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Helium isotope refrigeration

a
David S. Betts
a
School of Mathematical and Physical Sciences, University of
Sussex , Falmer, Brighton, Sussex
Published online: 13 Sep 2006.

To cite this article: David S. Betts (1968) Helium isotope refrigeration, Contemporary Physics,
9:2, 97-114, DOI: 10.1080/00107516808202172

To link to this article: http://dx.doi.org/10.1080/00107516808202172

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 OOWTEMP. PHYS., 1968, VOL. 9, NO. 2, 97-114

Helium Isotope Refrigeration

DAVID S. BETTS
School of Mathematical and Physical Sciences,
University of Sussex, Falmer, Brighton, Sussex
SUMMARY.The recent development of the helium isotope refrigerator, using mixtures
of the two isotopes of helium, is probably the most important step forward in the
technique of producing low temperatures since adiabatic demagnetization. This
article attempts to describe the special properties of *He-4Hemixtures, and to show
how these properties are used to produce refrigeration below 0.1 OK. Design details
of a c t d refrigeratorsare given, and the direction of future improvements is suggested
by a consideration of simple models of the various refrigerator components.
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1. htroduction
The lowest steady temperature available to the experimentalist has been,
until quite recently, about 0.3 OK. Of course, much lower temperatures have
been achieved by adiabatic demagnetization of paramagnetic salts or nuclear
paramagnetic metals, but these temperatures cannot be held indefinitely
because of finite heat leaks. The helium isotope refrigerator has already
produced steady temperatures down to 0.01 OK in continuously-acting
operation and much lower temperatures down to 0-0045 OK in single-cycle
operation, with heat extraction rates easily capable of absorbing normal stray
heat leaks. Further improvements may be expected in the near future, but
already this method of refrigeration has distinct advantages over demagneti-
zation. It is cheaper, produces steady temperatures and does not need
complicated service equipment.
The structure of this article can be summarized as follows. First of all I
shall give some account of the basic physics governing the operation of the
dilution refrigerator (the reason for this name will become clear later). Then,
I shall introduce the type of continuously-acting cycle generally used until
now, describing in some detail the function of each component. For this
purpose I shall make approximate calculations using some typical numerical
values for quantities involved; for example, the circulation rate or the still
temperature. My aim is rather to give some feel for the magnitudes than to
suggest an exact recipe for success. A short section will then be given, showing
a comparison of various design details of the several currently functioning
refrigerators. Finally some space will be devoted to the ' single-cycle '
refrigerator and to other possible recirculating cycles. Any lack of clarity
or detail can probably be dealt with best by reference to the few original
papers mentioned or to their bibliographies.
H. London first suggested the use of a dilute solution of 3He in liquid 4He
as a refrigerant at a conference in Oxford as early as 1951. I n 1962 a most
important source paper appeared by H. London, Clarke and Mendoza. This
paper provided important background experimental data, and also gave
detailed proposals for the construction of a dilution refrigerator. Within a
few years several laboratories had reported some success. I n this article the
various refrigerators will be referred to by the names of the places of origin :
' Leiden ' (Das, Ouboter, Taconis 1964); ' Manchester ' (Hall, Ford, Thompson
0 C.P.
 98 David S. Betts

1966); ' Dubna-U.S.S.R. ' (Neganov, Borisov, Liburg 1966); ' Illinois '
(Vilches, Wheatley 1967).
I n equations and formulae, suffixes 3 and 4 refer to ,He and 4Herespectively;
C and D, or (c) and (d) complete with the brackets, refer t o the concentrated
and dilute phrases; S stands for still, and E for exchanger; and rate of change
is shown by the Newtonian fluxion dot.

2. Properties of liquid 3He-4He mixtures

Liquid mixtures of 3He and 4He form a single phase with any degree of
concentration a t temperatures down to 0.87 OK. Below that temperature
some concentrations become unstable and separate into two distinct phases,
the concentrated ( 3He-rich) phase floating on the denser dilute (4He-rich)
phase, with a visible surface between them. The concentrations in the two
phases are functions of temperature, but at absolute zero i t appears that the
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concentrated phase is pure 3He, whereas the dilute phase contains about
6 per cent of 3He. The origin of the 6 per cent will be discussed later. All
this can best be summarized in a simple diagram (fig. 1).

0.9

0
0 *3 .4 .S .b .7 -8 .9 1.0
MOLAR FRACTION OF 'He (X,)

Fig. 1. The phase equilibrium diagram for liquid mixtures of SHeand 4He.

