Journal of Volcanology and Geothermal Research 173 (2008) 217–229

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Journal of Volcanology and Geothermal Research

j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / j vo l g e o r e s

Chemical transport in geothermal systems in Iceland

Evidence from hydrothermal alteration
Hjalti Franzson a,⁎, Robert Zierenberg b, Peter Schiffman b
a
Iceland GeoSurvey, 9 Grensásvegur, 108 Reykjavík, Iceland
b
Department of Geology, University of California, Davis, One Shields Avenue, 95616, CA, USA

a r t i c l e i n f o a b s t r a c t

Article history: This study focuses on the chemical changes in basaltic rocks in fossil low- and high-temperature
Received 1 July 2007 hydrothermal systems in Iceland. The method used takes into account the amount of dilution caused by
Accepted 28 January 2008 vesicle and vein fillings in the rocks. The amount of dilution allows a calculation of the primary concentration
Available online 4 March 2008
of the immobile element Zr, and by multiplying the composition of the altered rock by the ratio of Zr
(protolith)/Zr (altered rock) one can compute the mass addition caused by the dilution of the void fillings, and
Keywords:
also make a direct comparison with the likely protoliths from the same areas. The samples were divided into
Iceland
three groups; two from Tertiary fossil high-temperature systems (Hafnarfjall, Geitafell), and the third group
basalt
geothermal systems from a low temperature, zeolite-altered plateau basalt succession. The results show that hydrothermally
hydrothermal alteration altered rocks are enriched in Si, Al, Fe, Mg and Mn, and that Na, K and Ca are mobile but show either depletion
chemical transport or enrichment. The elements that are immobile include Zr, Y, Nb and probably Ti. The two high-temperature
isocon method systems show quite similar chemical alteration trends, an observation which may apply to Icelandic fresh
water high-temperature systems in general. The geochemical data show that the major changes in the altered
rocks from Icelandic geothermal systems may be attributed to addition of elements during deposition of pore-
filling alteration minerals. A comparison with seawater-dominated basalt-hosted hydrothermal systems
shows much greater mass flux within the seawater systems, even though both systems have similar alteration
assemblages. The secondary mineral assemblages seem to be controlled predominantly by the thermal
stability of the alteration phases and secondarily by the composition of the hydrothermal fluids.
© 2008 Elsevier B.V. All rights reserved.

1. Introduction
The location of Iceland as a subaerial part of the Mid-Atlantic Ridge,
with a wealth of geothermal activity, makes it a unique area for the
study of water–rock interaction. Temperatures of fluid–rock interac-
tion range from about 2 to 3 °C in the groundwater systems to probable
supercritical values in the high-temperature geothermal areas (Elders
and Fridleifsson, 2005). The rocks that host the geothermal reservoirs
are of igneous origin, with basaltic compositions constituting about
90% of the volume with the remainder having more evolved com-
positions. The abundant geothermal resources are economically im-
portant and widely utilized, and have consequently been extensively
studied from geochemical, structural, geophysical and geological
points of view (e.g., Arnorsson et al., 1983; Bodvarsson, 1983; Marty
et al., 1991; Schiffman and Fridleifsson, 1991; Lonker et al., 1993; Riedel
et al., 2001). The geothermal resources range from low-temperature
systems, in which shallow groundwater has gained heat in response to
the prevalent regional geothermal gradient, to high-temperature
⁎ Corresponding author. Tel.: +354 528 1500; fax: +354 528 1699.
E-mail addresses: hf@isor.is (H. Franzson).
systems in which the high thermal gradient is due to shallow crustal
magmatic activity. The latter type is mostly confined to active volcanic
centres. However, fossil high temperature geothermal systems are
exposed by erosion allowing three dimensional access to the subsur-
face portions of the hydrothermal systems (e.g. Fridleifsson, 1983,
1984). The majority of the hydrothermal systems in Iceland have
waters derived from local meteoric water, although seawater-domi-
nated hydrothermal fluids occur in some near coastal geothermal
systems (Sveinbjornsdottir et al., 1986). The general similarity of both
source fluids and host rocks throughout much of Iceland allows
comparison among hydrothermal systems.
Rock properties play an important role in the petrophysical para-
meters of the individual systems and an increasing emphasis has been
placed on the study of reservoir characteristics. During the last
13 years, Orkustofnun (the National Energy Authority of Iceland), with
the financial support of Orkuveita Reykjavíkur (Reykjavik Energy), has
worked on a project with the main aim of defining the reservoir
characteristics of the rocks in the geothermal systems in Iceland.
While active geothermal systems have the advantage of allowing
direct comparison of rock alteration to fluid composition, this com-
parison only relates to a single stage, i.e., the present, in the evolution
of the system. In contrast, sampling of fossil geothermal fields allows

