crystals stirred up: 2. numerical insights into the

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Crystals stirred up: 2. Numerical insights into the formation of the earliest crust on the Moon Jenny Suckale, 1 Linda T. Elkins-Tanton, 2 and James A. Sethian 3 Received 17 February 2012; revised 7 June 2012; accepted 14 June 2012; published 11 August 2012. [1] This is the second paper in a two-part series examining the fluid dynamics of crystal settling and flotation in the lunar magma ocean. In the first paper, we develop a direct numerical method for resolving the hydrodynamic interactions between crystals and their feedback on the flow field in magmatic liquid. In this paper, we use this computational technique to test the leading model for the formation of the earliest crust on the Moon. The anorthositic lithology of the lunar crust is thought to have been formed by the flotation of buoyant plagioclase crystals at a time when the lunar mantle was still wholly or largely molten. This model is appealing from an observational point of view, but its fluid dynamical validity is not obvious, because (1) plagioclase probably started crystallizing very late (i.e., when the magma ocean was already 80% solidified) and (2) a significant portion of the shallow lunar crust consists of almost pure plagioclase (>90 vol. %), requiring very efficient plagioclase segregation. The goal of this study is to better understand the fluid dynamical conditions that hinder or facilitate crystal settling or flotation. Our approach complements earlier studies by explicitly linking the petrological and fluid dynamical evolution and by focusing on the effect of increasing crystal fraction. We find that crystal settling was probably possible throughout the entire solidification history of the lunar magma ocean as long as crystal sizes were sufficiently large (r > 1 mm) and crystal fraction sufficiently low (f < 13%). Citation: Suckale, J., L. T. Elkins-Tanton, and J. A. Sethian (2012), Crystals stirred up: 2. Numerical insights into the formation of the earliest crust on the Moon, J. Geophys. Res., 117, E08005, doi:10.1029/2012JE004067. 1. Introduction [2] The Apollo missions, the study of lunar meteorites, and remote sensing data have added critical constraints regarding the nature and age of many of the basic lithologies and landforms on the Moon and have sparked enduring progress in our understanding of the magmatic and thermal evolution of the Moon [Shearer et al., 2006]. This continued interest in the Moon is motivated not only by the desire to learn more about Earths closest companion, but also by the fact that the Moon provides a unique window to the early evolution of terrestrial planets. In contrast to Earth, where much of the primordial crust has been eradicated by tec- tonics and erosion, or other planetary surfaces that are unsampled or scantily sampled, the samples from the lunar surface provide relatively direct testimony of the processes at work during this early stage of terrestrial evolution. Refining our models of the early evolution of the Moon is thus not only important for lunar science, but for our general understanding of the evolution of terrestrial planets. [3] The abundance of plagioclase in samples from the lunar highlands first led to the hypothesis that the anortho- sitic crust might have formed through the flotation of pla- gioclase crystals in a magma ocean [e.g., Smith et al., 1970; Wood et al., 1970; Taylor and Jakes, 1974]. This idea has since been substantiated by other pieces of evidence ranging from the age of anorthosites (see Elkins-Tanton et al. [2011] for a compilation of age data) to the negative Euro- pium anomaly in mare rocks [Haskin et al., 1982; Ryder, 1982] and geophysical constraints [Solomon and Töksoz, 1973]. While the anorthositic lithologies in the lunar crust are the smoking-gun evidence in favor of plagioclase flota- tion, crystal segregation in a lunar magma ocean also pro- vides a compelling framework for relating the mare basalts to the sinking and accumulation of more dense and mafic sili- cates in the Moons mantle [Helmke et al., 1972; Philpotts et al., 1972] and for suggesting a possible origin of the incompatible-element-rich and isotopically uniform material referred to as KREEP (Potassium, Rare Earth Elements, 1 School of Engineering and Applied Science, Harvard University, Cambridge, Massachusetts, USA. 2 Department of Terrestrial Magnetism, Carnegie Institution for Science, Washington, D. C., USA. 3 Department of Mathematics, University of California, Berkeley, California, USA. Corresponding author: J. Suckale, School of Engineering and Applied Science, Harvard University, 29 Oxford St., Cambridge, MA-02139, USA. ([email protected]) ©2012. American Geophysical Union. All Rights Reserved. 0148-0227/12/2012JE004067 JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 117, E08005, doi:10.1029/2012JE004067, 2012 E08005 1 of 21

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Crystals stirred up:2. Numerical insights into the formationof the earliest crust on the Moon

Jenny Suckale,1 Linda T. Elkins-Tanton,2 and James A. Sethian3

Received 17 February 2012; revised 7 June 2012; accepted 14 June 2012; published 11 August 2012.

[1] This is the second paper in a two-part series examining the fluid dynamics of crystalsettling and flotation in the lunar magma ocean. In the first paper, we develop a directnumerical method for resolving the hydrodynamic interactions between crystals andtheir feedback on the flow field in magmatic liquid. In this paper, we use thiscomputational technique to test the leading model for the formation of the earliest cruston the Moon. The anorthositic lithology of the lunar crust is thought to have beenformed by the flotation of buoyant plagioclase crystals at a time when the lunar mantlewas still wholly or largely molten. This model is appealing from an observational pointof view, but its fluid dynamical validity is not obvious, because (1) plagioclaseprobably started crystallizing very late (i.e., when the magma ocean was already 80%solidified) and (2) a significant portion of the shallow lunar crust consists of almost pureplagioclase (>90 vol. %), requiring very efficient plagioclase segregation. The goal of thisstudy is to better understand the fluid dynamical conditions that hinder or facilitate crystalsettling or flotation. Our approach complements earlier studies by explicitly linking thepetrological and fluid dynamical evolution and by focusing on the effect of increasingcrystal fraction. We find that crystal settling was probably possible throughout the entiresolidification history of the lunar magma ocean as long as crystal sizes were sufficientlylarge (r > 1 mm) and crystal fraction sufficiently low (f < 13%).

Citation: Suckale, J., L. T. Elkins-Tanton, and J. A. Sethian (2012), Crystals stirred up: 2. Numerical insights into the formationof the earliest crust on the Moon, J. Geophys. Res., 117, E08005, doi:10.1029/2012JE004067.

1. Introduction

[2] The Apollo missions, the study of lunar meteorites,and remote sensing data have added critical constraintsregarding the nature and age of many of the basic lithologiesand landforms on the Moon and have sparked enduringprogress in our understanding of the magmatic and thermalevolution of the Moon [Shearer et al., 2006]. This continuedinterest in the Moon is motivated not only by the desire tolearn more about Earth’s closest companion, but also by thefact that the Moon provides a unique window to the earlyevolution of terrestrial planets. In contrast to Earth, wheremuch of the primordial crust has been eradicated by tec-tonics and erosion, or other planetary surfaces that are

unsampled or scantily sampled, the samples from the lunarsurface provide relatively direct testimony of the processesat work during this early stage of terrestrial evolution.Refining our models of the early evolution of the Moon isthus not only important for lunar science, but for our generalunderstanding of the evolution of terrestrial planets.[3] The abundance of plagioclase in samples from the

lunar highlands first led to the hypothesis that the anortho-sitic crust might have formed through the flotation of pla-gioclase crystals in a magma ocean [e.g., Smith et al., 1970;Wood et al., 1970; Taylor and Jakes, 1974]. This idea hassince been substantiated by other pieces of evidence rangingfrom the age of anorthosites (see Elkins-Tanton et al.[2011] for a compilation of age data) to the negative Euro-pium anomaly in mare rocks [Haskin et al., 1982; Ryder,1982] and geophysical constraints [Solomon and Töksoz,1973]. While the anorthositic lithologies in the lunar crustare the smoking-gun evidence in favor of plagioclase flota-tion, crystal segregation in a lunar magma ocean also pro-vides a compelling framework for relating the mare basalts tothe sinking and accumulation of more dense and mafic sili-cates in the Moon’s mantle [Helmke et al., 1972; Philpottset al., 1972] and for suggesting a possible origin of theincompatible-element-rich and isotopically uniform materialreferred to as KREEP (Potassium, Rare Earth Elements,

1School of Engineering and Applied Science, Harvard University,Cambridge, Massachusetts, USA.

2Department of Terrestrial Magnetism, Carnegie Institution for Science,Washington, D. C., USA.

3Department of Mathematics, University of California, Berkeley,California, USA.

