WO2023072299A1 - 一种调控金属/绝缘体界面热导的方法 - Google Patents

一种调控金属/绝缘体界面热导的方法 Download PDF

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WO2023072299A1
WO2023072299A1 PCT/CN2022/128946 CN2022128946W WO2023072299A1 WO 2023072299 A1 WO2023072299 A1 WO 2023072299A1 CN 2022128946 W CN2022128946 W CN 2022128946W WO 2023072299 A1 WO2023072299 A1 WO 2023072299A1
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metal
insulator
interface
ferroelectric
piezoelectric body
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French (fr)
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聂越峰
臧一鹏
卢明辉
颜学俊
狄琛
耿志明
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Nanjing University
Nanjing Tech University
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Nanjing Tech University
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
    • H01B3/002—Inhomogeneous material in general
    • H01B3/004—Inhomogeneous material in general with conductive additives or conductive layers
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10D—INORGANIC ELECTRIC SEMICONDUCTOR DEVICES
    • H10D64/00—Electrodes of devices having potential barriers
    • H10D64/60—Electrodes characterised by their materials
    • H10D64/66—Electrodes having a conductor capacitively coupled to a semiconductor by an insulator, e.g. MIS electrodes
    • H10D64/665—Electrodes having a conductor capacitively coupled to a semiconductor by an insulator, e.g. MIS electrodes the conductor comprising a layer of elemental metal contacting the insulator, e.g. tungsten or molybdenum
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H01B1/02—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of metals or alloys
    • H01B1/023—Alloys based on aluminium
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B13/00—Apparatus or processes specially adapted for manufacturing conductors or cables
    • H01B13/0016—Apparatus or processes specially adapted for manufacturing conductors or cables for heat treatment
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B13/00—Apparatus or processes specially adapted for manufacturing conductors or cables
    • H01B13/22—Sheathing; Armouring; Screening; Applying other protective layers
    • H01B13/222—Sheathing; Armouring; Screening; Applying other protective layers by electro-plating
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
    • H01B3/02—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of inorganic substances
    • H01B3/10—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of inorganic substances metallic oxides
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10D—INORGANIC ELECTRIC SEMICONDUCTOR DEVICES
    • H10D64/00—Electrodes of devices having potential barriers
    • H10D64/60—Electrodes characterised by their materials
    • H10D64/66—Electrodes having a conductor capacitively coupled to a semiconductor by an insulator, e.g. MIS electrodes
    • H10D64/68—Electrodes having a conductor capacitively coupled to a semiconductor by an insulator, e.g. MIS electrodes characterised by the insulator, e.g. by the gate insulator
    • H10D64/689—Electrodes having a conductor capacitively coupled to a semiconductor by an insulator, e.g. MIS electrodes characterised by the insulator, e.g. by the gate insulator having ferroelectric layers

Definitions

  • the invention belongs to the technical field of material science, and more specifically relates to a method for adjusting and controlling the thermal conductivity of a metal/insulator interface.
  • Heat dissipation is one of the main limiting factors restricting the continuous increase of chip transistor density and computing power.
  • the regulation of thermal conductivity of nanostructured materials and the dynamic regulation of thermal transport properties of functional materials are key issues in basic research and electronic device applications.
  • exotic heat transport behavior may emerge, such as materials exhibiting negligible thermal resistance and ballistic propagation of phonons.
  • the thermal resistance is mainly determined by the scattering of phonons at the boundary; thus, the conversion efficiency of thermal energy between supports at the interface becomes very important. Since electrons and phonons dominate heat conduction in metals and insulators, respectively, heat transfer must occur between them if heat is to be allowed to pass through the metal-insulator interface.
  • This electron (metal)-phonon (insulator) coupling can occur indirectly or directly.
  • electron-phonon coupling occurs on the metal side, which subsequently requires phonon coupling between the metal and the insulator, as at the junction between two insulators.
  • electron-phonon coupling occurs between free electrons in metals and phonons in insulators.
  • the control of interfacial thermal conductance is hampered by the unclear mechanism of interfacial electron-phonon coupling.
  • the present invention provides a method for regulating the thermal conductance of the metal/insulator interface; by selecting an insulator material with polarization characteristics instead of ordinary insulation The material is combined with the metal, and the polarization direction or polarization intensity of the polarized material is changed through an external electric field or stress or other methods, thereby effectively solving the problem of cumbersome and low-efficiency regulation of the thermal conductance adjustment process at the interface between the metal and the insulator in the prior art .
  • a method for regulating the thermal conductivity of a metal/insulator interface according to the present invention, the metal is arranged on the surface of the insulator, and the contact surface between the metal and the insulator is a metal/insulator interface; the insulator includes
  • Ferroelectrics Apply an external electric field or stress to ferroelectrics, and adjust the thermal conductivity of the metal/insulator interface by adjusting the magnitude of the external electric field or stress or the angle between its direction and the metal/insulator interface;
  • a piezoelectric body Apply stress to the piezoelectric body, and adjust the thermal conductivity of the metal/insulator interface by adjusting the magnitude of the stress or the angle between its direction and the metal/insulator interface;
  • pyroelectrics by adjusting the temperature of the pyroelectrics to regulate the thermal conductance of the metal/insulator interface.
  • the direction of the external electric field or stress is adjusted between a direction parallel to the metal/insulator interface and a direction perpendicular to the metal/insulator interface.
