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At least 37 records · Page 2

Nonlinear nanoelectrodynamics of a Weyl metal

Chiral Weyl fermions with linear energy-momentum dispersion in the bulk accompanied by Fermi-arc states on the surfaces prompt a host of enticing optical effects. While new Weyl semimetal materials keep emerging, the available optical probes are limited. In particular, isolating bulk and surface electrodynamics in Weyl conductors remains a challenge. We devised an approach to the problem based on near-field photocurrent imaging at the nanoscale and applied this technique to a prototypical Weyl semimetal TaIrTe 4 . As a first step, we visualized nano-photocurrent patterns in real space and demonstrated their connection to bulk nonlinear conductivity tensors through extensive modeling augmented with density functional theory calculations. Notably, our nanoscale probe gives access to not only the in-plane but also the out-of-plane electric fields so that it is feasible to interrogate all allowed nonlinear tensors including those that remained dormant in conventional far-field optics. Surface- and bulk-related nonlinear contributions are distinguished through their “symmetry fingerprints” in the photocurrent maps. Robust photocurrents also appear at mirror-symmetry breaking edges of TaIrTe 4 single crystals that we assign to nonlinear conductivity tensors forbidden in the bulk. Here, nano-photocurrent spectroscopy at the boundary reveals a strong resonance structure absent in the interior of the sample, providing evidence for elusive surface states.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC

Energy transfer between localized emitters in photonic cavities from first principles

Radiative and nonradiative resonant couplings between defects are ubiquitous phenomena in photonic devices used in classical and quantum information technology applications. In this work, we present a first-principles approach to enable quantitative predictions of the energy transfer between defects in photonic cavities, beyond the dipole-dipole approximation and including the many-body nature of the electronic states. As an example, we discuss the energy transfer from a dipolelike emitter to an 𝐹 center in MgO in a spherical cavity. We show that the cavity can be used to controllably enhance or suppress specific spin-flip and spin-conserving transitions. Specifically, we predict that an ∼10–100 enhancement in the resonant energy transfer rate can be gained in the case of the 𝐹 center in MgO at ∼10 nm distances from a dipolar source, using rather moderate cavity with quality factor 𝑄 ∼ 400. We also show that a similar suppression in the transfer rate can be achieved by off-tuning the cavity resonance relative to the emitter transition energy. The framework presented here is general and readily applicable to a wide range of devices where localized emitters are embedded in microspheres, core-shell nanoparticles, and dielectric Mie resonators. Hence, our approach paves the way to predict how to control energy transfer in quantum memories and in ultrahigh-density optical memories, and in a variety of quantum information platforms.

First-principles calculations

Quantitative Infrared-to-Terahertz Nanospectroscopy of Semiconductors

Semiconductor technology now employs few-nanometer features, necessitating tools probing electronic properties on the same length scale. While the concentration of free charge carriers is routinely measured, the scattering rate remains challenging to access at the nanoscale. Here, we present ultrabroadband (5–50 THz) synchrotron infrared nanospectroscopy as a quantitative metrology tool for semiconductors. This technique can determine both the charge carrier concentration and scattering rate with percent-level accuracy, and it is inherently capable of ∼10 nm spatial resolution. We study silicon with different doping levels and confirm the method’s accuracy by statistical analysis and comparison with established far-field infrared spectroscopy. Near-field measurements systematically reveal charge-carrier concentrations ∼30% lower than far-field values, consistent with increased surface sensitivity and surface depletion. Our work establishes synchrotron infrared nanospectroscopy as a precise tool for quantitative nanoscale semiconductor characterization and paves the way toward all-optical characterization of surface depletion effects.

