CN110994345A - Tunable laser based on self-trapping exciton - Google Patents
Tunable laser based on self-trapping exciton Download PDFInfo
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- CN110994345A CN110994345A CN201911302804.6A CN201911302804A CN110994345A CN 110994345 A CN110994345 A CN 110994345A CN 201911302804 A CN201911302804 A CN 201911302804A CN 110994345 A CN110994345 A CN 110994345A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01S—DEVICES USING THE PROCESS OF LIGHT AMPLIFICATION BY STIMULATED EMISSION OF RADIATION [LASER] TO AMPLIFY OR GENERATE LIGHT; DEVICES USING STIMULATED EMISSION OF ELECTROMAGNETIC RADIATION IN WAVE RANGES OTHER THAN OPTICAL
- 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
- H01S3/163—Solid materials characterised by a crystal matrix
- H01S3/1645—Solid materials characterised by a crystal matrix halide
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01S—DEVICES USING THE PROCESS OF LIGHT AMPLIFICATION BY STIMULATED EMISSION OF RADIATION [LASER] TO AMPLIFY OR GENERATE LIGHT; DEVICES USING STIMULATED EMISSION OF ELECTROMAGNETIC RADIATION IN WAVE RANGES OTHER THAN OPTICAL
- H01S3/00—Lasers, i.e. devices using stimulated emission of electromagnetic radiation in the infrared, visible or ultraviolet wave range
- H01S3/09—Processes or apparatus for excitation, e.g. pumping
- H01S3/091—Processes or apparatus for excitation, e.g. pumping using optical pumping
- H01S3/094—Processes or apparatus for excitation, e.g. pumping using optical pumping by coherent light
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01S—DEVICES USING THE PROCESS OF LIGHT AMPLIFICATION BY STIMULATED EMISSION OF RADIATION [LASER] TO AMPLIFY OR GENERATE LIGHT; DEVICES USING STIMULATED EMISSION OF ELECTROMAGNETIC RADIATION IN WAVE RANGES OTHER THAN OPTICAL
- H01S3/00—Lasers, i.e. devices using stimulated emission of electromagnetic radiation in the infrared, visible or ultraviolet wave range
- H01S3/10—Controlling the intensity, frequency, phase, polarisation or direction of the emitted radiation, e.g. switching, gating, modulating or demodulating
- H01S3/10007—Controlling the intensity, frequency, phase, polarisation or direction of the emitted radiation, e.g. switching, gating, modulating or demodulating in optical amplifiers
- H01S3/10023—Controlling the intensity, frequency, phase, polarisation or direction of the emitted radiation, e.g. switching, gating, modulating or demodulating in optical amplifiers by functional association of additional optical elements, e.g. filters, gratings, reflectors
- H01S3/1003—Controlling the intensity, frequency, phase, polarisation or direction of the emitted radiation, e.g. switching, gating, modulating or demodulating in optical amplifiers by functional association of additional optical elements, e.g. filters, gratings, reflectors tunable optical elements, e.g. acousto-optic filters, tunable gratings
Abstract
The invention belongs to the field of photoelectric devices, and discloses a tunable laser based on a self-trapping exciton, wherein a gain medium of the laser comprises a material with a self-trapping exciton luminescent property, and the laser output laser wavelength can be tunable within a visible light range from 400nm to 750nm by utilizing the luminescent properties of large Stokes shift and wide spectral range of the self-trapping exciton of the gain medium through the mode selection effect of a resonant cavity. The invention can effectively expand the wavelength range of the laser output by the tunable laser by taking the material with the self-trap exciton luminescent property as the gain medium of the laser, thereby obtaining the large-range tunable laser. Compared with the prior art, the invention fills the blank of the tunable laser with wide spectrum and large range in visible light and near ultraviolet regions, has no problems of stability, toxicity and the like compared with the current dye laser, and has obvious advantages.
Description
Technical Field
The invention belongs to the field of photoelectric devices, and particularly relates to a tunable laser based on a self-trapping exciton, wherein a gain medium of the laser has effective self-trapping exciton (self-trapped exciton) emission, and particularly, the all-solid-state wide-spectrum large-range tunable laser can be obtained.
Background
Compared with the traditional solid-state laser, the wide-range tunable laser has a wide band tuning range, the band is generally as wide as more than 50nm, and the application is wide. The tuning range of a large-range tunable laser extremely depends on a gain medium (generally, the gain medium generally requires large gain and small loss, and an energy level system is a three-level or four-level system so as to form a reversed particle number; for the gain medium with a small light emitting range, only laser with a single wavelength can be output), the wide-range tunable laser mainly comprises a semiconductor laser, a color center laser and a vibration level laser in an infrared band, various dye lasers and titanium-doped sapphire lasers are currently the most important visible light tunable lasers, the tuning range of the dye laser is extremely wide, but the light stability of the dye cannot be solved later, and the development of the dye laser is severely restricted. Titanium doped sapphire has very good performance, but the wide tunable range can only achieve red light, and therefore, tuning can only be performed over a very small fraction of the visible range.
