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Supporting Information: Abstract We present a new method for estimating the composition of water-bearing primary arc basalt
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and its source mantle conditions. The PRIMACALC2 model uses a thermodynamic fractional crystallization
Supporting Information S1-S3
model COMAGMAT3.72 and runs with an Excel macro to examine the mantle equilibrium and trace element
calculations of a primary basalt. COMAGMAT3.72 calculates magma fractionation in 0–10 kb at various com-
Correspondence to:
J.-I. Kimura, positions, pressure, oxygen fugacity, and water content, but is only applicable for forward calculations. PRI-
jkimura@jamstec.go.jp MACALC2 first calculates the provisional composition of a primary basalt from an observed magma. The
basalt composition is then calculated by COMAGMAT3.72 for crystallization. Differences in elemental con-
Citation: centrations between observed and the closest-match calculated magmas are then adjusted in the primary
Kimura, J.-I., and A. A. Ariskin (2014),
basalt. Further iteration continues until the calculated magma composition converges with the observed
Calculation of water-bearing primary
basalt and estimation of source mantle magma, resulting in the primary basalt composition. Once the fitting is satisfied, back calculations of trace
conditions beneath arcs: PRIMACALC2 elements are made using stepwise addition of fractionated minerals. Mantle equilibrium of the primary
model for WINDOWS, Geochem.
basalt is tested using the Fo-NiO relationship of olivine in equilibrium with the primary basalt, and thus with
Geophys. Geosyst., 15, 1494–1514,
doi:10.1002/2014GC005329. the source mantle. Source mantle pressure, temperature, and degree of melting are estimated using petro-
genetic grids based on experimental data obtained in anhydrous systems. Mantle melting temperature in a
Received 7 MAR 2014 hydrous system is computed by adjusting T with a parameterization for a water-bearing system. PRIMA-
Accepted 7 APR 2014 CALC2 can be used either in dry or water-bearing arc magmas and is also applicable to mid-ocean ridge
Accepted article online 10 APR 2014 basalts and nonalkalic ocean island basalts.
Published online 29 APR 2014
1. Introduction
Because erupted magmas have been subjected to fractional crystallization and assimilation, the estimation
of chemical composition of primary magmas is important for examining source mantle processes. However,
even if a subordinate role of crustal assimilation is assumed, the reconstruction of fractionation conditions
of a primary magma is a complex procedure because of the various possible crystallization paths within
intracrustal magma chamber systems [Almeev et al., 2013a, 2013b; Grove and Kinzler, 1986].
Olivine maximum fractionation calculations have been used in the estimation of primary basalts [Danyush-
evsky et al., 2000; Herzberg and Asimow, 2008; Herzberg et al., 2007] and have been proven to be useful for
less-fractionated magmas. In many arc lavas, however, the role of fractionation is generally large because of
the existence of a thick sialic crust and because fractionation includes crystals other than olivine [Grove and
Baker, 1984; Tatsumi and Suzuki, 2009].
Once a fractionating magma reaches multiple saturation and begins to move along a cotectic, it is not pos-
sible to trace which side of the cotectic the magma originated from, nor where it joined the cotectic [e.g.,
Ariskin et al., 1993]. Moreover, arc magmas contain varying amounts of water [Plank et al., 2013] and volatiles
[Wallace, 2005], and water in particular affects the liquid line of descent (LLD) [Almeev et al., 2013a, 2013b;
Sisson and Grove, 1993]. Therefore, back calculation models are not able to identify the unique primary
magma composition that fractionated to an observed composition [Danyushevsky and Plecov, 2011], and
only a family of plausible candidates can be identified.
Although difficult to obtain, a reasonable estimate of a primary basalt composition is important, since it ena-
bles better examination of the genetic conditions of the basalt in the source mantle using (1) a petrogenetic
grid for mantle melting (e.g., PRIMELT2 model) [Herzberg and Asimow, 2008; Herzberg et al., 2007; Niu, 1997;
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Geochemistry, Geophysics, Geosystems 10.1002/2014GC005329
Till et al., 2012]; (2) thermodynamic phase equilibria model calculations (e.g., pMELTS) [Asimow et al., 2004;
Ghiorso et al., 2002; Kuritani et al., 2014b]; or (3) forward mass balance calculations (e.g., Arc Basalt Simulator
(ABS) 3 and 4 models) [Kimura et al., 2009, 2010, 2006].
To achieve the aforementioned goal, we developed an iterative algorithm designed to calculate the compo-
sition of primary basalt in relation to 10 major and 26 trace elements from basalt to basaltic andesite arc
magmas, mid-ocean ridge magmas, and subalkalic ocean island magmas. PRIMACALC version 2 (hereafter
referred to as PRIMACALC2) is an Excel based WINDOWS application software which allows estimates of a
primary basalt using back calculations along the fractional crystallization path of a magma and the source
mantle conditions in a dry to wet system. In this paper, we describe the calculation scheme within PRIMA-
CALC2 and the applications of the model.
The PRIMACALC2 program package, containing a PRIMACALC_2.00(COM3.72).xls Excel spreadsheet and a
COMAGMAT folder containing COMAGMAT3.72 FORTRAN code and relevant files, can be found with a brief
installation guide in supporting information S1. We have confirmed that PRIMACALC2 runs with WINDOWS
XP, 7 and 8, and with Excel 2003, 2007, and 2013 using a 32 bit mode. A Mac PC can also run PRIMACALC2
using WINDOWS OS mode. For 64 bit Excel users, PRIMACALC_2.00(COM3.72)w64.xls is available upon
request to the corresponding author of this study.
