Tim Bayer

Zeptosecond precision pulse shaping.

We investigate the temporal precision in the generation of ultrashort laser pulse pairs by pulse shaping techniques. To this end, we combine a femtosecond polarization pulse shaper with a polarizer and employ two linear spectral phase masks to mimic an ultrastable common-path interferometer. In an all-optical experiment we study the interference signal resulting from two temporally delayed pulses. Our results show a 2σ-precision of 300 zs = 300 × 10(-21) s in pulse-to-pulse delay. The standard deviation of the mean is 11 zs. The obtained precision corresponds to a variation of the arms length in conventional delay stage based interferometers of 0.45 Å. We apply these precisely generated pulse pairs to a strong-field quantum control experiment. Coherent control of ultrafast electron dynamics via photon locking by temporal phase discontinuities on a few attosecond timescale is demonstrated.

Coherent strong-field control of multiple states by a single chirped femtosecond laser pulse

We present a joint experimental and theoretical study on strong- field photo-ionization of sodium atoms using chirped femtosecond laser pulses. By tuning the chirp parameter, selectivity among the population in the highly excited states 5p, 6p, 7p and 5f, 6f is achieved. Different excitation pathways enabling control are identified by simultaneous ionization and measurement of photoelectron angular distributions employing the velocity map imaging technique. Free electron wave packets at an energy of around 1eV are observed. These photoelectrons originate from two channels. The predominant 2+1+1 resonance enhanced multi-photon ionization (REMPI) proceeds via the strongly driven two-photon transition 4s 3s, and subsequent ionization from the states 5p, 6p and 7p whereas the second pathway involves 3+1 REMPI via the states 5f and 6f. In addition, electron wave packets from two-photon ionization of the non-resonant transiently populated state 3p are observed close to the ionization threshold. A mainly qualitative five-state model for the predominant excitation channel is studied theoretically to provide insights into the physical mechanisms at play. Our analysis shows that by tuning the chirp parameter the dynamics is effectively controlled by dynamic Stark shifts and level crossings. In particular, we show that under the experimental conditions the passage through

Strong-field control landscapes of coherent electronic excitation

We report on physical mechanisms behind resonant strong-field coherent control. To this end, we study multi-photon ionization of potassium atoms using intense shaped femtosecond laser pulses. The measured photoelectron spectra are discussed in terms of selective population of dressed states (SPODS). A physically motivated pulse parameterization is introduced which opens up two-dimensional parameter spaces comprising pulse sequences as well as chirped pulses. The control topologies of these subspaces are mapped out experimentally and are presented in the form of strong-field control landscapes (SFCLs). In the SFCLs, complementary realizations of SPODS via photon locking and rapid adiabatic passage are observed. Moreover, the combined effect, termed Multi-RAP, arises when both mechanisms are at play simultaneously. In order to better understand the performance of adaptive optimization procedures, we experimentally study their capability to find optimal solutions on a given parameter space. The evolution of different optimization procedures is visualized by means of control trajectories on the surface of the measured SFCL.

Electron Vortices in Femtosecond Multiphoton Ionization

Multiphoton ionization of potassium atoms with a sequence of two counter-rotating circularly polarized femtosecond laser pulses produces vortex-shaped photoelectron momentum distributions in the polarization plane describing Archimedean spirals. The pulse sequences are produced by polarization shaping and the three-dimensional photoelectron distributions are tomographically reconstructed from velocity map imaging measurements. We show that perturbative ionization leads to electron vortices with c_{6} rotational symmetry. A change from c_{6} to c_{4} rotational symmetry of the vortices is demonstrated for nonperturbative interaction.

Coupled electron-nuclear wavepacket dynamics in potassium dimers

Recently we have demonstrated control of valence-bond excitation of a molecule due to the interplay of the induced charge oscillation with the precisely tailored phase of the driving laser field (Bayer et al 2013 Phys. Rev. Lett. 110 123003). In this contribution we describe in more detail the two-colour experiment—a control pulse sequence followed by an ionizing probe pulse of a different wavelength. We provide details on the quantum dynamics simulations carried out to reproduce and to analyse the experimental results. The procedure for averaging over the focal intensity distribution in the interaction region and the method for orientation averaging, which are both crucial for the reproduction of our strong-field measurements, are also described in detail. The analysis of the temporal evolution of the expectation values of the wavepackets on the relevant potentials, the induced energetic shifts in the molecule and the modulation in the charge oscillation provides further insights into the interplay of the coupled nuclear-electron dynamics. Because the measured photoelectron spectra reveal the population of the target states we describe the quantum mechanical approach to calculate the photoelectron spectra and rationalize the results using Mullikens difference potential method.

