Prog. Cwstol Growth and Charact 199% Vol. 13.pp. 197-229. 0146493Lsa So.

00 + so
Printed in Grsst Britain.All rightarsrsrved. CopyrlghfC,PsrgamonJournals Ltd.

ACRT: A REVIEW OF MODELS

J. C. Brice, P. Capper, C. L. Jones* and J. J. G. Gosney*
Philips Research Laboratories, Redhill, Surrey RHl 5HA, U.K. and lMullard
Southampton, Millbrook, Southampton, Hants, U.K.

/Received 22nd August 1986/

ABSTRACT

The accelerated crucible rotation technique produces fluid, thermal and mass flows in sealed
and open crucibles. Optimum use of the mathod is only possible when these flows can ba
quantified. This paper reviews work on the theoretical models which have been used to
describe the flows and presents a set of models which is sufficient to describe the flows
which occur in most of the situations which are likely to occur in crystal growth systems.

1. INTRODUCTION

Fluid flow occurs in a liquid inside a cylindrical container which is rotated about its axis
at deliberately veried rates. This accelerated crucible rotation technique (ACRT) can be used
to produce stirring in sealed containera and is thus potentially useful for crystal growth.
However, to exploit the method in an optimum way, it is necessary to bs able to describe the
flow in the system in reasonable detail. Thls is not easy. Even just looking at the
mathematics involved (sea for example Teman 111 or Ladyzhenskaya [2]) is enough to discourage
most people. Reading these and other relevant texts makes it clear that the problem really is
complicated. However, after a great deal of work which can be traced back for at least 100
years, there is enough theoretical and experimental evidence to give a picture which Includes
all the main factors and which gives numerical results which should not bs in error by more
than a factor of two and which in most cares are probably correct to about 10%. This paper is
an attempt to present that picture or at least those parts of it which are relevant to crystal
growth.

There are three regimes which xust be described:

(a) When small accelerations are used, essentially only axially sysasetric azimuthal flow is
produced. This does not enhance either solute or heat flow but if there is an
appredable radial gradient of the fluid rotation rate (i.e. significant shear) the
symmetry of the heat and ~SWS flow will ba increased. This is a useful effect because
lack of syasaetry particularly when the directions of the flows change with tie leads to
inhomogeneity in the crystals produced.

(b) For moderate accelerations, significant axial and radial flovs occur and these enhance
maes and heat transport which is the usual aim of atrempcs to stir growth systems. In
the case of ACRT. the stirred volume for moderato accelerations is restricted to a
region near to the base of the column. The height of this region varies with the
conditions used but it is important to remember that the flow near to the base does not
mix with flow occurring in the upper regions of long columns of liquids. The flow in
system of this type are axially symmetric.

197
198 J. C. Brice et a/.

Cc) For large accelerations, the flows become unstable and asymmetric. Again, what happens
depends on height above the base. The region near to the base is stable to higher
accelerations than regions remote from the base. Our interest in unstable flow is
largely restricted to defining the conditions under which it will occur. However,
unstable flow does produce good (even if time dependent) mixing and it can be
advantageous to use ACRT with the top of the column in unstable flow but with stable
flow near to the base. The conditions for this are given later.

Section 2 of this paper discusses the flows in these regimes and outlines the notation used.
Later sections then discuss the various regimes in detail. However. before turning to these
topics, some background information should be given.

Readable accounts of the basic ideas of fluid mechanics are given by Batchelor [3] and Cole
141. The works of Levich [51, Goldstein [61 and Schlichting [7] give much useful information
but the most relevant monograph is by Greenspan [81. When it is necessary to consider the
stability of the flows, the book by Chandrasekhar [9] is the best source. In what follows
references to Batchelor [3], Greenspan [El and Chandrasekhar [9] are denoted respectively by
B, G and C followed by a section number.

While a number of workers used methods which seem to have been essentially ACRT for flux
growth from about 1960, the first clear published reference seems to be due to Zaitsov et al
[lOI in 1968. The process was named by Scheel and Schulz-Dubois [ll] in 1971 and the ideas
involved were developed both experimentally [12] and theoretically [13] in 1972. Since
that date there has been a steady series of papers 114-181 and reviews [19-221 dealing mostly
with flux growth. The method has also been applied to zone refining [22], Bridgman growth
123-261 and crystal pulling [27-321. A number of other ctyetal growth studies have also been
published, for example 133-351 and there is a large literature relating to fields outside
crystal growth. These non-crystal growth papers are mentioned when they are needed to
illuminate areas not yet studied in a crystal growth context.

2. THE FLOWREGIMESOF INTEREST

2.1 The System Considered and the Notation Used

Figure 1 shows the system which is of interest. This is a crucible wfth a radius a (cm)
filled to a depth H (cm) with fluid. The origin of the coordinates r and z is the centre of

Fig. 1 The system considered which comprises a crucible filled to a depth H with
a liquid column of diameter 2a (full line) or having a conical base
(broken line). Note that the centre of the base is the origin of the
coordinate system.
 ACRT: a review of models 199

The crucible rotates at a rate Cc and step changes in S& are written hn,. .\ gr?nerl: ilslid
particle has an absolute rotation rate iI and a rotation rate relstive to :::e c?~ci-Le ,J? Y.
The absolute velocities of the particle are U radially, U vertically and :’ %zi:~:t-i:l:l. Rates
relative to the crucible are u, w and v respectively but, of course, u - ‘i’ and Y - 4.

A number of dimensionless parameters are commonly used to describe such systems. These are:

(a) The Prandtl number

Pr - v/k

where k is the thermal diffusivity (cm 2 s -1) and v is the kinematic viscosity (cm2s-1).

(b) The Schmidt number

SC = V/D (2)
where D is the diffusion constant (cm2s-1).

Cc) The Reynolds number for which

Re - a2@J&/v

is our normal definition and when use is made of a Reynolds number which does not match this
definition, other symbols are used.

The other widely used symbols are 5E. 6T and 6, which are respectively the Ekman
(momentum) boundary layer thickness (cm), the thermal boundary layer thickness and the
diffusion boundary layer thickness. All these layers are those on the base of the crucible.
Other symbols are defined as required.

