CN108512029B - Ultra-wideband random laser scattering material based on amorphous bismuthate, laser device, preparation and application - Google Patents
Ultra-wideband random laser scattering material based on amorphous bismuthate, laser device, preparation and application Download PDFInfo
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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
- H01S3/30—Lasers, i.e. devices using stimulated emission of electromagnetic radiation in the infrared, visible or ultraviolet wave range using scattering effects, e.g. stimulated Brillouin or Raman effects
- H01S3/307—Lasers, i.e. devices using stimulated emission of electromagnetic radiation in the infrared, visible or ultraviolet wave range using scattering effects, e.g. stimulated Brillouin or Raman effects in a liquid
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Abstract
The invention relates to an ultra-wideband random laser scattering material based on amorphous bismuthate, a laser device, a preparation method and an application thereof, wherein the scattering material comprises the following chemical components in mole percentage: bi2O3:45‑65%,B2O3:20‑35%,Ga2O3: 0 to 20 percent. The preparation method comprises the steps of mixing required raw materials, melting at high temperature, annealing at the temperature close to the glass transition temperature after compression molding of high-temperature melt, then ball-milling the bulk materials into powder, wherein the prepared powder material is used for constructing various structures which can provide random laser resonance optical feedback, such as suspension, solid tabletting, substrate spin coating and the like, and ultra-wideband random laser is observed in the wide spectrum range of 530-870nm by changing the types of gain media and exciting with laser with different wavelengths. The invention has simple manufacturing method and flexible form, and can be well used in the fields of optical communication, digital storage, energy conversion and the like.
Description
Technical Field
The invention relates to the technical field of laser devices, in particular to an adjustable ultra-wideband random laser scattering material, a laser device, preparation and application.
Background
In recent years, the study of random lasers has become a popular problem in the field of micro-nano lasers. Random laser has many obvious differences from the traditional laser in the generation mechanism and the light-emitting characteristic, the random laser radiation is from a disordered medium with optical activity, optical feedback is provided through multiple scattering of the radiation light in the medium, and therefore, larger gain is obtained, and laser resonance can be realized without an additional resonant cavity. The random laser has the characteristic of omnibearing emission, and when the observation angle is different, the spectral line structure and the emission intensity can also change, and the light-emitting characteristic can fluctuate randomly in time, space and spectrum. Compared with the traditional laser, the random laser has the obvious advantages of simple preparation process, low cost and unique emission characteristic.
In 1966, Basov et al (prog. quant. Electron.1970,1: 107-. In 1968, the light amplification behavior in random gain media was theoretically calculated for the first time by Letokhov [ J.Exp.Theor.Phys.1968,26:835-840 ]. The random laser has a unique physical mechanism, has great research significance in the basic research of micro-nano photonics, and has wide application prospects in the fields of photonic integration, nano optoelectronic devices, optical sensing, special waveband laser generation, laser anti-counterfeiting, medical imaging and the like.
However, the highly controllable random lasers reported to date have been mainly produced by using crystalline scattering centers (e.g., ZnO, ZrO)2And TiO 22) For example, 1994, professor Lawandy university of Brownian Nature 1994,368:436-]The first experiment reports that the dye solution containing the titanium dioxide nano-scattering particles can realize stimulated radiation amplification. In 1999, professor Hu Cao university of northwest USA [ Phys. Rev. Lett.1999,82:2278-]And the coherent random laser output is realized by the nano zinc oxide particles. However, the crystalline scattering centers described above are usually obtained by chemical routes, with the significant disadvantages of being complex to prepare, costly, low in yield and difficult to achieve large scale integration.
Chinese patent document CN105762634A discloses a flexible thin film random laser with adjustable polarization degree and a preparation method thereof. The random laser is of a film-shaped structure and consists of polyvinyl alcohol, polyalcohol and dye nematic liquid crystal microdroplets, wherein the polyalcohol and the dye nematic liquid crystal microdroplets are positioned in a film formed by the polyvinyl alcohol. Based on the optical anisotropy of nematic liquid crystal, the orientation of nematic liquid crystal molecules in a polyvinyl alcohol film is changed by mechanically stretching the polyvinyl alcohol film containing dye nematic liquid crystal microdroplets under the condition of laser pumping, so that random laser emission with adjustable polarization degree is realized, and the polarization direction of the random laser is parallel to the stretching direction.
