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At least 595 records · Page 33

Probing and manipulating magnetic and 2D quantum materials using ultrafast laser and high harmonic sources

The ability to probe the full dynamic response of quantum materials on the length- and time-scales (Å to attoseconds on up) fundamental to charge, spin and phonon interactions is leading to a host of new discoveries. The coupled interactions between charges, spins, orbital and lattice degrees of freedom are key to determining the state of a material, whether metallic, insulating, superconducting or magnetic. Under thermal equilibrium conditions these states can be tuned by varying the temperature, pressure, chemical doping or dimensionality. However, their inherent complexity and rich phase landscape make them challenging to understand or manipulate deterministically. Fortunately, ultrafast light sources have undergone remarkable advances in recent years, achieving what was merely a dream three decades ago, i.e., full coherent control of light fields spanning the THz to the X-ray regions. Here, these new capabilities are providing powerful new tools for coherently manipulating and probing quantum materials using light. Recent advances in high harmonic generation (HHG) have provided new techniques for uncovering new phases and couplings in 2D and magnetic materials, using femtosecond lasers to coherently manipulate and tune the properties and interactions in the material, and HHG as a probe to map out these new phases and couplings. There are several beautiful recent observations of exciting new states in materials using light, but in some cases, the limited experimental data points made it challenging to validate an interpretation. The new ability of ultrafast HHG-based photoemission and magneto-optic spectroscopies to precisely probe multiple phases, electronic and magnetic order parameters, when combined with scanning the laser excitation fluence, is allowing us to map how material phases, magnetic states, and electron-phonon-spin couplings in these delicate materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Time-dependent equation-of-motion coupled-cluster simulations with a defective Hamiltonian

Here simulations of laser-induced electron dynamics in a molecular system are performed using time-dependent (TD) equation-of-motion (EOM) coupled-cluster (CC) theory. The target system has been chosen to highlight potential shortcomings of truncated TD-EOM-CC methods [represented in this work by TD-EOM-CC with single and double excitations (TD-EOM-CCSD)], where unphysical spectroscopic features can emerge. Specifically, we explore driven resonant electronic excitations in magnesium fluoride in the proximity of an avoided crossing. Near the avoided crossing, the CCSD similarity-transformed Hamiltonian is defective, meaning that it has complex eigenvalues, and oscillator strengths may take on negative values. When an external field is applied to drive transitions to states exhibiting these traits, unphysical dynamics are observed. For example, the stationary states that make up the time-dependent state acquire populations that can be negative, exceed one, or even complex-valued.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Resonance ionization mass spectrometry for isotopic abundance measurements

Resonance ionization mass spectrometry (RIMS) is a relatively new laser-based technique for the determination of isotopic abundances. The resonance ionization process depends upon the stepwise absorption of photons from the laser, promoting atoms of the element of interest through progressively higher electronic states until an ion is formed. Sensitivity arises from the efficiency of the resonant absorption process when coupled with the power available from commercial laser sources. Selectivity derives naturally from the distinct electronic structure of different elements. This isobaric discrimination has provided the major impetus for development of the technique. Resonance ionization mass spectrometry was used for analysis of the isotopic abundances of the rare earth lutetium. Isobaric interferences from ytterbium severely effect the ability to measure small amounts of the neutron-deficient Lu isotopes by conventional mass spectrometric techniques. Resonance ionization for lutetium is performed using a continuous-wave laser operating at 452 nm, through a sequential two-photon process, with one photon exciting the intermediate resonance and the second photon causing ionization. Ion yields for microgram-sized quantities of lutetium lie between 10(6) and 10(7) ions per second, at overall ionization efficiencies approaching 10(-4). Discrimination factors against ytterbium greater than 10(6) have been measured. Resonance ionization for technetium is also being explored, again in response to an isobaric interference, molybdenum. Because of the relatively high ionization potential for Tc, three-photon, two-color RIMS processes are being developed.

