CA T ENA VOL.

5, i - 8 I BRAUNSCHWEIG1978

THE CALCULATIONOF LEAD-210 DATESASSUMING A CONSTANTRATE

OF SUPPLYOF UNSUPPORTED21°Pb TO THE SEDIMENT

P.G. Appleby
Department of Applied Mathematics & TheoretlcaT Phygl~C~
University of Liverpool
F. Oldfield
Department of Geography, University of Liverpool
(received September 30, 1977; revised version accepted December 9, 1977)

SUMMARY
The paper describes a method of calculating sediment age from 21°Pb profiles where
changes in accumulation rate have affected i n i t i a l 210pb concentration. Previously
published age/depth profiles derived from 21°pb measurements have assumed a con-
stant i n i t i a l concentration of unsupported 210pb per unit dry weight at eac~ stage
of accumulation, despite variations in accumulation rates. In sediments from three
sites which have experienced rapid acceleration in accumulation in recent times,
the assumption is not compatible with the measured unsupported 21°Pb concentra-
tions, lhe alternative assumption of a constant rate of supply of unsupported
21°Pb to the sediments per unit time allows calculation of age throughout the pro-
f i l e s irrespective of evidence for rapidly accelerating accumulation. The methods
of calculation used are outlined, illustrated and discussed in the light of evi-
dence obtained from the sediments of Lough Erne and Lough Neagh, N. Ireland and
lakes Ipea and Egari in the Highlands of Papua New Guinea. They provide a means
of dating variations in accumulation rate resulting from human activity in the
drainage basin.

ZUSAIV~IENFASSUNG
Es wird eine Methode zur Berechnung des Sedimentalters beschrieben, die auf 210pb-
Profilen beruht, bei denen Ver~nderungen der Akkumulationsgeschwindigkeit die an-
f~ngliche 21°pb-Konzentration beeinfluBt haben. FrUhere Alters-Tiefen-Profile
aufgrund von 210pb-Messungen sind von konstanter Anfangskonzentration von 21°pb
im Trockengewicht in jedem Sedimentationsstadium ausgegangen, obwohl Unterschiede
in den Akkumulationsraten berUcksichtigt werden. In Sedimenten von den Standorten
mit groBer Beschleunigung der Akkumulation in jUngerer Zeit ist diese AnnBhme
nicht mit der gemessenen z10pb-Zufuhr je Zeiteinheit erlaubt dagegen eine Alters-
berechnung unabh~ngig vonder stark beschleunigten Akkumulation. Die Berechnungs-
methoden werden erl~utert und diskutiert anhand der Befunde an den Sedimenten der
nordirischen Lough Erne und Lough Neagh sowie der Seen Ipea und Egari im Hochland
von Papua Neu Guinea. Sie stellen ein Hilfsmittel zur Datierung unterschiedlicher
Sedimentationsraten in Abh~ngigkeit von menschlicher Aktivit~t in den Einzugsge-
bieten dar.