36 MATERIALS SCIENCE

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

Atmospheric, Non-Combusting Droplet Sizing and Spray Imaging Results From a Non-Proprietary Aero Gas Turbine Engine Pressure Swirl Atomizer using Shadowgraphy and Planar Laser Scatter

Members from industry and federal agencies of the United States have developed a collaborating group focused on improving the understanding of the atomization processes common to gas turbine engines. The group is aimed on providing high quality data using x-ray diagnostics in the internal geometry and the near-field dense spray as well as optical diagnostics in the visible spectrum, downstream of the nozzle. This paper reports results from one of the two non-proprietary injectors designs from the group: the primary-secondary injector. In particular, we characterize the spray from only the primary, pressure-swirl atomizing circuit using water through the nozzle. We observed Sauter mean diameter decreased with increased water pressure drop across the nozzle. SMD was also collected at three axial distances and showed decreased size with distance from the nozzle. Planar laser sheet droplet scattering provided qualitative assessment of the spray. Higher water pressure drops provided better atomization than lower pressure drops. The addition of swirling air flow through the injector alleviates and improves the atomization quality, particularly at the lower water pressure drops.

optical diagnostics

Polarization‐Engineered Near‐Field Generation Using a Hybrid Tip–Antenna System

Precise control of light polarization at the nanoscale is critical for accessing chiral optical responses and manipulating spin–photon interactions in advanced materials. Yet, conventional scattering-type near-field probes predominantly generate out-of-plane linear polarization and offer little control over phase or polarization state. Here, in this study, we introduce a polarization-engineered near-field methodology based on a combined metallic tip and planar dipole nanoantenna system. Using full-wave electromagnetic simulations, we show that the tip acts as a vertically oriented plasmonic resonator, while the antenna supports an in-plane dipolar mode. By tuning the tip–antenna geometry and tip height, the two orthogonal field components attain comparable amplitudes and a controllable ∼90° phase offset, producing circularly polarized nano-light in the antenna gap. The proposed system effectively functions as a nanoscale quarter-wave plate, converting linearly polarized illumination into circularly polarized hotspots without external polarization optics. This method establishes an experimentally accessible route toward polarization-programmable near-field nanoscopy, enabling chiral spectroscopy, selective excitation of spin/valley degrees of freedom, and quantum optical investigations at the nanoscale.

36 MATERIALS SCIENCE

Interfacial Strong Coupling and Negative Dispersion of Propagating Polaritons in Freestanding Oxide Membranes

Membranes of complex oxides like perovskite SrTiO3 extend the multi-functional promise of oxide electronics into the nanoscale regime of 2D materials. Here, it is demonstrated that freestanding oxide membranes supply a reconfigurable platform for nano-photonics based on propagating surface phonon polaritons. Infrared near-field imaging and spectroscopy enabled by a tunable ultrafast laser are applied to study pristine nano-thick SrTiO3 membranes prepared by hybrid molecular beam epitaxy. As predicted by coupled mode theory, it is found that strong coupling of interfacial polaritons realizes symmetric and antisymmetric hybridized modes with simultaneously tunable negative and positive group velocities. By resolving reflection of these propagating modes from membrane edges, defects, and substrate structures, their dispersion is quantified with position-resolved nano-spectroscopy. Remarkably, polariton negative dispersion is found to be both robust and tunable through choice of membrane dielectric environment and thickness, and proposes a novel design for in-plane Veselago lensing harnessing this control. This work lays the foundation for tunable transformation optics at the nanoscale using polaritons in a wide range of freestanding complex oxide membranes.

freestanding oxide membranes

Pattern-enhanced Resonant Soft X-ray Scattering for Operando monitoring of electrochemical solid-liquid interfaces

Unveiling interfaces at sub-nanometer scales is essential for advancing the understanding of complex chemical transformations. However, characterizing solid-liquid interfaces with high dimensional sensitivity and temporal resolution remains challenging, due to their dynamic nature and inaccessibility by conventional probes. Here we present an approach, Pattern-enhanced Resonant Soft X-ray Scattering, to overcome the challenges. Rooted in a “sample-as-optics” philosophy, this technique utilizes precisely engineered line-grating nanopatterns to modulate near-field X-ray illumination, coherently enhancing scattering signals from the line-gratings. We implement the method using Ni line-grating nanopatterns in electrochemical water oxidation. The periodic nanostructures serve as diffractive optical elements to reveal the Ni oxidation gradients and structural dynamics at the electrode-electrolyte interfaces. Finite-element simulations corroborate the observed trends by modeling variations in compositions and structures during electrocatalysis. Through integrating advanced sample design with coherent wave nature of soft X-rays, our approach opens accessible pathways to operando exploring chemical evolution and sub-nanometer dimensional variations simultaneously in electrochemical systems. This non-destructive method is efficient and element-specific, making it valuable for probing chemical and dimensional dynamics with appropriate modeling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