2. Calculation Scheme
Figure 1 shows a screen shot of PRIMACALC2 with the calculation flow chart. PRIMACALC2 is built on an
Excel spreadsheet consisting of CONTROL_PANEL, PRIMACALC1, PRIMELT2_MOD, PLOT, COM_Result,
TRACECALC, PRIMACOT, TRIPLOT, CMAS_CALC, PREMELT2_MOD2, Katz, and INPUT1_file Worksheets (see
PRIMACALC_2.00(COM3.72).xls in supporting information S1). In this chapter, we use a step-by-step expla-
nation of the method used by PRIMACALC2 to calculate the composition of a primary basalt.
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PRIMACALC ver.2.00 calculation flow (bottom) with corresponding screen panel (upper)
PRIMACALC_2.00_20131224 CODE INPUT COMAGMAT 3.72 CODE EXAMPLE Powered by COMAGMAT_3.72 and PRIMELT2, programed by JIK OL to CS-MS-A
50
CLYSTALIZATION MODE FRC 1 1: FRC Default Element INPUT NORM COM372 MODEL MODEL OUTPUT A
PRESSURE_CONDITION ISO 1 1: ISO 2: DEC Isobaric/Decomp. Sample VCH-02 VCH-02 Cs/Condi. OL.max P.Bas_1 P.Bas_2 Recalc.
45 Next Cs Sample DIFF(T-C) RND_TXT
SET_SET P_MAX P [kbar] 5 5 3 10 <10kb SiO2 47.63 48.29 48.10 47.78 47.22 47.22 48.29 47.32 SiO2 0.094 47.22
40
SET_MAX P_STEP P [kbar] 11 11 11 0 .1 TiO2 1.15 1.16 1.15 1.08 1.01 1.01 1.16 1.01 TiO2 0.006 1.01 A
SET_NUL/ MIN P [kbar] 0 0 0 2.5 Al2O3 17.60 17.84 17.73 16.49 15.48 15.48 35
17.84 15.54 Al2O3 0.056 15.48 Y2
EDGE
MINERAL_CHEMISTRY 3 Unused FeO 9.09 9.21 9.60 9.37 9.57 9.57 9.21
30 9.37 FeO -0.195 9.57
DiEnPy
LOW-Ca_Px_MODEL 1 1 0: PIG 1: OPX Default MnO 0.17 0.17 0.16 0.17 0.17 0.17 0.17 0.17 MnO 0.004 0.17 COT3
25 Py
NUMBER OF COMPOSITION 1 Unused MgO 8.54 8.66 8.65 11.74 13.80 13.80 8.66 13.80 MgO 0.003 13.80 COT4
OXYGEN_SYSTEM
OXYGEN_BUFFER_CONDI
OPE
CON
1
1
3
1: OPE
1: CON
Default
Default
CaO
Na2O
110.22
2.72
10.36
2.76
10.33
2.73
29.59
2.55
69.00
2.40
89.00
2.40
10.36
20
2.76
15
9.02
2.41
CaO
Na2O
0.015
0.014
9.00
2.40
COT5
COT6
COT7
INIT_OXYGEN_BUFFER NNO 2 1: QFM 2: NNO 3: IW 4: HM K2O 1.31 1.33 1.32 1.23 1.15 1.15 1.33 1.15 K2O 0.002 1.15 TD
LSiPy
LOG_UNIT_SHIFT_OXBUFFER 0 0 P2O5 0.23 0.23 0.23 - 0.20 0.20 0.23
10 0.20 P2O5 0.001 0.20 Pxs
FINAL_OXYGEN_BUFFER (VAR) Unused PRESS for START SUM 99.55 100.00 100.00 100.00 100.00 100.00 0.00 Thermal devide
0.00 Cr2O3 8.991 0.00
5
XSTALLIZATION_INCRIM.[%] 1 Default COMAGMAT Rb 41.64 41.64 - 38.55 35.16 35.16 0.00 0.00 LOI 9.064 0.00
XSTALLIZATION_RANGE_MAX 75 Default Ba 401.69 401.69 - 371.94 339.19 339.19 0
100.00 100.00 Column 17
CALC. 50 60 70 80 90 100
TEMP_CONVERGENCE 0.5 Default Th 2.58 2.58 - 2.39 2.18 2.18 CS Di En(MS)
PHASE_COMP[mol%]
#
0.25
0
Default
Unused 3
PRESS for START
PMC2_CALC. CONDITIONS
U
Nb
0.72
2.68
0.72
2.68
-
-
0.67
2.48
0.61
2.27
0.61
2.27
100
7 AN An
FIT
H2O_IN_PRIMARY_MELT[wt.%] 2 2 <7wt.% 2 Precision (Diff / X) Ta 0.16 0.16 - 0.14 0.13 0.13 90
EDGE
OUTPUT_FILE_NAME 00000001 Default 4 Iteration run (no.#) K 10858 10858 - 10054 9170 9170 TD
80 0GPa
MAJOR_COMP 47.13 1.00 15. Excel PMC2_MANTLE COMP. La 12.09 12.09 - 11.20 10.23 10.23 1GPa
TRACE_COMP (DUMMY) 0.0000 Unused 90.0 PMC1_OL.max Fo Ce 27.14 27.14 - 25.13 22.94 22.94 70 2GPa
3GPa
# 0 Unused 8.0 PRIMC mante FeO* Pb 2.55 2.55 - 2.36 2.15 2.15 60 4GPa
# 0 Unused 38.0 PRIMC mantle MgO Pr 3.65 3.65 - 3.38 3.09 3.09 5GPa
50 2 6GPa
# Null PMC2_OLIVINE D(Ni) Sr 608 608 - 563 514 514 F=0.0
F0.0
DO NOT ALTER CELL POSITIONS!!! L Li, Metz, Bea, Wang Nd 16.43 16.43 - 15.21 13.88 13.88 P=1 F0.1
40 3 0.1
F0.2
Ni (wt.%) IN OLIVINE INCOMPATIBLE TRACE ELEMENT Sm 4.00 4.00 - 3.71 3.38 3.38 0.2
30 4 F0.3
0.7 100 Zr 95.98 95.98 - 88.87 81.16 81.16 F0.4
5 0.3
Hf 2.54 2.54 - 2.35 2.14 2.14 F0.5
20 6
F0.6
0.6 Eu 1.35 1.35 - 1.25 1.14 1.14 0.4
6
Hz
10 0.6 0.5
Gd 4.16 4.16 - 3.85 3.52 3.52 Gt
4-5
10 PGPa - - 0.05 - 2.4 2.4 20
50 4 An(plag)
5 F%(Herz) - - - - 9 9 10
48 2 H2O*10
46 0 0 %Xfrac. - - - 8.0 17 17 0 %Xtal.
