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DOE OSTI2021

Density-independent plasmons for terahertz-stable topological metamaterials

Significance Plasmons, collective electron density oscillations in metals or doped semiconductors, provide an efficient way to couple light and matter at subwavelength scales. Usually, plasmons are carrier density ( n ) dependent, which may cause unstable functionalities of plasmons, especially for cutting-edge terahertz technology. Here, we reveal a unified mechanism for generating unusual n -independent plasmons (DIPs), where terahertz DIPs can be excited in some low-dimensional topological semimetals. Stable terahertz spectroscopy from narrowband to broadband and even a quantization can be achieved in topological metamaterials. Our study not only broadens the concept of plasmons by combining with exotic topological states but also paves a way to designing a compact device for stable terahertz applications.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Probing plasmons in three dimensions by combining complementary spectroscopies in a scanning transmission electron microscope

The nanoscale optical response of surface plasmons in three-dimensional metallic nanostructures plays an important role in many nanotechnology applications, where precise spatial and spectral characteristics of plasmonic elements control device performance. Electron energy loss spectroscopy (EELS) and cathodoluminescence (CL) within a scanning transmission electron microscope have proven to be valuable tools for studying plasmonics at the nanoscale. Each technique has been used separately, producing three-dimensional reconstructions through tomography, often aided by simulations for complete characterization. Here we demonstrate that the complementary nature of the two techniques, namely that EELS probes beam-induced electronic excitations while CL probes radiative decay, allows us to directly obtain a spatially- and spectrally-resolved picture of the plasmonic characteristics of nanostructures in three dimensions. Furthermore, the approach enables nanoparticle-by-nanoparticle plasmonic analysis in three dimensions to aid in the design of diverse nanoplasmonic applications.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Sensitive singular-phase optical detection without phase measurements with Tamm plasmons

Spectrally-tailored interactions of light with material interfaces have offered many exciting applications in sensing, photo-detection, and optical energy conversion. In particular, complete suppression of light reflectance at select frequencies accompanied by sharp phase variations in the reflected signal forms the basis for the development of ultra-sensitive singular-phase optical detection schemes such as Brewster and surface plasmon interferometry. However, both the Brewster effect and surface-plasmon-mediated absorption on planar interfaces are limited to one polarization of the incident light and oblique excitation angles, and may have limited bandwidth dictated by the material dielectric index and plasma frequency. To alleviate these limitations, we design narrow-band super-absorbers composed of plasmonic materials embedded into dielectric photonic nanostructures with topologically-protected interfacial Tamm plasmon states. These structures have planar geometry and do not require nanopatterning to achieve perfect absorption of both polarizations of the incident light in a wide range of incident angles, including the normal incidence. Their absorption lines are tunable across a very broad spectral range via engineering of the photon bandstructure of the dielectric photonic nanostructures to achieve reversal of the geometrical phase across the interface with the plasmonic absorber. We outline the design strategy to achieve perfect absorptance in Tamm structures with dissipative losses via conjugate impedance matching. We further demonstrate via modeling how these structures can be engineered to support sharp asymmetric amplitude resonances, which can be used to improve the sensitivity of optical sensors in the amplitude-only detection scheme that does not require use of bulky and expensive ellipsometry equipment

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Ultrafast infrared plasmon switching in aligned carbon-nanotube optical resonators

Reconfigurable plasmonic materials are crucial components in active photonic devices for optical communication, signal processing, and sensing applications. Certain candidates including transparent conducting oxides, small-bandgap semiconductors (i.e. Ge, InSb), and conducting polymers can exhibit switchable free carrier concentrations triggered by optical, electrical or thermal excitations. Here, we show that aligned films of single-walled carbon nanotubes (SWCNTs) can serve as all-optically tunable plasmonic material in the mid-infrared range, thereby adding them to the library of switchable plasmonic materials. Interband optical pumping with femtosecond laser pulses results in the photoexcitation of free charge carriers, which transiently blueshifts the plasmon resonances of patterned, periodic SWCNT nano-resonators spanning the mid-infrared spectral range from 1700 to 2700 cm -1 . Furthermore. the ultrafast plasmon modulation exhibits a nearly single-picosecond decay time, attributed to interband carrier relaxation and inter-tube charge transfer. Given that aligned films of SWCNTs have high thermal stability, excellent photostability, epsilon-near-zero property, and extremely large optical anisotropy, their dynamic tunability represents a promising pathway towards active optical devices in the technologically important mid-infrared range.

