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DOE OSTI2023

Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource

We present a dedicated end-station for solution phase high repetition rate (MHz) picosecond hard x-ray spectroscopy at beamline 15-2 of the Stanford Synchrotron Radiation Lightsource. A high-power ultrafast ytterbium-doped fiber laser is used to photoexcite the samples at a repetition rate of 640 kHz, while the data acquisition operates at the 1.28 MHz repetition rate of the storage ring recording data in an alternating on-off mode. The time-resolved x-ray measurements are enabled via gating the x-ray detectors with the 20 mA/70 ps camshaft bunch of SPEAR3, a mode available during the routine operations of the Stanford Synchrotron Radiation Lightsource. As a benchmark study, aiming to demonstrate the advantageous capabilities of this end-station, we have conducted picosecond Fe K-edge x-ray absorption spectroscopy on aqueous [FeII(phen)3]2+, a prototypical spin crossover complex that undergoes light-induced excited spin state trapping forming an electronic excited state with a 0.6–0.7 ns lifetime. In addition, we report transient Fe Kβ main line and valence-to-core x-ray emission spectra, showing a unique detection sensitivity and an excellent agreement with model spectra and density functional theory calculations, respectively. Notably, the achieved signal-to-noise ratio, the overall performance, and the routine availability of the developed end-station have enabled a systematic time-resolved science program using the monochromatic beam at the Stanford Synchrotron Radiation Lightsource.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Development of local-power-free, remote α -particle detection using optical fibers

We demonstrate the application of fluorescence optical fiber coupled to a telecom grade fiber as a sensor for alpha particles using alpha-specific ZnS(Ag) scintillation materials whose wavelength is down-shifted into a low-loss region of the telecom grade fiber transmission band. Telecom-grade fiber optics offer a solution for sensing alpha radiation in deep repositories and cask storage for radioactive materials due to the stability of SiO 2 under normal environmental conditions and its relative radiation hardness at low radiation doses. Long-term nuclear waste storage facilities require sensors for the detection of leakage of radioactive materials that are maintenance-free, do not require power and can survive with no ‘wear out’ mechanisms for decades. By accomplishing the wavelength transformation, we maximize efficiencies in the detection of α-particles and signal transport and can detect alpha scintillation at distances on the order of >1 km with a sensor that is ~3% efficient and can be easily scaled as a sensor array. This paper describes the construction and testing of the sensor including manufacture of the controlled thickness films, verification of the wavelength shift from 450 to 620 nm and optimization of the sensitivity as a function of thickness. We also model the relative sensitivity of the film as a function of film thickness, and we demonstrate a signal-to-noise ratio of 10 at a range of greater than 1 km.

alpha particles↗

DOE OSTI2021

Medium-induced radiative kernel with the Improved Opacity Expansion

We calculate the fully differential medium-induced radiative spectrum at next-to-leading order (NLO) accuracy within the Improved Opacity Expansion (IOE) framework. This scheme allows us to gain analytical control of the radiative spectrum at low and high gluon frequencies simultaneously. The high frequency regime can be obtained in the standard opacity expansion framework in which the resulting power series diverges at the characteristic frequency ω c ~ q^L 2 . In the IOE, all orders in opacity are resumed systematically below ωc yielding an asymptotic series controlled by logarithmically suppressed remainders down to the thermal scale T « ω c , while matching the opacity expansion at high frequency. Furthermore, we demonstrate that the IOE at NLO accuracy reproduces the characteristic Coulomb tail of the single hard scattering contribution as well as the Gaussian distribution resulting from multiple soft momentum exchanges. Finally, we compare our analytic scheme with a recent numerical solution, that includes a full resummation of multiple scatterings, for LHC-inspired medium parameters. Furthermore, we find a very good agreement both at low and high frequencies showcasing the performance of the IOE which provides for the first time accurate analytic formulas for radiative energy loss in the relevant perturbative kinematic regimes for dense media.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Compact Superconducting RF Accelerators for Water Treatment

Jefferson Lab is actively exploring the environmental applications of compact irradiation facilities utilizing Superconducting Radio Frequency (SRF) accelerator technology ? a well-established technology primarily used in large research machines. Recent advancements, such as the application of thin films of superconducting alloys in radio frequency (RF) resonators and the development of high-capacity cryocoolers, have made it feasible to employ this key technology in compact, standalone irradiation facilities. The main advantage over conventional systems based on normal conducting technology is the significantly enhanced efficiency in beam power generation, enabling exposure to substantially higher radiation doses. In the realm of addressing contaminants in wastewater treatment, particularly concerning persistent substances known as "forever chemicals," this technology presents an attractive solution, given the required considerable effort i.e. dose to break them down. Experiment Numbers:

