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At least 73 records · Page 4

In-situ investigation of the vibrational properties of H 2 O CO 2 -bearing and dry K-rich basaltic glasses at high pressure by mid infrared spectroscopy

Here, the vibrational properties of CO 2 –H 2 O-bearing and dry synthetic K-rich basaltic glasses were investigated at room temperature and pressures between 0.0001–5.5 GPa using the diamond anvil cell combined with in situ reflectance and transmittance Fourier Transform infrared micro-spectroscopy. The absorption coefficient a(v) calculated from the Kramers-Kronig relation shows that glasses are dominated by the Q 2 aluminosilicate unit followed by Q 1 , Q 3 . The variation in Q n concentration upon compression suggests that glasses undergo polymerization from ambient pressure to 2 GPa followed by less marked structural changes up to 4 GPa, above which the structure is further polymerized. Once decompressed, glasses retained a polymerized structure. Our results show that 1.03 wt% CO 2 -1.42 wt% H 2 O in a glass with 3.10 wt% K 2 O and 46.77 wt% SiO 2 prevent the formation of fully polymerized connections when cold-compressed. Our results can be used to explain the effect of volatiles and alkali on the rheology of natural basaltic magmas.

36 MATERIALS SCIENCE↗

The CLAS12 Forward Tagger

This document presents the technical layout and the performance of the CLAS12 Forward Tagger (FT). The FT, composed of an electromagnetic calorimeter based on PbWO$_4$ crystals (FT-Cal), a scintillation hodoscope (FT-Hodo), and several layers of Micromegas trackers (FT-Trk), has been designed to detect electrons and photons scattered at polar angles from 2$^\circ$ to 5$^\circ$ and to meet the physics goals of the hadron spectroscopy program and other experiments running with the CLAS12 spectrometer in Hall B.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Laser-Plasma Spatiotemporal Cyanide Spectroscopy and Applications

This article reports new measurements of laser-induced plasma hypersonic expansion measurements of diatomic molecular cyanide (CN). Focused, high-peak-power 1064 nm Q-switched radiation of the order of 1 TW/cm 2 generated optical breakdown plasma in a cell containing a 1:1 molar gas mixture of N 2 and CO 2 at a fixed pressure of 1.1 × 10 5 Pascal and in a 100 mL/min flow of the mixture. Line-of-sight (LOS) analysis of recorded molecular spectra indicated the outgoing shockwave at expansion speeds well in excess of Mach 5. Spectra of atomic carbon confirmed increased electron density near the shockwave, and, equally, molecular CN spectra revealed higher excitation temperature near the shockwave. Results were consistent with corresponding high-speed shadowgraphs obtained by visualization with an effective shutter speed of 5 nanoseconds. In addition, LOS analysis and the application of integral inversion techniques allow inferences about the spatiotemporal plasma distribution.

36 MATERIALS SCIENCE↗

457-nm radiation source based on a diode laser for precision spectroscopy of magnesium atoms

We report on the development of a highly stable source of 457-nm radiation based on a diode laser and a tapered amplifier operating in a double-pass scheme. The diode laser frequency was stabilised by a high-Q reference Fabry – Perot interferometer and doubled in a PPSLT nonlinear crystal placed in an enhancement cavity. At a maximum output power of 200 mW at a wavelength of 457 nm, the laser linewidth was less than 5 kHz. The radiation source operation was demonstrated in experiments on precision spectroscopy of cold magnesium atoms in a magneto-optical trap. (lasers)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Optical Spin Polarization of a Narrow‐Linewidth Electron‐Spin Qubit in a Chromophore/Stable‐Radical System

Abstract Photoexcited organic chromophores appended to stable radicals can serve as qubit and/or qudit candidates for quantum information applications. 1,6,7,12‐Tetra‐(4‐ tert ‐butylphenoxy)‐perylene‐3,4 : 9,10‐bis(dicarboximide) (tpPDI) linked to a partially deuterated α,γ‐bisdiphenylene‐β‐phenylallyl radical (BDPA‐ d 16 ) was synthesized and characterized by time‐resolved optical and electron paramagnetic resonance (EPR) spectroscopies. Photoexcitation of tpPDI‐BDPA‐ d 16 results in ultrafast radical‐enhanced intersystem crossing to produce a quartet state ( Q ) followed by formation of a spin‐polarized doublet ground state ( D 0 ). Pulse‐EPR experiments confirmed the spin multiplicity of Q and yielded coherence times of T m =2.1±0.1 μs and 2.8±0.2 μs for Q and D 0 , respectively. BDPA‐ d 16 eliminates the dominant 1 H hyperfine couplings, resulting in a single narrow line for both the Q and D 0 states, which enhances the spectral resolution needed for good qubit addressability.