0 5 10 15 0 5 10 15 0 5 10 15 1400 1300 1200 1100 1000
MgO PM - - - - - 38
Figure 1. Schematic calculation flow and screenshot of PRIMACALC2. (1) Input natural magma composition (major element, incompatible trace element, and Ni). (2) First back calculation
to primary basalt at MgO 5 14 wt % by COMAGMAT3.72 fractionation template using a typical arc magma of Tatsumi and Suzuki [2009] calculated at 3 kb and a given H2O. (3) Forward
crystallization calculation conditions in COMAGMAT3.72, given H2O, P, and fO2 used with the calculated primary basalt in step 2. (4) Elemental differences found between the closest-
match calculation result and the natural magma, and the adjusted composition of primary basalt. (5) Steps 3 and 4 are automatically repeated until the solution is stabilized and the pri-
mary basalt composition is calculated. (6) Repeat steps 3–5 by checking that the NiO in the olivine within the primary magma satisfies the mantle-olivine Ni-Fo array of mantle equilib-
rium. (7) Calculate mantle P, T, and F in dry conditions using PRIMELT2; source mantle MgO is also obtained iteratively. (8) Recalculate T in the water-bearing mantle iteratively by Katz
et al. [2003] for a given H2O in the primary basalt, with T(dry), P, and F in the mantle. The calculations give chemical compositions of the primary basalt (10 major and 27 trace elements);
conditions of magma fractionation (given initial H2O, P, and fO2): % crystallization, mineral mode, mineral composition, major element, and H2O content in the fractionated magmas
with Fe21/Fe*; and conditions of mantle for the primary basalt (given H2O): P, T, and F (wet) conditions of mantle and MgO (fertility) in the source mantle.
which is believed to represent the typical condition of an arc magma chamber [Tatsumi and Suzuki, 2009].
We tested the versatility of the COMAGMAT3.72 thermodynamic model by comparing the model outputs
to the experimental results of Tatsumi and Suzuki [2009], performed under the same P-T-XH2O conditions,
but with a slightly lower fO2 at QFM12 rather than QFM13 used in Tatsumi and Suzuki [2009]. The calcu-
lated LLDs show excellent agreement with those by experiments as shown in Figure 2. The versatility of
COMAGMAT3.72 has also been shown for use with arc magmas in Eastern Kamchatka and for MORB in the
previous studies [Almeev et al., 2012, 2013a, 2013b, 2007, 2008].
Water saturation in a closed magma chamber is considered in COMAGMAT3.72. When the system is water
saturated, excess H2O is isolated as a separate phase and does not affect phase equilibria. Figure 3a shows
an example of 2.5 wt % water in the primary basalt, saturated at MgO 5 5 wt %. No further increase of
H2O is considered. Water content (Figure 3a), melt compositions (Figure 3b), mineral compositions (Figure
3c), proportions of the fractionated minerals (Figure 3e), and magmatic temperature T, fO2, and Fe21/Fe*
(total Fe as Fe*) (Figure 3f) are calculated for each 0.5 wt % incremental step of MgO in the host melt. The
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3.5 16
FeO/MgO FeO
3 14
TH CA
12
2.5
10
2
8
1.5
6
1
4
0.5 Provisional “primary basalt” 2
SiO2 SiO2
0 0
45 50 55 60 65 70 75 45 50 55 60 65 70 75
1.8 16
1.6
TiO2 MgO Numbers are water content
14
COM_0.0
1.4 12 COM_0.5 TS09_0.5
1.2 COM_1.0 TS09_1.0
10
1 COM_1.5 TS09_1.5
8 COM_2.0
0.8
6 COM_2.5 TS09_2.5
0.6
TS09_3.0
0.4 4
0.2 2
0
SiO2 0
SiO2
45 50 55 60 65 70 75 45 50 55 60 65 70 75
20 16
18
Al2O3 CaO
14
16
12
14
12 10
10 8
Lines from COMAGMAT3.72
8 6
dots from experiments by
6 Tatsumi & Suziki (2009)
4
4
2 2
0
SiO2 0
SiO2
45 50 55 60 65 70 75 45 50 55 60 65 70 75
Figure 2. Comparisons of liquid lines of descent of a typical arc basalt with different water content between COMAGMAT3.72 model calcu-
lations and experimental results by Tatsumi and Suzuki [2009]. Numbers with COM and TS09 show H2O contents in the COMAGMAT3.72
and experimental systems, respectively. TH (tholeiitic) and CA (cacl-alkaline) boundary from Miyashiro [1974].
PRIMACALC1 Worksheet includes the calculated results of LLD with initial values of H2O 5 0–2.5 wt % in
3.0–14.5 wt % MgO. All the data are stored in lookup tables in the cell area $AL$788–$DC$1412 for minerals,
and in $CD$1–$DE$784 for melts in the PRIMACALC1 Worksheet. With the data table, back calculations of a
fractionated magma in the range 3.0–14.0 wt % MgO are available.
The first back calculation requires H2O wt % to be present in the primary magma because the initial water
content largely affects the LLDs, and thus the fractionation sequence (Figures 2 and 3a) [Grove and Baker,
1984; Tatsumi and Suzuki, 2009]. Cell $C$20 in the CONTROL_PANEL Worksheet defines initial H2O as user
input. The model LLD templates are for the H2O 5 0–2.5 wt % range, and any excess H2O is then forced to
be set at 2.5 wt % in PRIMACALC1. Note that PRIMACALC2 accepts up to 7 wt % water in the starting com-
position of a primary basalt, but the first back calculations only use values up to 2.5 wt %. More water is
valid in the second step iteration run, and the first step assumption is compensated after the second run
(see section 2.3).
