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JGR Solid Earth - 2019 - Yang - Using Major Element Logratios To Recognize Compositional Patterns of Basalt Implications
JGR Solid Earth - 2019 - Yang - Using Major Element Logratios To Recognize Compositional Patterns of Basalt Implications
JGR Solid Earth - 2019 - Yang - Using Major Element Logratios To Recognize Compositional Patterns of Basalt Implications
10.1029/2018JB016145
Compositional Patterns of Basalt: Implications
Key Points:
• Major element patterns of
for Source Lithological and Compositional
experimental basaltic melts on
different lithologies are explored
Heterogeneities
using major element logratios
• Several useful logratio‐based
Zong‐Feng Yang1 , Jie Li1, Qing‐Bao Jiang1, Fei Xu2, Shuang‐Yan Guo1, Yue Li1, and Jun Zhang1
chemical markers are proposed to 1
identify source lithology of basalts
State Key Laboratory of Geological Processes and Mineral Resources, China University of Geosciences, Beijing, China,
2
• The uncertainties of traditional Institute of Crustal Dynamics China Earthquake Administration, Beijing, China
chemical markers and the
advantages of the logratio‐based
markers are discussed Abstract Understanding the source lithology of basalts can greatly impact our understanding of
magmatic processes, which can help us gain insight into mantle heterogeneity and crustal material
Supporting Information:
recycling. However, many uncertainties remain about how to recognize the relationship between major
• Supporting Information S1
• Table S1 element patterns of basalts and source lithological and/or compositional diversities using typical petrological
• Table S2 methods. In this study, discriminant functional analysis and multivariate regression are carried out using
major element logratios for literature experimental melts of four primitive mantle‐like lherzolites and six
mafic lithologies (five pyroxenites and one hornblendite). A parameter called FCMS (FCMS = ln (FeO/
Correspondence to:
CaO) − 0.058 * (ln (MgO/SiO2))3 − 0.636 * (ln (MgO/SiO2))2 − 1.850 * ln (MgO/SiO2) − 1.170, all the major
Z.‐F. Yang,
yangzfeng2008@163.com elements in weight percent) is proposed to identify source lithologies for basaltic melts. When the logratios
ln(K2O/Al2O3), ln (TiO2/Na2O), and ln (Na2O/K2O) are incorporated into FCMS, the temperature and
pressure effects on the compositional heterogeneity of peridotites melts can be significantly reduced; a more
Citation:
Yang, Z.‐F., Li, J., Jiang, Q.‐B., Xu, F., powerful parameter called FCKANTMS (FCKANTMS = ln (FeO/CaO) − 0.08 * ln(K2O/Al2O3) − 0.052 * ln
Guo, S.‐Y., Li, Y., & Zhang, J. (2019). (TiO2/Na2O) − 0.036 * ln (Na2O/K2O) * ln (Na2O/TiO2) − 0.062 * (ln (MgO/SiO2))3 − 0.641 * (ln (MgO/
Using major element logratios to
SiO2))2 − 1.871 * ln (MgO/SiO2) − 1.473, all the major elements in weight percent) can be obtained. Olivine
recognize compositional patterns of
basalt: Implications for source fractional crystallization and accumulation, although they can significantly change most major element
lithological and compositional contents and ratios, usually increase or decrease FCMS and FCKANTMS by only 0–0.15, which is one order
heterogeneities. Journal of Geophysical
of magnitude lower than their variations in the primary experimental melts of different lithologies.
Research: Solid Earth, 124, 3458–3490.
https://doi.org/10.1029/2018JB016145 Importantly, approximately 80% and 50% low to moderate degree (F < 60%) partial melts (n = 303) of mafic
lithology (with or without volatiles in source materials) can be distinguished from melts of peridotite and
Received 27 MAY 2018 transitional lithologies when FCKANTMS combined with ln (CaO/TiO2) and ln (SiO2/
Accepted 10 MAR 2019
(CaO + Na2O + TiO2)). Thus, the chemical markers could be used to constrain source lithology and origin of
Accepted article online 18 MAR 2019
Published online 9 APR 2019 natural basalts.
Plain Language Summary Basaltic melts can be experimentally produced from a variety of
mafic and ultramafic lithologies. Understanding the source lithology of basalts can greatly impact our
understanding of magmatic processes, which can help us gain insight into mantle heterogeneity and crustal
material recycling. However, many uncertainties remain about how to identify the source lithology of
basalts using traditional petrological methods. In this study, major element patterns of experimental basaltic
melts are explored using major element logratios. We find that most peridotite melts can be distinguished
from pyroxenite and hornblendite melts by the logratio‐based chemical markers. Thus, the chemical
markers could be used to constrain source lithology and origin of natural basalts.
1. Introduction
1.1. Identification of Source Compositional and/or Lithological Heterogeneities in Basalts
Although the upper mantle consists predominantly of lherzolite and harzburgite, many geological processes,
such as crustal material recycling and mantle metasomatism, can result in mineralogical and compositional
heterogeneities, producing a variety of mafic and ultramafic rocks, including metasomatized peridotite,
pyroxenite, hornblendite, and many other transitional lithologies between these. For clarity, in this paper,
©2019. American Geophysical Union.
unless otherwise stated, peridotite is used to refer to olivine‐rich lithologies, including dunite, harzburgite,
All Rights Reserved. lherzolite, wehrlite, and any transitional lithologies between these; mafic rock or lithology is used to refer
to olivine‐poor and olivine‐free lithologies, including olivine pyroxenite, garnet pyroxenite, clinopyroxenite,
hornblendite, eclogite, and any transitional lithologies between these. The mineralogical and compositional
heterogeneities in the lithosphere and/or the asthenosphere have been widely used to explain the petrologi-
cal and geochemical diversity of mantle‐derived rocks (e.g., Allegre & Turcotte, 1986; Dick & Zhou, 2015;
Halliday et al., 1995; Herzberg, 2011; Hirschmann & Stolper, 1996; Hofmann & White, 1982; Kogiso et al.,
2004; Lambart et al., 2013; Lustrino, 2005; Niu & O'Hara, 2008; Pilet et al., 2008; Sobolev et al., 2007;
Yang & Zhou, 2013) and may also contribute to the seismic velocity variations in the upper mantle (e.g.,
Anderson & Bass, 1984; Bruneton et al., 2004; Chen et al., 1996; Eeken et al., 2018; Foulger et al., 2013).
However, the geochemistry of either basalts or olivine phenocrysts that is used to argue for source lithologi-
cal and/or compositional heterogeneities is to some extent compromised by variations in intensive para-
meters such as temperature and pressure. During these variations, melting and crystallization occur,
which in turn triggers many debates on the origin of mantle‐derived magmas and the mantle geodynamic
processes that they underwent in both oceanic and continental settings (e.g., Davis et al., 2013; Gale et al.,
2014; Herzberg, 2011; Lambart et al., 2013; Li & Ripley, 2010; Matzen et al., 2013; Niu, 2016; Niu et al.,
2011; Putirka et al., 2011; Yang et al., 2016).
Much experimental work on the partial melting of a variety of peridotitic and mafic rocks has been carried out
over the past several decades (e.g., Green, 2015; Kogiso et al., 2004; Kushiro, 2001; Lambart et al., 2013; Wyllie,
1995 and references therein), providing a fundamental experimental basis for understanding how the P‐T‐X
(i.e., pressure, temperature, and composition) of mantle‐derived magmas vary and are related to each other
(e.g., Ghiorso et al., 2002; Hirschmann et al., 1998; Lambart et al., 2016). However, the relationship between
the major element patterns of basaltic melts and lithological and/or compositional variations in source materi-
als is still unclear because the major element characteristics of basaltic melts are strongly affected not only by
source composition, melting temperature, and pressure but also by magmatic processes such as fractional crys-
tallization and magma mixing (e.g., Dick & Zhou, 2015; Herzberg & O'Hara, 2002; Jennings et al., 2016;
Kushiro, 2001; Lambart et al., 2013; Langmuir et al., 1992; Niu et al., 2011; Putirka et al., 2011; Yang et al.,
2016). Partial melting experiments suggest that peridotitic rocks with Mg# (MgO/(MgO + FeO), molar ratios)
ranging from 0.85 to 0.9 at different pressures can produce melts that evolve to primitive MORB (middle ocean
ridge basalt) when different degrees of olivine fractionation occur (e.g., Hirose & Kushiro, 1993; Kushiro, 2001).
To distinguish major element patterns in melts derived from peridotite with different Mg#, the mantle potential
temperature must be determined (e.g., Lambart et al., 2013). However, from the petrological perspective, the
source bulk composition must be assumed to determine mantle potential temperature (e.g., Dalton et al.,
2014; Langmuir et al., 1992). This dilemma might be one of the most important petrological reasons for the
debate over whether MORB major element patterns result from variations in mantle potential temperature
or source compositional diversity (e.g., Gale et al., 2014; Niu, 2016).
For the CaO‐MgO‐Al2O3‐SiO2 system, the compositional characteristics of melts in equilibrium with a lher-
zolite mineral assemblage depend only on pressure or temperature (e.g., O'Hara, 1965; Presnall &
Gudfinnsson, 2011). This Gibbs phase rule‐constrained phase relation, however, does not exist in natural
multiple component systems (e.g., Lambart et al., 2013; Langmuir et al., 1992; Yang & Zhou, 2013). For
example, experimental melts in equilibrium with olivine‐free pyroxenite mineralogy may, in some cases, dis-
play phase relations similar to those in equilibrium with harzburgite and lherzolite mineralogy when 8 to 10
major oxides are considered simultaneously (e.g., Herzberg, 2011; Kogiso et al., 2004; Lambart et al., 2013;
Yang & Zhou, 2013). A recent experimental phase relation study suggests that when the compositional vari-
ables Mg#, NaK# ((Na2O + K2O)/(Na2O + K2O + CaO)), P2O5, and pressure are specified, typical garnet pyr-
oxenite melts can be distinguished from garnet peridotite melts in phase diagrams (Grove et al., 2013). In
addition, this Gibbs phase rule‐inspired empirical model cannot successfully explain the compositional pat-
terns of melts derived from iron‐rich peridotite PHN1611, and some olivine pyroxenite and lherzolite melts
still display identical phase relations. Moreover, the thermodynamic model of Grove et al. (2013) suggests
that Hawaiian tholeiite glasses in the phase diagrams are in equilibrium with harzburgite, rather than
derived from an olivine‐free pyroxenite source as indicated by olivine chemistry and simple major element
plots (Herzberg, 2006; Herzberg, 2011; Sobolev et al., 2005).
Recent thermodynamic calculations suggest that at the same mantle potential temperature, olivine pyroxe-
nite generated through mechanical mixing between MORB and typical mantle lherzolite can produce melts
with significantly higher FeO and lower CaO contents than melts derived from lherzolite (Jennings et al.,
2016), which is consistent with experimental petrology results (Kogiso et al., 1998) and has been used to
argue that some iron‐rich subalkaline picrites are derived from such an olivine pyroxenite source.
