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At least 487 records · Page 27

Qualification of Processing Batches for Tank Closure Cesium Removal Through In-Tank Batch Contact Testing - 20470

The Tank Closure Cesium Removal (TCCR) process at the Savannah River Site (SRS) is currently processing waste from Tank 10H, generating decontaminated salt solution that is sent to Tank 11H. Transfers out of Tank 11H are then disposed of on site as a grout wasteform in the SRS Saltstone Processing Facility. This is a full-scale demonstration of the use of Crystalline Silicotitanate (CST) for the decontamination of aqueous nuclear waste supernate. CST primarily removes cesium from the high sodium alkaline feed, but also adsorbs strontium, actinides, and some other trace metals. The TCCR unit is an at-tank set of four ion exchange columns, with two typically being operated in series during waste processing. Tank 10H is serving a dual function as both the salt dissolution tank as well as the feed tank for the TCCR system. Prior to operation of TCCR, Tank 10H must undergo dissolution campaigns, dissolving the salt cake to form an aqueous salt solution (supernate). After each dissolution campaign, the supernate created must be qualified prior to processing through the TCCR system. Qualification includes detailed characterization of the supernate as well as in-tank batch contact tests to determine the equilibrium loading of Cs-137 on the CST ion exchange media (IONSIV{sup TM} R9120-Ba). In support of the in-tank batch contact testing, Savannah River National Laboratory (SRNL) developed a CST sample holder, also referred to as a 'tea-bag', to hold a measured amount (∼0.1 grams) of pretreated CST between stainless steel screens. The tea-bag fits within a standard stainless steel sample vial that has been modified to allow the flow of supernate to the CST. This sample holder is then immersed in the waste tank allowing free contact between the CST beads and the surrounding liquid, at an effectively infinite liquid-to-solid phase ratio. A pair of tea-bags are deployed in the tank for a period of 10 days for each batch, after which the CST is recovered, digested, and analyzed to determine the loading of cesium isotopes on the CST. This result then supports the TCCR column thermal loading limits for processing as part of the TCCR safety basis. This paper will discuss the design and testing of the CST sample holder, as well as results from the first few batches of waste qualified and subsequently processed through the TCCR system. In addition, results from analyses of Tank 11H samples, showing decontamination of the product will be included. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Rapid Droplet Sampling Interface for Low-Volume, High-Throughput Mass Spectrometry Analysis

Here, we present a rapid droplet sampling interface (RDSI) electrospray ionization mass spectrometry (ESI-MS) system as a high-throughput, low-volume, noncontact, and minimal-carryover approach for characterization of liquids. Liquid characterization was achieved by combining droplet ejection with an open-face microflow capillary with a 2.5 μL/min continuous flow of carrier solvent. Through this implementation, single 0.3 nL droplets containing the analyte effectively mix with 4–8 nL of carrier solvent and create a combined electrospray plume. The carrier solvent continuously cleaned the system, eliminating carryover. A sampling rate of 5 Hz was achieved for droplets containing 1 μM propranolol or 5 μM leu-enkephalin with each droplet fully baseline-resolved (138 ± 32 ms baseline-to-baseline). Using a SCIEX API4000 mass spectrometer, a lower limit of quantification (LLOQ) of propranolol was 15 nM, corresponding to 1.16 fg of propranolol in the droplet, and was linear across 3 orders of magnitude. Further, quantitation could be achieved by adding an isotopically labeled internal standard, as done in conventional ESI. Signal transients were faster than the acquisition speed of the mass spectrometer, resulting in artificially high reproducibility of 15–30% RSD droplet-to-droplet. Analyte–solvent mixing ratios could be controlled by adjusting droplet positioning along the open-face capillary with an optimal position about 0.4 mm from the tip end. The range of analyte coverage was exemplified by measures of peptides and drugs in methanol, water, and buffer solutions. In a comparison to the Open Port Sampling Interface (OPSI) implemented on the same system, the RDSI had 78× greater sensitivity, 6× greater throughput and used significantly less carrier solvent.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Testing shell-model interactions at high excitation energy and low spin: Nuclear resonance fluorescence in Ge 74

