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At least 757 records · Page 42

Ultrafast terahertz emission from emerging symmetry-broken materials

Abstract Nonlinear optical spectroscopies are powerful tools for investigating both static material properties and light-induced dynamics. Terahertz (THz) emission spectroscopy has emerged in the past several decades as a versatile method for directly tracking the ultrafast evolution of physical properties, quasiparticle distributions, and order parameters within bulk materials and nanoscale interfaces. Ultrafast optically-induced THz radiation is often analyzed mechanistically in terms of relative contributions from nonlinear polarization, magnetization, and various transient free charge currents. While this offers material-specific insights, more fundamental symmetry considerations enable the generalization of measured nonlinear tensors to much broader classes of systems. We thus frame the present discussion in terms of underlying broken symmetries, which enable THz emission by defining a system directionality in space and/or time, as well as more detailed point group symmetries that determine the nonlinear response tensors. Within this framework, we survey a selection of recent studies that utilize THz emission spectroscopy to uncover basic properties and complex behaviors of emerging materials, including strongly correlated, magnetic, multiferroic, and topological systems. We then turn to low-dimensional systems to explore the role of designer nanoscale structuring and corresponding symmetries that enable or enhance THz emission. This serves as a promising route for probing nanoscale physics and ultrafast light-matter interactions, as well as facilitating advances in integrated THz systems. Furthermore, the interplay between intrinsic and extrinsic material symmetries, in addition to hybrid structuring, may stimulate the discovery of exotic properties and phenomena beyond existing material paradigms.

36 MATERIALS SCIENCE↗

Low-Loss Charge Transfer Plasmons in Graphene/α-RuCl 3 Heterostructures Below 40 K

Charge transfer at material interfaces governs a wide range of physical properties, from electronic band structures to emergent collective excitations. In two-dimensional (2D) material heterostructures, charge transfer phenomena play important roles in enabling novel quantum phases, proximity effects, and tunable plasmonic responses. One representative charge transfer interface is formed between α-RuCl 3 , a van der Waals material with high electron affinity, and graphene. Significant charge transfer across this interface induces the formation of charge-transfer plasmon polaritons (CPPs), hybrid excitations between light and charge oscillations. However, previous studies found that as the charge transfer process takes place, α-RuCl 3 becomes lossy, which limits the quality factor of CPPs. Here, we investigate CPPs down to 10 K using a home-built scattering-type scanning near-field optical microscope (s-SNOM) optimized for low-temperature measurements. Our study reveals a dramatic suppression of plasmon loss channels below 40 K, contributing to a significant enhancement in the plasmonic quality factor. This reduction in loss is likely attributed to the blue shift of the correlation-induced Mott gap in α-RuCl 3 with decreasing temperature, along with the reduction of phonon scattering at low temperature. In conclusion, our results highlight the potential of using s-SNOM and CPPs to study complex 2D interfaces and reveal correlated electron dynamics in the underlying material.

36 MATERIALS SCIENCE↗

Stimulated Emission from Below the Bandgap in Giant Quantum Shells

Colloidal semiconductor nanocrystals (NCs) have emerged as promising candidates for developing solution-processable optical gain media, with potential applications in integrated photonic circuits and lasers. However, the deployment of NCs in these technologies has been hindered by nonradiative Auger recombination of multiexciton states, which shortens the optical gain lifetime and reduces its spectral range. Here, we demonstrate that these limitations can be overcome by using giant colloidal quantum shells (g-QSs), comprising a quantum-confined CdSe shell grown over a large (~14 nm) CdS bulk core. Such bulk-nanoscale architecture minimizes exciton–exciton interactions, leading to suppressed Auger recombination and one of the broadest gain bandwidths reported for colloidal nanomaterials, spanning energies both above and, remarkably, below the bandgap. Ultrafast transient absorption and photoluminescence measurements demonstrate that the high-energy portion of optical gain arises from states containing more than 15 excitons per particle while the unusual sub-bandgap gain behaviour results from an Auger-assisted radiative recombination, a mechanism that has traditionally been viewed as a loss pathway. Altogether, these results reveal a unique gain regime associated with bulk-nanocrystal hybrid systems, which offers a promising path toward solution-processable light sources.

