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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Broadband hard X-ray attosecond pulses from extremely chirped electron beams

Attosecond pulses from free-electron lasers have opened the doors to atomic site-specific studies of bound electronic dynamics on their natural, sub-femtosecond timescales. Key to their success has been electron beam shaping techniques enabling the generation of sub-femtosecond current spikes with peak currents on the order of 10 kA. We demonstrate in an RF linac the generation of current spikes with extreme chirps on the order of 350 MeV/micron, directly competitive with the chirps expected from beam-driven plasma wakefield accelerators. Leveraging chirp-taper compensation, we use these highly chirped beams to generate hard X-ray attosecond pulses with bandwidths exceeding 30 eV, a factor of two beyond previous demonstrations. We simultaneously present the first explicit experimental evidence of chirp-taper compensation in an attosecond XFEL, finding that optimal tapering improves the bandwidth and pulse energy by factors of two and five, respectively, for our conditions. In addition to the immediate utility of such broadband hard X-ray pulses, electron beams with such extreme chirps can be utilized for unique new experimental modalities by performing further compression after the undulators. Such post-lasing compression can enable subsequent superradiant light emission at longer wavelengths, or direct excitation of quantum systems with the beam's intense space-charge field for unique attosecond pump-probe possibilities.

43 PARTICLE ACCELERATORS↗
DOE OSTI2023

Direct reconstruction of isolated XUV or soft x-ray attosecond pulses from high-harmonic generation streaking spectra

Characterization of an isolated attosecond pulse (IAP) in the extreme ultraviolet (XUV) or soft x-ray (SXR) region is essential for its applications. Here we propose to retrieve an IAP in the time domain directly through the modulation of high-harmonic generation (HHG) spectra in the presence of a time-delayed intense few-cycle infrared or mid-infrared laser. The retrieval algorithm is derived based on the strong-field approximation and an extended quantitative rescattering model. We show that both isolated XUV pulses with a narrow spectral bandwidth and isolated SXR pulses with a broad bandwidth can be well characterized through the HHG streaking spectra. Such an all-optical method for characterizing the IAP differs from the commonly used approach based on the streaked photoelectron spectra that would require electron spectrometers. We check the robustness of the retrieval method by changing the dressing laser or by adjusting the steps of time delay. We also show that the XUV pulse can be accurately retrieved by treating the HHG streaking spectra calculated from solving the time-dependent Schrödinger equation for single atoms as the ‘experimental’ data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Circularly Polarized Attosecond Pulses Enabled by an Azimuthal Phase and Polarization Grating

High-harmonic generation (HHG) is an extreme nonlinear optical process that can map the properties of an infrared driving laser beam onto short wavelength attosecond pulse trains. However, current techniques for generating circularly polarized high harmonics for probing magnetic materials and chiral systems have limitations: two-color collinear counter-rotating driving lasers result in a low cutoff photon energy, while single-color non-collinear counter-rotating schemes suffer from low conversion efficiency. In this work, we generate circularly polarized attosecond pulse trains by using a structured laser driver which has a rotating polarization and phase grating along the azimuthal coordinate. Furthermore, our experimental and numerical results demonstrate the production of left and right circularly polarized harmonics, which naturally separate upon propagation. Our approach uses a single laser color in a collinear geometry, that can be scaled for high efficiency. Simulations show this scheme can extend into the soft x-ray region when driven by mid-infrared driving lasers, while preserving the same high phase-matching cutoff photon energy as for linearly-polarized high harmonics.

attosecond science↗
DOE OSTI2026

Quantum Interference in Two-Atom Resonant X-ray Scattering of an Intense Attosecond Pulse

