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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Ultrafast adiabatic frequency conversion

Abstract Ultrafast adiabatic frequency conversion is a powerful method, capable of efficiently and coherently transfering ultrashort pulses between different spectral ranges, e.g. from near-infrared to mid-infrared, visible or ultra-violet. This is highly desirable in research fields that are currently limited by available ultrafast laser sources, e.g. attosecond science, strong-field physics, high-harmonic generation spectroscopy and multidimensional mid-infrared spectroscopy. Over the past decade, adiabatic frequency conversion has substantially evolved. Initially applied to quasi-monochromatic, undepleted pump interactions, it has been generalized to include ultrashort, broadband, fully-nonlinear dynamics. Through significant theoretical development and experimental demonstrations, it has delivered new capabilities and superior performance in terms of bandwidth, efficiency and robustness, as compared to other frequency conversion techniques. This article introduces the concept of adiabatic nonlinear frequency conversion, reviews its theoretical foundations, presents significant milestones and highlights contemporary ultrafast applications that may, or already do, benefit from utilizing this method.

Margules, Peleg (ORCID:0000000335573370)↗
DOE OSTI2020

Hydrodynamic conditions in laser irradiated buried layer experiments

The calculation of open shell ionization level and radiative properties of materials in Non-Local Thermal Equilibrium (NLTE) is currently still a major challenge for any atomic model. The predictions of various NLTE atomic codes at these conditions still differ significantly. In recent years, a new buried layer platform was developed at the Lawrence Livermore National Laboratory and the Laboratory for Laser Energetics. This platform is used to measure ionization distribution and emission of open L-shell, mid-Z ions and open M-shell, high-Z ions at NLTE conditions that are relevant in many laser plasma applications. These experiments offer a unique chance for benchmarking the atomic models. In order to perform these experiments, a uniform well characterized plasma source is required. In this work, we present one-dimensional (1D) and two-dimensional simulations of the experimental platform. These simulations were used for both the design and the analysis of the experiments. The simulations demonstrate the different phases of hydrodynamic evolution of the target and identify the time windows in which uniform conditions can be achieved. A 1D expansion of the target was found to be adequate to describe the target's evolution for most of the experiment duration. The fast 1D simulations were compared with recent experimental results from the Omega laser facility. The sensitivity of the results to several modeling parameters such as the electron flux limiter and laser resonant absorption is reported.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

High-resolution infrared spectroscopy of jet cooled CH 2 Br radicals: The symmetric CH stretch manifold and absence of nuclear spin cooling

Direct laser absorption of a slit supersonic discharge expansion provides the first high-resolution spectroscopic results on the symmetric CH stretch excitation (ν 1 ) of the bromomethyl (CH 2 Br) radical in the ground electronic state. Narrowband (<1 MHz) mid-infrared radiation is produced by difference-frequency generation of two visible laser beams, with the open shell halohydrocarbon radical generated by electron dissociative attachment of CH 2 Br 2 in a discharge and rapidly cooled to T rot = 18 ± 1 K in the subsequent slit-jet supersonic expansion. A rovibrational structure in the radical spectrum is fully resolved, as well as additional splittings due to spin-rotation effects and 79 Br/ 81 Br isotopologues in natural abundance. Spectroscopic constants and band origins are determined by fitting the transition frequencies to a non-rigid Watson Hamiltonian, yielding results consistent with a vibrationally averaged planar radical and an unpaired electron in the out-of-plane p π orbital. Additionally, extensive satellite band structure from a vibrational hot band is observed and analyzed. The hot band data is compared to CFOUR/VPT2 (CCSD(T)cc-pVQZ) ab initio anharmonic predictions of the vibration rotation alpha matrix, which permits unambiguous assignment to CH 2 symmetric-stretch excitation built on the singly excited CH 2 out-of-plane bending mode (ν 1 + ν 4 ← ν 4 ). Longitudinal cooling of the Doppler width in the slit-jet expansion geometry also reveals partially resolved hyperfine structure on transitions out of the lowest angular momentum states in excellent agreement with predictions based on microwave studies. High level ab initio MOLPRO calculations [CCSD(T)-f12b/VnZ-f12 (n = 3, 4, CBS)] are also performed with explicitly correlated f12 electron methods for the out-of-plane CH 2 bending mode over the halogen series CH 2 X (X = F, Cl, Br, I), which clearly reveals a non-planar geometry for X = F (with a ΔE ≈ 0.3 kcal/mol barrier) and yet planar equilibrium geometries for X = Cl, Br, and I. Finally, a detailed Boltzmann analysis of the transition intensities provides support for negligible collisional equilibration of the entangled H atom nuclear spin states on the few hundred microsecond time scale and high collision densities of a slit supersonic expansion.

