Contrib Mineral Petrol (1993) 114:510-518
Contributions to
Two-feldspar geothermometry: a review and revision
for slowly cooled rocks
Herbert Kroll a, Christos Evangelakakis 1, and Gerhard Voll z
lnstitut ffir Mineralogie, Wesff'~ilischeWilhelms-Universit/it, Correnstrasse 24, D-48149 M/inster, Germany
2 Institut ffir Mineralogie, Universitfit zu K61n, Zfilpicher Strasse 49, D-50674 K61n 1, Germany
Received November 23, 1992 / Accepted April 26, 1993
Abstract. Recent improvements in the experimental and
thermodynamic basis of two-feldspar geothermometry
allow one to recover temperatures of coexistence more
reliably. Some problems, however, persist: (1) the experi-
mental solvi by Seck (1971a) and Elkins and Grove
(1990) differ from each other; (2) it is not known to
what extent N a - K - C a exchange equilibrium is ap-
proached; (3) both solvi are probably metastable with
regard to A1, Si order; (4) it is difficult to judge how
closely high-temperature natural feldspars compare to
this situation; (5) the thermodynamic treatment neglects
phase transformations; (6) the temperature dependence
of the Margules parameters used to model non-ideal
mixing behaviour may not be linear; (7) it is not clear
which expressions should be used to describe ideal activi-
ties. With these caveats in mind we treat the problem
of retrograde resetting in high-grade metamorphic rocks
that were slowly cooled under essentially dry conditions.
Coexisting feldspars from such rocks commonly do not
plot on a c o m m o n isotherm. Thus temperatures derived
from such pairs using any of the proposed two-feldspar
geothermometers will necessarily be in error. We suggest
that the non-equilibrium compositions result from retro-
grade intercrystalline K - N a exchange. This exchange
continues after the plagioclase and alkali feldspar have
already become essentially closed systems with respect
to A1 - Si exchange, which is a prerequisite for (Na,K) -
Ca exchange. We use a modified version of the Fuhrman
and Lindsley (1988) programme to reverse the K - N a
exchange and derive concordant temperatures.
Introduction
Natural feldspars are solid solutions primarily composed
of K-feldspar (Or,KA1Si3Os), Na-feldspar (Ab,NaA1-
SilOs) and Ca-feldspar (An,CaA12Si2Os). Barth (1934,
1951) first suggested that the distribution of the Ab corn-
Correspondence to: H. Kroll
Mineralogy and
Petrology
9 Springer-Verlag 1993
ponent between coexisting plagioclase and alkali feld-
spar could be used to estimate the temperature of equili-
bration. Since then, two-feldspar geothermometry has
been investigated by experiment (Iiyama 1966; Seck
1971a, b; Johannes 1979; Elkins and Grove 1990) and
thermodynamic modelling (Stormer 1975; Powell and
Powell 1977; Whitney and Stormer 1977; Brown and
Parsons 1981; Haselton eta1. 1983; Ghiorso 1984;
Green and Usdansky i986; F u h n n a n and Lindsley
1988). Lucid discussions of fundamental problems were
provided by Brown and Parsons (1981, 1985).
In the following, we first review the experimental and
thermodynamic basis of the two-feldspar geothermome-
ter and point out inherent problems. We then discuss
the inter- and intracrystalline exchange processes that
occur in feldspar pairs during retrograde resetting. We
suggest a procedure to recover the original equilibrium
compositions so that two-feldspar geothermometry can
be applied meaningfully.
Experimental basis of two-feldspar geothermometry
K - - N a - - Ca exchange
Two-feldspar geothermometry relies primarily on experimental
data bases from Seck (1971a, b) and Elkins and Grove (1990).
Seek (1971a, b) used ternary gels as starting material and per-
formed experiments between 650 and 900~ C at HaO pressures up
to 10 kbar. Elkins and Grove (1990) started from crystalline materi-
al and reacted mixes of two or three feldspars at 700 to 900~ C
and 1 to 3 kbar Pn,o. For both sets of experiments attainment
of K - Na-- Ca excliange equilibrium is di •cult to judge. Scck
(1971 a, b) checked the assumption of equilibrium by experiments
in which he reacted two different feldspar pairs that had the same
bulk composition as the previously crystallized ternary gel. In each
set of experiments the alkali feldspars approached identical compo-
sitions. Johannes (1979) criticized Seek (1971a, b) on the basis
of his own experiments in the ternary system stating that "it is
very unlikely that equilibrium has been reached and that one homo-
geneous plagioclase has been formed in the cross test of Scck".
Despite this criticism, the two-feldspar geothermometer pro-
gramme of Fuhrman and Lindsley (1988), which employs Margules
 51i

parameters derived from Seck's data, gives temperatures for natu- T h e r m o d y n a m i c modelling
ral feldspar assemblages that are reasonable when compared with of the t w o - f e l d s p a r g e o t h e r m o m e t e r
the results of other geothermometers.
