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At least 181 records · Page 10

Subnanometer Visualization of Spatially Varying Local Field Resonances that Drive Tip-Enhanced Optical Spectroscopy

Our knowledge of the electromagnetic fields that power modern nanoscale optical measurements, including (non)linear tip-enhanced Raman and photoluminescence, chiefly stems from numerical simulations. Aside from idealized in silico vs heterogeneous (nano)structures in the laboratory, challenges in quantitative descriptions of nanoscale light–matter interactions more generally stem from the very nature of the problem, which lies at the interface of classical and quantum theories. This is particularly the case in ultrahigh spatial resolution measurements that are sensitive to local optical field variations that take place on subnanometer length scales. Here this work approaches this challenge through extinction-based spectral nanoimaging experiments. We demonstrate <1 nm spatial resolution in hyperspectral extinction measurements that track spatially varying plasmon resonances. We describe the principles behind our experiments and highlight more general implications of our observations.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Superconducting coherence peak in near-field radiative heat transfer

Enhancement and peaks in near-field radiative heat transfer (NFRHT) typically arise due to surface phonon-polaritons, plasmon-polaritons, and electromagnetic (EM) modes in structured materials. However, the role of material quantum coherence in enhancing near-field radiative heat transfer remains unexplored. Here, we unravel that NFRHT in superconductor-ferromagnetic systems displays a unique peak at the superconducting phase transition that originates from the quantum coherence of Bogoliubov quasiparticles in superconductors. Our theory takes into account evanescent EM radiation emanating from fluctuating currents related to Cooper pairs and Bogoliubov quasiparticles in stark contrast to the current-current correlations induced by free electrons in conventional materials. Our proposed NFRHT configuration exploits ferromagnetic resonance at frequencies deep inside the superconducting band gap to isolate this superconducting coherence peak. Furthermore, we reveal that Cooper pairs and Bogoliubov quasiparticles have opposite effects on near-field thermal radiation and isolate their effects on many-body radiative heat transfer near superconductors. As a result, our proposed phenomenon can have applications for developing thermal isolators and heat sinks in superconducting circuits.

Dipole approximation↗

Spatio-temporal electric field distributions in an atmospheric plasma jet impinging on a microchannel array surface

The electric field distribution in the ionization waves (IWs) propagating over a microchannel array dielectric surface, with the channels either empty or filled with distilled water, is measured by ps electric field induced second harmonic generation. The surface IW is initiated by the atmospheric pressure N 2 –Ar plasma jet impinging on the surface vertically and powered by ns pulse discharge bursts. The results show that the electric field inside the microchannels, specifically its horizontal component, is enhanced by up to a factor of 2. The field enhancement region is localized within the channels. The vertical electric field inside the channels lags in time compared to the field measured at the ridges, indicating the transient reversal of the IW propagation direction across the channels (toward the jet). This is consistent with the phase-locked plasma emission images and confirmed by the kinetic modeling predictions, which show that the IW ‘jumps’ over the empty channels and propagates into the channels only after the jump between the adjacent ridges. When the channels are filled with water, the wave speed increases by up to 50%, due to the higher effective dielectric constant of the surface. No evidence of a significant electric field enhancement near the dielectric surface (ceramic or water) has been detected, within the spatial resolution of the present diagnostic, ~100 μ m.

plasmas and liquids↗

All-optical nanoscopic spatial control of molecular reaction yields on nanoparticles

Molecular adsorbate reactions on nanoparticles play a fundamental role in areas such as nano-photocatalysis, atmospheric, and astrochemistry. They can be induced, enhanced, and controlled by field localization and enhancement on the nanoparticle surface. In particular, the ability to perform highly controlled near-field-mediated reactions is key to deepening our understanding of surface photoactivity on nanosystems. Here, using reaction nanoscopy, we experimentally demonstrate all-optical nanoscopic control of surface reaction yields by tailoring the near fields on nanoparticles with waveform-controlled linear and bicircular two-color laser pulses, respectively. We observe site-selective proton emission from the dissociative ionization of adsorbate molecules on Si O 2 nanoparticles as a function of the polarization and relative phase of the two-color pulses. The angularly resolved close-to-uniform mapping between the surface reaction yields and the measured ion momentum enables the observation and spatial control of molecular reactions on the nanoparticle surface with nanoscopic resolution. The experimental results are modeled and reproduced qualitatively by classical trajectory Monte Carlo simulations. Our work paves the way toward reliable all-optical control of photocatalytic chemical reactions on nanoscale surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Large enhancement of the in-field critical current density of YBCO coated conductors due to composite pinning landscape

