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新型固体中子俘获-探测结的界面构形及界面表面膜动力学特性精确测量的研究
中文摘要

 本论文工作致力于界面构形及其应用、界面表面膜特性的相关研究,包括固体中子俘获-探测结的特定界面构形及其制备方案的研发和界面表面膜动力学相关特性的研究共两部分内容,具体为: 第一部分关于界面构形的研究工作:针对国际上均在大力发展的固体中子探测材料和器件的研究,研发适于其应用需求的新型高效的固体中子俘获-探测结的若干特定的界面构形及其制备方案,以及所研发的固体中子俘获-探测结的界面构形相关参数对中子探测效率影响关系的模拟实验研究等。该部分研究工作对应叙述于本论文的第1章和第2章。 第1章概述了中子及其基本特性、中子的产生及分类、中子源及其种类、中子与原子核的相互作用,以及中子技术的应用等有关中子探测的背景知识。 第2章详述了中子探测的基本原理与基本方法、主要技术指标及分类,中子探测器的发展趋势,固体中子探测器的发展现状;详述了间接型半导体中子探测器和直接型半导体中子探测器的工作机理,新型固体中子探测器的设计思想,间接型固体中子俘获-探测结的界面几何形貌与结构的尺度及几何参数的最优化设计,间接型固体中子俘获-探测结具有三维微观结构Si衬底的B-Si界面构形的制备方案(蚀刻法制作孔洞柱状三维结构的硅衬底和直接用多孔硅作为衬底两种方案),直接型固体中子俘获-探测结分别具有B₅C与n-Si交互叠合多层膜界面构形、三维Si-BC微观结构界面构形的制备方案,以及多个固体中子俘获-探测P-N结复合关联测量的方案;给出了所研发的中子俘获-探测结的界面构形相关参数对中子探测效率影响的模拟实验研究结果,包括点源入射和面源入射各自情况下的中子计数与俘获-探测结界面孔洞直径及孔洞间距的关系、中子计数在俘获-探测结界面不同孔间距下与孔洞直径的关系、中子计数与俘获探测结界面孔洞深度的关系、不同¹⁰B纯度的材料下中子计数与俘获-探测结界面孔洞直径的关系、中子计数与中子能量的关系、中子计数与入射角度的关系 藉此,探究和解决了中子在被俘获时的长自由程与中子被俘获后所产生的带电粒子在被探测时的短自由程的矛盾等若干关键的基础物理、材料和电子技术方面的问题,为研制新型、高效率且便于携带的性价比高的、实用的固体中子探测材料与器件奠定基础,以期解决中子探测仍基本停滞在气体探测器的技术基础上而对其发展应用有着相当局限性之问题,而中子探测及其相关技术在包括中子本身在内的基础科学研究、能源、医疗、工农业经济生产、前沿高科技以及防恐反恐、军事国防等领域的诸多方面起着愈来愈重要的关键作用。 第二部分关于界面表面膜相关特性的研究工作:基于石英晶体微天平(Quartz Crystal Microbalance,QCM)和表面等离子共振(Surface Plasmon Resonance,SPR)等技术,分别研究了QCM和SPR对固液界面吸附膜质量特异性响应的机理分析、定量探讨固液界面上孤立分子构象的简便方法、研究QCM信号对其晶体表面界面沉积的PVB薄膜的玻璃化转变行为的表征等。该部分研究工作对应叙述于本论文的第3章至第5章。 第3章详述了基于QCM和SPR技术对固液界面吸附膜质量特异性响应的机理分析,研究结果表明:SPR信号与固液界面吸附膜质量之间的正比关系缘于吸附膜折射率和浓度之间的线性关系,且吸附膜折射率的变化范围较小;QCM信号与吸附膜质量成正比的前提是吸附膜粘度和浓度之间成线性关系,且吸附膜的粘度变化较小;SPR输出信号和QCM输出信号各自对表面吸附膜质量的比值分别取决于吸附膜的折射率增量和特性粘度。 第4章详述了修正QCM的Sauerbrey方程的理论推导,得出QCM表征其晶体表面上的固-液界面特性的输出信号Δf与表面质量Δm之间的简单比例关系,分析了比例系数的物理意义;修正的Sauerbrey方程表明,Δf/Δm依赖于吸附体的特性粘度,且可依此半定量地描述固-液界面上离散吸附物的构象及构象变化。 第5章详述了藉由QCM技术对石英晶体界面聚乙烯丁醛(PVB)沉积膜的玻璃化转变行为的探究。研究结果表明:PVB薄膜在温度接近于PVB块体膜的玻璃化转变温度时,其储能模量G'迅速下降;在谐振频率的高次谐波中,玻璃化转变温度Tg没有明显变化;当PVB薄膜的厚度减小到小于0.5μm时,玻璃化转变温度Tg也随着薄膜厚度的减小而降低。 由此,探究了吸附或沉积于界面的表面膜的相关动力学特性,加深理解了表面膜的微观结构和构象变化,从而有助于表面膜的制备改良及其实际应用的拓展。 关键词:新型固体中子俘获-探测结;界面构形的最优化设计;固体中子探测效率;界面表面膜动力学性质;石英晶体微天平QCM和表面等离子体共振SPR; QCM与SPR对界面吸附膜质量的特异性响应;界面吸附膜分子构象;界面沉积PVB膜玻璃化转变