Miller, C. M.↗

Controlled Assembly of Upconverting Nanoparticles for Low-Threshold Microlasers and Their Imaging in Scattering Media

Micron-sized lasers fabricated from upconverting nanoparticles (UCNP) coupled to whispering gallery mode (WGM) microresonators can exhibit continuous-wave anti-Stokes lasing useful for tracking cells, environmental sensing, and coherent stimulation of biological activity. The integration of these microlasers into organisms and microelectronics requires even smaller diameters, however, which raises threshold pump powers beyond practical limits for biological applications. To meet the need for low lasing thresholds and high fidelity fabrication methods, we use correlative optical and electron microscopy to uncover the nanoparticle assembly process and structural factors that determine efficient upconverted lasing. We show that 5 μm microspheres with controlled submonolayer UCNP coatings exhibit, on average, 25-fold lower laser thresholds (1.7 ± 0.7 kW/cm 2 ) compared to the mean values of the lowest threshold UCNP lasers, and variability is reduced 30-fold. WGMs are observed in the upconversion spectra for TiO 2 -coated microspheres as small as 3 μm, a size at which optical losses had previously prevented such observations. Finally, we demonstrate that the WGM signatures of these upconverting microlasers can be imaged and distinguished through tissue-mimicking phantoms. These advances will enable the fabrication of more efficient upconverting lasers for imaging, sensing, and actuation in optically complex environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Laser-induced graphitization of polydopamine leads to enhanced mechanical performance while preserving multifunctionality

Polydopamine (PDA) is a simple and versatile conformal coating material that has been proposed for a variety of uses; however in practice its performance is often hindered by poor mechanical properties and high roughness. Here, we show that blue-diode laser annealing dramatically improves mechanical performance and reduces roughness of PDA coatings. Laser-annealed PDA (LAPDA) was shown to be >100-fold more scratch resistant than pristine PDA and even better than hard inorganic substrates, which we attribute to partial graphitization and covalent coupling between PDA subunits during annealing. Moreover, laser annealing provides these benefits while preserving other attractive properties of PDA, as demonstrated by the superior biofouling resistance of antifouling polymer-grafted LAPDA compared to PDA modified with the same polymer. Our work suggests that laser annealing may allow the use of PDA in mechanically demanding applications previously considered inaccessible, without sacrificing the functional versatility that is so characteristic of PDA.

36 MATERIALS SCIENCE↗

Fiber Laser Development for LISA

We have developed a linearly-polarized Ytterbium-doped fiber ring laser with single longitudinal-mode output at 1064nm for LISA and other space applications. Single longitudinal-mode selection was achieved by using a fiber Bragg grating (FBG) and a fiber Fabry-Perot (FFP). The FFP also serves as a frequency-reference within our ring laser. Our laser exhibits comparable low frequency and intensity noise to Non-Planar Ring Oscillator (NPRO). By using a fiber-coupled phase modulator as a frequency actuator, the laser frequency can be electro-optically tuned at a rate of 100kHz. It appears that our fiber ring laser is promising for space applications where robustness of fiber optics is desirable.

Numata, Kenji↗

Adaptive system for wavefront correction of the PEARL laser facility

The results of the operation of a wavefront correction system based on a deformable bimorph mirror of the PEARL subpetawatt laser facility are presented. An improvement in the quality of focusing of laser radiation, which led to an increase in the Strehl ratio from 0.3 to 0.6, is demonstrated. The features of the compensation for phase distortions of the wavefront in the case of a low pulse repetition rate, as well as the correct allowance for the noise of the CCD camera when calculating the Strehl ratio are investigated. (paper)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Laser-Pulse/Fiber-Optic Liquid-Leak Detector

Several potential leak sites monitored using single sensing fiber. Fluid systems monitored quickly for leaks in remote, hazardous, or inaccessible locations by system of compact, lightweight fiber-optic leak sensors presently undergoing development. Sensors installed at potential leak sites as joints, couplings, and fittings. Sensor read by sending laser pulse along fiber, then noting presence or relative amplitude of return pulse. Leak-monitoring technique applicable to wide range of fluid systems and minimizes human exposure to toxic or dangerous fluids.