Qiu, Yunfan↗

Stability of beta-induced Alfvén eigenmodes (BAE) in DIII-D

Although the stability of ellipticity, toroidal and reversed-shear Alfvén eigenmodes (EAE, TAE, RSAE) are relatively well understood, less is known about the stability of lower-frequency modes such as the beta-induced Alfvén eigenmode (BAE) but, because they are often unstable in present devices and are implicated in fast-ion transport, understanding their stability is vital. BAE stability is studied in primarily weak or reversed shear DIII-D plasmas with sub-Alfvénic deuterium beams. Modes are classified based on electron cyclotron emission, beam emission spectroscopy, magnetics, and interferometer data. The study is limited to the initial two seconds of the discharge, where the evolving q profile provides an effective scan of the dependence of stability upon q. In a dedicated experiment, BAEs are unstable at times in the discharge when the minimum of the safety factor q min is close to a rational number. The observed mode frequencies are usually close to analytic estimates of the BAE accumulation point and the eigenfunction peaks in the vicinity of q min . Unstable BAEs usually occur in bursts that chirp rapidly in frequency. To isolate the importance of thermal and beam gradients in driving the modes, the beam and electron cyclotron heating power is altered for 50–100 ms durations in reproducible discharges. As expected from the resonance condition, BAEs depend sensitively on the beam power and injection geometry. Modes only persist for ~25 ms because the anisotropic beam population only interacts strongly with the modes over a relatively narrow range of q. Lastly, a database of over 1000 beam-heated discharges shows that BAEs are more likely to be unstable when the poloidal beta exceeds 0.5.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Sequential order dependent dark-exciton modulation in bi-layered TMD heterostructure

We report the emergence of dark-excitons in transition-metal-dichalcogenide (TMD) heterostructures that strongly rely on the stacking sequence, i.e., momentum-dark K-Q exciton located exclusively at the top layer of the heterostructure. The feature stems from band renormalization and is distinct from those of typical neutral excitons or trions, regardless of materials, substrates, and even homogeneous bilayers, which is further confirmed by scanning tunneling spectroscopy. To understand the unusual stacking sequence, we introduce the excitonic Elliot formula by imposing strain exclusively on the top layer that could be a consequence of the stacking process. We further find that the intensity ratio of Q- to K-excitons in the same layer is inversely proportional to laser power, unlike for conventional K-K excitons. This can be a metric for engineering the intensity of dark K-Q excitons in TMD heterostructures, which could be useful for optical power switches in solar panels.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Origin of light-induced metastability in ZrTe 5

Here we study the nonequilibrium electronic structure of a model Dirac semimetal ZrTe 5 by using time-and-angle resolved photoemission spectroscopy and density functional theory–based electron and phonon calculations. By measuring the electronic dispersion near the Γ point at time delays up to 10 picoseconds, we discovered that the band spectral weight does not recover during the measured temporal window, revealing the existence of a light-induced metastable state in the electronic structure of this material. Our calculations find that the photoexcited A 1⁢g phonon mode leads to a band renormalization that both supports our experimental observations at the zone center and predicts changes to the band structure outside of our experimental window, ultimately showing the evolution from a direct to an indirect gap semimetal; such band renormalization dramatically reduces the electron-hole recombination rate giving rise to the metastability in this system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Consistency between reflection momentum-resolved electron energy loss spectroscopy and optical spectroscopy measurements of the long-wavelength density response of Bi 2 Sr 2 CaCu 2 O 8 + x

