阅读说明：本技术 一种自供电式全钙钛矿发光二极管 (Self-powered full perovskite light emitting diode ) 是由 罗军生 林枋艳 万中全 贾春阳 于 2021-08-31 设计创作，主要内容包括：一种自供电式全钙钛矿发光二极管,属于电致发光器件技术领域。包括自下而上依次设置的透明导电基底、载流子传输层、钙钛矿吸光层、衔接层、钙钛矿有源层、载流子注入层、透明电极；其中,所述衔接层为双功能载流子传输层,同时作为钙钛矿太阳能电池的载流子抽取层和钙钛矿发光二极管的载流子注入层。本发明采用钙钛矿太阳能电池自供电,无需外接电源,有效解决了器件持续续航的问题,丰富了器件的应用场景,同时还大幅减小器件尺寸,有利于器件的微型化和集成化；本发明提供的一种自供电式全钙钛矿发光二极管,制备工艺简单,省时省能,便于大规模生产。(A self-powered all perovskite light emitting diode belongs to the technical field of electroluminescent devices. The device comprises a transparent conductive substrate, a carrier transmission layer, a perovskite light absorption layer, a linking layer, a perovskite active layer, a carrier injection layer and a transparent electrode which are arranged from bottom to top in sequence; the connecting layer is a difunctional carrier transmission layer and is used as a carrier extraction layer of the perovskite solar cell and a carrier injection layer of the perovskite light-emitting diode. According to the invention, the perovskite solar cell is self-powered, an external power supply is not required, the problem of continuous endurance of the device is effectively solved, the application scenes of the device are enriched, the size of the device is greatly reduced, and the miniaturization and integration of the device are facilitated; the self-powered all-perovskite light emitting diode provided by the invention is simple in preparation process, time-saving and energy-saving, and convenient for large-scale production.)

1. A self-powered full perovskite light emitting diode is characterized by comprising a transparent conductive substrate, a current carrier transmission layer, a perovskite light absorption layer, a linking layer, a perovskite active layer, a current carrier injection layer and a transparent electrode which are sequentially arranged from bottom to top; wherein the connection layer is a difunctional carrier transport layer.

2. A self-powered all-perovskite light emitting diode according to claim 1, wherein the linker layer is an electron transporting material or a hole transporting material, the carrier transporting layer is a hole transporting layer or an electron transporting layer, and the carrier injecting layer is a hole injecting layer or an electron injecting layer.

3. A self-powered all-perovskite light emitting diode according to claim 1, wherein when the linker layer is an electron transport material, the carrier transport layer is a hole transport layer and the carrier injection layer is a hole injection layer; when the connecting layer is made of a hole-transporting material, the carrier-transporting layer is an electron-transporting layer, and the carrier-injecting layer is an electron-injecting layer.

4. A self-powered all-perovskite light emitting diode according to claim 1, wherein when the linker layer is an electron transporting material, a hole injection promoting layer is further provided between the perovskite active layer and the carrier injection layer.

5. A self-powered all-perovskite light emitting diode according to claim 1, wherein the perovskite light absorbing layer material has a greater range of light absorption than the perovskite active layer material.

6. A self-powered all-perovskite light-emitting diode according to claim 1, wherein the perovskite light-absorbing layer is of a multilayer structure, and when the linking layer is an electron transport material, the perovskite light-absorbing layer is of a multilayer structure consisting of a first perovskite light-absorbing layer, an electron transport layer, an ITO thin film, a hole transport layer and a second perovskite light-absorbing layer which are arranged in sequence from bottom to top; when the connection layer is made of a hole transmission material, the perovskite light absorption layer is of a multilayer structure consisting of a first perovskite light absorption layer, a hole transmission layer, an ITO (indium tin oxide) film, an electron transmission layer and a second perovskite light absorption layer which are sequentially arranged from bottom to top.

