Intermediates and interfaces in materials and energy technologies probed by beta decayed spin spectroscopy and other physical methods

了解与环境友好的健康和能源应用有关的辐射诱发过程（辐射溶解），对于进一步发展这些应用和开发新的应用十分重要。离子液体和超临界流体在热液条件下和界面处的某些辐射分解过程尚不清楚。虽然纳米材料在放射生物学中被认为是辐射增敏剂，但人们对液体和纳米或微观结构界面的电离辐射化学知之甚少。NSERC发现基金将帮助我的团队在未来五年内填补我们对这种流体和界面的理解方面的知识空白。我们将使用最先进的泵探测方法和基于瞬态衰变的光谱技术，以及我们正在开发的基于切伦科夫辐射的新分析化学技术，在辐射和各种热力学条件下（从极冷到高温和高压条件）探测活性中间体和化学环境。我们已经开发了许多最先进的设备来连接我们研究所需的粒子束，我们将继续为本研究计划中提出的研究开发更多的设备。水和固体物质界面上的辐射效应在放射生物学中具有重要意义。同样重要的是要了解在存在腐蚀产物的反应堆冷却剂中以及在与核废料储存有关的环境中的辐射效应。所有这些都需要使用快速时间分辨方法彻底了解不同材料界面处的辐射效应。我们将提供实验数据和工具来促进这种理解。在高度非均匀的空间非平衡阶段和稍后的辐射能量沉积均匀阶段，一组可靠的实验数据可用于描述辐射的化学性质，这是至关重要的。我们将提供在亚皮秒到微秒时间尺度上产生的各种反应物质的信息。这些活性物质不仅在放射生物学和核应用中，而且在绿色化学应用中都是所需和不需要的反应的前体。我们的结果对于那些致力于为辐射过程建立可靠预测模型的团体所进行的复杂模拟来说是至关重要的。我们的研究项目很有挑战性，因为它需要多方面的调查。它包括开发新的光谱和分析方法，以探测同时在原位的恶劣辐射和热力学条件，使用外来光谱技术，在凝聚态中使用超快技术，研究寿命非常短的物种，并不断开发用于非常不同实验条件的靶容器。

An understanding of radiation-induced processes (radiolysis) relevant to environmentally friendly health- and energy-related applications is important for the further development of these applications and for the development of new applications. Certain radiolysis processes in ionic liquids and supercritical fluids under hydrothermal conditions and at the interfaces are not understood. Although nanomaterials have been proposed as radiosensitizers in radiobiology, the ionizing radiation chemistry at the interface of liquids and nano- or microstructures is poorly understood. The NSERC Discovery Grant will help my group fill knowledge gaps in our understanding of such fluids and interfaces over the next five years. We will use state-of-the-art pump probe methods and transient beta-decay-based spectroscopy techniques, along with a new analytical chemistry technique we are developing based on Cherenkov radiation, to probe reactive intermediates and the chemical environment under irradiation and under a wide range of thermodynamic conditions, from extremely cold to high temperature and pressure conditions. We have developed many state-of-the-art setups to interface the particle beams required for our studies, and we will continue to develop more for the proposed studies in this research program. Radiation effects at the interface of water and solid material are important for radiobiology. It is also important to understand the radiation effects in the coolants of a reactor in the presence of corrosion products, as well as in environments relevant to nuclear waste storage. All of these require a thorough understanding of the radiation effects at the interface of different materials using fast time resolved methods. We will provide experimental data and tools to facilitate this understanding. A reliable set of experimental data that can be used to develop descriptions of the chemical nature of radiation, both during highly nonhomogeneous spatial non-equilibrium stages and later during homogenous stages of energy deposition by radiation, is critical. We will provide information for a wide range of reactive species created on the sub-picosecond time scale to the microsecond time scale. Such reactive species are involved as precursors of wanted and unwanted reactions not only in radiobiology and nuclear applications but also in green chemistry applications. Our results are critical as inputs for complex simulations conducted by groups that are working to create reliable predictive models for radiation processes. Our research program is challenging because it requires multifaceted investigations. It includes developing new spectroscopic and analytical methods to probe simultaneous harsh radiation and thermodynamic conditions in situ, using exotic spectroscopic techniques, using ultrafast techniques in the condensed phase, investigating species that are very short-lived, and continually developing target vessels for very different experimental conditions.