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Recent advances in laser synthesis and processing of 2D materials are described that address key issues of scalable synthesis, precise heterogeneity control, and transformative manufacturing. Here, laser spectroscopy is used to remotely characterize and optimize the structure and functionality of 2D materials, enabling their in-situ diagnostic-based synthesis and processing.
The study of lipid molecular fossils by traditional biomarker analysis requires bulk sample crushing, followed by solvent extraction, and then the analysis of the extract by gas chromatography-mass spectrometry (GC–MS). This traditional analysis mixes all organic compounds in the sample regardless of their origins, with a loss of information on the spatial distribution of organic molecules within the sample. These shortcomings can be overcome using the chemical mapping of intact samples. Spectroscopic techniques such as UV fluorescence or Raman spectroscopy, laser ablation inductively coupled plasma mass spectrometry, and time-of-flight secondary ion mass spectrometry (ToF-SIMS) are among those elemental and molecular mapping techniques. This study employed femtosecond (fs) laser ablation combined with single-photon ionization, a method called fs-laser desorption postionization mass spectrometry (fs-LDPI-MS). In this work, a pulsed ~75 fs, 800 nm laser was used to ablate the geological sample, which was then photoionized after a few microseconds by a pulsed 7.9 eV vacuum ultraviolet laser. An organic carbon-rich geological sample was used for this study to map hydrocarbon biomarkers in sediments that were previously studied by GC–MS. The petrography of this sample was examined by optical and fluorescence microscopy. It is demonstrated here that fs-LDPI-MS combined with petrography for multimodal imaging can expose buried compounds within the sample via in situ layer removal. When used in conjunction with traditional organic geochemical analysis, this method has the potential to determine the spatial distribution of organic biomarkers in geological material. Finally, fs-LDPI-MS imaging data are compared with ToF-SIMS imaging that is commonly used for such studies.
Optical emission spectroscopy and laser absorption spectroscopy are two highly complementary techniques for diagnosing plasmas, specifically in the determination of important parameters such as temperature and density. In this work, we characterized a laser-produced plasma by combining emission and tunable absorption spectroscopy. Plasmas are produced by focusing pulses from a frequency quadrupled Nd:YAG laser onto a glass target containing a minor concentration of aluminum in an ambient atmosphere of ~100 Torr N 2 . Here, emission spectroscopy is used to investigate the line behavior of Al and Ca, electron density, and excitation temperature at times = 5 μs, while absorption spectroscopy is used to investigate the line behavior of Al and Ca, species density, and kinetic temperature at times = 5-100 μs. A comparison is made between the excitation temperature measured from emission using the Boltzmann plot method and the kinetic temperature measured from absorption; the implications of this comparison on local thermodynamic equilibrium and line-of-sight averaging are discussed. By combining the two methods of optical emission and laser absorption spectroscopy, a comprehensive characterization of the plasma over the entire lifetime of its evolution is possible, leading to a greater understanding of the plasma behavior including particle condensation.
We present the first results obtained from the S3 Low-Energy Branch, the gas cell setup at SPIRAL2-GANIL, which will be installed behind the S3 spectrometer for atomic and nuclear spectroscopy studies of exotic nuclei. The installation is currently being commissioned offline, with the aim to establish optimum conditions for the operation of the radio frequency quadrupole ion guides, mass separation and ion bunching, providing high-efficiency and low-energy spatial spread for the isotopes of interest. Transmission and mass-resolving power measurements are presented for the different components of the S3-LEB setup. In addition, a single-longitudinal-mode, injection-locked, pumped pulsed-titanium–sapphire laser system has been recently implemented and is used for the first proof-of-principle measurements in an offline laser laboratory. Laser spectroscopy measurements of erbium, which is the commissioning case of the S3 spectrometer, are presented using the 4f126s23H6→4f12(3H)6s6p optical transition.
Metal halide perovskites have emerged as promising materials for optoelectronic applications in the last decade. A large amount of effort has been made to investigate the interplay between the crystalline lattice and photoexcited charge carriers as it is vital to their optoelectronic performance. Among them, ultrafast laser spectroscopy has been intensively utilized to explore the charge carrier dynamics of perovskites, from which the local structural information can only be extracted indirectly. Here, we have applied a time-resolved X-ray diffraction technique to investigate the structural dynamics of prototypical two-dimensional lead-free halide perovskite Cs 3 Bi 2 Br 9 nanoparticles across temporal scales from 80 ps to microseconds. We observed a quick recoverable (a few ns) photoinduced microstrain up to 0.15% and a long existing lattice expansion (~a few hundred nanoseconds) at mild laser fluence. Once the laser flux exceeds 1.4 mJ/cm 2 , the microstrain saturates and the crystalline phase partially transfers into a disordered phase. This photoinduced transient structural change can recover within the nanosecond time scale. Furthermore, these results indicate that photoexcitation of charge carriers couples with lattice distortion, which fundamentally affects the dielectric environment and charge carrier transport.
