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Deposition by thermal evaporation of thin films of titanium and zirconium for tritium targets

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1959 Br. J. Appl. Phys. 10 91

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 Deposition
- by thermal evaporation of thin films of titanium and
zirconium for tritium targets
~y V. D. SCOTT,BSc., and L. W. OWES, BSc., Atomic Weapons Research Establishment, Aldermaston, Berks.
[Paperjivst received 25 May, and in “finalform 19 September, 19581
Equipment and procedure are described for applying thin films of titanium and zirconium as
tritium carriers to backings of copper, gold and platinum. A large proportion of the coatings
prepared absorbed high atom ratios of tritium, titanium being more satisfactory in this respect
than zirconium. It is suggested that defects in the coating arise mainly from the undesirable
reaction of the metals with residual gases, particularly oxygen, during evaporation in the vacuum
chamber. Firstly, this causes stress, brittleness. and owing to lack of adhesion, blistering of the
deposit; secondly absorption of tritium is inhibited by the oxide film on the metal surface, and
the total amount absorbed reduced as a result of there being fewer lattice sites available for the
tritium. An electron diffraction examination showed that although the deposits appeared
bright and metallic, a thin protective oxide film was present on the evaporated titanium and
zirconium.

When tritium is bombarded with protons or deuterons a deposited was determined by weight. Electron diffraction
Source of neutrons is obtained. In order to achieve a compact studies of the deposits were carried out using target blanks
source of tritium, it is preferably absorbed in a metal which of 1 cm diameter, reducing rings being fitted into the target
has a high affinity for the gas, such as titaniilm or zirconium. support to accommodate them.
ways in which such targets may be prepared have been
described by Graves, Roderigues, Goldblatt and Meyer.(’)
Since the bombarding particles can penetrate only a very
limited thickness of the target material, tritium absorbed to
a greater depth is ineffective. Thus thin films of metals
with a high afinity for tritium deposited on some other
non-absorbent metal achieve the object with the maximum
of economy of tritium. The production of targets by the
thermal evaporation of thin films of zirconium has been
described by Arrol, Wilson and Evans,(’) and by Lillie and
Conner.(j)
The apparatus and method is extended here, with certain
modificatiom, to include titanium as well as zirconium.
The principal causes for failure of the targets is discussed in
detail.
EXPERIMENTAL DETAILS

