CN111769435B - A method for generating laser multi-pulse and application of metal halide perovskite multiple quantum well material in laser multi-pulse generation - Google Patents
A method for generating laser multi-pulse and application of metal halide perovskite multiple quantum well material in laser multi-pulse generation Download PDFInfo
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- CN111769435B CN111769435B CN202010663280.XA CN202010663280A CN111769435B CN 111769435 B CN111769435 B CN 111769435B CN 202010663280 A CN202010663280 A CN 202010663280A CN 111769435 B CN111769435 B CN 111769435B
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Images
Classifications
-
- 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
- H01S3/00—Lasers, i.e. devices using stimulated emission of electromagnetic radiation in the infrared, visible or ultraviolet wave range
- H01S3/14—Lasers, i.e. devices using stimulated emission of electromagnetic radiation in the infrared, visible or ultraviolet wave range characterised by the material used as the active medium
- H01S3/16—Solid materials
- H01S3/169—Nanoparticles, e.g. doped nanoparticles acting as a gain material
-
- 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
- H01S3/00—Lasers, i.e. devices using stimulated emission of electromagnetic radiation in the infrared, visible or ultraviolet wave range
- H01S3/05—Construction or shape of optical resonators; Accommodation of active medium therein; Shape of active medium
- H01S3/08—Construction or shape of optical resonators or components thereof
- H01S3/08086—Multiple-wavelength emission
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- Physics & Mathematics (AREA)
- Electromagnetism (AREA)
- Engineering & Computer Science (AREA)
- Plasma & Fusion (AREA)
- Optics & Photonics (AREA)
- Chemical & Material Sciences (AREA)
- Nanotechnology (AREA)
- Luminescent Compositions (AREA)
Abstract
本发明公开了一种激光多脉冲的产生方法以及金属卤化物钙钛矿多量子阱材料在激光多脉冲产生中的应用，属于激光脉冲调控技术领域。产生方法包括：用脉冲激光激发金属卤化物钙钛矿多量子阱材料，并探测受激辐射信号。金属卤化物钙钛矿多量子阱材料包含不同厚度的钙钛矿量子阱，较厚的量子阱带隙较窄，较薄的量子阱带隙较宽。宽带隙相被激发光激发之后，产生的载流子会逐渐向窄带隙相传输。由于不同方向的传输速率不同，从宽带隙相向窄带隙相的载流子传输会分多步完成。上述技术不依赖于复杂光学设备，易于微型化和集成化。由此得到的超短激光双(多)脉冲可用于光谱学、光学成像、光通信或非线性光纤等领域。
The invention discloses a method for generating laser multi-pulse and the application of metal halide perovskite multi-quantum well material in the generation of laser multi-pulse, belonging to the technical field of laser pulse regulation. The generation method includes: exciting the metal halide perovskite multiple quantum well material with a pulsed laser, and detecting the stimulated emission signal. Metal halide perovskite multiple quantum well materials contain perovskite quantum wells of different thicknesses, with thicker quantum wells having narrower band gaps and thinner quantum wells having wider band gaps. After the wide band gap phase is excited by the excitation light, the generated carriers will gradually transfer to the narrow band gap phase. Due to the different transfer rates in different directions, the carrier transfer from the wide-bandgap phase to the narrow-bandgap phase is completed in multiple steps. The above technologies do not rely on complex optical devices and are easy to miniaturize and integrate. The resulting ultrashort laser double (multi) pulses can be used in the fields of spectroscopy, optical imaging, optical communication or nonlinear optical fibers.
Description
Technical Field
The invention relates to the technical field of laser pulse regulation and control, in particular to a laser multi-pulse generation method and application of a metal halide perovskite multi-quantum well material in laser multi-pulse generation.
Background
Multi-pulse lasers have found wide application in many fields, such as multi-pulse excitation of solids or plasmas, pulsed laser-based spectroscopy, optical imaging, optical communication, and nonlinear optical fibers.
At present, the approaches for realizing laser pulse multiplication include technologies such as delay lines and interferometers, multi-order wave plates and polarizers, birefringent crystal arrays and liquid crystal arrays. These optical devices are generally not conducive to miniaturization and device integration. Also, the generation of two coherent pulses under excitation of one pulse through a gain medium has not been achieved.
In view of this, the invention is particularly proposed.
