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At least 253 records · Page 14

Structural Phase Transitions between Layered Indium Selenide for Integrated Photonic Memory

The primary mechanism of optical memoristive devices relies on phase transitions between amorphous and crystalline states. The slow or energy-hungry amorphous–crystalline transitions in optical phase-change materials are detrimental to the scalability and performance of devices. Leveraging an integrated photonic platform, nonvolatile and reversible switching between two layered structures of indium selenide (In 2 Se 3 ) triggered by a single nanosecond pulse is demonstrated. The high-resolution pair distribution function reveals the detailed atomistic transition pathways between the layered structures. With interlayer “shear glide” and isosymmetric phase transition, switching between the α- and β-structural states contains low re-configurational entropy, allowing reversible switching between layered structures. Broadband refractive index contrast, optical transparency, and volumetric effect in the crystalline–crystalline phase transition are experimentally characterized in molecular-beam-epitaxy-grown thin films and compared to ab initio calculations. Finally, the nonlinear resonator transmission spectra measure of incremental linear loss rate of 3.3 GHz, introduced by a 1.5 µm-long In 2 Se 3 -covered layer, resulted from the combinations of material absorption and scattering.

36 MATERIALS SCIENCE↗

Tailoring the Thickness‐Dependent Optical Properties of Conducting Nitrides and Oxides for Epsilon‐Near‐Zero‐Enhanced Photonic Applications

Abstract The unique properties of the emerging photonic materials, conducting nitrides and oxides, especially their tailorability, large damage thresholds, and, importantly, the so‐called epsilon‐near‐zero (ENZ) behavior, have enabled novel photonic phenomena spanning optical circuitry, tunable metasurfaces, and nonlinear optical devices. This work explores direct control of the optical properties of polycrystalline titanium nitride (TiN) and aluminum‐doped zinc oxide (AZO) by tailoring the film thickness, and their potential for ENZ‐enhanced photonic applications. This study demonstrates that TiN–AZO bilayers support Ferrell–Berreman modes using the thickness‐dependent ENZ resonances in the AZO films operating in the telecom wavelengths spanning from 1470 to 1750 nm. The bilayer stacks also act as strong light absorbers in the ultraviolet regime using the radiative ENZ modes and the Fabry–Perot modes in the constituent TiN films. The studied Berreman resonators exhibit optically induced reflectance modulation of 15% with picosecond response time. Together with the optical response tailorability of conducting oxides and nitrides, using the field enhancement near the tunable ENZ regime can enable a wide range of nonlinear optical phenomena, including all‐optical switching, time refraction, and high‐harmonic generation.

Saha, Soham↗

Silicon-Lattice-Matched Boron-Doped Gallium Phosphide: A Scalable Acousto-Optic Platform

The compact size, scalability, and strongly confined fields in integrated photonic devices enable new functionalities in photonic networking and information processing, both classical and quantum. Gallium phosphide (GaP) is a promising material for active integrated photonics due to its high refractive index, wide bandgap, strong nonlinear properties, and large acousto-optic figure of merit. Here, this study demonstrates that silicon-lattice-matched boron-doped GaP (BGaP), grown at the 12-inch wafer scale, provides similar functionalities as GaP. BGaP optical resonators exhibit intrinsic quality factors exceeding 25,000 and 200,000 at visible and telecom wavelengths, respectively. It further demonstrates the electromechanical generation of low-loss acoustic waves and an integrated acousto-optic (AO) modulator. High-resolution spatial and compositional mapping, combined with ab initio calculations, indicate two candidates for the excess optical loss in the visible band: the silicon-GaP interface and boron dimers. These results demonstrate the promise of the BGaP material platform for the development of scalable AO technologies at telecom and provide potential pathways toward higher performance at shorter wavelengths.

