Near-Field Radiative Heat Transfer Modulation with an Ultrahigh Dynamic Range through Mode Mismatching.

Modulating near-field radiative heat transfer (NFRHT) with a high dynamic range is challenging in nanoscale thermal science and engineering. Modulation depths [(maximum value - minimum value)/(maximum value + minimum value) × 100%] of ≈2% to ≈15.7% have been reported with matched modes, but breaking the constraint of mode matching theoretically allows for higher modulation depth. We demonstrate a modulation depth of ≈32.2% by a pair of graphene-covered SU8 heterostructures at a gap distance of ≈80 nm. Dissimilar Fermi levels tuned by bias voltages enable mismatched surface plasmon polaritons which improves the modulation. The modulation depth when switching from a matched mode to a mismatched mode is ≈4.4-fold compared to that when switching between matched modes. This work shows the importance of symmetry in polariton-mediated NFRHT and represents the largest modulation depth to date in a two-body system with fixed gap distance and temperature.

Controlled Multistep Self-Assembling of Colloidal Droplets at a Nematic Liquid Crystal-Air Interface.

We present a controlled cascade of self-assemblings of colloidal droplets at a nematic liquid crystal-air interface into large-scale ordered structures. Changing the tilt of the droplet-induced elastic dipoles via its dependence on the nematic film thickness, we are able to control the dipole-dipole interaction and thus the self-assembling regime. For a progressively large tilt, droplets form anisotropic lattices, which then transform into arrays of repulsive chains, then to bands of half-period-shifted densely bound chains. These structures with chain order at the inner scale aggregate into different large-scale clusters that have a pronounced circular pattern and are stabilized by the many-body elastocapillary attraction.

Inhomogeneity-Induced Casimir Transport of Nanoparticles.

We propose a scheme for transporting nanoparticles immersed in a fluid, relying on quantum vacuum fluctuations. The mechanism lies in the inhomogeneity-induced lateral Casimir force between a nanoparticle and a gradient metasurface and the relaxation of the conventional Dzyaloshinskiǐ-Lifshitz-Pitaevskiǐ constraint, which allows quantum levitation for a broader class of material configurations. The velocity for a nanosphere levitated above a grating is calculated and can be up to a few microns per minute. The Born approximation gives general expressions for the Casimir energy which reveal size-selective transport. For any given metasurface, a certain particle-metasurface separation exists where the transport velocity peaks, forming a "Casimir passage." The sign and strength of the Casimir interactions can be tuned by the shapes of liquid-air menisci, potentially allowing real-time control of an otherwise passive force, and enabling interesting on-off or directional switching of the transport process.

Lasing properties of a cholesteric liquid crystal containing aggregation-induced-emission material.

We demonstrate band edge lasing action from a cholesteric liquid crystal (CLC) containing an aggregation-induced-emission (AIE) dye as gain material. AIE materials do not suffer aggregation-caused quenching, have strong resistance to photobleaching, and can show large Stokes shift. The amplified spontaneous emission (ASE) and lasing emission of the dye-doped CLC cell have been characterized, the lasing threshold has been estimated, and its resistance to photobleaching has been measured. AIE materials with their unique properties are especially suitable for acting as gain materials in liquid crystal lasers where defect structures lower the threshold for nanoscale aggregation effects. Our studies have shown that such AIE-dye-doped CLC is capable of lasing action with unusually large Stokes shift at moderate threshold with strong resistance to photobleaching.

Orientationally ordered colloidal co-dispersions of gold nanorods and cellulose nanocrystals.

Nematic-like and helicoidally orientational self-assemblies of gold nanorods co-dispersed with cellulose nanocrystals to form liquid crystalline phases are developed. Polarization-sensitive extinction spectra and two-photon luminescence imaging are used to characterize orientations and spatial distributions of gold nanorods. Cholesteric-isotropic phase coexistence and continuous domains of single-phase regions are observed and qualitatively discussed on the basis of entropic and electrostatic interactions in co-dispersions of rigid rods of different aspect ratios. Potential applications include biologically compatible plasmonic composite nanomaterials for solar biofuel production and polarization-sensitive plasmonic papers and fabrics.

Preparation of Nanocomposite Plasmonic Films Made from Cellulose Nanocrystals or Mesoporous Silica Decorated with Unidirectionally Aligned Gold Nanorods.