Disclosure of Invention
One of the purposes of the invention comprises providing a laser multi-pulse generation method, wherein a metal halide perovskite multi-quantum well material is used as a gain medium, and two pulses or a plurality of stimulated radiation pulses are excited by a single pulse through a multi-step energy relaxation process in the material. Compared with the existing method for generating ultrashort laser double pulses, the method has the advantages of simple process, low cost, easy miniaturization and easy integration into devices.
Another object of the present invention includes providing a use of a metal halide perovskite multiple quantum well material for generating laser multipulses.
The invention also provides the application of the laser multi-pulse obtained by the above production method in spectroscopy, optical imaging, optical communication or nonlinear optical fiber.
The application is realized as follows:
in a first aspect, the present application provides a method for generating multiple laser pulses, comprising the steps of: and exciting the metal halide perovskite multi-quantum well material by using pulse laser, and detecting an excited radiation signal.
The laser multi-pulse comprises an ultrashort laser double-pulse or an ultrashort laser multi-pulse.
In an alternative embodiment, the intensity of the pulsed laser is 0.1-1000. mu.J/cm2The pulse width is 10fs-100ns, and the frequency is 1Hz-100 MHz.
In an alternative embodiment, the metal halide perovskite multi-quantum well material has the general structural formula L2An-1MnX3n+1Or DAn-1MnX3n+1Wherein L represents a long-chain positive divalent organic cation, D represents a long-chain positive divalent organic cation, A represents a short-chain positive monovalent cation, M represents a positive divalent metal cation, and X represents a negative monovalent anion.
The inorganic layer structure of the metal halide perovskite multi-quantum well material is [ MX [ ]6]4-Is represented by, n represents [ MX [ ]6]4-The number of layers of (a). The metal halide perovskite multi-quantum well material is formed by mixing quantum wells with different n values.
Wherein [ MX ]6]4-The layers are connected together through embedded A ions, and [ MX ] is embedded through L or D ions6]4-Separated layers of [ MX ] of different thicknesses6]4-The layers are coupled to each other by van der waals forces, thereby forming a quantum well structure.
In alternative embodiments, the long chain monovalent organic cation includes, but is not limited to, Isopropylamine (IPA)+) Naphthalene Methylamine (NMA)+) Phenylmethylamine (PMA)+) Phenylethylamine (PEA)+) Phenyl Trimethylamine (PTA)+) Butylamine (BA)+) Isobutylamine (i-BA)+) Tert-butylamine (t-BA)+) Ethylamine (EA)+) Hexylamine (HA)+) Octylamine (OA)+) Aniline (PhA)+) And Amphetamine (PPA)+) At least one of (1).
Preferably, the long chain divalent organic cation includes, but is not limited to, Ethylenediamine (EDA)2+)1, 4-xylylenediamine (BAB)2 +) Decamethylenediamine (DDA)2+) Propylene Diamine (PDA)2+) Ethylenedioxydiethylamine (EDBE)2+)1, 6-Hexanediamine (HDA)2+)1, 8-Octanediamine (ODA)2+)1, 4-phenylenediamine (PhDA)2+) M-phenylenediamine (mPhDA)2+) O-phenylenediamine (oPhDA)2+) And 1, 4-dimethyldiamine (PhDMA)2+) At least one of (1).
In alternative embodiments, short chain monovalent cations include, but are not limited to, Formamidine (FA)+) Methylamine (MA)+)、Cs+、Rb+、K+And Na+At least one of (1).
In an alternative embodiment, the positive divalent metal cation includes, but is not limited to, Pb2+、Sn2+、Mn2+And Ca2+At least one of (1).
In alternative embodiments, the negative monovalent anion includes, but is not limited to, F-、Cl-、Br-、I-And (BF)4)-At least one of (1).
In an alternative embodiment, the metal halide perovskite multi-quantum well material is in the form of a thin film.
In an alternative embodiment, the metal halide perovskite multi-quantum well material is a thin film of said metal halide perovskite multi-quantum well having a thickness of 50-2000 nm.
In an alternative embodiment, the metal halide perovskite multi-quantum well material is obtained by post-treating a thin film formed on the surface of a substrate by a perovskite precursor solution.
For example, the following steps may be performed:
(1) preparing a perovskite precursor solution;
(2) depositing a perovskite precursor solution on the surface of a substrate to form a thin film;
(3) and carrying out post-treatment on the perovskite thin film deposited on the surface of the substrate.
