CN113437641A - Organic laser device and preparation method thereof - Google Patents

Organic laser device and preparation method thereof Download PDF

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CN113437641A
CN113437641A CN202110699243.9A CN202110699243A CN113437641A CN 113437641 A CN113437641 A CN 113437641A CN 202110699243 A CN202110699243 A CN 202110699243A CN 113437641 A CN113437641 A CN 113437641A
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laser device
organic laser
dielectric layer
active layer
organic
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赖文勇
姬东周
刘城芳
谢辉
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Nanjing University of Posts and Telecommunications
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Nanjing University of Posts and Telecommunications
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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
    • H01S5/00—Semiconductor lasers
    • H01S5/30—Structure or shape of the active region; Materials used for the active region
    • H01S5/3004—Structure or shape of the active region; Materials used for the active region employing a field effect structure for inducing charge-carriers, e.g. FET
    • H01S5/3009—MIS or MOS conffigurations
    • 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
    • H01S5/00—Semiconductor lasers
    • H01S5/10—Construction or shape of the optical resonator, e.g. extended or external cavity, coupled cavities, bent-guide, varying width, thickness or composition of the active region
    • H01S5/12—Construction or shape of the optical resonator, e.g. extended or external cavity, coupled cavities, bent-guide, varying width, thickness or composition of the active region the resonator having a periodic structure, e.g. in distributed feedback [DFB] lasers
    • 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
    • H01S5/00—Semiconductor lasers
    • H01S5/30—Structure or shape of the active region; Materials used for the active region
    • H01S5/36—Structure or shape of the active region; Materials used for the active region comprising organic materials

Abstract

The invention relates to an organic laser device and a preparation method thereof. The preparation method of the organic laser device comprises the following steps: (1) preparing a dielectric layer on the grid; (2) preparing an optical resonant cavity and an active layer on the dielectric layer; (3) and preparing a source electrode and a drain electrode on the active layer. The preparation method can conveniently introduce the resonant cavity, is simple and feasible, has low cost, is suitable for constructing the flexible organic laser device, can realize the transmission of field effect carriers and the laser emission at the same time, and has important application prospect in the aspect of electrically pumping the organic laser device.