7. A self-powered all perovskite light emitting diode as claimed in claim 6 wherein the material of the first perovskite light absorbing layer is (FA)_0.83Cs_0.17Pb(I_0.5Br_0.5)₃、(FA)_0.8Cs_0.2Pb(I_0.7Br_0.3)₃、(FA)_0.6Cs_0.4Pb(I_0.65Br_0.35)₃、Cs_0.05(FA)_0.8(MA)_0.15PbI_2.55Br_0.45Or Cs_0.2(FA)_0.8PbI_1.8Br_1.2(ii) a The second perovskite light absorption layer is made of (FA)_0.75Cs_0.25Sn_0.5Pb_0.5I₃、((FA)SnI₃)_0.6((MA)PbI₃)_0.4、(MA)_0.3(FA)_0.7Sn_0.5Pb_0.5I₃Or (FA)_0.5(MA)_0.45Cs_0.05Pb_0.5Sn_0.5I₃。

8. A self-powered all-perovskite light-emitting diode according to claim 2, wherein when the junction layer is an electron transport material, the material is ZnO, Mg: ZnO, ZnO: PEI, BCP, PCBM, C₆₀Is said hole transportThe material of the layer is NiO_xAnd PEDOT is one or more of PSS and PTAA, wherein x is 0.85-1.

9. A self-powered all-perovskite light emitting diode according to claim 2, wherein when the tie layer is a hole transport material, the material is NiO_xPEDOT is PSS or PTAA, wherein x is 0.85-1; the material of the electron transport layer is TiO₂、SnO₂Mg ZnO, PCBM, BCP or C₆₀。

10. The self-powered all-perovskite light-emitting diode according to claim 4, wherein the material of the hole injection promotion layer is MoO₃Or PEI, with a thickness of 2-15 nm.

Technical Field

The invention belongs to the technical field of electroluminescent devices, and particularly relates to a self-powered all-perovskite light emitting diode.

Background

The light emitting diode has the advantages of long service life, energy conservation, small volume and the like, and is widely applied to the field of life. Currently used organic light emitting diodes are limited in use in higher resolution areas due to insufficient color purity. The perovskite material is an excellent semiconductor material and is widely used for solar cells, and the maximum photoelectric conversion efficiency of the Perovskite Solar Cells (PSCs) can reach 25.5 percent at present and can be comparable with the traditional silicon-based solar cells. Meanwhile, the perovskite material is also used for constructing a light emitting diode with high brightness, high efficiency and narrow emission line width, and the band gap of the perovskite material can be flexibly regulated and controlled by changing the components of the perovskite material, so that full-spectrum light emission is realized. However, most conventional leds require an external power source to start operation, and the external power source is inconvenient for the leds to be used in emergency conditions. The whole perovskite solar cell and the light emitting diode integrated device are simply connected in series through a lead to form a closed loop, and due to the existence of the series lead between the devices, the structure can not really realize the miniaturization and integration of the devices.

Disclosure of Invention

The invention aims to provide a self-powered all-perovskite light emitting diode aiming at the problems in the background technology, and the integration of a perovskite solar cell and the perovskite light emitting diode is realized.

In order to achieve the purpose, the technical scheme adopted by the invention is as follows:

a self-powered full perovskite light emitting diode is characterized by comprising a transparent conductive substrate, a current carrier transmission layer, a perovskite light absorption layer, a linking layer, a perovskite active layer, a current carrier injection layer and a transparent electrode which are sequentially arranged from bottom to top; the connecting layer is a difunctional carrier transmission layer and is used as a carrier extraction layer of the perovskite solar cell and a carrier injection layer of the perovskite light-emitting diode.

Furthermore, the linking layer is an electron transport material or a hole transport material, the carrier transport layer is an electron transport layer or a hole transport layer, and the carrier injection layer is a hole injection layer or an electron injection layer.

Further, when the linking layer is made of an electron transport material, the carrier transport layer is a hole transport layer, and the carrier injection layer is a hole injection layer; when the connecting layer is made of a hole-transporting material, the carrier-transporting layer is an electron-transporting layer, and the carrier-injecting layer is an electron-injecting layer.

Further, when the tie layer is an electron transport material, a hole injection promoting layer is further provided between the perovskite active layer and the carrier (hole) injection layer.

