Ultrabroadband and Wide-Angle Hybrid Antireflection Coatings With Nanostructures
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Ligand-Controlled Rates of Photoinduced Electron Transfer in Hybrid CdSe Nanocrystal/Poly(viologen) Films
This paper describes a study of the rates of photoinduced electron transfer (PET) from CdSe quantum dots (QDs) to poly(viologen) within thin films, as a function of the length of the ligands passivating the QDs. Ultrafast (<10 ps), quantitative PET occurs from CdSe QDs coated with HS-(CH2)n-COOH for n = 1, 2, 5, and 7 to viologen units. The observed decrease in the magnitude of the PET rate constant with n is weaker than that expected from the decay of the electron tunneling probability across extended all-trans mercaptocarboxylic acids but well-described by electron tunneling across a collapsed ligand shell. The PET rate constants for films with n = 10 and 15 are much slower than those expected based on the trend for n = 1–7; this deviation is ascribed to the formation of bundles of ligands on the surface of the QD that make the tunneling process prohibitively slow by limiting access of the viologen units to the surfaces of the QDs. This study highlights the importance of molecular-level morphology of donor and acceptor materials in determining the rate and yield of interfacial photoinduced electron transfer in thin films.
36 MATERIALS SCIENCE↗
Exciton dressing by extreme nonlinear magnons in a layered semiconductor
Collective excitations presenting nonlinear dynamics are fundamental phenomena with broad applications. A prime example is nonlinear optics, where diverse frequency mixing processes are central to communication, sensing, wavelength conversion, and attosecond physics. Leveraging recent progress in van der Waals magnetic semiconductors, we demonstrate nonlinear opto-magnonic coupling by presenting exciton states dressed by up to 20 harmonics of magnons, resulting from their nonlinearities, in the layered antiferromagnetic semiconductor CrSBr. We also create tunable optical side bands from sum- and difference-frequency generation between two optically bright magnon modes under symmetry breaking magnetic fields. Moreover, the observed difference-frequency generation mode can be continuously tuned into resonance with one of the fundamental magnons, resulting in parametric amplification of magnons. These findings realize the modulation of the optical frequency exciton with the extreme nonlinearity of magnons at microwave frequencies, which could find applications in magnonics and hybrid quantum systems, and provide new avenues for implementing opto-magnonic devices.
Diederich, Geoffrey M.↗
The interplay between chromophore and protein determines the extended excited state dynamics in a single-domain phytochrome
Phytochromes are a diverse family of bilin-binding photoreceptors that regulate a wide range of physiological processes. Their photochemical properties make them attractive for applications in optogenetics and superresolution microscopy. Phytochromes undergo reversible photoconversion triggered by the Z ⇌ E photoisomerization about the double bond in the bilin chromophore. However, it is not fully understood at the molecular level how the protein framework facilitates the complex photoisomerization dynamics. In this work, we have studied a single-domain bilin-binding photoreceptor All2699g1 ( Nostoc sp. PCC 7120) that exhibits photoconversion between the red light-absorbing (P r ) and far red-absorbing (P fr ) states just like canonical phytochromes. We present the crystal structure and examine the photoisomerization mechanism of the P r form as well as the formation of the primary photoproduct Lumi-R using time-resolved spectroscopy and hybrid quantum mechanics/molecular mechanics simulations. We show that the unusually long excited state lifetime (broad lifetime distribution centered at ~300 picoseconds) is due to the interactions between the isomerizing pyrrole ring D and an adjacent conserved Tyr142. The decay kinetics shows a strongly distributed character which is imposed by the nonexponential protein dynamics. Our findings offer a mechanistic insight into how the quantum efficiency of the bilin photoisomerization is tuned by the protein environment, thereby providing a structural framework for engineering bilin-based optical agents for imaging and optogenetics applications.
