The exfoliation and deposition of large (10-100 μm) Ti0.87O2 and small (0.1-1 μm) Ti0.91O2 nanosheets from lepidocrocite-type protonated titanates was investigated for getting high quality films. Exfoliation was carried out with different tetra-alkyl ammonium ions (TAA(+)) and varying TAA(+)/H(+) ratios, and the colloidal solutions were characterized by small-angle X-ray scattering (SAXS) and ultraviolet-visible (UV-vis) spectroscopy. Using Langmuir-Blodgett deposition the titanate nanosheets were directly transferred onto a Si substrate. The resulting films were characterized by atomic force microscopy (AFM).The results indicate that the H1.07Ti1.73O4 titanate exfoliated at very low ratios of TAA(+)/H(+); no lower threshold for exfoliation was observed for the TAA(+) concentration. Nanosheets exfoliated at very low ratios of TAA(+)/H(+) typically showed a small size and porous surface. Subsequent exfoliation of the remaining layered titanate particles yielded much higher quality nanosheets. The optimized deposition parameters for Langmuir-Blodgett films suggest that the surface pressure is a key parameter to control the coverage of the film. The bulk concentration of nanosheets was found to be a less important deposition parameter in the LB deposition process. It only influenced whether the desired surface pressure could be reached at a given maximum degree of compression.

Nanosheets of Ti0.87O2 and Ca2Nb3O10 were synthesized and transferred onto Si substrates by Langmuir-Blodgett deposition. Using pulsed laser deposition, SrRuO3 films were formed on top of these samples. The underlying nanosheets determined both the morphology and crystallographic orientation of the films. SrRuO3 grew preferentially in the [110]pc direction on Ti0.87O2 nanosheets, while growth proceeded in the [001]pc direction on Ca2Nb3O10 nanosheets (pc refers to the pseudocubic unit cell of SrRuO3). Besides macroscopic control over the out-of-plane crystal direction, single crystal orientations were measured by electron backscatter diffraction on the level of individual nanosheets, indicating that epitaxial growth was achieved on the nanosheets as imposed by their well-defined crystal lattices. The nanosheets also had a clear effect on the magnetic properties of the films, which showed anisotropic behavior only when a seed layer was used. A monolayer consisting of a mixture of both types of nanosheets was made to locally control the nucleation of SrRuO3. In this context, SrRuO3 was used as model material, as it was used to illustrate that nanosheets can be a unique tool to control the orientation of films on a (sub-)micrometer length scale. This concept may pave the way to the deposition of various other functional materials and the fabrication of devices where the properties are controlled locally by the different crystallographic orientations.

Perovskite oxide heteroepitaxy is realized on the top of inorganic nanosheets that are covering the amorphous oxide surfaces of Si substrates. Utilizing pulsed laser deposition, thin films of SrRuO3 in a (001)pc and (110)pc orientation on nanosheets of Ca2Nb3O10 and Ti0.87O2 are grown, respectively. The two types of nanosheets are patterned to locally tailor the crystallographic orientation and properties of SrRuO3. The success of our approach is demonstrated by electron backscatter diffraction and spatial magnetization maps. An unprecedented control of perovskite film growth on arbitrary substrates is illustrated in this work, and the methods that are developed to deposit SrRuO3 thin films are a viable starting point for growth of artificial heteroepitaxial thin films that require a bottom electrode. Control is not just reached in the direction of film growth, as the crystal orientation and film properties are regulated laterally on the surface of micropatterned nanosheets. Local control of magnetic properties is illustrated, which holds out prospects for the fabrication of next‐generation devices like noncollinear magnetic random access memories.

Large area low-cost patterning is a challenging problem in graphene research. A resist-free, single-step, large area and cost effective soft lithographic patterning strategy is presented for graphene. The technique is applicable on any arbitrary substrate that needs to be covered with a graphene film and provides a viable route to large-area patterning of graphene for device applications.

Typical surface areas of 5 × 5 mm(2) were patterned with high-aspect-ratio micrometer- and submicrometer-sized structures of yttria-stabilized zirconia using a combination of micromolding in capillaries and sol-gel chemistry. The influence of precursor solution concentration and mold geometry on the final shape and dimensions of the patterned structures was investigated. At a precursor concentration of [Zr] = 0.724 mol/dm(3), isolated objects-due to the controlled cracking of patterned films-such as crosses (height 1.4 μm, width 6.0 μm) and "dog bones" (height 800-900 nm, width 900 nm) or patterned films (height 450 nm) were obtained, depending on the mold geometry. Lower precursor concentrations led to differently sized and shaped structures, with changes in dimensions of more than an order of magnitude. Employing a precursor concentration of [Zr] = 0.036 mol/dm(3) yielded isolated rings (height 100-150 nm, line width 20 nm) and squares (height 40 nm, line width 40 nm). A better understanding of the relationship between the precursor concentration, mold geometry, and observed coherent crack patterns in as-dried sol-gel structures may lead to new techniques in patterning isolated features.