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Nuclear Physics A155 (1970) 235-244; @ North-Holland Publishing Co.

, Amsterdam
Not to be reproduced by photoprint or microfilm without written permission from the publisher




Natuurkundig Laboratorium, Vrije Universiteit, Amsterdam, The Netherlands

Received 12 May 1970

Abstract: The lifetimes of the 2 rotational states in ZZsTh, 234.236U, 238, 240pu and 248Cm and of

the 4+ rotational states in 228Th and 236U have been measured using the delayed coincidence
technique. From the 2+ lifetimes the quantities B(E2; 2+ + O+), f&, and b are derived and
compared with theoretical predictions. The values of the ratio B(E2; 4+ + 2+)/S(E2; 2+ + O+)
in 22sTh and 236U are found to be 1.42kO.16 and 1.27f0.16, respectively, in good agreement
with the rotational-model prediction.
RADIOACTIVITY 228Th, 232U, 238*240Pu 243Am, 242*244Cm Cf; measured ace
E delay. 224Ra, 22sTh, 234*236U, 238*240Pu, ;48Cm levels, deduied T+, B(E2), Qe, /I.
23gNp, level deduced T+

1. introduction
It has been known for a long time that the nuclei beyond z24Ra show large equilib-
rium deformations. Generally the lowest excited states of doubly even nuclei in this
region are rotational states characterized by K = 0, I = 0, 2, 4, . . .
Within the framework of the unified model the decay properties of the 2+ and 4+
rotational states are given by
B(E2; 2+ + Of) = & Q;, (1)

B(E2; 4+ -+ 2+) = g Q;.

In this paper we describe measurements on the lifetimes of the 2+ rotational

states in 22*Th, 234U, 236U, 238Pu, 240Pu and 24sCm and of the 4+ states in 228Th
and 236U. These lifetimes determine the intrinsic quadrupole moments Q, and from
that the deformation parameters. The results may be compared with the predictions
from the Nilsson model l- ).
Combination of eqs. (1) and (2) leads to
B(E2; 4+ -+ 2+)
= 1.43. (3)
B(E2; 2+ + 0+)
This relation is a consequence of the adiabatic assumption in the unified model
and can be tested by measuring the lifetimes of both the 2+ and 4+ states. In the rare
236 n. ToN et al.

earth region many 2+ and 4+ lifetimes have been measured 4- ). In most cases good
agreement exists between theory and experiment.
In the heavy element region only three lifetimes of 4+ states have been measured 1).
In view of these scarce experimental data we performed measurements on the 4+
states in Th and 236U.

2. Experimental procedure

The first two excited states of the nuclei of interest are populated by a-decay,
typically 20-30 % to the 2+ state and 0.02-0.3 % to the 4+ state. De-excitation occurs
by strongly converted gamma transitions. The lifetime measurements were performed
using the delayed coincidence technique. For the detection of the u-particles we used
an titec surface barrier solid state detector, which combines a fast rise time (c 3 ns)
with a good energy resolution (< 25 keV). The low-energy conversion electrons were
detected by a plastic scintillator-photomultiplier combination (Naton 136+




Fig. 1. 4 ns delay checking arrangement.

The electronic equipment consists basically of a conventional fast-slow delayed

coincidence system. As fast discriminators we used Ortec 260 time pick-off units.
The output signals of the two time pick-off units act as the start and stop pulses for
an Ortec 405 time-to-pulse-height converter. The linearity of the time-to-pulse-height
conversion was tested using uncorrelated start and stop pulses. In the region of
interest the differential nonlinearity is less than 3 %.
Time calibration was performed using the Ortec Model 425 nanosecond delay.
This device consists of 1, 2, 4, 8 and 16 ns delays, each of which is guaranteed within
100 ps. Since the delays are accomplished by coaxial cables the output pulses will be
somewhat distorted which may lead to systematic errors. These errors can be avoided
to a large extent by measuring the delay in an arrangement where the time-to-pulse-

height converter receives stop pulses via the same way as in the real experiments. For
this purpose we used a testing arrangement the fast part of which is shown in fig. 1.
Two sources of 6oCo at a relative distance of 60 cm provide two prompt peaks with
a time difference of 4 ns. By measuring alternately with 4 ns delay in and out
the true length of this delay can be determined. Averaging three measurements we
found 4.025 f 0.030 ns.
In our test measurements it appeared that for higher counting rates the time spec-
trum was distorted due to pile-up effects in the electron channel. In order to suppress



Fig. 2. Prompt time spectra for different settings of the electron single channel analyser window.

these pile-up effects we employed the Ortec 404 pile-up inspector which provides an
inhibit pulse when two fast electron pulses occur within a time interval of 2 /.Ls.
Prompt time spectra were measured using the 40 and 328 keV levels in zosT1. In
fig. 2 the prompt time spectrum is shown for different settings of the electron single-
channel analyser window. As expected time resolution gets worse with decreasing
electron energy. In our experiments the lowest window setting was 43-50 keV, so the
prompt slope was always better than 100 ps.