The run products of Elkins and Grove (1990) outline smooth
isothermal curves. The fact that these are approached from binary
Basic formalism
and ternary compositions suggests that they obtained a metastable
If two ternary feldspar solid solutions (El, plagioclase; AF, alkali
or stable equilibrium. Unlike Seck (1971a), Elkins and Grove
feldspar) are in equilibrium, the activities a] of their three compo-
(1990) could check whether the tie-line connecting the product pla-
nents i are equal in each phase j:
gioclase and alkali feldspar passed through the bulk composition,
P1 AF
or whether the bulk composition plotted within the triangle of RTln aAb RTlnaAb
= (i)
plagioclase - alkali feldspar melt, in cases where a melt phase gTln(IPl, z RT]naAo~ (2)
had developed. This they took as another indication of equilibrium. R Tin aPA1,.--. . .R. ~ - ..AF
An, (3)
In several experiments, however, this condition was not fulfilled,
because the reactions had not gone to completion. where
aAb= )~Ab~TAb,etc. (4)
State of Al, Si order )~ is the ideal activity, ~ is the activity coefficient; p can be expressed
in terms of Margules parameters WG (Wohl 1946, 1953). The Mar-
Neither Seck (1971a, b) nor Elkins and Grove (1990) attempted gules parameters are usually assumed to vary linearly with tempera-
to estimate the degree of A1,Si order in the experimental feldspars. ture and pressure, e.g.
In Seck's (1971a, b) experiments crystallization of gels certainly W ~ b O r = W~AbOr - - r ~ A b O r ~- pWVAbor - (5)
resulted in highly disordered run products, because in gels growth
rates are fast compared to ordering rates. In the course of the Equations (1)-(3) can each be solved for T, and three tempera-
experiments the feldspars approached their equilibrimia state of tures TAb, To~, TAn,respectively, may be obtained for given feldspar
order to a varying and unknown degree. Elkins and Grove (1990) compositions at a given P. Ideally these temperatures should agree,
used ordered and disordered starting materials, but did not detect if the two feldspar compositions represent equilibrium.
an effect on the width of the solvus. Probably the newly grown
products were disordered regardless of the starting material. Thus
the thermodynamic data used to model the ternary solvus may Ideal activity
not be completely appropriate for N a - K -- Ca exchange equilibri-
um as well as equilibrium A1,Si ordering. The magnitude of this The choice of the ideal activities (Eq. 4) affects the values of the
problem is unknown. It may be negligible at high temperatures, Margules parameters, because ~ depends on X. Ghiorso (1984),
but will increase at lower temperatures. Green and Usdansky (1986), and Fuhrman and Lindsley (1988)
The effect of increasing A1,Si order in feldspars is to increase expressed X in terms of the Al-avoidance rule. Following Price
and widen the solvus (Bachinsky and Mfiller 1971). Temperatures (1985) this gives
estimated using a disordered solvus are low, when the coexisting XAb= 4XA. X ~ xT~ (XsTi2)2 (6)
phases are ordered. It is likely that natural feldspars, especially
when crystallizing from melt, grow with a high degree of disorder, Xor=4X A X~,~ xxll (XsX~)2 (7)
so K, Na and Ca are distributed between disordered phases. Brown 2A.= x~. (x~d) ~ (x~?) ~, (8)
and Parsons (1985) note that subsequent to growth ordering will
occur, which will require redistribution of K, Na, and Ca. Ordering where X{ denotes atomic fractions of Na, K or Ca on the irregular
is an intracrystalline process with small step-widths (some A,), A site and of A1 and Si on the two non-equivalent tetrahedral
whereas redistribution of Na, K, and Ca is an intercrystalline pro- TI and T2 sites (X~i2 = 1 for strict Al-avoidance). These formula-
cess with large step-widths (gin to ram), which has to be accompa- tions permit easy correction for minor components, such as Fe 3 +-,
nied by A 1 - S i exchange to maintain charge balance. One might Sr-, or Ba-feldspar, by incorporating their respective A1,Si contents
therefore cxpcct that K - - N a - - C a and AI--Si exchange will not into the tetrahedral site occupancies.
keep pace with A1,Si ordering thereby creating a non-equilibrium Lindslcy and Nekvasil (1989) and Elkins and Grove (1990) pre-
situati on. ferred mole fractons of Ab, Or, and An as ideal activities:
The experimental solvi are probably metastable with respect J?~=x~ (9)
to A1,Si order. The natural feldspars may or may not achieve an
equilibrium degree of order. As a consequence, two incompatible 2o~=Xo, (10)
situations are compared. However, if one restricts the application X%=x~.. (il)
of the models to high-temperature phase assemblages ( T > 750~ C), Random mixing of units of Ab, Or, and An necessarily preserves
the error might be tolerable. The situation becomes more compli- local charge balance, whereas random mixing of Na, K, Ca on
cated, if, at a lower temperature, the alkali feldspar exsolves plagio- the A site and independent mixing of A1 and Si on the T sites
clase (perthite) or the plagioclase exsolves alkali feldspar (anti- does not. It is unlikely that mixing on the A and T sites is not
perthite). Firstly, the increased order requires a wider solvus than coupled to some degree.
has experimentally been determined. Secondly, if exsolution occurs In contrast to the Al-avoidance model, the molecular mixing
via a nucleation and growth mechanism, the situation may be simi- model does not provide an umambigous way to account for minor
lar to the one described above with respect to initial disorder and substitutions. A projection must be used, and usually XAb+XO~+
subsequent ordering. At present this situation cannot be handled XA~ is normalized to I.
by an experimental geothermometer.

Temperature dependence of Margules parameters

The assumption that W e is linearly dependent on temperature (Eq.