  • ferroelectrics it includes PbTiO 3 , BiFeO 3 , BaTiO 3 , LiNbO 3 , PbZr x Ti 1-x O 3 , [(PbMg 0.33 Nb 0.67 O 3 ) 1-x :(PbTiO 3 ) x ] One or a combination of several; where x ⁇ (0,1).
  • the specific operation steps are:
  • an out-of-plane electric field or an in-plane electric field at the metal/ferroelectric interface is applied so that the polarization direction of the ferroelectric is perpendicular to the direction of the metal/ferroelectric interface or parallel to the direction of the metal/ferroelectric The direction of the electrical interface;
  • a metal/piezoelectric body/adhesive layer/flexible substrate composite structure is prepared, applying stress to the flexible substrate drives the metal/piezoelectric body structure to deform, and adjusting the interface thermal conductivity by adjusting the magnitude of the applied stress .
  • the metal/piezoelectric body/adhesive layer/flexible substrate composite structure is a film structure.
  • the preparation steps of the metal/piezoelectric body/adhesive layer/flexible substrate composite structure are:
  • the material of the adhesive layer includes epoxy resin, and the heating and curing conditions are 80°C to 100°C for 0.5h to 1.5h; the material of the water-soluble layer includes Sr 3 Al 2 O 6 , and the removal method is Soak in deionized water for 48h to 72h.
  • the plating method of the metal layer includes a vacuum evaporation method, a magnetron sputtering method or a chemical vapor deposition method.
  • the metal includes Al or Au, and its thickness is 60nm ⁇ 120nm.
  • an ordinary insulator is provided on the other side of the insulator opposite to the metal to obtain a three-layer structure of metal/insulator/ordinary insulator; Corresponding methods regulate the thermal conductance at the metal/insulator interface.
  • the insulator thickness of the intermediate layer is preferably 2 nm to 10 nm.
  • the ordinary insulator mentioned in the present invention refers to an insulator that does not have spontaneous polarization, and the relative movement of internal positive and negative charges hardly occurs under external conditions, and belongs to ferroelectrics, piezoelectrics and pyroelectrics. Insulators, therefore do not have ferroelectricity, piezoelectricity and pyroelectricity.
  • the above definition of the common insulator is for the three-layer structure of metal/insulator/common insulator, which is used to facilitate the heat conduction between the common insulator and the metal; The other side of the insulator opposite to the metal can only be provided with an ordinary insulator, and this position can still be provided with metal or the insulator or other materials described in the present invention.
  • An application of the present invention can selectively open or close the heat transport channel of the interface by regulating the polarization direction of the ferroelectric, and can be applied to thermal logic devices.
  • a kind of method of regulating and controlling metal/insulator interface heat conduction of the present invention metal is arranged on insulator surface, and the contact surface of described metal and insulator is metal/insulator interface; Described insulator comprises ferroelectric; The external electric field or stress is applied to the body, and the thermal conductivity of the metal/insulator interface is regulated by adjusting the magnitude of the external electric field or stress or the angle between its direction and the metal/insulator interface; or a piezoelectric body; applying stress to the piezoelectric body, by Adjust the magnitude of the stress or the angle between its direction and the metal/insulator interface to regulate the thermal conductivity of the metal/insulator interface; or pyroelectrics; adjust the thermal conductivity of the metal/insulator interface by adjusting the temperature of the pyroelectrics.
  • ferroelectrics since they have spontaneous polarization, and the polarization intensity can be reversed with the direction of the external electric field, the original polarization direction or polarization of the ferroelectric can be changed after the external electric field is applied. Intensity, while for the metal/ferroelectric structure, when the external electric field is applied so that the polarization direction of the ferroelectric is perpendicular to or tends to be perpendicular to the metal/ferroelectric interface, the charges in the ferroelectric will accumulate at the interface.
  • the coupling of metal electrons and insulator phonons at the interface will be promoted, thereby improving the interface thermal conductivity; on the contrary, when an external electric field is applied, the polarization direction of the ferroelectric is parallel or tends to be parallel to the metal/ferroelectric At the bulk interface, the charge accumulated at the interface disappears, so the coupling effect of metal electrons and insulator phonons at the interface decreases, and the thermal conductivity decreases. Therefore, the metal can be regulated by adjusting the direction of the external electric field and the angle between the metal/insulator interface. /insulator interface thermal conductivity; and the principle of adjusting the magnitude of the external electric field is similar.
  • the spontaneous polarization direction of the ferroelectric When the spontaneous polarization direction of the ferroelectric is adjusted, there is a certain angle between the metal/insulator interface, and the magnitude of the electric field strength or stress can also be adjusted.
  • the degree of charge accumulation at the interface regulates the thermal conductance.
  • the piezoelectric body due to the deformation energy generated under the pressure state, the positive and negative charge centers in the interior no longer overlap, thereby changing the degree of charge accumulation at the interface, and then adjusting the thermal conductivity.
  • the degree of charge accumulation at the interface For pyroelectrics, due to the corresponding changes in spontaneous polarization intensity under different temperature conditions, the degree of charge accumulation at the interface can be changed, thereby adjusting the thermal conductivity.
  • the principle of the present invention is similar to the regulation of the thermal conductivity of ferroelectrics, piezoelectrics or pyroelectrics and metal interfaces, by adjusting the degree of accumulated charge at the metal/insulator interface to regulate the thermal conductivity of the metal/insulator interface. Therefore, the present invention changes the traditional complex control method, and creatively proposes that the thermal conductance of the metal/insulator interface can be regulated by regulating the accumulated charge at the interface, thereby effectively improving the control efficiency and convenience of the thermal conductance of the interface. Management matters.