Further, when the joining layer is an electron transport material, the joining layer can be used as an electron extraction material of the perovskite solar cell and an electron injection material of the perovskite light emitting diode, and specifically, the joining layer can be ZnO, Mg: ZnO (the molar ratio of Mg to ZnO is (0.01-0.1): 1), ZnO: PEI (PEI is polyetherimide, the mass ratio of ZnO to PEI is 5: 1-10: 1), BCP (2, 9-dimethyl-4, 7-diphenyl-1, 10-phenanthroline), PCBM ([6, 6-diphenyl-1, 10-phenanthroline), and PCBM]-phenyl-C₆₁-methyl butyrate), C₆₀Etc., the thickness of the layer being 30-100 nm.

Furthermore, when the connecting layer is a hole transport material, the connecting layer can be used as a hole extraction material of the perovskite solar cell and a hole injection material of the perovskite light emitting diode at the same time, and specifically is NiO_x(x is 0.85-1), PEDOT (poly (3, 4-ethylenedioxythiophene)/polystyrene sulfonate (the molar ratio of PEDOT to PSS is 1 (2-20)), and PTAA (poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine)]) Etc., the thickness of the layer being 30-100 nm.

Furthermore, the absorption range of the perovskite light absorption layer material to light is larger than that of the perovskite active layer material, and the thickness of the perovskite light absorption layer is regulated and controlled, so that the incident light is completely absorbed, and the perovskite is avoidedThe active layer is influenced by light to generate a photovoltaic effect; accordingly, the material of the perovskite light-absorbing layer is (MA) PbX₃(X＝Br、Cl)(MA⁺Is CH₃(NH₃)⁺)、(MA)PbI_3-xCl_x(x＝1～2)、(MA)PbI_3-xBr_x(x＝1～2)、(MA)_1-x(DMA)_xPbI₃(x is 0.70 to 0.95) (DMA is dimethylamine molecule), Cs_0.05((FA)_1-x(MA)_x)_0.95Pb(I_1-xBr_x)₃(x＝0.05～0.95)(FA⁺Is CH (NH)₂)₂ ⁺)、(FA)_0.6Cs_0.4Pb(I_0.65Br_0.35)₃And the thickness of the perovskite light absorption layer is 400-1000 nm; the perovskite active layer is Made of (MA) PbI₃、CsPbX₃(X＝Cl、Br、I)、(NMA)₂(FA)_n-1Pb_nI_3n+1(n-0.5-0.9) (NMA is 1-naphthylmethylamine ion), (FA)_1–x(GA)_xPbBr₃(x＝0.2～0.95)(GA⁺Is CH₆N₃ ⁺) Etc., the thickness of the perovskite active layer is 40-100 nm.

Furthermore, the perovskite light absorption layer can be of a multilayer structure, and when the linking layer is an electron transmission material, the perovskite light absorption layer is of a multilayer structure consisting of a first perovskite light absorption layer, an electron transmission layer, an ITO thin film, a hole transmission layer and a second perovskite light absorption layer which are arranged from bottom to top in sequence; when the connecting layer is a hole transmission material, the connecting layer is a multilayer structure consisting of a first perovskite light absorption layer, a hole transmission layer, an ITO film, an electron transmission layer and a second perovskite light absorption layer which are arranged from bottom to top in sequence.

Wherein the first perovskite light absorption layer is made of (FA)_0.83Cs_0.17Pb(I_0.5Br_0.5)₃、(FA)_0.8Cs_0.2Pb(I_0.7Br_0.3)₃、(FA)_0.6Cs_0.4Pb(I_0.65Br_0.35)₃、Cs_0.05(FA)_0.8(MA)_0.15PbI_2.55Br_0.45、Cs_0.2(FA)_0.8PbI_1.8Br_1.2Etc.; the second perovskite light absorption layer is made of (FA)_0.75Cs_0.25Sn_0.5Pb_0.5I₃、((FA)SnI₃)_0.6((MA)PbI₃)_0.4、(MA)_0.3(FA)_0.7Sn_0.5Pb_0.5I₃、(FA)_0.5(MA)_0.45Cs_0.05Pb_0.5Sn_0.5I₃And the like.