Conventional high-vacuum evaporation equipment was

used, provision being made to allow the entry of hydrogen,
or another gas, into the work chamber (Fig. 1). The tungsten
fdament on to which the metal charge was bound with fine
tungsten wire, was reduced in diameter either side of the
source to produce hotter regions during the passage of
cufient. T h a , the titanium or zirconium was prevented Fig. 1. Arrangement of components inside work chamber
h e n molten from flowing to cooler regions nearer the A , bel!-jar; B, water-cooled baseplate; C, rubber L-gasket;
electrodes. For tile production of thicker deposits, two D,metal chamber; E, tungsten evaporator filament for sup-
identical evaporation sources were included. In addition to porting and heating charge; F, heavy copper connexions;
the use of the metal radiation shields shown in the diagram, G, copper upright; H, water-cooled electrode: J, metal charge;
K, thinned portions; L,targets; M , target support; N, heating
heating of the bell-jar was further reduced by coating the element for tarpts; P, thermocouple; Q, lower radiation
interior with a reflecting layer of aluminium, which at the shield; R, upper radiation shield.
high temperatures involved in the evaporation did not
restrict visual observation during the deposition. Formerly, RESULTS
outgassing of components and metal deposition were accom-
plished with a single evacuation using moveable shields (a) Asserrwent of targets. Bright metallic-looking films of
operated by rotary seals. However, in order to obtain the titanium and zirconium were obtained on copper, goid,
best possible vacuum with this equipment the shields were nickel and platinum backings by the above method.
omitted. The procedure was therefore performed in stages, Roughening of the surface and prolonged outgassing treat-
the apparatus being allowed to cool each time before opening ment appeared to have beneficial effects on adhesion of the
the chamber to the atmosphere. film.
Target blanks, 1$ in. in diameter were prepared by abrasive Over 95% of titanium targets were accepted for impreg-
treatment on 000 emery paper foliowed by degreasing in nation, the coating thicknesses ranging from the equivalent
benzene vapour, and given prolonged outgassing treatment of 50 to 2500 pg cm2, and giving Brehmstrahlung counts
commencing.~deposition. The thickness of metal from 100 to over 1000 counts/s. Atom ratios of titanium:
VOL. 10, FEBRUARY 1959 91 BRITISH JOURNAL OF APPLIED PHYSICS
 V. D. Scott and L. W. owen
tritium better than 1 : 1 were frequently obtained without A zirconium deposit showed either the face-centred cubic
(U = 5.08 A), Or the tetragonal (CIR =)5I'.' dioxide (See
obvious flaking of the deposit, and exceptionally up to a
ratio of I : 2. Fig. 3). it was not possible to distinguish which of these
With zirconium, approximately 20% of the targets were zirconium dioxide modifications occurred owing to ring
of poor appearance and were lacking in adhesion. Thick- broadening. A blue-coloured deposit, obtained when air
ntsses produced ranged from the equivalent of 50 to was admitted too soon after evaporation onto the hot speci-
500 pg/cm2, according to requirements. In general, blistering men, also gave this pattern. Zirconium nitride was not
of the deposits usually occurred when impregnation had observed.
reached an atom ratio of nearly I : 1. DISCUSSION
(b) Electron difroction study. A reflection electron
diffraction pattern from the evaporated titanium deposit Two principle causes for failure of the coating were flaking
(Fig. 2) indicates a face-centred cubic structure with a latticeof the deposit from the backing and low absorption of
parameter of 4.28 A (calibration with graphite powder, tritium. These defects are considered to arise mainly from
dllo = 1-230A). Arcing of the diffraction rings (Fig. 1) the reaction of the evaporated metal with residual oxygen,
shows (111) and (100) one-degree orientation. and probably nitrogen, in the evacuated space of the bell jar,
At the commencerr-nt nf-~~poration there is an appreciable
drop in pressure suggesting gottering action and it seems
fairly certain that initially a film is deposited relatively rich
in oxide. This film may be lacking in cohesion, but is almost
certainly of poor mechanical properties and constitutes a
barrier to obtaining sound adhesion. Continued deposition
of titanium and zirconium would occur with less reaction
with residual gases however, depending upon the leak rate
and the pumping speed of the system, etc. The total gas
absorbed during evaporation is considered to determine the
efficiency with which tritium is absorbed since the oxygen
would take up lattice sites otherwise available for tritium.
Since very small amounts of oxygen rendered titanium and
zirconium brittle, the extent of gas reactions occurring
throughout the deposition would clearly affect the brittleness
Fig. 2. Titanium monoxide on evaporated titanium
film, showing (111) and (100) orientation of the coating. As adhesion is likely to be poor, brittleness
becomes a more important factor since cracking of the film
would lead to spalling. Cracking and spalling of the film
Available thermodynamical datac4) indicates that this thin could be initiated by stress induced as a result of the different
surface film on the titanium deposits is the monoxide, with thermal expansion coeficient of the substrate. Stress in the
little, if any, nitride present; also the occurrence of nitride film should be minimized by keeping evaporation and
surfam fi1ms appears Only to have been reported after impregnation temperatures fairly low, the target temperature
heating the specimens to above about 'OO" c ' ( 5 * 6The )
during evaporation being preferably about one half of that
experimental conditions in the oxidation work of Conjeaud(') employed for impregnation.
can perhaps be usefu11ycompared with the present work. It is clearly desirable to restrict the time of deposition
His electron diffraction study of thin single-crystal films of since there would be less reaction with the residual gases in
a-titanium, oxidized in air at a pressure of 2.10-2mm of the chamber, but in practice the rate of evaporation is
mercury, showed the formation of titanium monoxide at limited to that which does not endanger filament burn-out.
3000 ' a mixture Of anatase and rutile above 400" ' and The oriented patterns of titanium monoxide observed in
only rutile above 550" C. the electron diffraction examination of the films indicated
The presenm Of Other Oxide forms was not Observed at this
staw Of the 'peration* Introduction Of hydrogen into the that the oxide was formed while it was hot, i.e. immediately
after evaporation in the vacuum system, and not later during
system immediately after evaporation did not appear to cooling i n vacuum or when air was introduced onto the
affect this fi1m' nor did heat treatment up to 300" c in cooled targets. Exposure of the titanium target to air for
hydrogen gas at a pressure Of a few mi11imetres Of mercuv* several weeks did nc: :kZt.;: the nature of this oxide film,
neither was the oxide film upon zirconium affected by a
similar time interval between evaporation and impregnation.
These observations indicate that special storage precautions
are unnecessary for the freshly-evaporated targets awaiting
impregnation.
Electron diffraction studies on evaporated zirconium films
revealed the presence of zirconium dioxide but not the
monoclinic form observed by Hickman and Gulbransed')
when heating zirconium and some alloys.

