From quantum control of electron hole dynamics in polyatomic molecules towards attosecond pulse shaping

阿秒科学是随着强激光场引起的相干电子-离子碰撞的发现而出现的，通常被称为再碰撞。在一个光学周期内，电子从原子或分子中被移除，被振荡的激光场加速，并被驱回与母离子重新碰撞和辐射重组。这个过程-高次谐波产生（HHG）-产生数十个eV宽相干光谱，并有两个重要的应用。首先，高次谐波发射被用来产生阿秒光脉冲，然后可以用于时间分辨泵浦探测实验。第二，超宽相干谐波谱携带了关于潜在非线性响应的阿秒信息，这些信息是可以提取的。我们的建议有助于这两个应用程序。其主要目的是为在XUV领域研究阿秒脉冲整形器奠定理论基础。我们将开发用于控制阿秒脉冲的属性（光谱相位，振幅和偏振）的方法，因为它们是通过控制电离和复合之间的电子空穴动力学产生的。后者将通过在阿秒时间尺度上控制离子的不同电子状态之间的激光诱导跃迁和/或控制电离机制来实现。我们希望我们的方法将有助于多电子动力学的高次谐波谱的发展，应用于成形阿秒XUV脉冲，这将开辟在阿秒时间尺度上控制物质的新方法。

Attosecond Science has emerged with the discovery of coherent electron-ion collisions induced by a strong laser field, usually referred to as re-collisions . Within one optical period an electron is removed from an atom or molecule, accelerated by the oscillating laser field, and driven back to re-collide and radiatively recombine with the parent ion. This process - high harmonic generation (HHG) - produces tens of eV-broad coherent spectra and has two crucial applications. First, high harmonic emission is used to generate attosecond pulses of light, which can then be used in time-resolved pump-probe experiments. Second, ultra-broad coherent harmonic spectrum carries attosecond information about the underlying nonlinear response, which can be extracted. Our proposal contributes to both applications. Its main objective is to lay the theoretical foundation for attosecond “pulse shapers” in XUV domain. We will develop methods for controlling the properties (spectral phases, amplitudes and polarizations) of attosecond pulses as they are produced by controlling electron-hole dynamics between ionization and recombination. The latter will be achieved by controlling laser-induced transitions between different electronic states of the ion on attosecond time scale and/or controlling the ionization regime. We expect that our approaches will contribute to the development of HHG spectroscopy of multielectron dynamics, with application to shaped attosecond XUV pulses that will open new ways of controlling matter on attosecond time scale.