YBa 2 Cu 3 O 7 -based coated conductors (CCs) achieve the highest critical current densities (J c ) of any known superconductor and are a key technology for applications such as rotatory machines, high-field magnets and power transmission. Incorporation of nano-sized non-superconducting second phases as additional vortex pinning centers has been considered the most amenable route to further enhance J c at an industrial scale, and has been successfully used in commercial CCs. The resulting pinning landscape is quite complex, with both synergistic and competing interactions among the various types of defects. Particle irradiation, on the other hand, allows for a controlled post-processing incorporation of a well-defined defect morphology. We have previously shown that irradiation with protons and other light ions can further enhance the in-field J c in commercial state-of-the-art CCs. Here we develop a combined irradiation process that increases J c above values previously achieved by irradiating with only one species. Our new approach involves sequentially irradiating with 250 MeV Au ions and 4 MeV protons. For example, at T ~ 27 K (liquid neon) and μ 0 H ~ 4 T, a region of interest for rotatory machines applications, we obtain J c ~ 5 MA cm -2 , which is about 40% higher than the values produced by the individual irradiations. Finally, we conclude that this is due to the synergistic pinning effects of the introduced splayed, non-uniform columnar defects and small clusters.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Field Programmable Gate Arrays for Enhancing the Speed and Energy Efficiency of Quantum Dynamics Simulations

We present the first application of field programmable gate arrays (FPGAs) as new, customizable hardware architectures for carrying out fast and energy-efficient quantum dynamics simulations of large chemical/material systems. Instead of tailoring the software to fixed hardware, which is the typical case for writing quantum chemistry code for central processing units (CPUs) and graphics processing units (GPUs), FPGAs allow us to directly customize the underlying hardware (even at the level of specific electrical signals in the circuit) to give a truly optimized computational performance for quantum dynamics calculations. By offloading the most intensive and repetitive calculations onto an FPGA, we show that the computational performance of our real-time electron dynamics calculations can even exceed that of optimized commercial mathematical libraries running on high-performance GPUs. In addition to this impressive computational speedup, we show that FPGAs are immensely energy-efficient and consume 4 times less energy than modern GPU or CPU architectures. These energy savings are a practical and important metric for supercomputing centers (many of which exceed over $1 million in power costs alone), as exascale computing capabilities become more widespread and commonplace. Taken together, the implementation techniques and performance metrics of our study demonstrate that FPGAs could play a promising role in upcoming quantum chemistry and materials science applications, particularly for the acceleration and energy-efficient execution of quantum dynamics calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electrostatically Enhanced Buried Interface Binding of Self‐Assembled Monolayers for Efficient And Stable Inverted Perovskite Solar Cells

Inverted p‐i‐n structure perovskite solar cells (PSCs) have outperformed traditional n‐i‐p PSCs in recent years. A key advancement is the use of self‐assembled monolayers (SAMs) as hole transport layers. One class of widely used SAMs is carbazole‐based phosphonic acids. However, it is found that these SAMs lack strong binding with transparent conducting oxides (TCO) and perovskite. The weak binding strength results in suboptimal interfacial adhesion of the buried interface, which limits the device's stability. Here, interfacial binding is enhanced by increasing the dipole moment that creates a strong interfacial electric field that enhances electrostatic interactions at the TCO/perovskite interface, while incorporating tailored functional groups in SAMs to improve chemical anchoring to TCO and binding to perovskite. Specifically, the donor‐acceptor SAM molecule 4‐(7‐(4‐(bis(4‐methoxyphenyl)amino)‐2,5‐difluorophenyl)benzo[c][1,2,5]thiadiazol‐4‐yl)benzoic acid (PAFTB) is employed, which features an enhanced dipole moment along with electron‐donating and electron‐withdrawing functional groups to optimize interfacial interactions. Compared to extensively used [2‐(9H‐carbazol‐9‐yl)ethyl]phosphonic acid (2PACz), PAFTB enhances total interfacial adhesion by 2.8 times, thereby improving the thermal stability of the layer. Using this approach, PSCs are demonstrated with a certified quasi‐steady‐state power conversion efficiency of 24.9% and maintain 80% of the initial efficiency after 900 h of maximum power point tracking at 85 °C.

