Frustrated tunneling ionization (FTI) has recently been identified as a mechanism behind the strong-field excitation of atoms and molecules. Based on a classical notion, it offers a time-dependent view on atomic excitation and supports the existence of bound, nearly-stable states in strong laser fields. FTI completes the pantheon of important strong-field phenomena arising from non-perturbative interaction. It has sparked a renewed interest in strong-field excitation and illuminates related processes comprising strong field dissociation and ionization of molecules and coherent generation of EUV radiation. FTI naturally links the internal and the macroscopic dynamics, offering an understanding of the surprising strong-field acceleration of neutral atoms, the observation of which was made possible by a momentum-selective direct detection of neutral excited atoms. In an SFA approach using Kramers-Henneberger basis states we rigorously establish FTI as a quantum mechanical tunneling process into the Kramers-Henneberger states. Remarkably, the SFA approach is governed by an analog of the Keldysh parameter, describing the transition from tunneling to multiphoton excitation similar to the strong-field ionization. With the ability to measure the center-of-mass (CM) momentum we discuss the possibility to use the CM degrees of freedom of atoms and molecules as a "built-in" monitoring device for observing their internal dynamics in non-perturbative laser fields.

The structure and photoexcitation dynamics of high lying doubly excited states of the strontium atom with high angular momenta are studied in the vicinity of the Sr$^+(N=5)$ threshold. The spectra recorded using resonant multiphoton isolated core excitation are analyzed with calculations based on configuration interaction with exterior complex scaling, which treats the correlated motion of the two valence electrons of Sr from first principles. The results are rationalized with a model based on multichannel quantum-defect theory and transition dipole moments calculated with a perturbative treatment of electron correlations. Together, both approaches reveal that most of the lines observed in the spectra arise from the interaction of a single optically active state, coupled to the initial state by an electric-dipole transition, with entire doubly-excited Rydberg series. The long-range electron correlations responsible for this interaction unexpectedly vanish for identical values of the initial and final principal quantum numbers, a fact related to the quasi hydrogenic nature of the high-$l$ Rydberg electron. This special situation, and in particular the vanishing interaction, leads to the surprising observation of an electric \emph{quadrupole} isolated-core excitation with a similar intensity as the neighboring electric dipole transitions.

The extension of nonlinear spectroscopic techniques into the x-ray domain is in its infancy but holds the promise to provide unique insight into the dynamics of charges in photoexcited processes, which are of fundamental as well as applied interest. We report on the observation of a third order nonlinear process in lithium fluoride at a free-electron laser. Exploring the yield of four wave mixing (FWM) in resonance with transitions to strongly localized core exciton states vs. delocalized Bloch states, we find resonant FWM to be a sensitive probe for the degree of charge localization: substantial sum- and difference-frequency generation is observed exclusively when in a one- or three-photon resonance with a LiF core exciton, with a dipole forbidden transition affecting details of the nonlinear response. Our reflection-geometry-based approach to detect FWM signals enables the study of a wide variety of condensed matter sample systems, provides atomic selectivity via resonant transitions and can be easily scaled to shorter wavelengths at free electron x-ray lasers.

In a combined experimental and theoretical study we investigate the 7 dnl and 8pnl (n 11,1 = 9-12) doubly excited planetary states of Sr. The experimental spectrum was obtained using a five-photon resonant excitation scheme. The method of configuration interaction with exterior complex scaling was used to compute the energy-level structure and dynamics of the two highly excited electrons from first principles. Good quantitative agreement was obtained with the spectra we recorded, and the theoretical calculations shed light on their complex structure and the signatures of electron correlations therein. The two-electron probability densities we calculated reveal the strongly correlated angular motion of the two electrons in the 7dnl and 8pnl planetary states, and confirm quantitatively the predictions of the frozen-planet approximation describing electron dynamics as the polarization of the fast inner electron by the electric field of the outer "frozen" electron.

Addressing the ultrafast coherent evolution of electronic wave functions has long been a goal of nonlinear x-ray physics. A first step toward this goal is the investigation of stimulated x-ray Raman scattering (SXRS) using intense pulses from an x-ray free-electron laser. Earlier SXRS experiments relied on signal amplification during pulse propagation through dense resonant media. By contrast, our method reveals the fundamental process in which photons from the primary radiation source directly interact with a single atom. We introduce an experimental protocol in which scattered neutral atoms rather than scattered photons are detected. We present SXRS measurements at the neon K edge and a quantitative theoretical analysis. The method should become a powerful tool in the exploration of nonlinear x-ray physics.

