Single-shot carrier-envelope-phase-tagged ion-momentum imaging of nonsequential double ionization of argon in intense 4-fs laser fields

Johnson, Nora G.; Herrwerth, Oliver; Wirth, Adrian; De, Sankar; Ben‐Itzhak, I.; Lezius, M.; Bergues, Boris; Kling, Matthias F.; Senftleben, Arne; Schröter, C. D.; Moshammer, R.; Ullrich, J.; Betsch, K. J.; Jones, Robert R.; Sayler, A. M.; Rathje, Tim; Rühle, Klaus; Müller, Walter; Paulus, Gerhard G.

doi:10.1103/physreva.83.013412

Cited by 78 publications

(91 citation statements)

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“…In our present experimental studies on the CEP control of the deprotonation of acetylene, we employ CEP-tagged reaction microscopy (REMI) 24 (for details see the Methods section). The interaction of acetylene molecules with intense few-cycle pulses results in the dissociative ionization and isomerization of the molecule yielding a variety of reaction products 7 .…”

Section: Resultsmentioning

confidence: 99%

Subfemtosecond steering of hydrocarbon deprotonation through superposition of vibrational modes

et al. 2014

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Subfemtosecond control of the breaking and making of chemical bonds in polyatomic molecules is poised to open new pathways for the laser-driven synthesis of chemical products. The break-up of the C-H bond in hydrocarbons is an ubiquitous process during laser-induced dissociation. While the yield of the deprotonation of hydrocarbons has been successfully manipulated in recent studies, full control of the reaction would also require a directional control (that is, which C-H bond is broken). Here, we demonstrate steering of deprotonation from symmetric acetylene molecules on subfemtosecond timescales before the break-up of the molecular dication. On the basis of quantum mechanical calculations, the experimental results are interpreted in terms of a novel subfemtosecond control mechanism involving non-resonant excitation and superposition of vibrational degrees of freedom. This mechanism permits control over the directionality of chemical reactions via vibrational excitation on timescales defined by the subcycle evolution of the laser waveform.

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Section: Resultsmentioning

confidence: 99%

Subfemtosecond steering of hydrocarbon deprotonation through superposition of vibrational modes

et al. 2014

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“…Taking advantage of recent progress in phase-tagging [32] to overcome these difficulties, we report in this Letter the measurement of CEP-dependent spatial asymmetries in the dissociation of H + 2 , from an ion beam, which we quantitatively compare with ab initio theory. Roudnev and Esry have shown that these CEP effects are due to interference of different photon number pathways to 1sσ g and 2pσ u final states, having opposite nuclear parity, whose relative phase is controlled by the CEP [33].…”

Section: Pacs Numbers: XXXmentioning

confidence: 99%

Carrier-Envelope Phase Control over Pathway Interference in Strong-Field Dissociation ofH2+

et al. 2013

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The dissociation of an H + 2 molecular-ion beam by linearly polarized, carrier-envelope-phase-tagged 5 fs pulses at 4×10 14 W/cm 2 with a central wavelength of 730 nm was studied using a coincidence 3D momentum imaging technique. Carrier-envelope-phase-dependent asymmetries in the emission direction of H + fragments relative to the laser polarization were observed. These asymmetries are caused by interference of odd and even photon number pathways, where net-zero photon and 1-photon interference predominantly contributes at H + +H kinetic energy releases of 0.2 -0.45 eV, and net-2-photon and 1-photon interference contributes at 1.65 -1.9 eV. These measurements of the benchmark H + 2 molecule offer the distinct advantage that they can be quantitatively compared with ab initio theory to confirm our understanding of strong-field coherent control via the carrier-envelope phase. PACS numbers: XXXOne ultimate goal of ultrafast, strong-field laser science is to coherently control chemical reactions [1][2][3]. A prerequisite to achieving this goal is to understand the control mechanisms and reaction pathways. To this end, tailoring the electric field waveform of few-cycle laser pulses to control reactions and uncover the underlying physics has become a powerful tool [4][5][6]. It has been applied to the dissociative ionization of H 2 and its isotopologues [7][8][9][10][11][12] and has recently been extended to more complex diatomic molecules, such as CO [13][14][15], and to small polyatomic molecules [16,17].Conceptually, one of the most basic features of a fewcycle laser pulse to control is the carrier-envelope phase (CEP). When the laser's electric field is written as E(t) = E 0 (t) cos(ωt + φ), E 0 (t) is an envelope function, ω is the carrier angular frequency, and φ is the CEP. In fact, all of the few-cycle waveform experiments cited above used the CEP as the control parameter.For example, Kling et al. used 5 fs, 1.2×10 14 W/cm 2 pulses with stabilized CEP to dissociatively ionize D 2 and found asymmetries in the emission direction of D + ions for kinetic energy releases (KER) above 6 eV [7,8]. The diminished dissociation signal in a circularly polarized laser field indicated that recollision played a role. Recollision entails a tunnel-ionized electron undergoing a collision with its parent ion after acceleration by the oscillating laser field [18,19]. The energy exchange between the laser-driven electron and the parent ion can promote the D + 2 to the 2pσ u excited state. Coupling of the 2pσ u and 1sσ g states [20] on the trailing edge of the laser pulse during the dissociation of D + 2 was suggested as the explanation for the CEP-dependent asymmetry [7,8].Another example comes from Kremer et al. who exposed an H 2 target to 6 fs, 4.4×10 14 W/cm 2 CEPstabilized laser pulses and observed asymmetries for KER values between 0.4 and 3 eV [9] -energies they attributed to bond softening (BS) [21] and not electron recollision, which has higher KER. They proposed that the initial ionization of H 2 generates a coherent wav...

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“…Even more insight into the process was gained in kinematically complete studies where the correlated two-electron momentum distributions were measured 11 and investigated for different laser parameters [12][13][14][15] . Measurements of the dynamics of NSDI in near-single cycle laser pulses have been restricted to recoil-ion spectra, which did not allow for the direct retrieval of the correlated electron-emission dynamics 16,17 . The sub-cycle dependence of electron correlation spectra has been explored by various theoretical studies, where the double-ionization dynamics were confined to a single cycle of a laser pulse 12,18 .…”

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Attosecond tracing of correlated electron-emission in non-sequential double ionization

et al. 2012

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Despite their broad implications for phenomena such as molecular bonding or chemical reac tions, our knowledge of multi electron dynamics is limited and their theoretical modelling remains a most difficult task. From the experimental side, it is highly desirable to study the dynamical evolution and interaction of the electrons over the relevant timescales, which extend into the attosecond regime. Here we use near single cycle laser pulses with well defined electric field evolution to confine the double ionization of argon atoms to a single laser cycle. The measured two electron momentum spectra, which substantially differ from spectra recorded in all previous experiments using longer pulses, allow us to trace the correlated emission of the two electrons on sub femtosecond timescales. The experimental results, which are discussed in terms of a semiclassical model, provide strong constraints for the development of theories and lead us to revise common assumptions about the mechanism that governs double ionization.

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Single-shot carrier-envelope-phase-tagged ion-momentum imaging of nonsequential double ionization of argon in intense 4-fs laser fields

Cited by 78 publications

References 30 publications

Subfemtosecond steering of hydrocarbon deprotonation through superposition of vibrational modes

Subfemtosecond steering of hydrocarbon deprotonation through superposition of vibrational modes

Carrier-Envelope Phase Control over Pathway Interference in Strong-Field Dissociation ofH2+

Attosecond tracing of correlated electron-emission in non-sequential double ionization

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