Furthermore, the carrier transport layer is an electron transport layer or a hole transport layer, and the thickness of the carrier transport layer is 50-100 nm. Wherein the material of the hole transport layer is NiO_x(x is 0.85-1), PEDOT is PSS and PTAA; the material of the electron transport layer is TiO₂、SnO₂、Mg:ZnO、PCBM、BCP、C₆₀And the like.

Furthermore, the carrier injection layer is a hole injection layer or an electron injection layer, and the thickness of the carrier injection layer is 30-200 nm. Wherein the material of the hole injection layer is FB (fluorene-2, 7-diboronic acid pinacol ester), TFB (poly (9, 9-dioctylfluorene-CO-N- (4-butylphenyl) diphenylamine)), TPD (N, N '-diphenyl-N, N' -bis (3-methylphenyl) -1,1 '-biphenyl-4, 4' -diamine), TPBI (1,3, 5-tris (1-phenyl-1H-benzimidazol-2-yl) benzene); the electron injection layer is made of ZnO, ZnO-PEI, CBP (4,4' -bis (9-carbazole) biphenyl) and the like.

Further, the transparent electrode is made of LiF/Al and Cs₂CO₃Al, etc., the thickness of the transparent conductive layer is 80-200 nm.

Further, the transparent conductive substrate is flexible transparent conductive substrates such as ITO (indium tin oxide) conductive glass, FTO (fluorine tin oxide) conductive glass, or PEN (polyethylene naphthalate) plastic film with ITO.

Further, the material of the hole injection promoting layer is MoO₃Or PEI, with a thickness of 2-15 nm.

Compared with the prior art, the invention has the beneficial effects that:

according to the self-powered all-perovskite light emitting diode provided by the invention, the perovskite solar cell is self-powered without an external power supply, so that the problem of continuous endurance of the device is effectively solved, the application scene of the device is enriched, the size of the device is greatly reduced, and the miniaturization and integration of the device are facilitated; the self-powered all-perovskite light emitting diode provided by the invention is simple in preparation process, time-saving and energy-saving, and convenient for large-scale production.

Drawings

Fig. 1 is a schematic structural diagram of a self-powered all-perovskite light emitting diode provided in embodiments 1(a) and 2(b) of the present invention;

FIG. 2 is a graph of the energy level relationship of the materials of the layers when the tie layer is an electron transporting material;

FIG. 3 is a graph of the energy level relationship of the materials of the layers when the tie layer is a hole transporting material;

fig. 4 is a schematic structural diagram of a perovskite-tandem solar cell-perovskite light emitting diode integrated device provided in embodiment 3 of the present invention.

Detailed Description

The technical scheme of the invention is detailed below by combining the accompanying drawings and the embodiment.

According to the self-powered all-perovskite light emitting diode provided by the invention, under the illumination condition, the perovskite light absorption layer absorbs photons to generate excitons, the excitons are separated at the interface between the perovskite light absorption layer and the adjacent layer to generate electrons and holes, the electrons are injected into the electron transport layer, and the holes are injected into the hole transport layer. And the photo-generated carriers are transmitted by using the wires and the connecting layer between the transparent conductive substrate and the transparent electrode of the perovskite light emitting diode respectively, and finally, the injection of the photo-generated carriers into the active layer is realized.

Example 1: self-powered all-perovskite green light emitting diode with linking layer as electron transmission layer

As shown in fig. 1(a), a schematic structural diagram of a self-powered all-perovskite light emitting diode provided in example 1 is shown; wherein, 1 is transparent conductive substrate ITO, 2 is hole transport layer PTAA, 3 is perovskite light absorption layer Cs_0.05((FA)_0.95(MA)_0.05)_0.95Pb(I_0.95Br_0.05)₃4 is a connecting layer PCBM/BCP, 5 is a perovskite active layer (FA)_1–x(GA)_xPbBr₃And 6 is a hole injection promoting layer MoO₃7 is a hole injection layer TPBI, 8 is a transparent electrode LiF/Al. Wherein, 1, 2, 3 and 4 layers form a p-i-n type perovskite solar cell, and 4, 5, 6 and 8 layers form an n-i-p type perovskite light emitting diode. The selected material energy level relation satisfies the figure 2, wherein, (1) is a hole transport material, (2) is a perovskite light absorption material, (3) is an electron transport junction layer material, (4) is a perovskite active layer material, and (5) is a hole injection material.