5) introduces another problem. Kimberley (1980) and Kaiping and
Kroll (1989) found that a linear fit of W e is often not satisfactory,
as it may cause the calculated solvus to close at temperatures that
are low by comparison with experiment. The linear fit tends to
512

Table 1. Comparison of calculated temperatures for granttlite-facies ternary feldspar pairs

Two-feldspar P Composition (1) Composition (2) Composition (EG) Composition (FL)

samples (kbar)
Ab Or An Ab Or An Ab Or An Ab Or An

VSL 16 8 P1 71.3 0.7 28.0 69.3 2.7 28.0 66.0 6.0 28.0 66.5 5.5 28.0
AF 21.0 77.4 1.5 21.0 77.9 1.0 23.0 75.4 1.5 19.0 79,4 1.5
T 669 416 820 698 603 682 752 751 751 705 704 706
VSL 48 8 Pl 70.6 2.9 26.5 68.6 4,9 26.5 62.0 11.5 26.5 62.2 11.3 26.5
Parent grains AF 23.2 73.0 3.8 25.2 73.0 1.8 32.2 64.0 3.8 27.6 68.6 3.8
T 658 610 1260 754 807 708 904 903 903 850 852 851
VSL 48 8 P1 72.2 ! .0 26.8 70.2 3.0 26.8 69.6 3.6 26.8 69.8 3.4 26.8
Recrystallised i1 AF 18.5 80.8 0.7 16.5 82.8 0.6 17.1 82.2 0.7 14.2 85.1 0.7
T 642 454 649 650 610 648 649 650 650 610 610 610
VSL 51 8 PI 79.3 1.7 19.1 77.3 3.7 19.1 67.9 13.1 19.1 68.3 12.7 19.t
AF 38.7 58.0 3.3 37.7 58.0 2.3 37.1 59.6 3.3 33.3 63.4 3.3
T 746 499 1011 774 634 737 882 881 881 844 845 844
VSL 207 8 Pl 72.4 1.6 26.0 72.4 3.6 24.0 67.8 6.2 26.0 68.3 5.7 26,0
AF 22.0 76.6 1.4 22.0 77.1 0.9 23.6 75.0 1.4 19.7 78.9 1.4
T 681 518 801 693 635 670 746 747 747 705 704 704
VSL 464 8 P1 69.7 1.7 28.6 69.7 3.7 26.6 63.8 7.6 28.6 64.2 7.2 28.6
AF 28.0 69.8 2.2 28.0 70.3 1.7 25.9 71.8 2.2 21.7 76.1 2.2
T 769 534 818 787 661 737 809 810 810 763 761 762
VSL 505 8 PI 80.0 1.6 18.4 78.0 3.6 18.4 68.2 13.4 18.4 68,5 13.1 18.4
AF 35.0 61.8 3.2 35.0 63.3 1.7 37.3 59.5 3.2 33,6 63.2 3.2
T 711 484 1149 778 622 756 880 879 879 844 844 843
VSL 510 8 P1 62.1 2.5 35.4 62.1 4.5 33.4 57.8 6.8 35.4 58.2 6.4 35.4
AF 20.4 77.2 2.4 20.4 78.2 1.4 23.0 74.6 2.4 18.8 78.8 2.4
T 716 619 900 742 717 726 821 821 821 761 763 761
VSL 512 8 P1 67.2 1.0 31.8 67.2 3.0 29.8 60.8 7.4 31.8 59.5 7.8 31.8
AF 23.7 74.0 2.3 23.7 75.0 1.3 24.5 73.3 2.3 19.5 78.0 2.3
T 727 473 869 754 632 693 818 819 819 770 769 770
VSL 516 8 P1 80.0 2.0 18.0 78.0 4.0 18.0 67.8 14.2 18.0 68.0 14.0 18.0
AF 34.2 62.4 3.4 34.2 64.4 1.4 38.2 58.4 3.4 34.5 62.1 3.4
T 699 520 1244 756 628 762 889 889 889 854 855 854
VSL 522 8 Pl 79.9 1.8 18.2 77.9 3.8 18.2 67.6 14.1 18.2 67.5 14.2 18.2
AF 23.5 73.4 3.2 25.5 73.4 1.2 37.1 59.8 3.2 33.2 63.7 3.2
T 607 503 1522 689 620 828 884 885 885 851 852 851
BSL 43-1 11.5 P1 73.5 0.9 25.7 73.5 2.9 23.7 66.3 8.1 25.7 66.7 7.7 25.7
AF 26.7 71.1 2.1 26.7 71.6 1.6 24.9 72.9 2.1 20.5 77.3 2.1
T 767 448 821 782 616 743 813 811 812 764 766 764
BSL 88-27a 8.3 P1 61.5 1.2 37.3 59.5 3.2 37.3 57.2 5.5 37.3 57.5 5.2 37.3
AF 19.0 79.1 1.9 19.0 79.6 1.4 20.2 77.9 1.9 16.3 81.8 1.9
T 702 505 824 739 668 719 780 779 779 724 723 723
SL119-2 9.3 P1 71.4 1.2 27.4 71.4 3.2 25.4 65.4 7,2 27.4 65.8 6.8 27.4
Recrystallised l AF 23.9 74.2 1.9 24.4 74.8 1.4 24.5 73.6 1.9 20.3 77.8 1.9
T 722 484 845 743 628 745 792 789 792 746 744 745
SL 119-2 8 P1 71.3 0.7 28.0 71.3 2.7 26.0 68.0 4.0 28.0 68.4 3.6 28.0
Recrystallised iI AF 22.7 76.5 0.8 20.7 78.5 0.8 18.1 81.1 0.8 14.5 84.7 0.8
T 711 417 608 683 594 652 665 663 663 623 624 623
BSL 143-2 8.7 P1 73.4 2.4 24.2 71.4 4.4 24.2 65.9 9.9 24.2 66.4 9.4 24.2
AF 30.3 67.1 2.6 28.3 69.1 2.6 29.8 67.6 2.6 25.5 71.9 2.6
T 763 577 908 789 665 784 845 846 845 799 800 801
K 287-1 8 P1 72.3 2.2 25.3 72.3 3.7 23.8 67.9 6.6 25.3 68.4 6.1 25.3
AF 17.3 81.4 1.4 17.3 82.4 0.4 23.9 74.8 1.4 20.0 78.7 1.4
T 627 553 901 631 627 561 750 751 752 710 709 711

Table 1 (continued)
Mesoperthitc samples P (kbar) Composition (1)
Ab Or An
VSL 294 61.4 36.1 2.4
8 T EG: 845 FL: 824
VSL 523 44.9 50.2 4.8
8 T EG: 926 FL: 895
VSL 706 76.2 22.0 1.8
8 T EG: 793 FL: 774
VSL718 48.5 51.3 0.2
8 T EG: 770 FL: 759
Note: Composition (1), (2), (EG), (FL): (1) original composition,
(2) composition "corrected" within 2 tool% analytical uncertainty
using the original Fuhrman and Lindsley (1988) programme, (EG)
and (FL) compositions obtained after correction for assumed retro-
grade resetting at constant An using Margules parameters of Elkins
and Grove (1990) (EG), and Fuhnnan and Lindsley (I988) (FL),
