CN107069417B - Plasmon random laser array device based on two-dimensional material - Google Patents
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- H01S3/00—Lasers, i.e. devices using stimulated emission of electromagnetic radiation in the infrared, visible or ultraviolet wave range
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- H—ELECTRICITY
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- 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 discloses a plasmon random laser array device based on a two-dimensional material, which consists of arrayed laser cavity units, wherein the overall structure position relationship of the random laser array device sequentially comprises a pump light source (1), a substrate (2), a bottom electrode (31), a dielectric layer (4), a laser cavity unit (6) surrounded by a spacer layer (5) and a top electrode (32) from bottom to top; two ends of the peripheral driving circuit (7) are respectively connected with the bottom electrode (31) and the top electrode (32), and the bottom electrode (31), the dielectric layer (4), the laser chamber unit (6) and the top electrode (32) form a closed loop. The random laser array uses the two-dimensional material nanosheet with high photoluminescence efficiency as a random gain medium, effectively enhances the scattering of light through the local surface plasmon effect (LSPR) of the metal nanoparticles, and reduces the threshold value of a laser. Dynamic adjustment of radiation spectrum and directivity can be achieved by changing the working voltage of the laser cavity.
Description
Technical Field
The invention belongs to the fields of laser technology, two-dimensional materials, metal nano materials, micro-opto-electro-mechanical technology and the like, and particularly relates to a plasmon random laser array device based on two-dimensional materials.
Background
The random laser is a laser with a novel principle without a resonant cavity, and compared with the traditional laser, the random laser does not need the resonant cavity, laser is formed by multiple scattering effects in a random gain medium contained in the random laser, and the random gain medium can effectively scatter and amplify light. For random lasers, techniques are often required to introduce new sources of nano-light, utilizing various nanostructures to enhance light-to-substance interaction. The scattering characteristic of the random gain medium is further enhanced, so that the threshold value of the random laser is reduced, and the energy consumption and other performances of the random laser are improved. The future development trend of random lasers is arraying, fast tunable laser wavelength and radiation direction and dynamization. However, the prior art is far from meeting the above requirements, such as: TiO 22Thin film random laser and ZnO thin film randomThe laser and the random laser doped with dye particles in the colloidal solution cannot realize dynamic tuning, which greatly limits the application of the random laser in a series of aspects such as photoelectric integration, photonic integration and the like. In order to fully expand the application of random lasers, new technologies need to be introduced to meet the application requirements.
Two-dimensional materials, which have strong planar chemical bonds but weak layer-to-layer coupling, allow the bulk material of the layered structure to be separated into individual atomic layers. The van der waals family of materials is the most common two-dimensional material. The material comprises transition metal sulfides such as graphene, hexagonal boron nitride h-BN, molybdenum disulfide (MoS2) and the like. For molybdenum disulfide, layers are coupled by van der waals force, the upper layer and the lower layer of each layer are hexagonal planes consisting of sulfur atoms and are separated by the middle metal molybdenum atom layer, so that a sandwich is formed. Two-dimensional materials such as molybdenum disulfide have many excellent optical properties, such as: the forbidden band width is related to the layer number of the material; under the irradiation of an external light source, bound excitons are formed between layers, so that a strong photoluminescence effect is generated. Localized Plasmon Resonance (LSPR) is a Resonance enhancement effect caused by the strong interaction between a metal nanostructure and light intensity in a sub-wavelength range, and forms a strong optical field on the Surface of the metal nanostructure. In addition, for a composite structure of two-dimensional materials such as molybdenum disulfide and the like and metal nanoparticles, the doping of the two-dimensional materials can be realized through hot electron-hole pairs generated by the LSPR effect of the metal nanoparticles, and the band gap of the two-dimensional materials can be regulated.
Electrowetting (EW) is a phenomenon in which a droplet is deformed or displaced by changing the wettability of the droplet on a substrate, that is, by changing the contact angle, by changing the voltage between the droplet and an insulating substrate. The electrowetting technology is a method for realizing dynamic tuning of liquid drops on a micrometer scale by utilizing an oil-water two-phase interface effect. The technology has the advantages of high response speed, large adjustable range, adjustable area and radian, low cost and the like. Is a novel dynamic tunable technology and has been widely applied in the aspects of micro-lenses, electrowetting displays, microfluidic laboratories and the like. The invention provides a random laser which combines the technology with the LSPR effect of the plasmon nanoparticles and is used for developing a brand new concept, and has the characteristics of low laser threshold, directivity, dynamic tunable laser spectrum and the like.
