Large Aperture Orientation-Patterned Gallium Arsenide for High Power Frequency Conversion
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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High-Pulse Energy / High-Repetition Rate Laser
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43 PARTICLE ACCELERATORS↗
Extended X-ray absorption spectroscopy using an ultrashort pulse laboratory-scale laser-plasma accelerator
Laser-driven compact particle accelerators can provide ultrashort pulses of broadband X-rays, well suited for undertaking X-ray absorption spectroscopy measurements on a femtosecond timescale. Here the Extended X-ray Absorption Fine Structure (EXAFS) features of the K-edge of a copper sample have been observed over a 250 eV window in a single shot using a laser wakefield accelerator, providing information on both the electronic and ionic structure simultaneously. This capability will allow the investigation of ultrafast processes, and in particular, probing high-energy-density matter and physics far-from-equilibrium where the sample refresh rate is slow and shot number is limited. For example, states that replicate the tremendous pressures and temperatures of planetary bodies or the conditions inside nuclear fusion reactions. Using high-power lasers to pump these samples also has the advantage of being inherently synchronised to the laser-driven X-ray probe. A perspective on the additional strengths of a laboratory-based ultrafast X-ray absorption source is presented.
43 PARTICLE ACCELERATORS↗
Real-time observation of multi-electron processes in atoms and diatomic molecules
We report on the implementation of a reliable experimental approach to observe, in real-time, electron dynamics in atoms and molecules at the attosecond time scale. The experimental approach combines a source of shape-controlled attosecond pulses, a stabilized XUV/IR interferometer for time-resolved measurements, and a multi-particle imaging system (Coltrims). In addition, we report new capabilities to control electron dynamics in quantum systems.
74 ATOMIC AND MOLECULAR PHYSICS↗
Probing Plasmonic Near-Fields in Oxide-Modified Aluminum Nanocubes Using Photon-Induced Near-Field Electron Microscopy
Plasmonic nanoparticles generate strong electric fields near their surface upon photoexcitation, enabling applications in sensing, spectroscopy, and photocatalysis. Electron microscopy techniques – such as cathodoluminescence and electron energy loss spectroscopy – have been leveraged to produce nanoscale maps of localized surface plasmon (LSP) modes. More recently, photon-induced near-field electron microscopy (PINEM) has emerged as a powerful technique for imaging evanescent near-fields generated by ultrafast laser excitation. In this work, we employ PINEM within an ultrafast electron microscope, complemented by numerical calculations to investigate how optical polarization, surface modification, and light intensity affect the evanescent fields associated with LSPs on oxide-modified aluminum nanocubes. Polarization control of the incident light field enables spatial mapping of the nanocube’s LSPs at the single particle level. Systematic variation of the oxide layer thickness reveals that increased coating thickness correlates with a stronger PINEM signal and a greater energy gain of probing electrons. Additionally, higher light intensities at fixed polarization and oxide coating further amplify the PINEM signal. These findings demonstrate the utility of PINEM as a high-resolution technique for optical near-field imaging and spectroscopy of single plasmonic nanoparticles. The ability to probe single particle behavior offers new opportunities for advancing the design and characterization of nanophotonic and plasmonic materials.
PINEM↗
A composite electrodynamic mechanism to reconcile spatiotemporally resolved exciton transport in quantum dot superlattices
Quantum dot (QD) solids are promising optoelectronic materials; further advancing their device functionality requires understanding their energy transport mechanisms. The commonly invoked near-field Förster resonance energy transfer (FRET) theory often underestimates the exciton hopping rate in QD solids, yet no consensus exists on the underlying cause. In response, we use time-resolved ultrafast stimulated emission depletion (STED) microscopy, an ultrafast transformation of STED to spatiotemporally resolve exciton diffusion in tellurium-doped cadmium selenide–core/cadmium sulfide–shell QD superlattices. We measure the concomitant time-resolved exciton energy decay due to excitons sampling a heterogeneous energetic landscape within the superlattice. The heterogeneity is quantified by single-particle emission spectroscopy. This powerful multimodal set of observables provides sufficient constraints on a kinetic Monte Carlo simulation of exciton transport to elucidate a composite transport mechanism that includes both near-field FRET and previously neglected far-field emission/reabsorption contributions. Uncovering this mechanism offers a much-needed unified framework in which to characterize transport in QD solids and additional principles for device design.
