Philosophical Magazine A

ISSN: 0141-8610 (Print) 1460-6992 (Online) Journal homepage: http://www.tandfonline.com/loi/tpha20

Ion-induced spike effects on metal surfaces

S. E. Donnelly & R. C. Birtcher

To cite this article: S. E. Donnelly & R. C. Birtcher (1999) Ion-induced spike effects on metal
surfaces, Philosophical Magazine A, 79:1, 133-145, DOI: 10.1080/01418619908214279

To link to this article: http://dx.doi.org/10.1080/01418619908214279

Published online: 12 Aug 2009.

Submit your article to this journal

Article views: 31

View related articles

Citing articles: 13 View citing articles

Full Terms & Conditions of access and use can be found at

http://www.tandfonline.com/action/journalInformation?journalCode=tpha20

Download by: [Amity University], [gaurav gupta] Date: 23 September 2015, At: 23:25
 PHILOSOPHICAL
MAGAZINE
A, 1999, VOL.79, No. 1, 133-145

Ion-induced spike effects on metal surfaces

By S. E. DONNELLY
Joule Physics Laboratory, Science Research Institute, University of Salford,
Salford M5 4WT, England

and R. C. BIRTCHER
Materials Science Division Argonne National Laboratory Argonne, Illinois,
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

60439, USA

[Received 16 September 1997 and accepted in revised form 12 March 19981

ABSTRACT
The effects of single Xe ion impacts on the surfaces of Au, Ag, In and Pb have
been studied using in-situ transmission electron microscopy. Individual ion
impacts produce surface craters with associated expelled material. The cratering
efficiency scales with the density of the irradiated metal. Calculation indicates
that, when collision cascades occur near surfaces (within about 5nm) with
energy densities sufficient to cause local melting, craters will occur. Crater
formation occurs as a result of the explosive outflow of material from the hot
molten core of the cascade. This would appear to indicate that, although the
number of atoms in a spike is small and its duration short, it is reasonable to
use macroscopic concepts such as vibrational temperature, melting and flow to
describe spike effects.

5 1. INTRODUCTION

1.1. Spike effects

The concept of displacement and thermal spikes resulting from single ion impacts
was first discussed in the scientific literature in the 1950s by researchers such as
Brinkman, Seeger and Seitz and Koehler. The interaction of a high-energy ion
with a solid can be described successfully, up to a certain energy density, as a series
of binary collisions involving the impinging ion and recoiling substrate atoms in
what is normally described as a collision cascade. This description breaks down,
however, when, as first suggested by Brinkman (1954, 1956), the mean free path
between displacement collisions approaches the interatomic spacing of the substrate.
Under these circumstances, a highly disturbed region is formed, in which the mean
kinetic energy of the atoms may be up to several electron volts; this is known as an
energy or displacement spike. At some (short) time after the initial energy deposition
the kinetic energy in the spike may be shared in a relatively continuous distribution
by all the atoms within the spike region. Under some conditions this may give rise to
an effective temperature within the spike zone significantly above that required for
melting; this phase is generally referred to as a thermal spike.
Spikes are small (typically of the order of a few nanometres in diameter), requir-
ing techniques with a high spatial resolution to obtain information about their
structure. In addition, spikes are of short duration (calculations of thermal spike
lifetimes generally yield values of the order of lops) and, compared with this time
0141-8610/YY $12 00 ’ .1 1999 TdylOr & I-mnaa Ltd
 134 S. E. Donnelly and R. C . Birtcher

scale, measurements on processes resulting from ion impacts inevitably take place a
long time after the impact. Any measurement is thus of the effects of the displace-
ment spike, the ensuing thermal spike and any defect annealing processes (both
thermal and ion beam assisted) that may subsequently take place.
As far as theoretical understanding of spike processes is concerned, major
advances have been made in the last decade or so owing to the availability of
high-powered computers, enabling molecular dynamics (MD) simulations to be car-
ried out on 'crystallites' of increasing size, although, as yet, primary recoil energies
are limited to 10-20keV. At times a few picoseconds or so after the simulated
impact, M D simulations of heavy ions incident on crystalline metals have revealed
that, on occasion, spike zones are formed in which an analysis of atom positions and
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

energies reveals a radial pair distribution function typical of a fluid (or an amor-
phous solid) and an effective temperature significantly above melting (Diaz de la
Rubia et a/. 1989, Averback 1994).
Paralleling these findings, the direct observation of amorphous zones due to
individual impacts in some crystalline semiconductor materials (Ruault et a/. 1984,
Narayan et uf. 1985) and disordered zones in ordered metallic alloys (Jenkins and
Wilkins 1976) has provided clear evidence that displacement spikes are produced in
dense cascades and that the resulting disordered zones may be quenched into the
material. However, fundamental questions about the high nature of the thermal
spike, posed by Thompson (1981) in a review of high-density cascade effects, still
remain substantially unanswered:

