Sebastian Eckart

We investigate the dynamical phase evolution of Coulomb-focused electrons in strong-field ionization. We diffract the electrons with an ultrashort standing light wave to track their time-dependent phase. Our findings show that low-energy electrons exhibit a unique chromosome-shaped diffraction pattern, distinct from higher-energy electrons. Our numerical model quantitatively reproduces the experimental results, confirming this pattern maps the electron’s time-dependent phase evolution as it escapes from a Coulomb potential. Our pulsed diffraction grating technique offers a new way to sense an electron’s quantum phase at very large distances without interfering its release mechanism.

We experimentally demonstrate that individual molecules of formic acid are chiral even when they are in the vibronic ground state, which has a planar equilibrium structure. We ionize the C 1s shell of the molecule and record the photoelectron in coincidence with positively charged fragments. This provides two consecutive measurements of the structure of one molecule, the first by photoelectron diffraction imaging and the second by Coulomb explosion imaging. We find that both measurements show the same handedness of the specific molecule. The phenomenon of being achiral on average but chiral at the level of individual molecules is general to prochiral molecules and is a consequence of the three-dimensional zero-point delocalization of the nuclei in the vibrational ground state.

We present a scheme to synthesize a three-dimensional laser field that produces a chiral electron momentum distribution upon strong-field ionization of atoms. Our approach employs two orthogonally propagating two-color laser beams. This results in a time-dependent three-dimensional electric field vector of the combined light field that varies for different positions within the focal volume. For each position, we conduct a simulation of the corresponding electron momentum distribution that includes nonadiabatic dynamics and Coulomb interaction after tunneling. For suitable laser parameters, only a small region of the focal volume contributes to the final momentum distribution. Thus, integrating over all position coordinates, a specific chiral laser field dominates. This leads to a volume-averaged electron momentum distribution, which is chiral, as well. This work will serve as a benchmark for future strong-field experiments aiming at the synthetization of well-defined, three-dimensional laser fields.

After core ionization of CO_{2}, typically an Auger-Meitner decay takes place, leading to the formation of a dicationic molecule that may dissociate into CO^{+} and O^{+}. We demonstrate experimentally that the recoil momentum of the photoelectron determines which of the two equivalent bonds breaks during dissociation. At 20 keV photon energy, we observe an asymmetry of up to 25% for bond cleavage that depends on the emission direction of the photoelectron. Furthermore, we show that this effect leads to a significant nondipole effect in molecular dissociation in the laboratory frame: O^{+} fragments are more likely to be emitted in the direction opposite to the light propagation than along it.

Because of the Heisenberg uncertainty principle, the structure of a molecule fluctuates about its mean geometry, even in the ground state. Observing this fundamental quantum effect experimentally—particularly, revealing the collective nature of the structural quantum fluctuations—remains an unmet challenge for complex molecules. In this work, we achieved this for an 11-atom molecule by inducing its Coulomb explosion with an x-ray free-electron laser. We show that the structural fluctuations manifest themselves in correlated variations of ion momenta obtained through coincident detection of the atomic fragments from individual molecules. Our analysis scheme allows extracting these variations, despite our measurements covering only a fraction of the full 33-dimensional momentum space, thereby establishing a general approach for extracting information on high-dimensional structural dynamics using Coulomb explosion.

The transfer of photon momentum is indispensable in initiating and directing light-matter interactions, which underpins a plethora of fundamental physical processes from laser cooling to laser particle acceleration. The transferred photon momentum is distributed between the photoelectron and the residual ion upon ionization. Our study presents a general and consistent framework for photon momentum transfer covering an arbitrary number of absorbed photons. Our results bridge the gap between the previously considered limiting cases of single-photon and multi-photon strong-field ionization and suggest revising the current consensus for the multi-photon limit by demonstrating that with each additional photon absorbed above the ionization threshold, the photoelectron acquires on average twice the momentum of the absorbed photon. Our work paves the pathway towards a comprehensive understanding of the fundamental processes of photon momentum transfer in light-matter interactions, with implications for both theoretical physics and practical applications that harness the transfer of photon momentum.

We report on strong field ionization of S- and R-propylene oxide in circularly polarized two-color laser fields. We find that the relative helicity of the two single-color laser fields affects the photoelectron circular dichroism (PECD). Further, we observe that PECD is modulated as a function of the subcycle release time of the electron. Our experimental observations are successfully described by a heuristic model based on electrons in chiral initial states, which are selectively liberated by the laser field and, after tunneling, interact with an achiral Coulomb potential. Published by the American Physical Society 2024

High-intensity laser fields can ionize atoms and molecules and also initiate molecular dissociation. This review is on the recent progress made using experiments that harness the potential of cold-target recoil-ion momentum spectroscopy and femtosecond laser pulses with tailored intense fields. The possibility to image the molecular structure and the orientation of small molecules via the detection of the momenta of the ions is illustrated. The process of non-adiabatic tunnel ionization is analyzed in detail focusing on the properties of the electronic wave packet at the tunnel exit. It is reviewed how the electron gains angular momentum and energy during tunneling in circularly polarized light. The electron is a quantum object with an amplitude and a phase. Most experiments in strong field ionization focus on the absolute square of the electronic wave function. The technique of holographic angular streaking of electrons enables the retrieval of Wigner time delays in strong field ionization, which is a property of the electronic wave function’s phase in momentum space. The relationship between the phase in momentum space and the amplitudes in position space enables access to information about the electron’s position at the tunnel exit. Finally, recent experiments studying entanglement in strong field ionization are discussed.

Similar to the optical diffraction of light passing through a material grating, the Kapitza-Dirac effect occurs when an electron is diffracted by a standing light wave. In its original description, the effect is time independent. Here, we extended the Kapitza-Dirac effect to the time domain. By tracking the spatiotemporal evolution of a pulsed electron wave packet diffracted by a 60-femtosecond (where one femtosecond = 10 ⁻¹⁵ seconds) standing wave pulse in a pump-probe scheme, we observed time-dependent diffraction patterns. The fringe spacing in the observed pattern differs from that generated by the conventional Kapitza-Dirac effect. By exploiting this time-resolved diffraction scheme, we can access the time evolution of the phase properties of a free electron and potentially image ionic potentials and electronic decoherences.