Sedimentology (1984) 31,251-267

Syntaxial overgrowths in muddy ctinoidal limestones:

cathodoluminescence sheds new light on an old problem

G . M. W A L K D E N and J . R . B E R R Y
Department of Geology, University of Aberdeen, Marischal College, Aberdeen A39 IAS, U.K.

ABSTRACT

Lower Carboniferous shallow water limestones of Asbian and Brigantian age in Britain commonly contain
abundant interparticle micrite and characteristically display large syntaxial calcite overgrowths on crinoid
and echinoid grains. These overgrowths appear to have developed at the expense of the micrite and are
widely regarded as neomorphic replacements. However, cathodoluminescence of these has revealed growth
features which indicate that they are not neomorphic but originated as passive cement fills of solution voids
surrounding echinoderm grains.
We introduce the term solution corona for these grain selective voids and consider that three processes
may have contributed to their development, namely : high-Mg calcite stabilization of host grains, crystal
ripening, and meteoric dissolution. Cyclic subaerial emergence was a critical factor in these processes, and
we contrast the morphology of the overgrowths in question with forms produced in basinal limestones
which never experienced comparable early meteoric conditions.
These early-formed solution coronas around echinoderm grains are therefore a useful indicator of
meteoric diagenesis and have important implications for porosity evolution. The syntaxial cements which
fill the solution coronas show distinct phases of growth in cathodoluminescence which reflect a progression
from near-surface meteoric conditions to deep burial with pressure solution.

INTRODUCTION
The problem
A common diagenetic texture in ancient skeletal
limestones is the clear syntaxial cement overgrowth
developed in optical continuity with monocrystalline
host grains such as crinoid ossicles or echinoid plates.
Many Palaeozoic and Mesozoic grainstones and
packstones contain an abundance of crinoid syntaxial
overgrowths which have clearly grown into original
intergranular pores as passive cement fills (Evamy &
Shearman, 1965,1969; Freeman, 1971 ; Meyers, 1974,
1978). However, in this study we have examined
Lower Carboniferous packstones and wackestones in
which the overgrowths are unusual in being generally
surrounded by a matrix of micrite or microspar (e.g.
Fig. 1). In these rocks a simple model of passive
cementation of primary pores cannot be applied (e.g.
Bathurst, 1958, 1975).
The texture is widespread in late Dinantian lime-
stones of central and southern Britain, particularly
those of Asbian age (George et al., 1976), but in
particular we have studied rocks from the Derbyshire
Carbonate Platform (Walkden, 1977) in which
Bathurst (1958) first described the texture.
Bathurst (1958, 1975) and Orme & Brown (1963)
considered the overgrowths to be neomorphic replace-
ments of micrite, and the model developed by Bathurst
involves simultaneous dissolution of carbonate mud
and precipitationofovergrowththrough the migration
of ions across a thin (micron-sized) solution film. The
process is initiated and maintained through the
dominance both in size and monocrystalline state of
the crinoid host grain over the surrounding fine
carbonate mud and Bathurst (1975, p. 493) noted that
the resultant syntaxial crystals have sometimes inter-
sected rigid grains such as foraminifera and bryozoa.
Using standard petrographic methods it is difficult
to challenge the thin film model, but the application
of cathodoluminescence reveals details of crystal

25 1
252 G . M . Walkden and J . R . Berry

growth inconsistent with a neomorphic process. In

this paper we examine these difficulties and review
the problems created by existing alternative models.
We propose a new explanation for the appearance of
large syntaxial overgrowths on crinoids in muddy
Dinantian carbonates, and describe the sequence of
diagenetic changes that these overgrowths record.

Fig. 1. Representative crinoid syntaxial overgrowth texture
in two late Dinantian crinoidal packstones. (A) Typical
fabric comprising discontinuous and irregular syntaxial
calcite haloes surrounding most crinoid grains (e.g. A),
regardless of size. Micritized crinoids (e.g. B) display no
overgrowths. Asbian-Hillhead, Derbyshire. Scale bar-
0.5 mm. (B) Extreme development of the texture with large
continuous calcite haloes surrounding all unmicritized
crinoid grains. The sample comes from within 1 m of an
overlying palaeokarst. Asbian-Buxton, Derbyshire. Scale
b a r 4 . 5 mm.
The sediments
The late Dhantian limestones studied in most detail
come from the 200m sequence of shallow marine
Asbian carbonates that comprise the lagoonal portion
of the Derbyshire Carbonate Platform, central north-
ern England. The sequence consists of 1-10 m thick
cycles built of crinoid peloid packstones with subor-
dinate grainstones and wackestones, and cycle bound-
aries are marked by subaerial omission surfaces
displaying calcretes, palaeokarsts and palaeosols
(Walkden, 1972, 1974). The general characteristics of
these rocks are typical of shelf and platform Asbian
carbonates throughout southern Britain (e.g. Somer-
ville, 1979; Wright, 1982; Walkden, in press), and
representative successions have also been examined
in Cumbria, Yorkshire, North Wales and the Men-
dips, all of which contain rocks displaying the same
problematic texture. Representative samples from the
overlying Brigantian have also been examined where
the sedimentarysettingwascomparable (e.g. Walkden
& Davies, 1983) and samples from contrasting basinal
settings have been investigated for comparison.
Over 100 cathodoluminescence slides from Derby-
shire have been examined as part of a systematic
study of the diagenetic history of the platform (Berry,
1984). The packstones containing the problematic
texture are generally poorly sorted and are dominated
by crinoids which comprise an average of 35% of
allochems. Other common allochems include forami-
nifera, dasycladaceans, brachiopods and peloids, and
intergranular space is occupied mainly by mud or by
syntaxial calcite spar.
Compaction in the rocks studied is minimal, with
intergranular space averaging at 46.7% of total rock
volume over 24 representative slides. Compactive
distortion of grains and grain to grain pressure-
solution are generally absent. This lack of significant
compaction, in a succession that eventually developed
major interbed stylolite seams, implies early lithifica-
tion and much direct evidence for this is found in the
occurrence of calcretes palaeokarsts and lithoclasts.
Undeformed mollusc moulds are found throughout.
 Syntaxial overgrowths in limestones 253

