Highly versatile, two-color setup for high-order harmonic generation using spatial light modulators.

We present a novel, interferometric, two-color, high-order harmonic generation setup based on a turn-key Ytterbium-doped femtosecond laser source and its second harmonic. Each interferometer arm contains a spatial light modulator with individual capabilities to manipulate the spatial beam profiles and to stabilize the relative delay between the fundamental and the second harmonic. In addition, separate control of the relative power and focusing geometries of the two color beams is implemented to conveniently perform automated scans of multiple parameters. A live diagnostics system gives continuous information during ongoing measurements.

Sub-cycle ionization dynamics revealed by trajectory resolved, elliptically-driven high-order harmonic generation.

The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-cycle change of the initial velocity distribution of the electron and its excursion time. The resonant enhancement is observed only for the long trajectory contribution of a particular harmonic when a window resonance in argon, which is off-resonant in the field-free case, is shifted into resonance due to a large dynamic Stark shift.

Spectral phase measurement of a Fano resonance using tunable attosecond pulses.

Electron dynamics induced by resonant absorption of light is of fundamental importance in nature and has been the subject of countless studies in many scientific areas. Above the ionization threshold of atomic or molecular systems, the presence of discrete states leads to autoionization, which is an interference between two quantum paths: direct ionization and excitation of the discrete state coupled to the continuum. Traditionally studied with synchrotron radiation, the probability for autoionization exhibits a universal Fano intensity profile as a function of excitation energy. However, without additional phase information, the full temporal dynamics cannot be recovered. Here we use tunable attosecond pulses combined with weak infrared radiation in an interferometric setup to measure not only the intensity but also the phase variation of the photoionization amplitude across an autoionization resonance in argon. The phase variation can be used as a fingerprint of the interactions between the discrete state and the ionization continua, indicating a new route towards monitoring electron correlations in time.

Attosecond pulse walk-off in high-order harmonic generation.

We study the influence of the generation conditions on the group delay of attosecond pulses in high-order harmonic generation in gases. The group delay relative to the fundamental field is found to decrease with increasing gas pressure in the generation cell, reflecting a temporal walk-off due to the dispersive properties of the nonlinear medium. This effect is well reproduced using an on-axis phase-matching model of high-order harmonic generation in an absorbing gas.

Macroscopic effects in noncollinear high-order harmonic generation.

We study two-color high-order harmonic generation using an intense driving field and its weak second harmonic, crossed under a small angle in the focus. Employing sum- and difference-frequency generation processes, such a noncollinear scheme can be used to measure and control macroscopic phase matching effects by utilizing a geometrical phase mismatch component, which depends on the noncollinear angle. We further show how spatial phase effects in the generation volume are mapped out into the far field allowing a direct analogy with temporal carrier envelope effects in attosecond pulse generation.

High-order harmonic generation using a high-repetition-rate turnkey laser.

We generate high-order harmonics at high pulse repetition rates using a turnkey laser. High-order harmonics at 400 kHz are observed when argon is used as target gas. In neon, we achieve generation of photons with energies exceeding 90 eV (∼13 nm) at 20 kHz. We measure a photon flux of up to 4.4 × 10(10) photons per second per harmonic in argon at 100 kHz. Many experiments employing high-order harmonics would benefit from higher repetition rates, and the user-friendly operation opens up for applications of coherent extreme ultra-violet pulses in new research areas.

Efficient high-order harmonic generation boosted by below-threshold harmonics.

High-order harmonic generation (HHG) in gases has been established as an important technique for the generation of coherent extreme ultraviolet (XUV) pulses at ultrashort time scales. Its main drawback, however, is the low conversion efficiency, setting limits for many applications, such as ultrafast coherent imaging, nonlinear processes in the XUV range, or seeded free electron lasers. Here we introduce a novel scheme based on using below-threshold harmonics, generated in a "seeding cell", to boost the HHG process in a "generation cell", placed further downstream in the focused laser beam. By modifying the fundamental driving field, these low-order harmonics alter the ionization step of the nonlinear HHG process. Our dual-cell scheme enhances the conversion efficiency of HHG, opening the path for the realization of robust intense attosecond XUV sources.

Probing single-photon ionization on the attosecond time scale.

We study photoionization of argon atoms excited by attosecond pulses using an interferometric measurement technique. We measure the difference in time delays between electrons emitted from the 3s(2) and from the 3p(6) shell, at different excitation energies ranging from 32 to 42 eV. The determination of photoemission time delays requires taking into account the measurement process, involving the interaction with a probing infrared field. This contribution can be estimated using a universal formula and is found to account for a substantial fraction of the measured delay.

Attosecond electron spectroscopy using a novel interferometric pump-probe technique.

We present an interferometric pump-probe technique for the characterization of attosecond electron wave packets (WPs) that uses a free WP as a reference to measure a bound WP. We demonstrate our method by exciting helium atoms using an attosecond pulse (AP) with a bandwidth centered near the ionization threshold, thus creating both a bound and a free WP simultaneously. After a variable delay, the bound WP is ionized by a few-cycle infrared laser precisely synchronized to the original AP. By measuring the delay-dependent photoelectron spectrum we obtain an interferogram that contains both quantum beats as well as multipath interference. Analysis of the interferogram allows us to determine the bound WP components with a spectral resolution much better than the inverse of the AP duration.

Phase measurement of resonant two-photon ionization in helium.