36 MATERIALS SCIENCE↗
Relativistic Modeling of Ultra-Short Electron Pulse Propagation
The ultrafast electron microscopy, electron diffraction, electron crystallography, and nanocrystallography methods opened the possibility of studying the coherent structural dynamics of matter. The time resolution of the ultrafast electron microscopy and electron diffraction methods determined by the duration of electron pulses is the key parameter of experimental setups. This paper treats electron pulse dynamics in the field free drift region specifically for applications in atomic imaging. The electron beam is modeled as a system of particles (N) with N = 1000 and N = 10 000 electrons. The beam propagates for a certain period of time (1–4 ns); during its propagation, electron distribution parameters (over coordinates and velocities) are calculated to characterize the temporal profile and uncertainty in the electron wavelength at the sample. The results of applying relativistic dynamic equations show that nonrelativistic results are satisfactorily applicable (with 15 per cent or better accuracy) for modeling short electron pulse elongation and broadening at 30 keV and lower energies. However, the results of such modeling may be significantly in error for intermediate energies (300 keV), and for the fast relativistic beams (3 MeV) they become completely wrong. The relative reduction in Coulomb repulsion effects at higher energies is known, however; we give a comprehensive treatment that allows a quantitative picture. Using high-energy electron pulses results in almost complete elimination of the repulsive Coulomb effect. Dispersion of electron velocities becomes much lower at higher energies. For 3 MeV electrons, electron pulse duration as well as its radius does not noticeably change even after traveling for 4 ns (1.2 m). Even at 300 keV, the pulse duration increase is negligible until 1 ns (0.2 m). A simple mean-field model suggested in [13] has been extended to arbitrarily fast relativistic electron pulses with good correspondence to direct dynamic modeling.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
The emergence of macroscopic currents in photoconductive sampling of optical fields
Photoconductive field sampling enables petahertz-domain optoelectronic applications that advance our understanding of light-matter interaction. Despite the growing importance of ultrafast photoconductive measurements, a rigorous model for connecting the microscopic electron dynamics to the macroscopic external signal is lacking. This has caused conflicting interpretations about the origin of macroscopic currents. Here, we present systematic experimental studies on the signal formation in gas-phase photoconductive sampling. Our theoretical model, based on the Ramo–Shockley-theorem, overcomes the previously introduced artificial separation into dipole and current contributions. Extensive numerical particle-in-cell-type simulations permit a quantitative comparison with experimental results and help to identify the roles of electron-neutral scattering and mean-field charge interactions. The results show that the heuristic models utilized so far are valid only in a limited range and are affected by macroscopic effects. Our approach can aid in the design of more sensitive and more efficient photoconductive devices.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
A benchtop shock physics laboratory: Ultrafast laser driven shock spectroscopy and interferometry methods
Common Ti:sapphire chirped pulse amplified laser systems can be readily adapted to be both a generator of adjustable pressure shock waves and a source for multiple probes of the ensuing ultrafast shock dynamics. Here, we detail experimental considerations for optimizing the shock generation, interferometric characterization, and spectroscopic probing of shock dynamics with visible and mid-infrared transient absorption. While we have reported results using these techniques elsewhere, in this work we detail how the spectroscopies are integrated with the shock and interferometry experiment. The interferometric characterization uses information from beams at multiple polarizations and angles of incidence combined with thin film equations and shock dynamics to determine the shock velocity, particle velocity, and shocked refractive index. Visible transient absorption spectroscopy uses a white light supercontinuum in a reflection geometry, synchronized to the shock wave, to time resolve shock-induced changes in visible absorption such as changes to electronic structure or strongly absorbing products and intermediates due to reaction. Mid-infrared transient absorption spectroscopy uses two color filamentation supercontinuum generation combined with a simple thermal imaging microbolometer spectrometer to enable broadband single shot detection of changes in the vibrational spectra. These methods are reflected here in the study of shock dynamics at stresses from 5 to 30 GPa in organic materials and from a few GPa to >70 GPa in metals with spatial resolution of a few micrometers and temporal resolution of a few picoseconds. This experiment would be possible to replicate in any ultrafast laser laboratory containing a single bench top commercial chirped pulse amplification laser system.