single-walled carbon nanotubes↗

DOE OSTI2019

Plasmonic Lenses for Tunable Ultrafast Electron Emitters at the Nanoscale

Simultaneous spatio-temporal confinement of energetic electron pulses to femtosecond and nanometer scales is a topic of great interest in the scientific community, given the potential im- pact of such development on a wide spectrum of scientific and industrial applications. For example, in ultrafast electron scattering, nanoscale probes would enable accurate maps of structural dynamics in materials with nanoscale heterogeneity, thereby understanding the role of boundaries and defects on macroscopic properties. On the other hand, advances in this field are mostly limited by the electron source brightness and size. We present the design, fabrication, and optical characterization of bullseye plasmonic lenses for next-generation ultrafast electron sources. Using electromagnetic simulations, we examine how the interplay between light-plasmon coupling, plasmon propagation, dispersion, and resonance governs the properties of the photoemitted electron pulse. We also illus- trate how the pulse duration and strength can be tuned by geometric design, and predict sub-10 fs pulses with nanoscale diameter can be achieved. We then fabricated lenses in gold films and char- acterized their plasmonic properties with cathodoluminescence spectromicroscopy, demonstrating suitable plasmonic behavior for ultrafast, nanoscale photoemission.

43 PARTICLE ACCELERATORS↗

DOE OSTI2019

Ultrafast Multiharmonic Plasmon Generation by Optically Dressed Electrons

Interactions between electrons and photons are a source of rich physics from atomic to astronomical scales. Here, we examine a new kind of electron-photon interaction in which an electron, modulated by light, radiates multiple harmonics of plasmons. The emitted plasmons can be femtosecond in duration and nanometer in spatial scale. The extreme subwavelength nature of the plasmons lowers the necessary input light intensity by at least 4 orders of magnitude relative to state-of-the-art strong-field processes involving bound or free electrons. Here, the results presented here reveal a new means of ultrafast (10–1000 fs) interconversion between photonic and plasmonic energy, and a general scheme for generating spatiotemporally shaped ultrashort pulses in optical materials. More generally, our results suggest a route towards realizing analogues of fascinating physical phenomena like nonlinear Compton scattering in plasmonics and nanophotonics with relatively low intensities, slow electrons, and on nanometer length scales.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2019

In vivo nucleic acid detection and imaging within whole plants using plasmonic nanosensors

The ability to monitor gene expression within living plants is of importance in many applications ranging from plant biology research to biofuel development; however, no method currently exists without requiring sample extraction. Herein, we report a multimodal imaging method based on plasmonic nanoprobes for in vivo imaging and biosensing of microRNA biotargets within whole plant leaves. This method integrates three different but complementary techniques: surfaceenhanced Raman scattering (SERS), X-ray fluorescence (XRF), and plasmonics-enhanced two-photon luminescence (TPL). The multimodal method utilizes plasmonic nanostars, which not only provide large Raman signal enhancement, but also allow for localization and quantification by XRF and plasmonics-enhanced TPL, owing to gold content and high two-photon luminescence cross-sections. For the sensing mechanism, inverse molecular sentinel (iMS) nanoprobes are used for SERS bioimaging of microRNA within Arabidopsis thaliana leaves to provide a dynamic SERS map of detected microRNA targets while also quantifying nanoprobe concentrations using XRF and TPL. This report lays the foundation for the use of plasmonic nanoprobes for in vivo functional imaging of nucleic acid biotargets in whole plants, a tool that will allow the study of these biotargets with previously unmet spatial and temporal resolution.

