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Hans Jakob Woerner

Publications and source records attributed to Hans Jakob Woerner.

4 recordsLinked to original sources

Circular RABBITT goes under threshold

We introduce circular under-threshold RABBITT (cuRABBITT) as a new interferometric method to probe discrete electronic excitations in atoms with attosecond resolution. By combining circularly polarized attosecond pulses with broadband (``rainbow'') spectral analysis, we directly access two-photon ionization amplitudes and their relative phases. Time-dependent Schrödinger simulations, supported by Green's function theory, reveal strong resonances in helium and argon and a Cooper-like minimum in xenon. These results demonstrate that cuRABBITT provides continuous spectral mapping of bound-state resonances and extends Fano's propensity rule into the under-threshold regime. Our work establishes cuRABBITT as a powerful attosecond metrology technique, opening the way to polarization-resolved studies of resonant dynamics in atoms and molecules.

physics.atom-ph↗

Few-femtosecond electronic and structural rearrangements of CH$_4^+$ driven by the Jahn-Teller effect

The Jahn-Teller effect (JTE) is central to the understanding of the physical and chemical properties of a broad variety of molecules and materials. Whereas the manifestations of the JTE on stationary properties of matter are relatively well studied, the study of JTE-induced dynamics is still in its infancy, largely owing to its ultrafast and non-adiabatic nature. For example, the time scales reported for the distortion of CH$_4^+$ from the initial $T_{\rm d}$ geometry to a nominal $C_{\rm 2v}$ relaxed structure range from 1.85~fs over 10$\pm$2~fs to 20$\pm$7~fs. Here, by combining element-specific attosecond transient-absorption spectroscopy and quantum-dynamics simulations, we show that the initial electronic relaxation occurs within 5~fs and that the subsequent nuclear dynamics are dominated by the $Q_2$ scissoring and $Q_1$ symmetric stretching modes, which dephase in 41$\pm$10~fs and 13$\pm$3~fs, respectively. Significant structural relaxation is found to take place only along the e-symmetry $Q_2$ mode. These results demonstrate that CH$_4^+$ created by ionization of CH$_4$ is best thought of as a highly fluxional species that possesses a long-time-averaged vibrational distribution centered around a $D_{\rm 2d}$ structure. The methods demonstrated in our work provide guidelines for the understanding of Jahn-Teller driven non-adiabatic dynamics in other, more complex systems.

physics.chem-ph↗

Two-center Interference in the Photoionization Delays of Kr2

We present the experimental observation of two-center interference in the ionization time delays of Kr2. Using attosecond electron-ion-coincidence spectroscopy, we simultaneously measure the photoionization delays of krypton monomer and dimer. The relative time delay is found to oscillate as a function of the electron kinetic energy, an effect that is traced back to constructive and destructive interference of the photoelectron wave packets that are emitted or scattered from the two atomic centers. Our interpretation of the experimental results is supported by solving the time-independent Schrodinger equation of a 1D double-well potential, as well as coupled-channel multiconfigurational quantum-scattering calculations of Kr2. This work opens the door to the study of a broad class of quantum-interference effects in photoionization delays and demonstrates the potential of attosecond coincidence spectroscopy for studying weakly bound systems.

physics.atom-ph↗

Coherent Manipulation of Quantum Delta-kicked Dynamics: Faster-than-classical Anomalous Diffusion

Large transporting regular islands are found in the classical phase space of a modified kicked rotor system in which the kicking potential is reversed after every two kicks. The corresponding quantum system, for a variety of system parameters and over long time scales, is shown to display energy absorption that is significantly faster than that associated with the underlying classical anomalous diffusion. The results are of interest to both areas of quantum chaos and quantum control.

quant-ph↗