In an alternative embodiment, the precursor materials from which the perovskite precursor solution is prepared comprise a long chain organic amine salt, a short chain organic amine salt and a divalent metal halide, wherein the short chain organic amine salt may be partially or fully substituted with an alkali metal halide.
In alternative embodiments, long chain organic amine salts include, but are not limited to, isopropylamine hydroiodide (IPAI), naphthylamine hydroiodide (NMAI), phenylmethylamine hydroiodide (PMAI), phenylethylamine hydroiodide (PEAI), phenyltrimethylamine hydroiodide (PTAI), butylamine hydroiodide (BAI), isobutylamine hydroiodide (i-BAI), tert-butylamine hydroiodide (t-BAI), ethylamine hydroiodide (EAI), hexylamine Hydroiodide (HAI), octylamine hydroiodide (OAI), aniline hydroiodide (PhAI), amphetamine (PPAI), ethylenediamine hydroiodide (EDAI)2)1, 4-xylylenediamine dihydroIodate (BABI)2) Decamethylenediamine Dihydroiodate (DDAI)2) Propylene Diamine (PDAI)2) Dihydroiodate, Ethylenedioxybisethylamine Dihydroiodate (EDBEI)2)1, 6-Hexanediamine Dihydroiodate (HDAI)2)1, 8-Octanediamin Dihydroiodate (ODAI)2)1, 4-phenylenediamine dihydroiodate (PhDAI)2) M-phenylenediamine dihydroiodate (mpHDAI)2) O-phenylenediamine dihydroiodate (oPhDAI)2) And 1, 4-dimethyldiamine dihydroiodate (PhDMAI)2) At least one of (1).
In alternative embodiments, the short-chain organic amine salt includes, but is not limited to, at least one of formamidine hydrochloride (FACl), formamidine hydrochloride (MACl), formamidine hydrobromide (FABr), methylamine hydrobromide (MABr), formamidine hydroiodide (FAI), and methylamine hydroiodide (MAI).
In alternative embodiments, the alkali metal halide includes, but is not limited to, at least one of CsI, RbI, KI, NaI, LiI, CsBr, RbBr, KBr, NaBr, LiBr, CsCl, RbCl, KCl, NaCl, and LiCl.
In alternative embodiments, the divalent metal halide includes, but is not limited to, PbI2、PbBr2、PbCl2、SnI2、SnBr2、SnCl2、MnI2、MnBr2And MnCl2At least one of (1).
In an alternative embodiment, the perovskite precursor solution is obtained by mixing the precursor materials at 20-120 ℃ for 0.5-48h, for example, at 60 ℃ for 1 h.
In an alternative embodiment, the concentration of the perovskite precursor solution is between 0.1 and 2 mol/L.
In an alternative embodiment, the perovskite precursor solution further comprises an additive.
In alternative embodiments, the additive includes, but is not limited to, at least one of hydrochloric acid, hydrobromic acid, methyl amine chloride, methyl amine bromide, polyvinylpyrrolidone, polyvinyl alcohol, and polyethylene oxide.
In alternative embodiments, the deposition means includes, but is not limited to, at least one of spin coating, doctor blading, spraying, printing, and evaporation.
In an alternative embodiment, the spin coating is performed at 500-6000rpm, for example 3000 rpm.
In an alternative embodiment, the post-treatment comprises an annealing treatment.
In alternative embodiments, the annealing process comprises a thermal annealing process, a solvent annealing process, or a vacuum annealing process.
In an alternative embodiment, the annealing treatment is carried out at 60-180 deg.C for 3-120min, for example at 100 deg.C for 10 min.
In a second aspect, the present application provides the use of a metal halide perovskite multiple quantum well material for generating laser multipulses.
In a third aspect, the present application provides the application of the laser multi-pulse obtained by the above-mentioned generation method in spectroscopy, optical imaging, optical communication or nonlinear optical fiber, especially in miniaturized and integrated devices.