Interfacial adhesion↗

Tip-Enhanced Multipolar Raman Scattering

We record nanoscale chemical images of thiobenzonitrile (TBN)-functionalized plasmonic gold nanocubes via tip-enhanced Raman spectroscopy (TERS). The spatially averaged optical response is dominated by conventional (dipolar) TERS scattering from TBN but also contains weaker spectral signatures in the 1225-1500 cm-1 region. The weak optical signatures dominate some of the recorded single pixel spectra. We can uniquely assign these Raman forbidden transitions to multipolar Raman scattering, which implicates spatially varying enhanced electric field gradients at plasmonic tip-sample nanojunctions. Specifically, we can assign observations of tip-enhanced electric dipole-magnetic dipole as well as electric dipole-electric quadrupole driven transitions. These signals need to be understood and accounted for in the interpretation of TERS spectral images, particularly in on-going quests aimed at chemical reaction mapping via TERS.

Wang, Chih-Feng↗

Local dynamic responses of magnetic reconnection to three-dimensional perturbations in a laboratory plasma

The dynamic responses of magnetic reconnection to localized three-dimensional (3D) magnetic field perturbations imposed by a pair of figure-8-shaped coils are investigated in the Magnetic Reconnection Experiment (MRX) device. Both the magnetic field geometry and current sheet profiles are altered by external perturbations. For the case when the inductive electric field associated with these perturbations aligns with the preexisting reconnection electric field, O-type magnetic structures appear within an elongated current sheet. When these magnetic structures are ejected downstream at the speed close to the ion outflow velocity, the inductive electric field is enhanced considerably. Despite that the imposed perturbation amplitude is larger than 30% of the original reconnecting magnetic field, the overall reconnection process remains robust without current sheet disruptions. This technique to form O-type magnetic structures can serve as an additional experimental knob for future systematic laboratory investigations of 3D magnetic reconnection and related instabilities without disrupting two-dimensional current sheet.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

High-Field Nuclear Magnetic Resonance (NMR) Spectroscopy

Nuclear magnetic resonance (NMR) is a non-destructive spectroscopic technique that provides detailed molecular structural information via the electronic environments of nuclei in materials. Higher magnetic field strengths enhance the resolution of NMR, enabling discernment of unique chemical environments that might not be possible at low fields. Herein, the application of high-field NMR to catalyst and electrochemical system characterization are detailed. A brief description of NMR and quadrupolar nuclei are presented where the effects of magnetic field are described. Examples of high-field NMR are provided with particular focus on employing NMR to elucidate the structure of oxides of aluminum and vanadium for catalyst applications. The role of high-field NMR to conduct challenging experiments for energy storage materials is also explored and numerous other nuclei which require high-field measurement are briefly summarized.

Catalyst, Spectroscopy, NMR, High-field, Quadrupol↗

NUMERICAL CALCULATION OF LOSSES OF TRAPPED VORTICES UNDER STRONG RF MEISSNER CURRENT AND DC SUPERHEATING FIELD IN TYPE II SUPERCONDUCTORS

Research on the vortex dynamics and enhancing of superheating field in superconductors has attracted much attention in accelerator physics community to develop next-generation high-performance accelerator cavities. However, the extreme dynamics of curvilinear elastic vortices driven by very strong currents close to the depairing limit or superheating field of a superconductor with a nanostructured surface has not been well understood. We calculated the superheating field Hsh and critical momentum kc characterizing the wavelength of the instability ?m of the Meissner state to flux penetration by solving numerically the Ginzburg?Landau equations. A bulk superconductor, superconductor with the inhomogeneous surface disorder (S-S), and multilayered surface (S-I-S) have been thoroughly investigated in this work. Our result showed that S-S and S-I-S structures can enhance the superheating field well above their clean limit. In this work extensive numerical simulation of the power dissipated by an oscillating vortex segment driven by the surface ac Meissner currents was performed. Our simulations take into account the nonlinear vortex line tension, vortex mass, Bardeen?Stephen viscous vortex drag applicable at low fields, and nonlinear Larkin-Ovchinnikov (LO) viscous drag coefficient ?(v) at high fields and pinning force. We showed that the LO decrease of ?(v) with the vortex velocity v could radically change the field dependence of the surface resistance Ri(H) caused by trapped vortices. At low frequencies Ri(H) exhibits a conventional increase with H. However, as frequency increases, the surface resistance becomes a nonmonotonic function of H which decreases with H at higher fields irrespective of the pinning distribution. Overheating can mask the descending field dependence of Ri(H) as frequency increases. Our numerical simulations also show that the LO effect can cause a vortex bending instability at high field amplitudes and frequencies, giving rise to the formation of dynamic kinks along with the vortex when a vortex is pinned strongly to one end. Nonlinear losses of trapped vortices in thick films under high-amplitude RF fields as functions of frequency, mean free path and pinning characteristics have been calculated.

