Jointly published by Journal of Radioanalytical and Nuclear Chemistry, Articles,

Elsevier Science S. A., Lausanne and Vol. 198, No. 1 (1995) 247-252
Akaddmiai Kiadt, BtMapest

Short Communications

CONTRIBUTION TO THE CYCLOTRON TARGETRY

IV. MEASUREMENT OF 18F, 21Na, AND 23Ne PRODUCTION YIELDS
IN DEUTERON INDUCED REACTION ON NEON GAS

F. HELUS, V. UHLIR, H. GASPER, W. MAIER-BORST

Deutsches Krebsforschungszentrum, Heidelberg (Germany)

(Received April 27, 1995)

The radionuclide 18F is of considerable interest for biochemical and physiological studies using
positron emission tomography (PET). Of all methods used for its production only two have found wide
application since their yield is high enough and the chemical form of the,product is suitable for
fluorination of organic compounds. Proton irradiation of enriched water using 1~ 8F reaction and
deuteron bombardment of gaseous neon 20Ne(d,001gF process are the commonly used effective
cyclotron production procedures. In our previous papers 1,2 the different reactions and target parameters
of the deuteron irradiation of neon gas were reported. In the present work, the production yields for the
(d,cz), (d,n) and (d,p) reactions were determined.

In practice, deuteron irradiation of neon gas produces 18F in the lSF[F2] chemical
form with a relative low specific activity because of addition of non-active stable 19F
carrier. The available nuclear data information and excitation functions concerning the
2~ process was until recently rather scarce.
Excitation functions of (d,cz) reaction - deuteron bombardment of neon - were
studied by GUILLAUME,3 NOZAKI,a and newly by BACKHAUSEN.5 His results are
cited by GANDARIUS-CRUZ and OKAMOTO. 6 Construction of excitation functions
according to systematic trends is not possible with sufficient accuracy in the region of
light nuclei with Z < 20. 7 However, by the deuteron irradiation of neon gas two other
reactions (d,n) and (d,p) take place. We have measured their saturation activity products.
The measurements of angular distribution and absolute cross sections and the
consequences from the physical measurements of simultaneous particle cross section
were not mentioned in the published radiochemical papers. These published data are
very important for understanding reaction processes and it is worthwhile considering
that aspect. The angular distributions of emited a-particles from (d,cx) reaction on ~'qe
leading to the ground states and several excited states of residual nuclei have been

0236-5731/95/US $ 9.50
Copyright 9 1995 Akad~miai Kiadt, Budapest
,4ll rights reserved
F. HELUS et al.: CONTRIBUTION TO THE CYCLOTRON TARGETRY, IV.

measured at an incident energy of 14.7 MeV by TAKAMATSU,s MORAND, 9 and

PESSOA. 10
Some published papers of yield figures and excitation functions do not make
differences between the production of lSF and all other short-lived coproduced
radionuclides and do not mention the time of measurement after the end of the
bombardment. Because of this fact and the different practice of measurement techniques
of originated activity, we decided to repeat the measurement of production yields in our
experimental target arrangement on our cyclotron facility.
Both older works cited above, in particular the GUILLAUME paper, 3 because of
lack of information have to be judged critically. NOZAKI4 used in experimental
arrangement a number of special cylinders connected" in series. The cylinders were
completely evacuated and then filled with neon gas. This method, first described by
CUMMING, 11 was adopted by other authors. The target assembly was bombarded with
the beam current which was measured by an integrator. The cylinders were measured,
each cylinder from both sides, with a multi-channel analyzer. The measured T-spectrums
were treated by COVELL's method and range - energy relationships were used for
calculation of beam energy in each position and the thick target yields. The main
disdvantage of the methOd ~t is that the calculated energies may have considerable
uncertainties, mainly in the last samples of the row, because of the superimposed errors
of the foil thickness.
GUILLAUME3 shows in his work the figure of excitation curve, however, in the
article, no notice is made of the experimental arrangement, measurement techniques and
calculation of data presented in the figure.
BACKHAUSENs measured excitation functions for the indirect formation of 18F via
its 1.67 sec 18Ne precurso r using stacked neon gas target. The cylindrical target system
was arranged and adjusted similar to a stacked foil system, mentioned by NOZAKI.
Silver coated cylinders were filled with neon at normal pressure.
Theoretical yield of 18F formed via deuteron irradiation of neon gas can be calculated
from the excitation functions measured and were published by authors mentioned
above.3,4 There are quite evident discrepancies between these calculations and
practical resulting activity. Later published measurement of excitation curves by
BACKHAUSEN5 and cited by OKAMOTO can not be compared with these3,4 results
published earlier.
Compariso n of differential yield data from different laboratories are somewhat
discrepant. The following parameters may have had influence on the published yield
figures: measurement technique, construction target material, parameter of targe body,
different energy absorbed in the target material (neon gas) and gas pressure, beam
current and current density, target gas temperature, humidity of the target gas and other
effects.

