CN119937068A - Metamaterial anti-reflection film for radioisotope thermophotovoltaic cells and its preparation method and application - Google Patents
Metamaterial anti-reflection film for radioisotope thermophotovoltaic cells and its preparation method and application Download PDFInfo
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Abstract
本申请公开一种放射性同位素热光伏电池用的超材料减反膜及其制备方法与应用。放射性同位素热光伏电池用的超材料减反膜，为全介质超材料减反膜；全介质超材料减反膜由下至上依次包括：第一反射层、第二反射层及Si纳米谐振微结构层。本申请的减反膜具有高度的灵活性，可以通过调整超材料的结构参数来调控减反膜的折射率及电磁波的反射特性，从而精确优化其在目标波段和宽角度范围下的性能表现，实现与放射性同位素热光伏电池所用热光伏组件相匹配的近红外光波段的高效减反效果，减少光的反射损失，提高光电转换效率，进而提升放射性同位素热光伏电池的整体电学输出性能。
The present application discloses a metamaterial anti-reflection film for radioisotope thermophotovoltaic cells and a preparation method and application thereof. The metamaterial anti-reflection film for radioisotope thermophotovoltaic cells is an all-dielectric metamaterial anti-reflection film; the all-dielectric metamaterial anti-reflection film includes, from bottom to top, a first reflection layer, a second reflection layer and a Si nano-resonance microstructure layer. The anti-reflection film of the present application has a high degree of flexibility, and the refractive index of the anti-reflection film and the reflection characteristics of electromagnetic waves can be adjusted by adjusting the structural parameters of the metamaterial, so as to accurately optimize its performance in the target band and wide angle range, achieve a high-efficiency anti-reflection effect in the near-infrared light band that matches the thermophotovoltaic components used in radioisotope thermophotovoltaic cells, reduce light reflection losses, improve photoelectric conversion efficiency, and thus improve the overall electrical output performance of radioisotope thermophotovoltaic cells.
Description
Technical Field
The application relates to the technical field of metamaterial for nuclear power technology, in particular to a metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell, and a preparation method and application thereof.
Background
The radioisotope thermophotovoltaic cell (Radioisotope Thermophotovoltaic Battery, RTPVB) is a device which takes the heat energy decayed by a radioisotope heat source as a source item and converts the heat energy into electric energy by utilizing the photovoltaic effect in an infrared radiation mode, has the advantages of long service life, high volume power density, light structure, strong environmental adaptability and the like, and is regarded as an ideal power supply type under extreme conditions such as deep space, deep sea, polar region and the like.
The radioisotope thermophotovoltaic cell mainly comprises a radioisotope heat source, a heat radiator, a filter and a thermophotovoltaic module. The radioisotope source deposits and converts decay energy into heat energy in the radioisotope source, the surface temperature of the radioisotope source can reach more than 1200K, the heat radiator emits heat energy of the heat source in an infrared radiation mode, the heat energy is incident to the thermal photovoltaic assembly after being regulated and controlled by the filter, the light energy is converted into electric energy through a photovoltaic effect, and all components are mutually coupled and regulated in the whole process, so that efficient energy conversion and electric energy output are realized. The thermophotovoltaic module is used as a key component for final electric energy output, and plays an important role in the whole energy conversion process. However, due to the fact that certain air impedance exists in the surface window layer material of the thermal photovoltaic module, about 30% of incident photons are reflected, partial photon energy loss is caused, the thermal photovoltaic module cannot fully absorb the incident photons, and the final electrical output performance and energy conversion efficiency of the radioactive radioisotope thermal photovoltaic cell are further affected.
The method for reducing photon reflection of the thermal photovoltaic module is that an antireflection film is added on the surface of the thermal photovoltaic module, the traditional antireflection film is an optical film composed of a plurality of layers of different materials or refractive index layers, and reflected light on the optical surface is reduced or eliminated through interference effects among the layers, so that the light transmittance is improved. However, such conventional anti-reflection films do not match well with near infrared light emitted from radioisotope heat sources because of their difficulty in achieving efficient anti-reflection over a wide frequency band and wide angular range of near infrared light.
