S. Amelinckx et al., GEOMETRICAL ASPECTS OF THE DIFFRACTION SPACE OF SERPENTINE ROLLED MICROSTRUCTURES - THEIR STUDY BY MEANS OF ELECTRON-DIFFRACTION AND MICROSCOPY, Acta crystallographica. Section A, Foundations of crystallography, 52, 1996, pp. 850-878
The geometry of the reciprocal space of cylindrically and conically ro
lled microstructures is described. The simpler cylindrical case is fir
st discussed, followed by the conical case; in both cases, the observa
tions and then the theory are described. The theory is compared with o
bservations on chrysotiles, the structural and microstructural feature
s of which are briefly recalled. The reciprocal space of an infinite 3
D crystal consists of a lattice of discrete nodes. If a crystalline sh
eet is curled up into a cylindrical scroll (or into concentric cylinde
rs), the corresponding reciprocal space is obtained by rotating this s
et of lattice points about a line parallel to the cylinder axis throug
h the origin of reciprocal space. The lattice nodes thereby describe g
eometrical loci that, in this simple case, are circles in planes perpe
ndicular to the rotation axis. For a general orientation of the rotati
on axis, each node produces its own circle. This is the case when the
fibre has chiral character. For certain symmetrical orientations of th
e axis, 'degeneracy' occurs and two (Or more) nodes may lead to the sa
me circular locus. This is the case for achiral fibres. The curvature
often causes disorder in the stacking of successive cylindrical sheets
- this leads to 'coronae' instead of sharp circles - especially in th
e concentric cylinder case. In the diffraction pattern, these produce
spots that are streaked in the sense away from the axis. In ideal cyli
ndrical scrolls, the structures in successive layers, as viewed along
a radial line c, are shifted relative to each other over 2 pi times th
e layer thickness; this may lead to superperiods along the normal c to
the sheet planes if this shift is commensurate with the lattice vecto
rs in the sheet plane, i.e. with its translation symmetry. The superpe
riod is clearly related to the sheet thickness, which may be more than
one bilayer. If the 2D crystalline sheet is curled up into a cone, th
e reciprocal-space loci become curves that are situated on spheres of
constant spatial frequency, called spherical spirals instead of the ci
rcles in the cylindrical case. Each reciprocal-lattice node describes
such a spiral traced out by a node point subject to the coupled rotati
ons about the cone axis and about the local normal to the cone surface
. The equations of such spirals are derived and their symmetry propert
ies are studied analytically. The spiral's shape is a function of the
semi-apex angle of the cone. For an arbitrary cone angle, these curves
are not closed; they completely fill a band on the surface of the sph
ere. For certain discrete cone angles, which turn out to be essentiall
y determined by the condition of good epitaxic fit between successive
sheets of the cone, the spherical spirals become closed curves. The co
nditions under which several node points, belonging to the same spatia
l frequency, trace out the same spherical spiral are discussed: i.e. t
he conditions for degeneracy are formulated. The point symmetries of t
he sets of spherical spirals belonging to the same spatial frequency a
re found to depend on characteristic values of the semi-apex angle. Al
l turns of a conical scroll are in fact formed from a single sheet. Th
e structure in any given turn is rotated relative to that in the adjac
ent turn over a constant angle, only determined by the semi-apex angle
. If this rotation angle is commensurate with 2 pi, superperiods can b
e formed, visible as reinforcements in streaks that are parallel to th
e generators of the cone formed by the set of normals to the conical s
urface. Also, this superperiod depends on the thickness of the sheet a
s well as on its rotation symmetry. Diffuse scattering is found to be
concentrated on a V-shaped hyperboloid-like surface, the point of the
V being situated on a spherical spiral. The intersection of this surfa
ce with the Ewald plane leads to V-shaped streaks attached by their ap
exes to the spots. They are the homologues of the simple streaks in th
e cylindrical case. Under certain conditions of beam incidence, the in
tersection is hyperbole branch. Spot positions have been computed for
a few characteristic diffraction conditions; they are found to represe
nt adequately the observed spot patterns. A Mercator-like projection m
ethod is proposed to represent the spherical spirals in a plane and to
construct geometrically the intersections with the Ewald plane for di
fferent angles of incidence. Throughout the paper, the analogies and t
he differences between the diffraction features of cylindrical and con
ical scrolls are emphasized and illustrated by observations on chrysot
ile.