scholarly journals The measurement of ultrafast electronic and structural dynamics with X-rays

2019 ◽  
Vol 377 (2145) ◽  
pp. 20170481 ◽  
Author(s):  
J. P. Marangos
Keyword(s):  
Structural Dynamics ◽  
High Harmonic ◽  
High Impact ◽  
X Rays ◽  
Free Electron Lasers ◽  
Theme Issue ◽  
X Ray ◽  
Ultrafast Science ◽  
Photon Sources ◽  
New Generation

In this theme issue, leading researchers discuss recent work on the measurement of ultrafast electronic and structural dynamics in matter using a new generation of short duration X-ray photon sources. These photon sources, based upon high harmonic generation from lasers and X-ray free-electron lasers, look set to have a high impact on ultrafast science. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.

scholarly journals Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers

2019 ◽  
Vol 377 (2145) ◽  
pp. 20170464 ◽  
Author(s):  
Philippe Wernet
Keyword(s):  
Structural Dynamics ◽  
Free Electron ◽  
Short Pulse ◽  
Exchange Interactions ◽  
X Rays ◽  
Free Electron Lasers ◽  
Substitution Reactions ◽  
X Ray ◽  
Orbital Interactions

X-ray free-electron lasers with intense, tuneable and short-pulse X-ray radiation are transformative tools for the investigation of transition-metal complexes and metalloproteins. This becomes apparent in particular when combining the experimental observables from X-ray spectroscopy with modern theoretical tools for calculations of electronic structures and X-ray spectra from first principles. The combination gives new insights into how charge and spin densities change in chemical reactions and how they determine reactivity. This is demonstrated for the investigations of structural dynamics with metal K-edge absorption spectroscopy, spin states in excited-state dynamics with metal 3p-3d exchange interactions, the frontier-orbital interactions in dissociation and substitution reactions with metal-specific X-ray spectroscopy, and studies of metal oxidation states with femtosecond pulses for ‘probe-before-destroy’ spectroscopy. The role of X-ray free-electron lasers is addressed with thoughts about how they enable ‘bringing back together’ different aspects of the same problem and this is thought to go beyond a conventional review paper where these aspects are formulated in italic font type in a prequel, an interlude and in a sequel. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays'.

scholarly journals Few-Cycle Infrared Pulse Evolving in FEL Oscillators and Its Application to High-Harmonic Generation for Attosecond Ultraviolet and X-ray Pulses

Atoms ◽  
2021 ◽  
Vol 9 (1) ◽  
pp. 15
Author(s):  
Ryoichi Hajima
Keyword(s):  
Harmonic Generation ◽  
Short Pulse ◽  
High Harmonic ◽  
High Harmonic Generation ◽  
Pulse Generation ◽  
Solid State Lasers ◽  
Linear Accelerators ◽  
X Ray ◽  
Ultrafast Science ◽  
Historical Remarks

Generation of few-cycle optical pulses in free-electron laser (FEL) oscillators has been experimentally demonstrated in FEL facilities based on normal-conducting and superconducting linear accelerators. Analytical and numerical studies have revealed that the few-cycle FEL lasing can be explained in the frame of superradiance, cooperative emission from self-bunched systems. In the present paper, we review historical remarks of superradiance FEL experiments in short-pulse FEL oscillators with emphasis on the few-cycle pulse generation and discuss the application of the few-cycle FEL pulses to the scheme of FEL-HHG, utilization of infrared FEL pulses to drive high-harmonic generation (HHG) from gas and solid targets. The FEL-HHG enables one to explore ultrafast science with attosecond ultraviolet and X-ray pulses with a MHz repetition rate, which is difficult with HHG driven by solid-state lasers. A research program has been launched to develop technologies for the FEL-HHG and to conduct a proof-of-concept experiment of FEL-HHG.

scholarly journals Table-top extreme ultraviolet second harmonic generation

2021 ◽  
Vol 7 (21) ◽  
pp. eabe2265
Author(s):  
Tobias Helk ◽  
Emma Berger ◽  
Sasawat Jamnuch ◽  
Lars Hoffmann ◽  
Adeline Kabacinski ◽  
...  
Keyword(s):  
Second Harmonic Generation ◽  
Harmonic Generation ◽  
First Principles ◽  
Extreme Ultraviolet ◽  
Second Harmonic ◽  
High Harmonic ◽  
Electronic Structure Calculations ◽  
Free Electron Lasers ◽  
X Ray ◽  
Structure Calculations