Corresponding author: J. Suckale, School of Engineering and AppliedScience, Harvard University, 29 Oxford St., Cambridge, MA-02139, USA.([email protected])

©2012. American Geophysical Union. All Rights Reserved.0148-0227/12/2012JE004067

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Phosphorous) concentrated in the Procellarum terrain area[Warren and Wasson, 1979].[4] Geochemical data on returned samples and lunar

meteorites points toward significant differentiation in thelunar magma ocean, but the theoretical plausibility of wide-spread crystal segregation in magma oceans has remainedcontentious. Skepticism is justified because the characteristicconvective speed in a magma ocean is typically severalorders of magnitude higher than the typical settling or flota-tion speed of individual crystals. A simple comparison of thetwo speeds indicates that crystals tend to remain entrained inthe turbulent convection until the ambient flow field hasslowed down sufficiently during the late stretches of solidi-fication, implying that crystal settling is limited to the latestages of magma-ocean solidification [Tonks and Melosh,1990; Abe, 1993; Solomatov and Stevenson, 1993b; Abe,1995, 1997; Solomatov, 2000]. The characteristic convec-tive speed in the magma ocean might, however, not be therelevant parameter determining settling efficiency if crystalsettling occurs primarily in the vicinity of solid boundaries[Martin and Nokes, 1988]. Martin and Nokes [1988] offer adifferent view of crystal settling in vigorously convectingsystems by arguing that because the convective speed decaysto zero at solid boundaries, settling may occur along theseboundaries independent of the vigor of convection.[5] The model by Martin and Nokes [1988] offers a com-

pelling starting point for understanding crystal settling in thelunar magma ocean, but it was derived only for the specialcase of a very dilute suspension (0.3 vol.% crystals).Extending the framework to theMoon requires constraints onhow increasing crystal fractions limit crystal settling or flo-tation, which is the goal of this study. The effect of a finitecrystal fraction in suspension on settling is particularlypertinent for the Moon, because plagioclase only begins tocrystallize once the magma ocean is approximately 70–80%solidified [Palme et al., 1984; Snyder et al., 1992; Elkins-Tanton et al., 2011]. If crystal settling was indeed limitedprimarily to the late stages of magma-ocean solidification[Tonks and Melosh, 1990; Abe, 1993; Solomatov andStevenson, 1993b; Abe, 1995, 1997; Solomatov, 2000], thecrystal fraction in suspension at this stage would be wellbeyond the point at which the crystalline magma developsa finite yield stress associated with load-bearing, three-dimensional networks [Philpotts et al., 1998, 1999; Saaret al., 2001] that impede the relative motion of individualcrystals.

[6] The crystal fraction in suspension in the lunar magmaocean depends on the competition between two timescales:the solidification time, which we define as the time it takesfor the magma ocean to solidify by one additional volumepercent, and the residence time of the crystals, which wedefine as the time it takes 99% of the crystals originally insuspension to settle out assuming that no additional nucle-ation occurs during said time period [Martin and Nokes,1988]. To estimate these two timescales throughout thesolidification history of a magma ocean, we couple a com-putation of the thermal and petrological evolution of themagma ocean at the planetary scale (following Meyer et al.[2010] and Elkins-Tanton et al. [2011]) with direct numeri-cal simulations of the fluid dynamics at the scale of indi-vidual crystals [Suckale et al., 2012]. While the first suite ofcomputations yields an estimate for the solidification time,the second suite of computations constrains the characteristiccrystal settling time at varying crystal fractions. To convertsettling times into residence times, we rely on the model byMartin and Nokes [1988] implying that we only considercrystal settling in the nonturbulent boundary layers of themagma ocean.

2. Model

[7] The flow field in the magma ocean is governed bothby thermal convection, driven by the drastic temperaturecontrast between the upper and lower surface of the magmaocean, and by compositional convection, driven by thedensity difference between the magmatic fluid and themineral phases in suspension. The scales at which these twoeffects operate are drastically different; thermal convectiondrives flow at the planetary scale [e.g., Tonks and Melosh,1990; Solomatov, 2000] with characteristic length scales onthe order of hundreds of km (105m). Thermal convectionalso determines the solidification time of the magma ocean,which can range from thousands to hundreds of thousands ofyears [Meyer et al., 2010; Elkins-Tanton et al., 2011] or1010�1012 s. Compositional convection, on the other hand,is associated with the settling or flotation of crystals that aretypically from tens of mm to cm in size (10�7�10�2 m) withcharacteristic settling times as low as seconds. The spatialscale at which compositional convection dominates is thusroughly 7 to 12 orders of magnitude smaller than for thermalconvection and the temporal scale about 10 to 12 orders ofmagnitude. It is therefore sensible to model the two con-tributions to convection separately. Most previous studiesfacing this dilemma [e.g., Höink et al., 2005, 2006] haveopted to focus on the planetary scale and include onlyselected aspects of small-scale crystal dynamics. Herewe adopt a complementary viewpoint and focus on crystaldynamics in detail while only taking selected aspects of thethermal processes at the planetary scale into account (seeSuckale et al. [2012] for details).

2.1. Model at the Planetary Scale

[8] The planetary-scale model fulfills two key purposes:it captures the thermal evolution of the magma ocean andtracks the geochemical evolution of the evolving liquid andthe crystallizing mineral phases. We consider a lunar magmaocean of 1000 km depth [Elkins-Tanton et al., 2011]. The

Table 1. Approximate Physical Parameters for the Lunar MagmaOcean

Physical Parameter Symbol Unit Lunar Magma Ocean

Depth h km 1000Characteristic velocity vf m/s 0.001–100Fluid density rf kg/m3 2900–3100Crystal density rc kg/m3 2750–4600Crystal radius r m 0.01–0.001Settling velocity vp m/s 10�4�10�1

Gravitational acceleration g m/s2 1.6Fluid viscosity mf Pa s 0.01–0.1Thermal diffusivity k m2/s 10�6

Thermal expansivity a /� 3 � 105Temperature range DT � 1000

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motivation behind adopting this relatively large depth valueas compared with previous estimates [Solomon and Chaiken,1976; Solomon, 1977; Kirk and Stevenson, 1989] is that theresidence time of crystals increases with the thickness of themagma ocean [Martin and Nokes, 1988]. It is thereforereasonable to expect that crystal settling in a shallowmagma ocean tends to be more efficient than in a deepmagma ocean. We therefore study the limiting case of adeep lunar magma ocean, but our conclusions are morebroadly applicable to a range of magma-ocean depth.[9] During the early and intermediate stages of solidifi-

cation (i.e., 80 vol.% solidified), we model the lunar magmaocean as a rapidly convecting body with a liquid surface thatradiates heat into space. We argue that mafic magma-oceanliquids quenching at the cool upper surface are unlikely toform a stable lid at this stage, because they are heavy withrespect to the surrounding liquid and thus inherently unsta-ble [Walker et al., 1980; Walker and Kiefer, 1985; Spera,1992; Elkins-Tanton et al., 2011]. During the late stages ofsolidification, the growing plagioclase lid gradually shiftsheat flux and goes from being convective and radiative tobeing primarily conductive. Once the lid has attained athickness of 5 km, the heat flux through the lid is calculatedby solving the heat conduction equation in a sphericalgeometry while accounting for the latent heat of solidifica-tion and secular cooling of the body [Elkins-Tanton et al.,2011]. The parameters used in the calculation are summa-rized in Table 1.[10] We assume that the magma ocean is entirely molten

initially with the bulk composition suggested by Buckand Toksöz [1980]. The compositional evolution of thelunar magma ocean is determined by the fractionation ofmagma-ocean cumulates in assemblages determined a priori(Figure 1) following Elkins-Tanton et al. [2011]. Thecumulate stratigraphy in Figure 1 divides the solidificationof the lunar magma ocean into four stages: (1) early solidi-fication when only olivine crystallizes, (2) intermediatesolidification when olivine (10%) and orthopyroxene (90%)crystallize, (3) late solidification starting approximately at80 vol.% solidified (corresponding to a pressure of 0.6 GPa)when plagioclase (50%) begins to crystallize together witholivine (20%) as well as ortho- (10%) and clinopyroxene

(20%), and finally (4) very late solidification from 0.5 GPaor �87 vol.% solidified at which point the crystallizingmineral assemblage contains 20% clinopyroxene, 30%orthopyroxene, 40% plagioclase, and 10% oxides (consistingof 20 wt.% pleonaste (Mg,Fe)Al2O4, 30 wt.% chromiteFeCr2O4, 20 wt.% ulvöspinel Fe2TiO4, and 30 wt.% ilmeni-teFeTiO3). Previous studies have estimated slightly differentcrystallization sequences [Snyder et al., 1992; Hess andParmentier, 1995; Van Orman and Grove, 2000] but agreeroughly in the most important aspect, which is that plagio-clase crystallization starts at approximately 80%.[11] Compositions of mineral phases are calculated in

equilibrium with the liquid composition at the respectivestage of solidification using experimentally determinedmineral-melt exchange coefficients [Elkins-Tanton, 2008].The percentage of interstitial liquid retained during

Figure 1. Solidifying mineral assemblages in the lunar magma ocean based on fractional crystallizationfollowing Elkins-Tanton et al. [2011]. The height of the boxes indicates the abundance of the respectivemineral phase in a well-mixed phase assemblage. The gray shades introduced here correspond to thoseused throughout the paper to represent the respective mineral phase.