Absorption↗

Acurex Parabolic Dish Concentrator (PDC-2)

The design approach, rationale for the selected configuration, and the development status of a cost effective point-focus solar concentrator are discussed. The low-cost concentrator reflective surface design is based on the use of a thin, backsilvered mirror glass reflector bonded to a molded structural plastic substrate. The foundation, support, and drive subassembles are described. A hybrid, two-axis, Sun tracking control system based on microprocessor technology was selected. Coarse synthetic tracking is achieved through a microcomputer-based control system to calculate Sun position for transient periods of cloud cover as well as sundown and sunrise positioning. Accurate active tracking is achieved by two-axis optical sensors. Results of the reflective panel demonstration tests investigating slope error, hail impact survivability, temperature/humidity cycling, longitudinal strength/bending stiffness, and torsional stiffness are discussed.

Overly, P.↗

(abstract) Galileo PPR Observations of Shoemaker-Levy 9

The Galileo spacecraft Photopolarimeter Radiometer (PPR), a hybrid visual/thermal IR instrument designed primarily to measure properties of the Jovian atmosphere, was employed for SL9 as a staring high-speed photometer at 945 and 678 nm, taking advantage of Galileo's direct view of the impact point.The PPR was able to acquire data at times when no other Galileo optical instruments could operate.

Galileo Jupiter Shoemaker-Levy 9 IR observations p↗

Coupled Retrieval of Aerosol Properties and Surface Reflection Using the Airborne Multi-Angle SpectroPolarimetric Imager (AirMSPI)

The Airborne Multi-angle SpectroPolarimetric Imager (AirMSPI) has been flying aboard the NASA ER-2 high altitude aircraft since October 2010. In step-and-stare operation mode, AirMSPI acquires radiance and polarization data at 355, 380, 445, 470*, 555, 660*, 865*, and 935 nm (* denotes polarimetric bands). The imaged area covers about 10 km by 10 km and is observed from 9 view angles between ±67° off of nadir. We have developed an efficient and flexible code that uses the information content of AirMSPI data for a coupled retrieval of aerosol properties and surface reflection. The retrieval was built based on the multi-pixel optimization concept, with the use of a hybrid radiative transfer model that combines the Markov Chain and adding/doubling methods. The convergence and robustness of our algorithm is ensured by applying constraints on (a) the spectral variation of the Bidirectional Polarization Distribution Function (BPDF) and angular shape of the Bidirectional Reflectance Distribution Function (BRDF); (b) the spectral variation of aerosol optical properties; and (c) the spatial variation of aerosol parameters across neighboring image pixels. Our retrieval approach has been tested using over 20 AirMSPI datasets having low to moderately high aerosol loadings (~0.02<AOD550-nm<~0.45) and acquired during several field campaigns. Results are compared with AERONET aerosol reference data. We also explore the benefits of AirMSPI’s ultraviolet and polarimetric bands as well as the use of multiple view angles.

Xu, Feng↗

Large-mode-area optical fibers and optical fiber amplifiers in the eye-safe regime

The present technology provides large mode area optical fibers engineered to have normal dispersion around 1600 nm, enabling high power Raman amplification at eye safer wavelengths. The fibers can have a main core and one or more side cores disposed relative to the main core so that modes of the main core and the one or more side cores hybridize into supermodes with modified dispersion.

Pax, Paul H.↗

Process Development for Printing Copper Conductible Ink on Flexible Substrates Using Aerosol Jet Technology

Rise in demand for wearable consumer electronics products has given an impetus to the development of flexible electronics technology encompassing flexible substrates and compatible circuitry. Also, additive manufacturing of flexible electronics is emerging rapidly via several techniques such as Inkjet and Aerosol Jet Printing (AJP). The basic component of all flexible circuits to be printed by these technologies is conductible ink, which is generally silver ink. Few studies exist on the printing of copper conductible ink and not many copper ink formulations are available in the market as that of silver inks. This study aims to develop a process development study for deposition of copper conductible lines on flexible substrates using the aerosol jet printing technology. The process development study includes investigation of photosintering parameters for obtaining desirable electrical resistance and shear load to failure values for the printed line. Different pre-drying techniques such as oven pre-drying and platen pre-drying have been used for improving the electrical and mechanical properties of the conductive traces. Techniques such as optical microscopy and white light interferometry have been used for the characterization of print quality of the conductible lines.

printed electronics↗

Defect-Limited Mobility and Defect Thermochemistry in Mixed A-Cation Tin Perovskites: (CH3NH3)1-xCsxSnBr3