respectively; Ab, Or, An in mol%; P1, plagioclase feldspar; AF,
alkali feldspar; T(Ab), T(Or), T(An) [~ are calculated from Eqs
(1), (2), (3), respectively, in samples containing only mesoperthites,
temperatures were determined from the isotherms, on which their
compositions plot. Analysis of sample K287-1 was kindly provided
by Dr. Schumacher, Mfinster. It should be noted that the values
of W~no, and W~O,A,should be interchanged in Table 1 of Fuhrman
and Lindsley (1988), as well as the values of WVbo, and WOrAb v is generally h o m o g e n e o u s and m o s t l y not antiperthitic.
in Table 4 of Elkins and Grove (1990)
cause too steep a decrease of W ~ at high temperatures. They found
that hyperbolic functions (hyperbolic tangent and inverse hyperbol-
ic sine) were more appropriate. When using the assumption of
linearity, one should therefore be aware of its possible shortcom-
ings.
Structural phase transformations
At high temperature, equilibrated feldspars adopt one of three
space groups: C2/m (potassic alkali feldspars), CI (sodic alkali
feldspars and plagioclases), and I1 (calcic plagioclases). The phase
transitions are presumably continuous. They are currently ne-
glected in modelling the G-surface of ternary feldspars, because
this would require three sets of Margules parameters rather than
one. Even the alkali feldspar solvus, although investigated by sever-
al workers, has mostly been modelled assuming that no phase tran-
sition is present (see, however, Merkel and Blencoe 1982). Kroll
et al. (1986) treated excess volumes of high-temperature alkali feld-
spars as two different populations, ( K - ) analbite and ( N a - ) sani-
dine. They found WVbo~>W~orAb,whereas Hovis (1988) neglecting
the phase transition found WVbo~<wV~Ab.These results imply dif-
ferent pressure dependencies of the solvus. Hovis et al. 0991) sug-
gest that the high precision of calorimetric data indicates that ef-
fects due to the displacive monoclinic-triclinic transtbrmation must
be small. This may also be trne for the diffusive order/disorder
transition. For the time being, one may assume that the phase
transitions in high-temperature feldspars have a negligible effect
on the ternary solvus.
Influence of pressure on the height of the solvus
Hovis et al. (1991) developed new values for enthalpy and entropy
Margulcs parameters for the A b - O r join. From their data we
calculated pressure dependencies of 18.3~ for the solvus crest
and 12.9~ for the solvus limb at Orso, whereas 15.9~
513
and 12.3~ respectively, result from the data of Elkins and
Grove (1990). As demonstrated by Fuhrman and Lindsley (1988,
Fig. 3), the calculated increase of the alkali feldspar solvus resulting
from positive Wv parameters is counteracted in the ternary field
by negative values of WA,,O v r and WAborAn. This means that the
tcmperature estimate is fairly insensitive to the pressure estimate,
which is a fortunate feature of the two-feldspar geothermometer.
The currently used W v parameters, however, can be improved.
For plagioclases we determined from the data of KroU and Miiller
(1980) WVBA,= 0.094 J/bar and W~A,,Ab= --0.099 J/bar. For the me-
tastable A n - O r join we calculated from a more complete set of
data than was used by Fuhrman and Lindsley (1988) WVAA,Or=
WVoorA,=--0.268J/bar (Kroll and Mfiller 1980; Kroll and Barn-
bauer 1981; Kroll et al. 1986). An average ternary W v parameter
is derived from two disordered ternary feldspar series of Kroll
et al. (1986) as wVA,,OrA,=--0.57 J/bar.
Future treatment of the ternary solvus should utilize both the
recent W n and W s parameters of Hovis et al. (1991) and the W v
parameters given above.
Two-feldspar geothermometry
of granulite-faeies feldspars
Microprobe analyses
Feldspar pairs f r o m Sri L a n k a n rocks typically consist
o f spindle-perthites coexisting with plagioclase, which
Only those alkali feldspars have been analysed whose
exsolution textures were n o t affected by an aqueous fluid
phase, but were regular or modified by deformation,
at most. T h a t is, patch-, braid-, flame-, or vein-perthites,
which have p r o b a b l y developed f r o m regular meso- or
spindle-perthites due to interaction with an a q u e o u s
fluid phase, have been excluded, because the original
bulk compositions m a y have been altered.