With the given H2O, PRIMACALC1 chooses the designated LLD path and adds equilibrated minerals at a 0.5
wt % MgO step from the natural magma composition, until the bulk rock MgO reaches 14 wt %. Because of
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Geochemistry, Geophysics, Geosystems 10.1002/2014GC005329
&0
H2O &0
6DPSOH
&0
&0 3ULPDU\\\%DV
%DV
Water saturation &0
&0 2/B0D[
&0
&0
&0
&0
&0
&0
&0
&0 Sample/Primitive mantle
&0
a d
*G
6P
7P
+I
3U
6U
=U
(U
'\
5E
%D
7K
1E
7D
/D
&H
3E
1G
(X
7E
+R
<E
/X
.
<
8
&0
MgO
0W
SiO2 Cpx mode (%) 2OLY
6L2 3ODJ
([S &S[
([S 2S[
([S 0HOW
([S
([S ([S
([S ([S
([S
([S
MgO b MgO e
En(Cpx) Temperature (C)
(Q&S[
([S
([S
([S 7&
([S
([S
MgO c MgO f
Figure 3. View of the PRIMACALC1 Worksheet. (a) H2O versus MgO in melt, (b) SiO2 versus MgO in melt, (c) MgO(melt) versus En composition of clinopyroxene, (d) trace element composi-
tions, (e) mineral mode, and (f) magma temperature for both experimental [Tatsumi and Suzuki, 2009] (colored circles) and COMAGMAT3.72 results (lines).
the existing compositional difference between the model basalt and natural magma, it is possible that the
final MgO may not perfectly match MgO 5 14 wt % (see cell area $D$41–$AA$53 in the PRIMACALC1 Work-
sheet). Trace element compositions (Figure 3d) are also back calculated using the addition of minerals in
the cell area $D$55–$AA$80 of PRIMACALC1 Worksheet. For trace element partition coefficients (Ds)
between melts and minerals (see section 2.7). The first estimate of a primary basalt includes the trace ele-
ment composition, but this is only for reference and not used for further calculations. Only the major ele-
ment composition is used for further calculation steps. The PRIMACALC1 results are found in cell area
$D$43–$D$80 in the PRIMACALC1 Worksheet. The results also plot on the INCOMPATIBLE TRACE ELEMENT
panel in the CONTROL_PANEL Worksheet as PMC_1, along with other model results (Figure 1).
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100 0.7
b NiO (wt%) c
90 Oliv
0.6
80 Plag 2nd stage
olivine in
70 Cpx 0.5 pyroxenite
melting
60 Opx
0.4
Mt Mantle
50 olivine
Ilm 0.3 Ni array
40
FIT
30 0.2
Fo(ol)
PB1
20 PERI
An(pl)
0.1 PX
10 PCOT
H2O*10
T (C) Fo PB2
0 %Xtal. 0.0
1400 1300 1200 1100 1000 80 90 100
Figure 4. Calculation results in CONTROL_PANEL Worksheet of PRIMACALC2. (a) Forward fitting calculation results of COMAGMAT3.72
(blue dots) and the best fit result for the calculated primary basalt and magma compositions (red squares), showing a good fit to the target
magma composition (red circle). (b) Fractional crystallization sequence calculated by COMAGMAT3.72 showing mineral assemblage, min-
eral composition, H2O in the melt, and % crystallization (Ol: olivine, Plag: plagioclase, Cpx: clinopyroxene, Opx: orthopyroxne, Mt: magne-
tite, Ilm: ilmenite). (c) Calculated NiO content (wt %) and Fo in olivines in fractionation (yellow circles) and in the primary basalt (orange
square), showing a good fit with the olivine-mantle Ni array (orange parallelogram) [Takahashi, 1986]. Second stage clinopyroxene field
(green square) [Herzberg, 2011] is also shown for a pyroxenite source.
then added to or subtracted from the provisional primary basalt. The new basalt composition is then used
as the new input for the following iteration cycles. These iterations were continued until the natural and the
model magma compositions converge (Figure 4a).
In this iteration, the MgO content of the natural magma (therefore closest-match calculated magma) held
constant, and all the major element composition (including MgO) varied in the primitive basalt. In order to
obtain a better convergence, the subtracted/added element concentrations from/to the primary basalt are
given using half of the difference between the natural and the chosen calculated magmas. This simple
approach prevents an overshoot of the iteration and provides results that are precise enough (e.g., <0.37%
relative difference (%R.D.) in SiO2 and %R.D. < 5% in MgO; see major %R.D. in the CONTROL_PANEL). The
precision of iteration (given by [difference]/X, where X 5 2 defining added/subtracted amounts to 50% of
the R.Ds) and the number of the iteration are set in cells $E$20–$E$21 in the CONTROL_PANEL Worksheet.
Four iteration runs give sufficient convergence when X 5 2.
Figure 4b shows a fractional crystallization sequence including (1) mineral phases (olivine, plagioclase, clino-
pyroxene, orthopyroxene, magnetite, and ilmenite), (2) olivine Fo, (3) plagioclase An, (4) H2O content in
magma, and (5) the fractionated mass of the solid phases plotted against the magmatic temperature (T);
they were all calculated by the last COMAGMAT3.72 iteration run. Two red vertical lines delimit the range of
fractionation between the primary basalt and the target natural magma. This interval is used for back addi-
tion calculations in PRIMACALC2. The diagram is useful for observing which mineral phase(s) is incorporated
in the back calculations, defining whether or not H2O is saturated in the fractionated magma, and defining
the magma temperature in the shallow magma chamber.
