Sub-cycle steering of the deprotonation of acetylene by intense few-cycle mid-infrared laser fields

Li, H.; Kling, Nora G.; Gaumnitz, Thomas; Bürger, Christian; Schötz, Johannes; Liu, Qingcao; Ban, Loren; Pertot, Yoann; Wu, Jian; Azzeer, Abdallah M.; Vivie‐Riedle, Regina de; Wörner, Hans Jakob; Kling, Matthias F.

doi:10.1364/oe.25.014192

Cited by 10 publications

(6 citation statements)

References 49 publications

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“…The active space provided for the static electron correlation was adapted to the number of the valence electrons consisting of 10 molecular orbitals and the according electrons except for the 1s-core electrons of the carbon atoms, following Refs. 31 and 32. The calculations were performed using the program package MOLPRO 2012 (Refs.…”

Section: Methodsmentioning

confidence: 99%

Time-resolved nuclear dynamics in bound and dissociating acetylene

Bürger

Atia-Tul-Noor

Schnappinger

et al. 2018

Structural Dynamics

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We have investigated nuclear dynamics in bound and dissociating acetylene molecular ions in a time-resolved reaction microscopy experiment with a pair of few-cycle pulses. Vibrating bound acetylene cations or dissociating dications are produced by the first pulse. The second pulse probes the nuclear dynamics by ionization to higher charge states and Coulomb explosion of the molecule. For the bound cations, we observed vibrations in acetylene (HCCH) and its isomer vinylidene (CCHH) along the CC-bond with a periodicity of around 26 fs. For dissociating dication molecules, a clear indication of enhanced ionization is found to occur along the CH- and CC-bonds after 10 fs to 40 fs. The time-dependent ionization processes are simulated using semi-classical on-the-fly dynamics revealing the underling mechanisms.

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Section: Methodsmentioning

confidence: 99%

Time-resolved nuclear dynamics in bound and dissociating acetylene

Bürger

Atia-Tul-Noor

Schnappinger

et al. 2018

Structural Dynamics

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“…The reconstructed pulse duration is τ rec = (11.5 ± 0.8) fs and the Fourier-transform limit (FTL) is τ FTL = 7.9 fs. The CEP stability was independently verified by sending pulses attenuated to 340 µJ into a single-shot stereo-ATI phase meter [36,37]. The passive CEP stability of the two-cycle mid-IR pulses was found to be better than 300 mrad (rms) from a single-shot measurement performed over 30 minutes.…”

Section: Few-cycle Mid-ir Pulse Generationmentioning

confidence: 97%

Streaking of 43-attosecond soft-X-ray pulses generated by a passively CEP-stable mid-infrared driver

et al. 2017

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Attosecond metrology has so far largely remained limited to titanium:sapphire lasers combined with an active stabilization of the carrier-envelope phase (CEP). These sources limit the achievable photon energy to ∼100 eV which is too low to access X-ray absorption edges of most second- and third-row elements which are central to chemistry, biology and material science. Therefore, intense efforts are underway to extend attosecond metrology to the soft-X-ray (SXR) domain using mid-infrared (mid-IR) drivers. Here, we introduce and experimentally demonstrate a method that solves the long-standing problem of the complete temporal characterization of ultra-broadband (≫10 eV) attosecond pulses. We generalize the recently proposed Volkov-transform generalized projection algorithm (VTGPA) to the case of multiple overlapping photoelectron spectra and demonstrate its application to isolated attosecond pulses. This new approach overcomes all key limitations of previous attosecond-pulse reconstruction methods, in particular the central-momentum approximation (CMA), and it incorporates the physical, complex-valued and energy-dependent photoionization matrix elements. These properties make our approach general and particularly suitable for attosecond supercontinua of arbitrary bandwidth. We apply this method to attosecond SXR pulses generated from a two-cycle mid-IR driver, covering a bandwidth of ∼100 eV and reaching photon energies up to 180 eV. We extract an SXR pulse duration of (43±1) as from our streaking measurements, defining a new world record. Our results prove that the popular and broadly available scheme of post-compressing the output of white-light-seeded optical parametric amplifiers is adequate to produce high-contrast isolated attosecond pulses covering the L-edges of silicon, phosphorous and sulfur. Our new reconstruction method and experimental results open the path to the production and characterization of attosecond pulses lasting less than one atomic unit of time (24 as) and covering X-ray absorption edges of most light elements.

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“…Among the techniques targeting this issue are those employing pulses of few-cycle duration, which are inherently asymmetric or two color (o/2o) fields of multi-cycle duration. In the first case, the spatial asymmetry varies as a function of the Carrier Envelope Phase (CEP), [4][5][6] while in the latter by changing the relative phase of the field components. [7][8][9][10][11] The two-color scheme was initially introduced by Brumer and Shapiro.…”

Section: Introductionmentioning

confidence: 99%