arXiv subjects

Huynh V. S. Lam

Publications and source records attributed to Huynh V. S. Lam.

3 recordsLinked to original sources

arXiv2026

Heteroatom Position Controls Ultrafast Photodynamics of Oxazole and Isoxazole

The ultrafast photochemistry of heterocyclic compounds is central to photobiology and materials chemistry, yet direct experimental observation of their structural dynamics remains rare. Here we present the first real-time structural characterization of photoinduced ring opening and subsequent fragmentation in the isomeric pair oxazole and isoxazole using MeV ultrafast electron diffraction (UED), complemented by non-adiabatic molecular dynamics simulations. Upon photoexcitation at 200 nm, both isomers undergo ring opening followed by fragmentation into various products, but with strikingly different dynamics governed by heteroatom positioning. Trajectory Surface Hopping simulations reproduce the experimental diffraction signatures, which are surprisingly similar for both isomers, and reveal distinct mechanistic pathways for the two isomers. For isoxazole, all trajectories exclusively undergo N-O bond cleavage within 40 fs, followed by sequential fragmentation into HCN + ketene and HCO + vinyl nitrene channels on the hundreds-of-femtoseconds timescale. Oxazole, by contrast, shows significantly slower ring opening (290 fs) with only 85% efficiency, proceeding primarily through O-C cleavage and accessing a richer landscape of intermediates including nitrile ylide and O-pyramidalized structures. Simulated diffraction patterns derived from trajectory ensembles, convolved with the experimental instrument response function, are in agreement with the branching ratios observed by UED. This synergy between UED and trajectory surface hopping provides an atomistic picture of how the simple interchange of heteroatom connectivity in structural isomers fundamentally reshapes excited-state potential surfaces, conical intersection accessibility, and photochemical outcome.

physics.chem-ph↗

arXiv2026

Neural Network Based Molecular Structure Retrieval from Coulomb Explosion Imaging Data

Determining the structure and following the structural evolution of molecules undergoing chemical reactions is one of the key goals of ultrafast molecular physics and chemistry. Recently, Coulomb explosion imaging has emerged as a promising technique for imaging the evolving structure of individual molecules in the gas phase. However, its practical application for structure determination is hampered by the lack of suitable algorithms to directly retrieve the molecular structure from the measured fragment-ion momentum data. Here, we propose a scheme to solve the underlying inverse problem by employing neural networks to infer the initial atomic positions from the final ion momenta on an event-by-event basis. Using this scheme, we retrieve the structure of several polyhalomethane isomers from simulated Coulomb explosion imaging data with an average per-atom position error of approximately 0.1 atomic units, i.e., to within 5% of the typical bond lengths. This development paves the way for an automated structure retrieval from Coulomb explosion data one molecule at a time, making it ideally suitable for analyzing pump-probe experiments where several products are formed that need to be distinguished.

physics.chem-ph↗

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↗