CN105261713A - Optical-up converter capable of achieving conversion from near infrared light to visible light and preparation method thereof - Google Patents
Optical-up converter capable of achieving conversion from near infrared light to visible light and preparation method thereof Download PDFInfo
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Abstract
The invention discloses an optical-up converter capable of achieving conversion from near infrared light to visible light and a preparation method thereof. The optical-up converter is characterized in that the optical-up converter is a Ge/OLED optical-up converter which is obtained in a way that an organic light emitting diode (OLED) is integrated on an infrared-sensitive crystal Ge material; the infrared-sensitive crystal Ge material can be a Si-based Ge quantum dot, a Si-based Ge thin film or a single-crystal Ge substrate; and the OLED thin film comprises an organic hole injection layer, an organic hole transmission layer, an organic light emitting layer, an organic electronic transmission layer and an organic injection layer. According to the invention, by taking advantages of the infrared adsorption characteristics of the crystal Ge material and the visible light emitting characteristics of the OLED, under the effects of the external bias voltage, conversion from near infrared light to visible light can be achieved; and the optical-up converter is compatible with a Si-based integration circuit, so cost and complexity of infrared imaging can be greatly reduced.
Description
Technical field
The present invention relates to infrared imagery technique field, it is different from traditional infrared focal plane imaging technology, be specifically related to the Ge/OLED light up-conversion device of direct evaporation Organic Light Emitting Diode (OLED) film on crystal Ge material, under the effect of bias voltage outside, the conversion of near infrared signal to visible light signal can be realized, can be applicable to the image detection of object at night.
Background technology
Infrared imagery technique has important application in medical treatment, military affairs, night vision, satellite and the field such as civilian, is a focus of scientific research always.At present, traditional infrared focal plane imaging technology is the most ripe a kind of infrared imagery technique.But mainly there is following two problems in it: (1) detector and the interconnected of reading circuit are needed growth up to ten thousand indium posts and completed by upside-down mounting interconnection technology, this considerably increases process complexity and production cost, and there is integrity problem; (2) signal of telecommunication that Infrared Detectors obtains not only needs to read through reading circuit to obtain digital signal, and the very complicated and easy distortion by the process of computer processing digital signal also original image.In recent decades, researchers propose and a kind ofly realize the light upconverter of low-frequency infrared light to the near-infrared of higher-frequency or the conversion of high-frequency visible ray, and this avoids focal plane imaging technology institute problems faced to a great extent.In the eurypalynous smooth upconverter of crowd, the PD-LED light upconverter that Infrared Detectors (PD) and light-emitting diode (LED) are coupled to form is a kind of light upconverter with far-reaching application prospect.
Based on the difference of the semi-conducting material of PD and LED unit, light upconverter can be divided three classes: the light upconverter (being called for short PD-OLED light upconverter) of pure inorganic smooth upconverter, pure organic smooth upconverter and inorganic-organic hybridization.Pure inorganic smooth upconverter, because inorganic semiconductor material growth is subject to the restriction of Lattice Matching and Material selec-tion, the minimal wave length after realizing conversion under normal temperature is also only 0.87 μm.Pure organic smooth upconverter, although its growth cost is low and inherently can launch visible ray, organic semiconducting materials has very wide band gap width, and its infrared response wavelength is not all more than 1 μm at present, and this does not meet the requirement of infrared imaging.Since Deng Qingyun professors in 1987 and Vanslyke propose organic electroluminescence device, the OLED being described as " dreamlike display " achieves the development of advancing by leaps and bounds.In recent decades, a kind of light upconverter having more application prospect---PD-OLED light upconverter is also suggested thereupon and the parent being subject to more and more researchers looks at.Because organic material is by the restriction of Lattice Matching, can at any deposited on materials, inorganic material Infrared Detectors and OLED is integrated becomes freer.Therefore, the advantage that PD-OLED light upconverter has gathered Infrared Detectors and Organic Light Emitting Diode in one, can realize near, in, far infrared changes to the high efficiency of red, green, blue three primary colors visible ray.