With their complex low-spin structure, the germanium isotopes have accrued a large number of experimental data which challenge nuclear models. The structure of the 74 Ge isotope is investigated here with nuclear resonance fluorescence as part of an extensive campaign of experimental tests of the shell model in the germanium isotopic chain using a number of complementary techniques. Levels were excited with 3.10 – 5.44 MeV photon beams provided by the High Intensity Gamma-Ray Source at TUNL. Many new levels were identified and their spins, parities, branching ratios, and associated scattering cross section values were determined. Large-scale shell-model calculations, which include jj44b and JUN45 effective interactions developed to describe nuclei in this mass region, predict the new data satisfactorily. Herein this study extends the validation of these two interactions, which are candidates for computation of matrix elements to be used in the interpretation of neutrinoless double-β decay experiments in 76 Ge, into the low-spin, high excitation energy domain.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Distinguishing fissile uranium isotopes using an active well neutron coincidence counter

Proposed thorium-based nuclear fuel cycles are likely to require quantification and verification of 233 U within nuclear material. Because of their similar fission cross sections, active neutron nondestructive assay (NDA) systems may respond similarly to 233 U and 235 U. Traditional safeguards equipment has been optimized for 235 U and 238 U quantification associated with conventional uranium/plutonium fuel cycles and may not be directly applicable to 233 U quantification when mixed with other actinides. This work used models of the large volume active well coincidence counter (LV-AWCC) at Oak Ridge National Laboratory to evaluate the performance of this neutron NDA system to differentiate fissile uranium isotopes. The models were developed to simulate NDA system performance in response to a number of triangular radiation signature training device sources within the central cavity or well. This work predicted that the LV-AWCC can effectively differentiate 233 U from 235 U in certain modes of operation. In active mode, the LV-AWCC with the cadmium liner results in different doubles count rates between the fissile isotopes for a given fissile uranium mass. Without the cadmium liner, the uranium isotopes provide a statistically indistinguishable doubles count rate response for the fissile masses considered in this work (up to approximately 150 g). The cadmium liner serves to harden the neutron interrogation spectrum, which better exploits the notable difference in the 233 U and 235 U fission cross sections at approximately 1 eV. In passive mode, the two fissile isotopes exhibit different doubles and singles count rates regardless of liner presence because the passive source strength of 233 U is approximately 2 orders of magnitude stronger than that of 235 U due to the shorter half-life and correspondingly higher (α, n) yield. We conclude that using neutron interrogation in the LV-AWCC, two measurements are needed to quantify 233 U content in mixed uranium items. The first measurement is used to determine the total fissile uranium mass using a mode that cannot distinguish fissile isotopes (i.e., where a similar response is observed for both fissile uranium isotopes such as active doubles without cadmium or using a thermal neutron interrogation source). In conclusion, the second measurement is used to determine the 233 U content by using a differentiating technique (e.g., passive doubles, passive doubles to singles ratio, active doubles with cadmium).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Risk Analysis of Radiological Release from Pu-238 Targets During Manual Handling

Pu-238 Isotope Production Targets are routinely installed in the Advanced Test Reactor (ATR) core, transferred, and stored in the spent fuel canal. These evolutions involve manual handling and manipulation of the targets underwater using long handled tools. The ATR Safety Analysis Report (SAR) postulates a design basis accident which results in damage from manual manipulation of targets, and radiological consequences must be determined for receptors inside the reactor facility, as well as public receptors. This presentation presents the analysis used to determine the radiological consequences due to potential target damage in the ATR canal. The analysis considered radionuclide release fractions, damage ratios for handling evolutions, and entrainment of radionuclides in the canal water.

Advanced Test Reactor↗

Chemical and isotopic evolution of flowback fluids from the Utica Gas Shale Play, Eastern Ohio USA

