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At least 1,711 records · Page 95

New Photocathode materials for electron-ion-colliders

Our aim has been to explore new photocathode materials and schemes to develop strategies and technologies for next generation nuclear physics accelerator capabilities, particularly for Electron Ion Colliders (EIC). Thus, we investigated thin film deposition and ensuing properties for several adequate magnetic materials applicable to spin-polarized photocathodes. We also implemented a full experimental setup for light incidence at an acute angle onto the photocathode surface in order to excite surface Plasmon resonance hence increasing light absorption by a metallic surface. We successfully tested the setup with a thermionic cathode as well as Plasmonic silver-MgO samples and obtained very encouraging results. Our first results are very encouraging since the photocurrent measured on this preliminary plasmonic Ag-MgO sample under low power (~ 1mW) cw red light from a HeNe laser was 256 pA, thus two orders magnitude larger than that reported by others following also plasmonic approaches. We extended our studies to shorter wavelengths and we also started preliminary work on chemically ordered MnAl thin films –a component of the tertiary Ag-Mn-Al (silmanal) alloy in order to develop spin-polarized photocathodes capable of sustaining surface Plasmon resonance. It is worthwhile mentioning that a graduate student has been directly involved during this project ensuring the training of next generation of scientists in this area of research.

43 PARTICLE ACCELERATORS↗

Final Scientific/Technical Report for Program Title: Solar Powered Dewvaporation Desalination System

Desalination technologies have been used increasingly throughout the world to produce the drinking water from the brackish ground and sea water for the past few decades. Among the commercially available desalination technologies, reverse osmosis (RO) and multi-stage flash distillation are the most widely used technologies globally. However, these technologies are difficult to be directly integrated with green energies without converting them to electricity. Dewvaporation, a desalination process, uses saturated steam as a carrier-gas to evaporate water from saline feeds and form pure condensate. It has the major technical benefit of reusing energy, released from vapor condensation, multiple times. The current proposal has been planned to address this issue. In Phase I, we have successfully demonstrated the feasibility of a new plasmonic nanoparticle based approach through fabrication and evaluation of a solar powered water vapor generation module. The water vapor generation module allows generation of high temperature plasmon on a fiber bundle end, where strong water and plasmon interaction occurs generating water vapor. Plasmon enhanced water evaporation has been realized on plasmonic nanoparticle immobilized substrate with an energy conversion efficiency of over 50%.

14 SOLAR ENERGY↗

Engineering Symmetry-Breaking Nanocrescent Arrays for Nanolasing

This paper describes a symmetry-breaking plasmonic lattice structure that can support narrow resonances as optical feedback for nanolasing. A scalable technique is developed to fabricate nanocrescent arrays with low-structural symmetry unit cells to achieve in-plane quadrupolar lattice plasmon modes. These lattice plasmons with extremely narrow linewidths preserve nonzero net dipole moments under normal excitation. Ultrafast band-edge lasing can be switched on and off by changing the polarization of the incident pump light. In conclusion, the quadrupolar lattice plasmon lasing process is simulated with a semi-quantum model and the sharp tips on the nanocrescents accelerate the lasing buildup process and enhance stimulated emission.

36 MATERIALS SCIENCE↗

Efficient Modeling of Structural, Electronic, and Optical Properties of Silver and Gold Metal Nanoclusters and Alloys Using Optimized SCC-DFTB Parameters

