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At least 91 records · Page 5

High-speed fiber-coupled terahertz time-domain spectroscopy system using a bias-free plasmonic source

We demonstrate a high-speed fiber-coupled terahertz time-domain spectroscopy (THz-TDS) system using a bias-free plasmonic terahertz source. The system is powered by a compact, low-power femtosecond fiber laser oscillator that drives a dual-branch fiber amplifier to pump and probe a plasmonic terahertz source and detector, respectively. A polarization-maintaining, fiber-coupled optical delay line is employed to precisely control the temporal offset between the pump and probe beams through a compact, robust platform. Operating in the self-similar amplification regime, the fiber amplifiers are engineered to mitigate nonlinear pulse distortion and dispersion while delivering robust, high-energy pulses at a 1560-nm wavelength, with an output power exceeding 326 mW. In reflection mode, the THz-TDS system achieves a peak dynamic range of 81 dB and a bandwidth greater than 3.5 THz at a scan rate of 3.75 Hz. The utility of the system for rapid sensing is further demonstrated by quantifying the porosity and density of pharmaceutical tablets through measurements of their physical thickness and effective refractive index.

Jiang, Xinghe [University of California, Los Angel↗

Gate-tunable plasmons in mixed-dimensional van der Waals heterostructures

Abstract Surface plasmons, collective electromagnetic excitations coupled to conduction electron oscillations, enable the manipulation of light–matter interactions at the nanoscale. Plasmon dispersion of metallic structures depends sensitively on their dimensionality and has been intensively studied for fundamental physics as well as applied technologies. Here, we report possible evidence for gate-tunable hybrid plasmons from the dimensionally mixed coupling between one-dimensional (1D) carbon nanotubes and two-dimensional (2D) graphene. In contrast to the carrier density-independent 1D Luttinger liquid plasmons in bare metallic carbon nanotubes, plasmon wavelengths in the 1D-2D heterostructure are modulated by 75% via electrostatic gating while retaining the high figures of merit of 1D plasmons. We propose a theoretical model to describe the electromagnetic interaction between plasmons in nanotubes and graphene, suggesting plasmon hybridization as a possible origin for the observed large plasmon modulation. The mixed-dimensional plasmonic heterostructures may enable diverse designs of tunable plasmonic nanodevices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Highly luminescent ultra-thin films with rare earth for plasmonic applications

Amphiphilic complexes with luminescent rare earth metal ions suitable for Lanmuir-Blodgett (LB) deposition have been synthesized. LB monolayers with closely packed Eu complexes deposited directly on silver demonstrate significant far-field emission in contrast to the theoretical predictions of full quenching. Angular radiation and polarization patterns of the electric and magnetic dipole emission of Eu 3+ point to a high excitation efficiency of surface plasmon polaritons. Different luminescent behavior of closely packed emitters in comparison to diluted systems is tentatively attributed to the collective state of emitters in LB layers formed via near-field coupling with surface plasmons.

Munga, J.↗

Entangled two-plasmon generation in carbon nanotubes and graphene-coated wires

Here, we investigate the two-plasmon spontaneous decay of a quantum emitter near single-walled carbon nanotubes (SWCNTs) and graphene-coated wires (GCWs). We demonstrate efficient, enhanced generation of two-plasmon entangled states in SWCNTs due to the strong coupling between tunable guided plasmons and the quantum emitter. We predict two-plasmon emission rates more than twelve orders of magnitude higher than in free space, with average lifetimes of a few dozen nanoseconds. Given their low dimensionality, these systems could be more efficient for generating and detecting entangled plasmons in comparison to extended graphene. Indeed, we achieve a tunable spectrum of emission in GCWs, where sharp resonances occur precisely at the plasmons' minimum excitation frequencies. We show that by changing the material properties of the GCW's dielectric core, one could tailor the dominant modes and frequencies of the emitted entangled plasmons while keeping the decay rate ten orders of magnitude higher than in free space. By unveiling the unique properties of two-plasmon spontaneous emission processes in the presence of low-dimensional carbon-based nanomaterials, our findings set the basis for a novel material platform with applications to on-chip quantum information technologies.