After careful optical inspection, crystals cut Ib(001)
were selected for m i c r o p r o b e analysis. A defocussed
b e a m (50 lain-100 gin) was used to obtain bulk composi-
tions. D e p e n d i n g on the h o m o g e n e i t y o f the exsolution
pattern, the grains were partly or fully covered by b r o a d
spots t o u c h i n g each other (see Bohlen and Essene 1977,
for a discussion o f integrated analyses). Elements Na,
K, Ca, Ba, A1, Si, M g and Fe were routinely analysed.
N o systematic deviation f r o m stoichiometry could be
detected. W h e n the alkali feldspars were z o n e d with re-
spect to their distribution o f plagioclase lamellae, which
tend to be concentrated in the core, integrated core c o m -
positions were obtained. All results were normalized to
Or + Ab + A n = 100 m o l % and are given in Table 1.
Problem of retrograde resetting
Cation exchange g e o t h e r m o m e t r y is plagued to different
degrees by the p r o b l e m o f retrograde resetting (e.g. La-
saga 1983). Since each g e o t h e r m o m e t e r has its own clo-
sure temperature depending on the cooling rate, agree-
m e n t between temperatures f r o m different g e o t h e r m o m -
eters is, in principle, accidental. Retrograde resetting o f
feldspars f r o m slowly cooled, high-grade m e t a m o r p h i c
terrains has been noted by a n u m b e r o f workers (e.g.
M o r a a n d Valley 1985; B r o w n and Parsons 1988; Fuhr-
m a n and Lindsley 1988). In this case, the compositions
514

An et al. in press). As a result, we propose a modified ver-

sion of the two-feldspar geothermometer.

Sequence of exchange and exsolution events

In Fig. 2a the integrated compositions of a representa-
tive feldspar pair A - P are plotted [VSL522, Table 1,
" C o m p o s i t i o n (1)"]. Clearly, the data points do not lie
on a c o m m o n isotherm. The temperatures TAb, Toy, and
TA,, calculated from "Composition (1)", are also given
in Table 1. As discussed by Fuhrman and Lindsley
(1988), TAn is largely controlled by the slope of the tie-
line, whereas the An content o f the alkali feldspar mainly
influences TAn, and the Or content of the plagioclase
dominates Tot. As expected from the low Or content
of the plagioclase VSL522, Tot is the lowest of the three
Ab zo 40 50 8o Or temperatures. When allowing for 2 tool% analytical un-
certainty, Or in the plagioclase increases, so that Tot
Fig. 1. Microprobe analysis of coexisting Sri Lankan feldspar pairs also increases, but the " c o r r e c t e d " compositions [Ta-
[Table 1, Composition (1)]. Ternary miscibility gap calculated for ble 1, " C o m p o s i t i o n (2)"] still do not define an equilib-
P= 8 kbar using Margules parameters of Elkins and Grove (1990)
rium tie-line, and the temperatures are still discordant.
To carry the analysis one step further, we qualitatively
of coexisting plagioclase and alkali feldspars plot on dif-
ferent isotherms, with the Or content of the plagioclase
low compared to its Or content expected from the An
content of the coexisting alkali feldspar (Fig. 1). Thus,
without accounting for the retrograde changes in some
way, temperatures derived from any o f the proposed
thermometers will be in error.
The K deficiency of the plagioclase is commonly as-
cribed to K loss during slow cooling, not considering
possible changes in the alkali feldspar. Brown and Par-
sons (1988), however, point out that the different ease
of K - Na and A 1 - Si exchange between coexisting feld-
spars is responsible for their unusual compositions. We
will follow this line of reasoning.
Fuhrman and Lindsley (1988) devised a geothermom-
eter programme that allows for some uncertainty in feld-
spar analyses. Compositions provided by the user are
varied by the programme within an arbitrary limit of
2 mol%, so that the activity equations (1) (3) are ful-
filled as closely as possible. In case of equilibrium pairs,
the three temperatures Tab, Tot, and TAn derived from
(1) (3), respectively, correspond closely.
When applying this geothermometer to coexisting
metamorphic feldspars, Fuhrman and Lindsley (1988)
noted that the adjusted Or content of plagioclase system- Ab Or
atically increased by the allowed maximum of 2 tool%. Fig. 2a-e. Simplified model of cooling history and exsolution
But even after this " c o r r e c t i o n " , the temperature Tot events of a plagioclase - alkali feldspar pair (sample VSL 522).
is lower on average by l l 0 ~ than the corresponding a The low-temperature non-equilibrium pair A-P evolves from the
high-temperature equilibrium pair Ao-Po due to retrograde K --Na
temperatures TAb and TAn (calculated from their Ta- exchange, when the crystals Ao and Po have turned into closed
ble 4). It thus appears that the loss of K-feldspar compo- systems with respect to A1--Si exchange, b Plagioclase lamellae
nent may be larger than 2 mol% and could therefore Lo exsolve in the alkali feldspar Ao when it closed the intercrystal-
be outside analytical uncertainty. line A1-Si exchange. During cooling, the lamellae change their
We examine here the cooling history and exsolution composition from Lo to L2 via L1, where the intracrystalline AI -- Si
sequence of a plagioclase - alkali feldspar pair that is exchange ceases. The alkali feldspar matrix shifts from Ao to M2
via MI. The bulk composition changes from Ao to A due to inter-
typical for high-grade metamorphic terrains, in particu- crystalline K - N a exchange, e When the matrix M2 and lamellae
lar for the granulite-facies rocks o f Sri Lanka, the feld- L2 become closed systems with respect to K - Na exchange, film-
spars of which we have studied in detail (Evangelakakis lamellae and fine-scale strings (L3) unmix in a final exsolution
et al. 1991a, b, 1992, in press; Evangelakakis 1992; Voll event below the coherent solvus

discuss in a simphfied and idealized manner the processes,
which the feldspar pair undergoes during cooling. We
deliberately restrict ourselves to the discussion of inter-
actions between feldspars and ignore possible interac-
tions with other minerals and with an aqueous fluid
phase, which may alter the original compositions.