For this work, hydraulic fracturing flowback fluids were collected from two Utica/Point Pleasant well pads in eastern Ohio. One site was in the wet gas zone (UPPW), while the site ~50 km south consisted of four wells on the same pad in the dry gas zone (UPPS). Samples of input fluids also were collected before and during hydraulic fracturing. Flowback fluids are Na-Ca-Cl brines with total dissolved salt (TDS) concentrations that increase over several months from ~100 to 200 g/L. The slightly higher TDS of the dry gas fluids are in part due to recycled flowback used as input fluids, and in part due to lower volume of water used in hydraulic fracturing. Concentrations of most major ions (Ca 2+ , Mg 2+ , Na + , Sr2 + , Fe, Mn, Cl – , Br – ) are similar for the five wells sampled, although small but systematic changes occur in the major element ratios over time. Most notably, an increase in the Sr/Cl ratio corresponds to an increase in the 87 Sr/ 86 Sr ratio in the fluids, suggesting interactions with a more radiogenic Sr source in the subsurface. Dissolved Ba concentrations and Ra activities were different between the two sites, reflecting a high SO 4 2– fluid used at the UPPW site, and water-rock reactions occurring during hydraulic fracturing at the UPPS site. Water oxygen (δ 18 O) and hydrogen (δD) isotopes for input fluids used in the UPPW4 well and fresh water used for the UPPS wells fall on the Global Meteoric waterline (GMWL). Flowback fluids from both sites are relatively enriched in δ 18 O and δD compared to the input, but do not appear to follow a simple mixing trend, suggesting reaction and isotopic exchange with carbonates and fractionation due to imbibition in the rock. Cl isotopes, δ 37 Cl in the FP fluids varied from ~ –0.43 to +0.13‰, the largest variation was observed in the earlier stages of flowback, while in the later stages δ 37 Cl exhibited a small but systematic increase over time, suggesting diffusion control of isotopic composition. Some of the trace species measured (dissolved Fe, Mn, thiosulfate and organic acids) do not follow the same trends as the major ions, suggesting contributions from input fluids, or microbially mediated reactions are exerting control on their concentrations. Input water chemistry exerts an important control on the Sr and Ba concentrations in flowback water. High SO 4 2– in the input fluids used for hydraulically fracturing the wet gas well leads to precipitation of barite-celestite in flowback fluids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

In the nuclear explosion monitoring context, what is an anomaly?

Abstract In the early years of nuclear explosion monitoring, experts used downwind detections with meaningful ratios of radioactive species to identify an explosion. Today’s reality is sparse networks of radionuclide monitoring stations looking for weak signals. Analysts need to discriminate between industrial background radioactivity and nuclear explosion signals, even using the detection of one isotope. Aerosol and xenon measurements potentially related to nuclear tests in 2006 and 2013 announced by the Democratic People’s Republic of Korea and from worldwide civilian background radioactivity are considered when defining radionuclide detection anomalies to objectively guide the use of limited analyst resources and reduce the possibility of not detecting nuclear explosions.

Miley, Harry S.↗

Investigation of the 176 Yb Interference Correction during Determination of the 176 Hf/ 177 Hf Ratio by Laser Ablation and Solution Analysis on the Neoma MC-ICP-MS

We utilized the Neoma™, a recently released MC-ICP-MS platform offered by ThermoFisher Scientific, to assess the behavior of the Lu-Yb-Hf system during laser ablation analyses of various zircon standards as well as solution-based analyses of the JMC-475 Hf standard doped with varying quantities of Yb and Lu. The primary goal of this work was to characterize the behavior of the Yb interference correction on the Neoma™ platform since this is one of the biggest issues in the Hf isotope analysis community and because the Neoma™ platform will supplant the Neptune™ series instrument. During laser ablation analysis, we found that the overall data quality scales proportionally with the total Hf signal intensity, with higher signal analyses producing extremely accurate (within 1 ε Hf unit) and precise (sub ε Hf unit within-run standard errors) data. At low Yb signals (<0.1 V 173 Yb), we were not able to produce an accurate internal Yb mass bias factor. However, utilizing an empirical approach allows for the application of session-specific relationships between the Yb and Hf mass bias factors, determined by analysis of standards of varying Yb content, to produce accurate ε Hf values from zircons with higher Yb/Hf ratios even where the total Hf signal intensity is relatively low. Similar behavior was observed in the solution analyses. Lastly, while the behavior of the Yb interference correction on the Neoma™ platform appears comparable to the Neptune™ series MC-ICP-MS, further work will help refine the understanding of the controls on mass bias behavior, oxide formation, session-to-session stability, etc.

36 MATERIALS SCIENCE↗

Lignin lags, leads, or limits the decomposition of litter and soil organic carbon

Lignin’s role in litter and soil organic carbon (SOC) decomposition remains contentious. Lignin decomposition was traditionally thought to increase during midstage litter decomposition, when cellulose occlusion by lignin began to limit mass loss. Alternatively, lignin decomposition could be greatest in fresh litter as a consequence of co-metabolism, and lignin might decompose faster than bulk SOC. To test these competing hypotheses, we incubated 10 forest soils with C 4 grass litter (amended with 13 C-labeled or unlabeled lignin) over 2 yr and measured soil respiration and its isotope composition. Early lignin decomposition was greatest in 5 of 10 soils, consistent with the co-metabolism hypothesis. However, lignin decomposition peaked 6–24 months later in the other five soils, consistent with the substrate-limitation hypothesis; these soils were highly acidic. Rates of lignin, litter, and SOC decomposition tended to converge over time. Cumulative lignin decomposition was never greater than SOC decomposition; lignin decomposition was significantly lower than SOC decomposition in six soils. Net nitrogen mineralization predicted lignin decomposition ratios relative to litter and SOC. Although the onset of lignin decomposition can indeed be rapid, lignin still presents a likely bottleneck in litter and SOC decomposition, meriting a reconsideration of lignin’s role in modern decomposition paradigms.