The density fluctuation spectrum captures many fundamental properties of strange metals. Using momentum-resolved electron energy-loss spectroscopy (M-EELS), we recently showed that the density response of the strange metal Bi 2 Sr 2 CaCu 2 O 8+x (Bi-2212) at large momentum, q, exhibits a constant-in-frequency continuum reminiscent of the marginal Fermi liquid (MFL) hypothesis of the late 1980s. However, reconciling this observation with infrared (IR) optics experiments, which show a well-defined plasmon excitation at q ~ 0, has been challenging. Here we report M-EELS measurements of Bi-2212 using 4× improved momentum resolution, allowing us to reach the optical limit. For momenta q < 0.04 r.l.u., the M-EELS data show a plasmon feature that is quantitatively consistent with IR optics. For q > 0.04 r.l.u., the spectra become incoherent with an MFL-like, constant-in-frequency form. Here we speculate that, at finite frequency, ω, and nonzero q, some attribute of this Planckian metal randomizes the probe electron, causing it to lose information about its own momentum.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Terahertz Chiral Metamaterials Enabling Broadband Polarization Conversion Using Polarization Guiding Effect

Polarization control plays a vital role in terahertz (THz) photonics, enabling a wide range of applications from imaging and spectroscopy to sensing and wireless communication. However, conventional polarization control methods at THz frequencies are limited by narrow operational bandwidths and excessive absorption losses. In this work, we present a broadband THz polarization control based on the polarization guiding effect. We design and fabricate a THz polarization rotator capable of rotating incident linear polarization by 90°. The device consists of 24 twistingly stacked silicon–air metagrating layers that introduce a large degree of form birefringence, with each metagrating layer being 280 µm thick and sequentially twisted by 3.75°. Numerical simulations using the Berreman 4 × 4 method predict broadband operation of the device. Experimental validation using THz time-domain spectroscopy confirms efficient and broadband 90° polarization rotation from 0.2 to 1.25 THz. Based on this concept, we further propose THz Q-plates for the generation of broadband structured vector beams with radial and azimuthal polarization states. This work offers a scalable, material-agnostic platform for advanced THz polarization manipulation and vector beam engineering, opening new pathways for next-generation THz photonic devices.

36 MATERIALS SCIENCE↗

Charge separation in the photosystem II reaction center resolved by multispectral two-dimensional electronic spectroscopy

The photosystem II reaction center (PSII RC) performs the primary energy conversion steps of oxygenic photosynthesis. While the PSII RC has been studied extensively, the similar time scales of energy transfer and charge separation and the severely overlapping pigment transitions in the Qy region have led to multiple models of its charge separation mechanism and excitonic structure. Here, we combine two-dimensional electronic spectroscopy (2DES) with a continuum probe and two-dimensional electronic vibrational spectroscopy (2DEV) to study the cyt b559-D1D2 PSII RC at 77 K. This multispectral combination correlates the overlapping Qy excitons with distinct anion and pigment-specific Q x and mid-infrared transitions to resolve the charge separation mechanism and excitonic structure. Through extensive simultaneous analysis of the multispectral 2D data, we find that charge separation proceeds on multiple time scales from a delocalized excited state via a single pathway in which Pheo D1 is the primary electron acceptor, while Chl D1 and P D1 act in concert as the primary electron donor.

30 DIRECT ENERGY CONVERSION↗

Signatures of van Hove singularities in the anisotropic in-plane optical conductivity of the topological semimetal Nb 3 ⁢SiTe 6

In this work, we present a temperature-dependent infrared spectroscopy study on the layered topological semimetal Nb 3 ⁢SiTe 6 combined with density-functional theory calculations of the electronic band structure and optical conductivity. Our results reveal an anisotropic behavior of the in-plane (ac-plane) optical conductivity, with three pronounced excitations located at around 0.15, 0.28, and 0.41 eV for the polarization of the incident radiation along the c axis. These excitations are well reproduced in the theoretical spectra. Based on the ab initio results, the excitations around 0.15 and 0.28 eV are interpreted as fingerprints of van Hove singularities in the electronic band structure and compared to the findings for other topological semimetals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Rheology and dynamics of a solvent segregation driven gel (SeedGel)