Let us assume that at some high temperature the feld-
spar pair A o - P o shown in Fig. 2a is at equilibrium.
Each crystal represents an open system with respect to
the intercrystalline K - N a - C a as well as the A1-Si
exchange, so as to maintain charge balance. At the essen-
tially dry conditions, at which the rock is assumed to
cool, the A1-Si diffusivities are very low (Grove et al.
1984; Yund 1986; Liu and Yund 1992). It is therefore
to be expected that the K Ca exchange between the
two feldspar phases, which involves A1-Si exchange,
will cease very early in the retrograde history of the
rock, so that the crystals become essentially closed sys-
tems with respect to Ca transfer. On the other hand,
the N a - K exchange, which does not involve A1-Si
exchange, may continue down to lower temperatures.
Because the Ca concentrations remain virtually constant,
the compositions of the two phases will be shifted in
opposite directions parallel to the A b - O r join off the
common isotherm (Fig. 2a: Po--*P and Ao ~A), so that
the two feldspars no longer constitute an equilibrium-
pair.
After the crystals have evolved into closed systems
with respect to the A1-Si exchange, the CaA1 content
of the alkali feldspar becomes supercritical, so that pla-
gioclase lamellae are exsolved in an intracrystalline ex-
change process. In due course, the homogeneous alkali
feldspar transforms into a spindle-perthite (Fig. 2b). By
contrast, the plagioclase continues to exchange K versus
Na with the alkali feldspar rather than to exsolve its
Or content and to transform into an antiperthite. In
fact, all plagioclases listed in Table 1 were homogeneous.
Let us assume that the exsolution of the plagioclase
lamellae from alkali feldspar occurs below the strain-free
solvus and that it begins at a low degree of super-satura-
tion. Both assumptions are not critical, but simplify the
discussion. The composition Lo of the plagioclase lamel-
lae exsolved first is then close to the composition Po
of the plagioclase grains. During cooling, two processes
simultaneously occur in the alkali feldspar: Its bulk com-
position continuously changes from Ao to A, while the
lamellae L and the matrix M between the lamellae
change their compositions from Lo to L2 and from Mo
(~A0) to M2, respectively. The intracrystalline A I - S i
exchange between lamellae and matrix freezes in at some
temperature that is presumably lower than the tempera-
ture, at which the intercrystalline A1-Si exchange
freezes in. Lamellae and matrix have then assumed, for
example, the compositions L 1 and M1. From there on,
the lamellae no longer increase in volume, because this
would require influx of NaSi+CaA1 versus KSi from
the matrix. From L1 and M1 to L2 and M2, respectively,
the compositions change via N a - - K exchange only.
The bulk composition A and the compositions of the
lamellae L2 and the matrix M2 are given in Table 2.
The tie-line L 2 - M2 passes through A, as it should.
515
Bulk and phase compositions(mol%) of feldspars in sam-
Table 2.
ple VSL 522
VSL 522 Ab Or An Cn
Alkali feldspar A 23.3 72.9 3.1 0.7
Plagioclase P 79.9 1.8 18.2
LameltaeLz 79.8 0.9 19.3 -
Matrix M2 13.4 84.8 0.3 1.5
Lamellae L3 88-90 7-8 3-4 -
Matrix M3 9.5 90.3 0.0 1.7
Note: Notations A, P, L, M refer to Fig. 2. Composition L~ has
been determined on sample VSL 510 equivalent to VSL 522
using transmissionelectron microscopyequipped with an energy
dispersive analysis system. Otherwise, an electron microprobe
(wavelengthdispersiveanalysis)has been used on VSL 522
The lamellae Lz and the plagioclase P have the same
An content within error limits (Fig. 2 a, b; Table 2). This
is true not only for the sample under discussion, but
for all feldspar pairs we have investigated (Evangelakak-
is et al., in press). One possible explanation is the follow-
ing: If exsolution of the plagioclase lamellae Lo occurs
at a low degree of supersaturation, Lo and Po will have
similar compositions. As temperature decreases, the An
content of the lamellae also should decrease (e.g. Fuhr-
man and Lindsley 1988, Fig. 2). At the same time, how-
ever, the alkali feldspar changes its composition from
Ao towards A. The plagioclase that would be in equilib-
rium with A would be more An rich. As a result, the
two effects largely cancel themselves. Between L1 and
L2 the An content will be constant anyway, because
the A1-Si interchange has ceased and only the K - N a
interchange continues.
Furthermore, it is seen from Fig. 2a, b that the Or
content of P is slightly larger than that of L> This is
true for most feldspar pairs investigated. It is to be ex-
pected, because the intercrystalline K - N a exchange be-
tween plagioclase and alkali feldspar should cease at a
higher temperature than the intracrystalline K - N a ex-
change between lamellae and matrix.
