The self-assembly of monodisperse inorganic nanoparticles into highly ordered arrays (superlattices) represents an exciting route to materials and devices with new functions. It allows programming their properties by varying the size, shape, and composition of the nanoparticles, as well as the packing order of the assemblies. While substantial progress has been achieved in the fabrication of superlattice materials made of nanospheres, limited advances have been made in growing similar materials with anisotropic building blocks, which is particularly true for free-standing two-dimensional superlattices. In this paper, we report the controlled growth of free-standing, large-area, monolayered gold-nanorod superlattice sheets by polymer ligands in an entropy-driven interfacial self-assembly process. Furthermore, we experimentally characterize the plasmonic properties of horizontally aligned sheets (H-sheets) and vertically aligned sheets (V-sheets) and show that observed features can be well described using a theoretical model based on the discrete-dipole approximation. Our polymer-ligand-based strategy may be extended to other anisotropic plasmonic building blocks, offering a robust and inexpensive avenue to plasmonic nanosheets for various applications in nanophotonic devices and sensors.

We report on an anomalous size dependence of the room-temperature photoluminescence decay time from the lowest-energy state of PbS quantum dots in colloidal solution, which was found using the transient luminescence spectroscopy. The observed 10-fold reduction in the decay time (from ~2.5 to 0.25 μs) with the increase in the quantum dots' diameter is explained by the existence of phonon-induced transitions between the in-gap state-whose energy drastically depends on the diameter-and the fundamental state of the quantum dots.

We present an improved analytical model describing transmittance of a metal-dielectric-metal (MDM) waveguide coupled to an arbitrary number of stubs. The model is built on the well-known analogy between MDM waveguides and microwave transmission lines. This analogy allows one to establish equivalent networks for different MDM-waveguide geometries and to calculate their optical transmission spectra using standard analytical tools of transmission-line theory. A substantial advantage of our model compared to earlier works is that it precisely incorporates the dissipation of surface plasmon polaritons resulting from ohmic losses inside any metal at optical frequencies. We derive analytical expressions for transmittance of MDM waveguides coupled to single and double stubs as well as to N identical stubs with a periodic arrangement. We show that certain phase-matching conditions must be satisfied to provide opt al filtering characteristics for such waveguides. To check the accuracy of our model, its results are compared with numerical data obtained from the full-blown finite-difference time-domain simulations. Close agreement between the two suggests that our analytical model is suitable for rapid design optimization of MDM-waveguide-based compact photonic devices.

Carbon dots (CDots) are a promising biocompatible nanoscale source of light, yet the origin of their emission remains under debate. Here, we show that all the distinctive optical properties of CDots, including the giant Stokes shift of photoluminescence and the strong dependence of emission color on excitation wavelength, can be explained by the linear optical response of the partially sp2-hybridized carbon domains located on the surface of the CDots’ sp3-hybridized amorphous cores. Using a simple quantum chemical approach, we show that the domain hybridization factor determines the localization of electrons and the electronic bandgap inside the domains and analyze how the distribution of this factor affects the emission properties of CDots. Our calculation data fully agree with the experimental optical properties of CDots, confirming the overall theoretical picture underlying the model. It is also demonstrated that fabrication of CDots with large hybridization factors of carbon domains shifts their emission to the red side of the visible spectrum, without a need to modify the size or shape of the CDots. Our theoretical model provides a useful tool for experimentalists and may lead to extending the applications of CDots in biophysics, optoelectronics, and photovoltaics.

Metasurfaces with actively tunable features are highly demanded for advanced applications in electronic and electromagnetic systems. However, realizing independent dual-tunability remains challenging and requires more efforts. In this paper, we present an active metasurface where the magnitude and frequency of the resonant absorption can be continuously and independently tuned through application of voltage biases. Such a dual-tunability is accomplished at microwave frequencies by combining a varactor-loaded high-impedance surface and a graphene-based sandwich structure. By electrically controlling the Fermi energy of graphene and the capacitance of varactor diodes, we experimentally demonstrate the independent shifting of the working frequency from 3.41 to 4.55 GHz and tuning of the reflection amplitude between −3 and −30 dB, which is in excellent agreement with full-wave numerical simulations. We further employed an equivalent lumped circuit model to elucidate the mechanism of the dual-tunability resulting from the graphene-based sandwich structure and the active high-impedance surface. We speculate that such a dual-tunability scheme can be potentially extended to terahertz and optical regimes by employing different active/dynamical tuning methods and materials integration, thereby enabling a variety of practical applications.

Two-dimensional (2D) nanomaterials have been intensively investigated due to their interesting properties and range of potential applications. Although most research has focused on graphene, atomic layered transition metal dichalcogenides (TMDs) and particularly MoS2 have gathered much deserved attention recently. Here, we report the induction of chirality into 2D chiral nanomaterials by carrying out liquid exfoliation of MoS2 in the presence of chiral ligands (cysteine and penicillamine) in water. This processing resulted in exfoliated chiral 2D MoS2 nanosheets showing strong circular dichroism signals, which were far past the onset of the original chiral ligand signals. Using theoretical modeling, we demonstrated that the chiral nature of MoS2 nanosheets is related to the presence of chiral ligands causing preferential folding of the MoS2 sheets. There was an excellent match between the theoretically calculated and experimental spectra. We believe that, due to their high aspect ratio planar morphology, chiral 2D nanomaterials could offer great opportunities for the development of chiroptical sensors, materials, and devices for valleytronics and other potential applications. In addition, chirality plays a key role in many chemical and biological systems, with chiral molecules and materials critical for the further development of biopharmaceuticals and fine chemicals, and this research therefore should have a strong impact on relevant areas of science and technology such as nanobiotechnology, nanomedicine, and nanotoxicology.

This work presents a comprehensive study of electroabsorption in CdSe colloidal quantum dots, nanorods, and nanoplatelets. We experimentally demonstrate that the exposure of the nanoplatelets to a dc electric field leads to strong broadening of their lowest-energy heavy-hole absorption band and drastically reduces the absorption efficiency within the band. These are results of the quantum-confined Stark and Franz–Keldysh effects. The field-induced change in the nanoplatelets’ absorption is found to be more than 10 times the change in the absorption by the quantum dots. We also demonstrate that the electroabsorption by the nanorods is weaker than that by the quantum dots and nanoplatelets and reveal an unusual dependence of the differential absorption changes on the nanoplatelet thickness: the thicker the nanoplatelet, the smaller the change.

Fast and reliable separation of enantiomers of chiral nanoparticles requires elimination of all the forces that are independent of the nanoparticle handedness and creation of a sufficiently strong force that either pushes different enantiomers in opposite directions or delays the diffusion of one of them with respect to the other. Here we show how to construct such a completely chiral optical force using two counterpropagating circularly polarized plane waves of opposite helicities. We then explore capabilities of the related enantioseparation method by analytically solving the problem of the force-induced diffusion of chiral nanoparticles in a confined region, and reveal that it results in exponential spatial dependencies of the quantities measuring the purity of chiral substances. The proposed concept of a completely chiral optical force can potentially advance enantioseparation and enantiopurification techniques for all kinds of chiral nanoparticles that strongly interact with light.