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At least 55 records · Page 3

Ultrafast Waveguiding Quantum Dot Scintillation Detector

Picosecond timing of energetic charged particles and photons is a challenge for many high-energy physics and medical applications. InAs Quantum Dots (QDs) embedded in GaAs matrix are expected to have unsurpassed scintillation properties. The advantages come from highly efficient energy conversion, as well as from fast electron capture and radiative recombination in QDs. Here, we present design considerations and demonstration of an ultrafast, high photon yield room-temperature semiconductor scintillator. Due to the high refractive index of GaAs, the scintillator is fabricated in the form of a20 μm thick planar waveguide with an integrated InGaAs photodiode. QD luminescence of about 60% efficiency at room temperature has been shown, and modal attenuation stabilized at 1 cm -1 . Scintillation responses from 5.5 MeV alpha particles show an extremely fast decay time of 280 ps, a collection efficiency of 11% and a time resolution of 60 ps. This data confirms the unique potential properties of this scintillation detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Laser acceleration and deflection of 963 keV electrons with a silicon dielectric structure

Radio frequency particle accelerators are ubiquitous in ultrasmall and ultrafast science, but their size and cost have prompted exploration of compact and scalable alternatives such as the dielectric laser accelerator. We present the first demonstration, to the best of our knowledge, of high gradient laser acceleration and deflection of electrons with a silicon structure. Driven by a 5 nJ, 130 fs mode-locked Ti:sapphire laser at 907 nm wavelength, our devices achieve accelerating gradients in excess of 200 MeV/m and suboptical cycle streaking of 96.30 keV electrons. Lastly, these results pave the way for high gradient silicon dielectric laser accelerators using commercial lasers and subfemtosecond electron beam experiments.

43 PARTICLE ACCELERATORS↗

First experimental demonstration of time-resolved X-ray measurements with next-generation fast-timing MCP-PMT

We report the first successful time-resolved X-ray measurements at the APS 10-ID-B beamline by coupling ultrafast scintillators with photodetectors. Multiple scintillator and sensor pairs (LYSO, plastic scintillator, dynode PMTs, MCP-PMT), as well as a standalone detector (diamond), were tested to demonstrate the time-resolved measurements using hard X-rays at energies of 20 keV and above. The experimental results show that a number of choices exist for time-resolved high-energy X-ray beam measurement. Notably, by gating the photocathode, the Argonne fabricated fast-timing microchannel plate photomultiplier and LYSO crystal pair achieved fast signal detection with a rise time of 6 ns and a decay time of 33 ns. Furthermore, these experiments pave the way towards ultrafast imaging technologies using hard X-rays for many applications.

36 MATERIALS SCIENCE↗

High energy electron diffraction instrument with tunable camera length

Ultrafast electron diffraction (UED) stands as a powerful technique for real-time observation of structural dynamics at the atomic level. In recent years, the use of MeV electrons from radio frequency guns has been widely adopted to take advantage of the relativistic suppression of the space charge effects that otherwise limit the temporal resolution of the technique. Nevertheless, there is not a clear choice for the optimal energy for a UED instrument. Scaling to beam energies higher than a few MeV does pose significant technical challenges, mainly related to the inherent increase in diffraction camera length associated with the smaller Bragg angles. In this study, we report a solution by using a compact post-sample magnetic optical system to magnify the diffraction pattern from a crystal Au sample illuminated by an 8.2 MeV electron beam. Our method employs, as one of the lenses of the optical system, a triplet of compact, high field gradients (>500 T/m), small-gap (3.5 mm) Halbach permanent magnet quadrupoles. Shifting the relative position of the quadrupoles, we demonstrate tuning the magnification by more than a factor of two, a 6× improvement in camera length, and reciprocal space resolution better than 0.1 Å –1 in agreement with beam transport simulations.

