CN116948642A - Nano structure for enhancing nonlinear luminescence performance of perovskite and preparation method thereof - Google Patents
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Abstract
The invention provides a nano structure for enhancing the nonlinear luminescence performance of perovskite and a preparation method thereof, the nano structure comprises a luminescent layer and a substrate which are sequentially arranged from top to bottom, wherein the luminescent layer of the upper layer consists of a plurality of perovskite nano structure arrays which are mutually independent, and each perovskite nano structure is formed by mixing a transparent high polymer and perovskite. The large-scale nano pattern can be obtained by only a few simple steps, and has the advantages of low price, easy processing, large-area preparation and the like. In addition, the nano structure enables the perovskite to obtain an enhanced electromagnetic field, improves the nonlinear optical performance of the perovskite, and makes an important bedding for photoelectric application based on the micro-nano structure perovskite.
Description
Technical Field
The invention relates to the field of preparation of optoelectronic materials, in particular to a nano structure for enhancing nonlinear luminescence performance of perovskite and a preparation method thereof.
Background
In the prior art, all-inorganic halide perovskite (CsPbX 3 (x=cl, br, I)) is widely used in the photovoltaic field (chem.eng.j.393 (2020) 124767) due to tunable band gap, narrow full width at half maximum (FWHM), low temperature process and ease of synthesis (making it easy for mass production); adv. Mater.28 (2016) 9163-9168; nat. Nanotechnol.17 (2022) 813-816; ACS Nano 12 (2018) 8847-8854). Conventionally, photovoltaic devices have employed a planar perovskite configuration (perovskite materials are arranged and configured in the form of planar thin films).The optical properties of the perovskite planar thin film may be further enhanced or demonstrated by patterning it into nanoscale structures to enable more applications (Nat. Mater.13 (2014) 451-460; adv. Opt. Mater.10 (2022) 2200534). In solar cells, patterning improves efficiency by reducing surface reflectivity, tailored light capture, and higher external radiation efficiency and directionality (Nat. Commun.7 (2016) 13941;Nano Lett.16 (2016) 6467-6471). In light emitting applications, the nano-texture improves the outcoupling efficiency and gives new functions such as directionality and spectral tunability (Nat. Commun.10 (2019) 727; adv. Funct. Mater.27 (2017) 1606525). Another common application of nanopatterns is laser (ACS Nano 11 (2017) 5766-5773) in one-and two-dimensional Distributed Feedback (DFB) structures.
However, all-inorganic halide perovskites are due to their low stability characteristics, mainly due to their instability of lattice structure, and light, oxygen, water, etc. in the environment accelerate the degradation or phase change of the perovskite, further reducing its stability. Thus in practical patterning it is difficult to obtain a stable and efficient conversion, so that the material stays in the research stage. Currently, several patterning processes for all-inorganic halide perovskites have been proposed to increase conversion, which can be broadly categorized as: direct patterning and indirect patterning. Indirect patterning is mainly achieved by introducing additional layers, such as: the polymer layer, typically patterned using photolithographic techniques with poly-p-xylene or poly-methyl methacrylate (PMMA), can effectively inhibit direct contact between the perovskite and the photoresist. However, the indirect patterning method brings about a new problem that requires a more complicated process, thus bringing about an increase in cost (adv. Opt. Mate. 10 (2022) 2200534). Direct patterning methods include direct lithography (ACS Nano 13 (2019) 3823-3829) and inkjet printing (ACS appl. Mate. Inter.12 (2020) 22157-22162). Direct photolithography is a traditional method of patterning perovskite, the process is relatively cumbersome and complex, and perovskite is very sensitive to polar solvents (such as water, methanol and acetone) and high temperature environments, since photoresist or polar solvents inevitably collapse perovskite patterns, which also makes them generally incompatible with traditional photolithographic processes (adv.function.mate.27 (2017) 1606525;Light Sci.Appl.2 (2013) 56). Inkjet printing is the most widely used direct patterning technique for organic and perovskite materials; however, it has limitations in generating high resolution patterns (nanoscales 7 (2015) 4423-4431); high resolution of 5 μm has been successfully demonstrated using electrohydrodynamic printing (adv. Funct. Mate.29 (2019) 2100857), but further resolution improvements are difficult to achieve because the nozzle capacity and single jet volume of solution cannot be reduced indefinitely (adv. Funct. Mate.32 (2022) 0224957). In addition, the low stability of perovskite, and the disadvantageous balance between optical gain and optical loss in electroluminescent devices, etc., have resulted in difficulties in achieving electrically pumped lasers or laser diodes (Nature 617 (2023) 79-85) of perovskite.
