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At least 271 records · Page 15

Magnetic Control of Soft Chiral Phonons in PbTe

We report PbTe crystals have a soft transverse optical phonon mode in the terahertz frequency range, which is known to efficiently decay into heat-carrying acoustic phonons, resulting in anomalously low thermal conductivity. Here, we studied this phonon via polarization-dependent terahertz spectroscopy. We observed softening of this mode with decreasing temperature, indicative of incipient ferroelectricity, which we explain through a model including strong anharmonicity with a quartic displacement term. In magnetic fields up to 25 T, the phonon mode splits into two modes with opposite handedness, exhibiting circular dichroism. Their frequencies display Zeeman splitting together with an overall diamagnetic shift with increasing magnetic field. Using a group-theoretical approach, we demonstrate that these observations are the result of magnetic field-induced morphic changes in the crystal symmetries through the Lorentz force exerted on the lattice ions. Thus, our Letter reveals a novel process of controlling phonon properties in a soft ionic lattice by a strong magnetic field.

36 MATERIALS SCIENCE↗

Probing Quantum Anomalous Hall States in Twisted Bilayer WSe 2 via Attractive Polaron Spectroscopy

Moiré superlattices in semiconductors exhibit a rich variety of interaction-induced topological states, including quantum anomalous Hall (QAH) effects. A recent study hinted that twisted WSe 2 homobilayer (tWSe 2 ) could host a QAH state but lacked direct evidence of ferromagnetism, a key hallmark of this phase. Here, we report the first direct evidence of QAH states in tWSe 2 with spontaneous ferromagnetism. Specifically, we employ polarization-resolved attractive polaron spectroscopy on a dual-gated, 2° tWSe 2 and observe direct signatures of spontaneous time-reversal symmetry breaking at hole filling 𝜈 = 1. Together with a Chern number (𝐶) measurement via Streda formula analysis, we identify this magnetized state as a topological state, characterized by 𝐶 = 1. Furthermore, we demonstrate that these topological and magnetic properties are tunable via a finite displacement field, between a QAH ferromagnetic state and an antiferromagnetic state. Our findings position tWSe 2 as a highly versatile, stable, and optically addressable platform for investigating topological order and strong correlations in two-dimensional landscapes.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Carrier-Envelope Phase Control in Terahertz Pulse Generation Using InAs Ribbon Metasurfaces

Generation of broadband terahertz (THz) pulses with variable polarization and carrier-envelope phase can enable the tailoring of THz beam wavefronts for advanced applications in THz imaging and spectroscopy and for strong THz field optics. While metasurfaces composed of deeply subwavelength THz emitters have recently been demonstrated to define the polarization and spatial profile of the generated THz fields, precise phase control or synthesis of THz pulse waveforms remains a challenging problem. Here, we propose and demonstrate metasurfaces composed of indium arsenide (InAs) nanoscale ribbon arrays capable of generating THz pulses with variable carrier-envelope phase. We show that different THz generation mechanisms, each contributing distinct phases, can be activated in the ribbons, enabling carrier-envelope phase control spanning a range of π over a wide band of frequencies (∼1–3 THz). This is achieved solely through the ribbon array geometry using linearly polarized optical excitation of the ribbons. The arrays enable precise control of the THz phase and amplitude, opening the door to advanced structured THz wavefront synthesis using ultrathin dielectric metasurfaces.

carrier-envelope phase↗

Domain-dependent strain and stacking in two-dimensional van der Waals ferroelectrics

Van der Waals (vdW) ferroelectrics have attracted significant attention for their potential in next-generation nano-electronics. Two-dimensional (2D) group-IV monochalcogenides have emerged as a promising candidate due to their strong room temperature in-plane polarization down to a monolayer limit. However, their polarization is strongly coupled with the lattice strain and stacking orders, which impact their electronic properties. Here, we utilize four-dimensional scanning transmission electron microscopy (4D-STEM) to simultaneously probe the in-plane strain and out-of-plane stacking in vdW SnSe. Specifically, we observe large lattice strain up to 4% with a gradient across ~50 nm to compensate lattice mismatch at domain walls, mitigating defects initiation. Additionally, we discover the unusual ferroelectric-to-antiferroelectric domain walls stabilized by vdW force and may lead to anisotropic nonlinear optical responses. Our findings provide a comprehensive understanding of in-plane and out-of-plane structures affecting domain properties in vdW SnSe, laying the foundation for domain wall engineering in vdW ferroelectrics.