59 BASIC BIOLOGICAL SCIENCES↗
Control of magnon–photon coupling by spin torque
We demonstrate the influence of damping and field-like torques in the magnon–photon coupling process by classically integrating the generalized Landau–Lifshitz–Gilbert equation with RLC equation in which a phase correlation between dynamic magnetization and microwave current through combined Ampère and Faraday effects are considered. We show that the gap between two hybridized modes can be controlled in samples with damping parameter in the order of 10 –3 by changing the direction of the dc current density J if a certain threshold is reached. Furthermore, our results suggest that an experimental realization of the proposed magnon–photon coupling control mechanism is feasible in yttrium iron garnet/Pt hybrid structures.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Twisted Nonlinear Optics in Monolayer van der Waals Crystals
In addition to a plethora of emergent phenomena, the spatial topology of optical vortices enables an array of applications in optical communications and quantum information science. Multibeam nonlinear optical processes, augmented by optical vortices, are essential in this context, providing robust access to an infinitely large set of quantum states associated with the orbital angular momentum of light. Here, we push the boundaries of vortex nonlinear optics to the ultimate limits of material dimensionality. By exploiting multipulse difference frequency, sum frequency, and four-wave mixing in monolayer quantum materials, we demonstrate their ability to independently control the orbital angular momentum and radial distribution of vortex light-fields in addition to their wavelength. Due to the atomically thin nature of the host crystal, this control spans a broad spectral bandwidth in a highly integrable platform that is unconstrained by the traditional limits of bulk nonlinear optical materials. Our work heralds an innovative path for ultracompact and scalable hybrid nanophotonic technologies empowered by twisted nonlinear light–matter interactions in van der Waals nanomaterials.
36 MATERIALS SCIENCE↗
Quantum machine learning with differential privacy
Abstract Quantum machine learning (QML) can complement the growing trend of using learned models for a myriad of classification tasks, from image recognition to natural speech processing. There exists the potential for a quantum advantage due to the intractability of quantum operations on a classical computer. Many datasets used in machine learning are crowd sourced or contain some private information, but to the best of our knowledge, no current QML models are equipped with privacy-preserving features. This raises concerns as it is paramount that models do not expose sensitive information. Thus, privacy-preserving algorithms need to be implemented with QML. One solution is to make the machine learning algorithm differentially private, meaning the effect of a single data point on the training dataset is minimized. Differentially private machine learning models have been investigated, but differential privacy has not been thoroughly studied in the context of QML. In this study, we develop a hybrid quantum-classical model that is trained to preserve privacy using differentially private optimization algorithm. This marks the first proof-of-principle demonstration of privacy-preserving QML. The experiments demonstrate that differentially private QML can protect user-sensitive information without signficiantly diminishing model accuracy. Although the quantum model is simulated and tested on a classical computer, it demonstrates potential to be efficiently implemented on near-term quantum devices [noisy intermediate-scale quantum (NISQ)]. The approach’s success is illustrated via the classification of spatially classed two-dimensional datasets and a binary MNIST classification. This implementation of privacy-preserving QML will ensure confidentiality and accurate learning on NISQ technology.
97 MATHEMATICS AND COMPUTING↗
Ligand‐Induced Crystallization Control in MAPbBr 3 Hybrid Perovskites for High Quality Nanostructured Films
AbstractControlling the formation of hybrid perovskite thin films is crucial in obtaining high‐performance optoelectronic devices, since factors like morphology and film thickness have a profound impact on a film's functionality. For light‐emitting applications grain sizes in the sub‐micrometer‐range have previously shown enhanced brightness. It is therefore crucial to develop simple, yet reliable methods to produce such films. Here, a solution‐based synthesis protocol for the on‐substrate formation of MAPbBr3 (MA = methylammonium) nanostructures by adding the bifunctional rac‐3‐aminobutyric acid to the precursor solution is reported. This synthesis route improves key optical properties such as photoluminescence quantum yields and life times of excited states by inducing a controlled slow‐down of the film formation and suppressing agglomeration effects. In situ spectroscopy reveals a delayed and slowed down crystallization process, which achieves synthesis of perovskite structures with much reduced defect densities. Further, aggregation can be controlled by the amount of amino acid added and adjusting the synthesis protocol allows to produce cubic crystallites with targeted size from nanometer to micrometer scales. The nanocrystalline MAPbBr3 samples show enhanced amplified spontaneous emission (ASE) intensities, reduced ASE thresholds and purer ASE signals, compared to pristine films, even under intense optical driving, making them promising structures for lasing applications.