Aiming at the bottleneck problems that the threshold value of the conventional random laser is high, the laser wavelength and the radiation direction cannot be tuned, and the like, the invention provides the random laser array with the tunable spectrum from visible light to near-infrared bands by combining the new principle, the new technology and the new material, and has the advantages of low threshold value, simple process and the like. Has important significance for the application of random lasers in the aspects of photon and photoelectric devices.
Disclosure of Invention
The technical problem is as follows: the invention aims to solve the bottleneck problems of high laser threshold, untuneable radiation spectrum and directivity and the like of the conventional random laser. The plasmon random laser array device based on the two-dimensional material is provided, the two-dimensional material with high photoluminescence effect is used as a random gain medium, the laser threshold can be effectively reduced, the laser wavelength and the laser directivity can be dynamically tuned, the preparation process is simple, and the random laser can be prepared into an arrayed random laser.
The technical scheme is as follows: the overall structure position relation of the tunable random laser array device based on the two-dimensional material sequentially comprises a pumping light source, a substrate, a bottom electrode, a dielectric layer, a laser cavity unit and a top electrode, wherein the laser cavity unit is surrounded by a spacing layer; two ends of the peripheral driving circuit are respectively connected with the bottom electrode and the top electrode, and the bottom electrode, the dielectric layer, the laser cavity unit and the top electrode form a closed loop.
The substrate is a flexible substrate formed by a silicon wafer, a sapphire substrate, a mica substrate or a polymer material.
The bottom electrode and the top electrode are transparent conductive film electrodes, and the alternative material is Indium Tin Oxide (ITO), aluminum-doped zinc oxide (AZO) or graphene; the spacer layer is made of hydrophilic polymer materials such as polyethylene glycol, polyacrylamide, polyamide and the like.
The dielectric layer consists of two layers of dielectric media, the lower layer is an inorganic insulating dielectric layer, and the material is selected asSiN、Al2O3Or Si, the upper layer is a polymer dielectric layer with low surface stress, and the optional material is fluorine-containing polymer Cytop or Teflon; the upper dielectric layer is directly spin-coated on the lower dielectric layer, and the thickness ranges from 0.7 micrometer to 0.9 micrometer.
The laser cavity unit comprises a first solvent, a second solvent, a metal nanoparticle film and two-dimensional material nanosheets, wherein the metal nanoparticle film is formed by self-assembling metal nanoparticles at the interface of the first solvent and the second solvent, the two-dimensional material nanosheets are assembled on the surface of the metal nanoparticle film, and the metal nanoparticles can form Schottky contact with the two-dimensional material nanosheets. Thermal electron-hole pairs generated by the localized surface plasmon resonance effect of the metal nanoparticles can be doped into the two-dimensional material nanosheets and the energy bands of the two-dimensional material nanosheets are regulated; the metal nano-particles need to be modified by surface ligands, the two-dimensional material nano-sheets need to be modified by the surface ligands, and the selected materials comprise tetrabutylammonium bromide, hexadecyltrimethylammonium bromide, polyvinylpyrrolidone or sodium carboxymethyl cellulose.
The first solvent is selected from water or polar liquid of saline water, and the surface stress range is 50-90 dynes/cm; the second solvent is selected from alkane, hydrocarbon or alcohol, the surface stress range of the second solvent is 20-40 dynes/cm, and the second solvent is insoluble or slightly soluble in the first solvent.
The metal nano-particle is made of gold, silver, copper or a composite material of the metal, has the shape of a nano-rod, a nano-sphere, a nano-cone or a nano core-shell structure, and has the size ranging from dozens of nanometers to hundreds of nanometers.
The metal nano-particle film is self-assembled at the interface of the first solvent and the second solvent, and the local surface plasmon resonance peak of the metal nano-particle film is from visible light to near infrared band; before self-assembly, the metal nanoparticles need to be subjected to surface modification by a specific surface ligand.
The two-dimensional material nanosheet is subjected to surface ligand treatment and then self-assembled at the interface of the first solvent and the second solvent; the two-dimensional material nanosheet alternative material is graphene, hexagonal boron nitride h-BN, molybdenum disulfide, tungsten disulfide, hafnium disulfide or hafnium diselenide; the size range is dozens of nanometers to dozens of micrometers, the thickness is one layer to dozens of layers, and the forbidden band width is positioned in a visible light to near infrared wave band.
The peripheral driving circuit is used for controlling the working voltage of the laser chamber unit so as to control the hydrophobic angle of the liquid drop formed by the second solvent.
