Showing papers by "Jonathan A. Fan published in 2016"

Visible Light Metasurfaces Based on Single-Crystal Silicon

Abstract: Semiconducting nanostructures are promising as components in high-performance metasurfaces. We show that single-crystal silicon can be used to realize efficient metasurface devices across the entire visible spectrum, ranging from 480 to 700 nm. Alternative forms of silicon, such as polycrystalline and amorphous silicon, suffer from higher absorption losses and do not yield efficient metasurfaces across this wavelength range. To demonstrate, we theoretically and experimentally characterize the resonant scattering peaks of individual single-crystal silicon nanoridges. In addition, we design high-efficiency metagratings and lenses based on nanoridge arrays, operating at visible wavelengths, using a stochastic optimization approach. We find that at wavelengths where single-crystal silicon is effectively lossless, devices based on high aspect ratio nanostructures are optimal. These devices possess efficiencies similar to those made of titanium oxide, which is an established material for high-efficiency visible...

Oxygen vacancy promoted methane partial oxidation over iron oxide oxygen carriers in the chemical looping process

Abstract: We perform ab initio DFT+U calculations and experimental studies of the partial oxidation of methane to syngas on iron oxide oxygen carriers to elucidate the role of oxygen vacancies in oxygen carrier reactivity. In particular, we explore the effect of oxygen vacancy concentration on sequential processes of methane dehydrogenation, and oxidation with lattice oxygen. We find that when CH4 adsorbs onto Fe atop sites without neighboring oxygen vacancies, it dehydrogenates with CHx radicals remaining on the same site and evolves into CO2via the complete oxidation pathway. In the presence of oxygen vacancies, on the other hand, the formed methyl (CH3) prefers to migrate onto the vacancy site while the H from CH4 dehydrogenation remains on the original Fe atop site, and evolves into CO via the partial oxidation pathway. The oxygen vacancies created in the oxidation process can be healed by lattice oxygen diffusion from the subsurface to the surface vacancy sites, and it is found that the outward diffusion of lattice oxygen atoms is more favorable than the horizontal diffusion on the same layer. Based on the proposed mechanism and energy profile, we identify the rate-limiting steps of the partial oxidation and complete oxidation pathways. Also, we find that increasing the oxygen vacancy concentration not only lowers the barriers of CH4 dehydrogenation but also the cleavage energy of Fe–C bonds. However, the barrier of the rate-limiting step cannot further decrease when the oxygen vacancy concentration reaches 2.5%. The fundamental insight into the oxygen vacancy effect on CH4 oxidation with iron oxide oxygen carriers can help guide the design and development of more efficient oxygen carriers and CLPO processes.

Methane adsorption and dissociation on iron oxide oxygen carriers: the role of oxygen vacancies

Abstract: We performed ab initio DFT+U calculations to explore the interaction between methane and iron oxide oxygen carriers for chemical looping reaction systems. The adsorption of CH4 and CHx (x = 0–3) radicals on α-Fe2O3(001), and the influence of oxygen vacancies at the top surface and on the subsurface on the adsorption properties of the radicals was investigated. The adsorption strength for CH4 and C radicals at the top of the α-Fe2O3(001) surface in the presence of oxygen vacancies is lower than that on the stoichiometric surface. However, for methyl (CH3), methylene (CH2) and methine (CH) radicals, it is correspondingly higher. In contrast, the oxygen vacancy formation on the subsurface not only increases the adsorption strength of CH3, CH2 and CH radicals, but also facilitates C radical adsorption. We found that oxygen vacancies significantly affect the adsorption configuration of CHx radicals, and determine the probability of finding an adsorbed species in the stoichiometric region and the defective region at the surface. With the obtained adsorption geometries and energetics of these species adsorbed on the surface, we extend the analysis to CH4 dissociation under chemical looping reforming conditions. The distribution of adsorbed CH4 and CHx (x = 0–3) radicals is calculated and analyzed which reveals the relationship between adsorbed CHx radical configuration and oxygen vacancies in iron oxide. Also, the oxygen vacancies can significantly facilitate CH4 activation by lowering the dissociation barriers of CH3, CH2 and CH radicals. However, when the oxygen vacancy concentration reaches 2.67%, increasing the oxygen vacancy concentration cannot continue to lower the CH dissociation barrier. The study provides fundamental insights into the mechanism of CH4 dissociation on iron based oxygen carriers and also provide guidance to design more efficient oxygen carriers.

Epidermal radio frequency electronics for wireless power transfer.

Abstract: Epidermal electronic systems feature physical properties that approximate those of the skin, to enable intimate, long-lived skin interfaces for physiological measurements, human-machine interfaces and other applications that cannot be addressed by wearable hardware that is commercially available today. A primary challenge is power supply; the physical bulk, large mass and high mechanical modulus associated with conventional battery technologies can hinder efforts to achieve epidermal characteristics, and near-field power transfer schemes offer only a limited operating distance. Here we introduce an epidermal, far-field radio frequency (RF) power harvester built using a modularized collection of ultrathin antennas, rectifiers and voltage doublers. These components, separately fabricated and tested, can be integrated together via methods involving soft contact lamination. Systematic studies of the individual components and the overall performance in various dielectric environments highlight the key operational features of these systems and strategies for their optimization. The results suggest robust capabilities for battery-free RF power, with relevance to many emerging epidermal technologies.

Electrochemically Programmable Plasmonic Antennas

Abstract: Plasmonic antennas are building blocks in advanced nano-optical systems due to their ability to tailor optical response based on their geometry. We propose an electrochemical approach to program the optical properties of dipole antennas in a scalable, fast, and energy-efficient manner. These antennas comprise two arms, one serving as an anode and the other a cathode, separated by a solid electrolyte. As a voltage is applied between the antenna arms, a conductive filament either grows or dissolves within the electrolyte, modifying the antenna load. We probe the dynamics of stochastic filament formation and their effects on plasmonic mode programming using a combination of three-dimensional optical and electronic simulations. In particular, we identify device operation regimes in which the charge-transfer plasmon mode can be programmed to be “on” or “off.” We also identify, unexpectedly, a strong correlation between DC filament resistance and charge-transfer plasmon mode frequency that is insensitive to the...

Single metal crystals

Abstract: A single-crystalline metal is created on a substrate by liquefying a metal material contained within a crucible while in contact with a surface of the substrate, cooling the metal material by causing a temperature gradient effected in the substrate in a direction that is neutral along the surface of the substrate and, therein, growing the single-crystalline metal in the crucible.