36 MATERIALS SCIENCE↗
New Methods for Predicting Non-Born-Oppenheimer Chemistry
Current methods for modeling non-adiabatic molecular dynamics face fundamental limitations when treating geometric phase effects: quantum mechanical phenomena where nuclear wavepackets acquire phase shifts when encircling conical intersections. Existing approaches either neglect these effects entirely or rely on potential energy surfaces arising from the Born-Oppenheimer approximation, which introduce artificial singularities and can overestimate geometric phase contributions. This project developed a new theoretical framework based on exact factorization (XF) methods to overcome these limitations. We derived mathematical formulations for hybrid quantum-classical XF dynamics that selectively treat critical nuclear degrees of freedom quantum mechanically while propagating others classically. This approach addresses the computational intractability that has previously limited exact methods to toy systems. Key innovations include a new approach to systematically identifying nuclear coordinates requiring quantum treatment, as well as novel implementation strategies that interface with existing quantum chemistry codes. The project also developed a proof-of-concept code for treating Jahn-Teller systems and creation of educational materials on non-adiabatic dynamics geared at the graduate level. The theoretical framework developed will enable future systematically improvable calculations of nuclear quantum effects in realistic molecular systems, filling a critical gap in non-adiabatic dynamics methods. This foundation supports future development of predictive tools for designing energy-relevant photochemical processes where quantum coherence effects may be exploited to control reaction outcomes.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Hybrid framework for the simulation of stochastic chemical kinetics
Stochasticity plays a fundamental role in various biochemical processes, such as cell regulatory networks and enzyme cascades. Isothermal, well-mixed systems can be modelled as Markov processes, typically simulated using the Gillespie Stochastic Simulation Algorithm (SSA) [25]. While easy to implement and exact, the computational cost of using the Gillespie SSA to simulate such systems can become prohibitive as the frequency of reaction events increases. This has motivated numerous coarse-grained schemes, where the “fast” reactions are approximated either using Langevin dynamics or deterministically. While such approaches provide a good approximation when all reactants are abundant, the approximation breaks down when one or more species exist only in small concentrations and the fluctuations arising from the discrete nature of the reactions become significant. This is particularly problematic when using such methods to compute statistics of extinction times for chemical species, as well as simulating non-equilibrium systems such as cell-cycle models in which a single species can cycle between abundance and scarcity. In this paper, a hybrid jump-diffusion model for simulating well-mixed stochastic kinetics is derived. It acts as a bridge between the Gillespie SSA and the chemical Langevin equation. For low reactant reactions the underlying behaviour is purely discrete, while purely diffusive when the concentrations of all species are large, with the two different behaviours coexisting in the intermediate region. A bound on the weak error in the classical large volume scaling limit is obtained, and three different numerical discretisations of the jump-diffusion model are described. The benefits of such a formalism are illustrated using computational examples.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
An Indium Gallium Arsenide Visible/SWIR Focal Plane Array for Low Light Level Imaging
PIN photodiodes fabricated from indium gallium arsenide lattice-matched to indium phosphide substrates (In(.53)Ga(.47)As/InP) exhibit low reverse saturation current densities (JD < 10(exp -8) A/sq cm), and high shunt resistance-area products (RoA > 10(exp 6) omega-sq cm) at T=290K. Backside-illuminated, hybrid-integrated InGaAs FPAs are sensitive from 0.9 micrometers to 1.7 micrometers. 290K detectivities, D(*), greater than 10(exp 14) cm-(square root of Hz/W) are demonstrated. This represents the highest room temperature detectivity of any infrared material. The long wavelength cutoff (1.7 micrometers) makes In(.53)Ga(.47)As an idea match to the available airglow that has major peaks at 1.3 micrometers and 1.6 micrometers. The short wavelength 'cut-on' at 0.9 micrometers is due to absorption in the InP substrate. We will report on new InGaAs FPA epitaxial structures and processing techniques. These have resulted in improved performance in the form of a 10 x increase in detectivity and visible response via removal of the InP substrate. The resulting device features visible and SWIR response with greater than 15% quantum efficiency at 0.5 micrometers while maintaining the long wavelength cutoff. Imaging has been demonstrated under overcast starlight/urban glow conditions with cooling provided by a single stage thermoelectric cooler. Details on the material structure and device fabrication, quantitative characterization of spectral response and detectivity, as well as examples of night vision imagery are presented.