bioimaging↗

DOE OSTI2015

Superradiant amplification of terahertz radiation by plasmons in inverted graphene with a planar distributed Bragg resonator

It is shown theoretically that stimulated generation of terahertz radiation by plasmons in graphene with a planar distributed Bragg resonator is possible at two different frequencies for each plasmon mode. This behavior may be attributed to the superradiance of the collective plasmon mode, which is associated with superlinear increase in the radiative damping of the plasmons with increase in pumping power. As a result, the curves of the radiative damping and the plasmon gain as a function of the pumping power intersect at two points corresponding to different generation conditions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Quantum-enhanced plasmonic sensing

Quantum resources can enhance the sensitivity of a device beyond the classical shot noise limit and, as a result, revolutionize the field of metrology through the development of quantum-enhanced sensors. In particular, plasmonic sensors, which are widely used in biological and chemical sensing applications, offer a unique opportunity to bring such an enhancement to real-life devices. Here, we use bright entangled twin beams to enhance the sensitivity of a plasmonic sensor used to measure local changes in the refractive index. We demonstrate a 56% quantum enhancement in the sensitivity of a state-of-the-art plasmonic sensor when compared with the corresponding classical configuration and a 24% quantum enhancement when compared to an optimal single-beam classical configuration. We measure sensitivities on the order of 10 –10 RIU / √Hz, nearly 5 orders of magnitude better than previous proof-of-principle implementations of quantum-enhanced plasmonic sensors. Furthermore, these results promise significant enhancements in ultratrace label-free plasmonic sensing and will find their way into areas ranging from biomedical applications to chemical detection.

47 OTHER INSTRUMENTATION↗

DOE OSTI2019

Plasmon-mediated electrochemical reactions: the influence of nanoparticle structure (Final Report)

Harnessing the energy of the sun to drive chemical reactions is an important strategy for lowering the cost and energy consumption associated with producing chemicals of interest. One challenge inherent to using solar energy is finding ways to convert the light into more useful forms of energy that can be utilized by chemical reactions. This research project focuses on using nanoscale particles of gold and silver (~10-100 nanometers in size and known as plasmonic nanoparticles) that are capable of transforming light energy into chemical energy in order to facilitate electrochemical reactions at the nanoparticle surface. These reactions involve the transfer of electrons between a molecule of interest and the plasmonic nanoparticle, which serves as an electrode. When we shine light on the nanoparticle, it helps promote the transfer of electrons, improving the reaction efficiency and yield. An open question is how the shape and size of the nanoparticle affects its ability to transform light into useful energy for electrochemical reactions that can then be utilized by molecules near the surface. This requires us to study reactions between molecules and single nanoparticles, so we can understand the role that heterogeneity in nanoparticle structure plays. To do this, we use molecules that change color and emit light when they undergo an electrochemical reaction, providing a strategy to follow these reactions at the surface of single nanoparticles. Our experiments reveal the importance of controlling the interface between the molecules and the plasmonic nanoparticles, as well as the interface between the plasmonic nanoparticles and the supporting substrate. Moreover, it is critical to find molecules that show well-behaved electrochemical behavior, in order to verify that the observed behaviors are due to the plasmonic nanoparticles and not the molecular reporters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Probing and Understanding the Spatial and Energy Distributions of Plasmonic Hot Carriers via Single-Molecule Quantum Transport

The generation of hot carriers in plasmonic nanostructures offers new transformative opportunities for a range of applications, including solar energy harvesting, photochemistry, and photodetection. To better understand such phenomena, this project aims to develop an experimental approach to study and understand hot carrier distributions in photoexcited plasmonic nanostructures. The developed experimental approach, combining scanning probe-based single-molecule quantum transport measurements with plasmonic excitation methods, leverages nanoscopic single molecules as quantum energy filters to selectively access hot carriers in a variety of plasmonic nanostructures. This report summarizes the key outcomes, impacts, and lessons learned in the first two years of the project. Over the past two years, important progress was made in achieving the project's goals, including the development of the scanning probe-based experimental platform, fabrication of plasmonic nanostructures, and design and synthesis of the desired molecular candidates. Insights from this research will pave the path toward the development of technologies that will improve the way we harvest solar energy and drive chemical reactions and ultimately help transition the U.S. to a clean and sustainable society.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2023