47 OTHER INSTRUMENTATION↗
Ionization-Induced Subcycle Metallization of Nanoparticles in Few-Cycle Pulses
Strong-field laser-matter interactions in nanoscale targets offer unique avenues for the generation and detailed characterization of matter under extreme conditions. Field-driven, sub-cycle ionization-induced metallization of nanoscale solids in intense laser fields has been predicted (Peltz et al. Time-Resolved X-ray Imaging of Anisotropic Nano-plasma Expansion. Phys. Rev. Lett. 2014, 113, 133401), but its observation was hampered by a lack of a smoking gun. Here, we report the ultrafast metallization of isolated dielectric and semiconducting nanoparticles under intense few-cycle laser pulses. The highest-energy electron emission is found to be a decisive proof that shows a characteristic cutoff modification to a metallic limit for intensities high enough to ignite carrier avalanching in the volume of the particles. Furthermore, semiclassical Mean-field Mie Monte-Carlo transport simulations reveal the underlying dynamics and explain the observed evolution by near-field driven electron backscattering from the metallizing target.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Physically and chemically smooth cesium-antimonide photocathodes on single crystal strontium titanate substrates
The performance of x-ray free electron lasers and ultrafast electron diffraction experiments is largely dependent on the brightness of electron sources from photoinjectors. Here, the maximum brightness from photoinjectors at a particular accelerating gradient is limited by the mean transverse energy (MTE) of electrons emitted from photocathodes. For high quantum efficiency (QE) cathodes like alkali-antimonide thin films, which are essential to mitigate the effects of non-linear photoemission on MTE, the smallest possible MTE and, hence, the highest possible brightness are limited by the nanoscale surface roughness and chemical inhomogeneity. In this work, we show that high QE Cs 3 Sb films grown on lattice-matched strontium titanate (STO) substrates have a factor of 4 smoother, chemically uniform surfaces compared to those traditionally grown on disordered Si surfaces. We perform simulations to calculate roughness induced MTE based on measured topographical and surface-potential variations on the Cs 3 Sb films grown on STO and show that these variations are small enough to have no consequential impact on the MTE and, hence, the brightness.
43 PARTICLE ACCELERATORS↗
Aggregation of solutes in bosonic versus fermionic quantum fluids
Quantum fluid droplets made of helium-3 ( 3 He) or helium-4 ( 4 He) isotopes have long been considered as ideal cryogenic nanolabs, enabling unique ultracold chemistry and spectroscopy applications. The droplets were believed to provide a homogeneous environment in which dopant atoms and molecules could move and react almost as in free space but at temperatures close to absolute zero. Here, we report ultrafast x-ray diffraction experiments on xenon-doped 3 He and 4 He nanodroplets, demonstrating that the unavoidable rotational excitation of isolated droplets leads to highly anisotropic and inhomogeneous interactions between the host matrix and enclosed dopants. Superfluid 4 He droplets are laced with quantum vortices that trap the embedded particles, leading to the formation of filament-shaped clusters. In comparison, dopants in 3 He droplets gather in diffuse, ring-shaped structures along the equator. The shapes of droplets carrying filaments or rings are direct evidence that rotational excitation is the root cause for the inhomogeneous dopant distributions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Observation of photo-induced plasmon–phonon coupling in PbTe via ultrafast x-ray scattering
We report the observation of photo-induced plasmon–phonon coupled modes in the group IV–VI semiconductor PbTe using ultrafast x-ray diffuse scattering at the Linac Coherent Light Source. We measure the near-zone-center excited-state dispersion of the heavily screened longitudinal optical (LO) phonon branch as extracted from differential changes in x-ray diffuse scattering intensity following above bandgap photoexcitation. We suggest that upon photoexcitation, the LO phonon-plasmon coupled (LOPC) modes themselves become coupled to longitudinal acoustic modes that drive electron band shifts via acoustic deformation potentials and possibly to low-energy single-particle excitations within the plasma and that these couplings give rise to displacement-correlations that oscillate in time with a period given effectively by the heavily screened LOPC frequency.
36 MATERIALS SCIENCE↗
Nonuniform Flow Dynamics Probed by Nanosecond X-Ray Speckle Visibility Spectroscopy
We report observations of nanosecond nonuniform colloidal dynamics in a free flowing liquid jet using ultrafast x-ray speckle visibility spectroscopy. Utilizing a nanosecond double-bunch mode, the Linac Coherent Light Source free electron laser produced pairs of femtosecond coherent hard x-ray pulses. By exploring anisotropy in the visibility of summed speckle patterns which relates to the correlation functions, we evaluate not only the average particle flow rate in a colloidal nanoparticle jet, but also the nonuniform flow field within. The methodology presented here establishes the foundation for the study of nano- and atomic-scale inhomogeneous fluctuations in complex matter using x-ray free electron laser sources.