42 ENGINEERING↗

Single-particle detection of enhanced polarizability in Au-decorated semiconducting nanorods via scanning dielectric microscopy

Hybrid nanostructures that combine semiconducting and metallic components offer great potential for photothermal therapy, optoelectronics, and sensing, by integrating tunable optical properties with enhanced light absorption and charge transport. Boosting the integrated performance of these hybrid systems demands techniques capable of probing local variations of the physical properties inaccessible to bulk analysis. Here, we report the single-particle dielectric characterization of hybrid, semiconducting bismuth sulfide (Bi 2 S 3 ) nanorods (NR) decorated with metallic Au nanoparticles (NP), employing scanning dielectric microscopy, which uses electrostatic force microscopy in combination with finite-element numerical simulations. We reveal a pronounced enhancement in the local dielectric response of Bi2S3 upon Au decoration, attributed to interfacial polarization and electron transfer from Au to the Bi 2 S 3 matrix, thus suggesting a enhanced metallic-like polarizability at the single-particle level. Numerical simulations show that the response is dominated by the vertical component of the permittivity and that the decorating metallic Au NP produce only moderate shielding of the semiconductor Bi 2 S 3 NR core, indicating that the large increase in the dielectric response originates primarily from intrinsic modifications within the NR. Overall, these findings provide direct insight into structure–property relationships at the single-particle level, supporting the rational design of advanced hybrid nanostructures with tailored electronic functionalities.

36 MATERIALS SCIENCE↗

Topological nanophotonics for photoluminescence control

Rare-earth-doped nanocrystals are emerging light sources that can produce tunable emissions in colours and lifetimes, which has been typically achieved in chemistry and material science. However, one important optical challenge – polarization of photoluminescence – remains largely out of control by chemistry methods. Control over photoluminescence polarization can be gained via coupling of emitters to resonant nanostructures such as optical antennas and metasurfaces. However, the resulting polarization is typically sensitive to position disorder of emitters, which is difficult to mitigate. Recently, new classes of disorder-immune optical systems have been explored within the framework of topological photonics. Here we explore disorder-robust topological arrays of Mie-resonant nanoparticles for polarization control of photoluminescence of nanocrystals. We demonstrate polarized emission from rare-earth-doped nanocrystals governed by photonic topological edge states supported by zigzag arrays of dielectric resonators. We verify the topological origin of polarized photoluminescence by comparing emission from nanoparticles coupled to topologically trivial and nontrivial arrays of nanoresonators. We expect that our results may open a new direction in the study of topology-enable emission properties of topological edge states in many photonic systems.

36 MATERIALS SCIENCE↗

Growth of Large‐Sized 2D Ultrathin SnSe Crystals with In‐Plane Ferroelectricity

Abstract Tin (II) selenide (SnSe) is an emerging 2D material with many intriguing properties, such as record‐high thermoelectric figure of merit (ZT), purely in‐plane ferroelectricity, and excellent nonlinear optical properties. To explore these functional properties and related applications, a crucial step is to develop controllable routes to synthesize large‐area, ultrathin, and high‐quality SnSe crystals. Physical vapor deposition (PVD) constitutes a reliable method to synthesize 2D SnSe, however, effects of various growth parameters have not yet been systematically investigated, and current PVD‐synthesized flakes are often thick (>10 nm) with small lateral sizes (<10 µm). In this work, high‐quality 2D SnSe crystals are synthesized via low‐pressure PVD, which display in‐plane ferroelectric domains observed by piezoresponse force microscopy and polarization‐dependent reflection spectroscopy. Detailed studies regarding the roles of various parameters are further carried out, including substrate pre‐annealing, growth duration, temperature, and pressure, which enable to rationally optimize the growth and obtain 2D SnSe crystals with lateral sizes up to ≈23.0 µm and thicknesses down to ≈2.0 nm (3–4 layers). This work paves the way for the controlled growth of large‐area 2D SnSe, facilitating the future exploration of many interesting multiferroic properties and applications with atomic thickness.

2D materials↗

Anomalous neutron nuclear-magnetic interference spectroscopy

The electron–phonon interaction plays a critical role in materials’ electrical, thermal, optical, and superconducting properties. However, measuring the phonon mode-resolved electron–phonon interaction has been challenging. Here we propose neutron-scattering-based Anomalous Neutron nUclear-Magnetic Interference Spectroscopy (ANUBIS), where the co-existence of neutron nuclear scattering and magnetic scattering leads to anomalous dynamical structure factor under the presence of the electron–phonon interaction. Such anomalous structure factor is linear in electron–phonon coupling constant at the phonon wavevector, and is directly proportional to the momentum and energy-resolved dielectric function. The experimental configuration can be achieved using existing polarized inelastic neutron scattering setup, and an order-of-magnitude estimate shows the viability to observe the anomalous scattering signal is around to 10 –4 to 10 –3 relative to phonon scattering, which is examined through the preliminary experiments and achievable at emerging neutron facilities. As a result, our proposal offers an alternative neutron-based metrology to probe the crucial electronic properties.

