We introduce a simple and inexpensive procedure for epitaxial lift-off of wafer-size flexible and transparent foils of single-crystal gold using silicon as a template. Lateral electrochemical undergrowth of a sacrificial SiO layer was achieved by photoelectrochemically oxidizing silicon under light irradiation. A 28-nanometer-thick gold foil with a sheet resistance of 7 ohms per square showed only a 4% increase in resistance after 4000 bending cycles. A flexible organic light-emitting diode based on tris(bipyridyl)ruthenium(II) that was spin-coated on a foil exploited the transmittance and flexibility of the gold foil. Cuprous oxide as an inorganic semiconductor that was epitaxially electrodeposited onto the gold foils exhibited a diode quality factor of 1.6 (where = 1.0 for an ideal diode), compared with a value of 3.1 for a polycrystalline deposit. Zinc oxide nanowires electrodeposited epitaxially on a gold foil also showed flexibility, with the nanowires intact up to 500 bending cycles.
Epitaxial films through spin coating A simple way to coat a surface with a uniform film is by spin coating. The substrate is spun at high speed, and a droplet of solution containing the coating is added at the center, spreads out, and evaporates. This method is used to make polycrystalline inorganic coatings and amorphous films, such as polymers used in lithography. Kelso et al. performed spin coating with single-crystal substrates, carefully controlling the thickness of the spreading solution on the basis of its viscosity and the rotation rate. In this way, they achieved epitaxial growth—in which the crystallites are oriented by the substrate—for perovskites, zinc oxide, and sodium chloride. Science , this issue p. 166
Germanium (Ge) is a group IV semiconductor with superior electronic properties compared with silicon, such as larger carrier mobilities and smaller effective masses. It is also a candidate anode material for lithium-ion batteries. Here, a simple, one-step method is introduced to electrodeposit dense arrays of Ge nanowires onto indium tin oxide (ITO) substrates from aqueous solution. The electrochemical reduction of ITO produces In nanoparticles that act as a reduction site for aqueous Ge(IV) species, and as a solvent for the crystallization of Ge nanowires. Nanowires deposited at 95 °C have an average diameter of 100 nm, whereas those deposited at room temperature have an average diameter of 35 nm. Both optical absorption and Raman spectroscopy suggest that the electrodeposited Ge is degenerate. The material has an indirect bandgap of 0.90-0.92 eV, compared with a value of 0.67 eV for bulk, intrinsic Ge. The blue shift is attributed to the Moss-Burstein effect, because the material is a p-type degenerate semiconductor. On the basis of the magnitude of the blue shift, the hole concentration is estimated to be 8 × 10(19) cm(-3). This corresponds to an In impurity concentration of about 0.2 atom %. The resistivity of the wires is estimated to be 4 × 10(-5) Ω·cm. The high conductivity of the wires should make them ideal for lithium-ion battery applications.
Single-crystal Au is an excellent substrate for electrochemical epitaxial growth due to its chemical inertness, but the high cost of bulk Au single crystals prohibits their use in practical applications. Here, we show that ultrathin epitaxial films of Au electrodeposited onto Si(111), Si(100), and Si(110) wafers can serve as an inexpensive proxy for bulk single-crystal Au for the deposition of epitaxial films of cuprous oxide (Cu2O). The Au films range in thickness from 7.7 nm for a film deposited for 5 min to 28.3 nm for a film deposited for 30 min. The film thicknesses are measured by low-angle X-ray reflectivity and X-ray Laue oscillations. High-resolution TEM shows that there is not an interfacial SiOx layer between the Si and Au. The Au films deposited on the Si(111) substrates are smoother and have lower mosaic spread than those deposited onto Si(100) and Si(110). The mosaic spread of the Au(111) layer on Si(111) is only 0.15° for a 28.3 nm thick film. Au films deposited onto degenerate Si(111) exhibit ohmic behavior, whereas Au films deposited onto n-type Si(111) with a resistivity of 1.15 Ω·cm are rectifying with a barrier height of 0.85 eV. The Au and the Cu2O follow the out-of-plane and in-plane orientations of the Si substrates, as determined by X-ray pole figures. The Au and Cu2O films deposited on Si(100) and Si(110) are both twinned. The films grown on Si(100) have twins with a [221] orientation, and the films grown on Si(110) have twins with a [411] orientation. An interface model is proposed for all Si orientations, in which the -24.9% mismatch for the Au/Si system is reduced to only +0.13% by a coincident site lattice in which 4 unit meshes of Au coincide with 3 unit meshes of Si. Although this study only considers the deposition of epitaxial Cu2O films on electrodeposited Au/Si, the thin Au films should serve as high-quality substrates for the deposition of a wide variety of epitaxial materials.
Lu and Tang claim that the spin-coated films in our study are not epitaxial. They assume that all of the background intensity in the x-ray pole figures of the spin-coated materials is due to randomly oriented grains. There is no evidence for randomly oriented grains in the 2θ x-ray patterns. The background intensity in the pole figures is also comparable to the background from the single-crystal substrates, which is inconsistent with their assumption.
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