47 OTHER INSTRUMENTATION↗

Ultrafast laser triggered electron emission from ultrananocrystalline diamond pyramid tip cathode

Nitrogen-incorporated ultrananocrystalline diamond [(N)UNCD] pyramid tip cathode has been considered as a next-generation high peak current electron source for dielectric laser accelerators as well as other high peak current particle accelerator applications. In this work, we study non-linear photoemission from an (N)UNCD pyramid tip cathode using an ultrafast laser with the pulse length of 150 fs with the central wavelength of 800 nm in the peak intensity range of 10 9 –10 10 W/cm 2 . We demonstrated that as the incident laser intensity increases, the current emitted from the nano-tip first increases as a power function with an exponent of about 5 and then starts to roll over to an exponent of 3. This roll over is attributed to the Coulomb interaction between electrons emitted from the tip also known as the space charge. We also measured the photoemission electron energy spectra that show electrons with energies as high as ~10 eV. Based on the shape of the electron energy spectra, we conclude that the high-energy electrons are thermally emitted electrons due to ultrafast laser heating at the tip of the (N)UNCD pyramid tip cathode.

43 PARTICLE ACCELERATORS↗

Necessary Experimental Conditions for Single-Shot Diffraction Imaging of DNA-Based Structures with X-ray Free-Electron Lasers

It has been proposed that the radiation damage to biological particles and soft condensed matter can be overcome by ultrafast and ultraintense X-ray free-electron lasers (FELs) with short pulse durations. The successful demonstration of the “diffraction-before-destruction” concept has made single-shot diffraction imaging a promising tool to achieve high resolutions under the native states of samples. However, the resolution is still limited because of the low signal-to-noise ratio, especially for biological specimens such as cells, viruses, and macromolecular particles. Here, we present a demonstration single-shot diffraction imaging experiment of DNA-based structures at SPring-8 Angstrom Compact Free Electron Laser (SACLA), Japan. Through quantitative analysis of the reconstructed images, the scattering abilities of gold and DNA were demonstrated. Suggestions for extracting valid DNA signals from noisy diffraction patterns were also explained and outlined. To sketch out the necessary experimental conditions for the 3D imaging of DNA origami or DNA macromolecular particles, we carried out numerical simulations with practical detector noise and experimental geometry using the Linac Coherent Light Source (LCLS) at the SLAC National Accelerator Laboratory, USA. In conclusion, the simulated results demonstrate that it is possible to capture images of DNA-based structures at high resolutions with the technique development of current and next-generation X-ray FEL facilities.

59 BASIC BIOLOGICAL SCIENCES↗

Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution

Here, the development of many optical quantum technologies depends on the availability of solid-state single quantum emitters with near-perfect optical coherence. However, a standing issue that limits systematic improvement is the significant sample heterogeneity and lack of mechanistic understanding of microscopic energy flow at the single emitter level and ultrafast timescales. Here we develop solution-phase single-particle pump-probe spectroscopy with photon correlation detection that captures sample-averaged dynamics in single molecules and/or defect states with unprecedented clarity at femtosecond resolution. We apply this technique to single quantum emitters in two-dimensional hexagonal boron nitride, which suffers from significant heterogeneity and low quantum efficiency. From millisecond to nanosecond timescales, the translation diffusion, metastable-state-related bunching shoulders, rotational dynamics, and antibunching features are disentangled by their distinct photon-correlation timescales, which collectively quantify the normalized two-photon emission quantum yield. Leveraging its femtosecond resolution, spectral selectivity and ultralow noise (two orders of magnitude improvement over solid-state methods), we visualize electron-phonon coupling in the time domain at the single defect level, and discover the acceleration of polaronic formation driven by multi-electron excitation. Corroborated with results from a theoretical polaron model, we show how this translates to sample-averaged photon fidelity characterization of cascaded emission efficiency and optical decoherence time. Our work provides a framework for ultrafast spectroscopy in single emitters, molecules, or defects prone to photoluminescence intermittency and heterogeneity, opening new avenues of extreme-scale characterization and synthetic improvements for quantum information applications.