36 MATERIALS SCIENCE↗

Investigation of plasmon relaxation mechanisms using nonadiabatic molecular dynamics

Hot carriers generated from the decay of plasmon excitation can be harvested to drive a wide range of physical or chemical processes. However, their generation efficiency is limited by the concomitant phonon-induced relaxation processes by which the energy in excited carriers is transformed into heat. However, simulations of dynamics of nanoscale clusters are challenging due to the computational complexity involved. Here, in this paper, we adopt our newly developed Trajectory Surface Hopping (TSH) nonadiabatic molecular dynamics algorithm to simulate plasmon relaxation in Au 20 clusters, taking the atomistic details into account. The electronic properties are treated within the Linear Response Time-Dependent Tight-binding Density Functional Theory (LR-TDDFTB) framework. The relaxation of plasmon due to coupling to phonon modes in Au 20 beyond the Born–Oppenheimer approximation is described by the TSH algorithm. The numerically efficient LR-TDDFTB method allows us to address a dense manifold of excited states to ensure the inclusion of plasmon excitation. Starting from the photoexcited plasmon states in Au 20 cluster, we find that the time constant for relaxation from plasmon excited states to the lowest excited states is about 2.7 ps, mainly resulting from a stepwise decay process caused by low-frequency phonons of the Au 20 cluster. Furthermore, our simulations show that the lifetime of the phonon-induced plasmon dephasing process is ~10.4 fs and that such a swift process can be attributed to the strong nonadiabatic effect in small clusters. Our simulations demonstrate a detailed description of the dynamic processes in nanoclusters, including plasmon excitation, hot carrier generation from plasmon excitation dephasing, and the subsequent phonon-induced relaxation process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Collective Modes in Multilayer Graphene/𝛼−RuCl 3 Heterostructures

Collective modes in multilayer graphene, such as plasmons and phonons, exhibit sensitivity to displacement fields and interlayer coupling, distinguishing them from their counterparts in single-layer graphene. Here, we engineer collective modes in charge-transfer heterostructures composed of multilayer graphene and 𝛼−RuCl 3 . In heterostructures with a single 𝛼−RuCl 3 interface, the charge transfer generates displacement fields up to 7 V/nm at the interface between 𝛼−RuCl 3 and the adjacent graphene layer—the highest value achieved through charge-transfer methods. As a result of the broken inversion symmetry, we discover enhanced nonlinear optical response and modified phonon selection rules. Conversely, we find that multilayer graphene sandwiched between two 𝛼−RuCl 3 flakes causes displacement fields to cancel. There, we achieve carrier densities as high as 8 ×10 13 cm −2 in multilayer graphene and restore the phonon selection rules to their unperturbed state. Meanwhile, we demonstrate that plasmonic properties derive from the depletion of multiple valence bands. As a result of the quasilinear band dispersion, these “Dirac multiband plasmons” are relatively unaffected by displacement fields. On the other hand, the inverted heterostructure sequence—two multilayer graphene sheets encapsulating 𝛼−RuCl 3 —activates significant alteration of the plasmons via interlayer plasmon-plasmon coupling. Hence, multilayer graphene and 𝛼−RuCl 3 heterostructures offer a gate-free platform for engineering collective modes derived from inversion symmetry and interlayer coupling.