0377-0273/$ – see front matter © 2008 Elsevier B.V. All rights reserved.
doi:10.1016/j.jvolgeores.2008.01.027
218 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229
examination of the time integrated history of rock alteration, in-
cluding determination of the temporal evolution of mineralogy and
porosity.
The sampling strategy utilized in this study emphasized variably
eroded fossil geothermal systems, focussing on areas that had been
previously mapped with respect to their geological structures and
hydrothermal alteration. The assumption is that rocks in these fossil
systems are close analogues of those in presently-active geothermal
reservoirs. Approximately 500 samples were collected for these stu-
dies, a large proportion of which have been analyzed for total and
effective porosity, permeability, chemical composition, and petro-
graphic characteristics. This extensive data set has been especially
useful in determining the interrelationship between porosity and
permeability of Icelandic rocks (e.g., Sigurdsson and Stefansson, 1994;
Sigurdsson et al., 2000; Stefansson et al., 1997), and the relationship of
these physical properties to the degree of hydrothermal alteration
(e.g., Gudmundsson et al., 1995; Franzson et al., 1997, 2000; Franzson,
1999).
The main emphasis of this paper is to elucidate the nature of
chemical transport in Icelandic geothermal systems by correlating the
bulk composition of rock samples with their petrographical char-
acteristics. Using the petrographically determined percentage infilling
in the rocks, we will show that it is possible to assess the amount of
chemical dilution that has taken place. This allows the deduction of
the primary concentration of the immobile elements in the altered
rocks, and by correlating these with the relatively fresh volcanic rocks
equivalents, we assess the chemical change that has taken place
during the hydrothermal alteration. Furthermore, using the “isocon”
method (Grant, 1986) for determining mass transport, we also eval-
uate the chemical enrichment-immobility-depletion of various che-
mical components within individual samples.
2. Geological setting
This study is based on data from approximately 130 basaltic rock
samples and focuses on three locations (Fig. 1) as described below:
a) The Hvalfjordur basalt succession consists of ca. 4–3 myr old plateau
basalts which have been subjected only to zeolitic alteration
(chabazite–thomsonite to mesolite–scolecite, e.g., as described
from Eastern Iceland by Neuhoff et al., 1999). The Hvalfjordur area
Fig. 1. A simplified geological map of Iceland showing the Tertiary, Plio-Pleistocene and the volcanic zones. The areas sampled for the petrophysical study are dark shaded, and the
locations focussed on in this study (Hafnarfjall, Hvalfjordur and Geitafell) are also marked.
has been mapped in considerable detail and the rocks are well
characterized chemically (Franzson, 1979). Twenty two samples of
basaltic lava flows were taken from this area.
b) Hafnarfjall central volcano is a 5.5–4 myr old, deeply eroded cen-
tral volcano that has been mapped with respect to its structure,
geochemical evolution, and locally, its hydrothermal alteration
(Franzson, 1979). The volcanic products range from basalts to
rhyolites which have been subjected to variable degrees of hydro-
thermal alteration. Forty five samples are included in this study,
and off these twenty seven are lava flows, five very scoraceous or
tuffaceous tops of lava flows and twenty intrusions (mostly fine
grained dykes or sills).
c) Geitafell central volcano was formed about 6 myr ago, is deeply
eroded, and has been mapped in detail, both with respect to vol-
canic evolution and hydrothermal history (Fridleifsson, 1983). An
investigation has also been completed on the geochemical
evolution of the volcano (Thorlacius, 1991). Fifty five basalt sam-
ples are included in the study, where thirty are lavas, five very
tuffaceous or scoraceous lava tops and twenty intrusions (mostly
fine grained dykes or sills).
The three study areas are all Tertiary in age, and differ from younger
volcanic successions that host active geothermal systems principally
by their lack of hyaloclastite formations, which occur almost exclu-
sively in formations younger than the onset of glaciation at 3.3 myr (c.f.
Fig. 1). These older hydrothermal systems were subjected to an initial
phase of low-temperature alteration, followed by the main phase of
high-temperature alteration, and subsequently overprinted by low-
temperature alteration formed during the demise of the central
volcanic complex and succeeding erosion. It has been demonstrated by
extensive petrographic observations that mineral deposition during
the high temperature alteration regime in Icelandic hydrothermal
systems generally reduces rock permeability and the last low-tem-
perature alteration episode does not greatly affect the bulk rock com-
position. Petrography can provide important constraints on the
relative timing of alteration events. For example, minor late-stage
zeolite deposition, present in some of our samples, has been tenta-
tively interpreted as due to deposition from fluids trapped in relatively
impermeable rock. In general calcite does not occur within the
epidote–amphibole zone in presently-active high-temperature sys-
tems where temperatures exceed 290 °C. However, in the fossil
 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229 219

Fig. 2. The alteration zones used in Iceland, their dependence on temperature and the main alteration features of the primary basaltic rock components.

systems, calcite is occasionally superimposed on epidote–actinolite
zone mineral assemblages, implying carbonate deposition either
during cooling of the high-temperature system by inflow of colder
fluids or during the succeeding low-temperature episode. Hence,
changes in the chemical composition of rocks relative to their fresh
counterparts are believed to have occurred up to the highest tempe-
rature stage of alteration that the rock has undergone, with possible
effects due to precipitation of late-stage calcite.
The samples are all either volcanic rocks which have been gra-
dually buried by accumulation of younger volcanics, or intrusive rocks.
The age of the accumulated sequence is progressively older and more
altered as it is more deeply buried. However, the same cannot be
inferred about the intrusive rocks, as their minimum age is generally
unconstrained. This may be of importance when considering the
timing of alteration, especially within the most intense alteration
zones, as intrusions may occur during any stage of the alteration.
Rocks intruded at a later stage of alteration may only show a minor
alteration effect compared to those intruded earlier, even though they
were subjected to similar temperatures and pressures. Therefore,
contrasts in the degree of alteration within intrusive rocks and their
surrounding extrusive host rocks should be expected and may depend
on factors other than differences in permeability and porosity.
3. Petrographic data
The rock samples are all of basaltic composition, ranging from
olivine tholeiite to quartz normative tholeiite. They would dominantly
be holocrystalline, but with some glass fraction in the most scoracious
part of the lavas. The main primary components in basalts are relatively
Ca-rich plagioclase, clino-pyroxene (augite) and opaques (magnetite–
ilmenite), and with subordinate amount of olivine, especially in the
more primitive basalts. Hydrothermal alteration is essentially made up
of two components: (a) replacement of primary components in the
rocks by alteration minerals, and (b) precipitation of alteration mi-
nerals into voids in the rock. Hydrothermal alteration in active
Icelandic geothermal systems is systematically zoned with respect to
temperature (Fig. 2). The top zone, which contains relatively fresh
rocks, includes a sequence that does not show any indication of

