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Lithos 55 2001.

125
www.elsevier.nlrlocaterlithos

Fluids in metamorphic rocks


J.L.R. Touret )
Department of Petrology, Vrije Uniersiteit, De Boelelaan 1085, 1081HV Amsterdam, Netherlands
Received 1 September 1999; accepted 4 April 2000

Abstract
Basic principles for the study of fluid inclusions in metamorphic rocks are reviewed and illustrated. A major problem
relates to the number of inclusions, possibly formed on a wide range of PT conditions, having also suffered, in most cases,
extensive changes after initial trapping. The interpretation of fluid inclusion data can only be done by comparison with
independent PT estimates derived from coexisting minerals, but this requires a precise knowledge of the chronology of
inclusion formation in respect to their mineral host.
The three essential steps in any fluid inclusion investigation are described: observation, measurements, and interpretation.
Obseration, with a conventional petrographic microscope, leads to the identification and relative chronology of a limited
number of fluid types same overall composition, eventually changes in fluid density.. For the chronology, the notion of GIS
Group of synchronous inclusions. is introduced. It should serve as a systematic basis for the rest of the study.
Microthermometry measurements, completed by nondestructive analyses mostly micro-Raman., specify the composition
and density of the different fluid types. The major problem of density variability can be significantly reduced by simple
considerations of the shape of density histograms, allowing elimination of a great number of inclusions having suffered late
perturbations. Finally, the interpretation is based on the comparison between few isochores, representative of the whole
inclusion population, and PT mineral data. Essential is a clear perception of the relative chronology between the different
isochores. When this is possible, as illustrated by the complicated case of the granulites from Central Kola Peninsula, a good
interpretation of the fluid inclusion data can be done. If not, fluid inclusions will not tell much about the metamorphic
evolution of the rocks in which they occur. q 2001 Elsevier Science B.V. All rights reserved.
Keywords: Metamorphic rocks; Fluid inclusions; Microthermometry; Granulites

1. Introduction
Most metamorphic reactions involve a fluid phase,
which plays a major role for a number of rock-forming processes: element transport, kinetics of crystal
growth or evolution, control of external variables,
)

Tel.: q31-20-444-7270; fax: q31-20-646-2457.


E-mail address: touj@geo.vu.nl J.L.R. Touret..

such as activity or partial pressure of volatile components, etc. In recent years, the petrology of this fluid
phase has become one of the most active fields of
research in metamorphic petrology. It can be approached from a number of ways: thermodynamical
modeling of heterogeneous mineral equilibria, evaluation of fluid flow through rocks, analysis of the
stable isotope signature left by transient episodes of
fluid percolation, evaluation of geophysical data e.g.

0024-4937r01r$ - see front matter q 2001 Elsevier Science B.V. All rights reserved.
PII: S 0 0 2 4 - 4 9 3 7 0 0 . 0 0 0 3 6 - 0

J.L.R. Touretr Lithos 55 (2001) 125

electrical conductivity., etc. All these techniques require completely different instruments and concepts,
to the point that most research groups specialize in
one or two of them, often ignoring the others. But
there is at least one way of approaching directly this
now-missing fluid phase the expression is from
the late Phil Orville., namely through the study of
fluid remnants preserved as inclusions in minerals. In
recent years, this scientific discipline has progressively gained a recognized place. It was born at
least in its modern form almost simultaneously in
France Poty, 1969. and in the former Soviet Union
Dolgov et al., 1967., through a combination of
several factors, most of them not directly related, as
follows:
The development of ready-to-use heating and
especially freezing stages, firstly conceived for the
study of ore deposits, but very soon applied to all
other rock types.
Widespread use of equilibrium thermodynamics.
Supported by the immense task done by experimental mineralogists and petrologists, this has led to a
true quantification of metamorphic petrology, notably through a more and more precise reconstruction of PT conditions followed by metamorphic
rocks through time.
The interest in inclusions has been raised by the
unexpected discoveries the word is from the late
Prof. Winkler, Gottingen. of fluid remnants in rocks
or minerals where the mineral composition would
not have given any indication on their possible occurrence. The best-known example is probably the
widespread occurrence of CO 2 in granulites, but
other cases could be mentioned as well N2 in
eclogites or diamond, etc...
These results have shown that paying some attention to fluid inclusions in metamorphic rocks was
indeed of great interest. But, at the same time, it
became also obvious that this type of study was not
easy. A number of difficulties were immediately
apparent: small size, but great number of inclusions
in any rock sample, multiplicity of inclusion generations, possible fluid leakage or post-trapping
changes Roedder, 1984.. This indicates a great complexity of fluidrmineral interaction processes in
metamorphic rocks, and for a number of workers all
these problems have thrown some doubts on the
reliability of fluid inclusions, in general. This is
v

probably the reason why, despite the fact that the


basic principles of their studies have been well known
for at least a quarter of a century and that a number
of observations do not require any other instrument
than a conventional petrographical microscope, fluid
inclusions still continue to be almost ignored in most
basic petrology textbooks, with few significant exceptions e.g. Spear, 1993.. This attitude is not justified: fluid inclusions are part of the rock, they occupy roughly the same volume as most accessory
minerals; therefore, they are as deserving of study as
any rock-forming mineral. After all, the fact that
they are fluid is just a question of reference temperature: if observation could be done close to absolute
zero, everything would be solid! But too many
petrologists hesitate to engage in this type of study,
estimating that they will have to spend a great deal
of time and effort for a questionable result. I do not
want to claim here that everything is possible, and
that any sample can be completely understood within
minutes. Fluid inclusion studies in high-grade metamorphic rocks have been considered as especially
difficult for a long time Roedder, 1981.. These
rocks, however, present a decisive advantage, namely
the possibility to record extensive PT information
from the composition of coexisting minerals. This
leads to a specific method of fluid inclusion studies,
which has progressively developed in the last
decades, and which has already been presented in a
number of publications notably Touret, 1977, 1981,
1987.. Most of these papers, however, remained
rather theoretical, and I have preferred to adopt here
a more practical approach, with a number of examples directly taken from the working documents used
in the lab, but never reproduced in final publications.
All these examples correspond to high-grade rocks,
notably granulites and eclogites. Not only because
these rocks correspond to a field of research where I
have been active for many years, but also because
they may contain exceptionally well-preserved inclusions, much easier to study than in many low-grade
rocks. For the preservation of good, easy-to-study
inclusions, the most important factor is not the depth
at which rocks have been buried, but the conditions
which prevailed during the crystallization of the
rock-forming mineral assemblage and, above all, the
way by which the rocks have been brought back to
the Earths surface.

J.L.R. Touretr Lithos 55 (2001) 125

1.1. The first step: sample selection in the field


A fundamental aspect of fluid inclusion studies
refers to the notion of scale transfer. In a given rock,
each inclusion, typically few microns in size, constitutes an independent, isolated system, which basically may give two sets of data: fluid composition
and molar volume. They will be used for the definition of a fluid isochore, extrapolated to high PT
conditions and compared to independent estimates
derived from coexisting minerals. The extrapolation
may be extreme, covering sometimes a temperature
range in excess of 10008C, requiring a very rigorous
working procedure. Any studied inclusion must be
carefully located within the host crystal, the host
crystal within a thin section, the thin section within
the hand specimen, and finally the hand specimen
itself within the field exposure. Every step of this
scale transfer may involve significant errors, notably
on the representativity of the studied objects, but any
researcher should be fully convinced of the fact that
the real fluid inclusion study already begins in the
field. Whatever the sophistication of later investigations, the quality of the final results will largely
depend on the attention given to field sampling. The
importance of getting good samples is essential: with
the exception of rocks which are foreign to their
immediate environment e.g. some eclogites lenses
embedded in low-grade rocks, all xenoliths in volcanic rocks., any sample intended for fluid inclusion
studies requires a very detailed study of the outcrop
or exposure. Not only all different lithologies should
be carefully recorded, but also all kind of microstructural information, corresponding to ductile as well as
to brittle deformation. For instance, in relatively
massive rocks, trails of late inclusions are often
parallel to major joints or open fracture directions. In
principle, the sampling should be done by the person
who will make the investigation, as he will pay much
more attention to the type of microstructural data
that might be relevant for the final interpretation.
With some experience, any fluid inclusion student
will immediately spot which mineral has the best
chances of containing good inclusions, and he will
select the samples accordingly: the color of the
quartz, for instance, can be very helpful not too
milky, but also not too clear.. I know some cases
where resampling, specifically intended for fluid in-