However, this model cannot identify the source lithology for alkaline basalts and basalts with normal FeO
content and does not consider some minor components, such as TiO2, K2O, H2O, and CO2, that may
significantly affect the major element characteristics of melts derived from both peridotitic and mafic sources
(Grove et al., 2013; Herzberg, 2011; Lambart et al., 2013; Yang & Zhou, 2013). The overall degree of
matching for major element contents between natural basalts and a variety of experimental basaltic melts
has been used to identify the source lithology of Icelandic basalts (Shorttle & MacLennan, 2011), but this
method is largely dependent on which experimental melts are used for comparison, and the best choice can
always be obtained even if the result is wrong. Although intraplate low‐silica alkaline magmas show major
element patterns in simple Harker diagrams and phase relations similar to those of experimental melts
derived from CO2‐bearing peridotite and/or eclogite (Dasgupta et al., 2007; Mallik & Dasgupta, 2013; Mallik
& Dasgupta, 2014), they may also be produced by partial melting of mafic sources composed predominantly
of amphibole‐rich metasomatic veins (Pilet, 2015; Pilet et al., 2008; Yang et al., 2016). Our previous study
suggests that basaltic melts derived from mafic sources can be statistically distinguished from peridotite‐
derived melts in the FC3MS space (FeO/CaO − 3 * MgO/SiO2, all in weight percent; Yang & Zhou, 2013),
which has been used to identify the source lithologies of continental OIB (ocean island basalt)‐type basalts
(e.g., Chu et al., 2017; Dai et al., 2015; Li et al., 2015; Sheldrick et al., 2018; Xu et al., 2017; Yang et al., 2016;
Zhang & Guo, 2016), boninites (Zhao & Asimow, 2014), and continental flood basalts (e.g., Cheng et al.,
2018; Heinonen et al., 2018; Heinonen & Fusswinkel, 2017; Howarth & Harris, 2017); however, there are
some fertile peridotite melts that still cannot be separated from melts derived from either normal peridotitic
or mafic sources in the FC3MS space (Yang et al., 2016; Yang & Zhou, 2013).
Olivine phenocrysts with high Ni and low Ca and Mn (or high Fe/Mn) have been widely used to argue for an
olivine‐free pyroxenite source for both oceanic and continental basalts (e.g., Herzberg, 2006; Herzberg, 2011;
Li et al., 2016; Liu et al., 2015; Sobolev et al., 2005; Sobolev et al., 2007; Xu et al., 2012). Nevertheless, recent
high‐precision experimental petrology suggests that minor and trace element characteristics in olivine
strongly depend upon temperature, pressure, and coexisting melt composition (Matzen et al., 2013;
Matzen, Baker, et al., 2017). High‐Ni olivine can crystallize under low temperature conditions from high‐
temperature peridotite‐derived melts, and low‐Mn olivine can crystallize from MgO‐rich peridotite‐derived
melts (Matzen, Wood, et al., 2017). Detailed case studies suggest that high‐Ni and low‐Mn olivine pheno-
crysts in continental flood basalts of the Karoo meimechites most likely result from temperature and pres-
sure variations (Heinonen & Fusswinkel, 2017), but similar geochemical features in other continental
flood basalts indicate an olivine‐free pyroxenite source when combined with other geochemical characteris-
tics (Howarth & Harris, 2017). Low Ca and high‐Ni olivine in continental basalts from eastern China have
been widely used as support for an olivine‐free pyroxenite source (e.g., Li et al., 2016; Qian et al., 2015;
Wang et al., 2011), but the olivine compositions probably result from diffusive reequilibration between man-
tle olivine xenocrysts and host basaltic magmas (Yang et al., 2016). Additionally, olivine crystallized from
melts of olivine‐bearing pyroxenite and peridotite show very similar compositional characteristics, and it
is almost impossible to distinguish such melts from each other using traditional petrological methods
(Herzberg et al., 2014). Therefore, many uncertainties remain about how to recognize the relationship
between major element patterns of basalts and source lithological and/or compositional diversities using
typical petrological methods.
component system CaO‐MgO‐Al2O3‐SiO2 and cannot be directly compared with the SiO2 contents in natural
basalts that are 100 wt% renormalized to at least a 10‐component system. If SiO2 in Hawaiian tholeiites is
100 wt% renormalized to the CaO‐MgO‐Al2O3‐SiO2 system, all the Hawaiian tholeiites (Sobolev et al.,
2005) become andesitic in composition (SiO2 > 56 wt%), which is significantly different from experimental
basaltic melts. This subcompositional incoherence is another fundamental property of compositional data
that has not received enough attention in geological fields (Aitchison, 1986; Aitchison & Egozcue, 2005;
Le Maitre, 1982; Rock, 1988).
The essence of compositional data is ratios, because ratios do not change when compositional data are renor-
malized to 100% or considered in subcompositional space, and logratios would allow compositional data to
freely range from −∞ to +∞, which can be analyzed using standard statistical techniques (Aitchison, 1986;
Aitchison & Egozcue, 2005; Egozcue et al., 2003; Pawlowsky‐Glahn & Egozcue, 2006). The logratio method,
however, has only just begun to be realized in petrological and geochemical fields in recent years (e.g., Cortés
et al., 2007; Ó. Kovács et al., 2006; Rollinson, 1992; Verma et al., 2016; Yang & Zhou, 2013). Numerous stu-
dies involving pattern recognition of compositional data for rocks and minerals still focus on the raw concen-
tration form. One important reason might be that concentration data can be easily handled to explore many
petrological processes characterized by mass balance issues, such as magma mixing and fractional crystalli-
zation (Cortes, 2009). On the other hand, as noted by many statisticians, distinguishing real geological pro-
cesses from geometrical illusions is generally difficult when compositional data are treated in raw
concentration form (Aitchison, 1986; Pawlowsky‐Glahn & Egozcue, 2006; see Appendix A).
Combining the logratio method developed in the compositional data analysis field (Aitchison, 1986), the
idea obtained from our previous parameter of FC3MS used for source lithology identification (Yang et al.,
2016; Yang & Zhou, 2013), and the guidance of fundamental knowledge about experimental mineralogy
and petrology, both qualitative and quantitative multivariate regression and discriminant function analysis
of major element patterns from the literature on experimental basaltic melts derived from a variety of peri-
dotitic and mafic sources are carried out. We find that melts of peridotite and mafic lithology show signifi-
cantly different major element patterns in the logratio‐based space, even if source compositional
heterogeneity, variations in melting conditions (i.e., temperature and pressure), and significant amounts
of olivine fractionation and/or accumulation occur.
Figure 1. ln (FeO/CaO) versus ln (MgO/SiO2) for experimental melts of typical lherzolite, pyroxenite, and hornblendite in
(a) and relationships between FCMS (calculated using equation (2) in Table 1) and partial melting degree in (b). The
experimental bulk rock compositions are also shown in (a) and (b) indicated by black filled squares, which can also be
regarded as 100% batch partial melts of the sources. White and gray filled circles marked with L – 20 wt% Ol and
L + 20 wt% Ol represent equilibrium olivine subtraction and addition, respectively, with 1 wt% increments that are cal-
2+ T
culated using PRIMELT2, assuming Fe / Fe = 0.9 (Herzberg & Asimow, 2008). Note that FCMS is very insensitive to
fractional crystallization and accumulation of olivine (white and gray filled circles) as shown in (b). Linear regressions
shown in (b) are used to find to what extent melting degree can influence variation in FCMS for different sources (see
discussions in the main text). Primitive mantle‐like lherzolite melts include experimental batch melts of lherzolite KR4003
(Walter, 1998), KLB‐1 (Davis et al., 2011; Hirose & Kushiro, 1993), MBK, and MBK+ (Laporte et al., 2014). Pyroxenite
melts include experimental batch melts of olivine websterite M5‐103, garnet websterite M5‐40, garnet olivine clinopyr-
oxenite M7‐16 (Lambart et al., 2012; Lambart et al., 2009a, Lambart et al., 2013), garnet pyroxenite 77SL‐582 (Keshav et al.,
2004), and MIX1G (Hirschmann et al., 2003; Kogiso et al., 2003). Pyroxenites M5‐40, 77SL‐582, and MIX1G are very
similar in bulk composition, and all can be considered as having the average composition of natural pyroxenite. AG4
represents experimental melts of a carbonate‐bearing hornblendite (Pilet et al., 2008). The error bars in (a), smaller than
the size of symbols, are not shown. The average error bar of FCMS shown in (b) is calculated by assuming two
standard deviations of 6% for MgO and FeO and 3% for CaO and SiO2, which are estimated by examining both
experimental and analytical uncertainty on the experimental melts (see discussion in the main text). All the data for the
source bulk compositions and the experimental melts shown in (a) and (b) are presented in Tables S1 and S2.
(FeO/CaO) and ln (MgO/SiO2) approximately satisfy a cubic polynomial correlation trend (Figure 1a and
equation (1) in Table 1). As shown in Figure 1a, the lherzolite melts mostly are not lie on the cubic
polynomial curve because ln (FeO/CaO) and ln (MgO/SiO2) are strongly affected by melting degree
and pressure. For peridotite melts, both FeO/CaO and MgO/SiO2 show significant positive correlations
with pressure, and for low degree melts (F < 20%) of a specific peridotitic or mafic source at a given
Table 1
Equations Used to Derive Chemical Parameters of FCMS and FCKANTMS
Equations (1–8) (all the major oxides in wt%)
3 2
(1) ln (FeO/CaO) = 0.058 * (ln (MgO/SiO2)) + 0.636 * (ln (MgO/SiO2)) + 1.850 * ln (MgO/SiO2) + 1.170
3 2
(2) FCMS = ln (FeO/CaO) − 0.058 * (ln (MgO/SiO2)) – 0.636 * (ln (MgO/SiO2)) – 1.850 * ln (MgO/SiO2) − 1.170
(3) FCMS2 = FCMS − 0.080 * ln(K2O/Al2O3) − 0.182
(4) FCMS3 = FCMS2 − 0.052 * ln (TiO2/Na2O) − 0.096
(5) FCMS4 = FCMS3 – 0.036 * ln (Na2O/K2O) * ln (Na2O/TiO2) + 0.007
(6) FCKANT = ln (FeO/CaO) − 0.08 * ln(K2O/Al2O3) − 0.052 * ln (TiO2/Na2O) − 0.036 * ln (Na2O/K2O) * ln (Na2O/
TiO2) − 0.271
3 2
(7) FCKANT = 0.062 * (ln (MgO/SiO2)) + 0.641 * (ln (MgO/SiO2)) + 1.871 * ln (MgO/SiO2) + 1.201
(8) FCKANTMS = ln (FeO/CaO) − 0.08 * ln(K2O/Al2O3) − 0.052 * ln (TiO2/Na2O) − 0.036 * ln (Na2O/K2O) * ln
3 2
(Na2O/TiO2) − 0.062 * (ln (MgO/SiO2)) – 0.641 * (ln (MgO/SiO2)) – 1.871 * ln (MgO/SiO2) − 1.473
pressure, FeO/CaO is negatively correlated with MgO/SiO2 (see Figure S9 in Yang & Zhou, 2013). In
contrast, both the pyroxenites and the hornblendite melts, at a given ln (MgO/SiO2), mostly have
significantly higher or lower ln (FeO/CaO) than the lherzolite melts. Thus, ln (FeO/CaO) in a melt
derived from a mafic lithology minus a predicted ln (FeO/CaO) using ln (MgO/SiO2) by equation (1), a
parameter called FCMS (equation (2) in Table 1), can be obtained and which can be used to describe
the compositional difference between the melt of the mafic lithology and the lherzolite melts. FCMS
value in the lherzolite melts should be close to zero, but it can be significantly higher or lower than
zero in the pyroxenites and the hornblendite melts as shown in Figure 1b. Importantly, FCMS is only
slightly influenced by fractional crystallization and accumulation of olivine (Figure 1b) because olivine
subtraction and addition trends are very similar to the trend displayed by the cubic polynomial relation
between ln (FeO/CaO) and ln (MgO/SiO2) (Figure 1a).