36 MATERIALS SCIENCE↗

Exploring the Connection between Coherent Acoustic Phonons and Bright-Field Contrast in Ultrafast Electron Microscopy

Intense ultrafast photoexcitation of archetypal semiconducting materials, such as Ge and GaAs, ends in the rapid generation of large charge-carrier densities that propagate outward from the high-fluence region at initially hypersonic velocities. This produces a number of interesting effects that become interwoven with the underlying lattice; including the development of acoustic-type propagating oscillatory modes, excitation of coherent propagating strain waves, and coalescence of phase behaviors of the acoustic phonons and charge carriers via wave-particle drag. Using bright-field imaging in an ultrafast electron microscope, we directly imaged the behavior of photoexcited, nanoscale coherent strain waves in single-crystal Ge. In addition to single preferential wavevectors and initially hypersonic phase velocities (up to 35 nm/ps), we were able to directly resolve single-phonon constant velocities and an overall time-varying phase-velocity dispersion to the bulk speed of sound over approximately one nanosecond. Comparison to dispersion behaviors expected for symmetric and asymmetric Lamb-type modes showed good agreement with experiments, suggesting the preferential excitation of a single, symmetric first-order mode. Yet, quantitative comparison to the expected and measured contrast strengths associated with the coherent dynamics is needed in order to further elucidate the precise microscopic mechanisms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Origin and Evolution of Organic Matter Preserved in Stardust Cometary Aerogel Tracks

The STARDUST spacecraft captured dust samples from Comet 81P/Wild 2 at a relative velocity of 6.1 km/s in a low density silica aerogel and returned them to the Earth. One of the main of the scientific goals established for the mission was to determine whether comets contained complex organic materials and, contingently, the nature and abundance of this material. [1] Although contamination concerns due to carbonaceous impurities intrinsic to the flight aerogel remain, it is generally accepted that at least a fraction of the captured dust particles contain an indigenous organic component. [2] However, understanding the nature and abundance of this material is complicated by nature of the collection process. The rapid dissipation of particle s kinetic energy during its impact and deceleration cause both the particle and surrounding aerogel to experience an intense thermal pulse of upwards of 2000K for a period up to several hundred nanoseconds [3]. During this period thermal alteration and or destruction of organic species present in the impacting particle are likely to occur. We have used the technique of ultrafast two-step laser mass spectrometry (ultra L2MS) [4] to investigate how the nature and distribution of aromatic and conjugated organic species varies between and within aerogel cometary tracks and their associated terminal particles.

McKay, D.S.↗

Observation of the axion quasiparticle in 2D MnBi 2 Te 4

The axion is a hypothetical fundamental particle that is conjectured to correspond to the coherent oscillation of the θ field in quantum chromodynamics. Its existence would solve multiple fundamental questions, including the strong CP problem of quantum chromodynamics and dark matter, but the axion has never been detected. Electrodynamics of condensed-matter systems can also give rise to a similar θ, so far studied as a static, quantized value to characterize the topology of materials. Coherent oscillation of θ in condensed matter has been proposed to lead to physics directly analogous to the high-energy axion particle—the dynamical axion quasiparticle (DAQ). Here we report the observation of the DAQ in MnBi 2 Te 4 . By combining a two-dimensional electronic device with ultrafast pump–probe optics, we observe a coherent oscillation of θ at about 44 gigahertz, which is uniquely induced by its out-of-phase antiferromagnetic magnon. This represents direct evidence for the presence of the DAQ, which in two-dimensional MnBi 2 Te 4 is found to arise from the magnon-induced coherent modulation of the Berry curvature. The DAQ also has implications in light–matter interaction and coherent antiferromagnetic spintronics, as it might lead to axion polaritons and electric control of ultrafast spin polarization. Finally, the DAQ could be used to detect axion particles. We estimate the detection frequency range and sensitivity in the millielectronvolt regime, which has so far been poorly explored.

topological matter↗

Multi-scale time-resolved electron diffraction: A case study in moiré materials

Ultrafast-optical-pump — structural-probe measurements, including ultrafast electron and x-ray scattering, provide direct experimental access to the fundamental timescales of atomic motion, and are thus foundational techniques for studying matter out of equilibrium. High-performance detectors are needed in scattering experiments to obtain maximum scientific value from every probe particle. Here we deploy a hybrid pixel array direct electron detector to perform ultrafast electron diffraction experiments on a WSe 2 /MoSe 2 2D heterobilayer, resolving the weak features of diffuse scattering and moiré superlattice structure without saturating the zero order peak. Enabled by the detector’s high frame rate, we show that a chopping technique provides diffraction difference images with signal-to-noise at the shot noise limit. Finally, we demonstrate that a fast detector frame rate coupled with a high repetition rate probe can provide continuous time resolution from femtoseconds to seconds, enabling us to perform a scanning ultrafast electron diffraction experiment that maps thermal transport in WSe 2 /MoSe 2 and resolves distinct diffusion mechanisms in space and time.