Figure 2. Liquid and mineral phase densities as a functionof the depth of initial crystallization from the lunar magmaocean. Only plagioclase feldspar is buoyant with respect tothe coexisting magmatic liquid. The four horizontal linesdelimit the four phases of solidification defined by the crys-tallizing mineral assemblage (see Figure 1).

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solidification is 1%. Assuming that minerals retain theirsolidus temperature as crystallization proceeds, the phasedensities are computed from the Brich-Murnaghan equa-tion of state that includes the effects of composition,temperature, and pressure (see Figure 2). An importantcaveat of Figure 2 is that the densities toward the end ofsolidification are caused entirely by the choice of fraction-ating minerals, which is reasonable but not well constrained.[12] Basing our analysis on fractional instead of batch

crystallization will be justified in retrospect by the resultsfrom our local-scale model that crystals settle out efficiently,at least under certain, reasonable conditions (see sections 3and 4). That being said, there clearly is a more subtle con-nection between the compositional evolution of the magmaocean and crystal dynamics. For example, one would expectthat the efficacy of crystal settling will influence the com-position of the cumulates and hence the crystallizationsequence. We do not attempt to incorporate this type offeedback, partly because we suspect it to be of secondaryimportance and partly because it is not straightforward toassess in detail. Our local-scale model only targets crystalsettling in the nonturbulent boundary layers of the magmaocean (see section 2.2), while nucleation and crystal growthprobably also depend on the equilibrium between mineraland liquid phases in the turbulent flow regime comprisingthe majority of the magma ocean.

2.2. Model at the Local Scale

[13] The flow field in the interior of the lunar magmaocean is thought to be turbulent over a wide depth range[Solomatov, 2000]. In the vicinity of the solid boundaries,however, flow is nonturbulent and gradually slows downuntil the local flow speed first becomes comparable andeventually smaller than the settling speed of the crystals[Kraichnan, 1962; Castaing et al., 1989; Tonks and Melosh,1990; Spera, 1992]. The dynamics of the suspension thus

become increasingly dominated by compositional convec-tion, facilitating crystal settling and flotation. In our local-scale model we study crystal behavior only within thesenonturbulent boundary layers, and our results do not applyto the turbulent portion of the magma ocean. The only aspectin which the presence of turbulence is taken into account isby assuming that the magmatic liquid and the suspendedcrystals are well mixed when entering the boundary layer.[14] Compositional convection is driven by the motion of

individual crystals or crystal clusters under the effect ofgravity. We compute the motion of each crystal by inte-grating the crystal equation of motion using the localvelocity and density of the surrounding magmatic fluidwhile accounting for all crystal-crystal collisions. Deter-mining the flow field in the magma requires solving theNavier-Stokes equations including the boundary conditionsimposed by all the crystals in suspension. An approach ofthis type is commonly referred to as “direct” because itresolves the multiphase flow dynamics of the suspensionwithout relying on approximate drag formulas or settlingspeeds and without limiting the range and nature of hydro-dynamic interactions between crystals and between crystalsand magma. Direct numerical simulations are thus particu-larly advantageous for comparing crystal settling and flota-tion over a range of different crystal fractions because,contrary to many previous models (see Suckale et al. [2012]for a more detailed discussion), they resolve the effect ofincreasing crystal fraction on both the motion of thecrystals and on the flow field in the interstitial liquid. Forfurther details regarding our numerical methodology and forextensive benchmarks of our approach, please refer to thecompanion paper [Suckale et al., 2012].[15] Our computations rely on the following three sim-

plifying assumptions regarding the crystalline phase. First,we assume that all crystals are spherical and have the samesize. This simplification is clearly unrealistic, but provides avaluable first step for understanding the dynamics of mag-matic suspensions and has also been the basis of previousstudies of crystal settling [e.g., Solomatov and Stevenson,1993b]. Second, we currently neglect temperature effects atthe local scale, because temperature is unlikely to vary tre-mendously on the scale of individual crystals. Third, we do

Figure 3. Dependence of adiabat, liquidus, and soliduson depth, or equivalently hydrostatic pressure, in the lunarmantle. As the magma ocean cools, the adiabat mostly fallsbetween liquidus and solidus over the entire depth range,implying that crystals are stable at all depths.

Table 2. Properties of the Mineral Phases and the Magmatic Liquidfor the Four Different Phases of Magma-Ocean Solidification

Phase Density (kg/m3) Mineral fraction Viscosity (Pa s)

Phase 1Olivine 3250 100 % -Liquid 3100 - 0.1

Phase 2Orthopyroxene 3150 90 % -Olivine 3300 10 % -Liquid 3100 - 0.1

Phase 3Plagioclase 2670 50 % -Pyroxene 3350 30 % -Olivine 3700 20 % -Liquid 3300 - 1.0

Phase 4Plagioclase 2690 40 % -Pyroxene 3550 50 % -Oxides 4650 10 % -Liquid 3450 - 1.0

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not take nucleation, growth or dissolution of crystals intoaccount. We argue that dissolution is probably of limitedimportance because the adiabat falls in between liquidus andsolidus over much of solidification (see Figure 3), implyingthat crystals should be stable at all depths. We chose not toincorporate nucleation or crystal growth into our modelbecause settling or flotation depends primarily on the aver-age size of the suspended crystals and not on the details ofthe growth process.[16] Regarding the fluid phase, we assume that the magma

is compositionally and thermally well mixed. It can thus berepresented by a constant density and viscosity at crystallinescales for any given point in time. The flow field in the

nonturbulent boundary layers where we investigate crystalsettling represents a superposition of thermal convection atlarge spatial scales and compositional convection at smallspatial scales. While we fully resolve the compositionalcomponent, we simplify the thermal component by speci-fying influx and outflux along the boundaries of the com-putational domain such that mass is preserved. Morespecifically, we consider only vertical inflow, because onlythe vertical velocity component does work against gravity.Because the boundary layer in which settling occurs isdefined by the flow speed becoming comparable to the set-tling speed, we set the influx speed to the free settling speedof the heaviest mineral phase in suspension. Once the inflow

Figure 4. Four example simulations testing olivine settling during the early stages of magma-oceansolidification for four different crystal fractions f ≈ 3%, 12%, 20%, and 33%. All crystals have a 1 cmradius. (a1–d1) The randomly assigned initial positions of the olivine crystals in the computationaldomain. The other panels illustrate the local flow speed normalized by the influx speed and crystal posi-tions at nondimensional times (a2–d2) 0.5, (a3–d3) 1.0, (a4–d4) 1.5, and (a5–d5) 2.0.

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is specified, the outflow is determined self-consistently fromthe flow field inside the domain in order to capture the effectof the presence of crystals on the down-wind flow field[Suckale et al., 2012]. The boundary conditions along thesidewalls also allow for mass-preserving inflow and outflow.