Ge material has a lot of proper property advantage compared to Si material, such as there is large Exciton Bohr Radius (Ge:24.3nm, Si:4.9nm), high carrier mobility (mobility in electronics and hole is 2.75 times and 4 times of Si respectively), little energy bandgaps (be 0.8eV and 0.67eV for Ge direct band gap and indirect band gap respectively; Si direct band gap and indirect band gap are respectively 3.2eV and 1.12eV) and there is strong near infrared absorption.The present invention adopts crystal Ge material as the material of Infrared Detectors part, and integrate a kind of Ge/OLED light up-conversion device with OLED, utilize the INFRARED ABSORPTION performance of crystal Ge material and OLED to send out the characteristic of visible ray, the light up-conversion device that a kind of new near-infrared is changed to visible ray can be realized.
Summary of the invention
Provided by the inventionly a kind ofly can realize light up-conversion device that near-infrared changes to visible ray and preparation method thereof, its integrated device architecture schematic diagram refers to accompanying drawing 1, concrete preparation method, refers to accompanying drawing 2.It is characterized in that device part from top to bottom comprises successively: anode layer, crystal Ge material, insulating barrier, OLED thin layer and cathode layer.
The Ni that Al or 15nm that anode ohmic contact electrode employing Grown by Magnetron Sputtering 100nm is thick is thick, by annealing in process, forms ohmic contact with the N-shaped Si in Si base Ge quantum dot or Si base Ge film or p-type monocrystalline Ge substrate.
Crystal Ge material in the present invention can be Si base Ge quantum dot, Si base Ge film or monocrystalline Ge substrate.Wherein, the structure of Si base Ge quantum dot is N-shaped Si substrate/multilayer Ge quantum dot/p-type Si; The structure of Si base Ge film is n-Si substrate/monocrystalline Ge film; Monocrystalline Ge substrate is p-type doping.
Si base Ge quanta point material in the present invention, adopts ion beam sputtering technology to obtain.Due to the existence of quantum confined effect, show obvious INFRARED ABSORPTION performance at a certain infrared wavelength region near the mid-point on central axis.That is, using Si base Ge quantum dot as the infrared-sensitive material of light upconverter, can meet with a response the light upconverter that spectrum is narrower, conversion efficiency is higher.
Si base Ge film in the present invention, uses hypo-hyperthermia two-step method growing method to obtain by magnetron sputtering technique.Due to the difference of the thermal coefficient of expansion between Si and Ge, Ge film exhibits is tensile strain, and tensile strain can increase the carrier mobility of material, is conducive to obtaining of high-performance optical upconverter; Under normal temperature, the photoluminescence intensity of its accurate direct band gap (corresponding wavelength is 1.55 μm) is obviously better than the photoluminescence intensity of indirect band gap, this means that the Ge/OLED light upconverter formed using Si base Ge film as infrared-sensitive material not only has wider infrared response but also has stronger infrared response at 1.55 mu m wavebands.In addition, the interfacial structure of the Ge/OLED light upconverter that this Si base Ge film is formed as infrared-sensitive material is i-Ge/ organic substance, similar to the i-InGaAs/C60 interfacial structure that Chen proposes (see document: Chen, AdvMater, 24 (23), 3138 (2012)), it is expected to realize without pixel imaging, and this greatly can reduce the production cost of light up-conversion device and improve success rate.
Monocrystalline Ge material has an indirect band gap and an accurate direct band gap, just obviously can observe the luminescence generated by light signal relevant to them at normal temperatures, its photoluminescence spectra is wide compared to direct band gap material and low-dimensional quantum trap, quantum wire and quanta point material.Therefore using body Ge material as the light upconverter of crystal Ge material, there is wider infrared response.Monocrystalline Ge material at 1000 ~ 1900nm infrared band compared to body Si material, shows obvious INFRARED ABSORPTION performance, refers to accompanying drawing 3.
