CN111090137B - Flexible single photon source device with plasmon nano structure and preparation method thereof - Google Patents

Flexible single photon source device with plasmon nano structure and preparation method thereof Download PDF

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CN111090137B
CN111090137B CN201911276732.2A CN201911276732A CN111090137B CN 111090137 B CN111090137 B CN 111090137B CN 201911276732 A CN201911276732 A CN 201911276732A CN 111090137 B CN111090137 B CN 111090137B
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substrate layer
plasmon
single photon
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CN111090137A (en
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王志明
吴错
余鹏
马翠苹
林峰
童鑫
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University of Electronic Science and Technology of China
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Abstract

The invention discloses a flexible single photon source device with a plasmon nanometer structure and a preparation method thereof, wherein the flexible single photon source device comprises a substrate layer, a metal layer and a flexible substrate layer; the flexible substrate layer comprises a bow-tie type plasmon structure and quantum dots arranged at the center of the bow-tie type plasmon structure; the flexible substrate layer is made of polydimethylsiloxane. The flexible single photon source device of the plasmon nanometer structure is physically adjustable, the problem of accurately controlling the local state density of a light field in a plasmon gap is utilized, and the enhancement and control of the gap structure based on the proposed structure are the photon repetition rate. The processed plasmon structure is coated by utilizing the polydimethylsiloxane as the flexible substrate, the structure gap of the substrate can be adjusted by stretching and bending the substrate, and the substrate is combined with a colloidal quantum point light source to realize a single photon source with adjustable photon repetition rate, so that the high-precision single photon source with adjustable photon repetition rate is realized.