However, the random laser structure is limited to a thin film structure, and the liquid crystal material is used as a scattering body, so that the random laser structure has the obvious defects of high cost and difficulty in realizing ultra-wideband.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides an ultra-wideband random laser scattering material based on amorphous bismuthate, a laser device, a preparation method and an application.
The technical scheme of the invention is as follows:
an ultra-wideband random laser scattering material, which comprises the following chemical compositions in mole percentage: bi2O3:45-65%,B2O3:20-35%,Ga2O3:0-20%。
According to the present invention, it is preferred that the scattering material comprises a chemical composition in mole percent: bi2O3:50-65%,B2O3:20-30%,Ga2O3:10-20%。
According to the present invention, it is preferred that the scattering material comprises a chemical composition in mole percent: bi2O3:65%,B2O3:20%,Ga2O3:15%。
According to the invention, the preparation method of the ultra-wideband random laser scattering material comprises the following steps:
weighing the components according to the mol percentage, uniformly mixing, melting, pressing and forming a melt, annealing, and then ball-milling the obtained material, wherein the powder after ball-milling is the scattering material.
According to the present invention, the average particle diameter of the powder after ball milling is preferably 4 to 5 μm.
According to the preparation method of the scattering material, the melting temperature is 1050-;
preferably, the annealing temperature is 350-360 ℃, and the annealing time is 1-3 h. Annealing is performed around the glass transition temperature.
According to the invention, the ultra-wideband random laser device comprises a complex body and a carrier, wherein the complex body is composed of the scattering material and a gain medium, and the complex body is loaded in the carrier; or a composite body composed of the scattering material and the gain medium is made into a sheet form to be used as a laser device.
According to the laser device of the present invention, preferably, the gain medium is a laser dye, a rare earth ion or/and a semiconductor quantum dot;
preferably, the mass ratio of the scattering material to the gain medium is 10000-5000: 1.
according to the laser device of the present invention, the composite body may take various forms including a suspension, a solid preform, a waveguide structure, and the like;
preferably, when the complex is a suspension, the scattering material is dispersed in water, and the gain medium is added to disperse uniformly to obtain the suspension;
when the complex is a solid tablet, pressing the scattering material into a sheet at high pressure, and uniformly coating the surface of the sheet with the gain medium solution to obtain the complex in the form of the solid tablet; the gain medium solution permeates into the pores of the solid tablet;
when the complex is in a waveguide structure, dispersing the dispersion material in water to obtain a suspension, uniformly coating the suspension on the surface of the carrier, and uniformly coating the gain medium solution on the surface to obtain a film, namely the complex in the form of the waveguide structure.
According to the present invention, the carrier may take various forms, and preferably, a transparent tetragonal container, preferably a cuvette, a glass plate, etc. may be used. When the complex is a suspension, the suspension can be filled into a transparent square container to obtain the laser device. When the composite body is a solid tabletting or waveguide structure, the composite body is directly used as a laser device.
According to the invention, the scattering material (amorphous bismuthate material powder) is used as a strong scattering center, the gain curve can be adjusted by changing the type of the gain medium, and random laser is generated in the wide wavelength range of 530-870 nm.
According to the invention, the application of the amorphous bismuthate-based ultra-wideband random laser device is applied to the fields of optical communication, digital storage and energy conversion as a random laser device.
The invention provides a random laser device with various geometric structures, which is formed by an amorphous bismuthate material which is easy to prepare and high in yield and benefit, a random laser device with various geometric structures is formed by the amorphous bismuthate material with the refractive index of 2.378-2.118 in the spectral range of 400-1500nm, and an optical gain curve is adjusted by changing the type of a gain medium, so that effective laser resonance and a pumping threshold value are observed in the wide spectral range from visible light to near infrared. The laser is equivalent to the random laser based on crystalline strong scattering centers reported in the past. The results show that the amorphous medium can be used as a reliable platform for promoting the interaction of light and substances, constructing and amplifying random media and manufacturing high-efficiency luminescent devices.
The principle of the invention is as follows:
the invention replaces the traditional crystalline strong scattering center with amorphous material, provides optical feedback through multiple light scattering to emit coherent photons, thereby realizing high-efficiency random laser resonance, and forms laser in the ultra-wideband range of 530-870nm by adding different gain media.
