Attosecond spectroscopy reveals alignment dependent core-hole dynamics in the ICl molecule

  title={Attosecond spectroscopy reveals alignment dependent core-hole dynamics in the ICl molecule},
  author={Hugo J. B. Marroux and Ashley P. Fidler and Aryya Ghosh and Yuki Kobayashi and Kirill Gokhberg and Alexander I. Kuleff and Stephen R. Leone and Daniel M. Neumark},
  journal={Nature Communications},
The removal of electrons located in the core shells of molecules creates transient states that live between a few femtoseconds to attoseconds. Owing to these short lifetimes, time-resolved studies of these states are challenging and complex molecular dynamics driven solely by electronic correlation are difficult to observe. Here, we obtain few-femtosecond core-excited state lifetimes of iodine monochloride by using attosecond transient absorption on iodine 4d−16p transitions around 55 eV. Core… 
4 Citations

Source noise suppression in attosecond transient absorption spectroscopy by edge-pixel referencing.

Results show that edge-referencing methods bring the sensitivity of ATAS near the detector noise floor, and the combination of the two methods ensures the fidelity of the procedure and can be implemented on live data collection but also on existing datasets.

Unexpected dipole instabilities in small molecules after ultrafast XUV irradiation

We investigate the depletion of single-electron states in small molecules under the influence of very short XUV pulses. In N$_2$, for a certain window of XUV energies around 50 eV, we observe a

Ultrafast photo-induced processes in complex environments: The role of accuracy in excited-state energy potentials and initial conditions

Light induces non-equilibrium time evolving molecular phenomena. The computational modeling of photo-induced processes in large systems, embedded in complex environments (i.e., solutions, proteins,

Coupled nuclear-electronic decay dynamics of O2 inner valence excited states revealed by attosecond XUV wave-mixing spectroscopy.

An intriguing picture of the coupled nuclear-electronic dynamics is revealed by attosecond XUV wave-mixing spectroscopy, indicating that the decay dynamics are not a simple competition between isolated autoionization and predissociation processes.



Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy.

This review provides an overview of recentAttosecond measurements, focusing on the wealth of knowledge obtained by the application of isolated attosecond pulses in studying dynamics in gases and solid-state systems.

State-Resolved Probing of Attosecond Timescale Molecular Dipoles.

An experimental study of iodomethane attosecond transient absorption spectroscopy (ATAS) in the region of iodine 4d core-to-valence/Rydberg excitation observes pronounced differences between the ATAS signatures of valence and Rydberg states.

Attosecond transient absorption probing of electronic superpositions of bound states in neon. Detection of quantum beats

Electronic wavepackets composed of multiple bound excited states of atomic neon lying between 19.6 and 21.5 eV are launched using an isolated attosecond pulse. Individual quantum beats of the

Ultrafast quantum control of ionization dynamics in krypton

Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or

Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses

The application of isolated attosecond pulses to prompt ionization of the amino acid phenylalanine and the subsequent detection of ultrafast dynamics on a sub–4.5-femtosecond temporal scale, which is shorter than the vibrational response of the molecule.

Attosecond real-time observation of electron tunnelling in atoms

The real-time observation of this most elementary step in strong-field interactions: light-induced electron tunnelling is reported, and the process is found to deplete atomic bound states in sharp steps lasting several hundred attoseconds, suggesting a new technique, attose Cond Tunnelling, for probing short-lived, transient states of atoms or molecules with high temporal resolution.

Ligand‐field splittings and core‐level linewidths in I 4d photoelectron spectra of iodine molecules

High‐resolution I 4d photoelectron spectra (total instrumental resolution ∼0.06 eV) of seven simple iodine molecules, ICl, IBr, I2, HI, CH3I, CH2I2, and CF3I, have been recorded. Ligand‐field

Attosecond dynamics through a Fano resonance: Monitoring the birth of a photoelectron

Using spectrally resolved electron interferometry, the amplitude and phase of a photoelectron wave packet created through a Fano autoionizing resonance in helium is measured, raising prospects for detailed investigations of ultrafast photoemission dynamics governed by electron correlation, as well as coherent control over structured electron wave packets.

Direct observation of electron dynamics in the attosecond domain

The method is pushed into the attosecond regime by focusing on short-lived holes with initial and final states in the same electronic shell, which allows it to show that electron transfer from an adsorbed sulphur atom to a ruthenium surface proceeds in about 320 as.

Theory of strong-field attosecond transient absorption

Attosecond transient absorption is one of the promising new techniques being developed to exploit the availability of sub-femtosecond extreme ultraviolet (XUV) pulses to study the dynamics of the