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At least 19 records

Hyperfine structures and isotopic shifts of uranium transitions using tunable laser spectroscopy of laser ablation plumes

We report isotopic shifts and hyperfine structures of selected U transitions employing tunable spectroscopy viz: laser-induced fluorescence and laser absorption spectroscopy of laser ablation plumes. The laser-produced plasmas were produced during ns laser ablation on a natural U metal which contains 0.7% 235U. Our results show that isotopic shifts between 238U and 235U are entangled with hyperfine structures of 235U. The isotopic ratio obtained using laser-induced fluorescence is affected by optical saturation effect. Time-resolved laser absorption spectroscopy is carried out for evaluating the optical absorption and estimating the hyperfine constants.

(020.3260) Isotope shifts↗

Modeling of transient interference phenomena in colinear laser spectroscopy

Colinear laser spectroscopy of fast atomic beams has been established as one of the main tools to perform precision experiments with atoms containing short-lived nuclei. Although highly sensitive, the spectral resolution of these techniques is typically limited to several MHz. Here, we study the use of transient interference phenomena to potentially improve the experimental resolution. Previous attempts to implement Ramsey-type measurements with fast beams were limited by the lack of understanding of the observed line shapes. Additionally, by using a simple model, we provide a satisfactory description of the previously observed line shapes and propose alternative experimental schemes to improve the resolution in fast ion-beam experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Intracavity laser spectroscopy with a semiconductor disk laser-pumped cw Cr{sup 2+} : ZnSe laser

Absorption spectra of the air have been measured near 2.31 μm using intracavity laser spectroscopy with a semiconductor disk laser-pumped cw Cr{sup 2+} : ZnSe laser. It is shown that, at lasing times of at least 3 ms, the sensitivity of the laser to intracavity absorption increases. This allows one to reach an effective path length of 900 km and enables detection of weak lines with absorption coefficients down to 1 × 10{sup -9} cm{sup -1}. (laser spectroscopy)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The influence of tillage and fertilizer on the flux and source of nitrous oxide with reference to atmospheric variation using laser spectroscopy

Nitrous oxide (N 2 O) is the third most important long-lived greenhouse gas and agriculture is the largest source of N 2 O emissions. Curbing N 2 O emissions requires understanding influences on the flux and sources of N 2 O. We measured flux and evaluated microbial sources of N 2 O using site preference ( S P ; the intramolecular distribution of 15 N in N 2 O) in flux chambers from a grassland tilling and agricultural fertilization experiments and atmosphere. We identified values greater than that of the average atmosphere to reflect nitrification and/or fungal denitrification and those lower than atmosphere as increased denitrification. Our spectroscopic approach was based on an extensive calibration with 18 standards that yielded S P accuracy and reproducibility of 0.7 ‰ and 1.0 ‰, respectively, without preconcentration. Chamber samples from the tilling experiment taken ~ monthly over a year showed a wide range in N 2 O flux (0–1.9 g N 2 O-N ha -1 d -1 ) and S P (- 1.8 to 25.1 ‰). Flux and S P were not influenced by tilling but responded to sampling date. Large fluxes occurred in October and May in no-till when soils were warm and moist and during a spring thaw, an event likely representing release of N 2 O accumulated under snow cover. These high fluxes could not be ascribed to a single microbial process as S P differed among chambers. However, the year-long S P and flux data for no-till showed a slight direct relationship suggesting that nitrification increased with flux. The comparative data in till showed an inverse relationship indicating that high flux events are driven by denitrification. Corn ( Zea mays ) showed high fluxes and S P values indicative of nitrification ~ 4 wk after fertilization with subsequent declines in S P indicating denitrification. Although there was no effect of fertilizer treatment on flux or S P in switchgrass ( Panicum virgatum) , high fluxes occurred ~1 month after fertilization. In both treatments, S P was indicative of denitrification in many instances, but evidence of nitrification/fungal denitrification also prevailed. At 2 m atmospheric N 2 O S P had a range of 31.1 ‰ and 14.6 ‰ in the grassland tilling and agricultural fertilization experiments, respectively. These data suggest the influence of soil microbial processes on atmospheric N 2 O and argue against the use of the global average atmospheric S P in isotopic modeling approaches.