47 OTHER INSTRUMENTATION↗
Coordinated Analyses of Diverse Components in Whole Stardust Cometary Tracks
Analyses of samples returned from Comet 81P/Wild-2 by the Stardust spacecraft have resulted in a number of surprising findings that show the origins of comets are more complex than previously suspected. However, these samples pose new experimental challenges because they are diverse and suffered fragmentation, thermal alteration, and fine scale mixing with aerogel. Questions remain about the nature of Wild-2 materials, such as the abundances of organic matter, crystalline materials, and presolar grains. To overcome these challenges, we have developed new sample preparation and analytical techniques tailored for entire aerogel tracks. We have successfully ultramicrotomed entire "carrot" and "bulbous" type tracks along their axis while preserving their original shapes. This innovation allowed us to examine the distribution of fragments along the track from the entrance hole all the way to the terminal particle (TP). We will present results of our coordinated analysis of the "carrot" type aerogel tracks #112 and #148, and the "bulbous" type aerogel tracks #113, #147 and #168 from the nanometer to the millimeter scale. Scanning TEM (STEM) was used for elemental and detailed mineralogy characterization, NanoSIMS was used for isotopic analyses, and ultrafast two-step laser mass spectrometry (ultra L2MS) was used to investigate the nature and distribution of organic phases. The isotopic measurements were performed following detailed TEM characterization for coordinated mineralogy. This approach also enabled spatially resolving the target sample from fine-scale mixtures of compressed aerogel and melt. Eight of the TPs of track #113 are dominated by coarse-grained enstatite (En90) that is largely orthoenstatite with minor, isolated clinoenstatite lamellae. One TP contains minor forsterite (Fo88) and small inclusions of diopside with % levels of Al, Cr and Fe. Two of the TPs contain angular regions of fine-grained nepheline surrounded by enstatite. Their O isotopic compositions are in the range of meteoritic materials, implying that they originated in the inner Solar System. Complex aromatic hydrocarbons are distributed along aerogel tracks and in TPs. These organics are likely cometary but were affected by shock heating. Three TPs of track #147 and two of track 168 have completely different mineralogy. TP2 of track #147 entirely consists of Fe-Ni alloy (5 at% Ni) and TP3 contains Fa28 with partial olivine-pyroxene intergrowth and minor albite. TP4 contains pentlandite, Fe-olivine, albite and high Ca pyroxene with Na and Cr (kosmochlor component). TP1 of #168 contains Fe-olivine, albite and pentlandite, and the concentric TP2 has a core of olivine grains with co-existing indigenous amorphous SiO2 surrounded by a carbon mantle, which in turn is surrounded by a layer of compressed aerogel. The TP of the carrot track #112 is a (16)O-rich forsteritic olivine grain that likely formed in the inner Solar System. The track also contains submicron-sized diamond grains of likely Solar System origin.
Nakamura-Messenger, Keiko↗
Visualization and quantum control of light-accelerated condensates by terahertz multi-dimensional coherent spectroscopy
Abstract Characterizing and controlling high-order correlation of quantum systems is key for developing quantum devices and switching technologies. Although conventional static and ultrafast spectroscopy gives access to collective excitations characterizing quantum states, more exotic correlations cannot be easily separated from other contributions. Here we develop density matrix simulations to show that seventh-order-wave-mixing peaks with distinct temperature and field dependences in two-dimensional terahertz nonlinear spectra reveal light-induced correlations in non-equilibrium superconducting states. Above critical terahertz driving, these emerging peaks split from conventional peaks along the second axis introduced by pump-probe relative phase in two-dimensional frequency space. They are photo-generated by correlations between two-photon fluctuations and interacting quasi-particle and quasi-particle/Higgs superconductor excitations. By photo-inducing persistent symmetry breaking via light-wave propagation, we also demonstrate seventh-order-wave-mixing sensing of Higgs collective modes. Our theory suggests to use multi-dimensional spectroscopy for quantum sensing of light-driven superconductivity and paves a path for quantum operations by few-cycle-THz-periodic photocurrent modulation.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Electron Mobility and Trapping in Ferrihydrite Nanoparticles
Iron is the most abundant transition metal in the Earth's crust, and naturally occurring iron oxide minerals play a commanding role in environmental redox reactions. Although iron oxide redox reactions are well studied, their precise mechanisms are not fully understood. Recent work has shown that these involve electron transfer pathways within the solid, suggesting that overall reaction rates could be dependent on electron mobility. Initial ultrafast spectroscopy studies of iron oxide nanoparticles sensitized by fluorescein derivatives supported a model for electron mobility based on polaronic hopping of electron charge carriers between iron sites, but the constitutive relationships between hopping mobilities and interfacial charge transfer processes has remained obscured. We developed a coarse-grained lattice Monte Carlo model to simulate the collective mobilities and lifetimes of these photoinjected electrons with respect to recombination with adsorbed dye molecules for the essential nanophase ferrihydrite, and tested predictions made by the simulations using pump-probe spectroscopy. We acquired optical transient absorption spectra as a function of particle size and under a variety of solution conditions, and used cryogenic transmission electron microscopy to determine the aggregation state of the nanoparticles. We observed biphasic electron recombination kinetics over timescales that spanned picoseconds to microseconds, the slower regime of which was fit with a stretched exponential decay function. The recombination rates were weakly affected by nanoparticle size and aggregation state, suspension pH, and the injection of multiple electrons per nanoparticle. We conclude that electron mobility indeed limits the rate of interfacial electron transfer in these systems with the slowest processes relating to escape from deep traps, the presence of which outweighs the influence of environmental factors such as pH-dependent surface charge.
77 NANOSCIENCE AND NANOTECHNOLOGY↗