Attosecond coupled electron and nuclear dynamics in dissociative ionization of H2

Cattaneo, Laura; Vos, Jannie; Bello, Roger Y.; Palacios, Alicia; Heuser, Sebastian; Pedrelli, Luca; Lucchini, Matteo; Cirelli, Claudio; Martín, Fernando; Keller, U.

doi:10.1038/s41567-018-0103-2

Cited by 131 publications

(94 citation statements)

References 49 publications

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“…Briefly, due to the propagation across the potential-energy landscape the excited photoelectron wave packet aquires an energy-dependent phase which results in a measurable group delay, referred to as a photoionisation time delay. Relative delays between wave packets from different species [5][6][7], ionisation channels [8][9][10][11][12][13], and emission angles [14,15], have been measured to very high accuracy and serve as benchmarks for time-dependent quantum * jafuchs@phys.ethz.ch mechanical simulations in atoms [5,7,9,11,14,15], molecules [6,10,12,13], and solids [8,16].…”

Section: Introductionmentioning

confidence: 99%

Time delays from one-photon transitions in the continuum

Fuchs¹,

Douguet²,

Donsa³

et al. 2020

Optica

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Attosecond photoionisation time delays reveal information about the potential energy landscape an outgoing electron wavepacket probes upon ionisation. In this study we experimentally quantify, for the first time, the dependence of the time delay on the angular momentum of the liberated photoelectrons. For this purpose, electron quantum-path interference spectra have been resolved in energy and angle using a two-color attosecond pump-probe photoionisation experiment in helium. A fitting procedure of the angle-dependent interference pattern allows us to disentangle the relative phase of all four quantum pathways that are known to contribute to the final photoelectron signal. In particular, we resolve the dependence on the angular momentum of the delay of one-photon transitions between continuum states, which is an essential and universal contribution to the total photoionization delay observed in attosecond pump-probe measurements. For such continuumcontinuum transitions, we measure a delay between outgoing s-and d-electrons as large as 12 as close to the ionisation threshold in helium. Both single-active-electron and first-principles ab initio simulations confirm this observation for helium and hydrogen, demonstrating the universality of the observed delays.Recently, experimental evidence of a strong effect of the IR-induced cc-transitions on the angular dependence of the total photoemission delays has been reported [14,15] stimulating several independent investigations on the origin of this effect [21,[23][24][25][26][27]. In this work, arXiv:1907.03607v1 [physics.atom-ph]

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Section: Introductionmentioning

confidence: 99%

Time delays from one-photon transitions in the continuum

Fuchs¹,

Douguet²,

Donsa³

et al. 2020

Optica

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“…More recently, other authors have reported the first investigation of triatomic molecules for which the effect of a shape resonance were described in N 2 O, leading to a time delay of 160 as between the two outermost orbitals while a few attoseconds delay were observed in H 2 O in absence of the resonance [16,17]. Approaches combining RABBIT and coincidence measurements also allowed to investigate orientation dependent time delays [21,22], opening new avenues in this context. One of the advantages of the RABBIT technique is that the interference pattern arises from only 2 quantum paths.…”

Section: Introductionmentioning

confidence: 99%

High harmonic generation-2ω attosecond stereo-photoionization interferometry in N₂

et al. 2020

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We have investigated photoionization delays in N 2 by combining an extreme ultraviolet (XUV) attosecond pulse train generated by high harmonic generation (HHG) and a second harmonic femtosecond pulse with angularly resolved photoelectron spectroscopy. While photoionization delay measurements are usually performed by using a standard XUV-infrared scheme, here we show that the present approach allows us to separate electronic states that otherwise would overlap, thus avoiding the spectral congestion found in most molecules. We have found a relative delay between the X and A ionic molecular states as a function of the photon energy of up to 40 attoseconds, which is due to the presence of a shape resonance in the X channel. This approach can be applied to other small quantum systems with few active electronic states.

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“…Optical pulses with a sub-cycle duration are an appealing route to sculpt the temporal profile of electric fields E(t), which have a broad variety of prospective applications in strong-field physics, for example, in electron localization (2,3), relativistic laser-plasma interactions (4,5), plasma wakefield accelerators (6,7), and isolated attosecond pulse (IAP) generation. In particular for strong IAP generation, by overcoming the generated energy bottleneck for attosecond spectroscopy, sub-cycle pulses will definitely initiate a revolution (8,9) in chemical dynamics research (10,11). The most promising way to obtain a sub-optical-cycle pulse duration is to synthesize sub-pulses with different colors generated from separate sources (12).…”

Section: Introductionmentioning

confidence: 99%

Fully stabilized multi-TW optical waveform synthesizer: Toward gigawatt isolated attosecond pulses

Xue

Tamaru

et al. 2020

Sci. Adv.

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A stable 50 mJ three-channel optical waveform synthesizer is demonstrated and used to reproducibly generate a high-order harmonics supercontinuum in the soft-x-ray region. This synthesizer is composed of pump pulses from a 10-Hz-repetition-rate Ti:sapphire pump laser and signal and idler pulses from an infrared two-stage optical parametric amplifier driven by this pump laser. With the full active stabilization of all relative time delays, relative phases, and the carrier-envelope phase, a shot-to-shot stable intense continuum harmonic spectrum is obtained around 60 eV with pulse energy above 0.24 µJ. The peak power of the soft-x-ray continuum is evaluated to be beyond 1 GW with a 140 as transform limit duration. Furthermore, we found a characteristic delay dependence of the multi-cycle waveform synthesizer and established its control scheme. Compared with the one-color case, we experimentally observe an enhancement of the cut-off spectrum intensity by one to two orders of magnitude through the three-color waveform synthesis.

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Attosecond coupled electron and nuclear dynamics in dissociative ionization of H2

Cited by 131 publications

References 49 publications

Time delays from one-photon transitions in the continuum

Time delays from one-photon transitions in the continuum

High harmonic generation-2ω attosecond stereo-photoionization interferometry in N₂

Fully stabilized multi-TW optical waveform synthesizer: Toward gigawatt isolated attosecond pulses

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Attosecond coupled electron and nuclear dynamics in dissociative ionization of H2

Cited by 131 publications

References 49 publications

Time delays from one-photon transitions in the continuum

Time delays from one-photon transitions in the continuum

High harmonic generation-2ω attosecond stereo-photoionization interferometry in N2

Fully stabilized multi-TW optical waveform synthesizer: Toward gigawatt isolated attosecond pulses

Contact Info

Product

Resources

About

High harmonic generation-2ω attosecond stereo-photoionization interferometry in N₂