Calcite is also remarkable for the variety and perfection of its twinned crystals. Twinned crystals, though not of infrequent occurrence, are, however, far less common than simple (untwinned) crystals. No less than four well-defined twin-laws are to be distinguished:—

i. Twin-plane c (111).—Here there is rotation of one portion with respect to the other through 180° about the principal (trigonal) axis, which is perpendicular to the plane c (111); or the same result may be obtained by reflection across this plane. Fig. 7 shows a prismatic crystal (like fig. 4) twinned in this manner, and fig. 8 represents a twinned scalenohedron v {201}.

ii. Twin-plane e (110).—The principal axes of the two portions are inclined at an angle of 52° 30½′. Repeated twinning on this plane is very common, and the twin-lamellae (fig. 9) to which it gives rise are often to be observed in the grains of calcite of crystalline limestones which have been subjected to pressure. This lamellar twinning is of secondary origin; it may be readily produced artificially by pressure, for example, by pressing a knife into the edge of a cleavage rhombohedron.

iii. Twin-plane r (100).—Here the principal axes of the two portions are nearly at right angles (89° 14′), and one of the directions of cleavage in both portions is parallel to the twin-plane. Fine crystals of prismatic habit twinned according to this law were formerly found in considerable numbers at Wheal Wrey in Cornwall, and of scalenohedral habit at Eyam in Derbyshire and Cleator Moor in Cumberland; those from the last two localities are known as "butterfly twins" or "heart-shaped twins" (fig. 10), according to their shape.

iv. Twin-plane f (111).—The principal axes are here inclined at 53° 46′. This is the rarest twin-law of calcite.

Calcite when pure, as in the well-known Iceland-spar, is perfectly transparent and colourless. The lustre is vitreous. Owing to the presence of various impurities, the transparency and colour may vary considerably. Crystals are often nearly white or colourless, usually with a slight yellowish tinge. The yellowish colour is in most cases due to the presence of iron, but in some cases it has been proved to be due to organic matter (such as apocrenic acid) derived from the humus overlying the rocks in which the crystals were formed. An opaque calcite of a grass-green colour, occurring as large cleavage masses in central India and known as hislopite, owes its colour to enclosed "green-earth" (glauconite and celadonite). A stalagmitic calcite of a beautiful purple colour, from Reichelsdorf in Hesse, is coloured by cobalt.

Optically, calcite is uniaxial with negative bi-refringence, the index of refraction for the ordinary ray being greater than for the extraordinary ray; for sodium-light the former is 1.6585 and the latter 1.4862. The difference, 0.1723, between these two indices gives a measure of the bi-refringence or double refraction.

Although the double refraction of some other minerals is greater than that of calcite (e.g. for cinnabar it is 0.347, and for calomel 0.683), yet this phenomenon can be best demonstrated in calcite, since it is a mineral obtainable in large pieces of perfect transparency. Owing to the strong double refraction and the consequent wide separation of the two polarized rays of light traversing the crystal, an object viewed through a cleavage rhombohedron of Iceland-spar is seen double, hence the name doubly-refracting spar. Iceland-spar is extensively used in the construction of Nicol's prisms for polariscopes, polarizing microscopes and saccharimeters, and of dichroscopes for testing the pleochroism of gem-stones.