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At least 649 records · Page 36

Photoinduced surface voltage mapping study for large perovskite single crystals

Using a series of illumination sources, including white light (tungsten-halogen lamp), 445-nm, 532-nm, 635-nm, and 730-nm lasers, the surface photovoltage (SPV) images were mapped for centimeter-sized CH{sub 3}NH{sub 3}PbX{sub 3} (X = Cl, Br, I) perovskite single crystals using Kelvin probe force microscopy. The significant SPV signals were observed to be wavelength-dependent. We attribute the appreciable SPV to the built-in electric field in the space charge region. This study shines light into the understanding of photoinduced charge generation and separation processes at nanoscale to help advance the development of perovskite solar cells, optoelectronics, laser, photodetector, and light-emitting diode (LED).

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Propagating Structure Of A Microwave Driven Shock wave Inside A Tube

The thrust generation process of a microwave rocket is similar to a pulse detonation engine, and understanding the interactions between microwave plasma and shock waves is important. Shadowgraph images of the microwave plasma generated in a tube under atmospheric air were taken. The observed plasma and shock wave were propagating one-dimensionally at constant velocity inside the tube. In order to understand the flow field inside the rocket, one-dimensional CFD analysis was conducted. With the change of microwave power density, the structure of the flow field was classified into two regimes: Microwave Supported Combustion (MSC), and Microwave Supported Detonation (MSD). The structure of the MSD was different from the structure of a chemical detonation, which implied the existence of a preheating in front of the shock wave. Furthermore, the flight performance was estimated by calculating the momentum coupling coefficient. It was confirmed that the efficiency was nearly constant in the MSD regime, with the increase of microwave power density.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Mechanism of β-FeSi{sub 2} precipitates growth-and-dissolution and pyramidal defects' formation during oxidation of Fe-contaminated silicon wafers

Fe-implanted Si-wafers have been oxidized at 900 °C and 1100 °C in order to investigate the behaviour of Fe atoms at the growing SiO{sub 2}/Si interface and the impact on the integrity of microelectronic devices of an involuntary Fe contamination before or during the oxidation process. As-implanted and oxidized wafers have been characterized using secondary ion mass spectroscopy, atom probe tomography, and high-resolution transmission electron microscopy. Experimental results were compared to calculated implantation profiles and simulated images. Successive steps of iron disilicide precipitation and oxidation were evidenced during the silicon oxidation process. The formation of characteristic pyramidal-shaped defects, at the SiO{sub 2}/Si interface, was notably found to correlate with the presence of β-FeSi{sub 2} precipitates. Taking into account the competitive oxidation of these precipitates and of the surrounding silicon matrix, dynamic mechanisms are proposed to model the observed microstructural evolution of the SiO{sub 2}/Si interface, during the growth of the silicon oxide layer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The anisotropic nature of singlet fission in single crystalline organic semiconductors

The escalating global energy predicament implores for a revolutionary resolution—one that converts sunlight into electricity—holding the key to supreme conversion efficiency. This comprehensive review embarks on the exploration of the principle of generating multiple excitons per absorbed photon, a captivating concept that possesses the potential to redefine the fundamental confines of conversion efficiency, albeit its application remains limited in photovoltaic devices. At the nucleus of this phenomenon are two principal processes: multiple exciton generation (MEG) within quantum-confined environments, and singlet fission (SF) inside molecular crystals. The process of SF, characterized by the cleavage of a single photogenerated singlet exciton into two triplet excitons, holds promise to potentially amplify photon-to-electron conversion efficiency twofold, thereby laying the groundwork to challenge the detailed balance limit of solar cell efficiency. Our discourse primarily dissects the complex nature of SF in crystalline organic semiconductors, laying special emphasis on the anisotropic behavior of SF and the diffusion of the subsequent triplet excitons in single-crystalline polyacene organic semiconductors. We initiate this journey of discovery by elucidating the principles of MEG and SF, tracing their historical genesis, and scrutinizing the anisotropy of SF and the impact of quantum decoherence within the purview of functional mode electron transfer theory. We present an overview of prominent techniques deployed in investigating anisotropic SF in organic semiconductors, including femtosecond transient absorption microscopy and imaging as well as stimulated Raman scattering microscopies, and highlight recent breakthroughs linked with the anisotropic dimensions of Davydov splitting, Herzberg–Teller effects, SF, and triplet transport operations in single-crystalline polyacenes. Through this comprehensive analysis, our objective is to interweave the fundamental principles of anisotropic SF and triplet transport with the current frontiers of scientific discovery, providing inspiration and facilitating future ventures to harness the anisotropic attributes of organic semiconductor crystals in the design of pioneering photovoltaic and photonic devices.