X-ray near-field multi-slice ptychography for in-situ imaging

Abstract In-situ imaging of chemical reactions can provide valuable insight into nanoparticle growth and structural evolution. Hard X-ray imaging is an excellent tool for this purpose, as it combines high spatial resolution with high penetration depth, allowing for realistic reaction environments. While far-field ptychography is a well-established method at synchrotron radiation sources, its near-field analog has received less attention. In this work we show that near-field multi-slice ptychography is a competitive method for high-resolution in-situ imaging by studying the formation of gold nanocages via galvanic replacement. Our work extends near-field X-ray ptychography to sub-50 nm spatial resolution by using multilayer Laue lenses. These high numerical aperture optics enable to distinguish sample layers that are separated by less than 100 µm by multi-slicing techniques.

Science & Technology - Other Topics

Probing and Tuning Strain‐Localized Exciton Emission in 2D Material Bubbles at Room Temperature

In monolayer transition metal dichalcogenides bubbles-nanoscale deformations typically exhibiting a dome-like shape-Excitons are confined by the strain effect, which exhibits extraordinary emission properties, such as single photon generation, enhanced light emission, and spectrally tunable excitonic states. While the strain profiles of these bubbles are extensively studied, this work provides an approach 1) to directly visualize the associated exciton properties in bubbles formed in WSe2 monolayer, revealing an intrinsic emission wavelength shift of ≈40 nm, and 2) actively modify local strain, enabling further exciton emission tuning over a range of 50 nm. These are achieved by emission mapping and nanoindentation using a dielectric near-field probe, which enables the detection of local emission spectra and emission lifetimes within individual bubbles. Statistical analysis of 67 bubbles uncovers an emission wavelength distribution centered around 780 nm. Furthermore, saturation behavior in the power-dependent studies and the associated lifetime change reveal the localized nature of the strain-induced states. These findings provide direct insights into the strain-localized emission dynamics in bubbles and establish a robust framework for non-destructive, reversible, and predictable nanoscale emission control, presenting a potential avenue for developing next-generation tunable quantum optical sources.

2D materials bubbles

Imaging nanoscale carrier, thermal, and structural dynamics with time-resolved and ultrafast electron energy-loss spectroscopy

Time-resolved and ultrafast electron energy-loss spectroscopy (EELS) is an emerging technique for measuring photoexcited carriers, lattice dynamics, and near-fields across femtosecond to microsecond timescales. When performed in either a specialized scanning transmission electron microscope or ultrafast electron microscope (UEM), time-resolved and ultrafast EELS can directly image charge carriers, lattice vibrations, and heat dissipation following photoexcitation or applied bias. Yet, recent advances in theoretical calculations and electron optics are often required to realize the full potential of ultrafast EEL spectrum imaging. Here, in this review, we present a comprehensive overview of the recent progress in the theory and instrumentation of time-resolved and ultrafast EELS. We begin with an introduction to the technique, followed by a physical description of the loss function. We outline approaches for calculating and interpreting ground-state and transient EEL spectra spanning low-loss plasmons to core-level excitations analogous to x-ray absorption. We then survey the current state of time-resolved and ultrafast EELS techniques beyond photon-induced near-field electron microscopy, highlighting abilities to image carrier and thermal dynamics. Finally, we examine future directions enabled by emerging technologies, including electron beam monochromation, in situ and operando cells, laser-free UEM, and high-speed direct electron detectors. These advances position time-resolved and ultrafast EELS as a critical tool for uncovering nanoscale dynamic processes in quantum materials and solar energy conversion devices.