Disclosure of Invention
In order to solve the defects in the art, the application aims to provide a metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell, and a preparation method and application thereof.
According to one aspect of the present application, there is provided a metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell,
The metamaterial anti-reflection film sequentially comprises a first reflecting layer, a second reflecting layer and a Si quadrangular frustum nano resonance microstructure layer from bottom to top.
According to some embodiments of the application, the Si four-sided land nano-resonance microstructure layer is arranged regularly.
According to some embodiments of the application, the metamaterial anti-reflection film is an all-dielectric metamaterial anti-reflection film.
According to some embodiments of the application, each Si quadrangular frustum has an upper side length of 70-100nm, a lower side length of 150-200nm, and a height of 300-400nm.
According to some embodiments of the application, the spacing between every two Si quadrangular pyramid is 70-100nm.
According to some embodiments of the application, the material of the first reflective layer comprises MgF 2 or SiO 2, and the thickness of the first reflective layer is 40-70nm.
According to some embodiments of the application, the material of the second reflective layer comprises ZnS or TiO 2, and the thickness of the second reflective layer is 30-50nm.
According to another aspect of the present application, a method for preparing a metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell includes:
Sequentially preparing a first reflecting layer and a second reflecting layer on the surface of the thermal photovoltaic module;
continuously preparing a Si layer on the surface of the second reflecting layer;
coating photoresist on the surface of the Si layer, preparing a Cr layer after exposure and development, and etching to prepare the Si nano resonance microstructure layer.
According to some embodiments of the application, the first reflective layer and the second reflective layer are prepared using a chemical deposition process.
According to some embodiments of the application, the Cr layer has a thickness of 40-50nm.
According to still another aspect of the application, the metamaterial anti-reflection film for the radioisotope thermophotovoltaic cell prepared by the preparation method is used for preparing a thermophotovoltaic module.
Compared with the prior art, the application at least has the following beneficial effects:
compared with the traditional anti-reflection film, the anti-reflection film of the metamaterial for the radioactive isotope thermal photovoltaic cell has high flexibility, and the refractive index of the composite material and the reflection characteristic of electromagnetic waves can be regulated and controlled by regulating structural parameters (such as size, shape, arrangement mode and the like) of the metamaterial, so that the performance of the composite material under a target wave band and a wide angle range is accurately optimized, the efficient anti-reflection effect of a near infrared wave band matched with the radioactive radioisotope thermal photovoltaic cell is realized, the reflection loss of light is reduced, the photoelectric conversion efficiency is improved, and the overall performance of a thermal photovoltaic module is improved.
The metamaterial anti-reflection film is added with the high-refractive index microstructure on the basis of the double-layer reflecting layer film to form an all-medium metamaterial structure, and the transmission field is effectively changed by exciting proper surface current density and magnetic current density, so that the low-band-gap thermophotovoltaic module can realize efficient absorption of infrared photons.
According to the application, by utilizing the electric resonance and magnetic resonance effects in the metamaterial and through the design of the microstructure, the regulation and control of the propagation characteristics of electromagnetic waves are realized, the reflection of the electromagnetic waves on the interface of the medium and the antireflection film is regulated, and the reflection cancellation is realized, so that the purpose of antireflection is achieved.
According to the preparation method of the metamaterial anti-reflection film for the radioisotope thermophotovoltaic cell, the designed anti-reflection film is prepared and processed through magnetron sputtering, chemical vapor deposition, electron beam lithography and plasma etching technologies. Aiming at the problem of large photon reflection loss of a thermophotovoltaic module in a radioactive radioisotope thermophotovoltaic cell, a more efficient metamaterial anti-reflection film design scheme is provided.
Drawings
Fig. 1 is a schematic structural view of a metamaterial anti-reflection film according to an example embodiment of the present application.
