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At least 163 records · Page 9

Differential Absorption Lidar (DIAL) Measurements of Atmospheric Water Vapor Utilizing Robotic Aircraft

A new unpiloted air vehicle (UAV) based water vapor DIAL system will be described. This system is expected to offer lower operating costs, longer test duration and severe weather capabilities. A new high-efficiency, compact, light weight, diode-pumped, tunable Cr:LiSAF laser will be developed to meet the UAV payload weight and size limitations and its constraints in cooling capacity, physical size and payload. Similarly, a new receiver system using a single mirror telescope and an avalanche photo diode (APD) will be developed. Projected UAV parameters are expected to allow operation at altitudes up to 20 km, endurance of 24 hrs and speed of 400 km/hr. At these conditions measurements of water vapor at an uncertainty of 2-10% with a vertical resolution of 200 m and horizontal resolution of 10 km will be possible.

Hoang, Ngoc↗

Standoff Detection of Oil and Powder Mixtures at 12 Meters Using a Tunable Quantum Cascade Laser-Based System with a Close Focus Telescope and Uncooled Infrared Detector

We have designed and demonstrated a quantum cascade laser (QCL) based standoff system that utilizes an uncooled mercury cadmium telluride (MCT) detector with lock-in signal processing for chemical identification at a distance of 12.5 meters in indoor ambient light conditions. In the system, a tunable quad-QCL operating (1 MHz) in quasi-continuous wave mode between 8.45 and 10.03 μm (~1182 to 1000 cm –1 ) serves as the active mid-infrared source for remotely interrogating mineral, powder, and thin film oil samples including powder mixtures (6, 12.5, 25, and 50%) of crystalline quartz (SiO 2 ) in KBr. Light as reflected from a given sample is collected using a 10-inch (25.4 cm) Dall Kirkham telescope and coupled with ZnSe optics to an uncooled MCT detector. Furthermore, the mixture dependence of the highly transparent KBr and strongly absorbing quartz was found to fit a modified version of the Schatz reflectance model for compacted powder mixtures. All reflectance spectra reported are relative to an Au-coated diffuse reflector. A NIST traceable polystyrene standard reflector was also used to determine the QCL wavelength tuning range and calibration.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Controlling Selectivity in Plasmonic Catalysis: Switching Reaction Pathway from Hydrogenation to Homocoupling Under Visible–Light Irradiation

Plasmonic catalysis enables the use of light to accelerate molecular transformations. Its application to the control reaction selectivity is highly attractive but remains challenging. Here, we have found that the plasmonic properties in AgPd nanoparticles allowed different reaction pathways for tunable product formation under visible-light irradiation. By employing the hydrogenation of phenylacetylene as a model transformation, we demonstrate that visible-light irradiation can be employed to steer the reaction pathway from hydrogenation to homocoupling. Our data showed that the decrease in the concentration of H species at the surface due to plasmon-enhanced H2 desorption led to the control in selectivity. Furthermore, these results provide important insights into the understanding of reaction selectivity with light, paving the way for the application of plasmonic catalysis to the synthesis of 1,3-diynes, and bringing the vision of light-driven transformations with target selectivity one step closer to reality.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Active and tunable nanophotonic metamaterials

Abstract Metamaterials enable subwavelength tailoring of light–matter interactions, driving fundamental discoveries which fuel novel applications in areas ranging from compressed sensing to quantum engineering. Importantly, the metallic and dielectric resonators from which static metamaterials are comprised present an open architecture amenable to materials integration. Thus, incorporating responsive materials such as semiconductors, liquid crystals, phase-change materials, or quantum materials (e.g., superconductors, 2D materials, etc.) imbue metamaterials with dynamic properties, facilitating the development of active and tunable devices harboring enhanced or even entirely novel electromagnetic functionality. Ultimately, active control derives from the ability to craft the local electromagnetic fields; accomplished using a host of external stimuli to modify the electronic or optical properties of the responsive materials embedded into the active regions of the subwavelength resonators. We provide a broad overview of this frontier area of metamaterials research, introducing fundamental concepts and presenting control strategies that include electronic, optical, mechanical, thermal, and magnetic stimuli. The examples presented range from microwave to visible wavelengths, utilizing a wide range of materials to realize spatial light modulators, effective nonlinear media, on-demand optics, and polarimetric imaging as but a few examples. Often, active and tunable nanophotonic metamaterials yield an emergent electromagnetic response that is more than the sum of the parts, providing reconfigurable or real-time control of the amplitude, phase, wavevector, polarization, and frequency of light. The examples to date are impressive, setting the stage for future advances that are likely to impact holography, beyond 5G communications, imaging, and quantum sensing and transduction.