Computational methods

Tracing terahertz plasmon polaritons with a tunable-by-design dispersion in topological insulator metaelements

Abstract Collective oscillations of massless charge carriers in two-dimensional materials—Dirac plasmon polaritons (DPPs)—are of paramount importance for engineering nanophotonic devices with tunable optical response. However, tailoring the optical properties of DPPs in a nanomaterial is a very challenging task, particularly at terahertz (THz) frequencies, where the DPP momentum is more than one order of magnitude larger than that of the free-space photons, and DDP attenuation is high. Here, we conceive and demonstrate a strategy to tune the DPP dispersion in topological insulator metamaterials. We engineer laterally coupled linear metaelements, fabricated from epitaxial Bi 2 Se 3, with selected coupling distances with the purpose to tune their wavevector, by geometry. We launch and directly map the propagation of DPPs confined within coupled meta-atoms via phase-sensitive scattering-type scanning near-field nanoscopy. We demonstrate that the DPP wavelength can be tuned by varying the metaelements coupling distance, resulting in up to a 20% increase of the polariton wavevector Re(k p ) in dimers and triplets with a 1 μm spacing, with reduced losses and a >50% increase of the polariton attenuation length.

Optics

Plasmonic Hybridization and Near-Field Localization in Gold “Dog Bone” Nanoparticles

Gold nanoparticles with complex anisotropic geometries offer unique opportunities for tailoring plasmonic near-fields beyond the limits of conventional nanorods. Here we combine photon-induced near-field electron microscopy (PINEM) and full-wave simulations to resolve plasmon hybridization and near-field localization in gold dog-bone nanoparticles and their dimers with and without conformal SiO 2 shells. We demonstrate that the dog-bone geometry drives unconventional polarization-dependent field confinement, including pronounced tip-localized near-fields under both longitudinal and transverse excitation. Conformal SiO 2 shells red-shift the plasmon resonances through dielectric screening and prevent charge-transfer coupling in adjacent dimers. Depending on the dimer orientation and excitation polarization, coupled structures exhibit distinct bonding- and antibonding-like hybridized modes as well as interparticle near-field channels. However, weakly interacting dimers retain largely independent particle responses with geometry-governed asymmetries. The close agreement between PINEM measurements and simulations establishes a direct picture of how shape, dielectric environment, and nanoscale coupling together define plasmonic modes in complex anisotropic nanoparticles. These findings provide design principles for engineering localized optical fields in plasmonic nanoscale structures.

hybridization

Purcell enhancement of directional edge photocurrent in a van der Waals self-cavity

Cavities provide a means to manipulate the optical and electronic responses of quantum materials by selectively enhancing light-matter interaction at specific frequencies and momenta. While cavities typically involve external structures, exfoliated flakes of van der Waals (vdW) materials can form intrinsic self-cavities due to their small finite dimensions, confining electromagnetic fields into plasmonic cavity modes, characterized by standing-wave current distributions. While cavity-enhanced phenomena are well-studied at optical frequencies, the impact of self-cavities on nonlinear electronic responses—such as directional photocurrent—remains largely unexplored, particularly in the terahertz regime, critical for emerging ultrafast optoelectronic technologies. Here, we report a self-cavity-induced Purcell enhancement of directional photocurrents in the vdW semimetal WTe 2 . Using ultrafast optoelectronic circuitry, we measured coherent near-field THz emission resulting from nonlinear photocurrents excited at the sample edges. We observed enhanced emission at finite frequencies, tunable via excitation fluence and sample geometry, which we attribute to plasmonic interference effects controlled by the cavity boundaries. We developed an analytical theory that captures the cavity resonance conditions and spectral response across multiple devices. Our findings establish WTe 2 as a bias-free, geometry-tunable THz emitter and demonstrate the potential of self-cavity engineering for controlling nonlinear, nonequilibrium dynamics in quantum materials.

condensed-matter physics

Laser-driven ultrafast transmission electron microscopy

Recent advances in lasers and electron optics technology have allowed transmission electron microscopes to achieve high spatial and temporal resolution, making them capable of tracking atoms, charges and spin motions down to the attosecond and nanometre scales. This Primer discusses the most common and practical experimental implementation of time-resolved transmission electron microscopy and the stroboscopic mode for evaluating ultrafast reversible dynamics. An in-depth discussion of photo-induced near-field electron microscopy, a technique unique to laser-assisted electron microscopy, is also provided, covering its prospective applications in the study of coherent phenomena in quantum materials. The experimental strategies and limitations in investigating the structural dynamics of materials and nanostructures by imaging, diffraction and spectroscopy are also described in detail, with a direct comparison with more conventional and established techniques. Here, we provide key information for new researchers who intend to use ultrafast transmission electron microscopy to address new challenges in specific materials science, condensed matter and nanophotonics.

