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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Bond-length dependence of attosecond ionization delays in O 2 arising from electron correlation to a shape resonance

We experimentally and theoretically demonstrate that electron correlation can cause the bond-length sensitivity of a shape resonance to induce an unexpected vibrational state–dependent ionization delay in a nonresonant channel. This discovery was enabled by a high-resolution attosecond-interferometry experiment based on a 400-nm driving and dressing wavelength. The short-wavelength driver results in a 6.2–electron volt separation between harmonics, markedly reducing the spectral overlap in the measured interferogram. We demonstrate the promise of this method on O 2 , a system characterized by broad vibrational progressions and a dense photoelectron spectrum. We measure a 40-attosecond variation of the photoionization delays over the X 2 Π g vibrational progression. Multichannel calculations show that this variation originates from a strong bond-length dependence of the energetic position of a shape resonance in the b 4 Σ$^{-}_{g}$ channel, which translates to the observed effects through electron correlation. The unprecedented energy resolution and delay accuracies demonstrate the promise of visible-light–driven molecular attosecond interferometry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Intense infrared lasers for strong-field science

The advent of chirped-pulse amplification in the 1980s and femtosecond Ti:sapphire lasers in the 1990s enabled transformative advances in intense laser–matter interaction physics. Whereas most of experiments have been conducted in the limited near-infrared range of 0.8–1 μm, theories predict that many physical phenomena such as high harmonic generation in gases favor long laser wavelengths in terms of extending the high-energy cutoff. Significant progress has been made in developing few-cycle, carrier-envelope phase-stabilized, high-peak-power lasers in the 1.6–2 μm range that has laid the foundation for attosecond X ray sources in the water window. Even longer wavelength lasers are becoming available that are suitable to study light filamentation, high harmonic generation, and laser–plasma interaction in the relativistic regime. Long-wavelength lasers are suitable for sub-bandgap strong-field excitation of a wide range of solid materials, including semiconductors. In the strong-field limit, bulk crystals also produce high-order harmonics. In this review, we first introduce several important wavelength scaling laws in strong-field physics, then describe recent breakthroughs in short- (1.4–3 μm), mid- (3–8 μm), and long-wave (8–15 μm) infrared laser technology, and finally provide examples of strong-field applications of these novel lasers. Furthermore, some of the broadband ultrafast infrared lasers will have profound effects on medicine, environmental protection, and national defense, because their wavelengths cover the water absorption band, the molecular fingerprint region, as well as the atmospheric infrared transparent window.

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 OSTI2023

Electron bunch dynamics and emission in particle-in-cell simulations of relativistic laser–solid interactions: On density artifacts, collisions, and numerical dispersion

Sub-optical-cycle dynamics of dense electron bunches in relativistic-intensity laser–solid interactions lead to the emission of high-order harmonics and attosecond light pulses. The capacity of particle-in-cell simulations to accurately model these dynamics is essential for the prediction of emission properties because the attosecond pulse intensity depends on the electron density distribution at the time of emission and on the temporal distribution of individual electron Lorentz-factors in an emitting electron bunch. Here, we show that in one-dimensional collisionless simulations, the peak density of the emitting electron bunch increases with the increase in the spatial resolution of the simulation grid. When collisions are added to the model, the peak electron density becomes independent of the spatial resolution. Collisions are shown to increase the spread of the peaks of Lorentz-factors of emitting electrons in time, especially in the regimes far from optimum generation conditions, thus leading to lower intensities of attosecond pulses as compared to those obtained in collisionless simulations.

Physics↗
DOE OSTI2025

Bringing weak transitions to light

Abstract Weak transitions between quantum states are of fundamental importance for a broad range of phenomena from analytical biochemistry to precision physics, but generally challenge experimental detection. Due to their small cross sections scaling with the absolute square of their transition matrix elements, spectroscopic measurements often fail in particular in the presence of competing background processes. Here we introduce a general concept to break this scaling law and enhance the transition probability by exploiting a stronger laser-coupled pathway to the same excited state. We demonstrate the concept experimentally by attosecond transient absorption spectroscopy in helium atoms. The quasi-forbidden transitions from the ground state 1s 2 to the weakly coupled doubly excited 2p3dandsp 2,4− states are boosted by an order of magnitude. Enhancing single-photon-suppressed transitions can find widespread applicability, from spectral diagnostics of complex molecules in life and chemical sciences to precision spectroscopy of weak transitions in metastable atomic nuclei in the search for new physics.