Fig. 2 is a process flow diagram of a preparation process of a metamaterial anti-reflection film according to an example embodiment of the application.
Fig. 3 is a graph showing the reflectance of the metamaterial anti-reflection film and the Al 2O3/TiO2 anti-reflection film according to an exemplary embodiment of the present application.
Fig. 4 is a graph of quantum efficiency of an InGaAsP-3J thermophotovoltaic module of an exemplary embodiment of the present application and an anti-reflection film of a comparative example.
Fig. 5 is a schematic structural view and a transmission spectrum of example comparative example 2 of the present application.
Fig. 6 is a graph of blackbody thermal radiation power spectra at different temperatures according to an exemplary embodiment of the present application.
FIG. 7 is a graph showing the reflectance of a metamaterial anti-reflection film as a function of incident angle and wavelength according to an example embodiment of the present application.
Detailed Description
The technical solutions of the present application will be clearly and completely described in conjunction with the embodiments of the present application, and it is apparent that the described embodiments are some embodiments of the present application, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the application without making any inventive effort, are intended to be within the scope of the application.
It is particularly pointed out that similar substitutions and modifications to the application will be apparent to those skilled in the art, which are all deemed to be included in the application. It will be apparent to those skilled in the relevant art that variations and modifications can be made in the methods and applications described herein, or in the appropriate variations and combinations, without departing from the spirit and scope of the application. It will be apparent that the described embodiments are only some, but not all, embodiments of the application.
The application is carried out according to the conventional conditions or the conditions suggested by manufacturers if the specific conditions are not noted, and the raw materials or auxiliary materials and the reagents or instruments are conventional products which can be obtained commercially if the manufacturers are not noted.
The present application will be described in detail below.
The metamaterial anti-reflection film for the radioisotope thermophotovoltaic cell is an all-dielectric metamaterial anti-reflection film, and as shown in figure 1, the metamaterial anti-reflection film consists of a first reflecting layer and a second reflecting layer at the bottom and a Si nano resonance microstructure at the top.
The Si nano resonance microstructure at the top is formed by regularly arranging Si quadrangular tables, and the silicon has high refractive index and relatively low optical loss in the visible light and near infrared wavelength range, so that ohmic loss can be well reduced, and electromagnetic resonance intensity is improved. The bottom is formed by superposing a first reflecting layer and a second reflecting layer, for example, the first reflecting layer can be a MgF 2 thin layer or SiO 2, the second reflecting layer can be ZnS or TiO 2, wherein the refractive index of the ZnS layer is higher than that of the MgF 2 layer, and the coupling effect of incident photons and the window layer of the thermophotovoltaic assembly can be enhanced by the combination arrangement of decreasing the refractive indexes, so that the light loss when light is transmitted to the semiconductor active absorption layer is reduced.
By adjusting the size parameters of each part of the structure, the electromagnetic property of light in the nanoscale range can be regulated and controlled, and the low reflection effect of incident photons is realized.
Optionally, the structural parameters of the metamaterial anti-reflection film are that the upper edge length a=70-100 nm, the lower edge length b=150-200 nm, the height h=300-400 nm, the inter-unit distance d=70-100 nm, and the thicknesses of the first reflecting layer and the second reflecting layer are 40-70nm and 30-50nm respectively.
The interaction of the all-dielectric metamaterial anti-reflection film and incident photons of different wavebands can excite multiple resonance modes (Mie resonance and FP resonance), the multiple resonance modes can widen the reflectivity range of the anti-reflection film, the reflectivity is lower than 5% in the wavebands of 900-2000nm, and the high-efficiency photon absorption of the thermophotovoltaic module is realized in the wavebands of high quantum efficiency. At 950nm wavelength, the high refractive index Si nanostructure Mie resonance radiation has strong directivity, and thus will produce strong forward and weak back scattering characteristics, when the reflectivity is almost 0. At 1150nm wavelength, the all-dielectric metamaterial anti-reflection film provided by the application shows FP resonance phenomenon, and the photon reflectivity is reduced to below 5%.
