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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Electron interference in atomic ionization by two crossing polarized ultrashort pulses

Formation of geometrically regular interference patterns in the photoelectron momentum distributions (PMDs) corresponding to the photoionization of atoms by two single-color, crossing ultrashort pulses is investigated both analytically and numerically. It is shown that, in contrast to the photoionization by monochromatic pulses, PMDs for the ionization by crossing and co-propagating broadband pulses are essentially different (unless both pulses are linearly polarized), namely, when one pulse is linearly polarized along the propagation direction, ˆk, of the circularly polarized (CP) pulse, then interference maxima (minima) of the ionization probability have the form of three-dimensional single-arm regular spirals which are wound along ˆk. Next, the interference maxima (minima) of the ionization probability by a pair of crossing elliptically polarized pulses have the form of either Newton's rings or two-arm Fermat's spirals, depending on the position of a detection plane. Remarkably, these regular patterns occur only for certain values of the pulse ellipticities, and they become distorted for CP pulses. For both above-mentioned pulse configurations, the features of interference patterns depend on the time delay between pulses, their relative electric field amplitude, and relative carrier-envelope phase. Our predictions, illustrated by the numerical results for the ionization of H and He atoms by two orthogonal pulses, are quite general and we expect them to be valid for the ionization of any randomly oriented atomic or molecular target.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Absorption properties of graphene quantum dots under ultrashort optical pulses

Here, we study the interaction of graphene quantum dots (GQDs) with ultrashort and strong optical pulses theoretically. An important characteristic of such interaction is the energy accumulated by GQDs after the pulse. We show that the GQD absorbance has a highly nonlinear dependence on the field amplitude. At small-field amplitudes, the absorbance strongly depends on the frequency of the pulse and the band gap of a QD, i.e., its size. At large-field amplitudes, ~1 V/Å, the absorbance has a weak nonmonotonic dependence on the size of the dot with its maximum value of ≈ 4.5 % realized for GQD consisting of ≈ 60 atoms. As a function of the field amplitude, the absorbance also has a maximum, the position of which depends on the size of the dot.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Enhanced Self-Seeding with Ultrashort Electron Beams

In this paper, we describe a new method to produce intensity stable, highly coherent, narrow-band x-ray pulses in self-seeded free electron (FEL) lasers. The approach uses an ultrashort electron beam to generate a single spike FEL pulse with a wide coherent bandwidth. The self-seeding monochromator then notches out a narrow spectral region of this pulse to be amplified by a long portion of electron beam to full saturation. In contrast to typical self-seeding where monochromatization of noisy self-amplified spontaneous emission pulses leads to either large intensity fluctuations or multiple frequencies, we show that this method produces a stable, coherent FEL output pulse with statistical properties similar to a fully coherent optical laser.

43 PARTICLE ACCELERATORS↗
DOE OSTI2024

In situ characterization of two unknown ultrashort laser pulses using four-wave mixing in gas

Accurate characterization of two ultrashort laser pulses is of great interest in many ultrafast pump-probe experiments. We demonstrate a method based on four-wave mixing (FWM) in a gas which could be easily implemented into many existing pump-probe setups with minimal modifications for accurate, in situ characterization of both unknown pulses. This technique is tested on pairs of unknown pulses at wavelengths of 400/800 nm, and 266/400 nm. We measured the spectrogram of the pulse generated through FWM of the two unknown pulses by scanning the delay between two unknown pulses. The retrieval algorithm converges to accurately predict the intensity and the phase profiles of both unknown pulses with a trace error of < 1% and the accuracy is verified using an independent pulse characterization device.

Nambu, Noa (ORCID:0000000197303400)↗
DOE OSTI2024

Demonstration of a 1 TW peak power, joule-level ultrashort Tm:YLF laser

Here we report on the demonstration of a diode-pumped, Tm:YLF-based, chirped pulse amplification laser system operating at λ ≈ 1.9 µm that produces amplified pulse energies exceeding 1.5 J using a single 8-pass power amplifier. The amplified pulses are subsequently compressed to sub-300 fs durations by a diffraction grating pair, producing record >1 TW peak power pulses. To the best of our knowledge, this is the highest peak power demonstrated for any solid-state, near-2 µm laser architecture and illustrates the potential of Tm:YLF for the next generation of high-power, diode-pumped ultrashort lasers.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Ultrashort Laser Pulse Shaping and Characterization for Tailored Electron Bunch Generation

Temporally shaped laser pulses are desirable in various applications including emittance reduction and beam-driven acceleration. Pulse shaping techniques enable flexible controls over the longitudinal distribution of electron bunches emitted from the photocathode. While direct manipulation and measurement of an ultrashort pulse can be challenging in the time domain, both actions can be performed in the frequency domain. In this paper, we report the study and development of laser shaper and diagnostics at Argonne Wakefield Accelerator (AWA). Simulations of the shaping process for several sought-after shapes are presented along with the temporal diagnosis. Status of the experiment at the AWA facility is also discussed.

