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At least 55 records · Page 3

Near-field radiative heat transfer between irregularly shaped dielectric particles modeled with the discrete system Green's function method

Near-field radiative heat transfer (NFRHT) between irregularly shaped dielectric particles made of SiO 2 and morphology characterized by Gaussian random spheres is studied. Particles are modeled using the discrete system Green's function (DSGF) approach, which is a volume integral numerical method based on fluctuational electrodynamics. This method is applicable to finite, three-dimensional objects, and all system interactions are defined independent of thermal excitation by a generalized system Green's function. The DSGF method is deemed suitable to model NFRHT between irregularly shaped particles after verification against the analytical solution for chains of two and three SiO 2 spheres. The NFRHT results reveal that geometric irregularity in particles leads to a reduction of the total conductance from that of comparable perfect spheres at vacuum separation distances smaller than the particle size, a regime in which NFRHT is a surface phenomenon. At vacuum separation distances larger than the particle size, NFRHT becomes a volumetric process, and the total conductance between irregularly shaped particles converges to that of comparable perfect spheres. Spectral analysis reveals, however, that particle irregularity leads to damping and broadening of resonances at all separation distances, thereby highlighting the importance of the DSGF method for spectral engineering in the near field. The reduced spectral coherence when particle size is larger than the vacuum separation distance is attributed to coupling of surface phonon-polaritons within the randomly generated, distorted particle features. For particle size smaller than the vacuum separation distance, resonance broadening and damping are linked with the multiple localized surface phonon modes supported by the composite spherical harmonic morphologies of the Gaussian random spheres. In conclusion, this paper has direct implications for thermal management of packed particle systems, with applications in radiative property control, electronics, energy conversion, and nanomanufacturing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Unidirectional ray polaritons in twisted asymmetric stacks

Abstract The vast repository of van der Waals (vdW) materials supporting polaritons offers numerous possibilities to tailor electromagnetic waves at the nanoscale. The development of twistoptics—the modulation of the optical properties by twisting stacks of vdW materials—enables directional propagation of phonon polaritons (PhPs) along a single spatial direction, known as canalization. Here we demonstrate a complementary type of directional propagation of polaritons by reporting the visualization of unidirectional ray polaritons (URPs). They arise naturally in twisted hyperbolic stacks with very different thicknesses of their constituents, demonstrated for homostructures of$$\alpha$$ α -MoO 3 and heterostructures of$$\alpha$$ α -MoO 3 and$$\beta$$ β -Ga 2 O 3 . Importantly, their ray-like propagation, characterized by large momenta and constant phase, is tunable by both the twist angle and the illumination frequency. Apart from their fundamental importance, our findings introduce twisted asymmetric stacks as efficient platforms for nanoscale directional polariton propagation, opening the door for applications in nanoimaging, (bio)-sensing, or polaritonic thermal management.

Science & Technology - Other Topics↗

Interfacial Strong Coupling and Negative Dispersion of Propagating Polaritons in Freestanding Oxide Membranes

Membranes of complex oxides like perovskite SrTiO3 extend the multi-functional promise of oxide electronics into the nanoscale regime of 2D materials. Here, it is demonstrated that freestanding oxide membranes supply a reconfigurable platform for nano-photonics based on propagating surface phonon polaritons. Infrared near-field imaging and spectroscopy enabled by a tunable ultrafast laser are applied to study pristine nano-thick SrTiO3 membranes prepared by hybrid molecular beam epitaxy. As predicted by coupled mode theory, it is found that strong coupling of interfacial polaritons realizes symmetric and antisymmetric hybridized modes with simultaneously tunable negative and positive group velocities. By resolving reflection of these propagating modes from membrane edges, defects, and substrate structures, their dispersion is quantified with position-resolved nano-spectroscopy. Remarkably, polariton negative dispersion is found to be both robust and tunable through choice of membrane dielectric environment and thickness, and proposes a novel design for in-plane Veselago lensing harnessing this control. This work lays the foundation for tunable transformation optics at the nanoscale using polaritons in a wide range of freestanding complex oxide membranes.

freestanding oxide membranes↗

Phonon engineering of boron nitride via isotopic enrichment

Phonon polaritons (PhPs) enable a variety of applications, yet it requires PhPs supported in the desired frequency range. The two BN allotropes (cubic and hexagonal, cBN and hBN) are of particular interest, as their optic phonons fall within the so-called molecular-fingerprint region (~ 1000–1610 cm -1 ). However, there remains a spectral gap between PhPs covered by these two, limiting applications. Thus, we isotopically engineered hBN and cBN and examined the optic phonons. Furthermore, for hBN, enhancement of the optic phonon lifetimes and shifted frequencies are observed. However, lifetimes are observed to decrease with the enrichment of cBN by 10 B, 11 B, and 15 N. We propose that the reduced lifetimes are not due to intrinsic loss, but rather increased defect concentrations resulting from the modified growth, supported by first-principles calculations. Thus, reducing the extrinsic defects in isotopically engineered cBN may present a path toward overcoming these restrictions for applications in the molecular-fingerprint region.