36 MATERIALS SCIENCE↗

Resonant metasurface‐enabled quantum light sources for single‐photon emission and entangled photon‐pair generation

Light encodes information in multiple degrees of freedom (e.g., frequency, amplitude, and phase), enabling high‐speed, high‐bandwidth communication through fiber optics. Unlike classical light, quantum light (single or entangled photons) can transmit quantum states over long distances without loss of coherence, thereby coherently interconnecting quantum nodes for distributed quantum entanglement. Quantum light sources are critical for developing scalable quantum networks aimed at distributed quantum computing, quantum teleportation, and secure quantum communications. However, existing quantum light sources suffer from limited integrability, insufficient spectral and spatial tunability, and inefficiencies in achieving mass‐produced, deterministic, on‐demand quantum light generation. These limitations significantly hinder progress toward direct, on‐chip integration with quantum processing units and detectors – an essential step toward scalable quantum networks. Resonant metasurfaces that leverage photonic modes – such as Mie resonances, guided‐mode resonances, or symmetry‐protected bound states in the continuum – offer strong spatial and temporal confinement of electromagnetic fields, characterized by high quality factors and small mode volumes. These metasurfaces greatly enhance linear and nonlinear light‐matter interactions, making them ideal for efficient on‐chip quantum light generation and manipulation. Here, we describe recent advances in nanoscale quantum light sources and quantum photonic state manipulation enabled by resonant metasurfaces. We also provide an outlook on next‐generation miniaturized quantum light sources achievable through materials innovations in quantum emitters, the co‐design of resonant metasurfaces, and ultimately, the heterogeneous integration of emerging layered van der Waals materials with resonant metasurfaces.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Tunable graphene-based infrared reflectance filter having patterned nanoantenna layer and unpatterned graphene layer

An actively tunable optical filter can control the amplitude of reflected infrared light. The filter exploits the dependence of the excitation energy of plasmons in a continuous and unpatterned sheet of graphene, on the Fermi-level, which can be controlled by conventional electrostatic gating. An exemplary filter enables simultaneous modification of two distinct spectral bands whose positions are dictated by the device geometry and graphene plasmon dispersion. Within these bands, the reflected amplitude can be varied by over 15% and resonance positions can be shifted by over 90 cm−1. Electromagnetic simulations verify that tuning arises through coupling of incident light to graphene plasmons by a nanoantenna grating structure. Importantly, the tunable range is determined by a combination of graphene properties, device structure, and the surrounding dielectrics, which dictate the plasmon dispersion. Thus, the underlying design is applicable across a broad range of infrared frequencies.

Beechem, III, Thomas Edwin↗

Modeling strain and quantum confinement in GaAs/Ga x In 1−x P superlattices for spin-polarized electron sources

In this study, we systematically design and simulate a series of GaAs-based superlattice configurations aimed at enhancing heavy-hole–light-hole band splitting while simultaneously optimizing band alignment to reduce the conduction band barrier, thereby facilitating efficient electron transport. These combined effects are crucial for achieving high electron spin polarization and high quantum efficiency, the two key performance metrics of next-generation spin-polarized electron sources. We investigated three types of superlattice architectures: (1) compressively strained GaAs wells on GaInP barriers, yielding a maximum band splitting of 140 meV, (2) lattice-matched GaAs/GaInP structures, resulting in the maximum band splitting of 75 meV, and (3) tensile strained GaAs wells on GaInP barriers, with a maximum band splitting of 40 meV. The results demonstrate the tunability of heavy-hole–light-hole band splitting and establish a design framework for high-performance spin-polarized photocathodes based on a combination of strain engineering, quantum confinement, and optimized heterostructure design.

