Heterojunctions between different graphitic nanostructures, including fullerenes, carbon nanotubes and graphene-based sheets, have attracted significant interest for light to electrical energy conversion. Because of their poor solubility, fabrication of such all-carbon nanocomposites typically involves covalently linking the individual constituents or the extensive surface functionalization to improve their solvent processability for mixing. However, such strategies often deteriorate or contaminate the functional carbon surfaces. Here we report that fullerenes, pristine single walled carbon nanotubes, and graphene oxide sheets can be conveniently coassembled in water to yield a stable colloidal dispersion for thin film processing. After thermal reduction of graphene oxide, a solvent-resistant photoconductive hybrid of fullerene-nanotube-graphene was obtained with on-off ratio of nearly 6 orders of magnitude. Photovoltaic devices made with the all-carbon hybrid as the active layer and an additional fullerene block layer showed unprecedented photovoltaic responses among all known all-carbon-based materials with an open circuit voltage of 0.59 V and a power conversion efficiency of 0.21%. The ease of making such surfactant-free, water-processed, carbon thin films could lead to their wide applications in organic optoelectronic devices.
We report a simple method that uses (i) emulsion shearing with oxidation to make core-shell particles, and (ii) emulsion shearing with surface-tension driven phase segregation to synthesize particles with complex surface compositions and morphologies. Subjecting eutectic gallium-indium, a liquid metal, to shear in an acidic carrier fluid we synthesized smooth liquid core-shell particles 6.4 nm to over 10 μm in diameter. Aggregates of these liquid particles can be reconfigured into larger structures using a focused ion beam. Using Field's metal melts we synthesized homogeneous nanoparticles and solid microparticles with different surface roughness and/or composition through shearing and phase separation. This extension of droplet emulsion technique, SLICE, applies fluidic shear to create micro- and nanoparticles in a tunable, green, and low-cost approach.
The origin of the odd-even effect in properties of self-assembled monolayers (SAMs) and/or technologies derived from them is poorly understood. We report that hydrophobicity and, hence, surface wetting of SAMs are dominated by the nature of the substrate (surface roughness and identity) and SAM tilt angle, which influences surface dipoles/orientation of the terminal moiety. We measured static contact angles (θs) made by water droplets on n-alkanethiolate SAMs with an odd (SAM(O)) or even (SAM(E)) number of carbons (average θs range of 105.8-112.1°). When SAMs were fabricated on smooth "template-stripped" metal (M(TS)) surfaces [root-mean-square (rms) roughness = 0.36 ± 0.01 nm for Au(TS) and 0.60 ± 0.04 nm for Ag(TS)], the odd-even effect, characterized by a zigzag oscillation in values of θs, was observed. We, however, did not observe the same effect with rougher "as-deposited" (M(AD)) surfaces (rms roughness = 2.27 ± 0.16 nm for Au(AD) and 5.13 ± 0.22 nm for Ag(AD)). The odd-even effect in hydrophobicity inverts when the substrate changes from Au(TS) (higher θs for SAM(E) than SAM(O), with average Δθs |n - (n + 1)| ≈ 3°) to Ag(TS) (higher θs for SAM(O) than SAM(E), with average Δθs |n - (n + 1)| ≈ 2°). A comparison of hydrophobicity across Ag(TS) and Au(TS) showed a statistically significant difference (Student's t test) between SAM(E) (Δθs |Ag evens - Au evens| ≈ 5°; p < 0.01) but failed to show statistically significant differences on SAM(O) (Δθs |Ag odds - Au odds| ≈ 1°; p > 0.1). From these results, we deduce that the roughness of the metal substrate (from comparison of M(AD) versus M(TS)) and orientation of the terminal -CH2CH3 (by comparing SAM(E) and SAM(O) on Au(TS) versus Ag(TS)) play major roles in the hydrophobicity and, by extension, general wetting properties of n-alkanethiolate SAMs.
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