Moore, Samuel L. [Columbia University, New York, N↗

Broadband Asymmetric Transmission of Linearly Polarized Mid‐Infrared Light Based on Quasi‐3D Metamaterials

Abstract Metamaterials consisting of subwavelength resonators offer an exciting opportunity for realizing asymmetric transmission (AT) of linearly polarized light. However, to date, only moderate/narrow‐band AT responses have been obtained in metadevices based on stacked planar nanostructures. Here, leveraging a combination of a genetic algorithm (GA) based optimization method and a membrane projection lithography (MPL) fabrication approach, a quasi‐3D metamaterial for broadband AT of linearly polarized mid‐infrared light is demonstrated. Facilitated by the customized GA, an efficient exploration of 3D plasmonic meta‐atoms with broken mirror symmetry in the light propagation direction allows the satisfaction of the rigorous conditions for AT of linearly polarized waves over a broad wavelength range. Confirmed by surface current analysis, the observed AT behavior is attributed to the resonant coupling between the plasmonic nanostructures located on the two orthogonal walls of the MPL cavities. Incorporating an advanced inverse‐design method and a state‐of‐art fabrication technique, the methodology used in the present study provides a promising route for exploiting 3D metamaterials with sophisticated functionalities via effectively exploring the high‐dimensional parametric space offered by true 3D meta‐atoms.

Whiting, Eric B.↗

Electroluminescence and Plasmon-Assisted Directional Photoluminescence from 2D HgTe Nanoplatelets

In the visible range, 2D nanoplatelets (NPLs) have brought significant benefits compared to their 0D counterpart with an inherently anisotropic emission, a narrower photoluminescence (PL) signal, and new degrees of freedom to design heterostructures. Compared to the properties of cadmium chalcogenide NPLs in the visible, similar research is still mostly lacking in the infrared, in spite of existing synthetic paths to obtain narrow band gap semiconductors in 2D colloidal form. Here, in this paper, we focus on 2D HgTe NPLs and show how their PL can be stabilized through the proper choice of surface chemistry. We then demonstrate two important steps toward bright infrared light emitting diodes (LEDs) which are (i) the coupling to a plasmonic grating to control the magnitude and spatial direction of the PL signal and (ii) the observation of electroluminescence at 1300 nm, which is near telecom wavelength.

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↗

Slow light in a 2D semiconductor plasmonic structure

Spectrally narrow optical resonances can be used to generate slow light, i.e., a large reduction in the group velocity. In a previous work, we developed hybrid 2D semiconductor plasmonic structures, which consist of propagating optical frequency surface-plasmon polaritons interacting with excitons in a semiconductor monolayer. Here, we use coupled exciton-surface plasmon polaritons (E-SPPs) in monolayer WSe 2 to demonstrate slow light with a 1300 fold decrease of the SPP group velocity. Specifically, we use a high resolution two-color laser technique where the nonlinear E-SPP response gives rise to ultra-narrow coherent population oscillation (CPO) resonances, resulting in a group velocity on order of 105 m/s. Our work paves the way toward on-chip actively switched delay lines and optical buffers that utilize 2D semiconductors as active elements.

42 ENGINEERING↗

Frontier nonequilibrium materials science enabled by ultrafast electron methods

Most innovation in materials science and engineering resides in our ability to understand and control the intimate relationship between the structure of materials and their properties. Conventionally, the only route to discovering innovative new material properties has been to explore the structural and compositional phase space that is accessible at (or near) thermodynamic equilibrium. The characterization, manipulation and, ultimately, control of material properties far from equilibrium offers almost completely untapped possibilities for uncovering novel states and phases of materials. Investigations of materials far from equilibrium require the development of new techniques, which are capable of following dynamic processes in materials with extreme spatiotemporal resolution. Thus, ultrafast electron-based methods have become a major new frontier in materials science due to the capability of following dynamics on time scales as short as femtoseconds with the high spatial resolution and sensitivity afforded by electrons. The articles in this issue provide an exciting cross section of the novel research directions that have been enabled at this frontier. Imaging on ultrafast time scales carries critical information on phase transitions, fundamental processes involved in light-harvesting, magnetic, and plasmonic dynamics, the coupling of electronic and nuclear degrees of freedom in materials and has revealed previously hidden, nonequilibrium metastable states of matter that have no equilibrium analog.