The technical scheme of the application is further described below by combining specific embodiments.
Example 1
Sequentially plating MgF 2 with the thickness of 40nm and ZnS with the thickness of 30nm on the surface of the thermophotovoltaic module by using a chemical deposition (CVD) system;
Coating PMMA photoresist on the surface of the ZnS, and performing 90 ℃ soft drying operation on the photoresist for 50 seconds after finishing coating;
exposing the photoresist by using a large electron beam exposure system, soaking the exposed sample in positive photoresist developer for 40 seconds to dissolve the exposed photoresist to form a pattern array, and cleaning the sample by using clear water after development;
Plating Cr with the thickness of 50nm on the surface by using a magnetron sputtering technology, and taking the Cr as a hard mask for subsequent etching;
Placing the sample in acetone for soaking for 48 hours to enable photoresist to fall off, and performing ultrasonic cleaning in clean water for 10 minutes after soaking is finished;
And then, immersing the sample for 10min by using ceric ammonium nitrate solution, removing surface metal Cr, and cleaning the sample by using deionized water.
Example 2
Sequentially plating MgF 2 with the thickness of 70nm and ZnS with the thickness of 50nm on the surface of the thermophotovoltaic module by using a chemical deposition (CVD) system;
Plating Si with thickness of 350nm on ZnS surface by using an Inductively Coupled Plasma Enhanced Chemical Vapor Deposition (ICPECVD) system, coating PMMA photoresist on the Si surface, and carrying out soft baking and drying at 90 ℃ for 60 seconds after finishing coating;
Exposing the photoresist by using a large electron beam exposure system, soaking the exposed sample in positive photoresist developer for 60 seconds to dissolve the exposed photoresist to form a pattern array, and cleaning the sample by using deionized water after development;
plating Cr with the thickness of 45nm on the surface by using a magnetron sputtering technology, and taking the Cr as a hard mask for subsequent etching;
placing the sample in acetone for soaking for 48 hours to enable photoresist to fall off, and after soaking, performing ultrasonic cleaning in deionized water for 10 minutes;
And then, immersing the sample for 10min by using ceric ammonium nitrate solution, removing surface metal Cr, and cleaning the sample by using deionized water.
Example 3
Sequentially plating SiO 2 with the thickness of 55nm and TiO 2 with the thickness of 35nm on the surface of the thermophotovoltaic module by using a chemical deposition (CVD) system;
Coating PMMA photoresist on the surface of the Si, and performing soft baking and drying at 90 ℃ for 60 seconds after the coating is finished;
Exposing the photoresist by using a large electron beam exposure system, soaking the exposed sample in positive photoresist developer for 60 seconds to dissolve the exposed photoresist to form a pattern array, and cleaning the sample by using deionized water after development;
plating Cr with the thickness of 40nm on the surface by using a magnetron sputtering technology, and taking the Cr as a hard mask for subsequent etching;
placing the sample in acetone for soaking for 48 hours to enable photoresist to fall off, and after soaking, performing ultrasonic cleaning in deionized water for 10 minutes;
And then, immersing the sample in ceric ammonium nitrate solution for 10min to remove surface metal Cr, and cleaning the sample by using clean water.
Comparative example 1
A conventional Al 2O3/TiO2 antireflection film was prepared.
Placing a substrate in a reaction chamber, setting a deposition temperature of 1000 ℃, adjusting the flow rate, pressure and proportion of reaction gas, introducing an aluminum source precursor gas into the reaction chamber, enabling the aluminum source precursor gas and an oxygen source gas to react chemically, enabling the chemical reaction to be carried out on the surface of the substrate to generate an Al 2O3 film, stopping supplying the precursor gas and the oxygen source gas after a preset deposition time or the growth requirement of the Al 2O3 film is met, and cooling the reaction chamber to enable the substrate and the Al 2O3 film to be gradually cooled to room temperature.