Cohen, Marshall J.↗
The analysis of Raman scattering in a free-electron laser with a rectangular hybrid wiggler
A one dimensional theory of the stimulated Raman backscattering process in a free electron laser with rectangular hybrid wiggler (RHW) is analyzed. The dispersion relation in the rest frame of the electron beam and also a formula for the lab-frame spatial growth rate are derived. A numerical computation of the growth rate for RHW is conducted and a comparison with that for coaxial hybrid wiggler is made away from the resonance. The growth rate is found larger for the rectangular wiggler than for the coaxial wiggler. A much narrower magnetoresonance associated with the third spatial harmonic is also obtained compared to the first one.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Functional Imaging of Hybrid Nanostructures: Visualization of Mechanisms for Solar Energy Utilization
The report describes advances in understanding the interaction of light with hybrid nanostructured materials, and the influence of physical and electronic structure on the flow of excess energetic charge carriers to support the design and optimization of new materials for photoelectrical and photoelectrochemical energy conversion. Raman scattering, multi-wavelength optical excitation, and numerical modeling are combined with electrical transport measurements on model hybrid materials structures and devices to resolve, in energy and space, the absorption of light, the generation of excess energetic charge carriers, and the efficiency of their separation to generate electrical and chemical energy. Appropriate combinations of spatially-resolved, time-resolved, and spectrally-resolved measurements are used to isolate and quantify various steps in the energy conversion process, including geometrically and plasmonically enhanced absorption, the generation of carriers with excess energy, and the efficiency with which the carriers can move to and perform useful chemistry at interfaces.
14 SOLAR ENERGY↗
NASA Tech Briefs, October 2010
Topics covered include: Hybrid Architecture Active Wavefront Sensing and Control; Carbon-Nanotube-Based Chemical Gas Sensor; Aerogel-Positronium Technology for the Detection of Small Quantities of Organic and/or Toxic Materials; Graphene-Based Reversible Nano-Switch/Sensor Schottky Diode; Inductive Non-Contact Position Sensor; High-Temperature Surface-Acoustic-Wave Transducer; Grid-Sphere Electrodes for Contact with Ionospheric Plasma; Enabling IP Header Compression in COTS Routers via Frame Relay on a Simplex Link; Ka-Band SiGe Receiver Front-End MMIC for Transponder Applications; Robust Optimization Design Algorithm for High-Frequency TWTs; Optimal and Local Connectivity Between Neuron and Synapse Array in the Quantum Dot/Silicon Brain; Method and Circuit for In-Situ Health Monitoring of Solar Cells in Space; BGen: A UML Behavior Network Generator Tool; Platform for Post-Processing Waveform-Based NDE; Electrochemical Hydrogen Peroxide Generator; Fabrication of Single, Vertically Aligned Carbon Nanotubes in 3D Nanoscale Architectures; Process to Create High-Fidelity Lunar Dust Simulants; Lithium-Ion Electrolytes Containing Phosphorous-Based, Flame-Retardant Additives; InGaP Heterojunction Barrier Solar Cells; Straight-Pore Microfilter with Efficient Regeneration; Determining Shear Stress Distribution in a Laminate; Self-Adjusting Liquid Injectors for Combustors; Handling Qualities Prediction of an F-16XL-Based Reduced Sonic Boom Aircraft; Tele-Robotic ATHLETE Controller for Kinematics - TRACK; Three-Wheel Brush-Wheel Sampler; Heterodyne Interferometer Angle Metrology; Aligning Astronomical Telescopes via Identification of Stars; Generation of Optical Combs in a WGM Resonator from a Bichromatic Pump; Large-Format AlGaN PIN Photodiode Arrays for UV Images; Fiber-Coupled Planar Light-Wave Circuit for Seed Laser Control in High Spectral Resolution Lidar Systems; On Calculating the Zero-Gravity Surface Figure of a Mirror; Optical Modification of Casimir Forces for Improved Function of Micro- and Nano-Scale Devices; Analysis, Simulation, and Verification of Knowledge-Based, Rule-Based, and Expert Systems; Core and Off-Core Processes in Systems Engineering; Digital Reconstruction Supporting Investigation of Mishaps; and Template Matching Approach to Signal Prediction.
