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At least 289 records · Page 16

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DOE OSTI2020

Parallel Broadband Femtosecond Reflection Spectroscopy at a Soft X-Ray Free-Electron Laser

X-ray absorption spectroscopy (XAS) and the directly linked X-ray reflectivity near absorption edges yield a wealth of specific information on the electronic structure around the resonantly addressed element. Observing the dynamic response of complex materials to optical excitations in pump–probe experiments requires high sensitivity to small changes in the spectra which in turn necessitates the brilliance of free electron laser (FEL) pulses. However, due to the fluctuating spectral content of pulses generated by self-amplified spontaneous emission (SASE), FEL experiments often struggle to reach the full sensitivity and time-resolution that FELs can in principle enable. Here, we implement a setup which solves two common challenges in this type of spectroscopy using FELs: First, we achieve a high spectral resolution by using a spectrometer downstream of the sample instead of a monochromator upstream of the sample. Thus, the full FEL bandwidth contributes to the measurement at the same time, and the FEL pulse duration is not elongated by a monochromator. Second, the FEL beam is divided into identical copies by a transmission grating beam splitter so that two spectra from separate spots on the sample (or from the sample and known reference) can be recorded in-parallel with the same spectrometer, enabling a spectrally resolved intensity normalization of pulse fluctuations in pump–probe scenarios. We analyze the capabilities of this setup around the oxygen K- and nickel L-edges recorded with third harmonic radiation of the free electron laser in Hamburg (FLASH), demonstrating the capability for pump–probe measurements with sensitivity to reflectivity changes on the per mill level.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Selected Area Deposition of High Purity Gold for Functional 3D Architectures

Selected area deposition of high purity gold films onto nanoscale 3D architectures is highly desirable as gold is conductive, inert, plasmonically active, and can be functionalized with thiol chemistries, which are useful in many biological applications. Here, we show that high-purity gold coatings can be selectively grown with the Me 2 Au (acac) precursor onto nanoscale 3D architectures via a pulsed laser pyrolytic chemical vapor deposition process. The selected area of deposition is achieved due to the high thermal resistance of the nanoscale geometries. Focused electron beam induced deposits (FEBID) and carbon nanofibers are functionalized with gold coatings, and we demonstrate the effects that laser irradiance, pulse width, and precursor pressure have on the growth rate. Furthermore, we demonstrate selected area deposition with a feature-targeting resolutions of ~100 and 5 µm, using diode lasers coupled to a multimode (915 nm) and single mode (785 nm) fiber optic, respectively. The experimental results are rationalized via finite element thermal modeling.

3-dimensional nanostructures↗

DOE OSTI2021

Measurement of neutral gadolinium oscillator strengths using dual-comb absorption spectroscopy in laser-produced plasmas

The oscillator strengths of 43 transitions of neutral gadolinium from 530 to 535 nm were determined based on high-resolution absorption spectra measured by probing a laser-produced plasma (LPP) using time-resolved dual-comb spectroscopy (DCS). Absorption spectra were measured at various time delays, ranging from 33 to 252 µs after the onset of the plasma formation, over which the temperature and number density varied as the ablation plume evolved. A Boltzmann analysis was used to determine the excitation temperature and column density of Gd in the ablation plume, based on measured absorption from 20 Gd I spectral lines with known oscillator strengths. Oscillator strengths were then determined for additional dipole-allowed Gd I transitions identified in the absorption spectra, 19 of which were previously unreported. Oscillator strengths of all measured transitions were compared with literature values when available and show good agreement in most cases. Time-resolved measurement of atomic absorption in the cooling plasma provides access to a range of excitation temperatures and optical densities for the atoms in the ablation plume, allowing repeated measurements under different conditions, thereby improving confidence in the results. The high spectral bandwidth and resolution capabilities of DCS make it well-suited to measuring the dense optical spectrum of Gd, and the technique is applicable to other elements, especially lanthanides and actinides.