Hybrid organic-inorganic semiconductors crystallizing in the perovskite structure present a significant opportunity for realizing defect-tolerant semiconductors. In this work, we examine the solid solution, (CH3NH3)1-xCsxSnBr3, and identify the thermochemistry dictating the intrinsic carrier concentrations and how local structural distortions influences this electronic behavior. This family of compounds exhibits the expected systematic trend in decreasing optical gap with the cesium to methylammonium A-site mixing ratio, x, in the visible region. However, the carrier mobility, as determined from time-resolved microwave conductivity measurements, trends opposite to that expected from first-principles calculations combined with Boltzmann scattering theory calculations of the carrier mobility. We propose that this is a result of increasing carrier scattering with x in (CH3NH3)1-xCsxSnBr3 due to a significant increase in the carrier density with x. By examining the dependence of the carrier density as a function of x, we infer the compositional-dependence of the average enthalpy and nonconfigurational entropy per defect. While diffraction reveals a cubic aristotypic perovskite structure as a function of x at room temperature, the pair distribution functions obtained from synchrotron X-ray total scattering from these materials are better described by symmetry-adapted displacement modes of the Pm3m crystal structure, which we attribute to a large degree of anharmonic dynamics of the atom positions. This analysis shows that CH3NH3+-rich compositions retain mostly linear Sn-Br-Sn bonding environments through the displacements, while Cs+-rich compositions lead to more significantly bent Sn-Br-Sn environments. We propose that these bent bonding arrangements in Cs-rich compositions yield a higher propensity for defect formation. This also provides a rationale for carrier trapping that gives rise to anomalous microwave transients. Together, these results provide insight into the structure-dynamics-properties relationships in this highly anharmonic system with high amplitude atomic motions and low defect formation energies.

defect thermochemistry↗

Visualizing Electric and Magnetic Field Coupling in Au-Nanorod Trimer Structures via Stimulated Electron Energy Gain and Cathodoluminescence Spectroscopy: Implications for Meta-Atom Imaging

In this work, trimer meta-atoms composed of three gold rods in an equilateral triangular geometry were fabricated, and their near-field plasmonic responses were characterized via electron energy loss (EEL), cathodoluminescence (CL), and stimulated electron energy loss/gain (sEEL/sEEG) spectroscopy. The trimer structure hybridizes into a low-energy mode with all three rods coupling in-phase, which produces a circulating current and thus a magnetic field. The next highest-energy mode consists of two rods coupling out-of-phase and produces a net electric dipole. We investigate the near fields of hybridized magnetic and electric modes via EEL and CL and correlate their spectral characteristics and intensity maps. Then, by changing the length of the trimer rods, we tune the magnetic and electric modes to our laser energy and characterize the excited state via sEEL/sEEG spectroscopy. Exploration of the tilt dependence, relative to the optical source, of the two modes reveals that the electric mode sEEG intensity increases more than the expected sin 2 (θ) dependence of the optical electric field coupling (see the Supporting Information for a detailed description). After correcting for the tail of the close-proximity electric mode, we demonstrate sEEG via coupling of the magnetic component of the optical field to the magnetic meta-atoms, which has the expected cos 2 (θ) tilt dependence. This realization opens the possibility to explore the nanoscale excited-state near-field imaging of other magnetic meta-atom structures.

36 MATERIALS SCIENCE↗

Polariton Dynamics in Two-Dimensional Ruddlesden–Popper Perovskites Strongly Coupled with Plasmonic Lattices

Strong coupling between light and matter can produce hybrid eigenstates known as exciton-polaritons. Although polariton dynamics are important photophysical properties, the relaxation pathways of polaritons in different coupling regimes have seen limited attention. This paper reports the dynamics of hybridized states from 2D Ruddlesden-Popper perovskites coupled to plasmonic nanoparticle lattices. The open cavity architecture of Al lattices enables the coupling strength to be modulated by varying either the lead halide perovskite film thickness or the superstrate refractive index. Both experiments and finite-difference time-domain simulations of the optical dispersion diagrams showed avoided crossings that are a signature of strong coupling. Furthermore, our analytical model also elucidated the correlation between the exciton/plasmon mixing ratio and polariton coupling strength. Using fs-transient absorption spectroscopy, we found that both the upper and lower polaritons have shorter lifetimes than the excitons and that polaritons can show faster excited state dynamics when they have access to additional energy transfer channels.