Has the advantages that: compared with the prior art, the invention has the following advantages:
1. the invention provides a tunable random laser array device based on a two-dimensional material, which is prepared by utilizing the relation between LSPR (localized surface plasmon resonance) resonant peaks of metal nanoparticles and the distance of the LSPR resonant peaks, the doping effect of hot electron-hole pairs generated by the LSPR of the metal nanoparticles on two-dimensional material nano sheets, a Schottky contact structure formed by the metal nanoparticles and the two-dimensional material nano sheets, dynamic tuning of liquid drops by electrowetting, a two-phase interface self-assembly effect of the metal nanoparticles and the two-dimensional material nano sheets and other physical mechanisms and mechanisms for the first time. The problem that the existing random laser is as follows can be well solved: ZnO film random lasers, random lasers doped with dye particles in colloidal solutions and the like have the defects of high threshold, narrow radiation spectrum and untuned spectral directivity. And the programmable laser array can be realized through a peripheral driving circuit, the directivities of different laser units are respectively controlled to realize laser synthesis, and a random laser with high power and high beam quality is obtained. The method has important significance for the integration application of the random laser.
2. The invention provides a tunable random laser array device based on a plasmon nano structure, which has the advantage of wide spectrum tuning, a two-dimensional material with high photoluminescence efficiency is selected as a random gain medium, the forbidden bandwidth is mostly about 1.0-2.0 ev, and the peak value of metal nano particles LSPR can be adjusted through two parameters of pumping light source intensity and laser chamber working voltage during specific work, so that the doping effect of hot electrons generated by the metal nano particles on the two-dimensional material is tuned, the spectrum range of radiated random laser is enlarged, and the wavelength range of the radiated random laser is from visible light to near-infrared band.
3. The tunable random laser array device based on the plasmon nanostructure has the advantages of low power consumption and low threshold, and the surface local optical field generated by the LSPR effect of the metal nanoparticle film with the self-assembled two-phase interface can effectively enhance the absorption and scattering efficiency of the two-dimensional material nanosheet to light, so that random laser can be excited when the intensity of an external pumping light source is low, and the tunable random laser array device based on the plasmon nanostructure is low in power consumption and low in threshold.
Drawings
Figure 1 is a cross-sectional view of the entire random laser array,
fig. 2 is a top view of the entire laser array.
Figure 3 is a cross-sectional view of the laser chamber unit at no-voltage or low voltage,
fig. 4 is a top view of the laser chamber unit at high voltage.
The figure shows that: the device comprises a pumping light source 1, a substrate 2, a bottom electrode 31, a top electrode 32, a dielectric layer 4, a spacing layer 5, a laser chamber unit 6, a peripheral driving circuit 7, a first solvent 61, a second solvent 62, metal nanoparticles 63 and two-dimensional material nanosheets 65.
Detailed Description
The invention provides a plasmon random laser array device based on a two-dimensional material. The laser cavity unit is composed of a substrate, a bottom electrode, a dielectric layer, a laser cavity unit surrounded by a spacing layer, a top electrode, a pumping light source and a peripheral driving circuit. The peripheral driving circuit forms a closed loop by connecting the bottom electrode and the top electrode.
The laser cavity unit comprises a first solvent, a second solvent, a metal nanoparticle film and a two-dimensional material nanosheet, wherein the metal nanoparticle film is formed by self-assembling metal nanoparticles at the interface of the first solvent and the second solvent, and the two-dimensional material nanosheet is assembled on the surface of the metal nanoparticle film. The metal nanoparticles need to be surface ligand modified. The surface ligand can effectively reduce the surface activation energy of the metal nano particles, and reduce the repulsive force between the metal nano particles, so that the metal nano particles can be efficiently self-assembled into a film at the interface of the first solvent and the second solvent. The two-dimensional material nano-sheet can be self-assembled on the surfaces of the first solvent and the second solvent as effectively as metal nano-particles after being modified by a surface ligand.
The driving method of the laser chamber unit is as follows: when a pumping light source is used for exciting photoluminescence of two-dimensional material nanosheets and metal nanoparticle local surface plasmon resonance in a laser cavity from the bottom of the laser cavity, low-threshold random laser can be emitted by the unit edge of the laser cavity. For the overall directivity of the laser array, the drive signals can be digitally programmed and the addressing circuit can be controlled by the peripheral drive circuit. Random laser with dynamically tunable directivity is realized.
