CN104735833A - Electroluminescent device based on rare earth-doped TiO2 film and manufacturing method thereof - Google Patents
Electroluminescent device based on rare earth-doped TiO2 film and manufacturing method thereof Download PDFInfo
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- CN104735833A CN104735833A CN201510044205.4A CN201510044205A CN104735833A CN 104735833 A CN104735833 A CN 104735833A CN 201510044205 A CN201510044205 A CN 201510044205A CN 104735833 A CN104735833 A CN 104735833A
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Abstract
The invention discloses an electroluminescent device based on a rare earth-doped TiO2 film. The electroluminescent device based on the rare earth-doped TiO2 film comprises a silicon substrate, a luminous layer, a first electrode layer and a second electrode layer, wherein the luminous layer is a TiO2 film doped with Tm or Er or Eu. The electroluminescent device based on the rare earth-doped TiO2 film is characterized in that a SiO2 film is arranged between the silicon substrate and the luminous layer. The electroluminescent device is of a SiO2-TiO2:RE(RE=Tm, Er and Eu) double-layer structure, electrons can accelerate in an electric field of the SiO2 film so as to form a hot carrier, in this way, the electroluminescent device based on the rare earth-doped TiO2 film can be stimulated to emit light under a low forward bias condition, and the light emitted by the electroluminescent device is characteristic light emitted by Tm3 or Er3 or Eu3 rare earth ions in the visible light region and the infrared region.
Description
Technical field
The present invention relates to electroluminescence field, particularly relate to a kind of based on rear-earth-doped TiO
2electroluminescent device of film and preparation method thereof.
Background technology
Electroluminescence, can claim electroluminescence again, is that voltage by being added in two electrodes produces electric field, by the electronics percussion luminescence center that electric field excites, and causes a kind of physical phenomenon of the leap of electron solutions level, change, composite guide photoluminescence.
Electroluminescent device is with electroluminescent principle work, and it is made up of back electrode layer, insulating barrier, luminescent layer, transparent electrode layer and surface protection film, utilizes luminescent material under electric field action, produce the characteristic of light, converts electrical energy into luminous energy.
Owing to can provide the luminescence of the not temperature influence of specific wavelength, the electroluminescent device based on rear-earth-doped semiconductor material with wide forbidden band causes to be paid close attention to widely.Rear-earth-doped ZnS film is adopted once to cause commercial research (list of references: V.Marrello and A.Onton widely as the membrane electro luminescent device (TFEL) of fluorophor, Applied Physics Letters 34,525 (1979); Y.R.Do, Y.C.Kim, S.H.Cho, J.H.Ahn and J.G.Lee, AppliedPhysics Letters 82,4172 (2003)).Above-mentioned device mainly adopts the structure of metal-insulator semiconductor-insulator-metal, and electrical pumping difficulty, operating voltage is higher.Rear-earth-doped luminescent device based on Group III-V semiconductor has also carried out more research (list of references: Joo Han Kim, N.Shepherd, M.R.Davidson, and Paul H.Holloway, Applied Physics Letters 83,4279 (2003); D.S.Lee and A.J.Steckl, Applied Physics Letters 80,1888 (2002)), but its preparation requires higher to vacuum equipment, system operating voltage is high, and wherein indispensable Ga and In is faced with the restriction of scarcity of resources.Therefore, explore other there is resources advantage, prepare simple rare earth-doped semiconductor luminescent device and have important practical significance.
At TiO
2in there is number of drawbacks, wherein some defect, as Lacking oxygen, can be used as the approach that charge carrier good fortune penetrates compound, become luminescence center.Simultaneously lower phonon energy (< 700cm
-1) make TiO
2the probability that the non-good fortune of middle electronics penetrates transition is lower, and is easy to the injection and the transmission that realize charge carrier.Application number is that the patent of invention of 200710070055.X discloses a kind of electroluminescent device and preparation method thereof, by silicon substrate, from bottom to top successively at the TiO of silicon substrate front deposition
2the Ohm contact electrode composition of film and ITO electrode and silicon substrate backside deposition, achieves the electroluminescence of the titanium dioxide on silicon substrate.