2.3. Linking the Two Scales

[17] The models at the planetary and the local scales arelinked through the framework by Martin and Nokes [1988],which assumes that crystals circulate in a vigorously con-vecting magma body for a long time until they are eventuallyentrained into the boundary layer and settle out of suspen-sion. This point of view is clearly a simplification of theactual settling processes in vigorous convection and is basedon analog experiments that may not have the same scalingbehavior as magma oceans [Burgisser et al., 2005]. Despite

these limitations, we argue that the model provides a rea-sonable starting point for understanding crystal settling, atleast for the Moon. The Moon is in some sense a special casebecause, due to its relatively small size, the adiabat falls inbetween liquidus and solidus for the entire depth range of thelunar mantle, implying that crystals are stable at all depths(see Figure 3). Our model may, however, not pertain tolarge terrestrial planets such as Earth because additionalcomplexities such as dissolution of crystals and meltingat the base of the mantle due to a rapid increase in theGrüneisen parameter [Stixrude et al., 2009] would requireconsideration.[18] For the Moon, the model at the planetary scale

(section 2.1) yields an estimate of the solidification timescaletsol, defined as the time it takes for one additional volumepercent of the magma ocean to solidify, at different stages of

Figure 5. (a–h) Illustration of the statistical analysis used to estimate the average settling speed in amonocrystalline olivine suspension at crystal size (r = 1 cm) and crystal fraction (f ≈ 3%) from 8 simula-tions. The dark gray lines in Figures 5a–5h represent the vertical speed of a single olivine crystal. The redline represents the average speed at any given time as computed through a Loess filter with span 0.1s. Theinitial positions of the crystals for each computation are depicted in the small panel at the bottom left.(i) We apply a Loess filter to the average speeds from Figures 5a–5d to obtain an overall estimate forthe expected settling speed of olivine for this case.

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solidification. It also computes the density and relativeabundance of the crystallizing mineral phases as well as thedensity and viscosity of the magmatic liquid. The model atthe local scale (section 2.2) yields estimates of the settlingspeeds of the suspended mineral phases at the current crystalfraction. We convert these settling speeds to residence timestres using the framework by Martin and Nokes [1988]. Wedefine the characteristic residence time of crystals as the timeuntil 99% of the crystals originally in suspension havesettled out:

tres ¼ log 100ð Þ h=vs; ð1Þ

where h is the depth of the magma ocean and vs the set-tling speed of the crystals. If tres < tsol all crystals settleout and the next model cycle will start with reduced crystal

fraction. Otherwise, the crystal fraction increases by thecrystals that did not settle.[19] The simulations of crystal settling at the local scale

are computationally expensive, in particular since we eval-uate settling for three different crystal sizes with radii of1 mm, 5 mm, and 1 cm to test the importance of crystal size.We therefore divide the solidification history of the lunarmagma ocean into four phases describing the early, inter-mediate, late, and very late solidification based on the min-eral assemblages from Figure 1 and test the efficiency ofcrystal settling and flotation in detail for each one. For eachof these four phases, we assign representative values for thephase densities (see Table 2) based on the more detailedcomputation in Figure 2. We assume that the viscosity of themagmatic liquid increases by one order of magnitude fromphases 1 and 2 to phases 3 and 4. While more refined tools

Figure 6. Convergence test for crystals with radius 5 mm at 3 different crystal fractions (a1–a5) f ≈ 3%,(b1–b5) f ≈ 12%, and (c1–c5) f ≈ 20%. The simulations in each row are based on the same initial con-dition and spatial resolution increasing from 125 � 125, to 250 � 250, and to 375 � 375, to 500 � 500.The last panel in each row (Figures a5, b5, and c5) summarizes the mean settling speed as computedthrough Loess filtering for each computation. Very low resolutions such as 125 � 125 tend to increasethe mean settling speeds slightly, but for resolutions beyond that the predicted mean settling speeds agreewell. Unless otherwise stated, the 2D simulations shown in this paper were performed at resolutions of250 � 250.

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for estimating viscosity changes have been developed forterrestrial melts [Shaw, 1972; Bottinga and Weill, 1972]exist, they are probably not immediately transferrable tomagma-ocean liquids [Liebske et al., 2005].

3. Results

[20] The primary goal of our modeling is to evaluate underwhich conditions plagioclase may float during the latestretches of magma-ocean solidification on the Moon toform the earliest lunar crust. Simulating plagioclase flota-tion, however, requires to constrain the crystal fraction insuspension when plagioclase begins to crystallize. Wetherefore have to model crystal settling from the verybeginning of magma-ocean solidification to ultimatelyevaluate whether and under which conditions plagioclasemight be able to float.

3.1. Early Phase of Magma-Ocean Solidification

[21] The first suite of computations tests how efficientlyolivine settles out of suspension shortly after formation of themagma ocean. The planetary-scale model indicates that thesolidification time during the entire early stage is approxi-mately constant and exceptionally rapid (i.e., on the order of100 yrs/%), at least for simple radiative conditions withoutlid or atmosphere [Elkins-Tanton et al., 2011]. For the lunarmagma ocean as described in Table 1, residence times exceed

solidification time for crystals with radii r < 1 mm even whenthe interaction between crystals is ignored, implying thatvery small crystals are unlikely to settle out completely. Toconstrain the residence times of larger crystals, we quantifyhow fast crystal interactions reduce the settling speed ofolivine crystals with radii of 1 mm, 5 mm, and 1 cm.[22] Figure 4 shows four example computations (a–d)

for 1 cm olivine crystals. The mean spacing a between thecrystals is 10r (Figure 4a1), 5r (Figure 4b1), 4r (Figure4c1), and finally 3r (Figure 4d1). In 2D, these spacingscorrespond to crystal fractions f ≈ 3%, 12%, 20%, and33%. The influx into the computational domain is set to thefree settling speed of a single olivine crystal and is used tonormalize the flow field. The initial positions of the crystalsare assigned randomly. In simulation Figure 4a, mostcrystals are not in immediate contact with another crystal.As the crystal fraction increases, crystals cluster form drop-shaped clouds (e.g., Figures 4c3 and 4c4) and elongatedchains (e.g., Figure 4c5). For even larger crystal fraction,the clusters spread through most of the domain, leavinglimited space for the formation of channels with rapid flow(e.g., Figures 4d2–5).[23] To eliminate the potential effect of the assigned initial

conditions on settling, we perform several computationswith different randomized initial conditions for each crystalsize and crystal fraction. Figure 5 shows the settling speeds

Figure 7. Summary of the decrease in settling speed for olivine at (a1) r = 1 cm, (a2) r = 5 mm, and (a3)r = 1 mm during the early stages of magma-ocean solidification with increasing crystal fractions (f ≈ 3%,f ≈ 12%, f ≈ 20%, and f ≈ 33% in 2D). (b1–b3) The decrease in settling speed with increasing crystalfraction is due to hydrodynamic interactions between crystals and is associated with an increase of thepercentage of crystals in collisions.

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of individual olivine crystals (dark gray) and the mean set-tling speed (red) observed in 8 different computations(Figures 5a–5h). We estimate the mean settling speed foreach simulation by using a Loess filter with span 0.1s,where s is the standard deviation of the distribution of set-tling speeds at a given time. In Figure 5i we use the Loessfilter again to condense the estimated settling speeds fromeach of the computations (Figures 5a–5h) into one finalresult. We have also verified that the estimated settling speeddoes not depend on the grid resolution of the computation(see Figure 6 for an example).[24] Figure 7 summarizes the decrease in settling speed

with increasing crystal fraction for crystals with radii 1 cm(Figure 7a1), 5 mm (Figure 7a2), and 1 mm (Figure 7a3),respectively. It also quantifies the increasing tendency ofcrystals to cluster (Figures 7b1–7b3) with increasing crystalfraction. We find that the hydrodynamic interactionsbetween crystals notably affect settling already at very lowcrystal fractions, particularly for small crystals. For example,the settling speed of 1 mm crystals has already dropped toapproximately half (47%) of their free settling speed at acrystal fraction of ≈3%. At that same crystal fraction, thesettling speed of the 1 cm crystals is still ≈75% of their freesettling speed. This difference in the relative decrease insettling speed is primarily a fluid dynamical effect and notyet related to significantly different clustering behavior, asthe percentage of crystals in collision at any given point intime is similar (Figures 7b1 and 7b3). The result that

hydrodynamic interactions between crystals notably affectthe dynamics of the suspension already at very low crystalfractions is consistent with experimental studies [e.g.,Koyaguchi et al., 1990] and reasonable from a fluiddynamics point of view because the spatial range of hydro-dynamic interactions increases with fluid viscosity.[25] Based on the reduction in settling speed with

increasing crystal fraction (Figure 7), we estimate the resi-dence time of the crystals using equation (1) at finite crystalfraction (Table 3). The residence time at the highest crystalfraction (f ≈ 33%) should be taken with some caution,because, at that point, all crystals are clustered into adomain-spanning network (Figures 7b1–7b3), and it is notclear that the conceptual framework by Martin and Nokes[1988] is still applicable. We conclude that over the time ittakes the magma ocean to solidify one additional percent,crystals with r > 1 mm will probably settle out completely.Small crystals (r ≤ 1 mm) may still settle out, but only par-tially. Therefore, our modeling indicates that the crystalfraction in suspension probably remains low during the earlystage of magma-ocean solidification, implying that thefractional crystallization scenario is justified for modelingthe geochemical evolution of the magma ocean.

