arXiv subjects

Benjamin Wolter

Publications and source records attributed to Benjamin Wolter.

5 recordsLinked to original sources

arXiv2018

Imaging the Renner-Teller effect using laser-induced electron diffraction

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS$_2$) in the B$^1$B$_2$ excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS$_2$ molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement. We invoke the Renner-Teller effect to populate the B$^1$B$_2$ excited state in neutral CS$_2$, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS$_2$, which is known to appear as a two-center scatterer.

physics.chem-ph↗

arXiv2016

Transition from non-sequential to sequential double ionisation in many-electron systems

Obtaining a detailed understanding of strong-field double ionisation of many-electron systems (heavy atoms and molecules) remains a challenging task. By comparing experimental and theoretical results in the mid-IR regime, we have unambiguously identified the transition from non-sequential (e,2e) to sequential double ionisation in Xe and shown that it occurs at an intensity below $10^{14}$ Wcm$^{-2}$. In addition, our data demonstrate that ionisation from the Xe 5s orbital is decisive at low intensities. Moreover, using the acetylene molecule, we propose how sequential double ionisation in the mid-IR can be used to study molecular dynamics and fragmentation on unprecedented few-femtosecond timescales.

physics.atom-ph↗

arXiv2015

Strong-field physics with mid-IR fields

Strong-field physics is currently experiencing a shift towards the use of mid-IR driving wavelengths. This is because they permit conducting experiments unambiguously in the quasi-static regime and enable exploiting the effects related to ponderomotive scaling of electron recollisions. Initial measurements taken in the mid-IR immediately led to a deeper understanding of photo-ionization and allowed a discrimination amongst different theoretical models. Ponderomotive scaling of rescattering has enabled new avenues towards time resolved probing of molecular structure. Essential for this paradigm shift was the convergence of two experimental tools: 1) intense mid-IR sources that can create high energy photons and electrons while operating within the quasi-static regime, and 2) detection systems that can detect the generated high energy particles and image the entire momentum space of the interaction in full coincidence. Here we present a unique combination of these two essential ingredients, namely a 160kHz mid-IR source and a reaction microscope detection system, to present an experimental methodology that provides an unprecedented three-dimensional view of strong-field interactions. The system is capable of generating and detecting electron energies that span a six order of magnitude dynamic range. We demonstrate the versatility of the system by investigating electron recollisions, the core process that drives strong-field phenomena, at both low (meV) and high (hundreds of eV) energies. The low energy region is used to investigate recently discovered low-energy structures, while the high energy electrons are used to probe atomic structure via laser-induced electron diffraction. Moreover we present, for the first time, the correlated momentum distribution of electrons from non-sequential double-ionization driven by mid-IR pulses.

physics.atom-ph↗

arXiv2015

Imaging an aligned polyatomic molecule with laser-induced electron diffraction

Laser-induced electron diffraction is an evolving tabletop method, which aims to image ultrafast structural changes in gas-phase polyatomic molecules with sub-Ångström spatial and femtosecond temporal resolution. Here, we provide the general foundation for the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C-C and C-H bond lengths in aligned acetylene. Our approach takes the method beyond the hitherto achieved imaging of simple diatomic molecules and is based upon the combination of a 160 kHz mid-IR few-cycle laser source with full three-dimensional electron-ion coincidence detection. Our technique provides an accessible and robust route towards imaging ultrafast processes in complex gas phase molecules with atto- to femto-second temporal resolution.

physics.atom-ph↗

arXiv2014

Formation of very low energy states crossing the ionization threshold of argon atoms in strong mid-infrared fields

Atomic ionization by intense mid-infrared (mid-IR) pulses produces low electron energy features that the strong-field approximation, which is expected to be valid in the tunneling ionization regime characterized by small Keldysh parameters ($γ\ll 1$), cannot describe. These features include the low-energy structure (LES), the very-low-energy structure (VLES), and the more recently found zero-energy structure (ZES). They result from the interplay between the laser electric field and the atomic Coulomb field which controls the low-energy spectrum also for small $γ$. In the present joint experimental and theoretical study we investigate the vectorial momentum spectrum at very low energies. Using a reaction microscope optimized for the detection of very low energy electrons, we have performed a thorough study of the three-dimensional momentum spectrum well below 1 eV. Our measurements are complemented by quantum and classical simulations, which allow for an interpretation of the LES, VLES and of the newly identified ZES in terms of two-dimensional Coulomb focusing and recapture into Rydberg states, respectively.

physics.atom-ph↗