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At least 1,117 records · Page 62

Voltage-Controlled Differential Faraday Rotation from FMNWs and Magnetoelastic Silicone-Nickel Composites

Differential Faraday rotation has been observed from strain-Differential Faraday rotation has been observed from strain-modulated magnetoelastic membranes using millimeter-wave polarimetry at 61.25 GHz. The membranes, consisting of aligned chains of nickel micro-particles embedded in silicone rubber, were manufactured using a roll-to-roll electromagnetic processing line, mounted onto piezoelectric ceramic annuli, and immersed in externally-generated static magnetic fields. Experiments were conducted in which the membranes were periodically stretched by operating the piezoelectric crystals close to their radial resonant frequencies—thereby modulating nickel particle density as well as magnetic material properties. A customized quasi-optical apparatus was used to determine the Faraday-rotation difference between the strained and unstrained states of the magnetoelastic membranes. Possible applications that could emerge from this polymer-based technology include nonreciprocal millimeter-wave components with voltage-controlled frequency response and bio-inspired geomagnetic sensors for GPS-denied navigation. Investigations were conducted to estimate the maximum attainable differential Faraday rotation and the minimum detectable static magnetic field.

nickel↗

Spatially Resolved Near Field Spectroscopy of Vibrational Polaritons at the Small N Limit

Vibrational polaritons, which have been primarily studied in Fabry–Pérot cavities with a large number of molecules (N ~ 10 6 –10 10 ) coupled to the resonator mode, exhibit various experimentally observed effects on chemical reactions. However, the exact mechanism is elusively understood from the theoretical side, as the large number of molecules involved in an experimental strong coupling condition cannot be represented completely in simulations. This discrepancy between theory and experiment arises from computational descriptions of polariton systems typically being limited to only a few molecules, thus failing to represent the experimental conditions adequately. To address this mismatch, we used surface phonon polariton (SPhP) resonators as an alternative platform for vibrational strong coupling. SPhPs exhibit strong electromagnetic confinement on the surface and thus allow for coupling to a small number of molecules. As a result, this platform can enhance nonlinearity and slow down relaxation to the dark modes. In this study, we fabricated a pillar-shaped quartz resonator and then coated it with a thin layer of cobalt phthalocyanine (CoPc). By employing scattering-type scanning near-field optical microscopy (s-SNOM), we spatially investigated the dependency of vibrational strong coupling on the spatially varying electromagnetic field strength and demonstrated strong coupling with 38,000 molecules only–reaching to the small N limit. Through s-SNOM analysis, we found that strong coupling was observed primarily on the edge of the quartz pillar and the apex of the s-SNOM tip, where the maximum field enhancement occurs. In contrast, a weak resonance signal and lack of coupling were observed closer to the center of the pillar. This work demonstrates the importance of spatially resolved polariton systems in nanophotonic platforms and lays a foundation to explore polariton chemistry and chemical dynamics at the small N limit–one step closer to reconcile with high-level quantum calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Optical activation and detection of charge transport between individual colour centres in diamond

Understanding the capture of charge carriers by colour centres in semiconductors is important for the development of novel forms of sensing and quantum information processing, but experiments typically involve ensemble measurements, often impacted by defect proximity. In this study, we show that confocal fluorescence microscopy and magnetic resonance can be used to induce and probe charge transport between individual nitrogen-vacancy centres in diamond at room temperature. In our experiments, a ‘source’ nitrogen vacancy undergoes optically driven cycles of ionization and recombination to produce a stream of photogenerated carriers, one of which is subsequently captured by a ‘target’ nitrogen vacancy several micrometres away. We use a spin-to-charge conversion scheme to encode the spin state of the source colour centre into the charge state of the target, which allows us to set an upper bound to carrier injection from other background defects. We attribute our observations to the action of unscreened Coulomb potentials producing giant carrier capture cross-sections, orders of magnitude greater than those measured in ensembles.