43 PARTICLE ACCELERATORS↗
DOE OSTI2022

Control of valley polarization in gapped graphene by linearly polarized ultrashort optical pulse

We present a versatile model of gapped graphene to manipulate valley polarization by using ultrafast linearly polarized pulses of zero areas. First, a circularly polarized pulse of a single oscillation produces a valley-selective population of the conduction band by means of topological resonance. Then we apply a linearly polarized femtosecond-long pulse that changes the valley polarization. The magnitude of such a change depends on the amplitude and the direction of polarization of the pulse. In conclusion, our protocol provides a favorable platform for applications in valleytronics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

A review of ptychographic techniques for ultrashort pulse measurement

The measurement of optical ultrafast laser pulses is done indirectly because the required bandwidth to measure these pulses exceeds the bandwidth of current electronics. As a result, this measurement problem is often posed as a 1-D phase retrieval problem, which is fraught with ambiguities. The phase retrieval method known as ptychography solves this problem by making it possible to measure ultrafast pulses in either the time domain or the frequency domain. One well known algorithm is the principal components generalized projections algorithm (PCGPA) for extracting pulses from Frequency-Resolved Optical Gating (FROG) measurements. In this work, we discuss the development of the PCPGA and introduce new developments including an operator formalism that allows for the convenient addition of external constraints and the development of more robust algorithms. A close cousin, the ptychographic iterative engine will also be covered and compared to the PCGPA. Additional developments using other algorithmic strategies will also be discussed along with new developments combining optics and high-speed electronics to achieve megahertz measurement rates.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Ultraintense, ultrashort pulse X-ray scattering in small molecules

In this work, we examine X-ray scattering from an isolated organic molecule from the linear to nonlinear absorptive regime. In the nonlinear regime, we explore the importance of both the coherent and incoherent channels and observe the onset of nonlinear behavior as a function of pulse duration and energy. In the linear regime, we test the sensitivity of the scattering signal to molecular bonding and electronic correlation via calculations using the independent atom model (IAM), Hartree–Fock (HF) and density functional theory (DFT). Finally, we describe how coherent X-ray scattering can be used to directly visualize femtosecond charge transfer and dissociation within a single molecule undergoing X-ray multiphoton absorption.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

X-ray detection of ultrashort spin current pulses in synthetic antiferromagnets

Here, we explore the ultrafast generation of spin currents in magnetic multilayer samples by applying fs laser pulses to one layer and measuring the magnetic response in the other layer by element-resolved x-ray spectroscopy. In Ni(5 nm)/Ru(2 nm)/Fe(4 nm), the Ni and Fe magnetization directions couple antiferromagnetically due to the Ruderman–Kittel–Kasuya–Yosida interaction but may be oriented parallel through an applied magnetic field. After exciting the top Ni layer with a fs laser pulse, we also find that the Fe layer underneath demagnetizes, with a 4.1±1.9% amplitude difference between parallel and antiparallel orientation of the Ni and Fe magnetizations. We attribute this difference to the influence of a spin current generated by the fs laser pulse that transfers angular momentum from the Ni into the Fe layer. Our results confirm that superdiffusive spin transport plays a role in determining the sub-ps demagnetization dynamics of synthetic antiferromagnetic layers, but also evidence large depolarization effects due to hot electron dynamics, which are independent of the relative alignment of the magnetization in Ni and Fe.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Generation of gamma radiation by a subterawatt ultrashort laser pulse: optimisation of preplasma and pulse duration

We report an experimental and numerical study of the acceleration of electrons in a plasma interacting with a subterawatt laser pulse (intensity of ∼3 × 10{sup 18} W cm{sup −2} at a pulse duration of 50 fs). A preplasma layer on the surface of a molybdenum target is formed by an additional laser pulse with a duration of 8 ns and an intensity of ∼2 × 10{sup 12} W cm{sup −2}. It is shown that an increase in the laser pulse duration to 1700 fs at a constant energy (and a proportional decrease in intensity) leads to an increase in the yield of bremsstrahlung γ-radiation by more than an order of magnitude when the nanosecond pulse is ahead of the femtosecond one by 15 − 25 ns. Interferometry data and results of diagnostics of optical and γ-radiation of a plasma demonstrate that the collisional ionisation of atoms by electrons oscillating in the field of such a laser pulse plays an essential role in the formation of electron density profile. The sensitivity of the described effect to the level of amplified spontaneous emission is determined, despite the nanosecond pulse impact. Numerical simulations show that at a large pulse duration, the acceleration of electrons is stipulated by the beaking of plasma waves excited during stimulated Raman scattering of laser radiation. (paper)