The preparation method of the self-powered all-perovskite light-emitting green diode provided in embodiment 1 specifically includes the following steps:

step 1, ultrasonically washing a transparent ITO conductive substrate by using acetone and isopropanol in sequence, and treating the transparent ITO conductive substrate for 30min in an ultraviolet ozone cleaning instrument after blowing;

step 2, spin-coating a chlorobenzene solution (10mg/mL) of PTAA on an ITO substrate, and annealing at 100 ℃ for 5-10 min;

step 3, weighing CsI, FAI and PbI₂、MABr、PbBr₂Dissolving in mixed solvent of DMF (N, N-dimethylformamide) and DMSO (dimethyl sulfoxide) (volume ratio of DMF to DMSO is 4:1) to obtain Cs_0.05((FA)_0.95(MA)_0.05)_0.95Pb(I_0.95Br_0.05)₃Then adding 30 mol% of MACl into the precursor solution; then respectively spin-coating 10s and 30s on the PTAA layer at the rotation speeds of 1000rpm and 5000rpm, dropwise adding 100 mu L of chlorobenzene antisolvent in the first 10s after the spin-coating is finished, and heating and annealing at 150 ℃ for 40 min;

step 4, sequentially depositing PCBM with the thickness of 30nm and BCP with the thickness of 8nm on the perovskite layer obtained in the step 3 by adopting a vacuum evaporation method to obtain a junction layer;

step 5, adding FABr, GABr and PbBr₂Dissolving in 0.5ml of anhydrous N, N-dimethylformamide to obtain a precursor solution; then 0.15ml of the precursor solution was dropped into a crystallization inducing liquid composed of 5ml of toluene, 2ml of 1-butanol, 0.3ml of oleic acid and 24.2. mu.l of n-decylamine, and mixed for 10min with vigorous stirring; spin-coating at 3000rpm for 60s, and annealing at 80 deg.C for 10min to obtain perovskite active layer;

step 6, trueEmpty evaporation 4nm MoO₃；

Step 7, vacuum thermal deposition of 40nm TPBI;

and 8, carrying out vacuum thermal deposition on 5nm LiF and 120nm Al to serve as transparent electrodes.

Example 2: self-powered all-perovskite blue light emitting diode-the connecting layer is a hole transport layer

As shown in fig. 1(b), a schematic structural diagram of a self-powered all-perovskite light emitting diode provided in example 2 is shown; wherein 1 'is transparent conductive substrate FTO, 2' is electron transport layer TiO₂3' is perovskite light absorption layer MAPbI_3-xCl_xPSS/PTAA as junction layer 4', CsPbBr as perovskite active layer 5₃The quantum dots, 6 'are electron injection layers ZnO, and 7' are transparent electrodes LiF/Al. Wherein 1 '-4' layers form an n-i-p type perovskite solar cell, 4 '-7' layers of p-i-n type perovskite light emitting diodes have the energy level of the selected materials which meet the figure 3, wherein, the materials comprise an electron transmission material, a perovskite light absorption material, a hole transmission connection layer material, a perovskite active layer material and an electron injection material.

The embodiment 2 provides a preparation method of a self-powered all-perovskite blue light emitting diode, which specifically includes the following steps:

step 1, ultrasonically washing a transparent FTO conductive substrate by using acetone and isopropanol in sequence, and treating the substrate in an ultraviolet ozone cleaning instrument for 30min after blowing;