The cements grains display a syntaxial overgrowth and those that

With the exception of fenestral rocks and calcretes
most cements within macropores actually comprise
syntaxial calcite grown from a nearby crinoid. The
textural relationships of these overgrowths with the
surrounding grains and mud were clearly described
by Bathurst (1958), and their most important features
are their sharp and uniform extinction, their highly
irregular outlines and their uneven distribution (Figs
1-5). The shape of overgrowths never reflects their
internal crystalline regularity and outer margins are
usually embayed against grains or crosscut matrix. A
few overgrowths are better developed beneath grains
(cf. Freeman, 1971 ;Giiriir, 1979) but even in the most
extreme cases (e.g. Fig. 2), there is a discontinuous
calcite halo all round the grain. Most echinoderm
do not are usually obviously altered by micritization.
In cathodoluminescence the cements are distinc-
tively zoned (Figs 4 and 5), and the cement sequence
seen within crinoid syntaxial overgrowths is identical
to that found in unrelated primary and secondary
pores such as intergranular spaces, brachiopod inte-
riors, mollusc moulds (Fig. 6A) and calcrete fenestrae
(Fig. 6B). The same cements are also identifiable
under high magnification within intergranular mi-
crite.
Zone 1 cements are non-luminescent, but they
commonly contain several thin bright subzones. These
subzones characteristically overlie irregular or fretted
surfaces (e.g. Fig. 4) suggesting dissolution events (cf.
Meyers, 1978). This early, mostly non-luminescent,
generation of cements shows patchily developed

.
Fig. 2. Syntaxial overgrowth fabric surrounding two large crinoid grains (A and B) in a crinoid/peloid packstone. In plane
light (A) overgrowths surround the grain but are preferentially enlarged downwards. This geopetal texture is unrelated to
shelter porosity because it is not found beneath other large grains such as brachiopods. Under cathodoluminescence (B) early
mostly non-luminescent crystals with irregular morphologies (Zone 1) are followed by more regular growths with bright or
intermediate luminescence (Zones 2 and 3). Comparison of (A) and (B) shows that this zonal pattern is not concordant with
the final external shape of the overgrowth. Asbian-Hillhead, Derbyshire. Scale bar-0.5 mm.
254 G. M . Walkdenand J . R . Berry

Fig. 3. Confluent development of syntaxial overgrowths from two nearby crinoid grains (A and B). In plane polarized light (A)
the larger overgrowth shows clear twin planes, and remnant peloids with matrix, C, occupy the upper surface of the host grain
where overgrowth has failed to develop. The smaller grain, B, still adheres to matrix at the top. Under cathodoluminescence
(B) early non-luminescent (Zone 1) crystal growths are patchily distributed, overgrown by an unusual development of bright
Zone 2 and finally by better organized Zone 3 with intermediate luminescence. Zone 3 cements have developed on areas of the
host grain where there has previously been no overgrowth. The overall zonal pattern clearly illustrates the mismatch between
internal crystal organization and the final irregular outer shape of the overgrowth. Small early non-luminescent (Zone 1)
crystals can be seen grown inwards from the spar/micrite interface, D. Asbian-Buxton, Derbyshire. Scale b a r 4 . 5 mm.

anhedral to subhedral morphologies (Fig. 3B) on
crinoid hosts and the lack of luminescence may reflect
minimal uptake of manganese in an oxygenated
environment (Meyers, 1978). Since they are found in
secondary cavities in calcretes these cements clearly
post-date the first subaerial emergence of the sediment
and their general luminescence characteristics suggest
fluctuating chemical conditions. They are interpreted
as representing a relatively shallow largely oxidizing
meteoric diagenetic environment.
Zone 2 cements comprise a generally thin complexly
subzoned generation of brightly luminescent calcite.
They provide a prominent stratigraphic marker on
post large crystals (Figs 3B and 4) and may be
genetically related to Zone 3.
Zone 3 cements are uniform and moderately
luminescent. Indistinct oscillatory sub-zones in these
reflect subhedral to euhedral crystal forms (Figs 4 and
5) and they comprise the most abundant cements.
They are found in sufficient quantities for stable
isotope analysis and their composition ranges are
613C-2.1 to +1.8%, and 6'*0-145 to -125%,
PDB (eight separate analyses) averaging at
6 ' 3 C ~ 0 . 0 % 061802:
, - 13.4%,, PDB. These figures
are typical of late burial cements (Dickson &Coleman,
1980; Hudson, 1977), and are most likely to reflect
precipitation from a pore water depleted in "0 with
elevated temperatures, and probably originally meteo-
ric (e.g. Hudson, 1978).
Zone 4 cements consist of brightly luminescent
 Syntaxial overgrowths in limestones 255

Fig. 4. Under cathodoluminescence this well-developed

crinoid syntaxial overgrowth shows early non-luminescent
subhedral Zone 1 growths with well developed etch surfaces.
Each is emphasized by an immediately overlying thin bright
subzone which itself is probably etched. The zonal sequence
is directly comparable to that in Figs 2(B) and 3(B) and the
final generation of Zone 3 cements with intermediate
luminescence is euhedral and shows none of the early erosive
and oscillatory events. Zone 4 brightly luminescent cements
line some intercrystalline boundaries (e.g. top left). Asbian-
Hillhead, Derbyshire. Scale bar--0.5 mm.