Observation of internal quantum dynamics relies on correlations between the system being observed and the measurement apparatus. We propose using the c.m. degrees of freedom of atoms and molecules as a "built-in" monitoring device for observing their internal dynamics in nonperturbative laser fields. We illustrate the idea on the simplest model system-the hydrogen atom in an intense, tightly focused infrared laser beam. To this end, we develop a numerically tractable, quantum-mechanical treatment of correlations between internal and c.m. dynamics. We show that the transverse momentum records the time excited states experience the field, allowing femtosecond reconstruction of the strong-field excitation process. The ground state becomes weak-field seeking, an unambiguous and long sought-for signature of the Kramers-Henneberger regime.

Atomic excitation in strong optical laser fields has been found to take place even at intensities exceeding saturation. The concomitant acceleration of the atom in the focused laser field has been considered a strong link to, if not proof of, the existence of the so-called Kramers-Henneberger (KH) atom, a bound atomic system in an intense laser field. Recent findings have moved the importance of the KH atom from being purely of theoretical interest toward real world applications; for instance, in the context of laser filamentation. Considering this increasing importance, we explore the limits of strong-field excitation in optical fields, which are basically imposed by ionization through the spatial field envelope and the field propagation.

Excitation and ionization in strong laser fields lies at the heart of such diverse research directions as high-harmonic generation and spectroscopy, laser-induced diffraction imaging, emission of femtosecond electron bunches from nanotips, self-guiding, filamentation and mirrorless lasing during propagation of light in atmospheres. While extensive quantum mechanical and semiclassical calculations on strong-field ionization are well backed by sophisticated experiments, the existing scattered theoretical work aiming at a full quantitative understanding of strong-field excitation lacks experimental confirmation. Here we present experiments on strong-field excitation in both the tunneling and multiphoton regimes and their rigorous interpretation by time dependent Schrödinger equation calculations, which finally consolidates the seemingly opposing strong-field regimes with their complementary pictures. Most strikingly, we observe an unprecedented enhancement of excitation yields, which opens new possibilities in ultrafast strong-field control of Rydberg wave packet excitation and laser intensity characterization.

Atomic excitation in the tunneling regime of a strong-field laser-matter interaction has been recently observed. It is conveniently explained by the concept of frustrated tunneling ionization (FTI), which naturally evolves from the well-established tunneling picture followed by classical dynamics of the electron in the combined laser field and Coulomb field of the ionic core. Important predictions of the FTI model such as the n distribution of Rydberg states after strong-field excitation and the dependence on the laser polarization have been confirmed in experiments. The model also establishes a sound basis to understand strong-field acceleration of neutral atoms in strong laser fields. The experimental observation has become possible recently and initiated a variety of experiments such as atomic acceleration in an intense standing wave and the survival of Rydberg states in strong laser fields. Furthermore, the experimental investigations on strong-field dissociation of molecules, where neutral excited fragments after the Coulomb explosion of simple molecules have been observed, can be explained. In this review, we introduce the subject and give an overview over relevant experiments supplemented by new results.

Frustrated tunneling ionization (FTI) has recently been found to be an important exit channel of atomic strong-field ionization models such as the simple man's or rescattering model if one considers the Coulomb field explicitly. It leads to the population of bound excited states rather than to ionization after the electron has tunneled and quivered in the laser field. In this chapter we introduce the FTI model and describe experiments whose outcome supports its importance. In particular, we focus on strong-field excitation of atoms and the observation of neutral (ionic) excited fragments with high kinetic energy in strong-field fragmentation and Coulomb explosion of small molecules. Furthermore, we present experiments in which a direct position sensitive detection of excited neutral atoms reveals the exceptionally high acceleration of atoms in short pulsed strongly focused laser fields and discuss possible applications.

Using field ionization combined with the direct detection of excited neutral atoms we measured the distribution of principal quantum number n of excited He Rydberg states after strong-field excitation at laser intensities well in the tunneling regime. Our results confirm theoretical predictions from semiclassical and quantum mechanical calculations and simultaneously underpin the validity of the semiclassical frustrated tunneling ionization model. Moreover, since our experimental detection scheme is spin sensitive in the case of He atoms, we show that strong-field excitation leads to strong population of triplet states. The origin of it lies in the fact that high angular momentum states are accessible in strong-field excitation. Thus, singlet-triplet transitions become possible due to the increased importance of spin-orbit interaction rather than due to direct laser induced spin-flip processes.