Disclosure of Invention
In view of the above defects or improvement needs in the prior art, it is an object of the present invention to provide a tunable laser based on self-trapping excitons, wherein a material having a self-trapping exciton emitting property is used as a gain medium of the laser, so that the wavelength range of laser light output by the tunable laser can be effectively extended, and a wide-range tunable laser with a visible light band of 400nm to 750nm can be obtained. The materials with the self-trap exciton luminescent property represented by perovskite materials have good emission in a visible light waveband, excellent light stability and thermal stability and extremely small self-absorption, so the materials are particularly suitable for application in the field of continuously tunable lasers in the visible light range. Compared with the prior art, the invention fills the blank of the tunable laser with wide spectrum and large range in visible light and near ultraviolet regions, has no problems of stability, toxicity and the like compared with the current dye laser, and has obvious advantages.
In order to achieve the above object, according to the present invention, there is provided a tunable laser based on self-trapping excitons, wherein a gain medium of the laser comprises a material having a self-trapping exciton luminescent property, and the laser output laser wavelength can be tunable in a visible light range of 400nm to 750nm by a mode selection effect of a resonant cavity by using the luminescent property of the gain medium that the self-trapping exciton has a large stokes shift and a wide spectral range.
As a further preferred aspect of the present invention, the gain medium is made of a perovskite material.
As a further preferred aspect of the present invention, the gain medium is made of an all-inorganic perovskite material.
As a further preferred aspect of the present invention, the gain medium is Cs3Cu2I5Material, Cs4SnBr6Doping the material, or Bi with correspondingly obtained Cs2NaxAg1-xInCl6A Bi material; wherein, the Cs2NaxAg1-xInCl6The Bi material satisfies that x is more than or equal to 0.2 and less than or equal to 0.8.
As a further preferred aspect of the present invention, Cs is used as the gain medium2NaxAg1-xInCl6Bi material, and x is 0.4.
As a further preferred embodiment of the present invention, the laser is a dye laser, a fiber laser, a disk laser, or a solid laser.
As a further preferred aspect of the present invention, when the laser adopts a laser structure of a dye laser, the gain medium is a perovskite quantum dot solution or a solid gel of perovskite quantum dots.
As a further preferred aspect of the present invention, when the laser adopts a laser structure of a fiber laser, the gain medium includes, in addition to the optical fiber itself, a perovskite material coated on the surface of the optical fiber, or a perovskite quantum dot solution disposed outside for soaking the optical fiber; the resonant cavity is composed of a fiber grating or a fiber circulator or a free space cavity mirror.
As a further preferred aspect of the present invention, when the laser has a laser structure of a disk laser, the gain medium is a perovskite film formed by evaporation or spin coating;
preferably, the resonant cavity consists of a free space cavity mirror; or the resonant cavity consists of a distributed Bragg reflection film and a total reflection film which are respectively positioned on the upper surface and the lower surface of the perovskite film, at the moment, the distributed Bragg reflection film and the total reflection film are respectively used as an upper cavity mirror and a lower cavity mirror, wherein the distributed Bragg reflection film is a dielectric film prepared by a vacuum method, the total reflection film is preferably a silver film, and the silver film is also prepared by the vacuum method.
As a further preferred aspect of the present invention, when the laser has a laser structure of a solid-state laser, the gain medium is a perovskite crystal whose surface is polished, and an antireflection film made of a dielectric film is further deposited on the surface of the perovskite crystal; the resonant cavity consists of a cavity mirror in free space, and the cavity mirror is a high-reflection mirror with a visible light wave band of 400-750 nm.
Through the technical scheme, compared with the prior art, the tunable laser has the advantages that the characteristics of large self-trapped exciton (self-trapped exciton) stokes shift and wide spectrum are applied in the tunable laser, and the tunable laser with the output laser wavelength tunable within the visible light range of 400nm to 750nm can be obtained (specific tuning is achieved by utilizing mode selection of a resonant cavity to achieve tuning based on the light emission spectrum of a gain medium). The laser gain medium adopts a material with self-trapping exciton luminescent property, so that a large-range tunable laser can be obtained, and the wavelength of emitted laser can be continuously adjustable in the range of 400nm to 750 nm.
The laser gain medium is improved, materials with the self-sinking state exciton luminescent property are used as the laser gain medium, the materials with the self-sinking state exciton luminescent property have wide spectrum emission in a visible light range, the emission mechanism of the gain medium is self-sinking state exciton luminescence, and due to the wide spectrum and large Stokes shift characteristics of the self-sinking state exciton, a laser can be adjusted in a very wide range, and meanwhile, the large Stokes shift ensures minimum self-absorption, so that the loss of laser in the gain medium is reduced; the excitation wavelength is in near ultraviolet region, the emission wavelength is in visible light region, and the device has large Stokes shift and wide emission, the Stokes shift can reach over 100nm, and the emission wavelength range can be from 400nm to 750 nm. The broad spectrum represents a large, widely tunable range, with a large stokes shift ensuring low self-absorption.