Electron sources↗

Simulation of ultrafast transient absorption spectra of a perylene-based light harvesting antenna

Atomistic simulations of photo-induced responses in artificial light-harvesting molecular systems help to reveal the mechanisms of ultrafast intramolecular energy transfer between individual chromophores. These light-induced processes mimic the primary events occurring in natural photosynthesis. Modeling studies contribute to the design of more efficient molecular architectures enabling performance optimization for applications in light harvesting, energy conversion, and optoelectronics. Within this context, the direct comparison between simulated and experimental transient absorption pump–probe (TA-PP) spectra are especially valuable for validating theoretical approaches and deepening mechanistic understanding. Herein, we investigate the photoinduced dynamics of an antenna system composed of two naphthalene monoimides donor units covalently linked to a perylene derived acceptor. Following photoexcitation, the exciton rapidly self-traps on one of the donor units. Thereafter, efficient ultrafast energy transfer to the acceptor unit takes place via two possible pathways: either through transient exciton localization on the second donor unit or by direct transfer to the acceptor. The simulated TA-PP spectra clearly capture these distinct energy transfer pathways and enable a detailed comparison of their relative efficiencies. This highlights the system's potential for tunable exciton dynamics towards advancing light-harvesting and optoelectronic molecular materials.

36 MATERIALS SCIENCE↗

Investigation on the AgPt and AgPd hybrid alloy nanoparticles (HANPs) for the hybrid MoS 2 /ZnO/HANP UV photodetector application

We report hybrid photodetectors made of two or more nanomaterial components can offer the high potential for advanced photodetection applications with enhanced light absorption, improved efficiency and structural tunability. A hybrid UV photodetector (PD) configuration incorporating the plasmonic hybrid alloy nanoparticles (HANP), ZnO quantum dots (QDs) and MoS 2 nanoflakes, namely MoS2/ZnO/HANP PD, is demonstrated. The optimized MoS 2 /ZnO/HANP PD exhibits a high photocurrent of 5.66 mA at 0.34 mW/mm 2 under 385 nm illumination with two orders of improvement from the bare ZnO, which is one of the highest photocurrents by the ZnO-based PDs. It also demonstrates high figure-of-merits with the responsivity of 14,523 mA/W, detectivity of 8.13 x 10 11 jones, and external quantum efficiency (EQE) of 4,680 %, outperforming most of the ZnO-based hybrid architectures. The enhanced photoresponse is primarily attributed to the significantly enhanced hot electron generation by the AgPd HANPs and photocarrier collection through the ZnO QD layer. MoS 2 nanoflakes also provide additional photon absorption sites and boost the photo-carrier transfer process. HANPs are grown by adapting a dual-step solid-state dewetting process (SSD) approach and the superiority of AgPd HANPs is confirmed by systematic investigation, FDTD simulation and comparison of AgPt and AgPd HANPs.

MoS2↗

Dynamic Focusing with High-Quality-Factor Metalenses

Metasurface lenses provide an ultrathin platform in which to focus light, but weak light–matter interactions limit their dynamic tunability. Here we design submicron-thick, ultrahigh quality factor (high-Q) metalenses that enable dynamic modulation of the focal length and intensity. Using full-field simulations, we show that quality factors exceeding 5000 can be generated by including subtle, periodic perturbations within the constituent Si nanoantennas. Such high-Q resonances enable lens modulation based on the nonlinear Kerr effect, with focal lengths varying from 4 to 6.5 μm and focal intensities decreasing by half as input intensity increases from 0.1 to 1 mW/μm 2 . We also show how multiple high-Q resonances can be embedded in the lens response through judicious placement of the perturbations. Our high-Q lens design, with quality factors 2 orders of magnitude higher than existing lens designs, provides a foundation for reconfigurable, multiplexed, and hyperspectral metasurface imaging platforms.