2.2 The Effects of Small Accelerations

If the system is rotating at a uniform rate and a small change of rotation -7, is imposed, it
is -easy to see what will happen at levels remote from the base. If the change is a decrease,
the crucible rotates slower than the liquid. Liquid near to the wall is decelerated and at
any subsequent time we find a rotation rate gradient which dies away with time. Figure 2
shows what happens. This figure is drawn for the case when the final rotation rate is zero
and the characteristic time ?D is a2/14.86V. .Bn the line for a time 0.57~ the dotted
extension gives a simple model which we shall use. Figure 3 shows this model. In the upper
part the model is shown by the full line and the broken line shows what really happens. The
lower part of the -figure shows how the shear develops. Figure 4 makes it clear that the shear
will destray any non-axially symmetric pattern. Thus this flow will make symmetric any
non-sxially symmetric heat or solute flow patterns, provided that TR exceeds the time for s
few revolutions. From Figure 2 it is clear that for times greater than about 2Tp very
Little happens.

The process described here Is spfn-down. An increase in rotation rate (spin-up) produces very
similar effects. If we spin-down to a state other then rest or sptn-up from a non-zero
rotation rate essentially the same thfngs happen but the time constants are changed.

Near to the crucible base small amounts of radial and axial flow are produced but the large
effect is azimuthal shear flow. The extra damping produced by the base decreases YR as
discussed later.

If we think in terms of a step change in rotation rate and the Reynolds number defined by
equation (3). The low acceleration region corresponds to Re values below some limit which we
expect to be of the order of IO.

In come systems, we do not change ?, in a step-like way. We cope with continuous changes by
assumfng that Cl, varies as

0, - fioo+ no sin mt
200 J. C. Brice et al.

Fig. 2 Rotation

/f
rates at various times fn a crucible spun-down to rest

u
‘\
Actual
rate

a R 0 R a

Fig. 3 A simple model of spin-down.

 ACM: a review of models 201

t=o t =atAR,

t * 2rclAR, t = 47cIAR,

Fig. 4 Fluid distribution changes in spin-down.

It is then possible to model any perfodic motion in terms of m and its harmonics when m is
given by

111 = 277/T (5)

where T is the period of the motion. It will be shown later that the range of harmonics of
interest is rather small and if we choose the fundamental rate appropriately, we shall not be
interested in many harmonics. Just aa we can &fine the low acceleration region in terms of
Re for step changes, we expect a limit defined in terms of m and 0, which actually is that for
the low acceleratfon region:

n, < m/277 (6)

These limits are discussed in the next sub-section.

202 J. C. Brice ef al.

2.3 The Effects of Moderate Acceleration

Uith moderate accelerations, the flows remote from the crucible base are unchanged. For this
statement to be really true, remote means that z exceeds 20a but the statement is nearly
correct for z z 3a. Hovever, near to the crucible base there are appreciable radial and axial
flows. See Figure 5 which shows half of the bottom of a crucible. These flows are
established at the base in a time of about l/L& and decay at a rate 7~. They propagate

--

,_----_
‘1
I’ I

:
I tfttt tt
I
\\ .
I

11111 \
I
t‘\I ut I4 I
I

17 /
‘_-+_s’
-
-c 6E
*

Fig. 5 Flows near the base of the crucible. Note that only the right-hand half
appears on the figure.

from the base with a velocity which for a step change is (I&V)+ immediately after the
change and at later times is about (&?cv)+axp(-t/q)). When ?D is large, this gives a
spreading time H/(Af?,v)j for a column of height H. Because the flow decays there is a
distance z max past vhich the flow never penetrates. This distance is

Zmax = [_ (@k>)+exp(-t/rD)dt

The radial flow at the crucible base creates a momentum boundary layer vith a
thickness

6E = (“IL&)+

immediately after the change. We can define moderate accelerations as being ones such that

% < zmax (
i.e.
(V/t&)+ C (~+“)+TD (11)

which reduces to

dc)cT~ > 1 (12)

or since TD - a2/15Li

(13)
 ACAT: a review of models 203

If we take into account the fact that we expect & to increase with time so that

(14)
we should increase (13) by a factor a and obtain

Re * 40 (15)

aa the definition of the lower limit of erujerate acceleration. There aust also be an upper
limit which is given by the onset of instability. The limit derived in the next sub-section
is that
Rc s 270 (16)

for the onset of the first instability. However, as will be shown, this lowest instability
need not be a disaster and we expect to work with I&r up to sons larger limit (possible 500 or
more).

Crystal growers are not really interested in momentum boundary layers. However, the values of
6E are readily converted to 6D and ST by multiplying by an appropriate function so that

60 - GEf(SC) (17)

and

6T - dgf(yr) (18)

The function f(N) is given in Table 1. This table is adapted from the one for a rotating disc
but there is no obvious reason why it should not apply to the cases considered here.

Tsble I The Values of f(N)

N f(N)

co.05 0.7012(N)-’

0.05 14.3

0.10 8.06

0.20 4.59

0.50 2.42

1 .o 1.56

2 .o 1.08

5.0 0.725

10.0 0.546

20 .o 0.415

50.0 0.291

100 0.229
200 0.174

1 .000Nl/3

Uncertainties in f(N) are * 1% except for the limiting values which are accurate to f 0.2%.

2.4 The Effects of Large Accelerations

The subject of flow stability is complex and is considered in detail in Section 6. Here we
need only to consider the least stable part of en ACRT cycle i.e. spin-down. At positions
remote from the bottom of the crucible. transient vortex formation occurs when Re exceeds
204 J.C. &ice eta/.

about 270. See Figure 6. When Re exceeds about 500, these annular vortices persist for (L
significant fraction of the spin-down period And significantly decrease TB. Also, with
Re >-500 vortices form near to the crucible base. At still larger values of Re. the axes of
the vortices cease to be planar rings and the flow becomes time dependent. (The are.9 are not
only wavelike but also move up and down.) When Re reAches A few thousand. spin-up becomes
unstable And the boundary layer at the crucible base is also unstable.

Fig. 6 Flow near to the base of A crucible and the instabilities which appear
higher in the crucible when Re > 272.