The invention has the following functions: bi2O3And B2O3Ga, being network formers2O3For network decorations, B3+And Ga3+All are heavy metal ions, have higher ionic polarizability and endow the glass with higher refractive index. Laser dye, rare earth ions, semiconductor quantum dots, etc. are used as gain media, so that random laser light is observed in the wavelength range of 530-870 nm.
The invention has the beneficial effects that:
the invention selects amorphous bismuthate material as scattering medium, and realizes 530-870nm ultra-wideband random laser by using a single scattering element; the manufacturing method is simple, the form is flexible, and the laser can be made into suspension, solid tabletting and waveguide random laser devices; the method can be used in the fields of optical communication, digital storage, energy conversion and the like.
Drawings
FIG. 1: the structure of the ultra-wideband random laser device of example 1 is schematically shown.
FIG. 2: the samples obtained in example 1 were excited at different pump energies to produce normalized emission spectra.
FIG. 3: the structure of the ultra-wideband random laser device of example 2 is schematically shown.
FIG. 4: the samples obtained in example 2 were excited at different pump energies to produce normalized emission spectra.
FIG. 5: the structure of the ultra-wideband random laser device of example 3 is shown schematically.
FIG. 6: the samples obtained in example 3 were excited at different pump energies to produce normalized emission spectra.
Detailed Description
The present invention will be further described with reference to the following drawings and detailed description, but is not limited thereto.
Example 1
The chemical composition of the amorphous bismuthate material of this example was Bi2O3:65mol%;B2O3:20mol%;Ga2O3: 15mol percent. Glass raw material selects analytically pure Bi2O3、B2O3、Ga2O3. The preparation method comprises the steps of proportioning according to the mol percentage, grinding and uniformly mixing, placing the mixture in an alumina crucible, melting the mixture at a certain temperature, pouring a melt on a stainless steel plate, performing compression molding, annealing the melt for 2 hours at the temperature close to the glass transition temperature, then performing ball milling on a blocky material, taking the ball-milled powder as a strong scatterer, and dispersing the powder in water to form 15mg/mL suspension. And (3) taking more than 1mL of suspension, adding 0.1mL of 10mM rhodamine 101-ethanol solution, performing ultrasonic dispersion for 1 minute to obtain a suspension, and filling the suspension into a transparent cuvette to obtain the amorphous bismuthate-based ultra-wideband random laser device. The structure schematic diagram is shown in figure 1.
By deenergizing the prepared sample using a pulsed laser (wavelength: 532nm, pulse width: 25ps, repetition rate: 1Hz), broad spontaneous amplified radiation was observed, with the laser spike appearing at 610nm as the energy increased. The normalized emission spectra resulting from excitation at different pump energies are shown in fig. 2.
Example 2
The chemical composition of the amorphous bismuthate material of this example was Bi2O3:65mol%;B2O3:20mol%;Ga2O3: 15mol percent. Glass raw material selects analytically pure Bi2O3、B2O3、Ga2O3. The method comprises the steps of proportioning according to the mol percentage, grinding and mixing uniformly, placing the mixture in an alumina crucible, melting the mixture at a certain temperature, pouring a glass melt on a stainless steel plate, performing compression molding, annealing the glass melt for 2 hours at the temperature close to the glass transition temperature, performing ball milling on a block material, taking the ball-milled powder as a strong scatterer, and pressing the powder into a sheet (the pressure is 10MPa) through a tablet press. 10mL of 0.12g/mL polyvinyl alcohol-waterThe solution was mixed with 1mL of 10mM rhodamine 6G-ethanol solution. And (3) sucking 30 mu l of mixed solution by using a liquid transfer gun, dripping the mixed solution on the sheet to enable the mixed solution to penetrate into gaps of the solid tabletting, and drying in an oven for half an hour to obtain the amorphous bismuthate-based ultra-wideband random laser device. The structure schematic diagram is shown in fig. 3.
Broad spontaneous amplified radiation was observed by deenergizing the prepared sample using a pulsed laser (wavelength: 480nm, pulse width: 25ps, repetition rate: 1Hz), with the laser spike appearing at 575nm with increasing energy. The normalized emission spectra resulting from excitation at different pump energies are shown in fig. 4.
