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DOE OSTI2023

Sustainable chemistry with plasmonic photocatalysts

There is a pressing global need to increase the use of renewable energy sources and limit greenhouse gas emissions. Towards this goal, highly efficient and molecularly selective chemical processes that operate under mild conditions are critical. Plasmonic photocatalysis uses optically resonant metallic nanoparticles and their resulting plasmonic, electronic, and phononic light-matter interactions to drive chemical reactions. The promise of simultaneous high-efficiency and product-selective reactions with plasmon photocatalysis provides a compelling opportunity to rethink how chemistry is achieved. Plasmonic nanoparticles serve as nanoscale ‘antennas’ that enable strong light–matter interactions, surpassing the light-harvesting capabilities one would expect purely from their size. Complex composite structures, combining engineered light harvesters with more chemically active components, are a focal point of current research endeavors. In this review, we provide an overview of recent advances in plasmonic catalysis. We start with a discussion of the relevant mechanisms in photochemical transformations and explain hot-carrier generation and distributions from several ubiquitous plasmonic antennae. Then we highlight three important types of catalytic processes for sustainable chemistry: ammonia synthesis, hydrogen production and CO 2 reduction. To help elucidate the reaction mechanism, both state-of-art electromagnetic calculations and quantum mechanistic calculations are discussed. This review provides insights to better understand the mechanism of plasmonic photocatalysis with a variety of metallic and composite nanostructures toward designing and controlling improved platforms for green chemistry in the future.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

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↗

NASA NTRS2005

Voltage-induced broad-spectrum reflectivity change with surface-plasmon waves

Voltage-induced broad-spectrum reflectivity change with surface-plasmon waves is reported. When white light is incident at a metal/electro-optical material interface, surface-plasmon waves can be excited under phase match conditions. This surface-plasmon resonance depends on the dielectric constants of both the metal and the electro-optical material. Photons in the surface-plasmon resonance wavelength range are absorbed by the interface. Since metals have large imaginary parts of their dielectric constants, the surface-plasmon resonances are broad and may cover all visible wavelengths. Applying voltage to the electro-optical material to change its dielectric constant can result in a change in the reflectivity at the interface. Experimental results showed a reflectivity change from almost 0% to about 40% under an applied voltage using a liquid-crystal and nickel film structure, and the results had good agreement with theoretical calculations. The theoretical calculations also predicted a 90% reflectivity recovery by exciting surface-plasmon waves at a Rh-Al/electro-optical material interface. These results demonstrate that a high efficiency white light modulator can be built using surface-plasmon excitations.

white light modulator↗

DOE OSTI2022

Near–Band–Edge Enhancement in Perovskite Solar Cells via Tunable Surface Plasmons

Plasmonic perovskite solar cells (PSCs) using core-shell type plasmonic particles are designed, which possess the plasmon resonance in the near-infrared range. This can selectively strengthen the interaction of the perovskite layer with low-energy photons. The mesoporous PSCs employing the plasmonic particles have delivered a 10%-15% enhancement of external quantum efficiency in the plasmonic resonance range. This surface-plasmonic effect has been analyzed using complementary techniques, including selective wavelength excitation and time-dependent photoluminescence. Here it is shown that the metal-based core-shell-type plasmonic structures in PSCs optimize the scattering and absorption of incident light and the dynamics of photogenerated carriers. Furthermore, both optical and electronic effects increase the power conversion efficiency of PSCs from 17.49% to 19.88%, paving a way toward controlling the thickness of the photoactive layer for advanced devices such as tandem solar cells.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Elucidating the Roles of Local and Nonlocal Rate Enhancement Mechanisms in Plasmonic Catalysis