Source record↗
Silicon-On-Silicon Carbide Platform for Integrated Photonics
Silicon carbide (SiC)'s nonlinear optical properties and applications to quantum information have recently brought attention to its potential as an integrated photonics platform. However, despite its many excellent material properties, such as large thermal conductivity, wide transparency window, and strong optical nonlinearities, it is generally a difficult material for microfabrication. Here, it is shown that directly bonded silicon-on-silicon carbide can be a high-performing hybrid photonics platform that does not require the need to form SiC membranes or directly pattern in SiC. The optimized bonding method yields defect-free, uniform films with minimal oxide at the silicon–silicon–carbide interface. Ring resonators are patterned into the silicon layer with standard, complimentary metal–oxide–semiconductor (CMOS) compatible (Si) fabrication and measure room-temperature, near-infrared quality factors exceeding 10 5 . The corresponding propagation loss is 5.7 dB cm -1 . The process offers a wafer-scalable pathway to the integration of SiC photonics into CMOS devices.
36 MATERIALS SCIENCE↗
Additive manufacturing of soft magnets for electrical machines—a review
Not Available
36 MATERIALS SCIENCE↗
Atomically Abrupt Topological p–n Junction
Topological insulators (TI’s) are a new class of quantum matter with extraordinary surface electronic states, which bear great potential for spintronics and error-tolerant quantum computing. In order to put a TI into any practical use, these materials need to be fabricated into devices whose basic units are often p–n junctions. Interesting electronic properties of a ‘topological’ p–n junction were proposed theoretically such as the junction electronic state and the spin rectification. However, the fabrication of a lateral topological p–n junction has been challenging because of materials, process, and fundamental reasons. Here, we demonstrate an innovative approach to realize a p–n junction of topological surface states (TSS’s) of a three-dimensional (3D) topological insulator (TI) with an atomically abrupt interface. When a ultrathin Sb film is grown on a 3D TI of Bi 2 Se 3 with a typical n-type TSS, the surface develops a strongly p-type TSS through the substantial hybridization between the 2D Sb film and the Bi 2 Se 3 surface. Thus, the Bi 2 Se 3 surface covered partially with Sb films bifurcates into areas of n- and p-type TSS’s as separated by atomic step edges with a lateral electronic junction of as short as 2 nm. This approach opens a different avenue toward various electronic and spintronic devices based on well-defined topological p–n junctions with the scalability down to atomic dimensions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Green syntheses of stable and efficient organic dyes for organic hybrid light-emitting diodes
Organic hybrid light-emitting diodes (hybrid-LEDs) employ organic dyes as light converters on top of commercial blue inorganic LEDs, replacing incumbent inorganic phosphor light converters synthesized from rare-earth and/or toxic metallic elements to optimize device environmental sustainability. Here, we present two naturally derived organic dyes for hybrid-LEDs, highlighting stability and efficiency enhancement based on a novel “acceptor–acceptor” molecular design. This “acceptor–acceptor” skeleton comprises theobromine and thiadiazole, two electron-withdrawing groups that lower energy levels and suppress photooxidation. This differentiates these dyes from the widely adopted “donor–acceptor” skeleton, where photooxidation is facilitated by the presence of electron-donating units. Simultaneously, sidechains on organic dyes used to enhance solution processability, crucial for film transparency, introduce an additional photooxidation pathway. With this “acceptor–acceptor” skeleton, the destabilization from sidechains was offset by the stability enhancement from the electronic effects in the backbone. Additionally, when blended within an industrial polymer, poly(styrene-butadiene-styrene) (SBS), their enhanced solubility enables the formation of highly transparent films, crucial for reducing scattering loss in LEDs. Furthermore, resultant dye-SBS films achieved photoluminescence quantum yields (PLQYs) of around 90% under ambient conditions. Taking advantage of their transparency and solution processability, we fabricated a waveguide with this theobromine-dye-SBS composite, which was subsequentially assembled into an edge-lit LED device of no glare and enhanced aesthetics.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