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Results for “attosecond physics”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Analysis of two-color photoelectron spectroscopy for attosecond metrology at seeded free-electron lasers

The generation of attosecond pulse trains at free-electron lasers opens new opportunities in ultrafast science, as it gives access, for the first time, to reproducible, programmable, extreme ultraviolet (XUV) waveforms with high intensity. In this work, we present a detailed analysis of the theoretical model underlying the temporal characterization of the attosecond pulse trains recently generated at the free-electron laser FERMI. In particular, the validity of the approximations used for the correlated analysis of the photoelectron spectra generated in the two-color photoionization experiments are thoroughly discussed. The ranges of validity of the assumptions, in connection with the main experimental parameters, are derived.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Clocking Auger electrons

Intense X-ray free-electron lasers (XFELs) can rapidly excite matter, leaving it in inherently unstable states that decay on femtosecond timescales. The relaxation occurs primarily via Auger emission, so excited-state observations are constrained by Auger decay. In situ measurement of this process is therefore crucial, yet it has thus far remained elusive in XFELs owing to inherent timing and phase jitter, which can be orders of magnitude larger than the timescale of Auger decay. Here we develop an approach termed ‘self-referenced attosecond streaking’ that provides subfemtosecond resolution in spite of jitter, enabling time-domain measurement of the delay between photoemission and Auger emission in atomic neon excited by intense, femtosecond pulses from an XFEL. FUrthermore, using a fully quantum-mechanical description that treats the ionization, core-hole formation and Auger emission as a single process, the observed delay yields an Auger decay lifetime of \(2.2_{ - 0.3}^{ + 0.2}\) fs for the KLL decay channel.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Enhanced extreme ultraviolet high-harmonic generation from chromium-doped magnesium oxide

High-order harmonic generation (HHG) from crystals is emerging as a new ultrashort source of coherent extreme ultraviolet (XUV) light. Doping the crystal structure can offer a new way to control the source properties. Here, we present a study of HHG enhancement in the XUV spectral region from an ionic crystal, using dopant-induced vacancy defects, driven by a laser centered at a wavelength of 1.55 μm. Our numerical simulations based on solutions of the semiconductor Bloch equations and density-functional theory are supported by our experimental observations and demonstrate an increase in the XUV high harmonic yield from doped bulk magnesium oxide (MgO) compared to undoped MgO, even at a low defect concentration. The anisotropy of the harmonic emission as a function of the laser polarization shows that the pristine crystal's symmetry is preserved. Our study paves the way toward the control of HHG in solids with complex defects caused by transition-metal doping.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Probing ultrafast excited-state dynamics using EUV-IR six-wave-mixing emission spectroscopy

Non-linear processes such as four-wave-mixing have become instrumental in attosecond EUV spectroscopy. Using EUV high harmonics in conjunction with collinear near-infrared and mid-infrared fields, we extended this approach to high-order-mixing between three colors. Specifically, we find that atomic resonances in neon exhibit a significant cross section for six-wave mixing. The MIR probe frequency tunability in our multicolor scheme is employed to access several optically dark resonances and probe the quantum beat of a coherent electronic wavepacket using background-free EUV emission as a diagnostic. This technique can be easily extended to other atomic and molecular systems, and opens the door to multi-dimensional non-linear spectroscopy.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

High efficiency Al/Sc-based multilayer coatings in the EUV wavelength range above 40 nanometers

In this Letter, we have developed new and highly efficient periodic multilayer mirrors Al/Sc, Al/Sc/SiC, and Mo/Al/Sc with optimized reflectance at wavelengths between 40 and 65 nm. We have reached record values in measured peak reflectance: 57.5% at 44.7 nm and 46.5% at 51 nm, with Al/Sc/SiC at near-normal incidence. Furthermore, to the best of our knowledge, we have achieved the largest reported bandwidth with Mo/Al/Sc at 57 nm and the narrowest bandwidth with Al/Sc at a 60 nm wavelength. These new and promising results demonstrate that Al/Sc-based multilayer coatings are excellent candidates for future generations of extreme ultraviolet (EUV) instruments for solar physics, EUV lasers, and attosecond science, in a wavelength range that has not been fully explored.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Attosecond light science and its application for probing quantum materials

In this paper, we review the development and application of coherent short wavelength light sources implemented using the high harmonic generation (HHG) process. The physics underlying HHG brought quantum physics into the domain of attosecond time-scales for the first time. Here, the observation and manipulation of electron dynamics on such short time-scales—a capability not conceived—of just a few decades ago—is becoming both more-and-more sophisticated and useful as a route to achieve exquisite control over short wavelength light. New experimental techniques are enabling HHG light sources to provide new insights into fundamental quantum interactions in materials, making it possible for the first time to capture the fastest charge, spin, photon and phonon interactions and to achieve diffraction-limited imaging at short wavelengths.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Complex Attosecond Waveform Synthesis at FEL FERMI