36 MATERIALS SCIENCE↗

Ultrafast radiographic imaging and tracking: An overview of instruments, methods, data, and applications

Ultrafast radiographic imaging and tracking (U-RadIT) use state-of-the-art ionizing particle and light sources to experimentally study sub-nanosecond transients or dynamic processes in physics, chemistry, biology, geology, materials science and other fields. These processes are fundamental to modern technologies and applications, such as nuclear fusion energy, advanced manufacturing, communication, and green transportation, which often involve one mole or more atoms and elementary particles, and thus are challenging to compute by using the first principles of quantum physics or other forward models. One of the central problems in U-RadIT is to optimize information yield through, e.g. high-luminosity X-ray and particle sources, efficient imaging and tracking detectors, novel methods to collect data, and large-bandwidth online and offline data processing, regulated by the underlying physics, statistics, and computing power. We review and highlight recent progress in: (a.) Detectors such as high-speed complementary metal-oxide semiconductor (CMOS) cameras, hybrid pixelated array detectors integrated with Timepix4 and other application-specific integrated circuits (ASICs), and digital photon detectors; (b.) U-RadIT modalities such as dynamic phase contrast imaging, dynamic diffractive imaging, and four-dimensional (4D) particle tracking; (c.) U-RadIT data and algorithms such as neural networks and machine learning, and (d.) Applications in ultrafast dynamic material science using XFELs, synchrotrons and laser-driven sources. Hardware-centric approaches to U-RadIT optimization are constrained by detector material properties, low signal-to-noise ratio, high cost and long development cycles of critical hardware components such as ASICs. Interpretation of experimental data, including comparisons with forward models, is frequently hindered by sparse measurements, model and measurement uncertainties, and noise. Alternatively, U-RadIT make increasing use of data science and machine learning algorithms, including experimental implementations of compressed sensing. Machine learning and artificial intelligence approaches, refined by physics and materials information, may also contribute significantly to data interpretation, uncertainty quantification and U-RadIT optimization.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Phase controlled synthesis of transition metal carbide nanocrystals by ultrafast flash Joule heating

Nanoscale carbides enhance ultra-strong ceramics and show activity as high-performance catalysts. Traditional lengthy carburization methods for carbide syntheses usually result in coked surface, large particle size, and uncontrolled phase. Here, a flash Joule heating process is developed for ultrafast synthesis of carbide nanocrystals within 1 s. Various interstitial transition metal carbides (TiC, ZrC, HfC, VC, NbC, TaC, Cr 2 C 3 , MoC, and W 2 C) and covalent carbides (B 4 C and SiC) are produced using low-cost precursors. By controlling pulse voltages, phase-pure molybdenum carbides including β-Mo 2 C and metastable α-MoC 1-x and η-MoC 1-x are selectively synthesized, demonstrating the excellent phase engineering ability of the flash Joule heating by broadly tunable energy input that can exceed 3000 K coupled with kinetically controlled ultrafast cooling (>10 4 K s –1 ). Theoretical calculation reveals carbon vacancies as the driving factor for topotactic transition of carbide phases. The phase-dependent hydrogen evolution capability of molybdenum carbides is investigated with β-Mo 2 C showing the best performance.

01 COAL, LIGNITE, AND PEAT↗

Quantum Interference in Two-Atom Resonant X-ray Scattering of an Intense Attosecond Pulse

We theoretically investigate resonant x-ray scattering from two noninteracting Ne+ ions driven by an intense attosecond pulse using a nonrelativistic, QED-based time-dependent framework. Our model includes Rabi oscillations, photoionization, Auger decay, and quantum interference among elastic scattering and resonance fluorescence pathways. We analyze how the total scattering signal depends on pulse intensity, atomic configuration, and initial electronic state. We find that the total resonant scattering yield exceeds its nonresonant counterpart; the angular dependence of the signal qualitatively resembles a two-atom structure factor; and the visibility of interference fringes is sensitive to pulse area and the initial electronic state. Only a subset of final states reached via resonance fluorescence exhibits interference, determined by the indistinguishability of photon emission pathways. Fringe visibility is maximized in the linear scattering regime, where ionization is minimal and resonance fluorescence pathways can be largely indistinguishable. These results highlight optimal conditions for applying ultrafast resonant x-ray scattering to single-particle imaging.