Disclosure of Invention
In view of the above, the present invention aims to provide a nanostructure for enhancing nonlinear luminescence of perovskite and a preparation method thereof, which solve the problems of difficulty in manufacturing a large area, low cost and easiness in processing patterned perovskite nanostructure in the conventional process, and realize remarkable improvement of nonlinear luminescence. The existence of the nano structure in the perovskite obtains an enhanced electromagnetic field, improves the nonlinear optical performance of the perovskite, and is suitable for the fields of lasers, wavelength converters, optical logic gates and the like.
The technical scheme is as follows: the nanostructure for enhancing the nonlinear luminescence performance of perovskite comprises a luminescence layer and a substrate which are sequentially arranged from top to bottom, wherein the luminescence layer of the upper layer consists of a plurality of perovskite nanostructure arrays which are mutually independent, and each perovskite nanostructure is formed by mixing a transparent high polymer and perovskite; when the intrinsic photoluminescence wavelength of the perovskite is matched with the resonance wavelength generated by the nanostructure array, the nonlinear luminescence performance of the system is obviously improved, and the high polymer plays a role in protecting and stabilizing the perovskite while inducing the perovskite to crystallize.
Wherein, the liquid crystal display device comprises a liquid crystal display device,
a fabry-perot resonator (FP cavity) may be added to the light emitting layer or substrate to achieve either side lasing or vertical facet lasing.
The electrodes can be added on both sides, and the light emission enhancement or the laser can be realized through direct current or alternating current driving.
The shape of the nanostructure is any one of a sphere, a mongolian yurt, a cone or a polygon.
The perovskite nanocrystalline is of a general formula ABX 3 Wherein the cation at the A-position comprises MA + (CH 3 NH 3 + )、FA + ([(NH 2 ) 2 CH] + ) And Cs + The method comprises the steps of carrying out a first treatment on the surface of the The B-site being mainly Pb 2+ Or using different metal ions Sr 2+ 、Zn 2+ 、Ni 2+ 、Mn 2+ 、Cd 2+ 、Sn 2+ 、Co 2+ 、Eu 3+ 、Er 3+ 、Yb 3+ 、Bi 3+ Partial or complete substitution of Pb 2+ ；X＝Cl、Br、I。
The high molecular polymer is any one of PDMS (polydimethylsiloxane), PMMA (polymethyl methacrylate), PVDF (polyvinylidene fluoride), inorganic (perhydro) polysilazane PHPS n-butyl ether, PVP (polyvinylpyrrolidone) and photo-curing resin.
The preparation method of the nano structure for enhancing the nonlinear luminescence performance of perovskite specifically comprises the following steps:
step 1, continuously and ultrasonically washing a substrate in isopropanol, acetone and ethanol for 10-20 minutes respectively, and drying with nitrogen;
step 2, preparing a single-layer nano-structure array master plate on a substrate;
step 3, preparing a polymer mold, copying a single-layer nano-structure array master mask by using a polymer film, drying and curing, and then stripping the polymer mold from a substrate, wherein the obtained mold has the same size as the single-layer nano-structure array master mask;
step 4, coating a mixture of perovskite precursor liquid and high molecular polymer on a substrate, and patterning by using a polymer mold through a nanoimprint process;
step 5, the mold is gently separated from the stationary substrate at as low a rate as possible, and the well-defined nanostructure array pattern has been successfully transferred to the substrate.