Fig. 5. Under cathodoluminescence two syntaxial over-

growths on crinoids A and B meet along a largely plane
compromise boundary. The cement sequence is complete
with all four generations present. Zone 4 cements leave a
small residual pore space, C . The non-luminescent crystals
at D are authigenic quartz. Asbian-Buxton, Derbyshire.
Scale b a r 4 . 5 mm.
256 G . M . Walkden and J . R . Berry

Fig. 6. Secondary cavities with centripetally grown passive cement fills in cathodoluminescence. The cements comprise Zones
1-3 and thus display the same succession of generations as in crinoid syntaxial overgrowths. (A) Mollusc mould. Asbian-
Dowlow, Derbyshire. Scale bar-0.5 mm. (B) Horizontal vug within a dense micritic calcrete. Asbian-Hillhead, Derbyshire.
Scale b a r 4 . 5 mm.
 Syntaxial overgrowths in limestones
calcite found not only within pores (Fig. 5 ) but along
stylolite seams and intercrystalline boundaries (Fig.
4) within earlier cements. They are not developed
everywhere. Staining with potassium ferricyanide
shows these to be mainly ferroan calcite and they
either co-date or post-date local stylolitization.
T H E O R I G I N OF THE
OVERGROWTH TEXTURE:
T H I N FILM N E O M O R P H I S M AND ITS
ALTERNATIVES
The application of cathodoluminescence in the study
of these overgrowths has revealed features that are
difficult to explain by the thin film neomorphism
model.
(1) The growth zonation in the syntaxial crystals
(Figs 2-5) reflects a progressive change from initially
anhedral to increasingly euhedral crystal forms
throughout growth, and yet the outer margins of the
overgrowths in contact with the micrite are never
euhedral but are irregular and cut across zonal
boundaries. There is thus a considerable mismatch
between the internal growth morphology and the final
overgrowth shape.
( 2 ) Amongst the earliest growth zones there is
commonly evidence of solutional erosion of the
growing crystal (Fig. 4). Such dissolution could not
affect a coarse syntaxial crystal without also eroding
back the finer grained and presumably more soluble
enveloping micrite. This implies the creation of a
space between the crystal and the micrite but the
neomorphism model of Bathurst (1975) requires the
maintenance of a thin solution film at this interface.
(3) Four distinct phases of syntaxial crystal growth
can be determined (Figs 2-5) which reflect an evolving
diagenetic environment from shallow meteoric todeep
burial with pressure solution, and all of these post-
date early lithification phenomena such as calcretes
and palaeokarsts. Neomorphism would thus have
been initiated in a lithified rock and have continued
through considerable changes in diagenetic environ-
ment and rock geochemistry.
Despite these difficulties the alternatives hitherto
considered (e.g. Bathurst, 1975; Evamy & Shearman,
1965) seem even less promising. These are:
(a) PassiveJill of primary pore systems by an early
cement
This is the standard primary void cementation model
introduced earlier, that applies to overgrowths in
257
crinoidal grainstones. Applied to Dinantian pack-
stones and wackestones it creates considerable diffi-
culty as it requires that all syntaxial overgrowths
should be interpreted as the sites of original empty
pore space, so that all such primary porosity was
concentrated only in the immediate vicinity of
echinoderm grains and no others (Fig. 1).
The presence of enlarged overgrowths beneath
some crinoid grains might suggest that syntaxial
cements merely filled shelter pores underlying the
crinoids. However, in the great majority of cases a
continuous or discontinuous overgrowth completely
surrounds grains (e.g. Fig. 3), and shelter pores are
rare beneath other more suitable grains such as
brachiopod valves. Even if preferentialcement growth
had taken place in shelter pores beneath crinoids, but
not beneath other allochems, subsequent compactive
collapse would have buried and preserved good crystal
faces where pores had not been completely filled by
syntaxial cement. In addition there should be more
evidence of compaction in the rocks throughout.
Instead mechanical compaction was largely prevented
by early induration and all primary and secondary
pores, whether filled by crinoid overgrowths or not,
show the same succession of cements and therefore
filled synchronously.
Other explanations for such an unusual distribution
of primary porosity such as substrate-selective organic
coatings or gas generation seem contrived and the
primary pore model for the origin of the syntaxial
haloes can therefore be rejected.
(b) Displacement of mud matrix by growing syntaxial
crystals
The principal objection to the displacement alterna-
tive as applied to the Dinantian rocks in question is,
as stated in (3)above, that by the time theovergrowths
started to develop the rocks were already lithified.
Displacement would thus be most unlikely. In addi-
tion, as noted in (1) above, the outer boundaries of the
overgrowths are clearly not normal outward grown
crystal faces as might be expected in mud-displacive
growth.
(c) Late introduction of micrite
Examining Bajocian packstones from the French
Jura, Evamy & Shearman (1965) concluded that the
micritic matrix was a late arrival that followed the
development of syntaxial overgrowths. Their over-
growths were perfectly euhedral and the texture was
258 G . M . Walkden and J . R . Berry
so limited in extent that it was possible to demonstrate
a likely overlying source for the micrite.
In contrast the anhedral nature of the Dinantian
overgrowths and the large volume of interparticle
carbonate mud make it extremely difficult to apply the
micrite infiltration model. The major objection,
however, is that a close examination of micritic or
microspar components (e.g. Fig. 4), especially under
high magnification, reveals that these have undergone
the same overgrowth history as the crinoids. Late
arrival of micrite is therefore most improbable.
SYNTAXIAL OVERGROWTHS AS
FILLS
OF SECONDARY P O R E SPACE:
T H E S O L U T I O N CORONA MODEL
An alternative process not hitherto considered is that
the syntaxial crystals grew freely into secondary pore
spaces formed by dissolution of surrounding micrite.
This proposal involves the opening of an irregular
solution cavity (solution corona) around each echino-
derm grain, either during or after the initial induration
of the sediment. The syntaxial overgrowths developed
as passive fills of these cavities. This would account
for the contrast between the irregular outer boundary
of syntaxial crystals and their well organized internal
structure revealed through cathodoluminescence. Sev-
eral other points are critical:
(i) The sequence of zones within syntaxial over-
growths is identical to that of cements which are
passive fills of primary and secondary pore spaces
(e.g. voided mollusc grains, shelter pores and cavern-
ous calcrete, Fig. 6) demonstrating that growth in
each occurred synchronously.
(ii) Small crystals commonly line the crystal/micrite
interface having apparently grown inwards from the
surface of the micrite (Fig. 3). This relationship would
be almost impossible to achieve through a neomorphic
replacement process but it can be explained as
nucleation on the walls of a solution cavity.
(iii) There are cases where empty porespace still
exists between a syntaxial crystal and the micrite wall
(Fig. 5). This is impossible to explain through thin
film neomorphism, but clearly can be interpreted as
incomplete occlusion of a secondary cavity.
(iv) Some matrix micrite can usually be seen lying
directly against a crinoid fragment where overgrowth
hgs evidently been inhibited. It is hard to explain such
a relationship through a selective neomorphic process
but it is readily interpreted as the remaining contact
between a crinoid fragment and the walls of a solution
cavity (Figs 2 and 3).
(v) Instances where syntaxial overgrowths can be
interpreted as having eaten into surrounding grains
during growth are in fact rare and usually grains stand
proud at the crystal/sediment interface suggesting that
the matrix was more susceptible to destruction. A
good example is figured by Bathurst (1958, fig. 2) but
