High-resolution (3.7 A in optical diffraction) electron microscope images have been obtained from a series of n-parafflin monolamellar crystals with chain lengths from n-C36H74 to n-Cs2H,66. The higher molecular weight specimens, which do not undergo chain folding, form sectorized crystals and the molecular packing is found to include alternate bands of untilted and tilted chains along (130 is a result of slight surface roughness due to unequal chain lengths or surface protrusions of chains; the new decoration is also randomly distributed. For pure n-C6H122 lamellae, however, suggestions of regular bands containing rods along [100], due to surface discontinuities along (130), can also be seen. In contrast with polyethylene, these data suggest that crystal sectorization may be a function of chain-stem packing alone and that chain folds may play merely a secondary role in the polymer-e.g., by directing the collapse of pyramidal crystals on a flat surface.The major difference between lamellar crystals of n-paraffins and polyethylene is the sectorization of the latter imposed by chain folds (1, 2). As shown by extensive electron microscopic studies (3-9), large polyethylene crystals grown from dilute solution originally occur in suspension as hollow pyramids, which flatten onto a substrate surface to produce corrugations along the (130) direction in {110} sectors. Highresolution electron microscopy and electron microdiffraction studies of such collapsed pyramids (10) have shown that alternating bands of tilted and untilted chains are found in these corrugations and the prominent reflections from the tilted chain areas are {110} Friedel pairs, with orientation of these tilt axes dependent upon the sector. In agreement with earlier studies (3-9), the probable chain-fold direction has been identified by surface decoration with polyethylene crystallites grown from polymer deposited from the vapor phase (11). It is also no surprise that lamellae of very long paraffins, which can be crystallized with a single "hairpin" chain fold, also are sectorized with a chain-fold orientation very similar to polyethylene (12).Three years ago, a sectorized crystallization was also observed for long-chain paraffins n-CmH2m+2 where m 2 44 but, nevertheless, is still small enough to avoid chain folding in the crystals (13). As shown in Fig. la, bright-field electron micrographs reveal an alternation of sharp Bragg fringes directed along (130) in {110} sectors; nevertheless, there are no signs of corrugation in crystals obliquely shadowed with a fine layer of carbon-platinum (13); i.e., the sectorization effect is more subtle than found for polyethylene (Fib. lb). Although evidence for chain tilts could be seen in selected area electron diffraction patterns from individual {110} sectors (13), no direct evidence had been found for local variations of chain orientation which may correspond to an undulation of the lamellar surface.Given our earlier success in the molecular-resolution imaging of n-C44H90 lamellar crystals in the electr...