The single-layer nano-structure array master plate is obtained by processing any one of the traditional photoetching method, the focused ion beam method, the laser micro-processing method, the nanosphere self-assembly and the inkjet printing method.
The photoluminescence spectrum of the nano structure has wavelengths of 400-500nm, 500-600nm and 600-700nm respectively, wherein,
the photoluminescence spectrum of the nano structure is BCl at the wavelength of 400-500nm 2 、ACl、BBr 2 ABr powder is weighed according to the molar ratio of 1:1:0:0-0:0:1, the powder is pre-dissolved in DMF solvent after being mixed, forming a perovskite precursor solution with the concentration of 0.01 mmol/ml-0.5 mmol/ml and the photoluminescence spectrum of the nanostructure of 400-500 nm;
the photoluminescence spectrum of the nano structure is that BBr is used at the wavelength of 500-600nm 2 、ABr、BI 2 The AI powder is weighed according to the molar ratio of 1:1:0:0-1.8:1.8:1.2:1.2, and the powder is pre-dissolved in DMF solvent after being mixed to form perovskite precursor liquid with the concentration of 0.01 mmol/ml-0.5 mmol/ml and the photoluminescence spectrum of the nano structure of 500-600 nm;
the photoluminescence spectrum of the nano structure is that BBr is used at the wavelength of 600-700nm 2 、ABr、BI 2 The AI powder is weighed according to the molar ratio of 1.8:1.8:1.2:1.2-0:0:1:1, and the powder is pre-dissolved in DMF solvent after being mixed to form the perovskite precursor liquid with the concentration of 0.01 mmol/ml-0.5 mmol/ml and the photoluminescence spectrum of the nano structure of 600-700 nm.
The prepared single-layer nano-structure array can generate resonance peaks with resonance wavelengths of 400-500nm, 500-600nm and 600-700nm to match nano-structures with intrinsic photoluminescence wavelengths of 400-500nm, 500-600nm and 600-700 nm.
The beneficial effects are that: from the above, it can be seen that the nanostructure for enhancing the nonlinear luminescence performance of perovskite and the preparation method thereof provided in one or more embodiments of the present disclosure have several beneficial effects:
1. conventional patterning processes in semiconductors remain a photolithographic technique and perovskite patterning is unavoidable in many cases. However, the low stability of perovskite results in their performance being extremely susceptible to exposure to ultraviolet light due to the large amounts of solvents and high energy required for conventional lithographic processes. In addition, the micro/nano structure is manufactured by processes such as Electron Beam Lithography (EBL), reactive Ion Etching (RIE), and the like, and the problems of limited processing area, high cost, complex process design, time consumption, and the like are faced. Nanoimprinting is a processing technique that is not a chemical treatment; thus, the perovskite is no longer subject to degradation threats caused by the resist and the polar solvent. The low cost, large scale nanopatterns can be obtained here in a few simple steps.
2. A fabry-perot resonant cavity (FP cavity) is added to the light emitting layer or substrate, so that side laser or vertical cavity surface laser can be realized. The electrodes are added on the two sides, and the light emission enhancement or the laser can be realized through direct current or alternating current driving. The framework has a photonic waveguide consisting of FP cavity and electrodes. The lateral optical cavity formed improves field confinement in the perovskite gain medium while reducing optical losses in the charge conducting layer. It also promotes the establishment of Amplified Spontaneous Emission (ASE) due to improved collection of spontaneous seed photons and increased propagation paths in the perovskite medium. Thus, a large net optical gain is achieved by electrical pumping and ASE can be exhibited at room temperature. A fabry-perot resonator (FP cavity) may be added to the light emitting layer or substrate to achieve either side lasing or vertical facet lasing.
Drawings
For a clearer description of one or more embodiments of the present description or of the solutions of the prior art, the drawings that are necessary for the description of the embodiments or of the prior art will be briefly described, it being apparent that the drawings in the description below are only one or more embodiments of the present description, from which other drawings can be obtained, without inventive effort, for a person skilled in the art.