Electron-phonon interactions↗

Charge carrier coupling to the soft phonon mode in a ferroelectric semiconductor

Many crystalline solids possess strongly anharmonic “soft” phonon modes characterized by diminishing frequency as temperature approaches a critical point associated with a symmetry breaking phase transition. While electron–soft phonon coupling can introduce unique scattering channels for charge carriers in ferroelectrics, recent studies on the nonferroelectric lead halide perovskites have also suggested the central role of anharmonic phonons bearing resemblance to soft modes in charge carrier screening. Here we apply coherent phonon spectroscopy to directly study electron coupling to the soft transverse optical phonon mode in a ferroelectric semiconductor SbSI. Photogenerated charge carriers in SbSI are found to be exceptionally long lived and are associated with a transient electro-optical effect that can be explained by interactions between charge carriers and thermally stimulated soft phonon excitations. Furthermore, these results provide strong evidence for the role of electron–soft phonon coupling in the efficient screening of charge carriers and in reducing charge recombination rates, both desirable properties for optoelectronics.

36 MATERIALS SCIENCE↗

Tunable Electronic Energy Level Alignment and Exciton Diversity in Organic–Inorganic van der Waals Heterostructures

van der Waals stacking of two-dimensional (2D) materials offers a powerful platform for engineering material interfaces with tailored electronic and optical properties. While most van der Waals multilayers have featured inorganic monolayers, incorporating molecular monolayers introduces additional degrees of tunability and functionality. Here, in this study, we investigate hybrid bilayers composed of atomically thin perylene-based molecular crystals interfaced with monolayer transition metal dichalcogenides (TMDs), specifically MoS 2 and WS 2 . Using the ab initio many-body perturbation theory within the GW approximation and the Bethe-Salpeter equation approach, we predict emergent properties beyond those of the isolated constituent systems. Notably, we find substantial renormalization of monolayer molecular crystal band gap due to TMD-induced polarization. Furthermore, by varying the TMD monolayer, we demonstrate tuning of the energy level alignment of the bilayer and subsequent control over a diversity of lowest-energy excitons, which include strongly bound hybrid excitons and long-lived charge-transfer excitons. These findings establish organic-inorganic van der Waals heterostructures as a promising class of materials for tunable optoelectronic devices and quantum excitonic phenomena, expanding the design space for low-dimensional systems.

GW-BSE calculations↗

The Simons Observatory: science goals and forecasts for the enhanced Large Aperture Telescope

We describe updated scientific goals for the wide-field, millimeter-wave survey that will be produced by the Simons Observatory (SO). Significant upgrades to the 6-meter SO Large Aperture Telescope (LAT) are expected to be complete by 2028, and will include a doubled mapping speed with 30,000 new detectors and an automated data reduction pipeline. In addition, a new photovoltaic array will supply most of the observatory's power. The LAT survey will cover about 60% of the sky at a regular observing cadence, with five times the angular resolution and ten times the map depth of the Planck satellite. The science goals are to: (1) determine the physical conditions in the early universe and constrain the existence of new light particles; (2) measure the integrated distribution of mass, electron pressure, and electron momentum in the late-time universe, and, in combination with optical surveys, determine the neutrino mass and the effects of dark energy via tomographic measurements of the growth of structure at redshifts z ≲ 3; (3) measure the distribution of electron density and pressure around galaxy groups and clusters, and calibrate the effects of energy input from galaxy formation on the surrounding environment; (4) produce a sample of more than 30,000 galaxy clusters, and more than 100,000 extragalactic millimeter sources, including regularly sampled AGN light-curves, to study these sources and their emission physics; (5) measure the polarized emission from magnetically aligned dust grains in our Galaxy, to study the properties of dust and the role of magnetic fields in star formation; (6) constrain asteroid regoliths, search for Trans-Neptunian Objects, and either detect or eliminate large portions of the phase space in the search for Planet 9; and (7) provide a powerful new window into the transient universe on time scales of minutes to years, concurrent with observations from the Vera C. Rubin Observatory of overlapping sky.

