CN108063365B - Preparation method of electric pumping perovskite quantum dot laser - Google Patents
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- H01S5/00—Semiconductor lasers
- H01S5/20—Structure or shape of the semiconductor body to guide the optical wave ; Confining structures perpendicular to the optical axis, e.g. index or gain guiding, stripe geometry, broad area lasers, gain tailoring, transverse or lateral reflectors, special cladding structures, MQW barrier reflection layers
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- H01S—DEVICES USING THE PROCESS OF LIGHT AMPLIFICATION BY STIMULATED EMISSION OF RADIATION [LASER] TO AMPLIFY OR GENERATE LIGHT; DEVICES USING STIMULATED EMISSION OF ELECTROMAGNETIC RADIATION IN WAVE RANGES OTHER THAN OPTICAL
- H01S5/00—Semiconductor lasers
- H01S5/04—Processes or apparatus for excitation, e.g. pumping, e.g. by electron beams
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01S—DEVICES USING THE PROCESS OF LIGHT AMPLIFICATION BY STIMULATED EMISSION OF RADIATION [LASER] TO AMPLIFY OR GENERATE LIGHT; DEVICES USING STIMULATED EMISSION OF ELECTROMAGNETIC RADIATION IN WAVE RANGES OTHER THAN OPTICAL
- H01S5/00—Semiconductor lasers
- H01S5/30—Structure or shape of the active region; Materials used for the active region
Abstract
A preparation method of an electrically pumped perovskite quantum dot laser comprises the following steps: step 1: etching a first photonic crystal structure on a substrate to provide a resonant cavity and a surface emitting mechanism for a laser; step 2: preparing an electron transport layer, a perovskite quantum dot layer, a hole transport layer and a positive electrode on a negative electrode in sequence to form a first substrate; and step 3: and bonding the substrate etched with the first photonic crystal structure with the first substrate to finish the preparation. The invention can obtain the electric pump perovskite quantum dot laser structure with simple structure, and can effectively improve the external quantum efficiency of the perovskite quantum dots under the electric pump.
Description
Technical Field
The invention relates to the field of quantum dot lasers, in particular to a preparation method of an electrically pumped perovskite quantum dot laser.
Background
Perovskite materials refer to a class of materials having a perovskite crystal structure. The chemical formula of the material is ABX3, and A/B/X can be replaced by a plurality of elements. The perovskite material has narrow luminescence spectrum and color purity equivalent to CdSe quantum dots; and the luminous wavelength can be regulated and controlled by chemical components and the size of the nano crystal, and the luminous wavelength can cover the whole visible light spectrum.
The perovskite material has low cost. There are currently two methods of perovskite preparation: 1. a precursor solution method; the preparation process of the precursor solution method comprises the steps of firstly mixing the precursor of the perovskite and a solvent to obtain a mixed solution, spin-coating the mixed solution on a substrate, and finally annealing to form the film. 2. A nanocrystal dispersion method; the preparation process of the nano crystal dispersion method is that the prepared colloidal perovskite nano crystal forms a film by a solution deposition method such as a spin coating method or a dropping coating method. Both methods of preparing perovskite thin films do not require high temperatures and the material costs required for the perovskite itself are not high.
The perovskite material has high quantum efficiency. Taking the mixed perovskite material as an example, photophysical measurements at day-ahead show that the perovskite internal quantum efficiency of the thin-film structure can exceed 80%, the external quantum efficiency of the nano-crystal is 90%, and the external quantum efficiency is limited by factors such as coupling. At present, the external quantum efficiency of the perovskite LED of the electric pump in a near infrared band is 8.8%, the external quantum efficiency in a green light band is 8.53%, and the external quantum efficiency in a blue light band is 1.38%. Electrically pumped perovskite LEDs suffer from the limitation of low quantum efficiency.