Before vacuum evaporation OLED thin layer, first on crystal Ge material, grow the thick SiO of 200nm
2or SiN
xinsulating barrier.Etch this insulating barrier with lithographic technique again, become 1mm × 1mm, the square window of the mm sizes such as 2mm × 2mm, 3mm × 3mm.Sputtering this insulating barrier is to prevent the cathode electrode material of top device from directly contacting with crystal Ge, forms metal-semiconductor-metal and conducting, and then affect device operation; Etching isolation layer window is to control effective light-emitting zone.A kind of in the present invention can realize the efficient lighting area of light up-conversion device that near-infrared changes to visible ray and preparation method, is determined by the size of etched window.
The laminated construction sketch of the OLED thin layer in the present invention, refers to accompanying drawing 4, comprises organic hole injection layer, organic cavity transmission layer, organic luminous layer, organic electron transport layer and organic electron injecting layer successively from top to bottom.Wherein, organic hole implanted layer can adopt CuPc, PTCDA, MnO
3or V
2o
5deng transition metal oxide doping organic substance material; Organic cavity transmission layer can adopt NPB, TCTA or α-NPD; Organic luminous layer can adopt the luminescent layer of material as OLED of fluorescence and phosphorescence two kinds of emission mechanisms, and Alq selected by green-emitting fluorescent emissive material
3: C545T, its luminescence center wavelength is near 520nm, and green glow phosphorescent emissive material selects CBP:Irppy
3, its luminescence center wavelength location is also near 520nm; Organic electron transport layer can adopt Alq3, Bebq2, TPBi or BCP; Organic electron injecting layer can adopt LiF or LiF/C60 composite material.
A kind of light up-conversion device that can realize near-infrared and change to visible ray provided by the invention, its visible ray is top-emission pattern.And the different emission modes of visible ray can be realized by the material of control cathode layer and thickness.Therefore, device is for realizing top-emission, and negative electrode is necessary for semitransparent electrode, can be the one in Al (25nm), Al:Ag (5:20nm) or Mg:Ag (10:1nm) three kinds of electrode structures.
A kind of light up-conversion device that can realize near-infrared and change to visible ray provided by the invention, not only can realize the conversion of near-infrared to visible ray, and the crystal Ge material of different structure can be selected to realize the light upconverter of the outer response characteristic of Different Red.
Accompanying drawing explanation
Fig. 1 is the structural representation sketch of Ge/OLED light up-conversion device.
Fig. 2 is preparation technology's flow process of Ge/OLED light upconverter.Wherein, (a) SiO
2or SiN
xthe growth of insulating barrier, obtaining of (b) square window, the growth of (c) anode material, the growth of (d) OLED thin layer, the growth of (e) transparency electrode.
Fig. 3 is the normalization infrared absorption pattern of body Si and body Ge.Wherein, in 1000 ~ 1900nn infrared wavelength range, be almost transparent for body Si, and crystal Ge show obvious absorbent properties.
Fig. 4 is the laminated construction sketch of OLED.Comprise hole injection layer, hole transmission layer, light-emitting layer, electron transfer layer, electron injecting layer.
Fig. 5 is the surface topography map of crystal Ge material.Wherein, figure (a) is the three-dimensional AFM figure of the individual layer Ge quantum dot of ion beam sputtering growth, the bottom width of quantum dot be 50 ± 15nm, be highly 9 ± 4nm, density up to ~ 2 ' 10
9cm
-2, in distribution as unimodal; Figure (b) is the two-dimentional AFM figure of the Si base Ge film of Grown by Magnetron Sputtering, and its surface roughness is 0.62nm; Figure (c) is p-type monocrystalline Ge substrate surface two dimension AFM figure, and its surface roughness is 0.53nm.
Embodiment
Provided by the inventionly a kind ofly can realize light up-conversion device that near-infrared changes to visible ray and preparation method, different according to the structure of crystal Ge material, adopt three embodiment explanations.