3.2. Intermediate Phase of Magma-Ocean Solidification

[26] The lunar magma ocean solely crystallizes olivineuntil solids have filled the lunar interior to a pressure of0.3 GPa, which corresponds to approximately 16% solidi-fied. At this point, the crystallizing assemblage shifts to90% orthopyroxene and 10% olivine. The purpose of thesecond suite of computations is to estimate how this shiftfrom a mono- to a bicrystalline suspension affects the effi-ciency of crystal settling. More precisely, there are two dif-ferent questions at hand: The first question is whether crystalsettling is efficient enough to maintain a low crystal fractionin suspension and justify continued fractional crystallization.For answering that question, we focus on the behavior of themajority of crystals, not on the fate of individual mineralphases. The second question is whether the differences insettling speed for olivine as compared to orthopyroxene aresignificant enough to allow for a dynamic separation of thetwo mineral phases from each other during settling. The latterquestion thus entails a focus on the behavior of individualmineral phases. Throughout the remainder of the paper,we refer to the first problem as collective settling and to thesecond problem as differential settling.[27] The radiative cooling of the magma ocean is largely

unaffected by the progressing crystallization at depth. Weestimate that the characteristic solidification time is stillapproximately constant throughout the entire intermediatephase of the magma-ocean solidification and on the order ofseveral hundred yrs/%. In Figure 8, we test the settlingbehavior of the bicrystalline suspension for 1 cm crystals atcrystal fractions of f ≈ 3%, 12%, 20%, and 33%. The sus-pensions now contain two different mineral phases, olivine(dark gray) and orthopyroxene (light gray), with the densitieslisted in Table 2. The properties of the fluid are assumed to bethe same as in phase 1. The influx speed is again set to thefree settling speed of olivine, which is now slightly higherthan in Figure 4, because olivine has increased in density(Table 2).

Table 3. Overview of the Estimated Residence Times in Years atIncreasing Crystal Fraction for Different Mineral Phases and Sizesa

Mineral phase f ≈ 3% f ≈ 12% f ≈ 20% f ≈ 33%

Phase 1Olivine (r = 1 mm) 582 1369 1611 3426Olivine (r = 5 mm) 17 27 35 109Olivine (r = 1 cm) 4 5 6 18

Phase 2Orthopyroxene (r = 1 mm) 1054 1977 2259 2635Orthopyroxene (r = 5 mm) 22 30 32 36Orthopyroxene (r = 1 cm) 4 5 5 6Olivine (r = 1 mm) 376 510 1438 2635Olivine (r = 5 mm) 7 10 24 36Olivine (r = 1 cm) 2 3 4 6

Phase 3Plagioclase (r = 1 mm) 1442* 1514* 3029* 8654*Plagioclase (r = 5 mm) 25* 40* 87* 303*Plagioclase (r = 1 cm) 6* 15* 49* 101*Pyroxene (r = 1 mm) 8654 12116 12116* 8654*Pyroxene (r = 5 mm) 135 220 242* 303*Pyroxene (r = 1 cm) 32 38 52* 101*Olivine (r = 1 mm) 2019 10097 12116* 8654*Olivine (r = 5 mm) 42 202 242* 303*Olivine (r = 1 cm) 10 35 55* 101*

Phase 4Plagioclase (r = 1 mm) 475* 684* 2139* 8556Plagioclase (r = 5 mm) 9* 22* 178 684Plagioclase (r = 1 cm) 3* 7* 9 86Pyroxene (r = 1 mm) 2139 4278 6845 8556Pyroxene (r = 5 mm) 68 57 228 684Pyroxene (r = 1 cm) 13 9 9 86Oxides (r = 1 mm) 231 658 5704 8556Oxides (r = 5 mm) 7 13 228 684Oxides (r = 1 cm) 2 3 9 86

aThe cited values are only order of magnitude estimates and should not betaken too literally. The residence times marked by an asterisk are associatedwith flotation at the given influx speed.

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[28] The crystallizing mineral assemblage contains rela-tively few olivine crystals. To sample a sufficient number ofcrystals for both mineral phases, we perform a total of 11simulations at f ≈ 3%, 8 simulations at f ≈ 12% and 20%,and 5 simulations at f ≈ 33%. Figure 9 summarizes ourestimates of the average settling speed of olivine andorthopyroxene computed through the double Loess filteringprocedure described previously (section 3.1) for crystal sizesof 1 cm, 5 mm, and 1 mm. At low crystal fraction(Figures 9a1, 9b1, and 9c1), olivine settles approximatelytwice as fast as orthopyroxene. However, as the crystalfraction increases, the settling speed of olivine deceases

much more rapidly (dropping from approximately 89% to26% of the influx speed) than the settling speed of ortho-pyroxene (dropping from 44% to 26% of the influx speed).This effect partly results from using the free settling speed ofolivine as an influx and normalization speed, but this influxbias does not fully explain the differential slowdown.[29] The more rapid slowdown of olivine as compared to

orthopyroxene crystals can be understood through the rela-tive abundance of the two mineral phases in the crystal-line suspension: At intermediate to high crystal fraction alarge percentage of the crystals have formed clusters, thecomposition of which reflects the composition of the

Figure 8. Four example simulations A–D constraining crystal settling during the intermediate stages ofmagma-ocean solidification for four different crystal fractions f ≈ 3%, 12%, 20%, and 33% and crystalswith radius 1 cm. (a1–d1) The randomly assigned initial positions of the olivine (dark gray) and pyroxene(light gray) crystals in the computational domain. The other panels illustrate the local flow speed nor-malized by the influx speed and crystal positions at nondimensional times (a2–d2) 0.5, (a3–d3) 1.0,(a4–d4) 1.5, and (a5–d5) 2.0.

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suspension itself. The settling speed of the crystal clusterrepresents an average of the settling speeds of its individualcomponents and is therefore dominated by orthopyroxene.This insight leads to the hypothesis that at high enoughcrystal fraction the bicrystalline suspension approaches thebehavior of a monocrystalline suspension for which thecrystal density corresponds to the average density of ortho-pyroxene and olivine weighted by their respective abun-dance (yielding rmono ≈ 3165 kg/m3). We test this hypothesisin Figure 10. We observe the best agreement between themean settling speeds in the mono- as compared to thebicrystalline suspension for small crystals. At a crystalradius of 1 mm the difference in the two mean settlingspeeds is ≈2%. At r = 5 mm, the discrepancy has increased

to ≈5% and at r = 1 cm to about ≈15%, indicating that finiteReynolds number effects are probably the main reason fordifferences in settling behavior.[30] Using the average settling speeds determined in

Figure 9, we estimate the residence times using equation (1)and a reduced depth of the magma ocean (h = 770 km) toreflect progressing solidification. We conclude that crystalswith r > 1 mm continue to settle out completely duringthe intermediate phase of magma-ocean solidification onthe Moon. In fact, the residence times are lower thanduring the early stages of magma-ocean solidification (seeTable 3). The two main reasons are that (1) the densityof olivine increases slightly faster in density than theevolving magmatic liquid and (2) that the depth of the

Figure 9. Average settling speeds for olivine (dark gray) and orthopyroxene (light gray) at (a1–a4)r = 1 cm, (b1–b4) r = 5 mm, and (c1–c4) r = 1 mm during the intermediate stages of magma-oceansolidification. The estimate of settling speed is based on 12 simulations at f ≈ 3% (Figures 9a1–9c1),8 simulations at f ≈ 12% (Figures 9a2–9c2) and 20% (Figures 9a3–9c3), and 5 simulations atf ≈ 33% (Figures 9a4–9c4).

