Setting the photoelectron clock through molecular alignment

Abstract

The interaction of strong laser fields with matter intrinsically provides a powerful tool for imaging transient dynamics with an extremely high spatiotemporal resolution. Here, we study strong-field ionisation of laser-aligned molecules, and show a full real-time picture of the photoelectron dynamics in the combined action of the laser field and the molecular interaction. We demonstrate that the molecule has a dramatic impact on the overall strong-field dynamics: it sets the clock for the emission of electrons with a given rescattering kinetic energy. This result represents a benchmark for the seminal statements of molecular-frame strong-field physics and has strong impact on the interpretation of self-diffraction experiments. Furthermore, the resulting encoding of the time-energy relation in molecular-frame photoelectron momentum distributions shows the way of probing the molecular potential in real-time, and accessing a deeper understanding of electron transport during strong-field interactions.

Ultrafast light-induced dynamics in the microsolvated biomolecular indole chromophore with water

“…The experimental setup, schematically shown in Figure 1 c was described previously [53,54]. In brief, 95 bar of helium was bubbled through room-temperature water before passing through the sample reservoir of an Even-Lavie valve containing indole (Sigma-Aldrich, ≥ 99 %).…”

Time-resolving the UV-initiated photodissociation dynamics of OCS

“…We are currently experimentally investigating the OCS reaction system using laserinduced electron diffraction in the molecular frame. [23][24][25]61 Imaging the dynamics observed here with our previously achieved 5 pm spatial 23 and sub-100 fs temporal resolution would provide a very direct structural view on the ongoing dynamics. Alternatively, MeV ultrafast electron diffraction with sufficient time resolution is also within reach 22 and could provide significant information on this structurally simple model system.…”

“…[20][21][22] We are interested in exploring the possibilities for atomically resolved imaging of photoinduced chemical reactions using LIED. [23][24][25] In this paper, we present ion-imaging measurements that we have performed as the precursor to such a LIED experiment.…”

Ultrafast Hole Deformation Revealed by Molecular Attosecond Interferometry

“…Different from the previous research of hole which detects only the intensities and phases of different harmonics and therefore confirms the participation of HOMO and HOMO-1 of N 2 [49], our molecular attosecond interferometry can add an additional phase of the EWP, leading to the reconstruction of hole deformation from more than two orbitals. In other words, our method can be applied to the other polyatomic molecules that exhibit the alignment-dependent ionization channels, for instance, N 2 O 4 [50] [52,53], CF 3 I [54], and COS [55], in order to understand the channel-dependent dynamics during the strong field process. So far, the present work is limited to study the electron dynamics decoupled with nuclear motion.…”