Pathirana, Walive↗

The impact of magnetic fields on momentum transport and saturation of shear-flow instability by stable modes

The Kelvin–Helmholtz (KH) instability of a shear layer with an initially uniform magnetic field in the direction of flow is studied in the framework of 2D incompressible magnetohydrodynamics with finite resistivity and viscosity using direct numerical simulations. The shear layer evolves freely, with no external forcing, and thus broadens in time as turbulent stresses transport momentum across it. As with hydrodynamic KH, the instability here features a conjugate stable mode for every unstable mode in the absence of dissipation. Stable modes are shown to transport momentum up its gradient, shrinking the layer width whenever they exceed unstable modes in amplitude. In simulations with weak magnetic fields, the linear instability is minimally affected by the field, but enhanced small-scale fluctuations relative to the hydrodynamic case are observed. These enhanced fluctuations coincide with increased energy dissipation and faster layer broadening, with these features more pronounced in simulations with stronger fields. These trends result from the magnetic field reducing the effects of stable modes relative to the transfer of energy to small scales. As field strength increases, stable modes become less excited, thus transporting less momentum against its gradient. Furthermore, the energy that would otherwise transfer back to the driving shear because of the stable modes is instead allowed to cascade to small scales, where it is lost to dissipation. Approximations of the turbulent state in terms of a reduced set of modes are explored. While the Reynolds stress is well-described using just two modes per wavenumber at large scales, the Maxwell stress is not.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Quantum Logic Enhanced Sensing in Solid-State Spin Ensembles

We demonstrate quantum logic enhanced sensitivity for a macroscopic ensemble of solid-state, hybrid two-qubit sensors. We achieve over a factor of 30 improvement in the single-shot signal-to-noise ratio, translating to an ac magnetic field sensitivity enhancement exceeding an order of magnitude for time-averaged measurements. Using the electronic spins of nitrogen vacancy (NV) centers in diamond as sensors, we leverage the on-site nitrogen nuclear spins of the NV centers as memory qubits, in combination with homogeneous and stable bias and control fields, ensuring that all of the ~10 9 two-qubit sensors are sufficiently identical to permit global control of the NV ensemble spin states. We find quantum logic sensitivity enhancement for multiple measurement protocols with varying optimal sensing intervals, including XY8 and DROID-60 dynamical decoupling, as well as correlation spectroscopy, using an applied ac magnetic field signal. The results are independent of the nature of the target signal and broadly applicable to measurements using NV centers and other solid-state spin ensembles. Furthermore, this work provides a benchmark for macroscopic ensembles of quantum sensors that employ quantum logic or quantum error correction algorithms for enhanced sensitivity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Elastic-plastic conductor damage evaluation at over 0.4% strain using a high-stress REBCO coil

Abstract Recent reports on screening current stress simulations of high-field REBCO magnets frequently present peak stresses over 1 GPa. However, this result is probably an unrealistic artifact of purely elastic calculations, considering the macroscopic yield and fracture stresses of approximately 900 MPa and less than 1.1 GPa for Hastelloy substrate-coated conductors. Here, we evaluate elastic-plastic conductor damage at over 0.4% strain using a high-stress REBCO coil exposed to a high field to explore this elastic-plastic regime. The coil was located off-center in a low-temperature superconductor magnet so as to induce a significant screening current in the enhanced radial field. Voltage taps, a Hall sensor, and two strain gauges were used for the instrumentation. We obtained strains exceeding 0.4% near the outward edge during the coil current charge from 350 A to 390 A, where the coil was exposed to external axial and radial magnetic fields of 13 T and 0.5 T. Post mortem results showed wavy plastic deformation, electrical damage, and REBCO defects. An elastic-plastic simulation reproduced the measured strains and predicted that ∼1 GPa stress is sufficient to induce ∼0.9% strain, thus validating our initial concerns with purely elastic models. This paper provides our experimental and simulation results.