There are some researches show, realized the TiO mixing Tm, Er or Eu
2luminescence generated by light, with based on the electroluminescence of energy transferring, but based on the high strength rare earth doped Ti O of impact ionization
2the electroluminescent device of film yet there are no all reports.
For routine based on hot carrier collision excitation rare-earth luminescent center electroluminescent device for, need high electric field and relative very high voltage to excite device luminous, in existing report, luminous driving voltage based on the electroluminescent device of impact ionization lies prostrate more 30 to two hundred, and driving voltage is higher.
Summary of the invention
For the deficiency that prior art exists, the object of the invention is to open one based on rear-earth-doped TiO
2electroluminescent device of film and preparation method thereof, electroluminescent device of the present invention is the luminescent device based on collision excitation rare earth ion that one effectively can excite under low-voltage (< 10V).
For achieving the above object, the invention provides following technical scheme:
A kind of based on rear-earth-doped TiO
2the electroluminescent device of film, comprises silicon substrate, luminescent layer and the first electrode layer and the second electrode lay, and described luminescent layer is the TiO of doping Tm, Er or Eu
2film, is characterized in that, is provided with SiO between described silicon substrate and luminescent layer
2film.
Of the present invention based on rear-earth-doped TiO
2the electroluminescence of the electroluminescent device of film stems from collision excitation mechanism.In this case, the electronics in luminescent layer can obtain enough energy to excite RE wherein
3+ion (rare earth ion) is luminous.
When the first electrode layer connects positive voltage, and when the second electrode lay at the silicon substrate back side connects negative voltage, due to SiO
2the resistance ratio TiO of film
2the resistance of film is large, and the bias voltage that major part is applied on device drops to SiO
2on film, when applying sufficiently high bias voltage, electronics is injected into SiO by tunneling mechanism from substrate
2in film, and at SiO
2accelerate in the electric field of film, a part of electronics will obtain sufficiently high kinetic energy to be become so-called " hot electron ", and subsequently, this part hot electron enters into TiO
2in film and Derict impact excitation RE wherein
3+ion, produces RE
3+the characteristic luminescence of ion.
In the electroluminescent device of routine, the generation of hot carrier and be all carry out in single luminescent layer usually to the collision excitation of rare earth ion, the electric field being applied to luminescent layer needs up to 1 ~ 3MV/cm effectively to produce hot carrier, for producing so high electric field, the driving voltage be applied on electroluminescent device generally will at tens of volt and even 220V.Of the present invention based on rear-earth-doped TiO in comparison
2in the electroluminescent device of film, the generation of hot carrier (electronics) occurs in SiO
2in film, and to RE
3+the collision excitation of ion occurs in TiO
2in film, electronics is at SiO
2accelerate in film, the bias voltage of the three ten-day period of hot season is enough at SiO
2hot electron is produced in film.Therefore of the present invention based on rear-earth-doped TiO
2the electroluminescent device of film greatly reduces its driving voltage.
When adopting identical luminescent layer, SiO
2the luminous intensity impact of thickness on electroluminescent device of film is comparatively large, works as SiO
2when the thickness of film is too small, the voltage be applied on this layer is lower, and in this case can accelerate to is enough to excite RE
3+the quantity of the electronics of ion greatly reduces, and result causes only has few RE
3+ion can by collision excitation, and the electroluminescence of generation is also just very weak.So preferred, described SiO
2the thickness of film is 5 ~ 30nm.
The thickness of described luminescent layer is 60 ~ 150nm.
The doping content of described luminescent layer is: 0.5 ~ 2%.
Described silicon substrate is N-type or P type <100> silicon chip.
Preferably, the resistivity of silicon chip is about 0.001 ohmcm, is of a size of 15 × 15mm
2, thickness is 625 microns.
The invention also discloses based on rear-earth-doped TiO
2the preparation method of the electroluminescent device of film, comprises the following steps: prepare SiO in silicon substrate front by thermal oxidation method
2film; From bottom to top successively at SiO
2by the TiO of magnetron sputtering method dopant deposition Tm, Er or Eu on film
2film and DC sputtering deposition of first electrode layer; The second electrode lay is deposited by DC sputtering at the silicon substrate back side.
Preferably, the temperature of thermal oxidation is 1100 DEG C, and the thermal oxidation time is 6 ~ 14min.