Plasmonic metal nanoparticles (e.g., Ag, Au, and Cu) constitute a class of materials that interact with light via the excitation of localized surface plasmon resonance (LSPR). Numerous studies have reported substantial enhancements in the rates of chemical reactions on illuminated plasmonic nanoparticle catalysts compared to corresponding systems in the absence of illumination. There are two mechanisms that have been proposed to explain the LSPR-induced chemical reactivity. One mechanism assumes a local plasmon-induced hot charge-carrier-mediated activation of the reactants, while the other assumes an LSPR-induced equilibrium heating of the catalyst, which leads to energy transfer to and chemical reaction of the adsorbed reactants. Here, in this contribution, we developed a setup amenable to accurate in situ catalyst temperature and kinetic reaction rate measurements. We employed this setup to study the LSPR-induced rate enhancement in a case study of the CO oxidation reaction on plasmonic, monometallic Ag nanoparticle catalysts supported on α-Al 2 O 3 . We explored various Ag loadings and clustering levels. Our data show that the equilibrium heating of the catalyst cannot fully explain the illumination-induced plasmonic rate enhancements. This is the case even for high loading and clustering of Ag nanoparticles, where the equilibrium heating significantly increases. Based on the analysis, we propose that local effects, related to the plasmon-induced activation of adsorbates (reactants) via electronic excitation of the reactant or photothermal heating of the reactants that is highly localized to the individual nanoparticles, play a critical role in driving LSPR-induced chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Plasmon–emitter interactions at the nanoscale

Plasmon–emitter interactions are of central importance in modern nanoplasmonics and are generally maximal at short emitter–surface separations. However, when the separation falls below 10–20 nm, the classical theory deteriorates progressively due to its neglect of quantum effects such as nonlocality, electronic spill-out, and Landau damping. Here we show how this neglect can be remedied in a unified theoretical treatment of mesoscopic electrodynamics incorporating Feibelman d -parameters. Our approach incorporates nonclassical resonance shifts and surface-enabled Landau damping—a nonlocal damping effect—which have a dramatic impact on the amplitude and spectral distribution of plasmon–emitter interactions. We consider a broad array of plasmon–emitter interactions ranging from dipolar and multipolar spontaneous emission enhancement, to plasmon-assisted energy transfer and enhancement of two-photon transitions. The formalism gives a complete account of both plasmons and plasmon–emitter interactions at the nanoscale, constituting a simple yet rigorous platform to include nonclassical effects in plasmon-enabled nanophotonic phenomena.

Science & Technology - Other Topics↗

DOE OSTI2014

Imaging surface plasmon polaritons using proximal self-assembled InGaAs quantum dots

We present optical investigations of hybrid plasmonic nanosystems consisting of lithographically defined plasmonic Au-waveguides or beamsplitters on GaAs substrates coupled to proximal self-assembled InGaAs quantum dots. We designed a sample structure that enabled us to precisely tune the distance between quantum dots and the sample surface during nano-fabrication and demonstrated that non-radiative processes do not play a major role for separations down to ∼10 nm. A polarized laser beam focused on one end of the plasmonic nanostructure generates propagating surface plasmon polaritons that, in turn, create electron-hole pairs in the GaAs substrate during propagation. These free carriers are subsequently captured by the quantum dots ∼25 nm below the surface, giving rise to luminescence. The intensity of the spectrally integrated quantum dot luminescence is used to image the propagating plasmon modes. As the waveguide width reduces from 5 μm to 1 μm, we clearly observe different plasmonic modes at the remote waveguide end, enabling their direct imaging in real space. This imaging technique is applied to a plasmonic beamsplitter facilitating the determination of the splitting ratio between the two beamsplitter output ports as the interaction length L{sub i} is varied. A splitting ratio of 50:50 is observed for L{sub i}∼9±1 μm and 1 μm wide waveguides for excitation energies close to the GaAs band edge. Our experimental findings are in good agreement with mode profile and finite difference time domain simulations for both waveguides and beamsplitters.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2023

Optical N-plasmon: topological hydrodynamic excitations in graphene from repulsive Hall viscosity

Abstract Edge states occurring in Chern and quantum spin-Hall phases are signatures of the topological electronic band structure in two-dimensional (2D) materials. Recently, a new topological electromagnetic phase of graphene characterized by the optical N-invariant was proposed. Optical N-invariant arises from repulsive Hall viscosity in hydrodynamic many-body electron systems, distinct from the Chern and Z 2 invariants. In this paper, we introduce the topologically protected edge excitation—optical N-plasmon of interacting many-body electron systems in the topological optical N-phase. These optical N-plasmons are signatures of the topological plasmonic band structure in 2D materials. We demonstrate that optical N-plasmons exhibit unique dispersion relations, stability against various boundary conditions, and edge profiles when compared with the topologically trivial edge magneto plasmons. Based on the optical N-plasmon, we design an ultra sub-wavelength broadband topological hydrodynamic circulator, which is a chiral quantum radio-frequency circuit component crucial for information routing and interfacing quantum–classical computing systems. Furthermore, we reveal that optical N-plasmons can be effectively tuned by the neighboring dielectric environment without breaking the topological properties. Our work provides a smoking gun signature of topological electromagnetic phases occurring in 2D materials arising from repulsive Hall viscosity.