The curve encloses the unstable region and the two equilibrium concentra-
tions in a phase-separated mixture at temperature T are given by drawing a
horizontal isotherm, intersecting the curve at the two values of X, (X, is the
molar concentration of 3He, i.e. N3/(N3+ N4):similarly X4).
 Helium Isotope Refrigeration 99

At temperatures much below 1 OK dilute solutions behave in many ways

like gaseous 3He, but with an effective mass m* for the atoms which is greater
than the normal mass m,; m* 2: 2.5m3. The reason for this is that the 4He has
negligible entropy itself, so that it behaves simply as a background solvent
(except that its presence contributes to the magnitude of m*). It is relevant
t o point out that a dilute solution of 3He at sufficiently low temperatures
behaves like an ideal Ferm-Dirac gas. The degeneracy temperature for a
6 per cent mixture is readily calculated and comes out to be 0.37 O K . One
interesting corollary of this is that here is a true Fermi-Dirac system which
can readily be cooled to temperatures well below the degeneracy temperature.
At temperatures between, say, 0-5 OK and 1 OK, the system will be slightly
degenerate or almost classical, but above about 1 OK the simplicity breaks
down because of the greater importance of the 4He ‘ normal fluid ’.
Some cooling could be achieved even without the property of phase separation
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because when a degenerate Fermi-Dirac gas is expanded adiabatically, cooling

results according to the equation
Tf=Tt(V,/Vf)2’3
where the subscripts i andfrefer to initial and final temperatures and volumes.
A dilute mixture of 3He in liquid 4He could therefore be cooled by diluting it
with superfluid 4He introduced through a super-leak, the process being
equivalent to an adiabatic gas expansion. But there is also another different
cooling mechanism which exists by virtue of the phase-separation boundary.
Consider fig. 2.

T = 0.2OK

Fig. 2. Cooling by removal of pure 3He from the dilute phase of a separated
mixture a t 0.2 OK.

I n equilibrium at 0-2 OK the concentrations in the two phases stay constant

at roughly the values shown. If, somehow, 3He were removed from the lower,
dilute phase, then 3He atoms would move across the surface from the con-
centrated phase to re-establish equilibrium. It will be shown later that there
is a latent heat associated with this, so that the process is just like evaporation
from a liquid phase to a gas phase. Continuous removal of 3He atoms from
the dilute phase is analogous to the pumping of vapour from a liquid phase to
a gas phase. I n the ordinary liquid-vapour situation, the cooling is related to
the fact that the entropy of the vapour is greater than that of the liquid.
Similarly, in the present case, the entropy of the dilute phase is greater than
that of the concentrated phase. It also appears that 3He atoms are more
tightly bound in a pure liquid 4He environment than in pure liquid 3He, right
down to absolute zero, which accounts for the finite amount of 3He (up to
6 per cent) left in 4He towards absolute zero. The existence of this 6 per cent
 100 David S. Betts

mixture at absolute zero arises in the following way. Some rather precise
notation is needed if this is to be clear.
X,,the 3He concentration, will be written simply as X . pQ4(X)is the
chemical potential of a ,He atom in a mixture with concentration X. Strictly
it is also a function of temperature, but a t low enough temperatures this can
be ignored. Then, P , ~ ( X is
) made up of two parts, the first being the Fermi
energy k T f ( X )which appears because a ,He atom, added to a dilute mixture,
must be given enough energy to put it a t the Fermi surface. The atom cannot
have a lower energy because the lower levels are filled by ,He atoms already
present. The second part is the energy needed to place a ,He atom in the
proximity of the others. This is negative and can be written as - E,,(X).
Thus,
p34(X)= & T A X )-E34(X)*
T f ( X ) the
, Fermi temperature, is given by the expression
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~ ) V ( X ) is the molar volume.

where m* is the effective mass ( - 2 . 5 ~ ~and
p,, is the chemical potential of a 3He atom in pure liquid ,He. Again, the
temperature dependence can be ignored at low enough temperatures. p,, is
the energy needed to place a ,He atom in the liquid. It is negative and can
be written as - E,,; NE,, is therefore the molar latent heat of pure liquid ,He.
The principle which determines the two equilibrium concentrations at any
temperature is that the chemical potentials are equal. At very low tempera-
tures the concentrated phase of a phase-separated mixture is known to be
very nearly pure ,He, so the concentration in the dilute phase will be found
by solving for X o
k34(x0) 'p33

Or E34(X0) -E33 =kTf(XO)

Now E34(X)-E3, can be found experimentally by measuring the temperature
at which phase separation occurs for known concentrations X, doing a little
straightforward statistical mechanics, and extrapolating to lower concen-
trations. k T f ( X )can be calculated and the two functions are equal for one
unique value of X,i.e. X o , which comes out to be 6 per cent. Furthermore,
the experimental results can reasonably be extrapolated to zero concentration,
and one finds that a ,He atom is more tightly bound in pure liquid OHe at
absolute zero than in pure liquid ,He. Numerically,
-1 p34(0) -E,,] E 0.2 OK.
k