Chemistry↗

Energy flow networks: deep sets for particle jets

A key question for machine learning approaches in particle physics is how to best represent and learn from collider events. As an event is intrinsically a variable-length unordered set of particles, we build upon recent machine learning efforts to learn directly from sets of features or “point clouds”. Adapting and specializing the “Deep Sets” framework to particle physics, we introduce Energy Flow Networks, which respect infrared and collinear safety by construction. We also develop Particle Flow Networks, which allow for general energy dependence and the inclusion of additional particle-level information such as charge and flavor. These networks feature a per-particle internal (latent) representation, and summing over all particles yields an overall event-level latent representation. We show how this latent space decomposition unifies existing event representations based on detector images and radiation moments. To demonstrate the power and simplicity of this set-based approach, we apply these networks to the collider task of discriminating quark jets from gluon jets, finding similar or improved performance compared to existing methods. We also show how the learned event representation can be directly visualized, providing insight into the inner workings of the model. These architectures lend themselves to efficiently processing and analyzing events for a wide variety of tasks at the Large Hadron Collider. Implementations and examples of our architectures are available online in our EnergyFlow package.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Direct evidence of microstructure dependence of magnetic flux trapping in niobium

Abstract Elemental type-II superconducting niobium is the material of choice for superconducting radiofrequency cavities used in modern particle accelerators, light sources, detectors, sensors, and quantum computing architecture. An essential challenge to increasing energy efficiency in rf applications is the power dissipation due to residual magnetic field that is trapped during the cool down process due to incomplete magnetic field expulsion. New SRF cavity processing recipes that use surface doping techniques have significantly increased their cryogenic efficiency. However, the performance of SRF Nb accelerators still shows vulnerability to a trapped magnetic field. In this manuscript, we report the observation of a direct link between flux trapping and incomplete flux expulsion with spatial variations in microstructure within the niobium. Fine-grain recrystallized microstructure with an average grain size of 10–50 µm leads to flux trapping even with a lack of dislocation structures in grain interiors. Larger grain sizes beyond 100–400 µm do not lead to preferential flux trapping, as observed directly by magneto-optical imaging. While local magnetic flux variations imaged by magneto-optics provide clarity on a microstructure level, bulk variations are also indicated by variations in pinning force curves with sequential heat treatment studies. The key results indicate that complete control of the niobium microstructure will help produce higher performance superconducting resonators with reduced rf losses 1 related to the magnetic flux trapping.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Imaging properties and its improvements of scanning/imaging x-ray microscope

A scanning / imaging X-ray microscope (SIXM) system has been developed at SPring-8. The SIXM consists of a scanning X-ray microscope with a one-dimensional (1D) X-ray focusing device and an imaging (full-field) X-ray microscope with a 1D X-ray objective. The motivation of the SIXM system is to realize a quantitative and highly-sensitive multimodal 3D X-ray tomography by taking advantages of both the scanning X-ray microscope using multi-pixel detector and the imaging X-ray microscope. Data acquisition process of a 2D image is completely different between in the horizontal direction and in the vertical direction; a 1D signal is obtained with the linear-scanning while the other dimensional signal is obtained with the imaging optics. Such condition have caused a serious problem on the imaging properties that the imaging quality in the vertical direction has been much worse than that in the horizontal direction. In this paper, two approaches to solve this problem will be presented. One is introducing a Fourier transform method for phase retrieval from one phase derivative image, and the other to develop and employ a 1D diffuser to produce an asymmetrical coherent illumination.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Understanding palladium–tellurium cluster formation on WTe2: From a kinetically hindered distribution to thermodynamically controlled monodispersity

