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At least 163 records · Page 9

The Influence of Nonlocal Metal–Dielectric Environments on Physical and Chemical Processes

Plasmonic nanolayers and laminar metallic/dielectric multilayers were originally developed for optical cloaking applications and lensing applications that could potentially image objects whose size was below the diffraction limit. These assemblies were initially formed from gold or silver nanorods grown within an alumina mesh. However, more recently, assemblies with similar properties have also been prepared by sequential thin-layer deposition of alternating layers of gold and magnesium fluoride (MgF 2 ). These metal/dielectric composite materials enable control of the dielectric constant in the directions perpendicular to the layers and balance the real and imaginary dielectric constants of the assembly such that the speed and the amplitude of the waves traveling through the assembly are not attenuated. In this Account, we will also focus on a few of the applications ranging from surface wetting to fluorescence quenching to enhancement of photochemical reactions. First, we will share an introduction to processes used to create these materials, which are combinations of low refractive index metals and transparent higher index materials arranged in a scalable repeating fashion. Two fabrication methods were employed: an electrochemical deposition of Ag nanorods into an anodized alumina matrix which produced materials with an anisotropic negative refractive index material within the plane of the film and lamellar metal/dielectric layers in which the negative index perpendicular to the growth direction. These alternating layers of plasmonic metals and dielectric materials were ultimately chosen to prepare films for further testing, because of their relative ease of fabrication. We will continue with a discussion of a few of the applications of both of these nonlocal dielectric composite materials including more specialized plasmonic, composite, and hyperbolic metamaterials including fluorescence quenching, photochemical reactions, and surface wetting. In each of these applications, the unique response caused by the enhancement of the electric field and the interface between hyperbolic materials and plasmonic materials as they interact photophysically with their near neighbors is presented. In each of the applications, the enhanced electric field extends from the composite substrate layer to interact with its near neighbors and beyond. Furthermore, the presence of this extended interaction can be observed in the form of decreased emission lifetime, enhancement of photochemical reaction rates, and changes in the surface energies measured by contact angle goniometry. In this Account, all of these situations will be addressed. Finally, we will conclude with a summary and vision for the future as well as a discussion of the unique challenges and opportunities available as research active faculty at an HBCU.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effect of metamaterial engineering on the superconductive properties of ultrathin layers of NbTiN

The electronic transport and optical properties of high quality multilayers of NbTiN/AlN with ultrathin NbTiN layers were characterized. The anisotropy of the dielectric function of the multilayers confirmed their hyperbolic metamaterial properties. Here, the superconductive transition temperature, T c , of these engineered superconductors was enhanced up to 32% compared to the T c of a single ultrathin NbTiN layer while the resistivity per NbTiN layer remained unchanged. We have demonstrated that this T c increase can be attributed to enhanced electron–electron interaction in superconducting hyperbolic metamaterials. The measured critical fields are high and have an anomalous temperature dependence on the direction perpendicular to the magnetic field. These results demonstrate that the metamaterial engineering approach can be used to enhance H c2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Testing Low-Loss Microstrip Materials with MKIDs for Microwave Applications

Future measurements of the millimeter-wavelength sky require a low-loss superconducting microstrip, typically made from niobium and silicon-nitride, coupling the antenna to detectors. Here, we propose a simple device for characterizing these low-loss microstrips at 150 GHz. In our device we illuminate an antenna with a thermal source and compare the measured power at 150 GHz transmitted down microstrips of different lengths. The power measurement is made using Microwave Kinetic Inductance Detectors (MKIDs) fabricated directly onto the microstrip dielectric, and comparing the measured response provides a direct measurement of the microstrip loss. Our proposed structure provides a simple device (4 layers and a DRIE etch) for characterizing the dielectric loss of various microstrip materials and substrates. We present initial results using these devices. We demonstrate that the millimeter wavelength loss of microstrip lines, a few tens of millimeters long, can be measured using a practical aluminum MKID with a black body source at a few tens of Kelvin.