36 MATERIALS SCIENCE↗

Modulation of the Electronic and Vibrational Landscape in Lead Organic Chalcogenides

Metal organic chalcogenides (MOCs) are an emerging class of two-dimensional (2D) materials featuring tunable band gaps and strong light-matter interactions with great potential for optical and polaritonic applications. Lead organic chalcogenides (LOCs) stand out among MOCs for sustaining long-lived coherent optical phonons despite their distorted lattices. However, the strong electron–phonon coupling also leads to rapid charge carrier self-trapping, hindering carrier transport. Herein, we demonstrate that charge carrier self-trapping is suppressed in Se- and Te-based LOCs. Specifically, the expansive Se and Te orbitals give rise to more dispersive conduction bands and reduced electron effective masses, thereby mitigating carrier self-trapping. As a result of reduced carrier self-trapping, the Se- and Te-based LOCs exhibit enhanced band-to-band photoluminescence and improved charge transport performance. Furthermore, our results provide a synthetic route to Se- and Te-based LOC single crystals and demonstrate the potential of orbital engineering to tune their electronic and phononic properties.

Chalcogenides↗

Stabilizing in-transition phases of superlattices through shape control of silver nanocrystals

In nanoscale assemblies, observations of structures in the transition pathways between high-symmetry lattices are rare because of the inherent instability of the intermediate phases. Here, we report that silver nanocrystals with shapes similar to truncated octahedra (mecons) self-assemble into superlattices that are stable and resemble a previously unobserved phase that bridges face-centered and body-centered cubic structures along the Nishiyama-Wassermann martensitic pathway. These superlattices exhibited high structural purity and stability and created a robust and tunable dissymmetric phase landscape. Notably, light-matter coupling emerged in these silver nanocrystal superlattices through plasmon-photon hybridization at the quantum level.

36 MATERIALS SCIENCE↗

Optogenetics Illuminates Applications in Microbial Engineering

Optogenetics has been used in a variety of microbial engineering applications, such as chemical and protein production, studies of cell physiology, and engineered microbe–host interactions. These diverse applications benefit from the precise spatiotemporal control that light affords, as well as its tunability, reversibility, and orthogonality. This combination of unique capabilities has enabled a surge of studies in recent years investigating complex biological systems with completely new approaches. We briefly describe the optogenetic tools that have been developed for microbial engineering, emphasizing the scientific advancements that they have enabled. In particular, we focus on the unique benefits and applications of implementing optogenetic control, from bacterial therapeutics to cybergenetics. Lastly, we discuss future research directions, with special attention given to the development of orthogonal multichromatic controls. With an abundance of advantages offered by optogenetics, the future is bright in microbial engineering.

59 BASIC BIOLOGICAL SCIENCES↗

Develop On-Demand nanoplasmonic Device Concepts in a Semiconductor Compatible Hybrid System. Final Report

This report summarizes the research activities supported by the U.S. Department of Energy grant DE-SC-0010399. The goal of this project is to is to develop an on-demand nanoplasmonic platform that combines emerging oxide nanoelectronics with a low-loss semiconductor-friendly plasmonic materials. Toward this goal, several unique heterostructures formed between complex oxides and 2D layered materials have been developed. Based on these material systems, a set of atomic force microscope (AFM) based techniques have been developed that can allow long-living and reversible material phase transitions to be manipulated in nanoscale at room temperature. Using such technique and through interface coupling, we can effectively tune the plasmon propagations in unconventional plasmonic materials such as graphene and VO 2 . In addition, we also discovered a plethora of novel interface enabled electro-optic effects, including the spatial modulation of light using 2DEG, a giant programmable photothermoelectric effects at room temperature, a light induced superconducting transition, and a tunable giant third order optical nonlinearities. These major results are outlined in this report, along with lists of project participants and products.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Solid-State Laser Source of Tunable Narrow-Bandwidth Ultraviolet Radiation

A solid-state laser source of tunable and narrow-bandwidth UV light is disclosed. The system relies on light from a diode laser that preferably generates light at infrared frequencies. The light from the seed diode laser is pulse amplified in a light amplifier, and converted into the ultraviolet by frequency tripling, quadrupling, or quintupling the infrared light. The narrow bandwidth, or relatively pure light, of the seed laser is preserved, and the pulse amplifier generates high peak light powers to increase the efficiency of the nonlinear crystals in the frequency conversion stage. Higher output powers may be obtained by adding a fiber amplifier to power amplify the pulsed laser light prior to conversion.

