High-order harmonic generation at high laser intensities beyond the tunnel regime

We present studies of high-order harmonic generation (HHG) at laser intensities well above saturation. We use driving laser pulses which present a particular electron dynamics in the turn-on stage. Our results predict an increasing on the harmonic yield, after an initial dropping, when the laser intensity is increased. This fact contradicts the general belief of a progressive degradation of the harmonic emission at ultrahigh intensities. We have identified a particular set of trajectories which emerges in the turn-on stage of these singular laser pulses, responsible of the unexpected growth on the harmonic efficiency at this high intensity regime. Our study combines two complementary approaches: classical analysis and full quantum mechanical calculations resulting from the numerical integration of the 3-dimensional time-dependent Schr\"odinger equation complemented with the time-frequency analysis

Optimisation of Quantum Trajectories Driven by Strong-field Waveforms

Quasi-free field-driven electron trajectories are a key element of strong-field dynamics. Upon recollision with the parent ion, the energy transferred from the field to the electron may be released as attosecond duration XUV emission in the process of high harmonic generation (HHG). The conventional sinusoidal driver fields set limitations on the maximum value of this energy transfer, and it has been predicted that this limit can be significantly exceeded by an appropriately ramped-up cycleshape. Here, we present an experimental realization of such cycle-shaped waveforms and demonstrate control of the HHG process on the single-atom quantum level via attosecond steering of the electron trajectories. With our optimized optical cycles, we boost the field-ionization launching the electron trajectories, increase the subsequent field-to-electron energy transfer, and reduce the trajectory duration. We demonstrate, in realistic experimental conditions, two orders of magnitude enhancement of the generated XUV flux together with an increased spectral cutoff. This application, which is only one example of what can be achieved with cycle-shaped high-field light-waves, has farreaching implications for attosecond spectroscopy and molecular self-probing

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.Spanish Ministerio de Ciencia e Innovación through the Consolider Program SAUUL ( CSD2007-00013) and research project FIS2009-09522, from Junta de Castilla y León through the Program for Groups of Excellence (GR27) and from the EC’s Seventh Framework Programme ( LASERLAB-EUROPE, grant agreement n 228334)

High-order harmonic generation driven by plasmonic fields: a new route towards the generation of UV and XUV photons?

We present theoretical investigations of high-order harmonic generation (HHG) resulting from the interaction of noble gases with different kind of temporally and spatially synthesized laser fields. These fields, based on localized surface plasmons, are produced when, for instance, a metal nanoparticle or nanostructure, is illuminated by a few-cycle laser pulse. The enhanced field, which largely depends on the geometrical shape of the metallic nanostructure, has a strong spatial dependency in a scale comparable to the one where the electron dynamics takes place. We demonstrate that the spatial nonhomogeneous character of this laser field plays an important role in the HHG process and leads to a significant increase of the harmonic cutoff energy and modifications in the electron trajectories. The use of metal nanostructures appears to be an alternative way of generating coherent XUV light with a laser field whose characteristics can be spatially synthesized locally.Peer ReviewedPostprint (published version

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, which is comparable with the optical field. 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 article 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 ATI and HHG. 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-nano physics 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

High-order harmonic generation in fullerenes using few-and multi-cycle pulses of different wavelengths

We present the results of experimental and theoretical studies of high-order harmonic generation (HHG) in plasmas containing fullerenes using pulses of different duration and wavelength. We find that the harmonic cutoff is extended in the case of few-cycle pulses (3.5 fs, 29th harmonic) compared to longer laser pulses (40 fs, 25th harmonic) at the same intensity. Our studies also include HHG in fullerenes using 1300 and 780 nm multicycle (35 and 40 fs) pulses. For 1300 nm pulses, an extension of the harmonic cutoff to the 41st order was obtained, with a decrease in conversion efficiency that is consistent with theoretical predictions based on wave packet spreading for single atoms. Theoretical calculations of fullerene harmonic spectra using the single active electron approximation were carried out for both few-cycle and multicycle pulses

VUV frequency combs from below-threshold harmonics

Recent demonstrations of high-harmonic generation (HHG) at very high repetition frequencies (~100 MHz) may allow for the revolutionary transfer of frequency combs to the vacuum ultraviolet (VUV). This advance necessitates unifying optical frequency comb technology with strong-field atomic physics. While strong-field studies of HHG have often focused on above-threshold harmonic generation (photon energy above the ionization potential), for VUV frequency combs an understanding of below-threshold harmonic orders and their generation process is crucial. Here we present a new and quantitative study of the harmonics 7-13 generated below and near the ionization threshold in xenon gas. We show multiple generation pathways for these harmonics that are manifested as on-axis interference in the harmonic yield. This discovery provides a new understanding of the strong-field, below-threshold dynamics under the influence of an atomic potential and allows us to quantitatively assess the achievable coherence of a VUV frequency comb generated through below threshold harmonics. We find that under reasonable experimental conditions temporal coherence is maintained. As evidence we present the first explicit VUV frequency comb structure beyond the 3rd harmonic.Comment: 16 pages, 4 figures, 1 tabl

Gaussian-Schell analysis of the transverse spatial properties of high-harmonic beams

High harmonic generation (HHG) is a compact source of coherent, ultrafast soft x-ray radiation. HHG is increasingly being used as a source to image biological and physical systems. However, many imaging techniques such as coherent diffractive imaging, and ptychography require coherent illumination. Characterization the spatial coherence of HHG sources is vital if these sources are to kind widespread applications. Here a new method for characterizing coherent radiation is used to investigate the near- and far- field spatial properties of high harmonic radiation generated in a gas cell. The intensity distribution, wavefront curvature, and complex coherence factor are measured for a range of harmonic orders, and the Gaussian-Schell model is used to determine the properties of the harmonic beam in the plane of generation. Our results show the measured spatial properties of the harmonic beam are consistent with the finite spatial coherence of the driving laser beam as well as variations of the atomic dipole phase. These findings are used to suggest new approaches for controlling and optimizing the spatial properties of light for imaging applications