CN111262133A - Method for improving single-layer two-dimensional semiconductor light-emitting brightness - Google Patents

Method for improving single-layer two-dimensional semiconductor light-emitting brightness Download PDF

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CN111262133A
CN111262133A CN202010056849.6A CN202010056849A CN111262133A CN 111262133 A CN111262133 A CN 111262133A CN 202010056849 A CN202010056849 A CN 202010056849A CN 111262133 A CN111262133 A CN 111262133A
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dimensional semiconductor
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semiconductor
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CN111262133B (en
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吴汉春
吕燕会
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Beijing Institute of Technology BIT
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    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01SDEVICES 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
    • H01S5/00Semiconductor lasers
    • H01S5/30Structure or shape of the active region; Materials used for the active region
    • H01S5/32Structure or shape of the active region; Materials used for the active region comprising PN junctions, e.g. hetero- or double- heterostructures
    • H01S5/327Structure or shape of the active region; Materials used for the active region comprising PN junctions, e.g. hetero- or double- heterostructures in AIIBVI compounds, e.g. ZnCdSe-laser
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01SDEVICES 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
    • H01S5/00Semiconductor lasers
    • H01S5/04Processes or apparatus for excitation, e.g. pumping, e.g. by electron beams
    • H01S5/041Optical pumping
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01SDEVICES 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
    • H01S5/00Semiconductor lasers
    • H01S5/30Structure or shape of the active region; Materials used for the active region
    • H01S5/34Structure or shape of the active region; Materials used for the active region comprising quantum well or superlattice structures, e.g. single quantum well [SQW] lasers, multiple quantum well [MQW] lasers or graded index separate confinement heterostructure [GRINSCH] lasers
    • H01S5/347Structure or shape of the active region; Materials used for the active region comprising quantum well or superlattice structures, e.g. single quantum well [SQW] lasers, multiple quantum well [MQW] lasers or graded index separate confinement heterostructure [GRINSCH] lasers in AIIBVI compounds, e.g. ZnCdSe- laser

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  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
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Abstract

The invention relates to a method for improving the brightness of a single-layer two-dimensional semiconductor, belonging to the technical field of quantum optics and photon quantum information. The invention integrates a single-layer two-dimensional semiconductor and a three-dimensional semiconductor with a raised structure on the surface to form a composite heterostructure, thereby generating a greatly enhanced coupling system and greatly improving the luminous brightness of the single-layer two-dimensional semiconductor. The simple and efficient silicon-based composite heterostructure is fully extensible, is expected to be used as a quantum light source with high brightness, long-term stability and chip integration, and belongs to the technical field of quantum optics and photon quantum information.

Description

Method for improving single-layer two-dimensional semiconductor light-emitting brightness
Technical Field
The invention relates to a method for improving the brightness of a single-layer two-dimensional semiconductor, and belongs to the technical field of quantum optics and photon quantum information.
Background
Single Quantum Emitters (SQEs) are the core of quantum optics and photonic quantum information technology, SQEs being essential for many applications of quantum information processing. Single layer transition metal chalcogenides (TMDCs) have large exciton binding energies and long lifetimes of excitons in the layer at room temperature, which makes them particularly suitable for single quantum emitter applications. Core requirements for such non-classical light sources include long-term stability, high brightness, and on-chip integratability.
However, achieving high photoluminescence quantum yields remains challenging in single-layer two-dimensional materials. For example, a single layer WSe that will mechanically peel away2The photoluminescence enhancement of 8 times is realized only by integrating the silicon-based photonic structure; the luminescence of the single-layer two-dimensional material is enhanced by elastic strain engineering, and is enhanced by several times. The grown monolayer generally exhibits a lower photoluminescence quantum yield than its mechanically exfoliated monolayer, the WSe to be grown2A single layer of material was coupled to the circular bragg grating structure and exciton emission was observed to be enhanced by a factor of 7; recently reported WSe grown by solvent evaporation2The mechanical relaxation of the monomolecular film is decoupled from the substrate, and the photoluminescence emission enhancement is only an order of magnitude compared with the monomolecular film grown by coupling the substrate. Although many solutions have been proposed to enhance quantum emission of single-layer two-dimensional semiconductors, the realization of more efficient photon extraction efficiency, high integration and scalability still requires the opening up of new approaches. With a simple and efficient composite heterostructure of the present application, a greatly enhanced coupling system can be created, resulting in a greatly enhanced luminous efficiency of a single-layer two-dimensional semiconductor, such as WSe, which we have grown by Chemical Vapor Deposition (CVD) in the laboratory2The luminescence of a single layer of material is improved by two orders of magnitude.
