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At least 487 records · Page 27

Superior photo-carrier diffusion dynamics in organic-inorganic hybrid perovskites revealed by spatiotemporal conductivity imaging

Abstract The outstanding performance of organic-inorganic metal trihalide solar cells benefits from the exceptional photo-physical properties of both electrons and holes in the material. Here, we directly probe the free-carrier dynamics in Cs-doped FAPbI 3 thin films by spatiotemporal photoconductivity imaging. Using charge transport layers to selectively quench one type of carriers, we show that the two relaxation times on the order of 1 μs and 10 μs correspond to the lifetimes of electrons and holes in FACsPbI 3 , respectively. Strikingly, the diffusion mapping indicates that the difference in electron/hole lifetimes is largely compensated by their disparate mobility. Consequently, the long diffusion lengths (3~5 μm) of both carriers are comparable to each other, a feature closely related to the unique charge trapping and de-trapping processes in hybrid trihalide perovskites. Our results unveil the origin of superior diffusion dynamics in this material, crucially important for solar-cell applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Imaging Valley Excitons in a 2D Semiconductor with Scanning Tunneling Microscope-Induced Luminescence

Valley excitons dominate the optoelectronic response of transition-metal dichalcogenides and are drastically affected by structural and environmental inhomogeneities localized in these materials. Critical to understanding and controlling these nanoscale excitonic changes is the ability to correlate the imaging of excitonic states with crystalline structures on the atomic scale. Here, in this study, we apply scanning tunneling microscope-induced luminescence microscopy to image valley excitons in a semiconducting transition-metal dichalcogenide monolayer decoupled by a 10 nanometer-thick hexagonal-boron-nitride flake incorporated in a lateral homojunction on an Au electrode surface. This design enables the observation of chiral excitonic emission arising from neutral and charged valley excitons of the monolayer semiconductor at ambipolar voltages with a quantum efficiency up to similar to ~10 -5 photon/electron. The measured light helicity demonstrates considerable circular polarization dependent on the sample voltage, reaching as much as 40%. The real-space luminescence imaging maps$-$at subnanometer resolution$-$of the valley excitons reveal striking spatial variations associated with localized inhomogeneities, including surface impurities and possibly nanoscale dielectric and/or potential disorders in the monolayer. Our study introduces a promising format for 2D materials to explore and tailor their optoelectronic processes at the atomic scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Space- and time-resolved characterization of nanosecond time scale discharge at pressurized gas

The phenomenon of ultra-fast electrical gas breakdown was investigated. Nanosecond high-voltage pulses with durations of 1 and 5 ns and amplitudes of 100 and 200 kV, respectively, were used to study the parameters of the discharge in a pressured (1-7) x 10{sup 5} Pa air-filled gap. The development of the discharge and the plasma propagation velocity was examined using optical fast frame imaging. The generation of runaway electrons in the breakdown process was confirmed by electron imaging and time-resolved x-ray diagnostics. Runaway electron beam energy distribution was obtained for a 1 ns duration high-voltage pulse. The origin and the role of runaway electrons in the discharge initiation are also discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Simultaneous sample and spatial coherence characterisation using diffractive imaging

We demonstrate an algorithm that reconstructs the complex transmission function of an object from experimental X-ray diffraction data using partially coherent 1.4 keV X-rays that does not require a priori input of the coherence function. The quality of the reconstruction is significantly better than that obtained by assuming that the illumination is fully coherent. Our approach can be readily applied to diffraction imaging problems where a model for the spatial coherence can be assumed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quantum-Well Infrared Photodetector (QWIP) Focal Plane Assembly

A paper describes the Thermal Infrared Sensor (TIRS), a QWIP-based instrument intended to supplement the Operational Land Imager (OLI) for the Landsat Data Continuity Mission (LDCM). The TIRS instrument is a far-infrared imager operating in the pushbroom mode with two IR channels: 10.8 and 12 microns. The focal plane will contain three 640x512 QWIP arrays mounted on a silicon substrate. The silicon substrate is a custom-fabricated carrier board with a single layer of aluminum interconnects. The general fabrication process starts with a 4-in. (approx.10-cm) diameter silicon wafer. The wafer is oxidized, a single substrate contact is etched, and aluminum is deposited, patterned, and alloyed. This technology development is aimed at incorporating three large-format infrared detecting arrays based on GaAs QWIP technology onto a common focal plane with precision alignment of all three arrays. This focal plane must survive the rigors of flight qualification and operate at a temperature of 43 K (-230 C) for five years while orbiting the Earth. The challenges presented include ensuring thermal compatibility among all the components, designing and building a compact, somewhat modular system and ensuring alignment to very tight levels. The multi-array focal plane integrated onto a single silicon substrate is a new application of both QWIP array development and silicon wafer scale integration. The Invar-based assembly has been tested to ensure thermal reliability.