Different perovskites have different luminescent properties, and the present invention utilizes such specific perovskites, i.e., Cs, possessing self-trapped exciton luminescence2NaxAg1-xInCl6Bi material (x is more than or equal to 0.2 and less than or equal to 0.8, x can be particularly 0.4), Cs3Cu2I5Material, Cs4SnBr6The perovskite material with near ultraviolet excitation and broad spectrum self-trapping state exciton emission can realize excitation (namely near ultraviolet excitation) of the material under the near ultraviolet light with the wavelength of 200nm to 380nm, and meanwhile, the broad spectrum self-trapping state exciton emission can realize the emission of the self-trapping state exciton with the wavelength of 400nm to 750 nm. The invention can manufacture tunable laser with variable output wavelength by utilizing the characteristic of wide spectrum of self-trapping exciton-luminous perovskite and the mode selection effect of the resonant cavity, and the spectral range can cover the whole visible light wave band, namely 400 nm-750 nm.
Cs2NaxAg1-xInCl6:Bi、Cs3Cu2I5、Cs4SnBr6The materials with self-trap exciton luminescence have wide spectrum with half peak width more than 100nm, which is significantly wider than the single dye of the present wide-range tunable laser-dye laser with visible light band, thus having wider tuning range; and, viaIt is verified that the emission of the self-trapping excitons during their light emission from the self-trapping excitons can be considered as a four-level system, and population inversion is easily formed, thereby having an advantage as a laser gain medium in nature. In addition, since the triplet state of the dye does not emit light and has a long lifetime, a quencher must be introduced to rapidly quench the triplet state, which results in extremely low energy utilization efficiency, whereas the self-trapped exciton in the present invention does not emit light, and the light emission efficiency can be as high as 90%. And because all inorganic materials can be preferably adopted, the stability is higher compared with organic dye molecules, so that the laser has longer service life. In addition, most dye molecules are toxic, and the self-trapping exciton luminescent material disclosed by the invention is relatively weak in toxicity, so that the self-trapping exciton luminescent material has a wide application prospect.
The invention also provides four different device structures which can be applied to various different occasions. For example, when a device structure of a dye laser is adopted, the gain medium is perovskite quantum dot solution or solid gel of perovskite quantum dots, and a cavity mirror in free space is used as a resonant cavity. When the device structure of the fiber laser is adopted, the gain medium is perovskite quantum dot solution or perovskite quantum dot material coated on the surface of the optical fiber, evanescent waves of the micro-nano optical fiber are used for exciting the gain medium, and the fiber grating or the fiber circulator or the cavity mirror of a free space is used as a resonant cavity. The device structure of a disc laser is adopted, a gain medium is a perovskite film formed by evaporation or spin coating, and a distributed Bragg reflection film and a silver film total reflection film are respectively evaporated from top to bottom to serve as resonant cavities. When the device structure of the solid laser is adopted, the gain medium is a high-quality perovskite single crystal with a polished surface and an antireflection film plated, and a free-space cavity mirror is used as a resonant cavity.
The tunable laser can be tunable in a large range of visible light wave bands, particularly can be a wide-spectrum all-inorganic laser, and can be applied to the fields of ultrashort pulse, precision measurement and the like.
Drawings
FIG. 1 shows Cs2Na0.4Ag0.6In0.99Bi0.01Cl6(i.e., Cs2Na0.4Ag0.6InCl6Bi) and photoluminescence spectra (PLE) and (PL).
FIG. 2 shows Cs2Na0.4Ag0.6In0.99Bi0.01Cl6(i.e., Cs2Na0.4Ag0.6InCl6Bi) is heated on a 150 ℃ hot bench, and the result shows that the thermal stability is good.
FIG. 3 shows Cs2Na0.4Ag0.6In0.99Bi0.01Cl6(i.e., Cs2Na0.4Ag0.6InCl6Bi) in the air under the continuous irradiation of ultraviolet rays, and the result shows that the irradiation stability is good.
FIG. 4 shows Cs3Cu2I5Photoexcitation spectrum (PLE) and luminescence spectrum (PL).
FIG. 5 shows Cs4SnBr6Photoexcitation spectrum (PLE) and luminescence spectrum (PL).
Fig. 6 is a schematic structural view of a perovskite dye laser of the present invention.
FIG. 7 is a schematic structural diagram of a perovskite quantum dot fiber laser of the present invention; wherein FBG is fiber Bragg grating, WDM is wavelength division multiplexer, micro-nanofiber is micro-nanofiber, CNAIC QD is Cs2NaxAg1-xInCl6Bi (x is more than or equal to 0.2 and less than or equal to 0.8) quantum dots, and OSA is a spectrum analyzer.
FIG. 8 is a schematic structural diagram of a perovskite disk laser of the present invention.
Fig. 9 is a schematic structural view of a perovskite solid-state laser of the present invention.
FIG. 10 is a schematic diagram of luminescence of a trap exciton, wherein GS is a ground state, FE is a free exciton state, FC is a free carrier state, STE is a trap exciton state, and EgIs a band gap energy, EbAs exciton binding energy, EstTo sink energy by itself, EdIs lattice deformation energy, EPLIs the emission energy.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention. In addition, the technical features involved in the embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.