3. STABLE FLOWS REMOTE FROM THE BASE WITH STEP CHANCES

We are interested only in Azimuthal flows. Cases in which there are radial and axial flows
are dealt with in Section 6 which describes flows with large values of Re. As shown in the
Appendix, the equation of interest is

a&d+?& law
= --
(19)
r ar v at
ar2

which can be solved [361

e =‘-x (20)

for spin-up from rest. While for spin-down to rest the solution is

= x (21)
g
where

Ii
J,(ccnr/a)exp(-a~"t/=')
x = 2 (22)
II=1 anJo
 ACRT: a review of models 205

and the a,, are eolutfone of

Jl(nn) - 0 (23)

so that “n successively taker the values 0, 3.8317, 7.0156, 10.1735. 13.3237, 16.4706 etc. and
for n s 6. or,+1 - on - 3.15. The solutions to this equation for spin-down are shown in Figure
2. Batchelor lB4.51 derives essentially the same result from a elightly different starting
point. Figure 7 curve b shows how this solution behwee in terms of the model shown in
Pigure 3.

O.‘b b_\ iO.0”

ot.--$.~~o.,,

0.1 0.2 0.3

tv/a2

Fig. 7 The radius R of the. “solid” cylinder in spin-down for (a) the diffusion
model, (b) P rigorous model and (c) for the simple model discussed in the
text. E is the fraction of the initial energy which remains in the
system.

As the Appendix suggests, we can also, with some slight errors, solve this problem in terms of
s diffusion equation (Al.71 by replacing D byv. This gives solutions in equation (20) with

= Jo(anr/a)ex~(-a~“t/a~)
X = 2 (24)
t UnJ, (a,)
n-1

where the a,, are roots of

Jo(+) _ 0 (25)

i.e. the a, are successively 2.4048, 5.5201, 8.6537, 11.7915, 14.9309, 18.0711 and for larger
IL) on+1 - on w 3.14. This solution fe derived in [37 pp 198-2011. Curve a on Figure 7
compares this rolution with the previoue one ahown by mrve b. It can be seen that the
differences are likely to be negligible. This approach allows us to use the solutions for
finite- cylindore for vhieh wp find [37 pp 225-2271 that

ca m
(-l)“Jo(~r)cos[(2n+l)rrx/ZHlexp(-Y)
x-$ (26)
(2n+l)amJ, (amr)
206 J. C. &ice et al.

where

Y - ,vt[(o,&a*) + (211+1)*,*/48*] (27)

and the or, are solutions of

Jo(%) - 0 (28)

Compare with (25).

It is notevorthy that many authors quote values of rD deduced from the first terms of a
series of solution. When this is done, we find:

(a) From (22)

TD - a2/14.68;1 (29)

(b) From (24)

‘D - Gl5.7av (30)

(c) From (27)

TD - [(5.78/a*) + (9.87/g*)I-lv-1 (31)

However, taking a reasonable number of terms reduces the differences between the time
constants from the factor of about 2.5 suggested by (29) and (30) to about 12% when the decay
is about 63% complete. See Figure 7.

If we accept the model in Figure 3. we can treat the system as being composed of two coaxial
cylinders of which the inner one has a diameter which changes with time. This model was first
shown to be valid from calculations and simulations conducted using various fluids in
different,sised containers [24]. Couette flows were observed to follow the criterion of a
wide gap between the two ‘cylinders’ when H >> a (see Figure 8). This is an extremely useful

o.voo3
0.01

v 0.039
0 0.02
x 0.01
0 0.003

Container radius (cm)

Fig. a Variation of critical rotation rate with container radius and fluid
kinematic viscosity (-) predicted curves, (--_) experimental curves
(after [241).
 ACRT: a review of models 207

model vhfch ve ahnll use again in Section 6. It allows us to treat spin-down by cozwidering
the energy of the inner cylinder and the couple exerted on this cylinder by the viscous
f orccs. Referring to Figure 3, this couple (~4.51 has a argnitudc per unit length

c - 4P’J4/(R-2 - a-2) (32)

for spin-down to rest the kinetic energy of the inner cylinder is

E - xoA$ 2[(~4/4) + {.a4 + R(a-R)(2a2 + 5aR + 6R2)1/60] (33)

ThP rate of energy change with R is dR/dR and the coupls consumes energy at a rate Z?&. Thus
. . .
we can deduce tnat

I
2
dR
_-=- 240~ y + s(l-Y2)
dt 2 (34)
a c-2Sy=-9y4+22y3+7y2+6y+2

where y - R/a and for uov s - 0. (The parameter s comes from cousideration of the couple due
to viscous forces acting across the Ekman layer at the base and

s - a2/8R6g (35))

Prom equation (34) we can deduce the variation of R/a with time shown in Figure 7 by the full
line C which is for s - 0. This gives a value of TD of about l 2/l6.7v where the comparable
values for the other lines on Figure 7 are about a2/14.6~ and a2/12.5v. All the models agree
reasonabLy wall out to times of about 2TR which is really the limit of our interest. At
later times there vi11 be lfttle mixing of any kind. These models can probably all be
regarded as valid in this time range and have been tested. See for example 1361. The tests
show that they are valid in spin-up to Re - 700 and in spin-down to about 300. For greater
Re, the damping is much greater than the first two models predict. The third model can be
extended explicitly to take.account of the flows in the Ekman layer. Equation (35) assumes an
Ekman layer but does not take account of the flew through it. When this extra source of
damping is considered, the value of s is doubled. If we further consider the flows up and
down the side wall, a further correction is needed and we arrive at a value of 8 vhich is
about

8 - a2(bnc)+/3H(V)+ (36)

This extended model appears to be reasonable to me m 600 in spin-down and to Re - 2000 or more
in spin-up. Table 2 gives the values of the time ‘190 for the cylinder to decrease in diameter
to one tenth its original size, i.e. roughly the equivalent of 2TB. Note that the model is
further generalised in the next section.

4. STABLE FLOWSNEAR TO THE BASE.WITli STEP CHANCES

In the previous eection we discussed azimuthal flows for spin-up from rest and spin-down to
rest. In practice we may well wish to describe flow which involve end states vhich are not
rest. There seem to bs no models capable of dealing with step changes which reverse the sign
of the rotation, i.e. we cannot describe rotation reversal. It is actually likely that
rotation reversal will produce unstable flows. However , ve can easily discuss general changes
fromfil ton2 in terms of the third model discuseed in the previous section. Repeating all
the algebra is not necessary because the simple general result is that the values of ?B are
multfplied by a factor

J - (Cl + Q)/( IRl - Q2 I) (37)

Turning now to consider flows uear to the base, the first important result is that for
moderate accelerations e boundary layer is formed on the crucible base. This has an initial
thickness

SE - (v/AQina)+ (38)

where a is the cone angle defined on Figure 1. In most cases a - 90’ so that SE is given by

(v/A@ (39)
$ -
208 J. C. Brice et al.