Abstract A fundamental understanding of the transition metal dichalcogenide (TMDC)–metal interface is critical for their utilization in a broad range of applications. We investigate how the deposition of palladium (Pd), as a model metal, on WTe2(001), leads to the assembly of Pd into clusters and nanoparticles. Using X-ray photoemission spectroscopy, scanning tunneling microscopy imaging, and ab initio simulations, we find that Pd nucleation is driven by the interaction with and the availability of mobile excess tellurium (Te) leading to the formation of Pd-Te clusters at room temperature. Surprisingly, the nucleation of Pd-Te clusters is not affected by intrinsic surface defects, even at elevated temperatures. Upon annealing, the Pd-Te nanoclusters adopt an identical nanostructure and are stable up to ∼523 K. Density functional theory calculations provide a foundation for our understanding of the mobility of Pd and Te atoms, preferential nucleation of Pd-Te clusters, and the origin of their annealing-induced monodispersity. These results highlight the role the excess chalcogenide atoms may play in the metal deposition process. More broadly, the discoveries of synthetic pathways yielding thermally robust monodispersed nanostructures on TMDCs are critical to the manufacturing of novel quantum and microelectronics devices and catalytically active nano-alloy centers.

36 MATERIALS SCIENCE↗

SISGR: Atom chip microscopy: A novel probe for strongly correlated materials

Microscopy techniques co-opted from nonlinear optics and high energy physics have complemented solid-state probes in elucidating the order manifest in condensed matter materials. Up until now, however, no attempts have been made to use modern techniques of ultracold atomic physics to directly explore properties of strongly correlated or topologically protected materials. Our current program is focused on introducing a novel magnetic field microscopy technique into the toolbox of imaging probes. Our prior DOE ESPM program funded the development of a novel instrument using a dilute gas Bose-Einstein condensate (BEC) as a scanning probe capable of measuring tiny magnetic (and electric) DC and AC fields above materials. We successfully built the world's first “scanning cryogenic atom chip microscope”, and we now are in the process of characterizing its performance before using the instrument to take the first wide-area images of transport flow within unconventional superconductors, pnictides and oxide interfaces (LAO/STO), topological insulators, and colossal magnetoresistive manganites. We will do so at temperatures outside the capability of scanning SQUIDs, with ~10x better resolution and without 1/f-noise. A notable goal will be to measure the surface-to-bulk conductivity ratio in topological insulators in a relatively model-independent fashion. We have completed the construction of this magnetic microscope. The instrument uses atom chips—substrates supporting micron-sized current-carrying wires that create magnetic microtraps near surfaces for ultracold thermal gases and BECs—to enable single-shot and raster-scanned large-field-of-view detection of magnetic fields. The fields emanating from electronic transport may be detected at the 10 -7 flux quantum (Φ0) level and below; that is, few to sub-micron resolution of sub-nanotesla fields over single-shot, millimeter-long detection lengths. By harnessing the extreme sensitivity of atomic clocks and BECs to external perturbations, we are now in a position to use atom chips for imaging transport in new regimes. Scanning quantum gas atom chip microscopy introduces three very important features to the toolbox of high-resolution scanning microscopy of strongly correlated or topological materials: simultaneous detection of magnetic and electric fields (down to the sub-single electron charge level; no invasive large magnetic fields or gradients; simultaneous micro- and macroscopic spatial resolution; DC to MHz detection bandwidth; freedom from 1/ƒ flicker noise at low frequencies; and, perhaps most importantly, the complete decoupling of probe and sample temperatures. The atom chip microscope can operate at maximum sensitivity and resolution without regard to the substrate temperature. While the BEC is among the coldest objects realizable (100 nK temperatures are typical), the atom chip substrate can be