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

Frequency combs in optically injected terahertz ring quantum cascade lasers

Quantum cascade lasers (QCLs) have emerged as promising candidates for generating chip-scale frequency combs in mid-infrared and terahertz wavelengths. In this work, we demonstrate frequency comb formation in ring terahertz QCLs using the injection of light from a distributed feedback (DFB) laser. The DFB design frequency is chosen to match the modes of the ring cavity (near 3.3 THz), and light from the DFB is injected into the ring QCL via a bus waveguide. By controlling the power and frequency of the optical injection, we show that combs can be selectively formed and controlled in the ring cavity. Numerical modeling suggests that this comb is primarily frequency-modulated in character, with the injection serving to trigger comb formation. We also show that the ring can be used as a filter to control the output of the DFB QCL, potentially being of interest in terahertz photonic integrated circuits. Our work demonstrates that waveguide couplers are a compelling approach for injecting and extracting radiation from ring terahertz combs and offer exciting possibilities for the generation of new comb states in terahertz, such as frequency-modulated waves, solitons, and more.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Linear colliders based on laser-plasma accelerators

Laser-plasma accelerators are capable of sustaining accelerating fields of 10–100 GeV/m, 100–1000 times that of conventional technology and the highest fields produced by any of the widely researched advanced accelerator concepts. Laser-plasma accelerators also intrinsically accelerate short particle bunches, several orders of magnitude shorter than that of conventional technology, which leads to reductions in beamstrahlung and, hence, savings in the overall power consumption to reach a desired luminosity. These properties make laser-plasma accelerators a promising accelerator technology for a more compact, less expensive high-energy linear collider providing multi-TeV polarized leptons. In this submission to the Snowmass 2021 Accelerator Frontier, we discuss the motivation for a laser-plasma-accelerator-based linear collider, the status of the field, and potential linear collider concepts up to 15 TeV. Herein, we outline the research and development path toward a collider based on laser-plasma accelerator technology, and highlight near-term and mid-term applications of this technology on the collider development path. The required experimental facilities to carry out this research are described. We conclude with community recommendations developed during Snowmass.

43 PARTICLE ACCELERATORS↗
DOE OSTI2026

Generation of 3.3-mJ, 2.45-µm, sub-2-cycle laser pulses via hollow-core fiber pulse compression

We demonstrate nonlinear compression of mid-infrared pulses from a Cr:ZnSe chirped-pulse amplifier using a gas-filled stretched hollow-core fiber followed by bulk-material compression. Starting from 90 fs, 2.45 µm pulses with 5.3 mJ energy, spectral broadening in the gas-filled capillary combined with optimized dispersion management enables compression to 15 fs, less than two optical cycles at 2.45 µm, with 3.3 mJ pulse energy, corresponding to a peak power of approximately 0.12 TW. The simplicity of the approach, based on a single hollow-core fiber stage and bulk dispersion compensation, makes it scalable to higher energies and establishes a robust route to mid-infrared drivers for high harmonic generation and attosecond applications.

Britton, Mathew [SLAC National Accelerator Laborat↗
DOE OSTI2022

Ultrafast infrared plasmon switching in aligned carbon-nanotube optical resonators