Ultrashort polarization-tailored bichromatic fields

Abstract We present a novel concept for the generation of ultrashort polarization-shaped bichromatic laser fields. The scheme utilizes a 4f polarization pulse shaper based on a liquid crystal spatial light modulator for independent amplitude and phase modulation of femtosecond laser pulses. By choice of either a conventional (p) or a composite (p-s) polarizer in the Fourier plane, the shaper setup enables the generation of parallel linearly and orthogonal linearly polarized bichromatic fields. Additional use of a wave plate behind the setup yields co-rotating and counter-rotating circularly polarized bichromatic fields. The scheme allows to independently control the spectral amplitude, phase and polarization profile of the output fields, offering an enormous versatility of bichromatic waveforms.

Modelling of ultrafast coherent strong-field dynamics in potassium with neural networks

We investigate the applicability of neural networks (NNs) for the automated generation of effective computer models for coherent light?matter interactions. The simulation of Autler?Townes doublets from strong-field ionization of potassium atoms is chosen as a test system that exhibits distinct quantum-mechanical effects. Shaped femtosecond laser pulses are employed for studying the response of a quantum-mechanical system to a large variety of different electric fields, and the resulting data can be used for training a NN. We show that a NN is able to approximate the investigated process in parameter regions sampled by the training data and that it can be employed for the interpolation of control landscapes.

Ultrashort polarization-tailored bichromatic fields from a CEP-stable white light supercontinuum

We apply ultrafast polarization shaping to an ultrabroadband carrier envelope phase (CEP) stable white light supercontinuum to generate polarization-tailored bichromatic laser fields of low-order frequency ratio. The generation of orthogonal linearly and counter-rotating circularly polarized bichromatic fields is achieved by introducing a composite polarizer in the Fourier plane of a 4 f polarization shaper. The resulting Lissajous- and propeller-type polarization profiles are characterized experimentally by cross-correlation trajectories. The scheme provides full control over all bichromatic parameters and allows for individual spectral phase modulation of both colors. Shaper-based CEP control and the generation of tailored bichromatic fields is demonstrated. These bichromatic CEP-stable polarization-shaped ultrashort laser pulses provide a versatile class of waveforms for coherent control experiments.

Control of Ultrafast Electron Dynamics with Shaped Femtosecond Laser Pulses: From Atoms to Solids

In this chapter, we present an introduction to the fundamentals of femtosecond pulse shaping and review recent demonstrations of coherent control by pulse tailoring. We portray control of three-dimensional free-electron wave packets, strong-field control by selective population of dressed states (SPODS) and control of ionization processes in dielectrics. Prototypical spectral phase masks such as polynomial- and sinusoidal functions are discussed and concepts of polarization shaping such as the instantaneous frequency and the instantaneous polarization state are introduced and illustrated on representative examples. In addition, experiments on coherent control are reviewed. Coherence transfer from light to matter is studied on the interference of free-electron wave packets. We analyze control and adaptive optimization of three-dimensional designer free-electron wave packets by polarization shaping. Strong-field control via SPODS is introduced and elucidated on specific realizations via rapid adiabatic passage and photon locking. This concept is extended to strong-field control of the concerted electron-nuclear dynamics in molecules. Finally, we present recent experiments on control of ionization processes in dielectrics.

Coherent control of electrons, atoms and molecules with intense shaped light pulses

We report on a physical mechanism of coherent control with intense shaped femtosecond laser pulses. We study photoelectron spectra from multi-photon ionization of potassium atoms and dimers using tailored femtosecond laser pulses. Our results are interpreted in terms of Selective Population of Dressed States (SPODS). Two realizations of SPODS by Photon Locking (PL) via pulse sequences and Rapid Adiabatic Passage (RAP) via chirped pulses are discussed. New physical mechanisms arise, when both PL and RAP are at play simultaneously. Control by the combined efiect of PL and RAP is studied by mapping out a two-parameter Quantum Control Landscape (QCL) for selective population of dressed states.