54 ENVIRONMENTAL SCIENCES↗

Postirradiation Examination of HFIR-Irradiated Yttrium Hydrides

The US Department of Energy Microreactor Program is developing compact, high-temperature microreactors that require robust neutron moderators. Known for its high hydrogen retention and structural stability, YH x is a leading candidate for this purpose. As part of an ongoing evaluation, Oak Ridge National Laboratory conducted post-irradiation examinations on YH x specimens irradiated in the High Flux Isotope Reactor under the legacy Transformational Challenge Reactor program, focusing on their structural integrity, hydrogen retention, and thermal properties. The post-irradiation examination campaign primarily examined specimens from two irradiation campaigns, covering a range of hydrogen-to-yttrium atomic ratios (H/Y), neutron damage levels (0.1–2 displacements per atom), and targeted irradiation temperature of 600°C. The investigations included electron microscopy, high-energy x-ray diffraction, laser flash analysis, differential scanning calorimetry, and SiC thermometry analysis.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

An Evaluation of Actinide Reactivity with CO 2 , O 2 , and O 2 /He Gases using Inductively Coupled Plasma Tandem Mass Spectrometry: Application to Simultaneous Measurement of 241 Am/ 241 Pu Ratios in Unseparated Complex Matrices

Accurate actinide measurements are critical within the field of nuclear science. Traditional methods for actinide quantification require time-consuming sample processing prior to analysis. There is a need for rapid analytical techniques that still maintain a high degree of accuracy. In this work, actinide reactivity was assessed for multiple oxygen-containing reaction gases using quadrupole inductively coupled plasma tandem mass spectrometry (Q-ICP-MS/MS) to evaluate actinide analysis in complex sample matrices without analyte-matrix separation. A novel method was developed to measure 241 Am/ 241 Pu in complex sample matrices using O 2 /He reaction gas with no matrix removal or analyte pre-concentration. This inline method reduces matrix-derived polyatomic interferences that complicate traditional ICP-MS analyses by mass-shifting to 241 Am 16 O + and 241 Pu 16 O 2 + , allowing Am and Pu to be mass separated for simultaneous analysis. While mass shifting is efficient, a small portion of Am + (<1.3%) and Pu + (<1.4%) react to from AmO 2 + and PuO + , respectively. Therefore, a mass balance approach was used, in combination with reactivity determined from 242 Pu and 243 Am standard solutions, to correct for residual 241 PuO + and 241 AmO 2 + . The method was validated by measuring 241 Am/ 241 Pu in Pu isotope standards CRM-136 and CRM-137 (separated in March/April 1970 and February 2022, respectively) in both neat solutions and complex matrices containing diluted soil (NIST SRM 2711a, >1000 µg·g -1 ). Method detection limits of 15.9 and 9.6 fg·g -1 were determined for 241 Am and 241 Pu, respectively, and 241 Am/ 241 Pu ratios were measured with accuracies within <3.5%. In conclusion, this work presents the first direct analysis of 241 Am/ 241 Pu in unseparated complex matrices, advancing capabilities for rapid actinide measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exploring the use of thorium isotope compositions and concentrations as nuclear forensic signatures for uranium ore concentrates

This interlaboratory study measured thorium concentrations and isotope compositions in uranium ore concentrates from different geographical locations to examine whether thorium impurities may be useful forensic signatures for uranium ore concentrates found out of regulatory control. Measured 230 Th/ 232 Th in fifteen uranium ore concentrates record over three orders of magnitude of compositional variation. Results demonstrate that 230 Th/ 232 Th used in combination with U/Th ratios resulted in a unique signature for individual uranium ore concentrates from different processing locations. Data presented here suggest potential for 230 Th/ 232 Th and U/Th to be used as comparative signatures to investigate the provenance of seized uranium ore concentrates.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Gamma ray analysis of the K2 containers