The beneficial effect of this application includes:
the laser multi-pulse generation method provided by the application is simple in process and low in cost, the metal halide perovskite multi-quantum well material comprises perovskite quantum wells with different thicknesses, the thicker quantum well band gap is narrower, the thinner quantum well band gap is wider, and after the wide band gap phase is excited by exciting light, generated current carriers can be gradually transmitted to the narrow band gap phase. The carrier transport from the wide bandgap phase to the narrow bandgap phase is done in multiple steps due to the different transport rates in different directions. The technology does not depend on complex optical equipment, and is easy to miniaturize and integrate. The obtained ultrashort laser double (multi) pulse can be used in the fields of spectroscopy, optical imaging, optical communication or nonlinear light and the like.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings needed to be used in the embodiments will be briefly described below, it should be understood that the following drawings only illustrate some embodiments of the present invention and therefore should not be considered as limiting the scope, and for those skilled in the art, other related drawings can be obtained according to the drawings without inventive efforts.
FIG. 1 is a schematic diagram of a process for preparing a metal halide perovskite multi-quantum well thin film in example 1 of the present application;
FIG. 2(a) is a schematic view showing the microstructure of a metal halide perovskite multi-quantum well thin film in example 1 of the present application;
FIG. 2(b) is a schematic view of the carrier transport in the metal halide perovskite multi-quantum well thin film in example 1 of the present application;
FIG. 3 is an SEM image of a metal halide perovskite multi-quantum well thin film in example 1 of the present application;
FIG. 4 is an absorption spectrum of a metal halide perovskite multi-quantum well thin film in example 1 of the present application;
fig. 5 is a time-resolved photoluminescence spectrum of the metal halide perovskite multi-quantum well thin film under different excitation light intensities in the application example 1.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below. The examples, in which specific conditions are not specified, were conducted under conventional conditions or conditions recommended by the manufacturer. The reagents or instruments used are not indicated by the manufacturer, and are all conventional products available commercially.
The following specifically describes the method for generating laser multi-pulses and the application of the metal halide perovskite multi-quantum well material in laser multi-pulse generation.
The application uses a metal halide perovskite multi-quantum well material (multidimensional perovskite quantum well material for short) with the structural general formula of L2An-1MnX3n+1Or DAn-1MnX3n+1Wherein, L represents long-chain positive divalent organic cation, D represents long-chain positive divalent metal cation, A represents short-chain positive divalent cation, M represents positive divalent metal cation, and X represents negative monovalent anion. The metal halideThe inorganic layer structure of the compound perovskite multi-quantum well material is [ MX [ ]6]4-Is represented by, n represents [ MX [ ]6]4-The number of layers of (a). The metal halide perovskite multi-quantum well material is formed by mixing quantum wells with different n values.
Wherein [ MX ]6]4-Layers are connected together by intercalated A ions and separated by intercalation of L or D ions, of different thicknesses [ MX6]4-The layers are coupled to each other by van der waals forces, thereby forming a quantum well structure.
In alternative embodiments, the long chain monovalent organic cation includes, but is not limited to, Isopropylamine (IPA)+) Naphthalene Methylamine (NMA)+) Phenylmethylamine (PMA)+) Phenylethylamine (PEA)+) Phenyl Trimethylamine (PTA)+) Butylamine (BA)+) Isobutylamine (i-BA)+) Tert-butylamine (t-BA)+) Ethylamine (EA)+) Hexylamine (HA)+) Octylamine (OA)+) Aniline (PhA)+) And Amphetamine (PPA)+) At least one of (1).
Preferably, the long chain divalent organic cation includes, but is not limited to, Ethylenediamine (EDA)2+)1, 4-xylylenediamine (BAB)2 +) Decamethylenediamine (DDA)2+) Propylene Diamine (PDA)2+) Ethylenedioxydiethylamine (EDBE)2+)1, 6-Hexanediamine (HDA)2+)1, 8-Octanediamine (ODA)2+)1, 4-phenylenediamine (PhDA)2+) M-phenylenediamine (mPhDA)2+) O-phenylenediamine (oPhDA)2+) And 1, 4-dimethyldiamine (PhDMA)2+) At least one of (1).
In alternative embodiments, short chain monovalent cations include, but are not limited to, Formamidine (FA)+) Methylamine (MA)+)、Cs+、Rb+、K+And Na+At least one of (1).
In an alternative embodiment, the positive divalent metal cation includes, but is not limited to, Pb2+、Sn2+、Mn2+And Ca2+At least one of (1).
In alternative embodiments, the negative monovalent anion includes, but is not limited to, F-、Cl-、Br-、I-And (BF)4)-At least one of (1).