Environmental Sciences & Ecology↗

Laser spectroscopy for the study of exotic nuclei

Investigation into the properties and structure of unstable nuclei far from stability is a key avenue of research in modern nuclear physics. These efforts are motivated by the continual observation of unexpected structure phenomena in nuclei with unusual proton-to-neutron ratios. In recent decades, laser spectroscopy techniques have made significant contributions in our understanding of exotic nuclei in different mass regions encompassing almost the entire nuclear chart. This is achieved through determining multiple fundamental properties of nuclear ground and isomeric states, such as nuclear spins, magnetic dipole and electric quadrupole moments and charge radii, via the measurement of hyperfine structures and isotope shifts in the atomic or ionic spectra of the nuclei of interest. These properties offer prominent tests of recently developed state-of-the-art nuclear theory and help to stimulate new developments in improving the many-body methods and nucleon–nucleon interactions at the core of these models. With the aim of exploring more exotic short-lived nuclei located ever closer to the proton and neutron driplines, laser spectroscopy techniques, with their continuous technological developments towards higher resolution and higher sensitivity, are extensively employed at current- and next-generation radioactive ion beam facilities worldwide. Ongoing efforts in parallel promise to improve the availability of these even more exotic species at next-generation facilities. Very recently, an innovative application of laser spectroscopy on molecules containing short-lived nuclei has been demonstrated offering additional opportunities for several fields of research, e.g. fundamental symmetry studies and astrophysics. Here, in this review, the basic nuclear properties measurable with laser spectroscopy will be introduced. How these observables are associated with nuclear structure and nucleon–nucleon interactions will be discussed. Following this, a general overview of different laser spectroscopy methods will be given with particular emphasis on technical advancements reported in recent years. The main focus of this article is to review the numerous highlights that have resulted from studying exotic nuclei in different mass regions with laser spectroscopy techniques since the last edition in this series. Finally, the challenges facing the field in addition to future opportunities will be discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Spectral line-shape in collinear laser spectroscopy after atomic charge exchange

Collinear laser spectroscopy experiments on fast, neutral beams have been extensively used for studies on short-lived radioactive nuclei, taking advantage of its high sensitivity. The resulting resonance line-shape is known to show significant distortion, due to the energy exchange during the charge-exchange neutralization process, which can cause large systematic uncertainty in the determined centroid. A model for the line shape was constructed and simulated to be compared to measured Al, Si, and Ni hyperfine spectra. It is shown that the distortion is caused mainly by the transfer of electron into many different energy levels in the projectile atom and subsequent decays, rather than secondary inelastic collisions, which were often assumed in the line shape analysis before. Furthermore, the model can also be applied to other projectile–alkali pairs, providing a reliable line-shape with less fitting parameters than conventional phenomenological models.

Atom↗

Laser spectroscopy of sub-micrometre- and micrometre-thick caesium-vapour layers

We present high resolution laser spectroscopy of Cs vapours confined in a unique optical cell of sub-micrometric and micrometric thickness, where a strong spatial anisotropy is present for the time of interaction between the atoms and laser radiation. Similarly to the spectra of selective specular reflection, the Doppler-free spectra of absorption and fluorescence are observed, not revealing cross-over resonances that will be useful for frequency stabilisation, provided the cell is cheap and compact. A new resonance in the fluorescence of closed transition is studied, demonstrating its high sensitivity to elastic atom – atom and atom – dielectric surface collisions. The theoretical modelling performed is in agreement with the experimental observations. (laser spectroscopy)

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Laser Spectroscopy of Exotic Atoms and Molecules Containing Octupole-Deformed Nuclei

This project investigated the nuclear, atomic, and molecular structure of exotic atoms and molecules containing actinide isotopes. These short-lived radioactive systems are challenging to produce and study in the laboratory, yet they offer unique opportunities for fundamental science. These nuclei are predicted to exhibit pear-shaped (octupole) deformation, a rare collective nuclear behavior that dramatically enhances their sensitivity to fundamental physics phenomena such as time-reversal- and parity-violating effects. Such enhancements make them ideal probes for exploring open questions in our understanding of the universe such as the origin of the matter–antimatter asymmetry of the universe. To realize these measurements, the project led the development of a new laser spectroscopy experiment at MIT, and later commissioned at the Facility for Rare Isotope Beams (FRIB) at Michigan State University: the Resonance Ionization Spectroscopy Experiment (RISE). RISE combines the spectroscopic precision of collinear laser spectroscopy with the sensitivity of particle-detection techniques, enabling measurements of rare isotopes produced at rates as low as a few ions per second. The beamline was designed, built, and installed, and was successfully commissioned at FRIB during the grant period. RISE is now a permanent capability of the FRIB facility, and has produced several results on the study of rare atoms and molecules for nuclear structure and fundamental symmetries. In parallel with the FRIB program, the project contributed to the first precision laser-spectroscopy measurements of short-lived radioactive molecules. Working with international collaborators at CERN's ISOLDE facility, the team conducted pioneering experiments on radium monofluoride (RaF) and actinium monofluoride (AcF). The results from this work have been published in major journals of science, including Nature, Science, Nature Physics, Nature Communications, and Physical Review Letters. These findings have guided future experiments on the laser cooling of radioactive molecules, opening a new platform for precision tests of fundamental symmetries.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Ultrafast laser spectroscopy in complex solid state materials

This thesis summarizes my work on applying the ultrafast laser spectroscopy to the complex solid state materials. It shows that the ultrafast laser pulse can coherently control the material properties in the femtosecond time scale. And the ultrafast laser spectroscopy can be employed as a dynamical method for revealing the fundamental physical problems in the complex material systems.