(i) is it legitimate to use the concept of a vibrational temperature when the

number of atoms in the spike (typically of the order of lo4) may not be
sufficient to be described by Maxwell-Boltzmann statistics?
(ii) is the duration of the spike (typically of the order of lop1' s) sufficient for
any major mass transport to occur?

1 2. Ion-induced cratering
A number of workers have discovered small craters on metal surfaces bom-
barded with high-energy heavy ions which they attributed to the effects of spikes
or cascade collapse. In particular, Merkle and Jager (198 1) used transmission elec-
tron microscopy (TEM) to examine Au surfaces following irradiation with Bi and
Au ions in the energy range 10-500 keV and discovered craters on the irradiated
surfaces for energies above 50 keV, with fewer than 1% of ions giving rise to craters,
a percentage that increased when molecular ions were employed. Average crater sizes
for the different irradiations were typically about 5nm and some craters were
observed to be faceted. Although these workers believed that spike effects were
responsible, they concluded that relatively rare high energy-density cascades, in
which surface atoms were evaporated from rhe surface, gave rise to the craters.
The requirement that the relatively high sublimation energy be imparted to each
atom removed from the crater inevitably implied that only statistically rare high
energy-density cascades could be involved. In the Merkle-Jager model, all atoms
displaced to create the crater were sublimed from the surface, thus contributing to
the overall sputtering yield. In addition to the surface spikes giving rise to craters by
sublimation, these workers also concluded that subsurface spikes were responsible
for a small number of craters with associated lids, the spikes giving rise to localized
 Ion-induced spike eflects on metal surfaces 135

pressure rises sufficient to shear the material between the spike region and the sur-
face.
Irradiations of W surfaces using Ag and W atomic and molecular ions at much
lower energies (20 keV) and at a temperature of 10 K were carried out by Pramanik
and Siedman (1983). The surfaces were then imaged at atomic resolution using field-
ion microscopy and void-like near-surface contrast was obtained, implying features
with diameters in the range 2-3 nm which these workers attributed to surface voids
formed as a result of nucleation and growth within a displacement cascade.
Finally, Jenkins and English (1987), in research aimed primarily at studying the
collapse of displacement cascades to vacancy loops, discovered craters, using trans-
mission electron microscopy on Mo surfaces irradiated with ions of Mo, W and Sb.
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

Craters due to atomic ions were observed only for irradiations at elevated tempera-
ture (670K) whereas irradiation with Sbz and Sb:, gave rise to craters at room
temperature. Crater creation efficiencies (craters per ion) ranged from 0.4% for
the atomic ions to 3% for Sb:. Although no detailed discussion of these surface
features was presented, they were attributed to the collapse of individual cascades or
subcascades, the processes giving rise to vacancy loops within the specimen were
assumed to give rise to craters at the surface.
Although all the above researchers concluded that cratering resulted from indi-
vidual spike effects, we believe that their studies did not reveal the principal mechan-
ism responsible for cratering (and possibly other surface topographic effects) under
heavy-ion irradiation, namely melting and flow.
The present paper presents an in-situ study of ion-induced cratering on a number
of metals with the aim of establishing both criteria for the occurrence of cratering
and mechanisms of crater formation. The study highlights the importance of melting
and flow as a result of individual ion impacts in crater formation and thus addresses
the questions posed by Thompson, discussed above.

