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At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Burst delay line for generating ultrashort pulse bursts with interval tunability from femtoseconds to nanoseconds.

Ultrashort burst laser pulses are important for applications in laser processing and spectroscopy. However, existing burst generators face limitations in pulse time interval tunability and coaxiality. Here, we present a burst pulse generator that delivers coaxial ultrashort pulses with tunable pulse time intervals using a single translation stage. The constructed system produced eight femtosecond pulses with uniform intervals tunable from 100 fs to 1.93 ns, equivalent to burst-internal repetition rates spanning 10 THz to 0.52 GHz. We further demonstrated interval-dependent plasma emission in air filamentation, providing a compact platform to study burst-laser-induced phenomena.

Shimada, Keitaro↗
DOE OSTI2026

Few-femtosecond time resolution in optically pumped hard X-ray scattering at a free-electron laser

Capturing chemical dynamics in real time is a central goal of ultrafast science, necessitating measurements fast enough to track atomic motion on few-femtosecond timescales with high precision. We present time-resolved hard X-ray scattering that meets these criteria by combining 7 fs full-width at half maximum (FWHM) near-infrared laser pulses with sub10 fs FWHM hard X-ray pulses from a free-electron laser. Using heavy water’s electronic response to strong-field ionization as a benchmark, we achieve a sub-8 fs FWHM instrument response function. These optical pump X-ray probe measurements enable direct observation of chemical dynamics with angstrom spatial and few-fs temporal resolution.

Weckwerth, Eleanor [Stanford University, CA (Unite↗
DOE OSTI2021

High-temperature stable FBGs fabricated by a point-by-point femtosecond laser inscription for multi-parameter sensing

A high-temperature resistant fiber Bragg grating (FBG) with pronounced cladding modes is fabricated using a simple, fast, and flexible point-by-point femtosecond laser inscription. Cladding modes of different orders exhibit various sensitivities to changes in refractive index of the surrounding medium and temperature, while the Bragg wavelength is only dependent on the ambient temperature. By combining the resonance of cladding modes and the Bragg resonance, measurement of variations of temperature and surrounding refractive index can be achieved. Survivability of the cladding modes and the core mode in the fabricated FBG at elevated temperatures up to 1000°C is demonstrated.

Zhu, Chen (ORCID:0000000232567330)↗
DOE OSTI2021

Dynamic structural views in solar energy materials by femtosecond electron diffraction

Solar materials convert light into other forms of energy through excited state processes occurring on ultrafast time and atomic length scales. Understanding and controlling such nonequilibrium processes is essential for applications ranging from photovoltaics to photocatalysis. These processes are commonly studied by transient optical techniques, which resolve charge carrier dynamics. However, optical spectroscopy does not directly probe the atomic-scale motions that play a central role in the ultimate functionality of these materials. Filling this missing gap, ultrafast electron and x-ray scattering techniques enable monitoring of structural dynamics in materials with femtosecond time resolution. In this work, we focus on the use of ultrafast electron diffraction (UED) techniques to probe photoinduced energy conversion dynamics in solar energy materials. First, we discuss the use of UED as an ultrafast lattice thermometer allowing a direct probe of nonradiative relaxations such as hot carrier cooling and Auger recombination. Second, we present a time-resolved atomic pair distribution function analysis enabled by UED, which uncovers lattice deformations arising from excitation localization in materials. Finally, we provide an outlook looking toward new approaches for resolving in situ energy conversion dynamics and uncovering structure–property relationships in solar energy materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Probing Ultrafast Electron (De)localization Dynamics in Mixed Valence Complexes Using Femtosecond X-ray Spectroscopy (Final Report)

The central goal of this proposal was to directly visualize and quantify how electronic correlations, vibronic couplings, and local solute-solvent interactions control intramolecular electron motion on the femtosecond time scale. The proposed research program focused on solvated Ruthenium (Ru) based mixed-valence complexes, a prototypical class of transition-metal complexes, which are of significant interest for their potential applications in photochemical energy conversion. Electron movements following photochemical excitation are closely coupled with atomic/vibrational and solvent motion. To disentangle these various components requires tools designed to directly probe electron correlations and vibronic coupling (coherently coupled motions of electronic and vibrational coordinates) on the timescale of electron motion in the solution phase.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Temperature Measurements in Hypersonic Wind Tunnels via Femtosecond Coherent Anti-Stokes Raman Scattering

