Time-resolving the UV-initiated photodissociation dynamics of OCS

Karamatskos, Evangelos; Yarlagadda, Suresh; Patchkovskii, Serguei; Vrakking, Marc J. J.; Welsch, Ralph; Küpper, Jochen; Rouzée, Arnaud

doi:10.1039/d0fd00119h

Cited by 5 publications

(1 citation statement)

References 76 publications

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“…In collaboration with Arnaud Rouzée at MBI Berlin, some of us have set up a research program [102] and performed several experiments toward the disentangling of the actual structural dynamics of this bending and dissociation process. We've computed the expected wavepacket dynamics on the electronically-excited-state surfaces and experimentally recorded time-dependent transients of the dynamics using ion imaging [105]. These data show a clear and interesting discrepancy between the time-dependent yield of the photofragments and the computations and earlier spectroscopic results, which needs further investigation and could surely be resolved by a direct structural probe, such as LIED.…”

Section: Approaching Femtochemistry With Two-colour Pump-probe Liedmentioning

confidence: 90%

New perspectives in time-resolved laser-induced electron diffraction

Giovannini

Küpper

Trabattoni

2023

J. Phys. B: At. Mol. Opt. Phys.

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Imaging the microscopic world in real space and real-time is a grand challenge of science. In the landscape of time-resolved imaging techniques, laser-induced electron diffraction (LIED) has recently shown to be a promising candidate to push the frontiers of ultrafast molecular imaging. In this work, we review the main achievements of LIED research in terms of experimental results and advanced modeling. We also envision interesting perspectives toward the future advancement of time-resolved LIED imaging.

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Section: Approaching Femtochemistry With Two-colour Pump-probe Liedmentioning

confidence: 90%

New perspectives in time-resolved laser-induced electron diffraction

Giovannini

Küpper

Trabattoni

2023

J. Phys. B: At. Mol. Opt. Phys.

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Probing electron localization during molecular dissociation by femtosecond strong-field ion momentum spectroscopy

Zhao,

Xu,

et al. 2023

Commun Phys

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The study of molecular valence electron dynamics and their coupling with nuclear motion is one of the frontiers of ultrafast physics and ultrafast chemistry. With time-resolved strong-field ion momentum spectroscopy, we study electron valence and nucleus wavepacket evolution on a femtosecond timescale. Two orientation-dependent bond-breaks of N2O molecules from the same electronic state are studied, and the influence of orbital hybridization and polarization effect during molecular breaking is analyzed based on the measured time-resolved asymmetric Pzsum distributions, allowing a visual representation of electron localization during the dissociation of molecules into ions and atoms. Comparison of experimental and theoretical results on orientation-dependent dissociation dynamics allows us to understand how nuclear motions evolve during fragmentation and to control ultrafast molecular reactions.

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A laboratory frame density matrix for ultrafast quantum molecular dynamics

Gregory

Neville

Schuurman

et al. 2022

The Journal of Chemical Physics

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In most cases, the ultrafast dynamics of resonantly excited molecules are considered and almost always computed in the molecular frame, while experiments are carried out in the laboratory frame. Here, we provide a formalism in terms of a lab frame density matrix, which connects quantum dynamics in the molecular frame to those in the laboratory frame, providing a transparent link between computation and measurement. The formalism reveals that in any such experiment, the molecular frame dynamics vary for molecules in different orientations and that certain coherences, which are potentially experimentally accessible, are rejected by the orientation-averaged reduced vibronic density matrix. Instead, molecular angular distribution moments are introduced as a more accurate representation of experimentally accessible information. Furthermore, the formalism provides a clear definition of a molecular frame quantum tomography and specifies the requirements to perform such a measurement enabling the experimental imaging of molecular frame vibronic dynamics. Successful completion of such a measurement fully characterizes the molecular frame quantum dynamics for a molecule at any orientation in the laboratory frame.

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Time-resolving the UV-initiated photodissociation dynamics of OCS

Abstract: We present a time-resolved study of the photodissociation dynamics of OCS after UV- photoexcitation at λ = 237 nm. OCS molecules (X 1Σ+) were primarily excited to the 1 1A′′...

Cited by 5 publications

References 76 publications

New perspectives in time-resolved laser-induced electron diffraction

New perspectives in time-resolved laser-induced electron diffraction

Probing electron localization during molecular dissociation by femtosecond strong-field ion momentum spectroscopy

A laboratory frame density matrix for ultrafast quantum molecular dynamics

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