Before discussing to what extent variation in FCMS values can represent real distinction between experi-
mental melts derived from different sources, it is necessary to assess the influence of experimental petro-
logical errors on FCMS heterogeneity. Both experimental and analytical uncertainties on major oxides
FeO, CaO, MgO, and SiO2 could contribute to variation in FCMS values of experimental melts. The aver-
age error of FCMS values in the experimental melts is estimated to be ~0.08 by assuming two standard
deviations (SDs) of 6% for MgO and FeO and 3% for CaO and SiO2 which are estimated by examining
experimental and analytical uncertainty for the experimental melts shown in Figure 1. Experimental
melts of a given source produced at nearly identical P and T conditions usually have similar melting
degree, which, because of experimental uncertainty, can be considered as a single melt and thus can be
used to estimate both experimental and analytical uncertainties on both major oxides and FCMS. For
example, three near‐solidus melts (F = 2.4–3.6%) from pyroxenite M5‐103 produced at 1.5 GPa and
1,280–1,290 °C have FCMS ranging from 0.02 to 0.07 (Lambart et al., 2009a). Similarly, five experimental
melts from KLB‐1 produced at 3 GPa and 1,450–1,470 °C have FCMS ranging from −0.07 to 0.06 (Davis
et al., 2011). The heterogeneities of FCMS values in the two examples are well within the estimated aver-
age error. Note that variation in FCMS due to analytical uncertainty of electron microprobe usually sig-
nificantly lower than 0.08, typically lower than 0.02 because analytical errors on major oxides FeO, CaO,
MgO, and SiO2 usually three to four times lower than the average errors assumed above (supporting
information Figure S1).
As shown in Figure 1b, the strong linear correlations between melting degree and FCMS values of the pyr-
oxenite and the hornblendite melts suggest that compositional pattern of these melts is mainly controlled by
melting degree in the FCMS space. In contrast, FCMS values in the lherzolite melts also show somewhat het-
erogeneity when experimental errors are considered, but they do not show significant correlations with
melting degree and pressure (not shown) because they are intercorrelated as shown in the next section.
Experimental melts of PM‐like lherzolite produced at 1~7 GPa have FCMS of 0.00 ± 0.10 (SD, n = 53), which
is significantly lower than those of low to intermediate degree partial melts of pyroxenite and hornblendite
but is similar to those of near‐solidus melts of pyroxenite M5‐103. Thus, FCMS, although affected by experi-
mental errors, melting degree, and pressure, can distinguish the majority of the experimental melts of typical
pyroxenite and hornblendite from melts of peridotite.
2.2. Discriminant Function Analysis Using Linear Combination of Major Element Logratios
From a discriminant analysis perspective, to increase the difference in major element patterns between
melts of mafic lithology and peridotite, the variance of compositional markers within melts of each lithology
should be as low as possible, whereas the variance between melts of the two lithologies should be as high as
possible. However, FCMS values in melts of peridotite show significant heterogeneity, which is mainly a
result of the temperature and pressure effect that can be significantly reduced by introducing other major
element logratios, as shown below. It is widely recognized that, if source compositional characteristics (var-
iations in major and minor oxides, volatiles, and oxygen fugacity) are specified, the melting degree of a given
source is controlled only by temperature and pressure, and only two variables among melting degree, tem-
perature and pressure, are independent. The relationships between FCMS and the melting degree of experi-
mental melts shown in Figure 1b suggest that FCMS is strongly correlated with source compositional
characteristics and melting degree. Thus, the FCMS values of experimental melts should be a function of
source compositional characteristics, temperature (or melting degree), and pressure.
FCMS ¼ f ðP; T or F; X Þ;
where P = pressure, T = temperature, F = melting degree, and X = source compositional characteristics.
Notably, the partial melting mechanism (batch or fractional melting) also influences the FCMS value. The
relationships between FCMS values and batch melting degree for the four peridotites shown in Figure 1b
provide some insights into the fractional melting scenario. As near‐fractional melting of mantle peridotite
commonly occurs when batch melting degree larger than 1–2%, the near‐fractional melts can be considered
as aggregates of incremental near‐solidus batch melts. Because the linear regression solidus batch melts of
peridotite have FCMS value closing to zero (0.02 ± 0.10, SD; Figure 1b), FCMS values in mixtures between
these melts should also close to zero, although heterogeneity still exist. A thermodynamic calculation on low
degree partial melting (F < 20%) of a PM‐like peridotite indicates that FCMS values in polybaric near‐
fractional melts (i.e., polybaric incremental batch melts with 1% interval; −0.13 ± 0.12 [SD], n = 12;
Kinzler, 1997) are slightly lower than isobaric batch melts (−0.06 ± 0.08 [SD], n = 26; Kinzler & Grove,
1992b). A parameterization of experiments on lherzolite KR4003 suggests that near‐solidus melts produced
at 3–7 GPa and polybaric accumulated fractional melts (F < 30%) have FCMS of 0.10–0.15 and −0.03–0.13,
respectively (Herzberg et al., 2007). These suggest that the batch and near‐fractional melts of a peridotite,
may have a difference of ~0.1 in FCMS value, should have similar compositional pattern in the FCMS space.
Specifically, the two examples indicate that FCMS values in the near‐fractional melts mostly lower than the
batch melts, which is most likely due to that FCMS values show a weak positive correlation with melting
degree for melts derived from heterogeneous peridotite source (Figure S2b). In contrast, for the near‐
factional melts of typical pyroxenite and hornblendite, they can have higher FCMS values than batch melts
as, for a given mafic source, the near‐solidus batch melts have the highest FCMS values (Figure 1b). Hence,
near‐fractional and batch melts of a given source are indeed have different FCMS values, but the difference is
similar to experimental uncertainty, suggesting that for the source lithology identification, the statistical
results obtained from the batch melts also hold for the near‐fractional melts (see other discussions in
section 3.2.3). On the other hand, if a melt was formed by mixing between lherzolite‐ and mafic source‐
derived melts, it would, in most cases, have intermediate FCMS value, and mafic source signature can be
identified. A quantitative model for FCMS value in near‐fractional melts of different sources will be fully pre-
sented and discussed in another paper. Here we first focus on experimental batch melts.
Apart from Na2O, K2O, and Al2O3, other major oxides are very similar for the four experimental lherzolites
(Table S1) shown in Figure 1. Assuming that the four lherzolites represent one source composition, then the
variation in FCMS for the experimental lherzolite melts (Figure 1b) should be controlled by temperature (or
melting degree) and pressure. Thus, we can incorporate temperature (or melting degree)‐ and pressure‐
sensitive major element logratios into FCMS to find other chemical markers that show less heterogeneity
for the lherzolite melts. To retain and/or maximize the discriminant ability of FCMS between the experi-
mental melts of mafic source and lherzolite, major element logratios that are almost unaffected by olivine
fractional crystallization and accumulation should be selected to calibrate the influence of temperature
(or melting degree) and pressure on FCMS, as FCMS is also insensitive to olivine fractional crystallization
and accumulation. Most of the logratios between CaO, Na2O, TiO2, K2O, MnO, Cr2O3, and Al2O3 satisfy
such constraints, as these major oxides are commonly highly incompatible in olivine.
Figure 2. FCMS versus ln(K2O/Al2O3) in (a), FCMS2 versus ln (TiO2/Na2O) in (b), FCMS3 versus ln (Na2O/K2O) in (c), and
FCMS3 versus ln (Na2O/K2O)*ln (Na2O/TiO2) in (d) of experimental batch melts on four different lherzolites. Note that the
significant positive correlations between FCMS and ln(K2O/Al2O3) in experimental melts for lherzolites KR4003, KLB‐1,
and MBK suggest that the heterogeneity in FCMS does not due to experimental error. FCMS, FCMS2, and FCMS3 are
calculated by equations listed in Table 1. The average error bars in (a)–(d) are calculated by assuming two standard deviations
of 6% for MgO and FeO, 3% for CaO, Al2O3, and SiO2, 15% for TiO2, and 30% for K2O and Na2O, which are estimated by
examining both experimental and analytical uncertainty on the experimental melts. The linear regression line in (b) is
least‐squares fit for data from experimental melts of lherzolites MBK and KR4003, while the linear regression lines in (c) and
(d) are least‐squares fit for data from all the lherzolite melts. The data sources are the same as in Figure 1.
Partial melting experiments on lherzolite suggest that for low to moderate degree partial melts, ratios such as
CaO/Al2O3, TiO2/Na2O, TiO2/Al2O3, MnO/Al2O3, and Cr2O3/Al2O3 generally increase with increasing
pressure and, at similar pressure, K2O/Al2O3, Na2O/Al2O3, (TiO2 + K2O)/Al2O3, and (Na2O + K2O)/
Al2O3 decrease with increasing melting degree (e.g., Hirose & Kushiro, 1993; Laporte et al., 2014; Walter,
1998). For the major rock‐forming minerals of anhydrous lherzolite, K has been shown to be a highly incom-
patible element, while Al, Ca, Ti, and Na in most cases are moderately incompatible elements (e.g., Davis
et al., 2011; Davis & Hirschmann, 2013; Hirose & Kushiro, 1993; Kushiro, 1996; Kushiro, 2001; Laporte
et al., 2014; Prytulak & Elliott, 2007; Walter, 1998). CaO has been used in FCMS, and Al2O3 contents in
experimental melts of lherzolite are generally higher and have smaller analytical error than TiO2 and
Na2O. Thus, the K2O/Al2O3 ratio might be the best variable to model variations in the melting degree,
although a slight pressure effect still exists. Melts of lherzolites KLB‐1, KR4003, and MBK, both individually
and collectively, are found to display significant positive linear relationships between ln(K2O/Al2O3) and
FCMS (Figure 2a), suggesting that the melting degree indeed has significant influence on FCMS. At a given
FCMS, melts of lherzolite KLB‐1 have lower ln(K2O/Al2O3) than melts derived from the other lherzolites,
which most likely results from lherzolite KLB‐1 having the lowest ln(K2O/Al2O3) ratio and the lowest
K2O content of all the source materials (Table S1). We note that melts of lherzolite MBK are almost isobaric
(1–1.3 GPa), and the melting degree ranges from 0.9% to 22.8%; thus, the significant linear correlation
between ln(K2O/Al2O3) and FCMS and variations in their values should be mainly controlled by melting
degree (Figure 2a). Using the linear relationship between ln(K2O/Al2O3) and FCMS in melts of lherzolite
MBK, a parameter called FCMS2 (equation (3) in Table 1) can be obtained that, at constant pressure, has
nearly homogeneous features as a function of melting degree (or temperature). In other words, when
ln(K2O/Al2O3) is incorporated into FCMS, the melting degree (or temperature) effect on the heterogeneity
of the lherzolite melts in the FCMS2 space can be significantly reduced. Note that all the four lherzolites
individually have more homogeneous compositional features in the FCMS2 space (Figure 2b) than in the
FCMS space (Figure 2a).