Placing a substrate in a reaction chamber, setting the deposition temperature to be 200 ℃, introducing a titanium source precursor gas and an oxygen source gas into the reaction chamber, and enabling the precursor gas and the oxygen source gas to undergo chemical reaction, wherein the chemical reaction is carried out on the surface of the substrate to generate the TiO 2 film.
Comparative example 2
A metamaterial anti-reflection film is a structure of growing a metal cube array on a silicon oxide substrate.
As shown in fig. 5a, a two-dimensional metal cube array structure is designed on the cell surface, and this ultra-wideband transmission effect can be used to suppress the reflection on the cell surface.
As shown in fig. 5b, the transmission spectrum obtained by calculation at incidence angles of 0 ° and 68 ° respectively, wherein the geometric structure is dx=dy=320 nm, wx=wy=80 nm, h=320 nm, and the calculation result shows that the reflection enhancement transmission can be effectively reduced under the condition of incidence with a large angle for near infrared (800-2000 nm) incidence light with ultra-wide wave band, and is independent of polarization. At normal incidence, the transmission peak is around 1100nm, and at this time, the reflection is lowest, the highest transmission is around 90%, and the width is narrow.
As shown in FIG. 3, the metamaterial anti-reflection film can achieve the effect of low reflection and high absorption below 5% in the wave band of 900-2000 nm.
Comparative example 3
A multilayer dielectric structure comprises a substrate and an anti-reflection coating, wherein the anti-reflection coating comprises four layers, and the second layer is a cubic gold nanoparticle.
The comparative example employs a plurality of films of specific thickness and refractive index, so that the reflected light interferes or cancels after the incident light is reflected on the upper and lower surfaces of the films, thereby achieving the effect of reducing reflection.
However, in such a conventional multilayer film structure, the low reflection wavelength range is narrow and depends strongly on the optical properties of the material itself, which inevitably makes it impossible to meet the design goals of the antireflection film. The second refraction material uses cubic gold nano particles, when light interacts with the material, the electric field enhancement in the particles can increase the ohmic loss of the particles for the lossy metal material, and the heat energy loss is generated, so that the photon energy loss can be caused. The specific anti-reflection effect patent is not mentioned and cannot be compared.
The technical scheme of the application is that a Si quadrangular frustum microstructure is added on the basis of a double-layer dielectric film, and the periodic sub-wavelength all-dielectric metamaterial mainly utilizes the high refractive index characteristic of Si and the nano-scale structural dimension. When photons with proper wavelength interact with the Si microstructures, mie resonance is excited, each dielectric nano microstructure can be regarded as a Huygens source, the electric dipole and the magnetic dipole modes can be excited simultaneously, and the equivalent electric polarization corresponding to the electric dipole mode and the equivalent magnetic polarization corresponding to the magnetic dipole mode can be effectively regulated and controlled by adjusting the structural size of the nano microstructure. When the balance condition is satisfied by the electric resonance and the magnetic resonance, the reflection on the surface of the metamaterial is eliminated, and meanwhile, the phase manipulation of the transmitted light wave can cover the whole phase. In principle, the transmission efficiency of dielectric huyghen super-structured surface light wave manipulation can reach 100%. At longer wavelengths, the metamaterial microstructure excites Fabry-perot (FP) resonance, again producing a low reflection band. The combination of the two resonances widens the wavelength range of metamaterial anti-reflection and has good low reflection effect.
Experimental example
The antireflection films of example 1 and comparative example 1 were tested for reflectance.
The test results are shown in FIG. 3, from which it can be seen that the conventional Al 2O3/TiO2 antireflection film has a low reflection trough with a reflectivity of 3.8% at 800nm, and then the reflectivity is gradually increased, and the reflectivity is stabilized at about 20% after 2500 nm. The metamaterial anti-reflection film provided by the design has double wave troughs at wavelengths of 935nm and 1600nm, so that the wavelength range of low reflection is greatly widened, and the average reflectivity is lower than 3%. In the range of 900-3000nm, the reflectivity of the metamaterial anti-reflection film is lower than that of the traditional Al 2O3/TiO2 anti-reflection film, and the metamaterial anti-reflection film can be well matched with the thermal radiation spectrum at the front end of the thermal photovoltaic module, so that the full utilization of photon energy is ensured.
