arXiv subjects

Razib Obaid

Publications and source records attributed to Razib Obaid.

At least 19 recordsLinked to original sources

arXiv2026

Mutually phase-stable tunable attosecond soft X-ray attosecond pulses from a free-electron laser

We demonstrate the production of mutually phase-stable attosecond X-ray pulse pairs with tunable relative time delays and phases in a cascaded X-ray free-electron laser. We showcase the method in an experiment at the LCLS-II, in which a shaped electron beam is used in a split undulator configuration to generate the two attosecond pulses. We achieve mutual phase stability by reusing microbunching generated in the first undulator in order to seed the FEL process in the second at a detuned frequency. We measure controllable temporal delays between the two pulses directly in the time domain using angular streaking of photoelectrons, with a step size of 250 attoseconds. We then show that the behavior of the X-ray spectrum is consistent with phase stability between the two pulses, with a relative phase that can be easily tuned using inter-undulator phase shifters. This method is particularly well-suited to few to ten eV energy separations and sub to few femtosecond time delays, which are ideal for experiments in the soft X-ray regime for pushing the limits of our models for molecular dynamics and exerting direct coherent control over quantum systems.

physics.acc-ph↗

arXiv2026

X-ray Driven Trihydrogen Formation on Silica Nanosurfaces

The trihydrogen cation ($\mathrm{H_3^+}$) initiates the ion-molecule reactions that build molecular complexity in interstellar space. Whether its canonical formation reaction, $\mathrm{H_2^+ + H_2 \rightarrow H_3^+ + H}$, proceeds on inorganic surfaces under radiation-driven ionization has remained untested. Here we drive $\mathrm{H_3^+}$ formation on hydrated silica nanoparticles using intense 1.88 keV X-ray pulses, combining ion velocity map imaging, electron time-of-flight spectroscopy, and single-particle coherent diffractive imaging to resolve this chemistry on individual particles. The self-induced surface electric field on the V/nm scale drives interfacial charge transfer and water fragmentation. This field is the dominant parameter governing the relative yields of $\mathrm{H^+}$, $\mathrm{H_2^+}$, and $\mathrm{H_3^+}$ across particle size, composition, and aggregation. Density functional theory and nonadiabatic quantum molecular dynamics simulations trace this field-driven charge transfer, directly analogous to band bending at semiconductor photoelectrodes. These results establish surface-field-driven charge transfer as a unifying mechanism between radiation dominated astrophysical environments and field-driven surface catalysis.

physics.chem-ph↗

arXiv2026

Elucidating Norrish Type-I reactive pathways by ultrafast X-ray absorption spectroscopy

Norrish type I reactions selectively cleave carbon-carbon bonds directly adjacent to carbonyl groups. Despite their broad use in combination with aromatic carbonyls for additive manufacturing and dental UV curing applications, the nature of the photochemically active state and its population mechanism remain insufficiently understood. Detailed mechanistic insight requires mapping of the photoexcited population flow involving internal conversion and intersystem crossing. We present a time-domain study of gas phase acetophenone as a prototypical aromatic carbonyl combining soft X-ray time-resolved near-edge X-ray absorption fine structure (TR-NEXAFS) spectroscopy at the oxygen K-edge with ab initio multiple spawning (AIMS) simulations. Exploiting the specific sensitivity of TR-NEXAFS spectroscopy to states with $n\pi^*$ character, we observe population transfer from the initially excited $^1\pi\pi^*$ state to the $^1n\pi^*$ state with a time constant of $(0.13 \pm 0.02)$ ps after an initial induction period of $(0.12 \pm 0.02)$ ps without population transfer, in quantitative agreement with the AIMS simulations. The population in the $^1n\pi^*$ state subsequently decays via intersystem crossing, likely mediated by a $^3\pi\pi^*$ state, within $(3.17 \pm 0.66)$ ps to a long-lived $^3n\pi^*$ state, which is presumed to be active towards Norrish type I chemistry.

physics.chem-ph↗

arXiv2026

Advanced Control of Electron Beams: Tailoring X-ray Production with Programmable Laser Shaping

Leveraging the full scientific capabilities of next-generation high-repetition-rate free-electron lasers requires programmable control over electron-beam properties at their source. The photoinjector drive laser defines the electron beam's initial six-dimensional phase-space distribution, yet has historically been limited to Gaussian or static flat-top profiles, with most manipulation occurring downstream. Here we demonstrate software-programmable ultraviolet pulse shaping at the LCLS-II photoinjector as a source-level actuator that complements traditional accelerator controls. Using a coupled architecture combining dispersion-controlled nonlinear frequency conversion with spatial-light-modulator spectral shaping, we generate user-defined temporal structures and observe their imprint on electron bunches through high-resolution time-domain diagnostics. Laser-imposed multi-peaked modulation persists through acceleration, magnetic compression, and undulator transport with shot-to-shot repeatability, producing clearly resolved current structure in the compressed beam. Variance-based reconstruction from transverse deflecting cavity measurements reveals structured X-ray emission profiles exhibiting temporal features consistent with the programmed laser waveform. By providing rapid, software-controlled reconfiguration of electron-beam initial conditions, this source-level control approach establishes a programmable upstream actuator for future adaptive optimization and autonomous facility operation at high-repetition-rate light sources.