A femtosecond coherent anti-Stokes Raman scattering (fs CARS) instrument is developed to perform gas-phase thermometry in cold-flow hypersonic wind tunnels. Measurements are reported for Mach 8 and 14 pure-nitrogen flows. The fs CARS instrument includes a 100 fs pump/Stokes pulse and a spectrally narrow probe pulse from a second harmonic bandwidth compressor. Important experimental considerations such as limits on the pump/Stokes pulse energy are discussed. The fs CARS focusing and collimating optics are mounted on a two-axis translation stage system to scan the measurement location during a 30 second wind tunnel run. Single-laser-shot rotational CARS spectra are recorded at the laser repetition rate of 1 kHz in the wind tunnel freestream and near simple cone models. Spectral fitting is used to determine quantitative gas temperatures. Freestream temperatures at Mach 8 and 14 spanned ranges of 40–75 and 35–50 K, respectively, depending on tunnel operating conditions. Temperature variations across the central 100 mm span of the wind tunnel were quantified. Measured temperature jumps across conical bow shocks from various models varied by less than 1% from predicted values. Hypersonic boundary layer measurements were demonstrated. In conclusion, these measurements illustrate the utility and robustness of this instrument for the study of complex fluid flow phenomena in challenging ground test facilities.

Aerodynamics↗
DOE OSTI2023

Excited-State Dynamics of All the Mono-cis and the Major Di-cis Isomers of β-Apo-8′-Carotenal as Revealed by Femtosecond Time-Resolved Transient Absorption Spectroscopy

Cis isomers of carotenoids play important roles in light harvesting and photoprotection in photosynthetic bacteria, such as the reaction center in purple bacteria and the photosynthetic apparatus in cyanobacteria. Carotenoids containing carbonyl groups are involved in efficient energy transfer to chlorophyll in light-harvesting complexes, and their intramolecular charge–transfer (ICT) excited states are known to be important for this process. Previous studies, using ultrafast laser spectroscopy, have focused on the central-cis isomer of carbonyl-containing carotenoids, revealing that the ICT excited state is stabilized in polar environments. However, the relationship between the cis isomer structure and the ICT excited state has remained unresolved. In this study, we performed steady-state absorption and femtosecond time-resolved absorption spectroscopy on nine geometric isomers (7-cis, 9-cis, 13-cis, 15-cis, 13′-cis, 9,13′-cis, 9,13-cis, 13,13′-cis, and all-trans) of β-apo-8′-carotenal, whose structures are well-defined, and discovered correlations between the decay rate constant of the S1 excited state and the S0−S1 energy gap, as well as between the position of the cis-bend and the degree of stabilization of the ICT excited state. Our results demonstrate that the ICT excited state is stabilized in polar environments in cis isomers of carbonyl-containing carotenoids and suggest that the position of the cis-bend plays an important role in the stabilization of the excited state.

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

Remote Detection of Uranium Using Self-Focusing Intense Femtosecond Laser Pulses

Optical measurement techniques can address certain important challenges associated with nuclear safety and security. Detection of uranium over long distances presents one such challenge that is difficult to realize with traditional ionizing radiation detection, but may benefit from the use of techniques based on intense femtosecond laser pulses. When a high-power laser pulse propagates in air, it experiences collapse and confinement into filaments over an extended distance even without external focusing. In our experiments, we varied the initial pulse chirp to optimize the emission signal from the laser-produced uranium plasma at an extended distance. While the ablation efficiency of filaments formed by self-focusing is known to be significantly lower when compared to filaments produced by external focusing, we show that filaments formed by self-focusing can still generate luminous spectroscopic signatures of uranium detectable within seconds over a 10-m range. The intensity of uranium emission varies periodically with laser chirp, which is attributed to the interplay among self-focusing, defocusing, and multi-filament fragmentation along the beam propagation axis. Grouping of multi-filaments incident on target is found to be correlated with the uranium emission intensity. The results show promise towards long-range detection, advancing the diagnostics and analytical capabilities in ultrafast laser-based spectroscopy of high-Z elements.

42 ENGINEERING↗
DOE OSTI2022

Redox-controlled reorganization and flavin strain within the ribonucleotide reductase R2b–NrdI complex monitored by serial femtosecond crystallography

Redox reactions are central to biochemistry and are both controlled by and induce protein structural changes. Here, we describe structural rearrangements and crosstalk within the Bacillus cereus ribonucleotide reductase R2b–NrdI complex, a di-metal carboxylate-flavoprotein system, as part of the mechanism generating the essential catalytic free radical of the enzyme. Femtosecond crystallography at an X-ray free electron laser was utilized to obtain structures at room temperature in defined redox states without suffering photoreduction. Together with density functional theory calculations, we show that the flavin is under steric strain in the R2b–NrdI protein complex, likely tuning its redox properties to promote superoxide generation. Moreover, a binding site in close vicinity to the expected flavin O 2 interaction site is observed to be controlled by the redox state of the flavin and linked to the channel proposed to funnel the produced superoxide species from NrdI to the di-manganese site in protein R2b. These specific features are coupled to further structural changes around the R2b–NrdI interaction surface. The mechanistic implications for the control of reactive oxygen species and radical generation in protein R2b are discussed

