Attosecond Pulse Shaping Research Articles

Deciphering the role of three-color synthesized laser pulse parameters in N2 ionization and attosecond pulse shaping

Photoionization of atoms or molecules is a fundamental process in strong-field physics, essential for generating high-order harmonics and producing attosecond pulses. Here, we investigate how a three-color laser field, consisting of wavelengths at 800 nm and its second and third harmonics, photoionizes N2 molecules and evaluates its effect on the properties of attosecond pulses. It has been discovered that by altering the relative phase, these harmonics periodically influence molecular ionization, increasing the discreteness and strength of the attosecond pulse trains. Three-color field driving dramatically raises the pulse peak while decreasing the width of the strongest peak pulse, whereas two-color field driving just slightly enhances the pulse intensity and duration. Furthermore, the effectiveness of harmonic production is significantly increased by varying the laser intensity ratios. Even though the efficiency and pulse intensity of the three-color field are limited by conversion efficiency, attosecond pulses with higher intensities can be produced with proper parameter tuning at lower ionization rates. These findings offer a significant foundation for precisely controlling attosecond pulse generation. Ocis codes320.7110; 320.7120.

High-order harmonic generation from a thin film crystal perturbed by a quasi-static terahertz field

Studies of laser-driven strong field processes subjected to a (quasi-)static field have been mainly confined to theory. Here we provide an experimental realization by introducing a bichromatic approach for high harmonic generation (HHG) in a dielectric that combines an intense 70 femtosecond duration mid-infrared driving field with a weak 2 picosecond period terahertz (THz) dressing field. We address the physics underlying the THz field induced static symmetry breaking and its consequences on the efficient production/suppression of even-/odd-order harmonics, and demonstrate the ability to probe the HHG dynamics via the modulation of the harmonic distribution. Moreover, we report a delay-dependent even-order harmonic frequency shift that is proportional to the time derivative of the THz field. This suggests a limitation of the static symmetry breaking interpretation and implies that the resultant attosecond bursts are aperiodic, thus providing a frequency domain probe of attosecond transients while opening opportunities in precise attosecond pulse shaping.

Strong inelastic scattering of slow electrons by optical near fields of small nanostructures

The interaction of swift, free-space electrons with confined optical near fields has recently sparked much interest. It enables a new type of photon-induced near-field electron microscopy, mapping local optical near fields around nanoparticles with exquisite spatial and spectral resolution and lies at the heart of quantum state manipulation and attosecond pulse shaping of free electrons. The corresponding interaction of optical near fields with slow electrons has achieved much less attention, even though the lower electron velocity may enhance electron-near-field coupling for small nanoparticles. A first-principle theoretical study of such interactions has been reported very recently by N Talebi (2020 Phys. Rev. Lett. 125 080401). Building up on this work, we investigate, both analytically and numerically, the inelastic scattering of slow electrons by near fields of small nanostructures. For weak fields, this results in distinct angular diffraction patterns that represent, to first order, the Fourier transform of the transverse variation of the scalar near-field potential along the direction perpendicular to the electron propagation. For stronger fields, scattering by the near-field component along the electron trajectory results in a break-up of the energy spectrum into multiple photon orders. Their angular diffraction patterns are given by integer powers of the Fourier transform of the transverse potential variation and are shifting in phase with photon order. Our analytical model offers an efficient approach for studying the effects of electron kinetic energy, near field shape and strength on the slow-electron diffraction pattern and thus may facilitate the experimental observation of these phenomena by, e.g. ultrafast low-energy point-projection microscopy or related techniques. This could provide simultaneous access to different vectorial components of the optical near fields of small nanoparticles.

Electron choreography at the attosecond time scale

In this work, we report on coherent control of electron dynamics in atoms via attosecond pulse-shaping. We show that the photoelectron emission from argon gas produced by absorption of an attosecond pulse train (APT) made of odd and even harmonics can be manipulated along the direction of polarization of the light by tuning the spectral components (amplitude and phase) of the pulse. In addition, we show that APTs produced with a two-color (400- plus 800 nm) femtosecond driving field exhibit high temporal tunability, which is optimized for an intensity ratio between the two colors in the range of 0.1 to 5%.

Attosecond pulse shaping using a seeded free-electron laser.