(280.4788) Optical Sensing, (280.5395) Plasma Diag↗

DOE OSTI2023

Understanding the unique optical and vibrational signatures of sequential infiltration synthesis derived indium oxyhydroxide clusters for CO 2 absorption

Sequential infiltration synthesis (SIS) is a vapor phase synthesis technique with potential to exert precise control over metal oxyhydroxide incorporation into polymer scaffolds. Here, we observe strong size-dependent properties of InO x (OH) y few-atom clusters deposited with variable SIS cycle numbers within a polymethylmethacrylate (PMMA) matrix. Infrared spectroscopy and ultraviolet-visible absorption spectroscopy reveal that the metal atom coordination and optical properties of the clusters depend on the number of SIS cycles performed as well as the choice of processing parameters. The incorporation of indium oxyhydroxide in PMMA via SIS presents an opportunity to improve the CO 2 absorption capacity and gas selectivity of inexpensive polymers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Analysis of ultrafast magnetization switching dynamics in exchange-coupled ferromagnet–ferrimagnet heterostructures

Magnetization switching in ferromagnets has so far been limited to the current-induced spin–orbit–torque effects. Recent observation of helicity-independent all-optical magnetization switching (HI-AOS) in an exchange-coupled ferromagnet–ferrimagnet (FM-FEM) heterostructures expanded the range and applicability of such ultrafast heat-driven magnetization switching. Here we report the element-resolved HI-AOS dynamics of such an exchange-coupled system, using a modified microscopic three-temperature model. We have studied the effect of (i) the Curie temperature of the FM, (ii) FEM composition, (iii) the long-range Ruderman–Kittel–Kasuya–Yosida (RKKY) exchange-coupling strength, and (iv) the absorbed optical energy on the element-specific time-resolved magnetization dynamics. The phase-space of magnetization illustrates how the RKKY coupling strength and the absorbed optical energy influence the switching time. Our analysis demonstrates that the threshold switching energy depends on the composition of the FEM and the switching time depends on the Curie temperature of the FM as well as RKKY coupling strength. Importantly, this simulation anticipates new insights into developing faster and more energy-efficient spintronics devices.

36 MATERIALS SCIENCE↗

DOE OSTI2026

A Compact Monolithic Electro-Optic Package for Quantum Microwave-to-Optical Transduction

We present a novel quantum transduction package that integrates a macroscopic electro-optic crystal into a compact, monolithic assembly designed for superconducting quantum processors. The device provides an efficient and scalable interface between microwave and optical domains while preserving cryogenic compatibility. We performed full-wave and quantum dynamical simulations to assess the performance of the hybrid system, focusing on the interaction between a transmon-based microwave cavity and the crystal’s and cavity low-frequency microwave mode. The transmon operates both as an ancilla for the QPU and as a nonlinear element enabling four-wave mixing between cavity and electro-optic crystal microwave fields. Our results indicate that this architecture can coherently mediate quantum information transfer from the cavity to the electro-optic mode, offering a promising platform for on-chip quantum transduction within superconducting quantum networks.

Reineri, Alessandro [Fermilab] (ORCID:000000016175↗

DOE OSTI2026

A Compact Monolithic Electro-Optic Package for Quantum Microwave-to-Optical Transduction

Reineri, Alessandro [Fermilab] (ORCID:000000016175↗

DOE OSTI2026

Experimental Studies of Nonlinear Integrable Optics with Elliptic Potentials

The stable transport of charged particle beams is the core challenge in designing and operating accelerators. The current paradigm for transverse focusing is based on quadrupole and dipole elements, described as a linear integrable Hamiltonian by Courant and Snyder. The operational limits of high intensity accelerators are often determined by collective instabilities within the beam. Nonlinear elements may be added to suppress certain forms of these collective effects, but restrict the range of stable trajectories. These shortcomings motivate extending to a nonlinear integrable system which can offer the benefits of suppressing collective instabilities without limiting the stable trajectories. Danilov and Nagaitsev proposed a novel nonlinear integrable system with elliptical potentials, which could be implemented as magnetic elements in an accelerator. Such a system has been implemented for practical verification in the integrable optics test accelerator (IOTA), a small storage ring constructed for beam dynamics studies. Electron beam studies in IOTA treat the low-emittance beam as a macroparticle for detailed probing of the expected single particle dynamics. This dissertation details new measurements of the nonlinear integrable system relevant for practical implementation. Turn-by-turn measurements of the kicked beam responses are used for phase space reconstruction and analysis of the predicted nonlinear dynamics. The stability and aperture for various nonlinear configurations are measured with beam losses. Amplitude dependent detuning, a core figure of merit for suppressing instabilities, is measured and compared with high fidelity particle tracking simulations. The synchrotron radiation images of circulating beam allow direct measurements of the topology and lifetime in configurations where nonlinear focusing terms dominate.

