Laser-induced electron diffraction: Imaging of a single gas-phase molecular structure with one of its own electrons.

Among the many methods to image molecular structure, laser-induced electron diffraction (LIED) can image a single gas-phase molecule by locating all of a molecule's atoms in space and time. The method is based on attosecond electron recollision driven by a laser field and can reach attosecond temporal resolution. Implementation with a mid-IR laser and cold-target recoil ion-momentum spectroscopy, single molecules are measured with picometer resolution due to the keV electron impact energy without ensemble averaging or the need for molecular orientation.

Valleytronics in bulk MoS with a topologic optical field.

The valley degree of freedom of electrons in materials promises routes towards energy-efficient information storage with enticing prospects for quantum information processing. Current challenges in utilizing valley polarization are symmetry conditions that require monolayer structures or specific material engineering, non-resonant optical control to avoid energy dissipation and the ability to switch valley polarization at optical speed. We demonstrate all-optical and non-resonant control over valley polarization using bulk MoS a centrosymmetric material without Berry curvature at the valleys.

Enhanced optical conductivity and many-body effects in strongly-driven photo-excited semi-metallic graphite.

The excitation of quasi-particles near the extrema of the electronic band structure is a gateway to electronic phase transitions in condensed matter. In a many-body system, quasi-particle dynamics are strongly influenced by the electronic single-particle structure and have been extensively studied in the weak optical excitation regime. Yet, under strong optical excitation, where light fields coherently drive carriers, the dynamics of many-body interactions that can lead to new quantum phases remain largely unresolved.

High-harmonic spectroscopy of quantum phase transitions in a high-Tc superconductor.

We report on the nonlinear optical signatures of quantum phase transitions in the high-temperature superconductor YBCO, observed through high harmonic generation. While the linear optical response of the material is largely unchanged when cooling across the phase transitions, the nonlinear optical response sensitively imprints two critical points, one at the critical temperature of the cuprate with the exponential growth of the surface harmonic yield in the superconducting phase and another critical point, which marks the transition from strange metal to pseudogap phase. To reveal the underlying microscopic quantum dynamics, a strong-field quasi-Hubbard model was developed, which describes the measured optical response dependent on the formation of Cooper pairs.

Machine learning for laser-induced electron diffraction imaging of molecular structures.

Ultrafast diffraction imaging is a powerful tool to retrieve the geometric structure of gas-phase molecules with combined picometre spatial and attosecond temporal resolution. However, structural retrieval becomes progressively difficult with increasing structural complexity, given that a global extremum must be found in a multi-dimensional solution space. Worse, pre-calculating many thousands of molecular configurations for all orientations becomes simply intractable.

High density molecular jets of complex neutral organic molecules with Tesla valves.

Supersonic jets of gas-phase atoms and small molecules have enabled a variety of ultrafast and ultracold chemical studies. However, extension to larger, more complex neutral molecules proves challenging for two reasons: (i) Complex molecules, such as cis-stilbene, exist in a liquid or solid phase at room temperature and ambient pressure and (ii) a unidirectional flow of high-density gaseous beams of such molecules to the interaction region is required. No delivery system currently exists that can deliver dense enough molecular jets of neutral complex molecules without ionizing or exciting the target for use in gas-phase structural dynamics studies.

Two-dimensional retrieval methods for ultrafast imaging of molecular structure using laser-induced electron diffraction.

Molecular structural retrieval based on electron diffraction has been proposed to determine the atomic positions of molecules with sub-angstrom spatial and femtosecond temporal resolutions. Given its success on small molecular systems, in this work, we point out that the accuracy of structure retrieval is constrained by the availability of a wide range of experimental data in the momentum space in all molecular systems. To mitigate the limitations, for laser-induced electron diffraction, here we retrieve molecular structures using two-dimensional (energy and angle) electron momentum spectra in the laboratory frame for a number of small molecular systems, which have previously been studied with 1D methods.

Erratum: Publisher's Note: "Laser-induced electron diffraction of the ultrafast umbrella motion in ammonia" [Struct. Dyn. , 014301 (2021)].

[This corrects the article DOI: 10.1063/4.0000046.

Laser-induced electron diffraction of the ultrafast umbrella motion in ammonia.

Visualizing molecular transformations in real-time requires a structural retrieval method with Ångström spatial and femtosecond temporal atomic resolution. Imaging of hydrogen-containing molecules additionally requires an imaging method sensitive to the atomic positions of hydrogen nuclei, with most methods possessing relatively low sensitivity to hydrogen scattering. Laser-induced electron diffraction (LIED) is a table-top technique that can image ultrafast structural changes of gas-phase polyatomic molecules with sub-Ångström and femtosecond spatiotemporal resolution together with relatively high sensitivity to hydrogen scattering.

Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction.

Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision.

Few-cycle mid-infrared pulses from BaGaGeSe.

(BGGSe) is a newly developed nonlinear material that is attractive for ultrabroad frequency mixing and ultrashort pulse generation due to its comparably low dispersion and high damage threshold. A numerical study shows the material's capacity for octave-spanning mid-infrared pulse generation up to 18 µm. In a first experiment, we show that a long crystal length of 2.

Author Correction: All semiconductor enhanced high-harmonic generation from a single nanostructured cone.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Imaging an isolated water molecule using a single electron wave packet.

Observing changes in molecular structure requires atomic-scale Ångstrom and femtosecond spatio-temporal resolution. We use the Fourier transform (FT) variant of laser-induced electron diffraction (LIED), FT-LIED, to directly retrieve the molecular structure of HO with picometer and femtosecond resolution without a priori knowledge of the molecular structure nor the use of retrieval algorithms or ab initio calculations. We identify a symmetrically stretched HO field-dressed structure that is most likely in the ground electronic state.