clusion studies, has resulted in an order of magnitude


increase in the size and number of workable inclusions.
Each case must be approached independently,
according to local conditions and settings; there are,
however, a number of basic rules, which are easy to
follow, like the following:
In metamorphic rocks, fluids are present either
in veins segregations., typically made of a dominant
mineral mostly quartz or calcite., or in rock-forming
minerals within the massive rock. There is a distinct
change in the relative importance of both modes of
occurrence with increasing metamorphic grade: in
low-grade rocks, segregations are dominant, whereas
the opposite tends to be true in high-grade rocks.
Whenever possible, both sites should be sampled and
precisely compared. This requires a very precise
study of the geometry and the mineralogy of the
veins, which can change drastically over short distances. If some veins contain idiomorphic crystals
growing in open cavities alpine-type veins., these
must evidently require special attention. They are the
best place to identify primary or pseudo-secondary
inclusions, formed at the time of the opening of the
vein. But then the idiomorphic crystals themselves,
as well as the succession of different mineral phases,
must be investigated with the greatest care. In some
famous examples from the Western Alps e.g.
Camperio, Wagner et al., 1972., veins have remained
active over a wide range of PT conditions, with
notably sudden pressure drops corresponding to incremental openings of the fissure. Each opening may
correspond to a renewed fluid influx, leading to a
great variety of phenomena mineral growth or dissolution, phantoms or faden structures., which need
to be fully understood before starting the fluid inclusion study.
The study of large veins is a very specialized
task, more related to ore geology than to metamorphic petrology. Monomineralic veins occur often
along major fault or shear zones, witnessing the
passage of fluids issued from a very distant source.
In general, they are not or only in partial equilibrium
with the immediate surrounding, with evidence of
retrogression or growth of new, low-temperature
mineral phases carbonates, zeolites, etc... This introduces almost always a great complexity, with a great
number of different fluid pulses, which may be very
v

J.L.R. Touretr Lithos 55 (2001) 125

variable over short distances. The study of individual


inclusions in this type of environment might be very
deceiving. Only techniques that can provide a bulk
signature stable isotopes, crush-leach analyses of
relatively large samples. may give some results, with
always the risk of mixing up fluids of very different
age and origin. Smaller veins as an order of magnitude, of centimetric to decimetric scale. are far more
interesting, notably when they contain the same mineral assemblage as the surrounding rocks: andalusiteor sillimanite-bearing segregations in metapelites
might be taken as a typical example. In this case, the
segregation belongs to the metamorphic assemblage,
and it require to be studied and sampled with
the same care as the rest of the outcrop. Note that, as
a rule, relatively large veins are rather deceiving,
especially when filled with conspicuously milky
minerals quartz.. This color is precisely given by
millions of inclusions, too small and too abundant to
be correctly studied. Relatively clear quartz is more
interesting but if the vein is massive the fluid evolution within the vein itself typically from the edge
towards the center of the vein. might be difficult to
trace. Experience shows that the best veins are relatively small cm size.. These can easily be compared
to the surrounding rock, especially when they contain, besides the dominant mineral in most cases,
quartz., some mineral phases indicative of given
PT conditions Al-silicates, zeolites, etc.. The study
of larger veins may be rewarding best example to
date remains the systematic study of Alpine clefts,
Mullis et al., 1994., but it may take years to get a
clear picture of overall results almost a lifetime in
the case of the famous cleft of Camperio, Tessiner
Alps, Wagner et al., 1972..
Even if they contain, in general, less spectacular
inclusions, the study of massive rocks might be
finally less complicated at least less time-consuming than the study of veins, only for the
smaller size of the reference system typically: hand
specimen.. Similar rules of sample selection can be
applied notably avoiding milky crystals., as soon as
the rock texture is coarse enough average crystal
size, about 0.5 to 1 cm.. Besides all kinds of possible
microstructures foliation, schistosity, microfolding,
jointing. special attention should be given to any
evidence of retrogradation. There is a rather general
rule that the latest events in terms of metamorphic
v

assemblage, notably a partial retrogression of peak


metamorphic minerals, will correspond to the greatest number of inclusions. In many granulites, for
instance, metamorphosed at more than 7008008C,
most visible inclusions must have been formed below about 3008C. Note, however, that this does not
systematically indicate, contrary to some statements
Lamb et al., 1987., that the fluid contained in these
inclusions has been introduced from outside, independently from the granulite metamorphism. It may
also be that these late inclusions correspond to the
local reequilibration of fluids already present for a
long time in the rock system, sometimes even since
the premetamorphic stage Vry and Brown, 1991..
I will end these general considerations by stressing the importance of selecting key exposures, studied and sampled. carefully in great detail for all
lithologies. This represents a somewhat different approach than for classical metamorphic petrology,
which normally addresses to the reconstruction of
PT conditions, and therefore concentrating on
good garnet-bearing!. mineral assemblages. Most
metamorphic petrologists finding a thick quartzite
containing a small layer of garnet or staurolitebearing metapelite in the field will tend to concentrate on and, in many cases, only sample the garnetbearing unit. For fluid studies, both protoliths are
equally important, and they should be sampled with
the same care and attention. As a working rule, a
complete study of an exposure, which will result in
the selection of up to about 10 samples, should
require at least. a complete day of field work,
maybe more if some elaborate sampling method
drilling. is required or if lithologies are very variable. Always remember to carefully orientate the
sample: the geometrical information contained in the
orientation of the fluid inclusion plane may be
extremely important Lespinasse and Pecher,
1993..

It is extremely frustrating to discover at a late stage


of the investigation a prominent direction whose
orientation cannot be defined because of the lack of
a measurement which would have taken few seconds
at the time of the field sampling. Note, however, that
if the fluid population appears to be interesting
enough, these 10 samples may represent months of
work in the lab, with thousands of dedicated
measurements microthermometry., and conclusions
which can be extrapolated to a regional scale.

J.L.R. Touretr Lithos 55 (2001) 125

1.2. Back to basics: the fundamental principle of


fluid inclusion studies
Compared to any rock-forming minerals, fluid
inclusions pose a number of specific problems small
size, variability, possibility of evolution after initial
formation., but they present also a decisive advantage: they give not only the chemical composition of
the trapped fluid system, but also its molar volume.
Both sets of information are essentially different, but
complementary: the composition indicates if a fluid
is in equilibrium with a given mineral assemblage or
not. Then, if this condition is fulfilled, the molar
volume will specify the PT conditions at which
this equilibrium has been reached. The interpretation
relies on a number of assumptions, all related to the
lack of variations of a number of factors between the
PT conditions at which a set of minerals has
equilibrated and the present-day situation, at which
the inclusion composition and molar volume are
measured: no variation of the volume of the cavity,
no leakage, no reaction within the fluid system. In
practice, all these hypotheses rely on the isochoric
behavior of the fluid inclusion system, expressed by
the familiar PT box intersection criterion: the fluid
isochore should pass through the PT field defined
by the rock mineral assemblage Fig. 1.. It is evident, however, that this condition is important, but
neither necessary nor sufficient. The intersection,
often rather loosely defined because of possible errors in PT estimates if the PT box is big
enough, it will be intersected by almost any isochore!., may be coincidental. This may notably happen when a fluid is introduced from outside, without
a notable influence on the mineral assemblage. Alternatively, the fluid might well be trapped along a
good isochore, but outside the PT box of mineral
equilibration. In total, the intersection condition
must only be taken as a first, important indication,
which must be complemented by a number of other
arguments Touret, 1987..
1.3. Not one (PT box intersection), but (at least)
three conditions
When an inclusion is hermetically sealed, it contains a given mass of a fluid, under any physical
state liquid, solid, vapor, supercritical fluid.. If the
inclusion volume remains constant, then pressure

within the inclusion will be related to the temperature by the fluid isochore, in first approximation a
straight line in the PT space. Fig. 1..
If inclusions are formed at the time of the crystallization of a given mineral assemblage, if the fluid
trapped in the inclusion is representative of the free
fluid phase existing at these PT conditions, and if
no perturbation has later occurred, then the fluid
isochore must correspond to the PT conditions
defined by the mineral assemblage; all these conditions are required for the theoretical justification of
the intersection criterion. It would be evidently possible to refine this approach by solving the isochore
equation, namely by knowing at which precise point
of the isochore the inclusion has been formed. There
are indeed some possibilities, such as intersecting of
the isochores by another univariant P s F T . relation e.g. geothermal gradient., crossing different
isochores, finding in the fluid system internal fluid
thermometer, see a more elaborate discussion in
Touret, 1981.. But all these procedures are so loaded
with potential uncertainties or problems that they
have been very rarely used and, as a matter of fact,
they tend to disappear from the current fluid inclusion literature. The PT box isochore intersection
remains the only condition, too often directly used
for the interpretation of fluid inclusion data without
further justification.
It is, however, evident that the inverse problem,
namely inferring from an intersecting isochore that
the inclusion fluid represents the metamorphic free
fluid phase, is not straightforward: the intersection
can be coincidental, the inclusion may have been
formed on the isochore, but outside of the PT box,
etc. Evaluating the reliability of the fluid contained
in an inclusion is always a difficult problem, which
requires much thinking and an elaborate discussion.
The best probability to identify fluids in equilibrium with a given mineral assemblage that I will call
synmetamorphic fluids require not only one condition, namely the isochorerPT box intersection,
but, at least, two more as follows:
i. Inclusions should be primary with respect to
this mineral assemblage. This should notably be the
case for the minerals which have been used for the
definition of metamorphic PT conditions best example: garnet.. Note, however, that secondary inclusions may also be used, if but it requires demon-

