Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41

The new photoactivation facility at the 4:3 MV Stuttgart

DYNAMITRON: setup, performance, and first applications
D. Belica, J. Bessererb, C. Arlandinic, J. de Boerb, J.J. Carrolld, J. Enderse,1,
T. Hartmanne, F. K.appelerc, H. Kaisere, U. Kneissla,*, M. Loeweb, H. Masera,
P. Mohre, P. von Neumann-Cosele, A. Norda,2, H.H. Pitza, A. Richtere,
M. Schumannc, S. Volze, A. Zilgese
a
Institut fur . Stuttgart, Allmandring 3, D-70569 Stuttgart, Germany
. Strahlenphysik, Universitat
b
Sektion Physik, Ludwig-Maximilians Universitat . Munchen,
. D-85748 Garching, Germany
c
. Kernphysik, Forschungszentrum Karlsruhe, D-76021 Karlsruhe, Germany
Institut fur
d
Department of Physics and Astronomy, Youngstown State University, Youngstown, OH 44555, USA
e
Institut fur . Darmstadt, D-64289 Darmstadt, Germany
. Kernphysik, Technische Universitat

Received 26 October 2000; accepted 16 November 2000

Abstract

At the Stuttgart 4:3 MV DYNAMITRON accelerator a new bremsstrahlung irradiation facility was installed for
photoactivation experiments to complement the well-established arrangement for systematic photon-scattering studies
taking advantage of the high photon fluxes achievable at this high-current accelerator. The population or depopulation
of isomeric states in low-energy photon-induced reactions ðEg ¼ 0:5–4:0 MeV) can be studied with sensitivities far
beyond previous limits. The setup of this facility, its performance, and the absolute calibrations are described in detail.
First exemplary results for a test case, the reaction 115 In ðg; g0 Þ 115m In, are presented and analyzed in combination with
data from low-energy photon-scattering experiments (115 In ðg; g0 Þ 115 In). The quality of the results demonstrates the
powerful capability of this new installation. # 2001 Elsevier Science B.V. All rights reserved.

PACS: 25.20.Dc; 23.20.g; 23.20.Lv; 27.70.þj

115
Keywords: Low-energy bremsstrahlung facilities; Photoactivation; Nuclear resonance fluorescence; Isometric states; In

