Polysomatism,polytypism, defect microstructures,and reaction mechanisms in regularly and randomly interstratified serpentine and chlorite

High-resolution (HRTEM) and analytical electron (AEM) microscopic evidence for a polysomatic series based on regular interstratifications of serpentine (amesite) and chlorite (clinochlore) are reported from an altered skarn in Irian Jaya. The assemblage includes regular interstratifications of one clinochlore and two (2:1; three structural variants), three (3:1), and four (4:1) amesite composition 1:1 layers as well as randomly interstratified serpentine and chlorite. The order of abundance of regularly interstratified minerals is 1:1>2:1>4:1>3:1. Atomic-resolution images, image simulations, and comparison between calculated and observed diffracted intensities verify the proposed 1:1 and 2:1 structures and reveal details of their defect microstructures. AEM data show that compositions are linear combinations of the associated amesite and clinochlore. The 1:1, 2:1, 3:1, and 4:1 minerals occur both as discrete sub-micron crystals and as domains within serpentine or chlorite. Some crystals of the 2:1 phase were sufficiently large for study by X-ray precession and powder methods. Crystals of the regularly interstratified 2:1, 3:1, and 4:1 phases are usually bent. High-resolution images reveal that, within polygonal segments, the layers commonly exhibit a few degrees of curvature with segments separated by antigorite-type offsets. Deformed chlorite crystals are probably replaced by interstratified minerals during an aluminum metasomatic event. Al may have been deposited from sulfuric acid-rich solutions when they interacted with calcite and dolomite to form the anhydrite-rich corona around the phyllosilicate-rich region of the core. The interstratified chlorite (clinochlore composition) suggests aluminum addition by selective conversion of a sub-set of the chlorite layers to amesite. Defect microstructures suggest that crystals of regularly interstratified material grew by direct structural modification of preexisting chlorite. Regular interstratifications may form in response to thermally controlled limits on Al solubility in chlorite and heterogeneities in the distribution of Al-rich solutions during metasomatism. Regularly interstratified minerals coexist with randomly interstratified serpentine/chlorite, chrysotile, antigorite, lizardite, and several amesite and chlorite polytypes. Tentative chlorite and amesite identifications include one-layer (b=97°, probably IIbb), one-layer (b=90, possibly Ibb), two-, and three-layer chlorites, and 2H₁ (but possibly 1M or 1T), rhombohedral (3R or 6R), and twelve-layer (Tc; non standard) serpentine polytypes. The complex phyllosilicates attest to rampant chemical and structural disequilibrium.