J.L.R. Touretr Lithos 55 (2001) 125

Fig. 1. Isochoric principle of fluid inclusion interpretation, with corresponding model histograms Insert.. Top: One fluid generation, with
possible post-trapping changes during the retromorphic evolution. Tr. in.: Initial trapping fluid isochore 1, in mineral G1 ., Tr. f.: Final
X
Y
closure of the inclusion 2, 2 , 2 ., depending upon the PT path, in mineral G2 . Hatched: Safety corridor, in which the inclusion will be
preserved at any external PT conditions. Bottom: Case of several fluid generations, trapped during the retrograde evolution. PT paths:
PI s pseudo-isochoric, ITD s Isothermal decompression, IBC s Isobaric cooling.

stration! microfracturing and fracture healing has


occurred at constant pressure and temperature.
ii. The fluid composition of the inclusion must
be compatible with those predicted from the mineral
assemblage. Any significant deviation, for instance,
the fact that most inclusions in granulites are anhydrous, whereas a finite H 2 O pressure is imposed by
the possible occurrence of some hydrous mineral

phases, should be interpreted in terms of isochore


correction see the discussion on the case of Central
Kola granulites..
The question whether post-trapping changes have
occurred after initial formation of the inclusion is
obviously of fundamental importance. There is a
general belief, distinctly expressed by some of the
greatest names in the science of inclusions e.g.

J.L.R. Touretr Lithos 55 (2001) 125

Roedder, 1981., that deep inclusions, formed at


high PT conditions, will suffer more changes than
inclusions formed at shallower levels. In fact, a
simple look at Fig. 1 shows that this is not the case,
and that the driving force for post-trapping evolution
will be only dependent on the relative trajectories of
the fluid isochore, on one hand, and on the metamorphic PT path, on the other hand. This driving
force is directly expressed by the difference between fluid in the inclusion. and solid outside of
the inclusion. pressures. At any temperature, the first
one will be given by the isochore, the second one by
the metamorphic PT path. If both are equal or
sufficiently close, as in the pseudo-isochoric PT
path Fig. 1., no pressure difference, no gradient for
fluid leakage or volume changes. The inclusion,
whatever its depth of formation, will remain perfectly safe until the surface.
If differences between both trajectories are large
enough to induce pressure differences exceeding the
strength of the host mineral, the inclusion will explode in the case of fluid overpressure, implode for
fluid underpressure Fig. 1.. This will result in
marked modification in the shape of the cavity, as
well as in the formation of a tridimensional set
cluster. of smaller inclusions. This is what we call
transposed or decrepitated inclusions. Since the
pioneering work of Lemmlein 1945. also Lemmlein and Kliya, 1952., the typical shapes and pattern
of secondary inclusions after decrepitation are relatively well known, essentially from a great amount
of experimental work Naumov et al., 1966; Leroy,
1979, and many others.. The group of R.B. Bodnar
at Virginia State University, USA, notably has submitted artificial inclusions to realistic PT trajectories, and he has obtained shapes remarkably similar
to natural inclusions Vityk and Bodnar, 1995a,b..
This experimental work has also documented a difference between exploded inclusions, star-like from
which are issued a number of aligned small inclusions, and imploded ones, which show more a
circular shape surrounded by a rim of minute cavities
Boullier, 1999.. In this last case, the initial volume
of the cavity is grossly diminished, whereas it tends
understandably to increase in the case of exploded
inclusions. The extreme limit of size reduction corresponds to the collapsed inclusions Touret and
Huizenga, 1999., in which the inclusion cavity is

completely squeezed around one or several microcrystals initially floating in the inclusion fluid. The
degree of collapse is so great that it is obvious that,
if these crystals had not been there, the cavity would
simply have disappeared without leaving any trace of
its former occurrence.
It would of course be extremely interesting to
know at which pressure difference the cavity will
start to evolve. In this case, if we could find in a
given sample inclusion formed before and after the
decrepitation event, we could precisely constrain the
shape of the retrograde PT path Fig. 1.. This
problem has also been approached during experiments, mostly to recognize that so many factors are
involved nature of the fluid and host mineral, size
and shape of the inclusions, absolute PT conditions, etc.., that it is hopeless to expect quantitative
results. The definition of about 12 kb for the safety
corridor of inclusion during retrogression, which had
been proposed on the basis of early experiments
notably by Leroy, 1979., can only be taken as a
very rough order of magnitude. Some CO 2 inclusions in mantle xenoliths, apparently well protected
within the enclosing basalt, could withstand internal
fluid overpressures in excess of 10 kb!
If a careful observation of the inclusion shape
may indeed provide a number of interesting data, it
is also very important to realize that perturbations,
whatever they are, may also occur without leaving
any visible evidence. Inclusions may recover a perfect equilibrium shape, but the fluid isochore will
pass way out of the relevant PT box. Isochore
passing well below the PT box are relatively frequent, a direct evidence of important fluid leakage.
But isochores passing above the box have also been
found. In this case, the volume of the inclusions
must have decreased, without loss of the fluid content. The process must not be spontaneous, it requires some energy which can only come from local
deformation. A spectacular case corresponds to the
superdense inclusions observed in the mobilisate of
some migmatites van den Kerkhof and Olsen, 1990..
1.4. Organization of the inestigation: obseration,
measurement, interpretation
Any fluid inclusion investigation involves three
successive steps, which must be carefully evaluated

J.L.R. Touretr Lithos 55 (2001) 125

and planned: observation, measurements and interpretation. Firstly, the obseration, with conventional
petrographical microscope, should identify a limited
number of inclusions, to be analyzed by specifically
adapted techniques, from the thousands of inclusions
present in any sample. The second step corresponds
to measurements, involving always microthermometry, eventually completed by direct chemical analyses mostly Raman.. Finally, the interpretation is
done by comparing few selected inclusion data, assumed to be representative of the whole inclusion
population, with independent mineral PT estimates. All these steps are interrelated, with constant
feedback and mutual improvement: the first observed
inclusion might lead to the beginning of an interpretation, which needs to be carefully checked for further confirmation. It is essential to separate clearly
these three steps, as well as to define precisely each
objective. The importance of this organization is
exemplified by the number of inclusions concerned,
decreasing by several orders of magnitude at each
step. From the thousands if not millions. of inclusions occurring in any sample, only few tens sometimes few hundreds. can possibly be measured, and
the final interpretation will only rely on few typically less than five. single inclusions. This enormous
focussing of the objectives needs to be done in a
somewhat rational way, leaving, however, enough
flexibility to cope with the unexpected. This working
procedure at least the one used in our group will
be illustrated by worked examples, showing working
documents which, normally, are never published in
scientific papers often to my regret, as many contain
a wealth of interesting information!.. But, before
going into details, it is necessary to stress the importance of the sample preparation. Much time and
effort will be done in vain, if the object put under the
microscope does not meet a minimum of quality
requirements.
1.5. Some introductory remarks: the importance of
the quality of the Fluid Inclusion Section (FIS)
After a careful selection of the sample in the field,
the importance of the next step, namely the fabrication of the standard FIS or Fluid Inclusion Plate,
FIP., should not been underestimated. A FIS is a

double polished loose plate, of the size of normal


thin section approximately 3 = 5cm., but significantly thicker. The quality of the polishing, the ideal
thickness typically between 90 and 120 mm., depending on the transparency of the host crystal and
the inclusion size and abundance, are very important
factors. Every lab has its own technique, and every
worker has experienced how frustrating can be the
occurrence of too many scratches, loose grains of
polishing materials, or, even worse, artifact inclusions caused, notably, by the binding media fluid
immiscibility in epoxy can be very spectacular!..
These points, however, are so obvious that they do
not deserve any further comments. More important is
to remember a number of important recommendations as follows.
Before making the FIS, a rather long, expensive
operation, it is always rewarding to observe carefully
a normal thin section at high microscope magnification. Polished thin sections are better than covered
ones, but all can be used. Small inclusions less than
5 mm. are preserved, and if no interesting inclusion
is seen, there is not much hope that a specific
preparation will do better.
Pay the greatest attention to the mineral texture
and composition, at the scale of the thin section:
Whenever possible, mineral analyses used for inferring PT data should be done on the preparation
used for fluid inclusion studies alternatively, on a
polished thin section very close from the FIS..
For microthermometric measurements, the section will be broken into small pieces and, in many
cases, the rock-forming minerals will be studied
almost grain by grain. Is it essential to keep a good
record of the whole FIS, in order to replace the
broken fragments or isolated mineral grains in their
original position. We use normally high-quality photographs of the whole section, approximately enlarged to A4 format. This is rather expensive and, in
many cases, cheaper alternatives may give very good
results. For instance, when the mineral grains are
coarse enough and sufficiently transparent or contrasted., just put directly the FIS on a magnifying
copy machine and enlarge by successive steps, unless the required format is reached. Modern technique offers a number of other possibilities, such as
optical scanner, computer images by digital cameras,
etc. In any case, the final image, as the one illusv

J.L.R. Touretr Lithos 55 (2001) 125

Fig. 2. Example of a fluid inclusion section FIS., which first must be studied globally during the observation stage conventional
petrographic microscope., then broken in small pieces for microthermometric measurements. All inclusions identified in the broken pieces,
even if very small, must be eventually replaced into their original context. B. emplacement of the drawing of Fig. 4. Dabie Chan eclogite,
Central China, Sample 94M44, Bin Fu.

trated in Fig. 2, can be used as a base for actually


mapping the distribution of fluid inclusions, conveniently grouped and labeled in terms of fluid types.
The procedure that we use in our group is described
in some more details below.