Wieland, John [Michigan U.] (ORCID:000000028971852↗

DOE OSTI2024

Fungal elemental profiling unleashed through rapid laser-induced breakdown spectroscopy (LIBS)

ABSTRACT Elemental profiling of fungal species as a phenotyping tool is an understudied topic and is typically performed to examine plant tissue or non-biological materials. Traditional analytical techniques such as inductively coupled plasma–optical emission spectroscopy (ICP-OES) and inductively coupled plasma–mass spectrometry (ICP-MS) have been used to identify elemental profiles of fungi; however, these techniques can be cumbersome due to the difficulty of preparing samples. Additionally, the instruments used for these techniques can be expensive to procure and operate. Laser-induced breakdown spectroscopy (LIBS) is an alternative elemental analytical technique—one that is sensitive across the periodic table, easy to use on various sample types, and is cost-effective in both procurement and operation. LIBS has not been used on axenic filamentous fungal isolates grown in substrate media. In this work, as a proof of concept, we used LIBS on two genetically distinct fungal species grown on a nutrient-rich and nutrient-poor substrate media to determine whether robust elemental profiles can be detected and whether differences between the fungal isolates can be identified. Our results demonstrate a distinct correlation between fungal species and their elemental profile, regardless of the substrate media, as the same strains shared a similar uptake of carbon, zinc, phosphorus, manganese, and magnesium, which could play a vital role in their survival and propagation. Independently, each fungal species exhibited a unique elemental profile. This work demonstrates a unique and valuable approach to rapidly phenotype fungi through optical spectroscopy, and this approach can be critical in understanding these fungi's behavior and interactions with the environment. IMPORTANCE Historically, ionomics, the elemental profiling of an organism or materials, has been used to understand the elemental composition in waste materials to identify and recycle heavy metals or rare earth elements, identify the soil composition in space exploration on the moon or Mars, or understand human disorders or disease. To our knowledge, ionomic profiling of microbes, particularly fungi, has not been investigated to answer applied and fundamental biological questions. The reason is that current ionomic analytical techniques can be laborious in sample preparation, fail to measure all potential elements accurately, are cost-prohibitive, or provide inconsistent results across replications. In our previous efforts, we explored whether laser-induced breakdown spectroscopy (LIBS) could be used in determining the elemental profiles of poplar tissue, which was successful. In this proof-of-concept endeavor, we undertook a transdisciplinary effort between applied and fundamental mycology and elemental analytical techniques to address the biological question of how LIBS can used for fungi grown axenically in a nutrient-rich and nutrient-poor environment.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Rapid quantitative analysis of trace elements in plutonium alloys using a handheld laser-induced breakdown spectroscopy (LIBS) device coupled with chemometrics and machine learning

Here, we present the first reported quantification of trace elements in plutonium via a portable laser-induced breakdown spectroscopy (LIBS) device and demonstrate the use of chemometric analysis to enhance the handheld device's sensitivity and precision. Quantification of trace elements such as iron and nickel in plutonium metal via LIBS is a challenging problem due to the complex nature of the plutonium optical emission spectra. While rapid analysis of plutonium alloys has been demonstrated using portable LIBS devices, such as the SciAps Z300, their detection limits for trace elements are severely constrained by their achievable pulse power and length, light collection optics, and detectors. In this paper, analytical methods are evaluated as a means to circumvent the detection constraints. Three chemometric methods often used in analytical spectroscopy are evaluated; principal component regression, partial least-squares regression, and artificial neural networks. These models are evaluated based on goodness-of-fit metrics, root mean-squared error, and their achievable limits of detection (LoDs). Partial least squares proved superior for determining content of iron and nickel in plutonium metal, yielding LoDs of 15 and 20 ppm, respectively. These results of identifying the undesirable trace elements in plutonium components are critical for applications such as fabricating radioisotope thermoelectric generators or nuclear fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Large aperture and durable glass-engraved optical metasurfaces using nanoparticle etching masks: prospects and future directions

