Hyperbolic exciton polaritons in a van der Waals magnet.

Exciton polaritons are quasiparticles of photons coupled strongly to bound electron-hole pairs, manifesting as an anti-crossing light dispersion near an exciton resonance. Highly anisotropic semiconductors with opposite-signed permittivities along different crystal axes are predicted to host exotic modes inside the anti-crossing called hyperbolic exciton polaritons (HEPs), which confine light subdiffractionally with enhanced density of states. Here, we show observational evidence of steady-state HEPs in the van der Waals magnet chromium sulfide bromide (CrSBr) using a cryogenic near-infrared near-field microscope. At low temperatures, in the magnetically-ordered state, anisotropic exciton resonances sharpen, driving the permittivity negative along one crystal axis and enabling HEP propagation. We characterize HEP momentum and losses in CrSBr, also demonstrating coupling to excitonic sidebands and enhancement by magnetic order: which boosts exciton spectral weight via wavefunction delocalization. Our findings open new pathways to nanoscale manipulation of excitons and light, including routes to magnetic, nonlocal, and quantum polaritonics.

Observation of Highly Anisotropic Thermal Expansion of Polymer Films.

While dimensional change under thermal loading dictates various device failure mechanisms in soft materials, the interplay between microstructures and thermal expansion remains underexplored. Here, we develop a novel method to directly probe the thermal expansion for nanoscale polymer films using an atomic force microscope as well as confining active thermal volume. In a model system, spin-coated poly(methyl methacrylate), we find that the in-plane thermal expansion is enhanced by 20-fold compared to that along the out-of-plane directions in confined dimensions. Our molecular dynamics simulations show that the collective motion of side groups along backbone chains uniquely drives the enhancement of thermal expansion anisotropy of polymers in the nanoscale limit. This work unveils the intimate role of the microstructure of polymer films on its thermal-mechanical interaction, paving a route to judiciously enhance the reliability in a broad range of thin-film devices.

Ambipolar charge-transfer graphene plasmonic cavities.

Plasmon polaritons in van der Waals materials hold promise for various photonics applications1-4. The deterministic imprinting of spatial patterns of high carrier density in plasmonic cavities and nanoscale circuitry can enable the realization of advanced nonlinear nanophotonic5 and strong light-matter interaction platforms6. Here we demonstrate an oxidation-activated charge transfer strategy to program ambipolar low-loss graphene plasmonic structures. By covering graphene with transition-metal dichalcogenides and subsequently oxidizing the transition-metal dichalcogenides into transition-metal oxides, we activate charge transfer rooted in the dissimilar work functions between transition-metal oxides and graphene. Nano-infrared imaging reveals ambipolar low-loss plasmon polaritons at the transition-metal-oxide/graphene interfaces. Further, by inserting dielectric van der Waals spacers, we can precisely control the electron and hole densities induced by oxidation-activated charge transfer and achieve plasmons with a near-intrinsic quality factor. Using this strategy, we imprint plasmonic cavities with laterally abrupt doping profiles with nanoscale precision and demonstrate plasmonic whispering-gallery resonators based on suspended graphene encapsulated in transition-metal oxides.

Infrared plasmons propagate through a hyperbolic nodal metal.

Metals are canonical plasmonic media at infrared and optical wavelengths, allowing one to guide and manipulate light at the nanoscale. A special form of optical waveguiding is afforded by highly anisotropic crystals revealing the opposite signs of the dielectric functions along orthogonal directions. These media are classified as hyperbolic and include crystalline insulators, semiconductors, and artificial metamaterials. Layered anisotropic metals are also anticipated to support hyperbolic waveguiding. However, this behavior remains elusive, primarily because interband losses arrest the propagation of infrared modes. Here, we report on the observation of propagating hyperbolic waves in a prototypical layered nodal-line semimetal ZrSiSe. The observed waveguiding originates from polaritonic hybridization between near-infrared light and nodal-line plasmons. Unique nodal electronic structures simultaneously suppress interband loss and boost the plasmonic response, ultimately enabling the propagation of infrared modes through the bulk of the crystal.

Surface plasmons induce topological transition in graphene/α-MoO3 heterostructures.

Polaritons in hyperbolic van der Waals materials-where principal axes have permittivities of opposite signs-are light-matter modes with unique properties and promising applications. Isofrequency contours of hyperbolic polaritons may undergo topological transitions from open hyperbolas to closed ellipse-like curves, prompting an abrupt change in physical properties. Electronically-tunable topological transitions are especially desirable for future integrated technologies but have yet to be demonstrated. In this work, we present a doping-induced topological transition effected by plasmon-phonon hybridization in graphene/α-MoO3 heterostructures. Scanning near-field optical microscopy was used to image hybrid polaritons in graphene/α-MoO3. We demonstrate the topological transition and characterize hybrid modes, which can be tuned from surface waves to bulk waveguide modes, traversing an exceptional point arising from the anisotropic plasmon-phonon coupling. Graphene/α-MoO3 heterostructures offer the possibility to explore dynamical topological transitions and directional coupling that could inspire new nanophotonic and quantum devices.

Skin-Inspired Thermometer Enabling Contact-Independent Temperature Sensation via a Seebeck-Resistive Bimodal System.