Description

Flexible single photon source device with plasmon nano structure and preparation method thereof
Technical Field
The invention relates to the field of single photon sources, in particular to a flexible single photon source device with a plasmon nanometer structure and a preparation method thereof.
Background
In the process of continuously improving the integration scale, the processing speed and the data capacity in the post-molar age, the silicon-based photoelectric integration and the quantum information device play a vital role. The mainstream technical route for developing photoelectric information devices and quantum devices is to construct a novel nano device structure based on a traditional information system platform and combining with emerging photoelectric materials, and to realize low power consumption and high-efficiency information processing and transmitting functions by taking photons and the like as carriers. With improvements in the level of microfabrication and chemical fabrication, plasmonic optics have been rapidly developed in recent years. The wavelength of the surface plasmon of the metal nano structure is far smaller than that of light in a free space, so that the electromagnetic field can be bound to a size far smaller than the wavelength of the light, and the near field enhancement of the sub-wavelength size is realized. Based on this characteristic, surface plasmons have been widely used in the fields of nano lithography, nano photonics, bio-detectors, optical detection, and the like. The method has great application potential in the aspects of optical signal processing, safety communication and the like of mobile/data communication of integrated on-chip photonic devices and single photon sources. However, the spontaneous emission efficiency of a single quantum dot is low, and the emission direction is random, and the application is severely limited. In order to enhance the spontaneous emissivity and improve the spontaneous emission efficiency of the quantum dots and simultaneously realize directional single photon emission, one effective approach is to embed the quantum dots into the microcavity. Although the spontaneous radiance can be enhanced through the cavity, the single intrinsic radiance cannot be changed, and one radiance is obtained by one device parameter. In order to be effectively applied in practical application, the emissivity of a single-photon source needs to be controllable and variable.
Disclosure of Invention
The invention provides a flexible single photon source device with a plasmon nanometer structure and a preparation method thereof, aiming at overcoming the defects in the prior art.
The invention firstly provides a flexible single photon source device with a plasmon nanometer structure, which comprises a substrate layer, a metal layer and a flexible substrate layer; the flexible substrate layer comprises a bow-tie type plasmon structure and quantum dots arranged at the center of the bow-tie type plasmon structure; the flexible substrate layer is made of polydimethylsiloxane.
Preferably, the substrate layer is a silicon dioxide substrate layer or a monocrystalline silicon substrate layer.
More preferably, the silicon dioxide substrate layer is a silicon dioxide substrate layer with thermal oxidation of 285 nm.
Preferably, the metal layer is a copper metal layer.
Preferably, the bow-tie type plasmon structure is a plasmon gold nanostructure.
Preferably, the quantum dots are cadmium selenide quantum dots.
The invention also provides a preparation method of the flexible single photon source device with the plasmon nanometer structure, which comprises the following steps:
s1, providing a 285nm silicon dioxide substrate layer or a monocrystalline silicon substrate layer of a metal layer on which copper is pre-deposited to form a substrate layer and a metal layer, and depositing periodically arranged bow-tie type plasmonic structures on the metal layer;
s2 spin-coating photoresist on the surface of the bow-tie type plasmon structure, etching a positioning hole by using electron beam lithography, and then spin-coating a colloidal quantum dot solution, wherein the quantum dot falls on the positioning hole;
s3, finally, coating the periodic bowknot type metal nanowire structure layer and the quantum dots of cadmium selenide on the surface of the metal layer by using polydimethylsiloxane;
s4 etching away the copper metal layer with an etchant.
Preferably, the bow-tie type metal nanowire structure layer and the quantum dots of cadmium selenide are embedded in the polydimethylsiloxane flexible substrate.
Preferably, the bow-tie type plasmon structure in step S1 is prepared by depositing 200nm thick copper on a silicon dioxide/silicon substrate containing 285nm thick by electron beam evaporation or thermal evaporation, wherein the copper layer is a sacrificial layer. And then spin-coating polymethyl methacrylate photoresist on the surface of copper, depositing gold with the thickness of 50nm in an electron beam evaporation mode after an exposure and development process by using an electron beam lithography method, and then stripping and removing the photoresist to obtain the patterned plasmon gold bow-tie structure.
The invention has the beneficial effects that:
1. the flexible single photon source device of the plasmon nanometer structure is physically adjustable, the problem of accurately controlling the local state density of a light field in a plasmon gap is utilized, and the enhancement and control of the gap structure based on the proposed structure are the photon repetition rate. The processed plasmon structure is coated by utilizing the polydimethylsiloxane as the flexible substrate, the structure gap of the substrate can be adjusted by stretching and bending the substrate, and the substrate is combined with a colloidal quantum point light source to realize a single photon source with adjustable photon repetition rate, so that the high-precision single photon source with adjustable photon repetition rate is realized.
2. The flexible single photon source device of the plasmon nanostructure utilizes polydimethylsiloxane as a flexible substrate to couple the colloidal quantum dots in gaps of the bowtie metal nanostructure, fully utilizes the characteristics of flexibility, stretchability and bendability, and the adjustable local optical state density of the plasmon and the low cost of the colloidal quantum dots, can rapidly realize a single photon source with adjustable repetition rate at room temperature, and the photon repetition rate can be continuously adjusted from 30MHz to 30GHz, thereby filling the gap of mechanical adjustable photon repetition rate in the field of single photon sources.
Drawings
FIG. 1 is a schematic view of the radiation direction of the stimulated radiation of quantum dots according to a preferred embodiment of the present invention;
FIG. 2 is a top view of a flexible single photon source device of plasmonic nanostructures in accordance with a preferred embodiment of the present invention;
FIG. 3 is a perspective view of a flexible single photon source device of plasmonic nanostructures in accordance with a preferred embodiment of the present invention;