The composite system formed by the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with the surface provided with the convex structure improves the luminous intensity, mainly utilizes the special structure of the three-dimensional semiconductor to have larger carrier concentration at a specific position, and is coupled with the single-layer two-dimensional semiconductor at a contact position to generate interlayer exciton transition to inject extra excitons into the single-layer two-dimensional semiconductor, meanwhile, the single-layer two-dimensional semiconductor is subjected to local strain to generate continuous band gap change to generate exciton funnel effect, and the two effects finally greatly improve the luminous intensity of the single-layer two-dimensional semiconductor.
Disclosure of Invention
The invention aims to solve the problems of low photon extraction efficiency and limited integration and expansibility in the prior art, and provides a method for improving the single-layer two-dimensional semiconductor luminous brightness. The method provides a simple and efficient composite heterostructure, improves the luminous brightness of the single-layer two-dimensional semiconductor, and realizes the expandability of the manufacturing process and the integratability on a chip.
The purpose of the invention is realized by the following technical scheme.
A method for improving the luminous brightness of a single-layer two-dimensional semiconductor integrates the single-layer two-dimensional semiconductor into a three-dimensional semiconductor with a convex structure on the surface: the single-layer two-dimensional semiconductor is coupled with the three-dimensional semiconductor to generate an exciton funnel effect and an exciton injection effect, so that the aim of improving the light emission of the single-layer two-dimensional semiconductor is fulfilled.
The specific physical principle is as follows: the three-dimensional semiconductor with the surface provided with the convex structure enables the single-layer two-dimensional semiconductor to generate local strain, and the energy band structure of the single-layer two-dimensional semiconductor is changed to form an exciton funnel effect; interlayer exciton transition exists at the contact position of the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with a convex structure on the surface, and extra excitons can be injected into the single-layer two-dimensional semiconductor; the exciton injection efficiency depends on the gate voltage and can therefore be further adjusted with the gate voltage. The composite heterostructure composed of the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with the surface provided with the convex structure is utilized, the exciton funnel effect formed and the interlayer exciton transition jointly generate influence, and the purpose of improving the luminous brightness of the single-layer two-dimensional semiconductor is achieved.
The quantum light source with high brightness, long-term stability and chip integratability prepared by the method comprises the following steps: the laser diode comprises a single-layer two-dimensional semiconductor, a three-dimensional semiconductor with a raised structure on the surface, a dielectric layer, a conductive electrode, a lead and a laser light source; the single-layer two-dimensional semiconductor is placed on a three-dimensional semiconductor with a raised structure on the surface to form a composite heterostructure, a laser light source is used for irradiating the single-layer two-dimensional semiconductor, a dielectric layer is covered on the single-layer two-dimensional semiconductor, and a conducting wire and a conducting electrode are connected on the dielectric layer and the three-dimensional semiconductor with the raised structure on the surface, so that the composite heterostructure can be conveniently accessed into an electronic system and can be regulated and controlled by applying grid voltage.
The single-layer two-dimensional semiconductor is oneMaterials dimensionally in the nanoscale range. For example, but not limited to, these, including single layer WSe2、WS2、GaSe、MoSe2、MoS2、MoTe2、SnSe2GeSe, graphene, and the like.
The three-dimensional semiconductor with the convex structure on the surface is a substrate for coupling a single-layer two-dimensional semiconductor, and can be any silicon-based three-dimensional semiconductor with deformation or local deformation, such as a corrugated structure, and the wavelength, amplitude, lateral etching depth and doping concentration of the three-dimensional semiconductor are adjustable parameters. The raised structure of the three-dimensional semiconductor causes local strain of a single-layer two-dimensional semiconductor, so that the energy gap changes continuously to change the motion of carriers. The structure and size of different parameters are adopted according to different final plans and application scenes.