36 MATERIALS SCIENCE↗

Tunable phase-change metasurfaces coupled with mid-infrared molecular vibrations

Chiral optical metasurfaces have emerged as a promising platform in coupling with molecular vibrational fingerprints through the enhanced light-matter interaction under different circularly polarized light illumination. Here, this work reports the mode coupling between the mid-infrared phonon vibrations of polymethyl methacrylate (PMMA) molecules and the thermally tunable chiral metasurfaces based on the phase-change material Ge₂Sb₂Te₅ (GST-225). Phase-change chiral metasurfaces with high circular dichroism (CD) in absorption and tunable plasmonic resonance in the frequency range of 48–56 THz are demonstrated, which covers the phonon vibrational frequency of PMMA molecules at 52 THz. The mode splitting features are observed in the absorption and CD spectra when the metasurface resonance is tuned across the phonon vibrational frequency of PMMA molecules during the phase transition of GST-225. The underlying mechanism of molecule-metasurface coupling is further revealed by studying the electric field and power loss density distributions of the phonon–plasmon coupled modes under both left-handed and right-handed circularly polarized (LCP and RCP) light. The demonstrated results show the potential of dynamically tunable chiral metasurfaces for the applications in label-free molecular sensing, biomedical diagnostics, thermal imaging, and mid-infrared photonics.

Tang, Haotian [Missouri Univ. of Science and Techn↗

Orientation Sensitive SEIRA Sensors Based on Single-Walled Carbon Nanotube Near Fields

Molecular vibrations that bear information about intrinsic properties of chemical compounds are challenging to detect at submonolayer densities. Surface-enhanced infrared absorption (SEIRA) spectroscopy has been proven to be a viable approach to enhance and detect weak vibration signals. Here, in this study, we report a SEIRA sensor based on mid-infrared surface plasmon resonances supported by single-walled carbon nanotubes (SWCNTs). Due to the 1D nature of SWCNTs, their plasmon modes are highly polarized with the electromagnetic fields spatially confined to nanometer scales. Leveraging these characteristics of SWCNTs, we observe a polarization selective coupling between their surface plasmons and vibrational modes of chemical bonds introduced onto their surfaces. A maximum modulation of similar to 15% to the plasmon resonance peak is obtained for a submonolayer chemical group coverage. These findings suggest that SWCNTs may potentially serve as a highly sensitive SEIRA platform for revealing intricate information about molecular compositions and bond orientations.

36 MATERIALS SCIENCE↗

Plasmonic Core–Shell–Satellites with Abundant Electromagnetic Hotspots for Highly Sensitive and Reproducible SERS Detection

In this work, we develop a Ag@Al2O3@Ag plasmonic core–shell–satellite (PCSS) to achieve highly sensitive and reproducible surface-enhanced Raman spectroscopy (SERS) detection of probe molecules. To fabricate PCSS nanostructures, we employ a simple hierarchical dewetting process of Ag films coupled with an atomic layer deposition (ALD) method for the Al2O3 shell. Compared to bare Ag nanoparticles, several advantages of fabricating PCSS nanostructures are discovered, including high surface roughness, high density of nanogaps between Ag core and Ag satellites, and nanogaps between adjacent Ag satellites. Finite-difference time-domain (FDTD) simulations of the PCSS nanostructure confirm an enhancement in the electromagnetic field intensity (hotspots) in the nanogap between the Ag core and the satellite generated by the Al2O3 shell, due to the strong core–satellite plasmonic coupling. The as-prepared PCSS-based SERS substrate demonstrates an enhancement factor (EF) of 1.7 × 107 and relative standard deviation (RSD) of ~7%, endowing our SERS platform with highly sensitive and reproducible detection of R6G molecules. We think that this method provides a simple approach for the fabrication of PCSS by a solid-state technique and a basis for developing a highly SERS-active substrate for practical applications.

