Microstructure and Mechanism of Quartz Exsolution in Clinopyroxene
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摘要: 矿物出溶结构保存有早期母体矿物的物理化学条件信息，对其开展研究不仅有助于了解寄主岩石的来源深度，而且有助于研究减压折返的动力学演化过程.在世界许多高压-超高压带的榴辉岩和石榴辉石岩中，人们普遍发现单斜辉石中有定向排列的针状或棒状SiO2析出物，其矿物相主要为α石英，有时会伴生钙质角闪石等含水矿物.这些定向针状或棒状体通常平行于单斜辉石c[001]轴方向延伸，石英长轴可以为其c[0001]轴或a[1120]轴.电子背散射衍射(EBSD)测试结果表明，多数石英(96%)析出物与寄主单斜辉石具有结晶学取向关系：(1) 50%的石英c轴平行，并且[0001]Qz//[001]Cpx；(2)35%的石英至少有一个a轴平行，并且[1120]Qz//[001]Cpx；(3)11%的石英至少有一个s{1121}面平行，并且(1121)Qz//(100)Cpx.钙质角闪石析出物与寄主单斜辉石也具有密切结晶学取向关系：(100)Amp//(100)Cpx、[010]Amp//[010]Cpx、[001]Amp//[001]Cpx、[100]Amp∧[100]Cpx≈32°.上述定量显微构造证据表明，单斜辉石中定向石英析出物是由出溶作用所形成，并且多数石英出溶体形成于α石英稳定域.已有高温高压实验研究数据表明，单斜辉石中空位的形成和钙埃斯科拉组分(CaEs)的含量均受化学组成、压力、温度等多种因素综合影响：单斜辉石中CaEs含量对化学组成非常敏感，并受到共生矿物体系中自由SiO2相和蓝晶石的共同缓冲；相同化学组成和等压条件下，CaEs含量总体上随温度升高缓慢降低；相同化学组成和等温条件下，CaEs含量在＜6 GPa区间随压力升高而增加，在＞6 GPa区间随压力升高而降低.单斜辉石定向SiO2析出物的形成可能涉及多种因素，高压只是其中必要条件之一.榴辉岩质单斜辉石中“石英±角闪石”析出物很可能形成于开放体系，与熔流体活动密切相关，涉及多阶段物质扩散、晶体成核生长、重结晶、退变质反应等复杂作用过程.单斜辉石中定向SiO2析出物的显微结构特征并非超高压岩石的必要条件，这种特殊显微结构也不能作为证明超高压的充分条件.Abstract: Exsolution lamellae-bearing minerals preserve information on the physicochemical conditions of the precursor homogeneous host and are helpful in understanding the subduction depth as well as the processes of decompression recorded in the host rocks during exhumation. Oriented silica precipitates in clinopyroxene have been reported widely in eclogite and garnet pyroxenite from high pressure and ultrahigh pressure metamorphic terranes around the world.Most of such silica precipitates are identified as α-quartz which in part coexist with hydrous minerals such as calcic amphibole.Such oriented precipitates are elongated parallel to the c-axis of host clinopyroxene, while the long axes of quartz being either c[0001]or a[1120]. Electron backscatter diffraction (EBSD) analyses demonstrate that the majority (96%) of quartz precipitates have topotactic relationships with their host clinopyroxenes.Three types of crystallographic topotactic relationships have been identified between quartz and host clinopyroxene: (1) 50% quartz precipitates share the same orientation for the c-axes with [0001]Qz//[001]Cpx; (2) 35% quartz precipitates share the same orientation for the a-axes with [1120]Qz//[001]Cpx; and (3) 11% quartz precipitates share the same orientation for the s-planes with (1121)Qz//(100)Cpx.Other quartz axes and planes disperse in large or small girdles around the shared axes or planes.Calcic amphibole precipitates also have a strong crystallographic relationship with host clinopyroxene, i.e., (100)Amp//(100)Cpx, [010]Amp//[010]Cpx, [001]Amp//[001]Cpx, [100]Amp∧[100]Cpx≈32°. The results provide quantitative microstructural evidence supporting an exsolution origin for oriented quartz needles/rods in clinopyroxene and demonstrate that the exsolution of quartz from clinopyroxene occurred within the stability field of α-quartz rather than coesite.Integrated analyses of published high pressure and high temperature experiments show that the cation vacancy and Ca-Eskola (CaEs) component in clinopyroxene are affected by bulk chemistry, pressure and temperature. The solubility of SiO2 in clinopyroxene are sensitive to bulk chemistry, and the CaEs content in clinopyroxene at high pressure conditions is buffered by free silica phase and kyanite. The CaEs contents in clinopyroxene depend strongly on pressure, which shows rapid increase with pressure up to 6 GPa and then decrease with pressure. By contrast, the CaEs contents in clinopyroxene decrease slightly with temperature which indicates that the effect of temperature is relatively week.On the basis of the above integrated analyses on high pressure experiments and observations on mineral association and microstructural results from natural samples, we suggest that the formation mechanism of the oreiented silica in clinopyroxene is more complicated than we might initially assume. The oriented precipitates of α-quartz and calcic amphiboles in host clinopyroxene are probably formed during multi-stage mechanism involving exsolution, diffusion and exchange of multiple substances, nucleation and growth, recrystallization and some retrograded reactions, which are probably promoted by supercritical fluid or partial melting during exhumation. This study suggests that the texture of oriented quartz precipitates in clinopyroxene is neither necessary nor sufficient for UHP rocks, i. e., it cannot be used as an indisputable UHP-indicator.
