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At least 37 records · Page 2

Two- and three-body fragmentation of multiply charged tribromomethane by ultrafast laser pulses

We investigate the two- and three-body fragmentation of tribromomethane (bromoform, CHBr 3 ) resulting from multiple ionization by 28-femtosecond near-infrared laser pulses with a peak intensity of 6 × 10 14 W cm -2 . The analysis focuses on channels consisting exclusively of ionic fragments, which are measured by coincidence momentum imaging. The dominant two-body fragmentation channel is found to be Br + + CHBr 2 +. Weaker HBr + + CBr 2 +, CHBr + + Br 2 +, CHBr 2+ + Br 2 +, and Br + + CHBr 2 2+ channels, some of which require bond rearrangement prior to or during the fragmentation, are also observed. The dominant three-body fragmentation channel is found to be Br + + Br + + CHBr + . This channel includes both concerted and sequential fragmentation pathways, which we identify using the native frames analysis method. We compare the measured kinetic energy release and momentum correlations with the results of classical Coulomb explosion simulations and discuss the possible isomerization of CHBr 3 to BrCHBr–Br (iso-CHBr 3 ) prior to the fragmentation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High average power ultrafast laser technologies for driving future advanced accelerators

Large scale laser facilities are needed to advance the energy frontier in high energy physics and accelerator physics. Laser plasma accelerators are core to advanced accelerator concepts aimed at reaching TeV electron electron colliders. In these facilities, intense laser pulses drive plasmas and are used to accelerate electrons to high energies in remarkably short distances. A laser plasma accelerator could in principle reach high energies with an accelerating length that is 1000 times shorter than in conventional RF based accelerators. Notionally, laser driven particle beam energies could scale beyond state of the art conventional accelerators. LPAs have produced multi GeV electron beams in about 20 cm with relative energy spread of about 2 percent, supported by highly developed laser technology. This validates key elements of the US DOE strategy for such accelerators to enable future colliders but extending best results to date to a TeV collider will require lasers with higher average power. While the per pulse energies envisioned for laser driven colliders are achievable with current lasers, low laser repetition rates limit potential collider luminosity. Applications will require rates of kHz to tens of kHz at Joules of energy and high efficiency, and a collider would require about 100 such stages, a leap from current Hz class LPAs. This represents a challenging 1000 fold increase in laser repetition rates beyond current state of the art. Here, this whitepaper describes current research and outlook for candidate laser systems as well as the accompanying broadband and high damage threshold optics needed for driving future advanced accelerators.

47 OTHER INSTRUMENTATION↗

High-throughput homogenization of a quasi-Gaussian ultrafast laser beam using a combined refractive beam shaper and spatial light modulator

Efficiently shaping femtosecond, transverse Gaussian laser beams to flat-top beams with flat wavefronts is critical for large-scale material processing and manufacturing. Existing beam shaping devices fall short either in final beam homogeneity or efficiency. Here, we present an approach that uses refractive optics to perform the majority of the beam shaping and then uses a fine-tune device (spatial light modulator) to refine the intensity profile. For the beam that we selected, circularly asymmetric with intensity fluctuations, our method achieved a uniformity of 0.055 within 90% of the beam area at 92% efficiency. The optimization involved an iterative beam shaping process that converged to optimum within 10 iterations.

43 PARTICLE ACCELERATORS↗

Pulse duration dependent effects of ultrafast laser induced damage on a 1030 nm multi-layer dielectric mirror for high repetition rate, high average power laser systems

High repetition rate, high peak, and average power laser systems are crucial for next-generation particle accelerators, inertial confinement fusion, and secondary particle sources. These applications demand durable laser optics, particularly interference coatings on optics lasting millions of shots at high fluence. This study focuses on designing, testing, and simulating multi-layer dielectric (MLD) mirrors for pulse durations of 260 fs, 77 fs, and 25 fs at 1030 nm wavelength and 45-degree incidence angle with p -polarization. S-on-1 laser-induced damage thresholds (LIDT) for varying pulse numbers were determined, with single-shot LIDT values of 0.98 Jcm -2 , 1.63 Jcm -2 , and 2.3 Jcm -2 for 25 fs, 77 fs, and 260 fs respectively. A strong correlation between blister shape and local fluence was observed, implying that the layer expansion in a blister depends on local fluence. We have also examined mechanisms responsible for laser-induced stress generation and energy release rates in blister formation. Damage mechanisms are further explored by finite-difference time-domain (FDTD) simulations, incorporating Keldysh strong field ionization, whose predictions were in excellent agreement with the onset of damage determined experimentally. These findings offer insights for enhancing MLD coating technology, promising more efficient and resilient laser systems for diverse scientific and industrial applications.