Jhabvala, Murzy↗

Atomically Precise Surface Engineering for Producing Imagers

High-quality surface coatings, and techniques combining the atomic precision of molecular beam epitaxy and atomic layer deposition, to fabricate such high-quality surface coatings are provided. The coatings made in accordance with the techniques set forth by the invention are shown to be capable of forming silicon CCD detectors that demonstrate world record detector quantum efficiency (>50%) in the near and far ultraviolet (155 nm-300 nm). The surface engineering approaches used demonstrate the robustness of detector performance that is obtained by achieving atomic level precision at all steps in the coating fabrication process. As proof of concept, the characterization, materials, and exemplary devices produced are presented along with a comparison to other approaches.

Greer, Frank↗

In situ formation of pseudohalide anions induced by humid air and light passivates formamidinium‐based halide perovskites

Abstract Metal halide perovskites based on formamidinium (FA), or FA‐rich compositions have shown great promise for high‐performance photovoltaics. A deeper understanding of the impact of ambient conditions (e.g., moisture, oxygen, and illumination) on the possible reactions of FA‐based perovskite films and their processing sensitivities has become critical for further advances toward commercialization. Herein, we investigate reactions that take place on the surface of the FA 0.7 Cs 0.3 , mixed Br/I wide bandgap perovskite thin films in the presence of humid air and ambient illumination. The treatment forms a surface layer containing O, OH, and N‐based anions. We propose the latter originates from formamidine trapped at the perovskite/oxide interface reacting further to cyanide and/or formamidinate—an understudied class of pseudohalides that bind to Pb. Optimized treatment conditions improve photoluminescence quantum yield owing to both reduced surface recombination velocity and increased bulk carrier lifetime. The corresponding perovskite solar cells also exhibit improved performance. Identifying these reactions opens possibilities for better utilizing cyanide and amidinate ligands, species that may be expected during vapor processing of FA‐based perovskites. Our work also provides new insights into the self‐healing or self‐passivating of MA‐free perovskite compositions where FA and iodide damage could be partially offset by advantageous reaction byproducts. image

14 SOLAR ENERGY↗

Time-resolved 3D imaging of two-phase fluid flow inside a steel fuel injector using synchrotron X-ray tomography

The multiphase flow inside a diesel injection nozzle is imaged using synchrotron X-rays from the Advanced Photon Source at Argonne National Laboratory. Through acquisitions performed at several viewing angles and subsequent tomographic reconstruction, in-situ 3D visualization is achieved for the first time inside a steel injector at engine-like operating conditions. The morphology of the internal flow reveals strong flow separation and vapor-filled cavities (cavitation), the degree of which correlates with the nozzle's asymmetric inlet corner profile. Micron-scale surface features, which are artifacts of manufacturing, are shown to influence the morphology of the resulting liquid-gas interface. The data obtained at 0.1 ms time resolution exposes transient flow features and the flow development timescales are shown to be correlated with in-situ imaging of the fuel injector's hydraulically-actuated valve (needle). As more than 98.5% of the X-ray photon flux is attenuated within the steel injector body itself, we are posed with a unique challenge for imaging the flow within. Time-resolved imaging under these low-light conditions is achieved by exploiting both the refractive and absorptive properties of X-ray photons. The data-processing strategy converted these images with a signal-to-noise ratio of similar to 10 into a meaningful dataset for understanding internal flow and cavitation in a nozzle of diameter 200 mu m enclosed within 1-2 millimeters of steel.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Development of quantum dot materials for infrared cameras (Final CRADA Report)

The aim of this project was to develop scalable methods to produce infrared (IR) mercury telluride (HgTe) colloidal quantum dot (CQD) thin films and demonstrate their utility in a proof-of-concept monolithic SWIR focal plane array (FPA). These objectives were accomplished by scaling up the HgTe CQD synthesis, characterizing physical and electrical properties of HgTe CQDs, evaluating solution-processed coating methods for quality and efficiency, and developing a process flow to integrate HgTe CQDs with commercial-off-the-shelf silicon CMOS readout circuits by solution-processed coating to produce monolithic FPAs. The FPA is the image sensor in an infrared imaging system responsible for detecting and processing reflected or emitted light into an infrared image of the scene under observation. The quality of the image is determined by the sensitivity and resolution of the image sensor in the system. Higher resolution IR FPAs enable higher throughput in manufacturing quality assurance, wider field of view for autonomous navigation, and longer range surveillance for defense.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Computational and experimental characterization of high-brightness beams for femtosecond electron imaging and spectroscopy

