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Fabrication of Uniaxially Aligned Silica Nanogrooves with Sub-5 nm Periodicity on Centimeter-Scale Si Substrate Using Poly(dimethylsiloxane) Stamp
摘要： The large-area fabrication of aligned nanopatterns with sub-5 nm feature size is crucial for developing nanodevices. Highly ordered nanostructures fabricated through molecular self-assembly exhibit substantial potential for sub-5 nm patterning techniques. Previously, we had reported the fabrication of silica nanogrooves with sub-5 nm periodicity on a Si substrate by using the outermost surfaces of cylindrical surfactant micelles as a template. However, uniaxial alignment of nanogrooves on the entire substrate surface has not yet been achieved. In this study, uniaxially aligned silica nanogrooves were prepared on the entire surface of a Si substrate (2 × 2 cm) by utilizing a poly(dimethylsiloxane) (PDMS) stamp with a striped pattern. The PDMS stamp was placed on the surface of a surfactant thin film precoated on the substrate, although the stamp was not in direct contact with the substrate as in the case of the soft nanoimprint technique. The substrate was then exposed to water vapor, during which cylindrical micelles were aligned in the direction of the guide. Subsequently, by exposing the substrate to an NH3–water vapor mixture, the outermost surfaces of the aligned micelles facing the substrate were replicated with soluble silicate species. The formation of uniaxially aligned nanogrooves on the entire surface of the centimeter-scale substrate was verified by scanning electron microscopy observations and grazing-incidence small-angle X-ray scattering analysis. Thus, herein we provide a simple large-area fabrication method for uniaxially aligned nanopattern with ultra-fine pitch.
关键词： nanoimprint,nanopatterning,alignment control,directed self-assembly,liquid crystals
更新于2025-09-23 15:23:52
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Hierarchical Photonic Pigments <i>via</i> the Confined Self-Assembly of Bottlebrush Block Copolymers
摘要： Hierarchical, structurally colored materials offer a wide variety of visual effects that cannot be achieved with standard pigments or dyes. However, their fabrication requires simultaneous control over multiple length-scales. Here we introduce a robust strategy for the fabrication of hierarchical photonic pigments via the confined self-assembly of bottlebrush block copolymers within emulsified microdroplets. The bottlebrush block copolymer self-assembles into highly ordered concentric lamellae, giving rise to a near perfect photonic multi-layer in the solid-state, with reflectivity up to 100%. The reflected color can be readily tuned across the whole visible spectrum by either altering the molecular weight or by blending the bottlebrush block copolymers. Furthermore, the developed photonic pigments are responsive, with a selective and reversible color change observed upon swelling in different solvents. Our system is particularly suited for the scalable production of photonic pigments, arising from their rapid self-assembly mechanism and size-independent color.
关键词： photonic crystals,confined self-assembly,microspheres,structural colors,bottlebrush block copolymers
更新于2025-09-23 15:23:52
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Dispersion relations of elastic waves in three-dimensional cubical piezoelectric phononic crystal with initial stresses and mechanically and dielectrically imperfect interfaces
摘要： The shape of individual building blocks is an important parameter in bottom-up self-assembly of nano-structured materials. A simple shape change from sphere to spheroid can significantly affect the assembly process due to the modification to the orientational degrees of freedom. When a layer of spheres is placed upon a layer of spheroids, the strain at the interface can be minimized by the spheroid taking a special orientation. C70 fullerenes represent the smallest spheroids, and their interaction with a sphere-like C60 is investigated. We find that the orientation of the C70 within a close-packed C70 layer can be steered by contacting a layer of C60. This orientational steering phenomenon is potentially useful for epitaxial growth of multilayer van der Waals molecular heterostructures.