The random laser array structure and the preparation process are as follows: firstly, preparing an ITO electrode on a Si sheet (or sapphire, mica sheet and the like) through photoetching, etching and other processes, then preparing a dielectric layer above the ITO electrode, preparing an inorganic insulating dielectric layer through PECVD and ALD, and preparing a low-surface-stress polymer dielectric layer through a spin coating process. Then, a hydrophilic laser cavity wall grid layer is prepared by a nano-imprinting technology to form an array cavity structure, and the hydrophilic material is generally polyethylene glycol, polyacrylamide and other hydrophilic polymer materials. Adding the metal nano-particles and the two-dimensional material nano-sheets which are modified by the surface ligands into a first solvent and a second solvent, and then respectively filling the metal nano-particles and the two-dimensional material nano-sheets into a laser cavity unit and sealing. The surface ligand can effectively ensure that the metal nano-particles and the two-dimensional material nano-sheets are self-assembled into a film at the interface of the first solvent and the second solvent.
According to the invention, two-dimensional materials such as molybdenum disulfide are used as random gain media, the two-dimensional materials such as molybdenum disulfide are of interlayer structures similar to graphene, and the two-dimensional materials are coupled by weak van der Waals force. Compared with other photoluminescence random gain media, the multilayer molybdenum disulfide can form strong bound excitons between layers after absorbing photons, and the existence of the bound excitons enables the molybdenum disulfide to have a stronger photoluminescence effect, so that a random laser manufactured by using two-dimensional materials such as molybdenum disulfide has a lower laser threshold.
The metal nanoparticle film assembled at the interface of two mutually insoluble solvents can further reduce the threshold value of the random laser and effectively tune the wavelength of the radiated laser. Firstly, the metal nanoparticles can generate a Localized Surface Plasmon effect (LSPR) under the irradiation of a pump light source, so that light can be Localized in a range of depth sub-wavelength, and a strong Localized light field is formed near a Resonance peak, and the photoluminescence efficiency of the two-dimensional material nanosheet can be more effectively enhanced by the Localized light field, so that the threshold value of a laser is further reduced. According to the invention, the metal nano-particles and the two-dimensional material nano-sheets are jointly self-assembled at the two-phase interface, so that the distance between the metal nano-particles and the two-dimensional material nano-sheets is very small, when the metal nano-particles are irradiated by light to generate an LSPR effect, the absorption of light can be greatly enhanced, and hot electron-hole pairs can be generated after sufficient photon energy is absorbed. The generated hot electrons can play a role in doping the two-dimensional material nanosheets to realize regulation and control of light absorption and photoluminescence spectrums of the two-dimensional material. When the laser array works specifically, by changing the working voltage of the laser cavity, the contraction and relaxation of liquid drops formed by the second solvent can be realized due to the electrowetting effect, so that the inter-particle distance of the metal nano-particle film is changed. The change of the particle spacing can change the LSPR peak of the metal nanoparticle film, so that the doping of the two-dimensional nano material by hot electrons generated by the metal nanoparticles is regulated and controlled, the change of a photoluminescence spectrum is realized, and the adjustment of the random laser radiation spectrum of the invention is realized.
Example (c):
1. as shown in fig. 1, an M × N laser array structure is prepared, a transparent electrode is prepared on a substrate through photolithography, etching and other processes, a dielectric layer is prepared on the transparent electrode through ALD, and a low surface stress polymer dielectric layer is prepared through a spin coating process. Then, an M × N grid layer is prepared by a nanoimprint technology to form an array cavity structure, and the hydrophilic material is generally polyethylene glycol, polyacrylamide and other hydrophilic polymer materials. After the overall structure of the device is prepared, metal nanoparticles and two-dimensional material nanosheets are added into a first solvent or a second solvent, and then the first solvent and the second solvent are filled into a laser chamber and sealed through photoresist.
2. The prepared random laser array is connected to a peripheral driving circuit through a bottom electrode and a top connecting electrode, and a laser cavity unit is controlled through a digital signal of the driving circuit.
3. And a pumping light source is turned on to irradiate the laser cavity from the bottom to emit laser, the radiation spectrum and the directivity of the whole laser array can be controlled by the digital signal of the peripheral circuit, and the digital signal is used for controlling the unit working voltage of the laser cavity. The radiation spectrum is red-shifted when the operating voltage is changed from a low voltage to a high voltage.