Using liquid crystalline self-assembly of cellulose nanocrystals, we achieve long-range alignment of anisotropic metal nanoparticles in colloidal nanocrystal dispersions that are then used to deposit thin structured films with ordering features highly dependent on the deposition method. These hybrid films are comprised of gold nanorods unidirectionally aligned in a matrix that can be made of ordered cellulose nanocrystals or silica nanostructures obtained by using cellulose-based nanostructures as a replica. The ensuing long-range alignment of gold nanorods in both cellulose-based and nanoporous silica films results in a polarization-sensitive surface plasmon resonance. The demonstrated device-scale bulk nanoparticle alignment may enable engineering of new material properties arising from combining the orientational ordering of host nanostructures and properties of the anisotropic plasmonic metal nanoparticles. Our approach may also allow for scalable fabrication of plasmonic polarizers and nanoporous silica structures with orientationally ordered anisotropic plasmonic nanoinclusions.

Active shape-morphing elastomeric colloids in short-pitch cholesteric liquid crystals.

Active elastomeric liquid crystal particles with initial cylindrical shapes are obtained by means of soft lithography and polymerization in a strong magnetic field. Gold nanocrystals infiltrated into these particles mediate energy transfer from laser light to heat, so that the inherent coupling between the temperature-dependent order and shape allows for dynamic morphing of these particles and well-controlled stable shapes. Continuous changes of particle shapes are followed by their spontaneous realignment and transformations of director structures in the surrounding cholesteric host, as well as locomotion in the case of a nonreciprocal shape morphing. These findings bridge the fields of liquid crystal solids and active colloids, may enable shape-controlled self-assembly of adaptive composites and light-driven micromachines, and can be understood by employing simple symmetry considerations along with electrostatic analogies.

Optical manipulation of self-aligned graphene flakes in liquid crystals.

Graphene recently emerged as a new two-dimensional material platform with unique optical, thermal and electronic properties. Single- or few-atom-thick graphene flakes can potentially be utilized to form structured bulk composites that further enrich these properties and enable a broad range of new applications. Here we describe optical manipulation of self-aligned colloidal graphene flakes in thermotropic liquid crystals of nematic and cholesteric types. Three-dimensional rotational and translational manipulation of graphene flakes by means of holographic optical tweezers allows for non-contact spatial patterning of graphene, control of liquid crystal defects, and low-power optical realignment of the liquid crystal director using these flakes. Potential applications include optically- and electrically-controlled reconfigurable liquid crystalline dispersions of spontaneously aligning colloidal graphene flakes and new electro-optic devices with graphene-based interconnected transparent electrodes at surfaces and in the bulk of liquid crystals.

Shape-dependent oriented trapping and scaffolding of plasmonic nanoparticles by topological defects for self-assembly of colloidal dimers in liquid crystals.

We demonstrate scaffolding of plasmonic nanoparticles by topological defects induced by colloidal microspheres to match their surface boundary conditions with a uniform far-field alignment in a liquid crystal host. Displacing energetically costly liquid crystal regions of reduced order, anisotropic nanoparticles with concave or convex shapes not only stably localize in defects but also self-orient with respect to the microsphere surface. Using laser tweezers, we manipulate the ensuing nanoparticle-microsphere colloidal dimers, probing the strength of elastic binding and demonstrating self-assembly of hierarchical colloidal superstructures such as chains and arrays.

Templating of self-alignment patterns of anisotropic gold nanoparticles on ordered SWNT macrostructures.

We report a simple and versatile technique for oriented assembly of gold nanorods on aligned single-walled carbon nanotube (SWNT) macrostructures, such as thin nanotube films and nanotube fibers. The deposition and assembly is accomplished via drop drying of dilute gold nanorod suspensions on SWNT macrostructures under ambient conditions. Guided by anisotropic interactions, gold nanorods, and polygonal platelets spontaneously align with SWNTs, resulting in macroscopic arrays of locally ordered nanorods supported on aligned SWNT substrates. SEM reveals that the scalar order parameter of rods relative to the local average SWNT alignment is 0.7 for rods on SWNT films and 0.9 for rods on SWNT fibers. This self-alignment is enabled by anisotropic gold nanoparticle-SWNT interactions and is observed for a wide range of nanoparticles, including nanorods with aspect ratios ranging from 2-35, thin gold triangular and other polygonal platelets. The plasmonic properties of aligned gold nanorods together with superior electronic, chemical and mechanical properties of SWNTs make these hybrid nanocomposites valuable for the design of self-assembled multifunctional optoelectronic materials and optical metamaterials.