  • a kind of method of regulating and controlling metal/insulator interface heat conduction of the present invention it is on the structural foundation of metal/insulator, on described insulator again, be provided with common insulator on the other side of insulator opposite with metal, obtain metal
  • the present invention can regulate the thermal conductivity of the interface by adjusting the degree of accumulation of charges at the metal/insulator interface, through the above method, the thermal conductivity of the three-layer structure can be further adjusted under the action of the insulator in the intermediate layer, which is the difference between ordinary insulators and metals. The heat conduction between them provides convenience.
  • Fig. 1 is a sample structural diagram of metal/piezoelectric body/bonding layer/flexible substrate composite structure of the present invention
  • Fig. 2 is the physical figure of the tensile displacement platform of the present invention
  • Fig. 3 is a metal/ferroelectric sample of the present invention (the ferroelectric polarization direction on the left is perpendicular to the upper surface, and the ferroelectric polarization direction on the right is parallel to the upper surface);
  • Fig. 4 is a schematic diagram of the variation of the thermal resistance of the Al/BFO interface caused by the ferroelectric polarization reversal under the action of stress control in Example 1;
  • Fig. 5 is the XRD figure of BFO film in embodiment 1 under the uniaxial tensile stress along [100] direction;
  • Fig. 6 is a schematic diagram of the variation of Al/ LiNbO3 interface and LiNbO3 crystal thermal conduction in Example 2 under different polarization states (the direction of the arrow is represented as the polarization direction of LiNbO3 );
  • This embodiment provides a method for regulating the thermal conductance of the metal/insulator interface, specifically a method for regulating the thermal conductance of the interface of a metal aluminum/bismuth ferrite (BFO) sample under polarization evolution. Since the ferroelectric BFO itself also has Piezoelectricity, so in this embodiment, it is operated as a piezoelectric body, and stress is applied to it and the thermal conductivity of the metal/insulator interface is regulated by adjusting the magnitude of the stress.
  • the specific operation steps are:
  • the ferroelectric film BFO was separated from the substrate STO to obtain a sample with a BFO/Epoxy/PEN structure.
  • a metal Al layer with a thickness of 80 nm was coated on the surface of BFO by magnetron sputtering to obtain the Al/BFO/Epoxy/PEN sample shown in Figure 1.
  • the metal/piezoelectric body/adhesive layer/flexible substrate composite The construction of the structural sample is completed.
  • the specific adjustment method is: as shown in Figure 2, glue the two ends of the sample to the cantilever of the translation stage firmly, the original distance between the cantilever is L 0 , the position of the translation platform can be adjusted and the cantilever can be enlarged by the screw
  • the distance extension is ⁇ L
  • the extension rate of the cantilever distance is ⁇ L/L 0
  • the extension rate of the cantilever can be defined as the nominal stress applied on the sample
  • the actual stress can be measured by X-ray diffractometer The resulting lattice changes are obtained.
  • This embodiment provides a method for regulating the thermal conductivity of the metal/insulator interface, specifically the thermal conductivity of metal aluminum/lithium niobate (LiNbO 3 ) samples under different polarization conditions.
  • the specific operation steps are:
  • a metal layer of about 80nm is vapor-deposited on the surface of the LiNbO 3 crystal by magnetron sputtering to construct a metal/ferroelectric (Al/LiNbO 3 ) structure.
  • the polarization direction of the ferroelectric is perpendicular to the metal/ferroelectric interface, such as the left side of Figure 3, and by applying a transverse electric field parallel to the interface, the polarization direction is changed from perpendicular to the interface to parallel to the interface, such as the right side of Figure 3 , thus obtaining two states where the polarization directions are perpendicular to the direction of the upper surface and parallel to the direction of the upper surface, respectively.
  • This example provides a method for regulating the thermal conductivity of the metal/insulator interface, specifically the heat transport properties of metal gold/lithium niobate (LiNbO 3 ) samples under different polarization conditions, and the specific operation steps are basically the same as those in Example 2. , the main difference is that the metal Al is replaced by Au.
  • This embodiment provides a method for regulating the thermal conductivity of the metal/insulator interface, specifically the thermal conductivity of metal aluminum/zinc oxide (ZnO) samples under different polarization conditions.
  • the specific operation steps are basically the same as in Example 2, the main difference is :
  • the insulator lithium niobate was replaced with zinc oxide; in addition, the polarization intensity of zinc oxide was regulated by changing the temperature conditions.
  • This embodiment provides a method for regulating the thermal conductivity of the metal/insulator interface, specifically the thermal conductivity of metal aluminum/BFO/STO samples under different polarization conditions.
  • the specific operation steps are basically the same as in Example 1, the main difference is:
  • the other side of the BFO opposite to the metal aluminum is provided with a common insulator STO; the thickness of the BFO layer is 5nm.
  • This comparative example provides a method for regulating the thermal conductance of the metal/insulator interface, specifically the thermal conductance of the metal aluminum/ SrTiO3 sample under different polarization conditions.
  • the specific operation steps are basically the same as in Example 2, the main difference is that:
  • the insulator lithium niobate is the common insulator SrTiO 3 .
  • a range of 1-50 should be understood to include the group selected from the group consisting of , 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44 , 45, 46, 47, 48, 49, or 50, any number, combination of numbers, or subrange, and all fractional values between the above integers, for example, 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8 and 1.9.