2. Observation with conventional microscope


The objective of the microscope observation, before any measurement, is more than a simple cursory
identification of the inclusions. It should aim at the
definition of fluid types and, above all, at a relative
chronology of the different inclusion generations. In
the discussion of the fundamental principles of inclusion interpretation, I have stressed the importance of
this chronology. It will be sufficient here to repeat
that the only clue is observation, and that any interpretation will be severely limited if no reliable result
has been obtained for this essential part of the study.
It is easy to find in the literature a number of
statements where authors claim that they did their
best, but that finding out this chronology was impossible. May be their samples were not adapted to this
type of investigation and, if so, why did they choose

them? But I have also the impression that, in many


cases, not enough time and efforts have been spent.
A partial chronology is always possible and I could
mention a number of cases where, after a first,
hopelessly complicated and negative impression, a
logical organization has progressively emerged,
sometimes after days of careful, painstaking work
behind the microscope. Good observation requires
time and effort. It will never be done in vain,
provided that it follows some strict rules for the
evaluation and the reproduction drawings. of the
results.
2.1. Definition of fluid types. The importance of
correct drawings
A fluid type is defined as a set of inclusions
having roughly. the same chemical composition e.g.
low-salinity aqueous, CO 2-rich, etc.., eventually
variable density in nature, a sufficiently great number of inclusions will never have the same density!.,
approximately trapped at the same time. The term
approximate indicates indeed that the precise timing of the inclusion formation is rarely known. It
may also covers a number of different issues: it may

10

J.L.R. Touretr Lithos 55 (2001) 125

be that the fluid type has occurred only briefly as a


free volatile phase at the time of initial inclusion
formation, but that a number of inclusions have
suffered post-trapping changes. Alternatively, several

fluid pulses of the same composition have occurred,


but at variable PT conditions. In any case, the
notion of timing is essential, and it requires to be
considered with the greatest care.

Fig. 3. Camera lucida drawing of cluster top. and trail-bound inclusions bottom., showing evidence of post-trapping perturbations
Swanenberg, 1980, all samples from RogalandrWest Agder, Norway.. Top left: Cluster of biphase H 2 ON2 inclusions, with variable
phase ratios. Upper right: Decrepitation cluster composed of monophase CO 2 inclusions. Bottom left: Poorly defined trails composed of
rearranged carbonic inclusions. A. Transposition of a pre-existing NS trail by decoration of subgrain boundaries S., B. Array of
decrepitation clusters.. Bottom right: Advanced transposition of a pre-existing NWSE oriented trail into short, subsidiary NS trails.

J.L.R. Touretr Lithos 55 (2001) 125

Compared to rock-forming minerals, fluid inclusions are short-lived objects. Their formation is instantaneous, or at least very short at geological time
scale. Since the early days of fluid inclusion studies,
a basic distinction exists between primary and secondary inclusions, according to criteria abundantly
discussed in the literature notably Roedder, 1984.. I
will not insist on these criteria, but recall that, in
massive rocks, the basic distinction is between isolated, clustered groups of few, typically 1020
neighboring inclusions, in the volume of the FIS.
and trail-bound inclusions Fig. 3.. Trail-bound inclusions, occurring in the surface of a former microcracks, are certainly secondary. Both terms are practically equivalent, with the further indication that trails
can conveniently be divided between intra- and intergrain trails Touret, 1981., an indispensable step for
starting the chronology of secondary inclusions see
below.. Isolated inclusions are, in principle, primary,
but this term should only be applied if additional
criteria are available direct relation with the growth
features of the host minerals.. Otherwise, better keep
the pure descriptive name isolated., eventually a
more neutral term, if you want to stress the time
difference with secondary inclusions e.g. early..
Clusters may have quite different origins, either
neighboring isolated cavities in this case, no difference with isolated inclusions., or, very often, inclusions formed by transposition of a former, larger
cavity. As it is impossible to distinguish between
these two cases without the knowledge of the fluid
density, the neutral term cluster. should be kept
throughout the phase of observation, and all categories isolated, cluster, trail-bound. strictly maintained for the rest of the study. Not much interest to
identify carefully these different categories, if later
all are mixed during microthermometric measurements.
The working method for a good observation
should meet a certain number of elementary requirements and follow some basic rules as follows.
A major objective is to select a limited number
of inclusions, later analyzed by microthermometry or
any other nondestructive technique Raman, FTIR,
Synchroton radiation, etc..; selected inclusions must
be found back at any time, either for a proper
location within the analytical instrument, or after, for
control or further investigation. Not a trivial problem
v

11

for small objects few mm in size. evenly distributed


in the volume of the FIS.
Contemporaneous fluid types, which by definition have a different composition, can only occur
together if they correspond to immiscible fluids. This
important conclusion can be tested, not only from the
phase relations of the different fluid systems, but
also morphologically, from the occurrence of neighboring domains containing preferentially one fluid.
Note, however, that alternative hypotheses may also
occur, notably fluid incoming from different sources
and along different pathways, as well as a local
control of the fluid composition by fluidrmineral
interaction. In most cases, careful observation allows
to distinguish between these different possibilities, as
illustrated below for the case of Dabie Shan eclogite
Fig. 6..
Trail-bound inclusions are as a rule far more
abundant that early, isolated or clustered cavities.
There are also those for which the relative chronology is the most easy to decipher, from intersection
criteria and structural orientation of the microcracks.
They must be investigated first, then ignored, allowing the observer to concentrate on older inclusions.
In conclusion, the identification of the different
fluid types and of their relative chronology is a key
aspect of any fluid inclusion studies. It requires
much time and effort, and it must be supported by
detailed, accurate illustrations. Partial conclusions
might be rather subjective e.g. trail intersection
criteria., requiring constant crosschecking, reevaluation and discussion.
Figs. 46 illustrate the working method that we
use in our group, involving the notion of GSI see
below.. These cases have been selected, not only to
give some typical examples of the distribution of
fluid inclusions in metamorphic rocks, but also to
show the type of conclusions which can be derived
from a careful observation of these drawings: transposition of an early trail along a new direction in the
case of Fig. 4, mode of crack healing in Fig. 5, and
variation of fluid composition according to the nature of host mineral in Fig. 6.
Let us remark that, for evaluating the distribution
of inclusions in three-dimensional space, drawings
are much better than photographs, sharp only in a
very narrow focussing range at the high magnification normally imposed by the small inclusion size
v

12

J.L.R. Touretr Lithos 55 (2001) 125

Fig. 4. Drawing Working document. of a GSI, following the procedure used at the Fluid Lab., VU Amsterdam. Dabie Shan eclogite,
Sample Bin Fu, Location B, Fig. 2.. The inclusions are disposed along a former trail oriented XY, strongly transposed along the
Z-direction. All inclusions are reequilibrated during this transposition. Near each measured inclusion, the number indicates the homogenization temperature T h ., always to liquid in 8C.. Each of these inclusions is separately drawn on a working sheet for microthermometric
results, with the indication of all measurements initial and final melting, homogenization. and the volume ratio of different phases
liquidrvapor. at room temperature.