Venkatesh, Akilesh↗

Investigation of an Ultrafast Harmonic Resonant RF Kicker

An Energy Recovery Linac (ERL) based multi-turn electron Circulator Cooler Ring (CCR) is envisaged in the proposed Jefferson Lab Electron Ion Collider (JLEIC) to cool the ion bunches with high energy (55 MeV), high current (1.5 A), high repetition frequency (476.3 MHz), high quality magnetized electron bunches. A critical component in this scheme is a pair of ultrafast kickers for the exchange of electron bunches between the ERL and the CCR. The ultrafast kicker should operate with the rise and fall time in less than 2.1 ns, at the repetition rate of ~10s MHz, and should be able to run continuously during the whole period of cooling. These -and-fall time being combined together, are well beyond the state-of-art of traditional pulsed power supplies and magnet kickers. To solve this technical challenge, an alternative method is to generate this high repetition rate, fast rise-and-fall time short pulse continuous waveform by summing several finite number of (co)sine waves at harmonic frequencies of the kicking repetition frequency, and these harmonic modes can be generated by the Quarter Wave Resonater (QWR) based multifrequency cavities. Assuming the recirculator factor is 10, 10 harmonic modes (from 47.63 MHz to 476.3 MHz) with proper amplitudes and phases, plus a DC offset are combined together, a continuous short pulse waveform with the rise-and-fall time in less than 2.1 ns, repetition rate of 47.63 MHz waveform can be generated. With the compact and matured technology of QWR cavities, the total cost of both hardware development and operation can be reduced to a modest level. Focuse on the technical scheme, three main topics will be discussed in this thesis: the synthetization of the kicking pulse, the design and optimization of the deflecting QWR multi-integer harmonic frequency resonator and the fabrication and bench measurements of a half scale copper prototype. In the kicking pulse synthetization part, we begin with the Fourier Series expansion of an ideal square pulse, and get a Flat-Top waveform which will give a uniform kick over the bunch length of the kicked electron bunches, thus the transverse emittance of these kicked electron bunches can be maintained. By using two identical kickers with the betatron phase advance of 180 degree or its odd multiples, the residual kick voltage wave slopes at the unkicked bunch position will be totally cancelled out. Flat-Top waveform combined with two kicker scheme, the transverse emittance of the cooling electron bunches will be conserved during the whole injection, recirculation, and ejection processes. In the cavity design part, firstly, the cavity geometry is optimized to get high transverse shunt impedance thus less than 100 W of RF losses on the cavity wall can be achieved for all these 10 harmonic modes. To support all these 10 harmonic modes, group of four QWRs are adopted with the mode distribution of 5:3:1:1. In the multi-frequency cavities such as the five-mode-cavity and the three-mode-cavity, tunings are required to achieve the design frequencies for each mode. Slight segments of taper design on the inner conductor help to get the frequencies to be exactly on the odd harmonic modes. Stub tuners equal to the number of resonant modes are inserted to the outer conductor wall to compensate the frequency shifts due manufacturing errors and other perturbations during the operation such as the change of the cavity temperature. Single loop couple is designed for all harmonic modes in each cavity. By adjusting its loop size, position and rotation, it is possible to get the fundamental mode critical coupled and other higher harmonic modes slightly over coupled. A broadband circulator will be considered for absorbing the reflected power. Finally in this part, multipole field components due to the asymmetric cylindrical structure around the beam axis of the cavity as well as the beam-induced higher order mode (HOM) issues will be analyzed and discussed in this thesis. A half-scale copper prototype cavity (resonant frequencies from 95.26 MHz to 857.34 MHz) was fabricated to validate the electromagnetic characteristics. With this half scale prototype, the tuning processes of multiple harmonic frequencies, unloaded quality factor measurements of each mode, and bead-pull measurements are performed. The bench measurement results matched well with the simulation results, which have validated our cavity design and construction methods. Finally, a simple mode combining experiment with five separate signal generators was performed on this prototype cavity and the desired fast rise/fall time (1.2 ns), high repetition rate (95.26 MHz) waveform was captured, which finally proved our design of this ultrafast harmonic kicker.