We theoretically investigate resonant x-ray scattering from two noninteracting Ne+ ions driven by an intense attosecond pulse using a nonrelativistic, QED-based time-dependent framework. Our model includes Rabi oscillations, photoionization, Auger decay, and quantum interference among elastic scattering and resonance fluorescence pathways. We analyze how the total scattering signal depends on pulse intensity, atomic configuration, and initial electronic state. We find that the total resonant scattering yield exceeds its nonresonant counterpart; the angular dependence of the signal qualitatively resembles a two-atom structure factor; and the visibility of interference fringes is sensitive to pulse area and the initial electronic state. Only a subset of final states reached via resonance fluorescence exhibits interference, determined by the indistinguishability of photon emission pathways. Fringe visibility is maximized in the linear scattering regime, where ionization is minimal and resonance fluorescence pathways can be largely indistinguishable. These results highlight optimal conditions for applying ultrafast resonant x-ray scattering to single-particle imaging.

Venkatesh, Akilesh↗
DOE OSTI2024

“Beam à la carte”: Laser heater shaping for attosecond pulses in a multiplexed x-ray free-electron laser

Electron beam shaping allows the control of the temporal properties of x-ray free-electron laser pulses from femtosecond to attosecond timescales. Here, we demonstrate the use of a laser heater to shape electron bunches and enable the generation of attosecond x-ray pulses. We demonstrate that this method can be applied in a selective way, shaping a targeted subset of bunches while leaving the remaining bunches unchanged. This experiment enables the delivery of shaped x-ray pulses to multiple undulator beamlines, with pulse properties tailored to specialized scientific applications.

43 PARTICLE ACCELERATORS↗
DOE OSTI2025

Effect of Rabi dynamics in resonant x-ray scattering of intense attosecond pulses

Here, we theoretically study the effects of Rabi oscillations on resonant x-ray scattering in Ne + using intense attosecond and few-femtosecond pulses. The total photon yield strongly depends on the pulse area and has an upper bound at high intensities. Resonant scattering yields with attosecond pulses can be an order of magnitude higher than those far from resonances. Interference between resonance fluorescence and elastic scattering channels depends on the pulse area and initial state. Our results suggest that resonant x-ray scattering can be exploited for high-resolution, site-specific imaging.

Venkatesh, Akilesh [Argonne National Laboratory (A↗
DOE OSTI2025

Broadband coherent XUV light from e − / e + microbunching in an intense laser pulse

Attosecond pulses of coherent extreme ultraviolet (XUV) light are instrumental for investigating subatomic dynamics and can be produced using a free-electron laser (FEL). It has been suggested that an optical FEL, which employs a laser pulse in place of a conventional undulator, could enable a dramatically more compact implementation of such a light source. Yet, the high electron density and subsequent high emittance implied by an optical FEL makes this concept challenging to realize with an electron beam. There has been impressive progress in recent years producing collimated dense and relativistic beams of electrons and positrons in the laboratory. As we demonstrate here, the inherent stability of a quasi-neutral electron-positron beam mitigates Coulomb expansion, and renders it a promising alternative source of coherent light. Specifically, we show via computer simulations that broadband coherent light in the XUV domain, which takes the form of 8-as pulses at 92-as intervals, can be generated by microbunching of relativistic electrons and positrons in a laser pulse. This process occurs over a sub-millimeter length scale, enabling the development of light sources which are orders-of-magnitude more compact than existing sources, with potential applications in physics, chemistry, biology, and industry.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Attosecond control and measurement of chiral photoionization dynamics

Many chirality-sensitive light–matter interactions are governed by chiral electron dynamics. Therefore, the development of advanced technologies making use of chiral phenomena would critically benefit from measuring and controlling chiral electron dynamics on their natural attosecond timescales. Such endeavours have so far been hampered by the lack of characterized circularly polarized attosecond pulses, an obstacle that has recently been overcome. Here we introduce chiroptical spectroscopy with attosecond pulses and demonstrate attosecond coherent control over photoelectron circular dichroism (PECD), as well as the measurement of chiral asymmetries in the forward–backward and angle-resolved photoionization delays of chiral molecules. We show that co-rotating attosecond and near-infrared (IR) pulses can nearly double the PECD and even change its sign compared with single-photon ionization. We demonstrate that chiral photoionization delays depend on both polar and azimuthal angles of photoemission in the light-propagation frame, requiring 3D momentum resolution. We measure forward–backward chiral-sensitive delays of up to 60 as and polar-angle-resolved photoionization delays of up to 240 as, which include an asymmetry of about 60 as originating from chirality in the continuum–continuum transitions. Attosecond chiroptical spectroscopy opens the door to quantitatively understanding and controlling the dynamics of chiral molecules on the electronic timescale.