3. Osmotic pressure and enthalpy

When pure liquid 4He is connected through a super-leak to a dilute 3He-4He
-mixture a difference is observed between the liquid levels on the two sides.
The pressure difference is due mainly to the osmotic pressure exerted by the
,He. The 3He atoms in dilute solutions exert a huge osmotic pressure
(denoted by n) which can be considerably in excess of the vapour pressure of
pure ,He, particularly at low temperatures. These have been measured and
can also be calculated; for instance, a 6 per cent mixture at temperatures
 Helium Isotope Refrigeration 101

well below Tf (i.e. 0.37 OK) has an osmotic pressure given by the ordinary
Fermi-Dirac equation of state: 11V = (2/5)RTf.
Hence II(T < Tf) = 2RTf/5V E 2 cm of mercury. For comparison, the
vapour pressure of pure 3He is 9 microns of mercury at 1 OK and only 0.01
microns of mercury at 0.25 OK.
There is a further contribution to the internal pressure of a dilute solution.
This is the fountain pressure due to the 4He background. It arises from
temperature differences and is caused by the tendency of the superfluid to
move towards regions of higher temperature. Its magnitude can be calculated
from
p (fountain)=
J': (S/V), dT
where (8/V)4 is the entropy per unit volume of 4He. A substitution of known
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entropy values shows that even a t 0.6 OK the fountain pressure is only about
0.2 mm of mercury, much smaller than the osmotic pressures encountered in
practical dilution refrigerators. It is therefore legitimate to treat the effect
of fountain pressure as a negligible perturbation.
Processes of mixing or dilution are usually carried out at constant pressure
(rather than constant volume) and it follows that the quantities of heat
involved are enthalpies. This is also true of the processes taking place in the
dilution refrigerator, although in this case the large osmotic pressure has to be
included in the definition of the relevant enthalpy. H. London, Clarke and
Mendoza (1962) have defined a suitable enthalpy H and have obtained experi-
mental values of it. The dilution process can now be represented rather
neatly on an H versus T family of curves for various concentrations. Fig. 3
below is diagrammatic, and in fact only part of it has been obtained experi-
mentally.

ZCALI MOLE

0 ' I J
0 0.87OK
TO K
Fig. 3. The enthalpy, H,of 3He-4Hemixtures showing the various cooling processes
described in the text.
A straightforward dilution, uncomplicated by phase separation, could be
represented by EF, which means that a solution with X 3 = 5 0 per cent at
T,, diluted to X , = 3 0 per cent by the addition of superfluid *He, would cool
to T,. This process would work even at temperatures approaching absoIute
 102 David S. Betts

zero provided that the initial concentration were not greater than 6 per cent.
I n the phase-separation region, enclosed by the curve, the choice of initial
and final concentrations is restricted to equilibrium values. AB represents
the cooling achieved when concentrated 3He is diluted by passing across the
phase interface into the dilute phase. Both EF and AB are single-shot
processes. A continuously circulating cycle, operating a t T,, would remove
heat CD for every mole circulated.

4. A continuously-acting refrigeration cycle

Now, with some of the basic properties of dilute mixtures described, a model
recirculating dilution refrigerator can be introduced. Fig. 4 shows the main
components diagrammatically.

CIRCULATING PUMP
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FLOW CONTROLLER

CONCENTRATED VAPOUR
STILL
DILUTE LlOUlD

CONCENTRATED LIQUID
DILUTION CHAMBEP
DILUTE LIQUID

Fig. 4. A continuously-actingrefrigeration cycle.

It is approximately true to say that the 4He in the system does not circulate
but acts as a neutral bath. The 3He dissolves in i t , passes through and is
redistilled. This neglect of the 4He is not quite accurate, and the extent of
the circulation of 4He will be estimated a little later, but a t this stage it is
simpler t o leave it out of considerat'on.
Imagine the 3He starting its cycle a t the high pressure side of the pump.
It is first condensed in a 4He bath a t about 1 OK (this bath is not shown in
the diagram), and then passes down the flow controller in liquid form. It is
further cooled in the still to (typically) about 0.6 O K , and then to much lower
temperatures in the heat exchanger where it loses heat t o the cold counter-
flow until it is close to the temperature of the dilution chamber itself. It is
fed into the concentrated (upper) phase, passes across the interphase boundary
where the cooling actually occurs into the dilute (lower) phase. From there
it moves back through the heat exchanger under the influence of a concentration
gradient absorbing heat from the warm in-going concentrated phase. I n the
still, heat is applied, evaporating the 3He, which is pumped away up to room
temperat,ure, completing the cycle.

5. Heat extraction rate

One of the most important characteristics of the dilution refrigerator is its
heat exbraction rate, which will now be calculated. Consider the enthalpies
 Helium Isotope Refrigeration 103

of the 3He a t various points in the cycle, assuming that the 4He does not
circulate at all, and that its entropy is zero. Essentially the problem is that
of finding the difference between molar enthalpies in the concentrated and
dilute sides of the phase boundary. Straightforward thermodynamic arguments
can be used to show that H = N p + TS where S is entropy and p is chemical
potential; p is the same in both phases because they are in equilibrium and it
follows that the enthalpy difference is simply T[S(d)-S(c)] where X(d) and
X(c) are the molar entropies of the dilute and concentrated phases respectively.
Now
S(d)= gr2( T/Tf) R,
the entropy of a Fermi-Dirac gas, and S(c)N 3RT from specific heat measure-
ments. Thus, the heat extraction rate should be
k3[($n2/Tf) - 31 R T D 221 10h3RTD2
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where n3 is the molar circulation rate of 3He, T, is the temperature of the

dilution chamber, and Tf is calculated to be 0.37 OK for a 6 per cent mixture.
This heat extraction rate has been verified experimentally in the Illinois
refrigerator. Fig. 5 shows the theoretical heat extraction rate as a function
of temperature.