At present, research on perovskite lasers mainly focuses on optical pumps, and perovskite lasers of the optical pumps mainly adopt resonant cavity types such as whispering gallery modes, DFB (distributed feedback) and FP (Fabry-Perot) cavities and random lasers. However, the perovskite laser of the electric pump has not been reported, only the perovskite LED of the electric pump exists, and the quantum efficiency is only about 8.8%.
It has been known for a long time to use a photonic crystal as a resonant cavity of a laser, and Noda research group in 1999 realized a surface-emitting electrically pumped laser (Imada, Chutinan [1]) using a band edge mode of a point of a two-dimensional triangular lattice, etched a photonic crystal structure in n-InP, and then bonded an n-type region with p-InP having a quantum well, to realize an electrically pumped surface-emitting laser. Since the research on surface emitting lasers based on photonic crystals has been increasing, the structure of photonic crystals is also limited to two-dimensional and some three-dimensional based resonant cavities (Noda, Tomoda [2 ]). The lattice type of photonic crystal is also expanded to triangular lattice, tetragonal lattice (Noda, Yokoyama [3]), etc., and these photonic crystal structures are also gradually applied to other types of materials.
A photonic crystal laser for perovskite materials has not been reported so far, and patents related to photonic crystals, such as a structure having a photonic crystal and a surface emitting laser (granted patent No. CN 101369715B), utilize a band edge mode of the photonic crystal to realize surface emission, while a microcavity or an array or a coupled cavity array of the photonic crystal is not included, and none of the surface emitting lasers relates to perovskite materials and a unique electrical injection structure.
The patent literature (granted patent No. CN 101641847A) proposes photonic crystal lasers based on GaN materials, the photonic crystal layer being confined between the n-type cladding layer and the active layer or between the p-type layer and the active layer. Such a structure is not suitable for perovskite materials. At present, the electron transport layer and the hole transport layer of the perovskite are generally polymers with refractive indexes between 1.5 and 2, and the perovskite is not suitable for being used as a photonic crystal.
Disclosure of Invention
The invention aims to provide a preparation method of an electrically pumped perovskite quantum dot laser, which is easy to realize, can obtain an electrically pumped perovskite quantum dot laser structure with a simple structure, and can effectively improve the external quantum efficiency of perovskite quantum dots under an electric pump.
The invention provides a preparation method of an electrically pumped perovskite quantum dot laser, which comprises the following steps:
step 1: etching a first photonic crystal structure on a substrate to provide a resonant cavity and a surface emitting mechanism for a laser;
step 2: preparing an electron transport layer, a perovskite quantum dot layer, a hole transport layer and a positive electrode on a negative electrode in sequence to form a first substrate;
and step 3: and bonding the substrate etched with the first photonic crystal structure with the first substrate to finish the preparation.
The invention also provides a preparation method of the electrically pumped perovskite quantum dot laser, which comprises the following steps:
step 1: etching a photon first crystal structure on a substrate to provide a resonant cavity and a surface emitting mechanism for a laser;
step 2: preparing a perovskite quantum dot layer, a hole transport layer and a positive electrode on one side of the upper surface of an electron transport layer in sequence, and preparing a negative electrode on the other side of the upper surface of the electron transport layer to form a second substrate;
and step 3: and bonding the substrate etched with the first photonic crystal structure with a second substrate to finish the preparation.
The invention also provides a preparation method of the electrically pumped perovskite quantum dot laser, which comprises the following steps:
step 1: preparing an electron transport layer, a perovskite quantum dot layer, a hole transport layer and a positive electrode on a negative electrode in sequence;
step 2: and etching, namely etching the second photonic crystal structure on the positive electrode to provide a resonant cavity and a surface emitting mechanism for the laser.
The invention further provides a preparation method of the electrically pumped perovskite quantum dot laser, which comprises the following steps:
step 1: preparing an electron transport layer, a perovskite quantum dot layer, a hole transport layer and a positive electrode on a negative electrode in sequence;
step 2: and etching, namely etching a third photonic crystal structure on the negative electrode to provide a resonant cavity and a surface emitting mechanism for the laser.
