Brendan G. DeLacy

Transparent displays enabled by resonant nanoparticle scattering

We create a transparent display by projecting monochromatic images onto a polymer film embedded with nanoparticles that selectively scatter light at the projected wavelength. This approach features simplicity, wide viewing angle, scalability, and low cost.

Theoretical criteria for scattering dark states in nanostructured particles.

Nanostructures with multiple resonances can exhibit a suppressed or even completely eliminated scattering of light, called a scattering dark state. We describe this phenomenon with a general treatment of light scattering from a multiresonant nanostructure that is spherical or nonspherical but subwavelength in size. With multiple resonances in the same channel (i.e., same angular momentum and polarization), coherent interference always leads to scattering dark states in the low-absorption limit, regardless of the system details. The coupling between resonances is inevitable and can be interpreted as arising from far-field or near-field. This is a realization of coupled-resonator-induced transparency in the context of light scattering, which is related to but different from Fano resonances. Explicit examples are given to illustrate these concepts.

Fundamental Limits to Extinction by Metallic Nanoparticles

O. D. Miller, C. W. Hsu, 3 M. T. H. Reid, W. Qiu, B. G. DeLacy, J. D. Joannopoulos, M. Soljačić, and S. G. Johnson Department of Mathematics, Massachusetts Institute of Technology, Cambridge, MA 02139 Department of Physics, Massachusetts Institute of Technology, Cambridge, MA 02139 Department of Physics, Harvard University, Cambridge, MA 02138 U.S. Army Edgewood Chemical Biological Center, Research and Technology Directorate, Aberdeen Proving Ground, MD 21010

Optimization of broadband optical response of multilayer nanospheres

We propose an optimization-based theoretical approach to tailor the optical response of silver/silica multilayer nanospheres over the visible spectrum. We show that the structure that provides the largest cross-section per volume/mass, averaged over a wide frequency range, is the silver coated silica sphere. We also show how properly chosen mixture of several species of different nanospheres can have an even larger minimal cross-section per volume/mass over the entire visible spectrum.

Layer-by-layer self-assembly of plexcitonic nanoparticles

Colloidal suspensions of multilayer nanoparticles composed of a silver core, a polyelectrolyte spacer layer (inner shell), and a J-aggregate cyanine dye outer shell have been prepared for the first time. Absorption properties of the colloid were measured in the visible region. This multilayer architecture served as a framework for examining the coupling of the localized surface plasmon resonance exhibited by the silver core with the molecular exciton exhibited by the J-aggregate outer shell. The polyelectrolyte spacer layer promotes the formation of an excitonic J-aggregate while serving as a means of controlling the plasmon-exciton (i.e. plexciton) coupling strength through changing the distance between the core and the shell. An analytical expression based on Mie Theory and the Transfer Matrix Method was obtained for describing the optical response of these multilayered nanostructures. Computational and experimental results indicate that the absorption wavelength of the J-aggregate form of the dye is dependent on both the distance of the dye layer from the silver core and the degree of dye aggregation.

Transparent Displays Enabled by Resonant Nanoparticle Scattering

We create a transparent display by projecting monochromatic images onto a polymer film embedded with nanoparticles that selectively scatter light at the projected wavelength. This approach features simplicity, wide viewing angle, scalability, and low cost.

Effects of Molecular Structure and Solvent Polarity on Adsorption of Carboxylic Anchoring Dyes onto TiO2 Particles in Aprotic Solvents

Interactions of molecules with the surface of TiO2 particles are of fundamental and technological importance. One example is that the adsorption density and energy of the dye molecules on TiO2 particles affect the efficiency of dye-sensitized solar cells (DSSC). In this work, we present measurements characterizing the adsorption of the two isomers, para-ethyl red (p-ER) and ortho-ethyl red (o-ER), of a dye molecule potentially applicable for DSSC onto TiO2 particles by second harmonic scattering (SHS). It is found that while at the wavelengths used here o-ER has a much bigger molecular hyperpolarizability, p-ER exhibits strong SHS responses but o-ER gives no detectable SHS when the dyes are added to the TiO2 colloids, respectively. This observation indicates that o-ER does not adsorb onto TiO2, likely due to steric hindrance. Furthermore, we investigate how solvents affect the surface adsorption strength and density of p-ER onto TiO2 in four aprotic solvents with varying polarity. The absolute magnitude of the adsorption free energy was found to increase with the specific solvation energy that represents the ability of accepting electrons and solvent polarity. It is likely that resolvation of the solvent molecules displaced by the adsorption of the dye molecule at the surface in stronger electron-accepting and more polar solvents results in a larger adsorption free energy for the dye adsorption.

Cavity-based aluminum nanohole arrays with tunable infrared resonances

This work details the successful computational design, fabrication, and characterization of a cavity-based aluminum nanohole array. The designs incorporate arrays of aluminum nanoholes that are patterned on a dielectric-coated (SiO2 or ZnSe) aluminum base mirror plane. This architecture provided a means of exploring the coupling of the localized resonances, exhibited by the aluminum nanohole array, with the cavity resonance that is generated within the dielectric spacer layer, which resides between the base plane mirror and the nanohole array. Rigorous coupled wave analysis (RCWA) was first used to computationally design the structures. Next, a range of lithographic techniques, including photolithography, E-beam lithography, and nanosphere lithography, were used to fabricate the structures. Finally, infrared spectroscopy and scanning electron microscopy (SEM) were used to characterize the spectral and structural properties of the multilayered devices, respectively. The overall goal of this study was to demonstrate our ability to design and fabricate aluminum-based structures with tunable resonances throughout the infrared region, i.e. from the short-wave through longwave infrared regions of the electromagnetic spectrum (1.5 -12 µm).

Nanophotonic particle simulation and inverse design using artificial neural networks

New deep learning techniques may hold the key to solving intractable photonics problems. We propose a method to use artificial neural networks to approximate light scattering by multilayer nanoparticles. We find that the network needs to be trained on only a small sampling of the data to approximate the simulation to high precision. Once the neural network is trained, it can simulate such optical processes orders of magnitude faster than conventional simulations. Furthermore, the trained neural network can be used to solve nanophotonic inverse design problems by using back propagation, where the gradient is analytical, not numerical.

Thin-film coating of vibro-fluidized microparticles via R. F. Magnetron sputtering

Recent improvements in microparticle synthesis and handling have prompted new research into the engineering and fabrication of single and multilayered microspheres through traditional physical and chemical vapor depositions. At the University of Delaware, we have developed a custom batch coating process utilizing a vibro-fluidized mixing vessel to deposit thin-films onto the surface of microparticle substrates through R.F. magnetron sputtering. This process opens up a number of design possibilities for single and multilayered microsphere technologies that can be used to improve the optical performance of several optical filtering applications. Through the use of custom design and simulation software, we have optimized a number of filter designs and validated these findings through commercial software. Specifically, we have aimed to improve upon the mass extinction performance seen by traditional materials in the long wave infrared spectrum (LWIR, λ=8-12μm). In order to do this, we have run a series of experiments aimed at creating ultra-lightweight metallic hollow-spheres. Aluminum thin-films have been successfully deposited onto a number of substrates including hollow glass microspheres, high density polyethylene microspheres, and polystyrene foam spheres. By depositing the thin-films onto polymer substrates we have been able to remove the solid core after deposition through a thermal decomposition or chemical dissolution process, in an effort to reduce particle mass and improve mass extinction performance of the filter. A quantum cascade laser measurement system has been used to characterize the optical response of these fabricated aluminum hollow-spheres and have largely agreed with the expected simulated results.