Holographic Nano‐Imaging of Terahertz Dirac Plasmon Polaritons in Topological Insulator Antenna Resonators

Abstract Excitation of Dirac plasmon polaritons (DPPs) in bi‐dimensional materials have attracted considerable interest in recent years, both from perspectives of understanding their physics and exploring their transformative potential for nanophotonic devices, including ultra‐sensitive plasmonic sensors, ultrafast saturable absorbers, modulators, and switches. Topological insulators (TIs) represent an ideal technological platform in this respect because they can support plasmon polaritons formed by Dirac carriers in the topological surface states. Tracing propagation of DPPs is a very challenging task, particularly at terahertz (THz) frequencies, where the DPP wavelength becomes over one order of magnitude shorter than the free space photon wavelength. Furthermore, severe attenuation hinders the comprehensive analysis of their characteristics. Here, the properties of DPPs in real TI‐based devices are revealed. Bi 2 Se 3 rectangular antennas can efficiently confine the propagation of DPPs to a single dimension and, as a result, enhance the DPPs visibility despite the strong intrinsic attenuation. The plasmon dispersion and loss properties from plasmon profiles are experimentally determined, along the antennas, obtained using holographic near‐field nano‐imaging in a wide range of THz frequencies, from 2.05 to 4.3 THz. The detailed investigation of the unveiled DPP properties can guide the design of novel topological quantum devices exploiting their directional propagation.

Chemistry↗

DOE OSTI2019

A GaAs-based plasmonic source employing a nanoscale vertical cavity

In this paper, a new structure of a vertical cavity plasmonic source is presented. The structure, which is adopted from a metal–semiconductor–metal plasmonic photodetector, contains a gold substrate, n-type GaAs layer, active GaAs layer and p-type GaAs layer, respectively from bottom to up. A subwavelength aperture and metal gratings on both sides of the aperture are placed on the top of the device and act both as a gold clad and as the contact for applying DC bias. The metal gratings are improved by adding SiO{sub 2} between metal grooves and semiconductor. Applying voltage bias to p-and n-regions leads to photons generation in the active region. The generated photons in the active region excite a resonant surface plasmonic mode in the nanoscale cavity just below the aperture. One can use light outflowing from the nanoscale aperture, with wavelength of 882 nm, as a source to excite an arbitrary plasmonic guiding structure. The output beam has a suitable concentration so that in a 1000 nm distance from the aperture, still 37% of the power is concentrated in a width of 50 nm which is almost a unique specification among plasmonic sources, so far. The function of the device is validated using finite-difference time-domain numerical algorithm.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2013

Detecting Plasmon Resonance Energy Transfer with Differential Interference Contrast Microscopy

Gold nanoparticles are ideal probes for studying intracellular environments and energy transfer mechanisms due to their plasmonic properties. Plasmon resonance energy transfer (PRET) relies on a plasmonic nanoparticle to donate energy to a nearby resonant acceptor molecule, a process which can be observed due to the plasmonic quenching of the donor nanoparticle. In this study, a gold nanosphere was used as the plasmonic donor, while the metalloprotein cytochrome c was used as the acceptor molecule. Differential interference contrast (DIC) microscopy allows for simultaneous monitoring of complex environments and noble metal nanoparticles in real time. Using DIC and specially designed microfluidic channels, we were able to monitor PRET at the single gold particle level and observe the reversibility of PRET upon the introduction of phosphate-buffered saline to the channel. In an additional experiment, single gold particles were internalized by HeLa cells and were subsequently observed undergoing PRET as the cell hosts underwent morphological changes brought about by ethanol-induced apoptosis.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Plasmon-enhanced electron injection in dye-sensitized solar cells

Recent experiments have shown that the efficiency of photoinduced electron transfer from sensitizers (molecules or quantum dots) to semiconductors can be enhanced by coupling the sensitizers to plasmon resonances in metal nanoparticles. Here, we use a model Hamiltonian approach to show theoretically that there is an optimal coupling be- tween the sensitizer and plasmons that maximizes the electron-transfer efficiency. This optimum results from the competition between electron transfer, plasmon relaxation and plasmon decoherence. For coupling values that exceed the optimal value, the dy- namics of electron transfer from the sensitizer to the semiconductor can be significantly modified due to the sensitizer-plasmon coupling.

