Exploration of non-equilibrium phenomena at a reactive surface induced by a plasma

等离子体被广泛用于材料加工以及最近的化学合成。非平衡低温等离子体在室温附近产生高活性物种，(V)UV光子、离子、电子和振动激发的分子。在这个项目中，将在化学合成、材料加工和等离子体医学等不同应用的框架内研究非平衡等离子体与表面(无论是固体还是液体)相互作用的物理和化学。尽管对具有(-)表面的等离子体中的反应路径有了基本的了解，但仅从实验或理论上描述了分子与表面的反应性随选择的振动模式或电子激发而变化的极少数情况。事实上，分子动力学或DFT计算通常假设物种处于基态，没有内部自由度。此外，等离子体物种对表面反应性的影响仍然知之甚少。我的研究计划将重点放在通过结合最先进的等离子体和表面的诊断特征来基本理解激发分子与表面的相互作用和等离子体对后者的修饰。快速功率脉冲将用于调整等离子体特性及其在低气压和大气压条件下与表面的相互作用。第一个研究轴线是研究等离子体暴露下分子对催化剂表面的反应性变化。第二个研究方向是大气等离子体与水的相互作用和物种溶剂化动力学的研究。下一代电子产品需要对创新材料堆叠的图案进行原子控制。我的计划的第三个轴将集中在等离子体刻蚀反应堆中等离子体表面相互作用的精确控制上。该计划的总体目标是，针对每个主题，开发一种能够方便地访问等离子体/表面界面的反应堆，以实现对等离子体和材料性能的最先进诊断。这些实验将为在对等离子体表面相互作用的基本了解的基础上开发用于化学合成和材料处理的新反应堆铺平道路。它们还将作为模拟等离子体对表面本身的影响和原子尺度上的反应动力学的基准。该项目所获得的基础知识对于支持各种主题的更多应用研究至关重要，这些主题包括绿色和可持续的化学合成、水净化和生物医学应用。最重要的是，该计划还将培训4名HQP(3名博士，1名硕士)，使用最先进的设施、程序和工具，并为他们在学术界或工业界工作做好准备。他们将获得关于实验和理论工具的广泛知识，使他们能够应对社会相关挑战。

Plasmas are widely used for material processing as well as, more recently, for chemistry synthesis. Non-equilibrium low temperature plasmas produce highly reactive species, (V)UV photons, ions, electrons and vibrationally excited molecules near room temperature. In this program, the physics and chemistry of non-equilibrium plasmas in interaction with surfaces (either solid or liquid) will be studied in the framework of different applications such as chemical synthesis, material processing and plasma medicine. Despite a basic understanding of the reactive pathways in plasma with(-out) surfaces, only a very few cases of variation of molecular reactivity with surfaces upon selective vibrational modes or electronic excitation were described experimentally or theoretically. In fact, molecular dynamics or DFT calculations usually assume that the species are in their ground state and have no internal degree of freedom. Also the effects of the plasma species on the surface reactivity are still poorly understood. My research program will focus on the fundamental understanding of excited molecules interactions with surfaces and plasma modifications of the latter by combining in operando state of the art diagnostics characterization of both the plasma and the surface. Fast power pulsing will be used to tune plasma properties and its interactions with surfaces both at low and atmospheric pressure conditions. The first research axis is the investigation of the change of molecules reactivity toward catalyst surfaces under plasma exposure. The second axis of research is the interactions of atmospheric plasmas with water and the study of species solvation dynamics. Next generation electronics require atomic control of the patterning of innovative material stacks. The third axis of my program will be focused on the precise control of plasma surface interactions in plasma etch reactors. The overall goal of the program is, for each thematic, to develop a reactor with facile access to the plasma/surface interface for, in operando, state of the art diagnostics of the plasma and material properties. These experiments will pave the way for the development of new reactors for chemical synthesis and material processing based on a fundamental understanding of the plasma surface interactions. They will also serve as benchmark for modelling of the effect of the plasma on the surface itself and reaction dynamics at the atomic scale. The fundamental knowledge gained by this program will be critical for supporting more applied research in various topics such as green and sustainable chemical synthesis, water purification and biomedical applications. This program will, most importantly, also allow training 4 HQPs (3 PhD, 1 MSc) with state-of-the-art facilities, programs and tools and it will prepare them for work in academia or industry. They will have acquired a broad knowledge on experimental and theoretical tools allowing them to tackle society relevant challenges.