Fig. 3. Range in primary porosity in Icelandic rocks deduced from petrographic study of the rock samples (n = 127).
220 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229

Fig. 4. The relation between degree of infilling and the total percentage of alteration minerals (i.e., % alteration minerals divided by the total mode) of a sample. Samples are grouped
according to their alteration zone (from Franzson et al., 2000).

geothermal interaction and may at the most show minor oxidation due
to groundwater circulation. The temperature dependency, as seen in
Fig. 2, affects both the sequence of alteration minerals that fill voids, as
well as the ones that replace primary minerals. Thus olivine and glass
are completely altered near the upper boundary of the mixed layer clay
zone. Plagioclase and opaques are more resistant to alteration and may
be only partially altered to the minerals shown on Fig. 2, especially
when taking into account that some of the rock samples are low
porosity intrusions. Pyroxene shows in general similar resistance to
alteration as plagioclase. It is mainly seen altering into clays and then
actinolite at deeper levels.
Petrographic examination of the rock samples collected for this
study used point counting (200 points) to quantify primary porosity,
i.e. the original open space in rock prior to alteration (dominantly
vesicles and minor fractures), and to assess how much of that porosity
had been filled by deposition of alteration minerals. Two hundred
points were counted on each rock thin section. Fig. 3 shows the
distribution of primary porosity in Icelandic rocks, where porosity
ranges from zero up to about 70%. As alteration proceeds void space in
the rock is progressively filled with alteration minerals. Fig. 4 shows
the relationship between the degree of pore filling and the extent of
alteration, defined as the percentage of alteration minerals relative to
primary minerals. Rocks with a primary porosity, as petrographically
determined, below approximately 15% have variable degrees of
infilling (Fig. 5). In contrast, rocks that initially exceeded the 15%
primary porosity threshold tend to show near complete filling of the
primary pore-space. This implies a non-linear relationship between
permeability and porosity in the Icelandic basaltic samples.