Bicontinuous structures promise applications in a broad range of research fields, such as energy storage, membrane science, and biomaterials. Kinetically arrested spinodal decomposition is found responsible for stabilizing such structures in different types of materials. A recently developed solvent segregation driven gel (SeedGel) is demonstrated to realize bicontinuous channels thermoreversibly with tunable domain sizes by trapping nanoparticles in a particle domain. As the mechanical properties of SeedGel are very important for its future applications, a model system is characterized by temperature-dependent rheology. The storage modulus shows excellent thermo-reproducibility and interesting temperature dependence with the maximum storage modulus observed at an intermediate temperature range (around 28 °C). SANS measurements are conducted at different temperatures to identify the macroscopic solvent phase separation during the gelation transition, and solvent exchange between solvent and particle domains that is responsible for this behavior. Further, the long-time dynamics of the gel is further studied by X-ray Photon Correlation Spectroscopy (XPCS). The results indicate that particles in the particle domain are in a glassy state and their long-time dynamics are strongly correlated with the temperature dependence of the storage modulus.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of TMAO as co-solvent on the gelation of silica-PNIPAm core-shell nanogels at intermediate volume fractions

We study the structure and dynamics of poly(N-isopropylacrylamide) (PNIPAm) core-shell nanogels dispersed in aqueous trimethylamine N-oxide (TMAO) solutions by means of smallangle X-ray scattering and X-ray photon correlation spectroscopy (XPCS). Upon increasing the temperature above the lower critical solution temperature of PNIPAm at 33°C, a colloidal gel is formed as identified by an increase of I(q) at small q as well as a slowing down of sample dynamics by various orders of magnitude. With increasing TMAO concentration the gelation transition shifts linearly to lower temperatures. Above a TMAO concentration of approximately 0.40 mol/L corresponding to a 1:1 ratio of TMAO and NIPAm groups, collapsed PNIPAm states are found for all temperatures without any gelation transition. This suggests that reduction of PNIPAm-water hydrogen bonds due to the presence of TMAO results in a stabilisation of the collapsed PNIPAm state and suppresses gelation of the nanogel.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Design and implementation of a portable diagnostic system for Thomson scattering and optical emission spectroscopy measurements

A diagnostic system, which has a design goal of high-portability, has been designed at Oak Ridge National Laboratory (ORNL). This project aims at providing measurements of key plasma parameters (ne, Te, ni, Ti) for fusion-relevant devices, utilizing Thomson scattering (TS) and optical emission spectroscopy (OES). The innovative design employs mostly commercial off-the-shelf instrumentation and a traveling team of researchers to conduct measurements at various magnetic-confinement plasma devices. The TS diagnostic uses a Quantel Q-smart 1500 Nd:YAG laser with a 2ω harmonic generator to produce up to 850 mJ of 532 nm laser pulses at 10 Hz. Collection optics placed at the detection port consists of an 11 × 3 optical fiber bundle, where the TS diagnostic uses an 11 × 1 subset array of the fibers, the OES diagnostic uses another 11 fibers, and the remaining fibers are available to the host institution. The detection system is comprised of two separate IsoPlane-320 spectrometers with triple-grating turrets of various line spacing and two PI-MAX 4 intensified CCD detectors, used simultaneously to measure a broad range of ion, impurity, and electron parameters. The self-contained diagnostic package also includes a data processing and storage system. The design and initial implementation of the TS-OES diagnostic system are described. The experiments from the proof-of-principle operation of the portable package on a high density (∼2.5 × 1022 m−3) and low-temperature (∼5 eV) electrothermal arc source at ORNL are also discussed.

Kafle, N. (ORCID:000000028144787X)↗

Analytical harmonic vibrational frequencies with VV10-containing density functionals: Theory, efficient implementation, and benchmark assessments

VV10 is a powerful nonlocal density functional for long-range correlation that is used to include dispersion effects in many modern density functionals, such as the meta-generalized gradient approximation (mGGA), B97M-V, the hybrid GGA, ωB97X-V, and the hybrid mGGA, ωB97M-V. While energies and analytical gradients for VV10 are already widely available, this study reports the first derivation and efficient implementation of the analytical second derivatives of the VV10 energy. The additional compute cost of the VV10 contributions to analytical frequencies is shown to be small in all but the smallest basis sets for recommended grid sizes. Here, this study also reports the assessment of VV10-containing functionals for predicting harmonic frequencies using the analytical second derivative code. The contribution of VV10 to simulating harmonic frequencies is shown to be small for small molecules but important for systems where weak interactions are important, such as water clusters. In the latter cases, B97M-V, ωB97M-V, and ωB97X-V perform very well. The convergence of frequencies with respect to the grid size and atomic orbital basis set size is studied, and recommendations are reported. Finally, scaling factors to allow comparison of scaled harmonic frequencies with experimental fundamental frequencies and to predict zero-point vibrational energy are presented for some recently developed functionals (including r2SCAN, B97M-V, ωB97X-V, M06-SX, and ωB97M-V).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Partial Wave Analysis of Strange Mesons Decaying to K+p+p- in the Reaction ¿p ¿ K+p+p-¿(1520) and the Commissioning of the GlueX DIRC Detector