FIG. 4 is a perspective view of a flexible single-photon source device of plasmonic nanostructures in accordance with a preferred embodiment of the present invention;
FIG. 5 is a schematic diagram of the peeling of the flexible base of the flexible single-photon source device of plasmonic nanostructures from the substrate in accordance with a preferred embodiment of the present invention;
the specific reference numerals are:
1 a substrate layer; 2, a metal layer; 3 a flexible substrate layer; 31 a bow-tie plasmon structure; 32 quantum dots.
Detailed Description
In order that those skilled in the art will better understand the technical solutions of the present invention, the present invention will be further described in detail with reference to the following embodiments.
The invention firstly provides a flexible single photon source device with a plasmon nanometer structure, which comprises a substrate layer 1, a metal layer 2 and a flexible substrate layer 3; the flexible substrate layer 3 comprises a bow-tie type plasmon structure 31 and quantum dots 32 arranged at the center of the bow-tie type plasmon structure 31; the flexible substrate layer 3 is made of polydimethylsiloxane.
Preferably, the substrate layer 1 is a silicon dioxide substrate layer or a monocrystalline silicon substrate layer.
More preferably, the silicon dioxide substrate layer is a silicon dioxide substrate layer with thermal oxidation of 285 nm.
Preferably, the metal layer 2 is a copper metal layer.
Preferably, the bow-tie type plasmonic structure 31 is a plasmonic gold nanostructure.
Preferably, the quantum dots 32 are cadmium selenide quantum dots.
The invention also provides a preparation method of the flexible single photon source device with the plasmon nanometer structure, which comprises the following steps:
s1, providing a 285nm silicon dioxide substrate layer or a monocrystalline silicon substrate layer which is pre-deposited with a copper metal layer to form a substrate layer 1 and a metal layer 2, and depositing periodically arranged bow-tie type plasmonic structures 31 on the metal layer 2;
s2 spin-coating photoresist on the surface of the bow-tie type plasmon structure 31, etching a positioning hole by electron beam lithography, then spin-coating colloidal quantum dot solution, and enabling the quantum dot 32 to fall on the positioning hole;
s3, finally, coating the periodic bowknot type plasmon structure 31 and the cadmium selenide quantum dots 32 on the surface of the metal layer 2 by using polydimethylsiloxane;
s4 etching away the copper metal layer 2 with etching solution
Preferably, the bow-tie type plasmonic structure 31 and the cadmium selenide quantum dots 32 are embedded in a polydimethylsiloxane flexible substrate.
Preferably, the bow-tie type plasmon structure 31 in step S1 is prepared by depositing 200nm thick copper on a silicon dioxide/silicon substrate containing 285nm thick by electron beam evaporation or thermal evaporation, wherein the copper layer is a sacrificial layer. And then spin-coating polymethyl methacrylate photoresist on the surface of copper, depositing gold with the thickness of 50nm in an electron beam evaporation mode after an exposure and development process by using an electron beam lithography method, and then stripping and removing the photoresist to obtain the patterned bow-tie type plasmon structure 31.
The flexible single photon source device with the plasmon nanometer structure is shown in figures 2-5, and the specific preparation process is as follows:
providing a substrate layer 1, wherein the substrate layer 1 is made of a monocrystalline silicon substrate of thermal oxidation 285nm silicon dioxide; depositing a copper metal layer 2 on said substrate layer 1, techniques for depositing high-quality copper being known from many documents, preferably by means of electron beam evaporation; etching a bow-tie type plasmon structure 31 on the substrate of the metal layer 2 with copper by using an electron beam lithography mode; evaporating and depositing gold in the carved bow tie pattern by using an electron beam, and removing the photoresist to obtain a plasmon gold nanostructure; then, etching a round hole in the center of each bow tie in an electron beam lithography mode, and positioning the quantum dots 32 of the colloid; scattering the quantum dots 32 of the liquid drop colloid to each round hole point by a spin coating mode; after removing the photoresist, spin-coating the prepared polydimethylsiloxane on the surface of the whole device; after curing, placing the device into a copper etching agent for etching; and cleaning to obtain the flexible single photon source device with the plasmon nanometer structure.
As shown in FIG. 1, the flexible single photon source device of the plasmon nanostructure prepared by the method has a fast photon excitation rate and a concentrated radiation mode.
Example one
The preparation method of the flexible single photon source device with the plasmon nanometer structure comprises the following steps:
(1) providing a substrate layer 1, wherein the substrate layer 1 is made of a monocrystalline silicon substrate of thermal oxidation 285nm silicon dioxide;
(2) depositing a metal layer 2 of copper on the substrate layer 1 by electron beam evaporation;
(3) etching a pattern of the bow-tie type plasmon structure 31 on the substrate of the metal layer 2 with copper by using electron beam lithography;
(4) evaporating and depositing gold in the carved bow tie pattern by using an electron beam, and removing the photoresist to obtain a plasmon gold nanostructure;
(5) then, etching a round hole in the center of each bow tie in an electron beam lithography mode, and positioning the quantum dots 32 of the colloid;
(6) scattering the quantum dots 32 of the liquid drop colloid to each round hole point by a spin coating mode;
(7) after removing the photoresist, spin-coating the prepared Polydimethylsiloxane (PDMS) on the surface of the whole device;
(8) after curing, putting the device into a copper etching agent for etching for 5 minutes;
(9) and washing the substrate with deionized water for 20 minutes to obtain the flexible single photon source device with the plasmon nanometer structure.
(10) Using a focused continuous wave laser (488nm wavelength) to<An incident power of 100nW excites the single photon source device. To verify the presence of a single quantum dot, the fluorescence generated was separated by a non-polarizing beam splitter and projected onto a pair of single photon counting avalanche diodes (50 μm)2Micro-regions). The detectors are connected to a time dependent single photon counting module that measures the arrival time between photons on the two detectors, producing a second order correlation function.
The above is only a preferred embodiment of the present invention, and it should be noted that the above preferred embodiment should not be considered as limiting the present invention, and the protection scope of the present invention should be subject to the scope defined by the claims. It will be apparent to those skilled in the art that various modifications and adaptations can be made without departing from the spirit and scope of the invention, and these modifications and adaptations should be considered within the scope of the invention.