Noor, Mohamed Yaseen (ORCID:000000021036644X)↗

Rayleigh Scattering Density Measurements from Ultrafast Lasers in High-Pressure, Cryogenic Wind Tunnels

The Rayleigh scattering signal from femtosecond laser pulses is examined for its utility at making instantaneous density measurements in the NASA Langley 0.3-m Transonic Cryogenic Tunnel. An electron-multiplying CCD camera is used to visualize Rayleigh scattering signal taken concurrently with velocity measurements utilizing the femtosecond laser tagging velocimetry technique (FLEET). The results indicate a strong potential for making instantaneous measurements. Viable single-shot images are obtained over the full operational envelope of the facility, and shot-to-shot variations are found to be on average 6 percent (at 95 percent confidence level) and tend to decrease as the facility density is increased. The Rayleigh scattering signals observed before the optical focus exhibit a characteristically linear dependence on the mass-density of the gas, while signals after the focus exhibit a nonlinear (sublinear) density dependence, indicative of stronger absorption at higher densities. The measured Rayleigh scattering signals compare favorably to theoretical assessments made at the tunnel operating conditions.

Burns, Ross A.↗

Joint Experimental and Computational Characterization of Sum-Frequency Generation between a Continuous Wave Laser and an Ultrafast Frequency Comb Laser for Tunable Laser Development

Ultrafast optical frequency combs allow for both high spectral and temporal resolution in molecular spectroscopy and have become a powerful tool in many areas of chemistry and physics. Ultrafast lasers and frequency combs generated from ultrafast mode-locked lasers often need to be converted to other wavelengths. Commonly used wavelength conversions are optical parametric oscillators, which require an external optical cavity, and supercontinuum generation combined with optical parametric amplifiers. Whether commercial or home-built, these systems are complex and costly. Here, we investigate an alternative, simple, and easy-to-implement approach to tunable frequency comb ultrafast lasers enabled by new continuous-wave laser technology. Sum-frequency generation between an Nd:YAG continuous-wave laser and a Yb:fiber femtosecond frequency comb in a beta-barium borate (BBO) crystal is explored. The resulting sum-frequency beam is a pulsed frequency comb with the same repetition rate as the Yb:fiber source. SNLO simulation software is used to simulate the results and provide benchmarks for designing future systems to achieve wavelength conversion and tunability in otherwise difficult-to-reach spectral regions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanoscale ultrafast lattice modulation with a free-electron laser

Ultrafast optical laser-based techniques have enabled the probing of atomistic processes at their intrinsic temporal scales with femto- and attosecond resolution. However, the long wavelengths of optical lasers have prevented their interrogation and manipulation with nanoscale spatial specificity. Advances in hard X-ray free-electron lasers have enabled progress in developing X-ray transient-grating spectroscopy, a technique that aims to coherently control elementary excitations with nanoscale X-ray standing waves. Thus far, the realization of this technique at the nanoscale has been a challenge. Here we demonstrate X-ray transient-grating spectroscopy with spatial periods of the order of 10 nm via the subfemtosecond synchronization of two hard X-ray pump pulses at a precisely controlled crossing angle. This creates a thermal grating and preferentially excites coherent longitudinal acoustic phonon modes with the transient-grating wavevector. On probing with a third, variably delayed, X-ray pulse with the same photon energy, time-and-wavevector-resolved measurements of the modulation of the induced scattering intensity provide evidence of ballistic thermal transport at nanometre scales. Finally, these results highlight the potential of X-ray transient gratings as a powerful platform for studying nanoscale transport in condensed matter and the coherent control of nanoscale dynamics.

nonlinear optics↗

Ultrafast Laser-Excited Optical Emission of Xe under Loose-Focusing Conditions

The optical filament-based radioxenon sensing can potentially overcome the constraints of conventional detection techniques that are relevant for nuclear security applications. This study investigates the spectral signatures of pure xenon (Xe) when excited by ultrafast laser filaments at near-atmosphericpressure and in short and loose-focusing conditions. The two focusing conditions lead to laser intensity differences of several orders of magnitude and different plasma transient behavior. The gaseous sample was excited at atmospheric pressure using ∼7 mJ pulses with a 35 fs pulse duration at 800 nm wavelength. The optical signatures were studied by time-resolved spectrometry and imaging in orthogonal light collection configurations in the ∼400 nm (VIS) and ∼800 nm (NIR) spectral regions. The most prominent spectral lines of atomic Xe are observable in both focusing conditions. An on-axis light collection from an atmospheric air–Xe plasma mixture demonstrates the potential of femtosecond filamentation for the remote sensing of noble gases.