Abstract Metasurfaces (MSs), or surfaces consisting of engineered spatially oriented sub-wavelength elements—also known as meta-atoms—are quickly becoming a burgeoning field of interest due to their seemingly unparalleled control over the propagation of light. This article will discuss the emergence of a MS technology that is based on dewetting thin metal films to form dry etching masks for MS fabrication. The novelty this process presents is the ability to spatially vary mask features—which translates into spatially varying index of the finished surface—in a way that, rather than writing subwavelength elements one-by-one, writes entire areas at once to provide a route to easily scale the process up to meter-sized optics. Glass-engraved MSs have shown to be laser damage resistant, with damage thresholds close to the parent substrate damage thresholds. Furthermore, these surfaces have proven to be mechanically durable and capable of handling normal loads two orders of magnitude higher than that of an average fingerprint pressure. This indicates that accidental handling contact is not detrimental to the MS optical performance. Also discussed are the foreseeable technological challenges, potential solutions for those obstacles, and some currently unexplored directions for future efforts.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Optofluidic memory and self-induced nonlinear optical phase change for reservoir computing in silicon photonics

Nanophotonics allows to employ light-matter interaction to induce nonlinear optical effects and realize non-conventional memory and computation capabilities, however to date, light-liquid interaction was not considered as a potential mechanism to achieve computation on a nanoscale. Here, we experimentally demonstrate self-induced phase change effect which relies on the coupling between geometric changes of thin liquid film to optical properties of photonic waveguide modes, and then employ it for neuromorphic computing. In our optofluidic silicon photonics system we utilize thermocapillary-based deformation of thin liquid film capable to induce nonlinear effect which is more than one order of magnitude higher compared to the more traditional heat-based thermo-optical effect, and allowing operation as a nonlinear actuator and memory element, both residing at the same compact spatial region. The resulting dynamics allows to implement Reservoir Computing at spatial region which is approximately five orders of magnitude smaller compared to state-of-the-art experimental liquid-based systems.

42 ENGINEERING↗

DOE OSTI2023

A beamline for ultrafast extreme ultraviolet magneto-optical spectroscopy in reflection near the shot noise limit

High harmonic generation (HHG) makes it possible to measure spin and charge dynamics in materials on femtosecond to attosecond timescales. However, the extreme nonlinear nature of the high harmonic process means that intensity fluctuations can limit measurement sensitivity. Here we present a noise-canceled, tabletop high harmonic beamline for time-resolved reflection mode spectroscopy of magnetic materials. We use a reference spectrometer to independently normalize the intensity fluctuations of each harmonic order and eliminate long term drift, allowing us to make spectroscopic measurements near the shot noise limit. Here, these improvements allow us to significantly reduce the integration time required for high signal-to-noise (SNR) measurements of element-specific spin dynamics. Looking forward, improvements in the HHG flux, optical coatings, and grating design can further reduce the acquisition time for high SNR measurements by 1–2 orders of magnitude, enabling dramatically improved sensitivity to spin, charge, and phonon dynamics in magnetic materials.

47 OTHER INSTRUMENTATION↗

DOE OSTI2026

An ICP-OES method for the precise and accurate quantification of rare earth elements in natural water: A comparative study from mine waste sites in New Mexico, USA

Inductively coupled plasma techniques such as ICP-OES and ICP-MS are routinely used to determine the concentrations of rare earth elements (REE) in water samples. However, their performance for the determination of REE concentration in mine drainage waters from epithermal vein and porphyry copper mining districts has not been evaluated extensively. In this work, we develop an REE analysis method on an Agilent 5900 ICP-OES instrument and assess the accuracy and precision for the quantification of REE in the natural waters collected from mine adits and an acid seep of mine sites in the Steeple Rock and Hillsboro mining districts, New Mexico, USA. The total REE concentrations in the water samples were measured using the methods we developed for both ICP-OES and ICP-MS. The power of the new ICP-OES method lies in routine analysis of μg/L level concentrations normally analyzed using ICP-MS, including a U.S. Geological Survey standard reference sample, laboratory blank samples spiked with a National Institute of Standards and Technology traceable standard, and surface water samples from mine waste sites. This ICP-OES method achieves low quantification limits ranging from 0.2 to 5 μg/L and excellent analytical accuracy and precision for REE analysis. The precision of light (La-Gd) and heavy (Tb-Lu) REE analysis using this method are better than 5% at average concentrations above 5 ± 4 μg/L and 3 ± 2 μg/L, respectively, and 3% at average concentrations above 10 ± 9 μg/L and 5 ± 4 μg/L, respectively. This method also shows excellent sensitivity and reproducibility for our laboratory and field samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Approach to using 3D laser-induced breakdown spectroscopy (LIBS) data to explore the interaction of FLiNaK and FLiBe molten salts with nuclear-grade graphite