i. INTRODUCTION
Lakes and their drainage basins provide a uniquely favourable context within which
to study changing material flux in both t e r r e s t r i a l and aquatic ecosystems. Plac-
ing such work on a firm quantitative footing depends on the development of well
validated chronologies of sedimentation. Interest in recent human impact on rates
of erosion, nutrient loss and eutrophication makes the accurate and precise dating
of sediment accumulation over the last century or so of special importance.
In recent years, several papers have i l l u s t r a t e d the use of 21°pb ( h a l f - l i f e
22.26 y r . ) measurements in calculating dates and accumulation rates for recent
lacustrine, estuarine and marine sediments. The method relies on estimation of
the residual radioactivity arising from the presence in the sediments of unsuppor-
ted 21°pb derived from 'rain-out' onto the surface of the water body beneath which
the sediments have accumulated. Various laboratory techniques have been developed
for estimating the residual unsupported 21°Pb content. They involve measuring to-
tal 21opb a c t i v i t y either d i r e c t l y , using gamma emission (GAGGELER et al. 1976)
or indirectly using either the beta emitting daughter isotope 21°Bi (KRISHNASWAMY
et al. 1971, KOIDE et al. 1972, KOIDE et al. 1973, ROBBINS & EDGINGTON 1975) or
the alpha emiting grand-daughter isotope 21°po once this has been allowed to grow
into the sample (EAKINS & MORRISON 1977). Supported 21°Pb is determined by estab-
lishing the 226Ra content of the sample; subtraction of this from the total 21°Pb
gives an estimate of the unsupported 21°pb present at each depth in the sediment.
PENNINGTON et al. (1976) have summarized the assumptions which they have made in
order to derive age/depth curves from profiles of unsupported 21°pb concentration.
These include constant input of unsupported z1°Pb to the lake and a constant re-
sidence time in the lake. In practice what is implied is a constant net flux of
unsupported 21°Pb to the accumulating sediment surface. This is a function not on-
ly of the balance between inflow to and outflow from the lake but also in a l l pro-
b a b i l i t y of chemical conditions at the mud-water interface (cf. MORELet al. 1973,
BOOTH 1975). I f a constant flux of unsupported 21°Pb to the sediment is assumed,
and provided no significant migration of 21°pb has taken place within the sediment
column, unsupported 21°Pb a c t i v i t y w i l l decline down the sediment profile in ac-
cordance with i t s natural radioactive decay. The resulting age/depth curves from
Blelham Tarn show a high degree of internal consistency and good agreement with
other evidence for sediment age, as does the zlopb evidence from Windermere (ASTON
et al. 1973, PENNINGTON 1973). In order to calculate age/depth curves as presently
published i t has to be assumed that at each stage in accumulation the i n i t i a l con-
centration of unsupported 21opb in the sediment was constant despite any varia-
tions which may have occurred in accumulation rate. A necessary corollary of this
accumption is that in undisturbed cores concentration values must decline monoton-
i c a l l y with depth. In several cores from L. Erne, N. Ireland and lake Ipea in the
New Guinea Highlands there are significant increases in concentration with depth
at certain levels. Such inflexions in the concentration/depth profile are taken
as evidence for the dilution of unsupported 21Opb concentrations by accelerated
sediment accumulation at and above the point in the curve where the inflexion oc-
curs (Fig. 1). These data thus tend to cast doubt on the dates derived from the
constant i n i t i a l concentration ( c . i . c . ) model in lakes where accumulation rates
may have varied significantly in recent times. OLDFIELD et al. (in press) have
presented the results of calculations based on the alternative assumption of a
constant rate of supply ( c . r . s . ) of unsupported ZlOpb to the sediment through
time. This model accomodates dilution of 21°pb concentration by accelerated sedi-
mentation and, in the lakes studied so far, i t gives results which are consistent
internally and which agree more closely with such indirect external evidence of
sediment age as is available. All the results obtained so far suggest that the
dating of recent sediments in lakes which have experienced rapid changes in accu-
mulation rate w i l l depend on the evaluation and development of the type of model
outlined below. Although previous authors have referred to the p o s s i b i l i t y of
deriving dates from the integrated a c t i v i t y of the radionuclide (e.g. GOLDBERG
1963), no f u l l exposition of an appropriate method has been published.
 101 -- Lough Erne Prof,le SM I Fig. i:
-I / ~ --- Luugh £rne Profile FM 1 U n s u p p o r t e d 2 ] 0 p b c o n c e n t r a t i o n s vs.
k -- -- Upper Lough Erne Prof,le F M 2 d e p t h in t h r e e c o r e s f r o m L o u g h Erne,
' !
N. I r e l a n d a n d o n e f r o m L a k e Ipea,
P a p u a N e w G u i n e a . In a l l c o r e s , a t o n e
o r m o r e p o i n t s b e t w e e n 6 c m a n d 30 c m
below the sediment surface, concentra-
t i o n s i n c r e a s e w i t h depth. A l l c o r e s
were obtained with a Mackereth pneu-
m a t i c m i n i c o r e r w h i c h r e c o v e r s an u n -
I / i....' ",
disturbed mud/water interface.

