Cluster Radioactivity: An Overview After Twenty Years
Cluster Radioactivity: An Overview After Twenty Years
Cluster Radioactivity: An Overview After Twenty Years
301–310, 2007
CLUSTER RADIOACTIVITY:
AN OVERVIEW AFTER TWENTY YEARS
1. INTRODUCTION
Writing this paper brings us back to very exciting years when our experi-
mental research on cluster radioactivity first started (1988) and subsequently
grew up reaching a steady state in the period 1990–2000. What was peculiar
of that period was first of all the novelty of the phenomenon at that time
(1984) recently discovered and the consequent excitement which led several
experimental groups at Berkeley, Dubna, Orsay and finally Milano to develop
experimental techniques dedicated to investigate such peculiar, extremely rare
decay mode of heavy nuclei. However, this was not the only motivation of an
intense experimental investigation which, in the course of about twenty years
allowed to measure the decay properties of some twenty trans-lead exotic emit-
ters of clusters with mass numbers in the range 14-34. Indeed, most important
was the close connection between experimental and theoretical groups, the lat-
ter providing the former ones with predictions, in the form of extensive tables
or computer programs, which were extremely important in guiding experi-
mental investigations among the thousands of cases corresponding to different
302 Roberto Bonetti, Alessandra Guglielmetti 2
are overlapping. It was indeed shown by D. Poenaru [11] that the transmis-
sion probability through that part of the potential barrier before the saddle
point, i.e. the prescission phase, simulates the so-called spectroscopic factor
present in the “α decay”-like models, implicitly assumed to be unity in the
“fission”-like models.
Previous experimental studies on cluster radioactivity have allowed us
to accumulate data on clusters with mass number in the range A=14-32 [5].
When compared with theoretical models it is found however that despite their
seemingly different nature almost all of them reproduce the experimental half-
lives with the same kind of accuracy, i.e. within one-two orders of magnitude,
thus making practically impossible to decide in favour of one or another. How-
ever, from the experimental point of view the gap between alpha-radioactivity
and fission remains far from being filled, and observation of heavier and heav-
ier clusters is important in this respect. For example, calculations show that
the decay probability decreases with increasing fragment mass more steeply
for the α-decay rather than for the fission-like models [11].
Unfortunately in going to heavier mother nuclei not only has the exper-
imentalist to face with vanishing decay probabilities but also and especially
with increasing competition coming from fission fragments in addition to the
well known one from α particles. This fact has considerably slowed down the
experimental efforts in this field in recent years.
The aim of this experiment was to measure the cluster decay of 242 Cm,
the heaviest mother nucleus studied in this respect. All the models predict that
the most probable clusters should be 34 Si and 208 Pb respectively, a channel
which maximizes the decay Q-value due to strong shell effects.
In this study a particular care was directed towards the fission frag-
ment suppression, which is one of the major problems met by experiments
on transuranic nuclei, to the level of 10−9 relative to the initial one. This
was achieved by filtering the fission fragments with different kind of absorbers,
both solid and gaseous. As in previous studies, solid state track detectors of
the glass type have been used due to their selectivity in respect to the less
ionizing but much more abundant α particles. Particular care was also de-
voted to the track detectors calibration and to the control of the α fluence,
which is a critical point when dealing with branching ratios relative to α de-
cay (Bα = λcl /λα ) values of the level predicted for the present experiment,
10−16 − 10−17 .
The sources were prepared by irradiating a 241 Am sample with neutrons
produced by the Kurchatov research reactor and separating Cm by means of
radiochemistry techniques. They were used to irradiate two ensembles of track
detectors arranged in hemispheric geometry. Subsequent chemical etching, de-
tector scanning and comparison of the events found in the form of conic tracks
304 Roberto Bonetti, Alessandra Guglielmetti 4
When comparing such data with predictions given by the various theo-
retical models, we see that while the one of the fission-like model of Poenaru
[9] gives a remarkable agreement, within a factor of two, those of the “α
decay”-like models [7, 8] exhibit the largest discrepancy, up to one-two orders
of magnitude. We believe that such a behaviour could be physically mean-
ingful, in view of the fact that it is found here for the first time within the
wide systematics accumulated so far. It is interesting indeed to remark that
predictions of fission-like models like the one of Ref. 9 start to diverge from
those given by generalized α-decay models like the one of Ref. 7 for cluster
mass A ∼ 30 − 35.