Reconfigurable plasmonic materials are crucial components in active photonic devices for optical communication, signal processing, and sensing applications. Certain candidates including transparent conducting oxides, small-bandgap semiconductors (i.e. Ge, InSb), and conducting polymers can exhibit switchable free carrier concentrations triggered by optical, electrical or thermal excitations. Here, we show that aligned films of single-walled carbon nanotubes (SWCNTs) can serve as all-optically tunable plasmonic material in the mid-infrared range, thereby adding them to the library of switchable plasmonic materials. Interband optical pumping with femtosecond laser pulses results in the photoexcitation of free charge carriers, which transiently blueshifts the plasmon resonances of patterned, periodic SWCNT nano-resonators spanning the mid-infrared spectral range from 1700 to 2700 cm -1 . Furthermore. the ultrafast plasmon modulation exhibits a nearly single-picosecond decay time, attributed to interband carrier relaxation and inter-tube charge transfer. Given that aligned films of SWCNTs have high thermal stability, excellent photostability, epsilon-near-zero property, and extremely large optical anisotropy, their dynamic tunability represents a promising pathway towards active optical devices in the technologically important mid-infrared range.

single-walled carbon nanotubes↗
DOE OSTI2020

Coherent Manipulation of Single Electrons with Optical Photons in Condensed Helium-4

Single electrons are one of the simplest quantum objects in nature. In free space or conventional materials, single electrons hardly interact with optical (ultraviolet-visible-infrared) photons, so their quantum states cannot be easily manipulated by optics. Here, a notable exception is is theoretically demonstrated: A single electron in condensed helium-4 can be self-confined in a nanometric bubble of 1 to 2 nm radius and resonantly interact with mid-infrared photons of 3 to 12 μm wavelength. A femtosecond laser can drive the electron into Rabi oscillations and prepare it onto arbitrary superposition states between the ground and excited states. After the laser pulse, the electron bubble can exhibit remarkable nonequilibrium quantum dynamics and evolve toward various final states with various lifetimes. These processes are accompanied with intense phonon radiation.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Time-Resolved X-ray Emission Spectroscopy and Resonant Inelastic X-ray Scattering Spectroscopy of Laser Irradiated Carbon

The existence of liquid carbon as an intermediate phase preceding the formation of novel carbon materials has been a point of contention for several decades. Experimental observation of such a liquid state requires nonthermal melting of solid carbon materials at various laser fluences and pulse properties. Reflectivity experiments performed in the mid-1980s reached opposing conclusions regarding the metallic or insulating properties of the purported liquid state. Time-resolved X-ray absorption studies showed shortening of C–C bonds and increasing diffraction densities, thought to evidence a liquid or glassy carbon state, respectively. Nevertheless, none of these experiments provided information on the electronic structure of the proposed liquid state. Herein, we report the results of time-resolved resonant inelastic X-ray scattering (RIXS) and time-resolved X-ray emission spectroscopy (XES) studies on amorphous carbon (a-C) and ultrananocrystalline diamond (UNCD) as a function of delay time between the irradiating pulse and X-ray probe. For both a-C and UNCD, we attribute decreases in RIXS or XES signals to transition blocking, relaxation, and finally, ablation. Increased signal at 20 ps following the irradiation of the UNCD is attributed to the probable formation of nanoscale structures in the ablation plume. Further, differences in the amount of signal observed between a-C and UNCD are explained by the difference in sample thickness and, specifically, incomplete melting of the UNCD film. Comparisons to spectral simulations based on MD trajectories at extreme conditions indicate that the carbon state in our experiments is crystalline. Normal mode analysis confirmed that symmetrical bending or stretching of the C–C bonds in the diamond lattice results in XES spectra with small intensity differences. Overall, we observed no evidence of melting to a liquid state, as determined by the lack of changes in the spectral properties for up to 100 ps delays following the melting pulses.

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

Photonic Crystal Surface Emitting Diode Lasers with λ near 2 µm

Epitaxially regrown electrically pumped photonic crystal surface emitting lasers (PCSELs) operating near 2 µm were designed and fabricated within a III-V-Sb material system. A high-index-contrast photonic crystal layer was incorporated into the laser heterostructures by air-pocket-retaining epitaxial regrowth. Transmission electron microscopy studies confirmed uniform and continuous AlGaAsSb initial growth over the nano-patterned GaSb surface, followed by the development of the air-pockets. The PCSEL threshold current density had a minimal value of ~170 A/cm 2 in the 160–180 K temperature range when the QW gain spectrum aligned with the Γ 2 band edge of the photonic crystal. The devices operated in a continuous wave regime at 160 K. The divergence and polarization of the multimode laser beam emitted from the 200 µm × 200 µm PCSEL aperture were controlled by filamentation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Insight into the chemistry of TNT during shock compression through ultrafast absorption spectroscopies