1. Introduction

Investigations of long-lived isomeric states in

*Corresponding author. nuclei have a longstanding tradition in nuclear
E-mail address: kneissl@ifs.physik.uni-stuttgart.de spectroscopy. The long half-lives of isomers are
(U. Kneissl). caused by selection rules for the electromagnetic
1
Present address: NSCL, MSU, East Lansing, MI 48824,
USA.
decays of these excited states. Relative populations
2
Present address: Agilent Technologies Deutschland, of isomers in various nuclear reactions often were
.
D-71034 Boblingen, Germany. measured in the 1960’s and 1970’s to extract
0168-9002/01/$ - see front matter # 2001 Elsevier Science B.V. All rights reserved.
PII: S 0 1 6 8 - 9 0 0 2 ( 0 1 ) 0 0 2 2 5 - X
 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41
information on the spin dependence of the nuclear
level density following the Huizenga–Vanden-
bosch procedure [1]. In this context photonuclear
reactions were of special interest due to the low
transfer of angular momentum in photon-induced
reactions. Most of these studies were performed in
the energy range of the electric Giant Dipole
Resonance (GDR) or at higher photon energies. A
recent review [2] gives a comprehensive survey of
the investigations of isomers in photonuclear
reactions (mainly (g; xn)- or (g; xnf)-reactions).
At photon energies below the particle thresholds
(Eg 48 MeV) the studies of (g; g0 )-reactions suf-
fered in the past from the small cross-sections and
the lack of photon sources of high spectral
intensity. However, investigations of isomers in
low-energy photo-induced reactions (photoactiva-
tion) experienced an impressive revival during the
last decade due to the experimental progress
achieved and manifold physical motivations [3,4].
The population or depopulation of isomers by
resonant photoabsorption is also being considered
as a possible pumping scheme for a g-ray laser
[5,6]. The coupling between the ground state and
the isomeric level is of crucial astrophysical
importance for the understanding of the nucleo-
synthesis of several isotopes and for the test of
stellar models [7,8]. Last but not least, interesting
problems in nuclear structure physics can be
studied (see, e.g., Refs. [9–11]).
Isomers cannot be excited directly by real
photons from the ground state due to the limited
transfer of angular momentum in these reactions.
Hence, for the photo-induced population of
isomers intermediate states (IS) with a sufficient
ground state transition width G0 have to be excited
from the ground state. These IS can feed via g-
transitions and=or g-cascades the isomer. On the
other hand, in photon-scattering experiments
(Nuclear Resonance Fluorescence (NRF)) the
width ratio G20 =G (where G is the total width) can
be measured directly [12]. The combination of
both, photoactivation experiments and NRF-
investigations thus represents a unique tool for
nuclear structure investigations [13,14]. Both kinds
of photon-induced reaction studies can be per-
formed at the high-intensity bremsstrahlung beam
of the Stuttgart DYNAMITRON facility with
27
significantly improved sensitivities. In this article
the new irradiation facility is described, comple-
menting the existing NRF-setups [12]. First results
of photoactivation experiments and NRF-mea-
surements on the already extensively investigated
isotope 115 In, which served as a test case, are
presented to demonstrate the capabilities of the
combined techniques.
2. The photoactivation and photon-scattering
techniques using bremsstrahlung
Photoactivation and photon scattering off
bound nuclear states (NRF) share the principal
advantage of a well-known reaction mechanism.
Both the excitation- (photoabsorption) and deex-
citation-processes (electromagnetic decays) pro-
ceed via the well-known electromagnetic
interaction. Therefore, model independent infor-
mation can be extracted from both kinds of
experiments.
In photoactivation experiments the population
of an isomer has to proceed indirectly via the
resonant excitation of a higher-lying excited state,
a so-called intermediate state (IS), due to the large
difference between the spins of the ground state
and of the isomer. The decay of the IS can
subsequently feed the isomer via electromagnetic
decays (g-transitions or internal conversion pro-
cesses). The excitation energies and strengths of
the IS can be extracted from bremsstrahlung-
induced activation experiments by measuring the
activation yields YBS as a function of the
bremsstrahlung endpoint energy E0 . Since brems-
strahlung has a continuous energy spectrum, the
yields are given by the integral
Z E0
YBS ðE0 Þ  sðEg Þ NBS ðE0 ; Eg Þ dEg : ð1Þ
0
Here sðEg Þ is the total photoreaction cross-section
as a function of the excitation energy Eg .
NBS ðE0 ; Eg ) represents the continuous bremsstrah-
lung spectral density with an endpoint energy
E0 . The unquoted constant of proportionality
is determined by the usual quantities such as
target thickness, detector efficiencies and the
functions for the irradiation and counting times,
28 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41
respectively. Corresponding considerations hold
for the depopulation of long-lived isomers via
photoexcitation.
For a single IS, low-energy, thick-target brems-
strahlung spectra [15] give rise to a nearly linear
yield curve [16]. The onset of the yield curve is
given by the excitation energy of the first IS. Each
kink in the yield curve corresponds to the
excitation energy of a further IS. The change of
slope is proportional to the excitation strength of
the respective IS as shown schematically in Fig. 1,
assuming a hypothetical nucleus with IS at Ex ¼
1:2 and 1:9 MeV. Excitation energies and strengths
of IS, therefore, can be extracted from the
measured yield curves.
Unfortunately, the reputation of the photoacti-
vation technique was somewhat damaged in the
past due to contradictory conclusions drawn from
experiments with radioactive g-ray sources [17,18].
Fig. 1. Photoactivation of isomers using bremsstrahlung of
different endpoint energies (schematically). The population of
intermediate states (IS) can be inferred from the yield curve as
indicated in the bottom panel.
In the meanwhile, the possibility of so-called
nonresonant contributions to the photoactivation
of 115m In has been ruled out [19] (for a clarifying
discussion see also Ref. [20]). Furthermore, recent
complementary investigations of both, photoacti-
vation with bremsstrahlung of variable endpoint
energies and on-line NRF-experiments, as per-
formed by the Darmstadt group [13,14], showed
convincingly that the analysis of yield curves can
provide reliable data on IS energies and on the
corresponding integrated cross-sections. However,
it is essential for a correct analysis of the yield
curve that the experimental sensitivity is sufficient
to detect all low-lying IS or that the excitation
energies and strengths of unobserved IS are
known. Otherwise extracted cross-sections must
be considered as overestimated and are thus
questionable.
In NRF-experiments using continuous brems-
strahlung as a photon source all excited states with
a sufficient ground state decay width G0 are excited
simultaneously. Such experiments provide valu-
able data concerning the following spectroscopic
quantities: Precise excitation energies Ex can be
extracted from the spectra of the scattered
photons. The integrated cross-sections IS;0 are
proportional to G20 =G. Therefore, the ground-state
transition widths G0 , and the total widths G of the
excited states can be extracted from the scattering
intensities if all decay branchings are observed or
are known from other experiments. These quan-
tities can be converted into reduced transition
probabilities BðE1Þ "; BðM1Þ "; BðE2Þ " or life-
times t ¼ h=G. Angular-distribution measure-
ments provide the spins J of the photo-excited
levels (in the favourable cases of even–even nuclei).
Parities of the excited states can be determined by
measuring polarization observables, the linear
polarization of scattered photons via Compton
polarimetry [21] or the analyzing power when using
partially linearly polarized photons in the entrance
channel [22,23]. The formalism describing photon-
scattering experiments is summarized in previous
reviews [12,22].
Photoactivation and NRF-experiments comple-
ment each other in an ideal way. In NRF-
measurements the excitation energies and
strengths of the IS can be determined directly
 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41 29

and rather precisely, whereas the photoactivation methods. If the intermediate state can be observed
technique offers some unique advantages for in both the photon-scattering and photoactivation
investigations of the populations of the isomers. experiments, the ratio of the integrated cross-
In particular, a better sensitivity can be reached in sections directly provides the branching ratio Giso
most cases, due to the possible low-level, off-line =G0 without knowledge of the spin JIS and the
detection of the activation yields and due to higher total width G
photon fluxes at irradiation facilities as compared Iiso Giso
to the well-collimated narrow photon beams ¼ : ð6Þ
IS;0 G0
needed for NRF experiments. In photon scattering
the total intensity for elastic scattering integrated
over one resonance and the full solid angle is given
3. Experimental setup of the photoactivation
by
facility
 2
phc G0
IS;0 ¼ gJ G0 ð2Þ The new bremsstrahlung irradiation facility was
Ex G
installed recently at the Stuttgart DYNAMI-
where G0 and G are the ground-state and the total TRON accelerator for an improved study of the
transition widths and g is the statistical factor photoactivation of the famous 180 Ta isomer, a
depending on the ground state spin J0 and the spin reaction which is of crucial astrophysical relevance
J of the excited state to understand the nucleosynthesis of 180 Ta, nat-
2J þ 1 ure’s rarest stable isotope [24]. The general setup is
gJ ¼ : ð3Þ
2J0 þ 1 shown schematically in Fig. 2.
Therefore, mainly excited states with a predomi-
nant decay to the ground state (G0 =G 1) are
excited in NRF experiments.
On the other hand, in photoactivation experi-
ments IS can be detected with decay branchings
G0 =G51 which then populate the isomeric state.
Its characteristic decay can be observed out-of-
beam with little background. The new information
is the effective branching ratio Giso =G to the isomer
where Giso is the total isomer population width of
the IS. This interesting quantity can be determined
from the total detected activity Iiso which corre-
sponds to the integrated isomeric cross-section of
one IS (see, e.g. Ref. [4] and Refs. therein):
 2
phc Giso
Iiso ¼ ðs
GÞiso ¼ gIS G0 ð4Þ
Ex G
with the spin factor for the excitation of the
intermediate state (IS)
2JIS þ 1
gIS ¼ : ð5Þ
2J0 þ 1
The branching ratio Giso =G can normally not be
determined in NRF experiments. Therefore,
photoactivation and photon-scattering experi- Fig. 2. Experimental layout of the Stuttgart photoactivation
ments (NRF) are complementary spectroscopic facility.
30 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41