Transmission electron microscopy

Artificial Soiling Replication of Field Losses on Commercial Photovoltaic Modules

Here, this study demonstrates the capabilities of an indoor artificial soiling approach developed to closely replicate the natural, cyclic soil accumulation processes in the field-dust suspension, deposition, and sedimentation/cementation-for a subtropical climate. In this work, a near-field environment is replicated in an artificial soiling cubic chamber through controlled regulation of humidity, temperature, dust type, and dust concentration, based on site-specific historical climate data. Two different models (MA and MB) of full-size commercial photovoltaic modules from a single manufacturer, installed side by side in the mid-Atlantic United States, were retrieved and subjected to artificial soiling experiments and various characterization measurements, including short-circuit current, colorimetry, reflectance, X-ray fluorescence, laser diffraction, and optical microscopy. Both in the field and in our improved field-representative artificial soiling tests, the MA model experienced roughly twice the soiling loss as the MB model. To closely replicate the field soiling losses for a site-specific climate, it is critical to include: 1) The use of field-collected dust with identical dust chemistry and particle distribution instead of standardized ISO 12103 Arizona Road dusts, 2) the use of only a small amount of field-collected dust inside the chamber during the deposition process (e.g., 0.15 g), and 3) the preconditioning of the surface coating for the partial/full dose of UV stress as experienced in the field during sunlight exposure and the abrasion as experienced in the field during regular module cleaning activities, if/as needed. The field-representative artificial soiling method developed here could potentially be adopted for rank ordering of various antisoiling coatings developed by researchers and industry stakeholders.

14 SOLAR ENERGY

Plasmon-enhanced ultralow-threshold solid-state triplet fusion upconversion

Triplet fusion upconversion has potential applications in solar cells, photoredox catalysis, additive manufacturing and bioimaging. However, solid-state upconversion systems have struggled to measure up to their solution-phase counterparts, often requiring enormous optical power densities to operate at the maximum efficiency. Here we substantially improve the performance of upconversion films through excitation with surface plasmons that propagate along a planar silver-film interface, leading to an absorption enhancement that reduces the intensity threshold I th by a factor of 19 and enhances the external quantum efficiency by a factor of 17. From this, we achieve I th values as low as 3.4 mW cm −2 and an external quantum efficiency up to 0.094%. To demonstrate real-world viability, we couple the upconversion film to plasmons generated by the near-field of excitons in an organic light-emitting diode. As a result, this scheme is then used to fabricate a white-emitting organic light-emitting diode where blue emission sources from plasmon-excited upconversion, achieving a high colour rendering index of 86.2 and setting precedent for blue emission in the absence of high-energy polarons or triplets.

36 MATERIALS SCIENCE

Plasmons Enable Ultralow Threshold Solid-State Triplet Fusion Upconversion with a 2D Sensitizer

Solid-state triplet−triplet annihilation (TTA) upconversion has significant potential for application in light harvesting, optoelectronic devices, and bioimaging. However, the high optical powers required to achieve efficient upconversion have inhibited its adoption. In this work, we demonstrate plasmon-enhanced near-infrared (NIR)-to-blue TTA upconversion in a monolayer WSe2/organic heterojunction. Under far-field excitation, the device reaches a threshold of 19 mW/cm 2 and an external quantum efficiency (EQE) of 0.17% with an anti-Stokes shift of 1.1 eV. Plasmon excitation lowers the threshold to 0.9 mW/cm 2 and improves the EQE to 3.6%. We attribute the plasmon enhancement to surface plasmon polariton (SPP) near-field enhancement and dark-exciton absorption. Optimization of the WSe 2 transfer process is identified as a key factor for the device performance. This work demonstrates that plasmon excitation overcomes the low far-field absorption of 2D transition-metal dichalcogenide (TMD) sensitizers. Consequently, monolayer TMDs can achieve solid-state upconversion with a performance among the best reported.

2D materials