From the experimental point of view, both the emitted cluster and the
mother nucleus have been the heaviest ever studied for this rare kind of ra-
dioactivity; moreover, the branching ratio relative to alpha decay is one of the
smallest ever measured for hadronic decay modes of nuclei.
This experiment [12] aimed at measuring, on the other hand, a quite light
cluster, 22 Ne, emitted by the lightest isotope of the uranium isotopic series,
230 U. In addition to comparison with theoretical predictions, the motivation
was here that the large systematics accumulated on uranium isotopes in recent
years (A=232,3,4,5,6) [5] pointed out the different behavior of the partial half
lives for spontaneous fission and cluster radioactivities with the mass number
of the parent, the former being practically constant and the latter rapidly
varying as a consequence of shell and other structure effects. In view of the
additional feature that both spontaneous fission and cluster radioactivity have,
for this particular isotopic series, partial half lives of similar order of magni-
tude, it was found interesting to extend the systematics both from the light
and heavy sides. We will discuss here the measurement of cluster decay of the
lightest uranium isotope, 230 U, while the one on the heaviest, 238 U, is still in
progress, as will be discussed later.
The 230 U source was obtained, also in this case, by radiochemistry follow-
ing an intense proton irradiation of metallic thorium targets producing some
GBq activity of 230 Pa, subsequently β-decaying into 230 U. This is a further
example of how challenging is to obtain a sufficient number of mother nuclei
in the most advanced experiments on exotic decay. The detectors were still
of the glass type, this time arranged in 4π geometry. Six events were found
5 Cluster radioactivity 305
reous carbon catcher. At this point the 225 Ac source was simply obtained by
letting it β-decay; again, glass detectors in 2π geometry were used to detect
14 C cluster decay.
14 events were found in 86.2 cm2 glass surface. From the known source
intensity and irradiation time, the branching ratio for 14 C decay of 225 Ac
came out to be B = (4.5 ± 1.4)10−12 and the corresponding partial half life
T1/2 = (1.9 ± 0.6)1017 s, in very good agreement with the 1993 result [14].
One of the goals of the experiment was to find out which level of the 211 Bi
residual nuclide is preferentially fed by the 14 C decay of 225 Ac. Two hypothesis
have been put forward to explain its unexpectedly high decay rate, in analogy
with α decay, in terms of favoured transition either to the ground state or to
the first excited one of 211 Bi [14]. While theoretical arguments based on the
structure of the 225 Ac mother nucleus could justify both hypothesis, only an
experimental result could solve such ambiguity, thus possibly confirming the
use of 14 C radioactivity as a spectroscopic tool after the pioneering experiments
with 223 Ra decay [16].
The 225 Ac source was therefore used in a second set-up aimed at mea-
suring the 14 C spectrum with an energy resolution sufficient to study its fine
structure. The SOLENO spectrometer of IPN-Orsay was used for this pur-
pose. The basic idea is to use the selective features of the spectrometer to
reject the high flux of α particles, while keeping the good energy resolution
typical of Si detectors.
Unfortunately, the experiment turned out to be difficult due to multiple
α pile-up events because of the extremely high intensity of the source which
unfortunately fell in the energy region between 28 and 29 MeV where 14 C
events were expected. It was therefore impossible to unambiguously assign
the recorded events to 14 C.
However, the positive and consistent result obtained with track detectors
confirms the interest of 14 C decay of 225 Ac from the point of view of nuclear
structure. It also suggests that an experimental identification of the favoured
transition, a crucial information to test the proposed theoretical interpreta-
tions, is a very difficult task indeed.
7 Cluster radioactivity 307
thus possibly allowing to study even-odd effects in the light cluster itself.
The idea to run this experiment came out in 1993 but only more recently
it was possible to find a solution to obtain a strong enough 223 Ac source.
