Beyond the Rayleigh instability limit for multicharged finite systems: From fission to Coulomb explosion

Levy, Yaakov; Jortner, Joshua

doi:10.1073/pnas.142253999

Cited by 78 publications

(66 citation statements)

References 44 publications

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“…In the case of multiply charged clusters, the two competing processes for dissociation are the evaporation of a neutral atom or molecule and the ejection of charged subunits. The latter occurs through a fission process in which the cluster dissociates into two or three charged fragments that then separate due to coulombic repulsion [41]. The competing processes of evaporation and fission have been described by various liquid-drop models for clusters as diverse as atomic nuclei [42], multiply charged metal clusters [5,6], and highly charged solvent droplets [2,3].…”

Section: Nih-pa Author Manuscriptmentioning

confidence: 99%

Gas-phase dissociation pathways of multiply charged peptide clusters

Jurchen

García

Williams

2003

J. Am. Soc. Mass Spectrom.

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Numerous studies of cluster formation and dissociation have been conducted to determine properties of matter in the transition from the condensed phase to the gas phase using materials as diverse as atomic nuclei, noble gasses, metal clusters, and amino acids. Here, electrospray ionization is used to extend the study of cluster dissociation to peptides including leucine enkephalin with 7-19 monomer units and 2-5 protons, and somatostatin with 5 monomer units and 4 protons under conditions where its intramolecular disulfide bond is either oxidized or reduced. Evaporation of neutral monomers and charge separation by cluster fission are the competing dissociation pathways of both peptides. The dominant fission product for all leucine enkephalin clusters studied is a proton-bound dimer, presumably due to the high gas-phase stability of this species. The branching ratio of the fission and evaporation processes for leucine enkephalin clusters appears to be determined by the value of z 2 /n for the cluster where z is the charge and n the number of monomer units in the cluster. Clusters with low and high values of z 2 /n dissociate primarily by evaporation and cluster fission respectively, with a sharp transition between dissociation primarily by evaporation and primarily by fission measured at a z 2 /n value of ~0.5. The dependence of the dissociation pathway of a cluster on z 2 /n is similar to the dissociation of atomic nuclei and multiply charged metal clusters indicating that leucine enkephalin peptide clusters exist in a state that is more disordered, and possibly fluid, rather than highly structured in the dissociative transition state. The branching ratio, but not the dissociation pathway of [somatostatin 5 + 4H] 4+ is altered by the reduction of its internal disulfide bond indicating that monomer conformational flexibility plays a role in peptide cluster dissociation.Bulk properties of matter and the properties of isolated gas-phase atoms and molecules can have radically different characteristics in terms of structure, work function, ion solvation, etc. (for a review see reference [1]). One motivation behind cluster research is that the transitional characteristics between bulk and molecular properties can be discovered by studying intermediate states of matter. Investigators have explored a wide variety of materials, including charged droplets of various liquids [2,3], clusters of noble metals [4][5][6][7][8], metal-ligand clusters [1,[9][10][11], highly charged clusters of noble gasses [12,13], small molecules [14,15], and ultracold clusters of transition metals [16]. Recently, investigators have formed noncovalently bound clusters of biologically important molecules, including clusters of amino acids and small peptides [17][18][19][20][21][22][23][24][25][26][27][28], and have studied their dissociation processes [18,20,[26][27][28]. Multiply charged "clusters" of proteins consisting of multimeric, noncovalently associated protein complexes with a high degree of solution-phase structural specificity ...

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Section: Nih-pa Author Manuscriptmentioning

confidence: 99%

Gas-phase dissociation pathways of multiply charged peptide clusters

Jurchen

García

Williams

2003

J. Am. Soc. Mass Spectrom.

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“…In the following, we can introduce the 'recorded cluster size' as the sum of the fragment cluster sizes before unimolecular evaporation has occurred (see Figure 4a). The possible difference in produced and observed sizes is due to neutral fragment formation during break-up, as is predicted by classical molecular dynamics calculations on Morse clusters, 42 or the fast 'boiling off' of monomers 26 before break-up.…”

Section: Breakup Into Protonated Fragmentsmentioning

confidence: 90%

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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“…These dynamic studies were extended for the adiabatic nuclear dynamics of multicharged atomic and molecular clusters (129,130), which manifest unique fragmentation patterns, such as cluster fission and Coulomb explosion. We addressed (130) unifying features of fragmentation channels driven by Coulomb instabilities in clusters, nuclei, droplets, and spectral molasses, demonstrating that the Rayleigh stability limit X = E(Coulomb)/2E(surface) = 1 separates between spatially anisotropic fission (X < 1) and spatially isotropic Coulomb explosion (X > 1).…”

Section: From Dynamics Of Large Finite Systems To Ultracold Cloudsmentioning

confidence: 99%

REFLECTIONS ON PHYSICAL CHEMISTRY: Science and Scientists

Jortner

2006

Annu. Rev. Phys. Chem.

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Key Words physical chemistry in Israel, radiationless transitions, chemical and biological electron transfer, dynamics of finite systems, structure-dynamics-function relations ■ Abstract This is the story of a young person who grew up in Tel-Aviv during the period of the establishment of the State of Israel and was inspired to become a physical chemist by the cultural environment, by the excellent high-school education, and by having been trained by some outstanding scientists at the Hebrew University of Jerusalem and, subsequently, by the intellectual environment and high-quality scientific endeavor at the University of Chicago. Since serving as the first chairman of the Chemistry Department of the newly formed Tel-Aviv University he has been immersed in research, in the training of young scientists, and in intensive and extensive international scientific collaboration. Together with the members of his "scientific family" he has explored the phenomena of energy acquisition, storage and disposal and structure-dynamics-function relations in large molecules, condensed phase, clusters and biomolecules, and is looking forward to many future adventures in physical chemistry. "What to leave out and what to put in? That

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Beyond the Rayleigh instability limit for multicharged finite systems: From fission to Coulomb explosion

Cited by 78 publications

References 44 publications

Gas-phase dissociation pathways of multiply charged peptide clusters

Gas-phase dissociation pathways of multiply charged peptide clusters

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

REFLECTIONS ON PHYSICAL CHEMISTRY: Science and Scientists

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