关键词： interface,self-assembly,epitaxy,scanning tunnelling microscopy,graphene,van der Waals heterostructures,fullerene
更新于2025-09-23 15:23:52
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Mechanism of field-induced manipulation of Cu-phthalocyanines on a Bi surface using scanning tunneling microscope
摘要： We have revisited our hypothesis [K. Nagaoka et al., Jpn. J. Appl. Phys. 57 (2018) 020301] regarding the control of the motion and assembly of copper phthalocyanine (CuPc) molecules on a Bi(001) surface using a scanning tunneling microscope (STM) tip. The proposal that the observed diffusion and condensation are not due to the adsorption/desorption of molecules via the tip by applying a bias voltage was investigated for field-induced manipulation. Our experiments show that CuPc cannot move across steps or condense on different terraces on the Bi(001) surface. When confined to a nano-scale region, the CuPc molecules assemble into ordered single-layer islands. The island position can be manipulated using the STM tip, with an almost constant number of condensed molecules remaining inside the terrace. These results allowed us to rule out the possibility of picking-up and depositing molecules by the STM tip.
关键词： STM,phthalocyanine,self-assembly,field-induced manipulation,bismuth,surface science
更新于2025-09-23 15:23:52
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Layer-by-layer self-assembly of polyaniline nanofibers/TiO2 nanotubes heterojunction thin film for ammonia detection at room temperature
摘要： In this paper, for the first time, polyaniline nanofibers/TiO2 nanotubes (PANI/TiO2) heterojunction thin film has been prepared on Pt interdigital electrodes by layer-by-layer self-assembly method and applied in room temperature NH3 detection. It is found that the optimal self-assembly layer number is three (PANI/TiO2-3) compared to one layer (PANI/TiO2-1) and five layers (PANI/TiO2-5). The PANI/TiO2-3 thin film sensor possesses superior response characteristics compared with our other PANI based sensors, including higher response value (336%@5 ppm NH3), acceptable response/recovery time (110 s/1086 s@5 ppm NH3), low detection limit (0.5 ppm), and remarkable selectivity. The enhanced gas sensing performances could be ascribed to the tremendous variation of the carrier concentration caused by the p-n junctions as well as the increased specific surface area and pore volume. This work not only offers a superb strategy to fabricate heterojunction thin film but also accelerates the development of room-temperature operable NH3 sensors.
关键词： Ammonia detection,Layer-by-layer self-assembly,Polyaniline/TiO2 heterojunction,Thin film,Room temperature operation
更新于2025-09-23 15:23:52
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[IEEE 2018 IEEE CPMT Symposium Japan (ICSJ) - Kyoto, Japan (2018.11.19-2018.11.21)] 2018 IEEE CPMT Symposium Japan (ICSJ) - A 53-Gbit/s VCSEL-Based High Density Optical Assembly for Large Capacity Optical Interconnection
摘要： A 53-Gbit/s VCSEL-based compact optical module is proposed. In order to realize 50-Gbit/s-class optical transmission, high-bandwidth optical devices are important. Accordingly, the feasibilities of a high speed optical circuit applying high-bandwidth (> 20 GHz) optical devices were studied by simulation. Moreover, an optical module at the receiver (Rx) side was fabricated on the basis of simulation results by applying our developed high density optical assembly techniques, and it successfully demonstrated 53.125-Gbit/s PAM4 multimode optical transmission.
关键词： compact optical module,High-density optical assembly,Optical interconnect,4-level pulse amplitude modulation (PAM4)
更新于2025-09-23 15:22:29
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Photoinduced electron transfer kinetics of linked Ru-Co photocatalyst dyads
摘要： Two new supramolecular photocatalyst dyads based on the [Ru(2,2′-bipyridine)3]2+ photosensitizer linked to a macrocyclic Co(II)tetra(pyridyl) catalyst for proton reduction are reported. The dyads differ primarily in the bridging ligand which links the molecular modules; the first being a short and flexible linker, and the second a longer and electronically conjugated linker. Ultrafast transient optical spectroscopy was used to monitor the photoinduced kinetics of the dyads following visible excitation of the photosensitizer module. Direct comparison of transient spectra and kinetics indicates that there are indeed substantial differences between the ultrafast transient optical spectroscopy of the dyads, but there is no indication of oxidative quenching of the photosensitizer module by the catalyst module. These initial design and characterization studies of the linked Ru(II)—Co(II) dyads provide an important foundation for advanced designs of systems for efficient solar energy conversion by molecular architectures.