Embodiment 1:
Adopt Si base Ge quantum dot as crystal Ge material.The roughly step of ion beam sputtering technology growth Si base Ge quantum dot is: (1) is on N-shaped heavy doping Si (001) substrate of about 500 μm at thickness, grows the Si resilient coating of 50nm at 700 DEG C of temperature; (2) deposit the Ge of 2.3nm again, Ge atom is according to the pattern formation Ge quantum dot of first stratiform island growth again; (3) the Si separator of regrowth 30nm; (4) repeat step (2) and (3) and obtain the multilayer Ge quantum dot that periodicity is N layer; (5) on multilayer Ge quantum dot, finally grow the p-type Si layer of one deck 200nm, make it form a p-i-n junction structure Ge quantum dot infrared detector on the whole.Wherein, according to the 3 d surface topography figure of above growth parameter(s) at the individual layer Ge quantum dot of N-shaped Si Grown, accompanying drawing 5 (a) is referred to.
The SiO that direct growth one deck 200nm is thick on p-i-n junction structure Ge quantum dot infrared detector
2or SiN
xinsulating barrier.And wear this insulating barrier with lithographic technique etching, make it form the square window of a mm size, size can be 1 × 1mm, 2 × 2mm, 3 × 3mm etc.Or, with lithographic technique, p-i-n junction structure Ge quantum dot infrared detector is etched into the little table top of square of mm size, relends with the thick SiO of mask plate growth 200nm
2or SiN
xinsulating barrier (ensure to grown insulating barrier in non-mesa region, little table top does not grow insulating barrier, and then provide growth window for OLED).
Anode ohmic contact layer, adopt magnetically controlled sputter method to grow the thick Al of 100nm under N-shaped Si substrate back normal temperature, 400 DEG C of quick thermal annealing process 1min, can realize good ohmic contact afterwards.
The OLED structure of vacuum evaporation refers to accompanying drawing 4, comprises hole injection layer, hole transmission layer, luminescent layer, electron transfer layer and electron injecting layer.Wherein, layers of material choose and parameter as follows:
Hole injection layer adopts CuPc material, and thickness is 25nm;
Hole transmission layer adopts NPB material, and thickness is 45nm;
Luminescent layer can adopt the one in green-emitting fluorescent emissive material and phosphorescent emissive material, and thickness is 30nm, and wherein, green-emitting fluorescent emissive material adopts Alq3:C545T, and green glow phosphorescent emissive material adopts CBP:Irppy3;
Electron transfer layer adopts Alq
3material, thickness is 30nm;
Electron injecting layer adopts LiF or LiF and C
60composite structure, thickness is 1nm.
Cathode layer materials must ensure that the VISIBLE LIGHT EMISSION pattern of device is top-emission pattern.The growth of cathode material completes in the vacuum evaporation cavity of growth OLED thin layer, and cathode layer materials can be one of following three kinds of structures: (1) first grows the thick Al of 5nm, the Ag that regrowth 20nm is thick; (2) the thick Al of 25nm is grown; (3) the thick Mg of 10nm is first grown, the Ag that regrowth 1nm is thick.
This Ge/OLED light up-conversion device can realize the conversion of infrared light to the green glow of centre wavelength near ~ 520nm, and its infrared response spectrum is narrow, conversion efficiency is higher.
Embodiment 2:
Adopt Si base Ge film as crystal Ge material.Wherein, Si (100) substrate is N-shaped heavy doping, and thickness is about 500 μm.Si base Ge film, uses magnetron sputtering technique to adopt now the hypo-hyperthermia two-step method growing technology of comparative maturity to obtain.Its roughly growth step be: (1) is 1.5Pa at sputtering pressure, under sputtering power is 50W, growth temperature is the condition of 350 DEG C, grows the low temperature Ge layer of 60nm on a si substrate; (2) operating air pressure is constant, and sputtering power is 100W, grows the high temperature Ge layer of 1 ~ 2.5 μm at 650 DEG C of temperature.According to testing growth parameter(s) above, the two-dimensional surface shape appearance figure of the Si base Ge film obtained, refers to accompanying drawing 5 (b).