2D perovskite↗

Thermal Cycle Reliability of PBGA/CCGA 717 I/Os

Status of thermal cycle test results for a nonfunctional daisy-chained peripheral ceramic column grid array (CCGA) and its plastic ball grid array (PBGA) version. both having 560 I/Os. were presented in last year's conference. Test results included environmental data for three different thermal cycle regimes (-55 C/125 C, -55 C/100 C, and -50 C /75 C). Update information on these - especially failure type for assemblies with high and low solder volumes-were presented. The thermal cycle test procedure followed those recommended IPC-9701 for tin-lead solder joint assemblies. Revision A of this specification covers guideline thermal cycle requirements for Pb-free solder joints. Some background information discussed during release of this specification with its current guideline recommendations were also presented. In a recent reliability investigation a fully populated CCGA with 717 I/Os was also considered for assembly reliability. evaluation. The functional package is a field-programmable gate array that has much higher processing power than its previous version. This new package is smaller in dimension, has no interposer, and has a thinner column wrapped with copper for reliability improvement. This paper will also present thermal cycle test results for this package assembly and its plastic version with 728 I/Os. both of which were exposed to three different cycle regimes. Two cycle profiles were those specified by IPC- 9701A for tin-lead, i.e. -55 to 100 C and -55 to 125 C and one was a cycle profile specified by Mil-Std-883, i.e.. -65 C/150 C which is generally used for ceramic hybrid packages. Per IPC-9701 A, test vehicles were built using daisy chain packages and were continuously monitored. The effects of many process and assembly variables-including corner staking commonly used for improving resistance to mechanical loading such as drop and vibration loads--were also considered as part of the test matrix. Optical photomicrographs were taken at various thermal cycle intervals to document damage progress and behavior. Representative samples of these along with cross-sectional photomicrographs at higher magnification taken by scanning electron microscopy (SEM) to determine crack propagation and failure analyses for packages are also presented.

staking↗

Multi-pixel high-resolution three-dimensional imaging radar

A three-dimensional imaging radar operating at high frequency e.g., 670 GHz radar using low phase-noise synthesizers and a fast chirper to generate a frequency-modulated continuous-wave (FMCW) waveform, is disclosed that operates with a multiplexed beam to obtain range information simultaneously on multiple pixels of a target. A source transmit beam may be divided by a hybrid coupler into multiple transmit beams multiplexed together and directed to be reflected off a target and return as a single receive beam which is demultiplexed and processed to reveal range information of separate pixels of the target associated with each transmit beam simultaneously. The multiple transmit beams may be developed with appropriate optics to be temporally and spatially differentiated before being directed to the target. Temporal differentiation corresponds to a different intermediate frequencies separating the range information of the multiple pixels. Collinear transmit beams having differentiated polarizations may also be implemented.

Cooper, Ken B.↗

Increasing CO2 Conversion Efficiency with Optical Thermal Management in Concentrated Solar Reactors: New Dual-Stage Solar Reactor Design for Reduction of CO2 to Fuels

The proposed project will result in a new dual-stage solar chemical reactor designed to convert carbon dioxide (CO2) to value-added chemicals. Using sunlight as the main power source, a sustainable process will be developed that closes the loop on our industrial carbon cycle in an energy efficient and environmentally friendly manner. The hybrid photochemical and photothermal reactor design will vastly increase utilization of the solar spectrum and increase CO2 conversion efficiencies over Dimensional Energy’s current state-of-the-art.

10 SYNTHETIC FUELS↗

Decoding the Atomic Structure of Ga 2 Te 5 Pulsed Laser Deposition Films for Memory Applications Using Diffraction and First-Principles Simulations

Neuromorphic computing, reconfigurable optical metamaterials that are operational over a wide spectral range, holographic and nonvolatile displays of extremely high resolution, integrated smart photonics, and many other applications need next-generation phase-change materials (PCMs) with better energy efficiency and wider temperature and spectral ranges to increase reliability compared to current flagship PCMs, such as Ge 2 Sb 2 Te 5 or doped Sb 2 Te. Gallium tellurides are favorable compounds to achieve the necessary requirements because of their higher melting and crystallization temperatures, combined with low switching power and fast switching rate. Ga 2 Te 3 and non-stoichiometric alloys appear to be atypical PCMs; they are characterized by regular tetrahedral structures and the absence of metavalent bonding. The sp 3 gallium hybridization in cubic and amorphous Ga 2 Te 3 is also different from conventional p-bonding in flagship PCMs, raising questions about its phase-change mechanism. Furthermore, gallium tellurides exhibit a number of unexpected and highly unusual phenomena, such as nanotectonic compression and viscosity anomalies just above their melting points. Using high-energy X-ray diffraction, supported by first-principles simulations, we will elucidate the atomic structure of amorphous Ga 2 Te 5 PLD films, compare it with the crystal structure of tetragonal gallium pentatelluride, and investigate the electrical, optical, and thermal properties of these two materials to assess their potential for memory applications, among others.

