Evidence for Coulomb Explosion of Doubly Charged Microclusters

Sattler, K.; Mühlbach, J.; Echt, Olof; Pfau, P.; Recknagel, E.

doi:10.1103/physrevlett.47.160

Cited by 309 publications

(102 citation statements)

References 22 publications

Supporting

Mentioning

Contrasting

Unclassified

Order By: Relevance

“…Evidence for their dissociation was first observed by Sattler et al who, by measuring the mass and charge of Pb, Xe, and NaI clusters, observed half-integer cluster numbers that were interpreted to be doubly charged clusters [4]. It was found that the cluster size necessary to support two charges is much higher for Xe than for Pb or NaI due to the much weaker intermolecular attraction in Xe.…”

mentioning

confidence: 92%

“…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].…”

mentioning

confidence: 99%

See 1 more Smart Citation

Gas-phase dissociation pathways of multiply charged peptide clusters

Jurchen

García

Williams

2003

J. Am. Soc. Mass Spectrom.

View full text Add to dashboard Cite

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 ...

show abstract

mentioning

confidence: 92%

mentioning

confidence: 99%

Gas-phase dissociation pathways of multiply charged peptide clusters

Jurchen

García

Williams

2003

J. Am. Soc. Mass Spectrom.

View full text Add to dashboard Cite

show abstract

“…The observed fragment spectrum is, within statistical error, independent of the temperature T of the parent cluster for T ≤ 1500 K. These findings are consistent with and explain recent trends observed experimentally. Starting with the work of Sattler et al [1] on van der Waal's clusters, the study of the fragmentation (fission) of charged atomic or molecular clusters has proved a valuable experimental tool for investigating the intrinsic stability and binding forces of these objects. These studies and others yield important insights into the behavior of matter at the small size limit and the size-dependent evolution toward bulk properties.…”

mentioning

confidence: 99%

Charge-Induced Fragmentation of Sodium Clusters

et al. 2001

View full text Add to dashboard Cite

The fission of highly charged sodium clusters with fissilities X > 1 is studied by ab initio molecular dynamics. Na244+ is found to undergo predominantly sequential Na3 + emission on a time scale of 1 ps, while Na24 Q+ (5 ≤ Q ≤ 8) undergoes multifragmentation on a time scale ≥ 0.1 ps, with Na + increasingly the dominant fragment as Q increases. All singly-charged fragments Nan + up to size n = 6 are observed. The observed fragment spectrum is, within statistical error, independent of the temperature T of the parent cluster for T ≤ 1500 K. These findings are consistent with and explain recent trends observed experimentally. 36.40.Qv, 36.40.Wa, 31.15.Qg, 31.15.Ew Starting with the work of Sattler et al.[1] on van der Waal's clusters, the study of the fragmentation (fission) of charged atomic or molecular clusters has proved a valuable experimental tool for investigating the intrinsic stability and binding forces of these objects. These studies and others yield important insights into the behavior of matter at the small size limit and the size-dependent evolution toward bulk properties. Much recent work on fission has been devoted to metallic clusters, both experimentally [2][3][4][5][6][7][8][9][10][11] and theoretically [4,9,[12][13][14][15][16]. Fission of metallic clusters is particularly interesting on account of the similarities and differences with the nuclear fission process [12]. Over a century ago, Lord Rayleigh [17] studied the problem of the time development of the Coulomb instability of a surface-charged liquid drop, and conjectured that the excess charge would be removed by the emission of jets, rather than by fission into two parts of more or less equal size (as occurs for nuclei, where the charge is distributed uniformly through the volume).According to the Rayleigh criterion [17], a charged liquid drop is unstable against Coulomb forces when its fissility X > 1, where X = E Coul /(2E surf ) is proportional to the ratio of the Coulomb to surface energy of the drop. For a metallic cluster M N Q+ , assumed spherical with radius r s N 1/3 (r s is the Wigner-Seitz radius for the metal), this gives X = (16πr 3 s σ) −1 Q 2 /N , where σ is the surface tension, or X ≈ 2.5Q 2 /N for Na N Q+ . Now, fission experiments on metallic clusters where the cluster is charged by laser ionization [2][3][4][5][6][7] have so far produced only clusters with X < 1, for which an energy barrier exists against fission. Thermally activated fission may be observed, however, and the dominant charged fragment is found to be Na 3 + , which has a closed electronic shell and is particularly stable; Na + has not so far been observed. In a different type of experiment [8][9][10][11], sodium clusters are ionized by collision with a beam of highly charged ions, a technique that is expected to allow study of a much wider range of X and cluster temperatures. Coincidence measurements reveal multifragmentation processes in some cases, often with Na + as the dominant fragment. In this Letter, we offer the first systematic dynamical study ...

show abstract

“…Since the work of Sattler et al [22], massspectrometric investigations of the charging effects in cluster beams have clearly demonstrated the sizedependent Coulomb instability of clusters composed of a countable number of atoms [23,24,25].…”

Section: Introductionmentioning

confidence: 99%

Energetics of metal slabs and clusters: The rectangular-box model

2005

View full text Add to dashboard Cite

An expansion of energy characteristics of wide thin slab of thickness L in power of 1/L is constructed using the free-electron approximation and the model of a potential well of finite depth. Accuracy of results in each order of the expansion is analyzed. Size dependences of the work function and electronic elastic force for Au and Na slabs are calculated. It is concluded that the work function of low-dimensional metal structure is always smaller that of semi-infinite metal sample.A mechanism for the Coulomb instability of charged metal clusters, different from Rayleigh's one, is discussed. The two-component model of a metallic cluster yields the different critical sizes depending on a kind of charging particles (electrons or ions). For the cuboid clusters, the electronic spectrum quantization is taken into account. The calculated critical sizes of Ag 2− N and Au 3− N clusters are in a good agreement with experimental data. A qualitative explanation is suggested for the Coulomb explosion of positively charged Na n+ N clusters at 3≤ n ≤5.

show abstract

Evidence for Coulomb Explosion of Doubly Charged Microclusters

Cited by 309 publications

References 22 publications

Gas-phase dissociation pathways of multiply charged peptide clusters

Gas-phase dissociation pathways of multiply charged peptide clusters

Charge-Induced Fragmentation of Sodium Clusters

Energetics of metal slabs and clusters: The rectangular-box model

Contact Info

Product

Resources

About