Physics↗

DOE OSTI2020

Enhancing Graphene Plasmonic Device Performance via its Dielectric Environment

Graphene plasmons provide a compelling avenue toward chip-scale dynamic tuning of infrared light. Dynamic tunability emerges through controlled alterations in the optical properties of the system defining graphene’s plasmonic dispersion. Typically, electrostatic induced alterations of the carrier concentration in graphene working in conjunction with mobility have been considered the primary factors dictating plasmonic tunability. We find here that the surrounding dielectric environment also plays a primary role, dictating not just the energy of the graphene plasmon but so too the magnitude of its tuning and spectral width. To arrive at this conclusion, poles in the imaginary component of the reflection coefficient are used to efficiently survey the effect of the surrounding dielectric on the tuning of the graphene plasmon. By investigating several common polar materials, optical phonons (i.e., the Reststrahlen band) of the dielectric substrate are shown to appreciably affect not only the plasmon’s spectral location but its tunability, and its resonance shape as well. In particular, tunability is maximized when the resonances are spectrally distant from the Reststrahlen band, whereas sharp resonances (i.e., high-Q) are achievable at the band’s edge. Overall, these observations both underscore the necessity of viewing the dielectric environment in aggregate when considering the plasmonic response derived from two-dimensional materials and provide heuristics to design dynamically tunable graphene-based infrared devices.

36 MATERIALS SCIENCE↗

DOE OSTI2021

First-principles modeling of plasmons in aluminum under ambient and extreme conditions

The theoretical understanding of plasmon behavior is crucial for an accurate interpretation of inelastic scattering diagnostics in many experiments. In this work, we highlight the utility of linear response time-dependent density functional theory (LR-TDDFT) as a first-principles framework for consistently modeling plasmon properties. We provide a comprehensive analysis of plasmons in aluminum from ambient to warm dense matter conditions and assess typical properties such as the dynamical structure factor, the plasmon dispersion, and the plasmon lifetime. We compare our results with scattering measurements and with other TDDFT results as well as models such as the random phase approximation, the Mermin approach, and the dielectric function obtained using static local field corrections of the uniform electron gas parametrized from path-integral Monte Carlo simulations. We conclude that results for the plasmon dispersion and lifetime are inconsistent between experiment and theories and that the common practice of extracting and studying plasmon dispersion relations is an insufficient procedure to capture the complicated physics contained in the dynamic structure factor in its full breadth.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2017

Splashing transients of 2D plasmons launched by swift electrons

Launching of plasmons by swift electrons has long been used in electron energy–loss spectroscopy (EELS) to investigate the plasmonic properties of ultrathin, or two-dimensional (2D), electron systems. However, the question of how a swift electron generates plasmons in space and time has never been answered. We address this issue by calculating and demonstrating the spatial-temporal dynamics of 2D plasmon generation in graphene. We predict a jet-like rise of excessive charge concentration that delays the generation of 2D plasmons in EELS, exhibiting an analog to the hydrodynamic Rayleigh jet in a splashing phenomenon before the launching of ripples. The photon radiation, analogous to the splashing sound, accompanies the plasmon emission and can be understood as being shaken off by the Rayleigh jet–like charge concentration. Considering this newly revealed process, we argue that previous estimates on the yields of graphene plasmons in EELS need to be reevaluated.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2015

Nonlinear magneto-plasmonics

Nonlinear magneto-plasmonics (NMP) describes systems where nonlinear optics, magnetics and plasmonics are all involved. In such systems, nonlinear magneto-optical Kerr effect (nonlinear MOKE) plays an important role as a characterization method, and Surface Plasmons (SPs) work as catalyst to induce many new effects. Magnetization-induced second-harmonic generation (MSHG) is the major nonlinear magneto-optical process involved. The new effects include enhanced MSHG, controlled and enhanced magnetic contrast, etc. Nanostructures such as thin films, nanoparticles, nanogratings, and nanoarrays are critical for the excitation of SPs, which makes NMP an interdisciplinary research field in nanoscience and nanotechnology. In this review article, we organize recent work in this field into two categories: surface plasmon polaritons (SPPs) representing propagating surface plasmons, and localized surface plasmons (LSPs), also called particle plasmons. We review the structures, experiments, findings, and the applications of NMP from various groups.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Heat-activated Plasmonic Chemical Sensors for Harsh Environments