36 MATERIALS SCIENCE↗

Mini-cavity-dumped laser

Lasers for use in high precision satellite ranging systems consist typically of an oscillator followed by several amplifier stages. While the shortest optical pulses are achieved by using a mode locked oscillator, such an oscillator is incompatible with the compact design needed in future, highly mobile systems. The laser oscillator achieves pulse lengths approaching those obtainable by mode locking, but in a much more compact and stable design. The oscillator uses two LiNbO3 Pockels cells inside the resonator. One Q-switches the oscillator, and the other is used in a pulse slicing scheme to cavity dump a portion of the circulating optical energy. The length of the optical output pulse measured at 425 + or - 50 picoseconds.

Reed, E.↗

High-bandwidth CMOS-voltage-level electro-optic modulation of 780 nm light in thin-film lithium niobate

Integrated photonics operating at visible-near-infrared (VNIR) wavelengths offer scalable platforms for advancing optical systems for addressing atomic clocks, sensors, and quantum computers. The complexity of free-space control optics causes limited addressability of atoms and ions, and this remains an impediment on scalability and cost. Networks of Mach-Zehnder interferometers can overcome challenges in addressing atoms by providing high-bandwidth electro-optic control of multiple output beams. Here, we demonstrate a VNIR Mach-Zehnder interferometer on lithium niobate on sapphire with a CMOS voltage-level compatible full-swing voltage of 4.2 V and an electro-optic bandwidth of 2.7 GHz occupying only 0.35 mm 2 . Our waveguides exhibit 1.6 dB/cm propagation loss and our microring resonators have intrinsic quality factors of 4.4 × 10 5 . This specialized platform for VNIR integrated photonics can open new avenues for addressing large arrays of qubits with high precision and negligible cross-talk.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Orbitally selective resonant photodoping to enhance superconductivity

Signatures of superconductivity at elevated temperatures above T c in high-temperature superconductors have been observed near 1/8 hole doping for photoexcitation with infrared or optical light polarized either in the CuO 2 plane or along the c axis. While the use of in-plane polarization has been effective for incident energies aligned to specific phonons, c-axis laser excitation in a broad range between 5 μm and 400 nm was found to affect the superconducting dynamics in striped La 1.88 5Ba 0.115 CuO 4 , with a maximum enhancement in the 1/ω dependence to the conductivity observed at 800 nm. This broad energy range, specifically 800 nm, is not resonant with any phonon modes, yet induced electronic excitations appear to be connected to superconductivity at energy scales well above the typical gap energies in the cuprates. A critical question is, What can be responsible for such an effect at 800 nm? Using time-dependent exact diagonalization, we demonstrate that the holes in the CuO 2 plane can be photoexcited into the charge reservoir layers at resonant wavelengths within a multiband Hubbard model. This orbitally selective photoinduced charge transfer effectively changes the in-plane doping level, which can lead to an enhancement of T c near the 1/8 anomaly.

36 MATERIALS SCIENCE↗

Quantum Dot–Organic Molecule Conjugates as Hosts for Photogenerated Spin Qubit Pairs

The inherent spin polarization present in photogenerated spin-correlated radical pairs makes them promising candidates for quantum computing and quantum sensing applications. The spin states of these systems can be probed and manipulated with microwave pulses using electron paramagnetic resonance spectrometers. However, to date, there are no reports on magnetic resonance-based spin measurements of photogenerated spin-correlated radical pairs hosted on quantum dots. In the current work, we prepare dye molecule-inorganic quantum dot conjugates and show that they can produce photogenerated spin-polarized states. The dye molecule, D131, is chosen for its ability to undergo efficient charge separation, and the nanoparticle materials, ZnO quantum dots, are chosen for their promising spin properties. Transient and steady state optical spectroscopy performed on ZnO quantum dot-D131 conjugates shows that reversible photogenerated charge separation is occurring. Transient and pulsed electron paramagnetic resonance experiments are then performed on the photogenerated radical pair, which demonstrate that (1) the radical pair is polarized at moderate temperatures and well modeled by existing theories and (2) the spin states can be accessed and manipulated with microwave pulses. In conclusion, this work opens the door to a new class of promising qubit materials that can be photogenerated in polarized states and hosted by highly tailorable inorganic nanoparticles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Acoustic ground impedance meter

A method and apparatus are presented for measuring the acoustic impedance of a surface in which the surface is used to enclose one end of the chamber of a Helmholz resonator. Acoustic waves are generated in the neck of the resonator by a piston driven by a variable speed motor through a cam assembly. The acoustic waves are measured in the chamber and the frequency of the generated acoustic waves is measured by an optical device. These measurements are used to compute the compliance and conductance of the chamber and surface combined. The same procedure is followed with a calibration plate having infinite acoustic impedance enclosing the chamber of the resonator to compute the compliance and conductance of the chamber alone. Then by subtracting, the compliance and conductance for the surface is obtained.