Typical DC electron currents of 400–450 mA can

be used on the watercooled bremsstrahlung
production target in the whole energy range of
interest (0.5–4 MeV). To achieve the highest
possible photon flux, the distance between the
bremsstrahlung radiator target and the sample to
be activated is only about 9 cm. The sample can be
transported to the activation position by a
remotely controlled worm-driven support.
Several different methods are applied to monitor
the photon-beam characteristics. After passing the
activation targets the photon beam travels through
a lead collimator to the NRF-sites where two
setups are operated simultaneously to determine
the photon flux, the shape of the bremsstrahlung
spectrum, and the bremsstrahlung endpoint en-
ergy. The first setup is equipped with two large
HPGe detectors, with relative efficiencies of 100% Fig. 3. The target area of the Stuttgart bremsstrahlung
(compared to a 300  300 NaI detector), looking at a irradiation facility in detail.
mixed target of isotopes with well-known excita-
tions in the energy range 0.5–4 MeV
(7 Li; 13 C; 19 F; 27 Al, and 63;65 Cu) to sample the the target as close as possible to the bremsstrah-
spectral shape of the bremsstrahlung spectrum and lung radiator. By this construction it was possible
to determine the photon flux [15]. The second to have a distance of 9:2 cm between the brems-
setup consists of a lead target viewed by a BGO- strahlung production target and the activation
shielded third HPGe detector with the same position to achieve the highest possible photon
performance and with an additional detector of flux. The worm drive is operated by a stepping
30% relative efficiency for the measurement of the motor, which is controlled by a remote PC in the
bremsstrahlung endpoint energy. At the end of the counting room to obtain identical target positions
photon beam-line the total photon flux is for a series of activation targets. The activation
measured by means of a thick-wall ionization targets are mounted in an aluminium support to
chamber. ensure good electrical and thermal contacts.
Fig. 3 shows the target area of the new photo-
activation facility in more detail.
The bremsstrahlung production target (conver- 4. Calibrations and performance
ter target) consists of a gold plate with a thickness
of 7 g=cm2 . This thickness guarantees the 4.1. Bremsstrahlung endpoint energy
complete stopping of the incident electrons. The
converter target has 10 boreholes (with diameters The bremsstrahlung endpoint energy corre-
of 1 mm) for an efficient water cooling, provided sponds to the kinetic energy of the electrons
by a special high pressure (50 bar) cooling circuit. provided by the accelerator. A first determination
The whole target body is electrically insulated to of the electron energy can be obtained from the
allow the monitoring and integration of the reading of the rotating voltmeter measuring the
electron beam current. The samples to be activated high voltage of the DYNAMITRON-generator
are transported by a target feeder from outside a with a relative precision of about 10–20 keV
massive concrete shielding to the activation posi- (uncertainties of the absolute scale are about
tion. The target holder is connected to a worm 50 keVÞ. Unfortunately, the analyzing magnet of
drive by a shaft, which allows a 458 kink to place the beam-transport system is not suited to act as a
 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41 31

