The formation of water-in-oil-in-water (W/O/W) double emulsions can be well-controlled through an organized self-emulsification mechanism in the presence of rigid bottlebrush amphiphilic block copolymers. Nanoscale water droplets with well-controlled diameters form ordered spatial arrangements within the micron-scale oil droplets. Upon solvent evaporation, solid microspheres with hexagonal close packed nanopore arrays are obtained resulting in bright structural colors. The reflected color is precisely tunable across the whole visible light range through tailoring contour length of the bottlebrush molecule. In-situ observation of the W/O interface using confocal laser scanning microscopy provides insights into the mechanism of the organized self-emulsification. This work provides a powerful strategy for the fabrication of structural colored materials in an easy and scalable manner.
Capabilities of highly sensitive surface-enhanced infrared absorption (SEIRA) spectroscopy are demonstrated by exploiting large-area templates ($cm^2$) based on self-organized (SO) nanorod antennas. We engineered highly dense arrays of gold nanorod antennas featuring polarization-sensitive localized plasmon resonances, tunable over a broadband near- and mid-infrared (IR) spectrum, in overlap with the so-called functional group window. We demonstrate polarization-sensitive SEIRA activity, homogeneous over macroscopic areas and stable in time, by exploiting prototype self-assembled monolayers of IR-active octadecanthiol (ODT) molecules. The strong coupling between the plasmonic excitation and molecular stretching modes gives rise to characteristic Fano resonances in SEIRA. The SO engineering of the active hotspots in the arrays allows us to achieve signal amplitude improved up to 5.7%. This figure is competitive to the response of lithographic nanoantennas and is stable when the optical excitation spot varies from the micro- to macroscale, thus enabling highly sensitive SEIRA spectroscopy with cost-effective nanosensor devices.
The technique of passive daytime radiative cooling (PDRC) is used to cool an object down by simultaneously reflecting sunlight and thermally radiating heat to the cold outer space through the Earths atmospheric window. However, for practical applications, current PDRC materials are facing unprecedented challenges such as complicated and expensive fabrication approaches and performance degradation arising from surface contamination. Here, we develop a scalable paper-based material with excellent self-cleaning and self-cooling capabilities, through air-spraying ethanolic polytetrafluoroethylene (PTFE) microparticles suspensions embedded within the micropores of the paper. The formed superhydrophobic PTFE coating not only protects the paper from water wetting and dust contamination for real-life applications but also reinforces its solar reflectance by sunlight backscattering. The paper fibers, when enhanced with PTFE particles, efficiently reflect sunlight and strongly radiate heat through the atmospheric window, resulting in a sub-ambient cooling performance of 5$^{circ}$C and radiative cooling power of 104 W/m$^2$ under direct solar irradiance of 834 W/m$^2$ and 671 W/m$^2$, respectively. The self-cleaning surface of the cooling paper extends its lifespan and keep its good cooling performance for outdoor applications. Additionally, dyed papers are experimentally studied for broad engineering applications. They can absorb appropriate visible wavelengths to display specific colors and effectively reflect near-infrared lights to reduce solar heating, which synchronously achieves effective radiative cooling and aesthetic varieties in a cost-effective, scalable, and energy-efficient way.
Structural colors are produced by wavelength-dependent scattering of light from nanostructures. While living organisms often exploit phase separation to directly assemble structurally colored materials from macromolecules, synthetic structural colors are typically produced in a two-step process involving the sequential synthesis and assembly of building blocks. Phase separation is attractive for its simplicity, but applications are limited due to a lack of robust methods for its control. A central challenge is to arrest phase separation at the desired length scale. Here, we show that solid-state polymerization-induced phase separation can produce stable structures at optical length scales. In this process, a polymeric solid is swollen and softened with a second monomer. During its polymerization, the two polymers become immiscible and phase separate. As free monomer is depleted, the host matrix resolidifies and arrests coarsening. The resulting PS-PMMA composites have a blue or white appearance. We compare these biomimetic nanostructures to those in structurally-colored feather barbs, and demonstrate the flexibility of this approach by producing structural color in filaments and large sheets.
Elementary particles possess quantized values of charge and internal angular momentum or spin. These characteristics do not change when the particles interact with other particles or fields as long as they preserve their entities. Quantum theory does not explain this quantization. It is introduced into the theory a priori. An interacting particle is an open system and thus does not obey conservation laws. However, an open system may create dynamically stable states with unchanged dynamical variables via self-organization. In self-organized systems stability is achieved through the interplay of nonlinearity and dissipation. Can self-organization be responsible for particle formation? In this paper we develop and analyze a particle model based on qualitative dynamics and the Feigenbaum universality. This model demonstrates that elementary particles can be described as self-organized dynamical systems belonging to a wide class of systems characterized by a hierarchy of period-doubling bifurcations. This semi-qualitative heuristic model gives possible explanations for charge and action quantization, and the origination and interrelation between the strong, weak, and electromagnetic forces, as well as SU(2) symmetry. It also provides a basis for particle taxonomy endorsed by the Standard Model. The key result is the discovery that the Planck constant is intimately related to elementary charge.
Acting as artificial synapses, two-terminal memristive devices are considered fundamental building blocks for the realization of artificial neural networks. Organized into large arrays with a top-down approach, memristive devices in conventional crossbar architecture demonstrated the implementation of brain-inspired computing for supervised and unsupervised learning. Alternative way using unconventional systems consisting of many interacting nano-parts have been proposed for the realization of biologically plausible architectures where the emergent behavior arises from a complexity similar to that of biological neural circuits. However, these systems were unable to demonstrate bio-realistic implementation of synaptic functionalities with spatio-temporal processing of input signals similarly to our brain. Here we report on emergent synaptic behavior of biologically inspired nanoarchitecture based on self-assembled and highly interconnected nanowire (NW) networks realized with a bottom up approach. The operation principle of this system is based on the mutual electrochemical interaction among memristive NWs and NW junctions composing the network and regulating its connectivity depending on the input stimuli. The functional connectivity of the system was shown to be responsible for heterosynaptic plasticity that was experimentally demonstrated and modelled in a multiterminal configuration, where the formation of a synaptic pathway between two neuron terminals is responsible for a variation in synaptic strength also at non-stimulated terminals. These results highlight the ability of nanowire memristive architectures for building brain-inspired intelligent systems based on complex networks able to physically compute the information arising from multi-terminal inputs.