Fig. 5. The “rate” of deposition of alteration minerals into vesicle filling in relation to alteration zones and primary rock porosity. Note that there is apparently more rapid (i.e.,
efficient) deposition in rocks with N 15% primary porosity, as determined petrographically (from Franzson et al., 2000).
 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229
4. Chemical data
The chemical analyses were made by two commercial chemical
laboratories, The Caleb Brett Laboratory in England and McGill
University in Canada. Both used standardized XRF techniques. Values
for samples analyzed by both laboratories are generally within
analytical error. The samples were analyzed for major, minor, and
several trace elements. Loss on ignition (LOI) was measured in all the
samples, and in some samples, CO2 and Stotal were specifically ana-
lyzed. The trace elements analyzed included Zr, Y, Zn, Cu, Rb, Sr, Nb,
Ga, Ce, V, Pb, U, Th and As. All the analyses presented here have been
recalculated to 100%, without LOI, to allow direct comparison with
unaltered protoliths. The compositional range of relatively unaltered
rocks has been acquired from other sources for comparison with the
data on altered rocks presented here. Analyses describing the evolu-
tion trend within the Hafnarfjall central volcano and the Hvalfjordur
plateau basalt succession are from Franzson (1979), and analyses from
the Geitafell central volcano are from Thorlacius (1991). Chemical
analysis from the Krafla central volcano (Karl Gronvold, unpublished
data) and the Reykjanes–Langjokull volcanic zone (Sveinn Jakobsson,
unpublished data, 1999) have been used as reference samples for
comparison with the altered samples where relatively unaltered sam-
ples are unavailable from the respective areas.
Loss on ignition values range from zero up to about 13%. Fig. 6
shows the relationship between the % of remaining primary rock
component (i.e. = 100-(rock alteration + void filling)) in basaltic lava
flows and LOI, where the samples have been grouped into alteration
zones. The figure clearly shows a strong correlation between LOI and
the extent of alteration in these samples. It also shows an inverse
correlation between the percentage of primary component and the
minimum LOI for samples as a function of alteration grade. Smectite–
zeolite grade samples with LOI b 1% have a much higher percentage
(N80%) of primary components than epidote–amphibolite samples
with similar LOI values. This is probably due to more abundant of
alteration minerals with low-water contents in the higher grade
samples. LOI consists mainly of H2O+ and CO2. The latter was measured
separately in only part of the sample group. The results show that CO2
is typically b1% in samples with less than 60% alteration intensity with
higher CO2 values (b6.5%) only present where alteration is more
intense. A good correlation is between CO2 and calcite in the samples.
5. Methodology for calculating mass transfer
The methodology used in this study is based upon the petrographic
characteristics of Icelandic basalts altered in geothermal systems.
Fig. 6. Loss on ignition (LOI) plotted against the % primary rock component (i.e., 100-rock
alteration and void filling). Also shown are the best fit lines belonging to each of the
alteration groups.
221
Fig. 7. A sketch showing a simplified model for the dilution of a chemical rock com-
ponent with the introduction of vesicle filling. The Y-component in the rock is
symbolised in black and becomes relatively reduced when vesicle fillings are added to
the sample.
Specifically, the methodology arises from the key observation that
much of the alteration process entails the filling of primary pores by
secondary minerals, effectively diluting the chemical composition of
the protolith by mass addition (Fig. 7). This mass addition will dilute
most of the components in the original rock and thus whole rock
analyses will show lower concentrations of immobile elements even
though there has been no mass flux of these elements. The extent of
dilution is known through point-counting as discussed above. By
identifying components in the rock that have remained immobile
during alteration and taking into account this dilution effect, the
primary composition of the immobile element in the sample may be
calculated.
One way of assessing the effect of chemical dilution on the rock
composition is to plot the elemental concentration against the rock
dilution (Fig. 8). In this diagram the concentration from z to x
represents the concentration range measured for element A in
unaltered basalt. The tie lines from 100% dilution (point R) to points
z and x represent the amount of dilution of z and x, respectively,
assuming that the dilutant mineral (or minerals) contains no chemical
component A. If element A is immobile and has y concentration in the
sample, the dilution will cause the apparent decrease of that com-
ponent along the line towards R. One may therefore expect that all
immobile elements within the basalt range will, with increasing
dilution, be contained within the field labelled “a”. A mobile element
Fig. 8. Diagram showing effect of dilution on the concentration of hypothetical chemical
component A during alteration of basaltic rocks. Fields labelled “a”, “b”, and “c”:
represent, respectively, the range of diluted compositions following no mass transfer,
addition of component A, and loss of component A. See text for more details.
222 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229
Fig. 9. A plot showing the relation between SiO2% and % mineral deposition (dilution)
deduced from petrography for samples grouped into alteration zones. The lines
demarcate the basalt compositional field (c.f. lines z–R–x in Fig. 8). Deviation of the
samples outside the basalt field indicates apparent SiO2 enrichment.
may not follow the same trend. If vesicle fillings contain the mobile
element, which has been derived from outside the sample, the diluted
compositions will shift to the right of the line y–R (e.g., field b). If, on
the other hand, a chemical component is being removed from the
rock, the dilution will move compositions to the left of line y–R, and
these samples will group within the field indicated by c. Samples for
which the extent of addition or depletion of an element is small
relative to the variation of that element in the unaltered protolith may
not be distinguishable by this method. However, rocks that have
undergone significant mass flux should be readily identified.
In Fig. 9, the SiO2 concentrations of many of the altered samples
plot to the right of the primary basaltic compositional field, indicating
a strong SiO2 enrichment. This enrichment is seen in samples from all
of the alteration zones. Fig. 10 on the other hand, generally shows
indications of K2O depletion during hydrothermal alteration and dilu-
tion. Zircon is an example of an immobile element (Fig. 11), where a
majority of the samples are confined within the field of primary
basaltic composition. Some samples plotting to the right of the pri-
mary basalt compositional field have basaltic andesite compositions
and are retained for our purposes as they help define the fractionation
trend of the sample group. Fig. 11 shows (a) the strict confinement of
the samples within the basalt compositional range, as previously
mentioned, and (b) that most samples plot in the left side of the
basaltic field, in accordance with the observation that the majority of
Fig. 10. A plot showing the relation between K2O % and % mineral deposition. Lines
demarcate the basalt field (c.f. Fig. 8). Note that samples more commonly plot to the left
of the basalt field, indicating apparent depletion.
Fig. 11. A plot showing the relation between Zr and % mineral deposition. Most of the
samples fall within the basalt field, as defined by the lines, which indicates that the
element has remained relatively immobile.
the samples are normal basalts and that more evolved basaltic com-
positions with higher Zr contents are less abundant. These deductions
further imply that dilution must play the largest role in modifying the
chemical composition of basaltic rocks within the alteration zones
studied here. It is interesting that there are no apparent progressive
gradients in chemical transport discernable between samples in the
smectite–zeolite to the epidote–amphibole zones, which may indicate
that such changes, if present, are small compared to the chemical
dilution effect.
An important indication of the immobile elements is that their
ratios will remain constant by definition during dilution and depletion
of other chemical components (e.g. Barrett and MacLean, 1994; Leitch
and Lentz, 1994). Fig. 12 shows the Zr/Y ratios of the basalt samples
from successive alteration zones compared with values from the least
altered rocks analyzed from the Hvalfjordur and Reykjanes–Langjokull
volcanic zones (Sveinn Jakobsson unpublished data, and Karl Gronvold
unpublished data) and the Geitafell (Thorlacius, 1991) and Hafnarfjall
(Franzson, 1979) central volcanoes. The figure shows that the Zr/Y
ratios in altered rocks have a similar range to those in their fresh
counterparts and further confirms Y as also an immobile element in
these systems.
If an element is immobile, its original concentration prior to dilu-
tion can be found by extrapolating along the dilution line to the
original concentration of the element at 0% dilution, as shown along
Fig. 12. The Zr/Y ratios in the rock sample and a comparison with fresh volcanic rocks
(vertical bars) from Reykjanes–Langjokull volcanic zone (Sveinn Jakobsson, unpub-
lished data, 1999) and the least altered samples from the Hvalfjordur basalt, Hafnarfjall
and Geitafell central volcanoes (Franzson, 1979; Thorlacius, 1991). See text for further
explanation.
 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229 223

