Evidence of ultra-fast dissociation in ammonia observed by resonant Auger electron spectroscopy

Hjelte, I.; Piancastelli, M. N.; Jansson, C.; Wiesner, Karoline; Björneholm, Olle; Bäßler, M.; Sorensen, S. L.; Svensson, S.

doi:10.1016/s0009-2614(03)00161-1

Cited by 35 publications

(78 citation statements)

References 33 publications

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“…Similar findings have been reported for ammonia, where the ultrafast dissociation has been shown to lead to the NH 2 core-excited fragment. 27 However, we do not exclude the possibility that in the upper limit of the explored photon energy range further fragmentation can occur (see discussion below about Fig. 4).…”

Section: Resultsmentioning

confidence: 85%

Ultrafast dynamics in C 1s core-excited CF4 revealed by two-dimensional resonant Auger spectroscopy

Piancastelli

Guillemin

Simon

et al. 2013

The Journal of Chemical Physics

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Following core excitation in an isolated molecule, ultrafast dissociation of one particular chemical bond can occur, where "ultrafast" is defined as taking place during the lifetime of the core hole, of the order of few femtoseconds. The signature of such phenomenon can be observed in resonant Auger spectra following core excitation. We present here an investigation of ultrafast dissociation following C 1s-to-σ * core excitation in CF 4 , with high-resolution resonant Auger spectroscopy. We are able to characterize final states of both the molecular ion and the CF + 3 fragment. We use twodimensional (2D) maps to record resonant Auger spectra across the resonance as a function of photon energy and to characterize ultrafast dynamics. This method provides immediate visual evidence of one of the important characteristics of the study of spectral features related to molecular versus fragment ionic final states, and namely their dispersion law. In the 2D maps we are also able to identify the dissociation limit for one of the molecular final states. © 2013 AIP Publishing LLC.

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Section: Resultsmentioning

confidence: 85%

Ultrafast dynamics in C 1s core-excited CF4 revealed by two-dimensional resonant Auger spectroscopy

Piancastelli

Guillemin

Simon

et al. 2013

The Journal of Chemical Physics

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“…[11][12][13][14][15][16] Using the core-hole life time as an internal clock, which can be "accelerated" by detuned excitation, it was shown that it is possible to derive information about vibronic coupling 12,15,16 as well as ultrafast dissociation processes. [12][13][14] In the case of liquids, an influence of the (hydrogen-bonding) environment on the vibronic structure as well as on dissociation processes can be expected.…”

Section: Introductionmentioning

confidence: 99%

Nuclear dynamics in the core-excited state of aqueous ammonia probed by resonant inelastic soft x-ray scattering

et al. 2011

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The electronic structure of aqueous NH 3 and ND 3 has been investigated using resonant inelastic soft x-ray scattering. Spectral features of different processes involving nuclear dynamics in the core-excited state can be identified. When exciting into the lowest core-excited state, we find a strong isotope effect and clear evidence for ultrafast proton dynamics. Furthermore, a strong vibronic coupling is observed and, in the case of aqueous NH 3 , a vibrational fine structure can be resolved.

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“…It is theoretically predicted 55 that the first repulsive electronic state with two single charges residing on neighboring molecules, NH + 3 (2 a -1 1 ) -NH + 3 (2 a -1 1 ), lie at 24.7 eV. When the photon energy is below the N1s edge, photoionization of the 2a 1 molecular orbital (26.8 eV 56 ) may lead, via auto-ionization, to repulsive states that are energy-allowed. Direct double ionization can also occur, leading to the production of two holes (2e −2 , 2e −1 3a −1 1 or 3a −2 1 ) on a single molecule, and may transfer a proton to a neighboring site, within typically 200 fs.…”

Section: Breakup Into Unprotonated Fragmentsmentioning

confidence: 99%

The role of charge and proton transfer in fragmentation of hydrogen-bonded nanosystems: the breakup of ammonia clusters upon single photon multi-ionization

Oostenrijk

Walsh

Laksman

et al. 2018

Phys. Chem. Chem. Phys.

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The charge and proton dynamics in hydrogen-bonded networks are investigated using ammonia as a model system. The fragmentation dynamics of medium-sized clusters (1-2 nm) upon single photon multi-ionization is studied, by analyzing the momenta of small ionic fragments. The observed fragmentation pattern of the doubly-and triply-charged clusters reveals a spatial anisotropy of emission between fragments (back-to-back). Protonated fragments exhibit a distinct kinematic correlation, indicating a delay between ionization and fragmentation (fission). The different kinematics observed for channels containing protonated and unprotonated species provides possible insights into the prime mechanisms of charge and proton transfer, as well as proton hopping, in such a nanoscale system.

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Evidence of ultra-fast dissociation in ammonia observed by resonant Auger electron spectroscopy

Cited by 35 publications

References 33 publications

Ultrafast dynamics in C 1s core-excited CF4 revealed by two-dimensional resonant Auger spectroscopy

Ultrafast dynamics in C 1s core-excited CF4 revealed by two-dimensional resonant Auger spectroscopy

Nuclear dynamics in the core-excited state of aqueous ammonia probed by resonant inelastic soft x-ray scattering

The role of charge and proton transfer in fragmentation of hydrogen-bonded nanosystems: the breakup of ammonia clusters upon single photon multi-ionization

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