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Ionization is the dominant response of atoms and molecules to intense laser fields and is at the basis of several important techniques, such as the generation of attosecond pulses that allow the measurement of electron motion in real time. We present experiments in which metastable xenon atoms were ionized with intense 7-micrometer laser pulses from a free-electron laser. Holographic structures were observed that record underlying electron dynamics on a sublaser-cycle time scale, enabling photoelectron spectroscopy with a time resolution of almost two orders of magnitude higher than the duration of the ionizing pulse.

It is well established that electrons can escape from atoms through tunneling under the influence of strong laser fields, but the timing of the process has been controversial and far too rapid to probe in detail. We used attosecond angular streaking to place an upper limit of 34 attoseconds and an intensity-averaged upper limit of 12 attoseconds on the tunneling delay time in strong field ionization of a helium atom. The ionization field derives from 5.5-femtosecond-long near-infrared laser pulses with peak intensities ranging from 2.3 x 10(14) to 3.5 x 10(14) watts per square centimeter (corresponding to a Keldysh parameter variation from 1.45 to 1.17, associated with the onset of efficient tunneling). The technique relies on establishing an absolute reference point in the laboratory frame by elliptical polarization of the laser pulse, from which field-induced momentum shifts of the emergent electron can be assigned to a temporal delay on the basis of the known oscillation of the field vector.

We present an analytical expression for the observed signal in time- and phase-resolved pump-probe studies, with particular emphasis on terahertz time-domain spectroscopy. Maxwell's equations are solved for the response of damped, harmonic oscillators to a driving probe field in the perturbative regime. Our analytical expressions agree with the one previously reported in the literature [Nemec et al., J. Chem. Phys. 122, 104503 (2005)] in the Drude limit; however, they differ in the case of a vibrational resonance.

Atoms exposed to intense light lose one or more electrons and become ions. In strong fields, the process is predicted to occur via tunnelling through the binding potential that is suppressed by the light field near the peaks of its oscillations. Here we report the real-time observation of this most elementary step in strong-field interactions: light-induced electron tunnelling. The process is found to deplete atomic bound states in sharp steps lasting several hundred attoseconds. This suggests a new technique, attosecond tunnelling, for probing short-lived, transient states of atoms or molecules with high temporal resolution. The utility of attosecond tunnelling is demonstrated by capturing multi-electron excitation (shake-up) and relaxation (cascaded Auger decay) processes with subfemtosecond resolution.

A theoretical investigation is presented that examines the wavelength scaling from near-visible (0.8 micro m) to midinfrared (2 micro m) of the photoelectron distribution and high harmonics generated by a "single" atom in an intense electromagnetic field. The calculations use a numerical solution of the time-dependent Schrödinger equation (TDSE) in argon and the strong-field approximation in helium. The scaling of electron energies (lambda2), harmonic cutoff (lambda2), and attochirp (lambda -1) agree with classical mechanics, but it is found that, surprisingly, the harmonic yield follows a lambda -(5-6) scaling at constant intensity. In addition, the TDSE results reveal an unexpected contribution from higher-order returns of the rescattering electron wave packet.

The exposure of molecules to short, ultrastrong electric fields leads to multiple ionization and a subsequent Coulomb explosion. We present a comparative study where uracil molecules are exposed to fields generated by high-power laser pulses (tau approximately 75 fs, I > 10(16) W/cm2) or swift highly charged ions (0.5 MeV Xe25+) representing a half-cycle pulse of less than 10 fs duration. Molecular dynamics and structural information contained in the fragmentation pathways can be assessed separately. Despite the similar field strengths large differences in fragment kinetic energies are found which are related to field shape and duration with the aid of molecular dynamics simulations.

The generation of attosecond pulses by superposition of high harmonics relies on their synchronization in the emission. Our experiments in the low-order, plateau, and cutoff regions of the spectrum reveal different regimes in the electron dynamics determining the synchronization quality. The shortest pulses are obtained by combining a spectral filtering of harmonics from the end of the plateau and the cutoff, and a far-field spatial filtering that selects a single electron quantum path contribution to the emission. This method applies to isolated pulses as well as pulse trains.