line R to y in Fig. 8. Barrett and MacLean (1994) suggested that by
comparing the concentration of immobile elements prior to and after
hydrothermal alteration the mass changes that have taken place
during the hydrothermal alteration event can be calculated. The
calculation of mass change “removes the misleading effects of closure
(constant sum of 100%) on the relations between elements in un-
treated samples” (Barrett and MacLean, 1994). After determining the
primary concentration of a given immobile element (in this case Zr) by
the method described above, we can then calculate the reconstructed
composition for each rock component by multiplying the original
value by a factor equal to the concentration of Zr in the precursor
divided by the concentration of Zr in the altered sample. In this way,
we have now resurrected the “volume” of each chemical component
to what it was in the primary rock. If dilution represented the only
change in rock composition, then all elements other than those con-
tained in the pore-filling precipitates would reveal their original
values by the correction and would plot on the one-to-one line when
compared to an unaltered protolith. This allows us to test the hypo-
thesis that mass dilution during pore filling is the dominant chemical
change affecting the altered rocks. It is of course not always possible to
determine the composition of the unaltered protolith. However, since
Zr can be shown to be essentially immobile in these rocks, we can
bracket the potential compositional variations in primary composition
if we can determine the fractionation relationship between Zr and the
element of interest in unaltered rocks. By plotting the corrected Zr
concentration against another component and comparing it with the
fractionation trend of the respective volcano one can assess whether
enrichment, depletion or no apparent change has occurred during
alteration. The extensive data available on the composition of fresh
basaltic rocks from Iceland provides constraints on the fractionation
trends with respect to Zr. The limited range of fractionation, from the
spread of Zr concentrations in unaltered basalts, provides constraints
on the possible original variations in other elements and allows us to
recognize significant mass flux.
For this exercise, the samples have been subdivided into 3 groups as
described above, i.e. the Hafnarfjall and the Geitafell central volcanoes
and the Hvalfjordur plateau basalt succession. Although Icelandic vol-
canoes follow, in general, a “Thingmuli” tholeiitic evolutionary trend

Fig. 13. Chemical components plotted against Zr. Xs are least altered rocks from Hafnarfjall and Geitafell central volcanoes (Franzson, 1979; Thorlacius, 1991). Diamonds are rocks of
0–33% intensity alteration, squares are rocks of 33–66% alteration and triangles are rocks of 66–100% alteration. The line delineates the primary compositional field of the respective
volcanoes.
224 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229
Fig. 13 (continued ).
(Carmichael, 1964), individual centers may show small deviations from
that trend. Grouping the altered samples according to their petrogen-
esis allows more direct comparison to their primary counterparts and
results in a better resolution of compositional changes that have taken
place during the hydrothermal alteration. An additional advantage is
that this allows a comparison of enrichment/depletion between differ-
ent geothermal environments, and gives a scope for speculation of
heterogeneity in chemical alteration trends in Icelandic geothermal
systems.
For plotting purposes, the samples have been divided into three
groups based on their extent of alteration (Fig. 4) at 0–33%, 33–66%
and 66–100% alteration (vesicle filling + rock alteration), in order to
show gradual chemical changes, if any, from less to more altered
samples. Figs. 13 and 14 are examples of some of the chemical plots
where the relation between individual components is shown against
Zr concentration. Relatively unaltered rocks from the same area are
also plotted on these diagrams to indicate the compositional range of
the protoliths of the altered rocks. The overall results are summarized
in Table 1. It must be emphasized that the results depict the integrated
chemical changes that have taken place during the history of the
hydrothermal areas. In particular, the central volcanoes have probably
undergone several geothermal episodes throughout their lifetime,
which may exceed 1 myr. The Hvalfjordur basalt succession, on the
other hand, has only been subjected to low-temperature burial
alteration with the regional temperature gradient resulting in
temperatures ranging from about 30–100 °C, and is apparently devoid
of major geothermal anomalies.
The results from the central volcanoes can be divided into four
main categories:
(a) TiO2, Ce, Nb, Y and Zr show clear indications of being immobile
as they fall very near the fractionation line of the least altered
samples.
(b) The elements that most consistently show signs of enrichment
are SiO2, Al2O3, FeO, and to a lesser extent, MnO, MgO, Na2O,
CaO and possibly Cu.
(c) K2O and Sr are enriched in some samples, but are depleted in
others.
(d) Other elements do not show a clear trend. However, a lack of
comparison with fresh rock equivalents prevents an assessment
of elements such as Th, U, Pb, As, S, and partly Rb.
The hydrothermal chemical changes between the two central
volcanoes are similar. The chemical changes observed in the
Hvalfjordur plateau basalts are much more subtle, as expected, due
 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229 225

Fig. 14. Chemical components plotted against Zr. + are fresh rocks from the Reykjanes–Langjokull volcanic zone (Sveinn Jakobsson, unpublished data, 1999), x are least altered basalt
lavas from Hvalfjordur lava succession, squares are lavas from Krafla central volcano (Karl Gronvold, unpublished data), and triangles are the rock samples of this study.

