Ultrafast dissociation: An unexpected tool for probing molecular dynamics

Morin, Paul; Miron, Catalin

doi:10.1016/j.elspec.2012.06.002

Cited by 41 publications

(42 citation statements)

References 54 publications

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“…The kinetic energies of the resonant Auger electrons (for 1 S, 1 D and 3 P final states) were determined from the Cl + CIY from CH 3 Cl and were found to be approximately 177.3 eV, 179.3 eV and 180.7 eV, which are in good agreement with values reported earlier 8,48,49 .…”

Section: A1supporting

confidence: 79%

“…This distinction is an approximation, as in reality the system is only truly explained by a one-step process once the wave-packet dynamics and scattering times are on a similar time frame. 8 The time scale of molecular dissociation is rather sensitive to the masses of the constituent particles involved in the process. For example, in the case of increasing the mass of the neutral fragment by a factor of 15 (e.g.…”

Section: Introductionmentioning

confidence: 99%

“…For example, in the case of increasing the mass of the neutral fragment by a factor of 15 (e.g. when moving from HCl to CH 3 Cl) and assuming rigid motion of fragments, dissociation is expected to slow down considerably, 8,9 which in turn promotes competing molecular decay (i.e. electronic relaxation that takes place before nuclear rearrangement).…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Role of ultrafast dissociation in the fragmentation of chlorinated methanes

Kokkonen

Jänkälä

Patanen

et al. 2018

The Journal of Chemical Physics

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Photon-induced fragmentation of a full set of chlorinated methanes (CH3Cl, CH2Cl2, CHCl3, CCl4) has been investigated both experimentally and computationally. Using synchrotron radiation and electron-ion coincidence measurements, the dissociation processes were studied after chlorine 2p electron excitation. Experimental evidence for CH3Cl and CH2Cl2 contains unique features suggesting that fast dissociation processes take place. By contrast, CHCl3 and CCl4 molecules do not contain the same features, hinting that they experience alternative mechanisms for dissociation and charge migration. Computational work indicates differing rates of charge movement after the core-excitation, which can be used to explain the differences observed experimentally.

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Section: A1supporting

confidence: 79%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Role of ultrafast dissociation in the fragmentation of chlorinated methanes

Kokkonen

Jänkälä

Patanen

et al. 2018

The Journal of Chemical Physics

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“…Nowadays the acronym Ultra-Fast Dissociation (UFD) is commonly used to describe the dissociation taking place before the electronic de-excitation. A recent review by Morin and Miron [65] gives a historical perspective on the topic and summarizes a number of recent advances.…”

Section: Resonant Photoemissionmentioning

confidence: 99%

Electron spectroscopy using ultra brilliant synchrotron X-ray sources

Patanen

Svensson

Mårtensson

2015

Journal of Electron Spectroscopy and Related Phenomena

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Electron spectroscopy using ultra brilliant synchrotron X-ray sources. Journal of Electron Spectroscopy and Related AbstractThe development of photoelectron spectroscopy since the early days of the technique is discussed. The focus is on the interaction between instrumental development and scientific achievements. In particular the opportunities provided by the increasingly brilliant synchrotron radiation sources are discussed. The contribution is focused on core level studies. The recent development is demonstrated by using selected examples obtained at today´s most advanced synchrotron radiation facilities. The spectral resolution and intensity that can be reached at these facilities reveal new effects and provide detailed information on the investigated systems. The examples are mainly taken from studies of atoms and molecules where different effects can be most accurately identified and separated.2

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“…The narrow resonance near Á@! % À12:2 eV is the so-called atomic peak [3,24] related to the decay of the core-excited isolated oxygen atom following dissociation [11] (Fig. 2).…”

mentioning

confidence: 99%

Interference between Resonant and Nonresonant Inelastic X-Ray Scattering

et al. 2013

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A detailed study of inelastic x-ray scattering from the ground state to the 3 AE g ð3 À1 g 3s 1 g Þ state of the O 2 molecule is presented. The observed angular anisotropy shows that the vibrational excitations within this final state are strongly dependent on the polarization of the incident radiation. The analysis demonstrates that this is a manifestation of interference between resonant and direct nonresonant inelastic x-ray scattering. This interference provides a new tool to monitor nuclear dynamics by relative rotation of the polarization vectors of the incident and scattered photons. DOI: 10.1103/PhysRevLett.110.223001 PACS numbers: 33.20.Rm, 32.80.Aa, 33.20.Fb, 33.80.Gj The nonresonant scattering channel has so far been neglected when considering resonant inelastic scattering (RIXS) in the sub-keV range. On the other hand, the direct nonresonant (Thomson) scattering channel significantly contributes to resonant elastic scattering [1][2][3][4][5]. Nonresonant inelastic x-ray scattering (NIXS) is prominent in the hard x-ray range, and is exploited in well-established materials science methods [6][7][8][9]. To the best of our knowledge, however, a demonstration of the influence of the nonresonant channel on resonant inelastic scattering phenomena is lacking also for hard x rays.Here we show that NIXS influences scattering deep in the soft x-ray range, in the spectrum of the O 2 molecule excited at the 1s ! Ã resonance [10][11][12]. NIXS interference with the RIXS channel is reflected in the polarization dependence of vibrational excitations within a welldefined electronic final state. This phenomenology is an indication of NIXS-RIXS interference because the NIXS and RIXS channels have different polarization dependence and induce different nuclear dynamics. The observed angular anisotropy is pronounced, demonstrating that NIXS-RIXS interference is important in this case and suggesting that NIXS should be considered when analyzing state-ofthe-art resonant x-ray scattering spectra in general.The observed polarization dependence of the vibrational excitations is a consequence of NIXS-RIXS interference and does not indicate that the Born-Oppenheimer approximation is violated. In spite of the formal analogy with the interference between the resonant channel and the channel of nonresonant direct ionization in resonant Auger scattering, there is a qualitative difference between the two processes. The interference between the resonant channel and the channel of direct ionization is a typical non-BornOppenheimer effect [13][14][15][16]. Here the final state wave function cannot be written as a product of electronic and nuclear wave functions due to the mixing between the degenerate autoionizing core-excited state and the continuum state in which it is embedded. The picture is qualitatively different for x-ray Raman scattering where the energy spacing between the final and the core-excited state is very large (% 524 eV). In the absence of external fields, the nuclear motion in the gerade final state is independent...

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Ultrafast dissociation: An unexpected tool for probing molecular dynamics

Cited by 41 publications

References 54 publications

Role of ultrafast dissociation in the fragmentation of chlorinated methanes

Role of ultrafast dissociation in the fragmentation of chlorinated methanes

Electron spectroscopy using ultra brilliant synchrotron X-ray sources

Interference between Resonant and Nonresonant Inelastic X-Ray Scattering

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