positioned 1 μm away from the BEC and be as hot as 400 K or as cold as the cryostat can cool. This is because unlike superconducting probes, whose temperature is closely coupled to nearby materials, quantum gases are immune to radiative heating. The energy gap between a Rb atom’s ground state and first excited state far exceeds the typical energy of room-temperature blackbody radiation; such atoms are therefore transparent to radiation heating by materials at room temperature or below. We experimentally demonstrated a new atom chip trapping system that allows the placement and high-resolution imaging of ultracold atoms within microns from any ≤100 μm-thin, UHV-compatible material, while also allowing sample exchange with minimal experimental downtime. The sample is not connected to the atom chip, allowing rapid exchange without perturbing the atom chip or laser cooling apparatus. Exchange of the sample and retrapping of atoms has been performed within a week turnaround, limited only by chamber baking. Moreover, the decoupling of sample and atom chip provides the ability to independently tune the sample temperature and its position with respect to the trapped ultracold gas, which itself may remain in the focus of a high-resolution imaging system. We confine 100-nK BECs of 104 87Rb atoms near a gold-mirrored 100-μm-thick silicon substrate. The substrate can be cooled to 35 K without use of a heat shield, while the atom chip, 120-μm away, remains at room temperature. Atoms may be imaged with 1-μm resolution and retrapped every 16 s, allowing rapid data collection. Straightforward improvements will allow us to push sample temperatures close to 4 K, and improve imaging resolution from 1 μm down to a few-100 nm, thereby providing 10 -9 Φ0 detection sensitivity. We will test the utility of this technique by imaging the magnetic fields emanating from electronic transport and domain percolation in several interesting examples of strongly correlated or topologically protected materials. STM, transport, and x-ray scattering experiments have, among others, revealed the existence of a quantum liquid crystal state in iron (pnictide) and cuprate superconductors. This strongly correlated state of matter could also be detected by imaging the fluctuating transport (spatially and in time) of electrons as the phase/regime boundary is crossed between the pnictide non-Fermi liquid (cuprate strange metal) and the pnictide magnetic phase (cuprate pseudogap regime). Our ability to image wide-area inhomogeneous current flow from room-temperature to <10 K will allow us to study the developing domain structure and transport near twin boundary interfaces through the T N ≈50–150 K nematic transition recently identified in bulk transport experiments by Ian Fisher's group in underdoped Fe-arsinide superconductors. Again, this highlights a main feature of our cryogenic atom chip microscope: the ability to image transport regardless of the sample temperature since the BEC, at nK temperatures, is transparent to blackbody radiation, even when held a microns from the surface.

36 MATERIALS SCIENCE↗

Annular beam with segmented phase gradients

An annular beam with a single uniform-intensity ring and multiple segments of phase gradients is proposed in this paper. Different from the conventional superposed vortices, such as the modulated optical vortices and the collinear superposition of multiple orbital angular momentum modes, the designed annular beam has a doughnut intensity distribution whose radius is independent of the phase distribution of the beam in the imaging plane. The phase distribution along the circumference of the doughnut beam can be segmented with different phase gradients. Similar to a vortex beam, the annular beam can also exert torques and rotate a trapped particle owing to the orbital angular momentum of the beam. As the beam possesses different phase gradients, the rotation velocity of the trapped particle can be varied along the circumference. The simulation and experimental results show that an annular beam with three segments of different phase gradients can rotate particles with controlled velocities. The beam has potential applications in optical trapping and optical information processing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Near-Infrared Photon-Counting Camera for High-Sensitivity Observations