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Geochemistry, Geophysics, Geosystems 10.1002/2014GC005329
A full data set of the calculated major element compositions and the mineral mode and compositions are
shown in the COM_Result and the PLOT Worksheets. The calculated major element composition in the
closest-match model magma is given in COM372 Cs/Condi. in cell area $L$2–$L$13 in the CONTROL_PANEL.
Residues between the model and observed magmas are found in $L$216–$L$25. The compositions of
Ni(olivine), Fo(olivine), Mg#(melt), Fe21/Fe*(melt), H2O(melt), and the conditions of T(melt) and P(melt) in the magma
chamber are also in the same column $L$42–$L$50. These provide information related to the equilibrium of
the observed natural magma in the magma chamber conditions. The data are refreshed during iterations
and finally becomes valid after iteration converges.
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IN OLIVINE panels (Figure 1 and supporting information S1). These panels show a primitive mantle (PM)
[Sun and McDonough, 1989] normalized multielement plots of the primary magma and MgO versus NiO
plots of the olivine composition, respectively.
In addition to the PRIMACALC2 results, the olivine maximum fractionation model of PRIMELT2 [Herzberg
and Asimow, 2008; Herzberg et al., 2007] is also applied to the natural magma by using the P, Fe21/Fe*, and
olivine Fo composition for the primary basalt from PRIMACALC2 (see the PRIMELT2_MOD Worksheet). This
also calculates the major and trace element compositions OL.max in the primary basalt for comparison with
those by PRIMACALC1 and P.BAS_1 by PRIMACALC2. The PRIMELT2 results are in cell area $M$3–$M$53
OL.max in the CONTROL_PANEL Worksheet. Ni partitioning in olivine is calculated by Li and Ripley [2010] for
PRIMACALC2, whereas the Beattie et al. [1991] model is used in the PRIMELT2_MOD Worksheet. The differ-
ences between the two models are shown as NiO in olivine calculated for the primary basalts of OL.max
and P.Bas_1.
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Isotherm
2GPa 80
3GPa
70 0.15 1340 C O
b F estimate by Ol-An-Qz (Di) projection for c T estimate by MgO for hydrous magma
hydrous magma
0.5 1600
F(Ol-An-Qz (Di)) y = 0.9769x + 0.0359 y = 1.096x
0.4 1500
F (PRIMELT2)
T (PRIMELT2)
1400
0.3
1300
0.2
1200
0.1 1100
F (experiment) T (experiment)
0.0 1000
0.0 0.1 0.2 0.3 0.4 0.5 1000 1100 1200 1300 1400 1500 1600
Figure 6. (a) Petrogenetic CMAS grid used for P and F estimates; (b) comparison of experimental F and calculated F values hydrous peridotite system; (c) comparison of experimental T
and T from thermometry for hydrous peridotite melts; and (d) the conversion scheme of T(dry) to T(wet) mantle melting. In Figure 6a, Ol-An-Qz (projected from Di) plot is originally from
Herzberg and O’Hara [2002] modified by the authors using additional experimental data from REPL database [Hirschmann et al., 2008], including dry and hydrous (red circles) experi-
ments. Correlations between experimental F values and those calculated by Ol-An-Qz (Di) projection for the hydrous experiments of Hirose and Kawamto [1995] are shown in Figure 6b.
Figure 6c shows T estimates by MgO(melt) by Herzberg and O’Hara [2002] for the same hydrous peridotite melts showing 10% higher T (C) in calculations. Figure 6d shows a schematic
example of T(dry) to T(wet) conversion. T(wet) 5 1240 C is obtained when T(dry) 5 1340 C, F 5 0.1, H2O 5 3 wt %, and P 5 1.5 GPa are known (figure modified from Katz et al. [2003]).
CONTROL_PANEL Worksheet). The estimated P.Bas_1 composition always displays slight discrepancies from
the equilibrium parameters given by the Fe21-Mg relationship at the given P by Ol-An-Qz (Di) (see section
2.8) in the PRIMELT2 algorithm [Herzberg et al., 2007] (see also FeO21 versus MgO plots in the PRIMACOT
Worksheet). PRIMELT2 cautions addition/subtraction of olivine to/from P.Bas_1 and the amounts shown
(see cell $C$11 in PREMELT2_MOD2 Worksheet). To accommodate this problem, PRIMACALC2 has an addi-
tional function that can modify the source mantle FeO and MgO compositions to take the mantle fertility
into account for equilibration [Herzberg and Asimow, 2008; Herzberg et al., 2007]. These mantle compositions
are given in cells $E$24 and $E$25 in the CONTROL_PANEL Worksheet.
FeO in the mantle peridotite is a canonical value and is fairly uniform at 8 wt %, whereas MgO varies from
25 to 50 wt % [Bodinier and Godard, 2003]. We therefore set FeO 5 8 wt % and change values of MgO to
make the equilibration conditions from PRIMELT2 consistent with the primary basalt estimated by PRIMA-
CALC2 P.Bas_1. The automated calculation forces a discrepancy in the Fe21O-MgO equilibria (shown in the
[FeO(wo_Fe31)-MgO] panel in the PRIMACOT Worksheet) during iteration of the VBA run. The renewed
MgO appears in cell $E$25 in the CONTROL_PANEL. The resultant MgO is usually between 25 and 50 wt %,
possibly indicating source heterogeneity. The recalculated primary basalt composition using the new
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Geochemistry, Geophysics, Geosystems 10.1002/2014GC005329
mantle MgO content with a further addition/subtraction of olivine with PRIMELT2 to create a new equilib-
rium is shown by P.Bas_2 in cell area $O$3–$O$53. The original olivine NiO(olivine) and Fo compositions cal-
culated primarily by PRIMELT2 are shown in cells $O$42 and $O$43 for comparison.
