preferably 20nm～100nm described in the 1st step and the 3rd step.
10. like the preparation method of the described a kind of resonance tunnel-through Organic Light Emitting Diode of one of claim 6 to 9, it is characterized in that: the thickness of organic luminous layer is preferably 30nm～100nm described in the 4th step.
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| CN106876489A (en) * | 2017-02-10 | 2017-06-20 | 西安电子科技大学 | Based on CH3NH3PbI3Two-way HHET devices of p-type of material and preparation method thereof |
| CN113571998A (en) * | 2021-06-24 | 2021-10-29 | 深圳市时代速信科技有限公司 | Resonant tunneling diode terahertz oscillation source |
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| CN101432883A (en) * | 2006-03-22 | 2009-05-13 | 国立大学法人大阪大学 | Transistor element, its manufacturing method, light emitting element, and display |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106876489A (en) * | 2017-02-10 | 2017-06-20 | 西安电子科技大学 | Based on CH3NH3PbI3Two-way HHET devices of p-type of material and preparation method thereof |
| CN106876489B (en) * | 2017-02-10 | 2018-12-25 | 西安电子科技大学 | Based on CH3NH3PbI3Two-way HHET device of the p-type of material and preparation method thereof |
| CN113571998A (en) * | 2021-06-24 | 2021-10-29 | 深圳市时代速信科技有限公司 | Resonant tunneling diode terahertz oscillation source |
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Application publication date: 20120201 |