In general, the invention is applicable to lasers of various configurations, such as dye lasers, fiber lasers, disk lasers, solid state lasers. When a dye laser structure is employed, the gain medium is a perovskite quantum dot solution and a solid gel of perovskite quantum dots. When the fiber laser structure is adopted, the gain medium comprises perovskite quantum dot solution (at this moment, the optical fiber can be soaked in the perovskite quantum dot solution) or perovskite coated on the surface of the optical fiber besides the optical fiber, and the resonant cavity consists of a fiber grating or a circulator or a free space cavity mirror. When the disc laser structure is adopted, the gain medium is a perovskite film formed by vapor deposition or spin coating, and the upper cavity mirror and the lower cavity mirror can adopt a distributed Bragg reflection film or a total reflection film (such as a silver film) formed by dielectric films prepared by a vacuum method. When the structure of the solid laser is adopted, the gain medium is a perovskite crystal with a polished surface, an antireflection film formed by a medium film is evaporated on the surface of the gain medium, and the cavity mirror is a high-reflection mirror in a free space.
The following takes an example of an all-inorganic perovskite material with a broad spectrum emission property, and the specific examples are as follows:
example 1:
the preparation method of the dye laser in the embodiment specifically comprises the following steps:
a) and sequentially cleaning the glass bottle with deionized water for 10min, cleaning the glass bottle with acetone for 10min, cleaning the glass bottle with isopropanol for 10min, cleaning the glass bottle with deionized water for 10min, and blow-drying with a nitrogen gun.
b) 0.3366g (2mmol) CsCl, 0.0117g (0.2mmol) NaCl, 0.1146g (0.8mmol) AgCl, 0.2212g (1mmol) InCl were weighed out3,0.003g(0.01mmol)BiCl3Mixed on cleaned glassAdding 100ml of dimethyl sulfoxide (DMSO) into a glass bottle, heating and stirring at 80 deg.C until the raw materials are completely dissolved, adding 1ml of oleic acid, and mixing to obtain Cs2Na0.2Ag0.8InCl6A Bi precursor solution.
c) 10ml of isopropanol is taken and 0.4ml of Cs is added2Na0.2Ag0.8InCl6Stirring Bi precursor solution for 10min, standing for one day to obtain Cs2Na0.2Ag0.8InCl6Bi quantum dot solution.
d) The obtained Cs2Na0.2Ag0.8InCl6The Bi quantum dot solution is filled into a box, the dye box part of the dye laser is replaced, and the reflector of the dye laser is adjusted to obtain the dye laser which can be tuned in a large range.
Example 2:
the preparation method of the dye laser in the embodiment specifically comprises the following steps:
a) and sequentially cleaning the glass bottle with deionized water for 10min, cleaning the glass bottle with acetone for 10min, cleaning the glass bottle with isopropanol for 10min, cleaning the glass bottle with deionized water for 10min, and blow-drying with a nitrogen gun.
b) 0.3366g (2mmol) CsCl, 0.0468g (0.8mmol) NaCl, 0.0287g (0.2mmol) AgCl, 0.2212g (1mmol) InCl were weighed out3,0.003g(0.01mmol)BiCl3Mixing and placing in a cleaned glass bottle, adding 100ml of dimethyl sulfoxide (DMSO), heating and stirring at 80 ℃ until the raw materials are completely dissolved, adding 1ml of oleic acid, and mixing uniformly to obtain Cs2Na0.8Ag0.2InCl6A Bi precursor solution.
c) 1ml of isopropanol is taken and 0.4ml of Cs is added2Na0.8Ag0.2InCl6Stirring Bi precursor solution for 10min, and standing in a refrigerator at 4 deg.C for one day to obtain Cs2Na0.8Ag0.2InCl6Bi solid gel.
d) Using the obtained Cs2Na0.8Ag0.2InCl6Replacing the dye box part of the dye laser with Bi solid gel, and adjusting the reflector of the dye laser to obtain a large dye laserA range tunable dye laser.
Example 3:
in this embodiment, the method for manufacturing the fiber laser includes the following specific steps:
a) and sequentially cleaning the glass bottle with deionized water for 10min, cleaning the glass bottle with acetone for 10min, cleaning the glass bottle with isopropanol for 10min, cleaning the glass bottle with deionized water for 10min, and blow-drying with a nitrogen gun.
b) 0.3366g (2mmol) CsCl, 0.0234g (0.4mmol) NaCl, 0.0860g (0.6mmol) AgCl, 0.2212g (1mmol) InCl were weighed out3,0.003g(0.01mmol)BiCl3Mixing and placing in a cleaned glass bottle, adding 100ml of dimethyl sulfoxide (DMSO), heating and stirring at 80 ℃ until the raw materials are completely dissolved, adding 1ml of oleic acid, and mixing uniformly to obtain Cs2Na0.4Ag0.6InCl6A Bi precursor solution.
c) 10ml of isopropanol is taken and 0.4ml of Cs is added2Na0.4Ag0.6InCl6Stirring Bi precursor solution for 10min, standing for one day to obtain Cs2Na0.4Ag0.6InCl6Bi quantum dot solution.
d) And (3) installing one fiber grating on two translation stages through two fiber fixing stages, placing oxyhydrogen flames below the fiber grating, and controlling the translation stages to move in opposite directions to obtain the micro-nano optical fiber with the fiber grating at two ends.
e) Soaking the micro-nano optical fiber in Cs2Na0.4Ag0.6InCl6In the Bi quantum dot solution, a resonant cavity is formed by two fiber gratings, and 365nm pump light is input by a wavelength division multiplexer to obtain the fiber laser.