Thin films of trinitrotoluene (TNT) were shock compressed using the ultrafast laser shock apparatus at Los Alamos National Laboratory. Visible (VIS) and mid-infrared (MIR) transient absorption spectroscopies were simultaneously performed to probe for electronic and vibrational changes during shock compression of TNT. Additionally, three shock pressures (16 GPa, 33 GPa, and 45 GPa) were selected to observe no reaction, incipient reaction, and strongly developed reactions for TNT within the experimental time scale of <250 ps. Negligible absorption changes in MIR or VIS absorptions were observed at 16 GPa. At 33 GPa, MIR absorptions in the 3000 cm -1 –4000 cm -1 range were observed to increase during the shock and continue to increase during the rarefaction, in contrast to the VIS absorption measurements, which increased during the shock and almost fully recovered during rarefaction. At 45 GPa, both VIS and MIR absorptions were strong and irreversible. The intense and spectrally broad MIR absorptions were attributed to short lived intermediates with strong, spectrally broad absorptions that dominate the spectral response. The MIR and VIS absorption changes observed at 33 GPa and 45 GPa were credited to shock induced chemistry, most likely including the formation of a very broad hydrogenic stretch feature. The results from these experiments are consistent with the chemical mechanisms that include O–H or N–H formation such as CH 3 oxidation or C–N homolysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

A comparative study of multimodal data fusion strategies for planetary spectroscopy

Integrating heterogeneous data sources can improve scientific inference when different modalities capture complementary information, but doing so is challenging in high-dimensional, small-sample settings. In spectroscopy for planetary exploration, Laser-Induced Breakdown Spectroscopy (LIBS), Raman Spectroscopy (Raman), Visible Infrared Spectroscopy (VISIR), and Mid-Infrared Spectroscopy (MIR) each examine different aspects of composition and mineralogy, raising fundamental questions about when and how data fusion improves predictive performance. Using a Mars-relevant set of geologic standards with measurements from all four modalities, we present a rigorous systematic evaluation of four data fusion strategies: low-level (data) fusion, mid-level (feature) fusion, high-level (decision) fusion, and residual-boosting (sequential) fusion. We assess performance in predicting oxide composition via nested cross-validation and corrected significance testing to evaluate whether data fusion improves upon single-modality baselines. We show that data fusion does not uniformly improve accuracy, and that observed gains are modest, oxide-dependent, and sensitive to modality and model structure. To move beyond aggregate accuracy metrics, we use model coefficients, permutation importance, and residual gain analysis to examine how the fusion models weight individual modalities and to identify patterns of apparent complementarity or redundancy. Though focused on spectroscopy for planetary exploration, our framework for data fusion evaluation and interpretation extends to other scientific domains with heterogeneous and scarce data and provides a principled approach evaluating data fusion strategies, interpreting modality contributions, and understanding tradeoffs among data fusion strategies.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2025

Correlating hot-electron preheat from the two-plasmon decay instability to $ρR$ degradation for direct-drive implosions on OMEGA

Focused experiments were performed with the goal of isolating the impact of hot-electron preheat on compression in deuterium–tritium (DT) layered, direct-drive implosions on OMEGA. Preheat from the hot-electrons generated by two-plasmon–decay (TPD) activity was varied through the incident laser intensity, with the total preheat energy deposited into unablated DT fuel being inferred using hard x-ray measurements. Results show a clear correlation between the inferred preheat levels and $ρR$ degradation that is consistent with a derived, 1D preheat model. A fit to the results also provides an estimated range of $ρR$ degradation from non-preheat sources for the adiabat ≈5 implosions used in this study. A follow-up study using targets containing Si-doped (5.5%) CH ablators (CHSi) demonstrated results consistent with mid-Z dopants mitigating TPD activity by showing these targets had almost no $ρR$ degradation as the laser intensity was increased up to levels previously considered damaging.