47 OTHER INSTRUMENTATION↗

Modified Dirac Fermions in the Crystalline Xenon and Graphene Moiré Heterostructure

Abstract The interface between two‐dimensional (2D) crystals often forms a Moiré superstructure that imposes a new periodicity, which is a key element in realizing complex electronic phases as evidenced in twisted bilayer graphene. Acombined angle‐resolved photoemission spectroscopy measurements and first‐principles calculations reveal the formation of a Moiré superstructure between a 2D Dirac semi‐metallic crystal, graphene, and a 2D insulating crystal of noble gas, xenon. Incommensurate diffraction pattern and folded Dirac cones around the Brillouin zone center imply the formation of hexagonal crystalline array of xenon atoms. The velocity of Dirac fermions increases upon the formation of the 2D xenon crystal on top of graphene due to the enhanced dielectric screening by the xenon over‐layer. These findings not only provide a novel method to produce a Moiré superstructure from the adsorption of noble gas on 2D materials, but also to control the physical properties of graphene by the formation of a graphene‐noble gas interface.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

2-Aminoanthracene Crystallization in Its Compatible Polystyrene Block: RAFT Synthesis and Enhanced Charge Retention in Pentacene Transistor Gate Dielectrics

We synthesized polystyrene-block-polyanthrylaminomethylstyrene (PS-b-PAAS) via RAFT reaction and side chain modification where the PAAS block is 50%. By blending 2-aminoanthracene (2AA) with PS-b-PAAS, the co-aggregation behavior of the PAAS block and 2AA within the thin film was observed by optical microscopy (OM) and x-ray diffraction. At 5 and 10 wt% of 2AA within the thin film, OM results showed a clear morphological difference between PS matrix and PS-b-PAAS matrix. Differences in the 2AA excited state lifetime in these matrices were also established using transient absorption spectroscopy (TAS). Blends were used as gate dielectrics in pentacene transistors. We compared characteristic voltage (Vc, an indicator of threshold voltage) before and after charging of PS-b-PAAS blended with unsubstituted PS and both polymers individually blended with 2AA. For blended PS-b-PAAS and PS, as the concentration of PS-b-PAAS increases, the decreased Vc especially with negative charging of the pentacene indicated a larger concentration of charge carriers induced by the dielectric film. The charging experiments also revealed that the unique structure formed by the 2AA/PS-b-PAAS blend significantly affected the charge storage capability of the organic field-effect transistors (OFET). Furthermore, this work demonstrates the novel co-aggregation structure in the dielectrics, and furthermore its impact on charge storage capability in pentacene OFETs.

36 MATERIALS SCIENCE↗

Liberating a hidden antiferroelectric phase with interfacial electrostatic engineering

Antiferroelectric materials have seen a resurgence of interest because of proposed applications in a number of energy-efficient technologies. Unfortunately, relatively few families of antiferroelectric materials have been identified, precluding many proposed applications. Here, we propose a design strategy for the construction of antiferroelectric materials using interfacial electrostatic engineering. We begin with a ferroelectric material with one of the highest known bulk polarizations, BiFeO 3 . By confining thin layers of BiFeO 3 in a dielectric matrix, we show that a metastable antiferroelectric structure can be induced. Application of an electric field reversibly switches between this new phase and a ferroelectric state. The use of electrostatic confinement provides an untapped pathway for the design of engineered antiferroelectric materials with large and potentially coupled responses.

42 ENGINEERING↗

Physical Modeling of Coupled Thermohydraulic Behavior of Compacted MX80 Bentonite during Heating

Abstract This paper describes a tank-scale test setup and experimental methodology used to investigate coupled heat transfer and water flow processes during heating of compacted MX80 bentonite to high temperatures. Specifically, a temperature of 200°C was maintained by a cylindrical heating element at the center of a compacted bentonite layer containing an array of temperature, dielectric, and relative humidity sensors. In addition to providing an evaluation of the spatiotemporal variations in temperature, relative humidity, degree of saturation, and global volume, the coupled thermohydraulic properties of the bentonite were assessed. A wetting front was initially observed to move away from the central heater, followed by a drying process until reaching thermohydraulic equilibrium. The soil–water retention curve (SWRC) of the bentonite followed a wetting scanning path before following the primary drying path exhibiting a shift in water retention with elevated temperature. Results from the tank-scale test can be used for validation of numerical simulations of drying processes in the engineered barrier system of a high-level radioactive waste geological disposal repository and confirm that a temperature-dependent hysteretic SWRC with scanning paths is required to accurately capture the bentonite response.