Description

Organic laser device and preparation method thereof
Technical Field
The invention belongs to the technical field of laser, and particularly relates to an organic laser device and a preparation method thereof.
Background
The laser has high brightness, high directivity, high monochromaticity, high coherence and high energy, and is widely applied. The organic laser has the advantages of flexibility, low threshold value, low cost, adjustable wavelength and the like, and has extremely high application potential in various fields. At present, the research on organic electroluminescence and optically pumped organic laser is becoming mature, but the most attractive electrically pumped organic laser technology still does not make a final breakthrough, and a plurality of difficulties are urgently needed to be solved.
In recent years, organic light emitting field effect transistors (OLETs) have been considered as an effective way to achieve electrically pumped organic lasers with characteristics of high current density, suppression of electrode quenching, and unique device configuration. The configuration and the working mode of a typical OLET device are similar to those of OFET, and research on the OFET device is more beneficial to the design of a novel device, while in a laser, a resonant cavity is indispensable, and a DFB resonant cavity is the most important one in an organic laser.
However, in the current electrically pumped organic laser research, the introduction of DFB structures mainly relies on electron beam lithography, laser interference and nano-thermal imprinting techniques. The technologies generally have the problems of harsh process, high cost, low yield and the like, so that the development of a process capable of simply and effectively integrating a high-quality DFB resonant cavity into an OFET device has very important significance on the research of electrically pumped organic laser.
CN101388523A discloses a novel organic semiconductor solid-state laser and a method for manufacturing the same, the laser is manufactured with a distributed bragg resonator DBR or a distributed feedback resonator DFB on the anode of an organic electroluminescent diode by using a photolithography technique, and by combining photoluminescence and electroluminescence, a low ASE threshold organic thin film on the same device is pumped by using high-intensity OLED EL light, so as to avoid absorption of charges and excitons on light in an organic light emitting layer during OLED period, and exciton splitting generated by strong light, and realize OLED pumped laser, but the method has harsh process and high cost.
Disclosure of Invention
The invention provides an organic laser device and a preparation method thereof, aiming at solving the problems of complex process, high cost, low yield and the like of resonant cavity introduction in the existing electrically pumped organic laser.
In order to achieve the purpose, the invention is realized by the following technical scheme:
the invention relates to an organic laser device, which consists of a substrate, a grid electrode, a dielectric layer, an active layer, a source electrode and a drain electrode.
Preferably, the substrate is transparent glass or an organic polymer, more specifically, the substrate is one or more of glass, polyethylene terephthalate (PET), Polyimide (PI), polyvinyl alcohol (PVA), Polymethylsiloxane (PDMS), and polyurethane acrylate (PUA), and the thickness of the substrate is 2 μm to 1mm, more specifically, the thickness of the substrate is 50 μm to 500 μm.
The source electrode and the drain electrode are both one or more of metal and metal oxide, specifically, the metal is gold, silver, aluminum or copper, the metal oxide is one or more of zinc oxide, manganese dioxide or lead dioxide, the thickness of the source electrode and the thickness of the drain electrode are both 30 nm-300 nm, and more specifically, the thickness of the source electrode and the drain electrode is 50 nm-100 nm.
The grid electrode is a transparent electrode, such as one or more of a metal nanowire, a metal oxide, a conductive polymer and a carbon-based material, wherein the metal nanowire is a silver nanowire or a copper nanowire, the metal oxide is Indium Tin Oxide (ITO) or Indium Zinc Oxide (IZO), the conductive polymer is poly (3, 4-ethylenedioxythiophene)/polystyrene sulfonate (PEDOT: PSS), polythiophene, polypyrrole or polyaniline, and the carbon-based material is graphene or a carbon nanotube.
The thickness of the gate electrode is 100nm to 100 μm, and more specifically, the thickness of the gate electrode is 100m to 500 nm.
The dielectric layer material is a transparent organic dielectric material, the dielectric layer is one or more of Polydimethylsiloxane (PDMS), hydrogenated styrene-butadiene block copolymer, polymethyl methacrylate and transparent fluororesin, and most preferably: polydimethylsiloxane siloxane (PDMS). The thickness of the dielectric layer is 500 nm-3 μm, and more specifically, the thickness of the dielectric layer is 1 μm-2.2 μm.
The dielectric layer has an optical resonant cavity structure, and the optical resonant cavity is a Distributed Feedback (DFB) structure.
The duty cycle of the DFB structure on the dielectric layer is 30% to 70%, preferably 50%.
The trench depth of the DFB structure on the dielectric layer is 30nm to 100nm, preferably 50 nm.
The period range of the DFB structure on the dielectric layer is 200 nm-600 nm, and more preferably, the period of the DFB structure on the dielectric layer is one of 280nm, 320nm and 360 nm.