ACKNOWLEDGEMENTS

The authors wish to thank Mr. W. B. H. Lord, Senior

Superintendent of Metallurgy, Atomic Weapons Research
Fig. 3. Zirconium dioxide on evaporated zirconium Establishment, Aldermaston, Berkshire, who directed the
film work, fdr his advice and suggestions.
nniiisn JVUHNAL VP APPLIED PHYSICS 92 VOL. 10, FEBRUARY
1959
 Deposition by thermal evaporation of thin films of titanium and zirconium for tritium targets
REFERENCES (4) HUMPHREY, G. L. J. Amer. Chem. Soc., 73, p. 1587
(!I GRAVES$ E. R., RoDERIGUES, *.A.,
MEYER,D. T. Rev. Sei. Insrvum., 20 (1938).
(1951); 73, p. 2261 (1951).
M., and (5) RICHARDSON, L. S., and GRANT,N. J. Trans. Amer.
Inst. Min. (Metall.) Engrs, 200, p. 69 (1954).
(2) ARROL, W. J., WILSON,E. J., and EVANS,c. Atomic (6) WASILEWSKI, R. J., and KEHL, G. L. Metallurgia 50,
Energy Research Establishment Internal Report 1135 p. 225 (1954).
(1955). (7) CONJEAUD, P. J . Recherches du C.N.R.S., 32, p. 213
(1955).
(3) LILLIE, A. B., and CONKER, J. P. Rev. Sei. Instrum., 22, (8) HICKMAN, J. W., and GULBRANSEN, E. A. J. Analyt.
p. 210 (1951). Chem., 20, p. 158 (1948).

Experimental determination of the atomising efficiency of a

high-speed spinning disk atomiser
By D. J. RYLEY,M.Sc.(Eng.), A.M.I.Mech.E., Department of Mechanical Engineering, University of Liverpool
[Paperfirst received 3 July, and in final form 17 August, 19581
Electrically driven disks of 3 and 5 cm diameter were rotated at speeds 20 000-60 000 rev/min, and
samples of an aqueous spray were analysed for flow rates of 0.12, 0.42 and 0.77 cm3/s. The
reduction in disk speed during atomising was determined experimentally using an electronic
pulse counter and a miniature dynamometer was devised to simulate this reduction and measure
the power consumed. Atomising efficiencies for the electrically driven disk thus obtained are
compared briefly with the,efficiency employing air drive and also with that of a simple pressure
atomiser. In all cases efficiencies are less than 0.5 %.

LIST O F S Y M B O L S to axcomplish subdivision. In the spinning disk atomiser

U = surface tension (dyn/cm)
d = Sauter mean diameter of droplet
g = gravitational constant (cm/s2)
D = disk diameter (cm) ~
the latter is difficult to assess by an analytical method. The
test liquid is normally fed vertically on to the centre of the
(cm)
disk and spreads evenly outwards being finally disrupted on
leaving the edgc. i r is not possible to analyse hydrodyna-

radius of disk shank (cm)
Y =
N = w/2n = disk speed (revis)
a; w = tension in brake band (g)
E = Young's modulus (g/cm2)
I = second moment of area (cm4)
I, L = cantilever free length (cm)
y, Y = cantilever deflexion (cm)
Q = flow rate of test liquid (cm3/s)
p = density (g/cm3)
p = pressure (gicm?)
p = viscosity (poise)
7 = nozzle efficiency
y = isentropic index for air
n = number of droplets
Sibscripts
1 = Reservoir conditions of air
2 = Expanded conditions of air
1NTRODUCTION
in any atomising device the energy usefully employed is
[hat which reappears as new surface created. Neglecting,
therefore, any energy associated with the production of
electrostatic charges, the useful energy may be regarded as
the product of the surface tension and the extension in area,
i.e.
Useful energy = 6a/d ergs/cm3
(1)
The efficiency of an atomisation process may be defined
'0 several ways, but fundamentally should be considered to
be the ratio of the energy in the newly created surface to the
imparted to the liquid by the atomising device employed
VOL. 10, FEBRUARY 1959
mically the motion of the water across the disk as the distri-
butions of radial and circumferential velocities are unknown.
The vertical velocity profile will also be a function of the
liquid velocity, of the air drag on the free surface and probably
of the disk surface texture inasmuch as slipping may occur.
It would seem, however, a fair first assumption that for low
flow rates the liquid is flung with a ve!ocity equal to the
circumferential velocity of the disk rim. If this be allowed
+
Liquid energy = (nDN)' ergs/g (2)
and the efficiency of atomisation might be defined as
Efficiency = 1 2 a j ( ~ D N ) ~ d (3)
The uncertainty associated with the assumption underlying
equation ( 2 ) couid be avoided if it were possible to measure
directly the power absorbed by the disk as it assumes its
liquid load. Atternpts have been made by other workers to
estimate the atomising efficiency by measuring the total
power input to an electric motor driving the atomiser, but
this is clearly unsatisfactory as the power measured includes
the normal friction and motor losses. The power required
for atomisation is small and may be only a minor fraction of
the total; and it is not possible to separate the effects with
any accuracy.
To measure the atomising power directly the method which
suggests as promising is to Observe the speed
reduction consequent upon application of the atomising load
and then to employ a suitable brake on the disk when dry to
accomplish the same speed reduction; the brake being capable
of measuring at the same time the power required. There
are, however, two major difficulties to be overcome, (a) the
speed reduction is extremely small for normal atomising
loads and has to be measured accurately for subsequent
93 BRITISH JOURNAL OF APPLIED PHYSICS