Engineering↗

Analysis of RF Surface Loss in a Planar 2D Qubit

The Josephson junction and shunt capacitor form a transmon qubit, which is the cornerstone of modern quantum computing platforms. For reliable quantum computing, it is important how long a qubit can remain in a superposition of quantum states, which is determined by the coherence time (T1). The coherence time of a qubit effectively sets the "lifetime" of usable quantum information, determining how long quantum computations can be performed before errors occur and information is lost. There are several sources of decoherence in transmon qubits, but the predominant one is generally considered to be dielectric losses in the natural oxide layer formed on the surface of the superconductor. In this paper, we present a numerical study of microwave surface losses in planar superconducting antennas of different transmon qubit designs. An asymptotic method for estimating the energy participation ratio in ultrathin films of nanometer scales is proposed, and estimates are given for the limits of achievable minimum RF losses depending on the electrical properties of the surface oxide and the interface of the qubit with the substrate material.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Controlled Dielectric Breakdown to Form Pinhole Passivated Contacts

This contribution explores a low-temperature route to forming dielectric pinholes to form poly-Si/dielectric/c-Si passivated contacts. The method utilizes controlled dielectric breakdown to form nanoscale pinholes in a thick (non-tunnelling) dielectric which, when annealed, allows dopant atoms to pass from doped poly-Si through the dielectric and into the c-Si wafer forming conductive pathways. We show that the pinholes can be repassivated with dopants and H diffusion which results in increased PL signals after processing. The method can be expanded to optimized dielectric passivation stacks (not just a single layer) and can be formed in parallel over the faces of the wafer in selected areas (only under the grid).

controlled dielectric breakdown↗

Control of work functions of nanophotonic components

Work function is an essential material’s property playing important roles in electronics, photovoltaics, and more recently, in nanophotonics. We have studied effects of organic, and inorganic dielectric materials on work functions of Au films in single layered, and multilayered structures. We found that measured work function of metallic surfaces can be affected by dielectric materials situated 10–100 nm away from the metallic surface. We have found that, (i) the glass underneath ~ 50 nm gold slab reduces the work function of gold, (ii) Rh590:PMMA increases the work function of a gold film deposited on top of the polymer, and (iii) reduces it if Rh590:PMMA is deposited on top of Au. (iv) With increase of the Rh590 concentration in PMMA, n, the work function first decreases (at n < 64 g/l), and then increases (at n > 64 g/l). (v) The work function of a Fabry–Perot cavity or an MIM waveguide is almost the same as that of single Au films of comparable thickness. The experimental results can be qualitatively explained in terms of a simple model taking into account adhesion of charged molecules to a metallic surface, and formation of a double layer of charges accelerating or decelerating electrons exiting the metal and decreasing or increasing the work function.

36 MATERIALS SCIENCE↗

Controlled Dielectric Breakdown to Form Pinhole Passivating Contacts

This contribution explores an alternate route to forming pinhole-based poly-Si/dielectric/c-Si passivating contacts. The method utilizes controlled dielectric breakdown or electroforming to produce nanoscale pinholes in a thick (non-tunnelling) dielectric which, when annealed, allows dopant atoms to pass from doped poly-Si through the pinholes and into the c-Si wafer, forming conductive pathways. We show that the pinholes lose passivation after electroforming but can be repassivated with a forming gas anneal. N-type contacts show contact resistivities of ~20 mOhm-cm2, but p-type contacts are ~100 mOhm-cm2. Devices show a distinct kink in the J-V curve indicative of a barrier to transport. The method can be expanded to optimized dielectric passivation stacks (not just thin, single layers) and can be formed in parallel over the faces of the wafer in selected areas (pinholes only under the grid lines).

CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SU↗

Thermodynamic Theory of Proximity Ferroelectricity

Proximity ferroelectricity has recently been reported as a new design paradigm for inducing ferroelectricity, where a nonferroelectric polar material becomes a ferroelectric one by interfacing with a thin ferroelectric layer. Strongly polar materials, such as AlN and ZnO, which were previously unswitchable with an external field below their dielectric breakdown fields, can now be switched with practical coercive fields when they are in intimate proximity to a switchable ferroelectric. Here, we develop a general Landau-Ginzburg theory of proximity ferroelectricity in multilayers of nonferroelectrics and ferroelectrics to analyze their switchability and coercive fields. The theory predicts regimes of both “proximity switching,” where the multilayers collectively switch, and “proximity suppression,” where they collectively do not switch. The mechanism of the proximity ferroelectricity is an internal electric field determined by the polarization of the layers and their relative thickness in a self-consistent manner that renormalizes the double-well ferroelectric potential to lower the steepness of the switching barrier. Further reduction in the coercive field emerges from charged defects in the bulk that act as nucleation centers. The application of the theory to proximity ferroelectricity in Al x−1⁢ Sc x ⁢N/AlN and Zn 1−x ⁢Mg x ⁢O/ZnO bilayers is demonstrated. The theory further predicts that dielectric-ferroelectric and paraelectric-ferroelectric multilayers can potentially lead to induced ferroelectricity in the dielectric or paraelectric layers, resulting in the entire stack being switched, an exciting avenue for new discoveries. This thawing of “frozen ferroelectrics,” paraelectrics, and potentially dielectrics with high dielectric constants promises a large class of new ferroelectrics with exciting prospects for previously unrealizable domain-patterned optoelectronic and memory technologies.

36 MATERIALS SCIENCE↗

A High-Frequency Planar Transformer with Medium-Voltage Isolation

This paper presents the design of a low-loss, high-frequency planar transformer having medium-voltage (10’s of kV) isolation capability while transformer primary and secondary windings are interleaved to reduce losses. Medium-voltage isolation between adjacent printed circuit board (PCB) layers is extremely challenging using traditional PCB dielectrics. The isolation requirement is met using PCB with 7 kV/mil polyimide (Panasonic Felios RF775) as the dielectric, and by an appropriate layout of the windings and the inter-winding vias. The transformer is used to implement a dual active bridge (DAB) converter in a stackable dc-ac architecture where the dc port is connected to a photovoltaic (PV) string and ac outputs are connected in series to achieve direct PV string-to-medium voltage conversion without the need for low-voltage collection or a bulky line frequency transformer. Since each DAB transformer processes time-varying power, a design methodology is developed to minimize line-cycle-averaged losses. Experimental results are presented for a 1:1 planar transformer in a 7.5 kW SiC-based dc-to-ac module operating at 200 kHz. Isolation of 26 kV between the primary and secondary layers and between the windings and the core is verified using a hipot tester.

insulation resistance↗

A High-Frequency Planar Transformer with Medium-Voltage Isolation: Preprint

This paper presents the design of a low-loss, high-frequency planar transformer having medium-voltage (10's of kV) isolation capability while transformer primary and secondary windings are interleaved to reduce losses. Medium-voltage isolation between adjacent printed circuit board (PCB) layers is extremely challenging using traditional PCB dielectrics. The isolation requirement is met using PCB with $7$\,kV/mil polyimide (Panasonic Felios RF775) as the dielectric, and by an appropriate layout of the windings and the inter-winding vias. The transformer is used to implement a dual active bridge (DAB) converter in a stackable dc-ac architecture where the dc port is connected to a photovoltaic (PV) string and ac outputs are connected in series to achieve direct PV string-to-medium voltage conversion without the need for low-voltage collection or a bulky line frequency transformer. Since each DAB transformer processes time-varying power, a design methodology is developed to minimize line-cycle-averaged losses. Experimental results are presented for a 1:1 planar transformer in a 7.5\,kW SiC-based dc-to-ac module operating at 200 kHz. Isolation of 26 kV between the primary and secondary layers and between the windings and the core is verified using a hipot tester.

