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Physical Review A

Three-state selective population of dressed states via generalized spectral phase-step modulation

M. Wollenhaupt, Tim Bayer, Nikolay V. Vitanov, Thomas Baumert

Published May 26, 2010• 42 citations
Publisher

Abstract

We present a joint experimental and theoretical study of selective population of dressed states (SPODS) in a three-level system. Control is exerted by shaped intense femtosecond laser pulses generated by a generalized spectral phase-step modulation function. We show that both control parameters (i.e., the phase-step amplitude and position) can be used to switch population among each three dressed states with high selectivity. The dynamics of the system, and hence the resulting photoelectron signal is studied theoretically by analyzing the time evolution of the adiabatic dressed-state energies and populations.

DOI
10.1103/physreva.81.053422

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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 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.
We present the theoretical investigation of photoelectron spectroscopy resulting from the strong field induced multiphoton ionization in a typical three-level ladder-style system. Our theoretical results show that the photo-electron spectral structure can be alternatively steered by spectral phase modulation. This physical mechanism for strong field quantum control is explicitly exploited by the time-dependent dressed state population. It is concluded that the phase-shaped laser pulses can be used to selectively manipulate the multiphoton ionization process in complicated quantum systems.
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.
The resonant dynamic Stark effect, observed in the Autler-Townes (AT) splitting, plays a central role in ultrafast strong-field physics. Recent experiments have demonstrated the phase control of the AT doublet in atomic resonance-enhanced multiphoton ionization using intense resonant shaped femtosecond laser pulses [Bayer et al., Adv. Chem. Phys. 159, 235 (2016)]. Based on a two-state model, we showed that the underlying control mechanism is the selective population of dressed states (SPODS). In this work, we use a numerical model to calculate the photoelectron momentum distribution (PMD) based on the ab initio solution of the two-dimensional (2D) time-dependent Schr\"odinger equation (TDSE) to obtain a more complete physical picture of the nonperturbative control of the AT doublet. The 2D-TDSE model reproduces the ultrafast switching among the AT components while also revealing deviations from the signatures predicted by the two-state model. These deviations are attributed to the influence of additional intermediate states. To rationalize our observations, we propose a refined five-state model that includes all significantly populated bound states from the full calculation and accurately reproduces the 2D PMD. Based on the validated five-state model, we conduct a dressed-state analysis which provides a clear physical picture of the SPODS mechanism in a multistate system and sheds light on the role of the intermediate states in strong-field control.