Ramakrishna, S.↗

DOE OSTI2015

Examining Substrate-Induced Plasmon Mode Splitting and Localization in Truncated Silver Nanospheres with Electron Energy Loss Spectroscopy

In this paper, motivated by the need to study the size dependence of nanoparticle–substrate systems, we present a combined experimental and theoretical electron energy loss spectroscopy (EELS) study of the plasmonic spectrum of substrate-supported truncated silver nanospheres. This work spans the entire classical range of plasmonic behavior probing particles of 20–1000 nm in diameter, allowing us to map the evolution of localized surface plasmons into surface plasmon polaritons and study the size dependence of substrate-induced mode splitting. Finally, this work constitutes the first nanoscopic characterization and imaging of these effects in truncated nanospheres, setting the stage for the systematic study of plasmon-mediated energy transfer in nanoparticle–substrate systems.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Quantitative Reflection Imaging for the Morphology and Dynamics of Live Aplysia californica Pedal Ganglion Neurons Cultured on Nanostructured Plasmonic Crystals

We describe a reflection imaging system that consists of a plasmonic crystal, a common laboratory microscope, and band-pass filters for use in the quantitative imaging and in situ monitoring of live cells and their substrate interactions. Surface plasmon resonance (SPR) provides a highly sensitive method to monitor changes in physicochemical properties occurring at metal-dielectric interfaces. Polyelectrolyte thin films deposited using the layer-by-layer (LBL) self-assembly method provide a reference system for calibrating the reflection contrast changes that occur when the polyelectrolyte film thickness changes and provide insight into the optical responses that originate from the multiple plasmonic features supported by this imaging system. Finitedifference time-domain (FDTD) simulations of the optical responses measured experimentally from the polyelectrolyte reference system are used to provide a calibration of the optical system for subsequent use in quantitative studies investigating live cell dynamics in cultures supported on a plasmonic crystal substrate. Live Aplysia californica pedal ganglion neurons cultured in artificial seawater were used as a model system through which to explore the utility of this plasmonic imaging technique. Here, the morphology of cellular peripheral structures ≲80 nm in thickness were quantitatively analyzed, and the dynamics of their trypsin-induced surface detachment were visualized. These results illustrate the capacities of this system for use in investigations of the dynamics of ultrathin cellular structures within complex bioanalytical environments.

47 OTHER INSTRUMENTATION↗

DOE OSTI2017

Low-Loss Plasmonic Dielectric Nanoresonators

Material losses in metals are a central bottleneck in plasmonics for many applications. We propose and theoretically demonstrate that metal losses can be successfully mitigated with dielectric particles on metallic films, giving rise to hybrid dielectric–metal resonances. In the far field, they yield strong and efficient scattering, beyond even the theoretical limits of all-metal and all-dielectric structures. In the near field, they offer high Purcell factor (>5000), high quantum efficiency (>90%), and highly directional emission at visible and infrared wavelengths. Their quality factors can be readily tailored from plasmonic-like (~10) to dielectric-like (~10 3 ), with wide control over the individual resonant coupling to photon, plasmon, and dissipative channels. Compared with conventional plasmonic nanostructures, such resonances show robustness against detrimental nonlocal effects and provide higher field enhancement at extreme nanoscopic sizes and spacings. These hybrid resonances equip plasmonics with high efficiency, which has been the predominant goal since the field’s inception.

77 NANOSCIENCE AND NANOTECHNOLOGY↗