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At least 307 records · Page 17

A fluctuating hydrodynamics model for nanoscale surfactant-laden interfaces

A multispecies diffuse interface model is formulated in a fluctuating hydrodynamics framework for the purpose of simulating surfactant interfaces at the nanoscale. The model generalizes previous work to ternary mixtures, employing a Cahn-Hilliard free energy density combined with incompressible, isothermal fluctuating hydrodynamics where dissipative fluxes include both deterministic and stochastic terms. The intermolecular parameters in the free energy are chosen such that one species acts as a partially miscible surfactant. From Laplace pressure measurements, we show that in this model the surface tension decreases linearly with surfactant concentration, leading to Marangoni convection for interfaces with concentration gradients. In the capillary wave spectrum for interfaces with and without surfactant, we find that for the former, the spectrum deviates significantly from classical capillary wave theory, presumably due to Gibbs elasticity. In non-equilibrium simulations of the Rayleigh-Plateau instability, deterministic simulations showed that the surfactant delays pinching of a fluid cylinder into droplets. However, stochastic simulations indicate that thermal fluctuations disrupt the surfactant's stabilizing effect. Similarly, the spreading of a patch of surfactant, driven by Marangoni convection, was found to be partially suppressed by thermal fluctuations.

Capillary waves↗

Diamond surface functionalization via visible light–driven C–H activation for nanoscale quantum sensing

Nitrogen-vacancy (NV) centers in diamond are a promising platform for nanoscale NMR sensing. Despite significant progress toward using NV centers to detect and localize nuclear spins down to the single spin level, NV-based spectroscopy of individual, intact, arbitrary target molecules remains elusive. Such sensing requires that target molecules are immobilized within nanometers of NV centers with long spin coherence. The inert nature of diamond typically requires harsh functionalization techniques such as thermal annealing or plasma processing, limiting the scope of functional groups that can be attached to the surface. Solution-phase chemical methods can be readily generalized to install diverse functional groups, but they have not been widely explored for single-crystal diamond surfaces. Moreover, realizing shallow NV centers with long spin coherence times requires highly ordered single-crystal surfaces, and solution-phase functionalization has not yet been shown with such demanding conditions. In this work, we report a versatile strategy to directly functionalize C–H bonds on single-crystal diamond surfaces under ambient conditions using visible light, forming C–F, C–Cl, C–S, and C–N bonds at the surface. This method is compatible with NV centers within 10 nm of the surface with spin coherence times comparable to the state of the art. As a proof-of-principle demonstration, we use shallow ensembles of NV centers to detect nuclear spins from surface-bound functional groups. Our approach to surface functionalization opens the door to deploying NV centers as a tool for chemical sensing and single-molecule spectroscopy.

Science & Technology - Other Topics↗

Nanoscale dynamics of Dynamin 1 helices reveals squeeze-twist deformation mode critical for membrane fission

Dynamin 1 (Dyn1) GTPase, a principal driver of membrane fission during synaptic endocytosis, self-assembles into short mechanoactive helices cleaving the necks of endocytic vesicles. While structural information about Dyn1 helix is abundant, little is known about the nanoscale dynamics of the helical scaffolding at the moment of fission, complicating mechanistic understanding of Dyn1 action. To address the role of the helix dynamics in fission, we used High-Speed Atomic Force Microscopy (HS-AFM) and fluorescence microscopy to track and compare the spatiotemporal characteristics of the helices formed by wild-type Dyn1 and its K44A mutant impaired in GTP hydrolysis on minimal lipid membrane templates. In the absence of nucleotide, membrane-bound WT Dyn1 and K44A Dyn1 self-assembled into tubular protein scaffolding of similar diameter encaging the lipid bilayer. In both cases, the GTP addition caused scaffold constriction coupled with formation of 20 to 30 nm nanogaps in the protein coverage. While both proteins reached scaffold diameters characteristic for membrane superconstriction causing fission, the fission was detected only with WT Dyn1. We associated the fission activity with the dynamic evolution of the nanogaps: K44A Dyn1 gaps were static, while WT Dyn1 gaps actively evolved via repetitive nonaxisymmetric constriction-bending deformations caused by localized GTP hydrolysis. Modeling of the deformations implicated filament twist as an additional deformation mode which combines with superconstriction to facilitate membrane fission. Our results thus show that the dynamics of the Dyn1 helical scaffold goes beyond radial constriction and involves nonaxisymmetric deformations, where filament twist emerges as a critical driver of membrane fission.