J.L.R. Touretr Lithos 55 (2001) 125

13

Fig. 5. Another example of GSI, with indication of the microthermometric Th . measurements. CO 2 inclusions in a plane of microfracture
trail-bound, secondary inclusions.. Near each measured inclusion, the number indicates the homogenization temperature T h ., always to
liquid in 8C.. For a pure fluid, Th indicates immediately the fluid density. Iso-density lines thin contours. are labeled in grcm3 . They show
some high-density highlands within a lower density environment. This pattern strongly suggests that crack healing has occurred in an
ambience of fluid density decrease from a given isochore, pressure decrease or temperature increase, evidently very unlikely in the present
case.. Quartz vein in gold deposit, Sierra Leone Barrie and Touret, 1999..

typically =25 or =50 objectives.. Then, even for


nonborn artists, exact drawings are easily made by
the grid procedure, namely replacing in one microscope ocular the reticule by a grid we use 10 = 10.,
identical to the one printed on the drawing sheet.
Any serious microscope dealer should be able to
provide this type of very simple grid. If not, check
by colleagues from biology or micropaleontology, or
from any discipline using counting procedures of
small particles cells, microfossils. in a fluid medium.
These drawings represent a set of inclusions seen
within a single field of microscope. They require to
be done as long as the distribution of the different
fluid type has not been properly understood, a task
which can be rather long for a complex sample. Less
time, however, that it may look at first sight to
inexperienced people. After some training, most
drawings can be completed in 1 or 2 hours including the one represented in Fig. 4., not much com-

pared to the time which will be spent for microthermometric measurements. Any observer will also experience that such a detailed study, rarely done for
most petrological investigations, is very rewarding,
not only for fluid inclusions, but also for the study of
many other small features, such as accessory minerals or very fine microstructures. For those, the FIS
provides much better observation conditions than a
normal thin section, e.g. for the appreciation of the
idiomorphic shape of small mineral phases, and it
should be in very common use in all branches of
petrology notably in structural petrology, so easier
to appreciate the orientations when you can observe
in three dimensions!..
2.2. Notion of Groups of Synchronous Inclusions
(GSI). Fluid chronology
Besides the knowledge of the actual inclusion
distribution, drawings are the only way to reach the

14
J.L.R. Touretr Lithos 55 (2001) 125
Fig. 6. Final presentation of fluid inclusion data in quartz crystals from the Dabie Shan eclogite, China Sample 94M55, Bin Fu, same rock type than in Fig. 2.. Left: General
view of part of the FIS, characterized by the trace of a prominent shear zone black with white dots, 6.. All studied inclusions occur in quartz 5, heavy contours., mostly
enclosed in the various rock-forming minerals: Garnet 1., Omphacite 2., Amphibole 3., and Epidote 4.. Besides the shear zone 6., the rock show also a number of oblique,
parallel lines of fractures 7.. In all studied quartz crystals, indication of the dominant fluid type: High-salinity brine W1., low-salinity aqueous W2., Gaseous pure
CO 2 sG2., mixed aqueousgaseous GW.. Right: Actual distribution of inclusions GIS. in quartz enclosed within different mineral hosts: Garnet a., Omphacite b.,
Amphibole c., Epidote d.. Numbers: homogenisation temperatures in a. CO 2 inclusionssG2., final melting temperatures in b, c and d. W1 fluids.. G2 fluids occur only in
domains within or very close to the shear zone. This, together with the fact that most G2 inclusions are trail-bound a., suggests a late CO 2 introduction, from an external source.
The same conclusion yields for W2 low salinity aqueous. fluids, mostly disposed along trails roughly parallel to the lines of fractures 7.. W1 fluids, on the other hand, are more
clustered, as seen in b, c and d.. Their composition salinity. is more or less constant within a given mineral host, but varies strongly between different minerals Tm -y258C in
omphacite, about y158C in amphibole or epidote, would be less than y108C in garnet.. This suggests that W1 fluid composition has been controlled by local fluidmineral
interaction, at the time of the crystallization of the enclosing host Fu et al., submitted..

J.L.R. Touretr Lithos 55 (2001) 125

notion of GSI, a most important notion in any rock,


in general, and in metamorphic rocks, in particular.
A GSI corresponds to a limited number typically
between 10 and 20. of inclusions formed at the same
time, which will serve as the test population to
evaluate the homogeneity of microthermometric data
notably Th .. The most obvious case for synchronous
inclusions correspond to a secondary trail, and in this
respect the notion of GSI, introduced in a recent
publication Fonarev et al., 1998., corresponds
closely to FIP Fluid Inclusion Plane. or Fluid Inclusion Assemblage FIA. of American authors Goldstein and Reynolds, 1994.. Semantics is not very
important, and any acronym can be used. I only
prefer the name GSI, because the bidimensional
surface of an inclusion trail is often more complex
than a plane, also because it emphasizes the importance of timing in fluid inclusion making. A typical
example of GSI is shown in Fig. 5. It corresponds to
a plane of secondary inclusions in a quartz vein from
a gold deposit in Sierra Leone Barrie and Touret,
1999..
Once the GSI have been clearly identified, establishing the chronology of trapping is just a question
of patient, critical observation. The first distinction is
evidently between isolated primary. and secondary
trail-bound. inclusions. Further refinement requires
the following.
For the primary inclusions, a detailed analysis of
the mineral textures: old deformed. grains, recrystallized subgrains, etc. Even if inclusions can be found
in a number of other host minerals garnet, pyroxene,
feldspars, etc.., quartz remains by far the mineral in
which inclusions are the most abundant. But it is also
the mineral which suffers most easily deformation
andror recrystallization, on a wide range of PT
conditions. It must consequently be studied with the
greatest attention, and any technique able to reveal
its internal structure, notably cathodoluminescence,
can be extremely helpful Behr, 1989.. Cathodoluminescence for quartz is, however, much more difficult
than for other minerals, notably carbonates, but its
use should become almost mandatory in a near future.
In high-grade rocks, we do systematically search
fluid. inclusions in quartz included in other rockforming minerals, notably garnet. These quartz crystals have commonly escaped any deformation, and
v

15

they may contain few, but really primary inclusions.


Fig. 6 shows a spectacular case eclogites from
Dabie Shan, China., but there are a number of other
examples in the literature Blom, 1988; Vry and
Brown, 1991. which shows the interest of this type
of research.
For secondary trail-bound. inclusions, finding
out the chronology relies essentially on intersection
criteria of planar structures, with the additional complexity that these structure are not continuous, but
formed by a regular grid of more or less identical
inclusions shape and size.. I have illustrated in
earlier publications Touret, 1977, 1981. some cases
which are frequently observed: replacement of an
inclusion fluid by another while preserving the shape,
partial fluid mixtures, disappearance of few inclusions within the trail, etc. Possibilities are almost
unlimited and, in many cases, results are apparently
contradictory: Fluid A, apparently younger than B in
a given mineral grain, seems to be older in another.
It is our experience, however, that after careful observation, these uncertainties progressively decrease,
until a firm conclusion can finally be reached. Every
researcher has experienced an initial feeling of apparent chaos, which becomes more and more organized during the course of the observation and microthermometric measurements.
Much work is presently done by the Nancy group
Lespinasse, 1984; Lespinasse and Cathelineau,
1990. on the microstructural study of inclusion plane
orientation. Measurements are easy, either by elaborate techniques image analysis., or more simply, by
estimating under the microscope the orientation and
the dip of the plane by changing the focussing level..
Measurements of orientation are very easy for subvertical trails, but then the complete study requires a
set of three orthogonal FIS. The universal stage,
almost abandoned by the petrologists, could find
here a new field of application. It is again an important new field of research, too neglected by structural
geologists.
In conclusion, the rigorous methodology described above, which may look tedious, time consuming, is absolutely necessary to get a proper
preparation of the microthermometry measurements.
It allows, in most cases, to identify a few major fluid
types, typically between 2 and 5, which need to be
correctly labeled. Neutral names Type I, II, III, etc..
v

16

J.L.R. Touretr Lithos 55 (2001) 125

may be misleading for instance, successive numbers


implies almost instinctively some chronological order.. Moreover, they make the reading of any paper
rather difficult, notably because they do not give any
indication on the composition. Conversely, a name
which tends to give the complete composition becomes rapidly impossible H 2 ONaClCO 2 CH 4
inclusions, etc... Some recommendations have been
proposed in the literature Boiron et al., 1992., but
everyone is free to choose the best label adapted to
his case, provided that it is clear, informative and not
misleading. We tend in Amsterdam to privilege letters 2 maximum. for the first definition W s
aqueous, G for gas, M for mixed aqueous gazeous.,
eventually supplemented by indices W1, etc.. for
subtypes, with, in most cases, a chronological connotation W1 older than W2, etc... An example of this
labeling is given in Fig. 6.