Atomic and molecular interactions with photons↗
DOE OSTI2026

A tutorial on high-order harmonic generation in atoms, molecules, and condensed matter

This tutorial introduces strong-field-driven high-order harmonics, their experimental generation and characterization techniques, and their main applications including attosecond pulse generation and ultrafast spectroscopy of the target material. We begin from the use of atomic targets, where the first high-order harmonic generation (HHG) experiments were realized in the late 1980s. Then, we briefly discuss the basics of the microscopic generation mechanism and how various steps of the mechanism were exploited in applications such as generating isolated attosecond pulses and probing molecular orbitals. We introduce and describe the standard experimental approaches for condensed phase HHG, where we discuss unique technical challenges of the use of solid-state materials, such as the mitigation of plasma formation and laser damage. We cover the fundamentals of high-harmonic spectroscopy in condensed matter systems, such as wide bandgap dielectrics, semiconductors, liquid media, and 2D-crystals. We provide some examples of rapidly emerging spectroscopic capabilities, such as for probing crystal symmetries, Berry phases, and associated non-trivial topological properties of the source material. Finally, we provide an overview of the research field, including some of the challenges, opportunities, and open questions.

Attosecond pulses↗
DOE OSTI2024

Attosecond-pump attosecond-probe x-ray spectroscopy of liquid water

Attosecond-pump/attosecond-probe experiments have long been sought as the most straightforward method for observing electron dynamics in real time. Although there has been much success with overlapped near-infrared femtosecond and extreme ultraviolet attosecond pulses combined with theory, true attosecond-pump/attosecond-probe experiments have been limited. Here we used a synchronized attosecond x-ray pulse pair from an x-ray free-electron laser to study the electronic response to valence ionization in liquid water through all x-ray attosecond transient absorption spectroscopy (AX-ATAS). Our analysis showed that the AX-ATAS response is confined to the subfemtosecond timescale, eliminating any hydrogen atom motion and demonstrating experimentally that the 1b 1 splitting in the x-ray emission spectrum is related to dynamics and is not evidence of two structural motifs in ambient liquid water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Attosecond impulsive stimulated X-ray Raman scattering in liquid water

We report the measurement of impulsive stimulated x-ray Raman scattering in neutral liquid water. An attosecond pulse drives the excitations of an electronic wavepacket in water molecules. The process comprises two steps: a transition to core-excited states near the oxygen atoms accompanied by transition to valence-excited states. Thus, the wavepacket is impulsively created at a specific atomic site within a few hundred attoseconds through a nonlinear interaction between the water and the x-ray pulse. We observe this nonlinear signature in an intensity-dependent Stokes Raman sideband at 526 eV. Our measurements are supported by our state-of-the-art calculations based on the polarization response of water dimers in bulk solvation and propagation of attosecond x-ray pulses at liquid density.