Doping↗
DOE OSTI2024

Comparing Pr 3+ and Nd 3+ for deactivating the Er 3+ : 4 I 13/2 level in lanthanum titanate glass

Erbium lanthanum titanate glasses were prepared by levitation melting for the spectroscopic study of ways to promote the mid-infrared fluorescence. Two series of heavily erbium doped glasses (15 wt%) were prepared with the addition of either Pr 3+ or Nd 3+ in amounts relative to Er 3+ of 0.05, 0.1, and 0.2. Both ions quench the lower Er 3+ laser level with the Pr 3+ doing so more rapidly. Although high co-dopant concentrations result in higher energy transfer, as clearly evidenced in upconversion and downconversion fluorescence measurements, the mid-infrared lifetime also suffers a reduction and, therefore, a balance must be struck in the co-dopant concentration. Lifetime and spectral measurements indicate that, at a fixed relative co-dopant amount, Pr 3+ is more effective than Nd 3+ at removing the bottleneck of the Er 3+ 4 I 13/2 level. Moreover, consideration of the lifetimes alongside the absorption data of the individual ions indicates that despite the large absorption cross-section of Nd 3+ at 808 nm, the concentration needed to yield more absorbed power than utilizing direct 976 nm excitation of Er 3+ results in unfavorable lifetimes of the mid-infrared transition. In the end, Pr 3+ prevails as the superior co-dopant in terms of the effects on fluorescence lifetimes as well as potential laser system design considerations. In a unique self-doping approach, a reducing melt atmosphere of Ar instead of O 2 creates a small fraction of Ti 3+ . In 5Er 2 O 3 -12La 2 O 3 -83TiO 2 glass, the presence of Ti 3+ quenches the 4 I 13/2 emission about 2.6 times more than the 4 I 11/2 when lifetimes are compared to an O 2 melt environment. As an additional means of increasing the mid-infrared emission, the effect of temperature on the mid- and near- infrared lifetimes of a lightly doped lanthanum titanate composition is investigated between 77-300 K. The mid-infrared lifetime increases by ∼30% while the near-infrared lifetime increases by ∼10%, which suggests in addition to co-doping, active cooling of the gain media will further enhance performance.

Materials Science↗
DOE OSTI2024

Mid-infrared trace detection with parts-per-quadrillion quantitation accuracy: Expanding frontiers of radiocarbon sensing

Detection sensitivity is a critical characteristic to consider during selection of spectroscopic techniques. However, high sensitivity alone is insufficient for spectroscopic measurements in spectrally congested regions. Two-color cavity ringdown spectroscopy (2C-CRDS), based on intra-cavity pump–probe detection, simultaneously achieves high detection sensitivity and selectivity. This combination enables mid-infrared detection of radiocarbon dioxide ( 14 CO 2 ) molecules in room-temperature CO 2 samples, with 1.4 parts-per-quadrillion (ppq, 10 − 15 ) sensitivity (average measurement precision) and 4.6-ppq quantitation accuracy (average calibrated measurement error for 21 samples from four separate trials) demonstrated on samples with 14 C/C up to ∼ 1.5 × natural abundance ( ∼ 1,800 ppq). These highly reproducible measurements, which are the most sensitive and quantitatively accurate in the mid-infrared, are accomplished despite the presence of orders-of-magnitude stronger, one-photon signals from other CO 2 isotopologues. This is a major achievement in laser spectroscopy. A room-temperature-operated, compact, and low-cost 2C-CRDS sensor for 14 CO 2 benefits a wide range of scientific fields that utilize 14 C for dating and isotope tracing, most notably atmospheric 14 CO 2 monitoring to track CO 2 emissions from fossil fuels. The 2C-CRDS technique significantly enhances the general utility of high-resolution mid-infrared detection for analytical measurements and fundamental chemical dynamics studies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Radiation transfer in the spectra of short-pulse laser-heated targets

The conditions in laser-produced plasmas are frequently determined with x-ray spectroscopy by comparing calculated to measured spectra. Line spectra from K-shell transitions of low- to mid-atomic number elements are most often used since the important physical processes are well understood and reliable spectra can be readily measured and calculated. Radiation transfer effects due to large optical depths of strong lines can influence the spectra. In this work, the effects of radiation transfer on the emission spectra of short-laser pulse-heated targets are studied. The possible errors made in inferring electron temperature by not including radiation transfer are quantified. The inclusion of radiative transfer in spectral calculations improves the accuracy of typical temperature diagnostics and allows the use of strong lines for diagnostics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