Table-top high-energy 7 μm OPCPA and 260 mJ Ho:YLF pump laser.

We present a state-of-the-art compact high-energy mid-infrared (mid-IR) laser system for TW-level eight-cycle pulses at 7 μm. This system consists of an Er:Tm:Ho:fiber MOPA which serves as the seeder for a ZGP-based optical parametric chirped pulse amplification (OPCPA) chain, in addition to a Ho:YLF amplifier which is Tm:fiber pumped. Featuring all-optical synchronization, the system delivers 260 mJ pump energy at 2052 nm and 16 ps duration at 100 Hz with a stability of 0.

Symphony on strong field approximation.

This paper has been prepared by the Symphony collaboration (University of Warsaw, Uniwersytet Jagielloński, DESY/CNR and ICFO) on the occasion of the 25th anniversary of the 'simple man's models' which underlie most of the phenomena that occur when intense ultrashort laser pulses interact with matter. The phenomena in question include high-harmonic generation (HHG), above-threshold ionization (ATI), and non-sequential multielectron ionization (NSMI). 'Simple man's models' provide both an intuitive basis for understanding the numerical solutions of the time-dependent Schrödinger equation and the motivation for the powerful analytic approximations generally known as the strong field approximation (SFA).

Infrared electric field sampled frequency comb spectroscopy.

Probing matter with light in the mid-infrared provides unique insight into molecular composition, structure, and function with high sensitivity. However, laser spectroscopy in this spectral region lacks the broadband or tunable light sources and efficient detectors available in the visible or near-infrared. We overcome these challenges with an approach that unites a compact source of phase-stable, single-cycle, mid-infrared pulses with room temperature electric field-resolved detection at video rates.

All semiconductor enhanced high-harmonic generation from a single nanostructured cone.

The enhancement and control of non-linear phenomena at a nanometer scale has a wide range of applications in science and in industry. Among these phenomena, high-harmonic generation in solids is a recent focus of research to realize next generation petahertz optoelectronic devices or compact all solid state EUV sources. Here, we report on the realization of the first nanoscale high harmonic source.

Imaging the Renner-Teller effect using laser-induced electron diffraction.

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS) in the [Formula: see text] excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement.

Ultrafast nonlinear optical response of Dirac fermions in graphene.

The speed of solid-state electronic devices, determined by the temporal dynamics of charge carriers, could potentially reach unprecedented petahertz frequencies through direct manipulation by optical fields, consisting in a million-fold increase from state-of-the-art technology. In graphene, charge carrier manipulation is facilitated by exceptionally strong coupling to optical fields, from which stems an important back-action of photoexcited carriers. Here we investigate the instantaneous response of graphene to ultrafast optical fields, elucidating the role of hot carriers on sub-100 fs timescales.

Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene.

Visualizing chemical reactions as they occur requires atomic spatial and femtosecond temporal resolution. Here, we report imaging of the molecular structure of acetylene (CH) 9 femtoseconds after ionization. Using mid-infrared laser-induced electron diffraction (LIED), we obtained snapshots as a proton departs the [CH] ion.

High power multi-color OPCPA source with simultaneous femtosecond deep-UV to mid-IR outputs.

Many experimental investigations demand synchronized pulses at various wavelengths, ideally with very short pulse duration and high repetition rate. Here we describe a femtosecond multi-color optical parametric chirped pulse amplifier (OPCPA) with simultaneous outputs from the deep-UV to the mid-IR with optical synchronization. The high repetition rate of 160 kHz is well suited to compensate for low interaction probability or low cross section in strong-field interactions.

Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets.

The ability to directly follow and time-resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser-induced electron diffraction can meet these requirements, it was recently concluded that molecules with particular orbital symmetries (such as πg) cannot be imaged using purely backscattering electron wave packets without molecular alignment. Here, we demonstrate, in direct contradiction to these findings, that the orientation and shape of molecular orbitals presents no impediment for retrieving molecular structure with adequate sampling of the momentum transfer space.

0.5-keV Soft X-ray attosecond continua.

Attosecond light pulses in the extreme ultraviolet have drawn a great deal of attention due to their ability to interrogate electronic dynamics in real time. Nevertheless, to follow charge dynamics and excitations in materials, element selectivity is a prerequisite, which demands such pulses in the soft X-ray region, above 200 eV, to simultaneously cover several fundamental absorption edges of the constituents of the materials. Here, we experimentally demonstrate the exploitation of a transient phase matching regime to generate carrier envelope controlled soft X-ray supercontinua with pulse energies up to 2.

Three-wave mixing mediated femtosecond pulse compression in β-barium borate.

Nonlinear pulse compression mediated by three-wave mixing is demonstrated for ultrashort Ti:sapphire pulses in a type II phase-matched β-barium borate (BBO) crystal using noncollinear geometry. 170 μJ pulses at 800 nm with a pulse duration of 74 fs are compressed at their sum frequency to 32 fs with 55 μJ of pulse energy. Experiments and computer simulations demonstrate the potential of sum-frequency pulse compression to match the group velocities of the interacting waves to crystals that were initially not considered in the context of nonlinear pulse compression.

High-flux table-top soft x-ray source driven by sub-2-cycle, CEP stable, 1.85-μm 1-kHz pulses for carbon K-edge spectroscopy.

We report on the first table-top high-flux source of coherent soft x-ray radiation up to 400 eV, operating at 1 kHz. This source covers the carbon K-edge with a beam brilliance of (4.3±1.