The invention also provides a preparation method of the electrically pumped perovskite quantum dot laser, which comprises the following steps:
step 1: preparing an electron transport layer, a perovskite quantum dot layer and a hole transport layer on a negative electrode in sequence;
step 2: etching, namely etching the fourth photonic crystal structure on the hole transport layer to provide a resonant cavity and a surface emitting mechanism for the laser;
and step 3: and preparing a positive electrode on the hole transport layer etched with the photonic crystal structure.
The invention further provides a preparation method of the electrically pumped perovskite quantum dot laser, which comprises the following steps:
step 1: preparing an electron transport layer on a negative electrode;
step 2: etching, namely etching the fifth photonic crystal structure on the electron transmission layer to provide a resonant cavity and a surface emitting mechanism for the laser;
and step 3: and preparing a perovskite quantum dot layer, a hole transport layer and a positive electrode on the electron transport layer etched with the photonic crystal structure in sequence.
The method has the advantages that the method is easy to realize, the electric pump perovskite quantum dot laser structure with a simple structure can be obtained, and the external quantum efficiency of the perovskite quantum dots under the electric pump can be effectively improved.
Drawings
To further illustrate the technical content of the present invention, the following detailed description is provided in conjunction with the embodiments and the accompanying drawings, in which:
FIG. 1 is a flow chart illustrating the preparation of a first embodiment of the present invention;
FIG. 2 is a schematic cross-sectional view of a first embodiment of an electrically-injected perovskite laser of the present invention;
FIG. 3 is a schematic cross-sectional view of a second embodiment of an electrically-injected perovskite laser of the present invention;
FIG. 4 is a schematic cross-sectional view of a third embodiment of an electrically-injected perovskite laser of the present invention;
FIG. 5 is a schematic cross-sectional view of a fourth embodiment of an electrically-injected perovskite laser of the present invention;
FIG. 6 is a schematic cross-sectional view of a fifth embodiment of an electro-injected perovskite laser of the present invention;
fig. 7 is a schematic cross-sectional view of a sixth embodiment of an electro-injected perovskite laser of the present invention.
Detailed Description
Referring to fig. 1 and fig. 2, which are a flowchart and a structural diagram of a first embodiment of the present invention, the present invention provides a method for manufacturing an electrically pumped perovskite quantum dot laser, which includes the following steps:
step 1: etching a first photonic crystal structure 6 'on a substrate 6 to provide a resonant cavity and a surface emission mechanism for the laser, wherein the first photonic crystal structure 6' comprises photonic crystals of different lattices, different defect cavities or arrays or coupling cavity arrays, complete photonic crystals or a chirp gradient structure and a random structure;
step 2: preparing an electron transport layer 4, a perovskite quantum dot layer 3, a hole transport layer 2 and a positive electrode 1 on a negative electrode 5 in sequence to form a first substrate;
and step 3: and bonding the substrate 6 etched with the photonic crystal or the photonic crystal array with the first substrate to finish the preparation.
Wherein the bonding of the substrate 6 to the first substrate or the second substrate comprises direct bonding, BCB assisted indirect bonding or direct growth. The distance between the photonic crystal structure 6' and the perovskite quantum dot layer 3 meets the coupling condition; since the resonant structure is located below the active region, photons generated by recombination of carriers in the perovskite quantum dot layer 3 resonate in the photonic crystal structure 6' through the electron transport layer 4 and the negative electrode 5, and finally light is emitted from the positive electrode 1.
Wherein the first substrate is prepared in a manner not limited to the order of preparation from the negative electrode 5; the first substrate and the second substrate can also be obtained by adopting a preparation mode of sequentially preparing a hole transport layer 2, a perovskite quantum dot layer 3, an electron transport layer 4 and a negative electrode 5 from a positive electrode 1; the first and second substrates are commonly prepared in laboratories at present by preparing a positive electrode 1, a hole transport layer 2, a perovskite quantum dot layer 3, an electron transport layer 4 and a negative electrode 5 in sequence from glass.