Table 2 Decay Tfmes to y - 0.1

0 0.163
0.0003 0.15
0.003 0.13
0.03 0.11
0.05 0.095
0.1 0.075
0.2 0.058
0.3 0.048
0.5 0.037
1 0.025
2 0.016
3 0.012
5 0.069
10 0.043
>lO 0.045/s

initially. At later times we should rmltiply h by aXp(t/rB) to allow for the decay of
the flow. Here t is the time from the rotation change. The effective value of &E is the
reciprocal of tba average of l/k which is roughly

&Eeff _ T(~/hn~)t/~~[l-exp(-T/rg)l (40)

which makes it obvious that for effective stirring we want the period (T) between changes to
be reasonably small. Bowever, T should not be too small because it takes a time T, to
establish the layer. This time Is about

re - o.75/Klc (41)

and for effective stirring T >> Te is necessary.

After a time re the flow near to a flat base is given by

U - u = r~cexp[-(hnCIV)~s)sfn[(~c/v)~z] (42)

v - r~cexp~-~hnclV)fzlcos~~~clV)~zl (43)

v - (~cV)~[-l+exp~-(hS2c/V)~z~](sin((~c/V)sl
(44)
+ c0s~(~,/V)+z~1

and this flow extends a distance

% - (hn,h (45)

from the base. Figure 9 shows these flows. While it is never explicitly stated, all these
flows must decay with time probably as axp(-t/Q).

If the crucible base is conical all the flows are decreased. A correction to allow for this
is to

multiply TB by 2/ [I+(sina)-+I (46)

To establish the flow in a column of haight H takes a time ~8 given by

TH - 2Hl(hncv)t[l+(sina)-tl (47)

As noted in Section 2, there is a maximum height Eoax past which the flow never spreads. This
height is given by
 ACRT: a review of models 209

6E = (v/AR,)~r

Fig. 9 The distribution of velocities at various heights in the crucible.

=max - (~“)~~l+(si”o)-~l~~/2 (48)

In order to have a boundary layer it is necessary that

smax ’ 6e (49)

and

II ’ 6R (50)

These conditions reduce to

Re > 16 (51)

and

Re > a2fH2 (52)

The ruult4 given here are reasonably confirmed by 136, 38-41).

5. FLCWS WWRN
R CRANGESCONTINUOUSLY

So far we have considered step changes. Such changes are obviously impossible as no real
system can be subjected to infinite acceleration. Hovever, if the change takes place in a
time 1484 than l/m,-, the models considerad in the previous two sections apply. Here ve
consider changes which take longer than this limit.

Since WC srb interested in a periodic motion. WC c(Ln USC Fourier synthesis to model any system
for which v4 know the response to a sine wave. ‘Ihere ia 4 model (431 for a long cylinder
which describes the azimuthal velocity which occurs in response to a rotation rate variation
210 J. C. Brice ef al.

c = g sin(mt) (53)

The solution takes the form

= _an cos(mt)(ber’(kr)bei’(ka)-bei’(kr)ber’(ka)~
v = fir 0
t [ber’(ka)]* + [bei’(k

ber’(kr)ber’(ka) + bei’(kr)bei’(ka)
+ al?,sin(mtf
[ber’(ka)]* + [bei’(k ! (54)

Here k* - m/v and her’(x) and bei’ are the Kelvin functions plotted on Figure 10. The
solutions of this problem, which was set as port of the Cambridge mathematical Trip06 in 1883,

30 -

20 -

15 -

10 -

1..5-

0.6-

0.8 1 1.5 2 3 4 6 8
X

Fig. 10 The functions Ber’ and Bei’.

 ACRT: a review of models 211

are shown in Figures 10 to 15. Note that these figures cover times 0 ( at< 7. The other half
cycle (n < mt < 211) Can be obtained by reflecting the given curves through the line R * 0. It

0.5

k=
xl0
RIRO TtllS
--w-B
--
--_-L
0
0

:r’. 0 03
rla
1.0

Fig. 11 Angular velocities.

mt = X12
l.O-

ka = 2

Fig. 12 Angular velocities.

212 J. C.Brim et al.

_l.oL
0 0.5
rla
1.0

Fig. 13 Angular velocities.

mt = Xl2
l.O-- !’

0.5 -

1 ka =6

r/a

Fig. 14 AngUlar Velocities.

 ACRT: a review of models 213

mt= n/2
1.0
F _I

:ILL 0 0.5
r/a
1.0

Fig. 15 Angular volocitiea.

is obvious that for small ka the liquid follow the crucible motion and for large La nothing
much happens in the central regions. Thus since we are interested in stirring which requires
velocity gradienta, we are lntereated only in a limited range of ka values. Outside the range
3 c ka < 6, ACRT will do very little. Thus for useful stirring we want

9 < ma?/v < 36 (55)

and a~ large a value of no ao is permitted by stability considerations. (See Section 6).

The model diecussed above only deals with the azimuthal flow and is restricted to large I.
However, very similar result8 are to be expected at amall x. To a first order the results at
ems11 x should ba modelled by a decrease in the effective radius of the tube to take account
of the greater ratio of fixed surface to volume. Juat as in Section 1 we assumed that
boundary layer flow only occurred if rD >> re, we can say here that a boundary layer may
form if

f >> J- (56)
2Q
0

i.e. if

m << 2% (57)

Again. chLa emuhasiaes the need for a large value of Ro. The maximum value of no is one of
the topics dia&ssed in the next section.

6. INSTABLE FLOWS

ACRT is a periodic process. A detailed examination of a crystal grown by the method should
reveal a complete record of the rotatien changes Imposed. We uee ACRT to improve the stirring
214 J. C. Brice et al.

in a system. Flow instabilities quite often improve mixing but tend to do this in a time
dependent manner. In ACRT we might expect instability for only part of a cycle so that in
general an unstable system should give crystals which are less homogeneous than those which
come from a stable system. Here we examine the conditions for instability. Knowing these. we
have a choice.

In the case of rotating flows there is a very powerful theorum due to Rayleigh rC6.2, C661.
The Raylelgh criterion states that if R is the absolute angular velocity then the flow will
always be stable If

d(r*CI’)
___ > 0
d

The criterion was formulated for inviscid liquids. Viscosity increases stability. Thus we
have a situation in vhich if the criterion is satisfied, the flow must be stable but failure
to satisfy the criterion does not automatically make the flov unstable.