Lherzolites KR4003, MBK+, and MBK have similar ln(K2O/Al2O3) (Table S1), and ln(K2O/Al2O3) variation
in melts for lherzolites KR4003, MBK+, and MBK are mainly due to variation in melting degree; thus, at a
given ln(K2O/Al2O3), the higher FCMS values in partial melts of lherzolite KR4003 than those of lherzolites
MBK+ and MBK are most likely due to the pressure effect (Figure 2a). This conclusion can be supported by
the significant positive correlations between FCMS2 and ln (TiO2/Na2O) in experimental melts for lherzo-
lites KR4003 and MBK (Figure 2b), as numerous studies suggest that the TiO2/Na2O ratios of lherzolite melts
increase with pressure (e.g., Hirose & Kushiro, 1993, Laporte et al., 2014, Prytulak & Elliott, 2007, Walter,
1998). Using the linear relationship between ln (TiO2/Na2O) and FCMS2 in melts of lherzolites KR4003
and MBK (Figure 2b), a parameter called FCMS3 (equation (4) in Table 1) can be obtained. When ln
(TiO2/Na2O) is incorporated into FCMS2, the pressure effect on the heterogeneity of the lherzolite melts
in the FCMS3 space can be significantly reduced. As the temperature effect has been considered in
FCMS2, FCMS3 mostly accounts for both the pressure and temperature (or melting degree) effects on its het-
erogeneity. Note that a standard linear regression analysis was also carried out, and the results (not shown)
are similar to those of our current stepwise analysis using fundamental petrological knowledge in capturing
the relationships between ln(K2O/Al2O3), ln (TiO2/Na2O), and FCMS. Thus, our current stepwise analysis is
preferred because it can be easily understood from a petrological perspective.
Lherzolite KLB‐1 melts generally have higher FCMS2 (Figure 2b) and FCMS3 (Figure 2c) than the other
three lherzolite melts, suggesting that the compositional pattern of melts of PM‐like lherzolite in the
FCMS2 and FCMS3 spaces should be affected by other factors. A close examination of the source bulk com-
positions for the four experimental lherzolites indicates that they have significantly different Na2O/K2O
ratios, lherzolite KLB‐1 has the highest Na2O/K2O ratio, and all the experimental melts of lherzolite show
significant positive correlations between FCMS3 and ln (Na2O/K2O) (Figure 2c). These results suggest that
the source Na2O/K2O ratio has a significant influence on the FCMS3 value of the melts. We find that ln
(Na2O/K2O) * ln (Na2O/TiO2) also shows a statistically significant positive correlation with FCMS3
(Figure 2d). From a statistical perspective, ln (Na2O/K2O) is a better variable to use to calibrate source com-
positional diversity effect on the heterogeneity in FCMS3, but ln (Na2O/K2O) * ln (Na2O/TiO2) is preferred
as this parameter when combined linearly with FCMS3 can formulate a parameter called FCMS4 (equation
(5) in Table 1) which can maximize the compositional difference between the melts of lherzolite and mafic
sources. By integrating equations (4)–(6), a parameter called FCKANT (equation (6) in Table 1) can be
obtained. When FCKANT is plotted against ln (MgO/SiO2), the FCKANT and ln (MgO/SiO2) values for
the experimental melts of PM‐like lherzolite are found to approximately satisfy a cubic polynomial correla-
tion trend of equation (7) in Table 1 and Figure 3a. Compared with the polynomial correlation of ln (FeO/
CaO) and ln (MgO/SiO2) (Figure 1a), FCKANT and ln (MgO/SiO2) have a higher correlation coefficient, and
at a given ln (MgO/SiO2), the lherzolite melts differ from the mafic source melts more significantly in
FCKANT than in ln (FeO/CaO) (Figure 1a). Using the same method for derivation of FCMS (see discussion
in the above section), a parameter called FCKANTMS (equation (8) in Table 1) can be obtained which can
simultaneously minimize the compositional heterogeneity in experimental melts of PM‐like lherzolite and
expand the difference between melts of lherzolite and mafic source.
Notably, a standard linear regression analysis suggests that ln(K2O/Al2O3), ln (TiO2/Na2O), and ln (Na2O/
K2O) * ln (Na2O/TiO2) exhibit statistically significant linear correlations with FCMS and do not have signif-
icant collinearity problems (not shown); many other major element logratios can be combined with FCMS to
reduce the compositional heterogeneity in melts of PM‐like lherzolite, but these logratios also reduce the
compositional difference between melts of PM‐like lherzolite and mafic lithology and result in significant
pressure effects on melts of mafic lithology (not shown). The FCKANTMS values in melts of PM‐like
lherzolites have a mean of 0.00 ± 0.08 (SD, n = 53), and its variation does
not show statistically significant correlations with any other major oxide
logratios, suggesting that the compositional heterogeneity in the
FCKANTMS space should mainly result from experimental errors
and/or other unconstrained factors. Most experimental errors are signifi-
cantly larger than the analytical errors for the instruments because experi-
mental melts are not always homogeneous, sometimes may not be in full
equilibrium with solid residuals, and often suffer from Fe loss or gain
(Kushiro, 2001). For example, melts of lherzolite KLB‐1 have higher and
more heterogeneous FCKANTMS (0.06 ± 0.09 [SD], n = 13; Hirose &
Kushiro, 1993) than melts of lherzolite KR4003 (0.00 ± 0.07 [SD],
n = 13) and of lherzolites MBK and MBK+ (−0.03 ± 0.08 [SD], n = 17),
which is probably due to experimental error because melts are not com-
pletely in equilibrium as noted by Hirose and Kushiro (1993). The experi-
mental error for FCKANTMS is estimated to range from ~0.02 to ~0.1
based on a close examination of typical lherzolite melts (Figure S1), sug-
gesting that the heterogeneity of FCKANTMS in melts of PM‐like lherzo-
lites possibly results mainly from experimental uncertainties, and the SD
(0.08) of FCKANTMS probably represents its true compositional hetero-
geneity. Because of experimental uncertainties, we currently cannot
quantify the influence of other components on the compositional pattern
(i.e., FCMS and FCKANTMS) for melts of lherzolite, which may be clari-
fied by future well‐designed high‐precision experimental work.
As shown in Figure 3b, FCKANTMS in melts of the average pyroxenite is
strongly negatively correlated with melting degree, ranging from −0.05 to
0.86, which is generally lower than FCKANTMS in melts of hornblendite
AG4 and pyroxenite M7‐16 at a given melting degree. Importantly, for
melting degree <60%, melts of these mafic sources have significantly
higher FCKANTMS than melts of PM‐like lherzolite. In contrast, melts
of pyroxenite M5‐103 generally have lower FCKANTMS than melts of
PM‐like lherzolite, although low degree partial (F < 10%) melts are indis-
tinguishable. For lherzolite melts, both FCKANTMS and FCMS are close
Figure 3. The FCKANT versus ln (MgO/SiO2) for experimental melts of
typical lherzolite, pyroxenite, and hornblendite in (a) and the relationships to zero, but the SD of FCKANTMS is smaller than that of FCMS suggest-
between FCKANTMS and melting degree in (b). FCKANT and ing that lherzolite melts are more homogeneous in the FCKANTMS
FCKANTMS are calculated using equations (6) and (8) (Table 1), respectively. space than in the FCMS space. Five low degree melts (F < 40%) of pyrox-
Note that olivine fractional crystallization (white filled circles) and accumu- enite MIX1G all have FCKANTMS > 0.4 (Figures 3b), but only two melts
lation (gray filled circles), calculated using the same method in Figure 1,
have FCMS > 0.4 (Figures 1b). Moreover, FCKANTMS is stronger than
only slightly influence FCKANTMS and that FCKANTMS values in melts of
mafic lithology are either higher or lower than those in melts of primitive FCMS in distinguishing phologopite‐peridotite melts from mafic source
mantle‐like lherzolite. The data sources and the purpose of linear regression melts. For example, melts of phlogopite‐lherzolite BriPhl produced at
for melts derived from different sources are the same as in Figure 1. 3 GPa (Condamine et al., 2016) have FCKANTMS of 0.03 ± 0.14 (SD,
n = 6) which is significantly lower than FCMS of 0.22 ± 0.13 (SD,
n = 6). Thus, the compositional difference between melts of lherzolite and mafic lithology in the
FCKANTMS space is greater than that in the FCMS space (Figures 1b and 3b). This result suggests that
FCKANTMS is better than FCMS for identifying the source lithology of basaltic melts (see section 3.2.2
for further discussions).
As shown in Figure 4, experimental batch melts derived from typical hornblendite, pyroxenite, and peri-
dotite all have lower ln (CaO/TiO2) than their source materials, indicating that Ti is more incompatible
than Ca during partial melting. Specifically, melts derived from the pyroxenites and the hornblendite
have the maximum and minimum variations in ln (CaO/TiO2), respectively, and peridotite melts vary
between the other two melt types (Figure 4). This compositional pattern is mainly caused by different
Ca/Ti partitioning between amphibole (high‐Ca pyroxene) and melts (DCa/Ti = MineralCa/Ti/MeltCa/Ti),
and amphibole has significantly lower DCa/Ti than high‐Ca pyroxene (e.g., Pilet et al., 2008; Pilet et al.,
2010). Collectively, amphibole‐rich sources can produce melts with ln (CaO/TiO2) resembling that of their
Additionally, all the logratios used in FCMS and FCKANTMS in fact represent transformations of Alr and
Clr (see Appendix A). For example, ln (FeO/CaO) = ln (FeO/SiO2) − ln (CaO/SiO2), where ln (FeO/SiO2)
and ln (CaO/SiO2) are Alrs (Aitchison, 1986). If a number of high‐precision experimental melts are obtained
in the future, logratio‐based discriminant function analysis, and especially isometric‐logratio‐based
Figure 5. FCKANTMS (a) and FCMS (b) versus Mg# of evolved typical experimental melts of mafic lithology and perido-
tite due to fractional crystallization and accumulation. Olivine addition (L − Ol) and subtraction (L + Ol) with 1 wt%
increments shown in (a) and (b) are calculated using the software PRIMELT2 (Herzberg & Asimow, 2008), assuming
Fe2O3/TiO2 = 1 for red filled circles and Fe2O3/TiO2 = 0.5 for green filled circles. For low‐Mg# (<0.5) melts of mafic
lithology, even more than 30 wt% olivine addition still cannot produce Mg# of 0.7 such as that in equilibrium with typical
mantle olivine. The average errors for experimental melts are estimated using the same method as in Figure 2. The data
sources are the same as in Figure 1.