The active layer is one or more of a small molecular material and a polymer material with field effect transmission performance and laser performance, more specifically, the small molecular material is one or more of alpha, omega-bis (biphenyl-4-yl) -terthiophene (BP3T) or 4,4' -bis [ (N-carbazole) styryl ] biphenyl (BSBCz), the polymer material is one or more of poly (9, 9-dioctylfluorene-co-benzothiadiazole) (F8BT), poly (2-methoxy-5- (2-ethylhexyloxy) -1, 4-phenylacetylene (MEH-PPV), poly (9, 9-di-N-octylfluorene-2, 7-diyl) (PFO) and super yellow light-emitting PPV copolymer (SY), preferably, the active layer, i.e. the organic polymer light emitting semiconductor material, is selected from F8BT or BSBCz.
The thickness of the active layer is 10nm to 150nm, and more specifically, the thickness of the active layer is 50nm to 100 nm.
The invention relates to a preparation method of an organic laser device, which comprises the following steps:
(1) preparing a dielectric layer on the grid;
(2) preparing an optical resonant cavity on the dielectric layer to obtain a dielectric layer/grid electrode/substrate assembly with the optical resonant cavity;
(3) preparing an active layer on the dielectric layer to obtain an active layer/the dielectric layer/the grid/the substrate assembly with the optical resonant cavity;
(4) and preparing a source electrode and a drain electrode on the active layer to obtain the organic laser device.
According to the preparation method, the dielectric layer is prepared on the grid electrode through spin coating or imprinting, the optical resonant cavity on the dielectric layer is prepared through a micro-nano transfer printing method, the active layer is prepared through spin coating, vacuum thermal evaporation, shearing film drawing or ink-jet printing, and the source electrode and the drain electrode are prepared through vacuum thermal evaporation, ink-jet printing or screen printing.
The invention has the beneficial effects that: the invention integrates the DFB structure with the laser resonant cavity function in the OFET device by adopting a simple transfer printing mode, overcomes the problems of harsh process, high cost and low yield of the traditional process, and has the advantages of high precision, low-temperature preparation and flexible material selection. The substrate, the electrode and the dielectric layer are made of transparent materials, so that optical transmission in the device is facilitated; the grating period is flexible and adjustable, and the light pumping laser emission in a wide spectral range can be realized; meanwhile, the regular DFB structure in the dielectric layer can improve the molecular arrangement of the active layer, which is beneficial to improving the mobility of the device.
The invention provides a simple and feasible implementation scheme for the device design of the electrically pumped organic laser, and is particularly suitable for the application of the electrically pumped organic laser taking the OLET as the device configuration in the future.
Drawings
Fig. 1 is a schematic structural diagram of an organic laser device according to the present invention.
Fig. 2 is a laser characteristic diagram of an organic laser device manufactured by a solution method in example 1 of the present invention.
Fig. 3 is a transfer graph of an organic laser device prepared by a solution process in example 1 of the present invention.
Fig. 4 is a graph showing an output curve of an organic laser device manufactured by a solution process in example 1 of the present invention.
FIG. 5 is a graph showing laser characteristics of an organic laser device produced by vapor deposition in example 2 of the present invention.
Wherein: 1-a source electrode; 2-a drain electrode; 3-an active layer; 4-a dielectric layer; 5-a grid; 6-substrate.
Detailed Description
In the following description, for purposes of explanation, numerous implementation details are set forth in order to provide a thorough understanding of the embodiments of the invention. It should be understood, however, that these implementation details are not to be interpreted as limiting the invention. That is, in some embodiments of the invention, such implementation details are not necessary.
The analysis method in the examples of the present invention is as follows:
the electrical performance of the organic laser devices was tested using a Keithley 4200SCS semiconductor parameter analyzer.
Using Nd3+: YAG laser (continuous-laser), Optical Parametric Oscillator (OPO), fiber optic spectrometer (Andor-SR-500I-A) and CCD detector (DU420A-BU) were used to perform laser characterization tests of organic laser devices.
An embodiment of the present invention provides an organic laser device, as shown in fig. 1, including: the substrate, the grid, the dielectric layer, the active layer, the source electrode and the drain electrode, wherein the dielectric layer is provided with an optical resonant cavity and is of a distributed feedback type DFB structure, the duty ratio of the DFB structure is 50%, the depth of a groove is 30 nm-100 nm, and the period range is 200 nm-600 nm.
The preparation method of the organic laser device comprises the following steps:
(1) carrying out ultraviolet ozone treatment on the grid 5, and preparing a dielectric layer 4 on the grid 5;
(2) diluting the dielectric layer material by using a solvent, preparing a dielectric layer film on the silicon-based grating template by using a spin-coating method, and curing;
(3) transferring the dielectric layer film on the silicon-based grating template onto a grid to obtain a dielectric layer/grid/substrate assembly with a DFB structure;
(4) carrying out ultraviolet ozone treatment on the dielectric layer with the DFB structure, and preparing an active layer on the dielectric layer by utilizing spin coating, brush coating, pulling, ink-jet printing or vacuum evaporation;