Differentiating the product in (58) gives

rQ2 + r’/i?ld(RI > 0 (59)

;i;
or

InI + rdg > 0

dr
We have to be careful to remember that II
o* in (58) is positive which is vhy there are modulus
signs in (59) and (60).

From (60) it is obvious that spin-up in a step is stable provided the initial state was
uniform rotation or a stationary liquid. Spin-up from non-uniform states is best dealt with
by -using the nodal in the last sectiou. 6ee for example Figures 11 to 16. Such systems can

ka = 10

-Lo-
0 0.5 1.0
rla

Fig. 16 Angular velocities.

 ACRT: a review of models 215

be made absolutely stable by making them uni-directionally rotating i.e. the crucible follows
a law

a - sloe + n, sin(mt) (61)

provided that

Qoo 3 k&o (62)

This empirical rule applies in the range of interest to us, i.e. 3 < ka c 6 and appears to
apply up to La - 10. This can be seen by plotting the intersections of tangents at r = a with
the rotation axis. Of course, failure to comply with the Rayleigh criterion does not
automatically make the system unstable.

As an example, we look at the stability in spin-down of a system with a step reduction in

rotation rate. If we use the aDde1 shown by the full line in Figure 5, we can see that the
system is essentially a Couette flow system, i.e. we can model it with a system of two
concentric cylinders and consider liquid in the annulus between the pair [24]. In spin-down,
the outer cylinder is stationary and the inner one rotates. Systems like this have been
extensively studied. Di Prima and Swinney [441 give a comprehensive review which should be
regarded as required reading for students in the field. It can be shown that the flow is
unstable if

(AC)2(a-d)d3/y2 < Ta’ (63)

where Ta’ ia a mdified Taylor number which is a function of o - (a-d)/a. This function is
given in Table 3. The values tabulated are the experimental ones given in [44] vith the
omissions suggested by Di Prima and Swinney. The spread of the data suggest that
uncertainties should not exceed 1%. The table also gives the values of 1, the wavelength of
the instability (see Figure 6). Note that the instability is a pair of rolls.

If we rewrite (63) in the form

= (Re)‘(l - d/a)(d/aj3 < Ta’ (64)

it is obvious that it is more convenient to use a function

Ta” - Ta’/(d/aj3(l-d/a) (65)

and obtain a stability condition

Re < (Tao”)+ (66)

This new function is given in Table 3 and plotted on Figure 17. Note that (Ta”) has a
minimum at d/a - 0.53. Thus if we wish to find a condition in which flow is stable throughout
the &cay process we can use the condition that

Re < 272 (67)

We are also interested in situations in vhich the container is not brought to rest. There is
less information about these but Chandraaekhar [C71] does treat states for n + 1 with non-zero
rotation of the container and pofnts out that if Y is the ratio of the inner and outer
rotation rates. then the critical Taylor number varies as (l+Y)-1. If we consider a system
rotating steadfly at Co and then reduce the rotation rate by Lii, we have

Y = Go-W IQ, (68)

If ve take the Taylor number, multiply it by (l+Y), we obtain a stability condition

hn(2Ro-bn)(a-d)d3/v < (Te’lo+l (69)

or
216 J. C. Brice et al.

Table 3 Crttical Taylor and Reynolds Numbers for

Plow in the Annulus for Spin-Down to Rest

d/a (Ta’jc (Ta”) c (Re), :.

0 1696 co m 1 .Ol

0.025 1746 1.15 x l0a 10700 1 .oo

0.0375 1772 3.49 x 107 59 10 1 .oo

0.05 1802 1.52 x IO7 3899 1.00

0.075 1860 7.77 x 106 2787 1 .oo

0.10 1925 2.14 x 106 1463 1 .oo

0.125 1995 1.17 x 106 1082 1.00

0.15 2070 7.22 x 105 850 1 .oo

0.20 2244 3.51 x 105 592 1 .oo

0.25 2453 2.09 x 105 457 1.00

0.30 2708 1.43 x 105 378 1 .oo

0.35 3026 1.09 x 105 330 1.00

0.40 3429 a.93 x 104 298.8 1 .oo

0.50 4648 7.44 x 104 272.8 0.99

0.60 6996 8.10 x 104 284.6 0.99

0.64 8597 9.10 x 104 301.7 0.98

0.65 9097 9.46 x 104 307.6 0.98

0.70 14135 1.37 x 105 370 0.98

0.72 14503 1.39 x 105 373 0.98

0.75 18605 1.76 x 105 420 0.97

0.80 31085 3.04 x 105 551 0.97

0.85 62550 6.79 x lo5 a24 0.95

0.90 179053 2.47 x 106 1572 0.94

1 .oo m m

Uncertainties are about 1% in the worst cases

 ACRT: a review of models 217

Table 3 Critical Taylor and Reynolds Numbers for

Plow in the Annulur for Spin-Dovn to Rest

d/a (Ta’), (Ta”)c (Re), A

0 1696 m a 1.01

0.025 1746 1.1s x 108 10700 1.00

0.0375 1772 3.49 x 107 59 10 1.00
0.05 1802 1.52 x 107 3899 1 .oo
0.075 1860 7.77 x 106 2787 1 .oo
0.10 1925 2.14 x 106 1463 1.00
0.12s 1995 1.17 x 106 1082 1.00
0.15 2070 7.22 x lo5 850 1.00
0.20 2244 3.51 x 105 592 1.00
0.25 2453 2.09 x 105 457 1 .oo
0.30 2708 1.43 x 105 378 1 .oo
0.35 3026 1.09 x 105 330 1.00
0.40 3429 8.93 x lo4 298.8 1 .oo
0.50 4648 7.44 x 104 272.8 0.99
0.60 6996 8.10 x lo4 284.6 0.99
0.64 8597 9.10 x 104 301.7 0.98
0.65 9097 9.46 x 104 307.6 0.98
0.70 14135 1.37 x 105 370 0.98
0.72 14503 1.39 x 105 373 0.98
0.75 18605 1.76 x 105 420 0.97
0.80 31085 3.04 x 105 551 0.97
0.85 62550 6.79 x 105 824 0.95
0.90 179053 2.47 x 106 1572 0.94
1 .oo m m

Uncertainties are about 1% in the worst cases.

218 J. C. Brice er al.

1x103

Ta "

1 I I I I 1200
0 0.2 0.4 0.6 0.8 1.0
d/o

Fig. 17 Re, as a function of d/a for spin-down. Note that spin-up is stable.

