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Infrared dielectric properties of muscovite mica, one of the first van der Waals crystals, exfoliated on silicon and SiO2 substrates is studied using near-field nano-FTIR spectroscopy. The spectra ...

Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and biomimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO 3 (Li-SNO) contains a large amount of mobile Li + located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li + conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na + . The results highlight the potential of quantum materials and emergent physics in design of ion conductors.

Recently emerged layered transition metal dichalcogenides have attracted great interest due to their intriguing fundamental physical properties and potential applications in optoelectronics. Using scattering-type scanning near-field optical microscope (s-SNOM) and theoretical modeling, we study propagating surface waves in the visible spectral range that are excited at sharp edges of layered transition metal dichalcogenides (TMDC) such as molybdenum disulfide and tungsten diselenide. These surface waves form fringes in s-SNOM measurements. By measuring how the fringes change when the sample is rotated with respect to the incident beam, we obtain evidence that exfoliated MoS2 on a silicon substrate supports two types of Zenneck surface waves that are predicted to exist in materials with large real and imaginary parts of the permittivity. We have compared MoS2 interference fringes with those formed on layered insulator such as hexagonal boron nitride where only leaky modes are possible due to its small permittivity. Interpretation of experimental data is supported by theoretical models. Our results could pave the way to the investigation of surface waves on TMDCs and other van der Waals materials and their novel photonics applications.

Materials that provide independent control of infrared thermal radiation and haze in the visible could benefit many areas and applications, including clothing, packaging and photovoltaics. Here, we study this possibility for a metamaterial composite paper based on cellulose nanofibrils (CNF) and silicon dioxide (SiO2) microparticles with infrared (IR) Frohlich phonon resonances. This CNF-SiO2 composite shows outstanding transparency in the visible wavelength range, with the option of controlling light diffusion and haze from almost zero to 90% by varying the SiO2 microparticle concentration. We further show that the transparent metamaterial paper could maintain high thermal emissivity in the atmospheric IR window, as attributed to strong IR absorption of both the nanocellulose and the resonant SiO2 microparticles. The high IR emissivity and low visible absorption make the paper suitable for passive radiative cooling and we demonstrate cooling of the paper to around 3 degrees C below ambient air temperature by exposing it to the sky. Funding Agencies|Knut and Allice Wallenberg Foundation via a Wallenberg Scholarship; Knut and Alice Wallenberg foundationKnut & Alice Wallenberg Foundation; Linkoping University; Wallenberg Wood Science Center; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009 00971]; Swedish Foundation for Strategic ResearchSwedish Foundation for Strategic Research; Swedish Armed Forces Research and Technology programme

Phase separations in ternary/multinary semiconductor alloys is a major challenge that limits optical and electronic internal device efficiency. We have found ubiquitous local phase separation in In1-xGaxN alloys that persists to nanoscale spatial extent by employing high-resolution nanoimaging technique. We lithographically patterned InN/sapphire substrates with nanolayers of In1-xGaxN down to few atomic layers thick that enabled us to calibrate the near-field infrared response of the semiconductor nanolayers as a function of composition and thickness. We also developed an advanced theoretical approach that considers the full geometry of the probe tip and all the sample and substrate layers. Combining experiment and theory, we identified and quantified phase separation in epitaxially grown individual nanoalloys. We found that the scale of the phase separation varies widely from particle to particle ranging from all Ga- to all In-rich regions and covering everything in between. We have found that between 20 and 25% of particles show some level of Ga-rich phase separation over the entire sample region, which is in qualitative agreement with the known phase diagram of In1-xGaxN system.