43 PARTICLE ACCELERATORS↗

Revealing core-valence interactions in solution with femtosecond X-ray pump X-ray probe spectroscopy

Abstract Femtosecond pump-probe spectroscopy using ultrafast optical and infrared pulses has become an essential tool to discover and understand complex electronic and structural dynamics in solvated molecular, biological, and material systems. Here we report the experimental realization of an ultrafast two-color X-ray pump X-ray probe transient absorption experiment performed in solution. A 10 fs X-ray pump pulse creates a localized excitation by removing a 1 s electron from an Fe atom in solvated ferro- and ferricyanide complexes. Following the ensuing Auger–Meitner cascade, the second X-ray pulse probes the Fe 1 s → 3 p transitions in resultant novel core-excited electronic states. Careful comparison of the experimental spectra with theory, extracts +2 eV shifts in transition energies per valence hole, providing insight into correlated interactions of valence 3 d with 3 p and deeper-lying electrons. Such information is essential for accurate modeling and predictive synthesis of transition metal complexes relevant for applications ranging from catalysis to information storage technology. This study demonstrates the experimental realization of the scientific opportunities possible with the continued development of multicolor multi-pulse X-ray spectroscopy to study electronic correlations in complex condensed phase systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Technology to Establish a Factory for High QE Alkali Antimonide Photocathodes

Intense electron beams are key to a large number of scientific endeavors, including electron cooling of hadron beams, electron-positron colliders, secondary-particle beams such as photons and positrons, sub-picosecond ultrafast electron diffraction (UED), and new high gradient accelerators that use electron-driven plasmas. The last decade has seen a considerable interest in pursuit and realization of novel light sources such as Free Electron Lasers [1] and Energy Recovery Linacs [2] that promise to deliver unprecedented quality x-ray beams. Many applications for high-intensity electron beams have arisen in recent years in high-energy physics, nuclear physics and energy sciences, such as recent designs for an electron-hadron collider at CERN (LHeC) [3], and beam coolers for hadron beams at LHC and eRHIC [4,5]. Photoinjectors are used at the majority of high-brightness electron linacs today, due to their efficiency, timing structure flexibility and ability to produce high power, high brightness beams. The performance of light source machines is strongly related to the brightness of the electron beam used for generating the x-rays. The brightness of the electron beam itself is mainly limited by the physical processes by which electrons are generated. For laser based photoemission sources this limit is ultimately related to the properties of photocathodes [6]. Most facilities are required to expend significant manpower and money to achieve a workable, albeit often non-ideal, compromise photocathode solution. If entirely fabricated in-house, the photocathode growth process itself is laborious and not always reproducible: it involves the human element while requiring close adherence to recipes and extremely strict control of deposition parameters. Lack of growth reliability and as a consequence, slow adoption of viable photoemitter types, can be partly attributed to the absence of any centralized facility or commercial entity to routinely provide high peak current capable, low emittance, visible-light sensitive photocathodes to the myriad of source systems in use and under development. Successful adoption of photocathodes requires strict adherence to proper fabrication, operation, and maintenance methodologies, necessitating specialized knowledge and skills. Key issues include the choice of photoemitter material, development of a more streamlined growth process to minimize human operator uncertainties, accommodation of varying photoemitter substrate materials and geometries, efficient transport and insertion mechanisms preserving the photo-yield, and properly conveyed photoemitter operational and maintenance methodologies. AES, in collaboration with Cornell University in a Phase I STTR, developed an on-demand industrialized growth and centralized delivery system for high-brightness photocathodes focused upon the alkali antimonide photoemitters. To the end user, future photoemitter sourcing will become as simple as other readily available consumables, rather than a research project requiring large investments in time and personnel.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