Bang, Jeseok (ORCID:0000000247616334)↗

Detecting axion dark matter with black hole polarimetry

The axion, as a leading dark matter candidate, is the target of many ongoing and proposed experimental searches based on its coupling to photons. Ultralight axions that couple to photons can also cause polarization rotation of light which can be probed by the cosmic microwave background. In this work, we show that a large axion field is inevitably developed around black holes due to the Bose-Einstein condensation of axions, enhancing the induced birefringence effects. Therefore, measuring the modulation of supermassive black hole imaging polarization angles is a strong probe to the axion-photon coupling due to the formation of the axion condensation (axion star) which enhances the axion field. The oscillating axion field around black holes induces polarization rotation on the black hole image, which is detectable and distinguishable from astrophysical effects on the polarization angle, as it exhibits distinctive temporal variability and frequency invariability. In this work, we perform the theoretical calculation on the axion star formation rate and correspondingly the enhanced axion field value near supermassive black holes. Then, we present the range of axion-photon couplings within the axion mass range 10 − 21 – 10 − 16 eV that can be probed by the Event Horizon Telescope. The axion parameter space probed by black hole polarimetry will expand with the improvement in sensitivity on the polarization measurement and more black hole polarimetry targets with determined black hole masses. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Water structure and electric fields at the interface of oil droplets

Interfacial water exhibits rich and complex behaviour, playing an important part in chemistry, biology, geology and engineering. However, there is still much debate on the fundamental properties of water at hydrophobic interfaces, such as orientational ordering, the concentration of hydronium and hydroxide, improper hydrogen bonds and the presence of large electric fields. This controversy arises from the challenges in measuring interfacial systems, even with the most advanced experimental techniques and theoretical approaches available. Here we report on an in-solution, interface-selective Raman spectroscopy method using multivariate curve resolution to probe hexadecane-in-water emulsions, aided by a monomer-field theoretical model for Raman spectroscopy. Our results indicate that oil-water emulsion interfaces can exhibit reduced tetrahedral order and weaker hydrogen bonding, along with a substantial population of free hydroxyl groups that experience about 95 cm -1 redshift in their stretching mode compared with planar oil-water interfaces. Given the known electrostatic zeta potential characteristic of oil droplets, we propose the existence of a strong electric field (about 50-90 MV cm -1 ) emanating from the oil phase. This field is inferred indirectly but supported by control experiments and theoretical estimates. These observations are either absent or opposite in the molecular hydrophobic interface formed by small solutes or at planar oil-water interfaces. Instead, water structural disorder and enhanced electric fields emerge as unique features of the mesoscale interface in oil-water emulsions, potentially contributing to the accelerated chemical reactivity observed at hydrophobic-water interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electron emissions and hot spots in dual-phase LXe TPCs

Persistent photon and single-electron emissions - in the form of “electron trains” and localized “hot spots” - have been observed in multiple dual-phase liquid xenon (LXe) time projection chambers (TPCs), often persisting long after ionizing events. Here, we show that these phenomena are naturally explained by photon-triggered single-electron emission from resistive mixed-oxide films on stainless-steel (SS304 or s.s.) wires, which behave as leaky capacitors with long RC time constants at LXe temperature. Positive ions landing on these oxides can further enhance local fields and drive Malter-like electron emission. We outline the materials physics (Cr 2 O 3 /Cr 2 O 3-x /Cr(OH) 3 mosaics), quantify expected time scales (∼1 s under illumination), and demonstrate how small damaged regions with enhanced QE can produce persistent hot spots.

Va'vra, J. [SLAC National Accelerator Laboratory (↗

Experimental evidence of early-time saturation of the ion-Weibel instability in counterstreaming plasmas of CH, Al, and Cu

The collisionless ion-Weibel instability is a leading candidate mechanism for the formation of collisionless shocks in many astrophysical systems, where the typical distance between particle collisions is much larger than the system size. Multiple laboratory experiments aimed at studying this process utilize laser-driven (I≳10 15 W/cm 2 ), counterstreaming plasma flows (V≲ 2000 km/s) to create conditions unstable to Weibel-filamentation and growth. This technique intrinsically produces temporally varying plasma conditions at the midplane of the interaction where Weibel-driven B fields are generated and studied. Experiments discussed herein demonstrate robust formation of Weibel-driven B fields under multiple plasma conditions using CH, Al, and Cu plasmas. Linear theory based on benchmarked radiation-hydrodynamic FLASH calculations is compared with Fourier analyses of proton images taken ~5–6 linear growth times into the evolution. Our new analyses presented here indicate that the low-density, high-velocity plasma-conditions present during the first linear-growth time (~300–500 ps) sets the spectral characteristics of Weibel filaments during the entire evolution. It is shown that the dominant wavelength (~300 μm) at saturation persists well into the nonlinear phase, consistent with theory under these experimental conditions. However, estimates of B-field strength, while difficult to determine accurately due to the path-integrated nature of proton imaging, are shown to be in the ~10–30 T range, an order of magnitude above the expected saturation limit in homogenous plamas but consistent with enhanced B fields in the midplane due to temporally varying plasma conditions in experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