< (Ta”)o+,
bQ2(2Cl,,-AQ)a4/v (70)

For Ai-l - no, these relations reduce to the previous forms which do not suffer the restriction
n -t 1. Unfortunately, there seems to be no evidence that we can remove the restriction from
(69) and (70). However, it ssems reasonable to suggest that (69) and (70) are approximations
at d/a m 0.5. Here we obtain a general stability condition

A!X2n, - AQ)a4/u< 7.5 x lo4 (71)

Note that here we have been looking at instability in the annular flow region at positions
remote from the ends of the column. At the bottom of the column, the end face stabilises the
flow and the experimental situation is shown in Figure 18. On this figure the symbols
representing experimental results are two squares. Two open squares imply that the flow is
stable everywhere. An open square under a filled one implies stable flow at the bottom of the
column. Two filled squares correspond to unstable flow over the entire length of the column.

The additional stability at the base of the columns is a consequence of the axial flow.
Hocking and Skiepco (451 show that, in general, flow parallel to the rotation axis stabilises
Couette flow.

There is a general result [33] that for asl + no, doubly periodic flows occur for (Re) about
10% greater than the critical value. In these flows the axes of the rolls are not circles but
have a wavelike form. If @i? << R,, the double periodic flows only occur if the critical
Reynolds number is exceeded by a factor of 10 or more. See Figure 19.

One point which must be emphasised is that in the annular flow region we expect and find [39]
that the instability which occurs is in general transient.

Now we consider the other region where instability is likely. This region is the Ekman layer
which Is discussed fully by Greenspan (G6.31 who shows that there are two classes of
instability both of which are moving rolls. (See also [24]). Figure 20 gives the directions,
spacings and velocities of these rolls in terms of the parameters VR and &R’. Figure 19
 ACRT: a review of models 219

5.0 272 490

I I
4.0-n 0 II II
I TOP ,f i I
3.0- Fob’: I
H/a
2.0- ? JIl, u

1.5 - 0 ‘\,a@
[I fl’\’ 4
l.O-
n\i ’
All stable \ All unstable
\
\
0.5 -
,[I, ‘p ,n (
I
100 200 300 500 1000 2000 3000
(Re) = a*Aw/v

Fig. 18 Stability for crucibles with various H/a values. Each symbol is two
square*. Two open squares imply stable flows in all the regiona of the
liquid. A filled symbol over an unfilled one implies unstable flows for
x + a while for z 4 a the flcu io stable. Two filled symbols Imply
unstable growth for all E. A thick line at the base of an unfilled
symbol Implies that the Ekman layer is unstable. Data from the sources
mantioned in the text and Euteneuer (461.

-2ao-

QJO
0

-4000 -2000 0 2000 4000

Fig. 19 Stability regions.

220 J. C. &ice et al.

25 to 336,

Ffg. 20 Instabilltles of the Ekman layer.

gives the stability regions. Note that ( ) Is the Reynolds number computed using the
thickness of the Ekman layer [6R - (u/AQ) PE1 as the characteristic dimension and the
relative azimuthal velocity v as the velocity i.e.

(RE) = @R/V (72)

where VR is v at z - 6~ (73)

The Rossby number E is given by

E = VRf’R (74)

We can evaluate all the parameters for the case vhen all the driving force is provided by the
crucible base (I.e. for H <( a). In a more general case the wall and base make equal
contrlbuUons fG3.31 and hence we tend to underestimate the various flow rates by a factor
(2)). However, the nett effect on E is zero and (RR) Is underestimated by a factor (2)i.
We correct for this later. For the moment pBsume a a> H which allows us to use the simple
theory given by Greenspan LG2.31. This theory gives

% - (vlAw+ (75)

WE = -0.678AQ
(76)

QE - no + 0.322AQ
(77)
 ACRT: a review of models
221

Hence the uxium value of (IU) is

(ae) - 0.678s( lMl/w)+ (78)

and

E =
0.678M
0.322 M (79)

Note that in the expression for (Re) WC ignore the sign of M but in the upression for E we
cannot do this and WC use a eign convention that in spin-up M is positive, while in
spin-dovn. it is negative. (Hence in spin-down, E l 0). The spin-up section of Figure 21 is

ain down

I
160 lDinL
A l 0 unstable
140
(REI .124.5.3.88 (t)
_____-----c----
A unstable

-.-.-- /<’ __ Stable

, 40
/
/
/
34c(RE)<63 ,’ --20
_)

-1.2 -0.8 -0.4 0 0.4 0.8 1.2

(L) = V&I I-

Fig. 21 Instebilities of the Ehen layer. In the spin-down region, the upper
limit of the position of the stability line is set by the work of
Neitzel and Davis [39] who clearly show instability ia spin-down to rest
for RE - 63. Similarly, the lower limit is set by the work of Briley
and Walls 1381 who demonstrate stability to RE - 34. gence spin-down to
rest is unstable for Re l 4000 but stable for Be up to (It least 1160.

well established experimentally. For the moment assume that we can use the equations on the
right hand part of the figure in all regions. Then VI find a stability condition

0.67aa( 1AQl/w)+ < 56.3 + 39.6AsUtn, + 0.322~) (80)

or if

R, * Wn, (81)

1
= a2h(ln/v < 6896 1.04&&J
(Re) 1 + (92)
1 + 0.322%

For A smsll change we find

(lie) e 16180 (83)

222 J. C. Brice et a/.

is a worst case. For spin-up from rest (R, * +l, E - +l)

(Re) < 27584 (84)

and for spin-down to rest (R, - -1, E - -1) the right-hand side of (80) becomes negative i.e.
spin-down to rest is always unstable. Indeed for R, < -0.74 the boundary layer is unstable.
However, this result depends on extrapolating from experimental data at E > 0.2 and this may
not be valid. There are data (SM caption to Figure 20) which suggest that for E < 0

(RX) - 12~2 + 47E + 58 (85)

which gives (RS) - 23 at E - -1 i.e.

(Re) < 1150 (86)

for spin-down to rest.

Finally, we recall that our estimates of (RX) are likely to be low by a factor of around
(2)i. Hence we arrive at a general stability condition.

(Re) - a2Afl/V < 5230 [l + o.a1c + 0.21~232 (87)

where E is given by (79). Note that here we are considering the worst cases i.e. r + a.