momentum filter for electrons, since it is designed
for ion beams of much higher magnetic rigidity.
For electrons the weak fields and the strong effects
of the fringing fields prevent a precise momentum
analysis. Therefore, the spectra of scattered
photons taken with the two NRF-setups in the
experimental area are used to measure the end-
point energy and to monitor the shape of the
bremsstrahlung spectrum on-line.
At the second NRF-site (see Fig. 2) the incident
bremsstrahlung is scattered off a natural lead
target. This heavy element acts as a very efficient
nonresonant scatterer. Typical spectra of scattered
photons are depicted in Fig. 4.
In addition, the HPGe-detector is surrounded
by a BGO-Anti-Compton shield [25], mainly
acting as an active shielding against background
from natural activities and from cosmic rays. The
effect of the BGO-shield is clearly demonstrated in
the lower spectrum of Fig. 4. Above the endpoint
energy a suppression by a factor of about 15–20
can be achieved [25]. This suppression enables a
precise on-line determination of the endpoint
Fig. 4. Spectra of scattered photons from nat Pbðg; g0 ) taken
without (upper spectrum) and with Anti-Compton suppression
(lower spectrum). The ‘‘unsuppressed’’ spectrum has been
multiplied by a factor 10 in order to separate both spectra.
energy (30 keV). The background line at 2614
keV corresponds to the ground state transition of
the 3 state in 208 Pb. However, it should be
emphasized that this line comes from a natural
decay chain and is not due to a photoexcitation of
this E3 transition. In the suppressed spectrum,
furthermore, an 27 Al line (2982 keV) becomes
visible which can be used for additional absolute
energy calibration.
To verify the absolute calibration of the rotating
voltmeter, photon-scattering measurements were
performed at the first NRF-site using a mixed
target containing 27 Al and 13 C. These isotopes are
known to have low-lying states with large transi-
tion widths at 2982 and 3089 keV, respectively
[26,27]. Test measurements were performed at
energies corresponding to rotating voltmeter read-
ings of E0RVM ¼ 3109 and 3130 keV. The results
are shown in Fig. 5. At 3109 keV (see upper panel)
the endpoint energy is obviously not high enough
to excite the 13 C level (at 3089 keV) but is sufficient
for excitation of the 2982 keV level in 27 Al. The
corresponding g-transition dominates the very
Fig. 5. Spectra of photons scattered off a mixed target contain-
ing 27 Al and 13 C. Upper panel: Bremsstrahlung endpoint energy
corresponding to a rotating voltmeter reading of
E0RVM ¼ 3:109 MeV. Lower panel: Corresponding spectrum at
E0RVM ¼ 3:130 MeV, where the peak attributed to 13 C appears.
32 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41
clean spectrum. When increasing the energy by
only 21 keV the excitation of the 3089 keV level in
13
C clearly can be observed (see lower spectrum,
taken for a somewhat shorter collection time).
Using the known scattering cross-sections [26,27],
the absolute endpoint energy can be determined
with a precision of better than 20 keV from these
results. Combining all data obtained with these
different methods, the uncertainties in the quoted
endpoint energies should be of the order of
20 keV.
4.2. Shape of the bremsstrahlung spectra, absolute
photon flux
The measurement of the shape of continuous
electron bremsstrahlung spectra represents an
experimentally difficult task, in particular for
low-energy, thick-target bremsstrahlung. The use
of scintillator- or Ge–g-spectrometers [28] suffers
from the fact that the measured pulse height
spectra have to be unfolded and a precise knowl-
edge of the response matrix of the spectrometers is
needed for this procedure. The application of the
associated particle techniques using the photodi-
sintegration of the deuteron (spectroscopy of the
protons [29] or neutrons [30] in this two-body
break-up of known kinematics) is rather time
consuming and not practicable at low energies
(Eg 44 MeV). Magnetic spectrometers (Compton-
or pair spectrometers) provide very precise brems-
strahlung shape data [31]. Since such devices are
very difficult to install in the narrow geometry of
the Stuttgart irradiation facility, a simple techni-
que is applied, well established in nearly all recent
low-energy NRF studies. Simultaneously with the
photoactivations, NRF experiments were per-
formed on isotopes with low-lying, strong dipole
excitations of well known transition strengths (7 Li,
13
C, 19 F, 27 Al, and 63;65 Cu) [15,16]. From the
measured scattering intensities the incident photon
flux at the corresponding excitation energies can
then be determined. The continuous bremsstrah-
lung shape is sampled by these measurements
which, in addition, allow to check Monte-Carlo
simulations (using GEANT or EGS codes). In
Fig. 6 the results of a Monte-Carlo simulation
using the GEANT code (version 3.21) of a
Fig. 6. Shape and absolute flux of a bremsstrahlung spectrum
(E0 ¼ 3:1 MeV) calculated by Monte-Carlo simulations using
the code GEANT in comparison with experimental data from
photon-scattering experiments off a mixed target containing 13 C
and 27 Al.
bremsstrahlung spectrum with endpoint energy E0
¼ 3:1 MeV are compared with the data from NRF
experiments on a mixed target containing 13 C and
27
Al, showing good overall agreement.
In addition, the total photon flux is monitored
during the experiments by a thick-walled ioniza-
tion chamber [32] at the end of the photon beam
line (see Fig. 2). The reading of the ionization
chamber is compared with the electron current
incident on the insulated bremsstrahlung produc-
tion target. The ratio between the measured total
photon flux and the incident electron current
represents a crucial check for optimal electron
beam adjustment. During the 180m Ta-activation
experiments [24] 115 In has been activated simulta-
neously to serve as a further reference for the
absolute photon flux.
5. Detector systems
After the irradiation the activated samples can
be measured off-line in a separate counting room.
Fig. 7 shows schematically the setup used in the
180m
Ta activation experiments [24] for the detec-
tion of characteristic X-rays and low-energy g-
quanta. It consists of two planar low-energy Ge
photon detectors (LEP’s) facing each other.
Typical dimensions of the LEP crystals were a
diameter of 52 mm and a sensitive volume of
 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41
Fig. 7. The low-level X-ray counting system consisting of two
well-shielded LEP-Ge detectors, used in off-line measurements.
42 cm3 . Backgrounds were efficiently reduced by a
sophisticated shielding made of high-purity copper
and lead. The excellent energy resolution of about
470 eV at 55 keV enabled the separation of the Ka1
(55.79 keV) and Ka2 (54.61 keV) X-ray lines of
180
Hf following the EC-decay of the 180 Ta ground
state. The relative efficiencies of the detectors were
determined using a 133 Ba g-source. At 59.5 keV the
absolute efficiencies were measured by means of a
calibrated 241 Am source. Due to the narrow
geometry of the setup total absolute efficiencies
of about 20 and 28% (at 55 keV) could be
achieved for both detectors, respectively. The
estimated relative systematic uncertainties of these
values are below 10%.
For the 115 In activation experiments the
LEP-detectors were replaced by a high-purity
Ge–g-detector for the detection of the 336 keV
g-transition depopulating the 4.49 h isomer in
115
In. The relative efficiencies of the detectors used
in the various experiments amounted to 30 and
38%, respectively (compared to a 300  300 NaI
scintillation counter, at the 60 Co energy of
1.33 MeV). The energy dependence of the efficien-
cies was measured with radioactive sources (60 Co,
133
Ba, 152 Eu, and 228 Th). At 336 keV the total
absolute detection efficiencies were 8 and 11.5%
for the two detectors, respectively. For compar-
33
Fig. 8. Low-energy level scheme of 115
In (simplified version
from Ref. [33]).
ison, the corresponding values for the 1.33 MeV
line of the 60 Co decay were about 2 and 3%,
respectively. The estimated relative errors of the
determined absolute efficiencies are of the order of
12%.
115
6. First applications: Test case In
The isotope 115 In represents a nearly ideal case
for the application of the photoactivation techni-
que. Its first excited, isomeric state at 336 keV has
spin J p ¼ 1=2 and a half-life of t1=2 ¼ 4:49 h,
whereas the ground state (J p ¼ 9=2þ ) is practically
stable with a half-life of 4:41  1014 years. The
isomer decays with a relative probability of 45.8%
by an M4 336 keV g-transition to the ground state
(see the simplified low-energy level scheme in
Fig. 8 [33]).
Therefore, the population of the isomer is rather
easy to detect by g-spectroscopy. Furthermore, the
34 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41