36 MATERIALS SCIENCE↗

Ultrabroadband Spacetime Nanoscopy of Terahertz Polaritons in a van der Waals Cavity

Guiding, storing, and processing light at the nanoscale hinges on understanding how polaritons — hybrid quasiparticles of light and matter — propagate and interfere in both space and time. This work introduces a synchrotron-based technique, SYnchrotron SpaceTimE Mapping (SYSTEM), which captures real-time evolution of polariton wave packets with ∼10 nm spatial and sub-100 fs temporal resolution across an ultrabroadband 5–50 THz range. Here, SYSTEM directly visualizes the creation, interference, and decay of multiple high-quality Fabry-Pérot phonon polariton cavity modes in an α-MoO 3 microcavity. These real-space, real-time observations reveal wave-packet dynamics and cavity resonances with record-high quality factors (Q ≈ 100) in the single-digit terahertz regime near 9 THz. SYSTEM thus offers a powerful and broadly applicable platform for probing and engineering ultraslow, deeply subwavelength polaritons, opening new avenues for tailoring light–matter interactions and advancing next-generation THz nanophotonic technologies.

36 MATERIALS SCIENCE↗

Colossal Optical Anisotropy from Atomic-Scale Modulations

Materials with large birefringence (Δn, where n is the refractive index) are sought after for polarization control (e.g., in wave plates, polarizing beam splitters, etc.), nonlinear optics, micromanipulation, and as a platform for unconventional light–matter coupling, such as hyperbolic phonon polaritons. Layered 2D materials can feature some of the largest optical anisotropy; however, their use in most optical systems is limited because their optical axis is out of the plane of the layers and the layers are weakly attached. This work demonstrates that a bulk crystal with subtle periodic modulations in its structure—Sr 9/8 TiS 3 —is transparent and positive-uniaxial, with extraordinary index n e = 4.5 and ordinary index n o = 2.4 in the mid- to far-infrared. The excess Sr, compared to stoichiometric SrTiS 3 , results in the formation of TiS 6 trigonal-prismatic units that break the chains of face-sharing TiS 6 octahedra in SrTiS 3 into periodic blocks of five TiS 6 octahedral units. The additional electrons introduced by the excess Sr form highly oriented electron clouds, which selectively boost the extraordinary index n e and result in record birefringence (Δn > 2.1 with low loss). The connection between subtle structural modulations and large changes in refractive index suggests new categories of anisotropic materials and also tunable optical materials with large refractive-index modulation.

36 MATERIALS SCIENCE↗

Mid- to Far-Infrared Anisotropic Dielectric Function of HfS 2 and HfSe 2

The far-infrared (far-IR) remains a relatively underexplored region of the electromagnetic spectrum extending roughly from 20 to 100 µm in free-space wavelength. Research within this range has been restricted due to a lack of optical materials that can be optimized to reduce losses and increase sensitivity, as well as by the long free-space wavelengths associated with this spectral region. Here the exceptionally broad Reststrahlen bands of two Hf-based transition metal dichalcogenides (TMDs) that can support surface phonon polaritons (SPhPs) within the mid-infrared (mid-IR) into the terahertz (THz) are reported. In this vein, the IR transmission and reflectance spectra of hafnium disulfide (HfS 2 ) and hafnium diselenide (HfSe 2 ) flakes are measured and their corresponding dielectric functions are extracted. These exceptionally broad Reststrahlen bands (HfS 2 : 165 cm -1 ; HfSe 2 : 95 cm -1 ) dramatically exceed that of the more commonly explored molybdenum- (Mo) and tungsten- (W) based TMDs (≈5–10 cm -1 ), which results from the over sevenfold increase in the Born effective charge of the Hf-containing compounds. Further, this work therefore identifies a class of materials for nanophotonic and sensing applications in the mid- to far-IR, such as deeply sub-diffractional hyperbolic and polaritonic optical antennas, as is predicted via electromagnetic simulations using the extracted dielectric function.