Si base Ge film grows the thick SiO of one deck 200nm
2or SiN
xinsulating barrier.And wear this insulating barrier with lithographic technique etching, make it form the square window of a mm size, size can be 1 × 1mm, 2 × 2mm, 3 × 3mm etc.
Anode ohmic contact layer, adopt magnetically controlled sputter method under the back side normal temperature of Si base Ge film, grow the thick Al of 100nm, 400 DEG C are carried out quick thermal annealing process 1min afterwards, can realize good ohmic contact.
The OLED structure of vacuum evaporation refers to accompanying drawing 4, comprises hole injection layer, hole transmission layer, luminescent layer, electron transfer layer and electron injecting layer.Wherein, layers of material choose and parameter as follows:
Hole injection layer adopts CuPc material, and thickness is 25nm;
Hole transmission layer adopts NPB material, and thickness is 45nm;
Luminescent layer can adopt the one in green-emitting fluorescent emissive material and phosphorescent emissive material, and thickness is 30nm, and wherein, green-emitting fluorescent emissive material adopts Alq3:C545T, and green glow phosphorescent emissive material adopts CBP:Irppy3;
Electron transfer layer adopts Alq
3material, thickness is 30nm;
Electron injecting layer adopts LiF or LiF and C
60composite structure, thickness is 1nm.
Cathode layer must ensure that device is top light emission mode, optional equally by the one in following three kinds of structures: (1) first grows the thick Al of 5nm, the Ag that regrowth 20nm is thick; (2) the thick Al of 25nm is grown; (3) the thick Mg of 10nm is first grown, the Ag that regrowth 1nm is thick.The growth of cathode material completes in the vacuum evaporation cavity of growth OLED thin layer.
This Ge/OLED light up-conversion device can realize the conversion of infrared light to the green glow of 520nm of 1000 ~ 1900nm scope, and is expected to realize without pixel imaging.
Embodiment 3:
Direct employing monocrystalline Ge substrate is as crystal Ge material.P-type Ge material is easier than N-shaped Ge material forms ohmic contact wherein with metal, and the monocrystalline Ge substrate therefore selected is p-type doping, and its two-dimensional surface shape appearance figure, refers to accompanying drawing 5 (c).
At the SiO that p-type Ge (001) Grown one deck 200nm is thick
2or SiN
xinsulating barrier.And wear this insulating barrier by photoetching or plasma etching technology etching, make it form the square window of a mm size, size can be 1 × 1mm, 2 × 2mm, 3 × 3mm etc.
Anode ohmic contact layer, adopt magnetically controlled sputter method under the back side normal temperature of Ge substrate, grow the thick Ni of thick Al or 15nm of 100nm, 400 DEG C are carried out quick thermal annealing process 1min afterwards, can realize good ohmic contact.
The OLED structure of vacuum evaporation refers to accompanying drawing 4, comprises hole injection layer, hole transmission layer, luminescent layer, electron transfer layer and electron injecting layer.Wherein, layers of material choose and parameter as follows:
Hole injection layer adopts CuPc material, and thickness is 25nm;
Hole transmission layer adopts NPB material, and thickness is 45nm;
Luminescent layer can adopt the one in green-emitting fluorescent emissive material and phosphorescent emissive material, and thickness is 30nm, and wherein, green-emitting fluorescent emissive material adopts Alq3:C545T, and green glow phosphorescent emissive material adopts CBP:Irppy3;
Electron transfer layer adopts Alq
3material, thickness is 30nm;
Electron injecting layer adopts LiF or LiF and C
60composite structure, thickness is 1nm.
Cathode layer also must ensure that device is top light emission mode, optional equally with the one in following three kinds of structures: Al (5nm)/Ag (20nm); (2) Al (25nm); (3) Mg (10nm)/Ag (1nm).The growth of cathode material completes in the vacuum evaporation cavity of growth OLED thin layer.
The infrared light that this Ge/OLED light up-conversion device can realize 1000 ~ 1900nm wave-length coverage is the conversion of the green glow of 520nm to centre wavelength.