36 MATERIALS SCIENCE↗

Hybrid Molecular Beam Epitaxy for Single-Crystalline Oxide Membranes with Binary Oxide Sacrificial Layers

The advancement in thin-film exfoliation for synthesizing oxide membranes has led to possibilities for creating artificially assembled heterostructures with structurally and chemically incompatible materials. The sacrificial layer method is a promising approach to exfoliate as-grown films from a compatible material system, allowing for their integration with dissimilar materials. Nonetheless, the conventional sacrificial layers often possess an intricate stoichiometry, thereby constraining their practicality and adaptability, particularly when considering techniques such as molecular beam epitaxy (MBE). This is where easy-to-grow binary alkaline-earth-metal oxides with a rock salt crystal structure are useful. These oxides, which include (Mg, Ca, Sr, Ba)O, can be used as a sacrificial layer covering a much broader range of lattice parameters compared to conventional sacrificial layers and are easily dissolvable in deionized water. In this study, we show the epitaxial growth of the single-crystalline perovskite SrTiO 3 (STO) on sacrificial layers consisting of crystalline SrO, BaO, and Ba 1–x Ca x O films, employing a hybrid MBE method. Our results highlight the rapid (≤5 min) dissolution of the sacrificial layer when immersed in deionized water, facilitating the fabrication of millimeter-sized STO membranes. Using high-resolution X-ray diffraction, atomic-force microscopy, scanning transmission electron microscopy, impedance spectroscopy, and scattering-type near-field optical microscopy (SNOM), we demonstrate single-crystalline STO membranes with bulk-like intrinsic dielectric properties. The employment of alkaline earth metal oxides as sacrificial layers is likely to simplify membrane synthesis, particularly with MBE, thus expanding the research and application possibilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Panchromatic Imaging Fourier Transform Spectrometer for the NASA Geostationary Coastal and Air Pollution Events Mission

This paper summarizes the design and development of the Panchromatic Imaging Fourier Transform Spectrometer (PanFTS) for the NASA Geostationary Coastal and Air Pollution Events (GEO-CAPE) Mission. The PanFTS instrument will advance the understanding of the global climate and atmospheric chemistry by measuring spectrally resolved outgoing thermal and reflected solar radiation. With continuous spectral coverage from the near-ultraviolet through the thermal infrared, this instrument is designed to measure pollutants, greenhouse gases, and aerosols as called for by the U.S. National Research Council Decadal Survey; Earth Science and Applications from Space: National Imperatives for the Next Decade and Beyond1. The PanFTS instrument is a hybrid instrument based on spectrometers like the Tropospheric Emissions Spectrometer (TES) that measures thermal emission, and those like the Orbiting Carbon Observatory (OCO), and the Ozone Monitoring Instrument (OMI) that measure scattered solar radiation. Simultaneous measurements over the broad spectral range from IR to UV is accomplished by a two sided interferometer with separate optical trains and detectors for the ultraviolet-visible and infrared spectral domains. This allows each side of the instrument to be independently optimized for its respective spectral domain. The overall interferometer design is compact because the two sides share a single high precision cryogenic optical path difference mechanism (OPDM) and metrology laser as well as a number of other instrument systems including the line-of-sight pointing mirror, the data management system, thermal control system, electrical system, and the mechanical structure. The PanFTS breadboard instrument has been tested in the laboratory and demonstrated the basic functionality for simultaneous measurements in the visible and infrared. It is set to begin operations in the field at the California Laboratory for Atmospheric Remote Sensing (CLARS) observatory on Mt. Wilson measuring the atmospheric chemistry across the Los Angeles basin. Development has begun on a flight size PanFTS engineering model (EM) that addresses all critical scaling issues and demonstrates operation over the full spectral range of the flight instrument which will show the PanFTS instrument design is mature.

Imaging spectrometer(↗