  • “nested subranges” that extend from any endpoint within the range are specifically considered.
  • a nested subrange of the exemplary range 1-50 could include 1-10, 1-20, 1-30, and 1-40 in one direction, or 50-40, 50-30, 50 in the other direction -20 and 50-10.

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Abstract

本发明公开了一种调控金属/绝缘体界面热导的方法，属于材料科学技术领域。它包括将金属设置于绝缘体表面，所述金属与绝缘体的接触面为金属/绝缘体界面；所述绝缘体包括铁电体、压电体或热释电体。本发明能通过调控界面聚集电荷调控金属/绝缘体界面热导，从而有效提升界面热导的调控效率和便捷度，这对于电力电子器件的热管理具有重要意义。

Description

一种调控金属/绝缘体界面热导的方法
本申请要求于2021年11月01日提交中国专利局、申请号为CN202111282552.2、发明名称为“一种调控金属/绝缘体界面热导的方法”的中国专利申请的优先权，其全部内容通过引用结合在本申请中。
技术领域
本发明属于材料科学技术领域，更具体地说，涉及一种调控金属/绝缘体界面热导的方法。
背景技术
热耗散是制约芯片晶体管密度与计算能力继续上升的主要限制因素之一，纳米结构材料的热导调控和功能材料热输运性能的动态调节是基础研究和电子器件应用中的关键问题。随着电子器件的不断小型化，奇特的热输运行为可能会出现，如材料表现出可忽略的热阻和声子的弹道传播。在纳米尺度下，热阻主要由声子在边界处的散射决定；因此，界面处热能在载体之间的转换效率变得非常重要。由于电子和声子分别在金属和绝缘体的热传导中占主导地位，若想允许热通过金属-绝缘体界面，则热量传递必须在它们之间发生。这种电子(金属)-声子(绝缘体)耦合可以间接或直接发生。在间接的情况下，电子-声子耦合发生在金属侧，随后需要在金属和绝缘体之间发生声子耦合，就像在两个绝缘体之间的连接处一样。在直接的情况下，电子-声子耦合发生在金属中的自由电子和绝缘体中的声子之间。然而，由于界面电子-声子耦合的机理不明确，因而阻碍了界面热导的调控。
近年来，材料热输运性质的调控受到了广泛关注，目前已形成了多种热导调控的方法，包括化学元素掺杂、超晶格构筑、晶体结构优化、铁电晶体的畴壁或晶界密度控制。对于材料界面热导的调控而言，通过化学键合改性调节界面热输运、表面粗糙度工程或插入缓冲层改善界面热导已得到广泛应用。金属/绝缘体界面是现代电子器件中的常见界面结构，在诸如薄膜纳米电容器、纳米铁电存储器和铁电隧道结等新型电子器件中有大量的金属/绝缘体界面。因此，开发有效调节金属/绝缘体界面热阻的新策略是迫切需要的。金属中传导热能的主要载体为热化电子，而在绝缘铁电体中则为声子。
因此，如何提高金属/绝缘体界面的电子-声子耦合以提升界面热输运效率是 亟待解决的重要科学技术问题，这一问题的解决将为技术的推广应用奠定坚实基础。目前亟需设计一种能够简便有效调节金属和绝缘体界面热导的方法，从而运用于电子电子器件的设计与应用当中。
发明内容
1.要解决的问题
针对现有技术中调控金属和绝缘体界面热导调节工艺繁琐且效率较低的问题，本发明提供一种调控金属/绝缘体界面热导的方法；通过选取具有极化特性的绝缘体材料代替普通绝缘性材料与金属进行结合，通过外界电场或应力或其他方式改变极化材料的极化方向或极化强度，从而有效解决现有技术中调控金属和绝缘体界面热导调节工艺繁琐且效率较低的问题。
2.技术方案
为了解决上述问题，本发明所采用的技术方案如下：
本发明的一种调控金属/绝缘体界面热导的方法，将金属设置于绝缘体表面，所述金属与绝缘体的接触面为金属/绝缘体界面；所述绝缘体包括
铁电体；对铁电体施加外电场或应力，通过调节外电场或应力的大小或其方向与金属/绝缘体界面之间的夹角来调控金属/绝缘体界面热导；
或压电体；对压电体施加应力，通过调节应力的大小或其方向与金属/绝缘体界面之间的夹角来调控金属/绝缘体界面热导；
或热释电体；通过调节热释电体的温度来调控金属/绝缘体界面热导。
优选地，所述外电场或应力的方向在平行于金属/绝缘体界面方向和垂直于金属/绝缘体界面方向之间进行调节。
需要说明的是，对于调节应力大小的方式调节界面热导而言，需要满足铁电体自发极化的方向与金属/绝缘体界面之间的夹角不等于零，因为在等于零的情况下仅调节应力大小可能会使电荷在绝缘体两端聚集，无法实电荷聚集在界面处，因此在不等于零时即使单独调节应力大小也能调节界面的电荷聚集程度，进而调节热导。