0 2. EXPERIMENTAL DETAILS
Ion irradiations were carried out in a Hitachi A-9000 transmission electron
microscope operating at 300 keV at the IVEM/Accelerator Facility located at
Argonne National Laboratory (Allen ef al. 1989). Thin Au films were made by
thermal evaporation of 99.999 at.% pure starting material onto NaCl at a tempera-
ture of 350°C. This resulted in a largely single-crystal film with a (100) surface
normal. Specimens of Ag, Pb and In were produced from rolled annealed foils
with a 99.999% purity from which 3 mm discs were punched and electrochemically
thinned. The gold films were determined by Rutherford back scattering to have a
thickness of 62 f2 nm; the thickness of the electropolished specimens was not accu-
rately known but was of the order of 100 nm. In the IVEM/Accelerator Facility, the
ion beam is oriented 30" from the microscope axis; in our experiments the specimen
was tilted 15" towards the ion beam so that both ions and electrons were incident on
the specimen at 15" to the foil normal. Specimens were irradiated with Xe' ions at
energies in the range 50-400 keV at dose rates between 10" and 10l2 ionscm-2 s-'.
Craters are made visible in TEM in the same way as voids and bubbles by means
of their phase contrast under controlled amounts of objective lens defocusing.
Images are generally obtained in bright field, on a region of the (somewhat bent)
films in which no Bragg reflection is strongly excited. Under these conditions, under-
focusing the objective lens by typically IOOOnm yields reasonably sharp images in
which the crater is lighter than the background and is delineated by a dark Fresnel
 136 S. E. Donnelly and R. C. Birtcher

fringe. Similarly a small mound or particle on the surface appears darker than the
background with a light fringe around it. A similar degree of overfocus gives rise to
images in which this contrast is reversed; that is small craters appear darker than the
background and small particles appear lighter than the background.
Note that in static images, small craters may be indistinguishable from the,
bubbles which occur when Xe+ irradiations are continued to doses of 10’’ ionscm-*
or greater. In the video recordings of in-situ experiments, craters can be distinguished
from bubbles by their relatively short lifetime compared with those of the bubbles;
however, in order to avoid confusion between craters and bubbles, all results
reported here were obtained at Xe’ doses considerably below those at which bubbles
are observed.
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

In addition to normal photographic recording, images from a Gatan 622 video

camera and image intensification system were viewed with total magnifications of
approximately 2 million, and recorded on video tape with a time resolution of 33 ms
(6s. a single video frame).

9 3. RESULTSA N D DISCUSSION
3.1. Gold
Recent work on heavy-ion irradiation of electrochemically thinned Au foils
revealed that individual ions could punch holes through foils whose thickness was
estimated to be of the order of 20nm (Birtcher and Donnelly 1996). This, together
with other changes taking place in the foils, was taken to indicate that significant
plastic flow was occurring, under irradiation.
In this section, we look at the effects of individual heavy-ion impacts on slightly
thicker evaporated Au films on which the most noticeable defects (under appropriate
imaging conditions) observed by TEM are small craters. Before presenting and
discussing images of craters, however. it is perhaps important to give a description
of the impressions obtained when the live irradiation (or a videotaped record) is
observed. The monitor on the microscope provides an additional 20 x magnification
to the 1 0 0 0 0 0 ~generally used for the experiments. The area visible on the monitor
corresponded to an actual area of 1 lOnm x 85 nm. At the dose rates used in the
experiments (typically 2.4 x 10” ionscm-2 s-I), about 20 ions impact on the area
viewed every second and, with creation rates of between 0.02 and 0.05 craters per ion
on Au, this results on average in a new crater appearing in the area viewed every 1-
2 s. However, as will be discussed at the end of this section, craters are unstable under
irradiation and are rapidly filled in by material transported from other impact sites.
The impression obtained is, thus, one of a surface exhibiting almost fluid-like proper-
ties on which a crater (together with expelled material) suddenly appears and then
disappears over several seconds, during which time new craters appear. A frame-by-
frame analysis of the video recording (or experiments at lower dose rates), however,
reveals that the flow that causes crater annihilation is actually a discrete rather than a
continuous process.
Figure 1 shows three images, digitized from videotape, of fairly large craters
resulting from impacts of individual 200 keV or 400 keV Xe ions on Au. In each
case, the crater and associated expelled material appeared together between succes-
sive video frames and thus resulted from a single ion impact. The use of stereoscopic
techniques reveals that, at 400keV, craters appeared on both the entrance and
the exit surfaces of the film. This is consistent with the results of simulations to
 Ion-induced spike efects on meid surfaces 137

Figure 1. Examples of large craters with expelled material resulting from impacts of indivi-
dual Xe ions with a gold film. The ion energies are (u) 200 keV (6) 400 keV and (c)
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

