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Journal of Physics Conference Series

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

M. Wollenhaupt, Tim Bayer, Marc Krug, Cristian Sarpe, Thomas Baumert

Published Nov 1, 2007• 6 citations
Publisher

Abstract

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 effect of PL and RAP is studied by mapping out a two-parameter Quantum Control Landscape (QCL) for selective population of dressed states.

DOI
10.1088/1742-6596/88/1/012053

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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 effect of PL and RAP is studied by mapping out a two-parameter Quantum Control Landscape (QCL) for selective population of dressed states.
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.
We experimentally demonstrate a strong-field coherent control mechanism that combines the advantages of photon locking (PL) and rapid adiabatic passage (RAP). Unlike earlier implementations of PL and RAP by pulse sequences or chirped pulses, we use shaped pulses generated by phase modulation of the spectrum of a femtosecond laser pulse with a generalized phase discontinuity. The novel control scenario is characterized by a high degree of robustness achieved via adiabatic preparation of a state of maximum coherence. Subsequent phase control allows for efficient switching among different target states. We investigate both properties by photoelectron spectroscopy on potassium atoms interacting with the intense shaped light field.
We study the dynamics of potassium atoms in intense laser fields using femtosecond phase-locked pulse pairs in order to extract physical mechanisms of strong field quantum control. The structure of the Autler–Townes (AT) doublet in the photoelectron spectra is measured to analyse transient processes. The analysis shows that the physical mechanism is based on the selective population of dressed states (SPODS). Experimental results of closed loop optimization of SPODS are presented in addition. Applications to decoherence measurements with implications for quantum information are also proposed.
The properties of the photoelectron spectra in two resonant multi-photon ionization process are studied by means of dressed state theory and perturbation theory.The influences on the photoelectron spectra by the area of the first pulse and the delay between two pulses are discussed under strong-field scheme.It is shown that the photoelectron spectra can be modulated by the areas of the two pulses and the delay between them.Control of Autler-Townes doublet and the interferences in doublet can be realized by the area of the first pulse and the delay between the two pulses.The selective population of dressed states(SPODS)also can be realized by this coherent quantum mechanism.The population of dressed states cannot be selected by the area of the second pulse,but obviously it can be modulated.
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 1 eV 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 an uncommon three-state 'bow-tie' level crossing allows the preparation of coherent superposition states.