We study resonant two-color two-photon ionization of helium via the 1s3p (1)P(1) state. The first color is the 15th harmonic of a tunable Ti:sapphire laser, while the second color is the fundamental laser radiation. Our method uses phase-locked high-order harmonics to determine the phase of the two-photon process by interferometry. The measurement of the two-photon ionization phase variation as a function of detuning from the resonance and intensity of the dressing field allows us to determine the intensity dependence of the transition energy.

Spectral signature of short attosecond pulse trains.

We report experimental measurements of high-order harmonic spectra generated in Ar using a carrier-envelope-offset (CEO) stabilized 12 fs, 800 nm laser field and a fraction (less than 10%) of its second harmonic. Additional spectral peaks are observed between the harmonic peaks, which are due to interferences between multiple pulses in the train. The position of these peaks varies with the CEO and their number is directly related to the number of pulses in the train. An analytical model, as well as numerical simulations, support our interpretation.

Photoemission electron microscopy using extreme ultraviolet attosecond pulse trains.

We report the first experiments carried out on a new imaging setup, which combines the high spatial resolution of a photoemission electron microscope (PEEM) with the temporal resolution of extreme ultraviolet (XUV) attosecond pulse trains. The very short pulses were provided by high-harmonic generation and used to illuminate lithographic structures and Au nanoparticles, which, in turn, were imaged with a PEEM resolving features below 300 nm. We argue that the spatial resolution is limited by the lack of electron energy filtering in this particular demonstration experiment. Problems with extensive space charge effects, which can occur due to the low probe pulse repetition rate and extremely short duration, are solved by reducing peak intensity while maintaining a sufficient average intensity to allow imaging. Finally, a powerful femtosecond infrared (IR) beam was combined with the XUV beam in a pump-probe setup where delays could be varied from subfemtoseconds to picoseconds. The IR pump beam could induce multiphoton electron emission in resonant features on the surface. The interaction between the electrons emitted by the pump and probe pulses could be observed.

Coherent electron scattering captured by an attosecond quantum stroboscope.

We demonstrate a quantum stroboscope based on a sequence of identical attosecond pulses that are used to release electrons into a strong infrared (IR) laser field exactly once per laser cycle. The resulting electron momentum distributions are recorded as a function of time delay between the IR laser and the attosecond pulse train using a velocity map imaging spectrometer. Because our train of attosecond pulses creates a train of identical electron wave packets, a single ionization event can be studied stroboscopically. This technique has enabled us to image the coherent electron scattering that takes place when the IR field is sufficiently strong to reverse the initial direction of the electron motion causing it to rescatter from its parent ion.

Attosecond control of ionization by wave-packet interference.

A train of attosecond pulses, synchronized to an infrared (IR) laser field, is used to create a series of electron wave packets (EWPs) that are below the ionization threshold in .helium. The ionization probability is found to strongly oscillate with the delay between the IR and attosecond fields twice per IR laser cycle. Calculations that reproduce the experimental results demonstrate that this ionization control results from interference between transiently bound EWPs created by different pulses in the train. In this way, we are able to observe, for the first time, attosecond wave-packet interference in a strongly driven atomic system.

Attosecond pulse trains generated using two color laser fields.

We investigate the spectral and temporal structure of high harmonic emission from argon exposed to an infrared laser field and its second harmonic. For a wide range of generating conditions, trains of attosecond pulses with only one pulse per infrared cycle are generated. The synchronization necessary for producing such trains ensures that they have a stable pulse-to-pulse carrier envelope phase, unlike trains generated from one color fields, which have two pulses per cycle and a pi phase shift between consecutive pulses. Our experiment extends the generation of phase stabilized few cycle pulses to the extreme ultraviolet regime.

Reconstruction of attosecond pulse trains using an adiabatic phase expansion.

We propose a new method to reconstruct the electric field of attosecond pulse trains. The phase of the high-order harmonic emission electric field is Taylor expanded around the maximum of the laser pulse envelope in the time domain and around the central harmonic in the frequency domain. Experimental measurements allow us to determine the coefficients of this expansion and to characterize the radiation with attosecond accuracy over a femtosecond time scale. The method gives access to pulse-to-pulse variations along the train, including the timing, the chirp, and the attosecond carrier envelope phase.

Attosecond electron wave packet dynamics in strong laser fields.

We use a train of sub-200 attosecond extreme ultraviolet (XUV) pulses with energies just above the ionization threshold in argon to create a train of temporally localized electron wave packets. We study the energy transfer from a strong infrared (IR) laser field to the ionized electrons as a function of the delay between the XUV and IR fields. When the wave packets are born at the zero crossings of the IR field, a significant amount of energy (approximately 20 eV) is transferred from the field to the electrons. This results in dramatically enhanced above-threshold ionization in conditions where the IR field alone does not induce any significant ionization. Because both the energy and duration of the wave packets can be varied independently of the IR laser, they are valuable tools for studying and controlling strong-field processes.

Time-frequency characterization of femtosecond extreme ultraviolet pulses.

We present energy-resolved cross-correlation measurements of an extreme ultraviolet (XUV) pulse, generated as the fifth harmonic (15.5 eV) of an intense 80 fs laser pulse centered at 400 nm. Spectrally resolving the cross-correlation signal allows us to characterize the time-dependent frequency of the XUV pulse. We find that the fifth harmonic has a small negative chirp in excess of that predicted by perturbation theory. In addition, by manipulating the chirp of the driving laser we can induce and measure a positive or a negative chirp on the XUV pulse.