59 BASIC BIOLOGICAL SCIENCES↗

Polarons are probes of the dynamic nanoscale environments found in electrochemically doped π-conjugated polymers

Charge carriers (i.e., polarons) in electrochemically doped organic (semi)conductors are proposed to be regulated by several physicochemical features, including the chemical compositions and structures of the π-conjugated frameworks of the semiconductor building blocks, the chemistry of the electrolyte (considering both the salt and solvent), multiscale and time-dependent morphology variations across the material as a function of electrochemical processes, and assorted permutations of these and other factors. To address these hypotheses, we investigate the energetic, optoelectronic, chemical, and local structural properties of negative polarons (radical anions) as a function of electrochemical doping in the donor–acceptor, π-conjugated redox copolymer P(NDI2OD-T2), also referred to as N2200. A critical finding is that there is not just “one type” of polaron in electrochemically doped P(NDI2OD-T2). Rather, an ensemble of polarons exists, with the polarons having optoelectronic signatures that are defined by their nanoscale environments. Importantly, the polaron optical signatures serve as local probes for how the operando electrochemical environments are dynamically working in concert to facilitate charge transport. Collectively, the distinctive and extensive integration of theory and measurement science presented here establishes a baseline for the roles that semiconductor and electrolyte chemistries and dynamic structural features have on polarons in electrochemically doped organic semiconductors and how these factors influence the energetics and rates of polaron transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanoscale Defects as Probes of Time-Reversal Symmetry Breaking

Nanoscale defects such as nitrogen-vacancy (NV) centers can serve as sensitive and noninvasive probes of electromagnetic fields and fluctuations from materials, which in turn can be used to characterize these systems. Here we specifically discuss how NV centers can probe time-reversal symmetry breaking (TRSB) phenomena in low-dimensional electronic systems. We argue that the difference in relaxation rates Γ$_{±\hat{z}}$ of NV centers starting from 𝑚 = ±1 spin states to the ground state with 𝑚 = 0 directly probes TRSB. The effect arises from the difference in the fluctuation spectrum of left- and right-polarized electromagnetic fields emanating from such materials. In the quantum Hall setting, the NV center experiences (nearly zero) large additional contribution to its relaxation due to the presence of the material when its magnetic dipole (anti)aligns with the external field. More generally, the difference in the relaxation rates is sensitive to the imaginary part of the wave-vector-dependent Hall conductivity. We argue that this can be used to determine the Hall viscosity, which can potentially distinguish candidate fractional quantum Hall states and be used to infer the pairing angular momentum in TRSB superconductors. We compute the average relaxation rate [Γ$_{+\hat{z}}$ + Γ$_{-\hat{z}}$] near thin film superconductors and find that it exhibits a Hebel-Slichter-like enhancement below 𝑇 𝑐 . The difference Γ$_{+\hat{z}}$ −Γ$_{-\hat{z}}$ also inherits this peak but is only nonzero for 𝑇 < 𝑇 𝑐 and only if the superconductivity is chiral. We provide concrete estimates for observing this effect in stacked twisted bismuth strontium calcium copper oxide flakes.

NV centers↗

Time-Domain Extreme-Ultraviolet Diffuse Scattering Spectroscopy of Nanoscale Surface Phonons

Here, we report the observation of dynamic fringe patterns in the diffuse scattering of extreme ultraviolet light from surfaces, following femtosecond optical excitation. At each point on the detector, the diffuse scattering intensity exhibits oscillations at well-defined frequencies that correspond to surface phonons with wave vectors determined by the scattering geometry, indicating that the optical excitation generates coherent surface phonons propagating in all directions and spanning a wavelength range from 60 to 300 nm. This phenomenon is observed on a variety of samples, including single-layer and multilayer metal films, as well as bulk semiconductors. The measured surface phonon dispersions show good agreement with theoretical calculations. By comparing signal amplitudes from samples with different surface morphologies, we find that the excitation mechanism is linked to the natural surface roughness of the samples. However, the signal is still detectable on extremely smooth surfaces with subnanometer roughness. Our findings demonstrate a simple and effective method for optically exciting coherent surface phonons with nanoscale wavelengths on a wide range of solid samples and establish a foundation for surface phonon spectroscopy in a wave vector range well beyond the limit of conventional surface Brillouin scattering.