Tactile sensation is a powerful method for probing the temperature of an arbitrary object due to its intuitive operating mechanism. However, the disruptive interface commonly formed between the thermometer and the object gives rise to thermal contact resistance, which is the primary source of measurement inaccuracy. Here, we develop a bioinspired bimodal temperature sensor exhibiting robust measurement accuracy by precisely decoupling contact resistance from the associated thermal circuit. In our sensors, a micropatterned resistive thermometer is placed underneath a thermoelectric heat fluxmeter, which resembles thermoreceptors located in human biomembranes. The object temperature is probed by modulating the thermometer temperature within the sensor system and precisely extrapolating the zero-heat flux point of the Seebeck voltage developed across the fluxmeter. At this zero-heat flux point, the object and thermometer temperatures coincide with each other regardless of the contact resistance formed at the fluxmeter-object interface. An experimental study shows that our sensors display excellent measurement accuracy within ∼0.5 K over a wide range of contact resistance values. Our work opens up new avenues for highly sensitive tactile thermal sensation in thermal haptics, medical devices, and robotics if combined with flexible devices.

Hyperbolic Cooper-Pair Polaritons in Planar Graphene/Cuprate Plasmonic Cavities.

Hyperbolic Cooper-pair polaritons (HCP) in cuprate superconductors are of fundamental interest due to their potential for providing insights into the nature of unconventional superconductivity. Here, we critically assess an experimental approach using near-field imaging to probe HCP in Bi2Sr2CaCu2O8+x (Bi-2212) in the presence of graphene surface plasmon polaritons (SPP). Our simulations show that inherently weak HCP features in the near-field can be strongly enhanced when coupled to graphene SPP in layered graphene/hexagonal boron nitride (hBN)/Bi-2212 heterostructures. This enhancement arises from our multilayered structures effectively acting as plasmonic cavities capable of altering collective modes of a layered superconductor by modifying its electromagnetic environment. The degree of enhancement can be selectively controlled by tuning the insulating spacer thickness with atomic precision. Finally, we verify the expected renormalization of room-temperature graphene SPP using near-field infrared imaging. Our modeling, augmented with data, attests to the validity of our approach for probing HCP modes in cuprate superconductors.

Tunable Dielectric and Thermal Properties of Oxide Dielectrics via Substrate Biasing in Plasma-Enhanced Atomic Layer Deposition.

The ability to control the properties of dielectric thin films on demand is of fundamental interest in nanoscale devices. Here, we modulate plasma characteristics at the surface of a substrate to tune both dielectric constant and thermal conductivity of amorphous thin films grown using plasma-enhanced atomic layer deposition. Specifically, we apply a substrate bias ranging from 0 to ∼117 V and demonstrate the systematic tunability of various material parameters of Al2O3. As a function of the substrate bias, we find a nonmonotonical evolution of intrinsic properties, including density, dielectric constant, and thermal conductivity. A key observation is that the maximum values in dielectric constant and effective thermal conductivity emerge at different substrate biases. The impact of density on both thermal conductivity and dielectric constant is further examined using a differential effective medium theory and the Clausius-Mossotti model, respectively. We find that the peak value in the dielectric constant deviates from the Clausius-Mossotti model, indicating the change of oxygen fraction in our thin films as a function of substrate bias. This finding suggests that the increased local strength of plasma sheath not only enhances material density but also controls the dynamics of microstructural defect formation beyond what is possible with conventional approaches. Based on our experimental observations and modeling, we further build a phenomenological relation between dielectric constant and thermal conductivity. Our results pave invaluable avenues for optimizing dielectric thin films at the atomic scale for a wide range of applications in nanoelectronics and energy devices.

Heteroepitaxial vertical perovskite hot-electron transistors down to the monolayer limit.

Two-dimensional heterostructures combined with vertical geometries are candidates to probe and utilize the physical properties of atomically-thin materials. The vertical configuration enables a unique form of hot-carrier spectroscopy as well as atomic-scale devices. Here, we present the room-temperature evolution of heteroepitaxial perovskite hot-electron transistors using a SrRuO3 base down to the monolayer limit (∼4 Å). As a fundamental electronic probe, we observe an abrupt transition in the hot-electron mean free path as a function of base thickness, coinciding with the thickness-dependent resistive transition. As a path towards devices, we demonstrate the integrated synthesis of perovskite one-dimensional electrical edge contacts using water-soluble and growth-compatible Sr3Al2O6 hard masks. Edge-contacted monolayer-base transistors exhibit on/off ratios reaching ∼108, complete electrostatic screening by the base manifesting pure hot-electron injection, and excellent scaling of the output current density with device dimensions. These results open new avenues for incorporating emergent phenomena at oxide interfaces and in heterostructures.

Impact of thermally dead volume on phonon conduction along silicon nanoladders.

Thermal conduction in complex periodic nanostructures remains a key area of open questions and research, and a particularly provocative and challenging detail is the impact of nanoscale material volumes that do not lie along the optimal line of sight for conduction. Here, we experimentally study thermal transport in silicon nanoladders, which feature two orthogonal heat conduction paths: unobstructed line-of-sight channels in the axial direction and interconnecting bridges between them. The nanoladders feature an array of rectangular holes in a 10 µm long straight beam with a 970 nm wide and 75 nm thick cross-section. We vary the pitch of these holes from 200 nm to 1100 nm to modulate the contribution of bridges to the net transport of heat in the axial direction. The effective thermal conductivity, corresponding to reduced heat flux, decreases from ∼45 W m-1 K-1 to ∼31 W m-1 K-1 with decreasing pitch. By solving the Boltzmann transport equation using phonon mean free paths taken from ab initio calculations, we model thermal transport in the nanoladders, and experimental results show excellent agreement with the predictions to within ∼11%. A combination of experiments and calculations shows that with decreasing pitch, thermal transport in nanoladders approaches the counterpart in a straight beam equivalent to the line-of-sight channels, indicating that the bridges constitute a thermally dead volume. This study suggests that ballistic effects are dictated by the line-of-sight channels, providing key insights into thermal conduction in nanostructured metamaterials.