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magma ocean decreases as solidification continues, mak-ing it more likely for crystals to enter the boundary layer.[31] Although collective settling of the crystal mixture is

very efficient, we argue that it is unlikely for olivine andorthopyroxene to settle differentially and form a layered pileof cumulates because the difference in settling speed is small(see Table 3). This finding ties into the experimentallydetermined source regions for melting of the picritic lunarglasses that identify a source mineralogy rich in olivine andpyroxene [Delano, 1980; Chen and Lindsley, 1983; Wagnerand Grove, 1997; Elkins et al., 2000; Krawczynski andGrove, 2012].

3.3. Late Phase of Magma-Ocean Solidification

[32] The simulations presented in the last two sectionsindicate that the crystal fraction in suspension at the begin-ning of plagioclase crystallization is probably small as longas a significant portion of crystals grow to sizes of r > 1 mm.The goal of this section is to estimate the maximum crystalfraction at which plagioclase is able to decouple from thesuspension and float to the surface. Since the conductive lidis not yet created, the solidification time is only slightlyhigher than before (on the order of about 1000 yrs/%). Theresidence time of the suspended mineral phases, however, isalso expected to increase because of the elevated viscosity ofthe evolving magma-ocean liquid (see Table 2). One factorthat may aid flotation is that the nonturbulent boundary layersshould increase in thickness as solidification progresses, butwe do not take this process into account. The reason is thesignificant uncertainties associated with estimating thechanging thickness of the boundary layer in vigorouslyconvecting systems [Kraichnan, 1962; Castaing et al., 1989;Tonks and Melosh, 1990; Spera, 1992].[33] Figure 11 shows four computations that test settling

in a crystalline suspension containing 50% plagioclase(white), 30% pyroxene (light gray), and 20% olivine (darkgray) at crystal fractions of f ≈ 3%, 12%, 20%, and 33%.The densities of all suspension phases are listed in Table 2.The influx speed is again set to the free settling speed of

olivine. Comparing Figure 11 to the analogous figures pro-duced for the first two phases of solidification (Figures 4and 8), we find that the simultaneous presence of buoyantand heavy phases in suspension leads to pronounced chan-neling in the ambient fluid at least at low crystal fraction(Figures 11a2–11a5 and 11b3–11b4) and for large crystals(r > 1 mm).The size of the crystals matters because themotion of large crystals (r > 1 mm) creates long low-pressurewakes that facilitate crystal alignment. Small crystals (r =1 mm), on the other hand, are locally surrounded by Stokes-type flow.[34] The juxtaposed channels of predominately upward

oriented flow (red zones) contain mostly plagioclase crystalsand the downward oriented channels (blue zones) primarilyheavy phases, indicating that the channels are created andmaintained by the preferential spatial aggregation of thecrystals. Due to their dynamic nature, the channels areunstable to hydrodynamic perturbations, which either lead toa shifting of the channel in space (e.g., the upward orientedchannel in Figure 11a2 slowly moves to the center of thedomain in Figure 11a5) or to the destruction of an existingchannel, which is typically followed by a new channelforming somewhere else in the domain. The lifespan of thecreated channels depends sensitively on crystal fraction. Theupward oriented channel in the center of Figure 11b3, forexample, has a lifespan of about t = 1, while the channel inFigures 11a2–11a5 has a lifespan of about t = 2. At crystalfractions of ≈20%, channels become increasingly rare andvanish entirely at f ≈ 20% because they are crowded out bythe crystalline phase occupying more space.[35] To estimate the average settling speeds for each

mineral phase, we perform a total of 11 simulations atf ≈ 3%, 8 simulations at f ≈ 12% and 20%, and 5 simula-tions at f ≈ 33%. Our findings are summarized in Figure 12,with crystal radii decreasing from 1 cm (left), 5 mm (mid-dle), and 1 mm (right). Initially, each mineral phase moves ata distinctive speed determined by its density (Figures 12a1,12b1, and 12c1). Because plagioclase is buoyant with respectto the surrounding liquid, it floats as indicated by the negative

Figure 10. Comparison of the mean settling speed in a bicrystalline (dashed line) as compared to amonocrystalline (full line) suspension for 3 crystal sizes (left) r = 1 cm, (middle) 5 mm, and (right)1 mm at crystal fraction f ≈ 33%. The density of the crystals in the monocrystalline suspensions is setto the mean density of the crystals constituting the bicrystalline system.

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sign of its speed. The low settling speed of the pyroxenephases in Figure 12 and compared to Figure 9 is the conse-quence of its small density difference with respect to theambient fluid (see Table 2).[36] An interesting aspect of Figure 12 is that the loss of

differential motion between olivine and pyroxene occurs atlower crystal fraction (f ≈ 12%) now (Figures 12a2, 12b2,and 12c2) as compared to the intermediate phase of magma-ocean solidification (Figure 9 when a separate motion wasobserved until f ≈ 20% in 2D). At the same crystal fraction(f ≈ 12%) the flotation speed of plagioclase continues to be

easily distinguishable, highlighting that different mineralphases do not necessarily lock up at the same crystal frac-tion. Instead, the transition point from differential to col-lective settling is different for each mineral phase anddepends sensitively on the properties of the co-crystallizingphases, such as crystal size and density. Hence, plagioclaseflotation does not necessarily imply that olivine and ortho-pyroxene also settle differentially.[37] As summarized in Table 3, our simulations indicate

that plagioclase crystals with sizes r > 1 mm are able to floatto the surface of the magma ocean even in the absence of a

Figure 11. Four example simulations (a–d) testing plagioclase flotation during the late stages of magma-ocean solidification for four different crystal fractions f ≈ 3%, 12%, 20%, and 33% and crystals withradius 1 cm. (a1–d1) The randomly assigned initial positions of olivine (dark gray), ortho- and clinopyr-oxene (in light gray), and plagioclase (white) in the computational domain. The other panels illustrate thelocal flow speed normalized by the influx speed and crystal positions at nondimensional times (a2–d2)0.5, (a3–d3) 1.0, (a4–d4) 1.5, and (a5–d5) 2.0.

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conductive lid as long as the crystal fraction in suspension isbelow 20%. Even the residence time of 1 mm crystals is ofthe order of the solidification time, meaning that at least asignificant portion of small crystals should float. Once flo-tation begins, the solidification timescale will increase dra-matically as a conductive lid is formed on the top of themagma ocean, which drastically reduces heat loss to space.The key result here is that the most important criterion forwhether flotation occurs initially is the crystal fraction andnot necessarily the crystal size. As the crystal fractionincreases beyond 20%, plagioclase begins to get locked intothe suspension and is no longer able to decouple and float.Although differential settling is no longer possible at thispoint, collective settling of the crystal mix may still con-tinue. The crystal clusters will either sink to the bottom of

the magma ocean or to the top depending on how the aver-age density of the mineral assemblage compares to thedensity of the liquid. For the densities used here (seeTable 2), the locked-up suspension has a slightly negativebuoyancy with respect to the magmatic fluid, which leads tocollective flotation (Table 3). That being said, the uncer-tainties with estimating the fluid density at this late stage ofsolidification are considerable.

3.4. Final Phase of Magma-Ocean Solidification

[38] From approximately 87% solidified to the end ofsolidification the crystallizing assemblage contains mostlypyroxene (20% clinopyroxene and 30% orthopyroxene) andplagioclase (40%). In addition, heavy oxides (10%) begincrystallizing (see Table 2 for the assumed densities). The

Figure 12. Average settling speeds for olivine (dark gray), ortho- and clinopyroxene (in light gray), andplagioclase (white) at (a1–a4) r = 1 cm, (b1–b4) r = 5 mm, and (c1–c4) r = 1 mm during the late phaseof magma-ocean solidification. The estimate of the settling speed is based on 12 simulations at f ≈ 3%(Figures 12a1–12c1), 8 simulations at f ≈ 12% (Figures 12a2–12c2) and 20% (Figures 12a3–12c3),and 5 simulations at f ≈ 33% (Figures 12a4–12c4).