Doubly excited autoionizing states of alkaline earth atoms are explored by multistep laser spectroscopy, which is precisely the inverse process to dielectronic recombination, the recombination of hot electron with ions via an autoionizing state. Dielectronic recombination is an important mechanism leading to power loss in high temperature plasmas. Measurements included the autoionization rates of atoms in zero field and in the presence of electric and magnetic fields, as might be encountered in a plasma. To mimic the effects of the rapidly varying fields of electron collisions measurements were made in the presence of microwave electric fields. These experiments are analogous to experiments conducted with combined high intensity infrared and vuv laser fields, In laser/microwave experiments the effects of laser pulse envelope timing relative to the microwave phase were explored extensively.
Prompt and delayed gamma-ray spectroscopy of the neutron-deficient, semi-magic isotope 187Pb has been performed using the recoil-decay and isomer-decay tagging techniques at the Argonne Gas-Filled Analyzer. A new 5.15(15)-mu s isomeric state at only 308 keV above the spherical 3/2 - ground state is identified and classified as a shape isomer. A strongly-coupled band is observed on top of the isomer, which is nearly identical to the one built on the prolate 7/2 - [514] Nilsson state in the isotone 185 Hg. Based on this similarity and on the result of the potential-energy surface calculations, the new isomer in 187 Pb is proposed to originate from the same configuration. The retarded character of the 308-keV (7/2( - )→ 3/2$_{gs}^{-}$ transition with a deduced B(E2) = 5.6(2) x 10 -4 W.u. can be well explained by the significant difference between the prolate parent and spherical daughter configurations, leading to the shape isomerism. The excitation energy of the isomer is surprisingly low, being roughly half of the excitation energies of the known 0 + intruder bandheads in the neighboring 186,188 Pb isotopes. The combined results of the present work and the previous alpha-decay and laser spectroscopy studies present evidence for triple shape coexistence at low energy in the negative-parity configurations of 187 Pb, which is well reproduced by the potential-energy surface calculations.
Increased absorption of optical materials arising from exposure to ionizing radiation must be accounted for to accurately analyze laser-induced breakdown spectroscopy (LIBS) data retrieved from high-radiation environments. We evaluate this effect on two examples that mimic the diagnostics placed within novel nuclear reactor designs. The analysis is performed on LIBS data measured with 1% Xe gas in an ambient He environment and 1% Eu in a molten LiCl-KCl matrix, along with the measured optical absorption from the gamma- and neutron-irradiated low-OH fused silica and sapphire glasses. Significant changes in the number of laser shots required to reach a 3σ detection level are observed for the Eu data, increasing by two orders of magnitude after exposure to a 1.7 × 1017 n/cm2 neutron fluence. For all cases examined, the spectral dependence of absorption results in the introduction of systematic errors. Moreover, if lines from different spectral regions are used to create Boltzmann plots, this attenuation leads to statistically significant changes in the temperatures calculated from the Xe II lines and Eu II lines, lowering them from 8000 ± 610 K to 6900 ± 810 K and from 15,800 ± 400 K to 7200 ± 800 K, respectively, for exposure to the 1.7 × 1017 n/cm2 fluence. The temperature range required for a 95% confidence interval for the calculated temperature is also broadened. In the case of measuring the Xe spectrum, these effects may be mitigated using only the longer-wavelength spectral region, where radiation attenuation is relatively small, or through analysis using the iterative Saha–Boltzmann method.
