© 2014 Elsevier B.V. The broad bandwidth of an isolated attosecond pulse excites a vast number of states simultaneously, and the corresponding absorption features can be monitored with exceptional temporal resolution. Novel transient absorption experiments in gases using isolated attosecond pulses are performed in two regimes, one in which the attosecond pulse is overlapped in time with a near-infrared (NIR) pulse and one in which the NIR pulse follows the attosecond pulse. In the latter regime, the attosecond pulse first interacts with a sample, then the observed absorption features are modified by a NIR pulse, which interacts with the sample well after the attosecond pulse has passed. In these experiments, which seem counterintuitive when compared to conventional transient absorption spectroscopy, the weak attosecond pulse induces a polarization of the medium, which is then perturbed by the time-delayed NIR pulse. Recent measurements demonstrate the rich variety of information that can be extracted in this regime.

Light-induced states in He atoms were characterized using attosecond transient absorption spectroscopy. A 400 as pulse covering the 20-24 eV spectral range serves as the probe pulse, and the effect of a few-cycle near infrared pulse (12 fs, 780 nm) on the absorption spectrum is measured as a function of time delay and near-infrared intensities varying from (5.0 ± 2) × 1010 to (1 ± 0.4) × 1013 W/cm2. Light-induced states resulting from near-infrared coupling of 1s2p to 1s2s, 1s3d, and 1s3s states are observed. Absorption features that likely result from coupling of 1s3p to 1s4s, 1s4d, 1s5s, and 1s5d states are also observed. The light-induced states with the smallest detunings (1s3d and 1s3s) from the dressing frequency may shift to higher frequencies as the dressing intensity is increased. © 2013, Taylor & Francis.

The development of attosecond technology is one of the most significant recent achievements in the field of ultrafast optics; it opens up new frontiers in atomic and molecular spectroscopy and dynamics. A unique attosecond pumpprobe apparatus using a compact Mach-Zehnder interferometer is developed. The interferometer system is compact (∼290 cm²) and completely located outside of the vacuum chamber. The location reduces the mechanical vibration from vacuum components such as turbopumps and roughing pumps. The stability of the interferometer is ∼50 as RMS over 24 hours, stabilized with an active feedback loop. The pump and probe fields can be easily altered to incorporate multiple colors. In the interferometer, double optical gating optics are arranged to generate isolated attosecond pulses with a supercontinuum spectrum. The frequencies of the attosecond pulses can be selected to be in the extreme ultraviolet (XUV) region (25–55 eV, 140 as) or the vacuum ultraviolet (VUV) region (15–24 eV, ∼400 as) by metal filters. Furthermore, the near infrared probe field (1.65 eV) can be upconverted to the ultraviolet (3.1 eV). The frequency tunability in the XUV and VUV is critical for selecting excited states of target atoms and molecules.

Recording the transmitted spectrum of a weak attosecond pulse through a medium, while a strong femtosecond pulse copropagates at variable delay, probes the strong-field dynamics of atoms, molecules, and solids. Usually, the interpretation of these measurements is based on the assumption of a thin medium. Here, the propagation through a macroscopic medium of helium atoms in the region of fully allowed resonances is investigated both theoretically and experimentally. The propagation has dramatic effects on the transient spectrum even at relatively low pressures (50 mbar) and short propagation lengths (1 mm). The absorption does not evolve monotonically with the product of propagation distance and pressure, but regions with characteristics of Lorentz line shapes and characteristics of Fano line shapes alternate. Criteria are deduced to estimate whether macroscopic effects can be neglected or not in a transient absorption experiment. Furthermore, the theory in the limit of single-atom response yields a general equation for Lorentz- and Fano-type line shapes at variable pulse delay. © 2013 American Physical Society.

Attosecond transient absorption spectroscopy of highly excited states allows investigating the dynamics of both the decay and the light induced coupling between excited states. We present a rigorous quantum mechanical treatment that provides a generalized discussion of the on- and off-resonant decay dynamics, of resonant and non-resonant couplings to either discrete or continua states and the temporal evolution of the quantum beating of the excited wavepackets. The comparison of the model to experimental results obtained in xenon proves its general applicability. © OSA 2015.

The decay of highly excited states of xenon after absorption of extreme ultraviolet light is directly tracked via attosecond transient absorption spectroscopy using a time-delayed near-infrared perturbing pulse. The lifetimes of the autoionizing 5s5p66p and 5s5p67p channels are determined to be (21.9 ± 1.3) fs and (48.4 ± 5.0) fs, respectively. The observed values support lifetime estimates obtained by traditional linewidth measurements. The experiment additionally obtains the temporal evolution of the decay as a function of energy detuning from the resonance center, and a quantum mechanical formalism is introduced that correctly accounts for the observed energy dependence. © 2014 American Physical Society.

Attosecond transient absorption spectra near the energies of autoionizing states are analyzed in terms of the photon coupling mechanisms to other states. In a recent experiment, the autoionization lifetimes of highly excited states of xenon were determined and compared to a simple expression based on a model of how quantum coherence determines the decay of a metastable state in the transient absorption spectrum. Here it is shown that this procedure for extracting lifetimes is more general and can be used in cases involving either resonant or nonresonant coupling of the attosecond-probed autoionizing state to either continua or discrete states by a time-delayed near infrared (NIR) pulse. The fits of theoretically simulated absorption signals for the 6p resonance in xenon (lifetime = 21.1 fs) to this expression yield the correct decay constant for all the coupling mechanisms considered, properly recovering the time signature of twice the autoionization lifetime due to the coherent nature of the transient absorption experiment. To distinguish between these two coupling cases, the characteristic dependencies of the transient absorption signals on both the photon energy and time delay are investigated. Additional oscillations versus delay-time in the measured spectrum are shown and quantum beat analysis is used to pinpoint the major photon-coupling mechanism induced by the NIR pulse in the current xenon experiment: the NIR pulse resonantly couples the attosecond-probed state, 6p, to an intermediate 8s (at 22.563 eV), and this 8s state is also coupled to a neighboring state (at 20.808 eV).

Electronic wavepackets composed of multiple bound excited states of atomic neon lying between 19.6 and 21.5 eV are launched using an isolated attosecond pulse. Individual quantum beats of the wavepacket are detected by perturbing the induced polarization of the medium with a time-delayed few-femtosecond near-infrared (NIR) pulse via coupling the individual states to multiple neighboring levels. All of the initially excited states are monitored simultaneously in the attosecond transient absorption spectrum, revealing Lorentzian to Fano lineshape spectral changes as well as quantum beats. The most prominent beating of the several that were observed was in the spin-orbit split 3d absorption features, which has a 40 femtosecond period that corresponds to the spin-orbit splitting of 0.1 eV. The few-level models and multilevel calculations confirm that the observed magnitude of oscillation depends strongly on the spectral bandwidth and tuning of the NIR pulse and on the location of possible coupling states.