Padgett, M. E.↗

Particle-in-cell Monte Carlo-collision modeling of non-ideal effects in wave-heated dense microplasmas

A computational model for non-ideal plasma effects during the time evolution of a second-stage laser-heated discharge at high pressures is presented. The model extends a classical one-dimensional particle-in-cell Monte Carlo-collision (PIC-MCC) approach coupled with Maxwell's equations for the laser-heating process of a xenon plasma at 300 K temperature and 10–100 bar pressure. Plasma non-ideality resulting from Coulomb coupling at high plasma densities is manifested as a depression in the effective ionization potential of atoms and enhanced collision cross sections. These non-ideal effects are represented using the Ecker–Kröll model in the context of the PIC-MCC approach. We find that full ionization of the plasma is obtained on the picosecond timescale, starting from the skin layer and quickly expanding throughout the domain through an anomalous extension of the skin depth. More critically, we show that the inclusion of the non-ideal plasma effects results in more rapid ionization compared to an ideal plasma, especially at higher pressures. The ionization delay reduction is of the order of a fraction of a picosecond, corresponding to a 16% decrease at 100 bar. As the amplitude of the wave field is lowered, the ionization rate is lowered, making the plasma non-ideality effects more prominent.

Solmaz, Evrim (ORCID:0000000211830881)↗

Plasma Emission, Wave Speeds, and Temperatures of Laser-Supported Plasmas in Air

A study of the generation and subsequent expansion of plasmas using a single beam (532 nm) from the second harmonic generator of a Q-switched Nd:YAG laser is described. The plasmas in air are studied using an intensified charge-coupled device camera over periods of 1000 ns following the laser pulses. The plasma experimental results are interpreted in terms of wave speeds and plasma temperatures. Energy balance equations are considered to estimate the plasma temperatures and the laser-supported radiation (LSR) and the laser-supported detonation (LSD) wave speeds. Within 1000 ns observation time, the circular spectral images turn elliptical because of plasma expansion toward the laser beam. The plasma expansion increases with increasing laser irradiance. A laser irradiance range of [Formula: see text] yields LSR wave speeds between 45 and 170 km/s and LSD wave speeds of 90–130 km/s. The measured wave speeds are compared with the LSR and the LSR wave speed models. The plasma temperatures are between 90,000 and 120,000 K at 15 ns after the laser pulse based on measured emission spectra and are between 640,000 and 760,000 K at 3 ns based on the LSR model.

Engineering↗

SO3/H2SO4 continuous real-time sensor demonstration at a power plant

We present results from field testing of a new, innovative sensor developed to measure SO3/H2SO4 continuously and in real time at a coal-fired power plant. The system utilizes the sensitivity, specificity, and real-time capabilities of mid-infrared (Mid-IR) laser-based sensor technology, along with a heated, close-coupled cell mounted directly to a power plant duct. Measurements were made by the laser sensor over a 2-day period and compared to results from the accepted method, EPA 8A, which requires a 30-minute collection, labor intensive processing, and off-site analysis at a lab. In contrast to the condensation method, the laser sensor continuously samples flue gas and reports measurements of the concentration of SO3/H2SO4, SO2 ever second with unattended operation. This initial demonstration proved the sensor concept and paves the way for its use for optimizing sorbent injection used to neutralize SO3/H2SO4. Optimized sorbent injection will enable significant cost savings associated with efforts to mitigate the presence and effects of SO3/H2SO4 such as “Blue Plume”, air heater fouling, and duct corrosion. In particular, the real-time, actionable information will enable better control of additive injection in flex conditions and variable fuels.