Present invention also offers based on rear-earth-doped TiO
2the luminescent method of the electroluminescent device of film: the voltage applying 8.0 ~ 9.0 volts between the first electrode layer and the second electrode lay.
Beneficial effect of the present invention is:
Electroluminescent device provided by the invention is SiO
2-TiO
2: RE (RE=Tm, Er, Eu) double-decker, electronics can at SiO
2accelerate in the electric field of film to form hot carrier, make of the present invention based on rear-earth-doped TiO
2the electroluminescent device of film can under lower forward bias stimulated luminescence, the light sent is Tm
3+, Er
3+or Eu
3+rare earth ion is at the characteristic luminescence of visible region and infrared region.
Accompanying drawing explanation
Fig. 1 is for the present invention is based on rear-earth-doped TiO
2the structural representation of the electroluminescent device of film;
Fig. 2 is the luminous spectrogram of electroluminescent device under different voltage of embodiment 1;
Fig. 3 is the luminous spectrogram of the visible region of electroluminescent device under different voltage of embodiment 2;
Fig. 4 is the luminous spectrogram in the infrared light district of electroluminescent device under different voltage of embodiment 2;
Fig. 5 is the luminous spectrogram of electroluminescent device under different voltage of embodiment 3;
Fig. 6 is the luminous spectrogram of electroluminescent device under different voltage of embodiment 4;
Embodiment
As shown in Figure 1, a kind of based on rear-earth-doped TiO
2the electroluminescent device of film, comprises silicon substrate 1, the SiO in silicon substrate 1 front
2film 2, SiO
2film deposits successively luminescent layer 3 and the first electrode layer 4, silicon substrate 1 backside deposition has the second electrode lay 5.
Embodiment 1
(1) get resistivity to be about 0.001 ohmcm, to be of a size of 15 × 15mm
2, thickness 625 microns N-type <100> silicon chip as silicon substrate, after cleaning, silicon chip is placed in temperature 1100 DEG C, be full of flowing oxygen heat-treatment furnace process 8min, obtain the SiO that thickness is 20nm
2film.
(2) surface there is SiO
2the silicon chip of film is placed in radio frequency sputtering cavity, uses vacuum pump that pressure in cavity is evacuated to 4 × 10
-3after Pa, pass into pure Ar gas to 1Pa, use and be mixed with Tm
2o
3tiO
2ceramic target is carried out sputtering and is carried out deposit film, and the power of applying is 120W; In deposition process, silicon substrate temperature remains on 100 DEG C, and sedimentation time is 1 hour; Be placed in oxygen atmosphere by depositing the film obtained subsequently, in 700 DEG C of heat treatments 1 hour, the TiO of Tm was mixed in final formation
2film, film thickness is about 80nm.
(3) TiO of Tm is being mixed
2film is about the transparent ITO electrode of 150nm by DC reactive sputtering deposit thickness, use DC sputtering deposit thickness to be about the Au Ohm contact electrode of 150nm at the silicon substrate back side, both are all diametrically the circle of 10mm.
(4) analyze through Rutherford backscattering (RBS), mix the TiO of Tm
2in film, the ratio of Tm/Ti is about 0.005.
Au Ohm contact electrode in above-mentioned electroluminescent device is connect negative voltage, and ITO electrode connects positive voltage, tests the electroluminescent spectrum of this device under different voltage (EL), and as shown in Figure 2, as we know from the figure, electroluminescence collection of illustrative plates is Tm to result
3+the characteristic luminescence peak of ion, along with executing alive increase, electroluminescent intensity also increases thereupon.
Embodiment 2
(1) get resistivity to be about 0.001 ohmcm, to be of a size of 15 × 15mm
2, thickness 625 microns N-type <100> silicon chip as silicon substrate, after cleaning, silicon chip is placed in temperature 1100 DEG C, be full of flowing oxygen heat-treatment furnace process 6min, obtain the SiO that thickness is 10nm
2film.
(2) surface there is SiO
2the silicon chip of film is placed in radio frequency sputtering cavity, uses vacuum pump that pressure in cavity is evacuated to 4 × 10
-3after Pa, pass into pure Ar gas to 1Pa, use and be mixed with Er
2o
3tiO
2ceramic target is carried out sputtering and is carried out deposit film, and the power of applying is 120W; In deposition process, silicon substrate temperature remains on 100 DEG C, and sedimentation time is 1 hour; Be placed in oxygen atmosphere by depositing the film obtained subsequently, in 700 DEG C of heat treatments 1 hour, the TiO of Er was mixed in final formation
2film, film thickness is about 80nm.
