Formation of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mmultiscripts><mml:mi mathvariant="normal">H</mml:mi><mml:mn>3</mml:mn><mml:none /><mml:none /><mml:mo>+</mml:mo></mml:mmultiscripts></mml:math>due to Intramolecular Bond Rearrangement in Doubly Charged Methanol

De, Sankar; Rajput, Jyoti; Roy, A.; Ghosh, Pradip N.; Safvan, C. P.

doi:10.1103/physrevlett.97.213201

Cited by 61 publications

(35 citation statements)

References 13 publications

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“…This combined dynamics is also correctly captured by the simulations, illustrated also by the two animations given as Supplemental Material [32]. Hydrogen migration in similar molecules has also been observed in other contexts [13,33].…”

Section: A Ring Breakup Patterns and Hydrogen Dynamicssupporting

confidence: 48%

Internal energy dependence in x-ray-induced molecular fragmentation: An experimental and theoretical study of thiophene

Kukk

Wang

et al. 2015

Phys. Rev. A

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A detailed experimental and theoretical investigation of the dynamics leading to fragmentation of doubly ionized molecular thiophene is presented. Dissociation of double-ionized molecules was induced by S 2p core photoionization and the ionic fragments were detected in coincidence with Auger electrons from the core-hole decay. Rich molecular dynamics was observed in electron-ion-ion coincidence maps exhibiting ring breaks accompanied by hydrogen losses and/or migration. The probabilities of various dissociation channels were seen to be very sensitive to the internal energy of the molecule. Theoretical simulations were performed by using the semiempirical self-consistent charge-density-functional tight-binding method. By running thousands of these simulations, the initial conditions encountered in the experiment were properly taken into account, including the systematic dependencies on the internal (thermal) energy. This systematic approach, not affordable with first-principle methods, provides a good overall description of the complex molecular dynamics observed in the experiment and shows good promise for applicability to larger molecules or clusters, thus opening the door to systematic investigations of complex dynamical processes occurring in radiation damage.

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Section: A Ring Breakup Patterns and Hydrogen Dynamicssupporting

confidence: 48%

Internal energy dependence in x-ray-induced molecular fragmentation: An experimental and theoretical study of thiophene

Kukk

Wang

et al. 2015

Phys. Rev. A

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“…Ion-induced bond rearrangement processes have been observed before for, e.g., highly charged ions colliding on single molecules [30]. In this Letter we have shown that keV ions may induce very efficient routes to molecular growth processes when such rearrangement processes involve other molecules inside a cluster.…”

Section: H Y S I C a L R E V I E W L E T T E R S Week Ending 3 May 2013mentioning

confidence: 66%

Formations of DumbbellC118andC119inside Clusters ofC60
Zettergren
¹
,
Rousseau
²
,
Wang
³

et al. 2013
Phys. Rev. Lett.
65
2
48
0
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We report highly selective covalent bond modifications in collisions between keV alpha particles and van der Waals clusters of C 60 fullerenes. Surprisingly, C 119 þ and C 118 þ are the dominant molecular fusion products. We use molecular dynamics simulations to show that C 59 þ and C 58 þ ions-effectively produced in prompt knockout processes with He 2þ -react rapidly with C 60 to form dumbbell C 119 þ and C 118 þ . Ion impact on molecular clusters in general is expected to lead to efficient secondary reactions of interest for astrophysics. These reactions are different from those induced by photons. DOI: 10.1103/PhysRevLett.110.185501 PACS numbers: 61.48.Àc, 31.15.xv, 36.40.Qv Photodriven intracluster reactions have been observed in clusters of fullerenes [1,2] and in, e.g., clusters of methanol, water, dimethyl ether, and acetic acid molecules [3]. Clusters of fullerenes are of particular interest in this context as C 60 and C 70 recently have been observed in space [4,5] at temperatures indicating that they may reside on grains [4] or are in the solid phase (fullerite) [6]. The question of how fullerenes form in space and elsewhere [7][8][9] is still open and here we report experimental observations on specific very efficient fullerene growth processes inside small pieces of fullerite material. These ion-impact induced growth processes in which so-called dumbbell fullerene systems are formed are inherently different from the ones induced by photons [1,2] for reasons that will be discussed in the following.The lowest energy barrier for formation of covalently bound dumbbell C 120 from two neutral C 60 molecules is roughly one or two electron volts [10]. Thus, two C 60 molecules in their ground states may, in principle, form such a C 120 system when the center-of-mass kinetic energy is larger than this barrier. However, molecular dynamics simulations by Jakowski, Irle, and Morokuma [11] have shown that, in practice, much larger kinetic energies are needed to form dumbbell C 120 (* 60 eV) or single-cage C 120 (*100 eV) efficiently [11]. The reason is that at least one C 60 cage needs to rearrange to form covalent bonds with the other cage on very short, picosecond, time scales. This is highly unlikely in a single encounter at low kinetic energy, as the transferred energy is redistributed over the fullerene molecule and a critical energy needs to be localized in a specific bond in order to break it. On the other hand, the reverse reaction (dissociation) may proceed at much lower energies but after many vibrations and on much longer time scales. For C 60 -C 60 collisions at kinetic energies above 60/100 eV covalent bond formation becomes much more likely but will then also give internally hot dumbbell/single-cage C 120 . Single-cage C 120 will fragment through sequences of C 2 emissions yielding molecular mass distributions with an even number of carbon atoms [1] as C 2 loss is the lowest-energy dissociation channel at about 10 eV. The dumbbell C 120 ! C 60 þ C 60 dissociation energy is only a couple of eV [1...

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“…Several aspects of ion-impact molecular dissociation have been addressed using these powerful instruments, such as limitations of the Coulomb explosion model to reproduce molecular fragmentation dynamics [4], orientation effects in multiple ionization of molecules by fast ions [5] and studies on intra-molecular bond rearrangements in ion-molecule collisions [6].…”

Section: Introductionmentioning

confidence: 99%

Setup for measuring angular anisotropies in slow ion-molecule collisions

Kumar

Rajput

Sairam

et al. 2014

International Journal of Mass Spectrometry

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Formation ofH3+due to Intramolecular Bond Rearrangement in Doubly Charged Methanol

Cited by 61 publications

References 13 publications

Internal energy dependence in x-ray-induced molecular fragmentation: An experimental and theoretical study of thiophene

Internal energy dependence in x-ray-induced molecular fragmentation: An experimental and theoretical study of thiophene

Formations of DumbbellC118andC119inside Clusters ofC60
Zettergren
¹
,
Rousseau
²
,
Wang
³

et al. 2013
Phys. Rev. Lett.
65
2
48
0
View full text Add to dashboard Cite

Setup for measuring angular anisotropies in slow ion-molecule collisions

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Formation ofH3+due to Intramolecular Bond Rearrangement in Doubly Charged Methanol

Cited by 61 publications

References 13 publications

Internal energy dependence in x-ray-induced molecular fragmentation: An experimental and theoretical study of thiophene

Internal energy dependence in x-ray-induced molecular fragmentation: An experimental and theoretical study of thiophene

Formations of DumbbellC118andC119inside Clusters ofC60Zettergren1, Rousseau2, Wang3 et al. 2013Phys. Rev. Lett.652480View full textAdd to dashboardCite

Setup for measuring angular anisotropies in slow ion-molecule collisions

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About

Formations of DumbbellC118andC119inside Clusters ofC60
Zettergren
¹
,
Rousseau
²
,
Wang
³

et al. 2013
Phys. Rev. Lett.
65
2
48
0
View full text Add to dashboard Cite