20 FOSSIL-FUELED POWER PLANTS↗

Coating adhesion of a chromate-containing epoxy primer on Al2024-T3 surface processed by laser-interference

In this work, the coating adhesion test results are presented for a primer that was coated on laser-interference structured surfaces of as-received Al2024-T3 specimens, i.e., without employing any polishing, cleaning, or any other surface alteration techniques. All of the laser-interference processing was performed by splitting the primary beam of a Q-switched Nd:YAG pulsed nanosecond laser into two beams and focused them to the same spot. The specimens were spray painted with a chromate-containing epoxy primer, CA7233, compliant to MIL-PRF-23377 Type I Class C2 specification. The adhesion of primer on Al surface with different treatments was assessed using the ASTM D3359 X-cut and cross-hatch tests. It was found that the laser processed specimens meet the performance requirements in the coating adhesion specifications by having a higher or identical ranking for coating adhesion specimens than those prepared with current state-of-the-art chemical conversion or sulfuric acid anodizing. The rastering with either 4 mm/s or 6 mm/s with a laser fluence of 1.78 J/cm2 is recommended to attain acceptable coating adhesion, even higher than that with the anodizing surface treatment.These results indicate that laser-interference shows significant potential as a non-chemical surface preparation technique for these coatings.

36 MATERIALS SCIENCE↗

The influence of water, diet, and temperature on 87 Sr/ 86 Sr in fin spines of juvenile Atlantic Sturgeon Acipenser oxyrinchus oxyrinchus

Analysis of microchemistry in fish fin spines offers a non-lethal approach to address key questions relating to spatial patterns and habitat use of fish. Reconstruction of life history is based on chemical changes within calcified structures with an underlying assumption of elemental incorporation relative to environmental concentration. However, information is limited on the relative influence of water and diet concentrations of elements to corresponding concentrations within fin spines. Strontium (Sr) is commonly used in trace element studies because of its predictable changes within watersheds, with recent applications showing utility of 87 Sr/ 86 Sr for greater spatial resolution. Therefore, this study evaluated the influence of water and diet 87 Sr/ 86 Sr on pectoral fin spines of Atlantic Sturgeon A. oxyrinchus oxyrinchus in controlled laboratory experiments. In the first experiment, fish were exposed to a control, water spiked with 0.10 mg/L of 87 Sr or diet spiked with 0.25 µg/g or 0.50 µg/g of 87 Sr in replicated tanks for 12 weeks. In a second experiment, to determine the time duration required to occupy a different environment for fin spine chemistry to change, fish were maintained in water- or diet-spiked treatments for 1, 2, 3, or 6 weeks. Additionally, to determine if temperature has an influence on 87 Sr/ 86 Sr in fin spines, fish were held at 15 and 25°C for 12 weeks. Fin spines were analyzed using laser ablation multi-collector inductively coupled plasma mass spectrometry (LA-MC-ICP-MS), and water and diet samples were analyzed using solution based ICP-MS. Results from Experiment 1 indicate water is the primary contributor and diet a secondary contributor of 87 Sr/ 86 Sr in pectoral fin spines of Atlantic Sturgeon. Results from Experiment 2 indicate fin spine 87 Sr/ 86 Sr can be influenced by water after 1 week and diet after 12 weeks. Additionally, although sample size was limited (n=3), water temperature did not have an effect on 87 Sr/ 86 Sr fin spine chemistry. In conclusion, these results provide guidance for interpretation of 87 Sr/ 86 Sr in pectoral fin spines of sturgeon and indicate usefulness of the technique for retrospectively estimating movement and habitat use.