Claims (7)
1. can realize the light up-conversion device that near-infrared is changed to visible ray, it is characterized in that comprising successively from top to bottom: anode layer, crystal Ge material, insulating barrier, OLED thin layer and cathode layer.
2. a kind of light up-conversion device that can realize near-infrared and change to visible ray according to claim 1, is characterized in that described anode layer is positioned at the crystal Ge material back side, adopts metal A l or Ni material.
3. a kind of light up-conversion device that can realize near-infrared and change to visible ray according to claim 1, is characterized in that described crystal Ge material can be a kind of structure in Si base Ge quantum dot, Si base Ge film and monocrystalline Ge substrate.
4. a kind of light up-conversion device that can realize near-infrared and change to visible ray according to claim 1, is characterized in that described insulating barrier is positioned on crystal Ge material, selects thickness to be the SiO of 200nm
2or SiN
x.
5. a kind of light up-conversion device that can realize near-infrared and change to visible ray according to claim 1, it is characterized in that described OLED thin layer is that direct evaporation is on crystal Ge material, structure is from top to bottom followed successively by organic hole implanted layer, organic cavity transmission layer, organic luminous layer, organic electron transport layer and organic electron injecting layer, wherein:
Organic hole implanted layer can be CuPc, PTCDA, MnO
3or V
2o
5deng a kind of material in transition metal oxide doping organic substance material;
Organic cavity transmission layer can be a kind of material in NPB, TCTA and α-NPD;
Organic luminous layer can determine corresponding light-emitting material according to the wave-length coverage of required transmitting visible ray;
Organic electron transport layer can be a kind of material in Alq3, Bebq2, TPBi or BCP;
Organic electron injecting layer can be a kind of material in LiF or LiF/C60 composite material.
6. a kind of light up-conversion device that can realize near-infrared and change to visible ray according to claim 1, it is characterized in that described cathode layer is positioned on OLED thin layer, can by Al (25nm), the one in Al:Ag (5:20nm) or Mg:Ag (10:1nm) three kinds of structures is formed.
7. can realize a preparation method for the light up-conversion device that near-infrared is changed to visible ray, it is characterized in that the method comprises the following steps:
(1) at N-shaped Si Grown multilayer Ge quantum dot or Ge film, or directly clean Ge substrate, obtain crystal Ge material;
(2) on crystal Ge material, the thick SiO of one deck 200nm is grown
2or SiN
xinsulating barrier;
(3) form a square window figure by standard photolithography techniques, and wear the square window that this insulating barrier obtains mm size, as being 1 × 1mm, 2 × 2mm, 3 × 3mm etc. by wet etching etching;
(4) again the crystal Ge material that this has square window come unstuck and cleaned, and growing one deck anode metal material at the crystal Ge material back side, forming Ohm contact electrode;
(5) growth that vacuum evaporation equipment cavity carries out OLED layers of material is put into;
(6) evaporation cathodic metal material.
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| CN110649083A (en) * | 2019-10-10 | 2020-01-03 | 苏州英凡瑞得光电技术有限公司 | Up-conversion device for realizing conversion from near infrared light to visible light and preparation method thereof |
| CN110649083B (en) * | 2019-10-10 | 2022-02-08 | 苏州英凡瑞得光电技术有限公司 | Up-conversion device for realizing conversion from near infrared light to visible light and preparation method thereof |
| CN111063680A (en) * | 2019-12-06 | 2020-04-24 | 北京大学深圳研究生院 | Up-conversion device based on alternating current driving planar display unit |
| CN112420810A (en) * | 2020-11-10 | 2021-02-26 | 浙江大学杭州国际科创中心 | Charge injection device based on single-layer graphene/insulating layer/silicon/germanium structure |
| CN113809252A (en) * | 2021-08-04 | 2021-12-17 | 鹏城实验室 | Up-conversion device and manufacturing method thereof |
| CN113809252B (en) * | 2021-08-04 | 2024-04-09 | 鹏城实验室 | Up-conversion device and manufacturing method thereof |
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| CN105261713B (en) | 2017-09-29 |
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