the relationship is very difficult to prove conclusively
in rocks consisting largely of irregular peloids and
already fragmented grains. However, where an inter-
sected grain can be demonstrated the evidence is
equivocal as it could result from solution prior to the
emplacement of the overgrowth.
(vi) The syntaxial crystals sometimes show clear
signs of periodic solution which must in any case have
been accompanied by the development of a solution
space between the crystal and the inferentially more
soluble micrite wall (Fig. 4).
(vii) Other textural features worth noting are an
absence of undulose extinction, thought by Jacka &
Brand (1977) to be a useful criterion of neomorphic
replacements. Instead the overgrowths show clear
zonal expansion into pores and zonal restriction near
grain contacts (Fig. 2) considered by Meyers (1974) to
be characteristic of void-filling cement.
These observations create a clear demonstration
that a cavity was present around crinoids in advance
of the development of the syntaxial overgrowths-a
cavity for which we have introduced the term solution
corona. These cavities were then filled by syntaxial
calcites which are zonally indistinguishable from
nearby cements. Nevertheless, the model offers no
explanation for the exact cause of the dissolution, or
for the centering of coronas exclusively upon crinoids
as opposed to other grains such as foraminifera or
brachiopod?. Since solution coronas were initiated
early during diagenesis, and the factors causing their
grain selective nature must have operated at the same
time, it is useful to examine the general evidence for
the early diagenetic environment of the rocks before
returning to the causes of the solution corona phenom-
enon.
T H E EARLY DIAGENETIC
E N V I R O N M E N T OF LATE
D I N A N T I A N S H E L F A N D PLATFORM
CARBONATES
A reliable indicator of early diagenetic conditions is
 Syntaxial overgrowths in limestones
provided by the presence of cyclically repeated
subaerial omission surfaces which are seen especially
well in the Asbian successions (Walkden, in press).
These surfaces have been studied in detail by Walkden
(1974); Somerville (1979) and Wright (1982) and their
palaeokarsts, palaeosols and calcretes can be corre-
lated for considerable distances. They represent
emergent periods of thousands or tens of thousands of
years, during which time lenses of meteoric water
must have permeated the entire shelves and platforms,
leading to considerable diagenetic modification of the
marine carbonate sediments.
At the time of deposition the original marine
sediments would have consisted of high-Mg calcite
grains (crinoids, echinoids and possibly some forami-
nifera), low-Mg calcite grains (brachiopods, forami-
nifera, corals), and aragonite grains (molluscs,
dasycladacean algae). Peloids and micritic carbonate
are likely to have contained contributions from all the
above but in particular there may have been a high
proportion of aragonite mud derived from calcareous
algae. Partially disintegrated dasycladacean thalli are
present in large numbers in some thin sections and
algae are major contributors to modern carbonate
muds (Bathurst, 1975; Milliman, 1974).
Regardless of these former compositions the Di-
nantian limestones now contain no aragonite : mol-
luscan debris has suffered complete dissolution and
the resultant moulds are filled by blocky low-Mg
calcite with normal cathodoluminescence character-
istics. Microprobe analyses reveal no high-Mg cal-
cite, and evidently magnesium has been completely
removed suggesting an open diagenetic system. Do-
lomite is rare even as microdolomite within the
crinoid grains.
The effects described are typical of meteoric
diagenesis (Gavish & Friedman, 1969; Land, Mack-
enzie & Gould, 1967; Longman, 1980) and direct
evidence of early surface lithification is furnished by
the calcretes and microkarsts which have survived
burial and infill by later sediments (Walkden, 1974;
Walkden & Davies, 1983).
In view of these general diagenetic characteristics
three effects have been examined that might be
capable of contributing to early cavity formation at
the crinoid/micrite interface. The first involves the
consequences of the stabilization of high-Mg calcite
during early meteoric diagenesis, the second explores
a dissolution/precipitation process, effectively neo-
morphic, but distinct from the thin film neomorphism
model, and the third examines the likely contribution
of direct subaerial solution.
259
MODELS FOR THE ORIGIN OF
SOLUTION CORONAS
A high-Mg calcite stabilization model
We believe that the chemical changes that occur
locally in the pore fluids as a result of the conversion
of high-Mg calcite in the crinoid grains to low-Mg
calcite could initiate dissolution of matrix in the
immediate vicinity of the grain. As high-Mg calcite
stabilization proceeds, Ca2 ions in the porewater are
+
exchanged with Mg2+ions in the grain leaving a fluid
slightly enriched in magnesium and depleted in
calcium (Land, 1967).
The removal of calcium ions from the porewater,
means that it is no longer saturated with respect to
CaCO,, whether calcite or aragonite, so dissolution
may take place. Such dissolution would first affect the
most unstable components in the vicinity of the
crinoid, namely, the micritic, partly aragonitic mud
matrix. This process is summarized in the following
equation which combines a typical CaC0, dissolution
reaction (Bathurst, 1979, with high-Mg calcite stabi-
lization :
CaCO, + H20 + dissolution
C 0 2 e C a 2 + + 2HCO;
+I
unstable
Relatively fluid
Pore M g l * j b c a 2 +ion exchange
mud matrix
(Ca, Mg) CO3
Stabilizing crinoid
Ion exchange between crinoid grains and the
solution pushes the dissolution reaction in the right
hand direction because the replacement of Ca2+ by
Mg2+ in the fluid does not maintain saturation with
respect to CaC0,. In addition the solubility of calcium
carbonate is apparently independently enhanced
merely by increasing the proportion of Mg2+ions in
freshwater solutions (Akin & Lagerwerff, 1965).
Although the crinoid grains represent significant
local concentrations of high-Mg calcite it is unlikely
that the dissolution effect could remove more than a
small proportion of the total volume of matrix
represented by solution coronas. Nevertheless the
effect would be preferential to the high-Mg grains and
marked in the case of crinoids because they are the
largest grains of this composition present. Indeed
according to Land (1967) echinoderms may undergo
stabilization to low-Mg calcite more rapidly than
other high-Mg calcite grains.
Probe analyses of rocks which contain solution
260 G.M . Walkden and J . R.Berry
coronas have revealed that there are no microdolom-
ites within the body of the crinoid grains, indicating
that Mg2+has been lost to the solution at some point.
It is important to note that in some early Brigantian
shelf carbonates, which consist of impure wackestones
with shaly interlayers, microdolomites have been
identified within the crinoids, indicating retention of
magnesium. In these rocks the crinoid grains have no
solution coronas around them.
A dissolution/precipitationmodel
We have discounted thin film neomorphism for the
development of syntaxial overgrowths within the
rocks in question but the factors believed to drive such
a process, specifically the stability contrasts between
micrite and coarse spar resulting from their physical
and mineralogical differences (Bathurst, 1975; Chave
& Schmalz, 1966), are still valid.
Could the neomorphic process operate instead
across a water-filled porespace up to 500 pm across?
Could it continue into deep burial diagenesis by which
stage the fine particles must have fundamently
changed? If the major proportion of the micritic
matrix was aragonite then such a process might have
operated, but only as long as the aragonite itself
survived. It is not now possible to determine the
proportion of aragonite in the original mud but it
seems unlikely that its dissolution contributed signifi-
cantly to syntaxial crystal growth since the earliest
zones seen within the overgrowths are present in