Using a multilevel fast multipole method, coupled with the shadow imaging of femtosecond photoelectron pulses for validation, we quantitatively elucidate the photocathode, space charge, and virtual cathode physics, which fundamentally limit the spatiotemporal and spectroscopic resolution and throughput of ultrafast electron microscope (UEM) systems. We present a simple microscopic description to capture the nonlinear beam dynamics based on a two-fluid picture and elucidate an unexpected dominant role of image potential pinning in accelerating the emittance growth process. These calculations set theoretical limits on the performance of UEM systems and provide useful guides for photocathode design for high-brightness electron beam systems.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Angle sensitive single photon avalanche diode

An ideal light sensor would provide exact information on intensity, timing, location, and angle of incoming photons. Single photon avalanche diodes (SPADs) provide such desired high (single photon) sensitivity with precise time information and can be implemented at a pixel-scale to form an array to extract spatial information. Furthermore, recent work has demonstrated photodiode-based structures (combined with micro-lenses or diffraction gratings) that are capable of encoding both spatial and angular information of incident light. In this letter, we describe the implementation of such a grating structure on SPADs to realize a pixel-scale angle-sensitive single photon avalanche diode (A-SPAD) built in a standard CMOS process. While the underlying SPAD structure provides high sensitivity, the time information of the two layers of diffraction gratings above offers angle-sensitivity. Such a unique combination of SPAD and diffraction gratings expands the sensing dimensions to pave a path towards lens-less 3-D imaging and light-field time-of-flight imaging.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Narrow-band near-field nanoscopy in the spectral range from 1.3 to 8.5 THz

Nano-spectroscopy in the terahertz frequency range remains challenging despite recent technological progress in developing both THz emitter sources and near-field optical microscopy (SNOM). Here, we combine scattering-type SNOM with a free-electron laser light source, to tune into the 1.3–8.5 THz range. A significant portion of this range, namely, the frequencies above ∼3 THz, is not covered by previously reported near-field microscopy systems. However, it constitutes an indispensable regime where many elementary processes in solids including collective lattice excitations, charge, and spin transport occur. Our approach of nano-spectroscopy and nano-imaging provides a versatile analysis of nanostructures as small as 50 nm, hence beating the optical diffraction limit by λ/4600.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

A dedicated cone-beam CT system for musculoskeletal extremities imaging: Design, optimization, and initial performance characterization

Purpose: This paper reports on the design and initial imaging performance of a dedicated cone-beam CT (CBCT) system for musculoskeletal (MSK) extremities. The system complements conventional CT and MR and offers a variety of potential clinical and logistical advantages that are likely to be of benefit to diagnosis, treatment planning, and assessment of therapy response in MSK radiology, orthopaedic surgery, and rheumatology. Methods: The scanner design incorporated a host of clinical requirements (e.g., ability to scan the weight-bearing knee in a natural stance) and was guided by theoretical and experimental analysis of image quality and dose. Such criteria identified the following basic scanner components and system configuration: a flat-panel detector (FPD, Varian 3030+, 0.194 mm pixels); and a low-power, fixed anode x-ray source with 0.5 mm focal spot (SourceRay XRS-125-7K-P, 0.875 kW) mounted on a retractable C-arm allowing for two scanning orientations with the capability for side entry, viz. a standing configuration for imaging of weight-bearing lower extremities and a sitting configuration for imaging of tensioned upper extremity and unloaded lower extremity. Theoretical modeling employed cascaded systems analysis of modulation transfer function (MTF) and detective quantum efficiency (DQE) computed as a function of system geometry, kVp and filtration, dose, source power, etc. Physical experimentation utilized an imaging bench simulating the scanner geometry for verification of theoretical results and investigation of other factors, such as antiscatter grid selection and 3D image quality in phantom and cadaver, including qualitative comparison to conventional CT. Results: Theoretical modeling and benchtop experimentation confirmed the basic suitability of the FPD and x-ray source mentioned above. Clinical requirements combined with analysis of MTF and DQE yielded the following system geometry: a {approx}55 cm source-to-detector distance; 1.3 magnification; a 20 cm diameter bore (20 x 20 x 20 cm{sup 3} field of view); total acquisition arc of {approx}240 deg. The system MTF declines to 50% at {approx}1.3 mm{sup -1} and to 10% at {approx}2.7 mm{sup -1}, consistent with sub-millimeter spatial resolution. Analysis of DQE suggested a nominal technique of 90 kVp (+0.3 mm Cu added filtration) to provide high imaging performance from {approx}500 projections at less than {approx}0.5 kW power, implying {approx}6.4 mGy (0.064 mSv) for low-dose protocols and {approx}15 mGy (0.15 mSv) for high-quality protocols. The experimental studies show improved image uniformity and contrast-to-noise ratio (without increase in dose) through incorporation of a custom 10:1 GR antiscatter grid. Cadaver images demonstrate exquisite bone detail, visualization of articular morphology, and soft-tissue visibility comparable to diagnostic CT (10-20 HU contrast resolution). Conclusions: The results indicate that the proposed system will deliver volumetric images of the extremities with soft-tissue contrast resolution comparable to diagnostic CT and improved spatial resolution at potentially reduced dose. Cascaded systems analysis provided a useful basis for system design and optimization without costly repeated experimentation. A combined process of design specification, image quality analysis, clinical feedback, and revision yielded a prototype that is now awaiting clinical pilot studies. Potential advantages of the proposed system include reduced space and cost, imaging of load-bearing extremities, and combined volumetric imaging with real-time fluoroscopy and digital radiography.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Advances in coherent coupling between magnons and acoustic phonons