248
 F. HELUSet aL: CONTRIBUTIONTO THE CYCLOTRONTARGETRY,IV.

Experimental

The experimental approach and targetry for measuring the 18F formation cross
sections in the deuteron induced reaction is described in previous papers. 1,2 The beam
current was measured via Faraday cup as well as via monitor reactions. The monitoring
nuclear reaction 27Al(d,~tp)24Na was used for the accurate determination of the ion beam
current. The results obtained via monitor reactions agreed with the Faraday cup values
to within about 10%. The primary highest incident deuteron energy was 14.8 MeV of
the in steps chosen deuteron target initial energy. All experiments were carried out with
1 [.tA beam current, 7 minutes irradiation time, 6 mm collimator, under different target
pressures because of energy dependent particle range. Before starting the irradiation, the
target vessel was evacuated.
The main amount of the produced 18F is attached or bound to the walls of the target
vessel, or in our case on the used insert, and only a very small part (under 0.1%) of
produced 18F remain in the gas phase. Two traps close to the target are mounted in the
exhaust tubing system to capture the rest of 18F activity in gaseous phase carried away
with the neon gas.
The spatial distribution of the beam by different initial energy in the target was
observed using the quartz target in previous experiments. These results were used to
approximately extrapolate the dimension of the beam spot and in this way also the
optimal geometry (length and diameter) of target vessels.
The deuteron bombardinent was realized on the Heidelberg SC32 - NI cyclotron
(32 MeV H- and 15 MeV D3. The special target and target perifery was developed and
constructed in the workshop. For the measuring of the positron emitting produced 18F and
contaminants, a semiconductor 7-X-rays spectrometer with Ge(Li) detector and the
combination of two ionization chambers were used. The detection efficiency in
dependence on the detected photon energy was established by means of 7-elalons.

Results and discussion

After irradiation all originated activity was measured to calculate the total
balance of the products. Immediatelly after the EOB the gas phase passed through
the first trap containing ion exchanger papers for adsorbtion of 21Na, and then
passed into the evacuated second trap to catch the 23Ne. Both traps were placed
separately in an ionization chamber. Then the inserted aluminium foil was removed
from the target and measured. The measurement of the foil was repeated after
several hours to eliminate the influence of short lived co-produced activities, which
can originate in the inserted foil due to fast neutrons. The results are presented

249
F. HELUS et al.: CONTRIBUTION TO THE CYCLOTRON TARGETRY, IV.

4c- f
20-
j
10- ~
02 4 6 8 ~0 ~2 11 ;6 -"-
E(d)lMeV
Fig. I. 18F production yields

~20
~ 10G
- j

40

"2 4 6 8 10 12 14 16
E(d),MeV

Fig, 2. Saturation activities + 21Na; {3 23Ne

on Figs 1 and 2. Because of the very short half-life of 2~Na and 23Ne their saturation
activities are presented. In the case of 2~Na, the values were adjusted according to our
previous resultsJ 2 By 14.8 MeV initial target energy and 1 IxA beam current the
measured 18F production yield was 42 mCi/l.tAh (1.6.109 Bq]l.tAh).
Within the region of used deuteron energy, the activity values increased with the
energy. From the practice is known that firstly, the yield of the produced 18F in the
higher energy range (up to 15 MeV) is not directly proportional to the particle energy.
Secondly, the yield of the produced nuclide is not directly proportional to the used beam

