Chirp-control of resonant high-order harmonic generation in indium ablation plumes driven by intense few-cycle laser pulses.

We have studied high-order harmonic generation (HHG) in an indium ablation plume driven by intense few-cycle laser pulses centered at 775 nm as a function of the frequency chirp of the laser pulse. We found experimentally that resonant emission lines between 19.7 eV and 22.3 eV (close to the 13th and 15th harmonic of the laser) exhibit a strong, asymmetric chirp dependence, with pronounced intensity modulations. The chirp dependence is reproduced by our numerical time-dependent Schrödinger equation simulations of a resonant HHG by the model indium ion. As demonstrated with our separate simulations of HHG within the strong field approximation, the resonance can be understood in terms of the chirp-dependent HHG photon energy coinciding with the energy of an autoionizing state to ground state transition with high oscillator strength. This supports the validity of the general theory of resonant four-step HHG in the few-cycle limit.

Attosecond physics at the nanoscale.

Recently two emerging areas of research, attosecond and nanoscale physics, have started to come together. Attosecond physics deals with phenomena occurring when ultrashort laser pulses, with duration on the femto- and sub-femtosecond time scales, interact with atoms, molecules or solids. The laser-induced electron dynamics occurs natively on a timescale down to a few hundred or even tens of attoseconds (1 attosecond = 1 as = 10-18 s), which is comparable with the optical field. For comparison, the revolution of an electron on a 1s orbital of a hydrogen atom is ∼152 as. On the other hand, the second branch involves the manipulation and engineering of mesoscopic systems, such as solids, metals and dielectrics, with nanometric precision. Although nano-engineering is a vast and well-established research field on its own, the merger with intense laser physics is relatively recent. In this report on progress we present a comprehensive experimental and theoretical overview of physics that takes place when short and intense laser pulses interact with nanosystems, such as metallic and dielectric nanostructures. In particular we elucidate how the spatially inhomogeneous laser induced fields at a nanometer scale modify the laser-driven electron dynamics. Consequently, this has important impact on pivotal processes such as above-threshold ionization and high-order harmonic generation. The deep understanding of the coupled dynamics between these spatially inhomogeneous fields and matter configures a promising way to new avenues of research and applications. Thanks to the maturity that attosecond physics has reached, together with the tremendous advance in material engineering and manipulation techniques, the age of atto-nanophysics has begun, but it is in the initial stage. We present thus some of the open questions, challenges and prospects for experimental confirmation of theoretical predictions, as well as experiments aimed at characterizing the induced fields and the unique electron dynamics initiated by them with high temporal and spatial resolution.

Beyond carbon K-edge harmonic emission using a spatial and temporal synthesized laser field.

We present numerical simulations of high-order harmonic generation in helium using a temporally synthesized and spatially nonhomogeneous strong laser field. The combination of temporal and spatial laser field synthesis results in a dramatic cutoff extension far beyond the usual semiclassical limit. Our predictions are based on the convergence of three complementary approaches: resolution of the three dimensional time dependent Schrödinger equation, time-frequency analysis of the resulting dipole moment, and classical trajectory extraction. A laser field synthesized both spatially and temporally has been proven capable of generating coherent extreme ultraviolet photons beyond the carbon K edge, an energy region of high interest as it can be used to initiate inner-shell dynamics and study time-resolved intramolecular attosecond spectroscopy.

Isolated sub-fs XUV pulse generation in Mn plasma ablation.

We report studies of high-order harmonic generation in laser-produced manganese plasmas using sub-4-fs drive laser pulses. The measured spectra exhibit resonant enhancement of a small spectral region of about 2.5 eV width around the 31st harmonic (~50eV). The intensity contrast relative to the directly adjacent harmonics exceeds one order of magnitude. This finding is in sharp contrast to the results reported previously for multi-cycle laser pulses [Physical Review A 76, 023831 (2007)]. Theoretical modelling suggests that the enhanced harmonic emission forms an isolated sub-femtosecond pulse.

Enhancement of high harmonics from plasmas using two-color pump and chirp variation of 1 kHz Ti:sapphire laser pulses.

We have investigated resonance effects in high-order harmonic generation (HHG) within laser-produced plasmas. We demonstrate a significantly improved harmonic yield by using two-color pump-induced enhancement and a 1 kHz pulse repetition rate. Together with an increased HHG output, the even harmonics in the cutoff region were enhanced with respect to odd harmonics. We report the observation of a resonance-induced growth in intensity of 20th harmonic in silver plasma (2×), 26th harmonic in vanadium plasma (4×), and 28th harmonic in chromium plasma (5×).

Valley in the efficiency of the high-order harmonic yield at ultra-high laser intensities.

We study the process of high-order harmonic generation using laser pulses with non-adiabatic turn-on and intensities well above saturation. As a main point, we report the existence of a valley structure in the efficiency of single-atom high-order harmonic generation with increasing laser intensities. Consequently, after an initial decrease, the high-frequency radiation yield is shown to increase for higher intensities, returning to a level similar to the case below saturation. Such behavior contradicts the general belief of a progressive degradation of the harmonic emission at ultrahigh intensities, based on the experience with pulses with smoother turn-on. We shall show that this behavior corresponds to the emergence of a new pathway for high-order harmonic generation, which takes place during the pulse turn-on. Our study combines trajectory analysis, wavelet techniques and the numerical integration of 3-Dimensional Time Dependent Schrödinger Equation. The increase in efficiency raises the possibility of employing ultrahigh intensities to generate high-frequency radiation beyond the water window.