For this final calculation, Fo and NiO(olivine) are recalculated using the model of Beattie et al. [1991] and Jones
[1984] of Ni partitioning with the P.Bas_2 composition. The Fo versus NiO composition of the finally equilibrated
olivine for P.Bas_2 and the fractionation-accumulation trajectories of olivine by PRIMELT2 are in the Ni (wt %) in
olivine panel (see the big orange square and the small gray crosses, respectively, in Figure 4c). In many cases,
the Fo and NiO in olivine from the PRIMACALC2 (COMAGMAT3.72 and Li and Ripley [2010] Ni partitioning) in
P.Bas_1 and the PRIMELT2 P.Bas_2 results agree with each other (see the example in Figure 4c).
However, a large discrepancy occurs when, for example, Hawaiian basalts are calculated. The trials show
higher values of NiO (plot in the field of the ‘‘second stage olivine in pyroxenite melting’’ in Figure 4b) by
PRIMELT2, even though the NiO in olivine from PRIMACALC2 falls into the Fo-NiO mantle array. The high
NiO in olivine reproduces the pyroxenite source model proposed by Herzberg [2011]. However, any prob-
lems associated with this are not discussed here because the results for the low-K tholeiitic to medium-K
calc-alkaline arc magmas examined here did not show the problem. A caveat here is that P.Bas_2 uses Fo
and NiO(olivine) from the PRIMELT2 [Beattie et al., 1991; Jones, 1984] model. If a large discrepancy is found in
relation to the results of P.Bas_1 and P.Bas_2 in PRIMALCALC2, the user should note which values are used.
We use the P.Bas_2 model results throughout this paper. Validity of the estimation of source mantle fertility
is examined in section 4.
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20 37 Hakkoda
Eurasia Plate Sannomegata 15 39 26 32 Akitakoma
40˚ 40˚
rc
Kampu 13 50 25 33 Iwate
pa n a
Chokai 9 38
27 Funagata
Japan Sea 20
9 cm/y
NE Ja
17 46 Nasu
14 42 Takahara
arc 20
Pacific Plate
a p an 41 Asama
J 10 35
SW Fuji
35˚ 14 35
22 37
Izu-Oshima 35˚
22 29 Toshima
Niijima 10 32 Udonejima
Subduction vector
Izu-Bonin
arc
depth contour
arc
(10km interval)
yu
Volcanic front
Ry
Figure 7. Locations of examined volcanoes with depth contours of the Pacific Plate slab and the Philippine Sea Plate slab. Red text indi-
cates volcanic front volcanoes while blue text indicates rear-arc volcanoes. Numbers to the right of volcanoes show MgO in the source
mantle (wt %) and numbers to the left show degree of melting of the mantle (F%).
calculations include (1) saving the COMAGMAT3.72 control codes and the major element compositions
from the CONTROL_PANEL in supporting information; (2) running COMAGMAT3.72, which reads the text
files, calculates, and saves the output results in another text file; and (3) reading the output text file and
storing in the COM_Result Worksheet. All processes are coded in the Excel VBA macro. Additional conver-
gent calculations for T(wet) using the Katz Worksheet, and MgO(peridotite) in the mantle using the PRIMELT2_-
MOD2 and PRIMACOT Worksheets (see section 2.8) run with the iteration calculations. The calculation
precision (see section 2.4) and the number of the iteration run are set in cells $E$20 and $E$21 usually two
and four, respectively (see above section 2.4).
3.3. Output
The MgO versus SiO2, MgO versus Al2O3, and MgO versus CaO panels graphically show the fitting results
(see (4) and (5) in Figure 1 and Figure 4a). The mantle equilibrium of the olivines is tested by Ni (wt. %) IN
OLIVINE panel in the CONTROL_PANEL (Figures 1 and 4c), where the users can test the controlling parame-
ters of COMAGMAT3.72 iteratively. The fractionation sequence including the mineral phases and composi-
tions and the fractionated solid and H2O content in the magma plot are shown in one panel (T(C) versus
mineral assemblage/composition/H2O(melt)) (Figures 1 and 4b). Two CMAS plots ((7) in Figure 1) and the
trace multielement plots ((8) in Figure 1) show the calculation results. Finally, users can extract the results
from PRIMACALC2 using the copy function of Excel from the field $I$2–$O$53 of the CONTROL_PANEL.
4. Applications
We evaluate PRIMACALC2 by applying the software program to the Quaternary arc magmas from the Japa-
nese Islands. Figure 7 shows the locations of volcanoes from which the basalts to basaltic andesites exam-
ined in this study were reported. From the Izu collision zone, we examined the N-Izu volcanic front (VF) Izu-
Oshima, Toshima; Udonejima and rear-arc (RA) Niijima lavas [Kimura et al., 2010]; and Fuji [Watanabe et al.,
2006]. From the southern NE Japan arc, we examined Asama [Gust et al., 1997; Kaneko, 1995; Okamoto,
1979], Takahara, and Nasu [Ban et al., 2013] lavas. From the northern NE Japan arc, we examined Funagata
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100 100
90 a b
80
Oliv
70 Plag
Sample / PM
Cpx 10
60
Opx
50 Mt
Ilm
40 FIT
Fo(ol)
30 An(plag) 1
20 H2O x10 Rb Ba Th U Nb Ta K La CePb Pr Sr NdSm Zr Hf EuGd Tb Dy Y Ho Er TmYb Lu
%Xtal.
10
0 Sample Ol max. P.Bas_1 P.Bas_2
1300 1250 1200 1150 1100 1050 1000
0
100 100
90 c d
80
Oliv
70
Sample / PM
Plag
60 Cpx
Opx
50 Mt
Ilm 10
40 FIT
Fo(ol)
30 An(plag)
20 H2O x10
%Xtal.