优选地，对于铁电体，其包括PbTiO 3、BiFeO 3、BaTiO 3、LiNbO 3、PbZr xTi 1-xO 3、[(PbMg 0.33Nb 0.67O 3) 1-x:(PbTiO 3) x]中的一种或几种的组合；其中x∈(0，1)。
优选地，具体操作步骤为：
(1)选取铁电体材料作为绝缘体材料，在铁电体表面镀覆金属层形成金属/ 铁电体结构；
(2)在金属/铁电体结构中，施加金属/铁电体界面的面外电场或面内电场，使得铁电体极化方向垂直于金属/铁电体界面方向或者平行于金属/铁电体界面方向；
(3)采用时域热反射系统(TDTR)测量金属/铁电体结构的界面热导。
优选地，对于压电体，制备金属/压电体/粘结层/柔性基底复合结构，对柔性基底施加应力带动金属/压电体结构产生形变，通过调节施加应力的大小来调节界面热导。
优选地，所述金属/压电体/粘结层/柔性基底复合结构为薄膜结构。
优选地，所述金属/压电体/粘结层/柔性基底复合结构的制备步骤为：
(1)在压电体/水溶层/衬底复合薄膜表面涂覆粘结层，得到粘结层/压电体/水溶层/衬底复合薄膜，将得到的复合薄膜带有粘结层的一面倒扣在柔性基底上，加热固化；
(2)将固化后的复合薄膜中的水溶层溶解去除，使得压电体与衬底分离，得到压电体/粘结层/柔性基底复合薄膜；
(3)在压电体/粘结层/柔性基底复合薄膜的铁电体表面镀覆金属，得到金属/压电体/粘结层/柔性基底复合结构。
优选地，所述粘结层的材料包括环氧树脂，加热固化的条件为80℃～100℃加热0.5h～1.5h；所述水溶层的材料包括Sr 3Al 2O 6，去除方式是在去离子水中浸泡48h～72h。
优选地，所述金属层的镀覆方式包括真空蒸镀法或磁控溅射法或化学气相沉积法。
优选地，所述金属包括Al或Au，其厚度为60nm～120nm。
优选地，在所述绝缘体上，与金属相对的绝缘体另一面设有普通绝缘体，得到金属/绝缘体/普通绝缘体的三层结构；根据中间层的绝缘体种类，对所述三层结构作与绝缘体种类相应的方法调控金属/绝缘体界面热导。所述中间层的绝缘体厚度优选为2nm～10nm。
本发明中所述的普通绝缘体是指不存在自发极化、且在外在条件下几乎不会发生内在正负电荷相对移动的绝缘体，属于除铁电体、压电体和热释电体之外的绝缘体，因此也不具备铁电性、压电性和热释电性。需要说明的是，以上 对所述的普通绝缘体的限定是针对金属/绝缘体/普通绝缘体的三层结构而言的，用处在于为普通绝缘体和金属之间的热传导提供便利；而并非是指在与金属相对的绝缘体另一面只能设置普通绝缘体，该位置依然可以设有金属或本发明中所述的绝缘体或其他材料。
本发明的一种应用，通过调控铁电体的极化方向，可以选择性打开或者关闭界面的热输运通道，可应用于热逻辑器件当中。
3.有益效果
相比于现有技术，本发明的有益效果为：
(1)本发明的一种调控金属/绝缘体界面热导的方法，将金属设置于绝缘体表面，所述金属与绝缘体的接触面为金属/绝缘体界面；所述绝缘体包括铁电体；对铁电体施加外电场或应力，通过调节外电场或应力的大小或其方向与金属/绝缘体界面之间的夹角来调控金属/绝缘体界面热导；或压电体；对压电体施加应力，通过调节应力的大小或其方向与金属/绝缘体界面之间的夹角来调控金属/绝缘体界面热导；或热释电体；通过调节热释电体的温度来调控金属/绝缘体界面热导。通过上述方法，对于铁电体而言，由于其具有自发极化，而且极化强度可以随外电场的方向而反向，因此施加外电场后可以改变铁电体原本的极化方向或极化强度，而对于金属/铁电体结构，当施加外电场后使得铁电体的极化方向垂直于或倾向于垂直金属/铁电体界面时，铁电体中的电荷会在界面聚集，此时由于聚集电荷的存在会促进界面处的金属电子和绝缘体声子耦合，从而提高界面热导；相反地，当施加外电场使得铁电体的极化方向平行于或倾向于平行金属/铁电体界面时，界面聚集的电荷消失，因此界面处的金属电子和绝缘体声子的耦合作用降低，热导下降，因此能够通过调节外电场的方向与金属/绝缘体界面之间的夹角来调控金属/绝缘体界面热导；而调节外电场强度的大小原理类似，当铁电体的自发极化方向，通过调节与金属/绝缘体界面之间存在一定夹角，调节电场强度大小或应力大小也能调节界面的电荷聚集程度，进而调节热导。对于压电体而言，由于其在压力状态下产生形变能使其内部正负电荷中心不再重合，从而改变电荷在界面的聚集程度，进而调节热导。对于热释电体而言，由于其在不同的温度条件下能够产生自发极化强度的相应变化，从而改变电荷在界面的聚集程度，进而调节热导。综上，本发明对于铁电体、压电体或热释电体与金属界面热导调控的原理类似，通过相应的调节方式来调控金属/ 绝缘体界面的聚集电荷程度来调控金属/绝缘体界面热导，因此本发明一改传统的复杂调控方法，创造性地提出通过调控界面聚集电荷可以调控金属/绝缘体界面热导，从而有效提升界面热导的调控效率和便捷度，这对于电力电子器件的热管理具有重要意义。