0.8

0.6

JOULES/MOLE

0.4

0.2

TEMPERATURE

Fig. 5. The theoretical heat extraction rate at the dilution chamber.

It is not surprising to find that as absolute zero is approached, the heat

extraction rate falls off rapidly, being proportional to the square of the
temperature. This extraction rate has to cope with various unavoidable
heat leaks as follows:
(a)Stray heat leaks and vibrations.
 104 David S. Betts

( b ) Heat brought to dilution chamber by the incoming concentrated phase

because of imperfect heat exchange.
( c ) Heat conducted along the dilute phase from the still.
( d ) Metallic conduction between still and dilution chamber.
The relative importance of these contributions will be dealt with in due
course. First of all, however, it is important to establish how large a circulation
rate n, can reasonably be maintained, because the heat extraction rate is
proportional to n3. The key to this may be found by considering the operation
of the still.

6. The still
The temperature of the still must not be too small, otherwise the vapour
pressure over it will be too small and the circulation pump will not be able to
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pull the 3He round quickly enough. On the other hand, if it is too high, there
will be a greater resulting heat load for the heat exchanger, causing a larger
heat leak to the dilution chamber and consequently less cooling power. Also
in this case there would not be such good 3He enrichment on evaporation.
A reasonable compromise temperature seems to be T , = 0.6 OK.
Consider the consequences of this choice. I n the dilute phase the osmotic
pressure is everywhere the same, irrespective of temperature gradients (we
have already agreed to ignore fountain pressure). This behaviour is like that
of an ordinary gas whose pressure is everywhere the same, even when there
are temperature gradients. T , =0.6 OK is rather higher than the Fermi
temperature of the dilute phase in the still, and the 3He in the still may there-
fore be considered classical with osmotic pressure given by
n,V=X,RT,
where X , is understood to be the 3He concentration in the still. However,
in the dilution chamber the 3He is degenerate, with osmotic pressure given by
n,V =% X ,R T f with T f = 0.37 OK.
Hence, equating n,=n,, we get X, N 0.89/Ts per cent.
For T , = 0.6 OK, X , 2: 1.5 per cent.
Now, a 1.5 per cent mixture at 0.6 OK has a 3He vapour pressure of about
70 microns of mercury and a 4He vapour pressure of about 0.3 microns, that
is, there is a high degree of enrichment at 0.6 O K . (It would be less good at
higher temperatures. This calculation suggests a highly concentrated distillate,
but in reality it is likely to be considerably less good because of the 4He film
flow. The effects of this can be minimized by circulating 3He as fast as possible
and by having a narrow constriction in the pumping line immediately above
the still.) For an idea of throughput magnitudes, suppose a diffusion pump
with air speed 30litres/sec is used to pump on the still at 0-6 OK through
1 metre of tubing of diameter 4 cm. These are fairly realistic figures, and the
calculated resulting throughput of 3He comes out to be about mole/s.
Throughputs of this order or lower are used in existing refrigerators.
The circulation rate of 4He can also be estimated. If a constriction of
diameter d is placed in the pumping line immediately above the still, the rate
 Helium Isotope Refrigeration 105

of transfer of liquid 4He can be estimated from known film flow rates. At
0.6 OK one finds
n4= d mole/s.
Thus, for d = 0-5 cm, the rate of circulation of 4He might be about 5 per cent
of the 3He rate.
I have already estimated the heat extraction rate a t the dilution chamber.
It is 10n3RTD2. It is also of interest to estimate how much heat has to be put
into the still to maintain the desired circulation rate and still temperature.
Let this heating rate be Qs, in which case the total heat input to the system
in steady-state operation is 10n3RTD2+ 0,.
Now the molar enthalpy of the incoming concentrated liquid 3He at the
still is just Np33+T,S(c). The enthalpy of the outgoing, evaporated 3He gas
has its classical value of QRT,. But enthalpy is conserved in the process,
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and it follows that

107i3RTD2 + Qs =?i3[QRTs- N , 3 3- T ~ : S ( C ) ] .
When T D is below about 0.1 OK the term 1Ok3RTD2is small. The values of
all the quantities in the square brackets can be evaluated at the still tempera-
ture. For example, at 0.6 OK the square bracket is equal to about 40 joule/
mole. That is, &s/ri32:40 joule/mole, an expression which accords with
various experimental values. Clearly, an increase in 0, will cause an increase
in n, which in turn will increase the heat extraction rate and lower the
temperature of the dilution chamber. However, the magnitude of the effect
must depend on many factors.
One relation between T , and ?i3 is given by the requirement of enthalpy
conservation, as shown in this section. Another relation arises from a
consideration of ,He vapour pressure over the still and the pumping speed.
This was dealt with above. Thus n3 and T , are determined by 0, and
the pumping speed, but not in a way which can be reduced to a simple
mathematical expression. A further complication is that the rate of 4He
circulation, n4,is likely to be very sensitive to T, and this effect has not been
taken account of here.