In an alternative embodiment, the multi-dimensional perovskite quantum well material is in the form of a thin film. The multi-dimensional perovskite quantum well material may be a multi-dimensional perovskite quantum well thin film having a thickness of 50-2000nm, such as 50nm, 100nm, 200nm, 500nm, 800nm, 1000nm, 1500nm or 2000 nm.
The metal halide perovskite multi-quantum well material is obtained by carrying out post-treatment on a thin film formed on the surface of a substrate by a perovskite precursor solution.
By way of reference, the preparation process may, for example, comprise the following steps:
(1) preparing a perovskite precursor solution;
(2) depositing a perovskite precursor solution on the surface of a substrate to form a thin film;
(3) and carrying out post-treatment on the perovskite thin film deposited on the surface of the substrate.
In an alternative embodiment, the material from which the perovskite precursor solution is prepared must comprise a long chain organic amine salt, a short chain organic amine salt, lead halide, wherein the short chain organic amine salt may be partially or fully substituted with an alkali metal halide.
In alternative embodiments, long chain organic amine salts include, but are not limited to, isopropylamine hydroiodide (IPAI), naphthylamine hydroiodide (NMAI), phenylmethylamine hydroiodide (PMAI), phenylethylamine hydroiodide (PEAI), phenyltrimethylamine hydroiodide (PTAI), butylamine hydroiodide (BAI), isobutylamine hydroiodide (i-BAI), tert-butylamine hydroiodide (t-BAI), ethylamine hydroiodide (EAI), hexylamine Hydroiodide (HAI), octylamine hydroiodide (OAI), aniline hydroiodide (PhAI), amphetamine (PPAI), ethylenediamine hydroiodide (EDAI)2)1, 4-xylylenediamine dihydroiodate (BABI)2) Decamethylenediamine Dihydroiodate (DDAI)2) Propylene Diamine (PDAI)2) Dihydroiodate, Ethylenedioxybisethylamine Dihydroiodate (EDBEI)2)1, 6-Hexanediamine Dihydroiodate (HDAI)2)1, 8-Octanediamin Dihydroiodate (ODAI)2)1, 4-phenylenediamine dihydroiodate (PhDAI)2) M-phenylenediamine dihydroiodate (mpHDAI)2) O-phenylenediamine dihydroiodate (oPhDAI)2) And 1, 4-dimethyldiamine dihydroiodate (PhDMAI)2) At least one of (1).
In alternative embodiments, the short-chain organic amine salt includes, but is not limited to, at least one of formamidine hydrochloride (FACl), formamidine hydrochloride (MACl), formamidine hydrobromide (FABr), methylamine hydrobromide (MABr), formamidine hydroiodide (FAI), and methylamine hydroiodide (MAI).
In alternative embodiments, the alkali metal halide includes, but is not limited to, at least one of CsI, RbI, KI, NaI, LiI, CsBr, RbBr, KBr, NaBr, LiBr, CsCl, RbCl, KCl, NaCl, and LiCl.
In alternative embodiments, the divalent metal halide includes, but is not limited to, PbI2、PbBr2、PbCl2、SnI2、SnBr2、SnCl2、MnI2、MnBr2And MnCl2At least one of (1).
The perovskite precursor solution is obtained by mixing the precursor materials at 20-120 ℃ for 0.1-48h, for example at 60 ℃ for 1 h.
In alternative embodiments, the concentration of the perovskite precursor solution may be in the range of 0.1 to 2mol/L, such as 0.1mol/L, 0.5mol/L, 1mol/L, or 2mol/L, and the like.
In an alternative embodiment, the perovskite precursor solution may further contain additives. The additive may include, for example, at least one of hydrochloric acid (HCl), hydrobromic acid (HBr), polyvinylpyrrolidone (PVP), polyvinyl alcohol (PEG), and polyethylene oxide (PEO). The crystallization kinetics and the final morphology of the multi-dimensional perovskite quantum well material can be adjusted by adding the additive.
It is worth to be noted that the multi-dimensional quantum well thin film microstructures prepared from different precursor solutions are different, and the wavelength, pulse width and time interval of the obtained double pulses are also different. The specific components, proportion and concentration can be determined according to actual requirements.
In alternative embodiments, the deposition means may comprise at least one of spin coating, doctor blading, spraying, printing, evaporation. Preferably, the deposition can be performed by a one-step spin coating method.