Self-compression controlled by the chirp of the input pulse.

Self-compressed (SC) pulses have been achieved through the filamentation process in air without any additional dispersion compensation, using the input pulse chirp as the control parameter. For any studied input pulse energy (3-5 mJ), we have found two opposite sign input group-delay dispersion values for which SC pulses can be achieved systematically. In addition, we have observed that the energy coupled into the inner core of the filament is always of the order of 20% of the total input pulse energy, which opens the way to a scalable technique to obtain intense short pulses directly from the filamentation process.

Pulse-length dependence of the anisotropy of laser-driven cluster explosions: transition to the impulsive regime for pulses approaching the few-cycle limit.

We have experimentally observed anisotropic ion emission from Xe and Ar clusters under intense ultrashort (∼30 fs) laser irradiation, with up to 1.8 times more energetic ions emitted in the direction perpendicular to the laser polarization than in the parallel direction. As the pulse length was varied in the range of 8-160 fs, we found this anisotropy to first grow and then diminish. Treating electrons inside the unexpanded cluster as a harmonic oscillator qualitatively demonstrates how intracluster electric field can result in an ion emission anisotropy of this kind. Our observations give direct access to the initial charging dynamics present in the first few cycles of an intense laser field interacting with any nanoscale dielectric.

High harmonic emission from a superposition of multiple unrelated frequency fields.

We report observations and analysis of high harmonic generation driven by a superposition of fields at 1290 nm and 780 nm. These fields are not commensurate in frequency and the superposition leads to an increase in the yield of the mid-plateau harmonics of more than two orders of magnitude compared to using the 1290 nm field alone. Significant extension of the cut-off photon energy is seen even by adding only a small amount of the 780 nm field. These observations are explained by calculations performed in the strong field approximation. Most importantly we find that enhancement is found to arise as a consequence of both increased ionization in the sum-field and modification of the electron trajectories leading to an earlier return time. The enhanced yield even when using modest intensity fields of 5 x 10(13) Wcm(-2) is extended to the 80 eV range and is a promising route to provide a greater photon number for applications in XUV imaging and time-resolved experiments at a high repetition rate.

Spatial fingerprint of quantum path interferences in high order harmonic generation.

We have spatially and spectrally resolved the high order harmonic emission from an argon gas target. Under proper phase matching conditions we were able to observe for the first time the spatial fine structure originating from the interference of the two shortest quantum paths in the harmonic beam. The structure can be explained by the intensity-dependent harmonic phase of the contributions from the two paths. The spatially and spectrally resolved measurements are consistent with previous spatially integrated results. Our measurement method represents a new tool to clearly distinguish between different interference effects and to potentially observe higher order trajectories in the future with improved detection sensitivity. Here, we demonstrate additional experimental evidence that the observed interference pattern is only due to quantum-path interferences and cannot be explained by a phase modulation effect. Our experimental results are fully supported by simulations using the strong field approximation and including propagation.

Ionization effects on spectral signatures of quantum-path interference in high-harmonic generation.

The interference between the emission originating from the short and long electron quantum paths is intrinsic to the high harmonic generation process. We investigate the universal properties of these quantum-path interferences in various generation media and discuss how ionization effects influence the observed interference structures. Our comparison of quantum-path interferences observed in xenon, argon, and neon demonstrates that our experimental tools are generally applicable and should also allow investigating more complex systems such as molecules or clusters.

Quantum path interferences in high-order harmonic generation.

We have investigated the intensity dependence of high-order harmonic generation in argon when the two shortest quantum paths contribute to the harmonic emission. For the first time to our knowledge, experimental conditions were found to clearly observe interference between these two quantum paths that are in excellent agreement with theoretical predictions. This result is a first step towards the direct experimental characterization of the full single-atom dipole moment and demonstrates an unprecedented accuracy of quantum path control on an attosecond time scale.

Spatio-temporal characterization of few-cycle pulses obtained by filamentation.

Intense sub-5-fs pulses were generated by filamentation in a noble gas and subsequent chirped-mirror pulse compression. The transversal spatial dependence of the temporal pulse profile was investigated by spatial selection of parts of the output beam. Selecting the central core of the beam is required for obtaining the shortest possible pulses. Higher energy efficiency is only obtained at the expense of pulse contrast since towards the outer parts of the beam the energy is spread into satellite structures leading to a double-pulse profile on the very off-axis part of the beam. Depending on the requirements for a particular application, a trade-off between the pulse duration and the pulse energy has to be done. The energy of the sub-5-fs pulses produced was sufficient for the generation of high order harmonics in Argon. In addition, full simulation is performed in space and time on pulse propagation through filamentation that explains the double-pulse structure observed as part of a conical emission enhanced by the plasma defocusing.