physics.acc-ph↗

arXiv2026

Upstream Laser-based Longitudinal Enhancement of Relativistic Photoelectrons

Controlling the longitudinal phase space of high-brightness relativistic electron beams is crucial for advancing a broad spectrum of charged-particle-based instrumentation and scientific frontiers. A generalized method for achieving this control involves manipulating the photoemission laser's temporal distribution at the picosecond level, a long-standing technical challenge. Recent developments in laser shaping have enabled the creation of high-power, picosecond-scale symmetrical and asymmetrical temporal profiles, capable of fine-tuning complex space-charge dynamics and external field effects in relativistic charged-particle beams. Here, we demonstrate that rather than deviations from theorized, idealized laser distributions, a controlled asymmetry can be harnessed to counteract accelerator-induced distortions. By implementing spatiotemporal shaping of the ultraviolet photocathode laser at the LCLS-II superconducting injector, we achieve deterministic control over the longitudinal phase space without downstream corrections. We find that this optical asymmetry induces a self-linearizing effect across both low (40 pC) and high (80 pC) charge regimes, effectively suppressing nonlinear compression and energy chirp. Consequently, this approach is expected to preserve a low emittance comparable to that of ideal flattop or regular Gaussian profiles, while delivering superior current uniformity and shot-to-shot stability. These results establish spatiotemporal laser shaping as a compact, generalizable tool for directly optimizing beam brightness at the source.

physics.optics↗

arXiv2025

Nonlinear reversal of photo-excitation on the attosecond time scale improves ultrafast x-ray diffraction images

The advent of isolated and intense sub-femtosecond X-ray pulses enables tracking of quantummechanical motion of electrons in molecules and solids. The combination of X-ray spectroscopy and diffraction imaging is a powerful approach to visualize non-equilibrium dynamics in systems beyond few atoms. However, extreme x-ray intensities introduce significant electronic damage, limiting material contrast and spatial resolution. Here we show that newly available intense subfemtosecond (sub-fs) x-ray FEL pulses can outrun most ionization cascades and partially reverse x-ray damage through stimulated x-ray emission in the vicinity of a resonance. In our experiment, we compared thousands of coherent x-ray diffraction patterns and simultaneously recorded ion spectra from individual Ne nanoparticles injected into the FEL focus. Our experimental results and theoretical modeling reveal that x-ray diffraction increases and the average charge state decreases in particles exposed to sub-fs pulses compared to those illuminated with 15-femtosecond pulses. Sub-fs exposures outrun most Auger decays and impact ionization processes, and enhance nonlinear effects such as stimulated emission, which cycle bound electrons between different states. These findings demonstrate that intense sub-fs x-ray FEL pulses are transformative for advancing high-resolution imaging and spectroscopy in chemical and material sciences, and open the possibilities of coherent control of the interaction between x-rays and complex specimen beyond few atoms.

physics.optics↗

arXiv2025

A Hybrid Neural Architecture: Online Attosecond X-ray Characterization

The emergence of high-repetition-rate x-ray free-electron lasers, such as SLAC's LCLS-II, serve as our canonical example for autonomous controls that necessitate high-throughput diagnostics paired with streaming computational pipelines capable of single-shot analysis with extremely low latency. We present the Deterministic Characterization with an Integrated Parallelizable Hybrid Resolver architecture, a hybrid machine learning framework designed for fast, accurate analysis of XFEL diagnostics using angular streaking-based sinogram images. This architecture integrates convolutional neural networks and bidirectional long short-term memory models to denoise input, identify x-ray sub-spike features, and extract sub-spike relative delays with sub-30 attosecond temporal resolution. Deployed on low-latency hardware, it achieves over 10~kHz throughput with \SI{168.3}{\micro\second} inference latency, indicating scalability to 14~kHz with FPGA integration. By transforming regression tasks into classification problems and leveraging optimized error encoding, we achieve high precision with low-latency performance that is critical for real-time streaming event selection and experimental control feedback signals. This represents a key development in real-time control pipelines for next-generation autonomous science, generally, and high repetition-rate x-ray experiments in particular.