47 OTHER INSTRUMENTATION↗

Ultrafast Reactive Laser Sintering of Highly Conductive Garnet-Type LLZTO Solid Electrolytes

Rapid and scalable fabrication of garnet-type solid electrolytes remains a major challenge for the practical deployment of lithium metal batteries. Here, we report reactive laser sintering (RLS) as an ultrafast and potentially scalable strategy for fabricating garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid electrolytes. RLS of LLZTO enables simultaneous reaction and densification, achieving ∼95% relative density while minimizing lithium loss and suppressing secondary phase formation. Compared to conventional furnace sintering, RLS promotes enhanced grain growth and improved densification, leading to improved ionic conductivity (0.36 ± 0.08 mS cm −1 ) while maintaining comparable activation energies for Li + transport. Structural characterization by X-ray diffraction (XRD), Raman spectroscopy, and solid-state 6 Li/ 7 Li NMR confirms the formation of cubic garnet LLZTO with homogeneous microscale elemental distribution. In addition, nanoindentation measurements demonstrate that RLS preserves the mechanical properties of the garnet framework despite ultrafast localized thermal processing. By integrating simultaneous reaction and densification with tunable microstructural control, reactive laser sintering provides a promising manufacturing pathway for high-performance garnet solid electrolytes toward next-generation solid-state batteries.

CO2 laser↗

Laser-driven ultrafast transmission electron microscopy

Recent advances in lasers and electron optics technology have allowed transmission electron microscopes to achieve high spatial and temporal resolution, making them capable of tracking atoms, charges and spin motions down to the attosecond and nanometre scales. This Primer discusses the most common and practical experimental implementation of time-resolved transmission electron microscopy and the stroboscopic mode for evaluating ultrafast reversible dynamics. An in-depth discussion of photo-induced near-field electron microscopy, a technique unique to laser-assisted electron microscopy, is also provided, covering its prospective applications in the study of coherent phenomena in quantum materials. The experimental strategies and limitations in investigating the structural dynamics of materials and nanostructures by imaging, diffraction and spectroscopy are also described in detail, with a direct comparison with more conventional and established techniques. Here, we provide key information for new researchers who intend to use ultrafast transmission electron microscopy to address new challenges in specific materials science, condensed matter and nanophotonics.

Transmission electron microscopy↗

Laser-Induced Ultrafast Demagnetization and Spin Switching (Final Report)

The information technology revolution demands bigger and faster magnetic storage devices. The funded research focuses on a new frontier - Laser-induced ultrafast all-optical spin switching (AOS), where a single laser pulse can switch spins from one direction to another permanently, without a magnetic field, on a time scale of 1-10 picoseconds, 2-3 orders of magnitude faster than the existing technology. The funded research has successfully resolved a long-standing issue in ultrafast demagnetization whether the lattice contributes to the demagnetization. We developed a high level first-principles theory and employed a massively parallel computer to pin down the details of the physical mechanisms that are inaccessible to other methods. This unique feature allows us to compute the force on each atom in both bulk and monolayer systems. We find that it is indeed true there is a nonzero force on each atom, but the idea of vibration contribution is not crucial to our basic understanding of physics. This paves the way to future experimental, theoretical and technological developments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ultrafast laser-induced spin–lattice dynamics in the van der Waals antiferromagnet CoPS 3

CoPS 3 stands out in the family of the van der Waals antiferromagnets XPS 3 (X = Mn, Ni, Fe, and Co) due to the unquenched orbital momentum of the magnetic Co 2+ ions, which is known to facilitate the coupling of spins to both electromagnetic waves and lattice vibrations. Here, using a time-resolved magneto-optical pump–probe technique, we experimentally study the ultrafast laser-induced dynamics of mutually correlated spins and lattice. It is shown that a femtosecond laser pulse acts as an ultrafast heater and, thus, results in the melting of the antiferromagnetic order. At the same time, the resonant pumping of the 4 T 1g → 4 T 2g electronic transition in Co 2+ ions effectively changes their orbital momentum, giving rise to a mechanical force that moves the ions in the direction parallel to the orientation of their spins, thus generating a coherent B g phonon mode at the frequency of about 4.7 THz.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Plasma Heating and Ultrafast Semiconductor Laser Modulation Through a Terahertz Heating Field

Electron-hole plasma heating and ultrafast modulation in a semiconductor laser under a terahertz electrical field are investigated using a set of hydrodynamic equations derived from the semiconductor Bloch equations. The self-consistent treatment of lasing and heating processes leads to the prediction of a strong saturation and degradation of modulation depth even at moderate terahertz field intensity. This saturation places a severe limit to bandwidth achievable with such scheme in ultrafast modulation. Strategies for increasing modulation depth are discussed.

Li, Jian-Zhong↗