Computation of optical properties using conventional time-dependent density functional theory (TD-DFT) is time-consuming and memory-intensive. In this study, we investigate the accuracy and efficiency of the density functional tight binding (DFTB) framework with newly optimized Slater–Koster (SK) parameters for modeling the structural, electronic properties, and absorption spectra of silver and gold nanoclusters and their alloys. Our investigation of the ground state (GS) properties demonstrates that the newly developed GS-SK parameters enable DFTB to closely approximate DFT-calculated bond lengths for octahedron, tetrahedron, icosahedra, and truncated octahedron with sizes Ag n /Au n (n = 19, 20, 38, 55), nanoclusters and Ag 20 /Au 20 nanoalloys, with a maximum deviation of approximately 0.15 Å. Formation energy results indicate that the GS-SK parameters can closely estimate changes in formation energies with alloy composition, and the comparison of electronic structures for Ag 20 , Au 20 , and AgAu alloy nanoclusters using the DFTB approximation reveals good agreement in the projected density of states (DOS) profiles and energy levels. A second set of SK parameters, ES-SK, has been developed to describe excited state (ES) properties, including the absorption spectra of silver octahedron Ag 19 , tetrahedral Ag n (n = 20, 56, 84), truncated octahedron Ag 38 , and icosahedra Ag 55 closed-shell clusters and their gold and alloy counterparts over a broad range of alloy compositions. This parametrization uses TD-DFTB calculations and fine-tunes the d and p eigenvalues by comparing them to reference absorption spectra from first-principles TD-DFT. This enables the generation of absorption spectra that closely match the reference spectra when plasmon excitation is dominant, as demonstrated by studying the plasmonic properties of icosahedral Ag n and Au n (n = 309 and 561) nanoparticles. This includes the rapid loss in plasmon quality when Au partially replaces Ag in alloy clusters. Furthermore, these results provide a foundation for addressing computational bottlenecks in plasmonics and with new prospects for applications in the quantum plasmonics for bimetallic alloys.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Gate-Tunable Near-Field Heat Transfer

Active control over the flow of heat in the near-field holds promise for nanoscale thermal management, with applications in refrigeration, thermophotovoltaics, and thermal circuitry. Analogously to its electronic counterpart, the metal–oxide–semiconductor (MOS) capacitor, we propose a thermal switching mechanism based on accumulation and depletion of charge carriers in an ultrathin plasmonic film, via application of external bias. In our proposed configuration, the plasmonic film is placed on top of a polaritonic dielectric material that provides a surface phonon polariton (SPhP) thermal channel, while also ensuring electrical insulation for application of large electric fields. The variation of carrier density in the plasmonic film enables the control of the surface plasmon polariton (SPP) thermal channel. We show that the interaction of the SPP with the SPhP significantly enhances the net heat transfer. Here, we study SiC as the oxide and explore three classes of gate-tunable plasmonic materials, transparent conductive oxides, doped semiconductors, and graphene, and theoretically predict contrast ratios as high as 225%.

42 ENGINEERING↗

Low-power light guiding and localization in optoplasmonic chains obtained by directed self-assembly

Here, optoplasmonic structures contain plasmonic components embedded in a defined photonic environment to create synergistic interactions between photonic and plasmonic components. Here, we show that chains of optical microspheres containing gold nanoparticles in their evanescent field combine the light guiding properties of a microsphere chain with the light localizing properties of a plasmonic nanoantenna. We implement these materials through template guided self-assembly and investigate their fundamental electromagnetic working principles through combination of electromagnetic simulations and experimental characterization. We demonstrate that optoplasmonic chains implemented by directed self-assembly achieve a significant reduction in guiding losses when compared with conventional plasmonic waveguides and, at the same time, retain the light localizing properties of plasmonic antennas at pre-defined locations. The results reinforce the potential of optoplasmonic structures for realizing low-loss optical interconnects with high bandwidth.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Excitation wavelength dependent photon anti-bunching/bunching from single quantum dots near gold nanostructures

Here, we aim to investigate the change in photon emission statistics of single CdSe/CdS core/shell quantum dots (QDs) on dielectric modified gold nanoparticle (NP) substrates as a function of the excitation wavelength. Photons emitted from single QDs are typically “anti-bunched” and are independent of the excitation wavelength. However, when QDs are coupled to plasmonic substrates, even at the low excitation power regime, we observed a significant change in photoluminescence emission behavior of single QDs; i.e. the emission transformed from incomplete photon anti-bunched to bunched when the excitation was changed from “off” to “on” plasmon resonance. Theoretical studies based on electrodynamics modeling suggested that for the QD–Au NP system, the quantum yield of single excitons decreases while that of biexcitons increases. In addition, when excited at the “on” resonance condition, the absorption is highly enhanced, resulting in an increased population of higher order excitons of the QDs. The higher order exciton emission was directly observed as an additional peak appeared at the blue side of the exciton peak of single QDs. The combined effect of the change in quantum yield and the increase in the absorption cross-section switches the photons emitted by single QDs from anti-bunched to bunched. These results provided direct evidence that not only the plasmonic nanostructures but also the excitation wavelength can effectively control the photon emission statistics of single QDs in the hybrid metal–semiconductor system. Manipulating the multiexciton–plasmon interaction in a hybrid complex like this could possibly open up new doors for applications such as entangled photon pair generation and plasmon-enhanced optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-Energy Density science at the Linac Coherent Light Source