(Egozcue et al., 2003) work, may reveal much more information about the nature of the compositional
pattern of basaltic melts in a stricter mathematical form.
Mg# melts of peridotite, high‐Ca pyroxene commonly cannot crystallize until Mg# decreases to 0.5–0.6 after
significant amount of olivine crystallization, and in this case, at a given Mg#, FCKANTMS and FCMS in
melts derived from mafic lithology in general are significantly higher than those in highly evolved melts
derived from peridotite (see an example in section 5). When high‐pressure fractionation occurs, high‐Ca pyr-
oxene can become the liquidus phase and crystallize simultaneously with olivine, and under such circum-
stances, high‐pressure fractionation might approximate the partial melting trend in the relations between
FCKANTMS and FCMS and Mg#. For natural basalts, FCKANTMS and FCMS could be combined with
MgO content and other major or trace element ratios to clarify the potential influence of high‐Ca pyroxene
involved fractional crystallization, especially for a suite of cogenetic basaltic rocks (see an example in
section 5). Fully understanding the effect of complex fractional crystallization processes on the major ele-
ment patterns in basalts, though important, is beyond the scope of our current theoretical work, but such
processes should be considered cautiously when using FCKANTMS and FCMS to identify source composi-
tional and lithological heterogeneities of any natural basalts.
Figure 6. Olivine modal abundance versus Mg# (a) and FeO versus MgO (b) of experimental mafic and peridotitic mate-
rials. Olivine modal abundance is calculated by the empirical equation Ol (wt%) = 144.27ln((Fe + Mg + Ca + 2Na)/Si)
(molar, ratio), which is slightly higher than thermodynamic results (Yang et al., 2016). Using the relationship between
olivine modal abundance and Mg#, the experimental rocks and/or the synthetic mixtures are grouped into three types of
lithology, namely, peridotite, transitional lithology, and mafic lithology. Peridotite has Mg# > 0.89 and model olivine
modal abundance >50 wt%. Mafic sources have Mg# < 0.85 or model olivine modal abundance <30 wt%. Transitional
lithology has the intermediate compositional features 0.85 < Mg# < 0.89 and olivine modal abundance >30 wt% or
Mg# > 0.85 and olivine modal abundance 30–50 wt%. Parameterized samples are used in Figures 1 and 2 to derive FCMS
and FCKANTMS. The fields of natural mafic lithology (blue curve) and mantle peridotite (green curve) shown in the FeO‐
MgO diagram are after (Lambart et al., 2013). For detailed discussions of the relationship between lithology and bulk
compositions, see the main text. The experimental materials with olivine modal abundance <0–5 wt% are silica‐excess
pyroxenite (i.e., secondary olivine‐free pyroxenite and eclogite). All the experimental bulk compositions are presented in
Table S1. The data are from Baasner et al. (2016), Bartels et al. (1991), Borghini et al. (2017), Conceicao and Green (2004),
Condamine and Médard (2014), Condamine et al. (2016), Dasgupta et al. (2007, 2006, 2013), Davis et al. (2013, 2011),
Draper and Johnston (1992), Dvir and Kessel (2017), Falloon and Danyushevsky (2000), Foley et al. (2009), Funk and Luth
(2013), Gaetani and Grove (1998), Gerbode and Dasgupta (2010), Ghosh et al. (2014), Grove et al. (2013), Hirose and
Kawamoto (1995), Hirose and Kawamura (1994), Hirose and Kushiro (1993), Hirose and Kushiro (1998), Hirose (1997a,
1997b), Hirschmann et al. (2003), Keshav et al. (2004), Kessel et al. (2015), Kinzler (1997), Kinzler and Grove (1992a),
Kogiso and Hirschmann (2006), Kogiso et al. (1998), Kushiro (1996), Lambart et al. (2009a, 2009b), Laporte et al. (2014,
2004), Longhi (2002), Mallik et al. (2016, 2015), Medard et al. (2006), Mitchell and Grove (2015), Parman and Grove (2004),
Pertermann and Hirschmann (2003), Pickering‐Witter and Johnston (2000), Pilet et al. (2008), Salters et al. (2002), Schwab
and Johnston (2001), Sobolev et al. (2007), Sorbadere et al. (2013), Spandler et al. (2008), Tenner et al. (2012), Ulmer and
Sweeney (2002), Wagner and Grove (1998), Walter (1998), Wasylenki et al. (2003), Whitaker et al. (2007), Yaxley and
Green (1998), and Yaxley and Sobolev (2007).
natural peridotite, respectively. The transitional lithologies have MgO values of 26–44 wt%, and in the MgO‐
FeO relation, they plot either in the field of natural mafic lithology or in the field of natural peridotite
(Figure 6b). This result suggests that lithology separation using Mg# and olivine modal abundance is in
good agreement with natural observations. In fact, the current lithological distinction between mafic
lithology and peridotite may not always hold at various temperatures and pressures, but the lithology
separation shown in Figure 6a, from a statistical perspective, can constrain the overall compositional
characteristics of each lithology and also help us to explore the distinction in the major element patterns
of melts derived from different lithologies.
have FCKANTMS of −0.21 ± 0.21 (SD), which is lower than values for the solidus melts of typical PM‐like
lherzolite (FCKANTMS = 0.00 ± 0.08 [SD]) (Figure 3b). In contrast, the FCKANTMS values in melts of the
transitional lithology do not show a statistically significant correlation with melting degree (R2 < 0.05), and
the linear regression solidus melts have FCKANTMS of 0.13 ± 0.23 (SD), which is higher than that for melts
of peridotite (Figure S2a). Melts of the mafic lithology show a slight negative correlation between
FCKANTMS and melting degree, and the linear regression solidus melts have FCKANTMS of 0.47 ± 0.35
(SD), which is significantly higher than those for melts of both peridotite and transitional lithologies.
Compared with the above volatile‐free and hydrous melts, melts of the carbonated peridotite, the carbonated
transitional lithology, and the carbonated mafic lithology display large variations in FCKANTMS at given
melting degrees, and the linear regression solidus melts of the three carbonated lithologies all have lower
FCKANTMS than their volatile‐free and hydrous counterparts (Figure S2a). This result is mainly due to
the fact that carbonated silicate melts derived from carbonated lithologies have significant contributions
from carbonatitic melts characterized by extremely low FCKANTMS. However, some melts of the carbo-
nated mafic lithology have higher FCKANTMS than melts of volatile‐free mafic lithology because Fe‐Ti oxi-
des might become the most fusible phases during partial melting of carbonated eclogite and result in near‐
solidus melts with extremely high FeO (>20%) and high TiO2 (>10%) contents (Dasgupta et al., 2006).
3.2.2. Relationship Between FCMS and FCKANTMS
The relationships between FCMS and the melting degree for melts of the six lithologies shown in Figure S2b
are generally very similar to those for FCKANTMS (Figure S2a). Nevertheless, some significant differences
need to be addressed. The SD of the difference between the linear regression FCMS and the experimental
FCMS for melts of the peridotite is significantly higher than that for FCKANTMS, although the two values
are very similar for melts of the mafic lithology and the transitional lithology. This outcome is consistent
with the results for melts of typical peridotite used originally for parameterization (Figures 1b and 2b) where
FCKANTMS values are more homogeneous than those for FCMS. Moreover, the difference between FCMS
in regression solidus melts of the mafic lithology and the transitional lithology is smaller than that for
FCKANTMS (Figure S2), suggesting that FCKANTMS is a more powerful marker for distinction between
the two source melts. For all the experimental melts, FCMS and FCKANTMS show significantly positive lin-
ear relations and have similar ability for identification of the source lithology of basalt because they are all
strongly controlled by the polynomial relations between ln (FeO/CaO) and ln (MgO/SiO2) (equations (2) and
(9)), and their difference is 0.01 ± 0.10 (SD, n = 929; Figure S3). Therefore, for melts without any one com-
ponent of K2O, Na2O, TiO2, and Al2O3, FCKANTMS could be replaced by FCMS, but caution should be paid,
especially from a quantitative perspective, because these values may sometimes show significant differences
(Figure S3). A major difference is that FCKANTMS has fewer temperature and pressure effects than FCMS.
Given the above analysis and the fact that most experimental basaltic melts, especially high‐precision experi-
mental results obtained in recent years, have all eight components FeO, CaO, MgO, SiO2, K2O, Na2O, TiO2,
and Al2O3, discussions about the implications of pattern recognition for major elements of experimental
basaltic melts are focused on FCKANTMS but also generally hold true for FCMS.
3.2.3. The Upper Limit of FCKANTMS in Melts of Normal Peridotite and Transitional Lithology
We note that melts of olivine pyroxenite HK‐66 have FCKANTMS with a mean of 0.37 (SD = 0.08, n = 13;
Hirose & Kushiro, 1993), which is higher than the values for most melts of the transitional lithology and sig-
nificantly higher than those for melts of typical peridotite. Thus, 0.37 could be considered as the approximate
upper limit of FCKANTMS for melts of peridotitic (normal and low‐Mg# fertile peridotite) sources (Figures 7
and S2a). This boundary is similar to the FC3MS of 0.65 that has been proposed as the upper limit for melts of
peridotite (Yang & Zhou, 2013). Nevertheless, as discussed in section 4.6, FCKANTMS is more powerful than
FC3MS for identifying the source lithology of basalts. The upper limit of FCKANTMS in melts of normal
lherzolite (Mg# > 0.89) is estimated at 0.05 ± 0.10 (Figure 7 and Figure S2a) because PM‐like lherzolite
(Mg# = 0.892–0.896) melts have FCKANTMS of 0.00 ± 0.08 (SD, n = 53; Davis et al., 2011; Hirose &
Kushiro, 1993; Laporte et al., 2014; Walter, 1998), which is slightly lower than the FCKANTMS of
0.06 ± 0.13 (SD, n = 4) in melts of two fertile lherzolites PS6.1 and KPS2.1 (Mg# = 0.881; Davis &
Hirschmann, 2013).