level scheme of 115 In is well known in the low- perfect agreement with the kinks observed in the
energy part and all spectroscopic information on photoactivation yield curves. In addition, by
possible intermediate states is available [34]. For comparison with calculations in the framework
these reasons the 115 In isomer was chosen in the of the unified-model the structure of these IS could
present study as a test case, first to prove the be explained and the excitations characterized as
performance of the new Stuttgart irradiation M1 spin-flip transitions. The total yield curve
facility and secondly to check the reliability of could be well described up to about 4.6 MeV by
the analysis of bremsstrahlung-induced photoacti- adding a total integrated cross-section of about
vation data. After demonstrating the reliable 1 eV b (calculated from literature data) due to
analysis of the 115 In photoactivation data, the 115 unobserved IS’s at excitation energies below
In ðg; g0 Þ 115m In reaction can in turn be used as an 2 MeV.
115
independent photon-flux monitor in other photo- Low-energy NRF-experiments on In
activation experiments and for the verification of (Eg 43 MeV) were performed in 1969 by Alston
Monte-Carlo simulations of thick-target brems- [37]. Subsequent photon-scattering and photon
strahlung spectra [15,16]. self-absorption experiments (Eg 42 MeV) [38,39]
mainly provided the spectroscopic information on
6.1. Previous photoactivation and photon-scattering low-lying states in 115 In which were interpreted by
experiments on 115 In most authors as the corresponding IS in the
photoactivation process [17–19]. In a detailed
A sensitive photoactivation experiment on 115 In NRF-study by the Darmstadt group [40] a total
was performed already in 1967 by Booth et al. [35] of 32 transitions were observed up to an excitation
using an intense electron beam of a Van de Graaff energy of 5 MeV in fair agreement with the older
accelerator (up to about 150 mA). The population data [37–39] in the low-energy range (41:5 MeV).
of the isomer in 115 In could be detected down to
endpoint energies of about 1 MeV. Furthermore,
6.2. Present results of the 115 Inðg; g0 Þ115m In
the authors compared photon- and inclusive
photoactivation experiments
electron-induced yields to extract information
on the multipolarities involved in the excitation
6.2.1. g-spectra and half-life
within the virtual photon concept [36]. Later
Fig. 9 shows a typical g-spectrum taken for a
photoactivation experiments using radioactive
sample of natural In (16 mm diameter, 0.2 mm
sources (60 Co) [17,18] also assigned the 1078 keV
level as the most important low-energy IS, but
disagreed in the conclusions concerning the
population mechanism. A subsequent experiment
using bremsstrahlung of variable endpoint energy
[19] ruled out the claimed ‘‘non-resonant process’’
[17]. In Ref. [19] the integrated cross-sections for
the low-energy photoactivation of 115m In through
the 1078 keV level (J p ¼ 5=2þ ) are summarized, as
obtained in various previous experiments using
bremsstrahlung or 60 Co sources.
At higher excitation energies (Ex 52 MeV) large
integrated photoactivation cross-sections for
115m
In were found in improved experiments
performed at the S-DALINAC at Darmstadt
Fig. 9. Observed g-spectrum of a natural In-sample bombarded
[13,16]. Furthermore, two groups of strong excita- with bremsstrahlung of 3.1 MeV endpoint energy demonstrat-
tions around 2.8 and 3.3 MeV were detected in ing the sensitivity of the activation experiment (note the
complementary photon-scattering experiments in logarithmic ordinate scale, explanations see text).
 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41
thickness) bombarded with bremsstrahlung of an
endpoint energy of 3.1 MeV. The very clean
spectrum is dominated by the 336 keV line
corresponding to the M4 transition from the
isomeric state in 115 In to the ground state.
Furthermore, a clear line at 392 keV is evident
which is due to the M4 transition from the 1.658 h
J p ¼ 1=2 isomer in 113 In [41], which has an
abundance of 4.3% in natural In. The extreme
sensitivity which could be reached at the new
Stuttgart irradiation facility is demonstrated by
the detection of a weak line at 497 keV which
stems from a transition in 115 Sn. The correspond-
ing level is populated with a probability of only
4:7  104 in the b -decay of the 115 In isomer.
Special care was taken to observe the lowest IS
in the photoactivation of 115 In. At the lowest
endpoint energy of 0.92 MeV used in the present
investigations no activation could be detected (top
panel of Fig. 10).
The clear onset of the photoactivation was
observed starting from an endpoint energy of
0:96 MeV. As shown by the clean spectrum of
good statistics in the lowest part of Fig. 10, the
Fig. 10. The onset of photoactivation of the 115 In isomer at
0:934 MeV, illustrated by g-spectra for endpoint energies of
0.92, 0.99, and 1:2 MeV.
35
photoactivation of 115m In can easily be detected at
higher bremsstrahlung endpoint energies.
The detected activities were also characterized
by their half-lives. In Fig. 11 the results for a
natural In sample bombarded with bremsstrah-
lung of 3.8 MeV are depicted.
The upper curve shows the decay curve of the
336 keV g-transition depopulating the 4.49 h
115m
In isomer. The middle curve represents the
392 keV g-transition associated with the decay of
the 1.658 h isomer in 113 In ð113 In occurs with an
abundance of only 4.3% in the natural In). The
lowest data show the decay curve of the 497 keV
state in 115 Sn which is fed by the b -decay of the
115
In isomer with the very low relative branching
of 4:7  104 . The solid curves represent least
squares fits to the experimental data. The mea-
sured half-lives t1=2 are summarized in Table 1
with statistical uncertainties corresponding to
standard deviations.
Fig. 11. Measured decay curves after photoactivation of a
natural In sample using bremsstrahlung with an endpoint
energy of 3.8 MeV (for explanations see text). The isotopes and
half-lives are indicated at each decay curve. Note that the 113m In
data were multiplied by a factor of 10 in order to separate the
curves.
36 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41