PATENTS↗

Solution‐Processed Spin‐Polarized Light‐Emitting Diodes of Colloidal Quantum Wells and Magnetic Nanoparticles

Electrical injection of spin-polarized carriers into semiconductors enables circularly-polarized emission from spin-polarized light-emitting diodes (spin-LEDs). The incredible level of tunability of magnetic and electronic properties in colloidal nanocrystals offers unprecedented opportunities for the modulation of polarization of light in solution-processed spin-LEDs based on magnetic nanoparticles unlike epitaxially grown spin-LEDs restricted by a very limited range of materials for their exploitation, and solution-processed spin-LEDs based on chiral molecules, which do not allow the modulation of polarization in general. Here, it is shown that electrical injection of spin-polarized electrons from magnetic Fe 3 O 4 nanoparticles into CdSe/CdZnS core/shell colloidal quantum wells (CQWs) in solution-processed LEDs that allows for polarization modulation of electroluminescence. In this structure, a monolayer of face-down oriented CQWs is deposited as an active layer to avoid polarization losses due to the hopping of the electrons between the CQWs before the radiative recombination process. In this solution-processed spin-LED, the circular polarization reaches 4.5% at 3 K and survives up to 100 K. A net circular polarization is observed at zero magnetic field up to 100 K because of the remnant magnetization of the Fe 3 O 4 nanoparticles. This new colloidal spin-LED architecture presents significant prospects for future solution-processed advanced opto-spintronic devices.

circularly polarized electroluminescence↗

Recent advances of two-dimensional material additives in hybrid perovskite solar cells

Perovskite solar cells (PSCs) have become one of the state-of-the-art photovoltaic technologies due to their facile solution-based fabrication processes combined with extremely high photovoltaic performance originating from excellent optoelectronic properties such as strong light absorption, high charge mobility, long free charge carrier diffusion length, and tunable direct bandgap. However, the poor intrinsic stability of hybrid perovskites under environmental stresses including light, heat, and moisture, which is often associated with high defect density in the perovskite, has limited the large-scale commercialization and deployment of PSCs. The use of process additives, which can be included in various subcomponent layers in the PSC, has been identified as one of the effective approaches that can address these issues and improve the photovoltaic performance. Among various additives that have been explored, two-dimensional (2D) materials have emerged recently due to their unique structures and properties that can enhance the photovoltaic performance and device stability by improving perovskite crystallization, defect passivation, and charge transport. In this work, we provide a review of the recent progresses in 2D material additives for improving the PSC performance based on key representative 2D material systems, including graphene and its derivatives, transitional metal dichalcogenides, and black phosphorous, providing a useful guideline for further exploiting unique nanomaterial additives for more efficient and stable PSCs in the near future.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Utilizing Site Disorder in the Development of New Energy-Relevant Semiconductors

We report controlling site disorder in ternary and multinary compounds enables tuning optical and electronic properties at fixed lattice constants and stoichiometries, moving beyond many of the challenges facing binary alloy systems. Here, we consider possible enhancements to energy-related applications through the integration of disorder-tunable materials in devices such as light-emitting diodes, photonics, photovoltaics, photocatalytic materials, batteries, and thermoelectrics. However, challenges remain in controlling and characterizing disorder. Focusing primarily on II–IV–V 2 materials, we identify three metrics for experimentally characterizing cation site disorder. Complementary to these experiments, we discuss simulation methods to understand disordered materials. Nonidealities, such as off-stoichiometry and oxygen incorporation, can occur while synthesizing metastable disordered materials. While nonidealities may seem undesirable, we describe how if harnessed they could provide another knob for tuning disorder and subsequently properties. To illustrate the effects of disorder on device-relevant properties, we provide case examples of disordered materials and their potential in device applications.

36 MATERIALS SCIENCE↗