At composition Lz the lamellae are virtually depleted
in K. Because then no further K - N a exchange with
the matrix is possible, it becomes supersaturated with
Na. The supersaturation is decreased by two exsolution
processes.
Firstly, we sometimes observe Ab-rich rims around
the plagioclase lamellae L> Secondly, between the lamel-
lae we always observe exsolution of film lamellae and
fine-scale spindles (La in Fig. 2c and Table 2). Both are
coherently intergrown with their matrix (M3) (Evange-
lakakis et al., in press). Due to the nature of the inter-
growth, (A1,Si)-O bonds need not be broken during
nucleation and growth. Therefore, if at low temperatures
and dry conditions a final exsolution event occurs, it
is more likely for kinetic reasons to be coherent rather
than incoherent.
Estimation of closure temperatures
We may roughly estimate from existing interdiffusion
data the closure temperature Tc for the A1-Si inter-
516
change between L~ and M~. Following Dodson (1973,
1986)
E,/R
Tc { R.A.Do.T~.2], (12)
In \ - L2 . E~.dT/dt ]
where Do is the frequency factor and E,, is the activation
energy in the Arrhenius equation for diffusion, R is the
gas constant, dT/dt the rock cooling rate, A a geometri-
cal constant (8.7 for volume diffusion from a plane
sheet), and L is a characteristic diffusion distance (e.g.
half width of a plane sheet).
The cooling rate of Sri Lankan rocks can be estimated
from age determinations by H61zl et al. (1991). The cli-
max of metamorphism at 850-900 ~ C, 8-10 kbar (Faul-
haber and Raith 1991; Schumacher and Faulhaber, in
press) is dated at 610 Ma, while cooling ages of biotites
(Tc=350 ~ C-300 ~ C) gave 450 Ma. Thus d T / d t ~ -
3.5 ~ C/Ma on average.
Values for Do and Eo are more difficult to choose.
From homogenization experiments on a lamellar per-
isterite (dry heating in air at 1100~ C, 1 bar) Yund (1986)
estimated D < 1.8.10-21 m2/s for the NaSi-CaA1 inter-
diffusion. Yund and Tullis (1980) report Ea = 365 kJ/mol
as the activation energy for disordering A1,Si by dry
heating of albite. From the piston-cylinder experiments
of Goldsmith (1987), who performed ordering and disor-
dering experiments on albite using a NaC1 cell, Graham
and Elphick (1991) deduced E,=385kJ/mo1. Using
/3(1100 ~ C)=1.8.10 -21 mZ/s and Ea=375 kJ/mol we
get Do = 3.3- 10-8 mZ/s. Let us approximate the perthitic
alkali feldspar by a regular sequence of plagioclase la-
mellae and Or-rich matrix. For a lamellar distance of
2L = 20 l-tin, for example, interdiffusion of C a A I - KSi
would freeze in at T~.=825~ assuming /)(CaA1-
NaSi) =/3 (CaA1- KSi).
This temperature is high. We find in Sri Lankan rocks
coexisting feldspar pairs that have grown from late mo-
bilisate melts at temperatures as low as 750-700 ~ C (Voll
et al., in press). They later unmixed to become perthites.
A1-Si interdiffusion, therefore, persisted to tempera-
tures lower than 825~ C.
Recently, Baschek and Johannes (1992) homogenized
lamellar peristerites at 900 ~ C, 10 kbar at various water
actlvmes an o. For an o = 0 they found D(900 C ) = 1 .
9 , . -- O
10 2t m2/s.ZAssuming2as above Ea= 375 kJ/mol we get
Do= 5-10 -5 mZ/s. Now T c is much lower: 665~ for
2L = 20 gm, or 760~ C for 2L = 200 gm. These tempera-
tures are in better accordance with observation9 It should
be noted, however, that the results of Baschek and Jo-
hannes (1992) disagree with Liu and Yund (1992). From
hydrothermal homogenization experiments on a per-
isterite (90~1100 ~ C, 15 kbar, 0.6-2.5 wt% H;O) Liu
and Yund report Do = 3' 10-8 mZ/s and E, = 303 kJ/mol.
/3 calculated for 900 ~ C (1.10-21 m2/s) is virtually ident-
ical to the value of Baschek and Johannes (1992) at
aH_o = 0. Clearly, this needs an interpretation. It appears
that it is difficult at present to estimate reliably closure
temperatures for A1--Si exchange in perthites.
Application of a revised two-feldspar
geothermometer routine
If our interpretation of the exchange and exsolution his-
tory of feldspar pairs from Sri Lankan and other high-
grade rocks is correct, two-feldspar geothermometers us-
ing uncorrected integrated feldspar compositions (e.g.
A and P in Fig. 2a) will produce erroneous results. How-
ever, it is possible to find the minimum temperature,
at which the alkali feldspar and plagioclase were at equi-
librium, by reversing - at constant An contents - the
assumed retrograde intercrystalline K - N a exchange.
We modified the Fuhrman and Lindsley (1988) routine
for this task. The programme shifts the Ab,Or contents
of both alkali feldspar and plagioclase at constant An
contents until the equilibrium tie-line and the common
isotherm are found (e.g. A 0 - P o in Fig. 2a).