400 keV. Images have been digitized from the video recording of the experiment and
consist of an average of the eight successive frames immediately following the appear-
ance of the crater.

determine ion-induced damage in gold, using the Monte Carlo code TRIM (Ziegler
et al. 1985), which indicates that the damage distributions at this energy are such that
significant energy would be expected to be deposited at the back surface.
Inspection of the images in figure 1 reveals clearly that there has been significant
mass transport of material from the impact site, answering question (ii) above in the
affirmative. In addition, the expelled material in each of the images shown does not
have the same shape as its crater, implying that it has not been expelled as a solid
plug. In all four cases the form of the expelled material indicates that molten material
has been expelled from the impact site and that surface tension forces have acted,
producing, for instance, an apparently quenched droplet in figure 1 (b) and a sepa-
rated and seemingly spherical particle in figure l (c). Regardless of whether or not the
spatial and temporal dimensions of the spike are sufficient to permit the use of
Maxwell-Boltzmann statistics, the images indicate that macroscopic concepts such
as melting, flow in response to surface tension forces, and quenching provide a
satisfactory description.
Note that all the craters in figure 1 are larger than the average crater size (about
3 nm). With the more common smaller craters, there is generally, however, no clear
indication of expelled material.
Although, in the majority of craters where expelled material could be seen, the
above description seems appropriate, in a number of instances, small craters occa-
sionally appeared to be accompanied by a solid plug of material having the approx-
imate form of the crater. Such a crater is illustrated in figure 2. Similar images were

Figure 2. A small crater with what is believed to be an associated ‘lid’. The image has been
digitized from the video recording of the experiment and consists of an average of the
eight successive frames immediately following the appearance of the crater.
 138 S. E. Donnelly and R. C. Birtcher

also recorded by Merkle and Jager (1981) who used stereoscopic techniques to reveal
that lids protruding from the surface at steep angles accompanied the formation of
some craters by Bi ions on Au. For such craters, we follow the interpretation of
Merkle and Jager that these result from spikes a sufficient distance below the surface
such that a solid disc of material is punched out by the large pressure increase that
accompanies the thermal spike. M D simulations of 10 keV self-ion impacts on Au
(Averback 1994) indeed indicate that large pressures may occur in a spike. In this
work, pressures in the range 5-8GPa were observed to exist at the core of a very
small spike from 0.65 to 4.9ps following ion impact. The pressure spike would be
expected to result in the punching of a dislocation loop when
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

where p is the shear modulus of the Au, b is the magnitude of the Burgers vector of
the loop and R its radius (assumed to be the radius of the spike) (Greenwood et al.
1959). On the basis of this simple description, a spike 5 nm in diameter will punch out
loops for pressures in excess of 3 GPa, a significantly lower value than predicted by
simply considering the theoretical shear modulus as proposed by Merkle and Jager
(1981). When close to the surface, this process may result in the translation of a
'plug' of material to the surface via a sequence of loops punched out towards the
surface or by the explosive ejection of a solid disc of material.
Although all craters are stable at room temperature with the ion beam turned off,
ion impacts following crater creation are observed to lead to crater annihilation in
one or more discrete steps (Birtcher and Donnelly 1997). In some cases this is seen to
occur as a consequence of plastic flow from a neighbouring impact site, as illustrated
in figure 3, but in many cases the impact giving rise to annihilation or partial
annihilation of a crater is not detected. The numbers indicate the frames from
which the images have been taken (starting with frame 1) and thus show time
progression in units of 33ms. In other cases, the impact of the ion which causes
the full or partial annihilation is not observed. Small craters, less than 2-3nm in
diameter, are generally annihilated in a single step and consideration of the dose rate
used in the experiment (2.4 x 10" ionscm-' sC1) enables a cross-section for annihi-
lation of small craters to be determined, assuming that all impinging ions may
annihilate existing craters. The value for gold is 85 nm2; that is an ion impact within
a radius of approximately 5 nm of a small crater, will annihilate the crater.
Although the annihilation of a crater indicates that transport of material is
taking place from elsewhere to the site of the crater, it is not clear from the present
observations whether plastic flow is always an appropriate model. For some larger
craters (e.g. as shown in figure 3), plastic flow is seen to occur; however in those
many cases where craters disappear without the simultaneous appearance of a
nearby crater, annihilation may be due the diffusion of interstitials from cascades
occurring within the specimen. The mechanisms of crater annihilation are under
further investigation in our laboratories.
Figures 4 (a), ( b )and (c) shows craters observed on the surfaces of In, Ag and Pb
respectively following Xe ion irradiation. Note that, as with Au, craters are made
visible using phase contrast by controlled defocusing of the objective lens. The
specific details of cratering in these three materials will be briefly discussed below.
 Ion-induced spike efects on metal surfaces 139
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