The laser light source irradiates a single-layer two-dimensional semiconductor, and means that in the characterization process of Photoluminescence (PL), three-dimensional PL intensity mapping is obtained through line scanning on the whole structure. The laser wavelength and the laser power can be selected according to the single-layer two-dimensional semiconductor.
The dielectric layer is an insulating layer for applying a gate voltage. The preparation method of the dielectric layer can be spin coating, evaporation coating or sputtering.
The gate voltage is an electric field applied between the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with the surface having the protruding structure, and the injection and transition of excitons are influenced, so that the light emission of the single-layer two-dimensional semiconductor is influenced.
The conductive electrode is formed on the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with the surface having the convex structure by using any method. For example, a metal is plated by a coater after a template is formed by photolithography.
The connecting wire refers to a part having a function of connecting the composite heterostructure to the electronic system, and the connecting wire is not required to be provided as long as the composite heterostructure can be connected to the electronic system.
The electronic system is an electronic system capable of applying voltage between the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with the surface having the convex structure.
Advantageous effects
The invention provides a method for improving the luminous brightness of a single-layer two-dimensional semiconductor, which integrates the single-layer two-dimensional semiconductor and a three-dimensional semiconductor with a raised structure on the surface to form a composite heterostructure, generates a greatly enhanced coupling system and greatly improves the luminous brightness of the single-layer two-dimensional semiconductor. The simple and efficient silicon-based composite heterostructure is fully extensible, is expected to be used as a quantum light source with high brightness, long-term stability and chip integration, and belongs to the technical field of quantum optics and photon quantum information.
Drawings
FIG. 1 shows a three-dimensional semiconductor with a raised structure on the surface, step 1;
FIG. 2 is a step 2 of transferring a single layer of a two-dimensional semiconductor onto a three-dimensional semiconductor having a raised structure on a surface thereof;
FIG. 3 shows step 3, irradiating a single-layer two-dimensional semiconductor test PL with a laser light source;
FIG. 4 is a step 4 of connecting the composite heterostructure to an electronic system by a wire, and irradiating a single layer two dimensional semiconductor test PL with a laser light source;
FIG. 5 is a simplified three-dimensional view of a composite heterostructure formed of a single layer of a two-dimensional semiconductor and a three-dimensional semiconductor having a raised structure on the surface;
FIG. 6 is a schematic illustration of the principle of a composite heterostructure to enhance single-layer two-dimensional semiconductor luminescence;
FIG. 7 is an experimental test case;
FIG. 8 shows WSe2Exciton dynamics in a composite heterostructure formed by a monolayer and a three-dimensional periodic SiGe corrugated structure.
Detailed Description
In order to make the implementation objects, technical solutions and advantages of the present invention clearer, the following describes the scheme in the example of the present invention in more detail with reference to the accompanying drawings in the example of the present invention. In the drawings, the same or similar symbols denote the same or similar elements or elements having the same or similar functions. The described examples are examples of a portion, but not all, of the invention.
The examples described below with reference to the drawings are illustrative and intended to illustrate the invention and are not to be construed as limitations of the invention. All other embodiments based on the embodiments of the present invention can be obtained by those skilled in the art without any creative efforts, and the embodiments of the present invention are described in detail below with reference to the attached drawings.
In the description of the present invention, it is to be understood that the terms "intermediate", "reduced", "low", "higher", "lower", "larger", "large" and "stacked" are used in an orientation, position or relationship based on the knowledge of the orientation, position or relationship shown in the drawings for the convenience of description and simplicity of description, and do not indicate or imply that the referenced device or element must have a particular orientation, be constructed and operated in a particular orientation, and therefore, should not be taken as limiting the scope of the invention.
Example 1
A method for improving the luminous brightness of a single-layer two-dimensional semiconductor is disclosed, as shown in FIG. 5, a three-dimensional semiconductor with a convex structure on the surface is adopted: the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with a specific structure are coupled and simultaneously generate local strain to generate an exciton funnel effect, so that the aim of improving the light emission of the single-layer two-dimensional semiconductor is fulfilled.