Table 1 groundstate via an E2 excitation and exhibits a

Measured half-lives t1=2 of the isomers in 115 In and 113
In in 11.4% decay branching to the isomeric state at
comparison with the literature values [34,41]
336 keV via a g–g cascade through the 597 keV
Isomer Detected g-Transition Half-life t1=2 Literature value level (see Fig. 8). The level at 934 keV with its
115m 115 small 0.5% decay branch to the isomer gives only
In 336 keV in In 4.487(4) h 4.486(4) h
497 keV in 115
Sn 4.1(2) h a small contribution to the population of the
113m
In 392 keV in 113
In 1.63(1) h 1.6582(6) h isomer.
The next observed clear kink in the yield curve
at about 1.08 MeV is marked by an arrow in the
left part of Fig. 12 and is most probably due to the
The results are in good agreement with data excitation of the 5=2þ state at 1.078 MeV. At
from Refs. [34,41]. The sensitivity of the present higher energies further breaks could be detected at
photoactivation experiments even allowed to im- about 1.49, 1.61, 1.98, 2.42, and 2.95 MeV. In
prove the value for the b -decay branch of the Table 2 the identified IS and their integrated cross-
115
In isomer of 4:9ð4Þ  104 as compared to the sections Iiso are summarized.
literature value of 4:7ð7Þ  104 [42]. The error of The values for the energies EIS and the
the present result is mainly due to the uncertainty integrated cross-sections Iiso were obtained from
of the intensity of the 336 keV g-transition fits to the linear sections of the yield curve. The
((45:8  2:2)% per decay) [42]. uncertainties of the EIS are of the order of 30 keV.
The errors of the integrated cross-sections are
6.2.2. Yield curves, deduced intermediate-state dominated by the systematical ones due to the
energies and integrated cross-sections absolute calibrations, in particular the one of the
Activation yields were measured between 0.92 photon flux. Furthermore, the systematical errors
and 3.1 MeV. Fig. 12 shows the measured relative increase considerably for the higher-lying IS due to
yields, normalized to the number of incident error propagation in the yield curve analysis.
electrons and the respective irradiation times, as
a function of the bremsstrahlung endpoint energy.
The onset of the photoactivation was observed at a
Table 2
bremsstrahlung endpoint energy of about Intermediate states (IS) observed in the photoactivation of
0.99 MeV. Since the low-energy excitation scheme 115m
In, their properties, and assigned levels
of 115 In is well known, the corresponding first
EIS Intermediate states Assigned levels
essential IS should be ascribed to be the 5=2þ state
(keV)
at 0.941 MeV which can be populated from the Iiso Ex Jp
ðeV
bÞ (keV) ð h Þ

940 0:0084  ð0:0004Þstat:  934 7=2þ

ð0:0023Þsyst:
941 5=2þ
1085 0:140  ð0:001Þstat:  ð0:04Þsyst: 1078 11=2þ
1490 0:78  ð0:06Þstat:  ð0:21Þsyst: 1449 9=2þ
1463 7=2þ
1487 9=2þ
1497 7=2þ
1610 0:25  ð0:05Þstat:  ð0:07Þsyst: 1602 7=2þ
1608 7=2þ
1980 1:12  ð0:08Þstat:  ð0:31Þsyst:
Fig. 12. Observed yield curves for the photoactivation of the 2420 1:83  ð0:13Þstat:  ð0:50Þsyst:
115
In isomer. Left panel: Endpoint energies E0 41:3 MeV. Right 2950 3:10  ð0:42Þstat:  ð0:85Þsyst:
panel: E0 51:2 MeV.
 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41 37

Therefore, statistical and systematical errors are

quoted separately in Table 2.
For the lower-lying IS known levels can be
proposed as most probable candidates for these IS.
These levels are given in the right part of the Table
2. Due to the limited energy resolution in the yield
curve analysis and the increased level density at
higher excitation energies, no unambiguous assign-
ments of the IS can be given above about 2 MeV.