10
0 Sample Ol max. P.Bas_1 P.Bas_2
1350 1300 1250 1200 1150 1100 1050 1000 Rb Ba Th U Nb Ta K La CePb Pr Sr NdSm Zr Hf EuGd Tb Dy Y Ho Er TmYb Lu
1
Figure 8. (a, b) Fractional crystallization sequence and (b, d) trace element compositions of Izu-Oshima and Chokai basalts for observed (sample) and primary basalts estimated by oli-
vine maximum fractionation model (Ol max.) and PRIMACALC2 (P.Bas_1 and P.Bas_2). Note that the effects of plagioclase and clinopyroxene fractionation along with olivine fractionation
are shown by lower REE and higher Sr contents in P.Bas_2 in the Izu-Oshima basalt.
[Kimura and Yoshida, 2006], Iwate [Kuritani et al., 2014a], Hachmantai [Ban et al., 2013], Akitakoma [Ban et al.,
2013], and Hakkoda and Osore [Ban et al., 2013] lavas. From the NE Japan rear-arc, we examined Sannome-
gata [Kuritani et al., 2014b], Kampu [Ban et al., 2013], and Chokai [Kimura and Yoshida, 2006]. Low-K tholeiitic
basalt to basaltic andesite were inferred from lower crustal amphibolite melts at Zao [Tatsumi et al., 2008]
and Azuma [Takahashi et al., 2012] volcanoes, and lavas with significant crustal assimilation such as Haruna
volcano [Kobayashi and Nakamura, 2001] were omitted from the examinations.
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cases, the initial water content was considered not to be a significant constraint, and the magma chamber
P was considered to be the fundamental control.
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Geochemistry, Geophysics, Geosystems 10.1002/2014GC005329
fractionation. In the case of the Sannomegata basalt, the water content in the primary basalt is set at 4 wt
% and the magma chamber pressure at 1 GPa in PRIMACALC2 (supporting information S2) which is required
to satisfy NiO-Fo mantle equilibration of olivine.
Although water was estimated at 7 wt % in the primary Sannomegata basalt using the thermodynamic
phase equilibria [Kuritani et al., 2014b] and at 4–8 wt % using the trace element mass balance by ABS4
[Kimura and Nakajima, 2013], the water content estimated by PRIMACALC2 was not more than 5 wt %.
Water content in the fractionated magmas increased dramatically to >10 wt % after the onset of clinopyr-
oxene in a deep closed magma chamber for the Sannomegata basalt (Figure 8c). There are, however, large
errors in the COMAGMAT3.72 calculations, and thus the effects of water on crystal fractionation should be
investigated further, but it is worth noting that the fractional crystallization sequence in the crust should
control water by means of the emplacement depth of the magma chamber. COMAGMAT3.72 could be used
to explore such an effect by comparison of a crystal fractionation sequence to the observed magmas
[Almeev et al., 2013a, 2013b, 2007]. PRIMACALC2 output reflected the model characteristics and enabled
using these to constrain the mantle to crustal processes. But, as has been shown in previous work, individ-
ual magma chamber processes should be examined in detail using petrography, petrology, and geochemis-
try [Kobayashi and Nakamura, 2001; Takahashi et al., 2012; Tatsumi and Suzuki, 2009].
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Geochemistry, Geophysics, Geosystems 10.1002/2014GC005329
30 30 N-Izu VF
N-Izu RA
a b Fuji
NE Japan NVF
25 High 25 NE Japan SVF
NE Japan RA
20 20
F (%)
F (%)
15 15
10 10
5 5
DMM
Fertile Depleted
Low
0 0
1180 1200 1220 1240 1260 1280 1300 1320 1340 25 30 35 40 45 50 55
Temperature (C) MgO in mantle (wt%)
2.4
RA VF
2.2
c High
Depth
d Arc crust
(km) Moho
2 Partial melting
50
3% 5%
1.8 1200 Partial
(C) melting
P (GPa)
ss
n
ce
tio
Slab fluid
Ex
ra
1.6
yd
n
tio
H
ra
1350
ss
Ex ion
yd
ce
eh
100
t
ra
1.4
D
yd
Slab melt
eh
D
1.2
n
tio
g
tin
ra
el
yd
m
eh
ab
1
D
Sl
Low 150 t
us
0.8
cr
Temperature (C)
O
Figure 9. Intensive-extensive parameters estimated by PRIMACALC2 for N-Izu, southern NE Japan, and northern NE Japan arcs. (a) Mantle
melting temperature (T) versus degree of partial melting (F). Thick lines in light red and blue show the average of volcanic front and rear-
arc primary basalts, respectively. (b) MgO in the source mantle versus degree of melting. (c) Melting pressure (P) versus temperature. (d)
Across arc schematic cross section of mantle wedge. Black rectangles show P and T ranges of primary basalt segregation estimated by PRI-
MACALC2. Overall positive correlation between P and T suggests geotherm of the melting zone shown as 1200 and 1350 C contour lines.
For slab dehydration and melting conditions, see Kimura and Nakajima [2013].
source most significantly affects the T estimate, with subordinate effects to P and F (Figure 6). Therefore,
the conclusions given here are robust. The mantle P-T structure has been inferred by ABS models [Kimura
and Yoshida, 2006; Kimura and Nakajima, 2013; Kimura et al., 2009, 2010] and thermodynamic phase equili-
bria [Kuritani et al., 2014a, 2014b]. PRIMACALC2 shows similar results, with a completely different model
scheme.
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Geochemistry, Geophysics, Geosystems 10.1002/2014GC005329
and crustal plumbing system must represent a mixture of melts derived from a range of sources. The appa-
rent source composition derived from PRIMACALC2 must therefore represent some kind of mixture. This
implies that the spectrum of heterogeneity is even larger than that inferred, since mixing presumably
reduces the range of extremes. If so, the wide variation found between T-F-MgO would relate to the thermal
gradient in the mantle that forms greater F in the high T region, leaving a high MgO residue in the source.
The P estimate for Fuji is fairly constant at P 5 1.4–1.6 GPa (Figure 9c), and the Sr-Nd-Pb isotope composi-
tions are fairly uniform [Watanabe et al., 2006]. Thus the thermal heterogeneity, if persistent, is significant
even in the root of one single volcano.