The experimental arrangement was tested on the lifetimes of the 84.5 keV state in
z24Ra a,?d the 74 keV state in 23gNp. Both lifetimes have been measured several
times witi4 results within each others limits of error.
Our measurements are shown in figs. 3 and 4. The half-lives were extracted from
the slope of the experimental curve using a least-squares method.
238 H. TON et al.


Fig. 3. Time spectrum of the decay of the first excited state of z24Ra.



Fig. 4. Time spectrum of the decay of the 74 keV state in 23vNp.


Our results
T&(84.5 keV; 224Ra) = 0.748 kO.020 ns,
T+(74 keV; 23gNp) = 1.41kO.04 ns,

are in good agreement with the results of other authors I- ).

The errors in the lifetime values are calculated from the statistical error (extracted
from the least-squares calculation) and an estimated systematic error. Systematic
errors can arise from alinearities of the time-to-pulse-height conversion, from errors
in the time calibration and from pile-up effects. The systematic error is estimated to
be less than 2.5 %.


The sources of 232U, 238Pu, 240Pu, 242Cm, 244Cm and Cf were obtained by the
kind help of Mr. Kooi (Euratom, Transplutonium Group), Prof. Aten and Mr.
Boersma (I.K.O., Amsterdam). The radioactive material was electroplated onto
stainless steel discs 20, 21). The measured alpha resolution was less than 40 keV for
all sources. In the case of 232U a chemical separation was performed in order to get
rid of disturbing Th activities ).


Each of the 2+ lifetime measurements took about one day, while the 4+ lifetime
measurements lasted between one and two weeks. During these long times small
drifts in detectors and electronics may occur, leading to a distortion of the time
spectrum. It appeared that the most serious drifts were caused by changes in the
ambient temperature. We found a centroid shift of about 1 channel (60 ps) per C.
In view of possible temperature fluctuations the measurements were divided in runs
of 160 minutes. After each run the time spectrum was recorded on magnetic tape, the
centroid was calculated and, if necessary, the time spectrum was shifted in such a way
that the centroid coincided with the centroid of the first time spectrum. After that the
time spectrum was added to the foregoing spectra. The whole shifting and adding
procedure was carried out by the CDC 1700 computer in our laboratory.
In our measurements the mean centroid shift between two runs amounted 0.55
channels, while the maximum centroid shift was less than 1.5 channels. Consequently
only two or three channels of the time spectrum may be distorted due to the shifting
and adding procedure.
Figs. 5-8 show the delayed coincidence spectra for the 2 and 4 states mentioned
in sect. 1.
One special precaution was taken in the case of the 4+ lifetime measurements.
Here pile-up effects may arise due to the fact that the 4+ + 2+ transition is followed
by the 2+ + Of transition within a very short time. If the conversion electrons of
both the 4 + 2+ and 2+ + O+ transitions strike the electron detector the corre-
sponding signals will add. Consequently the time spectrum may be distorted due to
240 HI TON et al.

* 102


, -1012345~~-10123 -101 2 3 -1 012 3
TIME llO-gscc UNITS) TIME (lO-gsccUNITS)

Fig. 5. Decay of the 2+ and 4+ states in 22sTh. Fig. 6. Decay of the 2+ and 4+ states in W.

-1OI23L --lo12
TIME (lo-'src UNITS1 TIME ilO-gsec UNITS)

Fig. 7. Decay of the 2+ states in 234U and 238P~. Fig. 8. Decay of the 2+ states in 240Pu and

a small 2+ lifetime component. In order to avoid these pile-up effects a thin aluminium
foil (0.02 mm) was placed between the source and the electron detector. In this way
the low-energetic electrons of the 2+ -+ O+ transition are prevented to reach the
detector while the 4+ + 2+ electrons loose only part of their energy.

Using the slope method the lifetime can be determined from that part of the time
spectrum where the prompt spectrum is negligibly small. Unfortunately the prompt

peak position is not known exactly because it depends on the energies of the radiations,
intensities, etc. Therefore we used the following method: first the value of the lifetime
was determined roughly by drawing a straight line through the experimental measuring
points. As the shape of the prompt spectrum is rather well known the shape of the
theoretical time spectrum for this rough z-value can be calculated. After that the slope
of the theoretical spectrum can be determined using parts of the time spectrum with
different starting points. In this way one obtains the range of the time spectrum which
can be used for the lifetime determination. In view of the effects mentioned in subsect.
2.4 the first three channels of the allowed range were not used in the analysis. It turned
out that within statistical error the roughly calculated lifetime value was always equal
to the final value.
The results of the lifetime measurements, together with the results of other authors,
are given in table 1.
Experimental results

Nucleus I E (keV) T+ (100 PS) Other authors

2+ 51.5 4.09*0.10 4 0 10.3 [ref 14)]