(5) and preparing a symmetrical or asymmetrical source electrode and a drain electrode on the active layer by utilizing processes such as vacuum evaporation, ink-jet printing, screen printing and the like.
The substrate 6 is one or more of glass, polyethylene terephthalate (PET), Polyimide (PI), polyvinyl alcohol (PVA), Polymethylsiloxane (PDMS) and polyurethane acrylate (PUA), and the thickness of the substrate 6 is 2 mu m-1 mm.
The grid 5 is Indium Tin Oxide (ITO) or Indium Zinc Oxide (IZO), the conductive polymer is poly 3, 4-ethylene dioxythiophene/polystyrene sulfonate (PEDOT: PSS), polythiophene, polypyrrole or polyaniline, the carbon-based material is graphene or carbon nano tubes, silver nano wires or copper nano wires and the like, and the thickness of the grid 5 is 100 nm-100 mu m.
The thickness of the active layer 3 is 10nm to 150nm, and may be one or more of α, ω -bis (biphenyl-4-yl) -terthiophene (BP3T) or 4,4' -bis [ (N-carbazole) styryl ] biphenyl (BSBCz), poly (9, 9-dioctylfluorene-co-benzothiadiazole) (F8BT), poly 2-methoxy-5- (2-ethylhexyloxy) -1, 4-phenylacetylene (MEH-PPV), poly (9, 9-di-N-octylfluorene-2, 7-diyl) (PFO), and super yellow light-emitting PPV copolymer (SY).
The dielectric layer 4 is one or more of Polydimethylsiloxane (PDMS), hydrogenated styrene-butadiene block copolymer, polymethyl methacrylate and transparent fluororesin, and the thickness of the dielectric layer 4 is 500 nm-3 μm.
The thickness of the source electrode 1 and the drain electrode 2 is 30 nm-300 nm, and the source electrode 1 and the drain electrode 2 are gold, silver, aluminum or copper, zinc oxide, manganese dioxide or lead dioxide.
Example 1
Preparing an organic laser device by a solution method:
preparing a PDMS dielectric layer with a period of 320nm on an ITO electrode by a transfer printing method, preparing an active layer by spin coating, and preparing a source electrode and a drain electrode by vacuum evaporation.
(1) The dielectric layer is prepared by the following steps:
a. mixing Polydimethylsiloxane (PDMS) and a curing agent in a solution state at a volume ratio of 10:1, stirring for 30min at room temperature to mix uniformly, then mixing the mixture with cyclohexane at a volume ratio of 1:2, stirring for 2h, and discharging bubbles in the mixed solution in a vacuum environment, wherein the Polydimethylsiloxane (PDMS) in the solution state is Dow Corning SYLGARD 184-A, and the curing agent is Dow Corning SYLGARD 184B.
b. Spin-coating the mixed solution on a silicon-based grating template with the period of 320 nm;
c. c, closely attaching the spin-coated PDMS in the step b to ITO/glass treated by ultraviolet ozone for 15 min;
d. annealing the ITO/glass and the grating template for 5min at the temperature of 150 ℃, and separating after cooling;
e. and carrying out ultraviolet ozone treatment on the PDMS dielectric layer on the ITO/glass for 60 min.
(2) Preparing an active layer:
selecting F8BT as an active layer material, using toluene as a solvent, preparing a solution with the concentration of 20mg/mL, the spin-coating rotation speed of 3000rpm, the spin-coating acceleration of 2000rpm/s, the spin-coating time of 60s, and the thickness of the prepared active layer of 100 nm.
(3) Preparing a source electrode and a drain electrode:
preparing a source electrode and a drain electrode on the active layer by vacuum evaporation, wherein the source electrode and the drain electrode are made of Au and have the pressure of 1 x 10-4Pa or less, and a device channel ratio (W/L) of 2000 μm/100. mu.m.
In the prepared organic laser device, the active layer is F8BT prepared by a solution method and Nd is utilized3+: YAG laser, optical parametric oscillator, fiber spectrometer (Andor-SR-500I-A) and CCD detector (DU420A-BU) were subjected to laser characteristic test, as shown in FIG. 2, with incident light wavelength of 450nm, and transfer characteristic curve diagram of organic laser device prepared by Keithley 4200SCS semiconductor parameter analyzer test is shown in FIG. 3, where source-drain voltage V is shown in FIG. 3D100V; the graph of the output characteristics of the organic laser device prepared by the test is shown in FIG. 4, in which the gate voltage V isG＝0～100V。
Example 2
Preparing an organic laser device by an evaporation method:
(1) the organic laser device is different from the organic laser device in the embodiment 1 in the material and the preparation process of an active layer, wherein the material of the selected active layer is BSBCz, and the preparation process is a vacuum evaporation method; in a vacuum evaporation apparatus
Figure BDA0003129110510000071
Figure BDA0003129110510000072
The BSBCz film is evaporated at a rate of 100nm, and the vacuum degree of thermal evaporation is about 1 multiplied by 10-4Pa, the vapor deposition temperature is 250-300 ℃.
(2) Performance test of the organic laser device:
using Nd3+: YAG laser, optical parametric oscillator, fiber spectrometer (Andor-SR-500I-A) and CCD detector (DU420A-BU)Laser characteristics of the laser device as shown in fig. 5, the wavelength of incident light was 370 nm.
The preparation method of the organic laser device disclosed by the invention can be more conveniently introduced into the resonant cavity, is simple and feasible, has low cost, and is suitable for constructing a flexible organic laser device.
The above description is only an embodiment of the present invention, and is not intended to limit the present invention. Various modifications and alterations to this invention will become apparent to those skilled in the art. Any modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present invention should be included in the scope of the claims of the present invention.