(3) TiO of Er is being mixed
2film is about the transparent ITO electrode of 150nm by DC reactive sputtering deposit thickness, use DC sputtering deposit thickness to be about the Au Ohm contact electrode of 150nm at the silicon substrate back side, both are all diametrically the circle of 10mm.
(4) analyze through Rutherford backscattering (RBS), mix the TiO of Er
2in film, the ratio of Er/Ti is about 0.02.
Au Ohm contact electrode in above-mentioned electroluminescent device is connect negative voltage, and ITO electrode connects positive voltage, tests the electroluminescent spectrum of this device under different voltage (EL), and as shown in Figures 3 and 4, electroluminescence collection of illustrative plates is Er to result
3+ion is at characteristic luminescence peak that is visible and infrared region, and along with executing alive increase, electroluminescent intensity also increases thereupon.
Embodiment 3
(1) get resistivity to be about 0.001 ohmcm, to be of a size of 15 × 15mm
2, thickness 625 microns N-type <100> silicon chip as silicon substrate, after cleaning, silicon chip is placed in temperature 1100 DEG C, be full of flowing oxygen heat-treatment furnace process 10min, obtain the SiO that thickness is 30nm
2film.
(2) surface there is SiO
2the silicon chip of film is placed in radio frequency sputtering cavity, uses vacuum pump that pressure in cavity is evacuated to 4 × 10
-3after Pa, pass into pure Ar gas to 1Pa, use and be mixed with Eu
2o
3tiO
2ceramic target is carried out sputtering and is carried out deposit film, and the power of applying is 120W; In deposition process, silicon substrate temperature remains on 100 DEG C, and sedimentation time is 1 hour; Be placed in oxygen atmosphere by depositing the film obtained subsequently, in 700 DEG C of heat treatments 1 hour, the TiO of Eu was mixed in final formation
2film, film thickness is about 80nm.
(3) TiO of Eu is being mixed
2film is about the transparent ITO electrode of 150nm by DC reactive sputtering deposit thickness, use DC sputtering deposit thickness to be about the Au Ohm contact electrode of 150nm at the silicon substrate back side, both are all diametrically the circle of 10mm.
(4) analyze through Rutherford backscattering (RBS), mix the TiO of Eu
2in film, the ratio of Eu/Ti is all about 0.03.
Au Ohm contact electrode in above-mentioned electroluminescent device is connect negative voltage, and ITO electrode connects positive voltage, tests the electroluminescent spectrum of this device under different voltage (EL), and as shown in Figure 5, as we know from the figure, electroluminescence collection of illustrative plates is Eu to result
3+the characteristic luminescence peak of ion, along with the increase of the voltage applied, electroluminescent intensity also increases thereupon.
Embodiment 4
(1) get resistivity to be about 0.002 ohmcm, to be of a size of 15 × 15mm
2, thickness 675 microns P type <100> silicon chip as silicon substrate, after cleaning, silicon chip is placed in temperature 1100 DEG C, be full of flowing oxygen heat-treatment furnace process 8min, obtain the SiO that thickness is 20nm
2film.
(2) surface there is SiO
2the silicon chip of film is placed in radio frequency sputtering cavity, uses vacuum pump that pressure in cavity is evacuated to 4 × 10
-3after Pa, pass into pure Ar gas to 1Pa, use and be mixed with Tm
2o
3tiO
2ceramic target is carried out sputtering and is carried out deposit film, and the power of applying is 120W; In deposition process, silicon substrate temperature remains on 100 DEG C, and sedimentation time is 1 hour; Be placed in oxygen atmosphere by depositing the film obtained subsequently, in 700 DEG C of heat treatments 1 hour, the TiO of Tm was mixed in final formation
2film, film thickness is about 80nm.
(3) TiO of Tm is being mixed
2film is about the transparent ITO electrode of 150nm by DC reactive sputtering deposit thickness, use DC sputtering deposit thickness to be about the Au Ohm contact electrode of 150nm at the silicon substrate back side, both are all diametrically the circle of 10mm.