to its lower geothermal gradient. These do, however, indicate SiO2,
and K2O enrichment and subtle enrichments in Al2O3, FeO, MgO, Na2O
and possibly Sr. Comparison with some of the trace elements is
difficult due to lack of data from fresh rock equivalents.
6. Isocon plots
The data presented above allows us to evaluate the general beha-
viour of individual chemical components within a group of samples for
an entire hydrothermal field. The method also allows easy comparison
between the magnitude of compositional variation related to igneous
fractionation trends relative to those that can be attributed to hydro-
thermal alteration. The isocon method of determining mass flux has
the disadvantage of requiring sample by sample comparison to specific
precursor rock compositions. A distinct advantage of the isocon
method is that it allows direct evaluation of the mass flux of elements
in a specific sample, allowing easier recognition of coupled geochem-
ical behaviour between elements (e.g., K and Na). Our approach in
using the isocon plots was to first correct the altered rock geochemical
data for the known effects of dilution and to plot these extrapolated
values against appropriate precursor compositions to identify mass
flux variations that are not due to simple rock dilution by alteration
minerals.
The isocon diagrams (Fig. 15) compare the relationship between the
various components within four representative samples, two chosen
from each of the central volcanos. Two of the samples have a primary
226 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229

Table 1
Chemical changes in samples subjected to hydrothermal alteration from the Hvalfjordur basalt succession and Hafnarfjall and Geitafell central volcanoes

Chemical Hvalfjordur Hafnarfjall Geitafell

component
Depletion Unchanged Enrichment Depletion Unchanged Enrichment Depletion Unchanged Enrichment
SiO2 X x x
TiO2 X (x) (x)
Al2O3 (x) (x) (x) x x
FeO(tot) X (x) x x
MnO X x (x) (x)
MgO X (x) x (x) x x
CaO X (x) (x) x x (x) x x
Na2O X X (x) x x x x
K2O X (x) x (x) (x) x (x)
P2O5 X (x) x x
Ce X x x
Cu (x) x x (x)
V X ? ?
Zn x x x
Ga X ? ?
Nb X x x
Pb ? ? ?
Rb X ? ? ? (x)? (x)? (x)?
Sr (x) (x) x (x)? ?
Th ? ? x? ? ?
U ? ? ?
Y X x x
Zr X x x
As ? ?
S ? ? ?

x-affirmative, (x)-probable, (x)?-possible, ?-uncertain.