In an alternative embodiment, spin coating may be performed at 500-.
In an alternative embodiment, the post-treatment comprises an annealing treatment. The annealing process may in turn comprise a thermal annealing process, a solvent annealing process or a vacuum annealing process.
The annealing treatment may be carried out at 60 to 180 ℃ for 3 to 120min, for example, at 100 ℃ for 10 min.
Further, the present application provides a method for generating laser multi-pulses, comprising the steps of: a suitable pulsed laser (e.g., a single pulse laser) is used to excite a metal halide perovskite multiple quantum well material as described above, and the stimulated emission signal is detected. The laser multi-pulse comprises an ultrashort laser double-pulse or an ultrashort laser multi-pulse.
In alternative embodiments, the intensity of the pulsed laser may be in the range of 0.1-1000. mu.J/cm2E.g. 1. mu.J/cm2、10μJ/cm2、50μJ/cm2、100μJ/cm2、500μJ/cm2Or 1000. mu.J/cm2Etc., the pulse width may be 10fs-100ns, such as 10fs, 100fs, 1ps, 100ps, 1ns, 10ns, or 100ns, etc., and the frequency may be 1Hz-100MHz, such as 1Hz, 10Hz, 100kHz, 500kHz, 1000kHz, 10MHz, or 100MHz, etc.
It is worth noting that the specific excitation light wavelength and intensity can be adjusted according to the material system and the observed stimulated emission signal, in view of the different requirements of different material systems for excitation light.
In the perovskite material (perovskite thin film) with the multi-dimensional perovskite quantum well structure, a low-dimensional phase with a wider band gap and a high-dimensional phase with a narrower band gap exist, namely, in the multi-dimensional perovskite quantum well material, the low-dimensional perovskite with a wide band gap and the high-dimensional perovskite with a narrow band gap coexist. The excitation light pulse first excites the wide bandgap phase, producing a large number of excitons which are progressively localised to the narrow bandgap phase and which are transported perpendicular to the surface of the wide bandgap perovskite faster than parallel. Thus, the carriers transported in the vertical direction reach the narrow bandgap perovskite first, so that the optical gain of the narrow bandgap phase gradually increases, and when the gain exceeds the loss, the first stimulated emission pulse is generated. The subsequent exciton localization in the parallel direction continues and after a period of time a second stimulated emission pulse is generated. That is, under the irradiation of the excitation light, there are multiple energy relaxation processes between perovskites of different dimensions. This enables two or more laser pulses to be excited with one laser pulse.
The method gets rid of the dependence on a complex optical device in the prior art, only utilizes the intrinsic property of the material, uses the multi-dimensional perovskite quantum well material as a gain medium, and realizes the excitation of two pulses by using a single pulse by means of a multi-step energy relaxation process in the material.
The laser multi-pulse obtained by the method can be applied to spectroscopy, optical imaging, optical communication or nonlinear optical fibers, and can be particularly applied to miniaturization and integrated devices.
The features and properties of the present invention are described in further detail below with reference to examples.
Example 1
This example provides a network based on (NMA)2(FA)n-1PbnI3n+1Ultrashort double laser pulses of the multi-dimensional perovskite quantum well film.
Referring to the figure, a schematic diagram of the preparation process of the multi-dimensional perovskite quantum well thin film is shown in fig. 1.
The multi-dimensional perovskite quantum well film is prepared from a perovskite precursor liquid through a one-step spin coating method, wherein the precursor liquid mainly comprises the following components: naphthylammonium hydroiodide (NMAI, C)10H7CH2NH3I)114.45g, formamidine hydroiodide (FAI, NH)2CHNH3I)34.38g, lead iodide (PbI)2)184.40g, 2mL of N, N-Dimethylformamide (DMF).
The preparation method comprises the following steps: accurately weighing the reagents, placing the reagents in a glass bottle to serve as precursor liquid, and heating and stirring the precursor liquid at 60 ℃ for about 1 hour to fully dissolve the solute.
In a nitrogen-filled glove box, 50 μ L of perovskite precursor solution is dropped on a cleaned quartz b sheet, spin-coated at 3000rpm to form a film, and then placed on a 100 ℃ hot bench for annealing for 10 minutes.
The schematic view of the microstructure of the multi-dimensional perovskite quantum well thin film is shown in fig. 2(a), and the schematic view of carrier transmission in the multi-dimensional perovskite quantum well thin film is shown in fig. 2 (b).