关键词： Ruthenium,Cobalt,Photoinduced electron transfer,Modular assembly,Photocatalyst dyads
更新于2025-09-23 15:22:29
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Ordered Array of Metal Particles on Semishell Separated with Ultrathin Oxide: Fabrication and SERS Properties
摘要： Metal particles in gap cavities provide an interesting system to achieve hybrid local surface plasmon modes for local field enhancement. Here, we demonstrate a relatively simple method to fabricate Ag nanoparticles positioned on Ag semishells separated by a thin (~5 nm) dielectric layer. The obtained structure can provide strong local electric field enhancement for surface-enhanced Raman scattering (SERS). The fabrication of the ordered array structure was realized by nanosphere self-assembly, atomic layer deposition, and metal thin-film dewetting. Numerical simulation proved that, compared to the conventional metal semishell arrays, the additional Ag particles introduce extra hot spots particularly in the valley regions between adjacent Ag semishells. As a result, the SERS enhancement factor of the metal semishell-based plasmonic structure could be further improved by an order of magnitude. The developed novel plasmonic structure also shows good potential for application in plasmon-enhanced solar water-splitting devices.
关键词： particle in cavity,nanosphere lithography,surface-enhanced Raman scattering (SERS),surface plasmonic,monolayer self-assembly
更新于2025-09-23 15:22:29
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Chiral Recognition of L- and D- Amino Acid by Porphyrin Supramolecular Aggregates
摘要： We report of the interactions between four amino acids lysine (Lys), arginine (Arg), histidine (His), and phenylalanine (Phe) with the J-aggregates of the protonated 5,10,15,20-tetrakis(4-sulfonatophenyl)-porphyrin H4TPPS. Several aspects of these self-assembled systems have been analyzed: (i) the chiral transfer process; (ii) the hierarchical effects leading to the aggregates formation; and, (iii) the influence of the amino acid concentrations on both transferring and storing chiral information. We have demonstrated that the efficient control on the J-aggregates chirality is obtained when all amino acids are tested and that the chirality transfer process is under hierarchical control. Finally, the chiral porphyrin aggregates obtained exhibit strong chiral inertia.
关键词： porphyrin,self-assembly,amino acid,circular dichroism,supramolecular chirality
更新于2025-09-23 15:22:29
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Fingerprints of sp1 Hybridized C in the Near-Edge X-ray Absorption Spectra of Surface-Grown Materials
摘要： Carbon structures comprising sp1 chains (e.g., polyynes or cumulenes) can be synthesized by exploiting on-surface chemistry and molecular self-assembly of organic precursors, opening to the use of the full experimental and theoretical surface-science toolbox for their characterization. In particular, polarized near-edge X-ray absorption fine structure (NEXAFS) can be used to determine molecular adsorption angles and is here also suggested as a probe to discriminate sp1/sp2 character in the structures. We present an ab initio study of the polarized NEXAFS spectrum of model and real sp1/sp2 materials. Calculations are performed within density functional theory with plane waves and pseudopotentials, and spectra are computed by core-excited C potentials. We evaluate the dichroism in the spectrum for ideal carbynes and highlight the main differences relative to typical sp2 systems. We then consider a mixed polymer alternating sp1 C4 units with sp2 biphenyl groups, recently synthesized on Au(111), as well as other linear structures and two-dimensional networks, pointing out a spectral line shape specifically due to the presence of linear C chains. Our study suggests that the measurements of polarized NEXAFS spectra could be used to distinctly fingerprint the presence of sp1 hybridization in surface-grown C structures.
关键词： density functional theory,self-assembly,carbynes,on-surface chemistry,near edge X-ray absorption spectroscopy,C 1s absorption
更新于2025-09-23 15:22:29