Example 4:
in this embodiment, the method for manufacturing the fiber laser includes the following specific steps:
a) and sequentially cleaning the glass bottle with deionized water for 10min, cleaning the glass bottle with acetone for 10min, cleaning the glass bottle with isopropanol for 10min, cleaning the glass bottle with deionized water for 10min, and blow-drying with a nitrogen gun.
b) 0.3366g (2mmol) CsCl, 0.0293 were weighed outg(0.5mmol)NaCl，0.0716g(0.5mmol)AgCl，0.2212g(1mmol)InCl3,0.003g(0.01mmol)BiCl3Mixing and placing in a cleaned glass bottle, adding 100ml of dimethyl sulfoxide (DMSO), heating and stirring at 80 ℃ until the raw materials are completely dissolved, adding 1ml of oleic acid, and mixing uniformly to obtain Cs2Na0.5Ag0.5InCl6A Bi precursor solution.
c) 10ml of isopropanol is taken and 0.4ml of Cs is added2Na0.5Ag0.5InCl6Stirring Bi precursor solution for 10min, standing for one day to obtain Cs2Na0.5Ag0.5InCl6Bi quantum dot solution.
d) A single mode fiber is installed on two translation stages through two fiber fixing stages, oxyhydrogen flames are placed below the single mode fiber, the translation stages are controlled to move in opposite directions, and the micro-nano fiber is obtained.
e) Soaking the micro-nano optical fiber in Cs2Na0.5Ag0.5InCl6In the Bi quantum dot solution, two additional free space cavity mirrors are used as resonant cavities, and 365nm pump light is input by an optical fiber coupler to obtain the optical fiber laser.
Example 5:
in this embodiment, the method for manufacturing the fiber laser includes the following specific steps:
a) and sequentially cleaning the glass bottle with deionized water for 10min, cleaning the glass bottle with acetone for 10min, cleaning the glass bottle with isopropanol for 10min, cleaning the glass bottle with deionized water for 10min, and blow-drying with a nitrogen gun.
b) 0.3366g (2mmol) CsCl, 0.0410g (0.7mmol) NaCl, 0.0430g (0.3mmol) AgCl, 0.2212g (1mmol) InCl were weighed out3,0.003g(0.01mmol)BiCl3Mixing and placing in a cleaned glass bottle, adding 100ml of dimethyl sulfoxide (DMSO), heating and stirring at 80 ℃ until the raw materials are completely dissolved, adding 1ml of oleic acid, and mixing uniformly to obtain Cs2Na0.7Ag0.3InCl6A Bi precursor solution.
c) 10ml of isopropanol is taken and 0.4ml of Cs is added2Na0.7Ag0.3InCl6Precursor bodyStirring the solution for 10min, standing for one day to obtain Cs2Na0.7Ag0.3InCl6Bi quantum dot solution.
d) A single mode fiber is installed on two translation stages through two fiber fixing stages, oxyhydrogen flames are placed below the single mode fiber, the translation stages are controlled to move in opposite directions, and the micro-nano fiber is obtained.
e) Soaking the micro-nano optical fiber in Cs2Na0.7Ag0.3InCl6In the Bi quantum dot solution, a fiber circulator is used as a resonant cavity, and 365nm pump light is input by a fiber coupler to obtain the fiber laser.
Example 6:
in this embodiment, the method for manufacturing the fiber laser includes the following specific steps:
a) and sequentially cleaning the glass bottle with deionized water for 10min, cleaning the glass bottle with acetone for 10min, cleaning the glass bottle with isopropanol for 10min, cleaning the glass bottle with deionized water for 10min, and blow-drying with a nitrogen gun.
b) 0.3366g (2mmol) CsCl, 0.0234g (0.4mmol) NaCl, 0.0860g (0.6mmol) AgCl, 0.2212g (1mmol) InCl were weighed out3,0.003g(0.01mmol)BiCl3Mixing and placing in a cleaned glass bottle, adding 100ml of dimethyl sulfoxide (DMSO), heating and stirring at 80 ℃ until the raw materials are completely dissolved, adding 1ml of oleic acid, and mixing uniformly to obtain Cs2Na0.4Ag0.6InCl6A Bi precursor solution.
c) 10ml of isopropanol is taken and 0.4ml of Cs is added2Na0.4Ag0.6InCl6Stirring Bi precursor solution for 10min, standing for one day to obtain Cs2Na0.4Ag0.6InCl6Bi quantum dot solution.
d) The obtained Cs2Na0.4Ag0.6InCl6Putting Bi quantum dot solution into a centrifuge, centrifuging at 8000r/min for 3min, and pouring out supernatant to obtain Cs2Na0.4Ag0.6InCl6Bi quantum dots.
e) And (3) installing one fiber grating on two translation stages through two fiber fixing stages, placing oxyhydrogen flames below the fiber grating, and controlling the translation stages to move in opposite directions to obtain the micro-nano optical fiber with the fiber grating at two ends.
f) Mixing Cs2Na0.4Ag0.6InCl6Coating Bi quantum dots on the surface of the micro-nano optical fiber, forming a resonant cavity by two fiber gratings, and inputting pump light of 365nm by using a wavelength division multiplexer to obtain the optical fiber laser.