Science & Technology - Other Topics↗
DOE OSTI2025

Resonant propagation of extreme-ultraviolet pulses through strongly driven high-density media

We show that by combining strong-field dressing and resonant propagation of XUV pulses, the transition of absorption lines from their natural Lorentzian profiles through Fano and complex multipeak shapes all the way back to broadened near-Lorentzian profiles can be achieved, in the limit of optically thick samples. The final stage of this spectral modification can be understood in terms of a significant temporal stretching and delay of the resonant XUV pulse as it propagates through the dense gas, which alters the ultrafast absorption that is modified by the time-synchronized few-femtosecond laser pulse. We first demonstrate this concept in numerical calculations, both using a model system and through a fully coupled solution of the time-dependent Schrödinger equation and the Maxwell wave equation. The applicability and generality of the underlying mechanism is then illustrated in proof-of-principle attosecond transient absorption measurements in a helium gas with a widely varying atomic density. These results provide insights into the interaction of ultrashort laser pulses with dense media and its coherent control. Published by the American Physical Society 2025

He, Yu (ORCID:0000000152120176)↗
DOE OSTI2021

Generation of isolated soft x-ray attosecond pulses with mid-infrared driving lasers via transient phase-matching gating

Abstract Isolated attosecond pulses (IAPs) in the soft x-ray (SXR) region are highly desirable for attosecond time-resolved experiments. Here we identify a transient phase matching gating method for the generation of such IAPs with mid-infrared (MIR) lasers. This gating method works when a loosely focused, long-duration MIR Gaussian driving beam is slightly reshaped during its propagation in the gas medium under the ‘critical’ ionization condition. Quantitatively, the calculated coherence length of high harmonic is used to analyze the mechanism of the gating method, by using one-dimensional plane-wave beams and by comparing 2000 nm and 800 nm lasers. The robustness of the generation method is checked by varying laser’s carrier-envelope-phase and gas pressure. This gating method provides with an alternative route to efficiently produce tabletop ultrashort attosecond SXR light sources with the emerging MIR lasers.

Physics↗
DOE OSTI2024

Generation of attosecond gigawatt soft x-ray pulses through coherent Thomson backscattering

Collision between relativistic electron sheets and counterpropagating laser pulses is recognized as a promising way to produce intense attosecond x rays through coherent Thomson backscattering (TBS). In a double-layer scheme, the electrons in an ultrathin solid foil are first pushed out by an intense laser driver and then interact with the laser reflected off a second foil to form a high-density relativistic electron sheet with vanishing transverse momentum. However, the repulsion between these concentrated electrons can increase the thickness of the layer, reducing both its density and subsequently the coherent TBS. Here, we present a systematic study on the evolution of the flying electron layer and find that its resulting thickness is determined by the interplay between the intrinsic space-charge expansion and the velocity compression induced by the drive laser. How the laser driver, the target areal density, the reflector, and the collision laser intensity affect the properties of the produced x rays is explored. Multidimensional particle-in-cell simulations indicate that employing this scheme in the nonlinear regime has the potential to stably produce soft x rays with several gigawatt peak power in hundreds of terawatt ultrafast laser facilities. The pulse duration can be tuned to tens of attoseconds. Here, this compact and intense attosecond x-ray source may have broad applications in attosecond science.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Metrology of Time-Domain Soft X-Ray Attosecond Pulses and Reevaluation of Pulse Durations of Three Recent Experiments