The Matter in Extreme Conditions end station at the Linac Coherent Light Source holds great promise for novel pump-probe experiments to make new discoveries in high- energy density science. Recently, our experiments have demonstrated the first spectrally- resolved measurements of plasmons using a seeded 8-keV x-ray laser beam. Forward x-ray Thomson scattering spectra from isochorically heated solid aluminum show a well-resolved plasmon feature that is down-shifted in energy by 19 eV from the incident 8 keV elastic scattering feature. In this spectral range, the simultaneously measured backscatter spectrum shows no spectral features indicating observation of collective plasmon oscillations on a scattering length comparable to the screening length. Moreover, this technique is a prerequisite for Thomson scattering measurements in compressed matter where the plasmon shift is a sensitive function of the free electron density and where the plasmon intensity provides information on temperature.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Phase-resolved terahertz nanoimaging of W Te 2 microcrystals

The terahertz (THz) electrodynamics of few-layer W⁢Te 2 is dominated by the plasmon response. However, THz surface plasmons (SPs) with long wavelengths in two-dimensional exfoliated crystals are typically confined by the lateral geometry. Direct visualization of the plasmonic standing wave patterns is challenging due to the spatial confinement and low quality factor of the SP, especially for samples that are only a few monolayers thick. Here, we resolve subtle real-space features of the plasmonic response of W⁢Te 2 by augmenting more common scattering amplitude experiments with the phase contrast accomplished within the time-domain version of THz nanoimaging. Amplitude and phase images allow us to quantitatively evaluate the evolution of the plasmonic response at cryogenic temperatures in samples with variable thickness from 3 to 12 monolayers. Further, the proposed imaging modality is universally applicable to the THz near-field nanoscopy of low-dimensional materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Water purification

Production of decontaminated water from contaminated water using a vessel, an inlet to the vessel wherein the contaminated water is introduced into the vessel, an outlet to the vessel wherein the decontaminated water is removed from the vessel, a plasmonic-photocatalyst membrane connected to the vessel, plasmonic nanoparticles or nanostructures connected to the plasmonic-photocatalyst membrane, and a source of ultraviolet light that directs ultraviolet light onto the vessel, the plasmonic-photocatalyst membrane, the plasmonic nanoparticles or nanostructures, and the contaminated water to produce the decontaminated water from the contaminated water.

Brisbin, Ryan P.↗

Optical Response of Periodic Arrays of Graphene Nanodisks

Doped graphene nanostructures are a promising platform for photonics due to their exceptionally strong and tunable plasmonic resonances. When placed in a periodic array configuration, the plasmons supported by the individual nanostructures interact with each other and, under the appropriate conditions, can give rise to a collective mode known as a lattice resonance. Here, for this study, we perform a comprehensive analysis of the response of periodic arrays of graphene nanodisks and identify the conditions under which the system is able to support lattice resonances. We find that the ratio between the period of the array and the wavelength of the plasmon completely determines the behavior of the system. As a consequence, strong lattice resonances are achieved for micron-size nanodisks in the terahertz regime. We develop a theoretical model valid beyond the electrostatic approximation and use it to derive closed analytical expressions for the strength, the wavelength, and the width of the optical resonance of the arrays. The theoretical framework developed in this work paves the way for facile design and discovery of emerging properties of periodic arrays of graphene nanostructures that could enable applications in photonics and plasmonics.