The dark current of a transferred-electron photocathode with an InGaAs absorber, responsive over the 0.9-to-1.7- micron range, must be reduced to an ultralow level suitable for low signal spectral astrophysical measurements by lowering the temperature of the sensor incorporating the cathode. However, photocathode quantum efficiency (QE) is known to reduce to zero at such low temperatures. Moreover, it has not been demonstrated that the target dark current can be reached at any temperature using existing photocathodes. Changes in the transferred-electron photocathode epistructure (with an In- GaAs absorber lattice-matched to InP and exhibiting responsivity over the 0.9- to-1.7- m range) and fabrication processes were developed and implemented that resulted in a demonstrated >13x reduction in dark current at -40 C while retaining >95% of the approximately equal to 25% saturated room-temperature QE. Further testing at lower temperature is needed to confirm a >25 C predicted reduction in cooling required to achieve an ultralow dark-current target suitable for faint spectral astronomical observations that are not otherwise possible. This reduction in dark current makes it possible to increase the integration time of the imaging sensor, thus enabling a much higher near-infrared (NIR) sensitivity than is possible with current technology. As a result, extremely faint phenomena and NIR signals emitted from distant celestial objects can be now observed and imaged (such as the dynamics of redshifting galaxies, and spectral measurements on extra-solar planets in search of water and bio-markers) that were not previously possible. In addition, the enhanced NIR sensitivity also directly benefits other NIR imaging applications, including drug and bomb detection, stand-off detection of improvised explosive devices (IED's), Raman spectroscopy and microscopy for life/physical science applications, and semiconductor product defect detection.

Jurkovic, Michael↗

Imaging multiphoton ionization dynamics of CH 3 I at a high repetition rate XUV free-electron laser

XUV multiphoton ionization of molecules is commonly used in free-electron laser experiments to study charge transfer dynamics. However, molecular dissociation and electron dynamics, such as multiple photon absorption, Auger decay, and charge transfer, often happen on competing time scales, and the contributions of individual processes can be difficult to unravel. We experimentally investigate the Coulomb explosion dynamics of methyl iodide upon core–hole ionization of the shallow inner-shell of iodine (4d) and classically simulate the fragmentation by phenomenologically introducing ionization dynamics and charge transfer. Under our experimental conditions with medium fluence and relatively long XUV pulses (~75 fs), we find that fast Auger decay prior to charge transfer significantly contributes to the charging mechanism, leading to a yield enhancement of higher carbon charge states upon molecular dissociation. Furthermore, we argue for the existence of another charging mechanism for the weak fragmentation channels leading to triply charged carbon atoms. This study shows that classical simulations can be a useful tool to guide the quantum mechanical description of the femtosecond dynamics upon multiphoton absorption in molecular systems.

Optics↗

Nanoimaging of Electronic Heterogeneity in Bi 2 Se 3 and Sb 2 Te 3 Nanocrystals

Topological insulators (TIs) are quantum materials with topologically protected surface states surrounding an insulating bulk. However, defect-induced bulk conduction often dominates transport properties in most TI materials, obscuring the Dirac surface states. In order to realize intrinsic topological insulating properties, it is thus of great significance to identify the spatial distribution of defects, understand their formation mechanism, and finally control or eliminate their influence. For this study, the electronic heterogeneity in polyol-synthesized Bi 2 Se 3 and chemical vapor deposition-grown Sb 2 Te 3 nanocrystals is systematically investigated by multimodal atomic-to-mesoscale resolution imaging. In particular, by combining the Drude response sensitivity of infrared scattering-type scanning near-field optical microscopy with the work-function specificity of mirror electron microscopy, characteristic mesoscopic patterns are identified, which are related to carrier concentration modulation originating from the formation of defects during the crystal growth process. This correlative imaging and modeling approach thus provides the desired guidance for optimization of growth parameters, crucial for preparing TI nanomaterials to display their intrinsic exotic Dirac properties.