FIG. 4 is a graph of external quantum efficiency of a thermophotovoltaic module using different anti-reflection films. Compared with the thermal photovoltaic module using the conventional Al 2O3/TiO2 antireflection film, the thermal photovoltaic module using the metamaterial antireflection film has the advantage that the external quantum efficiency is obviously improved, so that the thermal photovoltaic module can generate more photocurrent. From the top cell to the bottom cell, it can be seen that the external quantum efficiency of each subcell gradually increases, especially for the bottom cell, by a maximum of 23%.
Fig. 6 shows the blackbody thermal radiation power spectrum of the metamaterial anti-reflection film of the application at different temperatures, and the graph shows that the intensity of the blackbody thermal radiation power is increased along with the temperature, and the peak value of the radiation spectrum is shifted rightwards, namely blue shift.
Fig. 7 shows the reflectance of the metamaterial anti-reflection film according to the present application as a function of the incident angle and wavelength, from which it can be seen that p-polarized light and s-polarized light have little effect on the reflection spectrum. With increasing incidence angle, a plurality of reflection peaks appear in the reflection spectrum, and no significant dependence of the reflection spectrum on the incidence angle can be observed in the range of 0 to 40 °. The metamaterial anti-reflection film has the characteristics of wide-angle response and polarization insensitivity.
The above description of the embodiments is only for aiding in the understanding of the method of the present application and its core ideas. It should be noted that it will be apparent to those skilled in the art that various modifications and adaptations of the application can be made without departing from the principles of the application and these modifications and adaptations are intended to be within the scope of the application as defined in the following claims.
Claims (10)
1. A metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell is characterized in that,
The metamaterial anti-reflection film sequentially comprises a first reflecting layer, a second reflecting layer and a Si quadrangular frustum nano resonance microstructure layer from bottom to top.
2. The metamaterial anti-reflection film for the radioisotope thermophotovoltaic cell according to claim 1, wherein Si quadrangular frustum pyramid in the Si quadrangular frustum pyramid nano resonance microstructure layer is regularly arranged;
Optionally, the metamaterial anti-reflection film is an all-medium metamaterial anti-reflection film.
3. The metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell according to claim 2, wherein each of the Si quadrangular pyramid has an upper side length of 70-100nm, a lower side length of 150-200nm, and a height of 300-400nm.
4. A metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell as claimed in claim 3, wherein a distance between two of said Si quadrangular pyramid stages is 70 to 100nm.
5. The metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell as claimed in any one of claims 1 to 4, wherein the material of the first reflection layer includes MgF 2 or SiO 2;
Optionally, the thickness of the first reflective layer is 40-70nm.
6. The metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell according to any one of claims 1 to 4, wherein the material of the second reflection layer includes ZnS or TiO 2;
Optionally, the thickness of the second reflective layer is 30-50nm.
7. A method of preparing a metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell as set forth in any one of claims 1 to 6, comprising:
Sequentially preparing a first reflecting layer and a second reflecting layer on the surface of the thermal photovoltaic module;
continuously preparing a Si layer on the surface of the second reflecting layer;
And coating photoresist on the surface of the Si layer, preparing a Cr layer after exposure and development, and etching to obtain the Si nano resonance microstructure layer.
8. The method of claim 7, wherein the first reflective layer and the second reflective layer are prepared by chemical deposition.
9. The method of claim 7, wherein the Cr layer has a thickness of 40-50nm.
10. A metamaterial anti-reflection film for a radioisotope thermophotovoltaic cell prepared by the preparation method of any one of claims 7 to 9, which is used for preparing a thermophotovoltaic module with efficient infrared photon absorption.
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