The experimental melts of all the lithologies that may be present in the source regions of natural basalts are
batch melts, and their major element patterns cannot be directly compared with those of natural basaltic
melts because the latter is near‐fractional melts (e.g., Johnson et al., 1990; Kelemen et al., 1997). However,
4.1. Fe/Mn
Experimental petrology suggests that Fe/Mn partitioning between major rock‐forming minerals of lherzolite
and melt (DFe/Mn = MineralFe/Mn/MeltFe/Mn) has the following relation: olivine > 1 > orthopyroxene > clino-
pyroxene ≈ garnet (e.g., Davis et al., 2013; Le Roux et al., 2010; Walter, 1998). Thus, many studies assume
that lherzolite partial melting cannot significantly fractionate the Fe/Mn ratio in either melt or source,
and Fe/Mn in melts of lherzolite should be mainly controlled by the source Fe/Mn (e.g., Humayun et al.,
2004; Sobolev et al., 2007). For near‐solidus partial melting, low‐pressure melts are in equilibrium with spi-
nel lherzolite mineral assemblages, while high‐pressure melts are in equilibrium with garnet lherzolite
mineral assemblages. The bulk DFe/Mn of garnet lherzolite is lower than that of spinel lherzolite, which pro-
duces Fe/Mn in high‐pressure melts generally 2–10 higher than those of low‐pressure melts of a given lher-
zolite source (Balta et al., 2011; Davis et al., 2013; Niu et al., 2011; Yang et al., 2016). This pressure effect has
not been carefully considered when using Fe/Mn in Hawaiian lavas to infer Mg# in source materials
(Humayun et al., 2004). On the other hand, because mantle peridotites exhibit large variation in Fe/Mn
(50–70) when Mg# ranges from 0.88 to 0.91 (Le Roux et al., 2010), Fe/Mn in peridotite‐derived melts still
may not reflect Mg# in the source even if the pressure effect is very small. Recent experimental petrology
on a phlogopite‐bearing lherzolite (Condamine et al., 2016) and two CO2‐H2O‐bearing lherzolites
(Baasner et al., 2016) in the garnet stability field produced melts with Fe/Mn ratios significantly higher than
those in melts of PM‐like lherzolite, although high Fe/Mn in the melts was mainly due to their high Fe/Mn
sources (Figure 8a). Thus, although Fe/Mn ratio in basalts might reflect contributions from high Fe/Mn
Figure 8. Fe/Mn variation as a function of melting degree in experimental batch melts of typical peridotite (PER.),
pyroxenite (PX.), and horblendite (HBL.) in (a) and the relationships between FCKANTMS and ln (SiO2/
(CaO + Na2O + TiO2)) and FeO versus SiO2 for the same experimental melts in (b) and (c), respectively. Small white filled
circles in (b) and (c), equilibrium olivine subtraction and accumulation trends with 1% increments that are calculated
using the same method as in Figure 1. Arrows marked with +CO2 in (b) and (c), compositional trends of carbonated
peridotite melts. Arrows marked with low P and high P in (c) indicate compositional trends of low and high pressure
peridotite melts, respectively. Gray arrows in (b) indicate compositional trends with decreasing melting degree for melts
derived from mafic lithology and peridoitite. For peridotite melts plotted in (b), >25% olivine fractional crystallization
can only slightly increase and decrease FCKANTMS and ln (SiO2/(CaO + Na2O + TiO2)), respectively. Similarly, for melts
of mafic lithology, olivine addition or subtraction cannot significantly change their compositional patterns in the rela-
tionship between FCKANTMS and ln (SiO2/(CaO + Na2O + TiO2)). Red filled circles in (b) and (c) represent a dynamic
melting process, where a 4.5‐GPa lherzolite melt (sample 45.03 from Walter, 1998) first undergoes 13% olivine fractional
crystallization with Mg# decreasing to 0.7 during ascending to the lithospheric mantle; then, the evolved melt reequili-
brates with harzburgite, dissolving orthopyroxene (L + Opx) and crystallizing olivine until Mg# = 0.7. The melt produced
by this dynamic melting process is similar to that from the model of Wagner and Grove (1998), which, at a given FeO
content, has higher SiO2 content than direct partial melts of lherzolite as shown in (c) but still preserves the compositional
pattern of peridotite melts in logratio‐based space as shown in (b). Note that the orthopyroxene used to assimilate the
peridotite melts is an experimental orthopyroxene BPC‐63 (Wagner & Grove, 1998) with Mg# of 0.88, but natural
orthopyroxene in lithospheric harzburgite should have Mg# significantly higher than 0.88, and in this case, the dynamic melts
in equilibrium with high‐Mg# harzburgite have lower FCKANTMS and higher ln (SiO2/(CaO + Na2O + TiO2)) (not shown)
than our current calculated melt shown in (b). Other details see caption to Figure 7. Peridotite melts include anhydrous
lherzolites KR4003 (Walter, 1998) and MBK+ (Laporte et al., 2014), carbonated hydrous lherzolites + CH (Lherz 0.4H 0.4C
and Lherz 0.7H 0.7C; Baasner et al., 2016), and phlogopite‐bearing lherzolite BriPhl and phlogopite‐bearing harzburgite
HzbPhl (Condamine et al., 2016). Mafic lithology melts include hornblendite AG4 (Pilet et al., 2008) and silica‐deficient
pyroxenites M5‐103 (Lambart et al., 2009a). MIX1G (Hirschmann et al., 2003; Kogiso et al., 2003), and 77SL‐582 (Keshav et al.,
2004). The average errors for experimental melts in (b) are estimated using the same method as in Figure 2.
melts of mafic lithology (Liu et al., 2008; Sobolev et al., 2007), these ratios can also be explained as the result
of variations in source composition and/or melting conditions (Balta et al., 2011; Davis et al., 2013; Niu et al.,
2011; Yang et al., 2016).
We note that experimental low to moderate degree partial melts of hornblendite AG4 exhibit slightly lower
Fe/Mn ratios than those in the source, and they are generally similar to those in PM‐like lherzolite melts and
significantly lower than those in typical pyroxenite melts (Figure 8a). Because DFe/Mn of amphibole is com-
monly >1 (Adam & Green, 2006; Pilet et al., 2008), amphibole‐rich peridotitic and mafic lithologies can pro-
duce melts with Fe/Mn ratios either indistinguishable from or lower than those in typical peridotite‐derived
melts, depending on the source Fe/Mn and residual mineralogy. In summary, the Fe/Mn ratio in basalts in
fact can hardly be used to infer source lithology and source Mg# if the above uncertainties are not carefully
considered and constrained (Table 2). However, the uncertainties can be largely resolved in the FCKANTMS
space, especially when combined with ln (SiO2/(CaO + Na2O + TiO2)) (Figure 8b). The FCKANTMS values
in melts of mafic lithology, at a given ln (SiO2/(CaO + Na2O + TiO2)), are mostly higher than the values in
melts of peridotite. Interestingly, high FCKANTMS and low or normal Fe/Mn ratios might be used to iden-
tify melts of amphibole‐rich sources, as shown in Figures 8a and 8b.
4.2. FeO‐SiO2
Many experimental petrological studies suggest that the FeO‐SiO2 relation for melts of anhydrous peridotite
is mainly controlled by melting pressure, and a strong negative correlation occurs between SiO2 and FeO
contents (Kushiro, 2001; Laporte et al., 2014; Walter, 1998). Melts of mafic lithology can also produce the
FeO‐SiO2 relation, but at a given FeO content, these melts have larger variations in SiO2 content than melts
of typical peridotite (Figure 8c). Because of this feature, high SiO2 and high FeO or low SiO2 and high FeO
have been considered as potential chemical markers for pyroxenite contribution (Dasgupta et al., 2010;
Lambart et al., 2013). However, experimental studies suggest that low‐SiO2 and high‐FeO melts can also
be produced from carbonated lherzolite at garnet‐stable pressure (Baasner et al., 2016) or from hornblendite
(Pilet et al., 2008; Figure 8c), as noted by Lambart et al. (2013). Thus, low SiO2 and high FeO can hardly dis-
tinguish melts of peridotite from melts of mafic lithology. Nevertheless, low‐SiO2 and high‐FeO melts of car-
bonated peridotite and mafic lithologies can mostly be separated from each other using the relationships
between FCKANTMS and ln (SiO2/(CaO + Na2O + TiO2)) (Figure 8b).
Production of high‐SiO2 and high‐FeO melts has been suggested to occur by a dynamic melting model in
which high‐pressure melts of lherzolite reequilibrate with harzburgite at low pressure, dissolving orthopyr-
oxene and crystallizing olivine, in a process proposed in many studies as an important petrogenetic model
for Hawaiian lavas (e.g., Putirka et al., 2011; Wagner & Grove, 1998). We note that melts produced in the
dynamic model have higher CaO contents than typical Hawaiian lavas at a given MgO content, as noted
by Wagner and Grove (1998). As we discussed above, however, both peridotite and mafic lithologies can pro-
duce melts with either high CaO or low CaO features, and the two melts are indistinguishable in the CaO‐
MgO relation if source compositional heterogeneities exist. Moreover, a mixture of three experimental melts
of H154 (Kinzler & Grove, 1992a), T‐762 (Falloon et al., 1988), and T‐3572 (Falloon & Danyushevsky, 2000)
has been suggested to support the idea that peridotite‐derived melts can have a high‐SiO2 and high‐FeO sig-
nature (Putirka et al., 2011), but melt H154 is derived from a pyroxenite source with Mg# = 0.72 and
MgO = 13.1, and the high‐FeO (11.2%) melt T‐762 was possibly contaminated by the iron capsule because
this melt has the highest FeO content within all the experiments of Falloon et al. (1988). Thus, such a mix-
ture cannot represent peridotite‐derived melt.
Our simple calculation suggests that a high‐pressure melt of PM‐like lherzolite reequilibrates with harzbur-
gite at low pressure, dissolving orthopyroxene and crystallizing olivine, and can produce a melt with higher
FeO content than direct partial melts of lherzolite at a given SiO2 content (Figure 8c); such a melt would be
similar to the high‐FeO and high‐SiO2 melts of pyroxenite MIX1G but still preserve the major element pat-
tern in melts of peridotite and can be distinguished from melts of mafic lithology in the relationships
between FCKANTMS and ln (SiO2/(CaO + Na2O + TiO2)). Additionally, melts of olivine websterite M5‐
103 and typical peridotite show indistinguishable patterns in the FeO‐SiO2 relation; they are also very simi-
lar for many other major elements (Al2O3, CaO, and MgO; Lambart et al., 2009a), but they are significantly
different in the plot of FCKANTMS and ln (CaO/TiO2) (Figure 5).