36 MATERIALS SCIENCE↗

Tunable Phonon Polariton Hybridization in a Van der Waals Hetero‐Bicrystal

Abstract Phonon polaritons, the hybrid quasiparticles resulting from the coupling of photons and lattice vibrations, have gained significant attention in the field of layered van der Waals heterostructures. Particular interest has been paid to hetero‐bicrystals composed of molybdenum oxide (MoO 3 ) and hexagonal boron nitride (hBN), which feature polariton dispersion tailorable via avoided polariton mode crossings. In this work, the polariton eigenmodes in MoO 3 ‐hBN hetero‐bicrystals self‐assembled on ultrasmooth gold are systematically studied using synchrotron infrared nanospectroscopy. It is experimentally demonstrated that the spectral gap in bicrystal dispersion and corresponding regimes of negative refraction can be tuned by material layer thickness, and these results are quantitatively matched with a simple analytic model. Polaritonic cavity modes and polariton propagation along “forbidden” directions are also investigated in microscale bicrystals, which arise from the finite in‐plane dimension of the synthesized MoO 3 micro‐ribbons. The findings shed light on the unique dispersion properties of polaritons in van der Waals heterostructures and pave the way for applications leveraging deeply sub‐wavelength mid‐infrared light‐matter interactions.

36 MATERIALS SCIENCE↗

Stoichiometric Control and Optical Properties of BaTiO 3 Thin Films Grown by Hybrid MBE

BaTiO 3 is a technologically relevant material in the perovskite oxide class with above-room-temperature ferroelectricity and a very large electro-optical coefficient, making it highly suitable for emerging electronic and photonic devices. An easy, robust, straightforward, and scalable growth method is required to synthesize epitaxial BaTiO 3 thin films with sufficient control over the film's stoichiometry to achieve reproducible thin film properties. Here the growth of BaTiO 3 thin films by hybrid molecular beam epitaxy is reported. A self-regulated growth window is identified using complementary information obtained from reflection high energy electron diffraction, the intrinsic film lattice parameter, film surface morphology, and scanning transmission electron microscopy. Subsequent optical characterization of the BaTiO 3 films by spectroscopic ellipsometry revealed refractive index and extinction coefficient values closely resembling those of stoichiometric bulk BaTiO 3 crystals for films grown inside the growth window. Even in the absence of a lattice parameter change of BaTiO 3 thin films, degradation of optical properties is observed, accompanied by the appearance of a wide optical absorption peak in the IR spectrum, attributed to optical transitions involving defect states present. Therefore, the optical properties of BaTiO 3 can be utilized as a much finer and more straightforward probe to determine the stoichiometry level present in BaTiO 3 films.

36 MATERIALS SCIENCE↗

Active Tuning of Optical Constants in the Visible–UV: Praseodymium-Doped Ceria—a Model Mixed Ionic–Electronic Conductor

Mixed ionic-electronic conductors offer chemical and electrical means for active tuning of their optical constants, e.g. with variations in oxygen non-stoichiometry in Pr 0.1 Ce 0.9 O 2-δ , enabling implementation of adaptive thin film optical devices. Here, we demonstrate in-situ chemo-tuning of the extinction coefficient in Pr 0.1 Ce 0.9 O 2-δ at elevated temperatures and provide a tuning model that treats the interdependence of mobile oxygen vacancies and small polarons coupled to variations in optically active praseodymium ions. Further, a new means for electro-tuning of the optical constants of mixed ionic-electronic conductors was demonstrated experimentally and modeled for Pr 0.1 Ce 0.9 O 2-δ thin films deposited on grid-like electrode structures. Modeling of non-steady state optical transmittance modulations in the latter allows for estimation of oxygen vacancy mobility that determines the switching speed of the device. Quenched-in values of nr and k to room temperature become nonvolatile, providing a modulation range in the extinction coefficient of Δk ~0.1 (change of ~800%) and in the refractive index of Δn r ~0.1 (relative to initial n r of ~2.35). Key figures of merit including, transmission optical modulation of ~0.04 per 1 mV nm -1 , switching energy per area of 670 pJ μm -2 and switching times of seconds, were demonstrated, with further improvements possible.