The composite heterostructure prepared by the method comprises: the laser diode comprises a single-layer two-dimensional semiconductor, a three-dimensional semiconductor with a raised structure on the surface, a dielectric layer, a conductive electrode, a lead and a laser light source; the single-layer two-dimensional semiconductor is placed on a three-dimensional semiconductor with a protruding structure on the surface to form a composite heterostructure, the single-layer two-dimensional semiconductor is irradiated by laser to observe the change of PL, a dielectric layer is covered on the single-layer two-dimensional semiconductor, and a conducting wire is connected to the dielectric layer and the three-dimensional semiconductor with the protruding structure on the surface, so that the composite heterostructure can be conveniently connected into an electronic system and can be regulated and controlled by applying grid voltage.
The working method of the quantum light source with high brightness, long-term stability and chip integratability comprises the following steps:
as shown in fig. 1, operation 1 prepares a three-dimensional semiconductor having a raised structure on its surface, here exemplified by preparing a three-dimensional periodic SiGe corrugated structure using standard Complementary Metal Oxide Semiconductor (CMOS) compatible processing techniques, including photolithography and reactive ion etching techniques.
As shown in FIG. 2, operation 2 transfers a single two-dimensional semiconductor layer to a three-dimensional semiconductor having a surface with a raised structure, here exemplified by WSe grown by a CVD method using wet transfer2The single layer of material is transferred onto a three-dimensional periodic SiGe corrugated structure.
As shown in FIG. 3, WSe was irradiated with a laser light source having a wavelength of 532nm2And (3) carrying out line scanning on different positions of the single-layer material on the whole structure to obtain three-dimensional PL intensity mapping, and observing the change of PL at different positions.
As shown in fig. 4, in operation 4, polymethyl methacrylate (PMMA) is spin-coated on a single two-dimensional semiconductor as a dielectric layer, and a wire is connected to the dielectric layer material and the three-dimensional periodic SiGe corrugated structure, so that the composite heterostructure is connected to a meter where a voltage can be applied. Applying different voltages, test WSe2The photoluminescence of the same position on the single-layer material is changed, and the relation with the voltage is observed.
As shown in fig. 6, for a brief explanation of the principle of increasing the light emitting brightness of a single-layer two-dimensional semiconductor, when the single-layer two-dimensional semiconductor is transferred to a three-dimensional semiconductor with a raised surface structure, the single-layer two-dimensional semiconductor is locally strained, which causes the energy band structure of the single-layer two-dimensional semiconductor to change, reflected as the change of the carrier concentration of the single-layer two-dimensional semiconductor, excitons will shift to the position where the local strain is the largest and the band gap is the smallest, and the light emitting intensity is increased to a middle level; meanwhile, the three-dimensional semiconductor with the convex structure on the surface has larger carrier concentration at a specific part, interlayer exciton transition exists at the contact part of the single-layer two-dimensional semiconductor and the three-dimensional semiconductor, extra excitons can be injected into the single-layer two-dimensional semiconductor, the luminous intensity of the single-layer two-dimensional semiconductor is improved to a higher level, and the exciton injection efficiency depends on the grid voltage, so that the regulation and control can be carried out by the grid voltage. Due to the special integration of the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with the surface provided with the convex structure, the two influences jointly contribute to generate a greatly enhanced coupling system, so that the luminous efficiency of the single-layer two-dimensional semiconductor based on growth is greatly improved.
As shown in fig. 7, this is experimental test data given for ease of understanding. The test material was WSe2A single layer semiconductor, graph A shows the sample in SiO2On the/Si substrate, measuring the PL intensity to 300; graph B shows that the sample has PL intensity of 40000, WSe measured on a three-dimensional periodic SiGe corrugated structure semiconductor2The PL strength of a single layer of material increases by more than two orders of magnitude. Graph C shows the PL intensity of the sample on the three-dimensional periodic SiGe corrugated structure semiconductor along with the change of the applied grid voltage, and the measured PL intensity increases along with the increase of the grid voltage, namely, the WSe can be further regulated and controlled through the grid voltage2The light emission intensity of (1).
As shown in FIG. 8, this is WSe2The exciton dynamics schematic diagram in the composite heterostructure formed by the monolayer and the three-dimensional periodic SiGe wrinkle structure shows that the combined effect of exciton funnel effect and exciton transition greatly improves the WSe2Luminescence of a single layer of material.