Zuckerwar, A. J.↗

Optically detected NMR in a diamond-anvil cell for geochemistry

Developments in quantum-information processing are being adapted to perform nuclear-magnetic resonance (NMR) measurements on solutions in very small volumes. Here we describe efforts to adapt the technology to a diamond-anvil cell (DAC), with the goal of conducting solution NMR measurements at elevated pressures and temperatures. At the center of the method is the use of diamonds that have a particular type of defect that pairs a nitrogen atom substitution for near-surface carbon with a vacancy. These NV sites have unpaired electrons that can be excited while conserving electron spins and the amount of light released upon decay of the excited state depends upon the orientation of the electron spin. Under certain conditions the NV centers can probe AC magnetic fields from nearby nuclei with exquisite sensitivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Anisotropic ultrahigh gain emission observed in rotational transitions in optically pumped HF gas.

Gain and laser oscillations are obtained on rotational transitions of the first excited vibrational state of HF gas at room temperature, resonantly pumped by the 2.7-micron lines of a pulsed HF laser. Pumping the P-branch transitions connecting the ground and first excited vibrational states produces gain at the coupled rotational transitions at 36, 42, 51, 63, 84, and 126 microns. The gain exhibits directional properties characteristic of a unidirectional amplifier predicted by a recent theory. The incremental gains of these lines are very large, in excess of 1/cm, and the lines oscillate easily without mirrors (superradiance).

Skribanowitz, N.↗

Resonance Scattering of Fe XVII X-Ray and EUV Lines

Over the years a number of calculations have been carried out to derive intensities of various X-ray and EUV lines in Fe XVII to compare with observed spectra. The predicted intensities have not agreed with solar observations, particularly for the line at 15.02 Angstroms; resonance scattering has been suggested as the source for much of the disagreement. The atomic data calculated earlier used seven configurations, 2s(sup 2) 2p(sup 6),2s(sup 2) 2p(sup 5)3s, 2s(sup 2) 2p(sup 5)3p, 2s(sup 2)2p(sup 5)3d, 2s2 p(sup 6)3s, 2s2p(sup 6)3p, and 2s2p(sup 6)3d, having n=3 orbitals and the scattering calculations in the distorted wave approximation were carried out only for incident energies above the threshold of the highest fine-structure level. These calculations have now been extended to thirteen configurations by adding six more configurations having n=4 orbitals, namely 2s(sup 2) 2p(sup 5)4s, 2s(sup 2) 2p(sup 5)4p, 2s(sup 2) 2p(sup 5)4d, 2s2p(sup 6)4s, 2s2p(sup 6)4p, and 2s2p(sup 6)4d, giving rise to 73 fine structure levels. The scattering calculations are carried out below as well as above the threshold of the highest fine-structure level. The incident energies below the threshold are 55.8, 65, 70, and 76 Ry and those above are 85, 127.5, 170, 212.5, 255, 340, and 425 Ry. The collision strengths are calculated up to total angular momentum L(sup T) = 33. Level populations and intensity ratios are calculated at various electron temperatures and densities. It is not possible to predict how the ratios would change when configurations with n=5 and 6 orbitals are added but some estimates have been made for a few transitions by Liedhal, who indicates an asymptotic convergence when n=5 and 6 orbitals are added. These improved calculations of Fe XVII change the intensity ratios compared to those obtained earlier, bringing the optically thin F(15.02)/F(16.78) ratio and several other ratios closer to the observed values: However, some disagreement with the solar observations still persists, even though the agreement of the presently calculated optically thin F(15.02)/F(15.26) ratio with the experimental results of Brown et al. and Laming et al. has improved. Some of the remaining discrepancy is still thought to be the effect of opacity, which is consistent with expected physical conditions for solar sources. EUV intensity ratios are also calculated and compared with observations. Level populations and intensity ratios are calculated, as a function of column density of Fe XVII, in the slab and cylindrical geometries. As found previously, the predicted intensities for the resonance lines at 15.02 and 15.26 Angstroms exhibit initial increases in flux relative to the forbidden line at 17.10 Angstroms and the resonance line at 16.78 Angstroms as optical thickness increases. The same behavior is predicted for the lines at 12.262 and 12.122 Angstroms. Predicted intensities for some of the allowed EUV lines are also affected by opacity.