We investigated the principal quantum number n distribution of excited states resulting from the interaction of Helium with strong, short laser pulses. We find excellent agreement with predictions of the semiclassical frustrated tunneling ionization (FTI) model [1] as well as fully quantum mechanical calculations. Furthermore, the excitation process directly populates triplet excited states due to the breakdown of the Russel-Saunders coupling scheme for high orbital angular momentum l states of Helium, which are predominantly populated in the strong laser field.

The seminal strong-field tunnelling theory introduced by L V Keldysh plays a pivotal role. It has shaped our understanding of atomic strong-field processes, where it represents the first step in complex ionisation dynamics and provides reliable tunnelling rates. Tunnelling rates, however, cannot be necessarily equated with ionisation rates. Taking into account the electron dynamics in the Coulomb potential following the tunnelling process, the process of frustrated tunnelling ionisation has been found to lead to excited Rydberg atoms. Here, we excite He atoms in the strong-field tunnelling regime into Rydberg states. A high percentage of these Rydberg atoms survive in high intensity laser fields. We exploit this fact together with their high polarisability to kinematically manipulate the Rydberg atoms with a second elliptically polarised focused strong laser field. By varying the spatial overlap of the two laser foci, we are able to selectively control the deflection of the Rydberg atoms. The results of semi-classical calculations, which are based on the frustrated tunnelling model and on the ponderomotive acceleration, are in accord with our experimental data.

Laser induced strong-field phenomena in atoms and molecules on the femtosecond (fs) time scale have been almost exclusively investigated with traveling wave fields. In almost all cases, approximation of the strong electromagnetic field by an electric field purely oscillating in time suffices to describe experimental observations. Spatially dependent electromagnetic fields, as they occur in a standing light wave, allow for strong energy and momentum transfer and are expected to extend strong-field dynamics profoundly. Here we report a strong-field version of the Kapitza-Dirac effect for neutral atoms where we scatter neutral He atoms in an intense short pulse standing light wave with fs duration and intensities well in the strong-field tunneling regime. We observe substantial longitudinal momentum transfer concomitant with an unprecedented atomic photon scattering rate greater than 10(16)s(-1).

The idea of atoms defying ionization in ultrastrong laser fields has fascinated physicists for the last three decades. In contrast to extensive theoretical work on atoms stabilized in strong fields only few experiments limited to intermediate intensities have been performed. In this work we show exceptional stability of Rydberg atoms in strong laser fields extending the range of observation to much higher intensities. Corresponding field amplitudes of more than 1 GV/cm exceed the thresholds for static field ionization by more than 6 orders of magnitude. Most importantly, however, is our finding that a surviving atom is tagged with a measure of the laser intensity it has interacted with. Reading out this information removes uncertainty about whether the surviving atom has really seen the high intensity. The experimental results allow for an extension of the investigations on the stabilization and interaction of a quasifree electron with a strong field into the relativistic regime.

We report on strong-field excitation of He atoms with two interfering laser pulses of various polarization. The results are explained within the frustrated tunneling ionization model which describes multi-photon excitation in the strong-field tunneling regime.

We present a theoretical quasiclassical treatment of the formation, during Coulomb explosion, of highly excited neutral H atoms (H*) for strongly driven H-2. This process, where after the laser field is turned off, one electron escapes to the continuum while the other occupies a Rydberg state, was recently reported in an experimental study [B. Manschwetus et al., Phys. Rev. Lett. 102, 113002 (2009)]. We find that two-electron effects are important in order to correctly account for all pathways leading to H* formation. We identify two pathways where the electron that escapes to the continuum does so either very quickly or after remaining bound for a few periods of the laser field. These two pathways of H* formation have distinct traces in the probability distribution of the escaping electron momentum components.

A new technique to investigate laser driven ion acceleration with fully isolated, mass-limited glass spheres with a diameter down to 8μm is presented. A Paul trap was used to prepare a levitating glass sphere for the interaction with a laser pulse of relativistic intensity. Narrow-bandwidth energy spectra of protons and oxygen ions have been observed and were attributed to specific acceleration field dynamics in case of the spherical target geometry. A general limiting mechanism has been found that explains the experimentally observed ion energies for the mass-limited target.

We report on our experiments on laser-driven ion acceleration using fully isolated mass-limited spheres with a diameter down to 8 mu m for the first time. Two-dimensional (2D) particle-in-cell (PIC) and hydro-code simulations were used to show that the pre-plasma at both the front and rear sides of the target strongly affect the efficiency of the ion acceleration. The mechanism of the plasma flow around mass-limited targets has not yet been identified for laser-driven ion acceleration. Our models indicate that this effect is the cause of the observed limitation to the ion-beam energy in both previous experiments and in our own.