3. Measurements (microthermometry, eventually


completed by Raman analyses)
3.1. Some general considerations
Once the fluid types have been identified, a reasonable number of inclusions must be selected, in
order to measure the fluid properties: composition
and molar volume. As for any fluid inclusion studies,
this is done by measuring the temperature of phase
transition, final melting Tm ., eventually supplemented by Raman analyses, for the composition,
homogenisation Th . for the density molar volumes..
Then, from these measurements, which may amount
to hundreds of inclusions in a single sample, few
typically less than 5. representative isochores
in fact, inclusions are selected, which can be
compared to mineral PT data Fig. 1 for the theory, 9 for a practical example.. This last phase of
interpretation is, in fact, the justification of the whole
study: only then it is possible to verify if the fluids
trapped in inclusions are compatible with the host
mineral assemblage and to what extent they have
been modified by post-trapping changes. In other
words, it is only at the very end of the study if we
finally know if all the efforts made were really
worthwhile. Note, however, that all steps of the
study observation, measurement, interpretation.,

even if clearly defined, must be done almost simultaneously: a few measurements are normally needed
for the characterization of the different fluid types, if
only to distinguish between gaseous and empty inclusions. It is also advisable to start some kind of
interpretation, as soon as some microthermometric
parameters are known, just to have an idea how fluid
inclusions relate to the rest of the rock history. These
preliminary attempts, however, must be done with
great care and critics, in order to avoid any biased
interpretation. In a rock where many inclusions are
present, it is too easy to select only those which give
good results, namely isochores, which for one reason or another, just pass through the relevant mineral
PT box. Another danger, especially for beginners,
is to sit down behind the stage and accumulate data,
hoping that some light will come some day from the
dark. In almost all cases, the night becomes unfortunately even darker, and then the most frantic efforts
are done, just to recuperate all the hours spent in
vain. Accumulating microthermometric data is an
active part of the whole research, not a passive
reading of numbers on a digital screen while listening to a walkman or a compact disc.
Measured inclusions must be precisely identified
on the GSI drawings e.g. Figs. 4 and 5. and, in
principle, a careful drawing of each measured inclusion must be done on a separate sheet, before starting
the microthermometric run. This procedure is absolutely necessary for two-phase LrV. inclusions at
room temperature. For inclusions which homogenize
to liquid, pressure increases very rapidly after homogenization. This may cause irreversible changes
leakage, volume increase of the cavity., which are
indicated by an increase of the volume of the gas
bubble when returning to initial conditions. But any
change can only be appreciated if the relative volume of the different phases had been carefully evaluated before heating. For monophase inclusions, this
rather tedious procedure might look somewhat unnecessary. But it can be very helpful, especially
when starting measurements on a new fluid type.
Many phase transition phenomena are not obvious
e.g. sublimation., and there are so many possibilities clathrate melting, complicated phase transition
in purely gaseous inclusions, etc.. that it is difficult
to predict what will happen, sometimes for few
seconds e.g. melting and homogenisation in dense

J.L.R. Touretr Lithos 55 (2001) 125

CO 2 inclusions.. False phase transitions may also


be a major problem: during freezing, the stage may
show minor movements, which need to be constantly
corrected by playing with the fine focussing of the
microscope andror the XY movement of the stage.
This may induce optical effects, notably some bright
points in subspherical cavities, which may be mistaken for gas bubbles. Experience is of course of
major importance, as it the need to only retain clear,
repetitive phenomena. But the best way to gain this
experience is to make precise drawings of any supposed phenomenon at the time of its appearance.
This will be greatly facilitated if a good sketch of the
inclusion contour is already available. Recording
microthermometric runs on videotape may also be
helpful, but the optical resolution of most recorder is
much less than the eye, and accumulating videos
become rapidly extremely boring. Again, quick
drawings are much faster, more precise and, finally,
far more informative.
3.2. Representation of compositional data: compositional diagrams and histograms
The basic problem is clear: how to reduce the
great variability of any inclusion population to few
representative values. The notion of GSI is the first,
most important starting point: if inclusions belonging
to the same generation already show a great dispersion, mixing many generations will only complicate
the situation. But some GSI may contain too few
measurable inclusions and, in most cases, it is necessary to compare GSI from different parts of the
investigated samples. This can only be done by some
statistical treatment of the data, through some kind of
variation diagrams or frequency histograms. Statistics are used in many disciplines, in a simple or
elaborate form. Compared to neighboring specialities
e.g. fission track., we can only realize that the
statistical treatment of fluid inclusion data is still in
its infancy. Far too often, representative values are
freely chosen, sometimes without giving the most
elementary information number of measurements,
range of instrumental error, etc... It is impossible to
discuss here this important problem at length, but I
will briefly comment on the most frequently used
modes of presentation: density histograms and compositionrdensity diagrams.

17

3.3. Density histograms


Data from inclusions belonging to fluid types with
a well-defined, relatively constant composition are
commonly presented in the form of density histograms, which for pure fluids are, in fact, Th histograms. I have already shown Fig. 1. how simple
considerations on the histogram shape e.g. distortion
towards high temperatures. may detect some perturbations, helping to concentrate on the most significant inclusions. This approach can be developed by
the notion of model histograms Touret, 1987.
which, roughly speaking, corresponds to the prediction of some histogram shape from a given hypothesis. An example is the modeling done by Darimont
and Coipel 1982. on necking-down processes, according to simple hypotheses on the temperature of
inclusion fragmentation. Others attempts have been
done for boiling fluids Touret, 1987., and there is
no doubt that this approach could be considerably
developed. In general, however, most papers do not
attempt any kind of statistical treatment. Data are
loosely accumulated in temperature intervals, and the
representative value is freely chosen from a more
or less clear maximum peak. on the histogram. It
might be difficult to do it otherwise, but, at least,
some basic information should always been given as
follows.
Always indicate the total number of measurements. Even if it can almost never said that a given
histogram is truly representative of the total number
of inclusion contained in the investigated sample,
500 measurements give more confidence than 5 or
10.
A peak should be defined by a sufficiently
high number of values, namely it must clearly differentiate from the background. This is normally done
in a rather subjective way, which, in fact, determines
the number of measurements to be done. Sometimes,
a peak is clear after few 10s of measurement, in
other occasions the number has to be much greater.
The only way to feel it is to build up the histogram
progressively, when the measurements are being
done.
In most stages notably in the Linkam., microthermometric results are expressed with a precision of 0.18C. This is far to be the real precision of
the measurements, and the data are collected within
v

18

J.L.R. Touretr Lithos 55 (2001) 125

temperature classes, broad or thin in function of the


overall variation range: about 18C for Tm , up to 5 or
even 108C for Th . As seen on Fig. 7, the size of the
temperature class has a great influence on the shape
of the histogram. This parameter should be carefully
evaluated and discussed before selecting the best
mode of presentation.

Finally, whatever the motivation, the selected


values should be clearly indicated on the histogram,
in the form of arrows above the histogram Fig. 7..
This is the only way by which the reader can rapidly
evaluate the degree of confidence that he can attach
to this selected value.
Besides histograms, it might be very instructive to
have an idea of the spatial distribution of the densities in a given histogram, notably within a plane of
secondary inclusions. This can be done by indicating
Th on the GSI drawings and, when some ordering
appears, by drawing iso-density contours by interpolation of the measured values. An example is given
in Fig. 6. It shows that, in the plane of the GSI,
relatively high-density inclusions correspond to some
islands within a lower density environment. Such a
density change can either occur by decreasing pressure at relatively. constant temperature or by increasing temperature at constant pressure. Needless
to say, the first hypothesis is the most probable for
healing a microcrack.
When comparing different GSI, the number of
histograms becomes rapidly a major problem: the
different histograms must be precisely compared,
with, notably, the same temperature scale. But a
figure with, let us say, more than 10 histograms is
practically unreadable. We prefer to show only the
range of variation of each histogram, supplemented
by a number of boxes which refers to the fluid
types occurring in the different samples. This procedure is illustrated in Fig. 8, which we will use for an
example of interpretation.
v

3.4. Compositional diagrams

Fig. 7. The importance of temperature classes for the shape of Th


histograms. Each histogram contains the same number of measurements 50., measured with the same precision results given
within 0.18C., but grouped in T classes from 0.258C in the top,
0.58C in the middle and 18C in the lower histogram. Arrows:
indication of the selected values if any. for further interpretation,
notably the selection of representative isochores.

When the composition of the different fluid types


may vary, principles discussed above remain valid,
but the situation is more complicated. The different
fluid types must be identified on a diagram compositionrdensity, in which, normally, the last variable
density. shows the greatest variation range.
This mode of representation is applicable to any
fluid system, but it simplifies in the case of binary
aqueous, referred to the H 2 ONaCl system wt.%
NaCl equivalent salinities in aqueous fluids.. XV
corresponds then to a Tm rTh diagram, widely used
for the representation of aqueous fluids. Each fluid

J.L.R. Touretr Lithos 55 (2001) 125

19

Fig. 8. T h data for CO 2-rich inclusions in granulites from the Central Kola peninsula, presented along the concept of GSI Fonarev et al.,
1998.. Each horizontal line represents a GSI, in one of the nine studied samples explanation of sample numbers, see text.. Each symbol on
a GSI line corresponds to a Th measurement. Boxes F1a, F1b, F12, F2, F2a.: Fluid types, corresponding to a given metamorphic phase:
F1a and b: M1 metamorphism, F2: M2 metamorphism, F12: transitional. F2a: primary inclusions in M2 garnet. 1 to 7, I to V arrows.: Th
data retained for the definition of the isochores drawn in Fig. 9.

types corresponds to a more or less. well-defined


domain in this diagram. Like for T h histograms, it is
possible to predict which trend will be given by
some phenomena, either geologically interesting
fluid mixing. or not fluid leakage.. Fluid types are
normally defined by loosely delimitated domains on
the ThrTm diagram, drawn subjectively by the researcher. It would be possible to get more precision
by contouring lines of iso-values, but this is very
rarely done.
The precision attached at the definition of the
different fluid types is very variable, depending on
the homogeneity of the different inclusions and the
time and effort that the investigator can devote to
their study. But, in any case, the database must be
well identified: how many inclusions have been mea-

sured, in which location, etc. The different types and


generation of inclusions must be correctly discriminated. Again, the inclusions retained for the definition of the representative isochores must be precisely
identified, in principle, by a clearly visible sign
arrow. on the diagram. Inclusion populations are
commonly variable that every researcher is free to
choose the values that he considers to be the best,
but he must indicate precisely where they are and
what are the motivations for his choice.
4. Interpretation: a detailed example (Central
Kola Peninsula granulites, Fonarev et al., 1998)
Once the fluid types have been clearly identified
and a small number typically less than about 5.