FIG. 1 is a scanning electron microscope image of perovskite nanostructure of example 2;
FIG. 2 is a graph showing the formants of perovskite nanostructures in example 2;
FIG. 3 is a non-linearly enhanced photoluminescence spectrum of the perovskite nanostructure of example 2, wherein the system was optically excited with an 800nm pulse laser system at a repetition rate of 1kHz and a pulse width of 120fs.
Detailed Description
For the purposes of promoting an understanding of the principles and advantages of the disclosure, reference will now be made in detail to the following specific examples.
The nanostructure for enhancing the nonlinear luminescence performance of perovskite comprises a luminescence layer and a substrate which are sequentially arranged from top to bottom, wherein the luminescence layer of the upper layer consists of a plurality of perovskite nanostructure arrays which are mutually independent, and each perovskite nanostructure is formed by mixing a transparent high polymer and perovskite; when the intrinsic photoluminescence wavelength of the perovskite is matched with the resonance wavelength generated by the nanostructure array, the nonlinear luminescence performance of the system is obviously improved, and the high polymer plays a role in protecting and stabilizing the perovskite while inducing the perovskite to crystallize. A fabry-perot resonator (FP cavity) may be added to the light emitting layer or substrate to achieve either side lasing or vertical facet lasing. The electrodes can be added on both sides, and the light emission enhancement or the laser can be realized through direct current or alternating current driving. The shape of the nanostructure is any one of a sphere, a mongolian yurt, a cone or a polygon. The perovskite nanocrystalline is of a general formula ABX 3 Wherein the cation at the A-position comprises MA + (CH 3 NH 3 + )、FA + ([(NH 2 ) 2 CH] + ) And Cs + The method comprises the steps of carrying out a first treatment on the surface of the The B-site being mainly Pb 2+ Or using different metal ions Sr 2+ 、Zn 2+ 、Ni 2+ 、Mn 2+ 、Cd 2+ 、Sn 2+ 、Co 2+ 、Eu 3+ 、Er 3+ 、Yb 3+ 、Bi 3+ Partial or complete substitution of Pb 2+ The method comprises the steps of carrying out a first treatment on the surface of the X=cl, br, I. The high polymer is PDMS (polydimethylsiloxane), PMMA (polymethyl methacrylate), PVDF (polyvinylidene fluoride),Any one of inorganic (perhydro) polysilazane PHPS n-butyl ether, PVP (polyvinylpyrrolidone) and photo-curing resin.
Example 1
A nanostructure that enhances the nonlinear luminescence properties of a perovskite, comprising:
the light-emitting layer comprises a plurality of perovskite nano-structure arrays which are mutually independent, and each perovskite nano-structure is formed by mixing a transparent high-molecular polymer and perovskite.
A Fabry-Perot resonant cavity (FP cavity) and an electrode are added on a light emitting layer or a substrate, so that side laser or vertical cavity surface laser is realized.
The substrate may be a quartz plate, a mica plate, a silicon wafer, conductive glass or a flexible material.
The luminescent layer is composed of a plurality of mutually independent perovskite nano-structure arrays, and the perovskite nano-structure has a general formula ABX 3 Wherein the cation at the A-position comprises MA + (CH 3 NH 3 + )、FA + ([(NH 2 ) 2 CH] + ) And Cs + The method comprises the steps of carrying out a first treatment on the surface of the The B-site being mainly Pb 2+ Or using different metal ions Sr 2+ 、Zn 2+ 、Ni 2+ 、Mn 2+ 、Cd 2+ 、Sn 2+ 、Co 2+ 、Eu 3+ 、Er 3+ 、Yb 3+ 、Bi 3+ Partial or complete substitution of Pb 2+ ；X＝Cl、Br、I。
The added FP cavity is used as a substrate and forms Bragg reflection waveguide together with the electrode at the top, so that the light field intensity in the transmission layer is effectively reduced, and the huge loss caused by the transmission layer is reduced. At the same time, the light field intensity in the light emitting layer gain medium is enhanced to increase the mode gain.