Zr content of about 150 ppm (H-99, G-62), while the others have about
300 ppm (H-54, G-28) representing relatively primitive and evolved
basalt compositions, respectively. The error bars attached to each of
the components represent the range of primary compositional values
expected at each Zr concentration value within the individual volcano
(Fig. 13). Although error limits on the recalculated compositions are
difficult to quantify, one may expect that the error would increase with
increasing dilution. This is easily observed in Fig. 8 where a small error
in petrographic estimation at high dilution could divert the extrapola-
tion line considerably down towards the base line. If the samples have
all been properly corrected with respect to mass addition, then the
median line should represent the line of no chemical change. Indeed,
the immobile elements (Ce, Zr, Y, Nb) tend to lie on this line. An
exception is Y in the Hafnarfjall samples, which may possibly be due to
a systematic analytical error in the primary trend in the volcano, as
deduced from the Zr/Y plot (Fig. 13). In contrast, Fig. 15 indicates a
tendency for slight Al2O3 and FeO enrichment in the altered samples,
as is also clearly indicated in Fig. 13. MgO can be either enriched or
depleted, as are Na2O and K2O. One might expect that Na2O and K2O
would generally show similar geochemical behaviour and Fig. 15
confirms that the alkalis are either both depleted or both enriched in
any given sample. Na2O and K2O are rather easily leached from rocks
during hydrothermal alteration and many rocks are in fact depleted in
them. One reason for enrichment may be due to remobilization from
nearby more felsic volcanic and intrusive rocks. This hypothesis could
be tested by looking at field relations of the altered basalt samples that
show alkali enrichment. The isocon plots generally confirm the
conclusions that have been attained through plots shown in Figs. 9–
14 and support the proposition that changes in chemical composition
of the altered rocks is mainly due to addition of mass to the rock by
deposition of alteration minerals in primary pores.
7. Discussion
Geothermal systems in Iceland have a number of common features.
The rocks are dominantly of basaltic composition, with minor
amounts of rocks having more evolved compositions within central
volcanic complexes. Most of the hydrothermal waters have low
salinity with chloride b200 ppm (Arnorsson and Andresdottir, 1995),
consistent with heating of local groundwaters. Exceptions are the
high-temperature systems on the Reykjanes Peninsula which show
salinity approaching that of seawater (Sveinbjornsdottir et al., 1986).
Fluid inclusion studies indicate, however, that much of the alteration
in the Reykjanes systems may have occurred during an initial
freshwater stage during the last glacial period (e.g., Franzson et al.,
2002). Studies on the alteration zones in several fields show quite
similar distributions of alteration minerals (Fig. 2). There also seems, in
general, to be a close correlation between alteration zones and the
progressive breakdown of the primary rock and the alteration
products formed. The alteration is, to a large extent dependent on
temperature, and the maximum temperature at any depth in the
explored systems is constrained by the boiling curve. The common
occurrence of hyaloclastites in the presently-active systems is not
shared by the fossil hydrothermal systems developed in Tertiary rocks,
which are dominantly in holocrystalline volcanic rocks erupted in the
absence of a glacial icecap. Volcanic glass is very readily altered during
geothermal activity, and this will increase the availability of chemical
components (e.g., SiO2) into thermal fluids. Therefore the chemical
flux in the presently-active geothermal systems may be higher than it
was for the Tertiary systems.
It must be emphasized that this study describes the overall changes
that have taken place during the whole lifetime of the hydrothermal
systems. Mineralogical studies of vesicle and vein fillings at Geitafell
central volcano show distinct episodes of alteration (Fridleifsson, 1983,
1984). The same pattern of chronologically distinct hydrothermal epi-
sodes has been recognized in many of the explored active high-tem-
perature systems (e.g., Lonker et al., 1993). The number of mineral
species in individual vesicles and veins in the high-temperature sys-
tems at Reykjanes, Nesjavellir, Olkelduhals and Svartsengi (Franzson,
1983, 2000; Franzson et al., 2002), based on about 2000 observations,
is very similar. About 70% show two void-filling minerals, about 25%
contain three and about 5% show four or more void-filling minerals.
The proportion of mono-mineralic veins and vesicles has not been
checked specifically. It is interesting to note that many minerals seem
 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229
Fig. 15. Isocon plots for four samples from Hafnarfjall (H-54, H-94) and Geitafell (G-28, G-62) central volcanoes. The samples were selected with about 150 and 300 ppm Zr, and from
the 66–100% alteration group and moderate SiO2 enrichments. See text for further explanation.
to grow to a certain threshold grain size, after which they are suc-
ceeded by another mineral (e.g. clays, epidote, prehnite, wairakite,
chalcedony and sometimes quartz). Other minerals like calcite, an-
hydrite (the latter in saline systems), and sometimes quartz, are more
rarely constrained by size and tend to fill the available space. Whatever
the reason, the limit of mineral size does increase the probability that
one could find at least two minerals in any one vesicle. Calcite is the
mineral that is most likely to fill available space. However, calcite
generally precipitates at a late stage in the mineral sequence after the
deposition of the other minerals. The above observations imply that
typical rocks in a given high temperature system retain open pore
space for sufficient time to record the effects of more than one geo-
thermal episode. Thus the enrichment/depletion trends tend to accu-
mulate over the lifetime of the system. It has also been noted that
changes in mineral deposition sequences can be correlated regionally
within individual geothermal fields (e.g. Franzson, 2000), which im-
plies that mineral deposition is controlled by large scale hydrological
changes in the geothermal system.
It is instructive to compare the low salinity Icelandic geothermal
systems with basalt-hosted seawater-derived hydrothermal fluids (Alt
and Teagle (2000) and references therein and Butterfield (2000) and
references therein), as evidenced in ophiolitic rocks and “black smoker”
hydrothermal systems. The overall similarity in the composition of ba-
salts from the seafloor, ophiolites and subaerial Iceland facilitates com-
parison of these systems. Their physical volcanology does show some
differences that could lead to differences in fluid–rock interaction.
Extensional tectonics and rift zone volcanism are common to each of
these settings, but the deep water eruptions, common on mid-ocean
227
ridges and ophiolites, are different from the subareal eruptions in Ice-
land (Batiza and White, 2000).
Seafloor eruptions produce more abundant glassy volcanics and
hyaloclastites than subaerial eruptions in the Tertiary, which should
enhance the alteration potential of seafloor rocks. However, Pleisto-
cene eruptions in Iceland often occurred beneath ice cover and resul-
ted in extensive formation of hyaloclastite. Seafloor pillow lavas and
sheet flows, which characteristically show drain-back features, have
very high intrinsic, large scale porosity and permeability, but the
permeability drops significantly in older, more deeply buried lavas
due to collapse and infilling by later eruptions (Perfit and Chadwick,
1998; Fornari et al., 2004). However, submarine lavas are rarely vesi-
culated. In contrast, flow top and bottom breccias and highly vesi-
culated flow tops in subaerial lavas provide laterally continuous zones
of high porosity that results in anisotropic permeability that favors
lateral flow and restricts vertical convection (Fornari and Embley,
1995; Fornari et al., 2004).
One major compositional difference between subarial and sub-
marine lavas is in the concentration of volatile elements, particularly