Capotondi, F. [Elettra-Sincrotrone Trieste (Italy)↗

Nanoscale Quantum Imaging of Field-Free Deterministic Switching of a Chiral Antiferromagnet

Recently, unconventional spin-orbit torques (SOTs) with tunable spin generation have opened new pathways for designing novel magnetization control for cutting-edge spintronics innovations. A leading research thrust is to develop field-free deterministic magnetization switching for implementing scalable and energy favorable magnetic recording and storage, which have been demonstrated in conventional ferromagnetic and antiferromagnetic material systems. Here, in this work, we extend this advanced magnetization control strategy to chiral antiferromagnet Mn 3 ⁢Sn using spin currents with out-of-plane canted polarization generated from low-symmetry van der Waals (vdW) material WTe 2 . Numerical calculations suggest that dampinglike SOT of spins injected perpendicular to the kagome plane of Mn 3⁢ Sn serves as a driving force to rotate the chiral magnetic order, while the fieldlike SOT of spin currents with polarization parallel to the kagome plane provides the bipolar deterministicity to the magnetic switching in the absence of an external magnetic field. We further introduce scanning quantum microscopy to visualize nanoscale evolutions of Mn 3 ⁢Sn magnetic domains during the field-free switching process, corroborating the exceptionally large magnetic switching ratio up to 90%. Our results highlight the opportunities provided by hybrid SOT material platforms consisting of noncollinear antiferromagnets and low-symmetry vdW spin source materials for developing next-generation spintronic logic devices.

2-dimesional systems↗

Nanoscale degeneracy lifting in a geometrically frustrated antiferromagnet

The local atomic and magnetic structures of the compounds A MnO 2 (A = Na, Cu), which realize a geometrically frustrated, spatially anisotropic triangular lattice of Mn spins, have been investigated by atomic and magnetic pair distribution function analysis of neutron total scattering data. Relief of frustration in CuMnO 2 is accompanied by a conventional cooperative symmetry-lowering lattice distortion driven by Néel order. In NaMnO 2 , however, the distortion has a short-range nature. A cooperative interaction between the locally broken symmetry and short-range magnetic correlations lifts the magnetic degeneracy on a nanometer length scale, enabling long-range magnetic order in the Na derivative. The degree of frustration, mediated by residual disorder, contributes to the rather differing pathways to a single, stable magnetic ground state in these two related compounds. This study demonstrates how nanoscale structural distortions that cause local-scale perturbations can lift the ground-state degeneracy and trigger macroscopic magnetic order.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nanoscale dynamics during self-organized ion beam patterning of Si. II. Kr + bombardment

Understanding the self-organized ion beam nanopatterning of elemental semiconductors, particularly silicon, is of intrinsic scientific and technological interest. This is the second component of a two-part coherent x-ray scattering and x-ray photon correlation spectroscopy (XPCS) investigation of the kinetics and fluctuation dynamics of nanoscale ripple development on silicon during 1 keV Ar + (part I) and Kr + bombardment at 65° polar angle. Here it is found that the ion-enhanced viscous flow relaxation is essentially equal for Kr + -induced patterning as previously found for Ar + patterning despite the difference in ion masses. However, the magnitude of the surface curvature-dependent roughening rate in the early-stage kinetics is larger for Kr + than for Ar + , consistent with expectations that the heavier ion gives an increased mass redistributive contribution to the initial surface instability. As with the Ar + case, fluctuation dynamics in the late stage show a peak in correlation times at the length scale corresponding to the dominant structural feature on the surface—the ripples. Finally, it is shown that speckle motion during the surface evolution can be analyzed to determine spatial inhomogeneities in erosion rate and ripple velocity. This allows the direction and speed of ripple motion to be measured in a real time experiment. In the present case, ripple motion is found to be into the projected direction of the ion source, in contrast to expectations from an existing sputter erosion driven model with parameters derived from binary collision approximation simulations.