physics.app-ph↗

arXiv2024

Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule

In molecular systems, the ultrafast motion of electrons initiates the process of chemical change. Tracking this electronic motion across molecules requires coupling attosecond time resolution to atomic-scale spatial sensitivity. In this work, we employ a pair of attosecond x-ray pulses from an x-ray free-electron laser to follow electron motion resulting from the sudden removal of an electron from a prototypical aromatic system, para-aminophenol. X-ray absorption enables tracking this motion with atomic-site specificity. Our measurements are compared with state-of-the-art computational modeling, reproducing the observed response across multiple timescales. Sub-femtosecond dynamics are assigned to states undergoing non-radiative decay, while few-femtosecond oscillatory motion is associated with electronic wavepacket motion in stable cation states, that will eventually couple to nuclear motion. Our work provides insight on the ultrafast charge motion preceding and initiating chemical transformations in moderately complex systems, and provides a powerful benchmark for computational models of ultrafast charge motion in matter.

physics.chem-ph↗

arXiv2024

Design and Performance of a Magnetic Bottle Electron Spectrometer for High-Energy Photoelectron Spectroscopy

We describe the design and performance of a magnetic bottle electron spectrometer~(MBES) for high-energy electron spectroscopy. Our design features a ${\sim2}$~m long electron drift tube and electrostatic retardation lens, achieving sub-electronvolt (eV) electron kinetic energy resolution for high energy (several hundred eV) electrons with close to 4$\pi$ collection efficiency. A segmented anode electron detector enables the simultaneous collection of photoelectron spectra in high resolution and high collection efficiency modes. This versatile instrument is installed at the TMO endstation at the LCLS x-ray free-electron laser (XFEL). In this paper, we demonstrate its high resolution, collection efficiency and spatial selectivity in measurements where it is coupled to an XFEL source. These combined characteristics are designed to enable high-resolution time-resolved measurements using x-ray photoelectron, absorption, and Auger-Meitner spectroscopy. We also describe the pervasive artifact in MBES time-of-flight spectra that arises from a periodic modulation in electron detection efficiency, and present a robust analysis procedure for its removal.

physics.ins-det↗

arXiv2024

"Beam `a la carte": laser heater shaping for attosecond pulses in a multiplexed x-ray free-electron laser

Electron beam shaping allows the control of the temporal properties of x-ray free-electron laser pulses from femtosecond to attosecond timescales. Here we demonstrate the use of a laser heater to shape electron bunches and enable the generation of attosecond x-ray pulses. We demonstrate that this method can be applied in a selective way, shaping a targeted subset of bunches while leaving the remaining bunches unchanged. This experiment enables the delivery of shaped x-ray pulses to multiple undulator beamlines, with pulse properties tailored to specialized scientific applications.

physics.acc-ph↗

arXiv2024

Spectrotemporal shaping of attosecond x-ray pulses with a fresh-slice free-electron laser

We propose a scheme allowing coherent shaping, i.e., controlling both the amplitude and phase, of attosecond x-ray pulses at free-electron lasers. We show that by seeding an FEL with a short coherent seed that overfills the amplification bandwidth, one can shape the Wigner function of the pulse by controlling the undulator taper profile. The examples of controllable pulse pairs and trains, as well as isolated spectrotemporally shaped pulses with very broad bandwidths are examined in detail. Existing attosecond XFELs can achieve these experimental conditions in a two-stage cascade, in which the seed is generated by a short current spike in an electron bunch and shaped in an unspoiled region within the same bunch. We experimentally demonstrate the production and control of phase-stable pulse trains using this method at the Linac Coherent Light Source II.

physics.acc-ph↗

arXiv2024

Attosecond X-ray Core-level Chronoscopy of Aromatic Molecules

Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, spectral congestion and spatial delocalization of valence electron wave functions set fundamental limits to the complexity of systems that can be studied and the information that can be retrieved, respectively. Using attosecond X-ray pulses from LCLS, we demonstrate the key advantages of measuring core-level delays: the photoelectron spectra remain atom-like, the measurements become element specific and the observed scattering dynamics originate from a point-like source. We exploit these unique features to reveal the effects of electronegativity and symmetry on attosecond scattering dynamics by measuring and calculating the photoionization delays between N-1s and C-1s core shells of a series of aromatic azabenzene molecules. Remarkably, the delays increase with the number of nitrogen atoms in the molecule and reveal multiple resonances. We identify two previously unknown mechanisms regulating the associated attosecond dynamics, namely the enhanced confinement of the trapped wavefunction with increasing electronegativity of the atoms and the decrease of the coupling strength among the photoemitted partial waves with increasing symmetry. This study demonstrates the unique opportunities opened by measurements of core-level photoionization delays for unraveling attosecond electron dynamics in complex matter.

physics.chem-ph↗

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↗

arXiv2024

Experimental Demonstration of Attosecond Pump-Probe Spectroscopy with an X-ray Free-Electron Laser