Science & Technology - Other Topics↗
DOE OSTI2023

Complete spectroscopy in the attosecond regime

Harnessing light waveforms at attosecond time scales provides information of the structure and dynamics of matter on it's natural time scales. For this reason attosecond metrology has been at the forefront of the optical sciences for more than a decade, and it represents the latest time-domain frontier of the quantum world. Attosecond light pulses are commonly generated using higher-order harmonic generation (HHG) , a process capable of generating XUV coherent pulses. In addition to generate attosecond pulses, HHG can be used to study the structure and dynamics of atoms and molecules by analyzing the spectral content of the XUV pulses. This approach is known as HHG spectroscopy and it provides a coherent, time-dependent approach to study structure and dynamics in the quantum world. In this proposal we will generate harmonics from two optical foci produced by a system of a two-dimensional spatial light modulator (SLM) and a lens. In the far eld the train of attosecond pulses will interfere creating harmonic-dependent fringes. The position of such fringes is a direct measurement of the relative phase between the two foci and they also carry information about the quantum state of the target atom or molecule. Therefore, by measuring the amplitude and relative phase of the emitted harmonics we will have access to both, the amplitude and phase of the dipole moments of the studied target. Because the two beams are completely indistinguishable from each other up to a few millimeters from the focus, both driving pulses share the exact beam path. So far we have measured a jitter of 700 zeptoseconds with a 12.5 attosecond resolution in the delay control of the two foci. These two time scales represent some of the best time controls ever achieved to date.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Probing Attosecond Bound Electron Dynamics Driven by Strong-Field Light Transients

The project aimed to drive strong-field excitation of bound electronic coherences in gas-phase atoms and molecules using a novel source of near-single-cycle optical field transients, based on industrial-grade Yb:solid-state laser technology. Key objectives included generating near-single cycle field transients and isolated attosecond pulses, reconstructing time-dependent wave packets in atoms and molecules, probing their decoherence using attosecond interferometry, and controlling the dynamic evolution of systems on attosecond to few-femtosecond timescales. A secondary goal of the project was to develop field-resolved measurement platforms as a novel approach for studying electron dynamics in atomic and molecular systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Angularly resolved photoionization dynamics in atoms and molecules combining temporally and spectrally resolved experiments at ATTOLab and Synchrotron SOLEIL

We report results for XUV-IR two-photon ionization of Ar, Ne, NO, and O2, where an XUV attosecond pulse train is superimposed with a synchronized IR pulse, obtained at the ATTOLab laser facility using electron–ion coincidence 3D momentum spectroscopy. Temporally resolved photoelectron angular distributions providing angle-resolved time-delays for np ionization of Ar and Ne, achieved by reconstruction of attosecond beating by interference of two-photon transitions through a unified formalism (Joseph et al. in J Phys B At Mol Opt Phys 53:184007, 2020), are summarized. For inner valence XUV-IR dissociative photoionization of NO and O2 molecules, we report electron–ion kinetic energy correlation diagrams and disentangle the dissociative photoionization processes relying on parallel XUV experiments at Synchrotron SOLEIL. For ionization into the NO+(c3Π) ionic state, extending the formalism developed for single-photon ionization, we focus on photoelectron angular distributions averaged on the delay between the XUV and the IR field in the field frame, molecular frame, and electron frame of reference.

Joseph, J↗
DOE OSTI2024

Controlling laser-dressed resonance line shape using attosecond extreme-ultraviolet pulse with a spectral minimum

High-harmonic generation from a gas target exhibits sharp spectral features and rapid phase variation near the Cooper minimum. By applying spectral filtering, shaped isolated attosecond pulses can be generated where the pulse is split into two in the time domain. Using such shaped extreme-ultraviolet (XUV) pulses, we theoretically study attosecond transient absorption (ATA) spectra of helium 2s2p autoionizing state which is resonantly coupled to the 2s 2 dark state by a time-delayed infrared laser. Our simulations show that the asymmetric 2s2p Fano line shape can be readily tuned into symmetric Lorentzian within the time delay of a few tens of attoseconds. Such efficient control is due to the destructive interference in the generation of the 2s2p state when it is excited by a strongly shaped XUV pulse. This is to be compared to prior experiments where tuning the line shape of a Fano resonance would take tens of femtoseconds. We also show that the predicted ATA spectral line shape can be observed experimentally after propagation in a gas medium. Our results suggest that strongly shaped attosecond XUV pulses offer the opportunity for controlling and probing fine features of narrow resonances on the few-ten attoseconds timescale.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