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"639/766/36/2796"
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Terawatt-attosecond hard X-ray free-electron laser at high repetition rate
by
Qin, Weilun
,
Decking, Winfried
,
Dijkstal, Philipp
in
639/624/1020/1087
,
639/766/36/2796
,
639/766/400/1106
2024
Ångstrom and attosecond are the fundamental spatiotemporal scales for electron dynamics in various materials. Although attosecond pulses with wavelengths comparable to the atomic scales are expected to be a key tool in advancing attosecond science, producing high-power hard X-ray attosecond pulses at ångstrom wavelengths remains a formidable challenge. Here, we report the generation of terawatt-scale attosecond hard X-ray pulses using a free-electron laser in a special operation mode. We achieved 9 keV single-spike X-ray pulses with a mean pulse energy of around 180 μJ, exceeding previous reports by more than an order of magnitude, and an estimated average pulse duration of 200 as at full-width at half-maximum. Exploiting the unique capability of the European XFEL, which can deliver ten pulse trains per second with each containing hundreds of pulses at megahertz repetition rates, this study demonstrates the generation of attosecond X-ray pulses at a 2.25 MHz repetition rate. These intense high-repetition-rate attosecond X-ray pulses present transformative prospects for structural and electronic damage-free X-ray measurements and attosecond time-resolved X-ray methodologies, heralding a new era in ultrafast X-ray science.
Using the European XFEL free-electron laser, researchers demonstrate terawatt-scale, attosecond hard X-ray pulses. Ten pulse trains per second, each containing hundreds of pulses at megahertz repetition rates, are achieved. Such short and intense pulses at high repetition rate enable unprecedented damage-free X-ray measurements with attosecond temporal resolution.
Journal Article
Imaging shapes of atomic nuclei in high-energy nuclear collisions
2024
Atomic nuclei are self-organized, many-body quantum systems bound by strong nuclear forces within femtometre-scale space. These complex systems manifest a variety of shapes
1
–
3
, traditionally explored using non-invasive spectroscopic techniques at low energies
4
,
5
. However, at these energies, their instantaneous shapes are obscured by long-timescale quantum fluctuations, making direct observation challenging. Here we introduce the collective-flow-assisted nuclear shape-imaging method, which images the nuclear global shape by colliding them at ultrarelativistic speeds and analysing the collective response of outgoing debris. This technique captures a collision-specific snapshot of the spatial matter distribution within the nuclei, which, through the hydrodynamic expansion, imprints patterns on the particle momentum distribution observed in detectors
6
,
7
. We benchmark this method in collisions of ground-state uranium-238 nuclei, known for their elongated, axial-symmetric shape. Our findings show a large deformation with a slight deviation from axial symmetry in the nuclear ground state, aligning broadly with previous low-energy experiments. This approach offers a new method for imaging nuclear shapes, enhances our understanding of the initial conditions in high-energy collisions and addresses the important issue of nuclear structure evolution across energy scales.
The collective-flow-assisted nuclear shape-imaging method images the nuclear global shape by colliding them at ultrarelativistic speeds and analysing the collective response of outgoing debris.
Journal Article
Attosecond science based on high harmonic generation from gases and solids
2020
Recent progress in high power ultrafast short-wave and mid-wave infrared lasers has enabled gas-phase high harmonic generation (HHG) in the water window and beyond, as well as the demonstration of HHG in condensed matter. In this Perspective, we discuss the recent advancements and future trends in generating and characterizing soft X-ray pulses from gas-phase HHG and extreme ultraviolet (XUV) pulses from solid-state HHG. Then, we discuss their current and potential usage in time-resolved study of electron and nuclear dynamics in atomic, molecular and condensed matters.
Different methods are demonstrated in recent years to produce attosecond pulses. Here, the authors discuss recent development and future prospects of the generation of such pulses from gases and solids and their potential applications in spectroscopy and ultrafast dynamics in atoms, molecules and other complex systems.
Journal Article
High-harmonic spectroscopy of ultrafast many-body dynamics in strongly correlated systems
2018
We bring together two topics that, until now, have been the focus of intense but non-overlapping research efforts. The first concerns high-harmonic generation in solids, which occurs when an intense light field excites a highly non-equilibrium electronic response in a semiconductor or a dielectric. The second concerns many-body dynamics in strongly correlated systems such as the Mott insulator. We show that high-harmonic generation can be used to time-resolve ultrafast many-body dynamics associated with an optically driven phase transition, with accuracy far exceeding one cycle of the driving light field. Our work paves the way for time-resolving highly non-equilibrium many-body dynamics in strongly correlated systems, with few femtosecond accuracy.
Journal Article
What will it take to observe processes in 'real time'?
by
Keller, Ursula
,
Pfeifer, Thomas
,
Mccurdy, C. William
in
639/624/400/584
,
639/766/36/2796
,
Applied and Technical Physics
2014
Even for simple systems, the interpretations of new attosecond measurements are complicated and provide only a glimpse of their potential. Nonetheless, the lasting impact will be the revelation of how short-time dynamics can determine the electronic properties of more complex systems.
Journal Article
Experimental demonstration of attosecond pump–probe spectroscopy with an X-ray free-electron laser
by
Marangos, Jon P.