79 ASTRONOMY AND ASTROPHYSICS↗

Room-temperature high-purity single-photon emission from carbon-doped boron nitride thin films

Hexagonal boron nitride (h-BN) has emerged as a promising platform for generating room temperature single photons exhibiting high brightness and spin-photon entanglement. However, improving emitter purity, stability, and scalability remains a challenge for quantum technologies. Here, we demonstrate highly pure and stable single-photon emitters (SPEs) in h-BN by directly growing carbon-doped, centimeter-scale h-BN thin films using the pulsed laser deposition (PLD) method. These SPEs exhibit room temperature operation with polarized emission, achieving a g (2) (0) value of 0.015, which is among the lowest reported for room temperature SPEs and the lowest achieved for h-BN SPEs. It also exhibits high brightness (~0.5 million counts per second), remarkable stability during continuous operation (>15 min), and a Debye-Waller factor of 45%. First-principles calculations reveal unique carbon defects responsible for these properties, enabled by PLD’s low-temperature synthesis and in situ doping. Our results demonstrate an effective method for large-scale production of high-purity, stable SPEs in h-BN, enabling robust quantum optical sources for various quantum applications.

36 MATERIALS SCIENCE↗

A physically unclonable function using NV diamond magnetometry and micromagnet arrays

A physically unclonable function (PUF) is an embedded hardware security measure that provides protection against counterfeiting. In this article, we present our work on using an array of randomly magnetized micrometer-sized ferromagnetic bars (micromagnets) as a PUF. We employ a 4μm thick surface layer of nitrogen-vacancy (NV) centers in diamond to image the magnetic field from each micromagnet in the array, after which we extract the magnetic polarity of each micromagnet using image analysis techniques. Finally, after evaluating the randomness of the micromagnet array PUF and the sensitivity of the NV readout, we conclude by discussing the possible future enhancements for improved security and magnetic readout.

Electromagnetism↗

Real-Time Alignment and Reorientation of Polymer Chains in Liquid Crystal Elastomers

Liquid crystal elastomers (LCEs) exhibit soft elasticity due to the alignment and reorientation of mesogens upon mechanical loading, which provides additional mechanisms to absorb and dissipate energy. This enhanced response makes LCEs potentially transformative materials for biomedical devices, tissue replacements, and protective equipment. However, there is a critical knowledge gap in understanding the highly rate-dependent dissipative behaviors of LCEs due to the lack of real-time characterization techniques that probe the microscale network structure and link it to the mechanical deformation of LCEs. In this work, we employ in situ optical measurements to evaluate the alignment and reorientation degree of mesogens in LCEs. The data are correlated to the quantitative physical analysis using polarized Fourier-transform infrared spectroscopy. The time scale of mesogen alignment is determined at different strain levels and loading rates. The mesogen reorientation kinetics is characterized to establish its relationship with the macroscale tensile strain, and compared to theoretical predictions. Overall, this work provides the first detailed study on the time-dependent evolution of mesogen alignment and reorientation in deformed LCEs. It also provides an effective and more accessible approach for other researchers to investigate the structural-property relationships of different types of polymers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Emergent Above-Gap Photoluminescence in Molecularly Engineered Hybrid Bilayer Crystals

Bilayer crystals, built by stacking two-dimensional (2D) covalent monolayers, give rise to coupled excitonic states whose properties are constrained by fixed lattice symmetry and orientation. Replacing one covalent monolayer with a 2D molecular crystal––held together by non-covalent forces––overcomes this limitation, as molecular functional groups afford tunable in-plane lattice geometry, intermolecular spacing, and interlayer coupling, providing a powerful knob for exciton engineering. Here, in this study, we report four-atom-thick hybrid bilayer crystals (HBCs) synthesized by directly growing single-crystalline PDI molecular crystal atop WS 2 monolayers, which exhibit a robust photoluminescence (PL) peak 120 meV above the WS 2 optical band gap alongside a belowgap emission. Both peaks display strong polarization anisotropy—nearing unity for the above-gap emission—and maintain a perfectly linear power-law dependence up to an excitation density of ~10 7 mW/cm 2 , indicative of coexisting localized and delocalized excitonic states. Substituting PDI with a PTCDA monolayer on WS 2 fully quenches PL, demonstrating molecular control over excitonic emission. Lattice scale ab initio GW and GW-BSE calculations reveal a significantly hybridized bilayer band structure in PDI/WS 2 that supports interlayer excitonic species both above and below the WS 2 gap with strong polarization anisotropy, in excellent agreement with experiment. Our work introduces a molecule-based bilayer platform for the bottom-up design and control of excitonic phenomena in atomically thin optoelectronic and quantum materials.