(1-5

01 0
Depth (crn)

2. THE C.R.S. MODEL

Assumidg that the supply of unsupported 21°pb to the sediment is the same for each
time interval, the i n i t i a l concentration Co(t ) of unsupported 21°pb in sediment of
age t years must satisfy

Co(t ) r ( t ) = const (1)

where r ( t ) g/cm2yr is the dry mass sedimentation rate at time t . Letting x be the
present depth of sediment of age t , the present concentration of unsupported 21°pb
at depth x is
C(x) = Co(t ) e - k t (2)

where
log 2 =
k = LF2-72-
~ 0.3114
is the radioactive decay constant of 21°pb. Further, since the sediment laid down
during a small period of time at occupies a layer of thickness
ax : pr(_~ ~t

where p(x) g/cm3 is the dry mass/unit wet volume of the sediment at depth x, the
rate of change of depth is

=~ (3)
P
where the superposed dot denotes differentiation with regard to t. Substituting
(2) and (3) in equation (1), i t follows that the depth/age function must satisfy
the differential equation
 p(x) C(x) ~ = p(O) C(O) ~(0) e-kt (4)

Suppose now that

A(x) = p(x) C(x) dx (5)

x

is the total residual unsupported 21°pb beneath sediments of depth x. From equa-
tion (4),
A = -pC~ = - p(O) C(O) ~(0) e-kt (6)

Integrating this equation with regard to the time t , we obtain

A(x) = p(O) C(O) R ( O ) ~ t ~e-kt dt

=~p(O) C(O) ~(0) e-kt (7) •

= a(0) e
-kt (8)

(c.f. GOLDBERG1963, 125). The age of the layer of depth x is therefore

t : ~ lo (9)

A(x) is calculated by numerical integration of the graph of pC/x.

From equations (4) and (7),

p C )~ = kA.

Hence from equation (3) the rate of sedimentation is given e x p l i c i t l y by

kA
r = T (I0)

An estimation of the acceleration in the rate of sedimentation can be made from

the ratio of the slopes of the graphs of log A/x and log C/x.
Since
dA kA
~i-£= - pC = - p-F '

the slope of the graph of log A/x is

d log A = --~-
~-~ kp (11)

Further, differentiating equation (6) with regard to time,

dC r 2
+ C ~ = -kCr ,
p
whence
 dC P+kr
: - pC r--gz-
i.e.

d kp
log C = - T (I + ~ r ) (12)
The age assuming constant i n i t i a l concentration of unsupported z1°Pb in the sedi-
ment is

The age discrepancy between the two dating methods is t h e r e f o r e

AO Cx

3. DISCUSSION
Figure 2 i l l u s t r a t e s the divergence in age obtained by using the c . i . c , and C.roS.
models on sediments of differing accumulation rates. Where there has been neither
significant acceleration nor deceleration in accumulation rate both methods give
the same results irrespective of the actual rate. This is Confirmed by the kough
Neagh p r o f i l e , in which there is l i t t l e systematic variation in accumulation rate
between the topmost dated level and the base of the profile on either basis of
calculation, and the c . r . s , derived dates a l l f a l l within the standard errors of
the original c . i . c , dates.
Maximum divergence between c . i . c , and c.r.s, based dates derives from periods of
accelerating accumulation rate. Where this acceleration gives rise to a dilution
of the unsupported z10pb in accordance with the c.r.s, model, the age discrepancy
between the two models is given by equation (13). In the c.r.s, model the graph of
concentration C against depth x need not decrease monotonically. Equation (12)
shows that the graph w i l l have zero slope i f the acceleration in the dry weight
sedimentation rate r satisfies

: -kr,

where

k = ~ : .03114,

and a positive slope i f

P < -kr.

