Block copolymer (BCP) self-assembly is a promising tool for next generation lithography as microphase separated polymer domains in thin films can act as templates for surface nanopatterning with sub-20 nm features. The replicated patterns can, however, only be as precise as their templates. Thus, the investigation of the morphology of polymer domains is of great importance. Commonly used analytical techniques (neutron scattering, scanning force microscopy) either lack spatial information or nanoscale resolution. Using advanced analytical (scanning) transmission electron microscopy ((S)TEM), we provide real space information on polymer domain morphology and interfaces between polystyrene (PS) and polymethylmethacrylate (PMMA) in cylinder- and lamellae-forming BCPs at highest resolution. This allows us to correlate the internal structure of polymer domains with line edge roughnesses, interface widths and domain sizes. STEM is employed for high-resolution imaging, electron energy loss spectroscopy and energy filtered TEM (EFTEM) spectroscopic imaging for material identification and EFTEM thickness mapping for visualisation of material densities at defects. The volume fraction of non-phase separated polymer species can be analysed by EFTEM. These methods give new insights into the morphology of polymer domains the exact knowledge of which will allow to improve pattern quality for nanolithography.
Heteroepitaxy on nanopatterned substrates is a means of defect reduction at semiconductor heterointerfaces by exploiting substrate compliance and enhanced elastic lattice relaxation resulting from reduced dimensions. We explore this possibility in the InAs/GaAs(111)A system using a combination of nanosphere lithography and reactive ion etching of the GaAs(111)A substrate for nano-patterning of the substrate, yielding pillars with honeycomb and hexagonal arrangements and varied nearest neighbor distances. Substrate patterning is followed by MBE growth of InAs at temperatures of 150 -350 C and growth rates of 0.011 nm/s and 0.11 nm/s. InAs growth in the form of nano-islands on the pillar tops is achieved by lowering the adatom migration length by choosing a low growth temperature of 150 C at the growth rate 0.011 nm/s. The choice of a higher growth rate of 0.11 nm/s results in higher InAs island nucleation and the formation of hillocks concentrated at the pillar bases due to a further reduction of adatom migration length. A common feature of the growth morphology for all other explored conditions is the formation of merged hillocks or pyramids with well-defined facets due to the presence of a concave surface curvature at the pillar bases acting as adatom sinks.
We analyze the shape and position of heteroepitaxial InAs islands on the top face of cylindrical GaAs(111)A nanopillars experimentally and theoretically. Catalyst-free molecular beam epitaxial growth of InAs at low temperatures on GaAs nanopillars results in InAs islands with diameters < 30 nm exhibiting predominantly rounded triangular in-plane shapes. The islands show a tendency to grow at positions displaced from the center towards the pillar edge.Atomistic molecular statics simulations evidence that triangular-prismatic islands centered to the pillar axis with diameters smaller than that of the nanopillars are energetically preferred.Moreover, we reveal the existence of minimum-energy states for off-axis island positions, in 2 agreement with the experiment. These findings are interpreted by evaluating the spatial strain distributions and the number of broken bonds of surface atoms as a measure for the surface energy. The influence of surface steps on the energy of the system is addressed as well.
A process sequence enabling the large-area fabrication of nanopillar-patterned semiconductor templates for selective-area heteroepitaxy is developed. Herein, the nanopillar tops surrounded by a SiNx mask film serve as nanoscale growth areas. The molecular beam epitaxial growth of InAs on such patterned GaAs[Formula: see text]A templates is investigated by means of electron microscopy. It is found that defect-free nanoscale InAs islands grow selectively on the nanopillar tops at a substrate temperature of 425 °C. High-angle annular dark-field scanning transmission electron microscopy imaging reveals that for a growth temperature of 400 °C, the InAs islands show a tendency to form wurtzite phase arms extending along the lateral [Formula: see text] directions from the central zinc blende region of the islands. This is ascribed to a temporary self-catalyzed vapor–liquid–solid growth on [Formula: see text] B facets, which leads to a kinetically induced preference for the nucleation of the wurtzite phase driven by the local, instantaneous V/III ratio, and to a concomitant reduction of surface energy of the nanoscale diameter arms.
restricted adatom migration together with an enhanced nucleation rate of the second atomic layer on monolayer islands leads to QD formation on the pillar tops. [12,13] Since these QDs have steeper sidewalls than conventional InAs QDs grown at higher temperatures on planar GaAs(001), [14] a more efficient elastic strain relaxation and possibly an increased critical volume for misfit defect formation are expected. Another promising feature of InAs heteroepitaxy on GaAs(111)A is the absence of Ga/In alloying. [15,16] In general, heterostructures consisting of mismatched semiconductor islands on nanopillar tops have aroused significant interest because of the enhanced capabilities to position the islands, to control their size, and to relieve misfit strains elastically. [17][18][19][20] The present study analyzes the size dependence of the elastic and plastic strain relaxation mechanisms including strain distributions in InAs QDs on GaAs nanopillar tops by means of atomic-resolution high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) imaging and molecular static simulations. Section 2 presents and discusses the results, and Section 3 draws conclusions. Finally, details on the performed experiments as well as theoretical calculations are given in Section 4.
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