7. Flow controller
The purpose of this is to sustain the pressure gradient between the high
pressure side of the pumping system and the outlet in the dilution chamber
at the required liquid throughput. Also, of course, the pressure at the top
end must be equal at least to the 3He condensation pressure a t the temperature
there. (For instance, a t 1.3 OK this pressure is about 3 cm mercury.) Suppose
the required pressure drop is A p and the viscosity of liquid 3He is q . Then the
length, I , and the internal diameter, d, of the flow controller, should satisfy
the Poiseuille equation
--K).
li TAP
3- 128V37

A sample substitution of numbers, with Ap=3 cm of mercury and

n3= mole/s, gives
 106 David S. Betts

It is also desirable to make the surface area of the controller (mld) as large as
possible so that the liquid 3He can be cooled t o the still temperature as
effectively as possible. At the same time the volume of liquid 3He in the
controller ( )mZd2) should not be excessive. Clearly the dimensions cannot be
optimized, but one suitable solution would be as shown below:
1=100 cm; d = 1 0 - 2 cm; mid-3 cm2; ~ d d 2 ~ 1 0 cm3.
- 2
The behaviour of the flow controller is self-regulating. That is, if the flow
rate through the pump should fall for any reason, then A p would fall, reducing
the flow through the controller and vice versa. There is a more important
detail. It would be very undesirable if too much 3He vapour were to pass
through the controller with 3He liquid. A certain amount could be tolerated
because it would simply condense a t the still where external heat is supplied
anyway, but if there were such an amount that some 3He vapour got through
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t,o the exchanger, then some efficiency would be sacrificed. However, for
equal pressure gradients, the molar vapour flow is much less than the molar
liquid flow. It follows that excessive vapour flow would result in an increase
in A p which would improve condensation.

8. The heat exchanger

The function of the exchanger is to prevent the returning liquid 3He from
bringing too much heat with it. The heat exchange is in fact limited by a
surface effect known as the Kapitza thermal boundary resistance. This
resistance is so large a t the sort of temperatures we are interested in, that it is
the dominant cause of the temperature difference between flow and counterflow,
ordinary conduction and convection effects being of relatively small importance.
Fig. 6 illustrates the difference in temperature distribution between an
' ordinary ' exchanger and one limited by a boundary resistance.
FLOW METAL COUNTER FLOW FLOW METAL COUNTER FLOW

, ' t
TEMP:
I

ORDINARY EXCHANGER
TEMP.
I
BOUNDARY-LIMITED EXCHANGER

Fig. 6. Temperature distributions in heat exchangers.

I n any heat exchanger it is important to know how much exchange area
is needed in order to produce the required efficiency. I do not want to be
reduced to making bald statements about the performance of existing heat
exchangers without having some model, however crude, to provide a physical
picture of what goes on. An exact calculation in the present case would be
extremely complicated even if all the input data concerning, for instance,
boundary resistances were available (which it is not). Consequently approxi-
mations must be made and I have devised the following model, which certainly
contains great oversimplifications but has the virtue of producing an expression
 Helium Isotope Refrigeration 107

for the contact area required for the attainment of a particular temperature.
The model relies on the following points.
(a) A complete solution would need specification of the thermal conductivity
of the heat exchanger itself. I n fact the Illinois refrigerator uses copper
exchangers, but others have used stainless steel. This model will assume the
conductivity to be high, which simplifies the mathematics a little, but a
parallel calculation could assume it to be low. The exchanger temperature is
T,.
( 6 ) The molar heat capacity of the dilute phase is known to be an order of
magnitude greater than that of the concentrated phase at the same temperature,
both being proportional to temperature below about 0-1 OK. The model will
assume that the dilute counterflow does not warm appreciably as it absorbs
heat in the exchanger, but remains at T,, the dilution chamber temperature.
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Of course, its temperature must eventually rise to the still temperature Ts.
I shall return to this point in Section 9, but anticipate here by simply stating
that the temperature rise mainly occurs very close to the still.
(c) Evidently perfect heat exchange never occurs, and the lowest tempera-
ture of the concentrated flow before entry into the dilution chamber is taken
to be T,. It follows that the heat brought into the dilution chamber by the
,He is
a,= ITS
TD
?i3Cp(c)dTE@,R(T,2- TD2) (1)

where Cp(c) is the molar thermal capacity for the concentrated phase.
The assumptions of the model are summarized in fig. 7.
The temperature dependence of the boundary resistances (defined as
temperature jump divided by heat flux) between copper and the concentrated