36 MATERIALS SCIENCE↗

Structural Color Production in Melanin-Based Disordered Colloidal Nanoparticle Assemblies in Spherical Confinement

Melanin is a ubiquitous natural pigment that exhibits broadband absorption and high refractive index. Despite its widespread use in structural color production, how the absorbing material, melanin, affects the generated color is unknown. Using a combined molecular dynamics and finite-difference time-domain computational approach, here we investigates structural color generation in one-component melanin nanoparticle-based supraparticles (called supraballs) as well as binary mixtures of melanin and silica (nonabsorbing) nanoparticle-based supraballs. Experimentally produced one-component melanin and one-component silica supraballs, with thoroughly characterized primary particle characteristics using neutron scattering, produce reflectance profiles similar to the computational analogs, confirming that the computational approach correctly simulates both absorption and multiple scattering from the self-assembled nanoparticles. These combined approaches demonstrate that melanin's broadband absorption increases the primary reflectance peak wavelength, increases saturation, and decreases lightness factor. Additionally, the dispersity of nanoparticle size more strongly influences the optical properties of supraballs than packing fraction, as evidenced by the production of a larger range of colors when size dispersity is varied versus packing fraction. For binary melanin and silica supraballs, the chemistry-based stratification allows for more diverse color generation and finer saturation tuning than does the degree of mixing/demixing between the two chemistries.

broadband absorption↗

Aggregation‐Induced Stimulated Emission of 100% Dye Microspheres

Dyes with aggregation-induced emission (AIE) properties have gained interest due to their bright luminescence in solid-state aggregates. While fluorescence from AIE dyes is widely exploited, relatively little is known about aggregation-induced stimulated emission. Here, stimulated emission of tetraphenylethene (TPE)-based organoboron AIE dyes, TPEQBN, in thin films and in microcavity lasers is investigated. Using femtosecond pump–probe spectroscopy, gain coefficients up to 230 cm -1 at 500 nm are measured. Using rate equations, concentration- and pump-dependent gain dynamics as well as laser build-up dynamics are analyzed. During laser oscillation, radiative stimulated emission allows high instantaneous quantum yield greater than 90% to be achieved. Solid-state microspheres made of 100% AIE dyes are fabricated via microfluidic emulsion and solvent evaporation method. Coupled with high gain and high refractive index of 1.76, microspheres as small as 2 µm in diameter show lasing by nanosecond pumping with a threshold of ≈10 pJ µm –2 . Polymer coated, but not bare, microspheres are internalized by live cells and generate narrowband cavity-mode emission from within the cytoplasm. This work shows the potential of AIE dyes as laser materials.

36 MATERIALS SCIENCE↗

Infrared Optical Anisotropy in Quasi‐1D Hexagonal Chalcogenide BaTiSe 3

Polarimetric infrared (IR) detection bolsters IR thermography by leveraging the polarization of light. Optical anisotropy, i.e., birefringence and dichroism, can be leveraged to achieve polarimetric detection. Recently, giant optical anisotropy is discovered in quasi-1D narrow-bandgap hexagonal perovskite sulfides, A 1+x TiS 3 , specifically BaTiS 3 and Sr 9/8 TiS 3 . In these materials, the critical role of atomic-scale structure modulations in the unconventional electrical, optical, and thermal properties raises the broader question of the nature of other materials that belong to this family. To address this issue, for the first time, high-quality single crystals of a largely unexplored member of the A 1+x TiX 3 (X = S, Se) family, BaTiSe 3 are synthesized. Single-crystal X-ray diffraction determined the room-temperature structure with the P31c space group, which is a superstructure of the earlier reported P6 3 /mmc structure. The crystal structure of BaTiSe 3 features antiparallel c-axis displacements similar to but of lower symmetry than BaTiS 3 , verified by the polarization dependent Raman spectroscopy. Fourier transform infrared (FTIR) spectroscopy is used to characterize the optical anisotropy of BaTiSe 3 , whose refractive index along the ordinary (E ⊥ c) and extraordinary (E ‖ c) optical axes is quantitatively determined by combining ellipsometry studies with FTIR. With a giant birefringence Δn ∼ 0.9, BaTiSe 3 emerges as a new candidate for miniaturized birefringent optics for mid-wave infrared to long-wave infrared imaging.