A passive plasmonics based chemical sensing system to be used in harsh operating environments was investigated and developed within this program. The initial proposed technology was based on combining technologies developed at the SUNY Polytechnic Institute Colleges of Nanoscale Science and Engineering (CNSE) and at the University of Minnesota (UM). Specifically, a passive wireless technique developed at UM was to utilize a heat-activated plasmonic design to passively harvest the thermal energy from within a combustion emission stream and convert this into a narrowly focused light source. This plasmonic device was based on a bullseye design patterned into a gold film using focused ion beam methods (FIB). Critical to the design was the use of thermal stabilizing under and overlayers surrounding the gold film. These stabilizing layers were based on both atomic layer deposited films as well as metal laminate layers developed by United Technologies Aerospace Systems (UTAS). While the bullseye design was never able to be thermally stabilized for operating temperatures of 500oC or higher, an alternative energy harvesting design was developed by CNSE within this program. With this new development, plasmonic sensing results are presented where thermal energy is harvested using lithographically patterned Au nanorods, replacing the need for an external incident light source. Gas sensing results using the harvested thermal energy are in good agreement with sensing experiments, which used an external incident light source. Principal Component Analysis (PCA) was used to reduce the wavelength parameter space from 665 variables down to 4 variables with similar levels of demonstrated selectivity. The method was further improved by patterning rods which harvested energy in the near infrared, which led to a factor of 10 decrease in data acquisition times as well as demonstrated selectivity with a reduced wavelength data set. The combination of a plasmonic-based energy harvesting sensing paradigm with PCA analysis and wavelength down selection offers a novel path towards simplification and integration of plasmonic-based sensing methods using selected wavelengths rather than a full spectral analysis. Integration efforts were designed and modeled for thermal and mass transport considerations by UTAS which led to the 3D printing of scaled models that would serve as the housing for the alternative energy harvesting plasmonic chemical sensor design developed by CNSE.

47 OTHER INSTRUMENTATION↗

DOE OSTI2016

Dual-Responsive Reversible Plasmonic Behavior of Core–Shell Nanostructures with pH-Sensitive and Electroactive Polymer Shells

In this paper, we report novel dual-responsive plasmonic core–shell anisotropic nanostructures composed of gold nanorod (AuNR) and responsive polyaniline (PANI) shells with plasmonic mode appearance reversibly modulated through orthogonal stimuli (i.e., electrical potential and pH change). In this system, the PANI shells provide AuNR cores with three different refractive index environments depending on stimuli (pH and electrical potential). Therefore, no additional secondary responsive component is necessary to induce the dual-responsive properties of AuNR cores. Furthermore, in this study, dual-responsive properties can be realized for nanostructures fixed on substrates, whereas previously reported dual-responsive plasmonic systems can only be controlled in solution. Here, the highest localized surface plasmonic resonance (LSPR) shift of the AuNR cores can be induced by changing both local pH and applying electric potential. Notably, a significant plasmon band shift by 107 nm is realized with only 8 nm thick PANI shell due to the large refractive index change at the gold–polymer interface. A maximum shift of the longitudinal plasmon mode of 149 nm is obtained by applying a modest electrical potential (below ±1 V), a large shift rarely reported in the literature for metal nanostructures. Moreover, our anisotropic core/shell nanostructures exhibit stable and reversible dual-responsive LSPR behavior over 100 cycles without degradation.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Mapping Photoemission and Hot-Electron Emission from Plasmonic Nanoantennas