4.3. MgO‐Al2O3
It has been suggested that many low Al2O3 OIBs cannot be produced
from a typical peridotite source, requiring contributions from high‐
pressure pyroxenite‐derived melts (Hirschmann et al., 2003; Kogiso
et al., 2004), and the Al2O3‐MgO relation has often been used to support
this argument in terms of major element patterns (Kogiso, 2007; Kogiso
& Hirschmann, 2006; Mallik & Dasgupta, 2012). A careful comparison
between the experimental melts of pyroxenite MIX1G and lherzolite
KR4003 suggests that high‐pressure (3–4.5 GPa) partial melts of lherzolite
can readily explain the Al2O3‐MgO relation of OIBs if various degrees of
olivine fractional crystallization occur; a similar conclusion has been
reached by Davis et al. (2011), although near‐solidus melts of pyroxenite
MIX1G have lower Al2O3 than melts of lherzolite KR4003 at 5 GPa
(Figure 9). We note that the Al2O3 concentrations in near‐solidus melts
of lherzolite at 3 to 4 GPa decrease significantly with small variations
in MgO concentration owing chiefly to the expanding stability field of
garnet (Walter, 1998). On the other hand, melts of Lherz 0.4H 0.4C at
Figure 9. Al2O3 versus MgO in experimental batch melts of pyroxenite
MIX1G (Hirschmann et al., 2003, Kogiso et al., 2003), lherzolite KR4003 2.8 GPa have significantly lower Al2O3 contents than melts of anhydrous
(Walter, 1998), and carbonated hydrous lherzolite Lherz 0.4H 0.4C (Baasner KR4003 at 3 GPa, suggesting that small amounts of H2O and CO2 present
et al., 2016); also shown are alkalic and tholeiitic OIBs after (Kogiso, 2007). in a peridotite source could dramatically change the Al2O3‐MgO relation.
Dashed, bold black and blue lines are estimated solidus melts for MIX1G Thus, melts of pyroxenite and peridotite should have indistinguishable
and KR4003, respectively. Black arrows marked with L‐Ol, olivine fractional
crystallization trends. major element patterns in the Al2O3‐MgO relation if melting conditions
(volatiles, pressure, and melting degree) cannot be determined
independently. In this case, however, they show significantly different major element patterns in the
FCKANTMS space (Figure 8b).
4.4. CaO‐MgO
It has been suggested that production of batch melts and initiation of fractional melts at pressures >2.5–
3 GPa of PM‐like lherzolite generally have higher CaO contents at a given MgO content than those for
pyroxenite‐derived melts (Herzberg, 2006; Herzberg & Asimow, 2008); thus, the CaO‐MgO relation has been
widely used to identify the source lithology of basalts (Yang et al., 2016, and references therein). Although
some melts of pyroxenite indeed have lower CaO contents than melts of typical lherzolite at a given MgO
content (Figure 10a), some pyroxenite‐derived melts, such as melts of pyroxenite MIX1G and 77SL582, have
high CaO contents and would be erroneously considered peridotite‐derived melts based on the CaO‐MgO
relation (Figure 10a), as noted by Herzberg and Asimow (2008). Another important but often neglected issue
is that low‐CaO basaltic melts can also be produced from peridotite sources and that CaO contents in alka-
line melts derived from iron‐rich and/or alkaline‐rich peridotite are significantly lower than the values in
alkaline‐poor melts derived from typical lherzolite (see detailed discussions in Yang et al., 2016; Yang &
Zhou, 2013), which has also been supported by the recent experimental partial melts of phlogopite‐bearing
garnet lherzolite and harzburgite (Condamine et al., 2016; Figure 10a). On the other hand, low‐CaO tholeii-
tic melts can be produced from harzburgite sources and would be plotted in the pyroxenite source field in the
CaO‐MgO relation (Yang et al., 2016). Additionally, low‐pressure lherzolite‐derived melts have low CaO
contents, although they may not contribute to intraplate basalts that commonly erupted beneath thick litho-
sphere (Figure 10a). From a compositional pattern perspective, if all the peridotite‐derived melts listed above
mixed with each other, the mixed melts would then have either a high CaO or low CaO feature. In this case,
these peridotite‐derived melts could not be distinguished from melts of mafic sources (i.e., pyroxenite and
hornblendite; Figure 10a). However, this difficulty can be largely resolved in the FCKANTMS space, espe-
cially in the relationship between FCKANTMS and ln (SiO2/(CaO + Na2O + TiO2)) (Figure 8b).
Figure 10. Major element patterns of the same experimental melts shown in Figure 8 in the plots of CaO versus MgO,
CaO/Al2O3 versus FeO/Al2O3, CaO/MgO versus FeO/MgO, and FC3MS versus Mg#. The upper limit (red dashed line
in (d)) of FC3MS in peridotite melts is after Yang and Zhou (2013). Note that, at 3 GPa, compared with anhydrous lher-
zolite melts, melts of phlogopite‐bearing lherzolite and harzburgite have lower CaO, CaO/Al2O3 and CaO/MgO, and
higher FC3MS. Small white filled circles (c, d) and arrows marked with L‐Ol (a) represent olivine fractional crystallization
trends, with 1% increments in (c) and (d) that are calculated using the same method as in Figure 1. Arrow marked
with +CO2 in (b) indicates compositional trend of carbonated peridotite melts. Arrows marked with low P and
high P in (b) and (c) indicate low and high pressure melts of peridotite, respectively. The data sources and symbols of the
experimental melts are the same as in Figure 8.
high‐pressure partial melting of volatile‐free lherzolite (Walter, 1998; Figure 10b). Recent thermodynamic
calculations suggest that at the same mantle potential temperature, pyroxenite melts would have lower
CaO and higher FeO than peridotite melts (Jennings et al., 2016), and when CaO and FeO are normalized
to either MgO or Al2O3, the effect of pressure on melt composition can be reduced. However,
experimental melts of typical peridotite and pyroxenite generally show similar compositional patterns in
the plot of CaO/Al2O3 versus FeO/Al2O3, and some pyroxenite melts exhibit high CaO/Al2O3 and low
FeO/Al2O3 features that are inconsistent with the thermodynamic prediction (Figure 10b). On the other
hand, typical lherzolite at elevated pressures and phlogopite‐bearing peridotite at 3 GPa can produce low‐
CaO/MgO melts, and they show patterns similar to those from melts of mafic lithology when olivine
fractional crystallization occurs (Figure 10c). Thus, the relations of CaO/Al2O3‐FeO/Al2O3 and
CaO/MgO‐FeO/MgO might not be useful chemical markers for source lithology identification of basalts,
although they might identify source lithology for basalts with high FeO (>15%; Jennings et al., 2016). In
Figure 13. Major element characteristics of two groups of hypothetical data for basaltic bulk compositions. (a)–(g) are commonly used to recognize major element
patterns in igneous rocks. (h) and (i) are logratio‐based methods for pattern analysis of compositional data. Note that blue filled circles and orange filled circles show
indistinguishable major element pattern in (a)–(g), but their patterns can be identified in (h) and (i). All the negative correlation trends between major element
contents are spurious correlations due to 100% normalization because, apart from FeO (Mg# = 70–72), each major element concentration is randomly generated
using a normal distribution.
rocks and/or melts with different major element patterns in logratio space may show indistinguishable
patterns in subcompositional space (i.e., Harker diagrams and simple major element ratios) owing chiefly
to spurious correlations and the constant sum problem of compositional data, as noted by many
statisticians (Aitchison, 1986; Aitchison & Egozcue, 2005; Egozcue et al., 2003; Pawlowsky‐Glahn &
Egozcue, 2006); this observation can explain why melts of peridotite and mafic lithologies with low and
high FCKANTMS, respectively, are difficult to distinguish in major element content‐ and ratio‐based
analysis, as discussed in the above section. We note that FCKANTMS is a polynomial relationship of
major element logratios, suggesting that logratios other than major element contents should be regarded
as the appropriate independent variables for compositional pattern analysis, especially from a statistical
perspective, which in effect has long been recognized in the compositional data analysis field but has
Figure 14. FCKANTMS versus Mg# (a), MgO (b), ln (SiO2/(CaO + Na2O + TiO2)) (c), and ln (CaO/TiO2) (d) for selected Mauna Kea shield stage lavas and glasses.
Black arrows marked with L‐Ol‐Cpx‐Pl, fractional crystallization trends of olivine, clinopyroxene, and plagioclase. Small white filled circles, equilibrium olivine
addition or subtraction with 1% increments calculated using the same method as in Figure 1. Small green filled circles indicate addition of olivines with forsterite
contents of Fo80, Fo86, Fo88, and Fo90.5 to two evolved compositions from MK‐1 lavas and high CaO glasses, 5% increments. The dashed lines in (a)–(d) are
boundaries for melts derived from different lithologies. The dashed line marked with Mg# = 0.7 in (c) indicate the upper boundary of normal peridotite and
harzburgite melts when their Mg# = 0.7. Other detailed explanations see caption to Figure 7. Note that some MK‐1 and high CaO lavas plotted below the lower
dashed line in (c) are due to accumulation of olivines, and their Mg# (>75) and MgO contents (>20%) are too high to be in equilibrium with Fo 91.5 olivine,
the maximum observed. Olivine fractionation and accumulation cannot fractionate ln (CaO/TiO2), and for clarity, only one example is shown. Error bars in
(a)–(c) are smaller than the size of the symbol. Major element data and compositional type classification of Mauna Kea lavas and glasses are from the references
listed in the main text.
received little attention in the petrology field (Aitchison, 1986; Aitchison & Egozcue, 2005; Egozcue et al.,
2003; Pawlowsky‐Glahn & Egozcue, 2006; Rollinson, 1992; Verma et al., 2016). As suggested by many
statisticians and mathematical geologists, for pattern recognition of major and trace elements, logratios
are the best variables to use because many geological and petrological implications derived from major
element content‐based analysis may suffer from geometrical illusion, as shown in Figure 13. However,
this conclusion does not suggest that Harker diagrams should be abandoned, because this simple method
is at least very useful in lithological classification and mass balance visualization.
SiO2 (MK‐2; Rhodes & Vollinger, 2004), and high CaO type lavas (Rhodes et al., 2012), as well as high CaO
and low CaO glasses (Stolper et al., 2004). The correlation trends of FCKANTMS versus Mg#, MgO, and ln
(SiO2/(CaO + Na2O + TiO2)) for MK‐1, MK‐2, and high CaO lavas are generally consistent with fractional
crystallization and accumulation trends of olivine (Figures 14a–14c). FCKANTMS values in the three types
lavas are somewhat scatter (>0.1) at a given MgO content, and the heterogeneity is significantly higher than
the analytical precision (<0.02). The scatter in FCKANTMS values in the lavas can be ascribed to accumula-
tion of olivines with forsterite content of Fo 80–90.5 as all the lavas contain only olivine phenocryst.
However, large variations in ln (CaO/TiO2) for MK‐1, MK‐2, and high CaO lavas suggest that their primary
magmas should have significant compositional heterogeneity because fractional crystallization and accumu-
lation of olivine cannot fractionate ln (CaO/TiO2) (Figure 14d). FCKANTMS and ln (CaO/TiO2) values in
low CaO and high CaO glasses with MgO > 7% are very similar to those of MK‐1 lavas and high CaO lavas
with MgO < 18%, respectively. Both high CaO and low CaO glasses with MgO < ~7% show elevated
FCKANTMS values along with decrease in Mg#, MgO contents, and ln (CaO/TiO2) values, indicative of oli-
vine, clinopyroxene, and plagioclase fractionation. However, similar correlation trends may also occur for
primary melts derived from mafic lithologies (Figures 4 and 12), and in such case, trace element pattern ana-
lysis can be helpful.