Nuclear graphite has historically been a key component of many nuclear reactor designs and has emerged as key to numerous advanced nuclear reactor design concepts. Molten salt reactors (MSRs) are one broad group of advanced reactor designs currently being pursued by industry for commercialization. Several MSR designs under consideration use graphitic materials that directly interface with a molten salt, whether it is a fuel salt, coolant salt, or both. Therefore, the interaction of graphite materials with molten salts must be understood. To gain this required understanding, a range of data is needed including porosity, strength, and composition as a function of different salt exposure parameters. In this study, a laser-induced breakdown spectroscopy (LIBS) measurement and data analysis methodology was developed to obtain spatially resolved elemental composition information for graphite samples exposed to a molten fluoride salt. Traditional univariate emission line analysis of atomic, ionic, and molecular optical emission signals was coupled via correlation analysis with spectral decomposition of the data using principal component analysis. Elemental depth profiling and elemental mapping were also performed to visualize salt–graphite interactions. LIBS was demonstrated to be useful for measuring key analytes such as fluorine and hydrogen, which are troublesome for other analysis techniques. Evidence for complex behavior was found, thereby demonstrating the usefulness of the developed approach for future systematic studies.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2021

A semi-analytical model for laser induced densification in fused silica at elevated temperatures

A semi-analytical model for deterministic surface smoothing of fused silica below the evaporation temperature threshold is presented. Using this model, a method for calculating deterministic track depths for laser polishing fused silica is derived and validated with experiments. In this work, model predictions were in good agreement with experiment across varying laser preheating temperature and power. With the semi-analytical method presented here, deterministic laser smoothing can be achieved in the densification regime to close the process loop of laser polishing.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Modulating above-room-temperature magnetism in Ga-implanted Fe 5 GeTe 2 van der Waals magnets

The creation of van der Waals (vdW) ferromagnets with tunable Curie temperature (T C ) and magnetic anisotropy is essential in developing vdW magnet-based devices. Here, we report an effective and reliable method for modulating the magnetic properties of vdW Fe 5 GeTe 2 by site-specific Ga + implantation. In this study, we report an easy axis in the ab-plane for bulk Fe 5 GeTe 2 (T C = 310 K) and an axis out of the plane for thin Fe 5 GeTe 2 flakes (T C = 290 K). Combining element-resolved photoemission electron microscopy and spatially resolved magneto-optic Kerr microscopy, we find that the implantation of a tiny amount of 10 –3 Ga + ·Å –3 in Fe 5 GeTe 2 greatly enhances the T C from 290 to 360 K and switches the magnetic easy axis from the out-of-plane c axis to the ab-plane. The room-temperature x-ray magnetic circular dichroism signal is enhanced from 0% to 9% at an implantation level of 10 –2 Ga + ·Å –3 . These results provide new opportunities for tailoring the magnetic properties of vdW materials beyond room temperature.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Assessment of errors in analytic modeling of permanent magnet electron spectrometers for laser-plasma accelerators

Here, we assess the error in three treatments of a critical electron beam diagnostic for laser-plasma acceleration (LPA) experiments: a permanent magnet electron spectrometer. Since LPA electron spectrometers are often difficult to calibrate due to the scarcity of well-characterized, tunable electron beam sources in the appropriate energy range and the mechanical complexity of electron spectrometers, the standard of calibration is Hall probe measurements. We first compare the electron spectrometer performance between SIMION calculations and the Hall probe measurements. We find up to a 60% (<8%) error in determining the absolute energy for electrons below (above) 80 MeV when using the SIMION-modeled magnetic field vs the measured magnetic field due to SIMION overpredicting fringe field strength. The difference in spectrometer energy resolution is within ∼10% between the modeled and measured fields. We then assess a simple block model, which is commonly used. We find that the simple block model presented here sufficiently captures the predicted as-built spectrometer performance for any application provided that the user can tolerate uncertainties on absolute energy determination up to 5% and errors on energy resolution up to 1%.

Electromagnetic optics↗