cements which line molluscan moulds. Most aragonite
may already have gone by the time the overgrowths
started to develop.
An alternative, however, is the phenomenon well
known to chemists as Ostwald Ripening where, under
experimental conditions, small micrometre-sized crys-
tals will dissolve in favour of larger growing ones
whilst merely sharing the same saturated solution (e.g.
Mahan, 1969; Lorens, 1981). Immediate proximity
across a solution film is not necessary. Applied to
recrystallizing limestones, and provided it operated
within a closed system, this process could conceivably
create a cavity at the crystal/micrite interface since
fine micrite with a total porosity of 50% or more would
be dissolving and reprecipitating as a large syntaxial
crystal with nil porosity. Added to this, the monocrys-
talline host grains were themselves actually porous,
containing a dense network of fine interconnected
canals. These pores would respond during crystalliza-
%on as if they were areas of damage to the crystal and
fill early, thus promoting removal of micrite around
the grain in the initial stages of diagenesis even before
any external syntaxial growth had appeared.
The inherent difficulty with the ripening model is
that the Dinantian limestones in question were
evidently not a closed system. Mg2+ions were flushed
out, and identical cements grew both in primary and
secondary porespaces (Fig. 6). Porewaters were thus
clearly oversaturated during periods of syntaxial
growth and there was no need for growing crystals to
draw upon surrounding micrite since an excess amount
of calcium carbonate in solution was available to them
from outside. Furthermore periodic solution of the
growing crystals themselves (Fig. 4)clearly indicates
external influences and considerable fluctuations in
water chemistry.
A meteoric solution model
Under conditions of subaerial diagenesis the most
obvious cause of dissolution within a body of limestone
is the direct action of undersaturated meteoric water.
Solutional secondary porosity is extensively developed
in some Recent and Pleistocene limestones (Bathurst,
1975; Stehli & Hower, 1961; Steinen, 1974) and
comparable pores and cavities are common in Di-
nantian limestones, especially in association with
palaeokarsts and calcretes.
Textural features of solution coronas such as their
irregular shape (Fig. 3), and occasional interconnec-
tion (Figs 3 and 5) with the possible removal of
allochems as well as matrix (Figs 3 and 4),lend support
to a meteoric solution model. In particular the
tendency for coronas to have enlarged preferentially
beneath grains (Fig. 2) could reflect the anisotropy of
the vadose zone.
In view of the widespread evidence for karstification
in late Dinantian limestones we consider that meteoric
solution could have been the main factor in the
development of solution coronas, but this model alone
does not adequately account for the centering of
coronas exclusively on crinoid grains. Although we
have argued that high-Mg calcite stabilization and
dissolution/precipitation had only limited effects,
these processes are specific to the crinoids and may
have been sufficient to initiate a cavity at the crinoid/
micrite interface. Thereafter the passage of under-
saturated meteoric groundwater would have enlarged
the cavities to produce a secondary porosity in the
normal way.
We thus consider that each of the three processes
could have been involved in solution corona formation
but meteoric dissolution may have been the most
important.
 Syntaxial overgrowths in limestones
S O L U T I O N CORONAS AND THEIR
C E M E N T FILLS
Integrating the development of the solution coronas
with the sequence of cements that fills them, we
reconstruct the diagenetic evolution of the rocks (Fig.
7) as follows :
Stage 1-unaltered marine sediment
The sediment was in its depositional environment and
consisted of crinoid fragments and other grains in a
matrix of unlithified carbonate mud, peloids and fine
bioclastic debris. All constituents had their original
mineralogies of aragonite and high- and low-Mg
calcite.
Stage 2-introduction into the meteoric environment :
development of an initial marginal cavity around crinoid
Marine sediments were uplifted into the meteoric
environment and an initial marginal cavity developed
by one or both of the two possible alternative processes
already discussed viz.,
(i) Phase stabilization-high-Mg calcite stabiliza-
tion began and proceeded rapidly. Pore fluids in the
vicinity of crinoids became enriched in magnesium
and depleted in calcium and this in turn led to solution
of the immediately surrounding micrite to produce a
laminar pore space.
(ii) Dissolution/precipitation-crinoid canal sys-
tems began to fill with syntaxial cement. The necessary
calcium carbonate for this cement was supplied either
through the dissolution of nearby aragonite, or by
Ostwald Ripening, or both. This led to the develop-
ment of a laminar pore space at the crinoid/micrite
interface which, if the process continued, progres-
sively increased in size ahead of the growing syntaxial
crystal.
By the end of this stage all matrix aragonite and
larger skeletal aragonite had dissolved releasing
CaCO, for cementation, and initial lithification of the
sediment was thus probably complete.
Stage 3-the further enlargement of porosity around
crinoid: production of a solution corona
At this stage there are several processes which may
have operated depending on the diagenetic environ-
ment and the fluid chemistry. Meteoric dissolution is
one effect and during periods of groundwater under-
saturation the initial marginal cavity around crinoids
26 I
would have become enlarged. If this occurred in the
vadose environment, the downward percolation of the
fluids may have created a geopetal corona. Dissolu-
tion/precipitation may still have been continuing, and
cement overgrowths became well established. These
earliest cements are the generation of mostly non-
luminescent calcites with thin bright subzones and
solution hiatuses (Zone 1) described earlier.
They are considered to have grown in a relatively
near-surface freshwater phreatic environment where
conditions were sufficientlyfluctuating to permit both
precipitation and dissolution. These cements devel-
oped within all accessible porespaces including mol-
lusc moulds and calcrete fenestrae. The bright sub-
zones within these cements usually have individually
recognizable characteristics and can be correlated
laterally over distances of up to 10 km, indicating that
they represent widespread events rather than random
local fluctuations. It is likely that the Zone 1 cements
grew in increments over more than one period of
subaerial emergence (Berry, 1984), and the bright
subzones could represent intervening stagnation in
the water table during marine submergence or they
may record actual pore water interchange events.
Ostwald ripening may have been most active during
stagnant phases.
Stage 4-stable 'deep' phreatic conditions :passive
occlusion of the solution coronas
This stage involved the development of the well-
organized syntaxial cement overgrowths of interme-
diate luminescence (Zone 3) which passively filled the
solution coronas and other primary and secondary
pores. The cements are everywhere uniform and free
from growth hiatuses or dissolution effects and there
was no return to Stage 3 growth conditions. On textural
grounds alone these cements must have grown in a
stable phreatic environment, where water chemistry
was uniform for long periods of time and no dissolution
took place. There was no further enlargement of the
coronas at this stage so their walls sometimes became
the sites for nucleation of small inward growing
crystals where these had not already been established.
Their isotopic composition suggests a moderately
deep diagenetic environment sealed off from surface
effects. However, they are unlikely to be pressure-
solution derived since they make up approximately
30% of the whole rock whilst stylolites produce only
an estimated 10% loss to the succession (Berry, 1984).
In any case Stage 4 cements are very obviously cut by
stylolites.
262 G . M . Walkdenand J. R. Berry