optical anisotropy↗

Broadband‐Tunable Third‐Harmonic Generation Using Phase‐Change Chalcogenides

Despite remarkable progress in passive nonlinear nanophotonics, dynamically controlled ultracompact nonlinear optical sources with high efficiency remain elusive. Nonvolatility, large refractive index contrast between amorphous and crystalline phases, low thermal threshold for crystallization, and particularly high‐third‐order nonlinear optical susceptibility of phase‐change alloy Ge 2 Sb 2 Te 5 (GST) make it a promising candidate for active subwavelength metaphotonic structures for realization of third‐harmonic generation (THG) devices. Herein, a GST‐based asymmetric Fabry–Perot cavity is numerically designed and experimentally demonstrated to show a dynamically reconfigurable structure with a large shift of the THG resonant band. In addition, continuous resonant spectral shifting bridged by a precisely controlled semicrystalline phase of GST is realized. Tunable THG with the fundamental wavelength ranging from 1150 to 1400 nm is presented, which corresponds to a broadband THG source in the violet‐blue visible wavelength range. Herein, the potential of GST subwavelength structures as a reliable platform for realization of the broadband‐tunable frequency‐conversion sources for applications such as THG microscopy and optical communication is indicated.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Imaging Photonic Resonances within an All‐Dielectric Metasurface via Photoelectron Emission Microscopy

Dielectric metasurfaces, through volume‐type photonic resonances, enable precise control of light‐matter interactions for applications including imaging, holography, and sensing. The application space of dielectric metasurfaces has extended from infrared to visible wavelengths by incorporating high refractive index materials, such as titanium dioxide (TiO 2 ). Understanding the fundamental and fabrication limits for these applications requires metrology with nanoscale resolution, sensitivity to electromagnetic fields within the meta‐atom volume, and far‐field excitation. In this work, photoelectron emission microscopy (PEEM) is used to image field distributions of photonic resonances in a TiO 2 metasurface excited with far‐field, visible‐wavelength illumination. The local volumetric field variations within the meta‐atoms are analyzed as a function of illumination angle and polarization by comparing photoelectron images to finite‐difference time‐domain simulations. This study determines the inelastic mean free path of very low‐energy (<1 eV) photoelectrons to be 35 ± 10 nm, which is comparable to the meta‐atom height thereby highlighting PEEM sensitivity to resonances within the volume. Additionally, the simulations reveal high sensitivity of PEEM images to an in‐plane component of the illumination k ‐vector. These results demonstrate that photoelectron imaging with subwavelength resolution offers unique advantages for examining light‐matter interactions in volume‐type (as opposed to surface) photonic modes within dielectric nanophotonic structures.

electron inelastic mean free path↗

Smart connected worker edge platform for smart manufacturing: Part 2—Implementation and on‐site deployment case study

Abstract In this paper, we describe specific deployments of the Smart Connected Worker (SCW) Edge Platform for Smart Manufacturing through implementation of four instructive real‐world use cases that illustrate the role of people in a Smart Manufacturing paradigm through which affordable, scalable, accessible, and portable (ASAP) information technology (IT) acquires and contextualizes data into information for transmission to operation technologies (OT). For case one, the platform captures the relationships between energy consumption and human workflows for improved energy productivity while workers interact with machines during semiconductor manufacturing. The platform utilizes human cognition to identify anomalous machine behavior for root cause analysis of system faults via neural network (NN) that recognize alarm postures of workers with cameras. For case two, a smart assembly line is demonstrated for state monitoring and fault detection. Machine learning (ML) models are used to recognize system states and identify fault scenarios with human intervention. For case three, the platform monitors human–machine interactions to classify manufacturing machine states for proper operations and energy productivity. Internal energy states of individual or collections of manufacturing equipment are determined via NN based algorithms that disaggregate signals associated with smart metering typically deployed at manufacturing facilities. These methods predict the real time energy profile of each machine from the total energy profile of a manufacturing site. For case four, a software defined sensor system built with scientific workflow engines is demonstrated for contextualizing data from laser surface refraction for characterization, and diagnostics in the processing of additively manufactured titanium alloy.

