Coherent control of quantum systems with designer light fields

今天，我们对激光产生的光场在时间和空间上都有令人难以置信的控制。我们可以控制激光脉冲的颜色、偏振和持续时间。我们可以联合收割机组合几乎任意的频率和脉冲宽度。我们可以控制激光束内光的空间特性。例如，我们可以创建中间有孔的光束，具有空间变化的偏振矢量的光束，或者波前看起来像空间中的开瓶器的光束。对激光场的这种程度的控制开辟了新的应用，我将探讨其中的一些应用。虽然圆偏振激光场是手性的，但是它们的波长通常比单个分子大得多，即，远离共振，分子仅经历均匀电场。我建议实现一个激光场，在空间中的每一点都是手性的，这将允许区分左手和右手分子比常用的方法，如光电子圆二色性更有效。 我将使用符合光电子光离子动量谱，称为COLTRIMS或反应显微镜，检测电离产率，光电子分子框架角分布和库仑爆炸成像的手性依赖的信号。除了开发一种新的结构诊断工具，我建议激发和图像在水中的超快弛豫过程。水二聚体作为液态水的最简单近似物，可以作为理解高能光子引发的过程的试验场。尽管软X射线在不同领域中具有极其重要的意义，但人们对水中的软X射线吸收了解甚少。了解水中X射线光子吸收的能量和电荷重新分布对于设计更有效的放射肿瘤学方案，解开对活组织的遗传毒性效应的物理基础以及在X射线衍射实验期间最大限度地减少生物样品的损伤至关重要。 这两个项目为扩展和未来的研究提供了充足的机会。

Today we have incredible control over the optical fields created by lasers, both in time and in space. We can control the color, polarization and duration of laser pulses. We can combine nearly arbitrary frequencies and pulse durations. We can control the spatial properties of the light within the laser beam. For example we can create beams with a hole in the middle, beams with a spatially varying polarization vector, or beams whose wave front looks like a corkscrew in space. This degree of control over laser fields opens up new applications, some of which I will explore. While circularly polarized laser fields are chiral their wavelength is generally much larger than a single molecule, i.e., away from resonances a molecule experiences only a homogeneous electric field. I propose to realize a laser field that is chiral at every point in space and that will permit to distinguish left and right-handed molecules much more efficiently than commonly used methods such as photoelectron circular dichroism. I will use coincidence photoelectron photoion momentum spectroscopy, known as COLTRIMS or reaction microscopy, to detect a chirality dependent signal in ionization yields, photoelectron molecular frame angular distribution and Coulomb explosion imaging. In addition to developing a new structural diagnostic tool, I propose to excite and image ultrafast relaxation processes in water. Water dimers as the simplest approximation to liquid water can serve as testing ground to understand the processes that are initiated by high energy photons. Soft X-ray absorption in water is understood poorly despite its paramount importance in different fields. Understanding the energy and charge redistribution on X-ray photon absorption in water is vital for the design of more-efficient radiooncology schemes, for disentangling the physical basis of genotoxic effects on living tissues and for minimizing the damage of biological samples during X-ray diffraction experiments. Both projects provide ample opportunity for expansion and future research.