36 MATERIALS SCIENCE↗

Temperature-dependent optical constants of vanadium dioxide thin films deposited on polar dielectrics

Coating polar dielectrics with thin film vanadium dioxide (VO 2 ) enables one to exploit the temperature-dependent phase transition within VO 2 to actively tune and modulate surface phonon polaritons at mid-infrared. However, controlling the behavior of such systems requires intimate knowledge of the temperature-dependent optical constants of VO 2 , which depend greatly on the growth conditions and substrate material. Here, in this work, we accurately determine the complex optical constants of VO 2 on polar dielectrics across the insulator-to-metal phase transition (IMT) using only normal incident reflectance spectra by analyzing the reflectance with Kramers–Kronig relations and thin film Fresnel equations. This non-ellipsometry technique offers an advantage in determining the refractive index using a standard infrared spectrometer.

36 MATERIALS SCIENCE↗

Two-dimensional talc as a natural abundant ultra-broadband hyperbolic material

Here, we demonstrate that two-dimensional talc, a naturally abundant phyllosilicate mineral, supports hyperbolic phonon-polaritons (HPhPs) across the mid- and far-infrared wavelengths. Using scattering scanning near-field optical microscopy (s-SNOM) and synchrotron infrared nano-spectroscopy (SINS), we reveal tunable HPhP modes in talc flakes with long lifetimes, high confinement, and quality factors of up to 5. We further observe Fabry–Pérot cavity modes in tapered flakes, confirmed by simulations and analytical modeling. Compared to synthetic crystals, talc offers an ultra-broadband, low-cost, and sustainable platform for infrared nanophotonics and optoelectronics.

36 MATERIALS SCIENCE↗

Near-field photonic thermal diode based on hBN and InSb films

A thermal diode is a two-terminal device that allows heat to transfer more easily in one direction (forward bias) than in the opposite direction (reverse bias). A photonic thermal diode operates in a contactless mode and may afford a large operating temperature range. Here, a near-field photonic thermal diode based on hexagonal boron nitride (hBN) and indium antimonide (InSb) films is theoretically demonstrated. In this work, the temperature dependence of the interband absorption of InSb is used to couple (or decouple) with the hyperbolic phonon polaritons in hBN. The numerical analysis predicts a rectification ratio greater than 17 for a 10 nm vacuum gap, when operating at an average temperature of 300 K and a temperature difference of 200 K. The calculated rectification ratio exceeds 35 at higher average temperatures with larger temperature differences.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Near-field spectroscopy of Dirac plasmons in Bi 2 Se 3 ribbon arrays

Plasmons supported in the massless electron surface states of topological insulators (TIs), known as Dirac plasmons, have great potential in next generation optoelectronics. However, their inherent confinement to the surface makes the investigation of Dirac plasmons challenging. Near-field techniques provide the ideal platform to directly probe Dirac plasmons due to the sensitivity to evanescent fields at the surface. Here, we demonstrate the use of aperture near-field spectroscopy for the investigation of localized terahertz (THz) Dirac plasmon resonances in Bi 2 Se 3 ribbon arrays with widths ranging from 10 to 40 µm. Unlike scattering THz near-field techniques, the aperture method is most sensitive to plasmons with the relevant lower-momenta corresponding to plasmon wavelengths on the scale of ~20 µm. The combination of THz time-domain spectroscopy and aperture near-field microscopy enables sampling of localized Dirac plasmons in the near-field zone in the 0.5–2.5 THz range. We map the plasmon dispersion, which reveals a coupled plasmon–phonon polariton interaction. The near-field spectra show a higher contrast of the upper polariton branch in comparison with far-field observations. The information revealed by aperture near-field spectroscopy could deepen our understanding of the behavior of Dirac plasmons, leading to the potential development of real-world TI devices.

42 ENGINEERING↗

Superconducting coherence peak in near-field radiative heat transfer

Enhancement and peaks in near-field radiative heat transfer (NFRHT) typically arise due to surface phonon-polaritons, plasmon-polaritons, and electromagnetic (EM) modes in structured materials. However, the role of material quantum coherence in enhancing near-field radiative heat transfer remains unexplored. Here, we unravel that NFRHT in superconductor-ferromagnetic systems displays a unique peak at the superconducting phase transition that originates from the quantum coherence of Bogoliubov quasiparticles in superconductors. Our theory takes into account evanescent EM radiation emanating from fluctuating currents related to Cooper pairs and Bogoliubov quasiparticles in stark contrast to the current-current correlations induced by free electrons in conventional materials. Our proposed NFRHT configuration exploits ferromagnetic resonance at frequencies deep inside the superconducting band gap to isolate this superconducting coherence peak. Furthermore, we reveal that Cooper pairs and Bogoliubov quasiparticles have opposite effects on near-field thermal radiation and isolate their effects on many-body radiative heat transfer near superconductors. As a result, our proposed phenomenon can have applications for developing thermal isolators and heat sinks in superconducting circuits.