sulfur. Sulfur concentrations of MORBs are typically about 1000 to
1500 ppm, in contrast to values of about 100 ppm in subarial lavas that
have degassed during eruption (Wallace and Anderson, 2000). Because
potentially acid-generating volatiles (e.g. SO2, HCl, CO2) are lost during
eruption, subsequent hydrothermal leaching will not involve these
species and the resultant hydrothermal fluids may not attain low pHs
that facilitate rock alteration. This is particularly true for hydrothermal
systems developed in plateau basalts, such as at Hvalfjordur. Magmatic
degassing during intrusive/eruptive events can result in short lived
228 H. Franzson et al. / Journal of Volcanology and Geothermal Research 173 (2008) 217–229
compositional changes in geothermal systems due to acidification
reactions (Armannsson et al., 1982). In hydrothermal systems devel-
oped in longer-lived central volcanoes (e.g. Hafnarfjall, Geitafell), late
stage intrusive rocks can supply both heat and acid-generating volatile
species that can change the pattern of alteration of the older, degassed
lava flows. Degassing of sulfur from basalt can affect the mobility of
other elements as well, particularly the base metals. For example,
submarine basalts erupted at higher pressures due to the weight of the
overlying water column and therefore do not degass sulfur as readily.
Copper in submarine basalts is typically concentrated as chalcopyrite
and is generally only mobilised by high temperature (N330 °C)
hydrothermal fluids due to the low solubility of chalcopyrite in
sulfide-bearing fluids. In contrast, copper in subareally erupted basalts
that have degassed sulfur, chalcopyrite may not be stable leaving
copper in a form that is easily leached and transported by low
temperature, oxidized fluids (Lincoln, 1981).
The upper temperature limits in shallow geothermal fields are
typically set by the boiling temperature curve of the fluid. In deeper,
higher salinity systems rapid changes in the physical and chemical
properties of the fluid at temperatures approaching the critical point
provide similar temperature constraints. The higher pressures and
salinities inherent in submarine geothermal systems therefore favour
higher ultimate temperatures of water–rock reaction in the deeper
portions of these system. It is interesting that the general zonation of
alteration minerals in Icelandic geothermal systems (Fig. 2) is similar
to those observed in drill holes throughout the oceanic crust (Alt and
Teagle, 2000 and references therein; Wilson et al., 2006) and
ophiolites (Schiffman et al., 1991; Gillis and Banerjee, 2000).
The major difference in subarial geothermal systems recharged by
meteoric water and submarine systems recharged by seawater is the
salinity of the fluid. Chloride complexing is significant for many cat-
ions and strongly enhances the solubility of most minerals, especially
at elevated temperatures. Higher concentrations of major element
cations in seawater-recharged hydrothermal fluids will also affect the
stability of alteration minerals making it all the more surprising that
the zonation of alteration minerals in seafloor hydrothermal systems
is so similar to that in Iceland. Although the general pattern of
alteration mineral zonation is similar, the extent of hydrothermal
alteration and mass flux from high temperature seafloor systems is
significantly different from that of the Icelandic geothermal systems.
The geochemical data presented in this paper document that the
major changes in the compositions of altered rocks from Icelandic
geothermal systems result from the addition of elements during
deposition of pore-filling alteration minerals. Isocon plots of altered
samples, corrected for dilution, show relatively small mass fluxes for
most elements, even at high degrees of alteration. This general
observation is true across the range of alteration zones even in rocks
that show epidote–amphibole alteration. In contrast, basalt/seawater
reaction results in significant metasomatism of the rocks (Seyfried and
Ding, 1995). As seawater is heated by circulating in the oceanic crust
on the recharge limb of hydrothermal convection cells, metasomatic
addition of seawater-derived Mg and Ca into basalts releases hydrogen
ions lowering the fluid pH (measured at 25 °C) into the 3–4.5 range
that is typical of black smoker fluids. Calculated in situ pH at high
temperature are about one unit lower than neutral (Ding and Seyfried,
1992). This low pH fluid has significant capacity for hydrogen meta-
somatism in the deep reaction zone and the rising limb of the con-
vective circulation. Acid alteration of the basalts releases a significant
flux of cations into the hydrothermal fluids resulting in highly cation-
leached alteration zones, enriched in aluminum and silica, in focussed
upflow zones where integrated water–rock ratios are high (Humphris
et al., 1998; Zierenberg et al., 1988, 1995, 1998; Teagle and Alt, 2004).
Silicified basalts in hydrothermal upflow zones can have silica con-
tents in excess of 80 wt.% (e.g. Zierenberg et al., 1995). Alternatively, Fe
and Mg metasomatism is hydrothermal upflow zones can result in
pervasive chloritization of basalt resulting in bulk compositions
approaching chlorite with SiO2 as low as 35 wt.% (Humphris et al.,
1998) and FeOT + MgO N 25 wt.% (Zierenberg et al., 1988). Thus the
most significant difference between seawater and meteoric water
recharged basalt-hosted hydrothermal systems is the mass flux from
the system, not the mineral assemblages which seem to be controlled
predominantly by the thermal stability of the alteration phases and
secondarily by the composition of the hydrothermal fluids.
8. Conclusions
This paper reports a method to compare hydrothermally altered
basaltic rocks and their protoliths that facilitates correction for mass
additions to the rock, during hydrothermal alteration. This method
takes into account the amount of mineral deposition into the rock, as
determined by petrography, and recalculates the mass addition using
the immobile element concentration. The derived recalculated com-
position of the altered rocks can then be compared with the least
altered protoliths from the same areas. The comparison showed that
hydrothermal alteration causes pronounced Si-enrichment as well as
a considerable Al, Fe, Mg and Mn enrichment. Elements such as Ca, Na,
K, are also mobile and can be either depleted or enriched. Immobile
elements include Zr, Y, Nb, Ce, and probably Ti. An important con-
clusion from this work is that the predominant process leading to
chemical flux in these rocks is deposition of alteration minerals in
primary pore space, but mass flux due to recrystallization and replace-
ment reactions are of secondary importance. This contrasts with
seawater-dominated hydrothermal systems where metasomatic reac-
tions result in extensive mass flux. Another important conclusion is
that similar chemical changes were experienced in the two Tertiary
central volcanoes studied, suggesting that these may represent a ge-
neral trend in Icelandic high-temperature systems. A study of a
sample suite of flood basalts within a low-temperature zeolite alter-
ation environment of Tertiary age also shows chemical changes akin to
the former, but the changes are more subtle. It is also significant that
the general zonation of alteration minerals in Icelandic alteration
zones is similar to those in seawater-dominated hydrothermal
systems in spite of the differences in the extent of metasomatism.
This implies that temperature, not fluid composition, provides the first
order control on mineral assemblages in basalt-hosted hydrothermal
systems.
Acknowledgements
We thank Howard Day and Shuwen Liu for very helpful discussion on
various aspects of this work, and the late Valgardur Stefansson for
critically reading the manuscript and his vigorous support. Patrick R. L.
Browne and an anonymous reviewer are thanked for critically reviewing
the paper and suggesting a number of improvements. This paper was
written during the sabbatical leave of the first author at the Geological
Department, University of California, Davis in the USA. The financial
support of Orkustofnun to complete this work is acknowledged.
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