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goal of this section is to verify whether the presence of avery heavy phase changes the settling behavior of the sus-pension. Due to the presence of a fully formed conductivelid, the solidification timescale at this stage is extremely long(on the order of 106 yrs/% and possibly even higher if tidalheating is taken into account [Meyer et al., 2010]), whichmeans that as long as plagioclase is able to decouple fromthe suspension, flotation should occur even if the differentialspeed is minimal.[39] Figure 13 shows four computations that test settling

in the crystalline suspension representing the final phase of

solidification of the lunar magma ocean at crystal fractionsof f ≈ 3%, 12%, 20%, and 33%. The influx speed is set tothe free settling speed of the oxides (see Table 2). The dis-tinct channelization of the ambient flow field observed inFigures 11a2–11a5 and 11b2–11b5 is still noticeable, butless pronounced for the mineral assemblage crystallizingduring the final stage of solidification. Our simulations sug-gest that the main reason for this is the presence of very heavyoxide phases that settle rapidly, which amplifies hydrody-namic instabilities and reduces the life span of channels. Thepresence of the oxides in suspension, however, also reduces

Figure 13. Four example simulations (a–d) testing plagioclase flotation during the final stages ofmagma-ocean solidification for four different crystal fractions f ≈ 3%, 12%, 20%, and 33% and crystalswith radius 1 cm. (a1–d1) The randomly assigned initial positions of the oxide (black) and pyroxenephases (light gray), as well as plagioclase (white). The other panels illustrate the local flow speed nor-malized by the influx speed and crystal positions at nondimensional times (a2–d2) 0.5, (a3–d3) 1.0,(a4–d4) 1.5, and (a5–d5) 2.0.

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the tendency of crystals to cluster at intermediate crystalfractions (f = 12% and 20%) as compared to phase 3, at leastfor crystal sizes above 1 mm (see Figure 14). The dynamicramification of reduced clustering is that more channels canform at f ≈ 20% as compared to the late phase of magma-ocean solidification (e.g., Figure 13c5).[40] In order to estimate the average settling speeds for

each mineral phase, we perform a total of 11 simulations atf ≈ 3%, 8 simulations at f ≈ 12% and 20%, and 5 simula-tions at f ≈ 33%. Our findings are summarized in Figure 15.The overall settling dynamics of the suspension are similarto that found in section 3.3 for the late stages of magma-ocean solidification. Similarly to before, plagioclase getslocked into suspension at a crystal fraction of ≈20%, imply-ing that continued plagioclase flotation requires f < 20%independent of crystal size. The two differences of settlingduring the final as compared to the late phase of solidification

are that (1) the settling speeds of all minerals are still appre-ciably different at f ≈ 20%, and (2) the high density of theoxide phases shifts the average density of the crystals insuspension, which means that at f > 20% the crystal mix willsettle to the bottom instead of float to the top of the magmaocean (Table 3).

3.5. Clustering and Crystal Collisions in 3D

[41] All of the computations shown so far were done in2D. The key advantage of 2D simulations is the added pre-cision of a high spatial and temporal resolution. Computa-tional expense becomes a concern, particularly at highcrystal fractions, because the speed of the suspended crystalsmay vary by several orders of magnitude and thus requiresvery small incremental time steps. That being said, it is notstraightforward to extrapolate insights obtained in 2D to 3D.

Figure 14. Overview of crystal clustering during phases 2–4 of magma-ocean solidification for three dif-ferent crystal radii, (a1–a4) r = 1 cm, (b1–b4) r = 5 mm, and (c1–c4) r = 1 mm, and four different crystalfractions, f ≈ 3% (Figures 14a1–14c1), f ≈ 12% (Figures 14a2–14c2), f ≈ 20% (Figures 14a3–14c3), andf ≈ 33% (Figures 14a4–14c4).

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[42] Apart from the obvious difference in the flow field in3D as compared to 2D, an important confounding factor inextrapolating our 2D results to 3D is the different scalingbehavior of the crystal fraction. For equi-sized spheresarranged in a body-centered cubic array, it is straightforwardto relate the crystal fraction and mean separation distance. In3D, the volume fraction scales with the mean separationdistance as f � a3, while in 2D it scales as f � a2. In otherwords, at the same mean separation distance, crystals fill upan area faster than a volume. The mean separation distanceswe focused on in our simulations (a ≈ 10r, 5r, 4r, and 3r)therefore correspond to larger crystal fractions in 2D(f2D ≈ 3%, 12%, 20%, and 33%) than in 3D (f3D ≈1%, 7%,13%, and 29%). The key conclusion from section 3 is thus

that plagioclase floats even in the absence of an alreadyformed conductive lid if the crystal fraction is <13% (in 3D)or <20% (in 2D).[43] One important observation from our 2D simulations

is that crystalline suspensions start to exhibit clusteringalready at relatively low crystal fraction in agreement withexperimental findings [Koyaguchi et al., 1990]. Our 3Dsimulations suggest that this insight is also true in 3D.In fact, at the samemean separation distance crystal interactionappears to result in a slightly more pronounced slowdown in3D as compared to 2D, but it is challenging to quantify howmuch of this effect is due to the reduced resolution anddomain size in 3D. Another finding of our 2D simulations isthat the presence of clusters changes the dynamics of a

Figure 15. Average settling speeds for oxides (black), ortho- and clinopyroxene (in light gray), and pla-gioclase (white) at (a1–a4) r = 1 cm, (b1–b4) r = 5 mm, and (c1–c4) r = 1 mm during the final stages ofmagma-ocean solidification. The estimate of the settling speed is based on 12 simulations at f ≈ 3%(Figures 15a1–15c1), 8 simulations at f ≈ 12% (Figures 15a2–15c2) and 20% (Figures 15a3–15c3),and 5 simulations at f ≈ 33% (Figures 15a4–15c4).

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suspension, because the settling speed of clusters isapproximately given by the average of the settling speeds ofthe constituent crystals at the same crystal fraction. Thisaveraging effect is easier to test, and we find it appears to bevery similar in 2D and 3D. Figure 16 shows an examplecomputation for a crystalline suspension consisting of oliv-ine and orthopyroxene during the intermediate stages ofmagma-ocean solidification at f3D ≈ 3%.

4. Discussion

[44] Our simulations indicate that plagioclase is able tofloat on the Moon despite the fact that plagioclase onlybegins to crystallize once the magma ocean is already 80%solidified. We find that the main impediment to plagioclaseflotation is not necessarily crystal size, as previously sug-gested [Tonks and Melosh, 1990; Solomatov and Stevenson,1993b, 1993a], but the crystal fraction in suspension. Sizemay play less of a role for plagioclase flotation than crystalfraction, because the residence time of plagioclase crystals insuspension is relatively short, owing primarily to the largedensity contrast between mineral phase and magma-oceanliquid (see Figure 2 and Table 2). If the density differencebetween plagioclase crystals and the magmatic liquid duringthe late phase of solidification is significantly less thanassumed here, our results might not be robust.[45] The main reason crystal fraction plays such a crucial

role for evaluating crystal settling and flotation are the strongand long-range interactions between crystals. Phases 1 and 2attest primarily to the effect that crystal-crystal interactionshave on settling behavior, such as the rapid reduction ofsettling speeds with increasing crystal fraction (e.g., phase 1,see section 3.1) and the dependence of settling speeds onrelative mineral abundances (e.g., phase 2, see section 3.2).Phase 3 (see section 3.2) illustrates that the hydrodynamicinteraction between crystals can lead to pronounced chan-nelization in the ambient flow field. The lifespan of thechannels depends on the crystal size, the relative abundanceof the crystallizing phases, and the density contrast betweencrystals and fluid (e.g., phase 4; see section 3.2).[46] Generally, the lifespan of the crystal clusters

increases with crystal fraction and is significantly largerthan the characteristic timescale over which settling or

flotation occurs for crystal fractions beyond 20% in 2Dand 13% in 3D. At that point, the relative motion ofindividual plagioclase crystals with respect to surroundingcrystals is suppressed because they are locked into sus-pension in the form of long-lived clusters. An importantcaveat here is that we do not currently account for thetypical crystallographic shape of plagioclase crystals or theeffect of a nonuniform crystal size distribution. It is cer-tainly possible that these factors would alter our estimatefor the crystal fraction at which lock-in occurs in the lunarmagma ocean. The general insight that crystal fractionplays a key role for determining differentiation, however,is less parameter-dependent and leads to three more gen-eral conclusions discussed in this section.