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1990

Femtosecond optical absorption studies of nonequilibrium electronic processes in high T(c) superconductors

The results are reported of femtosecond optical transient absorption experiments performed on the superconducting compounds YBa2Cu3O(7-x) (x about 0) and Bi2Sr2Ca2Cu3O(10+delta) (delta about 0) and nonsuperconducting YBa2Cu3O(6+y) (y less than 0.4) for sample temperatures ranging from about 7 K to room temperature. Nonequilibrium heating was found to occur on a subpicosecond time scale. A distinct, dramatic increase in the relaxation time was observed for the superconducting samples as the sample temperature was lowered below the critical temperatures of the respective films. Accompanying the increase in relaxation time was an increase in the peak fractional transmissivity change. No such changes were observed for the nonsuperconducting YBCO sample.

Chwalek, J. M.↗
NASA NTRS1991

Direct time integration of Maxwell's equations in linear dispersive media with absorption for scattering and propagation of femtosecond electromagnetic pulses

The initial results for femtosecond pulse propagation and scattering interactions for a Lorentz medium obtained by a direct time integration of Maxwell's equations are reported. The computational approach provides reflection coefficients accurate to better than 6 parts in 10,000 over the frequency range of dc to 3 x 10 to the 16th Hz for a single 0.2-fs Gaussian pulse incident upon a Lorentz-medium half-space. New results for Sommerfeld and Brillouin precursors are shown and compared with previous analyses. The present approach is robust and permits 2D and 3D electromagnetic pulse propagation directly from the full-vector Maxwell's equations.

Joseph, Rose M.↗
NASA NTRS1992

Direct time integration of Maxwell's equations in nonlinear dispersive media for propagation and scattering of femtosecond electromagnetic solitons

The initial results for femtosecond electromagnetic soliton propagation and collision obtained from first principles, i.e., by a direct time integration of Maxwell's equations are reported. The time integration efficiently implements linear and nonlinear convolutions for the electric polarization and can take into account such quantum effects as Kerr and Raman interactions. The present approach is robust and should permit the modeling of 2D and 3D optical soliton propagation, scattering, and switching from the full-vector Maxwell's equations.

Goorjian, Peter M.↗
NASA NTRS1992

Computational modeling of femtosecond optical solitons from Maxwell's equations

An algorithm is developed that permits the direct time integration of full-vector nonlinear Maxwell's equations. This capability permits the modeling of both linear and nonlinear instantaneous and dispersive effects in the electric polarization in material media. The modeling of the optical carrier is retained. The fundamental innovation is to notice that it is possible to treat the linear and nonlinear convolution integrals, which describe the dispersion, as new dependent variables. A coupled system of nonlinear second-order ordinary differential equations can then be derived for the linear and nonlinear convolution integrals, by differentiating them in the time domain. These equations, together with Maxwell's equations, are solved to determine the electromagnetic fields in nonlinear dispersive media. Results are presented of calculations in one dimension of the propagation and collision of femtosecond electromagnetic solitons that retain the optical carrier, taking into account as the Kerr and Raman interactions.

Goorjian, Peter M.↗
NASA NTRS1992

Femtosecond resolution of soft mode dynamics in structural phase transitions

The microscopic pathway along which ions or molecules in a crystal move during structural phase transition can often be described in terms of a collective vibrational mode of the lattice. In many cases, this mode, called a 'soft' phonon mode because of its characteristically low frequency near the phase transition temperature, is difficult to characterize through conventional frequency-domain spectroscopies such as light or neutron scattering. A femtosecond time-domain analog of light-scattering spectroscopy called impulsive stimulated Raman scattering (ISRS) has been used to examine the soft modes of two perovskite ferroelectric crystals. The low-frequency lattice dynamics of KNbO3 and BaTiO3 are clarified in a manner that permits critical evaluation of microscopic models for their ferroelectric transitions. The results illustrate the advantages of ISRS over conventional Raman spectroscopy of low-frequency, heavily damped soft modes.