2D materials↗

Aerosol Optical Tweezers Elucidate the Chemistry, Acidity, Phase Separations, and Morphology of Atmospheric Microdroplets

Aerosol particles represent unique chemical environments because of their high surface area-to-volume ratio that promotes the effects of interfacial chemistry in confined environments. Properties such as viscosity, diffusivity, water content, pH, and morphology—following liquid–liquid phase separation—can strongly alter how a particle interacts with condensable vapors and reactive trace gases, thus modifying its continual evolution and environmental effects. Our understanding of this chemical evolution of atmospheric particulate matter and its environmental impacts is largely limited by our ability to directly observe how these critical particle properties respond to the addition or reactive uptake of new chemical components. Aerosol optical tweezers (AOT) stably trap particles in focused laser beams, providing positional control and the retrieval of many of these critical properties required to understand and predict the chemistry of aerosolized microdroplets. The analytical power of the AOT stems from the retrieval of the cavity-enhanced Raman spectrum induced by the trapping laser. Analysis of the whispering gallery modes (WGMs) that resonate as a standing wave around the droplet’s interface, provide high accuracy measurements of the droplet’s size, refractive index (and thus a measurement of composition), and can distinguish between core–shell, partially engulfed, and homogeneous morphologies. In this study, we have advanced the ability to determine the properties of the core and shell phases in biphasic droplets, including obtaining high-accuracy pH measurements. These capabilities were applied to perform AOT physical chemistry experiments on authentic secondary organic aerosol (SOA) produced directly in the AOT chamber by ozonolysis of terpene vapors. The propensity of the SOA to phase separate as a shell from a wide range of nonpolar to polar core phases was observed, along with the discovery of a stable emulsified state of SOA particles in an aqueous salt droplet. Micron-thick SOA shells did not impede the gain or loss of water or squalane from the core to the surrounding air, indicating no significant diffusional limitations to condensational growth or partitioning even under dry conditions. These experiments formed the foundation of a new framework that predicts how the phase-separated morphology of complex aerosols containing organic carbon evolves during continual atmospheric oxidation processes. Increases in oxidation state will quickly drive conversion from a partially engulfed to core–shell morphology that has dramatically different chemical reactivity since the core phase is completely concealed by the shell. The recent advances in the experimental capabilities of the AOT technique such as presented here enable novel experimental methodologies that provide insights into the chemistry and multidimensional properties of aerosol microdroplets, and how these coevolve and respond to continual chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atomic-scale polarization switching in wurtzite ferroelectrics

Ferroelectric wurtzites have the potential to revolutionize modern microelectronics because they are easily integrated with multiple mainstream semiconductor platforms. However, the electric fields required to reverse their polarization direction and unlock electronic and optical functions need substantial reduction for operational compatibility with complementary metal-oxide semiconductor (CMOS) electronics. To understand this process, we observed and quantified real-time polarization switching of a representative ferroelectric wurtzite (Al 0.94 B 0.06 N) at the atomic scale with scanning transmission electron microscopy. The analysis revealed a polarization reversal model in which puckered aluminum/boron nitride rings in the wurtzite basal planes gradually flatten and adopt a transient nonpolar geometry. Independent first-principles simulations reveal the details and energetics of the reversal process through an antipolar phase. Furthermore, this model and local mechanistic understanding are a critical initial step for property engineering efforts in this emerging material class.

36 MATERIALS SCIENCE↗

Noncentrosymmetric Triangular Magnet CaMnTeO 6 : Strong Quantum Fluctuations and Role of s 0 versus s 2 Electronic States in Competing Exchange Interactions

Abstract Noncentrosymmetric triangular magnets offer a unique platform for realizing strong quantum fluctuations. However, designing these quantum materials remains an open challenge attributable to a knowledge gap in the tunability of competing exchange interactions at the atomic level. Here, a new noncentrosymmetric triangular S = 3/2 magnet CaMnTeO 6 is created based on careful chemical and physical considerations. The model material displays competing magnetic interactions and features nonlinear optical responses with the capability of generating coherent photons. The incommensurate magnetic ground state of CaMnTeO 6 with an unusually large spin rotation angle of 127°(1) indicates that the anisotropic interlayer exchange is strong and competing with the isotropic interlayer Heisenberg interaction. The moment of 1.39(1) µB , extracted from low‐temperature heat capacity and neutron diffraction measurements, is only 46% of the expected value of the static moment 3 µB . This reduction indicates the presence of strong quantum fluctuations in the half‐integer spin S = 3/2 CaMnTeO 6 magnet, which is rare. By comparing the spin‐polarized band structure, chemical bonding, and physical properties of AMnTeO 6 ( A = Ca, Sr, Pb), how quantum‐chemical interpretation can illuminate insights into the fundamentals of magnetic exchange interactions, providing a powerful tool for modulating spin dynamics with atomically precise control is demonstrated.

36 MATERIALS SCIENCE↗