The interaction between magnetic and acoustic excitations have recently inspired many interdisciplinary studies ranging from fundamental physics to circuit implementation. Specifically, the exploration of their coherent interconversion enabled via the magnetoelastic coupling opens a new playground combining straintronics and spintronics, and provides a unique platform for building up on-chip coherent information processing networks with miniaturized magnonic and acoustic devices. In this Perspective, we will focus on the recent progress of magnon-phonon coupled dynamic systems, including materials, circuits, imaging and new physics. In particular, we highlight the unique features such as nonreciprocal acoustic wave propagation and strong coupling between magnons and phonons in magnetic thin-film systems, which provides a unique platform for their coherent manipulation and transduction. We will also review the frontier of surface acoustic wave resonators in coherent quantum transduction and discuss how the novel acoustic circuit design can be applied in microwave spintronics.

36 MATERIALS SCIENCE↗

Images of the future - Two decades in astronomy

Future instruments for the 100-10,000 A UV-wavelength region will require detectors with greater quantum efficiency, smaller picture elements, a greater wavelength range, and greater active area than those currently available. After assessing the development status and performance characteristics of vidicons, image tubes, electronographic cameras, digicons, silicon arrays and microchannel plate intensifiers presently employed by astronomical spacecraft, attention is given to such next-generation detectors as the Mosaicked Optical Self-scanned Array Imaging Camera, which consists of a photocathode deposited on the input side of a microchannel plate intensifier. The problems posed by the signal processing and data analysis requirements of the devices foreseen for the 21st century are noted.

Weistrop, D.↗

Software optimization for electrical conductivity imaging in polycrystalline diamond cutters

We previously reported on an electrical conductivity imaging instrument developed for measurements on polycrystalline diamond cutters. These cylindrical cutters for oil and gas drilling feature a thick polycrystalline diamond layer on a tungsten carbide substrate. The instrument uses electrical impedance tomography to profile the conductivity in the diamond table. Conductivity images must be acquired quickly, on the order of 5 sec per cutter, to be useful in the manufacturing process. This paper reports on successful efforts to optimize the conductivity reconstruction routine, porting major portions of it to NVIDIA GPUs, including a custom CUDA kernel for Jacobian computation.

36 MATERIALS SCIENCE↗

Reconstruction and uncertainty quantification of lattice Hamiltonian model parameters from observations of microscopic degrees of freedom

The emergence of scanning probe and electron beam imaging techniques has allowed quantitative studies of atomic structure and minute details of electronic and vibrational structure on the level of individual atomic units. These microscopic descriptors, in turn, can be associated with local symmetry breaking phenomena, representing the stochastic manifestation of the underpinning generative physical model. In this work, we explore the reconstruction of exchange integrals in the Hamiltonian for a lattice model with two competing interactions from observations of microscopic degrees of freedom and establish the uncertainties and reliability of such analysis in a broad parameter-temperature space. In contrast to other approaches, we specifically specify a loss function inherent to thermodynamic systems and utilize it to estimate uncertainty in simulated realizations of different models. As an ancillary task, we develop a machine learning approach based on histogram clustering to predict phase diagrams efficiently using a reduced descriptor space. We further demonstrate that reconstruction is possible well above the phase transition and in the regions of parameter space when the macroscopic ground state of the system is poorly defined due to frustrated interactions. This suggests that this approach can be applied to the traditionally complex problems of condensed matter physics such as ferroelectric relaxors and morphotropic phase boundary systems, spin and cluster glasses, and quantum systems once the local descriptors linked to the relevant physical behaviors are known.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