7. DISCUSSION

In this paper. it has been assumed that all the flow is caused by changes in rotation rates.
This is a rather doubtful assumption. In a real crystal growth aystem there will be density
gradients due to temperature or concentration gradients and these will produce flows which
will interact with those created by rotation changes. The result can be large scale time
dependent flow as discussed by Greenspan [42]. To take a simple example. radial heat flow
into the liquid will tend to produce flow up the walls of the container and so make spin-up a
more vigorous process than in ideal ACRT. Similarly, spin-down will be made less effective.
Gradient driven convection usually reduces the resistance of systems to asymmetric and/or time
dependent flows, i.e. it reduces the stability of the system. These changes reduce the
utflity of the theory given here: the numbers applicable to real systems will differ from
those derived in this paper. However, the simple theory presented here is still a valuable
guide to getting the best out of ACRT, and it is worthwhile to attempt to give a summary of
the conditions necessary for the production of useful effects.

Looking first at systems subjected to step changes, it is clear that the period T between
changes must exceed the time constant for flow to be established, i.e.

T > l/hn (aa)

where AQ is the change bstween the upper rotation rate $ and the lower rate GL. If we
aim only to.produce uimuthal flow to improve the symmetry of the system, then we need a small
rotation rate change say

AG < gOVla2 (89)

and the period T should lie between one and two decay times i.e.

0.33a2/V b T(nu + ~L)/(&J - RL) + O.l63a2/.V (90)

If we want to produce axial flow in the region near the bottom of the crucible i.e. in the
region s < smaX where

smax = (f%u)+TD (91)

then we need to exceed the critical Reynolds number so that we have a condition

a2AM” >, 40 (92)

Ue now have a choice, we can either accept transient instability or avoid it either completely
or in the region I: < a. Complete avoidance requires
 ACRT: a review of models 223

a2hClfv -z 272 (93)

Accepting instability remote from the bottom of the crucible requires

272 c a2m/V 4 450 (94)

The condition of gross instability (a%l/v > 450) is almost certainly best avoided. Again,
there is a critical time period

a/(~W)~[l+(sina)~] c T < Za/(&%J)f[I+(sfna)f] (95)

where sin n is the angle of a conical base. (sin o - 1 for a flat base.) It is assumed here
that the condition

T > l/m (96)

is sotisf ied.

Turning now to systems in which the changes are continuous rather than discrete steps, the
conditions for producing useful stirring are

9 < ma2/v G 36 (97)

where

n - Qoo + &sin(mt) (98)

If

* cc 2nQ, (99)

there will be axial flow. If this condition is not obeyed, symmetry will be improved but
stirring will not be enhanced. Stability requires that

5-loo ’ k&o (100)

i.e. we are co=itted to unidirectional rotation. This is actually a fairly gsneral result:
rotation reversal is almost certain to produce instability but can lead to an increase in
homogeneity in crystals (241.

Finally, it is important to note that with stsble flow which is vigorous enough to produce
axial f-low, only a small volume of the fluid near to the base (L < soulx - a) is actually
stirred. En the stable flow regime, this volume does not mix with the bulk of the fluid.
Thus when using ACRT for a Bridgaan system the crystal grow” resembles one grown by a
zone-refining process rather than one grow” by normal freeting [231. This is a useful result
which can only be fully exploited when the theory of the process is understood.

8. CONCLUSIONS

While ACRT is a periodic process snd the periodicity must leave detectable traces in crystals
grow” using the method, it is potentially a very useful technique. At worst it improves the
symmetry of the heat and mass flou. When properly exploited it can produce excellent
localised stirriog. The theory given here should be adequate for many applications but
further study is necessary, particularly of systems in which there are density gradients.

ACRNOWLEDCEMBNT

This work has been carried out with the support of the Procurement Executive, Ministry of
Defence, sponsored by DCVD.
224 J.C. Brice et al.

REFERENCES

1. R. Teman, NavierStokes Equations: Theory and Numerical Analyaia,Amatardas, Worth

Holland (1979).

2. 0.~. Ladyrhenskaya, The tlathematical Theory of Viscous Incompreesible Flow, London,

Gordon and Breach (1963).

3. C.K. Batchelor. An Introduction to Fluid Dynamics, London, Cambridge University Press

(1967).

4. G.H.A. Cole, Fluid Dynamics, London, Hethuen (1962).

5. V.C. Levich, Physico-Chc+aical Hydrodynamics, New York, Prentice Hall (1962).

6. S. Goldstein, Modern Developments in Fluid Dynamics, Oxford University Press (1938).

7. H. Schlichting, Boundary Layer Theory, London, Pergamon (1955).

8. H.P. Greenspan, The Theory of Rotating Fluids, London, Cambridge University Press
(1968).

9. S. Chandrasekhar, Hydrodynamic and Hydromagnetic Stability, Oxford, Clarendon (1961).

10. B.V. Zaitsev, S.S. Gendelev, A.G. Titova and V.G. Kurilenko,Elektronnaja Technika Ser.
1, 10 (1968).

11. H.J. Scheel and E.O. Shulz-Dubois, J. Crystal Grovrh 5, 304 (1971).

12. H.J. Scheel, J. Crystal Growth 13/14, 560 (1972).

13. E.O. Schulz-Dubois, J. Crystal Growth l2, 81 (1972).

14. G. Wende and P. Gornert, Phys. Stat. Sol. Q. 263 (1977).

15.: H.J. Scheel, IBM Technical Diecloeure Bulletin 22, 2096 (1979).

16. I.H. Brunskill, R. Boutellier, W. Depmeier, 8. Schmid and H.J. Scheel, J. Crystal Growth
56, 541 (1982).

17. D. Rytz and H.J. Scheel, J. Crystal Growth 59, 468 (1982).

18. HvJ. Scheel and J. Sommerauer. J. Crystal Grovth62, 291 (1983).

19. D. Elwell and H.J. Schael, Crystal Growth from High Temperature Solutions, London,
Academic Press (1975).

20. H.J. Scheel, Prog. Crystal Growth Charact. 2, 277 (1982).

21. H:J. Scheel and E.O. Schulz-Dubois. In: Convective Transport and Instability
Phenomena, Ed. J. Zierep and H. Ortel, Karlschune, Braun (1982).