J.L.R. Touretr Lithos 55 (2001) 125

20

isochores have been selected, then the real, final


discussion can only start. It consist basically to
evaluate the respective importance and source of
each fluid phase present at any moment of the rock
history, as well as the interaction that it may have
had with the rock-forming minerals. Note that a
correct appreciation of this problem will considerably simplify the apparent diversity of inclusions in a
given rock sample, leading to the very wrong assumption that any fluid can be present anywhere.
When, in a recent abstract Johnson et al., 1996., I
read that CO 2-rich inclusions are abundant in greenschist, amphibolite and granulite settings in fact, in
all metamorphic terranes., and that their formation
and preservation of carbonic-rich inclusions is an
inescapable by-product of deformation and post-deformation annealing, I cannot avoid the overall impression that this presentation of facts does not correspond to the reality that I have seen in hundreds of
samples from all parts of the world as follows:
CO 2-rich inclusions may occasionally be found
in rocks from most metamorphic grades, but not
overall, and with major differences between the different metamorphic grades; in lower grades notably
greenschist-facies., almost exclusively along major
shear-zones like, incidentally some great Alpine
structures like the Simplon fault zone, the example
chosen by Johnson et al., 1996., in higher grades
above the beginning of migmatites melting, with a
sudden and marked increase when entering the granulite domain.
Post-metamorphic annealing lead indeed to the
disappearance of most inclusions, with aqueous fluids disappearing more easily than carbonic ones. But,
in general, this is done by selective H 2 O leakage
Bakker and Jansen, 1994., resulting in a CO 2-enrichment from a H 2 OCO 2 mixture. This mechanism, however, which can be documented from the
remaining CO 2 density, is by no means an inescapable way of producing CO 2 inclusions. They will not
be there if no CO 2 had already been present in the
initial fluid.
Rocks showing best evidence of deformation
and post-metamorphic annealing are eclogites. These
are conspicuously poor in CO 2 inclusions, except
when inherited from former granulites Andersen et
al, 1990, 1993. or introduced from outside along
deformation structures and shear zones Fu et al.,
v

submitted.. An illustration of this mechanism is given


in Fig. 6. In this example, it is relatively easy, only
from the mode of occurrence of the different fluid
types, to distinguish between internal fluids W1,
high salinity brines. produced by local fluidmineral
interaction at peak metamorphic conditions, and external fluids W2, low-salinity aqueous and G2,
CO 2-rich fluids. introduced from outside along shear
zones or microfractures. The next step would be of
course to analyze the inclusions to document the
fluidmineral interaction, but this can only be done
at the scale of the single crystal, by laser ablation or
any other kind of spot, punctual analysis. Alternative
techniques, such as crushing and leaching, would
mix different fluid generations and give very questionable results.
Each metamorphic terrane represents a specific
problem, and it is obviously impossible to discuss
here all possible cases in the recent issues of Fluid
Inclusion Research, the invaluable reference basis for
any inclusionist, several 10s of references are dealing
with metamorphic rocks every year.. Some cases are
relatively simple. As for the eclogite example discussed in Fig. 6, the case of the gold-bearing from
Sierra Leone, presented in Fig. 5, is relatively
straightforward, at least for a partial interpretation.
The figure shows a former microfracture, invaded by
a CO 2-rich fluid. The fracture has healed, and the
fact that isolated, high-density islands remain within
a lower density environment indicates that healing
has been accompanied by a decrease in the fluid
density. From any point along the initial isochore,
this density decrease can only occur either by pressure decrease or by temperature increase or by a
combination of both.. Temperature increase is very
unlikely, but not pressure decrease, known to be
almost systematic during the formation of quartz
veins at medium metamorphic grade e.g. the case of
alpine veins, Mullis et al., 1994.. Pressure decrease
must therefore be favored in the present case. It
could even be quantified if the metamorphic temperature of the vein formation could be estimated from
some adequate mineral assemblage, e.g. chlorite or
micas.
Regional problems are as a rule more complicated. Main aspects of the discussion always involve
the two steps that we have identified, namely the
selection of few isochores and their comparison with

J.L.R. Touretr Lithos 55 (2001) 125

PT mineral data. I will illustrate the details of this


discussion on a recent example Granulites from the
Central Kola peninsula, Fonarev et al., 1998., from a
well-investigated region which is probably more
complicated than most metamorphic domains of a
comparable metamorphic grade.
4.1. Regional setting
The Archean metamorphic rocks occurring in the
Central part of the Kola Peninsula, northeastern Baltic
Shield., contain a number of igneous enderbite,
basic granulites. or sedimentary metapelites, banded
iron formation. protoliths, all metamorphosed to
granulite grade. The metamorphic evolution, which
has taken place between about 3 and 2.5 Ga, is
complex, with three major metamorphic events M1,
M2, M3, respectively. clearly identified in the rock
texture and in the field M1: peak regional assemblage, M2 and M3 more local, related to major
shear-zones.. All three stages can be identified in
some samples, and they have been calibrated in
terms of P and T from a consistent system of
geothermometers and barometers T in 8C, P in

21

kbar.: M1: T s 670 " 20, P s 5.1 " 0.5; M2: 565 "
15, 4 " 0.5; M3: 500 " 20, 3.2 " 0.4 Fig. 9.. In the
investigated region, all rocks have been metamorphosed under the same conditions. There are no
significant differences in the PT values recorded
by the mineral assemblages between sheared and
unsheared rocks. Differences are only to be noticed
in the extension of each stage, M2- and M3-mineral
assemblages being more developed in sheared rocks.
All rocks contain a number of fluid types, notably
the familiar granulite fluids high-density CO 2 and
high-salinity brines., as well as less common fluids,
notably N2 especially in BIF. and CH4. The discussion and interpretation of fluid inclusion data will
here be based here exclusively on the CO 2-rich
inclusions, by far the most abundant and typical in
all studied samples.
4.2. Selection of representatie isochores
Fluid inclusions have been studied in nine representative samples, covering all major lithotypes.
These samples have also been chosen because they

Fig. 9. PT interpretation of the Central Kola granulites Fonarev et al., 1998.. Left: first attempt based on a loose CO 2 isochore selection
1 to 7., based on extreme Th values andror isochores passing through a given metamorphic episode. Right: final published. interpretation,
based on a rigorous selection of representative isochores I to V.. Details of isochore identification: see text.. 8 and VI: N2 isochores. M1,
M2, M3: Successive metamorphic episodes. d q or y.: Pressure difference recorded between fluid inclusions and contemporaneous
metamorphic mineral assemblage best estimate: between M2 and V.. Double thin arrow: Metamorphic PT path, heavy line arrow. s fluid
PT path during the metamorphic evolution.

22

J.L.R. Touretr Lithos 55 (2001) 125

show a clear indication of the three metamorphic


stages at the scale of the thin section. They comprise
metapelites sillimanitegarnet biotite plagiogneisses:
15r310.4, 7g, 14r117.4, 15r181.6 or gneiss: 3 h.,
enderbites 4 h, 7 m. and BIF 15r397.6, 4ar328.4..
For the CO 2-rich inclusions, T h results are reported
in Fig. 8 presented along the GSI concept. Each GSI
two to six for a given sample. corresponds to a
horizontal line in the diagram, showing the overall
Th variation range. Most GSIs contain primary or
pseudoprimary inclusions isolated or clustered..
Special attention has been given to inclusions within
or close to good PT mineral indicators, especially
garnets whenever possible, primary inclusions in
garnet or isolated inclusions in quartz inclusions
within garnet..
In principle, each GSI should be represented by a
Th histogram, as done in the Fonarev et al. 1998.
publication. All these partial histograms would have
complicated hopelessly the figure. For the purpose of
the present discussion, the direct representation of all
microthermometric results each symbol in Fig. 8
corresponds to a Th measurement. is sufficient to
illustrate these two major conclusions:
i. The extreme variability of different GSIs. Some
e.g. sample 15r181.6. are extremely well defined,
with Th variations not exceeding about 108C, others
show a variation range of more than 508C. In the
latter case, it is rather obvious that the lowest densities highest T h ., correspond to post-trapping perturbations leakage., as they are completely different
from most other measurements e.g. Sample 7g..
This hypothesis could suggest that, for any GSI,
most representative less perturbed. values are towards the high-density side of the diagram, but as
discussed below the story is certainly far more complicated.
ii. In average, most Th values cluster between
y15 and y258C. They would clearly correspond to
a maximum peak. on a composite histogram. It
would certainly not be a mistake to choose these
values as representative for the whole region. However, the discussion can be considerably elaborated
by taking into account the more precise relationships
between the inclusions and the metamorphic stages,
as well as compositional complexities which may
influence the position of an isochore for a given
homogenisation temperature.