The SEM image of the obtained multi-dimensional perovskite quantum well thin film is shown in fig. 3. The results in FIG. 3 show that: the obtained perovskite film is compact, uniform and flat.
The absorption spectrum of the obtained multi-dimensional perovskite quantum well film is shown in fig. 4. The results in FIG. 4 show that: the thin film is self-assembled to form a multi-quantum well structure containing quantum wells with different thicknesses (n), and the quantum wells with n being 2 are the most.
Then, a laser beam having a center wavelength of 400nm (pulse width of about 50fs, repetition frequency of 1 kHz) was used as excitation light, and the excitation light was focused by a cylindrical lens to form a stripe spot of 5mm × 0.2mm and focused on the perovskite thin film. The excitation light intensity is adjusted to be respectively as follows: 2. 4, 8, 11, 15, 23, 25, 35, 40, 50 and 70 muJ/cm2. The resulting emission was collected from the side of the film, introduced into an optical fiber coupled to a spectrometer (Acton, Spectra Pro 2500i) using a pair of lenses, and detected by a charge coupled device (Princeton Instruments, Pixis 400B). The time resolved luminescence spectra were measured using a fringe camera (Optronis Optoscope).
The photoluminescence spectrogram of the multidimensional perovskite quantum well thin film under different excitation light intensities is shown in figure 5. The results in FIG. 5 show that: when the pump light intensity of the multi-dimensional perovskite quantum well film reaches the stimulated radiation threshold value, two independent laser pulses can appear, the pulse width of the two independent laser pulses is 40ps, and the interval time is 70 ps.
In summary, the laser multi-pulse generation method provided by the application is simple in process and low in cost, the metal halide perovskite multi-quantum well material comprises perovskite quantum wells with different thicknesses, the thicker quantum well band gap is narrower, the thinner quantum well band gap is wider, and after a wide band gap phase is excited by excitation light, generated current carriers can be gradually transmitted to a narrow band gap phase. The carrier transport from the wide bandgap phase to the narrow bandgap phase is done in multiple steps due to the different transport rates in different directions. The technology does not depend on complex optical equipment, and is easy to miniaturize and integrate. The obtained ultrashort laser double (multi) pulse can be used in the fields of spectroscopy, optical imaging, optical communication or nonlinear light and the like.
The above is only a preferred embodiment of the present invention, and is not intended to limit the present invention, and various modifications and changes will occur to those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (19)
1. A method for generating multiple pulses of laser light, comprising the steps of: exciting the metal halide perovskite multi-quantum well material by using pulse laser, and detecting an excited radiation signal;
the generated laser multi-pulse comprises an ultra-short laser double-pulse or an ultra-short laser multi-pulse;
the intensity of the pulse laser is 2-1000 muJ/cm2The pulse width is 10fs-100ps, and the frequency is 1Hz-100 MHz;
the structural general formula of the metal halide perovskite multi-quantum well material is L2An-1MnX3n+1Or DAn-1MnX3n+1Wherein L represents a long-chain positive divalent organic cation, D represents a long-chain positive divalent organic cation, a represents a short-chain positive monovalent cation, M represents a positive divalent metal cation, and X represents a negative monovalent anion;
the long-chain normal monovalent organic cation is selected from at least one of isopropylamine, naphthylmethylamine, benzylamine, phenethylamine, phenyltrimethylamine, butylamine, isobutylamine, tert-butylamine, ethylamine, hexylamine, octylamine, aniline and amphetamine; the long-chain positive divalent organic cation is selected from ethylenediamine, 1, 4-xylylenediamine, decamethylenediamine, propylenediamine, ethylenedioxybisethylamine, 1, 6-hexamethylenediamine, 1, 8-octamethylenediamine, 1, 4-phenylenediamine, m-phenylenediamine, and mixtures thereof,At least one of o-phenylenediamine and 1, 4-dimethyldiamine; the short-chain monovalent cation is selected from formamidine, methylamine and Cs+、Rb+、K+And Na+At least one of; the positive divalent metal cation is selected from Pb2+、Sn2+、Mn2+And Ca2+At least one of; the negative monovalent anion is selected from F-、Cl-、Br-、I-And (BF)4)-At least one of;
the inorganic layer structure of the metal halide perovskite multi-quantum well material is [ MX [ ]6]4-Is represented by, n represents [ MX [ ]6]4-The number of layers of (a); the metal halide perovskite multi-quantum well material is formed by mixing quantum wells with different n values;
wherein [ MX ]6]4-Layers are connected together by intercalated A ions and separated by intercalation of L or D ions, of different thicknesses [ MX6]4-The layers are coupled to each other by van der waals forces, thereby forming a quantum well structure;
the metal halide perovskite multi-quantum well material is a thin film with the thickness of 800-2000 nm.