Pump-probe experiments with sub-femtosecond resolution are the key to understanding electronic dynamics in quantum systems. Here we demonstrate the generation and control of sub-femtosecond pulse pairs from a two-colour X-ray free-electron laser (XFEL). By measuring the delay between the two pulses with an angular streaking diagnostic, we characterise the group velocity of the XFEL and demonstrate control of the pulse delay down to 270 as. We demonstrate the application of this technique to a pump-probe measurement in core-excited para-aminophenol. These results demonstrate the ability to perform pump-probe experiments with sub-femtosecond resolution and atomic site specificity.

physics.acc-ph↗

arXiv2023

A compact single-shot soft X-ray photon spectrometer for free electron laser diagnostics

The photon spectrum from free-electron laser (FEL) light sources offers valuable information in time-resolved experiments and machine optimization in the spectral and temporal domains. We have developed a compact single-shot photon spectrometer to diagnose soft X-ray spectra. The spectrometer consists of an array of off-axis Fresnel zone plates (FZP) that act as transmission-imaging gratings, a Ce-YAG scintillator, and a microscope objective to image the scintillation target onto a two-dimensional imaging detector. This spectrometer operates in an energy range which covers absorption edges associated with several atomic constituents carbon, nitrogen, oxygen, and neon. The spectrometer's performance is demonstrated at a repetition rate of 120 Hz, but our detection scheme can be easily extended to 200 kHz spectral collection by employing a fast complementary metal oxide semiconductor (CMOS) line-scan camera to detect the light from the scintillator. This compact photon spectrometer provides an opportunity for monitoring the spectrum downstream of an endstation in a limited space environment with subelectronvolt energy resolution.

physics.ins-det↗

arXiv2022

Neon in ultrashort and intense x rays from free electron lasers

We theoretically examine neon atoms in ultrashort and intense x rays from free electron lasers and compare our results with data from experiments conducted at the Linac Coherent Light Source (LCLS). For this purpose, we treat in detail the electronic structure in all possible nonrelativistic cationic configurations using a relativistic multiconfiguration approach. The interaction with the x rays is described in rate-equation approximation. To understand the mechanisms of the interaction, a path analysis is devised which allows us to investigate what sequences of photoionization and decay processes lead to a specific configuration and with what probability. Thereby, we uncover a connection to the mathematics of graph theory and formal languages. In detail, we study the ion yields and find that plain rate equations do not provide a satisfactory description. We need to extend the rate equations for neon to incorporate double Auger decay of a $K$-shell vacancy and photoionization shake off for neutral neon. Shake off is included for valence and core ionization; the former has hitherto been overlooked but has important consequences for the ion yields from an x-ray energy below the core ionization threshold. Furthermore, we predict the photon yields from XUV and x-ray fluorescence; these allow one insights into the configurations populated by the interaction with the x rays. Finally, we discover that inaccuracies in those Auger decay widths employed in previous studies have only a minor influence on ion and photon yields.

physics.atom-ph↗

arXiv2022

At-the-edge Data Processing for Low Latency High Throughput Machine Learning Algorithms

High throughput and low latency data processing is essential for systems requiring live decision making, control, and machine learning-optimized data reduction. We focus on two distinct use cases for in-flight streaming data processing for a) X-ray pulse reconstruction at SLAC's LCLS-II Free-Electron Laser and b) control diagnostics at the DIII-D tokamak fusion reactor. Both cases exemplify high throughput and low latency control feedback and motivate our focus on machine learning at the edge where data processing and machine learning algorithms can be implemented in field programmable gate array based hardware immediately after the diagnostic sensors. We present our recent work on a data preprocessing chain which requires fast featurization for information encoding. We discuss several options for such algorithms with the primary focus on our discrete cosine and sine transform-based approach adapted for streaming data. These algorithms are primarily aimed at implementation in field programmable gate arrays, favoring linear algebra operations that are also aligned with the recent advances in inference accelerators for the computational edge.

physics.ins-det↗

arXiv2021

The Time-resolved Atomic, Molecular and Optical Science Instrument at the Linac Coherent Light Source

The newly constructed Time-resolved atomic, Molecular and Optical science instrument (TMO), is configured to take full advantage of both linear accelerators at SLAC National Accelerator Laboratory, the copper accelerator operating at a repetition rate of 120 Hz providing high per pulse energy, as well as the superconducting accelerator operating at a repetition rate of about 1 MHz providing high average intensity. Both accelerators build a soft X-ray free electron laser with the new variable gab undulator section. With this flexible light sources, TMO supports many experimental techniques not previously available at LCLS and will have two X-ray beam focus spots in line. Thereby, TMO supports Atomic, Molecular and Optical (AMO), strong-field and nonlinear science and will host a designated new dynamic reaction microscope with a sub-micron X-ray focus spot. The flexible instrument design is optimized for studying ultrafast electronic and molecular phenomena and can take full advantage of the sub-femtosecond soft X-ray pulse generation program.

physics.ins-det↗