36 MATERIALS SCIENCE↗

Nanoscale structural correlations in a model cuprate superconductor

Understanding the extent and role of inhomogeneity is a pivotal challenge in the physics of cuprate superconductors. While it is known that structural and electronic inhomogeneity is prevalent in the cuprates, it has proven difficult to disentangle compound-specific features from universally relevant effects. Here, in this study, we combine advanced neutron and x-ray diffuse scattering with numerical modeling to obtain insight into bulk structural correlations in HgBa 2 ⁢ CuO 4+δ . This cuprate exhibits a high optimal transition temperature of nearly 100 K, pristine charge-transport behavior, and a simple average crystal structure without long-range structural instabilities, and is therefore uniquely suited for investigations of intrinsic inhomogeneity. We uncover diffuse reciprocal-space patterns that correspond to prominent nanoscale correlations of atomic displacements perpendicular to the CuO 2 planes. The real-space nature of the correlations is revealed through three-dimensional pair distribution function analysis and complementary numerical refinement. We find that relative displacements of ionic and CuO 2 layers play a crucial role, and that the structural inhomogeneity is not directly caused by the presence of conventional point defects. The observed correlations are therefore intrinsic to HgBa 2 ⁢ CuO 4+δ , and thus likely important for the physics of cuprates more broadly. It is possible that the structural correlations are closely related to the unusual superconducting fluctuations and Mott-localization in these complex oxides. As advances in scattering techniques yield increasingly comprehensive data, the experimental and analysis tools developed here for large volumes of diffuse scattering data can be expected to aid future investigations of a wide range of materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nanoscale viscosity of confined polyethylene oxide

Complex fluids near interfaces or confined within nanoscale volumes can exhibit substantial shifts in physical properties compared to bulk, including glass transition temperature, phase separation, and crystallization. Because studies of these effects typically use thin film samples with one dimension of confinement, it is generally unclear how more extreme spatial confinement may influence these properties. In this work, we used x-ray photon correlation spectroscopy and gold nanoprobes to characterize polyethylene oxide confined by nanostructured gratings (<100nm width) and measured the viscosity in this nanoconfinement regime to be ~500 times the bulk viscosity. Here, this enhanced viscosity occurs even when the scale of confinement is several times the polymer's radius of gyration, consistent with previous reports of polymer viscosity near flat interfaces.

36 MATERIALS SCIENCE↗

High Explosive Ignition through Chemically Activated Nanoscale Shear Bands

Shock initiation and detonation of high explosives is considered to be controlled through hot spots, which are local regions of elevated temperature that accelerate chemical reactions. Using classical molecular dynamics, we predict the formation of nanoscale shear bands through plastic failure in shocked TATB high explosive crystal. By scale-bridging with quantum-based molecular dynamics, we show that shear bands exhibit lower reaction barriers. While shear bands quickly cool,they remain chemically activated and support increased reaction rates without the local heating typically evoked by the hot spot paradigm. We describe this phenomenon as chemical activation through shear banding

Chemistry - Inorganic↗

Nanoscale Conductivity Imaging of Correlated Electronic States in WSe 2 /WS 2 Moiré Superlattices

We report the nanoscale conductivity imaging of correlated electronic states in angle-aligned WSe 2 /WS 2 heterostructures using microwave impedance microscopy. Here, the noncontact microwave probe allows us to observe the Mott insulating state with one hole per moiré unit cell that persists for temperatures up to 150 K, consistent with other characterization techniques. In addition, we identify for the first time a Mott insulating state at one electron per moiré unit cell. Appreciable inhomogeneity of the correlated states is directly visualized in the hetero-bilayer region, indicative of local disorders in the moiré superlattice potential or electrostatic doping. Our work provides important insights on 2D moiré systems down to the microscopic level.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Giant Transport Anisotropy in ReS 2 Revealed via Nanoscale Conducting-Path Control

The low in-plane symmetry in layered 1T'-ReS 2 results in strong band anisotropy, while its manifestation in the electronic properties is challenging to resolve due to the lack of effective approaches for controlling the local current path. In this work, we reveal the giant transport anisotropy in monolayer to four-layer ReS 2 by creating directional conducting paths via nanoscale ferroelectric control. By reversing the polarization of a ferroelectric polymer top layer, we induce conductivity switching ratio of >1.5×10 8 in the ReS 2 channel at 300 K. Characterizing the domain-defined conducting nanowires in an insulating background shows that the conductivity ratio between the directions along and perpendicular to the Re-chain can exceed 5.5×10 4 in monolayer ReS 2 . Theoretical modeling points to the band origin of the transport anomaly, and further reveals the emergence of a flat band in few-layer ReS 2 . Our work paves the path for implementing the highly anisotropic 2D materials for designing novel collective phenomena and electron lensing applications.

