A two-dimensional epitaxial growth template for organic semiconductors was developed using a new method for transferring clean graphene sheets onto a substrate with controlled surface wettability. The introduction of a sacrificial graphene layer between a patterned polymeric supporting layer and a monolayer graphene sheet enabled the crack-free and residue-free transfer of free-standing monolayer graphene onto arbitrary substrates. The clean graphene template clearly induced the quasi-epitaxial growth of crystalline organic semiconductors with lying-down molecular orientation while maintaining the "wetting transparency", which allowed the transmission of the interaction between organic molecules and the underlying substrate. Consequently, the growth mode and corresponding morphology of the organic semiconductors on graphene templates exhibited distinctive dependence on the substrate hydrophobicity with clear transition from lateral to vertical growth mode on hydrophilic substrates, which originated from the high surface energy of the exposed crystallographic planes of the organic semiconductors on graphene. The optical properties of the pentacene layer, especially the diffusion of the exciton, also showed a strong dependency on the corresponding morphological evolution. Furthermore, the effect of pentacene-substrate interaction was systematically investigated by gradually increasing the number of graphene layers. These results suggested that the combination of a clean graphene surface and a suitable underlying substrate could serve as an atomically thin growth template to engineer the interaction between organic molecules and aromatic graphene network, thereby paving the way for effectively and conveniently tuning the semiconductor layer morphologies in devices prepared using graphene.

Human skin plays a critical role in a person communicating with his or her environment through diverse activities such as touching or deforming an object. Various electronic skin (E‐skin) devices have been developed that show functional or geometrical superiority to human skin. However, research into stretchable E‐skin that can simultaneously distinguish materials and textures has not been established yet. Here, the first approach to achieving a stretchable multimodal device is reported, that operates on the basis of various electrical properties of piezoelectricity, triboelectricity, and piezoresistivity and that exceeds the capabilities of human tactile perception. The prepared E‐skin is composed of a wrinkle‐patterned silicon elastomer, hybrid nanomaterials of silver nanowires and zinc oxide nanowires, and a thin elastomeric dielectric layer covering the hybrid nanomaterials, where the dielectric layer exhibits high surface roughness mimicking human fingerprints. This versatile device can identify and distinguish not only mechanical stress from a single stimulus such as pressure, tensile strain, or vibration but also that from a combination of multiple stimuli. With simultaneous sensing and analysis of the integrated stimuli, the approach enables material discrimination and texture recognition for a biomimetic prosthesis when the multifunctional E‐skin is applied to a robotic hand.

The development of layer-oriented two-dimensional conjugated metal–organic frameworks (2D c-MOFs) enables access to direct charge transport, dial-in lateral/vertical electronic devices, and the unveiling of transport mechanisms but remains a significant synthetic challenge. Here we report the novel synthesis of metal-phthalocyanine-based p-type semiconducting 2D c-MOF films (Cu2[PcM–O8], M = Cu or Fe) with an unprecedented edge-on layer orientation at the air/water interface. The edge-on structure formation is guided by the preorganization of metal-phthalocyanine ligands, whose basal plane is perpendicular to the water surface due to their π–π interaction and hydrophobicity. Benefiting from the unique layer orientation, we are able to investigate the lateral and vertical conductivities by DC methods and thus demonstrate an anisotropic charge transport in the resulting Cu2[PcCu–O8] film. The directional conductivity studies combined with theoretical calculation identify that the intrinsic conductivity is dominated by charge transfer along the interlayer pathway. Moreover, a macroscopic (cm2 size) Hall-effect measurement reveals a Hall mobility of ∼4.4 cm2 V–1 s–1 for the obtained Cu2[PcCu–O8] film. The orientation control in semiconducting 2D c-MOFs will enable the development of various optoelectronic applications and the exploration of unique transport properties.

Optimized geometry of single‐walled carbon nanotubes (SWCNTs) is vital to high‐performance transparent conductive films (TCFs). Herein, the geometry of SWCNTs, i.e., tube diameter, bundle length, and bundle diameter, are successfully tuned by introducing carbon dioxide (CO2) into floating catalyst chemical vapor deposition (FC‐CVD), where carbon monoxide (CO) is used as a carbon source and ferrocene as a catalyst precursor. Both tube diameter and bundle length increase with an increment of CO2 concentration, and the yield of SWCNTs can be significantly promoted with the appropriate amount of CO2. The role of CO2 in this behavior is further rationalized as enhancing CO decomposition or carbon dissolution into catalysts. The TCFs based on SWCNTs with optimized geometry by CO2 exhibit improved performance up to 86.8 Ω sq−1 at 90% transmittance after AuCl3 doping, achieving about 50% reduction of sheet resistance compared to the TCFs without CO2. The use of CO2 for directly tuning growth of SWCNTs blazes a new trail in the field of SWCNT based TCFs.

Atomically thin 2D materials are good templates to grow organic semiconductor thin films with desirable features. However, the 2D materials typically exhibit surface roughness and spatial charge inhomogeneity due to nonuniform doping, which can affect the uniform assembly of organic thin films on the 2D materials. A hybrid template is presented for preparation of highly crystalline small‐molecule organic semiconductor thin film that is fabricated by transferring graphene onto a highly ordered self‐assembled monolayer. This hybrid graphene template has low surface roughness and spatially uniform doping, and it yields highly crystalline fullerene thin films with grain sizes >300 nm, which is the largest reported grain size for C60 thin films on 2D materials. A graphene/fullerene/pentacene phototransistor fabricated directly on the hybrid template has five times higher photoresponsivity than a phototransistor fabricated on a conventional graphene template supported by a SiO2 wafer.