Donovan, Richard P.↗

Improving vertical detail in simulated temperature and humidity data using machine learning

Atmospheric models used for weather forecasting and climate predictions discretise the atmosphere onto a vertical grid. There are however atmospheric phenomena that occur on scales smaller than the thickness of those model layers. The formation of low-level clouds due to temperature inversions is an example. This leads to atmospheric models underestimating, or even missing, these clouds and their radiative effects. Using radiosonde observations as training data, a machine learning model is used to improve the vertical detail of modelled profiles of temperature and specific humidity. In addition, a physics-informed machine learning model is developed and compared to the traditional approach; showing improvements in the cloud fraction profiles calculated from its predictions. The vertically enhanced profiles also improve the representation of layers of convective inhibition and anomalous refractivity gradients. This work facilitates targeted improvements to the representation of certain atmospheric processes without the burden of increased memory and computational cost from increasing vertical resolution throughout the whole model.

54 ENVIRONMENTAL SCIENCES↗

Applicability of 1D site response analysis to shallow sedimentary basins: A critical evaluation through physics-based 3D ground motion simulations

One-dimensional site response analysis (1D SRA) remains the standard practice in considering the effect of local soil deposits and predicting site-specific ground motions, although its range of applicability to realistic seismic wavefields is still in question. In this 1D approach, horizontal and vertical ground shaking are assumed to be induced by vertically propagating shear and compressional waves, respectively. A recent study based on analytical two-dimensional (2D) plane waves and simple point source earthquake simulations has shown two mechanistic limitations in this 1D modelling technique for general inclined seismic waves, that is, systematic over-prediction of the vertical motion and wave trapping in the 1D soil column. In this article, we evaluate in detail the applicability of this 1D modelling approach to realistic three-dimensional (3D) simulated seismic wavefields in shallow sedimentary basins. Linear-viscoelastic 1D SRA predictions using two types of input motions that are commonly used in practice—rock outcrop and in-column motions, are compared with the reference true site response results from 3D earthquake simulations in terms of various measures in the frequency and time domain. It is shown that the horizontal motion in the 3D seismic wavefield exhibits dominant shear wave propagation phenomenon, while the vertical motion is a combined effect of compressional and shear waves and can be over-predicted by the 1D approach when the incident seismic waves are inclined. Direct evidence of the wave refraction process that leads to the vertical motion over-prediction is provided. 1D SRA with in-column inputs can yield motions that have significantly longer duration compared to the true 3D site response solution due to trapped waves, casting in doubt the frequent need for increased soil damping in existing site studies to compensate for wave attenuation due to scattering alone. Sensitivity investigation on the increase of soil profile damping by a multiplier D mul shows D mul values compatible with those found in the literature for both horizontal and vertical motions. It is shown that the level of D mul optimized for a best match of the spectral acceleration is dependent on the characteristic of the input motion and a larger D mul is typically required for the vertical component. In contrast, 1D SRA with outcrop motions predicts motions with shorter significant duration due to its inability to capture the basin-edge generated surface waves. A suite of ground motion simulations was performed to assess the sensitivity of the observations to the basin geologic structure including the velocity gradient, rock-basin impedance contrast and basin depth. The analysis results show that the accuracy of the simplified 1D procedure is dependent on the wavefield composition of both the input motions and the true 3D site response solution. While the horizontal motions in shallow sedimentary basins can, to the first order, be reasonably captured by the simplified 1D approach, 1D SRA for the vertical component is in general not reliable and contributions from inclined shear waves should be accounted for in site-specific evaluation of the vertical design ground motion.