Understanding plasmon-mediated electron emission and energy transfer on the nanometer length scale is critical to controlling light–matter interactions at nanoscale dimensions. In a high-resolution lithographic material, electron emission and energy transfer lead to chemical transformations. Here, we employ such chemical transformations in two different high-resolution electron-beam lithography resists, poly(methyl methacrylate) (PMMA) and hydrogen silsesquioxane (HSQ), to map local electron emission and energy transfer with nanometer resolution from plasmonic nanoantennas excited by femtosecond laser pulses. We observe exposure of the electron-beam resists (both PMMA and HSQ) in regions on the surface of nanoantennas where the local field is significantly enhanced. Exposure in these regions is consistent with previously reported optical-field-controlled electron emission from plasmonic hotspots as well as earlier work on low-electron-energy scanning probe lithography. For HSQ, in addition to exposure in hotspots, we observe resist exposure at the centers of rod-shaped nanoantennas in addition to exposure in plasmonic hotspots. Optical field enhancement is minimized at the center of nanorods suggesting that exposure in these regions involves a different mechanism to that in plasmonic hotspots. Our simulations suggest that exposure at the center of nanorods results from the emission of hot electrons produced via plasmon decay in the nanorods. Our results provide a means to map both optical-field-controlled electron emission and hot-electron transfer from nanoparticles via chemical transformations produced locally in lithographic materials.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2026

Plasmon-Induced Resonance Energy Transfer in Hybrid Nanomaterials

Plasmon-induced resonance energy transfer (PIRET) has emerged as a powerful mechanism for harnessing and redirecting plasmon energy before it dissipates into hot carriers or heat. By matching plasmon resonance frequencies with acceptor absorption bands, PIRET extends plasmon-driven processes beyond the charge transfer pathway, enabling selective energy flow into excitonic transitions. Here, this review highlights important progress in elucidating the fundamental plasmon decay processes and transitioning them into hybrid nanomaterials under PIRET. Employing specialized single-particle spectroscopic techniques based on scattering, extinction, and emission enables demonstration of PIRET in the face of competing mechanisms, such as interfacial charge transfer and thermalization. Finally, we complete this review by addressing strategies for active modulation of PIRET and present applications, ranging from plasmon photocatalysis to intracellular biochemical sensing.

Energy transfer↗

DOE OSTI2017

Doped Silicon Nanocrystal Plasmonics

Doped semiconductor nanocrystals represent an exciting new type of plasmonic material with optical resonances in the infrared. Unlike noble metal nanoparticles, the plasmon resonance can be tuned by altering the doping density. Recently, it has been shown that silicon nanocrystals can be doped using phosphorus and boron resulting in highly tunable infrared plasmon resonances. Due to the band structure of silicon, doping with phosphorus contributes light (transverse) and heavy (longitudinal) electrons, while boron contributes light and heavy holes and one would expect two distinct plasmon branches. In this work we develop a classical hybridization theory and a full quantum mechanical TDLDA approach for two-component carrier plasmas and show that the interaction between the two plasmon branches results in strongly hybridized plasmon modes. The antibonding mode where the two components move in phase is bright and depends sensitively on the doping densities. The low energy bonding mode with opposite charge alignment can only be observed in the quantum regime when strong Coulomb screening is present. The theoretical results are in good agreement with the experimental data.

42 ENGINEERING↗

DOE OSTI2019

Continuous Wave Resonant Photon Stimulated Electron Energy-Gain and Electron Energy-Loss Spectroscopy of Individual Plasmonic Nanoparticles

The unique optical properties of surface plasmon resonances in nanostructured materials have attracted considerable attention, broadly impacting both fundamental research and applied technologies ranging from sensing and optoelectronics to quantum computing. Electron energy-loss spectroscopy (EELS) in the transmission electron microscope has revealed valuable information about the full plasmonic spectrum of these materials with nanoscale spatial resolution. Here, in this study, we report a novel approach for experimentally accessing the photon-stimulated electron energy-gain and stimulated electron energy-loss responses of individual plasmonic nanoparticles via the simultaneous irradiation of a continuous wave laser and continuous current, monochromated electron probe. Stimulated gain and loss probabilities are equivalent and increase linearly in the low-irradiance range of 0.5 × 10 8 to 4 × 10 8 W/m 2 , above which excessive heating reduces the observed probabilities; importantly in our low-irradiance regime, the photon energy must be tuned in resonance with the plasmon energy for the stimulated gain and loss peaks to emerge. Theoretical modeling based on Fermi’s golden rule elucidates how the plasmon resonantly and coherently shuttles energy quanta between the electron probe and the radiation field and vice versa in stimulated electron energy-loss and -gain events. This study opens a fundamentally new approach to explore the quantum physics of excited-state plasmon resonances that does not rely on high-intensity laser pulses or any modification to the EELS detector.

(scanning) transmission electron microscope ((S)TE↗