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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,
)
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
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
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-
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.
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
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
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.
10
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.
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
12
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.
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..
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..
15
16
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
17
18
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.
20
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
23
24
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
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