Figure 3. The creation and subsequent annihilation of a crater during 400 keV Xe ion irra-
diation of Au. The numbers are frame numbers and thus indicate time progression in
units of 8s. Images are obtained by carrying out of an average of the eight successive
frames immediately following changes in the image. (The image at t = 0 is an average
of the eight frames immediately preceding the appearance of the crater). The crater,
which appears to be volcano shaped, is partially filled in by material (indicated by the
white arrow) expelled as a result of the creation of a small crater in frame 17. In frame
25, another crater is formed, in this case with what appears to be an associated lid
similar to that in figure 2 (indicated by the white arrow). In frame 30 an impact that is
not within the field of view deposits material in the region indicated, and in frame 44
the crater is almost entirely annihilated by another discrete event that again does not
leave a crater in the field of view.

Figure 4. Examples of craters resulting from (a) 400 keV Xe ion irradiation of In at 17 K, (b)
100 keV Xe ion irradiation of Ag at room temperature and ( c ) 200 keV Xe ion irradia-
tion of Pb at room temperature. The images have been digitized from video recordings
of the experiment and consist, in each case, of an average of the eight successive frames
immediately following the appearance of the crater.
 140 S . E. Donnelly and R. C. Birtcher

3.2. Silver
Cratering in Ag was observed to be qualitatively similar to that for Au although
the creation efficiency (0.6%) was almost an order of magnitude lower. Large irre-
gular craters up to 10 nm in diameter were occasionally observed and all craters were
observed to be filled in discretely as a result of subsequent ion impacts. Recent
studies of heavy-ion irradiation of a thin Ag layer sandwiched between two layers
of SOz (Birtcher et af. 1997) have revealed morphological changes that are also
indicative of the kind of flow processes responsible for cratering.

3.3. Lead
In general, images of craters in this material, were less clear than in the case of
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

Au, owing to the higher degree of defocus that had to be used to image the craters.
(The defocus used was typically 9 pm underfocus; 1 pm for Au. The necessity for a
higher degree of defocus probably indicates that the craters were shallower in this
case than for Au). Unlike gold, there was little evidence of material ejected from the
craters visible as particles on the surface. Approximately 0.7% of ion impacts
resulted in craters in Pb. As with Au and Ag, the observed craters are thermally
stable at room temperature when the ion irradiation is halted but under conditions of
continual irradiation are annihilated discretely by subsequent ion impacts.
A final important point with regard to Pb is that. until the specimen had been
bombarded with a dose of approximately 4 x 10" ionscmp2, no cratering was
observed. At lower doses, inspection of the diffraction pattern from the specimen
indicated that an amorphous (oxide) layer was present on the surfaces of the speci-
men. Beyond this dose, as cratering began to occur. the diffraction pattern revealed
that this layer had been removed by sputtering. The clear implication of this obser-
vation is that cratering is suppressed if an oxide layer is present on the specimen. This
is consistent with the finding by Merkle and JBger (1981) that a thin amorphous layer
of C deposited on Au films reduces the incidence of cratering on the Au surface.

3.4. Indium
Experiments were initially carried out on In at room temperature and these failed
to reveal any cratering. Some oxide appeared to be initially present on the In surface
as in the case of Pb but, even after examination of the diffraction pattern indicated
that this had been removed, cratering still did not occur. The absence of cratering at
room temperature, however, does not necessarily imply that craters did not form, as
the existence of a crater for a sufficiently long period to be observed may involve four
distinct processes, namely crater creation by spike induced local melting and flow,
annealing during the quenching phase of the spike, thermal annealing at the ambient
temperature and full or partial annihilation by subsequent ion impacts.
For a crater to be recorded on videotape it must persist for the order of one video
frame (33ms). At the dose rates used, the rate of annihilation by subsequent ion
impacts should always have been sufficiently low to permit craters to be observed;
however, as far as room-temperature thermal annealing was concerned, it is possible
that the high homologous temperature (0.6T,,,) may have resulted in a very rapid
annealing of craters by surface and bulk diffusion processes; although craters were
being created, they may not have survived sufficiently long to be recorded. To test
this possibility, specimens were irradiated with 400 keV Xe' ions at 17 K using a
cryogenic specimen holder in the transmission electron microscope. A frame-by-
frame analysis of the video recording of this experiment revealed the very occasional
 Ion-induced spike efecrs on metal surjaces 141

