arXiv subjects

Jordan T. O'Neal

Publications and source records attributed to Jordan T. O'Neal.

4 recordsLinked to original sources

arXiv2026

Tomographic Phase Imaging with Randomized Probe Imaging

We demonstrate tomographic phase imaging of cubic gold nanoparticles with sub-100 nm resolution requiring just a single far-field coherent diffraction pattern per projection. By using randomized probe imaging (RPI), a real-space amplitude and phase image can be reconstructed from a single diffraction pattern. These phase images are then fed into a standard tomographic workflow to retrieve the 3D volume. Nanoscale X-ray phase tomography has often relied on ptychography, which requires slow 2D scanning for each projection. By using RPI, the data collection is greatly sped up at the cost of some resolution. We compare an RPI-tomography volume to a ptychography-tomography volume of the same sample, finding high consistency between the two methods. To the best of our knowledge, this is the first application of RPI to tomography.

physics.optics↗

arXiv2025

Fluorescence intensity correlations enable 3D imaging without sample rotations

Lensless X-ray imaging provides element-specific nanoscale insights into thick samples beyond the reach of conventional light and electron microscopy. Coherent diffraction imaging (CDI) methods, such as ptychographic tomography, can recover three-dimensional (3D) nanoscale structures but require extensive sample rotation, adding complexity to experiments. X-ray elastic-scattering patterns from a single sample orientation are highly directional and provide limited 3D information about the structure. In contrast to X-ray elastic scattering, X-ray fluorescence is emitted mostly isotropically. However, first-order spatial coherence has traditionally limited nanoscale fluorescence imaging to single-crystalline samples. Here, we demonstrate that intensity correlations of X-ray fluorescence excited by ultrashort X-ray pulses contain 3D structural information of non-periodic, stationary objects. In our experiment, we illuminated a vanadium foil within a sub-200 nm X-ray laser beam focus. Without changing the sample orientation, we recorded 16 distinct specimen projections using detector regions covering different photon incidence angles relative to the X-ray free-electron laser (FEL) beam. The projections varied systematically as the fluorescing volume was translated along an astigmatism, confirming that FEL-induced fluorescence reflects real-space structural changes. Our results establish a new approach for lensless 3D imaging of non-periodic specimens using fluorescence intensity correlations, with broad implications for materials science, chemistry, and nanotechnology.

physics.optics↗

arXiv2024

Attosecond Delays in X-ray Molecular Ionization

The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. Accordingly, the past decade has produced a large volume of work on photoionization delays following single photon absorption of an extreme ultraviolet (XUV) photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required x-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. We have now measured the x-ray photoemission delay of core-level electrons, and here report unexpectedly large delays, ranging up to 700 attoseconds in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft x-ray pulses from a free-electron laser (XFEL) to scan across the entire region near the K-shell threshold. Furthermore, we find the delay spectrum is richly modulated, suggesting several contributions including transient trapping of the photoelectron due to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule, and multi-electron scattering effects. The results demonstrate how x-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.

physics.atom-ph↗

arXiv2021

Attosecond Coherent Electron Motion in Auger-Meitner Decay

In quantum systems, coherent superpositions of electronic states evolve on ultrafast timescales (few femtosecond to attosecond, 1 as = 0.001 fs = 10^{-18} s), leading to a time dependent charge density. Here we exploit the first attosecond soft x-ray pulses produced by an x-ray free-electron laser to induce a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized infrared laser pulse we create a clock to time-resolve the electron dynamics, and demonstrate control of the coherent electron motion by tuning the photon energy of the x-ray pulse. Core-excited states offer a fundamental test bed for studying coherent electron dynamics in highly excited and strongly correlated matter.

physics.chem-ph↗