(2)本发明的一种调控金属/绝缘体界面热导的方法，其在金属/绝缘体的结构基础之上，再在所述绝缘体上，与金属相对的绝缘体另一面设有普通绝缘体，得到金属/绝缘体/普通绝缘体的三层结构；根据中间层的绝缘体种类，对所述三层结构作与绝缘体种类相应的方法调控金属/绝缘体界面热导。由于本发明能够通过调节金属/绝缘体界面电荷的聚集程度来调控界面热导，因此通过上述方法，在中间层的绝缘体作用下能够进一步调节所述三层结构的热导，为普通绝缘体和金属之间的热传导提供了便利。
附图说明
图1是本发明的金属/压电体/粘结层/柔性基底复合结构样品结构图；
图2是本发明的拉伸位移台实物图；
图3是本发明的金属/铁电体样品(左边的铁电体极化方向垂直于上表面，右边的铁电体极化方向平行于上表面)；
图4是实施例1在应力调控作用下铁电体极化翻转引起的Al/BFO界面热阻变化示意图；
图5是实施例1中BFO薄膜在沿着[100]方向单轴拉伸应力下的XRD图；
图6是实施例2在不同极化状态下，Al/LiNbO 3界面及LiNbO 3晶体热导变化示意图(箭头方向表示为LiNbO 3的极化方向)；
图中：1、金属；2、压电体，3、粘结层；4、柔性基底；5、拉伸位移台；6、悬臂；7、螺杆；8、柔性基底；9、待测样品；10、金属；11、极化方向垂直于上表面的铁电体单晶；12、金属；13、极化方向平行于上表面的铁电体单晶。
具体实施方式
下文对本发明的示例性实施例的详细描述参考了附图，该附图形成描述的一部分，在该附图中作为示例示出了本发明可实施的示例性实施例，其中本发明的特征由附图标记标识。下文对本发明的实施例的更详细的描述并不用于限制所要求的本发明的范围，而仅仅为了进行举例说明且不限制对本发明的特点 和特征的描述，以提出执行本发明的最佳方式，并足以使得本领域技术人员能够实施本发明。但是，应当理解，可在不脱离由所附权利要求限定的本发明的范围的情况下进行各种修改和变型。详细的描述和附图应仅被认为是说明性的，而不是限制性的，如果存在任何这样的修改和变型，那么它们都将落入在此描述的本发明的范围内。此外，背景技术旨在为了说明本技术的研发现状和意义，并不旨在限制本发明或本申请和本发明的应用领域。
除非另有定义，本文所使用的所有的技术和科学术语与属于本发明的技术领域的技术人员通常理解的含义相同；本文中在本发明的说明书中所使用的术语只是为了描述具体的实施例的目的，不是旨在于限制本发明。
下面结合具体实施例对本发明进一步进行描述。
实施例1
本实施例提供一种调控金属/绝缘体界面热导的方法，具体为一种金属铝/铁酸铋(BFO)样品在极化演变下的界面热导调控方法，由于铁电体BFO本身也具备压电性，因此在本实施例中作为压电体操作，对其施加应力并通过调节应力大小的方式来调控金属/绝缘体界面热导，具体操作步骤为：
(1)准备工作：将表面旋涂有环氧树脂(Epoxy)的BiFeO 3/Sr 3Al 2O 6/SrTiO 3(BFO/SAO/STO)薄膜倒扣在柔性基底(PEN)上，在100℃条件下加热1小时使得环氧树脂固化，环氧树脂的作用是为了将铁电体薄膜与柔性基底牢牢的粘在一起，便于通过机械拉伸柔性基底以实现铁电体薄膜极化方向的调控，因此加热固化后铁电体薄膜与柔性基底紧紧贴合。将固化后的样品放入洁净的去离子水中浸泡48小时，待水溶层SAO完全溶解后，铁电体薄膜BFO与衬底STO分离，获得BFO/Epoxy/PEN结构的样品。运用磁控溅射法在BFO表面镀一层80nm厚的金属Al层，获得如图1所示的Al/BFO/Epoxy/PEN样品，此时金属/压电体/粘结层/柔性基底复合结构样品构筑完成。
(2)实验进行：通过旋动螺杆扩大悬臂的距离给薄膜样品施加应力，通过X射线衍射(XRD)系统和压电力显微镜(PFM)系统获得铁电样品的极化状态变化，通过TDTR系统测量不同应力下Al/BFO样品界面热导的变化。具体的调节的方式为：如图2所示，将样品的两端用胶牢牢粘在位移台的悬臂上，悬臂之间原始距离为L 0，通过螺杆可以调节位移台的位置并扩大悬臂之间的距离，当距离的延长量为ΔL时，则悬臂距离的延长率为ΔL/L 0，悬臂的延长率可定义为 施加在样品上的名义应力，实际应力可通过X射线衍射仪测得的晶格变化获得。
(3)结论分析：分析XRD和TDTR测得的数据，其中XRD数据如图5所示，在应力作用下(002)面、(011)面和(101)面的衍射峰位变化，薄膜产生的最大拉伸应力为3.5％。最终得出应力变化导致铁电薄膜的极化方向由垂直于Al/BFO界面转向平行与Al/BFO界面，极化偏转导致界面聚集电荷减少，从而导致界面热导下降。本实施例的检测结果如图4所示，这是由于一开始施加平行于界面的横向应力，可使得极化方向由平行于界面方向转向垂直于界面方向，铁电极化在应变作用下可使得界面聚集电荷增多，金属/压电体界面上的电子-声子耦合作用增强，从而增加界面的热导；而继续增大名义应力时，可使得极化方向由垂直于界面方向转向平行于界面方向，铁电极化在应变作用下的偏转可使得界面聚集电荷减少，金属/压电体界面上的电子-声子耦合作用减弱，从而降低界面的热导。
实施例2