41 EE - Solar Energy Technologies Office (EE-4S)↗

Possible Realization of Hyperbolic Plasmons in Few-Layered Rhenium Disulfide

Hyperbolic plasmons are a highly desired property in optoelectronics and biomolecular sensing. The necessary condition to realize hyperbolic plasmons is a significant anisotropy of the principal components of the dielectric function, such that at a certain frequency range, one component is negative and the other is positive, i.e., one component is metallic, and the other one is dielectric. Here, we study the effect of anisotropy in ReS 2 , and our theory shows that ReS 2 can host hyperbolic plasmons in the ultraviolet frequency range. The operating frequency range of the hyperbolic plasmons can be tuned with the number of ReS 2 layers. However, we note that the significantly large imaginary part of the macroscopic dielectric response in all layered variants of ReS 2 can result in substantial losses for the hyperbolic plasmons, as in the case with other known hyperbolic materials, with the exception of MoOCl 2 . We also note that ReS 2 hosts ultraviolet hyperbolic plasmons while ZrSiSe, WTe 2 , and CuS nanocrystals host infrared plasmons, providing a novel platform for optoelectronics in the ultraviolet range.

36 MATERIALS SCIENCE↗

Voltage‐Modulated Untwist Deformations and Multispectral Optical Effects from Ion Intercalation into Chiral Ceramic Nanoparticles

Abstract Reconfiguration of chiral ceramic nanostructures after ion intercalation should favor specific nanoscale twists leading to strong chiroptical effects. In this work, V 2 O 3 nanoparticles are shown to have “built‐in” chiral distortions caused by binding of tartaric acid enantiomers to the nanoparticle surface. As evidenced by spectroscopy/microscopy techniques and calculations of nanoscale chirality measures, the intercalation of Zn 2+ ions into the V 2 O 3 lattice results in particle expansion, untwist deformations, and chirality reduction. Coherent deformations in the particle ensemble manifest as changes in sign and positions of circular polarization bands at ultraviolet, visible, mid‐infrared (IR), near‐IR (NIR), and IR wavelengths. The g‐ factors observed for IR and NIR spectral diapasons are ≈100–400 times higher than those for previously reported dielectric, semiconductor, and plasmonic nanoparticles. Nanocomposite films layer‐by‐layer assembled (LBL) from V 2 O 3 nanoparticles reveal cyclic‐voltage‐driven modulation of optical activity. Device prototypes for IR and NIR range problematic for liquid crystals and other organic materials are demonstrated. High optical activity, synthetic simplicity, sustainable processability, and environmental robustness of the chiral LBL nanocomposites provide a versatile platform for photonic devices. Similar reconfigurations of particle shapes are expected for multiple chiral ceramic nanostructures, leading to unique optical, electrical, and magnetic properties.

36 MATERIALS SCIENCE↗

Impact of external screening on the valence and core level photoelectron spectra of monolayer W⁢S 2

Transition metal dichalcogenides (TMDs) represent an emerging class of layered materials with applications in microelectronics, optoelectronics, photonics, and catalysis. The confinement of charge carriers within the highly anisotropic, quasi-two-dimensional geometry of one-layer (1L) TMDs leads to reduced, variable dielectric screening, giving rise to a quasiparticle band gap that is highly susceptible to the surrounding dielectric environment. Here, exploiting the contrasting external dielectric environments of gold-supported and suspended 1L W⁢S 2 , we show how the electronic states of W⁢S 2 under the effective and ineffective screening environments align at a junction made within the same sheet of material. Photoelectron spectra point to the close alignment of the charge neutrality levels of W⁢S 2 in both environments, and the breakdown of rigid shifts between the valence states and core levels with the core levels shifting more than twice as much as the valence states. Furthermore, the effectively screened W⁢S 2 exhibits a valence state with the photoemission linewidth twice as large as the ineffectively screened suspended W⁢S 2 , presumably originated from the locally varying W⁢S 2 -Au distance and substrate disorders. Collectively, these findings provide key insights into the electronic behavior of W⁢S 2 and its photoemission process with the electronic states renormalized according to the external screening environments.

Dielectric properties↗