Attosecond streaking in a nano-plasmonic field

A theoretical study of the application of attosecond streaking spectroscopy to time-resolved studies of the plasmonic fields surrounding isolated, resonantly excited spherical nanoparticles is presented. A classification of the different regimes in attosecond streaking is proposed and identified in our results that are derived from Mie calculations of plasmon fields, coupled to classical electron trajectory simulations. It is shown that in an attosecond streaking experiment, the electrons are almost exclusively sensitive to the component of the field parallel to the direction in which they are detected. This allows one to probe the different components of the field individually by resolving the angle of emission of the electrons. Finally, simulations based on fields calculated by finite-difference time-domain (FDTD) are compared with the results obtained using Mie fields. The two are found to be in good agreement with each other, supporting the notion that FDTD methods can be used to reliably investigate non-spherical structures

Attosecond time-resolved photoelectron holography

Ultrafast strong-field physics provides insight into quantum phenomena that evolve on an attosecond time scale, the most fundamental of which is quantum tunneling. The tunneling process initiates a range of strong field phenomena such as high harmonic generation (HHG), laser-induced electron diffraction, double ionization and photoelectron holography—all evolving during a fraction of the optical cycle. Here we apply attosecond photoelectron holography as a method to resolve the temporal properties of the tunneling process. Adding a weak second harmonic (SH) field to a strong fundamental laser field enables us to reconstruct the ionization times of photoelectrons that play a role in the formation of a photoelectron hologram with attosecond precision. We decouple the contributions of the two arms of the hologram and resolve the subtle differences in their ionization times, separated by only a few tens of attoseconds

Attosecond control of electron dynamics in carbon monoxide

Laser pulses with stable electric field waveforms establish the opportunity to achieve coherent control on attosecond timescales. We present experimental and theoretical results on the steering of electronic motion in a multi-electron system. A very high degree of light-waveform control over the directional emission of C+ and O+ fragments from the dissociative ionization of CO was observed. Ab initio based model calculations reveal contributions to the control related to the ionization and laser-induced population transfer between excited electronic states of CO+ during dissociation

Probing Time-Dependent Molecular Dipoles on the Attosecond Time Scale

Photoinduced molecular processes start with the interaction of the instantaneous electric field of the incident light with the electronic degrees of freedom. This early attosecond electronic motion impacts the fate of the photoinduced reactions. We report the first observation of attosecond time scale electron dynamics in a series of small- and medium-sized neutral molecules (N2, CO2, and C2H4), monitoring time-dependent variations of the parent molecular ion yield in the ionization by an attosecond pulse, and thereby probing the time-dependent dipole induced by a moderately strong near- infrared laser field. This approach can be generalized to other molecular species and may be regarded as a first example of molecular attosecond Stark spectroscopy

Ultrafast modulation of electronic structure by coherent phonon excitations

Femtosecond x-ray absorption spectroscopy with a laser-driven high-harmonic source is used to map ultrafast changes of x-ray absorption by femtometer- scale coherent phonon displacements. In LiBH4, displacements along an Ag phonon mode at 10 THz are induced by impulsive Raman excitation and give rise to oscillatory changes of x-ray absorption at the Li K edge. Electron density maps from femtosecond x-ray diffraction data show that the electric field of the pump pulse induces a charge transfer from the BH4− to neighboring Li+ ions, resulting in a differential Coulomb force that drives lattice vibrations in this virtual transition state

Observation of correlated electronic decay in expanding clusters triggered by near-infrared fields

When an excited atom is embedded into an environment, novel relaxation pathways can emerge that are absent for isolated atoms. A well-known example is interatomic Coulombic decay, where an excited atom relaxes by transferring its excess energy to another atom in the environment, leading to its ionization. Such processes have been observed in clusters ionized by extreme- ultraviolet and X-ray lasers. Here, we report on a correlated electronic decay process that occurs following nanoplasma formation and Rydberg atom generation in the ionization of clusters by intense, non-resonant infrared laser fields. Relaxation of the Rydberg states and transfer of the available electronic energy to adjacent electrons in Rydberg states or quasifree electrons in the expanding nanoplasma leaves a distinct signature in the electron kinetic energy spectrum. These so far unobserved electron-correlation-driven energy transfer processes may play a significant role in the response of any nano- scale system to intense laser light

Signatures of Light-Induced Potential Energy Surfaces in H2+

Using theory and Cold Target Recoil Ion Momentum Spectroscopy we find signatures of light-induced molecular potential energy surfaces in the 3-dimensional proton momentum distributions of dissociating H+2. © 2020 Journal of Physics: Conference Series. All rights reserved

Observation of correlated electronic decay in expanding clusters triggered by near-infrared fields

When an excited atom is embedded into an environment, novel relaxation pathways can emerge that are absent for isolated atoms. A well-known example is interatomic Coulombic decay, where an excited atom relaxes by transferring its excess energy to another atom in the environment, leading to its ionization. Such processes have been observed in clusters ionized by extreme-ultraviolet and X-ray lasers. Here, we report on a correlated electronic decay process that occurs following nanoplasma formation and Rydberg atom generation in the ionization of clusters by intense, non-resonant infrared laser fields. Relaxation of the Rydberg states and transfer of the available electronic energy to adjacent electrons in Rydberg states or quasifree electrons in the expanding nanoplasma leaves a distinct signature in the electron kinetic energy spectrum. These so far unobserved electron-correlation-driven energy transfer processes may play a significant role in the response of any nano-scale system to intense laser light

Visualizing the Coupling between Red and Blue Stark States Using Photoionization Microscopy

In nonhydrogenic atoms in a dc electric field, the finite size of the ionic core introduces a coupling between quasibound Stark states that leads to avoided crossings between states that would otherwise cross. Near an avoided crossing, the interacting states may have decay amplitudes that cancel each other, decoupling one of the states from the ionization continuum. This well- known interference narrowing effect, observed as a strongly electric field- dependent decrease in the ionization rate, was previously observed in several atoms. Here we use photoionization microscopy to visualize interference narrowing in helium atoms, thereby explicitly revealing the mechanism by which Stark states decay. The interference narrowing allows measurements of the nodal patterns of red Stark states, which are otherwise not observable due to their intrinsic short lifetime

Attosecond investigation of extreme-ultraviolet multi-photon multi-electron ionization

Multi-electron dynamics in atoms and molecules very often occur on sub- to few-femtosecond time scales. The available intensities of extreme-ultraviolet (XUV) attosecond pulses have previously allowed the time-resolved investigation of two-photon, two-electron interactions. Here we study double and triple ionization of argon atoms involving the absorption of up to five XUV photons using a pair of intense attosecond pulse trains (APTs). By varying the time delay between the two APTs with attosecond precision and the spatial overlap with nanometer precision, we obtain information on complex nonlinear multi-photon ionization pathways. Our experimental and numerical results show that Ar2+ is predominantly formed by a sequential two-photon process, whereas the delay dependence of the Ar3+ ion yield exhibits clear signatures of the involvement of a simultaneous two-photon absorption process. Our experiment suggests that it is possible to investigate multi-electron dynamics using attosecond pulses for both pumping and probing the dynamics