Example 3
The chemical composition of the amorphous bismuthate material of this example was Bi2O3:65mol%;B2O3:20mol%;Ga2O3: 15mol percent. Glass raw material selects analytically pure Bi2O3、B2O3、Ga2O3. Mixing the materials according to the mol percentage, placing the mixture in an alumina crucible, melting the mixture at a certain temperature, pouring a glass melt on a stainless steel plate, performing compression molding, annealing the glass melt at the temperature close to the glass transition temperature for 2 hours, then performing ball milling on the block materials, and taking the ball-milled powder as a strong scatterer. The powder was dispersed in water to form a 15mg/mL suspension, and 0.2mL was spin-coated on a glass substrate (spin speed: 6000rpm, spin time: 30 s). Uniformly mixing 1mL of 0.3g/mL polyvinyl alcohol aqueous solution and 0.25mL of 10mM rhodamine 800 ethanol solution, uniformly dripping 0.2mL of the mixture on the sample, spin-coating to obtain a polyvinyl alcohol film containing rhodamine 800 (spin-coating speed: 6000rpm and spin-coating time: 60s), and drying for half an hour to obtain the amorphous bismuthate-based ultra-wideband random laser device. The schematic structure is shown in fig. 5.
By deenergizing the prepared sample using a pulsed laser (wavelength: 680nm, pulse width: 25ps, repetition rate: 1Hz), broad spontaneous amplified radiation was observed, with the laser spike appearing at 710nm as the energy increased. The normalized emission spectra resulting from excitation at different pump energies are shown in fig. 6.
Comparative example 1
As described in example 1, except that:
the chemical composition of the amorphous bismuthate material is Bi2O3:40mol%;B2O3:40mol%;Ga2O3:20mol%。
The prepared sample was deenergized using a pulsed laser (wavelength: 680nm, pulse width: 25ps, repetition rate: 1Hz), resulting in a decrease in the refractive index of the sample due to a decrease in the bismuth oxide content, and thus a decrease in the scattering ability, an increase in the pumping threshold, and a decrease in the output efficiency.
Claims (9)
1. An ultra-wideband random laser device is characterized by comprising a carrier and a complex body composed of a scattering material and a gain medium, wherein the complex body is loaded in the carrier; or a composite body consisting of the scattering material and the gain medium is made into a sheet form to be used as a laser device;
the scattering material is an amorphous bismuthate material and comprises the following chemical compositions in mole percentage: bi2O3:45-65%,B2O3:20-35%,Ga2O3:0-20%;
The gain medium is laser dye, rare earth ions or/and semiconductor quantum dots;
the mass ratio of the scattering material to the gain medium is 10000-5000: 1.
2. the ultra-wideband random laser device of claim 1, wherein said composite body is in the form of a suspension, a solid preform, or a waveguide structure;
when the complex is a suspension, dispersing the scattering material in water, adding the gain medium, and uniformly dispersing to obtain a suspension;
when the complex is a solid tablet, pressing the scattering material into a sheet at high pressure, and uniformly coating the surface of the sheet with the gain medium solution to obtain the complex in the form of the solid tablet; the gain medium solution permeates into the pores of the solid tablet;
when the complex is in a waveguide structure, dispersing the dispersion material in water to obtain a suspension, uniformly coating the suspension on the surface of the carrier, and uniformly coating the gain medium solution on the surface to obtain a film, namely the complex in the form of the waveguide structure.
3. The ultra-wideband random laser device of claim 1, wherein the scattering material comprises a chemical composition in mole percent: bi2O3:50-65%,B2O3:20-30%,Ga2O3:10-20%。
4. The ultra-wideband random laser device of claim 1, wherein said scattering material comprises a chemical composition in mole percent: bi2O3: 65%,B2O3:20%,Ga2O3:15%。
5. The ultra-wideband random laser device of claim 1, wherein the scattering material is prepared by the steps of:
weighing the components according to the mol percentage, uniformly mixing, melting, pressing and forming a melt, annealing, and then ball-milling the obtained material, wherein the powder after ball-milling is the scattering material.
6. The ultra-wideband random laser device of claim 5, wherein the average particle size of the powder after ball milling is 4-5 μm.
7. The UWB random laser device of claim 5 wherein the melting temperature is 1050-.
8. The UWB random laser device of claim 5 wherein the annealing temperature is 350-360 ℃, and the annealing time is 1-3 h.
9. Use of the ultra-wideband random laser device of claim 1 as a random laser device in the fields of optical communication, digital storage and energy conversion.
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