formation of craters at this temperature. Specifically, two craters were observed

during ion irradiation for about 30 min, implying a creation efficiency (very approxi-
mately) of 5 x lop5 craters per ion. These craters were observed to be discretely
annihilated by subsequent ion impacts as was the case for the other metals.

3.5. Criteria for occurrence of surfuce spike efects

Values of crater creation efficiencyE scale monotonically with density rather than
with atomic number or atomic weight as illustrated in figure 5 which summarizes our
findings for the four metals studied. The numbers beside each of the three points for
Au indicate the respective Xe ion energies in keV. The values for E (craters per
incident Xe ion expressed as a percentage) have been obtained by determining the
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

number of craters produced in a given time interval; with existence for one video
frame being sufficient for a crater to be recorded. The figure indicates a threshold
~ . data are also
density for crater production (by Xe ions) of the order of 7 g ~ m - The
given in table 1. In addition to the trend of increasing E with increasing substrate
density, the data for Au reveal a lower cratering efficiency for 200 keV Xe ions than
at either lower or higher ion energies; however, the contrast when imaging the
smallest craters is very dependent on the precise degree of defocus, resulting in an
larger uncertainty in the 50 keV value than in those at higher energies.
The correlation with density (rather than atomic mass) is perhaps not altogether
surprising as the energy density within cascades depends on this parameter.
However, the distance of an individual spike from the surface is clearly also impor-
tant.
In an attempt to model cascade-induced cratering, we follow Walker and
Thompson (1978) in defining the core volume V, of an individual cascade as an
ellipsoid with radii equal to the longitudinal straggling ay and a,, that is

6 8 10 12 14 16 18 20
Substrate Density (gm/cm3)
Figure 5 . Measured cratering efficiencies E under Xe ion bombardment as a function of
density of the irradiated metal.
 142 S. E. Donnelly and R. C. Birtcher

The mean energy density 0 (in electronvolts per atom) within an individual cascade is
then given by

where v ( E )is the amount of energy in the cascade deposited in collision events and N
is the atomic density of the metal. The 0.2 represents the fraction of total energy in
the cascade that is deposited within the ellipsoid defined by the straggling.
Using a version of the Monte Carlo code, TRIM, modified to yield individual
cascade dimensions (Bench et al. 1991, Bench 1992) we have calculated the mean
longitudinal and lateral straggling for 10000 ion trajectories, for each of the ion-
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

substrate-energy combinations of interest. In addition, we have obtained an approx-

imate value for v ( E )by assuming that it is equivalent, in each cascade, to the number
of atoms displaced within the cascade multiplied by the displacement energy used in
the calculation. We have then calculated values for V, and 8, using the above equa-
tions. Note that no attempt has been made to examine subcascades; the model
assumes a single cascade per incident ion and fits an ellipsoid to the damage dis-
tribution using the calculated straggling values. For any trajectories where distinct
subcascades may occur the calculation would be expected to yield a fairly inaccurate
result for 8.
We have then assumed that only cascades with energy densities sufficient to cause
melting will be able to cause cratering; the critical values of energy density 8 M at
melting being obtained as
dM(eVatom-') = EM + k(TM- To). (4)
where EM is the latent heat of melting, TM is the melting temperature for each of the
materials, To is the temperature at which the experiment was conducted and k is
Boltzmann's constant. We have then simply determined the percentage of total
cascades with centres lying within critical distance x, of the surface, for which
8 2 OM. Note that in the case of Au with an initial film thickness of 62nm, both
surfaces were included and the reduction in film thickness arising from sputtering of
the films was also taken into account.
Table 1 shows both the measured and the calculated values of E , for -u, equal to
5 nm and 10 nm. The agreement with the measured values is significantly better using
the smaller distance. Although the experimental value of E is greater at 50 keV than
at 200 keV it is nonetheless much smaller (4.8%) than the calculated value of almost
30%. However, the experimental crater count at this energy is undoubtedly an
underestimate, owing to the considerable difficulty in resolving, and obtaining suffi-
cient contrast to record very small craters. (In the calculations no 'cut-off is carried
out to eliminate small craters.) Note also that the calculated cratering efficiency on
the irradiated surface decreases with increasing energy as the ion penetration
increases but. in the case of Au, cratering on the recrr surface results in a larger
value of E at 400 keV than at 200 keV.
The precise values obtained for 8 in these calculations are, of course, dependent
on the definition of the core volume of the spike so that too much significance should
perhaps not be attached to the particular value of x, at which reasonable agreement
is obtained. However, the theoretical analysis does yield the important result that the
data cannot be modelled by assuming that only high-energy-density cascades (e.g.
8, > 1 eV atom-') give rise to cratering. Instead. it is clear that cascades with energy
 Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