本实施例提供一种调控金属/绝缘体界面热导的方法，具体为金属铝/铌酸锂(LiNbO 3)样品在不同极化条件下的热导，具体操作步骤为：
(1)准备工作：运用磁控溅射方法在LiNbO 3晶体表面蒸镀80nm左右的Al金属层，构筑金属/铁电体(Al/LiNbO 3)结构。通过施加纵向电场使得铁电体极化方向垂直于金属/铁电体界面，例如图3左，另外施加平行于界面的横向电场使得极化方向由垂直于界面转向平行于界面，例如图3右，因此获得两个极化方向分别垂直于上表面方向和平行于上表面方向的状态。
(2)实验进行：通过TDTR系统测量不同极化方向条件下Al/LiNbO 3样品热输运性质的变化。
(3)结论分析：分析TDTR测得的数据，得出极化方向垂直于上表面时的界面热导要大于极化方向平行于上表面时的界面热导，极化方向改变导致界面聚集电荷减少，从而导致界面热导下降。这是由于当铁电性材料的极化方向垂直于金属/铁电体界面时，由于界面聚集电荷的存在，会促进金属电子与绝缘体声子的耦合，从而导致提高界面热导；当铁电性材料的极化方向平行于界面时，界面聚集电荷消失，电子-声子耦合作用减弱，界面热导下降。
实施例3
本实施例提供一种调控金属/绝缘体界面热导的方法，具体为金属金/铌酸锂 (LiNbO 3)样品在不同极化条件下的热输运性质，具体操作步骤与实施例2基本相同，主要区别在于：更换了金属Al为Au。
分析TDTR最终测得的数据，得出测得的热输运变化趋势与实施例2中Al/LiNbO 3界面的热导变化趋势类似，极化方向垂直于上表面时的界面热导要大于极化方向平行于上表面时的界面热导，极化方向的改变导致热导产生变化。
实施例4
本实施例提供一种调控金属/绝缘体界面热导的方法，具体为金属铝/氧化锌(ZnO)样品在不同极化条件下的热导，具体操作步骤与实施例2基本相同，主要区别在于：
更换了绝缘体铌酸锂为氧化锌；另外通过改变温度条件来调控氧化锌的极化强度。
分析TDTR最终测得的数据，得出测得的热导变化趋势与实施例2中Al/LiNbO 3界面的热导变化趋势类似，极化强度的改变导致热导产生变化。
实施例5
本实施例提供一种调控金属/绝缘体界面热导的方法，具体为金属铝/BFO/STO样品在不同极化条件下的热导，具体操作步骤与实施例1基本相同，主要区别在于：在与金属铝相对的BFO另一面设有普通绝缘体STO；其中BFO层的厚度为5nm。
分析TDTR最终测得的数据，得出测得的Al/BFO界面热导变化趋势与实施例1中的热导变化趋势类似，应力的变化导致热导产生变化，并且在此基础之上使得金属铝和普通绝缘体STO之间也有着类似的热导变化趋势，产生了有效的热传导。
对比例1
本对比例提供一种调控金属/绝缘体界面热导的方法，具体为金属铝/SrTiO 3样品在不同极化条件下的热导，具体操作步骤与实施例2基本相同，主要区别在于：更换了绝缘体铌酸锂为普通绝缘体SrTiO 3。
分析TDTR最终测得的数据，得出测得的热导率变化趋势与实施例2中LiNbO 3晶体热导率的变化趋势类似，即使改变外加电场也几乎无法调控界面热导。
在上文中结合具体的示例性实施例详细描述了本发明。但是，应当理解， 可在不脱离由所附权利要求限定的本发明的范围的情况下进行各种修改和变型。详细的描述和附图应仅被认为是说明性的，而不是限制性的，如果存在任何这样的修改和变型，那么它们都将落入在此描述的本发明的范围内。此外，背景技术旨在为了说明本技术的研发现状和意义，并不旨在限制本发明或本申请和本发明的应用领域。
更具体地，尽管在此已经描述了本发明的示例性实施例，但是本发明并不局限于这些实施例，而是包括本领域技术人员根据前面的详细描述可认识到的经过修改、省略、例如各个实施例之间的组合、适应性改变和/或替换的任何和全部实施例。权利要求中的限定可根据权利要求中使用的语言而进行广泛的解释，且不限于在前述详细描述中或在实施该申请期间描述的示例，这些示例应被认为是非排他性的。在任何方法或过程权利要求中列举的任何步骤可以以任何顺序执行并且不限于权利要求中提出的顺序。因此，本发明的范围应当仅由所附权利要求及其合法等同物来确定，而不是由上文给出的说明和示例来确定。
除非另有限定，本文使用的所有技术以及科学术语具有与本发明所属领域普通技术人员通常理解的相同的含义。当存在矛盾时，以本说明书中的定义为准。厚度、温度、时间、或者其它值或参数以范围、优选范围、或一系列上限优选值和下限优选值限定的范围表示时，这应当被理解为具体公开了由任何范围上限或优选值与任何范围下限或优选值的任一配对所形成的所有范围，而不论该范围是否单独公开了。例如，1-50的范围应理解为包括选自1、2、3、4、5、6、7、8、9、10、11、12、13、14、15、16、17、18、19、20、21、22、23、24、25、26、27、28、29、30、31、32、33、34、35、36、37、38、39、40、41、42、43、44、45、46、47、48、49或50的任何数字、数字的组合、或子范围、以及所有介于上述整数之间的小数值，例如，1.1、1.2、1.3、1.4、1.5、1.6、1.7、1.8和1.9。关于子范围，具体考虑从范围内的任意端点开始延伸的“嵌套的子范围”。例如，示例性范围1-50的嵌套子范围可以包括一个方向上的1-10、1-20、1-30和1-40，或在另一方向上的50-40、50-30、50-20和50-10。