4:02*0.10 [ref. lo)]
4+ 186.6 1.69&0.07 1.61*0.05 [ref. I)]
2+ 43.5 2.52hO.07 2.66&0.20 [ref. 14)]
2f 45.3 2.35kO.06 2.32kO.20 [ref. 14)]
4+ 148.9 1.42hO.10
2+ 44.1 1.77 +0.05 183&O 15 [ref 14)]
2+ 42.9 1.64*0.05 1:73*0:15 [ref. 14)]
2+ 43.4 1.26f0.10

In the case of 24*Cm the lifetime is close to the limit imposed by the finite time
resolution. Therefore the error quoted is relatively large. Using the convolution
method we obtained a best fit for T+ = 125 ps, in agreement with the lifetime value
obtained from the slope.

3. Discussion

From the lifetime values the quantities B(E2), Q, and b were extracted. The results
for the 2+ states are shown in table 2. The total conversion coefficients were obtained
from the theoretical K and L conversion coefficients of Hager and Seltzer ) with
the assumption aMfN+... = 0.33~~ [refs. -)I. In the rare earth region this
assumption leads to agreement between experiment and theory to within 4 % [ref. )I.
In the heavy element region the experimental errors are somewhat higher ) and
therefore an error of 7 % in ur seems a reasonable choice.
In general good agreement exists between the results of lifetime measurements and
Coulomb excitation experiments. This is also true for other doubly even nuclei in
the heavy element region lo, 14*26, 29-32).
242 H. TON et al.

Values of the quantities B(E2), Qo and B.

Nucleus E aT T&+1 B(E2; 2+ -+ 0+) B(E2; QO in (b) B

(100PS) (e2 * b2) 2+ + o+)
(keV) Coulomb ext.

224Ra 84.5 21.2 7.48kO.20 0.79&0.06 6.3OhO.23 0.174 +0.007

=aTh 57.5 156 4.09*0.10 1.40f0.10 8.38hO.31 0.223 kO.008
234u 43.5 712 2.5210.07 2.0210.15 2.28f0.34 10.0710.38 0.225 &0.009
[ref. 26)]
[ref. 30)]
45.3 583 2.35*0.06 2.16k0.16 2.62f0.40 10.41*0.39 0.261&0.009
[ref. 26)]
[ref. 3o)]
*a*pu 44.1 780 1.7750.05 2.45kO.18 11.09*0.42 0.270&0.010
24OPu 42.9 885 1.64&0.05 2.68AO.20 2.58f0.06 11.60&0.44 0.281 +O.OlO
[ref. O)]
248Cm 43.4 988 1.26&0.10 2.94kO.31 12.1650.64 0.282+0.014


Fig. 9. Comparison of experimental and theoretical quadrupole moments of heavy doubly even nuclei.

In fig. 9 the experimental quadrupole moments are compared with the theoretical
predictions of Szymanski ) and Nilsson ). The main difference between these two
theories is a hexadecapole deformation term which has been taken into account by
Nilsson (.a4 # 0) and not by Szymanski (Ed = 0). Fig. 9 shows that the predictions
of Szymanski show better agreement with the experimental data.
For the nuclei *Th and 236U we have measured the lifetimes of both the 2+ and
4+ states. The corresponding values ratios B(E2; 4+ + 2+)/B(E2; 2+ -+ O+) are

*Th 1.4250.16,

Within the errors these values are in agreement with the rotational model predic-

Experimental values of B(E2; 4+ + 2+)/B(E2; 2+ + O+) in the rare earth and in the heavy element

Nucleus E(4+)/E(2+) B(E2; 4+ -+ 2+)/B(E2; 2+ -+ 0+) Refs.

%rn 3.01 l.lOf0.22 9

1s4Sm 3.26 1.4OhO.34
I-Gd 3.02 1.77&0.25 :;
l=Gd 3.24 1.35+0.11 9
=Gd 3.29 1.3210.13
16Dy 3.21 1.4OAO.23 :;
l=Dy 3.29 1.42hO.10 )
lG6Er 3.29 1.45f0.07 6.7

le8Er 3.31 1.47f0.07 6.7

*Hf 3.32 1.45f0.17 9
182W 3.29 1.24hO.12 9
184W 3.28 1.2810.12 9
186W 3.28 1.09+0.10
1860s 3.17 1.38hO.32 1;
l-03 3.08 1.4OhO.29 9
9OOs 2.93 1.19&0.24 9
lg*OS 2.31 1.1610.25 9

Th 3.24 1.4ObO.14 10
*24Ra 3.00 1.37h0.12 10:
=Th 3.23 1.42&0.16 present work
236U 3.29 1.27kO.16 present work

rotational model 3.33 1.43

Table 3 summarizes the known values of B(E2; 4+ --f 2+)/B(E2; 2+ + O+) for the
rare earth and the heavy element region. In general good agreement exists between
the experimental data and the rotational model prediction.

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