Attosecond Electron Dynamics in Molecular and Condensed Phase Systems

这是一个具有极高科学影响和应用潜力的高级研究项目，对英国具有重大战略意义，如可再生能源和生物分子技术。其目的是开发和应用尖端实验和理论工具的组合，以100阿秒的时间和纳米空间分辨率观察和模拟分子和凝聚态物质的动力学。我们将实现的时间分辨率比目前最先进的测量大分子和凝聚态物质的技术高出两个数量级。科学史表明，每当测量能力出现如此大的改进时，重大的新突破就不可避免。例如，最近发现，在物质的关键分子构件中，突然的电子激发之后，会发生一个普遍的主要事件——亚飞秒到几飞秒的电荷在纳米尺度上的迁移。这种电荷迁移预计在触发后续核动力学和控制化学变化方面极其重要，但其速度太快，无法用现有方法观察到。拟议的研究计划将应用由该小组开发的世界领先的实验和理论工具来研究电荷迁移的性质和其他以前未探索的阿秒尺度过程。我们将在凝聚态物质和大分子（包括生物分子的构建块）的研究中发挥先锋作用。从这项研究中获得的知识将导致对物质电子激发的第一个时刻的新理解，最终，例如，优化人工光采集，分子电子设备和生物分子分析的新方法。在电子水平上成像和控制物质的动力学，特别是远离平衡状态，以及理解量子相干性在分子和纳米级组装中的作用，已被美国能源部确定为基础能源科学五大科学挑战的关键组成部分。今天，2008年7月，第28-33页。我们的方案将使解决这些问题所需的实验和理论的协调努力和密切联系成为可能。英国有一个独特的机会在这一领域发挥世界领导作用，因为我们已经组建了一支杰出的团队，掌握了领导这一新的重要科学领域所需的所有技术和理论工具。我们的计划将利用我们已经开始开发的两种新型测量方法：高谐波产生（HHG）光谱学和阿秒泵浦探测光谱学，并将它们应用于大分子和凝聚态中的阿秒电子动力学测量。这是一项艰巨的挑战，将在实验和理论上开辟新的领域。这一挑战将由我们协调和平衡的项目来应对，该项目将汇集阿秒物理、量子化学、分子结构和动力学、超快和强场科学、纳米尺度和等离子体物理方面的理论和实验专业知识。该计划分为4个相互关联的项目，每个项目都对最终的研究成果做出了重大贡献：项目1：高谐波产生（HHG）光谱学项目2：阿秒泵-探针光谱学项目3：电荷迁移和核动力学的耦合项目4：探测凝聚相的阿秒动力学。

This is a programme of advanced research with potential for extremely high scientific impact and applications to areas of great strategic importance to the UK, such as renewable energy and biomolecular technology. The aim is to develop and apply a combination of cutting-edge experimental and theoretical tools to observe and model dynamics in molecules and condensed phase matter with 100 attosecond temporal and nanometre spatial resolutions. The temporal resolution we will achieve is two orders of magnitude beyond the current state-of-the-art for measurements in larger molecules and condensed matter. The history of science shows that whenever such large improvements in measurement capability occur major new breakthroughs are inevitable. For instance, it has recently emerged that sudden electronic excitation in key molecular building blocks of matter is followed by a universal primary event - sub-femtosecond to few femtosecond migration of electric charge across nanometres. This charge migration, expected to be extremely important in triggering subsequent nuclear dynamics and so controlling chemical change, is too fast to be observed with existing methods. The proposed research programme will apply the world-leading experimental and theoretical tools developed by the assembled team to study the nature of charge migration and other previously unexplored attosecond-scale processes. We will pioneer the investigation in both condensed phase matter and large molecules including the building blocks of biomolecules. The knowledge gained from this research will lead to a new understanding of the first moments in the electronic excitation of matter and ultimately to, for example, new approaches for optimising artificial light harvesting, molecular electronic devices and biomolecular analysis.Imaging and controlling dynamics of matter at the level of electrons, especially far from equilibrium, and understanding the role of quantum coherence in molecules and nanoscale assemblies have been identified by the US Department of Energy as key components of five grand scientific challenges to basic energy sciences (Phys.Today, July 2008, p28-33). Our programme will enable the concerted effort and close linking of experiment and theory needed to address these questions. The UK has a unique opportunity for world leadership in this area, as we have assembled an exceptional team that commands all of the technical and theoretical tools required to lead this new and important area of science.Our programme will exploit two new types of measurements that we have already begun to develop: high harmonic generation (HHG) spectroscopy and attosecond pump-probe spectroscopy, and will apply them to the measurement of attosecond electron dynamics in large molecules and the condensed phase. This is a formidable challenge that will open new frontiers both experimentally and theoretically. This challenge will be met by our coordinated and balanced programme that will bring together theoretical and experimental expertise in attosecond physics, quantum chemistry, molecular structure and dynamics, ultrafast and intense-field science, nanoscale and plasma physics.The programme is structured into 4 interlinked projects, each of which makes a major contribution to the eventual research outcomes: Project 1: High harmonic generation (HHG) spectroscopy Project 2: Attosecond pump-probe spectroscopy Project 3: Coupling of charge migration and nuclear dynamics Project 4: Probing attosecond dynamics in the condensed phase .