Claims (18)

  1. 一种调控金属/绝缘体界面热导的方法，其特征在于，将金属设置于绝缘体表面，所述金属与绝缘体的接触面为金属/绝缘体界面；
    所述绝缘体包括铁电体、压电体或热释电体；
    当所述绝缘体为铁电体时，对铁电体施加外电场或应力，通过调节外电场或应力的大小或其方向与金属/绝缘体界面之间的夹角来调控金属/绝缘体界面热导；
    当所述绝缘体为压电体时，对压电体施加应力，通过调节应力的大小或其方向与金属/绝缘体界面之间的夹角来调控金属/绝缘体界面热导；
    当所述绝缘体为热释电体时，通过调节热释电体的温度来调控金属/绝缘体界面热导。
  2. 根据权利要求1所述的方法，其特征在于，所述铁电体包括PbTiO 3、BiFeO 3、BaTiO 3、LiNbO 3、PbZr xTi 1-xO 3、[(PbMg 0.33Nb 0.67O 3) 1-x:(PbTiO 3) x]中的一种或几种的组合；
    所述x∈(0，1)。
  3. 根据权利要求1所述的方法，其特征在于，当所述绝缘体为铁电体时，所述外电场或应力的方向在平行于金属/绝缘体界面方向和垂直于金属/绝缘体界面方向之间进行调节。
  4. 根据权利要求1所述的方法，其特征在于，当所述绝缘体为铁电体、通过调节所述压力大小调控界面热导时，所述铁电体自发极化的方向与金属/绝缘体界面之间的夹角不等于零。
  5. 根据权利要求1所述的方法，其特征在于，当所述绝缘体为铁电体时，所述调控的具体操作步骤为：
    (1)选取铁电体材料作为绝缘体材料，在铁电体表面镀覆金属层形成金属/铁电体结构；
    (2)在金属/铁电体结构中，施加金属/铁电体界面的面外电场或面内电场，使得铁电体极化方向垂直于金属/铁电体界面方向或者平行于金属/铁电体界面方向；
    (3)采用TDTR测量金属/铁电体结构的界面热导。
  6. 根据权利要求1所述的方法，其特征在于，当所述绝缘体为压电体时，所述调控具体为：
    制备金属/压电体/粘结层/柔性基底复合结构，对柔性基底施加应力带动金属/压电体结构产生形变，通过调节施加应力的大小来调节界面热导。
  7. 根据权利要求6所述的方法，其特征在于，所述金属/压电体/粘结层/柔性基底复合结构为薄膜结构。
  8. 根据权利要求7所述的方法，其特征在于，所述金属/压电体/粘结层/柔性基底复合结构的制备步骤为：
    (1)在压电体/水溶层/衬底复合薄膜表面涂覆粘结层，得到粘结层/压电体/水溶层/衬底复合薄膜，将得到的复合薄膜带有粘结层的一面倒扣在柔性基底上，加热固化；
    (2)将固化后的复合薄膜中的水溶层溶解去除，使得压电体与衬底分离，得到压电体/粘结层/柔性基底复合薄膜；
    (3)在压电体/粘结层/柔性基底复合薄膜的压电体表面镀覆金属，得到金属/压电体/粘结层/柔性基底复合结构。
  9. 根据权利要求8所述的方法，其特征在于，所述粘结层的材料包括环氧树脂；
    所述加热固化的条件为：在80℃～100℃加热0.5h～1.5h。
  10. 根据权利要求8所述的方法，其特征在于，所述水溶层的材料包括Sr 3Al 2O 6；
    所述溶解去除为：在去离子水中浸泡48h～72h。
  11. 根据权利要求5或8所述的方法，其特征在于，所述金属层的镀覆的方式包括真空蒸镀法、磁控溅射法或化学气相沉积法。
  12. 根据权利要求1～10任一项所述的方法，其特征在于，所述金属包括Al或Au；
    所述金属的厚度为60nm～120nm。
  13. 根据权利要求1所述的方法，其特征在于，还包括在所述绝缘体上，与金属相对的绝缘体另一面设有普通绝缘体，得到金属/绝缘体/普通绝缘体的三层结构；根据中间层的绝缘体种类，对所述三层结构作与绝缘体种类相应的方法调控金属/绝缘体界面热导。
  14. 根据权利要求13所述的方法，其特征在于，所述普通绝缘体包括SrTiO 3。
  15. 根据权利要求13或14所述的方法，其特征在于，所述中间层的绝缘体厚度为2nm～10nm。
  16. 权利要求1～15任一项所述的方法在电力电子器件热管理中的应用。
  17. 根据权利要求16所述的应用，其特征在于，当所述绝缘体为铁电体时，所述电力电子器件包括热逻辑器件。
  18. 根据权利要求17所述的应用，其特征在于，当所述电力电子器件为热逻辑器件时，所述热管理的方法为：
    通过调控铁电体的极化方向，选择性打开或关闭金属/铁电体界面的热输送通道。
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