Nuclear Instruments and Methods in Physics Research B19/20 (1987) 865-871 865
North-Holland, Amsterdam
MOLECULAR WEIGHT DISTRIBUTION AND SOLUBILITY CHANGES IN
ION-BOMBARDED POLYSTYRENE
Orazio PUGLISI and Antonio LICCIARDELLO
Dipartimento di Scienze Chimiche dell'Universit~ di Catania, viale A. Doria 6, 95125 Catania, Italy
Lucia CALCAGNO and Gaetano FOTI
Dipartimento di Fisica, Corso Italia 57, 95129 Catania, Italy
Among the chemical and physical modifications induced by ion bombardment on polymers, solubility changes have attracted
considerable attention owing to the technological interest for microlithography purpose. The solubility changes are due to occurrence
of cross-linking and scission at molecular level with heavy modification of the molecular weight distribution too. The molecular
weight distribution of implanted polystyrene shows considerable changes upon bombardment. These changes have been followed on
bombarded nearly-monodisperse PS samples. The use of samples with known molecular weight distribution allows to apply the Gel
Theory for determining the chemical yields. This method is a direct, relatively simple tool for following the chemical modifications in
bombarded polymers.
1. Introduction
High energy ion bombardment of organic materials
produces several chemical and physical modifications in
the bombarded area [1]. Although these effects are
strictly correlated with each other only the physical
effects have been extensively investigated while little
work has been done on the chemical modification. The
reason for this might be that the beam-induced chem-
ical reactivity is generally considered an unwanted phe-
nomenon, often referred to as "radiation-damage". In
addition, there is the intrinsic difficulty of working with
very small sample amounts which renders problematical
the identification of the final products.
Beam effects on polymer systems represent a good
example of the possibility of exploiting this chemical
phenomenology for "synthesizing" new material with
different physical properties [2,3]. Here, the ion bom-
bardment induces the formation of a new polymeric
material with enhanced (positive-tone) or decreased
(negative-tone) solubility in a solvent. This phenomenon
can be exploited for microlithography purpose in order
to obtain lithographic features of sub-micron dimension
for VLSI devices [4,5].
Among the chemical effects occurring in ion-
bombardment polymers, those generated at low fluence
(10x2-1013 ions/cm 2) are attractive because at higher
fluences the overlap of the reacted regions renders the
system too complicated for the chemical mechanism
being identified.
Polystyrene (PS) has been chosen by us as a "proto-
type" polymer because of the volume of literature (about
conventional effects) on this system and this renders
easier the comparison between beam-effects and those
induced by conventional (thermal or photo-chemical)
treatments.
In addition PS is nowadays available as linear mac-
romolecule of known molecular weight (MW). These
samples are obtained by means of "living" polymeriza-
tion which yields PS samples with very narrow molecu-
lax weight distribution (MWD). These polymers are
nearly mono-disperse (of uniform length) and are suit-
able for study of the MWD change induced by ion
bombardment. Moreover, the use of polymer samples
with known MWD allows one to use the Inokuti's Gel
Theory [6] for obtaining the number of cross-links be-
tween the macromolecular chains. When MWD is known
and sufficiently narrow for approximating the size dis-
tribution to the particular case of polymer chains of
uniform length, the Inokuti's theory can be replaced by
simpler expressions first obtained by Flory many years
ago [7].
This paper reports a study of the effects induced on
PS by He + ion bombardment at 100 keV energy. Par-
ticular focus is on the MWD changes induced by ion
beam on nearly monodisperse PS samples. The aim is
that of linking the macroscopic modification induced by
the beam on PS, to the modifications occurring at
molecular level.
2. Experimental
The MWD determination of the polymer samples
before and after bombardment was determined by
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