Vennekate, John↗

DOE OSTI2024

Compact Superconducting RF Accelerators for Water Treatment

Vennekate, John↗

DOE OSTI2024

Effects of electron beam irradiation on CrMnV and CrMnTiV high entropy alloys: Nano-mechanical, structural, and thermodynamic perspectives

Beam exit windows are crucial components of any particle accelerator as they provide an interface between the beamline vacuum and target material at atmospheric media. For high beam power machines, special materials and designs are required to withstand high radiation and mechanical loads, while minimizing energy loss during transition and maximizing window lifetime. This research investigates the impact of electron beam exposure to bulk CrMnV and CrMnTiV high entropy alloys (HEAs) with the primary goal of identifying suitable candidate materials for the design of robust and durable exit window settings. The selection criteria include intrinsic characteristics, power dissipation, and mechanical responses. According to the thermodynamic calculations, both equiatomic CrMnV and the addition of 7% of Ti with equiatomic CrMnV yield solid-solutions phases. The structural and mechanical properties of CrMnV and CrMnTiV samples were tested using field emission scanning electron microscopy, atomic force microscopy, scanning electron microcopy with energy dispersive x-ray spectroscopy, x-ray diffraction, and nanoindentation before and after exposure to a dose of ~66 kGy from a 10 MeV e-beam accelerator. Despite exhibiting beam transmission characteristics comparable to Cr and V, the indentation hardness of HEAs exceeded that of the Cr and V samples by five to six times. The examination of the CrMnTiV irradiated samples revealed organized deformation patterns depicting new features, which we suspect twinning and twin boundaries due to the addition of Ti to CrMnV. Ti, a hexagonal-close-packed crystal structure, is commonly known for deformation twinning behavior.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Development of a Multi-Robot System for Autonomous Inspection of Nuclear Waste Tank Pits

This paper introduces the overall design plan, development timeline, and preliminary progress of the Autonomous Pit Exploration System project. This project aims to develop an advanced multi-robot system for the efficient inspection of nuclear waste-storage tank pits. The project is structured into three phases: Phase 1 involves data collection and interface definition in collaboration with Hanford Site experts and university partners, focusing on tank riser geometry and hardware solutions. Phase 2 includes the selection of sensors and robot components, detailed mechanical design, and prototyping. Phase 3 integrates all components into a cohesive system managed by a master control package which also incorporates digital twin and surrogate models, and culminates in comprehensive testing and validation at a simulated tank pit at the Idaho National Laboratory. Additionally, the system’s communication design ensures coordinated operation through shared data, power, and control signals. For transportation and deployment, an electric vehicle (EV) is chosen to support the system for a full 10 h shift with better regulatory compliance for field deployment. A telescopic arm design is selected for its simple configuration and superior reach capability and controllability. Preliminary testing utilizes an educational robot to demonstrate the feasibility of splitting computational tasks between edge and cloud computers. Successful simultaneous localization and mapping (SLAM) tasks validate our distributed computing approach. More design considerations are also discussed, including radiation hardness assurance, SLAM performance, software transferability, and digital twinning strategies.

Nuclear waste management↗

DOE OSTI2020

Soft x-ray spectrum unfold of K-edge filtered x-ray diode arrays using cubic splines

Cubic spline interpolation is able to recover temporally and spectrally resolved soft x-ray flux from an array of K-edge filtered x-ray diodes without the need for a priori assumptions about the spectrum or the geometry of the emitting volume. The mathematics of the cubic spline interpolation is discussed in detail. The analytic nature of the cubic spline solution allows for analytical error propagation, and the method of calculating the error for radiation temperature, spectral power, and confidence intervals of the unfolded spectrally resolved flux is explained. An unfold of a blackbody model demonstrates the accuracy of the cubic spline unfold. Tests of cubic spline performance using spectrally convolved detailed atomic model simulation results have been performed to measure the method's ability to conserve spectral power to within a factor of 2 or better in line-dominated regimes. The unfold is also demonstrated to work when information from the x-ray diode array is limited due to high signal-to-noise ratios or lack of signal due to over-attenuation or over-filtration of the x-ray diode signal. Here, the robustness of the unfold with respect to background subtraction and raw signal processing, signal alignment between diode traces, limited signal information, and initial conditions is discussed. Results from an example analysis of a halfraum drive are presented to demonstrate the capabilities of the unfold in comparison with previously established methods.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