Claims (7)

1. A flexible single photon source device with a plasmon nanometer structure is characterized in that: the metal-clad laminate comprises a substrate layer, a metal layer and a flexible substrate layer; the flexible substrate layer comprises a bow-tie type plasmon structure and quantum dots arranged at the center of the bow-tie type plasmon structure; the flexible substrate layer is made of polydimethylsiloxane;
the bow-tie type plasmon structure is a plasmon gold nanostructure; the quantum dots are cadmium selenide quantum dots.
2. The plasmonic nanostructure's flexible single photon source device of claim 1, wherein: the substrate layer is a silicon dioxide substrate layer or a monocrystalline silicon substrate layer.
3. The plasmonic nanostructure's flexible single photon source device of claim 2, wherein: the silicon dioxide substrate layer is a silicon dioxide substrate layer thermally oxidized to 285 nm.
4. The plasmonic nanostructure's flexible single photon source device of claim 1, wherein: the metal layer is a copper metal layer.
5. A method for preparing a flexible single photon source device with a plasmonic nanostructure according to claim 1, wherein the method comprises the following steps: the method comprises the following steps:
s1, providing a 285nm silicon dioxide substrate layer or a monocrystalline silicon substrate layer which is deposited with a copper metal layer in advance to form a substrate layer, and depositing periodically arranged bow-tie type plasmon structures on the copper metal layer;
s2 spin-coating photoresist on the surface of the bow-tie type plasmon structure, etching a positioning hole by using electron beam lithography, and then spin-coating a colloidal quantum dot solution, wherein the quantum dot falls on the positioning hole;
s3, finally, coating the periodic bowknot type metal nanowire structure layer and the quantum dots of the cadmium selenide on the surface of the substrate layer by using polydimethylsiloxane;
s4 etching away the copper metal layer with an etchant.
6. The method for preparing a flexible single photon source device with a plasmonic nanostructure according to claim 5, wherein the method comprises the following steps: the bowknot type metal nanowire structure layer and the quantum dots of the cadmium selenide are embedded into the polydimethylsiloxane flexible substrate layer.
7. The method for preparing a flexible single photon source device with a plasmonic nanostructure according to claim 5, wherein the method comprises the following steps: the preparation method of the bow-tie type plasmon structure in the step S1 is that copper with the thickness of 200nm is deposited on a silicon dioxide/silicon substrate with the thickness of 285nm by using an electron beam evaporation or thermal evaporation technology, and the copper layer is a sacrificial layer; and then spin-coating polymethyl methacrylate photoresist on the surface of copper, depositing gold with the thickness of 50nm in an electron beam evaporation mode after an exposure and development process by using an electron beam lithography method, and then stripping and removing the photoresist to obtain the patterned plasmon gold bow-tie structure.
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