High-order harmonic generation is a nonlinear optical process that enables the creation of light pulses at frequencies much higher than that from a seed laser. The host medium for this interaction is typically a gas. Now, the process has been observed in a bulk crystalline solid with important implications for attosecond science.

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Observation of high-order harmonic generation in a bulk crystal

Molecular structures are imaged with sub-angstrom precision and exposure times of a few femtoseconds. Molecular imaging, or the determination of the positions of atoms in molecules, is an important technique in the physical, chemical and biological sciences. But going beyond mere structure determination, recent technical developments offer the tantalizing prospect of access to ultrafast snapshots of biological molecules and condensed-phase systems undergoing structural changes. One approach uses laser-ionized bursts of coherent electron wave packets to self-interrogate the parent molecular structure. Here, Blaga et al. use this laser-induced electron diffraction (LIED) method to map the structural responses of oxygen and nitrogen molecules to ionization. By measuring a 0.1-angstrom displacement in the oxygen bond length occurring in a time interval of about 5 femtoseconds, the authors establish LIED as a promising approach for imaging of gas-phase molecules with unprecedented spatio-temporal resolution. Establishing the structure of molecules and solids has always had an essential role in physics, chemistry and biology. The methods of choice are X-ray and electron diffraction, which are routinely used to determine atomic positions with sub-angstrom spatial resolution. Although both methods are currently limited to probing dynamics on timescales longer than a picosecond, the recent development of femtosecond sources of X-ray pulses and electron beams suggests that they might soon be capable of taking ultrafast snapshots of biological molecules1,2 and condensed-phase systems3,4,5,6 undergoing structural changes. The past decade has also witnessed the emergence of an alternative imaging approach based on laser-ionized bursts of coherent electron wave packets that self-interrogate the parent molecular structure7,8,9,10,11. Here we show that this phenomenon can indeed be exploited for laser-induced electron diffraction10 (LIED), to image molecular structures with sub-angstrom precision and exposure times of a few femtoseconds. We apply the method to oxygen and nitrogen molecules, which on strong-field ionization at three mid-infrared wavelengths (1.7, 2.0 and 2.3 μm) emit photoelectrons with a momentum distribution from which we extract diffraction patterns. The long wavelength is essential for achieving atomic-scale spatial resolution, and the wavelength variation is equivalent to taking snapshots at different times. We show that the method has the sensitivity to measure a 0.1 A displacement in the oxygen bond length occurring in a time interval of ∼5 fs, which establishes LIED as a promising approach for the imaging of gas-phase molecules with unprecedented spatio-temporal resolution.

/pdf/imaging-ultrafast-molecular-dynamics-with-laser-induced-suox2noh60.pdf

Imaging ultrafast molecular dynamics with laser-induced electron diffraction

Strong-field physics, an extreme limit of light-matter interaction, is expanding into the realm of surfaces and nanostructures from its origin in atomic and molecular science. The attraction of nanostructures lies in two intimately connected features: local intensity enhancement and sub-wavelength confinement of optical fields. Local intensity enhancement facilitates access to the strong-field regime and has already sparked various applications, whereas spatial localization has the potential to generate strong-field dynamics exclusive to nanostructures. However, the observation of features unattainable in gaseous media is challenged by many-body effects and material damage, which arise under intense illumination of dense systems. Here, we non-destructively access this regime in the solid state by employing single plasmonic nanotips and few-cycle mid-infrared pulses, making use of the wavelength-dependence of the interaction, that is, the ponderomotive energy. We investigate strong-field photoelectron emission and acceleration from single nanostructures over a broad spectral range, and find kinetic energies of hundreds of electronvolts. We observe the transition to a new regime in strong-field dynamics, in which the electrons escape the nanolocalized field within a fraction of an optical half-cycle. The transition into this regime, characterized by a spatial adiabaticity parameter, would require relativistic electrons in the absence of nanostructures. These results establish new degrees of freedom for the manipulation and control of electron dynamics on femtosecond and attosecond timescales, combining optical near-fields and nanoscopic sources.

Field-driven photoemission from nanostructures quenches the quiver motion

The generation of extremely short isolated attosecond pulses requires both a broad spectral bandwidth and control of the spectral phase. Rapid progress has been made in both aspects, leading to the generation of light pulses as short as 67 as in 2012, and broadband attosecond continua covering a wide range of extreme ultraviolet and soft X-ray wavelengths. Such pulses have been successfully applied in photoelectron and photoion spectroscopy and recently developed attosecond transient absorption spectroscopy to study electron dynamics in matter. In this Review, we discuss significant recent advances in the generation, characterization and applications of ultrabroadband, isolated attosecond pulses with spectral bandwidths comparable to the central frequency. These pulses can in principle be compressed to a single optical cycle. This review discusses significant recent advances in the generation, characterization and application of ultrabroadband isolated attosecond pulses with a spectral bandwidth comparable to the central frequency, which can in principle be compressed to a single optical cycle.

The generation, characterization and applications of broadband isolated attosecond pulses

Attosecond science offers formidable tools for the investigation of electronic processes at the heart of important physical processes in atomic, molecular and solid-state physics. In the last 15 years impressive advances have been obtained from both the experimental and theoretical points of view. Attosecond pulses, in the form of isolated pulses or of trains of pulses, are now routinely available in various laboratories. In this review recent advances in attosecond science are reported and important applications are discussed. After a brief presentation of various techniques that can be employed for the generation and diagnosis of sub-femtosecond pulses, various applications are reported in atomic, molecular and condensed-matter physics.

https://iopscience.iop.org/article/10.1088/0953-4075/49/6/062001/pdf

Advances in attosecond science

A systematic experimental study of the ionization of argon by mid-infrared light confirms half-a-century-old predictions and paves the way to the development of brighter, shorter attosecond pulse sources.

/pdf/scaling-strong-field-interactions-towards-the-classical-12cygbw1je.pdf

Scaling strong-field interactions towards the classical limit

The discovery of an overlooked but apparently ubiquitous spike in the mid-infrared photoelectron spectra of molecular and atomic gases suggests that we don’t know as much as we thought we did about the ionization of matter in strong fields.

/pdf/strong-field-photoionization-revisited-2ee0mxo19y.pdf

Strong-field photoionization revisited

We present a study of the photoelectrons energy distribution from ionization of Argon by a linearly polarized, intense, mid-infrared laser field with special attention to the recently discovered Low Energy Structure (LES) [1] whose origin is not yet fully understood. In this paper we will go deeper in the analysis of the LES by studying its angular distribution and examine its behavior in circularly polarized light.

Mid-infrared strong field ionization angular distributions

https://www.nature.com/articles/s42005-021-00784-0.pdf

F. Catoire

Papers

Scaling strong-field interactions towards the classical limit

Strong-field photoionization revisited

Mid-infrared strong field ionization angular distributions

Publisher Correction: Angle-dependent interferences in electron emission accompanying stimulated Compton scattering from molecules

Publisher Correction: Angle-dependent interferences in electron emission accompanying stimulated Compton scattering from molecules