STAGE 1 Marine sediment

Grains and mud show o r i g i n a l t e x t u r e s and mineralogies.
A. c r i n o i d g r a i n (high-M c a l c i t e ) , 8. brachiopod
fragments (low-Mg c a l c i t e y , C. b i v a l v e fragment
( a r a g o n i t e ) , D. p e l o i d s (mixed composition),
E. mud m a t r i x (mixed composition).

STAGE 2 I n t r o d u c t i o n t o meteoric environment.

Grain and m a t r i x a r a g o n i t e s t a r t s t o d i s s o l v e . Laminar

c a v i t y around c r i n o i d g r a i n s begins t o develop by:
( i ) S o l u t i o n o f m i c r i t e d u r i n g high-Mg c a l c i t e
stabi l i s a t i o n
( i i ) D i s s o l u t i o n of m i c r i t e and p r e c i p i t a t i o n w i t h i n
c r i n o i d canal system through a r a g o n i t e diagenesis
and/or c r y s t a l r i p e n i n g .

STAGE 3 C a v i t y enlargement and passive cementation i n

shallow meteoric environment.

( i ) P e r i o d i c meteoric d i s s o l u t i o n enlarges a l l v o i d s
and creates s o l u t i o n coronas. Any e a r l y c r y s t a l growth
i s a l s o a f f e c t e d by s o l u t i o n .

( i i ) Continued dissolution/precipitation by c r y s t a l
r i p e n i n g creates s o l u t i o n coronas which grow i n advance
of expanding overgrowths. P e r i o d i c meteoric d i s s o l u t i o n
a f f e c t s b o t h voids and growing c r y s t a l s .