Referring to fig. 3, which is a structural diagram of a second embodiment of the present invention, the present invention provides a method for preparing an electrically pumped perovskite quantum dot laser, which includes the following steps:
step 1: etching a photon first crystal structure 6 'on a substrate 6 to provide a resonant cavity and a surface emission mechanism for the laser, wherein the first photon crystal structure 6' comprises photonic crystals of different crystal lattices, different defect cavities or arrays or coupling cavity arrays, complete photonic crystals or a chirp gradient structure and a random structure;
step 2: preparing perovskite quantum dots 3, a hole transport layer 2 and a positive electrode 1 in sequence on one side of the upper surface of an electron transport layer 4, and preparing a negative electrode 5 on the other side of the upper surface of the electron transport layer 4 to form a second substrate;
and step 3: and bonding the substrate 6 etched with the photonic crystal or the photonic crystal array with a second substrate to finish the preparation.
Wherein the bonding of the substrate 6 to the first substrate or the second substrate comprises direct bonding, BCB assisted indirect bonding or direct growth. The distance between the photonic crystal structure 6' and the perovskite quantum dot layer 3 meets the coupling condition; since the resonant structure is located below the active region, photons generated by recombination of carriers in the perovskite quantum dot layer 3 resonate in the photonic crystal structure 6' through the electron transport layer 4 and the negative electrode 5, and finally light is emitted from the positive electrode 1.
Referring to fig. 4, a structural diagram of a third embodiment of the present invention is shown, and the present invention provides a method for preparing an electrically pumped perovskite quantum dot laser, including the following steps:
step 1: preparing an electron transport layer 4, perovskite quantum dots 3, a hole transport layer 2 and a positive electrode 1 on a negative electrode 5 in sequence;
step 2: and etching, namely etching a second photonic crystal structure 1 'on the positive electrode 1 to provide a resonant cavity and a surface emission mechanism for the laser, wherein the second photonic crystal structure 1' comprises photonic crystals of different lattices, different defect cavities or arrays or coupling cavity arrays, complete photonic crystals or chirp gradient structures and random structures.
The photonic crystal structures 1 'and 2' are positioned above the active region, the positive electrode 1 is made of transparent ITO (indium tin oxide), the hole transport layer is made of transparent F8, and the negative electrode 5 is made of Ag or Al or a coating film to increase reflection; photons generated by the recombination of carriers in the perovskite quantum dot layer 3 resonate in the photonic crystal structure 1 'or 2', and finally light is emitted from the positive electrode 1.
Referring to fig. 5, a structure diagram of a fourth embodiment of the invention is shown, and the invention provides a method for preparing an electrically pumped perovskite quantum dot laser, including the following steps:
step 1: preparing an electron transport layer 4, perovskite quantum dots 3, a hole transport layer 2 and a positive electrode 1 on a negative electrode 5 in sequence;
step 2: and etching, namely etching a second photonic crystal structure 5 'on the negative electrode 5 to provide a resonant cavity and a surface emission mechanism for the laser, wherein the third photonic crystal structure 5' comprises photonic crystals of different lattices, different defect cavities or arrays or coupling cavity arrays, complete photonic crystals or chirp gradient structures and random structures.
The photonic crystal structures 5 'and 4' are positioned below the active region, the negative electrode 5 is made of transparent ITO (indium tin oxide) material, the electron transmission layer is made of transparent TpBi material, and the positive electrode 1 is made of Ag or Al or coated film to increase reflection; photons generated by recombination of carriers in the perovskite quantum dot layer 3 resonate in the photonic crystal structure 5 'or 4', and finally light is emitted from the negative electrode 5.
Referring to fig. 6, a structure diagram of a fifth embodiment of the present invention is shown, and the present invention provides a method for preparing an electrically pumped perovskite quantum dot laser, including the following steps:
step 1: preparing an electron transport layer 4, perovskite quantum dots 3 and a hole transport layer 2 on a negative electrode 5 in sequence;
step 2: etching, namely etching the fourth photonic crystal structure 2' on the hole transport layer 2 to provide a resonant cavity and a surface emitting mechanism for the laser;
and step 3: a positive electrode 1 is prepared on the hole transport layer 2 on which the photonic crystals are etched.