47 OTHER INSTRUMENTATION↗

Near-field probing of strong light-matter coupling in single IR antennae

Quantum well intersubband polaritons are traditionally studied in large scale ensembles, over many wavelengths in size.In this presentation, we demonstrate that it is possible to detect and investigate intersubband polaritons in a single sub-wavelength nanoantenna in the IR frequency range. We observe polariton formation using a scattering-type near-fieldmicroscope and nano-FTIR spectroscopy. In this work, we will discuss near-field spectroscopic signatures of plasmonic antennae withand without coupling to the intersubband transition in quantum wells located underneath the antenna. Evanescent fieldamplitude spectra recorded on the antenna surface show a mode anti-crossing behavior in the strong coupling case. Wealso observe a corresponding strong-coupling signature in the phase of the detected field. We anticipate that this near-fieldapproach will enable explorations of strong and ultrastrong light-matter coupling in the single nanoantenna regime,including investigations of the elusive effect of ISB polariton condensation.

36 MATERIALS SCIENCE↗

Second-harmonic generation in nonlinear plasmonic lattices enhanced by quantum emitter gain medium

In this work, we report on a theoretical study of second-harmonic generation (SHG) in plasmonic nanostructures interacting with two-level quantum emitters (QEs) under incoherent energy pump. We generalize the driven-dissipative Tavis–Cummings model by introducing the anharmonic surface plasmon-polariton (SPP) mode coupled to QEs and examine physical properties of corresponding SPP-QE polariton states. Our calculations of the SHG efficiency for strong QE-SPP coupling demonstrate orders of magnitude enhancement facilitated by the polariton gain. We further discuss time-domain numerical simulations of SHG in a square lattice comprising Ag nanopillars coupled to QEs utilizing a fully vectorial nonperturbative nonlinear hydrodynamic model for conduction electrons coupled to Maxwell–Bloch equations for QEs. The simulations support the idea of gain enhanced SHG and show orders of magnitude increase in the SHG efficiency as the QEs are tuned in resonance with the lattice plasmon mode and brought above the population inversion threshold by incoherent pumping. By varying pump frequency and tuning QEs to a localized plasmon mode, we demonstrate further enhancement of the SHG efficiency facilitated by strong local electric fields. The incident light polarization dependence of the SHG is examined and related to the symmetries of participating plasmon modes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Morphology and property tuning in ZnO–Ni hybrid metamaterials in vertically aligned nanocomposite (VAN) form

ZnO thin films have attracted significant interest in the past decades owing to their unique wide band gap properties, piezoelectric properties, non-linearity and plasmonic properties. Recent efforts have been made in coupling ZnO with secondary phases to enhance its functionalities, such as Au–ZnO nanocomposite thin films with tunable optical and plasmonic properties. In this work, magnetic nanostructures of Ni are incorporated in ZnO thin films in a vertically aligned nanocomposite (VAN) form to couple magnetic and plasmonic response in a complex hybrid metamaterial system. Nickel (Ni) is of interest due to its ferromagnetic and plasmonic properties along with gold (Au) which is also plasmonic. Therefore, two approaches, namely, tuning of the deposition pressure and use of a ZnO–Au seeding layer have been attempted to achieve unique Ni nanostructures in addition to tuning of the microstructure. Together, both approaches demonstrate a range of microstructures such as core–shell, nanodisk, nanocup, and nanocube-like morphologies not previously attempted. Additionally, there is effective tuning of properties. Specifically, the seeding layer thickness causes hyperbolic behavior as well as redshift in the surface plasmon resonance (SPR) wavelength. The addition of the ZnO–Au seeding layer directly influences the optical properties. Plus, regardless of the different approaches, the films demonstrate magnetic anisotropy based on the composition and microstructure of the film which impacted the saturation magnetization and coercivity. This study demonstrates the potential of ZnO-based complex hybrid metamaterials with coupled electro-magneto-optical properties for integrated photonic devices.

Bhatt, Nirali A. [Purdue Univ., West Lafayette, IN↗