250
 F. HELUS et al.: CONTRIBUTION TO THE CYCLOTRON TARGETRY, IV.

current. 13 Only up to certain beam current level can one expect linear increasing of the
production yield. Decisive for the total yield are the conditions of the plasma in the
irradiated gas phase (density and temperature). The gas densities along the beam axis
depend on both the energy loss per unit length and ion beam current, i.e., the dissipated
power in the gas. The dissipated power increases in tam the temperature of the gas.
Effects greater than 10% are seen for dissipated powers greater than 20 mW/mm.

Conclusions

Our measurements of the production yield (or thick target yields) contribute to the
~SF controversial question of 2~ reaction yield figures discussed and
published in last two decades. The advantage of our experimental procedure is that we
are able to measure the total yield of 18F produced via the 2~ reaction, and
saturation activities of co-produced 21Na and 23Ne.
It is very difficult to estimate exactly the excitation function for originated
radionuclides in a wide range of particle energy and beam current because of the
complicated state of plasma in the irradiated gas phase in the target. We have evaluated
the simple method using metal inserts for the measurement of 18F activity in the gas
target. To obtain absolutely exact excitation function, one needs experimental set up
used before by nuclear physics measurements and very low beam current of the
order- nA, because of beam slraggling, beam scattering (attenuation) and density
reduction. Only a part of the bombarded particles energy is used for the nuclear reaction
and production of the nuclide which is measured for the estimation of excitation
functions. The main part is involved in the excitation of atoms and molecules in higher
energy states of irradiated molecules while gas molecules are forced out of the beam in
a fashion proportionate to the beam current. Due to the above mentioned reasons we
estimated and presented the production yield as well as its practical use.

The operation of the Heidelberg Scanditronix MC32 NI compact cyclotron by G. WOLBER,

W. KONOWALCZYK, W. WEBER and J. REICHERT is gratefully acknowledged.

251
F. HELUS et al.: CONTRIBUTION TO THE CYCLOTRON TARGETRY, IV.

References

1. F. HELUS, V. UHLIR, et al., J. Radioanal. Nucl. Chem., 182 (1994) 237.

2. F. HELUS, V. UHLIR et al., J. Radioanal. Nucl. Chem., 182 (1994) 445.
3. M. GUILLAUME, Nucl. Instr. Methods, 136 (1976) 185.
4. T. NOZAKI, Int. J. Appl. Radioisotopes, 25 (1974) 393.
5. H. BACKHAUSEN, G. STOCKLIN, R. WEINREICH, Radiochim. Acta, 29 (1981) 1.
6. D. GANDARIUS-CRUZ, K. OKAMOTO, Report IAEA October 1988; INDC (NDS) - 209/GZ
7. K. A. KELLER, J. LANGE, H. MI3NZEL, in: LANDOLT-BI3RNSTEIN, Num. Data and Funct.
Relationship in Science and Technol., New Series, Group I, Vol. 5, Part c, Berlin, Heidelberg, New York,
1974.
8. K. TAKAMATSU, J. Phys. Soc. Japan, 17 (1962) No: 6, 896.
9. C. MORAND, H. BEAUMEVIEILLE, A DAUCHY, G. DUMAZET, M. LAMBERT, C. MEYNADIER,
I1Nuovo Cimento, 6A (1971) 380.
10. E. F. PESSOA, R. L. DANGLE, N. UETA, O. SALA, Nucl. Phys., 68 (1965) 337.
11. J. B. CUMMING, National Academy of Sciences, National Research Council, Nuclear Science Report
No. NAS NS-3107, 1962 (unpublished).
12. F. HELUS, V. UHLIR et al., J. Radioanal. Nucl. Chem., 196 (1995) 107.
13. M. OSELKA, J. E. GINDLER, A. M. FRIEDMAN, J. Appl. Rad. Isotopes, 28 (1977) 804.

252