Claims (9)
1. The utility model provides a plasmon random laser array device based on two-dimensional material which characterized in that: the overall structure position relation of the random laser array device sequentially comprises a pumping light source (1), a substrate (2), a bottom electrode (31), a dielectric layer (4), a laser chamber unit (6) surrounded by a spacing layer (5) and a top electrode (32) from bottom to top; two ends of the peripheral driving circuit (7) are respectively connected with the bottom electrode (31) and the top electrode (32), and the bottom electrode (31), the dielectric layer (4), the laser chamber unit (6) and the top electrode (32) form a closed loop;
the laser cavity unit (6) is composed of a first solvent (61), a second solvent (62), a metal nanoparticle thin film and two-dimensional material nano sheets (65), wherein the metal nanoparticle thin film is formed by self-assembling metal nanoparticles (63) at the interface of the first solvent (61) and the second solvent (62), the two-dimensional material nano sheets (65) are assembled on the surface of the metal nanoparticle thin film, and the metal nanoparticles (63) can form Schottky contact with the two-dimensional material nano sheets (65); thermal electron-hole pairs generated by the local surface plasmon resonance effect of the metal nanoparticles (63) can be doped into the two-dimensional material nanosheets (65) and the energy band of the two-dimensional material nanosheets can be regulated; the metal nanoparticles (63) need to be modified by a first surface ligand, and the two-dimensional material nanosheets (65) need to be modified by a second surface ligand, wherein the material is selected from tetrabutylammonium bromide, hexadecyltrimethylammonium bromide, polyvinylpyrrolidone or sodium carboxymethylcellulose.
2. The two-dimensional material based plasmonic random laser array device of claim 1, wherein: the substrate (2) is a flexible substrate formed by a silicon wafer, a sapphire substrate, a mica substrate or a polymer material.
3. The two-dimensional material based plasmonic random laser array device of claim 1, wherein: the bottom electrode (31) and the top electrode (32) are transparent conductive film electrodes, and the alternative materials are Indium Tin Oxide (ITO), aluminum-doped zinc oxide (AZO) or graphene; the spacer layer (5) is selected from polyethylene glycol, polyacrylamide and polyamide hydrophilic polymer materials.
4. The two-dimensional material based plasmonic random laser array device of claim 1, wherein: the dielectric layer (4) consists of two layers of dielectric media, the lower layer is an inorganic insulating dielectric layer, and the alternative material is SiN and Al2O3Or Si, the upper layer is a polymer dielectric layer with low surface stress, and the optional material is fluorine-containing polymer Cytop or Teflon; the upper dielectric layer is directly spin-coated on the lower dielectric layer, and the thickness ranges from 0.7 micrometer to 0.9 micrometer.
5. The two-dimensional material based plasmonic random laser array device of claim 1, wherein: the first solvent (61) is selected from water or saline polar liquid, and the surface stress range is 50-90 dynes/cm; the second solvent (62) is selected from alkane, hydrocarbon or alcohol, the surface stress range of the second solvent is 20-40 dynes/cm, and the second solvent (62) is insoluble or slightly soluble in the first solvent (61).
6. The two-dimensional material based plasmonic random laser array device of claim 1, wherein: the optional material of the metal nano-particles (63) is gold, silver and copper or a material obtained by compounding gold, silver and copper in pairs, the shape of the metal nano-particles is a nano-rod, a nano-sphere, a nano-cone or a nano core-shell structure, and the size range of the metal nano-particles is dozens of nanometers to hundreds of nanometers.
7. The two-dimensional material based plasmonic random laser array device of claim 1, wherein: the metal nanoparticle film is self-assembled at the interface of a first solvent (61) and a second solvent (62), and the local surface plasmon resonance peak of the metal nanoparticle film is from visible light to near infrared band; before self-assembly, the metal nanoparticles (63) need to be subjected to surface modification by specific first surface ligands.
8. The two-dimensional material based plasmonic random laser array device of claim 1, wherein: the two-dimensional material nanosheet (65) is self-assembled at the interface of the first solvent (61) and the second solvent (62) after being modified by the second surface ligand; the two-dimensional material nanosheet (65) is made of graphene, hexagonal boron nitride h-BN, molybdenum disulfide, tungsten disulfide, hafnium disulfide or hafnium diselenide; the size range is dozens of nanometers to dozens of micrometers, the thickness is one layer to dozens of layers, and the forbidden band width is positioned in a visible light to near infrared wave band.
9. The two-dimensional material based plasmonic random laser array device of claim 1, wherein: the peripheral driving circuit (7) is used for controlling the working voltage of the laser chamber unit and further controlling the hydrophobic angle of liquid drops formed by the second solvent (62).
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| CN111600187B (en) * | 2020-05-03 | 2021-03-02 | 北京师范大学 | Film random laser based on environment humidity tuning wavelength |
| CN114252094A (en) * | 2021-11-30 | 2022-03-29 | 电子科技大学 | Fano resonance enhancement-based photoelectric detection structure and preparation method thereof |
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