( i i i ) By t h e end of t h i s stage s o l u t l o n coronas are f u l l y

expanded and meteoric cements w i t h s o l u t i o n hiatuses
p a r t i a l l y f i l l a l l voids.

STAGE 4 Passive o c c l u s i o n i n s t a b l e b u r i a l p h r e a t i c
conditions.

Uniform cements d i s p l a y an i n c r e a s i n g degree O f c r y s t a l

o r g a n i s a t i o n and occlude s o l u t i o n coronas and o t h e r
voids. No f u r t h e r d i s s o l u t i o n e f f e c t s and microspar
grows from corona w a l l s .

Fig. 7. Alternative paths of evolution of solution coronas and their cement fills.
Stage 1 : marine sediment. Grains and mud show original textures and mineralogies. A, crinoid grain-high-Mg calcite; B,
brachiopod fragments-low-Mg calcite; C, bivalve fragment-aragonite; D, peloids-mixed composition; E, mud matrix-mixed
composition.
Stage 2: introduction to meteoric environment. Grain and matrix aragonite starts to dissolve. Laminar cavity around crinoid
gmins begins to develop by: (i) Solution of micrite during high-Mg calcite stabilization. (ii) Dissolution of micrite and
precipitation within crinoid canal system through aragonite diagenesis and/or crystal ripening.
 Syntaxial overgrowths in limestones 263

Fig. 8. Spired syntaxial overgrowths under cathodoluminescence. These early spires of brightly luminescent calcite contrast
strongly with the patchy poorly organized early stages of the non-luminescent initial overgrowths in Figs 2 4 . Such spires
normally quickly coalesce to form fewer and larger terminations. Bright specks within the crinoid itself are microdolomites
with a distinct red luminescence. Basinal turbidite, Asbian, Clitheroe, Lancashire. Scale b a r 4 . 5 mm.

By the end of this stage of diagenesis approximately
95% of the original porosity has been filled by cement.
Stage 5-jinalpore occluding cementation (not
illustrated in Fig. 7, see Fig. 5 )
This stage of cementation is characterized by the
generally very brightly luminescent generation of
mostly ferroan Zone 4 calcite. These bright cements
make up less than 5% of the total and so are
volumetrically and chemically in accord with an origin
by pressure solution (cf. Oldershaw & Scoffin, 1967).
Since they line both stylolites and intercrystalline
boundaries of earlier cements, but are never cut by
stylolites, they must be synchronous with or post-date
stylolitization. These cements are considered to have
formed under conditions of deep burial, probably in
excess of 1 km (Berry, 1984).
A more fully documented history of the cement
sequences discussed in the preceding sections will be
presented elsewhere.
OVERGROWTH MORPHOLOGY A N D
DIAGENETIC ENVIRONMENT
It has been suggested by Freeman (1971) and Walkden
& Berry (1984) that morphology of syntaxial over-
growths on crinoids can provide a useful indicator of
former diagenetic conditions. In the classic work of

Stage 3 : cavity enlargement and passive cementation in shallow meteoric environment. (i) Periodic meteoric dissolution
enlarges all voids and creates solution coronas. Any early crystal growth is also affected by solution. (ii) Continued dissolution/
precipitation by crystal ripening creates solution coronas which grow in advance of expanding overgrowths. Periodic meteoric
dissolution affects both voids and growing crystals. (iii) By the end of this stage solution coronas are fully expanded and
meteoric cements with solution hiatuses partially fill all voids.
Stage 4: passive occlusion in stable burial phreatic conditions. Uniform cements display an increasing degree of crystal
organization and occlude solution coronas and other voids. No further dissolution effects and microspar grows from corona
walls.
264 G.M . Walkden and J . R . Berry

Evamy & Shearman (1965) the earliest stages of
overgrowth in c-axial directions comprised well-
distributed crystal spires, probably reflecting the
surface distribution of stereom walls in the original
echinoid grain (e.g. Fig. 8), which progressively
coalesced during growth to produce fewer and larger
terminations. This spired pattern contrasts strongly
with that observed within all the late Dinantian
shallow water carbonates we have examined, where
c-axial overgrowths are initially irregular, closely
contouring the original substrate, and develop no
euhedral pattern until late. Freeman (1971) and
Meyers (1978) have described similar forms and we
regard the differences between the two styles as
significant.
The syntaxial crystals within solution coronas grew
initially in an unstable meteoric environment affected
by fluctuating water table levels and rapidly changing
water chemistry. Under these conditions a combina-
tion of surface tension effects and repeated solution
could have inhibited or repeatedly destroyed any early
spire growth. In the later stages of corona fill, uniform
cements reflect a more stable cementing environment,
in which the crystals were able to become better
organized and evolved towards a more euhedral
morphology.
In order to test this model we collected and examined
limestone turbidites of Asbian age from the Craven
Basin of northern England, which from their geologi-
cal setting are most unlikely to have experienced early
meteoric alteration of the type seen on the shelves and
platforms. In these rocks spired overgrowths of the
Evamy and Shearman type are commonplace in c-
axial directions (Fig. 8) and in the examples studied