The photonic crystal structures 1 'and 2' are positioned above the active region, the positive electrode 1 is made of transparent ITO (indium tin oxide), the hole transport layer is made of transparent F8, and the negative electrode 5 is made of Ag or Al or a coating film to increase reflection; photons generated by the recombination of carriers in the perovskite quantum dot layer 3 resonate in the photonic crystal structure 1 'or 2', and finally light is emitted from the positive electrode 1
Referring to fig. 7, a structural diagram of a sixth embodiment of the present invention is shown, and the present invention provides a method for preparing an electrically pumped perovskite quantum dot laser, including the following steps:
step 1: preparing an electron transport layer 4 on a negative electrode 5;
step 2: etching, namely etching a fifth photonic crystal structure 4' on the electron transmission layer 4 to provide a resonant cavity and a surface emitting mechanism for the laser;
and step 3: perovskite quantum dots 3, a hole transport layer 2 and a positive electrode 1 are sequentially prepared on the electron transport layer 4 etched with the photonic crystals.
The photonic crystal structures 5 'and 4' are positioned below the active region, the negative electrode 5 is made of transparent ITO (indium tin oxide) material, the electron transmission layer is made of transparent TpBi material, and the positive electrode 1 is made of Ag or Al or coated film to increase reflection; photons generated by recombination of carriers in the perovskite quantum dot layer 3 resonate in the photonic crystal structure 5 'or 4', and finally light is emitted from the negative electrode 5.
The method for manufacturing an electrically pumped perovskite quantum dot laser according to any of the embodiments above, wherein the material of the positive electrode 1 and the negative electrode is Al, Ag or transparent electrode ITO. Al and Ag provide reflection for the electrically pumped perovskite laser, and light is output from the transparent electrode ITO.
The above embodiments are further described in detail for illustrating the purpose, technical solutions and effects of the present invention, and it should be understood that the above embodiments are only exemplary embodiments of the present invention and are not intended to limit the present invention, and any modifications, equivalent changes and improvements made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Reference documents
1.Imada，M.，et al.，Multidirectionally distributed feedback photonic crystal lasers.Physical Review B，2002.65(19).
2.Noda，S.，et a1.，Full three-dimensional photonic bandgap crystals at near-infrared wavelengths.Science，2000.289(5479)：p.604-606.
3.Noda，S.，et al.，Polarization mode control of two-dimensional photonic crystal laser by unit cell structure design.Science，2001.293(5532)：p.1123-1125.
Claims (8)
1. A preparation method of an electrically pumped perovskite quantum dot laser comprises the following steps:
step 1: etching a first photonic crystal structure on a substrate to provide a resonant cavity and a surface emitting mechanism for a laser;
step 2: preparing an electron transport layer, a perovskite quantum dot layer, a hole transport layer and a positive electrode on a negative electrode in sequence to form a first substrate;
and step 3: bonding the substrate etched with the first photonic crystal structure with a first substrate to finish preparation;
wherein the first photonic crystal comprises photonic crystals of different lattices or different defect cavities or arrays of coupling cavities; the photonic crystal structure is a complete photonic crystal structure or a chirp gradient structure or a random structure;
the resonant wavelength of the photonic crystal structure is consistent with the luminescence wavelength of the perovskite material.
2. A preparation method of an electrically pumped perovskite quantum dot laser comprises the following steps:
step 1: etching a first photonic crystal structure on a substrate to provide a resonant cavity and a surface emitting mechanism for a laser;
step 2: preparing a perovskite quantum dot layer, a hole transport layer and a positive electrode on one side of the upper surface of an electron transport layer in sequence, and preparing a negative electrode on the other side of the upper surface of the electron transport layer to form a second substrate;
and step 3: bonding the substrate etched with the first photonic crystal structure with a second substrate to finish preparation; wherein the first photonic crystal comprises photonic crystals of different lattices or different defect cavities or arrays of coupling cavities; the photonic crystal structure is a complete photonic crystal structure or a chirp gradient structure or a random structure;
the resonant wavelength of the photonic crystal structure is consistent with the luminescence wavelength of the perovskite material.
