arXiv subjects

Enliang Wang

Publications and source records attributed to Enliang Wang.

8 recordsLinked to original sources

arXiv2026

Probing the structure of cyclic hydrocarbon molecules with X-ray-induced Coulomb explosion imaging

Coulomb explosion imaging (CEI) is a powerful experimental technique that maps a molecule's geometric structure onto the momenta of ionic molecular fragments produced by rapid multiple ionization. Here, we apply CEI induced by pulses from an X-ray free-electron laser in order to image and distinguish complex hydrocarbon isomers with the chemical formula C7H8: toluene, cycloheptatriene, and 1,6-heptadiyne. The measured fragment-ion momentum distributions show discernible differences between the three isomers and provide signatures of specific carbon and hydrogen sites in the molecule. In contrast to previous work, we demonstrate that distinct 'marker atoms' are not strictly required for constructing a meaningful molecular frame of reference for the interpretation of the momentum-space data. Our work paves the way for tracking the ultrafast motion of nuclei during isomerization reactions in pure hydrocarbons.

physics.chem-ph↗

arXiv2025

Decoding Molecular Geometries in Coulomb Explosion Imaging via Physics-Informed Deep Neural Network

Determining the absolute configuration of gas-phase molecules in position-space has long been a fundamental challenge in molecular physics. While strong-field-induced Coulomb explosion imaging (CEI) has emerged as a powerful tool for probing molecular stereochemistry in momentum-space, reconstructing the original three-dimensional structure of polyatomic molecules remains a long-standing challenge due to the inherent complexity of multidimensional inversion. Here, we introduce a deep learning framework that bridges this gap by directly recovering position-space molecular structures from Coulomb explosion momentum patterns. Our approach combines CEI simulations with a neural network trained to establish the mapping between momentum-space Newton plots and real-space geometries. The trained model demonstrates high fidelity in reconstructing the structure of CHF$_3$ from experimental CEI data. This generalizable framework can not only be extended to other molecular systems but also opens avenues for time-resolved structural analysis of molecular dynamics.

physics.atm-clus↗

arXiv2025

Imaging transient molecular configurations in UV-excited diiodomethane

Femtosecond structural dynamics of diiodomethane ($\mathrm{CH_2I_2}$) triggered by ultraviolet (UV) photoabsorption at 290 nm and 330 nm are studied using time-resolved coincident Coulomb explosion imaging driven by a near-infrared probe pulse. We map the dominant single-photon process, the cleavage of the carbon-iodine bond producing rotationally excited $\mathrm{CH_2I}$ radical, identify the contributions of the three-body ($\mathrm{CH_2} + \mathrm{I} + \mathrm{I}$) dissociation and molecular iodine formation channels, which are primarily driven by the absorption of more than one UV photon, and demonstrate the existence of a weak reaction pathway involving the formation of short-lived transient species resembling iso-$\mathrm{CH_2I{-}I}$ geometries with a slightly shorter I-I separation compared to the ground-state $\mathrm{CH_2I_2}$. These transient molecular configurations, which can be separated from the other channels by applying a set of conditions on the correlated momenta of three ionic fragments, are formed within approximately 100 fs after the initial photoexcitation and decay within the next 100 fs.

physics.chem-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

Differentiating Three-Dimensional Molecular Structures using Laser-induced Coulomb Explosion Imaging

Coulomb explosion imaging (CEI) with x-ray free electron lasers has recently been shown to be a powerful method for obtaining detailed structural information of gas-phase planar ring molecules [R. Boll et al. Nat. Phys. 18, 423-428 (2022)]. In this Letter, we investigate the potential of CEI driven by a tabletop laser and extend this approach to differentiating three-dimensional (3D) structures. We study the static CEI patterns of planar and nonplanar organic molecules that resemble the structures of typical products formed in ring-opening reactions. Our results reveal that each molecule exhibits a well-localized and distinctive pattern in 3D fragment-ion momentum space. We find that these patterns yield direct information about the molecular structures and can be qualitatively reproduced using a classical Coulomb explosion simulation. Our findings suggest that laser-induced CEI can serve as a robust method for differentiating molecular structures of organic ring and chain molecules. As such, it holds great promise as a method for following ultrafast structural changes, e.g., during ring-opening reactions, by tracking the motion of individual atoms in pump-probe experiments.

physics.atm-clus↗

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

Time-Resolved Coulomb Explosion Imaging Unveils Ultrafast Ring Opening of Furan

Following the changes in molecular structure throughout the entirety of a chemical reaction with atomic resolution is a long-term goal in femtochemistry. Although the development of a plethora of ultrafast technique has enabled detailed investigations of the electronic and nuclear dynamics on femtosecond time scales, direct and unambiguous imaging of the nuclear motion during a reaction is still a major challenge. Here, we apply time-resolved Coulomb explosion imaging with femtosecond near-infrared pulses to visualize the ultraviolet-induced ultrafast molecular dynamics of gas-phase furan. Widely contradicting predictions and observations for this molecule have been reported in the literature. By combining the experimental Coulomb explosion imaging data with ab initio molecular dynamics and Coulomb explosion simulations, we reveal the presence of a strong ultrafast ring-opening pathway upon excitation at 198 nm that occurs within 100 fs.

physics.chem-ph↗

arXiv2022

Observation and dynamic control of a new pathway of H$_3^+$ formation

We propose and experimentally demonstrate that the trihydrogen cation (H$_3^+$) can be produced via single photoionization of the molecular hydrogen dimer (H$_4$). Using near-infrared, femtosecond laser pulses and coincidence momentum imaging, we find that the dominant channel after single ionization of the dimer is the ejection of a hydrogen atom within a few hundred femtoseconds, leaving an H3+ cation behind. The formation mechanism is supported and well reproduced by an ab-initio molecular dynamics simulation. This is a new pathway of H$_3^+$ formation from ultracold hydrogen gas that may help explain the unexpected high abundance of H$_3^+$ in the interstellar medium in the universe.

physics.atm-clus↗