Alexander Blättermann

Reconstruction and control of a time-dependent two-electron wave packet

The concerted motion of two or more bound electrons governs atomic and molecular non-equilibrium processes including chemical reactions, and hence there is much interest in developing a detailed understanding of such electron dynamics in the quantum regime. However, there is no exact solution for the quantum three-body problem, and as a result even the minimal system of two active electrons and a nucleus is analytically intractable. This makes experimental measurements of the dynamics of two bound and correlated electrons, as found in the helium atom, an attractive prospect. However, although the motion of single active electrons and holes has been observed with attosecond time resolution, comparable experiments on two-electron motion have so far remained out of reach. Here we show that a correlated two-electron wave packet can be reconstructed from a 1.2-femtosecond quantum beat among low-lying doubly excited states in helium. The beat appears in attosecond transient-absorption spectra measured with unprecedentedly high spectral resolution and in the presence of an intensity-tunable visible laser field. We tune the coupling between the two low-lying quantum states by adjusting the visible laser intensity, and use the Fano resonance as a phase-sensitive quantum interferometer to achieve coherent control of the two correlated electrons. Given the excellent agreement with large-scale quantum-mechanical calculations for the helium atom, we anticipate that multidimensional spectroscopy experiments of the type we report here will provide benchmark data for testing fundamental few-body quantum dynamics theory in more complex systems. They might also provide a route to the site-specific measurement and control of metastable electronic transition states that are at the heart of fundamental chemical reactions.

High-order harmonic generation at 4 MHz as a light source for time-of-flight photoemission spectroscopy

We demonstrate high-order harmonic generation (HHG) at 4 MHz driven by a long-cavity femtosecond laser oscillator. The laser output is used directly in a tight focusing geometry, where the harmonics are generated from a gas jet with high backing pressure. The harmonic light source is applied to time-of-flight photoemission spectroscopy, and the characteristic electronic structure of Cu(111) is measured. Our results suggest a straightforward design of high-order harmonic generation at megahertz repetition rate and pave the way for applications in electron spectroscopy and microscopy.

Two-dimensional spectral interpretation of time-dependent absorption near laser-coupled resonances

We demonstrate a two-dimensional time-domain spectroscopy method to extract amplitude and phase modifications of excited atomic states caused by the interaction with ultrashort laser pulses. The technique is based on Fourier analysis of the absorption spectrum of perturbed polarization decay. An analytical description of the method reveals how amplitude and phase information can be directly obtained from measurements. We apply the method experimentally to the helium atom, which is excited by attosecond-pulsed extreme ultraviolet light, to characterize laser-induced couplings of doubly excited states.

Time-resolved four-wave-mixing spectroscopy for inner-valence transitions

Noncollinear four-wave-mixing (FWM) techniques at near-infrared (NIR), visible, and ultraviolet frequencies have been widely used to map vibrational and electronic couplings, typically in complex molecules. However, correlations between spatially localized inner-valence transitions among different sites of a molecule in the extreme ultraviolet (XUV) spectral range have not been observed yet. As an experimental step toward this goal, we perform time-resolved FWM spectroscopy with femtosecond NIR and attosecond XUV pulses. The first two pulses (XUV-NIR) coincide in time and act as coherent excitation fields, while the third pulse (NIR) acts as a probe. As a first application, we show how coupling dynamics between odd- and even-parity, inner-valence excited states of neon can be revealed using a two-dimensional spectral representation. Experimentally obtained results are found to be in good agreement with ab initio time-dependent R-matrix calculations providing the full description of multielectron interactions, as well as few-level model simulations. Future applications of this method also include site-specific probing of electronic processes in molecules.

In situ characterization of few-cycle laser pulses in transient absorption spectroscopy

Attosecond transient absorption spectroscopy has thus far been lacking the capability to simultaneously characterize the intense laser pulses at work within a time-resolved quantum-dynamics experiment. However, precise knowledge of these pulses is key to extracting quantitative information in strong-field highly nonlinear light-matter interactions. Here, we introduce and experimentally demonstrate an ultrafast metrology tool based on the time-delay-dependent phase shift imprinted on a strong-field-driven resonance. Since we analyze the signature of the laser pulse interacting with the absorbing spectroscopy target, the laser pulse duration and intensity are determined in situ. As we also show, this approach allows for the quantification of time-dependent bound-state dynamics in one and the same experiment. In the future, such experimental data will facilitate more precise tests of strong-field dynamics theories.

Watching the emergence of a Fano resonance in doubly excited helium

We report on the experimental observation of the buildup of the 2s2p Fano resonance in helium in the time domain, which has been under theoretical investigation for more than a decade. The emergence of the absorption line is temporally resolved by interrupting the natural decay of the excited state via saturated strong-field ionization at a variable time delay. We compare the experimental data with full ab-initio simulations to validate the time-gating by strong-field ionization and thereby confirm the recently developed theory for the formation of Fano line-profiles.

Impulsive control of the atomic dipole response in the time and frequency domain

The dipole response of an excited quantum system gives direct insight into the electron dynamics triggered by the incoming light. Spectroscopy techniques such as (attosecond) transient absorption spectroscopy make use of the fact that the dipole response leaves its characteristic fingerprint on the transmitted light. In this work, a general and comprehensive model is introduced, which allows for an analytic description of dipole dynamics triggered and modified by two ultrashort light pulses in both time and frequency domains. Based on this description, a two-dimensional spectral representation of time delay–resolved absorption data is developed. The power of the method to separate different pathways of light–matter interaction, which allows for their individual investigation, is demonstrated experimentally by studying electronic wave packet dynamics in doubly excited helium and inner-valence excited xenon. Furthermore, an in situ technique for characterization of the intense dressing laser pulse that drives (nonlinear) quantum dynamics in time-resolved absorption experiments is derived from the same analytic model and demonstrated experimentally. The possibility to characterize these ultrashort strong-field laser pulses directly within the spectroscopy target enhances the scope of transient absorption spectroscopy as it allows for the precise measurement and control of electron dynamics and increases the comparability between experiment and theory.

Fano Resonances in the Time Domain

The Fano phase formalism enables measurement and control of phase and amplitude of an emitting dipole. Here, we use this formalism to measure and understand the dynamics of bound atomic states in strong laser fields.