3. A preparation method of an electrically pumped perovskite quantum dot laser comprises the following steps:
step 1: preparing an electron transport layer, a perovskite quantum dot layer, a hole transport layer and a positive electrode on a negative electrode in sequence;
step 2: etching, namely etching a second photonic crystal structure on the positive electrode to provide a resonant cavity and a surface emitting mechanism for the laser; wherein the second photonic crystal comprises a photonic crystal of a different lattice or a different defect cavity or array or an array of coupling cavities; the photonic crystal structure is a complete photonic crystal structure or a chirp gradient structure or a random structure;
the resonant wavelength of the photonic crystal structure is consistent with the luminescence wavelength of the perovskite material.
4. A preparation method of an electrically pumped perovskite quantum dot laser comprises the following steps:
step 1: preparing an electron transport layer, a perovskite quantum dot layer, a hole transport layer and a positive electrode on a negative electrode in sequence;
step 2: etching, namely etching a third photonic crystal structure on the negative electrode to provide a resonant cavity and a surface emitting mechanism for the laser; wherein the third photonic crystal comprises a photonic crystal of a different lattice or a different defect cavity or array or an array of coupling cavities; the photonic crystal structure is a complete photonic crystal structure or a chirp gradient structure or a random structure;
the resonant wavelength of the photonic crystal structure is consistent with the luminescence wavelength of the perovskite material.
5. A preparation method of an electrically pumped perovskite quantum dot laser comprises the following steps:
step 1: preparing an electron transport layer, a perovskite quantum dot layer and a hole transport layer on a negative electrode in sequence;
step 2: etching, namely etching the fourth photonic crystal structure on the hole transport layer to provide a resonant cavity and a surface emitting mechanism for the laser;
and step 3: preparing a positive electrode on the hole transport layer etched with the photonic crystal structure; wherein the fourth photonic crystal comprises a photonic crystal of a different lattice or a different defect cavity or array or an array of coupling cavities; the photonic crystal structure is a complete photonic crystal structure or a chirp gradient structure or a random structure;
the resonant wavelength of the photonic crystal structure is consistent with the luminescence wavelength of the perovskite material.
6. A preparation method of an electrically pumped perovskite quantum dot laser comprises the following steps:
step 1: preparing an electron transport layer on a negative electrode;
step 2: etching, namely etching the fifth photonic crystal structure on the electron transmission layer to provide a resonant cavity and a surface emitting mechanism for the laser;
and step 3: preparing a perovskite quantum dot layer, a hole transport layer and a positive electrode in sequence on the electron transport layer etched with the photonic crystal structure; wherein the fifth photonic crystal comprises a photonic crystal of a different lattice or a different defect cavity or array or an array of coupling cavities; the photonic crystal structure is a complete photonic crystal structure or a chirp gradient structure or a random structure;
the resonant wavelength of the photonic crystal structure is consistent with the luminescence wavelength of the perovskite material.
7. A method of making an electrically pumped perovskite quantum dot laser as claimed in any one of claims 1 to 6 wherein the material at the positive and negative electrodes is Al, Ag or transparent electrode ITO.
8. A method of fabricating an electrically pumped perovskite quantum dot laser as claimed in claim 1 or 2 wherein the bonding of the substrate to the first or second substrate comprises direct bonding, BCB assisted indirect bonding or direct growth.
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| CN109687290B (en) * | 2019-02-22 | 2021-01-15 | 中国科学院半导体研究所 | Electric pumping perovskite composite cavity laser |
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| 电抽运有机准晶光子晶体激光器及其特性研究;蔡园园 等;《光学学报》;20150630;第35卷(第6期);第1-5页 * |
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