3
Table 1. Comparison of measured and calculated values of cratering efficiency E for Xe ions on the four materials of interest. Other parameters tabulated P
are atomic number 2, atomic weight M , density p, Xe ion energy Eo, irradiation temperature T and energy per atom necessary for melting.
s.
2
0
(Yo) E
P EO T el4 %
Z M ( g Cm-3) (keV) (K) (ev atom-') Measured xc = 5nm x, = 1Onm 5
Ag 47 108 10.50 100 293 0.20 0.6 0.5 18
In 49 115 7.31 400 17 0.07 0.005 0 0.04
9
2
0
Au 79 197 19.32 50 293 4.8 28.8 82 x
200 293 0.23 2.4 1.9 15 a
400 293 4.9 6.7" 17 Io,
P
Pb 82 207 11.35 200 293 0.08 0.7 0.3 2.7 r,

"Note that rear surface cratering makes a significant contribution to this value (6.3%).
2
 144 S. E. Donnelly and R. C. Birtcher

densities less than 1 eV per atom in close proximity to the surface are largely respon-
sible. For example, consideration of the distribution of cascade centres with depth
indicates that, to obtain agreement with experimental data for 200 keV Xe on Au,
almost all near-surface cascades must yield craters. Finally, although no attempt has
been made to correlate crater size with energy density, it is likely that the relatively
rare large craters (e.g. 10 nm or greater) d o result from high-energy-density cascades.
The necessary and sufficient condition for cratering to occur thus appears to be
simply that atoms within a cascade close to the surface must be given sufficient
energy to cause melting.
In a recent publication on molecular dynamics modelling of ion-induced spike
effects in solids, Averback and Ghaly (1994) developed a simple model for spike-
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

induced viscous flow effects and concluded that the parameter (FD/eM)', where FD is
the energy deposited per unit length of ion track (assumed linear) and eM is the
average energy of an atom at the melting point (somewhat higher than 0,) could be
used to determine whether cratering due to surface melting would occur for specific
systems. Application of this criterion to a range of materials led to the conclusion
that cratering due to melting and viscous flow would be expected to occur in a
number of relatively low-density materials including Si. Although not specifically
addressed in their paper, application of the Averback-Ghaly criterion to A1 also
predicts cratering in this material. Application of our analysis to low density materi-
als such as these, however, indicates that cratering would not be expected to occur
because of the low value of 0 occurring in these materials. Indeed, experiments in our
laboratories on A1 have consistently yielded no cratering whatsoever.
Although the density is incorporated into the parameter FD used by Averback
and Ghaly, their assumption of a linear ion track almost certainly leads to an under-
estimate of the importance of substrate density in determining whether melting and
flow will occur. Surface features resulting from single ion impacts are seen using
scanning tunnelling microscopy on a number of low-density materials but we believe
that these are not due to melting and flow.

