High-order above-threshold dissociation of molecules

Lu, Peifen; Wang, Junping; Li, Hui; Lin, Kang; Gong, Xiaochun; Song, Qiying; Ji, Qinying; Zhang, Wenbing; Ma, Jing; Li, Hanxiao; Zeng, Heping; He, Feng; Wu, Jian

doi:10.1073/pnas.1719481115

Cited by 33 publications

(19 citation statements)

References 37 publications

(48 reference statements)

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“…Figure 2d, f present the total energy spectra E sum of the (H + , H * ) and (H + , H + ) channels accessed via the direct and one-photon pathways, respectively. The discrete ATI (above threshold ionization) peaks spaced by the photon energy in the E sum spectrum imprint the quantized nature of the light energy, which allows us to reveal the total number of photons absorbed by the molecule 42,43 .…”

Section: Resultsmentioning

confidence: 99%

Electron-nuclear correlated multiphoton-route to Rydberg fragments of molecules

Zhang

Gong

et al. 2019

Nat Commun

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Atoms and molecules exposed to strong laser fields can be excited to the Rydberg states with very high principal quantum numbers and large orbitals. It allows acceleration of neutral particles, generate near-threshold harmonics, and reveal multiphoton Rabi oscillations and rich photoelectron spectra. However, the physical mechanism of Rydberg state excitation in strong laser fields is yet a puzzle. Here, we identify the electron-nuclear correlated multiphoton excitation as the general mechanism by coincidently measuring all charged and neutral fragments ejected from a H2 molecule. Ruled by the ac-Stark effect, the internuclear separation for resonant multiphoton excitation varies with the laser intensity. It alters the photon energy partition between the ejected electrons and nuclei and thus leads to distinct kinetic energy spectra of the nuclear fragments. The electron-nuclear correlation offers an alternative visual angle to capture rich ultrafast processes of complex molecules.

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Section: Resultsmentioning

confidence: 99%

Electron-nuclear correlated multiphoton-route to Rydberg fragments of molecules

Zhang

Gong

et al. 2019

Nat Commun

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“…We show the ion fragment energy is driven by Coulomb explosion and the internuclear separation at which ionization occurs during the dissociation of the molecule. At first multiple effects such as alignment [38], multiple fragmentation channels [31], wavepacket dynamics on multiple electronic states [39], rescattering [40], nonsequential double ionization [41], and other effects could seem to give a complex, if not uninterpretable spectra. Despite this, we show there is a clear and analytical predictability.…”

Section: Introductionmentioning

confidence: 99%

Molecular ionization of chloromethane in strong fields: nearest neighbor gateway to highly charged ions

Grugan

Ekanayake

White

et al. 2018

J. Phys. B: At. Mol. Opt. Phys.

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The strong and ultrastrong field-molecule interaction is a complex, many-body process involving multiple ionization processes. We present ion yields and molecular fragment energies for the ionization of chloromethane (CH 3 Cl) in a laser field with intensities spanning from 10 14 to 10 17 W cm −2 . As the laser intensity increases, ionization of CH 3 Cl is observed to pass from molecular tunneling, to enhanced ionization (EI), to an atomic-like response. The energy spectra of the ions show no dependence on the intensity and has its source in dissociative molecular ionization. A classical model of an aligned C-Cl ion is used to model the interaction. Following an initial molecular ionization process, our results show EI is a driving influence in the formation of low charge states until ionization become atomic-like and involves tightly bound ion states whose ionization is unaffected by nearest neighbor ions of similar ion charge.

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“…Intense light can couple nuclear and electron dynamics leading to hallmark phenomena of molecular strong-field physics such as correlated electron-nuclear energy sharing [1][2][3], bond softening [4], bond hardening [5], abovethreshold dissociation [2,6,7], light-induced conical and nonconical intersections [8,9], and enhanced ionization [10,11], all of which have been extensively studied in the hydrogen molecule H 2 (see, e.g., Refs. [12][13][14][15], and references therein).…”

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confidence: 99%

“…(1) The molecule is singly ionized by absorption of more than 10 NIR photons and a bound molecular ion is created (bound ionization, BI). (2) The bond between the two nuclei stretches, and the molecule absorbs three additional photons at the internuclear distance R 1 and dissociates along the 2pσ u state. (3) The molecule emits one photon at R 2 and breaks up into a singly charged ion and a neutral atom, via ATD [net two-photon pathway, shown by blue arrows in Fig.…”

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Clocking Enhanced Ionization of Hydrogen Molecules with Rotational Wave Packets

Peng

Camus

et al. 2020

Phys. Rev. Lett.

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Laser-induced rotational wave packets of H 2 and D 2 molecules were experimentally measured in real time by using two sequential 25-fs laser pulses and a reaction microscope. By measuring the timedependent yields of the above-threshold dissociation and the enhanced ionization of the molecule, we observed a few-femtosecond time delay between the two dissociation channels for both H 2 and D 2. The delay was interpreted and reproduced by a classical model that considers enhanced ionization and thus additional interaction within the laser pulse. We demonstrate that by accurately measuring the phase of the rotational wave packet in hydrogen molecules we can resolve dissociation dynamics which is occurring within a fraction of a molecular rotation. Such a rotational clock is a general concept applicable to sequential fragmentation processes in other molecules.

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High-order above-threshold dissociation of molecules

Cited by 33 publications

References 37 publications

Electron-nuclear correlated multiphoton-route to Rydberg fragments of molecules

Electron-nuclear correlated multiphoton-route to Rydberg fragments of molecules

Molecular ionization of chloromethane in strong fields: nearest neighbor gateway to highly charged ions

Clocking Enhanced Ionization of Hydrogen Molecules with Rotational Wave Packets

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