CONCENTRATED COPPER DILUTE

FLOW COUNTERFLOW
HOT END T

COLD END 13
TE

MODEL EXCHANGER
I
T,

Fig. 7. A simple model heat exchanger used as a basis for calculation.

and dilute phases are not simple and are in any case imperfectly known. For
the concentrated phase, a reasonable approximation is
dQ T3AT
z=Y' (2)

where A is the contact area, A T is the temperature jump and the factor
y 62x cm2s deg4 erg-'. The equality represents the low temperature
limiting case which will be used here. The resistance for the dilute phase
seems to be rather larger than this, but over-complication of the notation can
 108 David S . Betts

be avoided if we agree that the area of contact with the dilute phase should be
designed so that A l y is the same for flow and counterflow. Experimentally,
this situation is certainly desirable. Using eqn. (2) twice and eliminating the
exchanger temperature TE, one obtains

dQ - T 4 - T D 4
_
dA- 8Y *
But
dQ=n3Cp(C)dTN$?i3
R d(T2).
Thus

This can be integrated most usefully by taking the lower temperature limit
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to be T,and the upper to be large. The result can then be written in the form

T,2z T D 2coth [-]A2n,R

1
TD2
. y
(3)

It follows from eqn. (1) that

a, 2: Qk,RTD2[coth (-A T D 2) - 11 .
(4)
12n,R y
One can now estimate the lowest accessible temperature by equating q3 witih
the heat extraction rate 10ri,RTD2,which gives
l-~,Ry
TD2(min)N -
A .
The meaning of this is that the exchange area needed for the attainment of a
certain temperature is inversely proportional to the square of that temperature
and proportional to the molar circulation rate. Numerically, with 7i,=
mole/s the area needed is about 100 cm2 for 0.05 O K , 2500 cm2 for
0-01 OK. These figures are reasonably consistent with the various experimental
results. Fig. 8 shows a comparison of the predictions of eqn. 5 with actual
values attained in various refrigerators. There is seen t o be broad agreement
within a factor of about 2, which is about as good as one could reasonably
expect in view of the crudity of the model and the considerable variety in
experimental arrangements.
Eqn. 5 is of interest in several ways. It shows that lower temperatures can
be achieved by increasing A and also, perhaps unexpectedly, by decreasing ,n3.
Physically, the explanation may be simply that at lower n, the exchanger can
work more efficiently because both flow and counterflow spend longer in
contact with the exchange area. This effect, the reduction of TD(min)with
fi,, has been observed in the Manchester and the Illinois refrigerators, although
in the former case it was ascribed to a different cause. It would, of course,
be erroneous to suppose that indefinite reduction of n, to zero would cool the
dilution chamber to absolute zero because reduction of n, implies reduction
of the heat extraction rate until ultimately stray leaks would be the limiting
factor. These have been left out of the calculation, but are always present.
 Helium Isotope Refrigeration 109

+ MANCHESTER

+ DUBNA U.S.S.R.
+ILLINOIS
+ILLIWIS

-
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.01

0
0 IX107 2x10~ 3X107 4x10’ 5X107 A107

A/n (cm2sec/mole)

Fig. 8. Lowest temperatures achieved in various refrigerators, as functions of

exchange area divided by circulation rate, compared with theory.

The rather large contact areas needed can obviously be given by suitable
arrangements of concentric tubes which may, however, be rather cumbersome.
The problem has also been neatly solved by the use of porous sintered copper
sponge as the heat exchange medium. The design calculations which now
follow apply to such an exchanger, but equivalent considerations of pressure
drops and viscous dissipation would have to be borne in mind for other varieties.
In the sintering process, metallic powder is packed together and heated to
just below the melting point until the powder joins together by a process of
diffusion across the contact points. A little calculation on the geometry of
hexagonal close-packing of spheres shows that the contact area per unit
volume is theoretically 4-45ld where d is the diameter of the particles.
For d = 100pm, say, this comes out to be about 450 om2per cms. Of
course, the smaller the powder, the bigger the available area per unit volume.
However, if the powder is too small, the flow resistance of the exchanger
becomes too high. This is undesirable for two reasons:
( a ) The exchanger might inhibit the rate of circulation unduly, reducing
the heat extraction rate. One can estimate the effect by assuming Poiseuille
flow through the channels between particles and making some simplifying
wsumptions about geometry. One finds that, for an incompressible liquid
passing through such a sponge, the pressure drop would be in the region of
~ + Q x 104
Ap 2: dyn/cm2
ad2

r
where 9 is the viscosity, the rate of volume flow, and 1 and 01 are shown in
fig. 9. I n the concentrated phase this reduces to
 110 David S. Betts

at low temperatures, and in the dilute phase (6 per cent)

AREA

f
LENGTH
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Fig. 9. A sintered copper heat exchange unit.