Claims (10)

1. An organic laser device, the organic laser device is provided with an organic field effect transistor structure, and comprises a substrate (6), a grid electrode (5), an active layer (3), a source electrode (1) and a drain electrode (2), the organic field effect transistor structure is a bottom grid top electrode structure, and is characterized in that: a dielectric layer (4) is arranged above the grid electrode (5), the dielectric layer (4) is provided with an optical resonant cavity structure, and the substrate (6), the grid electrode (5) and the active layer (3) are made of transparent materials.
2. An organic laser device according to claim 1, wherein: the optical resonant cavity is of a distributed feedback type structure, the duty ratio of the distributed feedback type structure on the dielectric layer (4) is 30% -70%, the depth of the groove is 30 nm-100 nm, and the period range is 200 nm-600 nm.
3. An organic laser device according to claim 1, wherein: the substrate (6) is one or more of glass, polyethylene terephthalate, polyimide, polyvinyl alcohol, polymethylsiloxane and polyurethane acrylate, and the thickness of the substrate (6) is 2 mu m-1 mm.
4. An organic laser device according to claim 1, wherein: the grid (5) is one or more of a metal nanowire, a metal oxide, a conductive polymer and a carbon-based material, and the thickness of the grid (5) is 100 nm-100 mu m.
5. An organic laser device according to claim 4, wherein: the metal nanowire is a silver nanowire or a copper nanowire, the metal oxide is indium tin oxide or indium zinc oxide, the conductive polymer is poly (3, 4-ethylenedioxythiophene)/polystyrene sulfonate PEDOT, PSS, polythiophene, polypyrrole or polyaniline, and the carbon-based material is graphene or a carbon nanotube.
6. An organic laser device according to claim 1, wherein: the active layer (3) is one or more of a small molecule material and a polymer material with field effect transmission performance and laser performance, and the thickness of the active layer (3) is 10 nm-150 nm.
7. An organic laser device according to claim 6, wherein: the micromolecule material is one or more of alpha, omega-bis (biphenyl-4-yl) -terthiophene or 4,4' -bis [ (N-carbazole) styryl ] biphenyl, and the polymer material is one or more of poly (9, 9-dioctyl fluorene-co-benzothiadiazole), poly (2-methoxy-5- (2-ethylhexyloxy) -1, 4-phenylacetylene, poly (9, 9-di-N-octyl fluorene-2, 7-diyl) and super yellow luminous PPV copolymer.
8. An organic laser device according to claim 1, wherein: the dielectric layer (4) is one or more of polydimethylsiloxane siloxane, hydrogenated styrene-butadiene block copolymer, polymethyl methacrylate and transparent fluororesin, and the thickness of the dielectric layer (4) is 500 nm-3 mu m.
9. A method of manufacturing an organic laser device according to claim 1, characterized by: the preparation method comprises the following steps:
(1) preparing a dielectric layer (4) on the grid (5);
(2) preparing an optical resonant cavity on the dielectric layer (4);
(3) preparing an active layer (3) on the dielectric layer (4);
(4) and preparing a source electrode (1) and a drain electrode (2) on the active layer (3) to obtain the organic laser device.
10. A method for fabricating an organic laser device according to claim 9, wherein: the dielectric layer (4) is prepared on the grid electrode (5) through spin coating or imprinting, the optical resonant cavity on the dielectric layer (4) is prepared through a micro-nano transfer printing method, the active layer (3) is prepared through spin coating, vacuum thermal evaporation, shearing film drawing or ink jet printing, and the source electrode (1) and the drain electrode (2) are prepared through vacuum thermal evaporation, ink jet printing or screen printing.
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US20100140596A1 (en) * 2008-12-08 2010-06-10 Electronics And Telecommunications Research Institute Organic thin film transistor and method of manufacturing the same
CN111682398A (en) * 2020-06-11 2020-09-18 南京邮电大学 Wavelength-tunable organic thin-film laser device based on photoresponse and application thereof
CN111900620A (en) * 2020-07-22 2020-11-06 南京邮电大学 Wavelength-adjustable elastic organic laser and preparation method thereof

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101388523A (en) * 2008-10-30 2009-03-18 上海大学 Novel organic semi-conductor solid laser and preparation thereof
US20100140596A1 (en) * 2008-12-08 2010-06-10 Electronics And Telecommunications Research Institute Organic thin film transistor and method of manufacturing the same
CN111682398A (en) * 2020-06-11 2020-09-18 南京邮电大学 Wavelength-tunable organic thin-film laser device based on photoresponse and application thereof
CN111900620A (en) * 2020-07-22 2020-11-06 南京邮电大学 Wavelength-adjustable elastic organic laser and preparation method thereof

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Application publication date: 20210924