Free-electron lasers (FELs) can produce radiation in the short wavelength range extending from the extreme ultraviolet (XUV) to the X-rays with a few to a few tens of femtoseconds pulse duration. These facilities have enabled significant breakthroughs in the field of atomic, molecular, and optical physics, implementing different schemes based on two-color photoionization mechanisms. In this article, we present the generation of attosecond pulse trains (APTs) at the seeded FEL FERMI using the beating of multiple phase-locked harmonics. We demonstrate the complex attosecond waveform shaping of the generated APTs, exploiting the ability to manipulate independently the amplitudes and the phases of the harmonics. The described generalized attosecond waveform synthesis technique with an arbitrary number of phase-locked harmonics will allow the generation of sub-100 as pulses with programmable electric fields.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Ultrafast adiabatic frequency conversion

Abstract Ultrafast adiabatic frequency conversion is a powerful method, capable of efficiently and coherently transfering ultrashort pulses between different spectral ranges, e.g. from near-infrared to mid-infrared, visible or ultra-violet. This is highly desirable in research fields that are currently limited by available ultrafast laser sources, e.g. attosecond science, strong-field physics, high-harmonic generation spectroscopy and multidimensional mid-infrared spectroscopy. Over the past decade, adiabatic frequency conversion has substantially evolved. Initially applied to quasi-monochromatic, undepleted pump interactions, it has been generalized to include ultrashort, broadband, fully-nonlinear dynamics. Through significant theoretical development and experimental demonstrations, it has delivered new capabilities and superior performance in terms of bandwidth, efficiency and robustness, as compared to other frequency conversion techniques. This article introduces the concept of adiabatic nonlinear frequency conversion, reviews its theoretical foundations, presents significant milestones and highlights contemporary ultrafast applications that may, or already do, benefit from utilizing this method.

Margules, Peleg (ORCID:0000000335573370)↗
DOE OSTI2022

Generation of Intense Low-Divergence Isolated Soft-X-Ray Attosecond Pulses in a Gas-Filled Waveguide Using Three-Color Synthesized Laser Pulses

Isolated attosecond pulses (IAPs) in the soft-x-ray (SXR) region have been successfully produced via high-order harmonic generation in a gas medium at several laboratories, but pulse energies are much lower compared to the IAPs in the extreme ultraviolet. Here, we show that in a gas-filled hollow waveguide, an efficient gating method using a few-cycle three-color synthesizer is able to generate stronger SXR IAPs. We show that an 104-as IAP in the SXR region (central energy of 210 eV) with a higher pulse energy (0.9 nJ) and a lower divergence (within 1.5 mrad) can be generated with a three-color laser beam for input pulse energy at 0.62 mJ, under the condition of optimal gas pressure and waveguide length. The enhancement of the IAP is attributed to favorable phase matching of SXR high harmonics caused by the evolution of the three-color waveform during its propagation in the waveguide, which can be understood by analyzing the time shift of the waveform due to the interplay of the waveguide mode, atomic dispersion, and plasma dispersion. We check that the gating method is quite robust with respect to the phase jitter in the waveform. The advantage of this method is further demonstrated by comparing the generation of SXR high harmonics and attosecond pulses with two other schemes: the three-color waveform in a gas cell and a previously optimized two-color waveform in a gas-filled waveguide.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Attosecond time delay in atomic photoionization: Angular-dependent transition from dipole to quadrupole and spin-flip dynamics

The angular distribution of attosecond Wigner time delay has been investigated including both quadrupole and relativistic effects using the relativistic-random-phase approximation that is based on the Dirac equation and includes significant aspects of many-body correlations. Here the results show a dramatic evolution of the time delay from (essentially nonrelativistic) dipole to quadrupole and spin-flip dynamics as a function of angle, thereby providing a venue for studying these interactions at the attosecond level.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Non-linear enhancement of ultrafast X-ray diffraction through transient resonances

Diffraction-before-destruction imaging with ultrashort X-ray pulses can visualize non-equilibrium processes, such as chemical reactions, with sub-femtosecond precision in the native environment. Here, a nanospecimen diffracts a single X-ray flash before it disintegrates. The sample structure can be reconstructed from the coherent diffraction image (CDI). State-of-the-art X-ray snapshots lack high spatial resolution because of weak diffraction signal. Bleaching effects from photo-ionization significantly restrain image brightness scaling. We find that non-linear transient ion resonances can overcome this barrier if X-ray laser pulses are shorter than in most experiments. We compared snapshots from individual ≈ 100 nm Xe nanoparticles as a function of pulse duration and incoming X-ray fluence. Our experimental results and Monte Carlo simulations suggest that transient resonances can increase ionic scattering cross sections significantly beyond literature values. This provides a novel avenue towards substantial improvement of the spatial resolution in CDI in combination with sub-femtosecond temporal precision at the nanoscale.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Attosecond x-ray free-electron lasers utilizing an optical undulator in a self-selection regime