Because Mauna Kea lavas contain olivine with a maximum forsterite content of Fo 90.5, the primary mag-
mas of MK‐1 and MK‐2 lavas and low CaO glasses are estimated to have Mg#, 0.72–0.74, MgO, 16–19 wt%
(Herzberg, 2006; Rhodes et al., 2012). These primary magmas have FCKANTMS values of 0.35–0.47 which
are higher than those of melts derived from normal peridotite and transitional lithology (Figures 14a and
14b). Melts derived from harzburgite may have high FCKANTMS values, but their FCKANTMS still too
low at a given ln (SiO2/(CaO + Na2O + TiO2)) value. Hence, based on our statistical model in the logratio
space, the primary magmas of MK‐1 and MK‐2 lavas and low CaO glasses should be derived from a mafic
lithology source. The mafic lithology can be either an olivine‐free pyroxenite or an olivine‐bearing pyroxe-
nite because our model cannot distinguish them (see discussions in section 3). Notably, the high
FCKANTMS features in MK‐1 and MK‐2 lavas and low CaO glasses do not solely due to their low CaO con-
tents, because CaO content in peridotite‐ and pyroxenite‐derived melts can be indistinguishable (i.e., either
high or low) at a given MgO content as discussed in section 4.4, but melts derived from the two sources can
be identified in the FCKANTMS space, especially when combined with ln (SiO2/(CaO + Na2O + TiO2)).
Mixing between normal peridotite melts and dacitic magmas derived from garnet pyroxenite or eclogite
may also produce melts with high FCKANTMS values, and in this case, high SiO2 mixtures should have
higher FCKANTMS values than low SiO2 mixtures, which, however, is inconsistent with that MK‐1 high
SiO2 and MK‐2 low SiO2 lavas have indistinguishable FCKANTMS value.
In contrast, high CaO lavas and glasses have lower FCKANTMS values than other compositional types of
Mauna Kea lavas (Figures 14a–14d), and all have higher FCKANTMS values than normal peridotite melts
even when they corrected to magmas that can crystallize Fo 91.5 olivine, the maximum observed in
Hawaiian lavas (Herzberg et al., 2007). FCKANTMS values in the primary magmas of high CaO lavas and
glasses are estimated to range from 0.09 to 0.27, which are higher than the upper boundary for melts of nor-
mal peridotite (Figures 14a and 14b). Although harburgite melts may contribute to the high FCKANTMS
features, all high CaO lavas and glasses, when corrected to Mg# = 70 by olivine addition or subtraction,
are plotted above the upper boundary of peridotite melts in Figure 14c. Hence, based on our statistical
model, the primary magmas of high CaO lavas and glasses should be derived from a transitional lithology
or a mafic lithology. Note that the transitional lithology could be an olivine pyroxenite or a fertile peridotite
with Mg# < 0.89. If the trace element pattern of high CaO lavas and glasses can only be explained by a mix-
ture of a low degree partial melt of a normal mantle peridotite and a high degree partial melt of a mafic
cumulate (Huang & Humayun, 2016), the high FCKANTMS features (0.09–0.27) should be generated
through such magma mixing process because FCKANTMS value in high degree partial melts of pyroxenite
also higher than normal peridotite melts (Figure 3b).
6. Conclusions
1. A parameter called FCMS (FCMS = ln (FeO/CaO) − 0.058 * (ln (MgO/SiO2))3 − 0.636 * (ln (MgO/
SiO2))2 – 1.850 * ln (MgO/SiO2) − 1.170, all the major elements in weight percent) is proposed to
identify the source lithology of basaltic melts. When logratios of ln (K2O/Al2O3), ln (TiO2/Na2O), and ln
(Na2O/K2O) are incorporated into FCMS, the temperature and pressure effects on the compositional het-
erogeneity of melts of peridotites can be significantly reduced, and a more powerful parameter called
FCKANTMS (FCKANTMS = ln (FeO/CaO) − 0.08 * ln(K2O/Al2O3) − 0.052 * ln (TiO2/
Na2O) − 0.036 * ln (Na2O/K2O) * ln (Na2O/TiO2) − 0.062 * (ln (MgO/SiO2))3 – 0.641 * (ln (MgO/
SiO2))2 – 1.871 * ln (MgO/SiO2) − 1.473, all the major elements in weight percent) can be obtained.
Olivine fractional crystallization and accumulation, although they can significantly change most major
element contents and ratios, in most cases increase or decrease FCMS and FCKANTMS by only 0–
0.15, which is one order of magnitude lower than the variations in primary experimental melts of differ-
ent lithologies.
2. To determine whether FCKANTMS and FCMS can be used to identify the source lithology of basalts
when source compositional heterogeneity occurs, the experimental source materials are divided into
three types of lithology using Mg# (MgO/(MgO + FeOT), molar ratio) and model olivine modal abun-
dance (Ol (wt%) = 144.27ln((Fe + Mg + Ca + 2Na)/Si) (molar, ratio)). Experimental bulk compositions
with Mg# > 0.89 and olivine modal abundance >50 wt% are grouped into peridotite, compositions with
Mg# < 0.85 or olivine modal abundance <30 wt% are grouped into the mafic lithology, and those com-
positions in between are grouped into the transitional lithology. The FCKANTMS values in low to mod-
erate degree (F < 60%) experimental batch melts of different lithologies under both volatile‐free and
volatile‐bearing conditions generally show normal distributions and are significantly different from each
other at the 95% confidence level, except that melts of carbonated mafic lithology show statistically simi-
lar FCKANTMS (α > 0.05) values as melts of transitional and mafic lithologies. Harzburgite may produce
melts with very high FCKANTMS, and these melts may be erroneously regarded as derived from mafic
lithology, but they can be readily identified using FCKANTMS combined with ln (SiO2/
(CaO + Na2O + TiO2)). Importantly, approximately 80% and 50% low to moderate degree (F < 60%) melts
(n = 303) of mafic lithology (with or without volatiles in source materials) have higher FCKANTMS than
the upper limits for melts of peridotite and transitional lithologies, respectively, suggesting that for near‐
fractional melts, identification of source lithology can also be achieved in the FCKANTMS space. Further
statistical analysis of logratio‐based parameters of experimental melts may be useful to quantitatively
understand the major element patterns of fractional melts.
3. FCMS is very close to FCKANTMS, and they have similar abilities with respect to the source lithology
identification of basalts; thus, FCKANTMS could be estimated by FCMS for melts without the compo-
nents K2O, Al2O3, Na2O, and TiO2, but FCKANTMS should be given priority because it has fewer tem-
perature and pressure effects.
4. For identification of the source lithology of basalts, the uncertainties in the literature chemical markers
parameterized by major element contents, ratios, and phase relations can be largely reduced in the
FCKANTMS space, especially when combined with ln (CaO/TiO2) and ln (SiO2/
(CaO + Na2O + TiO2)). As suggested by many statisticians and mathematical geologists, the mathema-
tical problems (i.e., spurious correlations and constant sum) of compositional data analysis that have
long been overlooked in the fields of petrology and geochemistry should be, and could be, avoided by
using the logratio method. However, this conclusion does not suggest that traditional major element
content‐based analysis should be abandoned, because the simple method is at least very useful in litho-
logical classification and mass balance visualization.
5. The logratio‐based chemical markers are applied on Mauna Kea shield stage lavas and glasses. We find
that high SiO2 and low SiO2 lavas and glasses should be derived from a mafic lithology source. The mafic
lithology can be either an olivine‐free pyroxenite or an olivine‐bearing pyroxenite. High CaO lavas and
glasses should be derived from a transitional lithology or a mafic lithology, or they are generated by mix-
ing between normal peridotite melts and pyroxenite melts. The transitional lithology can be an olivine
pyroxenite or a fertile peridotite with Mg# < 0.89.
Appendix A
A1. Why Standard Statistical Techniques Cannot Be Applied on Compositional Data in Raw Form
Compositional data are data whose components represent a relative contribution of different parts to a
whole. They are usually expressed as percent, per mille, or parts per million, which sum to a constant
value (100, 1,000, or 106). This means that, given values for N − 1 variables, the Nth value is automatically
determined. The constant sum constraint forces at least one covariance (and thus at least one correlation
coefficient between components) to be negative. Correlation coefficients between raw components of com-
positional data are not free to range from −1 to +1. Consider a two‐part composition summing to a constant:
The correlation between the two components in this composition must be −1. For any system with more
than two components, any correlation coefficient will be affected to an unknown degree by spurious effects
induced by the constant sum constraint. The covariance relationships between components in a subcompo-
sition are not the same as they are in the full composition, and there is no relationship between the two cov-
ariance structures. This is known as subcompositional incoherence (Aitchison, 1986). As emphasized in the
main text (section 1.2), major element contents in a basalt relative to a four components system are intrinsi-
cally higher than those relative to a 10 components system. Rock (1988) described many problems that arise
in treating raw compositional data with standard statistical techniques that developed for unconstrained
variables: (1) Trends and clusters on petrological ternary and principal components diagrams can have little
or no geological significance; (2) skewness and leptokurtosis can be induced by closure; (3) dendrograms
obtained from cluster analysis can be severely biased; (4) some results from discriminant analysis can be illu-
sory; (5) multivariate methods can lead to unstable or sometimes erroneous results; (6) confidence limits or
values within a certain range can differ from those expected from Normally distributed data; and (7) con-
touring can be dangerous especially in three‐component systems.
A2. Using Logratio
Aitchison (1986) recognized that it is the relative variations of components, rather than their absolute
values, that provide the key to analyzing compositional data and developed an approach based on logratios.
There are three coordinates that can be used to analyze compositional data. (1) The Alr coordinates are sim-
ple: D − 1 of the components are divided by the remaining component and logarithms taken (Aitchison,
1986). (2) The Clr coefficients are produced by dividing the components by the geometric mean of the parts
and then taking logarithms. They are not as simple to interpret as the Alr coordinates, but they are still real
variables (Aitchison, 1986). (3) The isometric‐logratio coordinates are more complex, and there are different
rules on how to generate them (Egozcue et al., 2003). The resulting logratios are real variables that can be
analyzed using standard statistical techniques. The analyst must choose the most suitable transformation
for each given problem by taking into account their respective advantages and limitations. Nowadays, com-
positional data analysis commonly includes three steps: the representation of data in logratio type coordi-
nates; the statistical analysis of the coordinates as real random variables; and the interpretation of resulting
models either in coordinates or expressing the results in terms of the original units. Many software
packages are now available for the analysis of compositional data. For detailed discussions of the logratio
method in compositional data analysis, the reader is referred to specialist papers (Aitchison, 1986;
Aitchison & Egozcue, 2005; Egozcue et al., 2003; Pawlowsky‐Glahn & Egozcue, 2006) and
references therein.
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