Dougherty, Thomas P.↗
NASA NTRS1993

Direct time integration of Maxwell's equations in two-dimensional dielectric waveguides for propagation and scattering of femtosecond electromagnetic solitons

We present what are to our knowledge first-time calculations from vector nonlinear Maxwell's equations of femtosecond soliton propagation and scattering, including carrier waves, in two-dimensional dielectric waveguides. The time integration efficiently implements linear and nonlinear convolutions for the electric polarization, and the nonlinear convolution accounts for two quantum effects, the Kerr and Raman interactions. By retaining the optical carrier, the new method solves for fundamental quantities - optical electric and magnetic fields in space and time - rather than a nonphysical envelope function. It has the potential to provide an unprecedented two- and three-dimensional modeling capability for millimeter-scale integrated-optical circuits with submicrometer engineered inhomogeneities.

Joseph, Rose M.↗
NASA NTRS1993

FD-TD modeling of 2-D dielectric waveguides for propagation and scattering of femtosecond optical solitons

Experimentalists have produced all-optical switches capable of 100-fs responses. To adequately model such switches, nonlinear effects in optical materials (both instantaneous and dispersive) must be included. In principle, the behavior of electromagnetic fields in nonlinear dielectrics can be determined by solving Maxwell's equations subject to the assumption that the electric polarization has a nonlinear relation to the electric field. However, until our previous work, the resulting nonlinear Maxwell's equations have not been solved directly. Rather, approximations have been made that result in a class of generalized nonlinear Schrodinger equations (GNLSE) that solve only for the envelope of the optical pulses. In this paper, we present first-time calculations from the vector nonlinear Maxwell's equations of femtosecond soliton propagation and scattering, including carrier waves, in two-dimensional systems of dielectric waveguides exhibiting the Kerr and Raman quantum effects. We use the finite-difference time-domain (FD-TD) method in an extension of our 1-D work. There, in a fundamental innovation, we treated the linear and nonlinear convolutions for the electric polarization as new dependent variables. By differentiating these convolutions in the time domain, we derived an equivalent system of coupled, nonlinear second-order ODE's. These equations together with Maxwell's equations form the system that is solved to determine the electromagnetic fields in inhomogeneous nonlinear dispersive media. Backstorage in time is limited to only that needed by the time-integration algorithm for the ODE's, rather than that needed to store the time-history of the kernel functions of the convolutions (1000-10,000 time steps). Thus, a 2-D nonlinear optics model from Maxwell's equations is now feasible.

Joseph, Rose↗
NASA NTRS2005

Pulse energy dependence of subcellular dissection by femtosecond laser pulses

Precise dissection of cells with ultrashort laser pulses requires a clear understanding of how the onset and extent of ablation (i.e., the removal of material) depends on pulse energy. We carried out a systematic study of the energy dependence of the plasma-mediated ablation of fluorescently-labeled subcellular structures in the cytoskeleton and nuclei of fixed endothelial cells using femtosecond, near-infrared laser pulses focused through a high-numerical aperture objective lens (1.4 NA). We find that the energy threshold for photobleaching lies between 0.9 and 1.7 nJ. By comparing the changes in fluorescence with the actual material loss determined by electron microscopy, we find that the threshold for true material ablation is about 20% higher than the photobleaching threshold. This information makes it possible to use the fluorescence to determine the onset of true material ablation without resorting to electron microscopy. We confirm the precision of this technique by severing a single microtubule without disrupting the neighboring microtubules, less than 1 micrometer away. c2005 Optical Society of America.

Non-NASA Center↗
NASA NTRS2016

Femtosecond Laser Tagging Characterization of a Sweeping Jet Actuator Operating in the Compressible Regime

A sweeping jet (SWJ) actuator operating over a range of nozzle pressure ratios (NPRs) was characterized with femtosecond laser electronic excitation tagging (FLEET), single hot-wire anemometry (HWA) and high-speed/phase-averaged schlieren. FLEET velocimetry was successfully demonstrated in a highly unsteady, oscillatory flow containing subsonic through supersonic velocities. Qualitative comparisons between FLEET and HWA (which measured mass flux since the flow was compressible) showed relatively good agreement in the external flow profiles. The spreading rate was found to vary from 0.5 to 1.2 depending on the pressure ratio. The precision of FLEET velocity measurements in the external flow field was poorer (is approximately equal to 25 m/s) than reported in a previous study due to the use of relatively low laser fluences, impacting the velocity fluctuation measurements. FLEET enabled velocity measurements inside the device and showed that choking likely occurred for NPR ≥ 2.0, and no internal shockwaves were present. Qualitative oxygen concentration measurements using FLEET were explored in an effort to gauge the jet's mixing with the ambient. The jet was shown to mix well within roughly four throat diameters and mix fully within roughly eight throat diameters. Schlieren provided visualization of the internal and external flow fields and showed that the qualitative structure of the internal flow does not vary with pressure ratio and the sweeping mechanism observed for incompressible NPRs also probably holds for compressible NPRs.

Peters, Christopher J.↗