Example 7:
the preparation method of the disk laser in the embodiment specifically comprises the following steps:
a) and sequentially cleaning the polytetrafluoroethylene inner container with deionized water for 10min, cleaning the polytetrafluoroethylene inner container with acetone for 10min, cleaning the polytetrafluoroethylene inner container with isopropanol for 10min, cleaning the polytetrafluoroethylene inner container with deionized water for 10min, and blow-drying with a nitrogen gun.
b) 0.3366g (2mmol) CsCl, 0.0176g (0.3mmol) NaCl, 0.1003g (0.7mmol) AgCl, 0.2212g (1mmol) InCl were weighed out3,0.003g(0.01mmol)BiCl3Mixing, placing in a cleaned polytetrafluoroethylene inner container, adding 15ml of hydrochloric acid (the mass percentage concentration of the hydrochloric acid can be 30%), and assembling a hydrothermal kettle.
c) And (3) placing the hydrothermal kettle in a muffle furnace, setting the temperature of the muffle furnace to be 20 ℃, increasing the temperature to 180 ℃ in 20min, preserving the temperature for 600min, and then slowly reducing the temperature to the room temperature in 1000 min.
d) Taking out the hydrothermal kettle in a muffle furnace, pouring hydrochloric acid out of the inner container, taking out crystals, and ultrasonically cleaning the crystals for 5min by using ethanol to obtain Cs with a clean surface2Na0.3Ag0.7InCl6Bi crystal.
e) The colorless optical glass is wiped by alcohol, and a silicon dioxide-titanium dioxide film is plated on the surface of the colorless optical glass to serve as a distributed Bragg reflection film (certainly, the distributed Bragg reflection film made of other film materials known in the prior art can also be adopted), and the colorless optical glass is characterized in that the reflectivity of the colorless optical glass in an excitation light wave band is small, so that the excitation light can be conveniently incident, and the emissivity of the colorless optical glass in an emission light wave band is large, so that a.
f) The obtained Cs2Na0.3Ag0.7InCl6The Bi crystal is put into a tungsten boat and is fixed in a high vacuum resistance evaporation coating machine, and the coated glass is horizontally fixed on a substrate frame 20cm above the tungsten boat. Starting the mechanical pump to vacuumize until the air pressure is less than 8Pa, and then starting the molecular pump to vacuumize until the air pressure is less than 8 multiplied by 10-4Pa, slowly increasing the voltage at two ends of the tungsten boat to make Cs2Na0.3Ag0.7InCl6Evaporating Bi crystal to a glass substrate at a high temperature to form a film, and finally obtaining Cs2Na0.3Ag0.7InCl6A Bi film.
g) 0.5g of high-quality silver particles are placed in a tungsten boat and fixed in a high-vacuum resistance evaporation coating machine, and the coated glass is horizontally fixed on a substrate frame 20cm above the tungsten boat. Starting the mechanical pump to vacuumize until the air pressure is less than 8Pa, and then starting the molecular pump to vacuumize until the air pressure is less than 8 multiplied by 10-4Pa, slowly increasing the voltage at two ends of the tungsten boat to evaporate silver to the glass substrate at high temperature to form a film, wherein the formed silver film is a total reflection film and is used as the other part of the resonant cavity to finally obtain Cs2Na0.3Ag0.7InCl6Bi disk device.
h) Pumping at one end plated with a distributed Bragg reflection film by using a 365nm ultraviolet semiconductor laser to amplify the spontaneous radiation light generated by the perovskite thin film, and oscillating in a resonant cavity formed by the distributed Bragg reflection film and a silver film so as to generate laser.
Example 8:
the preparation method of the disk laser in the embodiment specifically comprises the following steps:
a) cleaning the FTO glass and the centrifugal tube with deionized water for 10min, cleaning the FTO glass and the centrifugal tube with acetone for 10min, cleaning the FTO glass and the centrifugal tube with isopropanol for 10min, cleaning the FTO glass and the centrifugal tube with deionized water for 10min, blow-drying with a nitrogen gun, putting the FTO glass on a graphite support in a tube furnace, and putting the centrifugal tube in an oxygen-free glove box.
b) 3.8972g (15mmol) CsI, 1.9045g (5mmol) Cu were weighed in an oxygen-free glove box2I2Mixing, placing in a clean centrifuge tube, adding 10ml of dimethyl sulfoxide (DMSO), and shaking to dissolve completelyAnd (5) solving. 30ml of dichloromethane was added to the centrifuge tube and shaken for 5 min.
c) Placing the centrifuge tube into a centrifuge, centrifuging at 7000r/min for 10min, and pouring out the supernatant after centrifugation.
d) 5mL of dichloromethane was added to the obtained precipitate, the mixture was placed in a centrifuge, centrifuged at 5500r/min for 3min, and the supernatant was decanted after centrifugation.
e) The obtained Cs3Cu2I5Drying in a vacuum drying oven for 24h to obtain Cs3Cu2I5And (3) powder.
f) 0.5g of Cs was taken3Cu2I5Powder is put into a tube furnace and pumped to low vacuum (<8Pa) and then rapidly heating the tube furnace to 340 ℃ and preserving heat for 30min, and then naturally cooling to room temperature to obtain Cs with FTO glass as a substrate3Cu2I5A thin film device.
g) In Cs3Cu2I5Two additional free space cavity mirrors are added at two ends of the thin film device to be used as resonant cavities, and a 365nm semiconductor laser is used for pumping to generate stimulated radiation.
