Ultrafast Relaxation Dynamics of the Ethylene Cation C2H4+

Ludwig, André; Liberatore, Elisa; Herrmann, J.; Kasmi, Lamia; López‐Tarifa, Pablo; Gallmann, L.; Röthlisberger, Ursula; Keller, U.; Lucchini, Matteo

doi:10.1021/acs.jpclett.6b00646

Cited by 26 publications

(49 citation statements)

References 33 publications

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“…In Ref. 10, the Keller group studied the relaxation dynamics of ethylene after sudden ionization by an attosecond pulse train (APT) in the extreme-ultraviolet (XUV) spectral region. After ionization, the molecule is left in an excited state, which can either relax to the cation ground state or lead to molecular fragmentation.…”

Section: Intramolecular Charge Transfermentioning

confidence: 99%

“…We then turn from charge migration to intramolecular charge transfer (ICT) and discuss the relaxation dynamics of the ethylene cation following ionization by an extreme-ultraviolet (XUV) attosecond pulse train (APT) 10 . A time-resolved experiment, realized in combination with a femtosecond near-infrared (IR) laser pulse, provided an improved isomerization time for the reaction

{normalH}_{2} C = {CH}_{2}^{+} \to HC - {CH}_{3}^{+}

of 30 ± 3 fs, and by comparison with ab-initio calculations the relevant conical intersections (CIs) could be identified.…”

Section: Introductionmentioning

confidence: 99%

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Charge migration and charge transfer in molecular systems

Wörner

Arrell

Banerji

et al. 2017

Structural Dynamics

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The transfer of charge at the molecular level plays a fundamental role in many areas of chemistry, physics, biology and materials science. Today, more than 60 years after the seminal work of R. A. Marcus, charge transfer is still a very active field of research. An important recent impetus comes from the ability to resolve ever faster temporal events, down to the attosecond time scale. Such a high temporal resolution now offers the possibility to unravel the most elementary quantum dynamics of both electrons and nuclei that participate in the complex process of charge transfer. This review covers recent research that addresses the following questions. Can we reconstruct the migration of charge across a molecule on the atomic length and electronic time scales? Can we use strong laser fields to control charge migration? Can we temporally resolve and understand intramolecular charge transfer in dissociative ionization of small molecules, in transition-metal complexes and in conjugated polymers? Can we tailor molecular systems towards specific charge-transfer processes? What are the time scales of the elementary steps of charge transfer in liquids and nanoparticles? Important new insights into each of these topics, obtained from state-of-the-art ultrafast spectroscopy and/or theoretical methods, are summarized in this review.

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Section: Intramolecular Charge Transfermentioning

confidence: 99%

{normalH}_{2} C = {CH}_{2}^{+} \to HC - {CH}_{3}^{+}

of 30 ± 3 fs, and by comparison with ab-initio calculations the relevant conical intersections (CIs) could be identified.…”

Section: Introductionmentioning

confidence: 99%

Charge migration and charge transfer in molecular systems

Wörner

Arrell

Banerji

et al. 2017

Structural Dynamics

Self Cite

181

163

View full text Add to dashboard Cite

show abstract

“…1 In many photochemical reactions, the products and their relative yields depend sensitively on the details of these coupled molecular dynamics and processes that occur within a few femtoseconds. [2][3][4][5][6][7] For example, near a conical intersection, where the evolving molecular geometry finds two or more electronic states of equal potential energy, nonadiabatic transitions can occur, enabling important non-radiative relaxation mechanisms, such as competing isomerization or dissociation pathways. 8,9 Considerable interest in investigating such dynamics on their natural femtosecond timescales has driven recent developments of time-resolved spectroscopic methods employing few-cycle infrared lasers and broadband attosecond pulses.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast photodissociation dynamics and nonadiabatic coupling between excited electronic states of methanol probed by time-resolved photoelectron spectroscopy

Champenois

Greenman

Shivaram

et al. 2019

The Journal of Chemical Physics

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The electronic and nuclear dynamics in methanol, following 156 nm photoexcitation, are investigated by combining a detailed analysis of time-resolved photoelectron spectroscopy experiments with electronic structure calculations. The photoexcitation pump pulse is followed by a delayed 260 nm photoionization probe pulse, to produce photoelectrons that are analyzed by velocity map imaging. The yield of mass-resolved ions, measured with similar experimental conditions, are found to exhibit the same time-dependence as specific photoelectron spectral features. Energy-resolved signal onset and decay times are extracted from the measured photoelectron spectra to achieve high temporal resolution, beyond the 20 fs pump and probe pulse durations. When combined with ab initio calculations of selected cuts through the excited state potential energy surfaces, this information allows the dynamics of the transient excited molecule, which exhibits multiple nuclear and electronic degrees of freedom, to be tracked on its intrinsic few-femtosecond timescale. Within 15 fs of photoexcitation, we observe nuclear motion on the initially bound photoexcited 2 1 A (S 2 ) electronic state, through a conical intersection with the 1 1 A (S 3 ) state, which reveals paths to photodissociation following C-O stretch and C-O-H angle opening.

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“…To improve the signal-to-noise ratio, the experiment was referenced shot-to-shot using a tuning fork chopper, which blocked every second IR probe pulse, enabling a direct subtraction of the XUV induced background. 23 From two consecutive shots the delay-dependent relative change of the fragment ion yield I Rel (t) was extracted according to:…”

Section: Resultsmentioning

confidence: 99%