Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation

Ibrahim, Heide; Wales, B.; Beaulieu, Samuel; Schmidt, Bruno E.; Thiré, Nicolas; Fowe, Emmanuel Penka; Bisson, Éric; Hebeisen, Christoph T.; Wanie, Vincent; Giguère, Mathieu; Kieffer, Jean‐Claude; Spanner, Michael; Bandrauk, André D.; Sanderson, Joseph; Schuurman, Michael S.; Légaré, François

doi:10.1038/ncomms5422

Cited by 119 publications

(99 citation statements)

References 38 publications

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“…Isomerization of acetylene (HCCH) to form vinylidene (H 2 CC) has been studied in the neutral molecule, as well as singly and doubly charged acetylene ions 1,2,[24][25][26][27][28][29][30][31][32][33][34][35][36] . Acetylene cations are important not only as a model for molecular dynamics and radiation damage investigations, but also in a range of applications, from plasma devices 37 , combustion 38 , semiconductor manufacturing 39 and to understanding planetary atmospheres 40 .…”

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Ultrafast isomerization initiated by X-ray core ionization

et al. 2015

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Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-ray-free electron lasers. Here we study X-ray-initiated isomerization of acetylene, a model for proton dynamics in hydrocarbons. Our time-resolved measurements capture the transient motion of protons following X-ray ionization of carbon K-shell electrons. We Coulomb-explode the molecule with a second precisely delayed X-ray pulse and then record all the fragment momenta. These snapshots at different delays are combined into a 'molecular movie' of the evolving molecule, which shows substantial proton redistribution within the first 12 fs. We conclude that significant proton motion occurs on a timescale comparable to the Auger relaxation that refills the K-shell vacancy.

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confidence: 99%

“…In the singly charged ion the ultrafast isomerization is not launched with 800 nm radiation, but has been demonstrated to proceed from the excited A 2 AE þ g state 26,35 . Core ionization, which was employed in the current work for initiating isomerization, occurs in the weak-field regime, unlike the strong-field 800 nm experiments.…”

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Ultrafast isomerization initiated by X-ray core ionization

et al. 2015

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“…As an example, acetylene, a commonly investigated molecule in strong-field physics, can be excited by the third harmonic (as was done in e.g. [44]) and the isomerization to vinylidene can be controlled with the ω/2ω field near conical intersections.…”

Section: Resultsmentioning

confidence: 99%

“…The setup is based on a Ti:sapphire laser system with pulse durations down to 25 fs and an energy of up to 720 µJ at a repetition rate of 10 kHz (Femtopower Compact Pro HR, Spectra Physics). We took special care to achieve a high yield in sum frequency generation (SFG), which was done in a collinear configuration, following the idea proposed by Kardaś et al [43], and the experimental implementation by Ibrahim et al [44] In short, the laser passes through the following series of optical components: a 200 µm thick β-barium borate (BBO) crystal cut at 27.2 • for second harmonic generation (SHG), a birefringent material to retard the fundamental beam (450 µm thick BBO cut at 70 • ), a λ/2 quartz wave-plate to rotate the fundamental beam with respect to the second harmonic, and a 100 µm thick BBO cut at 44.3 • , where sum frequency mixing allows for efficient SFG. In the second part of the setup, the second and third harmonic beams are separated from the fundamental beam using a combination of a custom-made triple band dichroic beamsplitters (BS) facilitating low group delay dispersion (below 50 fs 2 ), and supporting the full bandwidth of each harmonic.…”

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confidence: 99%

Compact and flexible harmonic generator and three-color synthesizer for femtosecond coherent control and time-resolved studies

et al. 2017

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Abstract:Intense, multi-color laser fields permit the control of the ionization of atoms and the steering of electron dynamics. Here, we present the efficient collinear creation of the second and third harmonic of a 790 nm femtosecond laser followed by a versatile field synthesizer for the three color fields' composition. Using the device, we investigate the strong-field ionization of neon by fields composed of the fundamental, and the second or third harmonic. The three-color device offers sufficient flexibility for the coherent control of strong-field processes and for time-resolved pump-probe studies. References and links1. T. Brabec and F. Krausz, "Intense few-cycle laser fields: Frontiers of nonlinear optics," Rev. Mod. Phys. 72, 545-591 (2000). 2. L. DiMauro and P. Agostini, "Ionization dynamics in strong laser fields," Adv. At. Mol. Opt. Phys. 35, 79-120 (1995). 3. K. Burnett, V. C. Reed, and P. L. Knight, "Atoms in ultra-intense laser fields," J. Phys. B At. Mol. Opt. Phys. 26, 561-598 (1993). 4. T. Brabec, Strong Field Laser Physics (Springer, 2009 and F. X. Kärtner, "High-energy pulse synthesis with sub-cycle waveform control for strong-field physics," Nat. Photonics 5, 475-479 (2011). 42. P. B. Corkum, "Plasma perspective on strong field multiphoton ionization," Phys. Rev. Lett. 71, 1994Lett. 71, -1997Lett. 71, (1993

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“…More recently, several studies have considered the response to strong fields. This has included single [16,17] and double [18,19] ionization, dissociative ionization of highly excited states [20], high harmonic generation [21][22][23][24] and more recently initiating isomerization of acetylene to vinylidene [25].…”

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confidence: 99%

Probing the role of excited states in ionization of acetylene

Dundas

Mulholland

Wardlow

et al. 2017

Phys. Chem. Chem. Phys.

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Ionization of acetylene by linearly-polarized, vacuum ultraviolet (VUV) laser pulses is modelled using timedependent density functional theory. Several laser wavelengths are considered including one that produces direct ionization to the first excited cationic state while another excites the molecules to a Rydberg series incorporating an autoionizing state. We show that for the wavelengths and intensities considered, ionization is greatest whenever the molecule is aligned along the laser polarization direction. By considering high harmonic generation we show that populating excited states can lead to a large enhancement in the harmonic yield. Lastly, angularly-resolved photoelectron spectra are calculated which show how the energy profile of the emitted electrons significantly changes in the presence of these excited states.

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Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation

Cited by 119 publications

References 38 publications

Ultrafast isomerization initiated by X-ray core ionization

Ultrafast isomerization initiated by X-ray core ionization

Compact and flexible harmonic generator and three-color synthesizer for femtosecond coherent control and time-resolved studies

Probing the role of excited states in ionization of acetylene

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