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Key words:
- ultrahigh pressure metamorphism /
- clinopyroxene /
- quartz exsolution /
- EBSD /
- topotaxy /
- petrology
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图 1 榴辉岩单斜辉石中石英出溶体显微照片
a.新鲜榴辉岩矿物组合为石榴石+绿辉石+金红石，其中半自形绿辉石中含丰富石英棒状体；b.放大图像显示不同长度和宽度的石英棒状体呈定向排列，其长轴延长方向平行寄主单斜辉石c[001]方向；c.弱退变质榴辉岩矿物组合为石榴石+单斜辉石+金红石+石英+角闪石+斜长石，退变质角闪石沿着石榴子石与单斜辉石颗粒边界分布，单斜辉石中含有若干定向粗大石英棒状体和大量细小石英析出体；d.石英析出体截面呈柱状或不规则多边形状，部分石英析出体一侧伴生细小角闪石，注意角闪石+石英析出体常与粒内微裂隙相邻；e.单斜辉石内部含有大量石英±角闪石析出体和粒间与粒内微裂隙；f.放大图像显示较粗大角闪石紧邻粒内开放式裂隙.a，b来自南大别双河新鲜榴辉岩(RP-28)；c，d，e，f来自苏鲁威海刘公岛弱退变质榴辉岩(WH08-4).a，b，c为光学显微镜单偏光图像；d，e，f为扫描电镜电子背散射图像；Amp.角闪石；Cpx.单斜辉石；Grt.石榴子石；Qz.石英；Rt.金红石
Fig. 1. Photographs showing parageneses and textures of clinopyroxene with quartz precipitations in eclogite
图 2 天然榴辉岩单斜辉石中主量元素和端元组分对应关系
a.单斜辉石中Na2O-Al2O3质量百分比对应关系；b.单斜辉石单位分子中Na-Si原子数对应关系；c.钙切尔马克(CaTs)分子与硬玉(Jd)分子对应关系；d.钙埃斯科拉(CaEs)分子与硬玉(Jd)分子对应关系.电子探针数据据Katayama et al.(2000)、Tsai and Liou(2000)、Dobrzhinetskaya et al.(2002)、Page et al.(2005)、梁金龙等(2006)、Proyer et al.(2009)和Xu et al.(2015)
Fig. 2. Relations for major element and end-number contents in clinopyroxene from natural eclogites
图 3 威海榴辉岩(WH08-4) 电子背散射照片和Si、Na、Al、Mg、Ca元素面分布照片
Fig. 3. BSE image and Si, Na, Al, Mg and Ca mappings of eclogite (WH08-4) from Weihai, eastern China
图 4 高温高压实验合成单斜辉石中CaEs和Si含量变化
a.CaEs摩尔含量随压力变化；b.Si原子数随压力变化；c.CaEs摩尔含量随温度变化；d.Si原子数随温度变化；e.CaEs摩尔含量与总阳离子数对应关系；f.Si与Al原子数对应关系；g.CaEs摩尔含量与Si原子数对应关系；h.Si与Na+K原子数对应关系.数据引自Wood and Henderson(1978)、Gasparik(1985, 1986)、Zhao et al.(2011)和Kawasaki and Osanai(2015)
Fig. 4. Variation of CaEs component and Si cation per formula unit in clinopyroxene synthesized in high pressure and high temperature experiments
图 5 石英和角闪石析出体与寄主单斜辉石结晶学取向对应关系
a.单斜辉石中角闪石析出体结晶学取向上半球散点图；b.单斜辉石中石英析出体结晶学取向上半球散点图；c.石英析出体结晶学取向反极图.EBSD测量数据来自两块榴辉岩：南大别双河新鲜榴辉岩(RP-28，170 Qz in 17 Cpx)和苏鲁威海刘公岛弱退变质榴辉岩(WH08-4，53 Amp and 2 015 Qz in 35 Cpx).为获得统计对比分析结果，所有寄主单斜辉石均旋转到同一取向，石英和角闪石的结晶学取向则随寄主单斜辉石作协同旋转.单斜辉石的结晶学参考坐标已在上半球等角度散点图中标出，即[001]cpx位于南北方向，[010]cpx位于东西方向，(100)cpx位于圆心.石英反极图分别沿着//[010]cpx，//[001]cpx和⊥(100)cpx三个方向投影
Fig. 5. Diagnostic crystallographic topotactic relationships between quartz and amphibole precipitates and host clinopyroxene
图 6 单斜辉石析出石英+角闪石的可能模式
a.超高压环境条件下，在柯石英稳定域内，超硅单斜辉石可以含有过量硅和一定空位；b.随着压力降低，亚稳态超硅单斜辉石释放出少量硅，这些析出硅在单斜辉石核部结晶生长；c.随着压力和温度进一步降低，在α石英稳定域，单斜辉石在开放体系熔流体活动的促进下丢失Na等化学组分，同时伴有大量硅析出并在单斜辉石核部结晶生长出大量α石英微晶；d.在α石英稳定域，早期石英微晶重结晶形成较为粗大的定向棒状体，并伴随后续硅的析出和结晶形成微细石英针状体；e.在裂隙附近，单斜辉石和石英析出体受熔流体活动影响，发生退变质反应形成石英+角闪石特殊结构
Fig. 6. Possible quartz+amphibole precipitate formation model in clinopyroxene
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