We have studied the ionization of Rydberg atoms by few-cycle radio-frequency pulses and used two-color fields to control the ionization dynamics. We show that the number of times that electrons are emitted during a pulse can be limited and that the duration of the electron emission can be shortened. These results, once they are transposed to the optical domain, may inspire new strategies for the production of single attosecond pulses.

Subfemtosecond light pulses can be obtained by superposing several high harmonics of an intense laser pulse. Provided that the harmonics are emitted simultaneously, increasing their number should result in shorter pulses. However, we found that the high harmonics were not synchronized on an attosecond time scale, thus setting a lower limit to the achievable x-ray pulse duration. We showed that the synchronization could be improved considerably by controlling the underlying ultrafast electron dynamics, to provide pulses of 130 attoseconds in duration. We discuss the possibility of achieving even shorter pulses, which would allow us to track fast electron processes in matter.

We report experiments on the characterization of a train of attosecond pulses obtained by high-harmonic generation, using mixed-color (XUV+IR) atomic two-photon ionization and electron detection on a velocity map imaging detector. We demonstrate that the relative phase of the harmonics is encoded both in the photoelectron yield and the angular distribution as a function of XUV-IR time delay, thus making the technique suitable for the detection of single attosecond pulses. The timing of the attosecond pulse with respect to the field oscillation of the driving laser critically depends on the target gas used to generate the harmonics.

We report a numerical study of the design of lattice heteropolymers that can refold when the properties of only a few monomers are changed. If we assume that the effect of an external agent on a heteropolymer is to alter the interactions between its constituent monomers, our simulations provide a description of a simple allosteric transition. We characterize the free energy surfaces of the initial and the modified chain molecule. We find that there is a region of conformation space where molecules can be made to refold with minimal free energy cost. This region is accessible by thermal fluctuations. The efficiency of a motor based on such an allosteric transition would be enhanced by "borrowing" heat from the environment in the initial stages of the refolding, and "paying back" later. In fact, the power cycle of many real molecular motors does involve such a borrowing activation step.

Available data may reflect a true but unknown random variable of interest plus an additive error, which is a nuisance. The problem in predicting the unknown random variable arises in many applied situations where measurements are contaminated with errors; it is known as the regression-to-the-mean problem. There exists a well known solution when both the distributions of the true underlying random variable and the contaminating errors are normal. This solution is given by the classical regression-to-the-mean formula, which has a data-shrinkage interpretation. We discuss the extension of this solution to cases where one or both of these distributions are unknown and demonstrate that the fully nonparametric case can be solved for the case of small contaminating errors. The resulting nonparametric regression-to-the-mean paradigm can be implemented by a straightforward data-sharpening algorithm that is based on local sample means. Asymptotic justifications and practical illustrations are provided.

The absolute timing of the high-harmonic attosecond pulse train with respect to the generating IR pump cycle has been measured for the first time. The attosecond pulses occur 190+/-20 as after each pump field maxima (twice per optical cycle), in agreement with the "short" quantum path of the quasiclassical model of harmonic generation.

The asymptotic velocity distribution of electrons ionized in half-cycle-pulse excitation of high Rydberg states (n=34), placed in a static electric field, is studied using electron velocity-map imaging. At weak half-cycle pulse strengths, the electrons escape over the saddle point in the potential. For strong half-cycle pulses, the electrons are emitted in the direction of the field kick. The much slower and less intense half cycle of opposite polarity, which necessarily follows the main half-cycle pulse, strongly affects the momentum distribution and reduces the excess energy of the electrons significantly.

In principle, the temporal beating of superposed high harmonics obtained by focusing a femtosecond laser pulse in a gas jet can produce a train of very short intensity spikes, depending on the relative phases of the harmonics. We present a method to measure such phases through two-photon, two-color photoionization. We found that the harmonics are locked in phase and form a train of 250-attosecond pulses in the time domain. Harmonic generation may be a promising source for attosecond time-resolved measurements.

Coherent dynamic x-ray scattering has been used to study the thermally excited layer fluctuations in freely suspended smectic films of the compound 4O.8. Using 8-keV x rays and films with a thickness around 0.3 &mgr;m we resolve relaxation times down to a few &mgr;s. A combination of damped and oscillatory behavior is observed for the layer undulations, which can be attributed to inertial effects. These are due to the surface contribution to the free energy which cannot be disregarded for thin films.