These considerations define an upper limit on desirable values of EIa. For

n3= mole/s and d = 100 pm, T = 0-05 O K , say,
A p ( c )21 1/6acm mercury.
(This is probably not a serious problem for d = 100 pm, but might be so for
d = 10 pm.)
( b ) Excessive flow resistance would cause dissipation of heat in the exchanger
itself. In the concentrated phase, assumed incompressible, work done
W = F'Ap(c) = 37ri3Ap(c),
200n321
i.e. WN-
ad2T2 '
This must be small compared with the heat extraction rate of the refrigerator,
i.e. 10ri3RTD2. For n3= mole/s and T, = 0.05 OK, this is 200 ergjs.
Hence, one ought to design so that l/a < 25 cm-l. (Again,this is easily satisfied
for d = 100 pm, but might not be for 10pm.)
Also, dissipation in the dilute phase must be small, but this requirement is
less restrictive than in the concentrated phase because of the higher specific
heat of the dilute phase, and because it is being warmed up anyway.
Evidently there cannot be a single copper heat exchanger extending right
from the still to the dilution chamber. If there were, heat would conduct
straight down the copper. This is avoided by linking one or more heat exchange
units between still and dilution chamber with short lengths of poorly conducting
capillary. There is good experimental evidence that it improves efficiency to
have more than one exchange unit, the reason almost certainly being bett,er
reversibility resulting from reduced temperature differences.

9. Conduction in the dilute phase

The still temperature is in the region of 0.6 OK and the dilution chamber is
well below 0.1 O K . They are joined by a continuous column of the superfluid
dilute phase. How much heat Qph will be conducted by the phonons?
The heat conduction equation is
 Helium Isotope Refrigeration 111

where K is the conductivity of the dilute phase and dT/dx the temperature
gradient along a capillary containing it. The specific heat equation governing
the heating of the dilute phase due to the heat flow &ph is

!! !! I ? ?
=n3Cp(d). (7)
dT
Near the still the 3He concentration is about 1-5 per cent, the Fermi degeneracy
temperature is about 0-15 OK, so the 3He behaves like a classical gas with
molar thermal capacity C,(d) = &R.
Combining eqns. (6) and (7), we get
-
d&,h
=-
5n3Rdx
Qph 2KA
(X)
i.e. Qph=QOexp - -x
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The heat leak therefore falls off exponentially away from the still, with a
characteristic length equal to 2KA/5n3R. The conductivity K is governed
by the most important scattering mechanism in the dilute phase, which is
p h ~ n o n - ~ Hatom
e collision. The resulting conductivity is inversely pro-
portional to 3He concentration and inversely proportional to temperature.
However, it has already been shown that, because of the constancy of osmotic
pressure, X3T = 8.9 x 10-3 OK near the still. Thus the conductivity turns out
to be independent of temperature, and equal to about 1.4 x lo5 erg units.
If a length of capillary with i.d. 0.5 mm, say, were inserted in the dilute phase
flow path immediately before entry to the still, the characteristic length for
?i3= 10-4 mole/s would be
2KA
-
5n3R
N cm.

Evidently, phonon conduction can be effectively inhibited by the use of a

' phonon stopper ' of dimensions, say, 1 cm long by 0.5 mm internal diameter.
The pressure drop across this phonon stopper would be completely negligible
for the figures used. It is of interest to point out here that the temperature
of the dilute phase in the heat exchanger does indeed remain at a low
temperature through the heat exchanger (assumed constant in our model),
but rises sharply t o 0.6 'K in the phonon-stopping section immediately before
the still. This occurs over the short characteristic length calculated above.

10. Convection in the dilute phase

I n any sensible refrigerator geometry the still is above the dilution chamber.
The still is warmer than the dilution chamber, therefore the mixture in the
still has less 3He and more 4He, therefore it is denser and there are conditions
for convection. This would be strongly inhibited by viscosity in narrow tubes,
but it has been found troublesome where tubes are too wide. I n particular it
=ems likely that the failure of the Leiden refrigerator to cool below 0.2 OE
was associated with convection in tubes 2.5 mm in diameter. Convective
instability was also strikingly observed in the Manchester refrigerator. This
effect can easily be designed out by using narrow capillaries, probably less
than about 1 mm diameter.
 112 David S. Betts

11. Actual refrigerator design details

I have now dealt with most of the physical principles influencing the design
of recirculating refrigerators. There are some other minor technical points
of interest which can be found in the original papers; to include them here
would be to complicate the narrative unnecessarily.
The details of existing refrigerators are summarized below.

Leiden
This was only able to achieve 0.22 OK as the lowest temperature, probably
because of convective instability in the dilute phase.

Manchester
The lowest temperature was about 0-06 OK with n, = 4 x 1 0 P mole/s and
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a still power of 0.125 mW. The heat extraction rate at 0.122 OK was 46 erg/s.
The best heat extraction rate a t 0.122 OK was obtained by increasing n, to
1.55 x mole/s, in which case the lowest temperature attained was
0.084 OK. The heat exchanger consisted of stainless steel tubing and had a
contact area of 15 cm2. Still temperatures were around 0-5OK to 0-6 OK.

