International Journal of Mass Spectrometry 358 (2014) 36–42
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International Journal of Mass Spectrometry
jou rn al h om epage: www.elsevier.com/locate/ijms
Generation of multiply charged tin and carbon ions in low intensity
Coulomb explosion of tetramethyl tin clusters: Role of screening
effects
Purav M. Badani, Soumitra Das, Pramod Sharma, Rajesh K. Vatsa
∗
Chemistry Division, Bhabha Atomic Research Centre, Mumbai 400 085, India
a r t i c l e i n f o
Article history:
Received 24 July 2013
Received in revised form
10 November 2013
Accepted 10 November 2013
Available online 18 November 2013
Keywords:
Coulomb explosion
Molecular clusters
Tetramethyl tin
Time-of-flight mass spectrometry
Screening effects
a b s t r a c t
Present work reports multiple ionization and subsequent Coulomb explosion of tetramethyl tin clusters
induced by gigawatt intensity laser pulses. The time-of-flight mass spectra and charge density mea-
surements revealed that the efficiency of laser–cluster interaction depends on ionization wavelength.
Extent of energy absorbed from optical pulses by the cluster medium was found to increase with laser
wavelength. Experimental results obtained in the present study have been rationalized on the basis of
three stage cluster ionization model, i.e. multiphoton ionization ignited – inverse bremsstrahlung heating
(IBS) – electron ionization. In addition to the experiments, theoretical calculations have been performed
to account for screening effects in clusters. Our calculations suggest that the charged particles, generated
upon initial multiphoton ionization of cluster constituents, significantly lower the Coulombic barrier of
atoms/molecules that are present in its vicinity. This, in turn, decreases the ionization energy of cluster
constituents, during subsequent steps of ionization, ultimately increasing the ionization level of clusters
via the process of enhanced ionization due to ion shielding. Thus, above calculations predict dominant
role of screening effects in evolution of higher charge state atomic ions during laser–cluster interaction.
© 2013 Elsevier B.V. All rights reserved.
1. Introduction
Clusters undergo Coulomb explosion upon interacting with
highly energetic electrons [1], particles [2] or photons [3,4]. This
phenomenon occurs due to extensive stripping of electrons from
constituent atoms/molecules of clusters resulting in buildup of
excessive positive charge on cluster. When the repulsive Coulom-
bic energy of clusters, arising from positive charges, overcomes
the total cohesive energy, cluster disintegrates violently result-
ing in generation of multiply charged atomic ions. Initial report
on Coulomb explosion dates back to 1981 when Sattler et al. [1]
observed doubly charged species upon electron impact ioniza-
tion of metallic and vander Waal clusters. In 1994, Castleman and
co-workers [5] observed extensive ionization and generation of
multiply charged atomic species (I
17+
and Ar
8+
) upon interaction
of (HI)
n
(Ar)
m
clusters with intense femtosecond laser pulses. Sub-
sequent studies on Coulomb explosion by other research groups
[6–10] revealed the dependence of cluster size, laser wavelength,
intensity, pulse duration, etc. on efficiency of energy transfer from
optical field into the cluster medium.
∗
Corresponding author. Tel.: +91 2225592438.
E-mail address: rkvatsa@barc.gov.in (R.K. Vatsa).
Several ionization mechanisms such as Ionization Ignition
Model (IIM) [11], Coherent Electron Motion Model (CEMM) [12,13],
Charge Resonance Enhanced Ionization (CREI) [14], etc., have been
proposed to account for occurrence of Coulomb explosion under
high intensity laser fields (I ∼ 10
15
W/cm
2
). However, these ion-
ization models could not explain low intensity (I ∼ 10
9
W/cm
2
)
induced Coulomb explosion of clusters [15–20]. In order to ratio-
nalize the phenomenon of Coulomb explosion at gigawatt laser
intensity, a three stage cluster ionization model, i.e. multipho-
ton ionization ignited – inverse bremsstrahlung heating (IBS) –
electron ionization, has been proposed [18,19]. According to this
model, Coulomb explosion is initiated via multiphoton ionization
of atoms/molecules present in clusters. Subsequently, electrons
released via inner ionization process are caged within the clus-
ters. These quasi free electrons, under the influence of Coulombic
field, extract energy from laser pulse via inverse bremmsstralung
process. Once the quasi free electrons gain enough energy, further
ionization takes place via electron ionization resulting in gener-
ation of multiply ionized species within clusters. Finally, these
charged clusters undergo Coulomb explosion due to strong elec-
trostatic repulsion.
Based on the above proposed three stage cluster ionization
model, the quasi free electrons, generated upon initial MPI of clus-
ter constituents, needs to acquire the energy equal to or greater
than the ionization energy (I.E.) of neighbouring species, so as to
1387-3806/$ – see front matter © 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.ijms.2013.11.007