6.3. Results of the present 115

Inðg; g0 Þ115 In NRF-
experiments

Complementary low-energy photon-scattering

experiments (NRF) have also been performed at
the Stuttgart bremsstrahlung facility [12]. The
main aim of these measurements was to identify
and to pin down directly the lowest intermediate
states (IS) responsible for the low-energy photo-
activation of 115m In. To increase the sensitivity at
low energies and to get information on a possible
feeding of low-lying states, two measurements
were carried out using bremsstrahlung endpoint
energies of 1.3 and 1:8 MeV, respectively. In view
of the existing NRF data at higher energies
reported by the Darmstadt group [40] no NRF
measurements at higher bremsstrahlung endpoint
energies were performed within the present work.
A natural indium target, which contains 95.7%
of 115 In, was used with a total mass of 3:2 g.
Fig. 13 shows part of the spectra of scattered
photons measured in the NRF experiment on nat In
using bremsstrahlung endpoint energies of 1.8 and
1:3 MeV, respectively.
The spectra are dominated by the strong M1
excitation of the 1133 keV level. However, besides
several labelled peaks from photon-flux calibration
targets (Cu, F) [27] or background lines (bg, 40 K),
a peak at 1078 keV could clearly be detected
(marked by an arrow) in both spectra, correspond-
ing to the 5=2þ level in 115 In. It can be excited from
the 9=2þ ground state by an E2 transition. This
level is the most important one in low-energy
photoactivation. The excitation of the 1291 keV
level could be observed only in the E0 ¼ 1:8 MeV
measurement since its excitation energy is too close
to the endpoint energy of the 1:3 MeV measure-
ment. Further known levels in 115 In could be
Fig. 13. Photon-scattering spectra observed in on-line NRF
experiments ð115 In ðg; g0 Þ 115 In). Upper part: Endpoint energy
E0 ¼ 1:8 MeV. Lower part: Endpoint energy E0 ¼ 1:3 MeV.
detected at higher excitation energies as given in
Table 3. Unfortunately, the excitation of the 0:94
1 MeV level as the first IS could not be detected,
due to its small ground state decay width [34] and
the larger background contributions at low photon
energies. Calculating the integrated scattering
cross-section IS;0 from the known half-life of 15:1
ps and the decay branching ratio [34] a value of
IS;0 ¼ 0:063 eV b is obtained which is below the
detection limit (IS;0 40:28 eV bÞ achievable in the
present NRF experiments at excitation energies
around 1 MeV (see Fig. 14). The detection limit
was estimated by requiring an area of a hypothe-
tical peak larger than 2 standard deviations of the
neighbouring background. The results of the
present photon-scattering experiments are sum-
marized in Table 3.
7. Discussion
7.1. Photoactivation cross-sections
In Table 4 the integrated cross-sections Iiso of
low-lying IS (EIS 43 MeV) observed in the present
38 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41

Table 3
Results of the present 115 In ðg; g0 Þ 115 In NRF experiments (bremsstrahlung endpoint energy E0 ¼ 1:8 MeV) and comparison with data
from previous NRF experiments: Excitation energies Ex (uncertainties 41 keV), integrated elastic resonance-scattering cross-sections
IS;0 , and the width ratios gJ G20 =G. The literature values are calculated from lifetimes and decay branchings compiled in Ref. [34]. The
spin factor gJ can be calculated for known spins: gJ ¼ ð2J þ 1Þ=ð2J0 þ 1Þ

Ex IS;0 gJ G20 =G
(keV) (eV b) (meV)

This work This work This work Ref. [37] Ref. [38] Ref. [39] Ref. [40] Literature ½34

934 40:28 40.07 0.22(1) 0.0063(7)

941 40.28 40.07 0.015(1)
1078 0.81(13)a 0.25(4) 0.31(9) 0.159(24) 0.42(15) 0.19(2)
1.11(21)b 0.33(6)
1133 29.0(45) 9.7(15) 6.3(11) 6.3(6) 8.59(48) 9.4(7) 8.42(39)
1291 3.79(59) 1.64(26) 1.35(35) 0.95(44) 1.31(11) 1.2(3) 1.46(16)
1449 2.07(34) 1.13(18) 0.7(2) 0.91(38) 0.90(11) 1.7(4) 0.94(18)
1485 1.18(20) 0.68(12) 0.88(22) 0.63(9) 0.8(21) 0.66(15)
1497 3.03(48) 1.77(28) 1.6(6) 1.33(16) 0.49(18) 1.31(15)
1602 0.96(24) 0.64(16)
1607 2.90(63) 1.95(42) 1.0(3) 1.58(29)
a
From the measurement with E0 ¼ 1:3 MeV.
b
From the measurement with E0 ¼ 1:8 MeV and corrected for feeding by using the known decay branching of the 1607 keV level
from literature [34].

integrated cross-sections Iiso given for the present

min
Fig. 14. Detection limit IS;0 in the present NRF experiments
using an endpoint energy E0 ¼ 1:3 MeV.
115
In photoactivation experiments are compared
with results from previous bremsstrahlung-in-
duced photoactivation measurements [13,35] and
literature data which were calculated using known
lifetimes and decay branching data as given in a
recent compilation [34].
The estimated uncertainties in the energies EIS
as deduced from the yield-curve analysis can be
estimated to be about 30 keV. The errors for the
data are obtained by linear addition of the
statistical errors and the larger systematical errors
(see Table 2). The systematical errors were
conservatively estimated by linear summation of
the uncertainties of the photon flux (10%), of the
absolute photon-detector efficiency (12%), and of
the conversion coefficient of the 336 keV transition
(5%) [42].
The present results are in good agreement with
the previous low-energy data of Booth et al. [35] as
well as with the literature values obtained using the
full spectroscopic information known for the low-
energy excitation scheme of 115 In [34]. This
documents the reliability of the present measure-
ments and analysis.
The somewhat higher cross-section value for an
IS at about 2:8 MeV reported recently [13] can be
explained since this experiment started at brems-
strahlung endpoint energies E0 52 MeV. The
contributions from lower-lying IS were calculated
from older literature data [43], which did not
include, however, the IS’s at about 1.98 and 2:4
MeV observed in the present work.
 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41 39