4.3. Fluids related to a gien metamorphic episode


(boxes in Fig. 8): F1 (stage M1) and F2 (stage
M2) fluids
The fact that some sensible PT mineral indicators, notably garnet, can easily be identified at the
scale of the thin section is of considerable help for
the identification of fluids related to a given metamorphic event. In general, most minerals have equilibrated at M1. Inclusions in these minerals are
designed as F1, subdivided in F1a average, most
common values. and F1b for a limited group of
inclusions, exclusively occurring in BIF, which show
significantly lower T h . A closer examination has
shown that these low homogenisation temperatures
result from the fluid composition, namely the occurrence of N2 , up to 35 mole% in some inclusions. For
the definition of the isochore, this compositional
effect has to be considered, and then it can be seen
indeed that the lowest T h , used for the definition of
isochore I, corresponds to a higher molar volume,
therefore is below F1a isochores pure CO 2 . in the
PT space Fig. 9..
F2 relates to inclusions in M2 minerals. Especially important is the subgroup F2a, which corresponds to primary inclusions in M2 garnet see Fig.
9 in Fonarev et al., 1998.. F12 corresponds to
inclusions transitional between M1 and M2. All these
types and subtypes are indicated by the boxes
represented in Fig. 8.
The selection of representative isochores is done
on this diagram arrows in Fig. 8.. Note that the
extreme values, for a pure CO 2 fluid y458C to
q308C., would correspond to isochores covering the
complete field of geological interest. Then, it would
be easy to select an isochore which fits with any
working hypothesis. I must recognize that it is a little
bit what had been done in a first attempt, corresponding to isochores defined by circled arabic numbers
on Fig. 8 1 to 7., drawn on the left diagram of Fig.
9. But two major arguments indicate that some aspects of this random, spontaneous selection were
erroneous, or at least misleading as follows:
There is absolutely no reason to privilege any
isochore exactly passing through the best estimates
of a given metamorphic event 4, 5 and 7..
For the highest densities lowest T h ., the compositional effect must imperatively be taken into
v

J.L.R. Touretr Lithos 55 (2001) 125

account: it makes no sense to consider a mixture


containing up to 35 mole% N2 as equivalent pure
CO 2 .
Therefore, we have chosen for the final published
interpretation the isochores I to V Roman numbers,
Figs. 8 and 9, right., with the following definition: I:
average range for F1 typical M1 fluid., II: lowest
Th , but high N2 content 35 mole%., III: Transitional
F12, IV: Average F2, and V: F2a primary inclusions in M2 garnet.. Isochore VI and 8. corresponds
to a different fluid pure N2 ., therefore it is not
indicated on Fig. 8.
4.4. Interpretation: successie episodes of isobaric
cooling, followed by sudden decompression
A quick look to Fig. 9 right. shows indeed that,
in general, M1-related isochores I to III. are above
higher pressures. M2 isochores IV and V.. This
relative position fits well with the overall characteristics of both metamorphic events: M1 occurs at
higher PT conditions than M2. Pure N2 fluids,
however, isochore VI., even if related to M1, record
much lower pressure than CO 2 fluids. Such a behavior is rather common in N2-rich inclusions: nitrogen
obviously diffuses more easily than CO 2 through any
host mineral.
A closer look, however, reveals a number of
problems. For the reference to a given metamorphic
event, the best-constrained isochore is V, corresponding to primary inclusions in a well-characterized M2 garnet. But this isochore passes significantly below M2, recording at M2 temperature a
fluid pressure lower by at least 1 kb than the metamorphic pressure. Again, this is a rather general
feature, observed in many granulites, or granulite-related metamorphic rocks: when syn-metamorphic inclusions are well identified, the fluid pressure
recorded in inclusions is almost systematically lower
than metamorphic pressure, typically by about 12
kb e.g. Touret and Huizenga, 1999.. The classical
explanation is selective water leakage. Almost all
granulites contain some hydrous phases, stable at
peak metamorphic conditions, which impose a finite
H 2 O pressure in the metamorphic fluid. In the case
of the Kola granulites, it can be estimated that the
quantity of H 2 O in the synmetamorphic fluid should

23

be at least 10% molar for M1, significantly more at


the lower temperature M2 stage. This water is no
longer present in the inclusions, and indeed the
easiest explanation is that it has disappeared by
selective leakage, as indicated by a number of experimental studies Bakker and Jansen, 1994.. The same
explanation may be given for isochore II, also well
below its metamorphic condition M1.. But, then,
isochore I, corresponding to the average fluid for
M1, passes above M1 box, by about 0.5 kb for the
M1 reference temperature of 6708C. Moreover, there
is absolutely no reason to believe that water leakage,
evidenced for M2 on the basis of F2a inclusions, has
also not taken place during M1. This would displace
the real position of isochore I towards higher pressures, at least to 23 kb above peak metamorphic
pressure for M1.
The only way to cope with this situation is to
invoke a period of isobaric cooling after M1, during
which either new inclusions are formed at corresponding PT values, or former inclusions are reset
towards higher densities. This type of evolution has
been well documented in various low-to-intermediate
pressure granulites from Southern India Nilgiri
granulites, Touret and Hansteen, 1988; Srikkantappa
et al., 1992., Finland West Uusimaa Complex,
Touret and Hartel, 1990. as well as in migmatites
van den Kerkhof and Olsen, 1990.. Note that density resetting, if any, imposes a departure from the
constant-volume principle: in order to increase the
density, the volume has to become smaller without
fluid leakage. This supposes that some external
source of energy provided by deformation?. must be
available.
In any case, M1 and post-M1 isochores are far
with the high-pressure field, but F2 fluids needs to
be close to M2 conditions. This can only be achieved
by a sudden decompression, which may incidentally
explain the strong leakage observed in some inclusions of F1 GSIs wide range of T h towards relatively high temperatures, e.g. sample 15r397.6 in
Fig. 8.
The fact that isochore IV average M2 isochore,
in principle, somewhat later than the truly primary
isochore. is above V, suggests that the same type of
evolution may have occurred after M2. These considerations explain the PT path which has been
indicated on Fig. 9. Note that isochore IV passes

24

J.L.R. Touretr Lithos 55 (2001) 125

through M3, but this intersection is purely coincidental, without any geological meaning.

5. Conclusion
Many aspects of fluid research are now at the
center of geological interest: models of fluid flow
through rocks, chemical studies of fluidrrock interaction processes, fluid signatures indicated by stable
isotopes, etc. In this panoply of scientific techniques,
the study of fluid inclusions should occupy a recognized place. A remarkable collective effort during
the past decades has provided us with all indispensable tools. Much work has been done to improve the
technology or theoretical knowledge of fluid systems
in most common geological conditions. In principle,
inclusions can now be studied in any rock type,
notably in metamorphic rocks where fluids play such
an important role. Still, the number of well-studied
occurrences remain rather limited. We must know
enter in a phase of systematization, during which a
number of further unexpected discoveries will certainly be done. It must always be remembered, however, that the best analytical tool, the most elaborate
theoretical interpretation will only give poor results
if applied on a bad inclusion. For the study of these
small objects, observation is essential, with the good
old microscope, to-day like a century ago, remaining
the most important instruments. In few years time,
we can still predict decisive technological advances,
notably for the complete analysis of the fluid inclusion content notably by LAS-ICP-MS.. But progress
in analytical capacities results always in more time
and money spent on the analyzed object, resulting in
the present case to the decrease of the number of
inclusions which will be possibly investigated. This
will only make more important the necessity to have
a rational selection of analyzed inclusions, according
to the principles that I have attempted to present in
this paper.

Acknowledgements
The work done in Amsterdam would not have
been possible without the support of the Vrije Universiteit and NWO ALW., the Dutch organization

for the development of scientific research. But an


essential part is due to the exceptional quality of the
technical and supporting staff, W. Koot et al. for the
preparation of the Fluid plates, E.A.J. Burke, W.
Lustenhouwer and S. Kars for the Lab. Microanalyze
microthermometry, Raman and Electron probes,
SEM.. Our way of studying inclusions in metamorphic and magmatic. rocks has slowly developed
through the work of all the researchers who have
been at the VU, mostly for the preparation of their
PhD thesis. Just to mention some names: A.M. van
den Kerkhof, T. Hansteen, M. Ploegsma, E.J. Zwart,
Ph. Muchez, J.M. Huizenga, M. Moree, L. BolderSchrijver, Bin Fu, and many others. T. Andersen and
M.L. Frezzotti are members a` part entiere
` of this
group, and I thank them for having forced me to put
on paper some aspects of our collective experience,
despite the pressure of present-day academic life.

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