Attosecond pulses in the soft x-ray (SXR) to water-window energy region offer the tools for creating and studying target-specific localized inner-shell electrons or holes in materials, enabling monitoring or controlling charge and energy flows in a dynamic system on attosecond timescales. Recently, a number of laboratories have reported generation of continuum harmonics in the hundred-electron-volt to kilovolt region with few-cycle long-wavelength mid-infrared lasers. These harmonics have the bandwidth to support pulses with durations of a few to a few-ten attoseconds. But harmonics generated in a gas medium have attochirps that cannot be fully compensated by materials over a broad spectral range; thus, realistically what are the typical shortest attosecond pulses that one can generate? To answer this question, it is essential that the temporal attosecond pulses be accurately characterized. By reanalyzing the soft x-ray attosecond metrology reported in three recent experiments using a newly developed broadband phase retrieval algorithm, we demonstrate here that the generated attosecond pulses in the first two papers have durations of about 60 as, longer than what they have reported. Similarly, the duration from the third experiment is retrieved to be about half of the 322-as upper limit cited in that work. We also introduce the autocorrelation (AC) of the streaking spectrogram. By comparing the ACs from the experiments and from the retrieved SXR pulses, the accuracy of the retrieved results can be directly visualized. Our retrieval method is fast and accurate, and it shall provide a powerful tool for the metrology of the emerging few-ten-attosecond pulses.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Shaping attosecond pulses by controlling the minima in high-order harmonic generation through alignment of CO 2 molecules

In this paper, we report a simple method for generating shaped attosecond pulses by using a CO 2 molecule. Unlike most other molecules, owing to its unique energy and angle dependence and the presence of deep minima in the photoionization transition dipole moment, the shape of harmonic spectra, especially the position and depth of minima, can be readily controlled by tuning the degree of alignment. The sensitive alignment dependence of the minima is due to the coherent interference of a laser-induced dipole from each molecule when CO 2 molecules are moderately aligned, but not when they are well aligned or when they are isotropically distributed. Such a sensitivity offers a simple way of controlling the spectral amplitude and phase of the generated harmonics and thus shaping the generated attosecond pulses, for example, producing structured attosecond pulses by splitting a single burst into two. We illustrate how such pulses are generated and how to characterize them. This method offers a simple way to shape attosecond pulses at the generation step. It can be easily implemented experimentally to generate attosecond pulses with strong phase variations for unique applications.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Light-Matter Interaction near the Schwinger Limit Using Tightly Focused Doppler-Boosted Lasers

Strong-field quantum electrodynamics (SF QED) is a burgeoning research topic dealing with electromagnetic fields comparable to the Schwinger field (≈1.32×10 18 V/m). While most past and proposed experiments rely on reaching this field in the rest frame of relativistic particles, the Schwinger limit could also be approached in the laboratory frame by focusing to its diffraction limit the light reflected by a plasma mirror irradiated by a multipetawatt laser. Here, we explore the interaction between such intense light and matter with particle-in-cell simulations. We find that the collision with a relativistic electron beam would enable the study of the nonperturbative regime of SF QED, while the interaction with a solid target leads to a profusion of SF QED effects that retroact on the interaction. In both cases, relativistic attosecond pair jets with high densities are formed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Attosecond synchronization of extreme ultraviolet high harmonics from crystals

The interaction of strong near-infrared (NIR) laser pulses with wide-bandgap dielectrics produces high harmonics in the extreme ultraviolet (XUV) wavelength range. These observations have opened up the possibility of attosecond metrology in solids, which would benefit from a precise measurement of the emission times of individual harmonics with respect to the NIR laser field. In this work, we show that, when high-harmonics are detected from the input surface of a magnesium oxide crystal, a bichromatic probing of the XUV emission shows a clear synchronization largely consistent with a semiclassical model of electron–hole recollisions in bulk solids. On the other hand, the bichromatic spectrogram of harmonics originating from the exit surface of the 200 μm-thick crystal is strongly modified, indicating the influence of laser field distortions during propagation. Our tracking of sub-cycle electron and hole re-collisions at XUV energies is relevant to the development of solid-state sources of attosecond pulses.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Control of electron recollision and molecular nonsequential double ionization

Abstract Intense laser pulses lasting a few optical cycles, are able to ionize molecules via different mechanisms. One such mechanism involves a process whereby within one optical period an electron tunnels away from the molecule, and is then accelerated and driven back as the laser field reverses its direction, colliding with the parent molecule and causing correlated non-sequential double ionization (NSDI). Here we report control over NSDI via spectral-phase pulse shaping of femtosecond laser pulses. The measurements are carried out on ethane molecules using shaped pulses. We find that the shaped pulses can enhance or suppress the yield of dications resulting from electron recollision by factors of 3 to 6. This type of shaped pulses is likely to impact all phenomena stemming from electron recollision processes induced by strong laser fields such as above threshold ionization, high harmonic generation, attosecond pulse generation, and laser-induced electron diffraction.

74 ATOMIC AND MOLECULAR PHYSICS↗