43 PARTICLE ACCELERATORS↗

Origin, Evolution And Imaging Of Vortices In Atomic Processes

Calculations of the time-dependent wave function for proton impact on atomic hydrogen using the Lattice-Time-Dependent-Schroedinger-Equation (LTDSE) method follow the wave function from microscopic to macroscopic times. Isolated zeros, now identified as vortices, appear when the target and projectile nuclei are separated by a few atomic units. Such structure has apparently been observed frequently in ab. initio. calculations. Our work shows that such structures persist to macroscopic distances and appear as 'holes' in electron momentum distributions. They can, in principle, be observed in reaction microscope studies. Such observation is formally justified by the 'imaging theorem', which can be derived from first principles. Similarly, two-electron momentum distributions as observed, e.g., in (e,2e) coincidence measurements may show isolated zeros. Calculations using correlated wave functions support the interpretation that a minima in (e,2e) for helium targets corresponds to a vortex. In this case the 'imaging theorem' can be applied to argue that there must be vortices in the two-electron wave function. A general discussion of vortices in quantum mechanics will be illustrated using exact LTDSE calculations, and, for interpretive purposes, the time-dependent first Born approximation. These calculations show that the plane wave B1 amplitudes have no vortices, but the time-dependent B1 amplitudes do. It will be further shown that angular momentum transfer is the key to forming vortices in the time-dependent theory.

74 ATOMIC AND MOLECULAR PHYSICS↗

Ultrafast probing of ejection dynamics of Rydberg atoms and molecular fragments from electronically excited helium nanodroplets

The ejection dynamics of Rydberg atoms and molecular fragments from electronically excited helium nanodroplets are studied with time-resolved extreme ultraviolet ion imaging spectroscopy. At excitation energies of 23.6 {+-} 0.2 eV, Rydberg atoms in n= 3 and n= 4 states are ejected on different time scales and with significantly different kinetic energy distributions. Specifically, n= 3 Rydberg atoms are ejected with kinetic energies as high as 0.85 eV, but their appearance is delayed by approximately 200 fs. In contrast, n= 4 Rydberg atoms appear within the time resolution of the experiment with considerably lower kinetic energies. Major features in the Rydberg atom kinetic energy distributions for both principal quantum numbers can be described within a simple elastic scattering model of localized perturbed atomic Rydberg atoms that are expelled from the droplet due to their repulsive interaction with the surrounding helium bath. Time-dependent kinetic energy distributions of He{sub 2}{sup +} and He{sub 3}{sup +} ions are presented that support the formation of molecular ions in an indirect droplet ionization process and the ejection of neutral Rydberg dimers on a similar time scale as the n= 3 Rydberg atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Free-electron crystals for enhanced X-ray radiation

Abstract Bremsstrahlung—the spontaneous emission of broadband radiation from free electrons that are deflected by atomic nuclei—contributes to the majority of X-rays emitted from X-ray tubes and used in applications ranging from medical imaging to semiconductor chip inspection. Here, we show that the bremsstrahlung intensity can be enhanced significantly—by more than three orders of magnitude—through shaping the electron wavefunction to periodically overlap with atoms in crystalline materials. Furthermore, we show how to shape the bremsstrahlung X-ray emission pattern into arbitrary angular emission profiles for purposes such as unidirectionality and multi-directionality. Importantly, we find that these enhancements and shaped emission profiles cannot be attributed solely to the spatial overlap between the electron probability distribution and the atomic centers, as predicted by the paraxial and non-recoil theory for free electron light emission. Our work highlights an unprecedented regime of free electron light emission where electron waveshaping provides multi-dimensional control over practical radiation processes like bremsstrahlung. Our results pave the way towards greater versatility in table-top X-ray sources and improved fundamental understanding of quantum electron-light interactions.

47 OTHER INSTRUMENTATION↗