The aim of this whitepaper is to highlight the current capabilities and priorities of the US Heavy Element community and to provide the framework for a coordinated advancement of nuclear science from these studies. This is an organized effort to reflect on what has been achieved in the field given the recommendations and initiatives of the 2015 NSAC Long Range Plan, and on what can be realized in the next decade given current and possibly expanded investments. Current investments have positioned the US community to be among the world leaders in studies of the nuclear and chemical properties of the heaviest elements. These include studies of reaction mechanisms, moving us ever closer to the “island of stability”, in spectroscopy, allowing us to better understand nuclear structure at these extreme proton numbers, in chemical behavior, looking to determine how these elements should be placed on the Periodic Table, in performing the first measurements where isotopes are directly identified by their mass numbers, and in laying the foundation for a potential US-led new element discovery experiment. At present, the highest priority of the US Heavy Element community is to capitalize on the current investments by supporting the operations of US facilities at optimal values. These facilities include the Argonne Tandem Linac Accelerator System at Argonne National Laboratory and other Department of Energy facilities such as the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory, which has a dedicated superheavy element program, as well as university laboratories, including Texas A&M University. The High Flux Isotope Reactor at Oak Ridge National Laboratory is crucial to providing the radioactive isotopes required for heavy element science targets. This facility should be supported to provide the actinide materials that are essential for US-based science. Production of stable, rare isotopes for beam material, including 48 Ca, 50 Ti, 54 Cr and 58 Fe, at the Stable Isotope Production and Research Center is critical to continued research in heavy element science and should be a priority. The continued development of targets for heavy element science and retaining US-based expertise is critical for the heavy element community. This is an area that is currently under pressure. For example, the target laboratory at Argonne National Laboratory serves a broad community and is currently under threat due to loss of critical personnel. The skills needed to make targets for nuclear science and develop new targetry methods need to be supported long term at Argonne, Oak Ridge and Lawrence Livermore National Laboratories as well as maintaining the programs at Oregon State University and San José State University as vital pipelines for training students. Advances in theory are the foundation to understand how nuclei behave and to predict those behaviors in new circumstances. Progress in these studies will necessitate continued and new investment and access to high-performance computing. The future health of the heavy element field is dependent on the continuous support of talented early-career professionals at all levels. It is critical that opportunities continue to be created for the next generation to become established in heavy element research so that we can ensure the field is attracting and retaining the best minds for continued success. It is also clear that to ensure diversity of ideas, perspectives and techniques, we need to recruit diverse personnel that are trained at the best facilities. The heavy element community is in support of continued investment to programs with initiatives in diversity, equity, and inclusion. Looking to the next decade of research, support needs to maintain and grow US leadership in heavy element science. Specifically, new investments in state-of-the-art instrumentation will be essential to scientific development of the field and in expanding scientific knowledge. Advances in the next generation of electron cyclotron resonance ion sources, multi-reflection time-of-flight devices, laser spectroscopy, trapping methods and next generation alpha and gamma spectroscopy systems should be prioritized.
The primitive carbonaceous chondrites are of interest to cosmochemical science because they contain relatively large amounts of ‘water’ (H 2 O and/or OH – ) within phyllosilicate minerals. This water is evidence for the accretion of ices by their parent planetesimals, and thus represents an archive of the isotopic compositions of H 2 O in the protoplanetary environments. Here, in this study, we used thermogravimetry-enabled laser spectroscopy (TGA-IRIS) analyses of the Orgueil and Tagish Lake meteorites to make δ 2 H, δ 18 O, and Δ′ 17 O measurements of the H 2 O and OH – contained in the different hydrous minerals that comprise each meteorite. In Orgueil, we measured mass-weighted averages of OH – in the saponite and serpentine phyllosilicate matrix to be δ 2 H = 192 ‰, δ 18 O = 1.5 ‰, which are unquestionably of extraterrestrial origin with Δ′ 17 O = 1.0 ‰. For Tagish Lake, analogous values of OH– in the saponite and serpentine phyllosilicate matrix are δ 2 H = 704 ‰, δ 18 O = 11.3 ‰, and are similarly unambiguously extraterrestrial with Δ′ 17 O = 0.82 ‰. We estimate that the parent H 2 O involved in aqueous alteration of Orgueil had δ 18 O value ≥ +23 ‰. In Orgueil, we interpret the phyllosilicate petrographic relationships, and the δ 18 O values of OH – in saponite and serpentine to indicate that saponite formed first, at a lower temperature by 35 to 53 °C than serpentine. This suggests that the Orgueil parent body experienced increasing temperature during the phase of active aqueous alteration (prograde) which set the δ 18 O OH values of the serpentine and saponite. In the case of Tagish Lake, serpentine formed at a lower temperature by 32 to 60 °C than saponite, for the simplest case with constant δ 18 O H2O values. If serpentine formed first, followed by saponite formation at 32 to 60 °C °C higher temperature, this suggests that Tagish Lake sample TL1 underwent prograde aqueous alteration as the parent body heated up. We find evidence that the parent H 2 O for Orgueil, Tagish Lake sample TL1, and Murchison (based on data from a previous study) may have had Δ′ 17 O values of >0.64 ‰.
New mass values measured with the TITAN MR-TOF-MS are reported for the short-lived isotopes 24-26 Ne, produced at TRIUMF's ISAC facility using a uranium carbide target and cold FEBIAD ion source. A least-squares adjustment within the framework of the Atomic Mass Evaluation was performed and the improved precision of the new mass values is highlighted. The improved mass accuracy in this N = 14mid-shell region can also point to the refinement in values of the charge radii. By reducing the mass uncertainty of isotopes, their contribution of the mass shift uncertainty in laser spectroscopy can be negated. The work is part of developments for reaching the N = 20 Island of Inversion, where high molecular contamination hinders mass measurements of the neon isotopes.