2D van der Waals materials↗

Harnessing Plasmonic Interference for Nanoscale Ultrafast Electron Sources

In this Letter we demonstrate the use of plasmonic focusing in conjunction with nonlinear photoemission to develop geometrically flat nanoscale electron sources with less than 40 pm-rad root mean squared (rms) normalized transverse emittance. Circularly polarized light is incident on a gold Archimedean spiral structure to generate surface-plasmon polaritons that interfere coherently at the center resulting in a 50 nm rms emission area. Furthermore, such a nanostructured flat surface enables simultaneous spatiotemporal confinement of emitted electrons at the nanometer and femtosecond level and can be used as an advanced electron source for high-repetition-rate ultrafast electron diffraction and microscopy experiments as well as the next generation of miniaturized particle accelerators.

43 PARTICLE ACCELERATORS↗

Nanoscale visualization of the thermally driven evolution of antiferromagnetic domains in FeTe thin films

Antiferromagnetic order, being a ground state of a number of exotic quantum materials, is of immense interest both from the fundamental physics perspective and for driving potential technological applications. For a complete understanding of antiferromagnetism in materials, nanoscale visualization of antiferromagnetic domains, domain walls, and their robustness to external perturbations is highly desirable. Here, we synthesize antiferromagnetic FeTe thin films using molecular-beam epitaxy. We visualize local antiferromagnetic ordering and domain formation using spin-polarized scanning tunneling microscopy. From the atomically resolved scanning tunneling microscopy topographs, we calculate local structural distortions to find a high correlation with the distribution of the antiferromagnetic order. This is consistent with the monoclinic structure in the antiferromagnetic state. Interestingly, we observe a substantial domain-wall change by small temperature variations, unexpected for the low-temperature changes used compared to the much higher antiferromagnetic ordering temperature of FeTe. This is in contrast to electronic nematic domains in the cousin FeSe multilayer films, where we find no electronic or structural change within the same temperature range. Further, our experiments provide the atomic-scale imaging of perturbation-driven magnetic domain evolution simultaneous with the ensuing structural response of the system. The results reveal surprising thermally driven modulations of antiferromagnetic domains in FeTe thin films well below the Néel temperature.

36 MATERIALS SCIENCE↗

In-Situ Nanoscale Focusing of Extreme Ultraviolet Solid-State High Harmonics

Extreme ultraviolet light delivering radiation with a wavelength shorter than approximately 100 nm is now available from solid-state sources. However, despite exceptional progress, efficient focusing of extreme ultraviolet photons to their ultimate diffraction limit remains a formidable challenge because of the precision of the focusing by curved, optical surfaces. Here we integrate coherent short-wavelength high-order harmonics from a MgO crystal, with a high-numerical-aperture, nanostructured, focusing element etched onto the surface of the crystal itself. We focus extreme ultraviolet light, seventh harmonic of an 800-nm laser, with a zone plate of numerical aperture 0.35, down to a waist radius of 150 nm, with 18% focusing efficiency. The estimated intensity approaches 10 7 W/cm 2 . Future developments may demonstrate nanoscale laser ablation and miniaturization of extreme ultraviolet coherent sources on a chip.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Sketched Nanoscale KTaO 3 -Based Superconducting Quantum Interference Device

The discovery of two-dimensional superconductivity in LaAlO 3 /KTaO 3 (111) and (110) interfaces has raised significant interest in this system. In this paper, we report the first successful fabrication of a direct current superconducting quantum interference device (dc-SQUID) in the KTO system. The key device elements, superconducting weak links, are created by conductive atomic force microscope lithography, which can reversibly control the conductivity at the LAO/KTO (110) interface with nanoscale resolution. The periodic modulation of the SQUID critical current 𝐼 c ⁡(𝐵) with magnetic field corresponds well with our theoretical modeling, which reveals a large kinetic inductance of the superconducting two-dimensional electron gas in KTO. The kinetic inductance of the SQUID is tunable by electrical gating from the back, due to the large dielectric constant of KTO. The demonstration of weak links and SQUIDs in KTO broadens the scope for exploring the underlying physics of KTO superconductivity, including the role of spin-orbit coupling, pairing symmetry, and inhomogeneity. It also promotes KTO as a versatile platform for a growing family of quantum devices, which could be applicable in the realm of quantum computing and information.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