The added FP cavity and the electrode can be bonded with each other by any one of spin coating, thermal evaporation, magnetron sputtering, atomic layer deposition and electron beam evaporation.
Example 2
The method comprises the steps of obtaining a patterned mould by copying a single-layer nanosphere mother plate with an original pattern, and then forming perovskite nano patterns by using the mould through a nano imprinting process;
step 1: preparing a substrate;
continuously ultrasonic washing the substrate in isopropanol, acetone and ethanol for 10-20 min respectively, and drying with nitrogen;
step 2: assembling a two-dimensional compact nanosphere array;
5-20 mL of Polystyrene (PS) nanosphere colloid solution with the concentration of 400nm (1-10wt%) and 2-100 mL of ethanol are mixed according to the volume ratio, and the ultrasonic treatment is carried out for 30-60 min; spreading the PS nanospheres on the water surface at a sample injection speed of 1-240 mL/h by using a syringe; then, the PS nanosphere monomolecular layer is transferred to a preset substrate by slowly pumping water or lifting the substrate; the nanospheres are tightly adhered to the base material by low-temperature baking (25-80 ℃);
ethanol is added to the water-based PS colloid solution as a dispersant to reduce surface tension, thereby allowing PS nanospheres to be more effectively dispersed on the water surface; the amount of ethanol additive depends on the size and concentration of the nanospheres;
the substrate can be a quartz plate, a mica plate, a silicon wafer or a flexible material;
step 3: carrying out dry etching treatment on the nanosphere array;
treating the two-dimensional compact nanosphere array in the step 1 by an inductively coupled plasma etching machine, and introducing combined gas (power is 80-150W, gas flow is 20-50 sccm, and time is 18-167 s) of oxygen and argon to obtain a nanosphere array subjected to dry etching treatment;
step 4: preparing a patterning mould;
duplicating the single-layer nano-structure array master plate by using a polymer film, drying and re-solidifying for 1-24 hours at 40-80 ℃, and then stripping the polymer die from the substrate to obtain a die which has the same size as the single-layer nano-structure array master plate;
the material of the mold in the step 4 may be any one of PDMS (polydimethylsiloxane), PMMA (polymethyl methacrylate), PVDF (polyvinylidene fluoride), inorganic (perhydro) polysilazane PHPS n-butyl ether, PVP (polyvinylpyrrolidone), and photo-curing resin.
Step 5: csPbBr 3 Mixing the perovskite precursor solution with the polymer;
by dissolving 0.05 to 1.0mmol CsBr and 0.05 to 1.0mmol PbBr in 2 to 20mL of N, N-Dimethylformamide (DMF) solvent 2 Obtaining 0.01-0.5 mmol/mL perovskite precursor solution and mixing with 0.1-2 g polymer powder; wherein, stirring at 800rpm-1200rpm for 30min-60min;
the polymer used in the step 5 can be any one of PMMA (polymethyl methacrylate), PVDF (polyvinylidene fluoride), inorganic (perhydro) polysilazane PHPS n-butyl ether, PVP (polyvinylpyrrolidone) and photo-curing resin.
Step 6: formation of CsPbBr 3 A nano pattern;
CsPbBr in step 5 3 The perovskite precursor solution mixture is spin coated onto a substrate and patterned by a nanoimprint process using a mold. Finally, the separation from the fixed substrate is gentle at as low a rate as possible, at which time CsPbBr is well-defined 3 The nanopattern has been successfully transferred to the substrate;
the system is excited by adopting an 800nm pulse laser system, the repetition rate is 1kHz, the pulse width is 120fs, and CsPbBr 3 Photoluminescence (PL) spectra of the nanostructures show Amplified Spontaneous Emission (ASE) at lower optical excitation fluxes in the near infrared, the magnitude of PL enhancement being tunable by altering the resonance produced by the nanostructures; when resonance is tuned to an intrinsic emission peak of the nanocrystal, the nonlinear luminescence performance of the system is obviously improved, and the high polymer plays a role in protecting and stabilizing perovskite while inducing perovskite crystallization; not only helps to promote the development of manufacturing the periodic nano-structure of the perovskite with any configuration and is also used for further application of the perovskite nano-structure in the photoelectric fields of light emitting diodes, solar cells, lasers and the like.