7.2. Photon-scattering cross-sections
The results of the present 115 In ðg; g0 ) photon-
scattering experiments are compared in Table 3 to
previous experimental NRF work and literature
values calculated from lifetimes and decay branch-
ings taken from the most recent compilation [34].
The comparison of the extracted quantities
gJ G20 =G which are proportional to the reduced
excitation probabilities BðPLÞ " shows a good
overall agreement. The weak excitation at 1602
keV could be detected for the first time in an NRF
experiment, although the corresponding 1602 keV
state had been observed already in (n; n0 g)-studies
[46]. On the other hand, the level at 1:463 MeV,
partially reported in previous photon-scattering
experiments [38–40] could not be detected in the
present experiments due to the strong background
contribution of the 40 K-line at 1460:8 keV [42] (see
Fig. 13).
7.3. Comparison of photoactivation and
photon-scattering data
The results from the present photoactivation
and photon-scattering experiments were combined
to extract the interesting branching ratios Giso =G0 .
These can be deduced from the measured photon-
scattering cross-section IS;0 and photoactivation
cross-sections Iiso (see Section 2). In Table 5 the
results of this analysis are summarized and
compared to literature values calculated from
known spectroscopic data as compiled in Ref. [34].
Where the excitation of several states can
contribute to the measured activation cross-section
a mean branching ratio Giso =G0 , given by the ratio
of the summed activation and scattering cross-
sections, is quoted in the comparison with the
literature data [34] (last column of Table 5). A fair
overall agreement is observed.
8. Conclusions and outlook
The photoactivation and photon-scattering ex-
periments on 115 In performed at the new brems-
strahlung photoactivation facility at the Stuttgart
DYNAMITRON served as a test for the reliability
and sensitivity of combined photon-scattering and
photoactivation experiments and their analysis.
The isotope 115 In was chosen since its 336 keV
ðt1=2 ¼ 4:49 hÞ isomer is the best studied example

Table 4
115m
Properties of low-lying intermediate states (IS) (EIS 43 MeV) observed by photoactivation of In. The literature values are
calculated from lifetimes and decay branchings compiled in Ref. [34]

EIS Iiso EIS Iiso EIS Iiso Ex Iiso

(MeV) ðeV
bÞ (MeV) ðeV
bÞ (MeV) ðeV
bÞ (MeV) ðeV
bÞ

This worka Ref. [35] Ref. [13] Literature [34]

0.934 0.00014(2)
0.94 0.0084(27) 0.935 0.0085(40) 0.941 0.0072(8)
1.085 0.140(41) 1.08 0.115(40) 1.078 0.119(8)
1.449 0.0029(5)
1.463 0.091(15)
1.486 0.006(1)
1.49 0.78(27) 1.45 0.59(20) 1.497 0.629(74)
1.602 ?
1.61 0.25(12) 1.57 0.25(15) 1.608 0.165(30)
1.98 1.12(39)
2.42 1.83(63)
2.95 3.1(13) 2.80 5.7(11)
a
The errors of the present data from this work are obtained by linear summation of statistical and systematical errors (see Table 2
and text).
40 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41

Table 5
Comparison of the results from the present 115 In ðg; g0 Þ 115m In photoactivation investigations and 115 In ðg; g0 Þ 115 In NRF experiments to
data from Ref. [34]

EIS G0
Giso =G Ex gj G20 =G gj Giso =G0
(keV) (meV) (keV) (meV) (%)

This work Ref. [34] This work Ref. [34] This work Ref. [34]

0.032(3) 934 40.065 0.006(1) 0.51(7)

1.7(2) 941 40.065 0.015(1) 11.4(17)
940 1.9(1) 1.7(2) 40.130 0.021(2) 51.5 8.1(11)
a
1085 43(4) 36(3) 0.27(3) 0.19(2) 15.7(19) 18.8(22)
1.6(3) 1449 1.13(18) 0.94(18) 0.17(4)
51(8) 1463
3(1) 1486 0.68(12) 0.66(15) 0.48(16)
367(43) 1497 1.77(28) 1.31(15) 28.0(47)
1490 450(32) 422(44) 3.58(35) 2.90(28) 12.6(15) 14.5(21)
1602 0.64(16)
111(20) 1608 1.95(42) 1.58(29) 7.1(18)
1610 169(34) 111(20) 2.59(45) 1.58(29) 6.5(17) 7.1(18)
a
Weighted mean of the results from the measurements using bremsstrahlung endpoint energies of 1.3 and 1:8 MeV.

in previous photoactivation experiments. In addi-
tion, the low-energy level scheme of 115 In is well
known [34], allowing for a crucial, rather indepen-
dent cross-check of the data extracted from the
present experiments. The good agreement with the
values calculated from known lifetimes and
branching ratios [34] gives confidence for future
results from combined photoactivation and
photon-scattering experiments. Furthermore, the
115
In ðg; g0 Þ 115m In reaction can be taken as a
reliable photon-flux monitor reaction in experiments
using low-energy bremsstrahlung photon sources.
The availability of high-flux DC bremsstrahlung
photon beams and of photon spectrometers of
high efficiency and excellent energy resolution
enables a new generation of both, photoactivation
and photon-scattering experiments. At the Stutt-
gart DYNAMITRON accelerator photoactivation
experiments can be performed with 50–100 times
better sensitivities than before, even without the
use of enriched targets. This experimental progress
allows to investigate the population (or depopula-
tion) of isomers down to excitation energies of
about 1 MeV. Thus, it is possible, in particular in
combination with low-energy, high-sensitivity
NRF experiments, to pin down all intermediate
states, to measure their excitation strengths and
for the first time their decay branching Giso =G0 . By
combining the complementary methods of photo-
activation and photon-scattering experiments the
population scheme of the isomers can be clarified.
Furthermore, with the advanced, present-day
sensitivity astrophysically relevant problems like
the effective half-lives of low-lying isomers under
stellar conditions can be tackled experimentally
[7,8,44,45]. The addressed interesting physics and
the recent experimental developments will open a
wide field of applications for low-energy photo-
induced reaction studies and will guarantee a
promising future of these techniques.
Acknowledgements
The authors wish to thank Prof. Dr. G. Sletten
.
and Prof. Dr. C. Gunther for lending the LEP-
detectors used in the experiments. The support by
the Deutsche Forschungsgemeinschaft under Con-
tract Nos. Kn 154=30, FOR 272=2-1, by the
Munich Tandem Accelerator Laboratory, by US
AFOSR under contract F49020-99-1-0263 and FZ
Karlsruhe is gratefully acknowledged.
 D. Belic et al. / Nuclear Instruments and Methods in Physics Research A 463 (2001) 26–41
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