The temperatures TAb, Tot, and TAo, which result
from equations (1)--(3), respectively, are vastly different,
when the original uncorrected compositions are kept
constant, with TA, being high and Tot being low [Ta-
ble 1, "Composition (1)"]. When allowing for 2 tool%
analytical error, the thermometer routine systematically
increases Or in the plagioclase by the maximum 2 tool%
and decreases An in the alkali feldspar, so that Tot is
raised and TA, is lowered. Though the temperatures be-
come more similar, they are still clearly discordant [Ta-
ble 1, "Composition (2)"]. On the other hand, when
the An contents of the plagioclase and alkali feldspar
are kept constant and the Ab,Or contents are allowed
to shift in order to find the common isotherm, the three
temperatures become necessarily equal [Table 1, "Com-
position (EG), (FL)", Fig. 3].
We have applied the geothermometer routine to the
Sri Lankan feldspars using the original Margules param-
eters of Fuhrman and Lindsley (1988) as well as those
of Elkins and Grove (1990). On average, the tempera-
tures T(FL) and T(EG) differ by 40-50 ~ C, with T(FL) <
An
Ab zo 4o 6o so Or
Fig. 3. Coexistingplagioclase alkalifeldspar pairs with composi-
tions resulting from the suggested correction procedure [Table 1,
Composition (EG)]. Miscibilitygap as in Fig. 2

T(EG). Temperatures calculated from Margules parame-
ters of Lindsley and Neksavil (1989) were slightly lower
than T(FL). We cannot provide much evidence for the
temperatures to be preferred and therefore give both
T(FL) and T(EG) in Table 1. The difference between
these temperatures is, of course, not related to the sug-
gested correction procedure, but reflects different experi-
mental data sets.
Voll et al. (in press) relate the obtained ~temperatures
to the geologic occurrence and the deformationN history
of the feldspars. They conclude that there is a very good
correlation between tectonic setting and two-feldspar
temperatures. They also compare several temperatures
derived from garnet-pyroxene pairs occurring together
with feldspars in the same thin sections and find a close
correspondence. Moreover, Schumacher and Faulhaber
(in press) report numerous garnet-pyroxene tempera-
tures scattered all over the high-grade rocks of Sri Lan-
ka. Although their temperatures were not derived from
the same hand specimens as were the two-feldspar tem-
peratures, they were determined from rocks of similar
tectonic settings. The agreement between their results
and ours is remarkable.
Discussion
The temperatures found from the corrected composi-
tions represent the closure temperatures To(A1-Si) for
the intercrystalline A 1 - S i exchange, below which the
feldspar pair is no longer an equilibrium pair. For feld-
spars that coexisted in equilibrium at the metamorphic
peak, To(A1-Si) gives the minimal peak temperature,
which should be close to the true peak temperature, be-
cause the intercrystalline A 1 - S i exchangc is expected
to cease early in the cooling history. Tc(A1-Si ) also
represents the maximum temperature of exsolution.
The temperatures T~(A1-Si) depend critically on the
integrated An content of the alkali feldspar. The alkali
feldspar may be zoned with respect to the distribution
of the plagioclase lamellae, which tend to be concentrat-
ed in the core. In such cases integrated core compositions
should be used. Because the slope of the ternary feldspar
solvus is very steep near the A b - O r join, a large error
in T~(A1- Si) is caused by a small error in the integrated
An content. We systematically varied the An content
within analytical uncertainty to obtain its effect on re-
sulting temperatures and found that a realistic estimate
of the error is about _+50~ C. On the other hand,
T~(AI-Si) is insensitive to the Or content of the alkali
feldspar if Or is larger than ~ 50 tool%, because the
solvus isotherms are about parallel to the A b - O r join
at Or-rich compositions.
During the correction procedure the uncorrected
compositions should shift in opposite directions, the pla-
gioclase " g a i n i n g " Or, the alkali feldspar " l o s i n g " Or.
This expectation is always fulfilled for the plagioclases.
Their compositions, when plotted in the ternary phase
diagram (Figs. 1, 3), shift in a direction that is about
normal to the isotherms. For the alkali feldspars the
expectation is mostly fulfilled when Fuhrman and Linds-
517
ley's (1988) Margules parameters are used, but is fre-
quently not fulfilled when Elkins and Grove's (1990)
parameters are employed. However, here the shift is al-
most parallel to the isotherms. Therefore, a small differ-
ence in position and curvature between the modelled
and the true solvus has a large effect.
The suggested correction procedure should not be ap-
plied to the non-equilibrium pair L 2 - M 2 (to find the
corrected compositions L1 and M1, Fig. 2b). This at-
tempt would probably face the difficulty that the mo-
delled solvus deviates too much from the true solvus
at the relatively low temperatures, at which L1 and M1
coexist.
From our experience with the Sri Lankan feldspars
we feel that the proposed correction procedure is valid
and that it is able to closely recover peak metamorphic
conditions. Compared to other geothermometers it has
the advantage of being rather insensitive to a pressure
estimate (e.g. Seck 1971b), because Margules volume
parameters indicate that the height of the ternary solvus
only weakly depends on pressure.
Acknowledgements. This work was supported by the Dcutsche
Forschungsgemeinschaft in the Priority Programme "Stoffbestand,
Struktur und Entwicklung der Unterkruste", which is gratefully
acknowledged. The manuscript benefited much from thorough re-
view by T.L. Grove, Cambridge, Mass.; D.H. Lindsley, Stony
Brook, N.Y.; D. Perkins, Grand Forks, N.D.; A. Seck, K61n;
and R.A. Yund, Providence, R.I.. We thank G. yon C611nfor care-
fully typing the manuscript and C. Middendorf for the photograph-
ic work.
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