The c . i . c , model is clearly not applicable to cores whose unsupported 21°Pb pro-
f i l e exhibits this behaviour.
Profiles of f a l l - o u t 137Cs provide an alternative method of dating recent levels
(PENNINGTON et al. 1973, RITCHIE et al. 1973). This has been done on four of the
cores from which 210pb profiles have been obtained in Lough Erne and Lake Ipea.
Where, as in three profiles out of the four obtained, there is some discrepancy
between the c.r.s, based 21°Pb dates and the 137Cs dates the l a t t e r are in every
case the more recent, sometimes by as much as 10 years. This is a very significant
discrepancy in relation to the degree of accuracy needed for dating and influx
calculation over the last 20 - 30 years (PENNINGTON 1974, BONNY 1976). I t is not
cr~ UPPER LOUGH ERNE LOWER LOUGH ERNE
o- Fig. 2:
L COREFM2 CORE FM I o- ~ CORE SM I
Selected 210pb
derived age/depth
10- profiles from
Lough Erne and
+~-~1963 ] Lough Neagh, N.
1963 Ireland and from
20~ 2o- '-P Lakes Egari and
13?Cs
Ipea, Papua New
Guinea. Each plot
compares c.i.c.
30. 30- "- and c.r.s, based
dates (see text).
Where available,
137Cs dates are
40, 40 40
shown. Lake Ipea
lies in the S.
Hemisphere. Thus
"• 5(} , I ~ , 50 50 ¸ the peak fall-out
of 137Cs is de-
.C 19'50 19'00 18'50
layed by one year.
(D.
Q) IPEA The upper pecked
LOUGH NEAGH EGARI
CORE& section of the
CORE B&3
Ipea 4 c.r.s.
,96~'Cs based age/depth
curve has been
obtained from
measurements on
the parallel and
adjacent Ipea 1
core.
,950 ,900 ,150 ,~
t
30" 30
,450 ,9'00 ,8'50

COMPARISON OF 21°pb DATES OBTAINED BY USE OF

4(}
ALTERNATIVE ASSUMPTION

[ ' Dates derived from cJ,c model with standard errors shown
- - Age/depth curves derived from c.rs rood.el
50 , ' , . . . . i . . . . . .
970 950 1900 1850
possible to say from the data so f a r obtained whether the discrepancies arise from
systematic errors in the c . r . s , model, from downward d i f f u s i o n of 137Cs in i n t e r -
s t i t i a l water, from a combination of these factors or from other causes, such as
the selective remobilisation of heavy metals from the sediment surface. Evidence
for downward d i f f u s i o n of 137Cs is apparently present in a l l the cores however
and strongest in those with the greatest divergence between 137Cs dates and c . r . s .
based 21°pb age.
A number of authors have drawn attention to a depression of unsupported 21°Pb con-
centration close to the mud water interface (KOIDE et al. 1973, PENNINGTON et al.
1976). Although i t remains possible that release of 21°Pb from surface mud to the
water is responsible for the anomaly i t also follows that i f the c.r.s, model is
appropriate in these cases, one contributory factor to the low surface concentra-
tions could be the presence of, and hence dilution of unsupported 210pb concentra-
tion by labile organic matter not yet reduced to the stable residues which form a
component of 'mature' sediment.
OLDFIELD et al. (in press) have shown that the variations in unsupported 210pb
concentrations and in cumulative total residual unsupported z1°Pb at each level
in the cores they obtained for PapUa New Guinea are, when normalized for depth by
reference to a synchronous volcanic ash layer, and compared within and between
lakes, consistent with the c.r.s, model and incompatible with the c . i . c , model.
This demonstration nevertheless f a l l s short of a f u l l validation of the c.r.s.
model. Where increased allocthonous minerogenic input to the lake sediments is re-
sponsible for the acceleration in accumulation, and especially where this includes
r e l a t i v e l y coarse grained material ( s i l t and sand) the low adsorptive capacity of
the influx is l i k e l y to increase the chances of dilution of unsupported 21°Pb con-
centration. The cases of extreme acceleration used so far to evaluate the c.r.s.
model f a l l into this category. Whether equally good validation would be obtained
in lake~ where accelerated accumulation has resulted largely from autocthonous
material generated by increased aquatic primary productivity remains to be seen.
A further complication is introduced by the possible influx to the lake of soil
carrying t e r r e s t r i a l l y adsorbed unsupported 21°pb into the lake, especially dur-
ing periods of accelerated erosion of fine grained surface material.
This discussion highlights the need for studies designed to test the accuracy of
both 137Cs and 21°pb dating in sites where independent evidence of sediment age
already exists. Lakes depositing annual laminae and drainage basins which have
given rise to diagnostic and precisely dated influx events in recent times require
systematic study before any one approach to 21°pb age calculation can be accepted
with confidence.

ACKNOWLEDGEMENTS

We wish to thank Mr. J.D. Eakins and Dr. R.S. Cambray f o r providing respectively
the 21°pb and 13?Cs data upon which t h i s paper is based, and Dr. R.W. Battarbee
for permission to use his data from Lough Erne and Lough Neagh.

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