The lack of available table-top extreme ultraviolet (XUV) sources with high enough fluxes and coherence properties has limited the availability of nonlinear XUV and x-ray spectroscopies to free-electron lasers (FELs). Here, we demonstrate second harmonic generation (SHG) on a table-top XUV source by observing SHG near the Ti M2,3 edge with a high-harmonic seeded soft x-ray laser. Furthermore, this experiment represents the first SHG experiment in the XUV. First-principles electronic structure calculations suggest the surface specificity and separate the observed signal into its resonant and nonresonant contributions. The realization of XUV-SHG on a table-top source opens up more accessible opportunities for the study of element-specific dynamics in multicomponent systems where surface, interfacial, and bulk-phase asymmetries play a driving role.

scholarly journals Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids

2019 ◽  
Vol 377 (2145) ◽  
pp. 20170463 ◽  
Author(s):  
Romain Geneaux ◽  
Hugo J. B. Marroux ◽  
Alexander Guggenmos ◽  
Daniel M. Neumark ◽  
Stephen R. Leone
Keyword(s):  
Time Scales ◽  
Harmonic Generation ◽  
Absorption Spectroscopy ◽  
Transient Absorption ◽  
High Harmonic ◽  
High Harmonic Generation ◽  
Transient Absorption Spectroscopy ◽  
Spectroscopic Techniques ◽  
X Rays ◽  
X Ray

Attosecond science opened the door to observing nuclear and electronic dynamics in real time and has begun to expand beyond its traditional grounds. Among several spectroscopic techniques, X-ray transient absorption spectroscopy has become key in understanding matter on ultrafast time scales. In this review, we illustrate the capabilities of this unique tool through a number of iconic experiments. We outline how coherent broadband X-ray radiation, emitted in high-harmonic generation, can be used to follow dynamics in increasingly complex systems. Experiments performed in both molecules and solids are discussed at length, on time scales ranging from attoseconds to picoseconds, and in perturbative or strong-field excitation regimes. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.

scholarly journals An optimized kHz two-colour high harmonic source for seeding free-electron lasers and plasma-based soft x-ray lasers

2009 ◽  
Vol 11 (8) ◽  
pp. 083033 ◽  
Author(s):  
G Lambert ◽  
J Gautier ◽  
C P Hauri ◽  
Ph Zeitoun ◽  
C Valentin ◽  
...  
Keyword(s):  
Free Electron ◽  
High Harmonic ◽  
Free Electron Lasers ◽  
X Ray ◽  
Harmonic Source

scholarly journals High Repetition Rate and Coherent Free-Electron Laser in the X-Rays Range Tailored for Linear Spectroscopy

Instruments ◽  
2019 ◽  
Vol 3 (3) ◽  
pp. 47 ◽  
Author(s):  
Vittoria Petrillo ◽  
Michele Opromolla ◽  
Alberto Bacci ◽  
Illya Drebot ◽  
Giacomo Ghiringhelli ◽  
...  
Keyword(s):  
Free Electron ◽  
Repetition Rate ◽  
Free Electron Laser ◽  
Extreme Ultraviolet ◽  
High Harmonic ◽  
High Repetition Rate ◽  
X Rays ◽  
Regenerative Amplifier ◽  
X Ray ◽  
High Repetition

Fine time-resolved analysis of matter—i.e., spectroscopy and photon scattering—in the linear response regime requires fs-scale pulsed, high repetition rate, fully coherent X-ray sources. A seeded Free Electron Laser (FEL) driven by a Linac based on Super Conducting cavities, generating 10 8 – 10 10 coherent photons at 2–5 keV with 0.2–1 MHz of repetition rate, can address this need. Three different seeding schemes, reaching the X-ray range, are described hereafter. The first two are multi-stage cascades upshifting the radiation frequency by a factor of 10–30 starting from a seed represented by a coherent flash of extreme ultraviolet light. This radiation can be provided either by the High Harmonic Generation of an optical laser or by an FEL Oscillator operating at 12–14 nm. The third scheme is a regenerative amplifier working with X-ray mirrors. The whole chain of the X-ray generation is here described by means of start-to-end simulations.