2. The production method according to claim 1, wherein the metal halide perovskite multi-quantum well material is obtained by post-treating a thin film formed on the surface of a substrate from a perovskite precursor solution.
3. The production method according to claim 2, characterized in that a perovskite precursor solution is prepared; depositing the perovskite precursor solution on the surface of a substrate to form a thin film; and performing post-treatment on the perovskite thin film deposited on the surface of the substrate.
4. A production method according to claim 2 or 3, characterized in that the precursor materials for preparing the perovskite precursor solution comprise long-chain organic amine salts, short-chain organic amine salts and divalent metal halides, wherein the short-chain organic amine salts are partially or fully substituted by alkali metal halides.
5. The production method according to claim 4, the long-chain organic amine salt includes at least one of isopropylamine hydroiodide, naphthylamine hydroiodide, phenylmethylamine hydroiodide, phenylethylamine hydroiodide, phenyltrimethylamine hydroiodide, butylamine hydroiodide, isobutylamine hydroiodide, tert-butylamine hydroiodide, ethylamine hydroiodide, hexylamine hydroiodide, octylamine hydroiodide, aniline hydroiodide, amphetamine, ethylenediamine dihydroiodate, 1, 4-xylylenediamine dihydroiodate, decamethylenediamine dihydroiodate, propylenediamine dihydroiodate, ethylenedioxydiethyleneamine dihydroiodate, 1, 6-hexamethylenediamine dihydroiodate, 1, 8-octamethylenediamine dihydroiodate, 1, 4-phenylenediamine dihydroiodate, m-phenylenediamine dihydroiodate, o-phenylenediamine dihydroiodate, and 1, 4-dimethyldiamine dihydroiodate.
6. The method of generating as claimed in claim 4, wherein the short chain organic amine salt comprises at least one of formamidine hydrochloride, methylamine hydrochloride, formamidine hydrobromide, methylamine hydrobromide, formamidine hydroiodide and methylamine hydroiodide.
7. The production method according to claim 4, wherein the alkali metal halide includes at least one of CsI, KI, NaI, LiI, CsBr, KBr, NaBr, LiBr, CsCl, KCl, NaCl, and LiCl.
8. The method of generating as defined in claim 4, wherein the divalent metal halide comprises PbI2、PbBr2、PbCl2、SnI2、SnBr2、SnCl2、MnI2、MnBr2And MnCl2At least one of (1).
9. The production method according to claim 4, characterized in that the perovskite precursor solution is obtained by mixing the precursor materials at 20-120 ℃ for 0.1-48 h.
10. A production method according to claim 4, characterized in that the concentration of the perovskite precursor solution is 0.1-2 mol/L.
11. The production method according to claim 4, characterized in that the perovskite precursor solution contains an additive.
12. The method of generating as defined in claim 11, wherein the additive includes at least one of hydrochloric acid, hydrobromic acid, methyl amine chloride, methyl amine bromide, polyvinylpyrrolidone, polyvinyl alcohol, and polyethylene oxide.
13. The method of claim 2, wherein depositing comprises at least one of spin coating, doctor blading, spraying, printing, and evaporation.
14. The method as claimed in claim 13, wherein the spin coating is performed at a speed of 500-6000 rpm.
15. The method of generating as defined in claim 2, wherein the post-processing comprises a thermal annealing process, a solvent annealing process or a vacuum annealing process.
16. The method of claim 15, wherein the annealing is performed at 60-180 ℃ for 3-120 min.
17. Use of a metal halide perovskite multiple quantum well material for generating laser multiple pulses.
18. Use of the laser multi-pulses obtained by the method of generating as claimed in any one of claims 1 to 16 in spectroscopy, optical imaging, optical communication or non-linear optical fibers.
19. Use according to claim 18, wherein the laser multi-pulses are used in miniaturized and integrated devices.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
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