The K2 containers contain PuO2 with 238 Pu being the most abundant isotope of all plutonium isotopes. The purpose of this analysis is to determine the light element impurities in the PuO2. These light elements can interact with the alpha particles from plutonium decay to release gamma rays, protons, and neutrons through the reactions (α,α’), (α,p), and (α,n) respectively. The gamma rays released by the interactions can be measured and compared with the gamma rays released by the plutonium. The ratios of the gamma rays from the interactions and the plutonium gamma rays allow for the determination of the impurities in the items. The elements that can be detected are Lithium (Z=3), Beryllium (Z=4), Boron (Z=5), Fluorine (Z=9), Sodium (Z=11), Magnesium (Z=12), Aluminum (Z=13), Silicon (Z=14), Phosphorous (Z=15), Chlorine (Z=17), and Potassium (Z=19).

07 ISOTOPE AND RADIATION SOURCES↗

Balmer emission measurements in JET-ILW hydrogen, deuterium, tritium and deuterium-tritium low-confinement mode plasmas

Measurements of Balmer-alpha (B-α) and Balmer-gamma (B-γ), where B = H, D, or T isotopes of hydrogen, emission across the low-field side (LFS) divertor in JET ITER-like Wall (ILW), low-confinement mode (L-mode) plasma indicate that the divertor plasma was more strongly detached in deuterium, tritium and deuterium–tritium than in hydrogen plasmas. These measurements are consistent with the lower degree of detachment in hydrogen versus tritium plasmas inferred from Langmuir probes (Groth et al., 2023). The ratio of B-γ to B-α is a suitable indicator of high density/low temperature conditions because B-α emission is dominated by electron impact excitation with a small electron–ion recombination component regardless of electron temperature and density (for conditions in tokamak plasmas) whilst for B-γ the recombination component increases and the excitation component decreases as the electron temperature decreases and the electron density increases. Within the uncertainty of the measurements, the electron density at the low-field side separatrix and the power crossing the separatrix are similar to permit these comparisons. The B-©/B-α ratio is well correlated with the onset of detachment as measured by Langmuir probes (McCracken et al., 1998; Groth et al., 2023). The ratios of B-γ and B-α varied between 0.005 and 0.035 for low-recycling, high-recycling and partially detached conditions, and were 60–70 % higher in partially detached hydrogen than in tritium plasmas. In contrast, the difference between deuterium, tritium and 40–60 % deuterium–tritium is within 10 % and thus within the uncertainties of the measurements. Profiles of the B-α and B-γ emission was measured with two filtered CCDs connected to the visible lost light leg of JET’s mirror link spectroscopy system (Meigs et al., 2010; Lomanowski et al., 2014). Spatially (radial) narrower B-α profiles were measured with increasing isotope mass, while similarly broadened B-γ profiles were measured.

Balmer↗

Imaging Based Detector with Efficient Scintillators for Neutron Diffraction Measurements

The Anger Camera developed by the detector group at the Oak Ridge National Laboratory was utilized for the present work for its unique advantage of employing multiple modules to obtain large active measurement area for detecting diffracted/scattered thermal neutrons. Considering the relatively small flux associated with diffracted/scattered neutrons, suitable efficiency with high spatial resolution is a requirement for utilizing two-dimensional imaging detectors. The potential to implement pulse shape (in addition to pulse height) discrimination-based scintillators further enhances the ability to detect diffracted neutrons with improved signal to noise ratio. In this paper, initial results associated with 6Li glass-based scintillator will be presented. The authors explored the feasibility of using this system to detect and quantify diffraction peaks and peak shifts at the Neutron Residual Stress Facility (NRSF2), High Flux Isotope Reactor (HFIR) in the Oak Ridge National Laboratory (ORNL). Suitable camera mounting and shielding had to be developed. Reference measurements using polycrystalline powders with known atomic planar spacing will be discussed along with measurement settings associated with expected resolution for peak shift measurements. Initial results are promising and demonstrate that a suitable scintillation-based neutron detecting system is viable for residual stress-based diffraction measurements. Small area detectors are also feasible with suitable consideration to scattering volume and distance to detector.