Dubm- U .S.S.R.
The lowest temperature reported is 0.025 OK with n, = 1.14 x mole/s
and a still power of about 4 mW. The heat 'extraction rate was 1300 erg/s
at 0.1 OK. The still temperature was about 0.6 OK. The heat exchanger again
consists of an arrangement of stainless steel tubes giving a contact area of
700 cm2. An earlier version had 140 cm2 contact area, and cooled to 0.056 OK
with k 3 = 1.84 x mole/s.

Illinois
The lowest temperature reported for a continuously-circulating system
(see below for single-shot system) was 0.020 OK with fz, = 1.1 x mole/s
and a still power of 0.247 mW. The heat extraction rate was about 78 erg/s
at 0.11 OK. The heat exchanger consisted of four sintered copper units with
particle size -44pm, presenting a total contact area of about 600 cmz to the
concentrated phase and twice that much to the dilute phase.

12. Single-cycle process

An obvious extension of this cooling technique is to use a continuously-
acting refrigerator to provide the starting temperature for a single-cycle
process. This has been done by the Illinois group and temperatures of
0.0045 OK have been achieved. Their arrangement is illustrated in fig. 10 in
diagrammatic form.
The operation of this single-cycle refrigerator is as follows. The single-cycle
dilution chamber and still are filled with mixture and cooled by the continuously
acting refrigerator with the thermal switch closed. The switch is then opened,
3He is pumped away from the single-cycle still, and the interphase boundary
in the single-cycle dilution chamber moves steadily upwards until no pure 3He
is left in the system. The amount of cooling can be calculated. With no
thermal load other than the mixture itself, a transfer of An, mole of ,He across
 Helium Isotope Refrigeration 113

CIRCULATING PUMP
PUMP

STILL STILL

HEAT THERMAL ANCHOR

EXCHANGER
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DILUTION THERMAL ANCHOR

CHAMBER

THERMAL SWITCH
DILUTION CHAMBER

Fig. 10. The Illinois single-cycle dilution refrigerator.

the boundary removes heat 10An3RT2erg as before. This will cool the two
phases by an amount AT, where
[ncC,(c) +nd C,(d)]AT = 10An3RT2,
n, is the number of moles of 3He in the concentrated phase, nd the number in
the dilute phase;

nd] AT = 10An3R T 2 .

When the dilution chamber is nearly full of concentrated 3He initially,

n&nc, and
-
AT = 3 . 3 -An3
*
T nC
This expression has been verified experimentally by the Illinois group. The
lowest attainable temperature will be given by q = 1M3R T I 2 where q is the
stray heat leak and T I is the limiting temperature. The important point
about the single-cycle refrigerator is that it is only indirectly dependent on
good heat exchange. The limiting temperature is therefore governed solely by
the stray heat leak. A t the time of writing the lowest temperature achieved
is 0.0045 OK.

13. Other possible continuously acting cycles

Finally, I should mention that the kind of continuously-acting refrigerator
I have mainly considered is not the only possible one. H. London, Clarke
and Mendoza (1962) suggested two others, both of which are variants of the
type illustrated in fig. 1 1 .
H C.P.
 114 Helium Isotope Refrigeration

nl EXCHANGER

DILUTION
CHAMBER

Fig. 11. Another possible continuously-acting dilution refrigerator.

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I n this system the circulating 3He never goes up t o room temperature.

It boils off from the still and is-recondensed by contact with a conventional
3He cryostat. Such a system has not been used, probably for two main
reasons: firstly that it is less easy to monitor the circulation rate, and secondly
that an auxiliary 3He cryostat is needed, thus complicating the service
plumbing.

14. Conclusion
The dilution refrigerator is likely t o be very widely used before much longer.
No doubt techniques will become fairly standardized and it is already possible
to buy a commercial refrigerator. I have tried to give a broad outline of the
present state of the art, but some details may well look old-fashioned within
a year or two. I should perhaps have referred more often to the original
literature, but all the other relevant references can be traced through the basic
ones which I have given.

REFERENCES
DAS,P., DE BRUYNOUBOTER,R., and TACONIS, K. W., 1964, Low Temperature
Physics LT9, Pt. B (New York: Plenum, 1965), p. 1253.
HALL,H. E., FORD, P. J., and THOMPSON, K., 1966, Cryogenics,6, 80.
LONDON, H., CLARKE,G. R., and MENDOZA,E., 1962, Phys. Rev., 128, 1992.
NEOANOV, B. S., BORISOV, N. S., and LIBURG,M. Yu., 1966, Soviet Phys. J E T P ,
23, 959.
VILCHES,0. E., and WHEATLEY, J. C., 1967, Physics Letters, 24A, 440, and unpub-
lished report.

The Author:
David S. Betts took his first degree at Oxford in 1958 and remained at the Clareiidoti
Laboratory to work for a D.Phi1. degree under the supervision of Dr. J. Wilks. This was
completed in 1962 and he then spent a further two years in Oxford as a Research Fellow. In
1964 he became Visiting Assistant Professor at Ohio State University before returning to a
Lectureahip at Sussex University in 1965.