The basalts from the southern NE Japan VF, including Asama, showed relatively low F and T, with depleted
sources (Figures 9a and 9b). There was a considerable overlap between the southern and northern VF in NE
Japan. However, the northern VF basalts tended to show higher F and T in comparison to N-Izu VF but with
similar depletion in the source (Figures 9a and 9b). The RA basalts from northern NE Japan has a higher
mantle T and F, with an intermediate mantle depletion similar to the depleted MORB source mantle [Work-
man and Hart, 2005] (Figure 9c).
Spatial distributions of average values of MgO and F in the source mantle are shown in Figure 6. The upper
mantle beneath the northern NE Japan VF is relatively fertile (27–37 wt %), but in southern NE Japan it is
depleted (41–46 wt % MgO). The mantle becomes fertile again in N-Izu VF (29–35 wt % MgO) (Figure 6). In
contrast, the RA mantle consistently shows intermediate depletion (32–39 wt % MgO) close to the DMM
value (35 wt % MgO), with the exception of the very depleted mantle (50 wt % MgO) beneath Kampu vol-
cano (Figure 6). F relates to T and P and may represent the production rate of the mantle. F is high (20%–
26%) in northern NE Japan, low (14%–20%) in the southern NE Japan VF, and remains lower (14%–22%) in
the VF of the N-Izu arc (Figure 6). F is low (9%–15%) in the NE Japan RA and remains low and constant
(10%) through Fuji to the N-Izu RA. All of these observations suggest RA characteristics of Fuji primary
basalt similar to those noted in a previous report [Tani et al., 2011].
The greater mantle depletion, and the lower degree of melting beneath the southern NE Japan VF, could
be related to the overlap of the Philippine Sea Plate slab onto the Pacific Plate slab that promoted depletion
of the mantle by a greater water supply to the source mantle [Nakamura and Iwamori, 2009; Nakamura
et al., 2008] and a poor development of the mantle wedge corner flow. Alternatively, intensive magma pro-
duction in the middle Miocene fore arc, due to an extremely high temperature mantle during the opening
of the Sea of Japan, depleted the subarc mantle beneath the southern NE Japan VF [Yamamoto and Hoang,
2009].
As shown above, PRIMACALC2 is a useful petrological tool for estimating primary basalt compositions,
including those of major/trace elements and water contents, as well as the P, T, F, and MgO source mantle
conditions, which generate the tholeiitic low-K to calc-alkaline medium-K primary basalts. Moreover, a com-
bined use with ABS models [Kimura and Nakajima, 2013; Kimura et al., 2009, 2010] provides (1) a robust esti-
mate of the primary basalt composition which is immediately used for ABS and (2) a unique test for the
estimates of the source mantle conditions beneath arcs by back calculation modelling. Because COMAG-
MAT3.72, and thus PRIMACALC2, can be applied to dry basalt systems with tholeiitic to mildly alkalic com-
positions, PRIMACALC2 is useful for MORB and some OIB, including those with tholeiitic to transitional
compositions.
5. Summary
We developed a numerical simulation model PRIMACALC2 for estimation of hydrous primary magma com-
positions and their genetic conditions in subduction zones. PRIMACALC2 uses COMAGMAT3.72 for the for-
ward calculation of crystal fractionation of hydrous magma in the intracrustal depth magma chamber at
given P, T, fO2, and H2O conditions, and back calculates major and trace element compositions to a primary
basalt in mantle equilibrium using the NiO-Fo relationship. PRIMACALC2 also calculates the P, T, and F con-
ditions of the source mantle, and the source mantle fertility expressed by MgO. Calculations were applied
to VF and RA basalts and to basaltic andesite magmas from N-Izu, southern NE Japan, and northern NE
Japan arcs. The results argue that the mantle beneath VF is melted at shallow depths (0.8–1.6 GPa), whereas
melting occurs deeper (1.4–2.3 GPa) beneath RA. Although a similar range of melting temperatures was
found beneath VF and RA, higher temperatures were observed from the deeper mantle. These results
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Geochemistry, Geophysics, Geosystems 10.1002/2014GC005329
suggest that the isotherm in the mantle is inclined toward RA, and that a normal mantle geotherm is main-
tained in the upper half of the mantle beneath VF and RA. Water contents of the primary magmas were
constrained by relationships between crystallization conditions and NiO contents in olivine in mantle equi-
librium. Initial H2O in the primary basalt positively correlated with NiO in olivine, whereas the magma cham-
ber P was negatively correlated, thus providing the petrologically useful constraints. Estimated water
contents in the primary magmas were 2–4 wt %, consistent with (or somewhat lower than) previous esti-
mates. Thus, PRIMACALC2 is a new powerful tool for estimation of the conditions and compositions of pri-
mary magmas generated in the arcs, as well as for decoding P, T, F, H2O parameters of their fractionation.
Notation
Important acronyms used in PRIMACALC2 are listed below.
Ni(ol)wt % NiO in olivine.
Fo(ol)% Fo content in olivine.
Mg# Bas Mg# 5 Mg/(Mg1Fe21) molar ratio in basalt.
Fe21/Fe* ferric iron content over total iron in basalt.
H2O(wt %) water content in basalt.
P(COM) magma chamber pressure set for COMAGMAT3.72.
TWC(KAZ) hydrous mantle temperature estimated by Katz et al. [2003].
TDC(Herz) dry mantle temperature estimated by Herzberg et al. [2007].
PGPa(COM/Herz) pressure at magma chamber given for COMAGMAT3.72 and that estimated for source
mantle by Herzberg et al. [2007].
F%(Herz) degree of partial melting estimated by Herzberg et al. [2007].
%Xfrac. total fractionated mineral weight in magma chamber.
MgO PM estimated MgO in the source mantle by Herzberg et al. [2007].
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