step 2, densifying the TiO₂The preparation of (1): transferring 369 mu L of tetraisopropyl titanate into a reagent bottle 1, then transferring 2.53mL of ethanol, and mixing by magnetic stirring; transferring 35 mu L of 2M hydrochloric acid into a reagent bottle 2, then transferring 2.53mL of ethanol, and mixing by magnetic stirring; dropwise adding the solution in the reagent bottle 2 into the reagent bottle 1, stirring for 2h, and filtering with a filter head to obtain compact TiO₂A precursor solution; compacting TiO₂Dropping the precursor on FTO till the FTO is fully paved, wherein the spin coating condition is 4000rpm and 50s, the heating platform is used for processing for 15min at 150 ℃, and then placing the wafer into a muffle furnace for calcining at 500 ℃ for 1 h;

step 3, mesoporous TiO₂The preparation of (1): m is_{Mesoporous TiO2 slurry}:m_EthanolDiluting according to the proportion of 1:7, magnetically stirring for 2h, and then performing ultrasonic treatment for 1 h; making mesoporous TiO₂Dropping the precursor on FTO conductive glass until the FTO conductive glass is fully paved, placing the FTO conductive glass on a hot bench for processing for 10min at 125 ℃ under the spin coating condition of 5000rpm and 30 s; placing the spin-coated wafer in a muffle furnace for calcining at 500 ℃ for 1 h;

step 4, PbI₂Adding the precursor solution and MAI into 5mL of gamma-butyrolactone in a molar ratio of 1:1 to obtain a precursor solution 1; to obtain (MA) PbI_3-xCl_xSingle crystal, CH is added into the precursor 1 solution in a molar ratio of 1:1₃NH₃Cl and PbCl₂Partial solute is replaced, and then precursor solution with the molar ratio of I to Cl of 14:1 is obtained; heating the obtained precursor solution at 70 ℃ and stirring for 12 h; subsequently, the solution was heated at 120 ℃ for several hours, some small (MA) PbI_3-xCl_xThe crystal seeds appear at the bottom of the vial; for the preparation of bulk (MA) PbI_3-xCl_xSingle crystal, namely putting the selected seeds into a precursor solution which is stirred for 12 hours at 70 ℃; 734Mg (MA) PbI_3-xCl_xAdding 600 mu L of CH into the single crystal₃NH₂Adding 400 mu L of acetonitrile into the mixed solution of EtOH (33 wt.%), diluting and synthesizing the solution with the concentration of 1.2M, and carrying out spin coating at the speed of 4000-6000 rpm for 60s to obtain a perovskite light absorption layer;

step 5, PEDOT, namely spin-coating a PSS solution on a light absorption layer at the rotating speed of 6000rpm for 30s, baking for 25min at the temperature of 150 ℃, after cooling a substrate to the room temperature, spin-coating a PTAA chlorobenzene solution of 5mg/mL on the PEDOT, namely the PSS layer, and baking for 25min at the temperature of 150 ℃;

step 6, CsPbBr₃Spin-coating the quantum dot precursor liquid at 2000rpm for 60s to obtain a perovskite active layer;

step 7, spin-coating the ZnO solution at 4000rpm for 60s, and annealing at 100 ℃ for 10min to obtain an electron injection layer ZnO;

step 8, carrying out vacuum thermal deposition on 5nm LiF and 100nm Al, wherein the vacuum degree is (a)<10^-4Pa) as a transparent electrode.

Example 3: the perovskite laminated solar cell-perovskite light emitting diode integrated device-the connecting layer is an electron transmission layer

As shown in fig. 4, a schematic structural diagram of the perovskite laminated solar cell-perovskite light emitting diode integrated device provided in example 3 is shown. Wherein, the linking layer is BCP, the I-VIII layers form a perovskite laminated solar cell, and the VIII-XII layers form a perovskite light-emitting diode. I is a transparent conductive substrate ITO, II is a hole transport layer PTAA, III is a first perovskite light absorption layer (FA)_0.6Cs_0.4Pb(I_0.65Br_0.35)₃IV is an electron transport layer C₆₀/SnO₂V is an ITO film, VI is a hole transport layer PEDOT, PSS/PTAA, VII is a second perovskite light absorption layer (FA)_0.5(MA)_0.45Cs_0.05Pb_0.5Sn_0.5I₃VIII is an electron transport connecting layer C₆₀the/BCP and IX are perovskite active layers CsPbBr₃X is a hole injection promoting layer MoO₃XI is a hole injection layer TPBI, and XII is a transparent electrode layer LiF/Al.