(4) analyze through Rutherford backscattering (RBS), mix the TiO of Tm
2in film, the ratio of Tm/Ti is about 0.01.
Au Ohm contact electrode in above-mentioned electroluminescent device is connect negative voltage, and ITO electrode connects positive voltage, tests the electroluminescent spectrum of this device under different voltage (EL), and as shown in Figure 6, as we know from the figure, electroluminescence collection of illustrative plates is respectively Tm to result
3+the characteristic luminescence peak of ion, along with the increase of the voltage applied, electroluminescent intensity also increases thereupon.
Claims (8)
1. one kind based on rear-earth-doped TiO
2the electroluminescent device of film, comprises silicon substrate, luminescent layer and the first electrode layer and the second electrode lay, and described luminescent layer is the TiO of doping Tm, Er or Eu
2film, is characterized in that, is provided with SiO between described silicon substrate and luminescent layer
2film.
2. according to claim 1 based on rear-earth-doped TiO
2the electroluminescent device of film, is characterized in that, described SiO
2the thickness of film is 5 ~ 30nm.
3. according to claim 1 based on rear-earth-doped TiO
2the electroluminescent device of film, is characterized in that, the thickness of described luminescent layer is 60 ~ 150nm.
4. according to claim 1 based on rear-earth-doped TiO
2the electroluminescent device of film, is characterized in that, the doping content of described luminescent layer is: 0.5 ~ 2%.
5. according to claim 1 based on rear-earth-doped TiO
2the electroluminescent device of film, is characterized in that, it is characterized in that, described silicon substrate is N-type or P type <100> silicon chip.
6. according to claim 1 based on rear-earth-doped TiO
2the preparation method of the electroluminescent device of film, is characterized in that, comprises the following steps: prepare SiO in silicon substrate front by thermal oxidation method
2film; From bottom to top successively at SiO
2by the TiO of magnetron sputtering method dopant deposition Tm, Er or Eu on film
2film and DC sputtering deposition of first electrode layer; The second electrode lay is deposited by DC sputtering at the silicon substrate back side.
7. preparation method according to claim 6, is characterized in that, the temperature of thermal oxidation is 1100 DEG C, process 6 ~ 14min.
8. according to any one of Claims 1 to 5 based on rear-earth-doped TiO
2the luminescent method of the electroluminescent device of film, is characterized in that, applies the voltage of 8.0 ~ 9.0 volts between the first electrode layer and the second electrode lay.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107321392A (en) * | 2017-07-28 | 2017-11-07 | 重庆理工大学 | Photocatalysis hollow quartz fiber and preparation method |
| CN109143745A (en) * | 2017-06-27 | 2019-01-04 | 深圳市光峰光电技术有限公司 | Shine collector, luminaire and projection light source |
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| CN1073314A (en) * | 1992-07-25 | 1993-06-16 | 天津理工学院 | Laminated optimiging new type film electroluminescence device |
| JP2007173739A (en) * | 2005-12-26 | 2007-07-05 | Tokyo Univ Of Science | Zinc oxide optical device, method of utilizing zinc oxide optical device and zinc oxide semiconductor laser |
| CN101630713A (en) * | 2009-08-03 | 2010-01-20 | 浙江大学 | Ultraviolet electroluminescence device based on titanium dioxide film |
| CN102364708A (en) * | 2011-11-14 | 2012-02-29 | 浙江大学 | Electroluminescence device and manufacturing method thereof |
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2015
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Patent Citations (4)
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| CN1073314A (en) * | 1992-07-25 | 1993-06-16 | 天津理工学院 | Laminated optimiging new type film electroluminescence device |
| JP2007173739A (en) * | 2005-12-26 | 2007-07-05 | Tokyo Univ Of Science | Zinc oxide optical device, method of utilizing zinc oxide optical device and zinc oxide semiconductor laser |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109143745A (en) * | 2017-06-27 | 2019-01-04 | 深圳市光峰光电技术有限公司 | Shine collector, luminaire and projection light source |
| CN107321392A (en) * | 2017-07-28 | 2017-11-07 | 重庆理工大学 | Photocatalysis hollow quartz fiber and preparation method |
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