,
Huang, Zhirong
,
Berrah, Nora
in
639/624/1020/1087
,
639/766/36/2796
,
Aminophenol
2024
Pump–probe experiments with subfemtosecond resolution are the key to understanding electronic dynamics in quantum systems. Here we demonstrate the generation and control of subfemtosecond pulse pairs from a two-colour X-ray free-electron laser. By measuring the delay between the two pulses with an angular streaking diagnostic, we characterize the group velocity of the X-ray free-electron laser and show control of the pulse delay down to 270 as. We confirm the application of this technique to a pump–probe measurement in core-ionized
para
-aminophenol. These results reveal the ability to perform pump–probe experiments with subfemtosecond resolution and atomic site specificity.
Researchers have demonstrated the generation and control of subfemtosecond pulse pairs from a two-colour X-ray free-electron laser and conducted pump–probe experiments in core-ionized molecules.
Journal Article
Attosecond spectral singularities in solid-state high-harmonic generation
by
Arusi-Parpar Talya
,
McDonald, Chris
,
Rubtsov, Alexey N
in
Alkalies
,
Banded structure
,
Condensed matter physics
2020
Strong-field-driven electric currents in condensed-matter systems are opening new frontiers in petahertz electronics. In this regime, new challenges are arising as the roles of band structure and coherent electron–hole dynamics have yet to be resolved. Here, by using high-harmonic generation spectroscopy, we reveal the underlying attosecond dynamics that dictates the temporal evolution of carriers in multi-band solid-state systems. We demonstrate that when the electron–hole relative velocity approaches zero, enhanced constructive interference leads to the appearance of spectral caustics in the high-harmonic generation spectrum. We introduce the role of the dynamical joint density of states and identify its mapping into the spectrum, which exhibits singularities at the spectral caustics. By studying these singularities, we probe the structure of multiple unpopulated high conduction bands.High-harmonic waves are generated from a MgO crystal under experimental conditions where the simple semi-classical analysis fails. High-harmonic generation spectroscopy directly probes the strong-field attosecond dynamics over multiple bands.
Journal Article
0.5-keV Soft X-ray attosecond continua
2016
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 2.9±0.1 pJ and a flux of (7.3±0.1) × 10
7
photons per second across the entire water window and attosecond pulses with 13 as transform limit. Our results herald attosecond science at the fundamental absorption edges of matter by bridging the gap between ultrafast temporal resolution and element specific probing.
Attosecond soft X-ray pulses hold promise for probing electronic dynamics in real time, but it is challenging to achieve element sensitivity while maintaining temporal resolution. Teichmann
et al
. report the cover of carbon, nitrogen and oxygen absorption edges with an isolated pulse supporting 13 as duration.
Journal Article
Decoherence and revival in attosecond charge migration driven by non-adiabatic dynamics
by
Kuleff, Alexander I.
,
Matselyukh, Danylo T.
,
Wörner, Hans Jakob
in
639/766/36/1121
,
639/766/36/2796
,
Absorption spectroscopy
2022
Attosecond charge migration is a periodic evolution of the charge density at specific sites of a molecule on a timescale defined by the energy intervals between the electronic states involved. Here we report the observation of charge migration in neutral silane (SiH
4
) in 690 as, its decoherence within 15 fs and its revival after 40–50 fs, using X-ray attosecond transient-absorption spectroscopy. We observe the migration of charge as pairs of quantum beats with a characteristic spectral phase in the transient spectrum, in agreement with theory. The decay and revival of the degree of electronic coherence is found to be a result of both adiabatic and non-adiabatic dynamics in the populated Rydberg and valence states. The experimental results are supported by fully quantum-mechanical ab initio calculations that include both electronic and nuclear dynamics, which additionally support the experimental evidence that conical intersections can mediate the transfer of electronic coherence from an initial superposition state to another one involving a different lower-lying state.
X-ray ultrafast transient absorption spectroscopy captures the charge migration in neutral silane molecules, which shows in the spectra as pairs of quantum beats.
Journal Article
Attosecond electron motion control in dielectric
by
Pervak Vladimir
,
Yabana Kazuhiro
,
Hui Dandan
in
Data processing
,
Dielectric strength
,
Electrons
2022
Attosecond science capitalizes on the extreme nonlinearity of strong fields—driven by few-cycle pulses—to attain attosecond temporal resolution and give access to the electron motion dynamics of matter in real time. Here we measured the relative electronic delay response of a dielectric system triggered by a strong field of few-cycle pulses to be of the order of a few hundred attoseconds. Moreover, we exploited the electronic response following the strong driver field to demonstrate all-optical light-field-sampling methodology with attosecond resolution. This methodology provides a direct connection between the driver field and induced ultrafast dynamics in matter. Also, we demonstrate control of electron motion in a dielectric using synthesized light waveforms. This on-demand control of electron motion paves the way for establishing long-anticipated ultrafast switches and quantum electronics. This advancement promises to increase the limiting speed of data processing and information encoding to rates that exceed one petabit per second, opening a new realm of information technology.Light-field-induced electron dynamics in a silicon dioxide dielectric system are exploited to directly measure the attosecond relative electronic delay response in the dielectric system, potentially extending the speed of data processing and information encoding into the petahertz realm.
Journal Article