EPCAPE-PT-LANL Measurements: Single Particle Soot Photometer

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Single Particle Soot Photometer (Droplet Measurements Technology) Data Notes: Contact us if you want additional data products from this instrument. Reported data is the black carbon (rBC) number and mass concentration with diagnostic flags. The SP2 measures incandescence from particles that is induced with a 1064 Nd-YAG laser. Particles that absorb the laser energy and then emit radiation is assumed to contain black carbon. The amount of intensity of radiation is related to the mass of absorbing material in the particle. Here, we calibrate the incandescence intensity to size selected Regal Black (Cabot) nebulized from solution. Data provided for the EPCAPE campaign used the combined broadband high-gain + low-gain channels (BHBL). Each channel has a lower threshold of detection equivalent to 2-s of the respective channel noise. Thresholding has been applied to select between the high-gain and low-gain channels. The detection limit is 80-540 nm (Deq) or 0.36- 55 fg. It is assumed that rBC is the only aerosol type that is in significant concentration in the sampled atmosphere that absorbs the laser energy. Particle data are integrated over 10 second windows to calculate a rBC number and mass concentration. QC/QA: • Diagnostic flags that impacted measured concentration: - Sample, Sheath, and Purge Flow Rates: Despite observing fluctuations in all flows, the rBC detection and mass quantification are generally observed to be stable, although large changes in sample flow rate did impact detection efficiency. A flag was implemented for sample flow deviations >12 cm3/min from the set point averaged over 30 seconds - Laser Power: Detection efficiency decreases with laser power and deviations in laser power also affect mass quantification. Flag for laser power is set for deviations in laser current from the set value >5 mA. - Primary Detector Threshold: Primary thresholding is the signal value which determines whether a “particle” is recorded. Thresholding errors occur when the threshold value is too HIGH and real particles are ignored. • Several periods without data: - 16-18 Nov: Ultra Zero Air generator failure, flows deviated significantly from set points. rBC # conc recovered but questionable. - 20-21 Nov: Offline for calibrations for several hours each day. - 25-27 Nov: Data is missing. - 30 Nov: Power outage 3 Dec: SP2 hard-drive full. - 3 Dec: Power Outage Header: - BHBL_NumbConc[#/cc]: Refers to the number concentration of refractory black carbon (rBC) measured from combined broadband high-gain and low-gain channels, expressed in particles per cubic centimeter. - BHBL_BCMass_Conc[ug/m3]: Refers to the mass concentration of refractory black carbon (rBC) measured from combined broadband high-gain and low-gain channels, expressed in micrograms per cubic meter. - NoData_Flag[bool]: A boolean flag that indicates whether no data was recorded during a measurement. - NoBC_Flag[bool]: A boolean flag indicating whether no black carbon particles were recorded during the measurement. - Laser_Flag[bool]: A boolean flag indicating deviations in laser current during the measurement. - SampleFlow_Flag[bool]: A boolean flag indicating deviations from the set sample flow rate during the measurement. - PrimThresh_Flag[bool]: A boolean flag indicating deviations from the set primary threshold during the measurement, potentially ignoring real particles. - Manual_Flag[bool]: A boolean flag indicating manual intervention or adjustments during the measurement. - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active or inactive during the measurement.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Monte Carlo Simulations of Polarized Radiative Transfer in Neutron Star Atmospheres

Soft X-ray emission from neutron stars affords powerful diagnostic tools for uncovering their surface and interior properties, as well as their geometric configurations. In the atmospheres of neutron stars, the presence of magnetic fields alters the photon-electron scattering cross sections, resulting in nontrivial angular dependence of intensity and polarization of the emergent signals. This paper presents recent developments of our Monte Carlo simulation, MAGTHOMSCATT, which tracks the complex electric field vector for each photon during its transport. Our analysis encompasses the anisotropy and polarization characteristics of X-ray emission for field strengths ranging from nonmagnetic to extremely magnetized regimes that are germane to magnetars. In the very low field domain, we reproduced the numerical solution to the radiative transfer equation for nonmagnetic Thomson scattering, and provided analytical fits for the angular dependence of the intensity and the polarization degree. These fits can be useful for studies of millisecond pulsars and magnetic white dwarfs. By implementing a refined injection protocol, we show that, in the magnetar regime, the simulated intensity and polarization pulse profiles of emission from extended surface regions becomes invariant with respect to the ratio of photon (ω) and electron cyclotron (ω B ) frequencies once ω/ω B ≲ 0.01. This circumvents the need for simulations pertinent to really high magnetic field strengths, which are inherently slower. Our approach will be employed elsewhere to model observational data to constrain neutron star geometric parameters and properties of emitting hot spots on their surfaces.

79 ASTRONOMY AND ASTROPHYSICS↗