Accelerator-based x-ray free-electron lasers (XFELs) are the latest addition to the revolutionary tools of discovery for the 21st century. The two major components of an XFEL are an accelerator-produced electron beam and a magnetic undulator, which tend to be kilometer-scale long and expensive. A proof-of-principle demonstration of free-electron lasing at 27 nm using beams from compact laser wakefield accelerators was shown recently by using a magnetic undulator. However, scaling these concepts to x-ray wavelengths is far from straightforward as the requirements on the beam quality and jitters become much more stringent. Here, we present an ultracompact scheme to produce tens of attosecond x-ray pulses with several GW peak power utilizing a novel aspect of the FEL instability using a highly chirped, prebunched, and ultrabright tens of MeV electron beam from a plasma-based accelerator interacting with an optical undulator. The FEL resonant relation between the prebunched period and the energy selects resonant electrons automatically from the highly chirped beam which leads to a stable generation of attosecond x-ray pulses. Furthermore, two-color attosecond pulses with subfemtosecond separation can be produced by adjusting the energy distribution of the electron beam so that multiple FEL resonances occur at different locations within the beam. Such a tunable coherent attosecond x-ray sources may open up a new area of attosecond science enabled by x-ray attosecond pump/probe techniques. Published by the American Physical Society 2024

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Three-dimensional theory of superradiant free-electron lasers

The solitonlike superradiant regime of free-electron lasers (FEL) offers a promising path towards ultrashort pulses, beyond the natural limit dictated by the bandwidth of the high-gain FEL instability. In this work we present a three-dimensional theory of the superradiant regime, including the effects of beam emittance and energy spread. Our work takes advantage of recent developments in nonlinear FEL theory to provide a fully analytical description of solitonlike superradiance. Our theory proves the existence of a diffraction-dominated steady-state regime in which the superradiant peak power grows indefinitely while leaving the pulse duration and on-axis intensity almost unchanged. These results are in excellent agreement with three-dimensional simulations and are supported by recent experimental results at the Linac Coherent Light Source. This work advances nonlinear FEL theory and provides a theoretical framework for the next generation of attosecond x-ray FELs. Published by the American Physical Society 2024

43 PARTICLE ACCELERATORS↗
DOE OSTI2020

Attosecond Time-Domain Measurement of Core-Level-Exciton Decay in Magnesium Oxide

Excitation of ionic solids with extreme ultraviolet pulses creates localized core-level excitons, which in some cases couple strongly to the lattice. In this paper, core-level-exciton states of magnesium oxide are studied in the time domain at the Mg L 2 , 3 edge with attosecond transient reflectivity spectroscopy. Attosecond pulses trigger the excitation of these short-lived quasiparticles, whose decay is perturbed by time-delayed near-infrared pulses. Combined with a few-state theoretical model, this reveals that the infrared pulse shifts the energy of bright (dipole-allowed) core-level-exciton states as well as induces features arising from dark core-level excitons. We report coherence lifetimes for the two lowest core-level excitons of 2.3 ± 0.2 and 1.6 ± 0.5 fs and show that these are primarily a consequence of strong exciton-phonon coupling, disclosing the drastic influence of structural effects in this ultrafast relaxation process.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Site-specific generation of excited state wavepackets with high-intensity attosecond x rays

High-intensity attosecond x rays can produce coherent superpositions of valence-excited states through two-photon Raman transitions. The broad-bandwidth, high-field nature of the pulses results in a multitude of accessible excited states. Multiconfigurational quantum chemistry with the time-dependent Schrödinger equation is used to examine population transfer dynamics in stimulated x-ray Raman scattering of the nitric oxide oxygen and nitrogen K-edges. Two pulse schemes initiate wavepackets of different characters and demonstrate how chemical differences between core-excitation pathways affect the dynamics. The population transfer to valence-excited states is found to be sensitive to the electronic structure and pulse conditions, highlighting complexities attributed to the Rabi frequency. The orthogonally polarized two- color-pulse setup has increased selectivity while facilitating longer, less intense pulses than the one-pulse setup. Population transfer in the 1s → Rydberg region is more effective but less selective at the nitrogen K-edge; the selectivity is reduced by double core-excited states. Result interpretation is aided by resonant inelastic x-ray scattering maps.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Laser-driven plasma sources of intense, ultrafast, and coherent radiation

High-power lasers can deliver extreme light intensities, but avoiding damage in optical components requires large beam sizes, hindering further advances. The use of plasma as a medium for generating and manipulating light avoids the damage thresholds of solid materials and can support extraordinarily bright radiation. In this work, we discuss here how parametric plasma amplification and relativistic high-order harmonic generation offer paths to the development of light sources with peak powers beyond the capabilities of solid-state optics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