Example 3
Step 1: preparing a substrate;
continuously ultrasonic washing the substrate in isopropanol, acetone and ethanol for 10-20 min respectively, and drying with nitrogen;
step 2: assembling a two-dimensional compact nanosphere array;
mixing 5-20 mL of Polystyrene (PS) nanosphere colloid solution with the concentration of 480nm and 1-10 wt% with 2-100 mL of ethanol according to the volume ratio, and carrying out ultrasonic treatment for 30-60 min; spreading the PS nanospheres on the water surface at a sample injection speed of 1-240 mL/h by using a syringe; then, the PS nanosphere monomolecular layer is transferred to a preset substrate by slowly pumping water or lifting the substrate; the nanospheres are tightly adhered to the base material by low-temperature baking (25-80 ℃);
ethanol is added to the water-based PS colloid solution as a dispersant to reduce surface tension, thereby allowing PS nanospheres to be more effectively dispersed on the water surface; the amount of ethanol additive depends on the size and concentration of the nanospheres;
the substrate can be a quartz plate, a mica plate, a silicon wafer or a flexible material;
step 3: carrying out dry etching treatment on the nanosphere array;
treating the two-dimensional compact nanosphere array in the step 1 by an inductively coupled plasma etching machine, and introducing combined gas (power is 80-150W, gas flow is 20-50 sccm, and time is 34-223 s) of oxygen and argon to obtain a nanosphere array subjected to dry etching treatment;
step 4: preparing a patterning mould;
duplicating the single-layer nano-structure array master plate by using a polymer film, drying and re-solidifying for 1-24 hours at 40-80 ℃, and then stripping the polymer die from the substrate to obtain a die which has the same size as the single-layer nano-structure array master plate;
the material of the mold in the step 4 may be any one of PDMS (polydimethylsiloxane), PMMA (polymethyl methacrylate), PVDF (polyvinylidene fluoride), inorganic (perhydro) polysilazane PHPS n-butyl ether, PVP (polyvinylpyrrolidone), and photo-curing resin.
Step 5: csPbBrI 2 Mixing the perovskite precursor solution with the polymer;
by reacting between 2 and 20mL of N, N-dimethylformamideDissolving 0.017-0.33 mmol CsBr, 0.017-0.33 mmol CsI, 0.034-0.66 mmol PbBr in amine (DMF) solvent 2 、0.034～0.66mmol PbI 2 Obtaining 0.01-0.5 mmol/mL perovskite precursor solution and mixing with 0.1-2 g polymer powder; wherein, stirring at 800rpm-1200rpm for 30min-60min;
the polymer used in the step 5 can be any one of PMMA (polymethyl methacrylate), PVDF (polyvinylidene fluoride), inorganic (perhydro) polysilazane PHPS n-butyl ether, PVP (polyvinylpyrrolidone) and photo-curing resin.
Step 6: formation of CsPbBrI 2 A nano pattern;
CsPbBri in step 5 2 The perovskite precursor solution mixture is spin coated onto a substrate and patterned by a nanoimprint process using a mold. Finally, the separation from the fixed substrate is gentle at as low a rate as possible, at which time the well-defined CsPbBri 2 The nanopattern has been successfully transferred to the substrate;
the system is excited by adopting an 800nm pulse laser system, the repetition rate is 1kHz, the pulse width is 120fs, and CsPbBri 2 Photoluminescence (PL) spectra of the nanostructures show Amplified Spontaneous Emission (ASE) at lower optical excitation fluxes in the near infrared, the magnitude of PL enhancement being tunable by altering the resonance produced by the nanostructures; when resonance is tuned to an intrinsic emission peak of the nanocrystal, the nonlinear luminescence performance of the system is obviously improved, and the high polymer plays a role in protecting and stabilizing perovskite while inducing perovskite crystallization; not only helps to promote the development of manufacturing the periodic nano-structure of the perovskite with any configuration and is also used for further application of the perovskite nano-structure in the photoelectric fields of light emitting diodes, solar cells, lasers and the like.