4. CONCLUSIONS
Spike effects produce surface cratering in materials in which cascades occur near
to surfaces and with energy densities sufficient to cause melting. In particular, for
heavy-ion irradiation of materials whose density is greater than approximately
7 gcm-', craters may occur where the spikes resulting from individual impacts
occur with centres within about 5nm of the surface. Crater formation occurs as a
result of the explosive outflow of material from the hot molten core of the spike. It
should be noted that, although cratering has previously been observed and attributed
to individual cascade effects, for the first time in the present work, the mechanism of
crater formation has been elucidated.
The presence of an oxide (or other) film on the surface appears to impede the
cratering process, as noted by Merkle and Jager. At temperatures where surface
defects are rapidly mobile, craters are annihilated before they are recorded on film
or videotape. Otherwise, crater annihilation occurs as a result of material transport
(by either diffusion or flow) from the sites of subsequent ion impacts.
Finally, returning to the two questions posed in the introduction, clear evidence
for melting and flow has been seen in the larger craters, implying that, in answer to
question (ii), the duration of the spike (at least at the surface) is sufficient for major
mass transport to occur. The present work has also indicated that the concept of
 Ion-induced spike efects on metd surfaces 145

vibrational temperature applied to near-surface spikes is useful for predicting

whether cratering will occur. In particular, if the energy in a near-surface spike is
calculated to be sufficient to cause melting when translated into a vibrational tem-
perature, then cratering is observed to take place. Whilst this does not strictly
address the legitimacy of using Maxwell-Boltzmann statistics to describe spike pro-
cesses, it does indicate that the application of macroscopic equilibrium considera-
tions can lead to a useful description of processes occurring under spike conditions.

ACKNOWLEDGEMENTS
We should like to thank B. Kestel for specimen preparation, E. Ryan, L. Funk,
P. Baldo, A. McCormick and S. Ockers for assistance with the in-situ TEM experi-
Downloaded by [Amity University], [gaurav gupta] at 23:25 23 September 2015

ments and G. Carter for useful discussion of spike effects. This work has been
supported by the US Department of Energy, BES-Materials Sciences, under con-
tract W-31-109-Eng-38 and by a collaborative research grant 910670 from NATO.
One of us (S.E.D.) acknowledges funding from the Materials Science Division at
Argonne National Laboratory (ANL) for extended visits to ANL in 1996 and 1997.

REFERENCES
ALLEN,C. W., FUNK, L. L., RYAN,E. A., and OCKERS, S. T., 1989, Nucl. Instrum. Meth. B.
4 W 1 , 553.
AVERBACK, R. S., 1994, J. nucl. Mater, 216, 49.
AVERBACK, R. S., and GHALY,M., 1994, J. appl. Phys., 76, 3908.
BENCH,M. W., 1992, PhD Thesis, University of Illinois.
BENCH,M. W., ROBERTSON, I. M., and KIRK,M. A., 1991, N M ~Instrum.. Meth. B, 59-60,
372.
BIRTCHER, R. C., and DONNELLY, S. E., 1996, Phys. Rev. Lett., 77, 4374; 1997, Phys. Rev. B,
56, 13 599.
BIRTCHER, R. C., DONNELLY S. E., THOME,L., and REHN,L., 1997, (to be published).
BRINKMAN, J. A,, 1954, J. appl. Phys.. 25, 951; 1956, Am. J . Phys., 24, 246.
DIAZDE LA RUBIA,T., AVERBACK, R. R., HSIEH, H., and BENEDEK, R., 1989, J. Mafer. Res.,
4, 579.
GREENWOOD, G. W., FOREMAN, A. J. E., and RIMMER, D. E., 1959, J. nucl. Mater.. 4, 305.
JENKINS,M. L., and ENGLISH,C., 1987, Mater. Sci. Forum, 15-18, 1003.
JENKINS,M. L., and WILKENS, M., 1976, Phil. Mag.. 34, 1155.
MERKLE, K. L., and JAGER,W., 1981, Phil. Mag. A, 44,741.
NARAYAN, J., OEN,0. S., FATHY,D., and HOLLAND, 0. W., 1985, Mater. Lett., 3, 67.
PRAMANIK, D., and SIEDMAN, D. N., 1983, J. appl. Phys., 44,741.
RUAULT, M. O., CHAUMONT J., PENISSON, J. M., and BOURRET A., 1984, Phil. Mag. A, 50,
667.
THOMPSON, D. A., 1981, Radiat. Effects, 56, 105.
WALKER, R. S., and THOMPSON, D. A., 1978, Radiat. Efects, 37, 113.
ZIEGLER,J. F., BIERSACK, J. P., and LITTMARK, U., 1985, The Stopping and Ranges of Ions in
Solids (Oxford: Pergamon).