Example 9:
the preparation method of the disk laser in the embodiment specifically comprises the following steps:
a) cleaning ITO glass and a centrifugal tube with deionized water for 10min, cleaning ITO glass and the centrifugal tube with acetone for 10min, cleaning ITO glass and the centrifugal tube with isopropanol for 10min, cleaning ITO glass and the centrifugal tube with deionized water for 10min, and then blowing dry with a nitrogen gun, placing the ITO glass on a graphite support in a tube furnace, and placing the centrifugal tube in an oxygen-free glove box.
b) 3.8972g (15mmol) CsI, 1.9045g (5mmol) Cu were weighed in an oxygen-free glove box2I2The mixture was placed in a clean centrifuge tube, 10ml of dimethyl sulfoxide (DMSO) was added, and the tube was shaken until completely dissolved.
c) In an oxygen-free glove box, adding Cs3Cu2I5The DMSO solution is coated on the ITO glass in a spinning way, and is annealed for 10min at 100 ℃ on a hot bench to obtain Cs3Cu2I5Thin film device。
d) In Cs3Cu2I5Two additional free space cavity mirrors are added at two ends of the thin film device to be used as resonant cavities, and a 365nm semiconductor laser is used for pumping to generate stimulated radiation.
Example 10:
the preparation method of the disk laser in the embodiment specifically comprises the following steps:
a) and cleaning the FTO glass with deionized water for 10min, cleaning the FTO glass with acetone for 10min, cleaning the FTO glass with isopropanol for 10min, cleaning the FTO glass with deionized water for 10min, blow-drying with a nitrogen gun, and vertically placing on the edge part of the tube furnace.
b) 0.8512g (4mmol) CsBr, 0.2785g (1mmol) SnBr were weighed2And mixing and placing in a clean quartz crucible.
c) Placing the quartz crucible at the center of the tube furnace, and evacuating to a low vacuum level (<8Pa) is carried out, the tube furnace is quickly heated to 550 ℃ and is kept warm for 60min, and then the temperature is naturally reduced to room temperature to obtain Cs4SnBr6A thin film device.
e) In Cs4SnBr6Two additional free space cavity mirrors are added at two ends of the thin film device to be used as resonant cavities, and 365nm semiconductor lasers are used for pumping to generate laser emission.
Example 11:
the preparation method of the solid laser in the embodiment specifically comprises the following steps:
a) and sequentially cleaning the polytetrafluoroethylene inner container with deionized water for 10min, cleaning the polytetrafluoroethylene inner container with acetone for 10min, cleaning the polytetrafluoroethylene inner container with isopropanol for 10min, cleaning the polytetrafluoroethylene inner container with deionized water for 10min, and blow-drying with a nitrogen gun.
b) 0.3366g (2mmol) CsCl, 0.0351g (0.6mmol) NaCl, 0.0573g (0.4mmol) AgCl, 0.2212g (1mmol) InCl were weighed out3,0.003g(0.01mmol)BiCl3Mixing, placing in a cleaned polytetrafluoroethylene inner container, adding 15ml of hydrochloric acid (the mass percentage concentration of the hydrochloric acid can be 30%), and assembling a hydrothermal kettle.
c) And (3) placing the hydrothermal kettle in a muffle furnace, setting the temperature of the muffle furnace to be 20 ℃, raising the temperature to 180 ℃ after 20min, preserving the temperature for 1000min, and then slowly lowering the temperature to the room temperature after 6000 min.
d) Taking out the hydrothermal kettle in the muffle furnace, pouring out hydrochloric acid in the inner container, taking out the crystal, and ultrasonically cleaning with ethanol for 5min to obtain Cs with larger volume and clean surface2Na0.6Ag0.4InCl6Bi crystal.
e) Selecting Cs with larger volume and better crystal quality2Na0.6Ag0.4InCl6The Bi crystal is polished to allow light to pass through the crystal with less loss.
f) And an antireflection film formed by a dielectric film is evaporated on the surface of the crystal, so that the transmissivity of the crystal is increased.
g) A resonant cavity consisting of high-reflection mirrors is added in free spaces at two ends of the crystal, and a 365nm ultraviolet semiconductor laser is used for pumping to generate laser output.
Example 12:
the preparation method of the solid laser in the embodiment specifically comprises the following steps:
a) and sequentially cleaning the polytetrafluoroethylene inner container with deionized water for 10min, cleaning the polytetrafluoroethylene inner container with acetone for 10min, cleaning the polytetrafluoroethylene inner container with isopropanol for 10min, cleaning the polytetrafluoroethylene inner container with deionized water for 10min, and blow-drying with a nitrogen gun.
b) 0.7794g (3mmol) CsI, 0.3809g (1mmol) Cu were weighed out2I2Mixing and placing in a cleaned polytetrafluoroethylene inner container, adding 15ml hydriodic acid (the mass percentage concentration of the hydriodic acid can be 40 percent) and 1ml hypophosphorous acid, preventing the hydriodic acid from being oxidized, and assembling the kettle.