The solution was to irradiate by an intense 66 MeV proton beam a thick
thorium target thus producing 227 Pa (T1/2 = 38 min) nuclides by means of
the 232 Th(p,6n) reaction, doing an on-line chemistry to separate Pa from Th,
depositing it on a golden-plated disk and letting it α decay in order to get
the wanted 223 Ac source. The only laboratory combining a proton beam with
the required energy and intensity and on-line radiochemistry was found to be
iThemba at Faure, South Africa. The Faure-Dubna-Milano-Moscow collabo-
ration was able to perform three irradiations of glass detectors ensembles in
2005. Detector analysis aiming at measuring both 14 C and 15 N emissions is
almost finished and results will be published quite soon.
308 Roberto Bonetti, Alessandra Guglielmetti 8
3. CONCLUSIONS
Table 1 shows all the experimental data available for cluster decay. As
one clearly sees, the progress made in this field is impressive since 1984, the
starting year of the story.
However it is also clear, as the experiments discussed in previous section
have pointed out, that large room is still available for further progress, both
from the experimental and (especially) the theoretical side. As a matter of
fact, we can mention at least three still open problems, namely the possible
existence of other islands of cluster radioactivity in which the residual nuclei
are close to other doubly-magic ones like 100 Sn or 132 Sn, the investigation of
even-odd effects and the study of the emission of heavy clusters in view of a
better understanding of the theoretical interpretation of this phenomenon.
Table 1
Cluster decay experimental data
Table 1 (continued)
Emitter Cluster Q(MeV) Detection B = λcl /λα lg10 T (s)
System
231 24
Pa Ne 60.42 BP1 (1.34 ± 0.17)10−11 22.88
230 22
U Ne 61.40 BP1 (4.8 ± 2.0)10−14 19.57
232 24
U Ne 62.31 PET (2.0 ± 0.5)10−12 21.08
232 24
U Ne 62.31 PSK50 (8.68 ± 0.93)10−12 20.42
232 24
U Ne 62.31 PSK50 (9.16 ± 1.10)10−12 20.40
233 24,25
U Ne 60.50,60.75 PET (7.5 ± 2.5)10−13 24.83
233 24,25
U Ne 60.50,60.75 PSK50 (7.2 ± 0.9)10−13 24.84
234 24,26
U Ne 58.84,59.47 PSK50 (9.06 ± 6.60)10−14 25.92
234 24,26
U Ne 58.84,59.47 PET (9.90 ± 9.90)10−14 25.88
235 24,25
U Ne 57.36,57.83 PET (8.06 ± 4.32)10−12 27.42
236 24,26
U Ne 55.96,56.75 PET < 9.2 · 10−12 >25.90
232 28
U Mg 74.32 PSK50 < 1.18 · 10−13 >22.26
233 28
U Mg 74.24 PSK50 < 1.30 · 10−15 >27.59
234 28 +0.8
U Mg 74.13 PET (2.3−0.6 27.54
234 28
U Mg 74.13 PSK50 (1.38 ± 0.25)10−13 25.14
235 28,29
U Mg 72.20,72.61 PET < 1.8 · 10−12 >28.09
236 28,30
U Mg 71.69,72.51 PET 2.0 · 10−13 27.58
237 30
Np Mg 75.02 PET < 8.0 ± 10−14 >26.93
237 30
Np Mg 75.02 PSK50 < 1.8 · 10−14 >27.57
236 28
Pu Mg 79.67 PET 2.0 · 10−14 21.67
236 28
Pu Mg 79.67 PHOSP. GLASS (2.7 ± 0.7)10−14 21.52
238 28,30
Pu Mg 75.93,77.03 LG750 (5.62 ± 3.97)10−17 25.70
238 32
Pu Si 91.21 LG750 (1.38 ± 0.50)10−16 25.27
240 34
Pu Si 90.95 PET < 6 · 10−15 >25.52
241 34
Am Si 93.84 POLY < 2.6 · 10−13 >22.71
241 34
Am Si 93.84 PET < 5.4 · 10−15 >24.41
241 34
Am Si 93.84 LG750 < 7.4 · 10−16 >25.26
242 34
Cm Si 96.53 LG750, GOI-104 10−16 23.15
REFERENCES