Hadron spectroscopy is a cornerstone of our understanding of the strong nuclear interactions. Studying the hadron spectrum led to the postulation of quarks and gluons, and the development of Quantum Chromodynamics (QCD), the theory of the strong nuclear force. Today hadron spectroscopy provides an important test of QCD, particularly in the non-perturbative energy regime. One such test is the existence of hybrid hadrons that have gluonic degrees of freedom, e.g. q ?qg states, that are allowed by QCD but have remained elusive in experimental searches. The GlueX experiment located at Thomas Jefferson National Accelerator Facility, is designed to map the light meson spectrum, including hybrid mesons, produced by a linearly polarized photon beam that is scattered off of a liquid hydrogen target. This dissertation concerns the installation and commissioning of the GlueX DIRC upgrade and the analysis of three reactions measured by the GlueX experiment. The GlueX DIRC is a particle identification detector installed as an upgrade to the GlueX experiment in 2019 to improve the experiment?s ability to distinguish pions and kaons. The DIRC uses Cherenkov photons radiated by charged particles that travel faster than the speed of light in the detector medium to determine the velocity of said particles. The velocity measurement is used in conjunction with momentum measurements from other detectors to determine the mass of the particle. The DIRC will be essential to the future of strange meson spectroscopy in GlueX. The reactions ?p ? K+K??+??p, ?p ? K+K??0?0p, ?p ? K+K??0?p were initially chosen for this analysis to search for the hybrid meson candidate ?(2170) and related resonances. The ?(2170) has been observed in e+e? collider experiments decaying to K+K??+?? and K+K??0?0, among other final states. The ?(2170) was not observed in this analysis. The reaction ?p ? K+?+???(1520), a subset of the ?p ? K+K??+??p reaction, was analyzed with a Partial Wave Analysis (PWA) in order to study strange mesons that decay to K+?+??. In the PWA, a useful model for the angular distributions was found but no significant structures could be observed due to statistical limitations.

Hurley, Andrew↗

Reduced fast-ion transport calculations of m = n = 1 fishbone-like instabilities in MAST-U

Fast-ion transport associated with an m = n = 1 fishbone-like burst in MAST-U discharge 47128 is investigated using a reduced guiding-center-based transport model (ORBIT-Kick) constrained by multi-diagnostic measurements. The two-dimensional beam-emission spectroscopy system provides measurements of the core poloidal mode structure and fluctuation amplitude, while EFIT++ reconstructions constrained by the motional Stark effect diagnostic indicate a flat q-profile with q 0 > 1⁠, indicating the absence of a resonant q = 1 surface and supporting a pressure-driven infernal-mode interpretation. Analytic m = n = 1 displacement profiles consistent with the measured core mode structure and equilibrium constraints are used as the mode structure inputs to ORBIT-Kick. The calculations show that the dominant resonances occur between the mode and co-passing fast ions, producing redistribution localized near the magnetic axis. Synthetic neutron camera signals from TRANSP-Kick recover up to 90% of the experimentally observed neutron deficit at the time of peak mode amplitude, indicating that the measured m = n = 1 mode is a dominant contributor to core fast-ion transport. However, the synthetic neutron signals recover rapidly, whereas the measured neutron emission continues to decrease after the peak amplitude. In conclusion, the remaining discrepancy may arise from contributions not included in the present single-harmonic model, including higher-m and higher-n harmonics, multi-harmonic interactions, and additional transport mechanisms, motivating future diagnostic development and modeling efforts to resolve and incorporate these additional contributions.

Wong, Henry H. [University of California, Los Ange↗