All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane

Rebholz, Marc; Ding, Thomas; Despré, Victor; Aufleger, Lennart; Hartmann, Maximilian; Meyer, Kristina; Stooß, Veit; Magunia, Alexander; Wachs, David; Birk, Paul; Mi, Yonghao; Borisova, Gergana Dimitrova; Castanheira, Carina da Costa; Rupprecht, Patrick; Schmid, Georg; Schnorr, Kirsten; Schröter, C. D.; Moshammer, R.; Loh, Zhi-Heng; Attar, Andrew R.; Leone, Stephen R.; Gaumnitz, Thomas; Wörner, Hans Jakob; Roling, Sebastian; Butz, Marco; Zacharias, H.; Düsterer, S.; Treusch, R.; Brenner, Günter; Vester, Jonas; Kuleff, Alexander I.; Ott, Christian; Pfeifer, Thomas

doi:10.1103/physrevx.11.031001

Cited by 19 publications

(13 citation statements)

References 53 publications

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“…Moreover, this isomerization is not a key process for molecular I 2 -loss at the lower electronic states of the cation. Recently, the transient [CH 2 -I-I] + isomeric ion 2 in the dissociation of the [CH 2 I 2 ] •+ molecular has been proven experimentally with the XUV FEL at Hamburg [64].…”

Section: Photofragmentations Of Halomethanesmentioning

confidence: 99%

Perspectives of Gas Phase Ion Chemistry: Spectroscopy and Modeling

et al. 2022

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The study of ions in the gas phase has a long history and has involved both chemists and physicists. The interplay of their competences with the use of very sophisticated commercial and/or homemade instrumentations and theoretical models has improved the knowledge of thermodynamics and kinetics of many chemical reactions, even if still many stages of these processes need to be fully understood. The new technologies and the novel free-electron laser facilities based on plasma acceleration open new opportunities to investigate the chemical reactions in some unrevealed fundamental aspects. The synchrotron light source can be put beside the FELs, and by mass spectrometric techniques and spectroscopies coupled with versatile ion sources it is possible to really change the state of the art of the ion chemistry in different areas such as atmospheric and astro chemistry, plasma chemistry, biophysics, and interstellar medium (ISM). In this manuscript we review the works performed by a joint combination of the experimental studies of ion–molecule reactions with synchrotron radiation and theoretical models adapted and developed to the experimental evidence. The review concludes with the perspectives of ion–molecule reactions by using FEL instrumentations as well as pump probe measurements and the initial attempt in the development of more realistic theoretical models for the prospective improvement of our predictive capability.

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Section: Photofragmentations Of Halomethanesmentioning

confidence: 99%

Perspectives of Gas Phase Ion Chemistry: Spectroscopy and Modeling

et al. 2022

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“…This can be done by either recording photoelectron 11 or fragment kinetic energy release 12 , 13 spectra of the target but also via the detection of the molecule’s absorption spectrum. 14 , 15 …”

Section: Introductionmentioning

confidence: 99%

“…This can be done by either recording photoelectron 11 or fragment kinetic energy release 12,13 spectra of the target but also via the detection of the molecule's absorption spectrum. 14,15 Photoelectron/photofragment ion spectroscopy gives detailed information on all produced fragments and electrons including their kinetic energies over a broad bandwidth. 16−18 It is even possible to reconstruct the three-dimensional (3D) momentum distribution of produced fragments or ejected photoelectrons.…”

Section: ■ Introductionmentioning

confidence: 99%

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XUV-Initiated Dissociation Dynamics of Molecular Oxygen (O₂)

et al. 2021

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We performed a time-resolved spectroscopy experiment on the dissociation of oxygen molecules after the interaction with intense extreme-ultraviolet (XUV) light from the free-electron laser in Hamburg at Deutsches Elektronen-Synchrotron. Using an XUV-pump/XUV-probe transient-absorption geometry with a split-and-delay unit, we observe the onset of electronic transitions in the O 2+ cation near 50 eV photon energy, marking the end of the progression from a molecule to two isolated atoms. We observe two different time scales of 290 ± 53 and 180 ± 76 fs for the emergence of different ionic transitions, indicating different dissociation pathways taken by the departing oxygen atoms. With regard to the emerging opportunities of tuning the central frequencies of pump and probe pulses and of increasing the probe–pulse bandwidth, future pump–probe transient-absorption experiments are expected to provide a detailed view of the coupled nuclear and electronic dynamics during molecular dissociation.

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“…2a) consists of multiple overlap- ping components. To deconvolve the overlapping spectral and temporal components of the experimental data, we have applied global analysis (GA) [81][82][83][84][85], which reduces the signal to a few principal spectral components S i (E), each with simple exponential time dynamics f i (t) convolved with the instrument response, viz.…”

mentioning

confidence: 99%

Momentum-Resolved Exciton Coupling and Valley Polarization Dynamics in Monolayer WS$_2$

Kunin¹,

Чернов²,

Bakalis³

et al. 2022

Preprint

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Coupling between exciton states across the Brillouin zone in monolayer transition metal dichalcogenides can lead to ultrafast valley depolarization. Using time-and angle-resolved photoemission, we present momentum-and energy-resolved measurements of exciton coupling in monolayer WS2. By comparing full 4D (kx, ky, E, t) data sets after both linearly and circularly polarized excitation, we are able to disentangle intervalley and intravalley exciton coupling dynamics. Recording in the exciton binding energy basis instead of excitation energy, we observe strong mixing between the B1s exciton and An>1 states. The photoelectron energy and momentum distributions observed from excitons populated via intervalley coupling (e.g. K − → K + ) indicate that the dominant valley depolarization mechanism conserves the exciton binding energy and center-of-mass momentum, consistent with intervalley Coulomb exchange. On longer timescales, exciton relaxation is accompanied by contraction of the momentum space distribution.

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All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane

Cited by 19 publications

References 53 publications

Perspectives of Gas Phase Ion Chemistry: Spectroscopy and Modeling

Perspectives of Gas Phase Ion Chemistry: Spectroscopy and Modeling

XUV-Initiated Dissociation Dynamics of Molecular Oxygen (O₂)

Momentum-Resolved Exciton Coupling and Valley Polarization Dynamics in Monolayer WS$_2$

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All-XUV Pump-Probe Transient Absorption Spectroscopy of the Structural Molecular Dynamics of Di-iodomethane

Cited by 19 publications

References 53 publications

Perspectives of Gas Phase Ion Chemistry: Spectroscopy and Modeling

Perspectives of Gas Phase Ion Chemistry: Spectroscopy and Modeling

XUV-Initiated Dissociation Dynamics of Molecular Oxygen (O2)

Momentum-Resolved Exciton Coupling and Valley Polarization Dynamics in Monolayer WS$_2$

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Product

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XUV-Initiated Dissociation Dynamics of Molecular Oxygen (O₂)