Morphology observations were made using a Hitachi regulatory 8100 Scanning Electron Microscope (SEM). The reflectance spectrum was measured by Lambda 950UV/Vis/NIR spectrophotometers. It is apparent that when the resonance is tuned to the intrinsic emission peak of the nanocrystal, the nonlinear luminescence performance of the system is significantly improved.
Overall, conventional patterning processes in semiconductors remain a photolithographic technique, and perovskite patterning is unavoidable in many cases. However, the low stability of perovskite results in their performance being extremely susceptible to exposure to ultraviolet light due to the large amounts of solvents and high energy required for conventional lithographic processes. In addition, the micro/nano structure is manufactured by processes such as Electron Beam Lithography (EBL), reactive Ion Etching (RIE), and the like, and the problems of limited processing area, high cost, complex process design, time consumption, and the like are faced. Nanoimprinting is an attractive method because it is a non-chemically treated processing technique; thus, the perovskite is no longer subject to degradation threats caused by the resist and the polar solvent. The nano pattern with low cost and large scale can be obtained by only a few simple steps;
a fabry-perot resonant cavity (FP cavity) is added to the light emitting layer or substrate, so that side laser or vertical cavity surface laser can be realized. The electrodes are added on the two sides, and the light emission enhancement or the laser can be realized through direct current or alternating current driving. The framework has a photonic waveguide consisting of FP cavity and electrodes. The lateral optical cavity formed improves field confinement in the perovskite gain medium while reducing optical losses in the charge conducting layer. It also promotes the establishment of Amplified Spontaneous Emission (ASE) due to improved collection of spontaneous seed photons and increased propagation paths in the perovskite medium. Thus, a large net optical gain is achieved by electrical pumping and ASE can be exhibited at room temperature. A fabry-perot resonator (FP cavity) may be added to the light emitting layer or substrate to achieve either side lasing or vertical facet lasing.
The present invention is intended to embrace all such alternatives, modifications and variances which fall within the broad scope of the appended claims. Accordingly, any omissions, modifications, equivalents, improvements, and the like, which are within the spirit and principles of the one or more embodiments of the invention, are intended to be included within the scope of the present disclosure.
Claims (10)
1. A nanostructure for enhancing the nonlinear luminescence properties of perovskite, characterized in that: the light-emitting device comprises a light-emitting layer and a substrate which are sequentially arranged from top to bottom, wherein the light-emitting layer consists of a plurality of mutually independent perovskite nano-structure arrays, and each perovskite nano-structure is formed by mixing a transparent high-molecular polymer and perovskite; the intrinsic photoluminescence wavelength of the perovskite can be matched to the resonance wavelength generated by the nanostructure array.
2. A nanostructure for enhancing nonlinear luminescence properties of perovskite according to claim 1, wherein the luminescent layer or substrate is provided with a fabry-perot resonator, thereby realizing side lasers, or vertical cavity surface lasers.
3. The nanostructure for enhancing nonlinear luminescence properties of perovskite according to claim 1, wherein electrodes are disposed on both sides of the nanostructure, and luminescence enhancement or laser is achieved by direct current or alternating current driving.
4. The nanostructure for enhancing nonlinear luminescence properties of perovskite according to claim 1, wherein the nanostructure has a shape of any one of a sphere, a mongolian yurt, a cone, or a polygon.