36 MATERIALS SCIENCE↗

Generation of fast photoelectrons in strong-field emission from metal nanoparticles

We investigated the generation and control of fast photoelectrons (PEs) by exposing plasmonic nanoparticles (NPs) to short infrared (IR) laser pulses with peak intensities between 10 12 and 3 × 10 13 W/cm 2 . Our measured and numerically simulated PE momentum distributions demonstrate the extent to which PE yields and cutoff energies are controlled by the NP size, material, and laser peak intensity. For strong-field photoemission from spherical silver, gold, and platinum NPs with diameters between 10 and 100 nm our results confirm and surpass extremely high PEs cutoff energies, up to several hundred times the incident laser-pulse ponderomotive energy, found recently for gold nanospheres [Saydanzad et al., Nanophotonics 12, 1931 (2023)]. As reported previously for dielectric NPs [Rupp et al., J. Mod. Opt. 64, 995 (2017)], at higher intensities the cutoff energies we deduce from measured and simulated PE spectra tend to converge to a metal-independent limit. We expect these characteristics of light-induced electron emission from prototypical plasmonic metallic nanospheres to promote the understanding of the electronic dynamics in more complex plasmonic nanostructures and the design of nanoscale light-controlled plasmonic electron sources for photoelectronic devices of applied interest.

electron source↗

Mixed Nanosphere Assemblies at a Liquid–Liquid Interface

The in-plane packing of gold (Au), polystyrene (PS), and silica (SiO 2 ) spherical nanoparticle (NP) mixtures at a water–oil interface is investigated in situ by UV–vis reflection spectroscopy. All NPs are functionalized with carboxylic acid such that they strongly interact with amine-functionalized ligands dissolved in an immiscible oil phase at the fluid interface. This interaction markedly increases the binding energy of these nanoparticle surfactants (NPSs). The separation distance between the Au NPSs and Au surface coverage are measured by the maximum plasmonic wavelength (λ max ) and integrated intensities as the assemblies saturate for different concentrations of non-plasmonic (PS/SiO 2 ) NPs. Further, as the PS/SiO 2 content increases, the time to reach intimate Au NP contact also increases, resulting from their hindered mobility. λ max changes within the first few minutes of adsorption due to weak attractive inter-NP forces. Additionally, a sharper peak in the reflection spectrum at NP saturation reveals tighter Au NP packing for assemblies with intermediate non-plasmonic NP content. Grazing incidence small angle X-ray scattering (GISAXS) and scanning electron microscopy (SEM) measurements confirm a decrease in Au NP domain size for mixtures with larger non-plasmonic NP content. The results demonstrate a simple means to probe interfacial phase separation behavior using in situ spectroscopy as interfacial structures densify into jammed, phase-separated NP films.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Demonstration of gold nanorod systems for enhanced total efficiency: Experimental and numerical analysis

This study investigates the photothermal performance of gold nanorods engineered to exhibit longitudinal plasmon resonances at 695 nm, 780 nm, and 970 nm. The work combines synthesis, structural characterization, extinction measurements, numerical modeling, and controlled temperature experiments to quantify how nanorod geometry, resonance tuning, concentration, and chamber shape jointly influence heat generation. Transmission electron microscopy confirms that increasing nanorod aspect ratio systematically shifts the longitudinal plasmon peak toward the near-infrared region. Extinction measurements show strong agreement with theoretical predictions, validating the numerical model across two independent datasets. Three chamber geometries were tested under laser excitation at 640 nm, 808 nm, and 980 nm: an ascending stepped base, a flat base, and a descending stepped base. Without nanorods, the ascending geometry produced the highest efficiency due to enhanced natural convection. After introducing gold nanorods, all geometries exhibited substantial thermal enhancement, with total efficiencies exceeding 20%. The strongest improvement was obtained for nanorods resonant at 780 nm with a mass concentration of 4.6 mg/mL implemented on the descending stepped-base geometry. This performance resulted from the combined effect of spectral overlapping with the 808 nm laser, the highest nanorod concentration, and localized heat accumulation that intensified buoyancy-driven flow. The findings demonstrate that total efficiency is governed by a synergistic interplay between optical resonance, nanoparticle concentration, and macroscopic chamber design, revealing the system-level coupling between nanoscale plasmonic absorption and macroscale heat-transfer phenomena. The results provide a validated framework for tuning nanoscale plasmonic absorbers and optimizing thermal systems for applications requiring efficient light-to-heat conversion.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Controlling the Fluctuating Tip-Enhanced Raman Spectra of Chloramben on Silver Nanocubes