22. F.V. Wald and R.O. Bell, J. Crystal Growth 3D, 29 (1974).

23. P. Capper and J.J. Gosney, U.K. Patent 2098879~ (1982).

24. P. Capper, J.J.G. 6osney and C.L. Jones, J. Crystal Growth 7D, 356 (1984).

25. A. Horowitz, D. Gasitt and J. Makovsky, J. Crystal Growth 6l, 323 (1983).

26. A. Horowitz, Ft. Goldstein and Y. Horowitz, J. Crystal Growth 6l, 317 (1983).

27. H.A. Chedtey and D.S. Robertson, J. Phys. D& 325 (1972).

28. H.J. Scheel and H. Muller-Krumbhaar, J. Crystal Growth 49, 291 (1980).
 ACAT: a review of models 225

29. M. Mihelcic, C. Schrock-Pauli, K. Wingerath. II. Wenrl, W. Uclhoff and A. van der Hart,
Kernforrchungaanlage Julich GmbH. Lnetitut fur Pcatkorpcrforschuag, Report Jul-1682
ISSN 0366-0885 (October 1980).

30. M. gihelcic et al*, J. Crystal Growth 53, 337 (1981).

31. M. FLihelcic et al**, Report Jul-1745 (1981).

32. M. Hihelcic et alt, J. Crystal Growth 57, 300 (1982).

33. S. Barman. E. Glanche, P. Cornart, R. Hergt and C. Backer, Kriatall und Technik 2, 895
(1974).

34. J. Aidelberg, J. Flicstein and FI. Schieber, J. CrystalGrovth 2l, 195 (1974).

35. W.J. Patrick and W.A. Uestdorf, U.S. Patent 4, 040, 895 (1977).

36. A.P. HUeod, Phil. Flag. -*

44/259 1 (1922).

37. B.S. Carslaw and J.C. Jaeger, Conduction of Heat in Solida, Oxford, Clarendon (1959).

30. W.R. Briley and H.A. Walls, Lecture Notes in Physics Vol. 8. p.377, Berlin, Springer
(1971).

39. G.P. Neitzeland S.H. Davis, J. Fluid Mech. m, 329 (1981).

40. H. Caller and T. Ranov, J. Basic Eng. (Trans. ASME), pp.445-454 (1968).

41. J.C. Brice. Current Topice in Materials Science Vol. 2, p.598, Ed. E. Kaldie and
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44. R.C. Di Prima and H.L. Swinney, Bydrodynamic Instabilities and Transitions to Turbulence
p.139, Rd. H.L. Swinney and J.P. Collub, Berlin, Springer (1981).

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46. G.A. Euteneuer, Acta Mechanica l3, 215 (1972).

* This ia an abridged version of (281.

** Part 2 of [ZB].
t An abridged version of [301-
226 J. C. Brice et al.

APPENDIX I: THE GOVERNINGEQUATIONS

The axisymmetric flov of a uniform incompressible fluid in a stationary cylindrical coordinate

system is governed by four equations:

(Al .l)

av av av a2v a2”
2-F+
u
TF+
w
27-r
??I=
I
“_.-.1*_-41,
a& a2 r ar r-
I (Al .2)

aw aw aw ap a& a& aw)

x+
u
3F;’
w
!
-I
z==;;-~++~++++f~
I
(Al .3)

au aw
z+z+; = 0 (Al .4)

Here x is the symmetry axis and the velocity w is parallel to s. The velocities u and v are
parallel to r and 0 respectively. P is the local pressure. The first three equations are the
Navier-Stokes equations. The last one expresses the continuity condition.

If we use a rotating system of sxes rotating at a rate R about the s axis, then v + v + rSl and
while equations (A1.3) and (Al.41 are not altered, we must add a tens 2vZ + rC2 to the left
hand side of (Al.l) and a term 2& to the Left hand side of (A1.2). Note that the addition is
vectoral: we have assumed that 6l and V are in the same direction. If this is not the case we
muat subtract the quoted extra terms.

Reverting now to a stationary set of axes, it is convenient to write (A1.2) in terms of 0’

(the local rotation rate). We obtain

awl azw’ 3 awl a&*

F = !
v-+--+
a,2 r ar z I
(A1.S)

This ie- a Very convenient equation which ia not changed when we transform the axes i.e.
w’ -+ w’ + R.

Note that when the second two terms on the right hand side of (A1.5) are small we obtain

(Al .6)

which resembles a diffusion equation

(A1.7)

However, the second terms in the brackets are not the same. Thus we can only use the
conveniently tabulated solutions of (A1.7) when ti’jdr * 0 or vhen (l/r)ao’/ar is negligible
compared with @W’/at2 and &‘/as2 is either large or known to be essentially zero. Thus the
solutions of (A1.7) which converge generally more rapidly than the solutions of (A1.6) can
really only be used to describe spin-up from rest. Remember that to use either (Al.6) or
(A1.7) we assume that %!‘/at dominates the left hand side of (A1.S).
 ACRT: a review of models 227

Some authors vticc the left hand sides of (Al.1) to (Al.31 in the form dli/dt or more ptzperly
DU/Dt where U - u, v, w. Thfr notation implies that the value of U is that sarn by a particle
moving wfch the flow. In transforming to a rotating coordinate system theqe auch*>r$ t???. to
transform the left hand aides by adding twice the vector product of IJ and X. However wither
of theae notation changes is particularly useful.
228 J. C. Brice et al.

THE AUTHORS

PETER CAPPER

Dr. Peter Capper graduated in 1971 from the University of Essex.

In 1974 he obtained his Ph.D., for a study of the flux growth of garnets,
from London University (externally at Portsmouth Polytechnic). He joined
Mullard Southampton in 1974 and worked initially on the growth and
assessment of bulk silicon. In 1976 he transferred to work on Cd,Hgl_,Te
(MT) eventually becoming Group Leader R and D supervising work on bulk and
epitaxial CdTe and CMT. At present he is a Senior Development Engineer at
Philips Research Laboratories (on secondment from Hullard Ltd.) and works on
the growth and assessment of epitaxial CMT. He has published approximately
35 papers and holds one patent (on ACRT applied to Bridgman growth).
 ACRT: a review of models 229

JOHN C. BRICE

John Brice was educated at Arnold School and Queens’ College, Cambridge
where he read Natural Sciences. He joined the Philips concern in 1956 and
has worked in the Redhill Laboratoriee since then on problems related to
materials for electronic devices. Re is the author of two books and some
sixty papers on crystal growth. In 1969 he was awarded his doctorate (for
published work) by the University of Cambridge.