Bhatia, A. K.↗

Density Functional Tight Binding Insights into Plasmonic Silver–Platinum Nanoparticles and Alloys for Enhanced Photocatalysis

Developing accurate and efficient Slater-Koster (SK) tight-binding parameter sets is essential for quantum plasmonic studies of alloyed metal nanoparticles, as conventional time dependent density functional theory (TD-DFT) calculations are computationally prohibitive for larger clusters. In this work, we develop and validate density functional tight binding (DFTB) parameter sets for both ground state (GS-SK) and excited state (ES-SK) calculations to study the structural, electronic, and optical properties of silver (Ag), platinum (Pt), and Ag–Pt nanoalloys. Our investigation of the ground state properties demonstrates that the GS-SK parameters enable DFTB to closely reproduce the electronic structures of platinum clusters with diverse sizes and geometries – showing qualitative agreement with DFT for density of states (DOS) profiles and energy levels. The ES-SK parameters accurately describe excited-state properties compared to TD-DFT reference calculations, including the broad, featureless absorption profiles of Pt that are dominated by interband transitions. Using the ES-SK parameters within a real-time TD-DFTB framework, we compute size-dependent optical absorption spectra of Ag, Pt and Ag-Pt nanocubes containing up to 1099 atoms (size ∼4.18 nm). A detailed study of Ag–Pt and Pt-Ag core–shell nanoparticles shows quenching of the Ag plasmon resonance even at monolayer coverage for Ag-Pt, but not for Pt-Ag. We also show how to define submonolayer Ag-core Pt-shell cubic structures that have similar optical properties to those generated experimentally for much larger particles, which offers potential for describing plasmon-enhanced photocatalysis. Collectively, the GS-SK and ES-SK parameter sets provide an accurate, computationally efficient approach for modeling the complex optical and electronic behavior of noble–transition metal nanostructures and their alloys.

SPR↗

Coupling buried etalon layers to an engraved metasurface for durable and large-aperture meta-optics

Many optical applications that could potentially benefit from the design flexibility provided by the metasurface approach are being prohibited by the limited scalability of the fabrication and the robustness of the end-result structures when using a resonant meta-elements-based approach. In this study, an alternative demonstrated approach with superior scalability and robustness is substrate-engraved metasurfaces, based on medium mixing homogenization, yet it suffers from very limited optical response. Here we propose advancing this approach by coupling the metasurface with buried etalon layers, leading to enhancement in the optical response. A transfer matrix analysis is used to study the parameter space, predicting that the patterned reflectance values range of a beam shaper could be raised from only 4% to 30% when the metasurface is engraved in silica, and even up to 66% when engraved into higher-index oxides. Using the method proposed here, the phase difference range across the metasurface could be increased by 0.4 radians beyond the range achievable by a metasurface engraved in silica and could reach even higher values when embedded in higher-index materials. Full-wave numerical simulations are used to demonstrate a cylindrical metareflector and a metalens, further validating the analysis.

47 OTHER INSTRUMENTATION↗

Coupling of electronic transition to ferroelectric order in a 2D semiconductor

A ferroelectric material often exhibits a soft transverse optical (TO) phonon mode which governs its phase transition. Charge coupling to this ferroelectric soft mode may further mediate emergent physical properties, including superconductivity and defect tolerance in semiconductors. However, direct experimental evidence for such coupling is scarce. Here we show that a photogenerated coherent phonon couples strongly to the electronic transition above the bandgap in the van der Waals (vdW) two-dimensional (2D) ferroelectric semiconductor NbOI 2 . Using terahertz time-domain spectroscopy and first-principles calculations, we identify this mode as the TO phonon responsible for ferroelectric order. This exclusive coupling occurs only with the above-gap electronic transition and is absent in the valence band as revealed by resonant inelastic X-ray scattering. Our findings suggest a new role of the soft TO phonon mode in electronic and optical properties of ferroelectric semiconductors.