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Accuracy of the duration estimates of ultrashort laser pulses using a single-shot second-order intensity autocorrelator

The accuracy of estimating the duration of single-cycle laser pulses with centre wavelengths of 910 and 780 nm is analysed using a single-shot second-order intensity autocorrelator. It is shown that estimates of the single-cycle pulse duration with an error of less than 5 % require the use of KDP crystals with a thickness of no more than 10 μm for the second harmonic generation. At the same time, to estimate the duration of a transform-limited pulse containing ten optical cycles, the crystal thickness can be up to 1 mm. In this case, at an optimum angle of convergence of the first-harmonic beams, the duration estimation error is less than 2 %. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Sensing ultrashort electronic coherent beating at conical intersections by single-electron pulses

In a theoretical study, we present an ultrafast technique for probing time-dependent molecular charge densities. An ultrafast optical pump first brings the molecule into an electronic nonstationary state. This is followed by coherent inelastic scattering of a broadband single-electron probe pulse with a variable delay T, which is detected spectrally. The technique is applied to reveal phase-sensitive background-free coherent electron beating in the conical intersection passage in uracil and reveals the otherwise elusive coherent beating of strongly coupled electrons and nuclei.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Modeling the sequential dissociative double ionization of O 2 by ultrashort intense infrared laser pulses

A density matrix approach for sequential double ionization (DM-SDI) of molecules has been developed recently and was applied to the N 2 molecule. In this article, we extended the DM-SDI model to O 2 , which is a more complicated system to model than N 2 , due to its electronic structures and spin-orbit and laser couplings in the manifold of doubly charged states. We obtained a good agreement on the kinetic energy release spectrum of O + + O + from previous experiments. Thanks to the low computational cost of the model, we explored the mechanism behind the ionization and dissociation dynamics as well as the effects of lasers on the spectrum. Furthermore, this work will pave the way to model sequential dissociative double ionization of larger molecules and to probe molecular dynamics by measuring kinetic energy release spectra from this process.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Transition metal dichalcogenide monolayers in an ultrashort optical pulse: Femtosecond currents and anisotropic electron dynamics

We theoretically study the interaction of an ultrafast intense linearly polarized optical pulse with monolayers of transition metal dichalcogenides (TMDCs). Such a strong pulse redistributes electrons between the bands and generates femtosecond currents during the pulse. Due to the large bandwidth of the incident pulse, this process is completely an off-resonant. While in TMDCs, the time-reversal symmetry is conserved, the inversion symmetry is broken, and these monolayers have axial symmetry along the armchair direction but not along with the zigzag one. The pulse, polarized along with asymmetric directions of TMDC monolayer, generates both longitudinal, i.e., along the direction of polarization, and transverse, i.e., in the perpendicular direction, currents. Such currents result in charge transfer through the system. Finally, we study different TMDC materials and show how the femtosecond transport in TMDC monolayers depend on their parameters, such as lattice constant and bandgap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Single-Shot Multi-keV X-Ray Absorption Spectroscopy Using an Ultrashort Laser-Wakefield Accelerator Source

We report that single-shot absorption measurements have been performed using the multi-keV x rays generated by a laser-wakefield accelerator. A 200 TW laser was used to drive a laser-wakefield accelerator in a mode which produced broadband electron beams with a maximum energy above 1 GeVand a broad divergence of ≈15 mrad FWHM. Betatron oscillations of these electrons generated 1.2 ± 0.2 x 10 6 photons/eV in the 5 keV region, with a signal-to-noise ratio of approximately 300:1. This was sufficient to allow high-resolution x-ray absorption near-edge structure measurements at the K edge of a titanium sample in a single shot. We demonstrate that this source is capable of single-shot, simultaneous measurements of both the electron and ion distributions in matter heated to eV temperatures by comparison with density functional theory simulations. The unique combination of a high-flux, large bandwidth, few femtosecond duration x-ray pulse synchronized to a high-power laser will enable key advances in the study of ultrafast energetic processes such as electron-ion equilibration.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