5. A nanostructure for enhancing nonlinear luminescence properties of perovskite according to claim 1, wherein said perovskite is of the general formula ABX 3 Wherein the cation in the A-position is MA + (CH 3 NH 3 + )、FA + ([(NH 2 ) 2 CH] + ) Or Cs + The method comprises the steps of carrying out a first treatment on the surface of the B is Pb 2+ Or using different metal ions Sr 2+ 、Zn 2+ 、Ni 2+ 、Mn 2+ 、Cd 2+ 、Sn 2+ 、Co 2+ 、Eu 3+ 、Er 3+ 、Yb 3+ 、Bi 3+ Partial or complete substitution of Pb 2+ The method comprises the steps of carrying out a first treatment on the surface of the X=cl, br or I.
6. The nanostructure for enhancing nonlinear luminescence of perovskite according to claim 1, wherein the high molecular polymer is any one of polydimethylsiloxane, polymethyl methacrylate, polyvinylidene fluoride, inorganic (perhydro) polysilazane PHPS n-butyl ether, polyvinylpyrrolidone, and photo-curing resin.
7. A method for preparing a nanostructure for enhancing nonlinear luminescence properties of perovskite according to any one of claims 1 to 6, comprising the steps of:
step 1, continuously and ultrasonically washing a substrate in isopropanol, acetone and ethanol for 10-20 minutes respectively, and drying with nitrogen;
step 2, preparing a single-layer nano-structure array master plate on a substrate;
step 3, preparing a polymer mold, copying a single-layer nano-structure array master mask by using a polymer film, drying and curing, and then stripping the polymer mold from a substrate, wherein the obtained mold has the same size as the single-layer nano-structure array master mask;
step 4, coating a mixture of perovskite precursor liquid and high molecular polymer on a substrate, and patterning by using a polymer mold through a nanoimprint process;
step 5, the mold is separated from the fixed substrate and the well-defined nanostructure array pattern has been successfully transferred to the substrate.
8. The method for preparing the nano-structure for enhancing the nonlinear luminescence property of the perovskite according to claim 7, wherein the single-layer nano-structure array master plate is obtained by any one of a traditional photoetching method, a focused ion beam method, a laser micro-processing method, a nanosphere self-assembly method and an inkjet printing method.
9. The method for preparing the nanostructure for enhancing the nonlinear luminescence property of perovskite according to claim 7, wherein the method for preparing the perovskite precursor solution comprises the following steps:
the photoluminescence spectrum of the nano structure is BCl at the wavelength of 400-500nm 2 、ACl、BBr 2 ABr powder is weighed according to the molar ratio of 1:1:0:0-0:0:1:1, and the powder is pre-dissolved in DMF solvent after being mixed to form perovskite precursor liquid with the concentration of 0.01 mmol/ml-0.5 mmol/ml and the photoluminescence spectrum of the nanostructure of 400-500 nm;
the photoluminescence spectrum of the nano structure is that BBr is used at the wavelength of 500-600nm 2 、ABr、BI 2 The AI powder is weighed according to the molar ratio of 1:1:0:0-1.8:1.8:1.2:1.2, and the powder is pre-dissolved in DMF solvent after being mixed to form perovskite precursor liquid with the concentration of 0.01 mmol/ml-0.5 mmol/ml and the photoluminescence spectrum of the nano structure of 500-600 nm;
the photoluminescence spectrum of the nano structure is that BBr is used at the wavelength of 600-700nm 2 、ABr、BI 2 The AI powder is weighed according to the molar ratio of 1.8:1.8:1.2:1.2-0:0:1:1, and the powder is pre-dissolved in DMF solvent after being mixed to form the perovskite precursor liquid with the concentration of 0.01 mmol/ml-0.5 mmol/ml and the photoluminescence spectrum of the nano structure of 600-700 nm.
10. The method of claim 7, wherein the single-layer nanostructure array produces formants with resonance wavelengths of 400-500nm, 500-600nm, 600-700nm to match nanostructures with intrinsic photoluminescence wavelengths of 400-500nm, 500-600nm, 600-700 nm.
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