The above detailed description is intended to illustrate the objects, aspects and advantages of the present invention, and it should be understood that the above detailed description is only exemplary of the present invention and is not intended to limit the scope of the present invention, and any modifications, equivalents, improvements and the like made within the spirit and principle of the present invention should be included in the scope of the present invention.

Claims (10)

1. A method for improving the brightness of a single-layer two-dimensional semiconductor is characterized in that: integrating a single-layer two-dimensional semiconductor into a three-dimensional semiconductor with a raised structure on the surface: the single-layer two-dimensional semiconductor is coupled with the three-dimensional semiconductor to generate an exciton funnel effect and an exciton injection effect, so that the aim of improving the light emission of the single-layer two-dimensional semiconductor is fulfilled.
The three-dimensional semiconductor with the surface provided with the convex structure enables the single-layer two-dimensional semiconductor to generate local strain, and the energy band structure of the single-layer two-dimensional semiconductor is changed to form an exciton funnel effect; exciton transition exists at the contact position of the single-layer two-dimensional semiconductor and the three-dimensional semiconductor, and extra excitons can be injected into the single-layer two-dimensional semiconductor; the exciton injection efficiency depends on the gate voltage and can therefore be further adjusted with the gate voltage. The composite heterostructure composed of the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with the surface provided with the convex structure is utilized, the exciton funnel effect formed and the interlayer exciton transition jointly generate influence, and the purpose of improving the luminous brightness of the single-layer two-dimensional semiconductor is achieved.
2. A quantum light source with high brightness, long-term stability and chip integratability prepared by the method of claim 1, wherein: the method comprises the following steps: the laser diode comprises a single-layer two-dimensional semiconductor, a three-dimensional semiconductor with a raised structure on the surface, a dielectric layer, a conductive electrode, a lead and a laser light source; the single-layer two-dimensional semiconductor is placed on a three-dimensional semiconductor with a raised structure on the surface to form a composite heterostructure, a laser light source is used for irradiating the single-layer two-dimensional semiconductor, a dielectric layer is covered on the single-layer two-dimensional semiconductor, and a conducting wire and a conducting electrode are connected on the dielectric layer and the three-dimensional semiconductor with the raised structure on the surface, so that the composite heterostructure can be conveniently accessed into an electronic system and can be regulated and controlled by applying grid voltage.
3. The quantum light source of claim 2, wherein: the single-layer two-dimensional semiconductor refers to a material in a nanometer scale range in one dimension. E.g., single layer WSe2、WS2、GaSe、MoSe2、MoS2、MoTe2、SnSe2GeSe, and graphene.
4. The method of claim 1, wherein: the three-dimensional semiconductor with the surface provided with the convex structure is any three-dimensional silicon-based semiconductor with deformation or local deformation. Such as a corrugated structure, the wavelength, amplitude, lateral etching depth and doping concentration of which are adjustable parameters. The raised structure of the three-dimensional semiconductor causes local strain of a single-layer two-dimensional semiconductor, so that the energy gap changes continuously to change the motion of a carrier, and the structure and the size of different parameters are adopted according to different final plans and application scenes.
5. The quantum light source of claim 2, wherein: the laser light source irradiates a single-layer two-dimensional semiconductor, and means that in the photoluminescence characterization process, a three-dimensional Photoluminescence (PL) intensity map is obtained by linear scanning on the whole structure.
6. The quantum light source of claim 2, wherein: the dielectric layer is an insulating layer for applying a gate voltage. The preparation method of the dielectric layer is spin coating, evaporation or sputtering.
7. The quantum light source of claim 2, wherein: the gate voltage is an electric field applied between the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with the surface having the protruding structure, and the injection and transition of excitons are influenced, so that the light emission of the single-layer two-dimensional semiconductor is influenced.
8. The quantum light source of claim 2, wherein: the preparation method of the conductive electrode is to form a template by a photoetching method and then plate a layer of metal by a film plating machine.
9. The quantum light source of claim 2, wherein: the connecting wire refers to a part having a function of connecting the composite heterostructure to the electronic system, and the connecting wire is not required to be provided as long as the composite heterostructure can be connected to the electronic system.
10. The quantum light source of claim 2, wherein: the electronic system is capable of applying a voltage between the single-layer two-dimensional semiconductor and the three-dimensional semiconductor with the surface having the convex structure.
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