英文摘要

 The work described in this thesis is devoted to the study and the development of the specific interface configurations of solid neutron capture-detection junction and their production scheme, and the dynamic properties of the surface films at the certain interfaces. The specific contents are as follows: The first part is about the research work on interface configuration, which includes the following aspects: In view of the research on solid neutron detection materials and devices which is being developed all over the world, a number of specific interfacial configurations and their production schemes of novel and efficient neutron capture-detection junctions suitable for their application requirements have been developed. The relationship between the interfacial configuration parameters of neutron capture-detection junction and the neutron detection efficiency have been simulated.This part of the study is described in the first and second chapters of this thesis. In chapter 1. the background knowledge of neutron detection is summarized, such as neutron and its basic characteristics, neutron generation and classification, neutron source and its species, interaction between neutron and nucleus, and application of neutron technology. In chapter 2, the following are the details: The basic principles and methods of neutron detection, the main technical specifications and classification, and the development trend of neutron detectors, and the development status of solid neutron detectors are introduced. The working mechanism of indirect semiconductor neutron detector and direct semiconductor neutron detector, and the design idea of novel solid neutron detector are also described in detail. The work accomplished is as follows: 1) optimization design of the interface geometric morphology and structure and geometric parameters of indirect solid neutron capture-detection junction. 2) the production scheme for B-Si interface configuration with three-dimensional microstructure of indirect solid neutron capture-detection junctions, which is made of cylindrical columnar silicon substrate by etching method or made of porous silicon directly. 3) the production scheme for Interface configuration with B₅C and n-Si laminated multilayer films, and three-dimensional Si-BC microstructure, respectively. 4)the scheme of composite correlation measurement of multiple solid neutron capture-detection P-N junctions. The results of the simulation experiment of the relationships between the interfacial configuration parameters of neutron capture-detection junction and the neutron detection efficiency are given, which include the following: between neutron count and diameter of hole and separation between holes in the case of point source incidence and non-point source incidence respectively; between neutron count and diameter of hole in the case of different separation between holes; between neutron count and depth of hole; between neutron count and diameter of hole made of materials of different ¹⁰B purity respectively; between neutron count and neutron energy; between neutron count and incidence Angle. In this way, some key problems about basic physics, materials and electronic technology are explored and solved, such as the contradiction between the long free path of captured neutrons and the short free range of charged particles produced from the captured neutrons. It lays a foundation for the development of novel, efficient and portable solid neutron detection materials and devices with high performance to price ratio, to solve the problem that neutron detection is still basically stagnant on the basis of gas detector technology and has some limitations on its development and application. Neutron detection and related technologies in basic scientific research including on neutron itself, energy and medical treatment, industrial and agricultural and economic production, highly advanced technology, counter-terrorism, military and defense, and other fields are playing a more and more important role. The second part is about the study on the properties of the surface film based on QCM and SPR techniques, such as quality specific response of SPR and QCM to the mass of adsorbates at interfaces, molecular conformation and its variation of films adsorbed at the interface, glass transition in films deposited at the interface. This part of the study is described in chapters 3 to 5 of this thesis. In chapter 3, specific responses of SPR and QCM to the mass of adsorbates at solid-liquid interfaces are described in detail. The results show that: the proportional relation between SPR signal and adsorbed mass at solid-liquid interfaces comes from a linear relation between surface refractive index and surface concentration, under a small variation of surface refractive index, while the proportional relation between QCM signal and adsorbed mass lies in a linear relation between surface viscosity and surface concentration, and a small variation of surface viscosity. The ratio of SPR and QCM signals to the surface mass is dominated by the refractive index increment and intrinsic viscosity, respectively. In chapter 4, the theoretical derivation of the modified Sauerbrey equation of QCM is described in detail. A simple proportional relation between Af which is the output signal of QCM for characterization of Solid-Liquid Interface proterties on crystal surface and surface mass at solid-liquid interfaces has been derived. The physical meaning of the proportional coefficient has been analyzed. According to the modified Sauerbrey equation, Δf/Δm relies on the intrinsic viscosity of adsorbates. which can semi-quantitatively describe the conformation of isolated adsorbates at solid-liquid interfaces. In chapter 5, the study on Glass Transitions in PVB Films adsorbed on Quartz Crystal surface is described in detail. The results show that: rapid drops in the storage moduli of the PVB films at temperature close to that of glass transition of bulk PVB. No significant change in glass transition temperature Tg was found in high harmonics of the resonant frequency. As the film thickness decreases to below half micrometer; the glass transition temperature Tg also decreases with decreasing of the film thickness. Therefore, the dynamic properties of the surface film adsorbed or deposited at the interface are explored, and the microstructure and conformation changes of the surface film are further understood, which is helpful to the popularization and improvement of the surface film in practical application. Keywords: A Novel Solid Neutron Capture-Detection Junction; The Optimum Design of Interface Configuration; Solid Neutron Detection Efficiency; Dynamic Properties of Surface Film at Interfaces; Quartz Crystal Microbalance(QCM) and Surface Plasmon Resonance(SPR); Specific Responses of SPR and QCM to The Mass of Adsorbates at Interfaces; The Conformation of Molecules at Interfaces; Glass Transition in PVB Film Deposited at Interfaces

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