36 MATERIALS SCIENCE↗

Co-templating of polyoxoniobates and silicate/germanate trimer-rings in crystals and inorganic gels

Polyoxometalate (POM) supramolecular gels are a growing family of materials, both for understanding fundamental self-assembly and fabricating flexible monolithic materials that retain the function of metal oxides. Here, we exploited the pH-dependent speciation of polyoxoniobates (PONbs), targeting the formation of PONb-containing supramolecular gels that contain other low molecular weight components (silicate, germanate, phosphate, and carbonate). The introduction of gaseous CO 2 into aqueous hexaniobate solutions resulted in the formation of both new crystalline phases and highly transparent gels. The crystalline phases, formulated Cs 24 [Nb 7 O 22 (NbO(CO 3 ) 2 ) 9 (Si 3 O 9 )]·19.6H 2 O and Cs 21 Na 3 [Nb 7 O 22 (NbO(CO 3 ) 2 ) 9 (Ge 3 O 9 )]·33.6H 2 O are templated by a rare planar [X 3 O 9 ] 6− (X = Si, Ge) ring. Crystalline phases were not obtained with phosphate; instead, the gels contain a mixture of phosphate-centred PONbs and network-forming phosphate. POM speciation within the gels, physical properties, and assembly mechanisms were benchmarked by solution and solid-state nuclear magnetic resonance (NMR) spectroscopy, vibrational spectroscopies, small-angle X-ray scattering (SAXS), and thermogravimetry-mass spectroscopy. Optical analysis and dielectric behavior of the gels confirmed that they are highly transparent ionic and electronic conductors. The alkali and hydroxide concentration controls the formation of crystalline materials or supramolecular gels while maintaining the same network building blocks, providing a rare opportunity to describe the molecular-level structure of inorganic amorphous materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

ZnO-Au x Cu 1-x Alloy and ZnO-Au x Al 1-x Alloy Vertically Aligned Nanocomposites for Low-Loss Plasmonic Metamaterials

Hyperbolic metamaterials are a class of materials exhibiting anisotropic dielectric function owing to the morphology of the nanostructures. In these structures, one direction behaves as a metal, and the orthogonal direction behaves as a dielectric material. Applications include subdiffraction imaging and hyperlenses. However, key limiting factors include energy losses of noble metals and challenging fabrication methods. In this work, self-assembled plasmonic metamaterials consisting of anisotropic nanoalloy pillars embedded into the ZnO matrix are developed using a seed-layer approach. Alloys of Au x Al 1-x or Au x Cu 1-x are explored due to their lower losses and higher stability. Optical and microstructural properties were explored. The ZnO-Au x Cu 1-x system demonstrated excellent epitaxial quality and optical properties compared with the ZnO-Au x Al 1-x system. Both nanocomposite systems demonstrate plasmonic resonance, hyperbolic dispersion, low losses, and epsilon-near-zero permittivity, making them promising candidates towards direct photonic integration.

36 MATERIALS SCIENCE↗

A feasibility study of a microwave water vapor measurement from a space probe along an occultation path

Stratospheric and mesospheric water vapor measurements were taken using the microwave lines at 22 GHz (22.235 GHz) and 183 GHz (183.31 GHz). The resonant cross sections for both the 22 GHz and the 183 GHz lines were used to model the optical depth of atmospheric water vapor. The range of optical depths seen by a microwave radiometer through the earth's limb was determined from radiative transfer theory. Radiometer sensitivity, derived from signal theory, was compared with calculated optical depths to determine the maximum height to which water vapor can be measured using the following methods: passive emission, passive absorption, and active absorption. It was concluded that measurements using the 22 GHz line are limited to about 50 km whereas the 183 GHz line enables measurements up to and above 100 km for water vapor mixing ratios as low as 0.1 ppm under optimum conditions.

Longbothum, R. L.↗