1D assumption↗

SERS and the scientific career of Richard P. Van Duyne (1945–2019)

This article describes the scientific career of our dear friend Richard P. Van Duyne. Rick was the discoverer of surface-enhanced Raman spectroscopy (SERS), and over the period from the mid-1970s until his death in 2019, he served as both the intellectual leader of the field, and the technical genius who pushed the field forward through his numerous inventions and discoveries. Rick's work went through many phases, and even involved a significant period of inactivity that Rick was able to break out of, but especially after 2000, there was a period of incredible creativity that ultimately led to a detailed understanding of what the SERS enhancement factor is all about and also led to fabrication techniques for making optimum SERS substrates such that applications of SERS to a wide variety of real-world problems in sensing became possible. In addition, Rick's SERS work spawned numerous related technologies, including index of refraction sensing based on localized surface plasmon resonance (LSPR) measurements, and the extension of SERS to its tip-enhanced cousin TERS, to electrochemical versions of SERS and TERS, and to ultrafast nonlinear techniques. The practical applications he pursued included diagnostics for diseases such as cancer, hand-held glucose sensing, and SERS studies related to art conservation. Furthermore, Rick's legacy will probably be best known through the numerous students, postdocs, and collaborators that passed through his lab and who are now active researchers in areas related to SERS at universities and industrial labs around the world.

47 OTHER INSTRUMENTATION↗

Coherent Random Lasing in Subwavelength Quasi‐2D Perovskites

Abstract Quasi‐2D lead halide perovskites have garnered increasing interest as lasing gain media. Relatively simple fabrication, high refractive index, and unique quantum well structure encourage their use in traditional cavity lasers and cavity‐free systems called random lasers (RLs). Despite tremendous advances reported thus far, coherent random lasing in quasi‐2D perovskite subwavelength films has not been reported. Consequently, coherent optical feedback mechanisms in quasi‐2D perovskite systems are still unexplored. Here, this work reports the observation of coherent random lasing in subwavelength quasi‐2D perovskite films. Statistical analysis of spectral measurements reveals Lévy‐like intensity fluctuations, replica symmetry breaking confirms random lasing, and the coherent modes are studied with spectral and spatial correlation techniques. The observed coherent lasing modes are found to be extended states that arise from the random crystal grain structure during fabrication and span the entire pump volume. These modes out‐compete diffusive lasing due to their coherence.

47 OTHER INSTRUMENTATION↗

Low-energy radiative backgrounds in CCD-based dark-matter detectors

The reach of sub-GeV dark-matter detectors is at present severely affected by low-energy events from various origins. We present the theoretical methods to compute the single- and few-electron events that arise from secondary radiation emitted by high-energy particles as they pass through detector materials and perform a detailed simulation to quantify them at (Skipper) CCD-based experiments, focusing on the SENSEI data collected at Fermilab near the MINOS cavern. The simulations account for the generation of secondaries from Cherenkov and luminescent recombination radiation; photo-absorption in the bulk, backside layer, pitch adapter, and epoxy; the photon reflection and refraction at interfaces; thin-film interference; the roughness of the interfaces; the dynamics of charges produced in the highly doped CCD-backside-layers; and the partial charge collection on the CCD backside. We consider several systematic uncertainties, notably those stemming from the backside modeling, which we estimate with a “fiducial” and an “extreme” charge-diffusion model, with the former model being preferred due to better agreement with partial-charge collection data. We find that Cherenkov photons constitute about 30% of the observed single-electron events for both diffusion models; radiative recombination contributes negligibly to the event rate for the fiducial model, although it can dominate over Cherenkov for the extreme model. We also estimate the fraction of 2-electron events that arise from 1-electron event coincidences in the same pixel, finding that the entire 2-electron rate can be explained by coincidences of radiative events and spurious charge. Accounting for both radiative and non-radiative backgrounds, we project the sensitivity of future Skipper-CCD-based experiments to different dark-matter models. For light-mediator models with dark-matter masses of 1, 5, and 10 MeV, we find that future experiments with 10-kg-year exposures and successful background mitigation could have a sensitivity that is larger by 9, 3, and 2 orders of magnitude, respectively, when compared to an experiment without background improvements.

79 ASTRONOMY AND ASTROPHYSICS↗