c) And (3) placing the hydrothermal kettle in a muffle furnace, setting the temperature of the muffle furnace to be 20 ℃, raising the temperature to 120 ℃ for 20min, preserving the temperature for 1000min, and then slowly lowering the temperature to room temperature for 6000 min.
d) Taking out the hydrothermal kettle in the muffle furnace, pouring out hydroiodic acid in the inner container, taking out the crystal, and ultrasonically cleaning with ethanol for 5min to obtain Cs with larger volume and clean surface3Cu2I5And (4) crystals.
e)Selecting Cs with larger volume and better crystal quality3Cu2I5The crystal is polished to allow light to pass through the crystal with less loss.
f) And an antireflection film formed by a dielectric film is evaporated on the surface of the crystal, so that the transmissivity of the crystal is increased.
g) A resonant cavity consisting of high-reflection mirrors is added in free spaces at two ends of the crystal, and a 365nm ultraviolet semiconductor laser is used for pumping to generate laser output.
As can be seen from FIGS. 1, 4 and 5, the material with self-trapped exciton luminescence in the present invention has a large Stokes shift, generally has a broad spectrum with a half-peak width of more than 100nm, can ignore the effect of self-absorption, and has a broad spectral range, almost covering the whole visible light range (400-. It can be seen from fig. 2 and 3 that the thermal stability and radiation stability of these materials are good, and it is ensured that a laser using these materials as a gain medium can stably operate for a long time.
Fig. 10 is a schematic diagram illustrating the light emission of the self-trapping exciton, and it can be seen from the light emission process of the self-trapping exciton illustrated in fig. 10 that the self-trapping exciton is emitted as a four-level system, and population inversion is easily formed, thereby having an advantage as a laser gain medium in nature.
The present invention also experimented with Cs2NaxAg1-xInCl6Other materials of Bi, wherein 0.2 is less than or equal to x is less than or equal to 0.8, for example, materials corresponding to x being 0.2 and x being 0.8, have photoluminescence spectra (PLE) and photoluminescence spectra (PL) which are not greatly different, but have slightly reduced luminescence intensity (the highest luminescence intensity x being 0.4).
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (10)
1. A tunable laser based on self-trapping excitons is characterized in that a gain medium of the laser comprises a material with the self-trapping exciton luminescent property, and the laser output laser wavelength can be tunable within the visible light range of 400nm to 750nm by utilizing the luminescent property of the gain medium, namely large Stokes shift and wide spectral range of the self-trapping excitons and through the mode selection effect of a resonant cavity.
2. The tunable laser based on self-trapped excitons as claimed in claim 1, wherein said gain medium is a perovskite material.
3. The tunable laser based on self-trapped excitons as claimed in claim 1, wherein said gain medium is an all-inorganic perovskite material.
4. The tunable laser based on self-trapped excitons as claimed in claim 3 wherein said gain medium is Cs3Cu2I5Material, Cs4SnBr6Doping the material, or Bi with correspondingly obtained Cs2NaxAg1-xInCl6A Bi material; wherein, the Cs2NaxAg1-xInCl6The Bi material satisfies that x is more than or equal to 0.2 and less than or equal to 0.8.
5. The tunable laser based on self-trapped excitons as claimed in claim 4, wherein said gain medium employs Cs2NaxAg1-xInCl6Bi material, and x is 0.4.
6. The tunable laser based on self-trapped excitons as claimed in claim 1, wherein the laser is a dye laser, fiber laser, disk laser, or solid-state laser.
7. The tunable laser based on self-trapped excitons as claimed in claim 6, wherein when the laser employs a dye laser structure, the gain medium is a solution employing perovskite quantum dots, or a solid-state gel employing perovskite quantum dots.
8. The tunable laser based on self-trapped excitons as claimed in claim 6, wherein, when the laser adopts a laser structure of a fiber laser, the gain medium comprises, in addition to the optical fiber itself, a perovskite material coated on the surface of the optical fiber or a perovskite quantum dot solution externally disposed for soaking the optical fiber; the resonant cavity is composed of a fiber grating or a fiber circulator or a free space cavity mirror.
9. The tunable laser based on self-trapped excitons as claimed in claim 6, wherein when the laser adopts the laser structure of a disk laser, the gain medium is a perovskite film formed by evaporation or spin coating;
preferably, the resonant cavity consists of a free space cavity mirror; or the resonant cavity consists of a distributed Bragg reflection film and a total reflection film which are respectively positioned on the upper surface and the lower surface of the perovskite film, at the moment, the distributed Bragg reflection film and the total reflection film are respectively used as an upper cavity mirror and a lower cavity mirror, wherein the distributed Bragg reflection film is a dielectric film prepared by a vacuum method, the total reflection film is preferably a silver film, and the silver film is also prepared by the vacuum method.
10. The tunable laser based on self-trapped excitons as claimed in claim 6, wherein, when the laser adopts a laser structure of a solid laser, the gain medium is a perovskite crystal with a polished surface, and an antireflection film made of a dielectric film is further evaporated on the surface of the perovskite crystal; the resonant cavity consists of a cavity mirror in free space, and the cavity mirror is a high-reflection mirror with a visible light wave band of 400-750 nm.
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