Fig. 9. The age relationship between aragonite removal and syntaxial overgrowths on crinoids in a basinal limestone turbidite.
Asbian-Clitheroe, Lancashire. Scale bar-0.5 mm. (A) In plane light a shelter pore created by a mollusc fragment, A,
contains a small echinoderm grain, B. The mollusc shows relics of original structure and the crinoid is enclosed by an euhedral
syntaxial crystal. The pore is filled by coarse blocky calcite. (B) Under crossed polars the mollusc fragment is evidently replaced
by coarse neomorphic spar showing undulose extinction which extends into the shelter pore and surrounds the crinoid
overgrowth. (C) In cathodoluminescence bright cements surround the crinoid and have grown as microspar fringes and
overgrowths on micrite and larger grains. These bright cements overlie the top surface of the mollusc and can be seen as small
discrete crystals nucleated on its underside.
The crinoid overgrowth grew initially as fine spires (e.g. on surface C) but the early growth zones in this crystal are hard to
diFjnguish owing to their lack of significantly contrasting luminescence. This syntaxial crystal was then buried by non-
luminescent non-syntaxial cement of the same generation as that responsible for the neomorphism of the mollusc.
 Syntaxial overgrowths in limestones 265

the overgrowths clearly predate aragonite diagenesis than by the development of solution voids and their
(Fig. 9). Furthermore replacement of aragonitic grains subsequent fill by centripetal cement. These observa-
was achieved by neomorphism, producing coarse tions suggest that it was only relatively late in the
blocky spar with undulose extinction (Fig. 9B) rather history of diagenesis that pore fluids became suffi-
266 G . M . Walkdenand J . R. Berry
ciently undersaturated with respect to aragonite to
enable the conversion to calcite. Confirmation that
the early flushing out of magnesium, inferred in the
shelf and platform limestones, never affected the
basinal limestones is provided by the presence of
microdolomites (confirmed by probe analyses) within
the crinoid cores (Fig. 8).
In none of the muddy basinal limestones studied
can any case be made for growth of syntaxial crystals
into secondary porespaces, along the lines of the
solution corona process, since internal zones closely
match the final overgrowth shape. Instead, displace-
ment or replacement must have operated as syntaxial
spires extended out into the interparticle matrix (Fig.
8). These overgrowths may represent an early marine
cement similar to some possible Pleistocene analogues
(Evamy & Shearman, 1969) although they may more
plausibly represent precipitation from deeper forma-
tion brines.
GEOLOGICAL IMPLICATIONS OF
C R I N O I D S O L U T I O N CORONAS
A N D THEIR CEMENTS
Solution coronas are useful indicators of early meteoric
diagenesis and their cement fills record a full diage-
netic history of the events leading up to final porosity
occlusion. In fact owing to the favourable character-
istics of crinoids as growth substrates they effectively
magnify details of cement stratigraphy not seen
elsewhere, and enable valuable observations to be
made.
From a petrographic standpoint the removal of
micrite replacive overgrowths from the realm of thin
film neomorphism leaves their significance as regards
microfacies interpretation unchanged, provided that
coronas are counted as micrite. Whether they are
recognized as secondary pores or regarded as replace-
ments has little bearing on conclusions regarding the
nature of the original sediment. However, from an
economic standpoint the new model for the origin of
crinoid syntaxial overgrowths has useful implications.
Rather than representing neomorphism of an origi-
nally microporous and unpromising reservoir rock the
overgrowths represent the passive fill of a secondary
porosity of considerable reservoir potential. In the late
Dinantian rocks early diagenetic oxygenation prob-
ably removed all potential for local hydrocarbon
generation, but final pore occluding cementation was
sufficiently delayed for these secondary pore systems
to have been available for laterally migrating, basin-
derived hydrocarbons, at a time when oil generation
had not yet begun on the platform.
CONCLUSIONS
(1) Seen in cathodoluminescence syntaxial over-
growths on crinoid grains in late Dinantian packstones
and wackestones display characteristics inconsistent
with any of the existing models for the development
of such textures. We thus discount primary pore fill,
thin film neomorphism and late infiltration of mud as
likely processes and offer a new model involving
selective solution around crinoid grains followed by
passive growth of syntaxial crystals within the result-
ant cavities. We have termed these solution cavities
solution coronas.
(2) The evidence provided by textural and geologi-
cal relationships suggests that dissolution operated
early during near-surface meteoric diagenesis, and
three processes have been examined which might
account for the development of solution coronas.
These are: (a) local undersaturation of pore fluids
during ionic exchange when high-Mg calcite was
being converted to low-Mg calcite; (b) dissolution/
precipitation across a fluid-filled pore, driven by
inherent stability contrasts between fine particulate
carbonate and large crystalline objects; and (c)
dissolution by undersaturated meteoric water. The
first two models may help to explain why solution
coronas are centred exclusivelyon echinoderm grains.
(3) The earliest zones within the syntaxial over-
growths are generally non-luminescent and are iden-
tical to those seen in cements filling mollusc moulds
and calcrete cavities. The overgrowths themselves
therefore post-date initial lithification. However, the
conditions recorded within these earliest zones reflect
fluctuating near-surface conditions and the solution
coronas are therefore a useful indicator of such
diagenetic environments.
(4) Later phases of overgrowth involve uniform
cements with dull luminescence and reflect conditions
of stable burial diagenesis with elevated temperatures
and isotopically light pore waters. No further enlarge-
ment of the coronas took place. The final phase of
overgrowth seen within coronas post-dates local
stylolitization and the cements are iron-rich. They are
likely to have been derived from pressure-solution,
but are volumetrically unimportant.
(5) The growth morphologies of syntaxial over-
growths in solution coronas are quite distinct from
those developed in basinal limestones of the same age
 Syntaxial overgrowths in limestones
which never experienced contemporaneous meteoric
diagenesis. The latter overgrowths show well-organ-
ized serrated growth patterns which developed prior
to aragonite diagenesis and m a y therefore reflect
precipitation from marine or marine derived fluids.
ACKNOWLEDGMENTS
We thank Robin Bathurst (Liverpool), Tony Dickson
(Cambridge), Ian Fairchild (Birmingham), John Hud-
son (Leicester) and Bill Meyers (Stony Brook) for
helpful criticisms, a n d gratefully acknowledge finan-
cial assistance from the N.E.R.C. (GMW and J R B )
and the Royal Society (JRB).
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