Dipole approximation↗

Ultrafast dynamics of a fermion chain in a terahertz field-driven optical cavity

In this article, we study the effect of a terahertz field-driven single cavity mode for ultrafast control of a fermion chain with dissipation-induced nonlinearity and quadratic coupling to an infrared-active phonon mode. Unlike the first-order phase transition in the nonequilibrium steady state of the system without a cavity or with a high-quality cavity, we find that a realistic dissipation in a low-quality driven cavity process prevents such a transition. Without realistic photon loss from the cavity, the transition only survives for the lower phonon-polariton branch with strong drive; a weak laser field fails to induce the phase transition and renders the polaritons symmetrical. The ability to control the phase transition is crucial for realizing strongly modulated steady states; we propose experimentally feasible regimes where this occurs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Plasmon coupling in topological insulator multilayers

Topological insulators (TIs) house two-dimensional Dirac plasmons on their surfaces. In TI thin films, plasmons on the top and bottom surfaces couple electrostatically, giving rise to an acoustic and an optical plasmon mode. By extension, a superlattice comprising TI layers and trivially-insulating layers could house multiple complex plasmon modes which could be used to create a new type of Dirac metamaterial. In this paper, we synthesize TI superlattices, fabricate them into stripe arrays, characterize their optical and plasmonic properties, and model the samples using transfer matrices. Furthermore, we excite plasmon modes that couple to the phonons in the superlattice, resulting in hybrid plasmon phonon polaritons. These modes are modeled using an analytical Fano resonance model and the extracted resonant positions are reproduced by transfer matrix modeling. We also excite an epsilon-near-zero mode in the top dielectric material (Bi 0.5 In 0.5 ) 2 Se 3 . Understanding the behavior of the polariton modes in this complex system will lend insight into the many-body interaction in low-dimensional systems.

36 MATERIALS SCIENCE↗

Negative refraction in hyperbolic hetero-bicrystals

We visualized negative refraction of phonon polaritons, which occurs at the interface between two natural crystals. The polaritons—hybrids of infrared photons and lattice vibrations—form collimated rays that display negative refraction when passing through a planar interface between the two hyperbolic van der Waals materials: molybdenum oxide (MoO 3 ) and isotopically pure hexagonal boron nitride (h 11 BN). At a special frequency ω 0 , these rays can circulate along closed diamond-shaped trajectories. We have shown that polariton eigenmodes display regions of both positive and negative dispersion interrupted by multiple gaps that result from polaritonic-level repulsion and strong coupling.

Science & Technology - Other Topics↗

Electronic and Vibrational Spectra of InP Quantum Dots Formed by Sequential Ion Implantation

We have performed sequential ion implantation of indium and phosphorus into silica combined with controlled thermal annealing to fabricate InP quantum dots in a dielectric host. Electronic and vibrational spectra were measured for the as-implanted and annealed samples. The annealed samples show a peak in the infrared spectra near 320/cm which is attributed to a surface phonon mode and is in good agreement with the value calculated from Frolich's theory of surface phonon polaritons. The electronic spectra show the development of a band near 390 nm that is attributed to quantum confined InP.

Hall, C.↗

Optical and Atomic Force Microscopy Characterization of PbI2 Quantum Dots

Lead iodide (PbI2) clusters were synthesized from the chemical reaction of NaI (or KI) with Pb(NO3)2 in H2O, D2O, CH3OH, and C3H7OH media. The observation of the absorption features above 350 nm with the help of integrating sphere accessory strongly suggests the quantum dot formation of PbI2 in solution. Spectral comparison between the synthesized PbI2 clusters in solution and PbI2 nanophase by impregnation of PbI2 in four different pore-sized porous silica indicates that the PbI2 cluster size in solution is less than 2.5 nm in lateral dimension. Atomic force microscopy (AFM) measurements show that the PbL clusters deposited onto three different molecularly flat surfaces are single-layered. The measured height is 1.0 - 0.1 nm. The swollen layer thickness can be attributed to the intralayer contraction from the strong lateral interaction among PbI2 molecules, which is supported by ab initio calculation. Raman scattering measurement of LO and TO modes of PbI2 in bulk and in the confined state were also conducted in 50-150 cu cm region. The observed three bands at 74, %, 106 1/cm are assigned to TO2, LO2, and LO, mode, respectively. The relatively small red-shift in LO modes may be caused by the surface phonon polaritons of PbI2 nanophase in the porous silica.

Mu, R.↗