36 MATERIALS SCIENCE↗

High-Resolution Laser Spectroscopy on the Hyperfine Structure of 255Fm (𝑍=100)

We report on high-resolution laser spectroscopy of 255Fm (𝑇1/2=20 h), one of the heaviest nuclides available from reactor breeding. The hyperfine structures in two different atomic ground-state transitions at 398.4 nm and 398.2 nm were probed by in-source laser spectroscopy at the RISIKO mass separator in Mainz, using the perpendicularly illuminated laser ion source and trap (PI-LIST) high-resolution ion source. Experimental results were combined with hyperfine fields from various atomic ab initio calculations, in particular using multiconfiguration Dirac-Hartree-Fock theory, as implemented in grasp18. In this manner, the nuclear magnetic dipole and electric quadrupole moments were derived to be 𝜇=−0.75⁢(5) 𝜇N and 𝑄s=+5.84⁢(13) eb, respectively. The magnetic moment indicates occupation of the 𝜈⁢7/2⁢[613] Nilsson orbital, while the large quadrupole moment confirms strong, stable prolate deformation consistent with systematics in the heavy actinides. Comparisons with available expectation values from nuclear theory show good agreement, providing a stringent benchmark for the used theoretical models. These results revise earlier data and establish 255Fm as a reference isotope for future high-resolution studies.

Ezold, Julie [ORNL] (ORCID:0000000250550022)↗

A field programmable gate array-based time-resolved scaler for collinear laser spectroscopy with bunched radioactive potassium beams

A new data acquisition system including a Field Programmable Gate Array (FPGA) based time-resolved scaler was developed for laser-induced fluorescence and beam bunch coincidence measurements. The FPGA scaler was tested in a collinear laser-spectroscopy experiment on radioactive {sup 37}K at the BEam COoler and LAser spectroscopy (BECOLA) facility at the National Superconducting Cyclotron Laboratory at Michigan State University. A 1.29 μs bunch width from the buncher and a bunch repetition rate of 2.5 Hz led to a background suppression factor of 3.1 × 10{sup 5} in resonant photon detection measurements. The hyperfine structure of {sup 37}K and its isotope shift relative to the stable {sup 39}K were determined using 5 × 10{sup 4} s{sup −1} {sup 37}K ions injected into the BECOLA beam line. The obtained hyperfine coupling constants A({sup 2}S{sub 1/2}) = 120.3(1.4) MHz, A({sup 2}P{sub 1/2}) = 15.2(1.1) MHz, and A({sup 2}P{sub 3/2}) = 1.4(8) MHz, and the isotope shift δν{sup 39,} {sup 37} = −264(3) MHz are consistent with the previously determined values, where available.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Measurement of the absorption line profiles of water vapour isotopomers at 1.39 {mu}m using the methods of diode laser spectroscopy

The issues related to high-precision measurement of the absorption line profiles of water vapour and its isotopomers using the methods of diode laser spectroscopy in the near IR range aimed at the analysis and detection of greenhouse gases are considered. The absorption line shape of H{sub 2}{sup 16}O is investigated as a function of pressure of different buffer gases. The influence of the instrument function of the diode laser (DL) on the precision of measuring the line profile is studied. From fitting the profile of Doppler-broadened H{sub 2}{sup 16}O absorption line to a model profile the lasing line width of the DL with a fibre pigtail is determined. The frequencies and intensities of absorption lines of water isotopomers H{sub 2}{sup 16}O, H{sub 2}{sup 17}O, H{sub 2}{sup 18}O, and HDO are measured in the range of DL oscillation. Analytical spectral regions are chosen for distant probing of water vapour using an airborne lab. (laser spectroscopy)

74 ATOMIC AND MOLECULAR PHYSICS↗

Measurements of water molecule isotopomer concentrations in a discharge of inert gas with addition of H{sub 2}O and D{sub 2} vapours by the method of external-cavity diode laser spectroscopy