Buffer-gas traps (BGTs) use inelastic interactions with nitrogen molecules to capture positrons from a continuous beam. These devices are invaluable for high-resolution studies of matter–antimatter interactions, antihydrogen research and positronium laser spectroscopy. We present a new project with the goal of producing a non-neutral plasma containing ${\sim }10^8$ low-energy positrons by installing a BGT on the NEPOMUC (NEutron induced POsitron source MUniCh) high-intensity positron beam. Details of the BGT are outlined and results are presented from experiments in which an electron beam, with a similar intensity and energy spread to the remoderated NEPOMUC beam, was used to create pulses of non-neutral electron plasma. The device is a vital component of the APEX (A Positron Electron eXperiment) project, which aims to create a low-temperature electron–positron pair plasma.
Betaine-30 (B30) was reported by Karl Dimroth and Christian Reichardt et al. in 1963 as a solvatochromic probe that can be easily synthesized, shows good solubility, and remains stable in various organic solvents and solutions. Its strongly negatively solvatochromic behavior arises from differential solvation between its electronic ground and excited states, making it a valuable tool for assessing solvent polarity using the E T (30) polarity scale, also devised by Dimroth and Reichardt. In addition, advancements in femtosecond laser spectroscopy in the 1990s greatly improved the understanding of B30’s relaxation dynamics following photoexcitation. In solvents capable of hydrogen bonding, such as alcohols, intermolecular hydrogen-bond rearrangement contributes to the multiple relaxation components observed. Since the 1990s, the applications of B30 have expanded beyond simple organic solvents to include complex solvent mixtures, such as electrolyte solutions for battery technologies and eutectic solvent mixtures. Furthermore, given the growing importance of these complex solvent mixtures, B30 is becoming an increasingly valuable tool for studying previously unexplored solvation properties.
As a powerful oxidant, atomic oxygen (O) holds considerable promise for a variety of biomedical and industrial applications. However, the inability to quantify solvated oxygen atoms has prevented the determination of the fundamental parameters governing its behaviour in relevant aqueous environments. Here, we directly image ground-state oxygen atoms in water using femtosecond two-photon absorption laser-induced fluorescence. Measurements show that oxygen atoms persist for tens of microseconds in water, penetrating hundreds of micrometres into the liquid. This observed longevity has significant implications, suggesting a need to re-evaluate existing models of solvated atomic oxygen reactivity and transport. Beyond atomic oxygen, this technique is broadly applicable to other solvated atomic species of interest, including nitrogen (N) and hydrogen (H). This work establishes that radical atomic species can be quantified in liquid with ultrafast laser spectroscopy, providing the basis for the determination of key properties including reaction rates, chemical lifetimes, and Henry’s law constants.
A new large-volume diamond anvil cell (DAC) has been developed for the Muon-catalyzed Fusion (μCF) Experiment (MuFusE), enabling the compression and heating of deuterium–tritium (d–t) mixtures to pressures and temperatures needed to advance μCF research. The MuFusE DAC achieves the large sample volumes necessary for high-precision fusion measurements while integrating cryogenic loading, all-metal sealing, and flexible bellows to maintain a secure environment during cell compression. Combined with remote pneumatic actuation and secondary containment, the DAC safely managed a 25 Ci tritium inventory while providing a clear optical path for in situ measurements of sample pressure and composition via laser spectroscopy. Utilizing 5 mm diameter diamond anvils oriented in the path of a high-intensity muon beam, the apparatus achieved a stable sample volume of 19.2 mm 3 at liquid density, pressures up to 933 MPa and temperatures up to 400 K—benchmarks that significantly exceed previously reported limits for static d–t targets.
We employed laser spectroscopy of atomic transitions to measure the nuclear charge radii and electromagnetic properties of the high-spin isomeric states in neutron-rich indium isotopes (𝑍 =49) near the closed proton and neutron shells at 𝑍 = 50 and 𝑁 = 82. Our data reveal a reduction in the nuclear charge radius and intrinsic quadrupole moment when protons and neutrons are fully aligned in 129 In (𝑁 = 80), to form the high spin isomer. Such a reduction is not observed in 127 In (𝑁 = 78), where more complex configurations can be formed by the existence of four neutron holes. These observations are not consistently described by nuclear theory.
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he nuclear root-mean-square charge radius of Ni 54 was determined with collinear laser spectroscopy to be R ( Ni 54 ) = 3.737 ( 3 ) fm . In conjunction with the known radius of the mirror nucleus Fe 54 , the difference of the charge radii was extracted as Δ R ch = 0.049 ( 4 ) fm . Based on the correlation between Δ R ch and the slope of the symmetry energy at nuclear saturation density ( L ), we deduced 21 ≤ L ≤ 88 MeV . The present result is consistent with the L from the binary neutron star merger GW170817, favoring a soft neutron matter EOS, and barely consistent with the PREX-2 result within 1 σ error bands. Our result indicates the neutron-skin thickness of Ca 48 as 0.15–0.21 fm.