4.1. The Possibility and Necessity of Early Settling

[47] A simple comparison of the convective speeds inmagma oceans with the settling speed of individual crystalshas led to the hypothesis that crystal fractionation is negli-gible during the early stages of solidification and only beginsat a later time when the convective flow field has sloweddown considerably [Abe, 1993, 1995, 1997; Solomatov,2000]. Our simulations indicate that crystal settling canstart at the very beginning of solidification because settling inthe nonturbulent boundary layers of the magma ocean aloneis sufficient to deplete the magma ocean of crystals, assumingthat the majority of crystals grow to sizes larger than 1 mm(see section 3).[48] Our simulations also show that crystal settling during

the late stages of magma-ocean solidification requires earlysettling. If crystal settling was negligible initially, mostcrystals would remain suspended and increasingly lock up toform a crystal network that impedes settling. A reduction insettling efficiency therefore results in a downward spiral ofsettling behavior: as fewer crystals settle out, the crystalfraction in suspension increases, which decreases the meansettling speeds and implies that even fewer crystals settle out.[49] Late-stage settling after a period of inefficient settling

at the early or intermediate stages of magma-ocean solidifi-cation thus requires that the crystal fraction in suspension isreduced below the point at which the suspension locked up.Several mechanisms could potentially provide the necessaryadditional melting including impactors, cumulate overturn ofthe solidified portion of the magma ocean, or tidal heating[Meyer et al., 2010]. It is possible that one or several of theseprocesses aided plagioclase flotation on the Moon, but itmay not be necessary to invoke additional melting to explaindifferentiation of the lunar magma ocean.[50] Another interesting ramification of the insight that

crystal fraction controls settling behavior is that an incom-pletely molten magma ocean or magma pond may evolvevery differently than an entirely molten magma ocean. Thereason is that the initial crystal fraction of a mushy magmaocean could easily exceed 20%, which may be too high forfluid dynamical settling to occur. In that case, batch crys-tallization may be more likely than fractional crystallization.Given current theories of lunar formation through a giantimpactor [Brush, 1996], we consider it unlikely that thelunar magma ocean was not entirely molten because the heatprovided by the impact is sufficient to melt the entire Moon.However, lack of complete initial melting might be

Figure 16. Crystal clustering during the intermediatestages of magma-ocean solidification in 3D at crystal frac-tion f3D ≈ 3%. Similar to 2D, clustering leads to an averag-ing of the settling speeds of the different mineral phases.

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important for understanding the evolution of a potentialmagma ocean on other planetary bodies.

4.2. Differentiation: Crystal Size Might Not Be the KeyParameter

[51] It has long been recognized that the size differencebetween Earth and the Moon may be one important factor inthe divergent geochemical evolution of the two planetarybodies. For example, Tonks and Melosh [1990] used thespecial relationship between adiabat, liquidus, and soliduson the Moon (see Figure 3) to argue that individual crystalscould continue to grow no matter where they were trans-ported in the lunar magma ocean. Eventually, crystals on theMoon would be large enough to overcome convectiveentrainment and settle into the cumulate pile. On Earth,however, continued crystal growth would not be possible,because the adiabat falls between liquidus and solidus onlyfor a limited depth range, and crystals would dissolve whentransported outside of that depth range. Our calculationsindicate that continued crystal growth as suggested by Tonksand Melosh [1990] is not required to explain crystal settlingin a lunar magma ocean. We find that crystals as small as1 mm in radius would settle out completely even duringthe early stages of magma-ocean solidification, which arecharacterized by exceptionally rapid flow.[52] As discussed previously (see section 2.3), the rela-

tionship between adiabat, liquidus, and solidus is an integralpart of our model because it implies that crystals are stablethroughout the entire magma ocean. Crystals may thus cir-culate for a long time before being entrained in the non-turbulent boundary layer where settling occurs, as assumedin the framework byMartin and Nokes [1988]. Since crystalsin a terrestrial magma ocean are not stable throughout theentire depth range of the mantle, our model in its current formis not directly applicable to large planets like Earth, and ourfindings about settling and plagioclase flotation do nottranslate in a straightforward manner to terrestrial scenarios.Our model could, however, be easily adapted to constrainmagma-ocean differentiation on other small bodies suchas Vesta.

4.3. Collective Settling Does Not Imply DifferentialSettling

[53] A consistent finding in all of our simulations is thatcollective crystal settling does not imply that the differentmineral phases separate from each other based on their rel-ative densities. Instead, crystal settling appears to be a nec-essary, but not a sufficient condition for differential settling.Two observations from our computations are noteworthy forproviding additional constraints on when crystal settlingresults in differential settling and a layered as opposed to amixed cumulate pile.[54] First, the properties of the co-crystallizing mineral

assemblage exerts an important control over the ability of agiven mineral phase to dynamically separate from othermineral phases in suspension, highlighting the potential forlinked geochemical and fluid dynamical models of magma-ocean evolution. Apart from the more obvious effect of sizeand density differences between the mineral phases, therelative abundances also play an important role. Relativeabundances affect settling for two reasons. First, settling

behavior at finite crystal fractions is dominated by thedynamics of crystal clusters instead of individual crystals.The composition of these clusters reflects the compositionof the suspension, which means that the more abundantmineral phases dominate the settling speed of the clusters.One example of this effect is the joint settling of olivine andorthopyroxene during the intermediate stages of magma-ocean solidification. The settling speed of olivine decreasesmuch more rapidly than that of orthopyroxene (see Figure 9)because olivine makes up only 10% of the suspension. Sec-ond, the presence of both a buoyant and a heavy mineralphase can lead to pronounced channeling in the ambientflow field, at least at low to intermediate crystal fraction, asobserved for phase 3 of magma-ocean solidification (seeFigure 11). The preferential aggregation of buoyant crystalsin upward oriented flow and of heavy crystals in downwardoriented flow increases the efficiency of differential settlingnotably, but is highly dependent on mineral abundances anddensities (see section 3.4).[55] Second, there is no single transition point between

collective settling and differential settling for suspendedmineral phases. Instead, there is a gradual transition that mayinvolve a transitional regime in which certain mineral phasesdecouple from the suspension and float or sink, while othersdo not decouple or decouple only partially. The late stage ofmagma-ocean solidification provides an example of this (seeFigure 12). Initially, all three mineral phases move at theirown characteristic speed with little interaction. At a crystalfraction of f ≈ 12%, however, plagioclase still has a distinctflotation speed, while the motion of olivine and pyroxene isalready almost indistinguishable (Figures 12a2, 12b2, and12c2). There are three reasons for this difference in differ-ential settling: First, the density difference between olivineand pyroxene is relatively small. Second, plagioclase is buoy-ant with respect to the fluid, while olivine and pyroxene areheavy and will thus tend to align in the same downwardoriented channels (Figures 11a2–11a5 and 11b2–11b5). Third,clusters involving crystals with similar densities tend to bemore stable than clusters of crystals with drastically differentdensities (see section 3.4).[56] The above factors influencing differential settling

imply that plagioclase flotation is facilitated in our model bythe fact that it is the only buoyant phase in suspension duringthe late and final phases of solidification. The potentialpresence of another buoyant mineral phase would likelyreduce the efficiency of plagioclase flotation, and the moreso the more comparable it is to plagioclase in size anddensity.

4.4. Conclusions

[57] We present a multiscale model of crystal settling andflotation that links the geochemical and fluid dynamicalevolution of the lunar magma ocean. The key goal of ouranalysis is to shed some new light on the question ofwhether plagioclase can float to the top of the magma oceanand form a primordial crust despite the fact that it onlybegins to crystallize once the magma ocean is already 80%solidified. Our simulations of plagioclase crystals in anolivine- and pyroxene-rich suspension reveal that the overallcrystal fraction in suspension may be the key parameter todetermine under which conditions plagioclase is able to

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decouple and float and not the crystal size. This findingindicates that settling or flotation during the late stages ofmagma-ocean solidification requires settling or flotationearly on to keep the crystal fraction low unless meltingassociated with impactors or cumulate overturn reduces thecrystal fraction. In the case of the Moon, our simulationssuggest that crystal settling might be efficient enough tokeep the crystal fraction in suspension sufficiently low andallow for late-stage plagioclase flotation.

[58] Acknowledgments. We thank Michael Krawczynski and twoanonymous reviewers for their insightful comments that have greatlyimproved this paper. This work was supported by the Director, Office ofScience, Computational and Technology Research, U.S. Department ofEnergy under contract DE-AC02-05CH11231 and the NSF AstronomyCAREER award 0747154 to Linda T. Elkins-Tanton.

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