Seals, Matthew↗

An Updated Picture of Presolar History from Short-lived Radioactive Isotopes and Inferences on the Birth of the Sun

We examine the origin of the short-lived radionuclides (SLRs; defined as having half-lives between 0.1 and 100 Ma) present in the early solar system (ESS) by investigating how predictions of their abundances in the interstellar medium (ISM) from steady-state equilibrium relate to their ESS values. For this, we take into account the non-negligible time t iso elapsed between the isolation of the presolar molecular cloud and the formation of the ESS, during which the SLRs decayed freely. We also consider the alternative scenario in which the presolar molecular cloud remained partially mixed with the ISM, with a mixing timescale t mix . We find that the ESS abundances of 107 Pd and 182 Hf produced by slow neutron captures (s-process) and of 53 Mn and 60 Fe produced by explosive nucleosynthesis can be consistently explained within these scenarios. Their required tiso is 9–12 Ma and their required tmix is 11–14 Ma (with one potential exception of t mix = 38 Ma), depending on galactic uncertainties, such as the galactic star formation history and efficiency and the star-to-gas mass ratio. Another s -process SLR, 205 Pb, has a more uncertain ESS value and falls within only some of these time values. The same applies to the SLRs produced by the p -process ( 92 Nb and 146 Sm), depending on the latter’s half-life. In agreement with previous studies, we find that the ESS abundances of the rapid neutron-capture isotopes ( 129 I, 244 Pu, and 247 Cm) and of the most short-lived radionuclides ( 26 Al, 36 Cl, and 41 Ca) cannot be explained by assuming steady-state equilibrium in the ISM.

79 ASTRONOMY AND ASTROPHYSICS↗

Operation of helium sub-atmospheric multistage cryogenic centrifugal compressor trains: Part 1 – Steady state modeling and speed ratio selection

Helium cryogenic systems which can provide cooling below the normal boiling point of helium (approximately 4.2 K) are often required by superconducting radio-frequency niobium resonators utilized in modern high-energy particle accelerators. Achieving temperatures below 4.2 K generally involves operating a cryogenic vessel with liquid helium under sub-atmospheric conditions, thereby lowering the saturation pressure and corresponding saturation temperature. Over the last several decades, multi-stage cryogenic centrifugal compressor trains (CC’s) have been operated efficiently and reliably within large-scale cryogenic systems to continuously evacuate helium vapor generated by a device within the vessel, maintaining sub-atmospheric conditions in the vessel while pressurizing the return vapor to above atmospheric conditions. Traditionally, these CC systems have been operated using empirically derived control philosophies and insight gathered from previous operational experience. Recent efforts at the Facility for Rare Isotope Beams (FRIB) have been aimed at the development of a theoretical basis to characterize the operation of multi-stage cryogenic centrifugal compressor train and utilizing predictive model results to generate control parameters. The objective of this research was identifying operational points which adequately balance cryogenic system efficiency, stability, and overall ease of operation. Furthermore, this manuscript provides an overview of the predictive model development, characterization of the FRIB cryogenic centrifugal compressors and implementation of the predicted performance results during steady-state system operation.

Compressor train control↗

The role of ambient gas confinement, plasma chemistry, and focusing conditions on emission features of femtosecond laser-produced plasmas

Ultrafast laser ablation coupled with optical emission spectroscopy is currently under development for standoff detection of elements and their isotopes for a wide range of application areas. In this work, we explore the role of ambient air pressure during the interaction of an ultrafast laser beam with two metallic targets (brass and uranium) with significantly different oxygen gas-phase reactivity. Plasma plumes were generated by focusing ~800 nm, ~35 fs pulses from an ultrafast laser system using a long focal length lens with f = 1 m. Two-dimensional spectral imaging was performed over the pressure range of 30 mTorr-700 Torr air to evaluate emission dynamics, plasma chemistry, signal-to-background ratio, and characteristic parameters (i.e. excitation temperature, electron density). An increase in ambient air pressure during ultrafast laser ablation leads to plume confinement and subsequent changes in the emission dynamics due to plasma chemistry as well as changes in plasma generation conditions (i.e. focused fs laser ablation versus filament ablation). Ablation crater morphologies were also investigated via scanning electron microscopy. Results indicate atomic emission intensity and signal-to-background ratios peak at moderate pressure levels (~50-100 Torr air) for both targets studied, although plasma chemistry influences uranium emission signatures. The emission features of the uranium plasma at pressures = 10 Torr showed the presence of atoms and oxide molecules which are co-located within the plume. We also find filament ablation leads to wider, more shallow craters compared to focused laser ablation. Our study provides unique insight into the interplay between plume dynamics, confinement, and oxygen chemistry of fs laser-produced plasmas and how these phenomena evolve with changing ambient air pressure.

Laser-produced plasma↗