scholarly journals Attosecond soft X-ray high harmonic generation

2019 ◽  
Vol 377 (2145) ◽  
pp. 20170468 ◽  
Author(s):  
Allan S. Johnson ◽  
Timur Avni ◽  
Esben W. Larsen ◽  
Dane R. Austin ◽  
Jon P. Marangos
Keyword(s):  
Harmonic Generation ◽  
Spectral Range ◽  
High Harmonic ◽  
High Harmonic Generation ◽  
Intense Laser ◽  
X Rays ◽  
X Ray ◽  
Optical Phenomenon ◽  
Highly Nonlinear ◽  
Attosecond Pulses

High harmonic generation (HHG) of an intense laser pulse is a highly nonlinear optical phenomenon that provides the only proven source of tabletop attosecond pulses, and it is the key technology in attosecond science. Recent developments in high-intensity infrared lasers have extended HHG beyond its traditional domain of the XUV spectral range (10–150 eV) into the soft X-ray regime (150 eV to 3 keV), allowing the compactness, stability and sub-femtosecond duration of HHG to be combined with the atomic site specificity and electronic/structural sensitivity of X-ray spectroscopy. HHG in the soft X-ray spectral region has significant differences from HHG in the XUV, which necessitate new approaches to generating and characterizing attosecond pulses. Here, we examine the challenges and opportunities of soft X-ray HHG, and we use simulations to examine the optimal generating conditions for the development of high-flux, attosecond-duration pulses in the soft X-ray spectral range. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.

scholarly journals X-Ray Free-Electron Lasers for the Structure and Dynamics of Macromolecules

2019 ◽  
Vol 88 (1) ◽  
pp. 35-58 ◽  
Author(s):  
Henry N. Chapman
Keyword(s):  
Free Electron ◽  
Conformational Dynamics ◽  
Cryogenic Cooling ◽  
X Rays ◽  
Free Electron Lasers ◽  
X Ray ◽  
Virus Particles ◽  
Structure And Dynamics ◽  
Small Crystals ◽  
Serial Crystallography

X-ray free-electron lasers provide femtosecond-duration pulses of hard X-rays with a peak brightness approximately one billion times greater than is available at synchrotron radiation facilities. One motivation for the development of such X-ray sources was the proposal to obtain structures of macromolecules, macromolecular complexes, and virus particles, without the need for crystallization, through diffraction measurements of single noncrystalline objects. Initial explorations of this idea and of outrunning radiation damage with femtosecond pulses led to the development of serial crystallography and the ability to obtain high-resolution structures of small crystals without the need for cryogenic cooling. This technique allows the understanding of conformational dynamics and enzymatics and the resolution of intermediate states in reactions over timescales of 100 fs to minutes. The promise of more photons per atom recorded in a diffraction pattern than electrons per atom contributing to an electron micrograph may enable diffraction measurements of single molecules, although challenges remain.

Accelerator-based X-ray sources: synchrotron radiation, X-ray free electron lasers and beyond

2019 ◽  
Vol 377 (2147) ◽  
pp. 20180231 ◽  
Author(s):  
Tetsuya Ishikawa
Keyword(s):  
Synchrotron Radiation ◽  
Storage Ring ◽  
Free Electron ◽  
Continuous Wave ◽  
Transitional Period ◽  
Light Sources ◽  
X Rays ◽  
Free Electron Lasers ◽  
Beam Emittance ◽  
X Ray

The evolution of synchrotron radiation (SR) sources and related sciences is discussed to explain the ‘generation’ of the SR sources. Most of the contemporary SR sources belong to the third generation, where the storage rings are optimized for the use of undulator radiation. The undulator development allowed to reduction of the electron energy of the storage ring necessary for delivering 10 keV X-rays from the initial 6–8 GeV to the current 3 Gev. Now is the transitional period from the double-bend-achromat lattice-based storage ring to the multi-bend-achromat lattice to achieve much smaller electron beam emittance. Free electron lasers are the other important accelerator-based light sources which recently reached hard X-ray regime by using self-amplified spontaneous emission scheme. Future accelerator-based X-ray sources should be continuous wave X-ray free electron lasers and pulsed X-ray free electron lasers. Some pathways to reach the future case are discussed. This article is part of the theme issue ‘Fifty years of synchrotron science: achievements and opportunities’.

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