59 BASIC BIOLOGICAL SCIENCES↗

Direct Observation of Shock‐Induced Disordering of Enstatite Below the Melting Temperature

Abstract We report in situ structural measurements of shock‐compressed single crystal orthoenstatite up to 337 ± 55 GPa on the Hugoniot, obtained by coupling ultrafast X‐ray diffraction to laser‐driven shock compression. Shock compression induces a disordering of the crystalline structure evidenced by the appearance of a diffuse X‐ray diffraction signal at nanosecond timescales at 80 ± 13 GPa on the Hugoniot, well below the equilibrium melting pressure (>170 GPa). The formation of bridgmanite and post‐perovskite have been indirectly reported in microsecond‐scale plate‐impact experiments. Therefore, we interpret the high‐pressure disordered state we observed at nanosecond scale as an intermediate structure from which bridgmanite and post‐perovskite crystallize at longer timescales. This evidence of a disordered structure of MgSiO 3 on the Hugoniot indicates that the degree of polymerization of silicates is a key parameter to constrain the actual thermodynamics of shocks in natural environments.

Hernandez, J. ‐A.↗

Floquet engineering of Kitaev quantum magnets

Abstract In recent years, there has been an intense search for materials realizing the Kitaev quantum spin liquid model. A number of edge-shared compounds with strong spin-orbit coupling, such as RuCl 3 and iridates, have been proposed to realize this model. Nevertheless, an effective spin Hamiltonian derived from the microscopic model relevant to these compounds generally contains terms that are antagonistic toward the quantum spin liquid. This is consistent with the fact that the zero magnetic field ground state of these materials is generally magnetically ordered. It is a pressing issue to identify protocols to drive the system to the limit of the Kitaev quantum spin model. In this work, we propose Floquet engineering of these Kitaev quantum magnets by coupling materials to a circularly polarized laser. We demonstrate that all the magnetic interactions can be tuned in situ by the amplitude and frequency of the laser, hence providing a route to stabilize the Kitaev quantum spin liquid phase.

36 MATERIALS SCIENCE↗

MeV x-ray production from a petawatt laser in the regime of a relativistically transparent preplasma, with applications to radiography

Bright sources of mega-electron volt (MeV) x-rays have many unique applications, including nuclear physics, radiation oncology, and imaging high areal density systems. High intensity lasers (>1018 W cm−2) incident on mm-thick metal targets can deliver MeV x-rays via the bremsstrahlung process, providing sources with ultrashort duration (∼ps) and small source size (∼100 μm). Here, we report on a reproducible regime of laser-driven MeV x-ray sources, where the x-ray dose can be further increased by 60% by coating the metal target with micrometers of plastic. High fidelity numerical simulations indicate that the interaction is a result of relativistic transparency in the preplasma. Though relativistic transparency is present in both cases, the greater sound speed and smaller ion inertia of the plastic target allow the laser to more deeply penetrate and couple more efficiently to electrons. Radiography with this system demonstrates a resolving power < 300 μm, important for imaging applications.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Cryogenically enhanced quasi-optical resonator for megawatt pulsed millimeter-wave sources

We report the design, cryogenic optimization, and performance modeling of a compact quasi-optical ring resonator intended to compress microwaves pulses at 170 and 250 GHz to the megawatt level. By combining ultra-low-loss CVD diamond and gold-doped silicon wafers with high-RRR copper mirrors, the calculated unloaded quality factor exceeds 4.3 × 10 5 at 20 K and yields simulated gains up to $\mathscr{G}$ = 4.1 × 10 3 . Coupling the resonator with a laser-driven semiconductor switch described by an extended Vogel model shows that 1 MW, nanosecond pulses can be generated from only 445 W of microwave drive power while dissipating 272 W into the cryostat. A practical cooling architecture using two Gifford–McMahon stages (20 and 80 K) is proposed, demonstrating that high-repetition-rate (10–20 kHz) operation is feasible with commercially available cryocoolers. The results outline a clear path toward cost-effective, table-top sources for extreme-ultraviolet lithography, dynamic nuclear polarization, and fusion systems.

Panisset, Constant [Ecole Polytechnique Federale L↗