Attosecond pulses are central to the investigation of valence- and core-electron dynamics on their natural timescales1-3. The reproducible generation and characterization of attosecond waveforms has been demonstrated so far only through the process of high-order harmonic generation4-7. Several methods for shaping attosecond waveforms have been proposed, including the use of metallic filters8,9, multilayer mirrors10 and manipulation of the driving field11. However, none of these approaches allows the flexible manipulation of the temporal characteristics of the attosecond waveforms, and they suffer from the low conversion efficiency of the high-order harmonic generation process. Free-electron lasers, by contrast, deliver femtosecond, extreme-ultraviolet and X-ray pulses with energies ranging from tens of microjoules to a few millijoules12,13. Recent experiments have shown that they can generate subfemtosecond spikes, but with temporal characteristics that change shot-to-shot14-16. Here we report reproducible generation of high-energy (microjoule level) attosecond waveforms using a seeded free-electron laser17. We demonstrate amplitude and phase manipulation of the harmonic components of an attosecond pulse train in combination with an approach for its temporal reconstruction. The results presented here open the way to performing attosecond time-resolved experiments with free-electron lasers.

Attosecond Pulse Shaping by Multilayer Mirrors

The emerging research field of attosecond science allows for the temporal investigation of one of the fastest dynamics in nature: electron dynamics in matter. These dynamics are responsible for chemical and biological processes, and the ability to understand and control them opens a new door of fundamental science, with the possibility to influence all lives if medical issues can thereby be addressed. Multilayer optics are key elements in attosecond experiments; they are used to tailor attosecond pulses with well-defined characteristics to facilitate detailed and accurate insight into processes, e.g., photoemission, Auger decay, or (core-) excitons. Based on the investigations and research efforts from the past several years, multilayer mirrors today are routinely used optical elements in attosecond beamlines. As a consequence, the generation of ultrashort pulses, combined with their dispersion control, has proceeded from the femtosecond range in the visible/infrared spectra to the attosecond range, covering the extreme ultraviolet and soft X-ray photon range up to the water window. This article reviews our work on multilayer optics over the past several years, as well as the impact from other research groups, to reflect on the scientific background of their nowadays routine use in attosecond physics.

Attosecond pulse shaping around a Cooper minimum.

High harmonic generation (HHG) is used to measure the spectral phase of the recombination dipole matrix element (RDM) in argon over a broad frequency range that includes the 3p Cooper minimum (CM). The measured RDM phase agrees well with predictions based on the scattering phases and amplitudes of the interfering s- and d-channel contributions to the complementary photoionization process. The reconstructed attosecond bursts that underlie the HHG process show that the derivative of the RDM spectral phase, the group delay, does not have a straightforward interpretation as an emission time, in contrast to the usual attochirp group delay. Instead, the rapid RDM phase variation caused by the CM reshapes the attosecond bursts.

Aperiodic CrSc multilayer mirrors for attosecond water window pulses

Extending single attosecond pulse technology from currently sub-200 eV to the so called 'water window' spectral range may enable for the first time the unique investigation of ultrafast electronic processes within the core states of bio-molecules as proteins or other organic materials. Aperiodic multilayer mirrors serve as key components to shape these attosecond pulses with a high degree of freedom and enable tailored short pulse pump-probe experiments. Here, we report on chirped CrSc multilayer mirrors, fabricated by ion beam deposition with sub-angstrom precision, designed for attosecond pulse shaping in the 'water window' spectral range.

Broadband multilayer mirror and diffractive optics for attosecond pulse shaping in the 280-500 eV photon energy range

Chirped broadband multilayer mirrors are key components to shape attosecond pulses in the XUV range. Compressing high harmonic pulses to their Fourier limit is the major goal for attosecond physics utilizing short pulse pump-probe experiments. Here, we report about the first implementation of multilayers and diffractive optics fulfilling these requirements in the water-window spectral range.

Colloquium: Optimal control of high-harmonic generation

High-harmonic generation provides an attractive light source of coherent radiation in the extreme-ultraviolet (XUV) and soft-x-ray regions of the spectrum and allows for the production of single attosecond pulses or pulse trains. This Colloquium covers the control of high-harmonic spectra by temporal and spatial pulse shaping of the driving laser pulses and its implications on time-resolved XUV spectroscopy and attosecond pulse shaping. It summarizes important steps for extending existing pulse shaping techniques and control schemes from the near-infrared or visible part to shorter wavelengths. Using adaptive pulse shaping of the driving laser pulses, several groups have demonstrated control of the high-harmonic spectrum, including the author's work on the complete control over the XUV spectrum of high-order harmonics, generated in a gas-filled hollow fiber. It is possible to achieve both the enhancement and the suppression of single or several selected harmonic orders. These arbitrarily shaped soft-x-ray spectra will allow for important modifications of the resulting harmonic pulses in the temporal domain. This constitutes first steps towards direct attosecond pulse shaping in the soft-x-ray domain. Moreover, high-harmonic generation in a hollow-core fiber can be enhanced by coupling into a single fiber mode using a feedback-controlled adaptive two-dimensional spatial light modulator.