We have studied the formation of near-field fringes when sharp edges of materials are imaged using scattering-type scanning near-field optical microscope (s-SNOM). The materials we have investigated include dielectrics, metals, a near-perfect conductor, and those that possess anisotropic permittivity and hyperbolic dispersion. For our theoretical analysis, we use a technique that combines full-wave numerical simulations of tip-sample near-field interaction and signal demodulation at higher orders akin to what is done in typical s-SNOM experiments. Unlike previous tip-sample interaction near-field models, our advanced technique allows simulation of the realistic tip and sample structure. Our analysis clarifies edge imaging of recently emerged layered materials such as hexagonal boron nitride and transition metal dichalcogenides (in particular, molybdenum disulfide), as well as traditional plasmonic materials such as gold. Hexagonal boron nitride is studied at several wavelengths, including the wavelength where it possesses excitation of phonon-polaritons and hyperbolic dispersion. Based on our results of s-SNOM imaging in different demodulation orders, we specify resonant and non-resonant types of edges and describe the edge fringes for each case. We clarify near-field edge-fringe formation at material sharp boundaries, both outside bright fringes and the low-contrast region at the edge, and elaborate on the necessity of separating them from propagating waves on the surface of polaritonic materials.

Black phosphorus (BP) possesses several extraordinary physical properties, which include in-plane anisotropy, thickness dependent direct bandgap and high carrier mobility. These physical properties make BP highly desirable from the point of view of fundamental science and modern optoelectronics applications. The excitement about this material has always been accompanied by unreserved skepticism due to its extraordinary degradation under ambient conditions. Here we show ambient degradation of exfoliated BP can be effectively suppressed using thin layer of hybrid metal organic chemical vapor deposition coating of boron nitride (BN) followed by atomic layer deposition coating of Al2O3. We have extensively studied the time dependent surface, optical and electrical properties of BP encapsulated by BN and/or Al2O3 using nanoscale infrared imaging and I–V characterizations. Our results show hybrid thin layer (~5 nm) BN/Al2O3 coated BP exfoliated on SiO2 substrate is protected from degradation in ambient for over 6 months, much longer than those coated only by BN or Al2O3 layers. Our theoretical modeling of the experimental degradation growth pattern shows that the influence of neighboring elements on the degradation of a given element is minimal for BP flakes with hybrid coating. Electrical characterization further confirms the effectiveness of BN/Al2O3 as encapsulation layer and gate dielectrics with minor changes after several weeks.

The appearance of stripe phases is a characteristic signature of strongly correlated quantum materials, and its origin in phase-changing materials has only recently been recognized as the result of the delicate balance between atomic and mesoscopic materials properties. A vanadium dioxide (VO2) single crystal is one such strongly correlated material with stripe phases. Infrared nano-imaging on low-aspect-ratio, single-crystal VO2 microbeams decorated with resonant plasmonic nanoantennas reveals a novel herringbone pattern of coexisting metallic and insulating domains intercepted and altered by ferroelastic domains, unlike previous reports on high-aspect-ratio VO2 crystals where the coexisting metal/insulator domains appear as alternating stripe phases perpendicular to the growth axis. The metallic domains nucleate below the crystal surface and grow towards the surface with increasing temperature as suggested by the near-field plasmonic response of the gold nanorod antennas.

Black phosphorus (BP) is an emerging two-dimensional material with intriguing physical properties. It is highly anisotropic and highly tunable by means of both the number of monolayers and surface doping. Here, we experimentally investigate and theoretically interpret the near-field properties of a-few-atomic-monolayer nanoflakes of BP. We discover near-field patterns of bright outside fringes and a high surface polarizability of nanofilm BP consistent with its surface-metallic, plasmonic behavior at mid-infrared frequencies

Nanophotonic (nanoplasmonic) structures confine, guide, and concentrate light on the nanoscale. Advancement of nanophotonics critically depends on active nanoscale control of these phenomena. Localized control of the insulator and metallic phases of vanadium dioxide (VO2) would open up a universe of applications in nanophotonics via modulation of the local dielectric environment of nanophotonic structures allowing them to function as active devices. Here we show dynamic reversible control of VO2 insulator-to-metal transition (IMT) locally on the scale of 15 nm or less and control of nanoantennas, observed in the near-field for the first time. Using polarization-selective near-field imaging techniques, we monitor simultaneously the IMT in VO2 and the change of plasmons on gold infrared nanoantennas. Structured nanodomains of the metallic VO2 locally and reversibly transform infrared plasmonic dipolar antennas to monopole antennas. Fundamentally, the IMT in VO2 can be triggered on femtosecond timescale to allow ultrafast nanoscale control of optical phenomena. These unique capabilities open up exciting novel applications in active nanophotonics.