Discharge plasma in inert gases with added water vapours and deuterium is studied by using the optimised diode laser spectroscopy with an external cavity. Formation of a spectrally dense grid of cavity transverse mode eigenfrequencies allows one to determine the parameters of Doppler broadening for absorption lines, a kinetic temperature of molecules, and their statistical sums. By using these parameters and the value of an absorption coefficient, correlations of concentrations are found for H{sub 2}O and HDO isotopomers at various ratios of plasma-forming gas components. An important contribution of initial gas molecules adsorbed on walls into the formation of plasma composition is stressed. It is found that the ratio of H{sub 2}O and HDO concentrations is the same at various ratios of H{sub 2}O and D{sub 2} concentrations in plasma-forming gases and is constant during the discharge burning process. (laser applications and other topics in quantum electronics)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

A trap-based pulsed positron beam optimised for positronium laser spectroscopy

We describe a pulsed positron beam that is optimised for positronium (Ps) laser-spectroscopy experiments. The system is based on a two-stage Surko-type buffer gas trap that produces 4 ns wide pulses containing up to 5 × 10{sup 5} positrons at a rate of 0.5-10 Hz. By implanting positrons from the trap into a suitable target material, a dilute positronium gas with an initial density of the order of 10{sup 7} cm{sup −3} is created in vacuum. This is then probed with pulsed (ns) laser systems, where various Ps-laser interactions have been observed via changes in Ps annihilation rates using a fast gamma ray detector. We demonstrate the capabilities of the apparatus and detection methodology via the observation of Rydberg positronium atoms with principal quantum numbers ranging from 11 to 22 and the Stark broadening of the n = 2 → 11 transition in electric fields.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Photoacoustic-based detector for infrared laser spectroscopy

In this contribution, we present an alternative detector technology for use in direct absorption spectroscopy setups. Instead of a semiconductor based detector, we use the photoacoustic effect to gauge the light intensity. To this end, the target gas species is hermetically sealed under excess pressure inside a miniature cell along with a MEMS microphone. Optical access to the cell is provided by a quartz window. The approach is particularly suitable for tunable diode laser spectroscopy in the mid-infrared range, where numerous molecules exhibit large absorption cross sections. Moreover, a frequency standard is integrated into the method since the number density and pressure inside the cell are constant. We demonstrate that the information extracted by our method is at least equivalent to that achieved using a semiconductor-based photon detector. As exemplary and highly relevant target gas, we have performed direct spectroscopy of methane at the R3-line of the 2v{sub 3} band at 6046.95 cm{sup −1} using both detector technologies in parallel. The results may be transferred to other infrared-active transitions without loss of generality.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Toward the Development of Molten Salt Reactor Diagnostics based on Resonantly Enhanced Laser Spectroscopy

One emerging concern within the safeguards community is how to best ensure compliance with nuclear security regulations within molten salt reactor (MSR) facilities. This problem is nontrivial as molten salts used for fuel or coolant are highly corrosive, chemically complex, and inherently require high operational temperatures. Laser spectroscopy methods such as laser-induced breakdown spectroscopy (LIBS) and laser-induced fluorescence (LIF) have previously been suggested for molten salt diagnostics due to their compatibility with liquid phase samples and potential for in-situ measurements [1]. In the former, the laser is used to ionize the sample, allowing for the characteristic light from electronic de-excitation as the resultant plasma cools to be used for material characterization. In the latter, a tunable light source is set be resonant with a specific transition, resulting in element specific excitation and the emission of fluorescence light. In our previous work [2], we demonstrated that LIF could be used for the detection of fission fragments such as Nd in solution through the separation of laser scatter and fluorescence within the time domain. Here, we present progress towards two alternate measurement schemes: LIF measurements based on spectroscopic discrimination of fluorescence emissions and resonant LIBS measurements that induce plasma using a light source set to the resonant frequency of a specific electronic transition. Both methods aim to exploit resonant excitation methods to enhance the emitted signal. The studies may provide routes for element-specific detection of constituents within complicated matrices and a means to better understand the chemical behavior of lanthanides and actinides relevant to MSRs.

98 - NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL↗

Probing Sizes and Shapes of Nobelium Isotopes by Laser Spectroscopy

Until recently, ground-state nuclear moments of the heaviest nuclei could only be inferred from nuclear spectroscopy, where model assumptions are required. Here, laser spectroscopy in combination with modern atomic structure calculations is now able to probe these moments directly, in a comprehensive and nuclear- model-independent way. In this work, we reported on unique access to the differential mean-square charge radii of 252,253,254 No, and therefore to changes in nuclear size and shape. State-of-the-art nuclear density functional calculations describe well the changes in nuclear charge radii in the region of the heavy actinides, indicating an appreciable central depression in the deformed proton density distribution in 252,254 No isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