The preparation process of the perovskite laminated solar cell-perovskite light emitting diode integrated device provided in embodiment 3 specifically comprises the following steps:

step 1, ultrasonically washing a transparent ITO conductive substrate by using acetone and isopropanol in sequence, and cleaning for 30min by using ultraviolet ozone after blowing;

step 2, spin-coating a chlorobenzene solution (10mg/mL) of PTAA on an ITO substrate, and annealing at 100 ℃ for 5-10 min;

step 3, preparing perovskite light absorption layer precursor liquid:

mixing FAI, CsI, PbI₂、PbBr₂Dissolving in a mixed solvent of DMSO and DMF (volume ratio of DMSO to DMF is 3:7) to obtain (FA)_0.6Cs_0.4Pb(I_0.65Br_0.35)₃A perovskite precursor liquid;

mixing MAI, FAI, CsI, PbI₂、SnI₂、SnF₂In a mixed solvent of DMSO and DMF (volume ratio of DMSO to DMF in the mixed solvent is 3:7), obtaining (FA)_0.5(MA)_0.45Cs_0.05Pb_0.5Sn_0.5I₃A perovskite precursor liquid;

step 4, mixing 100-200 mu L (FA)_0.6Cs_0.4Pb(I_0.65Br_0.35)₃Spin-coating the precursor solution on the PTAA layer, spin-coating the PTAA layer for 20s and 20s at the rotation speeds of 1000rpm and 5000rpm respectively, blowing nitrogen into the substrate for fast drying at the 20 th s, then annealing at 65 ℃ for 10min, and annealing at 100 ℃ for 10min to obtain a first perovskite light absorption layer;

step 5, adding C₆₀Thermally evaporating to a thickness of 30nm on the first perovskite light absorption layer;

step 6, under the vacuum condition, using [ (CH)₃)₂N]₄Sn and H₂O is respectively used as a Sn source and an O source, and SnO is deposited by adopting an atomic layer deposition method₂A thin film with a thickness of 15 nm;

step 7, growing an ITO film with the thickness of 10nm by magnetron sputtering;

step 8, PEDOT, namely coating a PSS solution on the ITO layer in a spinning mode at the speed of 5000rpm, and annealing for 20min at the temperature of 100 ℃;

step 9, spin-coating 5mg/mL PTAA chlorobenzene solution on a PEDOT (PSS) layer, and baking for 20min at 150 ℃;

step 10, 200 mu L (FA)_0.5(MA)_0.45Cs_0.05Pb_0.5Sn_0.5I₃Spin-coating the precursor solution on the PTAA layer, spin-coating the PTAA layer for 20s and 20s at the rotation speeds of 1000rpm and 5000rpm respectively, blowing nitrogen into the substrate for fast drying in the 20 th s, annealing at 65 ℃ for 10min, and annealing at 100 ℃ for 10min to obtain a second perovskite light absorption layer;

step 11, adding C₆₀Thermally evaporating to a second perovskite light absorption layer with the thickness of 30 nm; preparing BCP with the thickness of 8nm by using a vacuum evaporation method; obtaining a connecting layer;

step 12, CsBr and PbBr₂Dissolved in DMSO at a molar ratio of 1.5:1, followed by addition of phenethyl ammonium bromide (PEABr, 10 wt%) and polyethylene glycol (PEG, 3.8 wt%) to give CsPbBr₃A precursor solution; spin-coating the precursor solution on the electron transmission connection layer obtained in the previous step, spin-coating at 3000rmp for 60s, and then annealing at 80 ℃ for 5min to obtain a perovskite active layer;

step 13, vacuum evaporation of 5nm MoO₃；

Step 14, carrying out vacuum thermal deposition on 50nm TPBI;

and step 15, carrying out vacuum thermal deposition on 3nm LiF and 100nm Al to obtain the transparent electrode.

The embodiments of the present invention have been described above with reference to the accompanying drawings, but the present invention is not limited to the above embodiments, and various changes can be made in the objects of the invention without departing from the technical principles and inventive concept of the present invention.