Tip-enhanced Raman (TER) scattering from molecules residing at plasmonic junctions can be used to detect, identify, and image single molecules. This is most evident for flat molecules interrogated under extreme conditions of temperatures and pressure. It is also the case for (bio)molecular systems that feature preferred orientations/conformations under ambient laboratory conditions. More complex molecules that can adopt multiple conformations and/or that feature different protonation and/or charge states give rise to complex TER spectra. Here we illustrate how the latter can be controlled in the case of chloramben molecules coated onto plasmonic silver nanocubes. We show that characteristic molecular Raman spectra cannot be obtained when tunneling plasmons are operative, i.e., when the tip is in direct contact with the chemically functionalized plasmonic nanoparticles. We rationalize these observations and propose an approach to less invasive, and hence, more analytical TER spectral imaging.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Site-Selective Doping and Oxidation State Control of Copper in Gold Nanorods

We report the synthesis of plasmonic gold–copper nanostructures with tunable copper spatial distribution and oxidation state. Au–Cu alloy shells were deposited in aqueous solution onto colloidal gold nanorods that functioned as seeds, and the resulting shell morphology was found to depend strongly on the nanorod aspect ratio. For relatively fat gold nanorods (16 x 31 nm), Au–Cu growth was preferentially localized near the rod midsections, forming belt-like structures, whereas for skinnier nanorods (9 x 32 nm), Au–Cu growth produced patchy surface coverage around the entire rod. The shell thickness was tuned from 1 to 4 nm; upon air exposure, thicker shells exhibited a higher Cu(I) fraction compared to the initial shell. Incorporation of the Au–Cu shell led to pronounced shifts in the plasmonic features of the gold nanorods. These tunable plasmonic Au–Cu nanorods provide a materials basis for Cu-based plasmonic materials in the context of electrochemical CO₂ reduction.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Shape- and Orientation-Dependent Scattering of Isolated Gold Nanostructures Using Polarized Dark-Field Microscopy

In this work, we demonstrate a simple and robust method for measuring the shape- and orientation-dependent optical scattering of various plasmonic nanostructures adsorbed onto a solid surface using polarized dark-field microscopy. By analyzing the dark-field scattering images of gold nanostructures using grazing incidence polarized light with a bench-top microscope, we are able to correlate optical scattering from the individual nanostructures with their shape and orientation. Depending on the size, shape, and orientation of the plasmonic nanostructures, they exhibit characteristic angle- and polarization-dependent scattering signals. Extracting the red, green, and blue channels of the scattering signals from a color-imaging detector as a function of azimuthal angle provides a polar plot of color intensity values that is characteristic of the underlying nanostructure. Examples are presented for various nanostructures, including spherical nanoparticles, nanotriangles, and nanorods. Experimental results are complemented by numerical calculations of the scattering spectra of representative model nanostructures. We demonstrate that the polarization- and orientation-dependent scattering behavior is a consequence of various localized surface plasmon modes existing in the nanostructures and can be used to verify the shape of individual objects as well as quickly identify the orientation of numerous objects on a densely populated substrate. We anticipate that this method will provide a rapid and efficient complement to the typical structural analysis of nanoparticles that is achieved by electron microscopy as well as providing a simple method for generating detailed information of the optical scattering of various types of individual plasmonic nanostructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ambient Tip-Enhanced Photoluminescence with 5 nm Spatial Resolution

We achieve record spatial resolution in ambient tip-enhanced photoluminescence (TEPL) from CdSe/ZnS semiconductor quantum dots (QDs). Our approach only takes advantage of surface roughness at the apex of a sputtered plasmonic gold probe. When irradiated with visible light (633 and 532 nm lasers), nano-corrugated regions of the apex of an Au tip support 5-nm spatial resolution in TEPL imaging of QD aggregates on silicon. The reproducibility of our observations is illustrated using different plasmonic probes and samples. The origin of the observed near-field contrast, underlying the demonstrated high spatial resolution in TEPL, is discussed in the context of field enhancement at the metal tip-fluorophore interface.

Chemical Dynamics Initiative↗